Title of Invention

SPIROINDOLINE DERIVATIVES HAVING INSECTICIDAL PROPERTIES

Abstract An insecticidal compound of formula (I), wherein Y is a single bond, C=O, C=S or S(O)m where m is 0, 1 or 2; R1, R2, R3, R4, R8 A1, A2, A3, A4, B1, B2, B3 and B4 are specified organic groups or salts or N-oxides thereof; compositions containing them and their using in controlling insects, acarines, nematodes or molluscs.
Full Text

SPIROINDOLINE DERIVATIVES HAVING INSECTICIDAL PROPERTIES
The present invention relates to spiroindoline derivatives, to processes for preparing them, to insecticidal, acaricidal, moiluscicidal andnematicidal compositions comprising them and to methods of using them to combat and control insect, acarine, mollusc and nematode pests.
Spiroindoline derivatives with pharmaceutical properties are disclosed in for example WO9S25605, WO9429309, W09E2S297 and WO9964002. Synthetic routes to selected compounds with pharmaceutical properties are described in Proc. Nati. Acad. Sci. USA (1995),"92, 7001, Tetrahedron (1997), 53, 109S3 and Tetrahedron Letters (1997), 38, 1497. It has C1-4w surprisingly been found that certain spiroindolines have insecticidal properties.
The present invention therefore provides a compound of formula (I):

wherein Y is a single bond, C=0, OS or S(0)m where m is 0, 1 or 2;
R1 is hydrogen, optionally substituted alkyl, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbony!, amiC1-4carbonyl, optionally substituted alkylamiC1-4carbonyl, optionally substituted dialkylamiC1-4carbonyl, optionally substituted aryl, optionally substituted heteroaryl, optionally substituted alkoxy, optionally substituted aryloxy, optionally substituted heteroaryloxy, optionally substituted heterocyclyloxy, cyaC1-4, optionally substituted alkenyl, optionally substituted alkynyl, optionally substituted cycloalkyl, optionally substituted cydoaOcenyl, formyl, optionally substituted heterocyclyl, optionally substituted alkyhhio, C1-4 or NR13RM where R13 and R14 are independently hydrogen, COR15, optionally substituted alkyl, optionally substituted aryl, optionally substituted heteroaryl, optionally substituted heterocyclyl or R13 and RH together with the N

atom to which they are attached form a group -N=C(Rl6)-NRnR18; R*5 is H, optionally substituted alkyl, optionally substituted alkoxy, optionally substituted aryl, optionally substituted aryloxy optionally substituted heteroaryl, optionally substituted heteroaryloxy or NRI9R20; R16,R17 and R18 are each independently H or lower alkyl; R19 and R20 are independently optionally substituted alkyl, optionally substituted aryl or optionally substituted heteroaryl;
R2 and R3 are independently hydrogen, halogen, cyaC1-4, optionally substituted alkyl, optionally substituted alkoxy or optionally substituted aryl;
each R4 is independently halogen, nitro, cyaC1-4, optionally substituted C1-8 alkyl, optionally substituted C2-6 alkenyl, optionally substituted C2-6 alkynyl, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbonyl, optionally substituted alkylamiC1-4carbonyl, optionally substituted dialkylamiC1-4carbonyl, optionally substituted C3-7 cycloalkyl, optionally substituted aryl, optionally substituted heteroaryl, optionally substituted heterocyclyl, optionally substituted alkoxy, optionally substituted aryloxy, optionally substituted heteroaryloxy, optionally substituted alkylthio or R21R22N where R21 and R are, independently, hydrogen, C1-8alkyl, C3.7 cycloalkyl, C3-6 alkenyl, C3.6 alkynyl, C3.7 cycloalkyl(C1-4)alkyl, C2-6 haloalkyl, d-o alkoxy(C1-6alkyl, C1-6alkoxycarbonyl or R21 and R together with the N atom to which they are attached form a five, six or seven-membered heterocyclic ring which may contain one or two further heteroatoms selected from O, N or S and which may be optionally substituted by one or two Ct-6 alkyl groups, or 2 adjacent groups R4 together with the carbon atoms to which they are attached form a 4, 5, 6,or 7 membered carbocyclic or heterocyclic ring which may be optionally substituted by halogen; n is 0,1,2, 3 or 4;
R is optionally substituted alkyl, optionally substituted alkenyl, optionally substituted alkynyl, optionally substituted cycloalkyl, optionally substituted aryl, optionally substituted alkoxy, optionally substituted aryloxy, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbonyl or optionally substituted alkenylcarbonyl; A1, A2, A3, A4, B1, B2, B3 and B4 are independently hydrogen, halogen, hydroxy, cyaC1-4, optionally substituted C1-8 alkyl, optionally substituted C2-6 alkenyl, optionally substituted C2-6 alkynyl, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbonyl, optionally substituted alkylamiC1-4carbonyl, optionally substituted dialkylamiC1-4carbonyl, optionally substituted C3-7 cycloalkyl, optionally substituted aryl, optionally substituted

heteroaryl, optionally substituted heterocyclyl, optionally substituted alkoxy, optionally substituted aryloxy, optionally substituted heteroaryloxy, optionally substituted alkylthio, optionally substituted arylthio or R"3R24N where R23 and R24 are, independently, hydrogen, C|_8 alkyl, C3.7 cycloalkyl, C3-6 alkenyl, C^ alkynyl, C3*7 cycloalkyl(Ci.4)alkyl, C2-6 haloalkyl, Cue alkoxy(Ci-6)alkyl, Cj-6 alkoxycarbonyl or R23 and R24 together with the N atom to which they are attached fonn a five, six or seven-membered heterocyclic ring which may contain one or two further heteraatoms selected from O, N or S and which may be optionally substituted by one or two C _* alley! groups, or Ai and A^ together are =0, or A3 and A-* together are =0, or B| and B2 together are =0, or B3 and B4 together are =0, or A1together with B\ is a bond, or A3 together with B3 is a bond,
or A1 together with A2 form with the carbon to which they are bound a three- to seven-membered ring, and may be saturated or unsaturated, and that may contain one or two hetero atoms selected from the group consisting of N, O and S, and which may be optionally substituted by one or two Cj.6 alkyl groups;
or Aj together with B1 form with the carbon to which they are bound a three- to seven-membered ring, and may be saturated or unsaturated, and that may contain one or two hetero atoms selected from the group consisting of N, O and S, and which maybe optionally substituted by one or two Cue alkyl groups;
or B1 together with B2 form with the carbon to which they are bound a three- to seven-membered ring, and may be saturated or unsaturated, and that may contain one or two hetero atoms selected from the group consisting of N, O and S, and which may be optionally substituted by one or two C\* alkyl groups; or A1 together with A3 form a group -CH2-, -CH=CH- or -CH2CH2; or B1 together with B3 form a group –CH2 -CH=CH- or -CH2CH2; or salts or N-oxides thereof provided that when B1, B2, B3 and B4 are all H, either both Aj and A2 are different from H or both A3 and A4 are different from H.

The compounds of formula (I) may exist in different geometric or optical isomers or tautomeric forms. This invention covers all such isomers and tautomers and mixtures thereof in all proportions as well as isotopic forms such as deuterated compounds.
Each alkyl moiety either alone or as part of a larger group (such as alkoxy, alkoxycarbonyl, alkylcarbonyl, alkylamiC1-4carbonyl, dialkylamiC1-4carbonyl) is a straight or branched chain and is, for example, methyl, ethyl, n-propyl, n-butyl, n-pentyl, n-hexyl, iso-propyl, n-butyl, sec-butyl, iso-butyi» tert-butyi or neo-pentyl. The alkyl groups are suitably C\ to Ci: alkyl groups, but are preferably C1-C6 more preferably C1-6even more preferably preferably C1-6and most preferably C1-C6; alkyl groups.
When present, the optional subsiituents on an alkyl moiety (alone or as part of a larger group such as alkoxy, alkoxycarbonyl, alkylcarbonyl, alkylamiC1-4carbonyl, dialkylamiC1-4carbonyl) include one or more of halogen, nitro, cyaC1-4, NCS-, C3-7 cycloalkyl (itself optionally substituted with C1-C6 alkyl or halogen), C5-7 cycloalkenyl (itself optionally substituted with C1-6 alkyl or halogen), hydroxy, Ci-io alkoxy, C1-6 alkoxy(Ct_io)alkoxy, tri(C1-4)alkylsilyl(C1-6)alkoxy, C1-6 alkoxycarbonyl(Ci-io)alkoxy, C1-10 haloalkoxy, aryl(CM)-alkoxy (where the aryl group is'optionally substituted), C3-7 cycloalkyloxy (where the cycloalkyl group is optionally substituted with C1-6 alkyl or halogen), C2-10 alkenyloxy, C2.10 alkynyloxy, SH, C1-6 alkylthio, Ci-io haloalkylthio, aryl(C1-4)alkylthio (where the aryl group is optionally substituted), C3.7 cycloalkyhhio (where the cycloalkyl group is optionally substituted with C\.e alkyl or halogen), tri(CM)alkylsilyl(Ci,6)alkylthio, arylthio (where the aryl group is optionally substituted), C\+ alkylsulfonyl, Ci-e haloalkylsulfonyl, C1-6 alkylsulfmyl, Ci-6 haloalkylsulfinyl, arylsulfonyl (where the aryl group may be optionally substituted), tri(Ci_4)alkylsilyl, aryldi(CM>alkylsilyl, (Ci-Oalkjidiarylsilyl, triarylsilyl, C1-6 alkylcarbonyl, HO2C, C1-6 alkoxycarbonyl, amiC1-4carbonyl, Ci-6 alkylamiC1-4carbonyl, di(Ci-$ alkyl)amiC1-4carbonyl, N-(Ct-3 alky!)-N-(C1-3 alkoxy)amiC1-4carbonyl, Ci-6 alkylcarbonyloxy, arylcarbonyloxy (where the aryl group is optionally substituted), di(Cu6)aikylamiC1-4carbonyloxy, oxiroes such as =C1-4alkyl, =C1-4haloalkyl and =C1-4aryl (itself optionally substituted), aryl (itself optionally substituted), heteroaryl (itself optionally substituted), heterocyclyl (itself optionally substituted with Ci-e alkyl or halogen), aryloxy (where the aryl group is optionally substituted), heteroaryloxy, (where the heteroaryl group is optionally substituted), heterocyclyloxy (where the heterocyclyl group is optionally substituted with Ci-6 alkyl or halogen), amiC1-4, d-6 alkylamiC1-4, di(C].6)alkylamiC1-4, Ci-6

alkylcarbonylamiC1-4, N-(Ci-6)alkylcarbonyI-N-(Ci.6)alkylamiC1-4, C2.6 alkenylcarbonyl, C2-6 alkynylcarbonyl, C3.6 alkenyloxycarbonyl, C1-4 alkynyloxycarbonyl, aryloxycarbonyl (where the aryl group is optionally substituted) and arylcarbonyl (where the aryl group is optionally substituted).
Alkenyl and alkynyl moieties can be in the form of straight or branched chains, and the alkenyl moieties, where appropriate, can be of either the (E)- or (Z)-configuration. Examples are vinyl, allyl and propargyL
When present, the optional substituents on alkenyl or alkynyl include those optional substituents given above for an alkyl moiety.
In the context of this specification acyl is optionally substituted C1-6 alkylcarbonyl (for example acetyl), optionally substituted C2-6 alkenylcarbonyl, optionally substituted C2.6 alkynylcarbonyl, optionally substituted arylcarbonyl (for example benzoyl) or optionally substituted heteroarylcarbonyl.
Halogen is fluorine, chlorine, bromine or iodine.
Haloalkyl groups are alky] groups which are substituted with one or more of the same or different halogen atoms and are, for example, CF3, CF2CI, CF3CH2 or CHF2CH2.
In the context of the present specification the terms "aryl" and "aromatic ring system" refer to ring systems which may be moC1-4-, B1- or tricyclic. Examples of such rings include phenyl, naphthalenyl, anthracenyi, indenyl or phenanthrenyl. A preferred aryl group is phenyl. In addition, the terms "heteroaryr, "heteroaromatic ring" or "heteroaromatic ring
system" refer to an aromatic ring system containing at least one heteroatom and consisting
*
either of a single ring or of two or more fused rings. Preferably, single rings will contain up to three and B1cyclic systems up to four heteroatoms which will preferably be chosen from nitrogen, oxygen and sulphur. Examples of such groups include furyl, thienyl, pyrrolyl, pyrazolyl, imidazolyl, 1,2,3-triazoIyi, 1,2,4-triazolyl, oxazolyl, isoxazolyl, thiazolyl, isothiazolyi, 1,2,3-oxadiazolyl, 1,2,4-oxadiazolyl, 1,3,4-oxadiazolyl, 1,2,5-oxadiazolyl, 1,2,3-thiadiazolyI, 1,2,4-thiadiazolyI, 1,3,4-thiadiazolyl, 1,2,5-thiadiazolyl, pyridyl, pyrimidinyl, pyridazinyl, pyrazinyl, 1,23-triazinyl, 1,2,4-triazinyl, 1,3,5-triazinyl, benzofuryl, benzisofuryl, benzothienyl, benzisothienyl, indolyl, isoindolyl, indazolyl, benzothiazolyl, benzisothiazolyl, benzoxazolyl, benzisoxazolyl, benzimidazolyl, 2,1,3-benzoxadiazole quiC1-4linyl, isoquiC1-4linyl, cinC1-4linyl, phthalazinyl, quinazolinyl, quiC1-4xalinyl, naphthyridinyl, benzotriazinyl, purinyl, pteridinyl and indolizinyl. Preferred

examples of heteroaromalic radicals include pyridyl, pyrimidyl, triazinyl, thienyl, furyl, oxazolyl, isoxazolyl, 2,1,3-benzoxadiazole and thiazolyl.
The terms heterocycle and heterocyclyl refer to a C1-4n-aromatic ring containing up to 10 atoms including one or more (preferably one or two) heteroatoms selected from O, S and N. Examples of such rings include 1,3-dioxolane, tetrahydrofuran and morpholine.
When present, the optional substtfuents on heterocyclyl include Ci-6 alkyl and 0.6 haloalkyl as well as those optional substituents given above for an alkyl moiety.
Cycloalkyl includes cyclopropyi, cyclopentyl and cyclohexyl.
Cycloalkenyl includes cyclopentenyl and cyclohexenyl.
When present, the optional substituents on cycloalkyl or cycloalkenyl include Cj-3 alkyl as well as those optional substituents given above for an alkyl moiety.
Carbocyclic rings include aryl, cycloalkyl and cycloalkenyl groups.
When present, the optional substituents on aryl or heteroaryl are selected independently, from halogen, nitro, cyaC1-4, NCS-, C1-6 alkyl, C1-6haloalkyl, C1-6 alkoxy-(Ci.6)alkyl, C2-6 alkenyl, C0.6 haloalkenyl, C2-6 alkynyl, C3.7 cycloalkyl (itself optionally substituted with C1-6 alky) or halogen), C5.7 cycloalkenyl (itself optionally substituted with C1.6 alkyl or halogen), hydroxy, C1-6 alkoxy, C1-6 alkoxy(Ci-io)alkoxy, tri(CM)aIkyl-silyl(C1-6)alkoxy, C1-6 alkoxycarbonyl(C1.10)alkoxy, C1-10 haloalkoxy, aryl(CM)alkoxy (where the aryl group is optionally substituted with halogen or C1-6 alkyl), C3.7 cycloalkyloxy (where the cycloalkyl group is optionally substituted with C1-6 alkyl or halogen), C2-J0 alkenyloxy, C2-10 alkynyloxy, SH, C1-6 alkylthio, C1-6 haloalkylthio, aryI(CM)aIkylthio C3.7 cycloalkylthio (where the cycloalkyl group is optionally substituted with Cj-6 alkyl or halogen), tri(CM)-alkylsilyl(Ci4)alkylthio, arylthto, Ci-6 alkylsulfonyl, 0.6 haloalkylsulfonyl, C\^ alkylsulfinyl, CMhaloalkylsulfinyl, arylsulfonyl, tri(C)-4)alkylsilyl, aryldi(CM)-alkylsilyl, (CM)alkyldiarylsilyl, triarylsilyl, C1-6 alkylcarbonyl, H02C, C1-6 alkoxycarbonyl, amiC1-4carbonyl, Cn afkylamiC1-4carbonyl, di(d-6 alkyl)-amiC1-4carbonyl, N-(C1-3 alkyl)-N-(Ci-3 alkoxy)amiC1-4carbonyl,Ci-« alkylcarbonyloxy, arylcarbonyloxy, di(Ci.6)alkylamiC1-4-carbonyloxy, aryl (itself optionally substituted with Ci_6 alkyl or halogen), heteroaryl (itself optionally substituted with O* alkyl or halogen), heterocyclyl (itself optionally substituted with C1-6 alkyl or halogen), aryloxy (where the aryl group is optionally substituted with C1-6 alkyl or halogen), heteroaryloxy (where the heteroaryl group is optionally substituted with C1-6 alkyl of halogen), heterocyclyloxy (where the heterocyclyl

group is optionally substituted with Cj^ alkyl or halogen), amiC1-4, C1-6 alkylamiC1-4, di(Cj. 6)alkylamiC1-4, Ci-6 alkylcarbonylamiC1-4, N-(C1-6)aIkylcarbonyl-N-(C].6)alkylamiC1-4, arylcarbonyl, (where the aryl group is itself optionally substituted with halogen or d-6 alkyl) or two adjacent positions on an aryl or heteroaryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen or Ci^ alkyl. Further substituents for aryl or heteroaryl include aryl carbonyl amiC1-4 (where the aryl group is substituted by Ci_6 alkyl or halogen), (C|^)alkyloxycarbonylamiC1-4 (Ci^)alkyloxycarbonyl-N-(Ci-6)alkylamiC1-4, aryloxycarbonylamiC1-4 (where the aryl group is substituted by Cj-6 alkyl or halogen), aryioxycart>onyl-N-(Ci.6)alkylamiC1-4, (where the aryl group is substituted by C\* alkyl or halogen), arylsulphonylamiC1-4 (where the aryl group is substituted by Ci-6 alkyl or halogen), arylsulphonyl-N-(C].6)alkylamiC1-4 (where the aryl group is substituted by Ci-6 alkyl or halogen), aryl-N-(Ci_6)aIkylamiC1-4 (where the aryl group is substituted by Cj.6 alkyl or halogen), arylamiC1-4 (where the aryl group is substituted by Ci.6 alkyl or halogen), heteroaryl amiC1-4 (where the heteroaryl group is substituted by Ci-6 alkyl or halogen), heterocyclylamiC1-4 (where the heterocyclyl group is substituted by Q-e alkyl or halogen), amiC1-4carbonylamiC1-4, Ci-ealkylamiC1-4carbonyl amiC1-4, di(Ci-6)alkylamiC1-4carbonyl amiC1-4, arylamiC1-4carbonyl amiC1-4 where the aryl group is substituted by Ci-6 alkyl or halo^cn\ ?.rv!-N-^Cj.*^3lkvl»niiC1-4c?iii>onvlayn!C1-4 where the aiM o*oun is substituted by C\-$ alkyl or halogen), Ci-6alkylamiC1-4carbooyl-N-(Ci-6)aIkyl amiC1-4, di(Ci-6)alkylamiC1-4carbonyl-N-(Ci-6)alkyl amiC1-4, arylamiC1-4carixaij4-N-(Ci^)alkyl amiC1-4 where the aryl group is substituted by Q-6 alkyl or halogen) and aryl-N»(Ci.6)alkylamiC1-4carbonyl-N-(Ci-6)alkyI amiC1-4 where the aryl group is substituted by C|^ alkyl or halogen).
For substituted phenyl moieties, heterocyclyl and heteroaryl groups it is preferred that one or more substituents are independently selected from halogen, C\* alkyl, Q-6 haloalkyl, Ci-6 alkoxy(C|-6)alkyl, C\^ alkoxy, O* haloalkoxy, Ci-e alkylthio, Ci-6 haloalkylthio, C\s alkylsulfinyl, C\^ haloalkylsulfinyl, C\* alkylsulfonyl, Ci-6 haloalkylsulfonyl, C2-6 alkenyl, C2-6 haloalkenyl, C2-6 alkynyl, C3.7 cycloalkyl, nitro, cyaC1-4, CO2H, Ci-6 alkylcarbonyl, Ci-$ alkoxycarbonyl, R25R26N or R27R2*NC(0); wherein R25, R26, R27 and R28 are, independently, hydrogen or Ci-6 alkyl. Further preferred substituents are aryl and heteroaryl groups.
Haloalkenyl groups are alkenyl groups which are substituted with one or more of the same or different halogen atoms.It is to be understood that dialkylamiC1-4 substituents include those where the dialkyl groups together with the N atom to which they are attached form a five, six or seven-membered heterocyclic ring which may contain one or two further heteroatoms selected from O, N or S and which is optionally substituted by one or two independently selected (Ci^)alkyl groups. When heterocyclic rings are formed by joining two groups on an N atom, the resulting rings are suitably pyrrolidine, piperidine, thiomorpholine andmorpholine each of which may be substituted by one or two independently selected (Cu) alkyl groups.
Preferably the optional substituents on an alkyl moiety include one or more of halogen, nitro, cyaC1-4, HO2C, Q.10 alkoxy (itself optionally substituted by C1-6 alkoxy), aryl(Ci-4)alkoxy, C1-6 alkylthio, Ct-ioalkyicarbonyl, CLIO alkoxycarbonyl, Cue alkylamiC1-4carbonyl, di(Ci.e alkyl)amiC1-4carbonyl, (C\. Preferably the optional substituents on alkenyl or alkynyl include one or more of
*
halogen, aryl and C3.7 cycloalkyl.
A preferred optional substituent for heterocyclyl is C\* alkyl.
Preferably the optional substituents for cycloalkyl include halogen, cyaC1-4 and C1-3 alkyl.
Preferably the optional substituents for cycloalkenyl include C1.3 alkyl, halogen and cyaC1-4.
Preferably Y is a single bond, C=0 or S(0)m where m is 0,1 or 2.
More preferably Y is a single bond, C=0 or SO2.
Yet more preferably Y is a single bond or C=0.
Most preferably Y is C=0.
Preferably R1 is hydrogen, Cj-6 aflcyi, C\^ cyaC1-4alkyl, Cj-6 haloalkyl, C3-7 cycloalkyl(CM)alkyl, Ci-6 alkoxy(Ci^)alk>i, heteroaryl(Ci-6)alkyl (wherein the heteroaryl group maybe optionally substituted by halo, nitro, cyaC1-4, Ci-e alkyl, Q.6 haloalkyl, C1.6 alkoxy, Ci-6 haloalkoxy, Ci* alkylsulfonyl, C\* alkylsulfinyl, Ci-6 alkylthio, C\* alkoxycarbonyl, C\* alkylcaibonylamiC1-4, ar>icarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5,6 or 7 membered carbocyclic or heterocyclic
ring, itself optionally substituted with halogen), aryl(Ci.6)alkyl (wherein the aryl group may be optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, Ci-6 alkoxy, CM haloalkoxy, CM alkylsulfonyl, CM alkylsulfinyl, CM alkylthio, Ci-e alkoxycarbonyl, CM alkylcarbonylamiC1-4, arylcarbonyl, or two adjacent positions on the aryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), CM alkylcarbonylamtC1-4(C|.6)alkyl, aryl (which may be optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy, CM haloalkoxy, CM alkylsulfonyl, CM alkylsulfinyl, CM alkykhio, CM alkoxycarbonyl, CM alkylcarbonylamiC1-4, arylcarbonyl, or two adjacent positions cm the aryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), heteroaryl (which may be optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, C|-6 alkoxy, CM haloalkoxy, CM alkylsulfonyl, CM alkylsulfinyl, CM alkylthio, Ci-6 alkoxycarbonyl, Ci-6 alkylcarbonylamiC1-4, arylcarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), Ci-6 alkoxy, CM haloalkoxy, pheC1-4xy (wherein the phenyl group is optionally substituted by halogen, CM alkyl, CM alkoxy, CM haloalkyl, CM haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylarniC1-4), heteroaryloxy fontionallv substituted bv halo, nitro. cvaC1-4. Ci_« alkvl. Ci * haloalkvl. f\ haloalkoxy), heterocyclyloxy (optionally substituted by halo, CM alkyl, Cj-e'haloalkyl, CM alkoxy or C1-6 haloalkoxy), cyaC1-4, C2-6 alkenyi, C2-6 alkynyl, C3-6 cycloalkyl, C5.7 cycloalkenyl, heterocyclyl (optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy or CM haloalkoxy), CM alkylthio, CM haloalkylthio or NRI3R14 where R13 and R14 are independently hydrogen, Ci-6 alkyl, CM haloalkyl, CM alkoxy(Ci_ e)alkyl, phenyl (which may be optionally substituted by halogen, CM alkyl, CM alkoxy, CM haloalkyl, CM haloalkoxy, CN, C1-42, ayi, heteroaryl, amiC1-4, dialkylarniC1-4 or CM alkoxycarbonyl), phenyl (O^alkyl (wherein the phenyl group may be optionally substituted by halogen, C\^ alkyl, CM alkoxy, CM haloalkyl, C\^ haloalkoxy, CN, N02, aryl, heteroaryl, amiC1-4, dialkylarniC1-4, CM alkylsulfonyl, CM alkoxycarbonyl, or two adjacent positions on the phenyl ring may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), heteroaryl (Ci^)alkyl (wherein the heteroaryl group may be optionally substituted by halo, nitro, cyaC1-4, CM alkyl, d-6 haloalkyl, CM alkoxy, CM haloalkoxy. CM alkylsulfonyl, CM alkylsulfinyl, CM alkylthio,
C|-6 alkoxycarbonyl, CM alkylcarbonylamiC1-4, arylcarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen) or heteroaryl (which may be optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy or Ci-6 haloalkoxy, C|. 4 alkoxycarbonyl CM alkylcarbonylamiC1-4. phenyJoxycarbonylamiC1-4 (wherein the phenyl group is optionally substituted by halogen, CM alkyl, CUA alkoxy, CM haloalkyl, CM haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), amiC1-4, CM alkylamiC1-4 or phenylamiC1-4 (wherein the phenyl group is optionally substituted halogen, CM alkyl, CM alkoxy, CUA haloalkyl. CM haloalkoxy, CN, C1-4?, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4)). More preferably R1 is Ci-6 alkyl, CM haloalkyl, C\.6 alkoxy(Ci-6)alkyl, heteroaryl(C|. 3)alkyl (wherein the heteroaryl group may be optionally substituted by halo, nitro, cyaC1-4, CM alkyl, Ci-6 haloalkyl, CM alkoxy, CM haloalkoxy, CM alkylsulfonyl, CM alkoxycarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), phenyl(Ci-3)alkyl (wherein the phenyl group may be optionally substituted by halogen, CM alkyl, CM alkoxy, CM haloalkyl, CM haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4, dialkylamiC1-4, CM alkylsulfonyl, Ci-6 alkoxycarbonyl, or two adjacent positions on the phenyl ring may be cyclised to form a 5,6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), phenyl (which may be optionally substituted by halogen, CM alkyl, CM alkoxy, C\^ haloalkyl, C}^ haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4, dialkylamiC1-4, Ci-6 alkylsulfonyl, CM alkoxycarbonyl, or two adjacent positions on the phenyl ring may be cyclised to form a 5,6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), heteroaryl (which may be optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy, CM haloalkoxy, CM alkylsulfonyl, CM alkoxycarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5,6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), CM alkoxy, CM haloalkoxy, C2-6 alkenyl, heterocyclyl (optionally substituted by halo, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy or Cue haloalkoxy), CM alkylthio, CM haloalkylthio or NR,3RU where R13 and R14 are independently hydrogen, Cue alkyl or CM haloalkyl, CM a!koxy(CM)*IkyU C2-6 alkylcarbonyl, phenylcarbonyl, (where the phenyl is optionally substituted by halogen, C\* alkyl, CM alkoxy, CM haloalkyl, C\^ haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), phenyl(Ci_3)alkyl (wherein

the phenyl group may be optionally substituted by halogen, CM alkyl, CM alkoxy, CM haloalkyl, CM haloalkoxy, CN, N02, aryl, heteroaryl, amiC1-4, dialkylamiC1-4, Cj.6 alkylsulfonyl, Q-6 alkoxycarbonyl, or two adjacent positions on the phenyl ring may be cyclised to form a 5,6 or 7 membered carbocycKc or heterocyclic ring, itself optionally substituted with halogen) or heteroaryl(Ci.3)aIkyI (wherein the heteroaryl group may be optionally substituted by halo, nitro, cyaC1-4, C-L-6 aikyl, C»^ haloalkyl, C\.e alkoxy, C^ haloalkoxy, Ci-e alkylsulfonyl, C\^ aDcyisuliinyi, CM alkylthio, Cj.6 alkoxycarbonyl, O* alkylcarbonylamiC1-4, arylcarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5, 6 or 7 membered caubocyclic or heterocyclic ring, itself optionally substituted with halogen).
Even more preferably R1 is Q.e alky!, Cue haloalkyl, heteroaryl(Cio)alkyl (wherein the heteroaryl group may be optionally substituted by halo, cyaC1-4, Ci-c alkyl, Cj.6 haloalkyl and where the heteroaryl group is a thiazole, pyridine, pyrimidine, pyrazine or pyridazine ring), heteroaryl (optionally substituted by halo, cyaC1-4, Cue alkyl, Ci-6 haloalkyl and where the heteroaryl group is a pyridine, pyrimidine, 2,1,3-benzoxadiazole, pyrazine or pyridazine ring), d-6 alkoxy, Ci* alkoxy(C|-$)alkyl, Cj-6 alkylamiC1-4, C1-6alkoxy(Ci.6)alkylamiC1-4 or heteroaryl(Cio)a!kylamiC1-4 (wherein the heteroaryl group may be optionally substituted by halo, cyaC1-4, C?-* alkyl. Ci.* haloalkyl and where the heteroaryl group is a thiazole, pyridine, pyrimidine, pyrazine or pyridazine ring).
Most preferably R1 is pyridyl (optionally substituted by halo, Cio alkyl or C1-3 haloalkyl) especially halo-substituted pyridyL
It is preferred that R2 and R3 are independently hydrogen, Cj-e alkyl, Cut haloalkyl, C|-6 alkoxy or cyaC1-4.
More preferably R and R are independently hydrogen, halogen, C1.2 alkyl, C1-2 haloalkyl, C1.2 alkoxy, cyaC1-4.
Even more preferably R2 and R3 are independently hydrogen or CM alkyl.
Yet more preferably R2 and R3 are independently hydrogen or methyl.
Most preferably R2 and R3 are both hydrogen.
Preferably each R4 is independently halogen, cyaC1-4, C\-% alkyl, C|.g haloalkyl, Q* cyaC1-4alkyl, d-6 alkoxy(Ci-6)alkyl, C3-7 cycJoaIkyl(Cj^)alkyl, C5-$ cycloalkenyl(C|^)alkyI, C3-6 a!kenyloxy(Ci^)aIkyl, C^ aIkynyk>x) alkyl, Ci-6 a!koxycarbonyl(CN6)alkyl, C3-6 alkenyioxycarbonyl(Ci-6)alky!, C3.6 aIkyny]oxycarbonyl(C|.6)alkyl, aryloxycarbonyl(Ci.6)alkyl, CM alkylthio(C|.0)alkyl, C,_6 alkylsulf\nyKCi.6)alkyl, CM alkylsulfonyi(CM)alkyl, amiC1-4carbonyl(CM)alkyl, Ci-6 alkylamiC1-4carbonyl(Ci-6)alkyI, di(CM)alkylamiC1-4carbonyKCM)alkyl, phenyl(CM)alkyl (wherein the phenyl group is optionally substituted by halogen, CM alkyl, CM alkoxy, CM haloalkyl, C1.4 haloalkoxy, CN, C1-42, aryL heteroaryl, amiC1-4 or dialkylamiC1-4), heteroaryl(Ci-4)alkyl (wherein the heteroaryl group is optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haJoalky], CM alkoxy or CM haloalkoxy), heterocyclyl(CM)alkyl (wherein the heterocyclyl group is optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy or CM haloalkoxy), C2-6 alkenyl, amiC1-4carbonyl(C2-6)alkenyl, CM
alkylamiC1-4carbonyl(C2-6)alkenyl, di(Cj-6)alkylamiC1-4carbonyl(C2.6)alkenyl, phenyl(C2-4)-alkenyl, (wherein the phenyl group is optionally substituted by halogen, CM alkyl, CM alkoxy, CM haloalkyl, CM haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), Q-6 alkynyl, trimethylsiIyI(C2-6)alkynyl, amiC1-4carbonyl(C2-6)aIkynyI, CM alkylarniC1-4carbonyl(C2.6)alkynyl, di(Ci-6)alkylamiC1-4carbonyl(C2-6)alkynyl,Ci.6 alkoxycarbonyl, C3-7 cycloalkyl, C3.7 halocycloalkyl, C3.7 cyaC1-4cycloalkyl, C1-3 alkyl(C3-7)-cycloalkyl, C1.3 alkyl(C3.7)halocycloalkyl,phenyl (optionally substituted by halogen, Cu4 alkyl, CM alkoxy, CM haloalkyl, CM haloalkoxy, CN, C1-4?, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), heteroaryl (optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, Ci-6 alkoxy or CM haloalkoxy), heterocyclyl (wherein the heterocyclyl group is optionally substituted by halo, nitro, cyaC1-4. CM alkyl, CM haloalkyl, CM alkoxy or CM haloalkoxy), or 2 adjacent groups R4 together with the carbon atoms to which they are attached form a 4, 5,6 or 7 membered carbocyiic or heterocyclic ring which may be optionally substituted by halogen, C|.g alkoxy, CM haloalkoxy, pheC1-4xy (optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy or CM haloalkoxy), heteroaryloxy (optionally substituted by halo, nitro, cyaC1-4, CM alkyl, CM haloalkyl, CM alkoxy or Cue haloalkoxy), CM alkylthio or R'V^N where R19 and R20 are, independently, hydrogen, Ci-g alkyl, C3-7 cycloalkyl, QM alkenyl, C%4 alkynyl, C2* haloalkyl, CM alkoxycarbonyl or R19 and R20 together with the N atom to which they are attached form a five, six or seven-membered heterocyclic ring which may contain one or two further heteroatoms selected from O, N or S and which may be optionally substituted by one or two CM alkyl groups; n is 0, 1, 2 or 3.More preferably each R4 is independently halogen, cyaC1-4, C1-8 alkyl, C1-8 haloalkyl, C1-8 cyaC1-4alkyl, C1-6 alkoxy(C1-6)a!kyl, C2-6 alkynyl, trimethylsiiyl(C2-6)aIkynyl, C1-6 alkoxycarbonyl, C3.7 cycloalkyl, C1-3 alkyl (C3.7) cycloalkyl, phenyl (optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), heterocyclyl (optionally substituted by halo, nitro, cyaC1-4, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy or C1-6 haloalkoxy), C1-8 alkoxy, C1-6 haloalkoxy, pheC1-4xy (optionally substituted by halogen, C1-4 alkyl. C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), heteroaryloxy (optionally substituted by halo, nitro, cyaC1-4, C1-3 alkyl, C1-3 haloalkyl, C1-3 alkoxy or C1-3 haloalkoxy), di(C1-8)alkylamiC1-4, or 2 adjacent groups R4 together with the carbon atoms to which they are attached form a 4, 5, 6 or 7 membered carbocylic or heterocyclic ring which may be optionally substituted by halogen; n is 0,1,2 or 3.
Even more preferably each R4 is independently halogen, cyaC1-4, C1-8 alkyl, C1-8 haloalkyl, C1-8 cyaC1-4alkyl, C1-6 alkoxy(C1-6)alkyl, Co-6 alkynyl, heterocyclyl (optionally substituted by C1-4 alkyl), C1-4 alkoxy, C1-4 haloalkoxy, pheC1-4xy (optionally substituted by halo, cyaC1-4, C1-3 alkyl or C1.3 haloalkyl), heteroaryloxy (optionally substituted by halo, cyaC1-4, C1-3 alkyl or C1.3 haloalkyl), di(C|.8)alkylamiC1-4 or 2 adjacent groups R4 together with the carbon atoms to which they are attached form a 4. 5, 6 or 7 membered carbocylic or heterocyclic ring which may be optionally substituted by halogen; n is 0, 1, 2 or 3.
Yet more preferably each R4 is independently fluoro, chloro, bromo, cyaC1-4, C1-4 alkyl, C1-4 haloalkyl, C1-4 cyaC1-4alkyl orCi.3 alkoxy(Cj-3)alkyl; n is 0, 1 or 2.
Most preferably each R4 is independently fluoro, chloro, bromo, C1-4 alkyl or C1-4 haloalkyl; n is 1 or 2.
Preferably R8 is C1-4O alkyl, C1-4O haloalkyl, aryl(Ci_6)alkyl (wherein the aryl group is optionally substituted by halogen, C\^ alkyl, C}^ alkoxy, C1-4 haloalkyl, C\^ haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), heteroaryl(Ci^)alkyl (wherein the heteroaryl group is optionally substituted by halogen, C\^ alkyl, C\^ alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), arylcarbonyl-(C1-6)alkyl (wherein the aryl group may be optionally substituted by halogen, C1-4 alkyl, C\^ alkoxy, Cj. 4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4 and the alkyl group may be optionally substituted by aryl), C2^ alkenyl, C2-8 haloalkenyl, aryl(C2-6)-alkenyl (wherein the aryl group is optionally substituted halogen, C1-4 alkyl, C1-4 alkoxy, C1-6haloalkyl, C1-4 haloalkoxy, CN, C1-4:, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4, C1-6 alkoxycarbonyl, or two adjacent substituents can cyclise to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring), heleroaryl(C2-6)-alkenyl (wherein the heteroaryl group is optionally substituted halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4, C1-6 alkoxycarbonyl, or two adjacent substituents can cyclise to form a 5,6 or 7 membered carbocyclic or heterocyclic ring), C2-6 alkynyl, phenyl(C2-6)alkynyl (wherein the phenyl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), C3.7 cycloalkyl, C1-6 alkoxycarbonyi, C1-6 alkylcarbonyl, C1-6 haloalkylcarbonyl or aryl(C2-6)alkenylcarbony! (wherein the aryl group may be optionally substituted halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), or -C(R5I)(R52)-[CR53=CR 54]z-R55 where z is 1 or 2, R51 and R52 are each independently H, halo or C1-2 alkyl, R53 and R54 are each independently H, halogen, C1-4 alkyl or C\.4 haloalkyl and R55 is optionally substituted aryl or optionally substituted heteroaryl.
More preferably R8 is phenyl(C1-4)alkyl (wherein the phenyl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), heteroaryl(C1-6)alkyl (wherein the heteroaryl group is optionally substituted halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), phenyl(C2-6)alkenyl (wherein the phenyl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4), heteroaryl(C2-6)alkenyl (wherein the heteroaryl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4) or phenyl(C2-6)a!kynyl (wherein the phenyl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, C1-42, aryl* heteroaryl, amiC1-4 or dialkylamiC1-4, or -C(R51)(R52MCR53=CR54]z-R55 where z is 1 or 2, R51 and R52 are each independently H, halo or C1-2 alkyl, R53 and R54 are each independently H, halogen, C1-4 alkyl or C1-4 haloalkyl and R55 is optionally substituted aryl or optionally substituted heteroaryl.
Most preferably RB is-C(R51)(R52MCR53=CR54]z-R55 where z is 1 or 2, preferably 1, R51 and R52 are each independently H, halo or C1-2 alkyl, R53 and R54 are each independently H, halogen, C1-4 alkyl or C1-4 haloalkyl and R55 is phenyl substituted by halogen, C1-4 alkyl,

Ci-4 alkoxy, C1-4 haloalkyl, Cj-4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4 or heteroaryl substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C|. 4 haloalkoxy, CN, C1-42, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4.
R51 and R52 are preferably hydrogen.
R53 and R54 are preferably hydrogen or halogen, especially hydrogen. R55 is preferably phenyl substituted with one to three substituents selected from halogen, C1-4 alkyl, C\JI alkoxy, Cj^ haloalkyl, C1-4 haloalkoxy, CN, C1-4?, aryl, heteroaryl, amiC1-4 or dialkylamiC1-4.
Preferably Ai, A2, A3, A», 81,82,83 and B4 are independently each hydrogen, halo, cyaC1-4, C1-4 alkyl, hydroxy or two groups attached to the same carbon atom together with the carbon atom form a carbonyl group.
More preferably At, A2, A3, A4, B1, B2* B3 and B4 are independently independently hydrogen, fluoro, methyl, hydroxy or two groups or two groups attached to the same carbon atom together with the carbon atom form a carbonyl group.
One group of preferred compounds of formula (I) are those where Yis C(O) and R] is NRI3RM where R13 and R14 are as defined above.
The compounds in Tables I to MCLXVII below illustrate the compounds of the invention.
Table I provides 782 compounds of formula la

wherein Ai is hydrogen, B\ is CH3f B2, B3 and B* are all hydrogen and the values of R4*' R4b' R4c'R4d and R8 are given in Table 1




















































1
Table II provides 782 compounds of formula lb

wherein A* is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R8 are given in Table 1.
Table III provides 782 compounds of formula k


wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table IV provides 782 compounds of formula Id

wherein Aj is hydrogen, Bt is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c* R4d and R8 are given in Table 1.
Table V provides 782 compounds of formula le


wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4bt R4c- R4d and R8 are given in Table 1.
Table VI provides 782 compounds of formula If

wherein Aj is hydrogen, B| is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4* and R8 are given in Table 1.
Table VII provides 782 compounds of formula Ig


wherein Ai is hydrogen, B\ is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b? R4c' R4d and R8 are given in Table 1.
Table VIII provides 782 compounds of formula Ih

wherein Aj is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4d and R8 are given in Table 1.
Table IX provides 782 compounds of formula H


wherein Ai is hydrogen, B1 is CH3, B?, B3 and B4 are ail hydrogen and the values of R4a' R4b' R4c'R4d and R8are given in Table 1.
Table X provides 782 compounds of formula Ij

wherein A\ is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4Cl R4d and R8 are given in Table 1.
Table XI provides 782 compounds of formula Ik


wherein A1is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c'R4d and R8are given in Table 1.
Table XII provides 782 compounds of formula II

wherein A\ is hydrogen, B\ is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4c" R4d and R8 are given in Table 1.
Table XIII provides 782 compounds of formula Im

wherein A] is hydrogen, B\ is CH3, B2, B3 and B4 are ail hydrogen and the values of R4a* R4b' R4Ct R4d and R8 are given in Table 1.
Table XIV provides 782 compounds of formula In


wherein Ai is hydrogen, B1 is CH3, B2, B3 and B* are all hydrogen and the values of R4a' R4bl R4c' R4d and R8 are given in Table i.
Table XV provides 782 compounds of formula Io

wherein Ai is hydrogen, B1 is CH3, B2) B3 and B4 are all hydrogen and the values of R4a' R4b* R4c* R4d and R8 are given in Table 1.
Table XVI provides 782 compounds of formula Ip

wherein Ai is hydrogen, B1 is CH3, B2> B3 and B4 are all hydrogen and the values of R4a' R4b* R4c- R4d and R8 are given in Table 1.

Table XVII provides 782 compounds of formula Iq

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1.
Table XVIII provides 782 compounds of formula Ir

wherein A1is hydrogen, B1 is CH3, B;, B3 and B4 arc all hydrogen and the values of R41, R4b* R4c' R4d and R8 are given in Table 1.
Table XIX provides 782 compounds of formula Is


wherein A\ is hydrogen, B\ is CH3) B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table XX provides 782 compounds of formula It

wherein A\ is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c^R4d and R8are given in Table 1.
Table XXI provides 782 compounds of formula Iu


wherein Ai is hydrogen, B| is CH3, B2, B3 and B4 are ai! hydrogen and the values of R4a' R4b' R4c'R4d and R8are given in Table 1.
Table XXII provides 782 compounds of formula Iv

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1.
Table XXIII provides 782 compounds of formula Iw


wherein Ai is hydrogen, B1 is CH3, B2, B1 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table XXIV provides 782 compounds of formula Ix

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c* R4d and R8 are given in Table I.
Table XXV provides 782 compounds of formula ly


wherein A\ is hydrogen, Bt is CH3> B2, B3 and B4 are all hydrogen and the values of R4a* R4b> R4c' R4d and R8 are given in Table 1.
Table XXVI provides 782 compounds of formula Iz

wherein Ai is hydrogen, &\ is CH3, B2> B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given in Table 1.
Table XXVII provides 782 compounds of formula iaa


wherein Ai is hydrogen, B\ is CH5, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c'R4d and R8are given in Table 1.
Table XXVIII provides 782 compounds of formula lab

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1.
Table XXIX provides 782 compounds of formula lac


wherein Ai is hydrogen, B1 is CH3, B2> B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table XXX provides 782 compounds of formula lad

wherein A1is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4bt R4c* R4d and R8 are given in Table 1.
Table XXXI provides 782 compounds of formula Iae


wherein Ai is hydrogen, B1 is CH3, 82, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c' R4d and R* are given in Table 1.
Table XXXII provides 782 compounds of formula Iaf

wherein Ai is hydrogen, B* is CH3, B2, B3 and B4 are all hydrogen and the values of R4a> R4bl R4c- R4d and R8 are given in Table 1.
Table XXXIII provides 782 compounds of formula lag

wherein A( is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1.
Table XXXIV provides 782 compounds of formula lab


wherein A\ is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4bl R4c' R4d and R8 are given in Table 1.
Table XXXV provides 782 compounds of formula lai

wherein A\ is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table XXXVI provides 782 compounds of formula Iaj


wherein Ai is hydrogen, B| is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R8 are given in Table 1.
Table XXXVII provides 782 compounds of formula Iak

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R40' R4d and R8 are given in Table 1.
Table XXXVIII provides 782 compounds of formula la]


wherein Ai is hydrogen, B» is CH3, B^, B3 and B4 are all hydrogen and the values of R4a' R4b" R4c' R4d and R8 are given in Table 1.
Table XXXLX provides 782 compounds of formula lam

wherein A\ is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c'R4d and R8are given in Table 1.
Table XL provides 782 compounds of formula Ian


wherein A! is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c" R4d and R8 are given in Table 1.
Table XLI provides 782 compounds of formula Iao

wherein A\ is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4bl R4c' R4d and R8 are given in Table 1.
Table XLII provides 782 compounds of formula lap


wherein Ai is hydrogen, B\ is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table XLII1 provides 782 compounds of formula Iaq

wherein A1is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4bl R4c' R4d and R8 are given in Table 1.
Table XLIV provides 782 compounds of formula Iar


wherein Aj is hydrogen, B1 is CH3, B2, B1 and B4 are all hydrogen and the values of R4a* R4bt R4c'R4d and R8are given in Table 1.
Table XLV provides 782 compounds of formula las

wherein A1is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4cR4d and R8are given in Table 1.
Table XLVI provides 782 compounds of formula Iat


wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c,R4d and R8 are given in Table 1.
Table XLV1I provides 782 compounds of formula Iau

wherein Ai is hydrogen, B| is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c- R4d and R8 are given in Table 1.
Table XLVin provides 782 compounds of formula lav


wherein Aj is hydrogen, B| is CH3, B2, B3 and B4 are all hydrogen and the values of R4a> R4b* R4c' R4d and R8 are given in Table 1.
Table XLIX provides 782 compounds of formula law

wherein Aj is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4d and R8 are given in Table 1.
Table L provides 782 compounds of formula lax


wherein A] is hydrogen, B( is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b" R*' R4d and R8 are given in Table 1.
Table LI provides 782 compounds of formula lay

wherein A\ is hydrogen, B\ is CH3, B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c' R4d and R8 are given in Table 1.
Table L1I provides 782 compounds of formula Iaz

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4bl R4c' R4d and R8 are given in Table 1.
Table LIII provides 782 compounds of formula Iba


wherein A1is hydrogen, B] is CH3, B?, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c> R4d and R8 are given in Table 1.
Table LJV provides 782 compounds of formula Ibb

wherein Ai is hydrogen, B| is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given in Table 1.
Table LV provides 782 compounds of formula Ibc


wherein A\ is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R8 are given in Table 1.
Table LVI provides 782 compounds of formula Ibd

wherein A\ is hydrogen, B1 is CH3> B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table LVD provides 782 compounds of formula Ibe


wherein A\ is hydrogen, B| is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1.
Table LVIII provides 782 compounds of formula Ibf

wherein A( is hydrogen, B\ is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R40' R4d and R8 are given in Table 1.
Table LIX provides 782 compounds of formula Ibg


wherein Aj is hydrogen, Bt is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table LX provides 782 compounds of formula Ibh

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table LXI provides 782 compounds of formula IB1

wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R8 are given in Table 1.
Table LXII provides 782 compounds of formula IB1


wherein A1is hydrogen, B\ is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4c' R4* and R8 are given in Table 1.
Table LXIII provides 782 compounds of formula Ibk

wherein Aj is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c* R4d and R8 are given in Table 1.
Table LXIV provides 782 compounds of formula Ibl

wherein A1is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4*' R4b' R40* R4d and R8 are given in Table 1.
Table LXV provides 782 compounds of formula Ibni


wherein Ai is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R40' K* and R8 are given in Table 1.
Table LXVI provides 782 compounds of formula Ibn

wherein Aj is hydrogen, B1 is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4Cl R4d and R8 are given in Table 1.
Table LXVII provides 782 compounds of formula Ibo


wherein Ai is hydrogen, B| is CH3, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c,R4d and R8are given in Table 1.
Table CI provides 782 compounds of formula la wherein A\ is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a" R4b' R4c' R4d and R8 are given in Table 1. Table C1-4 provides 782 compounds of formula lb wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b R40, R4d and R8 are given in Table 1. Table CIII provides 782 compounds of formula Ic wherein At is hydrogen, B] is OH, B2, B3 and B4 are all hydrogen and the values of R4* R4b* R4^ R4d and Rf are given in Table 1. Table CIV provides 782 compounds of formula Id wherein Aj is hydrogen, B| is OH, B:, B3 and B4 are all hydrogen and the values of R4a' R4b' R4Ct R4d and R8 are given in Table 1. Table CV provides 782 compounds of formula Ie wherein A1is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CVI provides 782 compounds of formula If wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4Ct R4d and R8 are given in Table 1. Table CVII provides 782 compounds of formula Ig wherein A\ is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1. Table CVHI provides 782 compounds of formula Ih wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R^' R4d and R8 are given in Table 1. Table CIX provides 782 compounds of formula Ii wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4bl R4c' R4d and R8 are given in Table 1. Table CX provides 782 compounds of formula Ij wherein A1is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given in Table 1. Table CXI provides 782 compounds of formula Dc wherein Ai is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4* R4b* R40' R4*1 and R1 are given in Table 1. Table CXII provides 782 compounds of formula II wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c,R4dand Rsae given in Table 1. Table CXfll provides 782 compounds of formula Im wherein A\ is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4*" R4b' R^R4* and R8are given in Table 1. Table CXIV provides 782 compounds of formula In wherein A1is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4bf R46, R44 aod Rs are givoi in Table 1. Table CXV provides 782 compounds of formula Io wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4** R4b' R^' Rw and R1 are given in Table 1.

Table CXVI provides 782 compounds of formula Ip wherein Ai is hydrogen, B] is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4bl R4c' R4d and R8 are given in Table 1. Table CXVII provides 782 compounds of formula Iq wherein Aj is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R8 are given in Table I. Table CXVIII provides 782 compounds of formula Ir wherein Aj is hydrogen, B» is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b> R40 R4d and R8 are given in Table 1. Table CXIX provides 782 compounds of formula Is wherein A1is hydrogen, B1 is OH, B?, B3 and B4 are all hydrogen and the values of R4a* R4bl R* R40 and Rf are given in Table 1. Table CXX provides 782 compounds of formula It wherein A* is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CXXI provides 782 compounds of formula Iu wherein A\ is hydrogen, B\ is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. TaB1c CXXII provides 782 compounds of formula Iv wherein Ai is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R* are given in Table 1. Table CXXIII provides 782 compounds of formula Iw wherein Aj is hydrogen, B\ is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CXXIV provides 782 compounds of formula Ix wherein Ai is hydrogen, B\ is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R* are given in Table 1. Table CXXV provides 782 compounds of formula Iy wherein At is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4d and Rs are given in Table 1. Table CXXVI provides 782 compounds of formula Iz wherein Ai is hydrogen, B\ is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4c' R4d and Rs are given in Table 1. Table CXXVII provides 782 compounds of formula Iaa wherein A\ is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4bt R4c' R4* aad R* are given in Table 1. Table CXXVUl provides 782 compounds of formula lab wherein Aj is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4bf R4c* R4* aod R8 are given in Table 1. Table CXXIX provides 782 compounds of formula lac wherein At is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R40, R44 and R8 are given in Table 1. Table CXXX provides 782 compounds of formula lad wherein Ai is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4a> R4b* R40, R4"5 and R1 are given in Table 1. Table CXXXI provides 782 compounds of formula Iae wherein At is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4* R4* R4*' R44 and R8 arc given in Table 1.

Table CXXXII provides 782 compounds of formula Iaf wherein Aj is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b R4c' R4d and R8 are given in Table 1. Table CXXXIII provides 782 compounds of formula lag wherein Ai is hydrogen, B( is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1. Table CXXXIV provides 782 compounds of formula Iah wherein A\ is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4**' R4*' R^and R* are given in Table 1. Table CXXXV provides 782 compounds of formula lai wherein A: is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R^'R^and R8are given in Table 1. Table CXXXVI provides 782 compounds of formula Iaj wherein A* is hydrogen, B( is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4*' R4c' R4* and R8 are given in Table 1. Table CXXXVII provides 782 compounds of formula Iak wherein Ai is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1. Table CXXXVIII provides 782 compounds of formula Ial wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c'R4d and R8 are given in Table 1. Table CXXXIX provides 782 compounds of formula lam wherein A\ is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1. Table CXL provides 782 compounds of formula Ian wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a> R4b> R4c* p.4d and P.8 are given in Table !. Table CXLI provides 782 compounds of formula Iao wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c'R4dand R*are given in Table 1. Table CXLII provides 782 compounds of formula lap wherein At is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c'R4dand R*are given in Table 1. Table CXLIII provides 782 compounds of formula Iaq wherein A^ is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given in Table 1. Table CXLIV provides 782 compounds of formula Iar wherein Ai is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4* R4b* R4c" R4d and R1 are givra in Table 1. Table CXLV provides 782 compounds of formula las wherein Ai is hydrogen, Bt is OH, B2, B3 and B4 are all hydrogen and the values of R41' R4b' R4c' R4d and R1 art given in Table 1. Table CXLVI provides 782 compounds of formula Iat wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4"' R4bt R^'R4*1 and R1 are given in Table 1. Table CXLVII provides 782 compounds of formula lau wherein A* is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4*1 R4b' R^R^and R* are given in Table 1.

Table CXLVIII provides 782 compounds of formula lav wherein A* is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R8 are given in Table 1. Table CXLIX provides 782 compounds of formula law wherein Ai is hydrogen, B| is OH, B2» B3 and B4 are all hydrogen and the values of R4a' R4b' R4c R^ and R8 are given in Table 1. Table CL provides 782 compounds of formula lax wherein A} is hydrogen, B( is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' K46 and R8 are given in Table 1. Table CLI provides 782 compounds of formula lay wherein Aj is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c' R4d and R8 are given in Table 1. Table CLII provides 782 compounds of formula Iaz wherein Ai vs hydrogen, B\ is OH, B2» B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table I. Table CLII1 provides 782 compounds of formula Iba wherein Aj is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table I. Table CLIV provides 782 compounds of formula Ibb wherein Aj is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CLV provides 782 compounds of formula Ibc wherein Ai is hydrogen, B1 is OH, B2> B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R8 are given in Table 1. Table CLVI provides 782 compounds of formula Ibd wherein At is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c- R4d and R8 are given in Table 1. Table CLVII provides 782 compounds of formula Ibe wherein Ai is hydrogen, Bt is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table I. Table CLVIII provides 782 compounds of formula Ibf wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table I. Table CLIX provides 782 compounds of formula Ibg wherein Ai is hydrogen, B| is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CLX provides 782 compounds of formula Ibh wherein Ai is hydrogen, B} is OH, B2, B3 and B4 are all hydrogen and the values of R43f R4b' R40, R4d and R8 are given in Table 1. Table CLXI provides 782 compounds of formula IB1 wherein At is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4*- R4* and R1 are given in Table I. Table CLXII provides 782 compounds of formula IB1 wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c> R44 and R8 are given in Table 1. Table CLXIII provides 782 compounds of formula Ibk wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4jL R4b" R4^ R*1 and R8 are given in Table 1.

Table CLXIV provides 782 compounds of formula Ibl wherein A} is hydrogen, B1 is OH, B2) B3 and B4 are all hydrogen and the values of R4a* R4b' R4c,R4dand R8are given in Table 1. Table CLXV provides 782 compounds of formula Ibm wherein Aj is hydrogen, B1 is OH, B2, Bz and B4 are all hydrogen and the values of R4a* R4bl R4c* R4d and R8 are given in Table 1. Table CLXVI provides 782 compounds of formula Ibn wherein Ai is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4* R4*' R4c' R** and R8 are given in Table 1. Table CLXVII provides 782 compounds of formula Ibo wherein A: is hydrogen, B1 is OH, B2, B3 and B4 are all hydrogen and the values of R4a* R4** R40, R4* and R8 are given in Table 1. Table CCI provides 782 compounds of formula la wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c'R4dand R8are given in Table 1. Table CCII provides 782 compounds of formula lb wherein At is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given in Table 1. Table CCHI provides 782 compounds of formula Ic wherein A\ is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4c* R4d and R8 are given in Table 1. Table CCIV provides 782 compounds of formula Id wherein Ai is hydrogen, B\ is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c' R4d and R8 are given in Table 1. Table CCV provides 782 compounds of formula le wherein A1is hydrogen, B| is F, B2, B3
and "RA are all hydraeen and the values ar*» oivpn in Tahlp 1
Table CCVI provides 782 compounds of formula If wherein A) is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1. Table CCVII provides 782 compounds of formula Ig wherein Aj is hydrogen, B\ is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1. Table CCVIII provides 782 compounds of formula Hi wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4*' R4bl R4c* R4d and R* are given in Table 1. Table CCIX provides 782 compounds of formula Ii wherein Ai is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4bf R4c' R4d and R1 are given in Table 1. Table CCX provides 782 compounds of formula Ij wherein A1is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4bf R40* R4d and R8 are given in Table 1. Table CCXI provides 782 compounds of formula Dc wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a> R4b* R^R4** and R1 are given in Table 1. Table CCXII provides 782 compounds of formula II wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4** R4bt R4*- R4* and R8 are given in Table 1.

Table CCXI1I provides 782 compounds of formula Im wherein A1is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1. Table CCXIV provides 782 compounds of formula In wherein A( is hydrogen, B* is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c'R4d and R8 are given in Table 1. Table CCXV provides 782 compounds of formula Io wherein At is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R** R44 and R* are given in Table 1. Table CCXVI provides 782 compounds of formula Ip wherein AT h hydrogen, B1 is F, B:, B3 and B4 are all hydrogen and the values of R4a" R4b* R4c* R4* and Rsare given in Table 1. Table CCXVH provides 782 compounds of formula Iq wherein At is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b> R4c' R4d and R8 are given in Table 1. Table CCXVEQ provides 782 compounds of formula Ir wherein Aj is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R40, R4d and R8 are given in Table 1. Table CCX1X provides 782 compounds of formula Is wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c* R4d and R8 are given in Table 1. Table CCXX provides 782 compounds of formula It wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4bl R4c' R4d and R8 are given in Table 1. Table CCXX1 provides 782 compounds of formula Iu wherein A1is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R43, R4b' R4c* R4d and Rg are given in Table 1. Table CCXXII provides 782 compounds of formula Iv wherein A\ is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and Rs are given in Table 1. Table CCXXD1 provides 782 compounds of formula Iw wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1. Table CCXXIV provides 782 compounds of formula Ix wherein A* is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4at R4b* R4Cf R4d and R8 are given in Table 1. Table CCXXV provides 782 compounds of formula Iy wherein Ai is hydrogen, B1 is F, B2j B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1. Table CCXXVI provides 782 compounds of formula Iz wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4*1 R4* and R1 are given in Table 1. Table CCXXVEl provides 782 compounds of formula Iaa wherein At is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4** R*' R** aad R8 are given in Table 1. Table CCXXVIII provides 782 compounds of formula lab whereto Ai is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4t R4* R4*' R44 and R8 are given in Table 1.

Table CCXXIX provides 782 compounds of formula lac wherein Ai is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c' R4d and R8 are given in Table 1. Table CCXXX provides 782 compounds of formula lad wherein Aj is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a> R4bl R4c' R44 and R8 are given in Table 1. Table CCXXXI provides 782 compounds of formula Iae wherein A1is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R40* R4d and R8 are given in Table 1. Table CCXXXII provides 782 compounds of formula Iaf wherein A; is feydrogea, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4*' R4** R4** and R* are given in Table !. Table CCXXXIII provides 782 compounds of formula lag wherein Ai is hydrogen, B\ is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4* and R8 are given in Table 1. Table CCXXXIV provides 782 compounds of formula Iah wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R8 are given in Table 1. Table CCXXXV provides 782 compounds of formula Iai wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4d and R8 are given in Table 1. Table CCXXXVI provides 782 compounds of formula Iaj wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CCXXXVII provides 782 compounds of formula Iak wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c*R4dand Rsare given in Table I. Table CCXXXVIII provides 782 compounds of formula Ial wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c,R4d and R8are given in Table 1. Table CCXXXIX provides 782 compounds of formula lam wherein At is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4c' R4d and R8 are given in Table 1. Table CCXL provides 782 compounds of formula Ian wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b" R4c*R4d and R8are ©VCT in Table 1. Table CCXLI provides 782 compounds of formula Iao wherein Aj is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a" R4b> R4c* R4d and R* are given in Table 1. Table CCXLII provides 782 compounds of formula lap wherein A1is hjdrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4* R4b* R^' R4d and R8 ae given in Table 1. Table CCXLIII provides 782 compounds of formula Iaq wherein At is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4* R4b' R40, R4d and R8 MC given in Table 1. Table CCXLIV provides 782 compounds of formula Iar wherein A1is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R46, R^* R4*1 and R* are given in Table 1.

Table CCXLV provides 782 compounds of formula las wherein Aj is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CCXLVI provides 782 compounds of formula Iat wherein A] is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c,R4d and R8are given in Table 1. Table CCXLVII provides 782 compounds of formula Iau wherein A{ is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CCXLVm provides 782 compounds of formula lav wherein A; is hydrogen, B\ is F, B:, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R1 are given in Table 1. Table CCXLIX provides 782 compounds of formula law wherein Aj is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CCL provides 782 compounds of formula lax wherein A1is hydrogen, B\ is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CCLI provides 782 compounds of formula wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1. Table CCLII provides 782 compounds of formula Iaz wherein A\ is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c,R4d and R8 are given in Table 1. Table CCLIII provides 782 compounds of formula Iba wherein A1is hydrogen, B| is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R8 are given in Table 1. Table CCLIV provides 782 compounds of formula Ibb wherein A\ is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4d and R8 are given in Table 1. Table CCLV provides 782 compounds of formula Ibc wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R8 are given in Table 1. Table CCLVI provides 782 compounds of formula Ibd wherein A\ is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R40' R4d and R8 are given in Table 1. Table CCLVII provides 782 compounds of formula Ibe wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R1 are given in Table 1. Table CCLVIII provides 782 compounds of formula Ibf wherein Ai is hydrogen, B? is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R40, R4d and Rs are given in Table 1. Table CCLIX provides 782 compounds of formula Ibg wherein A1is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4tt R4b' R40, Rw and R*arc given in Table 1. Table CCLX provides 782 compounds of formula Ibh wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a" R4b> R4** R4*1 and R1 are given in Table 1.

Table CCLXI provides 782 compounds of formula IB1 wherein A\ is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4h' R4c,R4d and R8 are given in Table 1. Table CCLXI1 provides 782 compounds of formula IB1 wherein Aj is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c*R4dand R?are given in Table 1. Table CCLXIII provides 782 compounds of formula Ibk wherein Aj is hydrogen, B1 is F, B?» B3 and B4 are all hydrogen and the values of R4a' R4b* R4c* R4d and R8 are given m Table 1. Table CCLXIV provides 782 compounds of formula Ibl wherein Ai is hydrogen, B\ is F, B2, B3 and B4 are all hydrogen and the values of R4*' R4** R40* R44 and R8 are given in Table 1. Table CCLXV provides 782 compounds of formula Ibm wherein A? is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b" R4^ R4d and R8 are given in Table 1. Table CCLXVI provides 782 compounds of formula Ibn wherein Ai is hydrogen, B1 is F, B2, B3 and B4 are all hydrogen and the values of R4a' R4b| R40' R4d and R8 are given in Table 1. Table CCLXVII provides 782 compounds of formula Ibo wherein Ai is hydrogen, B\ is F, B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4cR4dand R8 are given in Table 1. Table CCCI provides 782 compounds of formula la wherein A\ is hydrogen, B| is F, B2 is F, B3 and B4 are both hydrogen and the values of R4a* R4bt R4c' R4d and R8 are given in Table 1. Table CCCII provides 782 compounds of formula lb wherein Ai is hydrogen, B1 is F, B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1. Table CCCIII provides 782 compounds of formula Ic wherein Ai is hydrogen, B\ is F, B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R^R^and R8are given in Table 1.
Table CCCIV provides 782 compounds of formula Id wherein Ai is hydrogen, B| is F, B2 is F, B3 and B4 are both hydrogen and the values of R4a* R4b' R4c,R4dand R8 are given in Table 1.
Table CCCV provides 782 compounds of formula Ie wherein Ai is hydrogen, B| is F, B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b* R^ R4d and R8 are given in Table 1. Table CCCVI provides 782 compounds of formula If wherein A1is hydrogen, B1 is F, B2 is F, B3 and B4 are both hydrogen and the values of R4a> R4bf R*' R44 and R* are ^ven in Table 1.
Table CCCVII provides 782 compounds of formula Ig wherein A1is hydrogen, B1 is F, B2 is F, B3 and B4 are both hydrogen and the values of R4*' R* R^* RM and R1 are given in Table 1.

Table CCCVIII provides 782 compounds of formula Ih wherein Aj is hydrogen, B1 is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a> R4b' R4c'R4dand R8are given in Table
1.
Table CCC1X provides 782 compounds of formula Ii wherein Aj is hydrogen, B\ is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a' R4b> R4c' R4d and R8 are given in Table
1.
Table CCCX provides 782 compounds of formula Ij wherein Aj is hydrogen, B1 is F, B2 is F,
B3 and B4 are both hydrogen and the values of R4a' R4b* R4c' R46 and R* arc given in Table 1.
Table CCCXI provides 782 compounds of formula Ik wherein A1is hydrogen, B1 is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a* R4b' R4c' R46 and R8 are given in Table
1.
Table CCCXII provides 782 compounds of formula II wherein A1is hydrogen, B1 is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table
1.
Table CCCXIII provides 782 compounds of formula Im wherein Ai is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b> R4c' R4d and R8 are given in
Table 1.
Table CCCXIV provides 782 compounds of formula In wherein Aj is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a* R4b* R4c' Rw and R8 are given in
Table 1.
Table CCCXV provides 782 compounds of formula Io wherein Ai is hydrogen, B1 is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4iu R4b' R4c' R4d and R8 are given in Table
1.
Table CCCXVI provides 782 compounds of formula Ip wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b* R^R^and R8 are given in
Table 1.
Table CCCXVII provides 782 compounds of formula Iq wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R40, R^and R8 are given in
Table 1.
Table CCCXVD1 provides 782 compounds of formula Ir wherein A* is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a* R4**' R^'R^and R8 are given in
Table 1.

Table CCCXIX provides 782 compounds of formula Is wherein A, is hydrogen, B1 is F, B1 is
F, B3 and B4 are both hydrogen and the values of R43, R4b' R4c'R4dand R8 are given in Table
1.
Table CCCXX provides 782 compounds of formula It wherein Ai is-hydrogen, B1 is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a' R4b' R^R^and R8 are given in Table
1.
Table CCCXXI provides 782 compounds of formula lu wherein A\ is hydrogen, B1 is F, B1
is F, B3 and B4 are both hydrogen and the values of R4a- R*' R^R^and R8are given in
Table 1.
Table CCCXXII provides 782 compounds of formula Iv wherein A] is hydrogen, B] is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b> R4cR4dand R8 are given in
Table I.
Table CCCXXITI provides 782 compounds of formula Iw wherein Ai is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4cR4d and R8 are given in
Table 1.
Table CCCXXIV provides 782 compounds of formula Ix wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4bl R40, R4d and R8 are given in
Table 1.
Table CCCXXV provides 782 compounds of formula Iy wherein Ai is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b* R4c> R4d and R8 are given in
Table 1.
Table CCCXXVI provides 782 compounds of formula Iz wherein At is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b> R4c' R*6 and R8 arc given in
Table 1.
Table CCCXXVH provides 782 compounds of formula Iaa wherein A; is hydrogen, B| is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a> RAbt R40, R4* and R8 are given in
Table 1.
Table CCCXXVIII provides 782 compounds of formula lab wherein Ai is hydrogen, Bt is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a" R4b* R^R^and R8are given in
Table 1.

Table CCCXXIX provides 782 compounds of formula lac wherein A? is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b* R4c,R4d and R8 are given in
Table 1.
Table CCCXXX provides 782 compounds of formula lad wherein Ai is hydrogen, B[ is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a* R4b' R4c* R** and R8 are given in
Table 1.
Table CCCXXXI provides 782 compounds of formula Iae wherein Ai is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4* R4b* R^'R^and R8 are given in
Table 1.
Table CCCXXXII provides 782 compounds of formula Iaf wherein Aj is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4bl R4*' R4d and R8 are given in
Table 1.
Table CCCXXXIII provides 782 compounds of formula lag wherein A\ is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a* R4b* R4c'R4dand R8are given in
Table 1.
Table CCCXXXIV provides 782 compounds of formula Iah wherein A] is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CCCXXXV provides 782 compounds of formula Iai wherein Ai is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a* R4bt R^R^and R8 are given in
Table 1.
Table CCCXXXVI provides 782 compounds of formula Iaj wherein Aj is hydrogen, B] is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b* R^'R^and R8are given in
Table 1.
Table CCCXXXVII provides 782 compounds of formula Iak wherein Ai is hydrogen, B| is
F, B2 is F, B3 and B4 are both hydrogen and the values of R4a* R4b' R^R4* and R8 are given in
Table 1.
Table CCCXXXVD3 provides 782 compounds of formula Ial wherein Ai is hydrogen, B1 is
F, B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4**' R4^ R44 and R8 are given in
Table 1.

Table CCCXXXLX provides 782 compounds of formula lam wherein A( is hydrogen, B1 is
F, B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CCCXL provides 782 compounds of formula Ian wherein At is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a- R4b' R4c> R4d and R8 are given in
Table 1.
Table CCCXLI provides 782 compounds of formula Iao wherein Ai is hydrogen, B; is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a> R4*' R4c- R4*3 and Rs are given in
Table 1.
Table CCCXLII provides 782 compounds of formula lap wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a> R4b' R4c* R4d and R8 are given in
Table 1.
Table CCCXLIII provides 782 compounds of formula Iaq wherein At is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CCCXLIV provides 782 compounds of formula Iar wherein Ai is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4"1 R4b' R4c> R4d and R8 are given in
Table 1.
Table CCCXLV provides 782 compounds of formula las wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b" R40, R4d and R8 are given in
Table 1.
Table CCCXLVI provides 782 compounds of formula Iat wherein Ai is hydrogen, B] is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a> R4b' R4c- Rw and R8 are given in
Table 1.
Table CCCXLVII provides 782 compounds of formula Iau wherein At is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of Ria% R4bl R**" RM and R8 are given in
Table 1. .
Table CCCXLVITJ provides 782 compounds of formula lav wherein A1is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4** R4bl R^R^aod R8 are given in
Table 1.

Table CCCXLIX provides 782 compounds of formula law wherein Ai is hydrogen, B| is F, B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' Rdd and R8 are given in Table 1.
■> t -. - ^~
Table CCCL provides 782 compounds of formula lax wherein A\ is hydrogen, B( is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a' R4b' R^R^and R8are given in Table
1.
Table CCCLI provides 782 compounds of formula lay wherein A\ is hydrogen, B* is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a' R4b' R40- R**and Rf are given in Table
1.
Table CCCLD provides 782 compounds of formula Iaz wherein Ai is hydrogen, B\ is F, B2 is
F, B3 and B4 are both hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table
1.
Table CCCLHI provides 782 compounds of formula Iba wherein A] is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a* R4b* R4c> R4d and R8 are given in
Table 1.
Table CCCLIV provides 782 compounds of formula Ibb wherein A\ is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in
Table 1.
Table CCCLV provides 782 compounds of formula Ibc wherein A* is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b> R4c' R4* and R8 are given in
Table 1.
Table CCCLVI provides 782 compounds of formula Ibd wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a* R4b' R4c'R4* and R8 are given in
Table 1.
Table CCCLVU provides 782 compounds of formula Ibe wherein Ai is hydrogen, B\ is F, B2
is F, B3 and B4 are both hydrogen and the values of R43, R4b' R4Cl Ku and R8 are given in
Table l.
Table CCCLVIII provides 782 compounds of formula Ibf wherein A1is hydrogen, B* is F, B2
is F, B3 and B4 are both hydrogen and the values of R4*1 R4b* R4* R^and R*are given in
Table!.

Table CCCLIX provides 782 compounds of formula Ibg wherein A] is hydrogen, B| is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b> R4c'R4d and R8 are given in
Table 1.
Table CCCLX provides 782 compounds of formulaTbh wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c-R4d and R8 are given in
Table 1.
Table CCCLXI provides 782 compounds of formula IB1 wherein Ai is hydrogen, B| is F, B2
is F, B1 and B4 are both hydrogen and the values of R4* R44"' R4c' R4*1 and R8 are given in
Table 1.
Table CCCLXII provides 782 compounds of formula IB1 wherein Ai is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c" R4* and R8 are given in
Table 1.
Table CCCLXIII provides 782 compounds of formula Ibk wherein Ai is hydrogen, B1 is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CCCLXIV provides 782 compounds of formula Ibl wherein A1is hydrogen, B1 is F, B2
is F, B3 and B4 are both hydrogen and the values of R4a> R4bl R4c,R4d and R8 are given in
Table 1.
Table CCCLXV provides 782 compounds of formula Ibm wherein At is hydrogen, B| is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a Table 1.
Table CCCLXVI provides 782 compounds of formula Ibn wherein At is hydrogen, B] is F,
B2 is F, B3 and B4 are both hydrogen and the values of R4a' R4b' R40, R4* and R8 are given in
Table 1. ■
Table CCCLXVD provides 782 compounds of formula Ibo wherein A-, is hydrogen, B» is F,
B2 is F, B3 and B4 are both hydrogen and the values of R44' R4b' R^R^and R8are given in
Table 1.
Table CDI provides 782 compounds of formula la wherein A1is hydrogen, B1 is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R40- R** and R* are given in
Table 1.

Table CDII provides 782 compounds of formula lb wherein Ai is hydrogen, B| is CH3, B1 is
CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c,R4d and R8 are given in
Table 1.
Table CDHI provides 782 compounds of formula Ic"wherein Ai is hydrogen, B\ is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c R-" and R8 are given in Table
1.
Table CDIV provides 782 compounds of formula Id wherein Ai is hydrogen, B1 is CH3, B1 is
CH3, B3 and B4 are both hydrogen and the values of R4a' R4b- R40, R1* and R8 are given in
Table 1.
Table CDV provides 782 compounds of formula Ie wherein A1is hydrogen, B| is CH3, B1 is
CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4e' R4d and R8 are given in
Table 1.
Table CDVI provides 782 compounds of formula If wherein A1is hydrogen, B1 is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c,R4d and R8 are given in
Table 1.
Table CDVII provides 782 compounds of formula Ig wherein Ai is hydrogen, B, is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CDVIII provides 782 compounds of formula Ih wherein Ai is hydrogen, B1 is CH3) B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4bl R^R^and R8 are given in
Table 1.
Table CDIX provides 782 compounds of formula Ii wherein Ai is hydrogen, B1 is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c'Rwand R8 are given in
Table 1.
Table CDX provides 782 compounds of formula Ij wherein A1is hydrogen, Bt is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a> R4b> R4c' RM and R* are given in
Table 1.
Table CDXI provides 782 compounds of formula Ik wherein Ai is hydrogen, B1 is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a> R4b' R^R44 and R8 are given in
Table 1.

Table CDXII provides 782 compounds of formula II wherein A\ is hydrogen, B} is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a> R4b' R4c' R4d and R8 are given in
Table L
Table CDXIII provides 782 compounds of formula Im wherein A\ is hydrogen, Bt is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b> R4c' R44 and R8 are given in
Table 1.
Table CDXIV provides 782 compounds of formula In wherein Ai is hydrogen, B* is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b* R^R^aad R?are given in
Table 1.
Table CDXV provides 782 compounds of formula Io wherein Ai is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a* R415, R4c> R44 and R8 are given in
Table 1.
Table CDXVI provides 782 compounds of formula Ip wherein Ai is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a* R4b* R4c' R4d and R8 are given in
Table 1.
Table CDXVII provides 782 compounds of formula Iq wherein Ai is hydrogen, B| is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c,R4dand R8are given in
Table 1.
Table CDXVm provides 782 compounds of formula Ir wherein Ai is hydrogen, B\ is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a* R4b' R^'R44 and R8 are given in
Table I.
Table CDXIX provides 782 compounds of formula Is wherein Ai is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a> R4b? R4c* R*6 and Rs are given in
Table 1.
Table CDXX provides 782 compounds of formula It wherein A\ is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a* R4b' R4Ct R* aod R8 are given in
Table 1.
Table CDXXI provides 782 compounds of formula Iu wherein Ai is hydrogen, B\ is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R41' R4b' R4^ R* and R8 are given in
Table 1.

Table CDXXII provides 782 compounds of formula Iv wherein A] is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in
Table 1.
Table CDXXIU provides 782 compounds of formula I\v wherein A\ is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R^'R4* and R8are given in
Table 1.
Table CDXXIV provides 782 compounds of formula Ix wherein A\ is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4bl R* R-* and R8 are given in
Table 1.
Table CDXXV provides 782 compounds of formula ly wherein A\ is hydrogen, B» is CH3,
B2 is CH3» B3 and B4 are both hydrogen and the values of R4a' R4b' R^'R^ and R8 are given in
Table 1.
Table CDXXVI provides 782 compounds of formula Iz wherein Ai is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4cR4d and R8 are given in
Table 1.
Table CDXXV1I provides 782 compounds of formula Iaa wherein A] is hydrogen, B| is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4Cl R4d and R8 are given in
Table 1.
Table CDXXV1II provides 782 compounds of formula lab wherein Aj is hydrogen, B1 is
CH3s B2 is CH3, B3 and B4 are both hydrogen and the values of R4a- R4^ R4c R4d and R8 are
given in Table 1.
Table CDXXIX provides 782 compounds of formula lac wherein A1is hydrogen, B1 is CH3,
B2 is CH3) B3 and B4 are both hydrogen and the values of R4a? R4b* R^R4*1 and R8 are given in
Table 1.
Table CDXXX provides 782 compounds of formula lad wherein A] is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4bf R40' R44 and R8 are given in
Table 1.
Table CDXXX1 provides 782 compounds of formula lae wherein A] is hydrogen, B| is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R^ R** and R8 are given in
Table 1.

Table CDXXXII provides 782 compounds of formula laf wherein Ai is hydrogen, B| is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c'R4d and R8 are given in
Table 1.
Table CDXXXIII provides 782 compounds of formula lag wherein A] is hydrogen, B| is
CH3, B2 is CH3, B3 and B4 are both hydrogen and the values of R4a* R4fc' R4c,R4dand R8 are
given in Table 1.
Table CDXXXIV provides 782 compounds of formula Iah wherein A* is aydrogen, B1 is
CH3, B2 is CH3, B3 and B4 are both hydrogen and the values of R4* R*^ R4^ R** and R8 are
given in Table 1.
Table CDXXXV provides 782 compounds of formula lai wherein Aj is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a* R4b' R40, R4d and R8 are given in
Table 1.
Table CDXXXVI provides 782 compounds of formula laj wherein A* is hydrogen, B| is
CH3, B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b* R4c,R4d and R8 are
given in Table 1.
Table CDXXXVII provides 782 compounds of formula Iak wherein Aj is hydrogen, B1 is
CH3, B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b* R4c' R4d and R8 are
given in Table 1.
Table CDXXXVIO provides 782 compounds of formula Ial wherein At is hydrogen, B1 is
CH3, B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4*" R40, R4" and R8 are
given in Table 1.
Table CDXXXIX provides 782 compounds of formula lam wherein A\ is hydrogen, B1 is
CH3, B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4*' R^R4* and R8 are
given in Table 1.
Table CDXL provides 782 compounds of formula Ian wherein A1is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a* R4b* R40, R4* aid R* are given in
Table 1.
Table CDXLI provides 782 compounds of formula Iao wherein At is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4^ RM and R8 are given in
Table 1.

Table CDXLI1 provides 782 compounds of formula lap wherein A1is hydrogen, B| is CH3,
B2 is CH3, B1 and B4 are both hydrogen and the values of R4a' R4bl R4c'R4d and R8 are given in
Table 1.
Table CDXLITI provides 782 compounds of formula Iaq wherein A1is hydrogen, Bt is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c" R4* and R8 are given in
Table 1.
Table CDXLJV provides 782 compounds of formula Iar wherein Ai is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R*4, R4b' Rfc R* and R8 are given in
Table 1.
Table CDXLV provides 782 compounds of formula las wherein Aj is hydrogen, B1 is CH3,
B2 is CH3j B3 and B4 are both hydrogen and the values of R4a- R4b' R40, R44 and R8 are given in
Table 1.
Table CDXLVI provides 782 compounds of formula Iat wherein Ai is hydrogen, Bt is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CDXLVTJ provides 782 compounds of formula Iau wherein Ai is hydrogen, B) is CH3,
B2 is CH3) B3 and B4 are both hydrogen and the values of R4a' R4b' R4c,R4d and R8 are given in
Table 1.
Table CDXLVIII provides 782 compounds of formula lav wherein Ai is hydrogen, B1 is
CH3, B2 is CH3, B3 and B4 are both hydrogen and the values of R4** R4"0- R4c given in Table 1.
Table CDXLIX provides 782 compounds of formula law wherein Ai is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b> R^R*5and R* are given in
Table 1.
Table CDL provides 782 compounds of formula lax wherein At is hydrogen, B| is CH3, B2 is
CH3, B3 and B4 are both hydrogen and the values of R4a- R4b> R4c' R*1 and Rs are given in
Table 1.
Table CDLI provides 782 compounds of formula lay wherein Ai is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4*' R4b' R4t R** and R8 are given in
Table 1.

Table CDL1I provides 782 compounds of formula laz wherein Ai is hydrogen, B* is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CDLIII provides 782 compounds of formula Tba wherein Ai is hydrogen^B1 *s CH3, B2
is CH3> B3 and B4 are both hydrogen and the values of R4a' R4b* R4c K46 and Rs are given in
Table 1.
Table CDLIV provides 782 compounds of formula Ibb wherein \\ is hydrogen, B; is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R43, R4bt R* R4* and R8 are given in
Table 1.
Table CDLV provides 782 compounds of formula Ibc wherein A1is hydrogen, B] is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b* R4^ R4d and R8 are given in
Table i.
Table CDLVI provides 782 compounds of formula Ibd wherein A1is hydrogen, B| is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a> R4b' R4c> R4d and R8 are given in
Table 1.
Table CDLVII provides 782 compounds of formula Ibe wherein Ai is hydrogen, B\ is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4bl R40' R4d and R8 are given in
Table 1.
Table CDLVIII provides 782 compounds of formula Ibf wherein Ai is hydrogen, B| is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R^R44 and R8 are given in
Table 1.
Table CDLIX provides 782 compounds of formula Ibg wherein Aj is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R41, R4b' R40* R4* and R8 are given in
Table 1.
Table CDLX provides 782 compounds of formula Ibh wherein A* is hydrogen, B| is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b> R4^ R4* and R8 are given in
Table 1.
Table CDLXI provides 782 compounds of formula IB1 wherein A1is hydrogen, B1 is CH3, B2
is CH3, B3 and B4 are both hydrogen and the values of R4*' R4b' R** R** and R8 are given in
Table 1.

Table CDLXII provides 782 compounds of formula IB1 wherein A\ is hydrogen, B> is CH3,
B2 is CH3l B3 and B4 are both hydrogen and the values of R4a' R4b* R4c'R4dand R8are given in
Table l.
Table CDLXIII provides 782 compounds of formula Ibk wherein Ai is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c*R44and R8are given in
Table 1.
Table CDLXIV provides 782 compounds of formula Ibl wherein A\ is hydrogen, B» is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4tt R4b' R40 R*4 and Rs are given in
Table 1.
Table CDLXV provides 782 compounds of formula Ibm wherein Ai is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in
Table 1.
Table CDLXVI provides 782 compounds of formula Ibn wherein Aj is hydrogen, B1 is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table CDLXVII provides 782 compounds of formula Ibo wherein Ai is hydrogen, B\ is CH3,
B2 is CH3, B3 and B4 are both hydrogen and the values of R4a' R4b* R4c* R4d and R8 are given in
Table 1.
Table DI provides 782 compounds of formula la wherein A\ is hydrogen, B1 and B3 are both
CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4c' R44 and R8 are given in
Table 1.
Table DII provides 782 compounds of formula lb wherein Ai is hydrogen, B1 and B3 are both
CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b- R^R^and R8 are given in
Table 1.
Table Dili provides 782 compounds of formula Ic wherein A1is hydrogen, B1 and B3 are
both CH3) and B2 and B4 are both hydrogen and the values of R4a' R4b* R^R44 and R8 are
given in Table 1.
Table DIV provides 782 compounds of formula Id wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R*° R44 and Rs are
given in Table 1.

Table DV provides 782 compounds of formula Ie wherein Ai is hydrogen, B| and B3 are both
CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b' R4c,R4d and R8 are given in
Table i-
Table DV1provides 782 compounds of formula If wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4fc* R40, R44 and R8 are
given in Table 1.
Table DVII provides 782 compounds of formula Ig wherein A1is hydrogen Bt and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b" R4^ R4* and R8 are
given in Table 1.
Table DVin provides 782 compounds of formula Ih wherein A\ is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b' R4^ R4*3 and R8 are
given in Table 1.
Table DIX provides 782 compounds of formula Ii wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4c* R4d and R8 are
given in Table 1.
Table DX provides 782 compounds of formula Ij wherein A\ is hydrogen, B1 and B3 are both
CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4c' Rw and R8 are given in
Table 1.
Table DXI provides 782 compounds of formula Dc wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b> R4^ R** and R8 are
given in Table 1.
Table DXII provides 782 compounds of formula H wherein Ai is hydrogen, B1 and B3 are
both CH3> and B2 and B4 are both hydrogen and the values of R4a' R4b' R^R4*1 and R8 are
given in Table 1.
Table DXIII provides 782 compounds of formula Im wherein A1is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4bf R*' R^ and R8 are
given in Table 1.
Table DXIV provides 782 compounds of formula In wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a> R4* R*' R4*5 and R8 are
given in Table 1.

Table DXV provides 782 compounds of formula Io wherein A] is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are
given in Table 1.
Table DXVI provides 782 compounds of formula Ip wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R^R^and R8are
given in Table 1.
Table DXVII provides 782 compounds of formula Iq wherein A\ is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b" R4^ R4* and Rfi are
given in Table 1.
Table DXVIII provides 782 compounds of formula Ir wherein A\ is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b| R4^ R44 and R8 are
given in Table 1.
Table DXIX provides 782 compounds of formula Is wherein Ai is hydrogen, B| and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b' R4c' R4d and R8 are
given in Table 1.
Table DXX provides 782 compounds of formula It wherein Ai is hydrogen, B| and B3 are
both CH3> and B2 and B4 are both hydrogen and the values of R4a> R4b* R4c> R4d and R8 are
given in Table 1,
Table DXXI provides 782 compounds of formula Iu wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4c*R4d and R8 are
given in Table 1.
Table DXXII provides 782 compounds of formula Iv wherein A1is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4*- R44 and R8 are
given in Table 1.
Table DXXIII provides 782 compounds of formula Iw wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4c* R4* and R8 are
given in Table 1.
Table DXXIV provides 782 compounds of formula Ix wherein Ai is hydrogen, B\ and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R46* R4*" R** and R8 are
given in Table 1.

Table DXXV provides 782 compounds of formula Iy wherein Aj is hydrogen, B* and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a" R4b R4c' R4d and R8 are
given in Table 1.
Table DXXV1 provides 782 compounds of formula Iz wherein Ai is hydrogen, B\ and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R^ R4d and R8 are
given in Table 1.
Table DXXVII provides 782 compounds of formula Iaa wherein Ai is hvdrogen, B| and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4*^ R*^ R4* and R8 are
given in Table 1.
Table DXXVI1I provides 782 compounds of formula lab wherein Aj is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4* R4^ R4*' K46 and R8 are
given in Table 1.
Table DXXIX provides 782 compounds of formula lac wherein A\ is hydrogen, B] and B3
are both CH3v and B2 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and R8 are
given in Table 1.
Table DXXX provides 782 compounds of formula lad wherein A» is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4bl R4c*R4d and R8 are
eiven in Table 1.
Table DXXXI provides 782 compounds of formula Iae wherein Ai is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4** R^'R4* and R8 are
given in Table 1.
Table DXXXII provides 782 compounds of formula Iaf wherein A1is hydrogen, B| and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4*' R*' R4* and R8 are
given in Table 1.
Table DXXXIII provides 782 compounds of formula lag wherein A\ is hydrogen, B] and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4^ R^R44 and R8 are
given in Table 1.
Table DXXXTV provides 782 compounds of formula Iah wherein Ai is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4** R^ R^R4* and R8 are
given in Table 1.

Table DXXXV provides 782 compounds of formula Iai wherein At is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b> R4c,R4d and R8 are
given in Table 1.
Table DXXXVI provides 782 compounds of formula laj wherein Ai is hydrogen, B\ and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4*' R4c' R46 and R8 are
given in Table 1.
Table DXXXVI1 provides 782 compounds of formula Iak wherein A1is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4* R^ Rw and R8 are
given in Table 1.
Table DXXXVIH provides 782 compounds of formula Ial wherein A1is hydrogen, B\ and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4** R4c* R4d and R8 are
given in Table 1.
Table DXXXLX provides 782 compounds of formula lam wherein A1is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b> R4Cl R4d and R8 are
given in Table 1.
Table DXL provides 782 compounds of formula Ian wherein A\ is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b> R4cR4d and R8 are
given in Table 1.
Table DXLI provides 782 compounds of formula Iao wherein A\ is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R^'R4* and R8 are
given in Table 1.
Table DXLII provides 782 compounds of formula lap wherein A\ is hydrogen, B1 and B3 are
both CH3s and B2 and B4 are both hydrogen and the values of R4a' R4b' R^'R** and R8 are
given in Table 1.
Table DXLIII provides 782 compounds of formula Iaq wherein At is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b- R4* R** and R8 are
given in Table 1.
Table DXLIV provides 782 compounds of formula Iar wherein A\ is hydrogen, B\ and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4K R^ R4* and R8 are
given in Table 1.

Table DXLV provides 782 compounds of formula las wherein Ai is hydrogen, B] and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4c> R4d and R8 are given in Table 1.
Table DXLVI provides 782 compounds of formula Iat wherein Ai is hydrogen, B1 and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R40, R^ and R8 are given in Table 1.
Table DXLVTI provides 782 compounds of formula Iau wherein A\ is hydrogen, B* and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4* R4^ R44 and R8 are given in Table 1.
Table DXLVin provides 782 compounds of formula lav wherein A\ is hydrogen, B1 and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4*** R^R4* and R8 are given in Table 1.
Table DXL1X provides 782 compounds of formula law wherein Aj is hydrogen, B1 and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DL provides 782 compounds of formula lax wherein A» is hydrogen, B1 and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b' R4*' R4* and R8 are given in Table 1.
Table DLI provides 782 compounds of formula lay wherein A\ is hydrogen, B| and B3 are both CH3) and B2 and B4 are both hydrogen and the values of R4a* R4b' R4c* R44 and R8 are given in Table 1.
Table DLII provides 782 compounds of formula Iaz wherein A\ is hydrogen, B1 and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R^R^and R8 are given in Table 1.
Table DLIII provides 782 compounds of formula Iba wherein A1is hydrogen, B1 and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4^ R44 and R* are given in Table 1,
Table DLIV provides 782 compounds of formula Ibb wherein Ai is hydrogen, B1 and B3 are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b* R4^ RH »d R8 are given in Table 1.

Table DLV provides 782 compounds of formula Ibc wherein Ai is hydrogen, B] and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4c'R4dand R8 are
given in Table 1.
TaB1e DLVI provides 782 compounds of formula Ibd wherein Ai is hydrogen, B> and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a> R4b' R4c*R4dand Rgare
given in Table 1.
Table DLVII provides 782 compounds of formula Ibe wherein A\ is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are Both hydrogen and the values of R4^ R4b' R^ KM and R8 are
given in Table 1.
Table DLVIH provides 782 compounds of formula Ibf wherein A1is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4c> R4d and R8 are
given in Table 1.
Table DLIX provides 782 compounds of formula Ibg wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4c' R4d and R8 are
given in Table 1.
Table DLX provides 782 compounds of formula Ibh wherein A* is hydrogen, B\ and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4c'R4d and R8 are
given in Table 1.
Table DLXI provides 782 compounds of formula IB1 wherein A1is hydrogen, B\ and B3 are
both CH3» and B2 and B4 are both hydrogen and the values of R4a' R4b' R^'R^and R8 are
given in Table 1.
Table DLXII provides 782 compounds of formula IB1 wherein Ai is hydrogen, B1 and B3 are
both CH3s and B2 and B4 are both hydrogen and the values of R4a- R4b* R4^ R^ and R* are
given in Table 1,
Table DLXIII provides 782 compounds of formula Ibk wherein Ai is hydrogen, B\ and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4** R** and R8 are
given in Table 1.
Table DLXIV provides 782 compounds of formula Ibl wherein Ai is hydrogen, B1 and B3 are
both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b* R4^ R** and R8 are
given in Table 1.

Table DLXV provides 782 compounds of formula Ibm wherein Aj is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are
given in Table 1.
Table DLXVI provides 782 compounds of formula Ibn wherein A] is hydrogen, 3\ and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a* R4b R40 R4* and R8 are
given in Table 1.
Table DLXVII provides 782 compounds of formula Ibo wherein A1is hydrogen, B1 and B3
are both CH3, and B2 and B4 are both hydrogen and the values of R4a' R4b R4** R^ and R8 are
given in Table 1.
Table DCI provides 782 compounds of formula la wherein Ai is hydrogen, B5 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a* R4b' R* R4* and R8 are
given in Table 1.
Table DCII provides 782 compounds of formula lb wherein Ai is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b> R4c' R4d and R8 are
given in Table 1.
Table DCIII provides 782 compounds of formula Ic wherein A1is hydrogen, B| and B4 are
both CH3( and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are
oiven in TAHIP 1
a. _.
Table DCIV provides 782 compounds of formula Id wherein A1is hydrogen, B1 and B4are
both CH3l and B2 and B3 are both hydrogen and the values of R4a* R4b* R4^ R44 and R8 are
given in Table 1.
Table DCV provides 782 compounds of formula Ie wherein Aj is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a> R4bl R^R^and R*are
given in Table 1.
Table DC VI provides 782 compounds of formula If wherein Ai is hydrogen. B| and B4 are
both CH3i and B2 and B3 are both hydrogen and the values of R4a' R4*5, R4^ R44 and R8 are
given in Table 1.
Table DCVII provides 782 compounds of formula Ig wherein Aj is hydrogen, B1 and B4 are
both CH3l and B2 and B3 are both hydrogen and the values of R4a' R4b' R4** R44 and R8 are
given in Table 1.

Table DCVIil provides 782 compounds of formula Di wherein Ai is hydrogen, B] and B4 are
both CH3( and B2 and B3 are both hydrogen and the values of R4a' R4b* R4c> R4dand R8 are
given in Table I.
Table DC1X provides 782 compounds of formula Ii wherein Ai is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c' R4* and RR are
given in Table 1.
Table DCX provides 782 compounds of formula Ij wherein A\ is hydrogen, B\ and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b* R*^ R4* and R* are
given in Table 1.
Table DCXI provides 782 compounds of formula Ik wherein A1is hydrogen, B] and B4 are
both CH3( and B2 and B3 are both hydrogen and the values of R4a" R4b' R4c' R4* and R8 are
given in Table 1.
Table DCXII provides 782 compounds of formula II wherein Aj is hydrogen, B| and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b* R4c* R4d and R8 are
given in Table I.
Table DCXIII provides 782 compounds of formula Im wherein A\ is hydrogen, B1 and B4 are
both CH3, and B2 and B3are both hydrogen and the values of R4a* R4b' R4c'R4dand R8are
given in Table 1.
Table DCXIV provides 782 compounds of formula In wherein Ai is hydrogen, B1 and B4 are
both CH3. and B2 and B3 are both hydrogen and the values of R4a> R4b> R4c> RM and R8 are
given in Table 1.
Table DCXV provides 782 compounds of formula Io wherein Ai is hydrogen, 3» and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R^R^and R*are
given in Table 1.
Table DCXV1 provides 782 compounds of formula Ip wherein A1is hydrogen, B\ and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4^ R** and R8 are
given in Table 1.
Table DCX VII provides 782 compounds of formula Iq wherein Aj is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a* R4b* R40* RM and R8 are
given in Table 1.

Table DCXVIII provides 782 compounds of formula Ir wherein A1is hydrogen, B1 and B4
are both CH3i and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are
given in Table 1.
Table DCXIX provides 782 compounds of formula Is wherein A1is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b* R4c* R4* and Rs are
given in Table 1.
Table DCXX provides 782 compounds of formula It wherein A) is hydrogen, B: and B* are
both CH3, and B2 and B3 are both hydrogen and the values of R4a- R4b' R4^ R4" and R8 are
given in Table 1.
Table DCXXI provides 782 compounds of formula Iu wherein Ai is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c* R^and R8 are
given in Table 1.
Table DCXXII provides 782 compounds of formula Iv wherein Aj is hydrogen, B1 and B4are
both CH3. and B2 and B3 are both hydrogen and the values of R4a* R4b' R4c' R4d and R8 are
given in Table 1.
Table DCXXIII provides 782 compounds of formula Iw wherein Ai is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b> R4c* R4d and R8 are
eivenin Table 1.
Table DCXXIV provides 782 compounds of formula Ix wherein Ai is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a" R4b' R4^ R4d and R8 are
given in Table 1.
Table DCXXV provides 782 compounds of formula Iy wherein Ai is hydrogen, B| and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R*' R46 and Rg are
given in Table I.
Table DCXXVI provides 782 compounds of formula Iz wherein Ai is hydrogen, B\ and B4
are both CH3t and B2 and B3 are both hydrogen and the values of R4a' R4b* R4^ R4* and R* are
given in Table 1.
Table DCXXVII provides 782 compounds of formula Iaa wherein Ai is hydrogen, B] and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a* R4b* R^R4* and R8are
given in Table 1.

Table DCXXVIII provides 782 compounds of formula lab wherein Ai is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are
given in Table 1.
Table DCXXLX provides 782 compounds of formula lac wherein Aj is hydrogen, B1 and B4
ire both CH3i and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c R4d and R8 are
>iven in Table 1.
Table DCXXX provides 782 compounds of formula lad wherein Aj is hydrogea, Bs and B4
we both CH3i and B2 and B3 are both hydrogen and the values of R4*' R4K R* R^ and R8 are
given in Table 1.
Table DCXXXI provides 782 compounds of formula lae wherein A\ is hydrogen, B\ and B4
are both CH3i and B2 and B3 are both hydrogen and the values of R4a* R4b R^' R4* and R8 are
given in Table 1.
Table DCXXXII provides 782 compounds of formula Iaf wherein Ai is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4B1 R4c' R4d and R8 are
given in Table 1.
Table DCXXXUI provides 782 compounds of formula lag wherein Aj is hydrogen, B1 and B4
are both CH3i and B2 and B3 are both hydrogen and the values of R4a' R4b* R4Ct R4d and R8 are
given in Table 1.
Table DCXXXIV provides 782 compounds of formula Iah wherein Ay is hydrogen, B\ and
B4 are both CH3( and B2 and B3 are both hydrogen and the values of R4a' R4b' R4*' Rw and R8
are given in Table 1.
Table DCXXXV provides 782 compounds of formula Iai wherein At is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4* R4bf R4^ R46 and R8 are
given in Table 1.
Table DCXXXVI provides 782 compounds of formula Iaj wherein Aj is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4*' R4b' R4** R4* and R8 are
given in Table 1.
Table DCXXXVH provides 782 compounds of formula Iak wherein A1is hydrogen, B1 and
B4 are both CH3, and B2 and B3 are both hydrogen and the values of R4a R4** R4^ R4* and R8
are given in Table 1.

Table DCXXXVID provides 782 compounds of formula Ial wherein Ai is hydrogen, B1 and
B4 are both CH3t and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c,R4d and R8
are given in Table 1.
Table DCXXXIX provides 782 compounds of formula lam wherein Ai is hydrogen, B1 and
B4 are both CH3. and B2 and B3 are both hydrogen and the values of R4a* R4b' R4*' R*6 and R8
are given in Table 1.
Table DCXL provides 782 compounds of formula Ian wherein Ai is hydrogen, B? and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a* K4*' R4* R4* and R8 arc
given in Table 1.
Table DCXLI provides 782 compounds of formula Iao wherein Aj is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b* R4c* R4* and R8 are
given in Table 1.
Table DCXLII provides 782 compounds of formula lap wherein A\ is hydrogen, B| and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4B1 R4c' R4d and R8 are
given in Table 1.
Table DCXLIII provides 782 compounds of formula Iaq wherein Ai is hydrogen, B| and B4
are both CH3. and B2 and B3 are both hydrogen and the values of R4a' R4b given in Table 1.
Table DCXLIV provides 782 compounds of formula Iar wherein Aj is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4^ R4* and R8 are
given in Table 1.
Table DCXLV provides 782 compounds of formula las wherein A1is hydrogen, B| and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a> R4b- R^'R^and R8 are
given in Table 1.
Table DCXLVI provides 782 compounds of formula Iat wherein A1is hydrogen, B| and B4
are both CH3( and B2 and B3 are both hydrogen and the values of R4*' R4b' R^* R4* and R8 are
given in Table 1.
Table DCXLVII provides 782 compounds of formula Iau wherein A] is hydrogen, B1 and B4
are both CH3t and B2 and B3 are both hydrogen and the values of R4a> R4b' R4*^ R*4 and R8 are
given in Table 1.

Table DCXLVUI provides 782 compounds of formula lav wherein A( is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b* R4c R4d and R8 are
given in Table 1.
Table DCXLIX provides 782 compounds of formula law wherein A\ is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b* R^R^and R8are
given in Table 1.
Table DCL provides 782 compounds of formula lax wherein Ai is hydrogen, B4 and 34 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a> R4b' R4*' *C* aad R8 are
given in Table 1.
Table DCLI provides 782 compounds of formula lay wherein Ai is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c' R4* and R8 are
given in Table 1.
Table DCLII provides 782 compounds of formula Iaz wherein Ai is hydrogen, B| and B4 are
both CH3( and B2 and B3 are both hydrogen and the values of R4a' R4b* R4c' R4d and R8 are
given in Table 1.
Table DCLIII provides 782 compounds of formula Iba wherein Aj is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b* R4c' R4d and R8 are
given in Table I.
Table DCLIV provides 782 compounds of formula Ibb wherein Ai is hydrogen, B1 and B4 are
both CH3> and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c' Rw ami R8 are
given in Table 1.
Table DCLV provides 782 compounds of formula Ibc wherein A\ is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b> R40' R** and R8 are
given in Table L
Table DCLVI provides 782 compounds of formula Ibd wherein Ai is hydrogen, B[ and B4 are
both CH3l and B2 and B3 are both hydrogen and the values of R4a' R4b' R40* RH and R8 are
given in Table 1.
Table DCLVD provides 782 compounds of formula Ibe wherein Ai is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4hl R4^ R** and R8 are
given in Table 1.

Table DCLVIII provides 782 compounds of formula Ibf wherein A] is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R43' R4b' R4c' R4d and R8 are
given in Table 1.
Table DCLIX provides 782 compounds of formula Ibg wherein Aj is hydrogen, B1 and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a- R4b' R^R^and R8 are
given in Table 1.
Table DCLX provides 782 compounds of formula Ibh wherein Ai is hydrogen, B* and B4 are
both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b R* R4* and R8 are
given in Table 1.
Table DCLXI provides 782 compounds of formula IB1 wherein Ai is hydrogen, B1 and B4 are
both CH3f and B2 and B3 are both hydrogen and the values of R4a' R4b' R4** R46 and R8 are
given in Table 1.
Table DCLXII provides 782 compounds of formula IB1 wherein A\ is hydrogen, B1 and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4c' R4d and R8 are
given in Table 1.
Table DCLXIII provides 782 compounds of formula Ibk wherein A1is hydrogen, B| and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a* R4b' R4^ R4d and R8 are
given in Table 1.
Table DCLXIV provides 782 compounds of formula Ibl wherein Ai is hydrogen, B| and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b' R4^ R4* and R8 are
given in Table 1.
Table DCLXV provides 782 compounds of formula Ibm wherein A1is hydrogen, Bt and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a' R4b> R^'R46 and R8 are
given in Table 1.
Table DCLXVI provides 782 compounds of formula Ibn wherein A1is hydrogen, Bt and B4
are both CH3, and B2 and B3 are both hydrogen and the values of R4a* R4b' R^R^ and R8 are
given in Table 1.
Table DCLXVII provides 782 compounds of fonnula Ibo wherein A1is hydrogen, B1 and B4
are both CH3( and B2 and B3 are both hydrogen and the values of R4a" R4b" R* R4*1 and R8 are
given in Table 1.
Table DCCI provides 782 compounds of formula la wherein Ai is hydrogen, B1, B2, B3 and
B4 are all CH3 and the values of R4a* R4b- R4* R4d and R8 are given in Tabk 1.

Table DCCII provides 782 compounds of formula lb wherein A1is hydrogen, B1, B2, B3 and
B4 are all CH3 and the values of R4a' R4bt R4c' R4d and R8 are given in Table L
Table DCCH1 provides 782 compounds of formula Ic wherein Aj is hydrogen, Bu B2» B3 and
B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in fable 1.
Table DCCIV provides 782 compounds of formula Id wherein Aj is hydrogen, Bu B?, B3 and
B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCV provides 782 compounds of formula Ie wherein Ai is hydrogen, B1, B2, B3 and
B4 are all CH3 and the values of R4* R4b' R4c' R4d and R8 are given in Table I.
Table DCCVI provides 782 compounds of formula If wherein Ai is hydrogen, Bu B?, B3 and
B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCVII provides 782 compounds of formula Ig wherein Aj is hydrogen, Bu B1, B3
and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and Rfi are given in Table 1.
Table DCCVIII provides 782 compounds of formula Ih wherein A] is hydrogen Bu B2i B3
and B4 are all CH3 and the values of R43' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCIX provides 782 compounds of formula Ii wherein Ai is hydrogen, Bu B2, B3 and
B4 are all CH3 and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1.
Table DCCX provides 782 compounds of formula Ij wherein A\ is hydrogen, Bu B2, B3 and
B4 are all CH3 and the values of R4a* R4b' R4c'R4d and R8 are given in Table 1.
Table DCCXI provides 782 compounds of formula Dc wherein A1is hydrogen Bu B2, B3 and
B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCXII provides 782 compounds of formula II wherein Ai is hydrogen, Bu B2, B3
and B4 are all CH3 and the values of R4a* R4b' R4Ct R4d and R8 are given in Table 1.
Table DCCXEQ provides 782 compounds of formula Im wherein A\ is hydrogen, Bu B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c'R4d and R8 are given in Table 1.
Table DCCXIV provides 782 compounds of formula In wherein Ai is hydrogsn, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c> R4*1 and R8 are given in TaB1c 1.
Table DCCXV provides 782 compounds of formula Io wherein Ai is hydrogen, Bu B2, B3
and B4 are all CH3 and the values of R4a' R4bl R4c' R4d and R8 are given in Table 1.
Table DCCXVI provides 782 compounds of formula Ip wherein A\ is hydrogen, Bu B2, B3
and B4 are all CH3 and the values of R4*' R4b* R40, Rw and R8 are given in Table 1.
Table DCCXVII provides 782 compounds of formula Iq wherein Ai is hydrogen, Bu B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4CT R^ and R8 are given in Table 1.

Table DCCXVIII provides 782 compounds of formula Ir wherein A1is hydrogen, B1, B2, B3
and B4 are all CH3 and Ihe values of R4a* R4b* R4c' R4d and R8 are given in Table 1.
Table DCCX1X provides 782 compounds of formula Is wherein A\ is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a> R4t>* R4c' R4d and R8 are given in Table L
Table DCCXX provides 782 compounds of formula It wherein Aj is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a> R4b' R4c' R4d and R8 are given in Tabk L
Table DCCXXI provides 782 compounds of formula Iu wherein Ai is hydrogen, B1, B:, B3
and B4 are all CH3 and the values of R4a' R4b' Rdc* R4d and R8 are given in Table 1.
Table DCCXXII provides 782 compounds of formula Iv wherein A* is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1.
Table DCCXXID provides 782 compounds of formula Iw wherein A\ is hydrogen, B|, B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCXXIV provides 782 compounds of formula Ix wherein A\ is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCXXV provides 782 compounds of formula Iy wherein Ai is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4h> R4c* R4d and R8 are given in Table 1.
Table DCCXXVI provides 782 compounds of formula Iz wherein Ai is hydrogen, B|, B2> B3
and B* are all CHi and the values of R4a' R4b' R4c,R4danH R8ar* oiv^n in TaKI* 1
Table DCCXXVQ provides 782 compounds of formula Iaa wherein A1is hydrogen, B1, B2,
B3 and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCXXVUI provides 782 compounds of formula lab wherein A\ is hydrogen, B1, B2,
B3 and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCXXIX provides 782 compounds of formula lac wherein Ai is hydrogen, B1, B2,
B3 and B4 are all CH3 and the values of R4a' R4b' R4c* R4* and R8 are given in Table I.
Table DCCXXX provides 782 compounds of formula lad wherein Ai is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCXXXI provides 782 compounds of formula Iae wherein Ai is hydrogen, B\, B2,
B3 and B4 are all CH3 and the values of R4a' R4b* R4c> R4d and R8 are given in Table 1.
Table DCCXXXU provides 782 compounds of formula laf wherein A\ is hydrogen, B1, B2,
B3 and B4 are all CH3 and the values of R4a* R4b' R4** R4* and R8 are given in Table 1.
Table DCCXXXIU provides 782 compounds of formula lag wherein Ai is hydrogen, B1, B2,
B3 and B4 are all CH3 and the values of R4a* R4b* R4c* R4* and R8 are given in Table 1.

Table DCCXXXIV provides 782 compounds of formula Iah wherein Ai is hydrogen, Bu B2, B3 and B4 are all CH3 and the values of R4a' R4b R4c
Table DCCL provides 782 compounds of formula lax wherein A\ is hydrogen, 3), B?, B3 and
B4 are all CH3 and the values of R4a* R4b' R4c' R4d and R8 are given in Table 1.
Table DCCLI provides 782 compounds of formula lay wherein Ai is hydrogen, B|, B2* B1
and B4 are-all CH3 and the values of R4a Table DCCLII provides 782 compounds of formula Iaz wherein A] is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4**' R4"' R4d and R8 are given in Table 1.
Table DCCIHI provides 782 compounds of formula Iba wherein Ai is hydrogen, Bu B1, B3
and B4 are all CH3 and the values of R4a* R4b' R4c* R4d and R8 are given in Table I.
Table DCCLIV provides 782 compounds of formula Ibb wherein A3 is hydrogen, B], B:, B3
and B4 are all CH3 and the values of R4a* R4b* R4c' R4d and R8 are given in Table 1.
Table DCCLV provides 782 compounds of formula Ibc wherein A1is hydrogen, Bu B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCLVI provides 782 compounds of formula Ibd wherein A* is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1.
Table DCCLVII provides 782 compounds of formula Ibe wherein Ai is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4b* R4c* R4d and R8 are given in Table 1.
Table DCCLVIII provides 782 compounds of formula Ibf wherein Ai is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a' R4bt R4c- R4d and R8 are given in Table 1.
Table DCCLIX provides 782 compounds of formula Ibg wherein Ai is hydrogen, Bu B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table i.
Table DCCLX provides 782 compounds of formula Ibh wherein A) is hydrogen, B(, B2, B3
and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCLXI provides 782 compounds of formula IB1 wherein A1is hydrogen, B1, B2, B3
and B4 are all CH3 and the values of R4a" R4bl R4c> R4d and R8 are given in Table 1.
Table DCCLXII provides 782 compounds of formula IB1 wherein Ai is hydrogen B1, B2, B3
and B4 are all CH3 and the values of R4a' R4bt R4c' R4d and R8 are given in Table 1.
Table DCCLXIII provides 782 compounds of formula Ibk wherein Ai is hydrogen, B1, B2» B3
and B4 are all CH3 and the values of R4a> R4bt RAc* R4d and R8 are given in Table 1.
Table DCCLXIV provides 782 compounds of formula Ibl wherein Ai is hydrogen, B(, B2, B3
and B4 are all CH3 and the values of R4a' R4b> R4c' R^ and R8 are given in Table 1.
Table DCCLXV provides 782 compounds of formula Ibm wherein Ai is hydrogen, B1, B2,
B3 and B4 are all CH3 and the values of R4a> R4b- R** R4* and R8 are given in Table 1.

Table DCCLXV1 provides 782 compounds of formula Ibn wherein Ai is hydrogen, Bt, B2,
B3 and B4 are all CH3 and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table DCCLXVII provides 782 compounds of formula Ibo wherein A1is hydrogen, B1s B2,
B3 and B4 are all CH3 and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1.
Table DCCCI provides 782 compounds of formula la wherein Ai is hydrogen, 3i and B2 are
together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R4^ R4* and R8 are
given in Table 1.
Table DCCCII provides 782 compounds of formula lb wherein A\ is hydrogen, 3i and B2 are
together =0 and B3 and B4 are both hydrogen and the values of R4** R4b* R^R^and R8are
given in Table 1.
Table DCCCffl provides 782 compounds of formula 1c wherein A\ is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R4c' R4d and R8
are given in Table 1.
Table DCCCIV provides 782 compounds of formula Id wherein A\ is hydrogen, B\ and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R4c' R4d and R8
are given in Table I.
Table DCCCV provides 782 compounds of formula le wherein A» is hydrogen, B\ and B2 are
together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b> R^R^and R8 are
given in Table 1.
Table DCCCVI provides 782 compounds of formula If wherein Ai is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R^R4* and R8
are given in Table 1.
Table DCCCVII provides 782 compounds of formula Ig wherein Ai is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R4^ R44 and R8
are given in Table 1.
Table DCCCVIII provides 782 compounds of formula Ih wherein A1is hydrogen, B| and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R4*- R*4 and R8
are given in Table 1.
Table DCCCIX provides 782 compounds of formula Ii wherein Ai is hydrogen, B1 and B2 are
together =0 and B3 and B4 are both hydrogen and the values of R4t' R4b* R4*- R44 and R8 are
given in Table 1.

Table DCCCX provides 782 compounds of formula Ij wherein Ai is hydrogen, B* and B2 are
together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R4c R4d and R8 are
given in Table 1.
Table DCCCXI provides 782 compounds of formula Ik wherein A) is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R4^ R4* and R8
are given in Table 1.
Table DCCCXII provides 782 compounds of formula II wherein Ai is hydicgca, 33 and B;
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R4* R** and R8
are given in Table 1.
Table DCCCXIII provides 782 compounds of formula Im wherein A\ is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R4c' R4d and R8
are given in Table 1.
Table DCCCXIV provides 782 compounds of formula In wherein A] is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R43, R4b' R4c' R4d and R8
are given in Table 1.
Table DCCCXV provides 782 compounds of formula Io wherein A1is hydrogen, B| and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R4c* R4d and R8
are eiven in Table 1.
Table DCCCXVI provides 782 compounds of formula Ip wherein A\ is hydrogen, Bf and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R*c,R4dand R8
are given in Table 1.
Table DCCCXVII provides 782 compounds of formula Iq wherein At is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a> R4b- R^R^and R8
are given in Table 1.
Table DCCCXVID provides 782 compounds of formula Ir wherein A] is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4** R^R^and
R8 are given in Table 1.
Table DCCCXIX provides 782 compounds of formula Is wherein Ai is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R^ R^R^and R8
are given in Table 1.

Table DCCCXX provides 782 compounds of formula It wherein A1is hydrogen, Bt and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R4c,R4dand R8
are given in Table 1.
Table DCCCXXI provides 782 compounds of formula lu wherein Aj is hydrogen, 3i and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R^R^and R8
are given in Table 1.
Table DCCCXXO provides 782 compounds of formula Iv wherein A\ is hydroee.% Bȣ and B^
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R^R^and R*
are given in Table 1.
Table DCCCXXI1I provides 782 compounds of formula Iw wherein A\ is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R^R4** and
R8 are given in Table 1.
Table DCCCXXIV provides 782 compounds of formula Ix wherein A\ is hydrogen, B| and
B2 are together =0 and B3 and Ba are both hydrogen and the values of R4a' R4bt R4c' R4d and
R are given in Table 1.
Table DCCCXXV provides 782 compounds of formula Iy wherein At is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b> R40' R4d and R8
are given in Table 1.
Table DCCCXXV1 provides 782 compounds of formula Iz wherein Ai is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4h* R^R44 and
R8 are given in Table 1.
Table DCCCXXVII provides 782 compounds of formula laa wherein A1is hycfrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R^R4* and
R are given in Table 1.
Table DCCCXXVDI provides 782 compounds of formula lab wherein A1is hydrogen, B|
and B2 are together =0 and B3 and B4 are both hydrogen and the values of R4** R4*1 R^R44
and R are given in Table 1.
Table DCCCXXIX provides 782 compounds of formula lac wherein Aj is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R*' R4** R4(J and
R8 are given in Table 1.

Table DCCCXXX provides 782 compounds of formula lad wherein Ai is hydrogen, B\ and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R^R4* and
R8 are given in Table 1.
Table DCCCXXXI provides 782 compounds of formula Iae wherein A] is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R40 R4* and
R8 are given in Table 1.
Table DCCCXXXII provides 782 compounds of formula Iaf wherein At is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R43, R4*' R* R44 and
R8 are given in Table 1.
Table DCCCXXXIII provides 782 compounds of formula lag wherein A) is hydrogen, B»
and B2 are together =0 and B3 and B4 are both hydrogen and the values of R4*' R4bt R^R4*
and R8 are given in Table 1.
Table DCCCXXXIV provides 782 compounds of formula Iah wherein Ai is hydrogen, B1
and B2 are together =0 arid B3 and B4 are both hydrogen and the values of R4a' R4b' R*' R4d
and R8 are given in Table 1.
Table DCCCXXXV provides 782 compounds of formula Iai wherein A] is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R4c' R4d and
R8 are given in Table 1.
Table DCCCXXXVI provides 782 compounds of formula Iaj wherein Aj is hydrogen, B| and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R^R4* and
R are given in Table 1.
Table DCCCXXXVII provides 782 compounds of formula Iak wherein Ai is hydrogen, B1
and B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4*' R^'R4*
and R8 are given in Table 1.
Table DCCCXXXVIII provides 782 compounds of formula Iai wherein Ai is hydrogen, B1
and B2 are together =0 and B3 and B4 are both hydrogen and the values of R4*' R4** R40* R4d
and R8 are given in Table 1.
Table DCCCXXXIX provides 782 compounds of formula lam wherein A? is hydrogen, B1
and B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R* R4*' R44
and R8 are given in Table 1.

Table DCCCXL provides 782 compounds of formula Ian wherein A\ is hydrogen, B» and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a> R4b' R4c' R4J and R8
are given in Table 1.
Table DCCCXLI provides 782 compounds of formula Iao wherein Ai is Hydrogen, B| and B2
are together =0 and B3 and B4 are both hydrogen and the values of R43, R4b* R^R^and R8
are given in Table 1.
Table DCCCXLII provides 782 compounds of formula lap wherein A\ is hydrogen. B? and
B: are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4a' R^ R4* and
R8 are given in Table 1.
Table DCCCXLI1I provides 782 compounds of formula Iaq wherein A\ is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R40, R4d and
R8 are given in Table 1.
Table DCCCXLIV provides 782 compounds of formula Iar wherein A\ is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and
R are given in Table 1.
Table DCCCXLV provides 782 compounds of formula las wherein A( is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R4c' R4d and
R8 are given in Table 1.
Table DCCCXLVI provides 782 compounds of formula Iat wherein A( is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R4" R4** and
R8 are given in Table 1.
Table DCCCXLVU provides 782 compounds of formula Iau wherein Ai is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4bl R** R*1 and
R are given in Table 1.
Table DCCCXLVEI provides 782 compounds of formula lav wherein A1is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R^ R^R*1 and
R8 are given in Table 1.
Table DCCCXLIX provides 782 compounds of formula law wherein A1is hydrogen, B| and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4* R*^ R4d and
R8 are given in Table 1.

Table DCCCL provides 782 compounds of formula lax wherein Ai is hydrogen, B] and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a R4d and R8
are given in Table 1.
Table DCCCLI provides 782 compounds of formula lay wherein Ai is hydrogen, B1.and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R4* R4dand R8
are given in Table 1.
Table DCCCLII provides 782 compounds of formula Iaz wherein A\ is hydrogen, B1 and B:
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4*** R4*' K4* and R8
are given in Table 1.
Table DCCCLIII provides 782 compounds of formula Iba wherein A\ is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4* and R8
are given in Table 1.
Table DCCCLIV provides 782 compounds of formula Ibb wherein A] is hydrogen, B( and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R4c* R4d and R8
are given in Table 1.
Table DCCCLV provides 782 compounds of formula Ibc wherein Ai is hydrogen, B| and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R4c* R4d and R8
are given in Table 1.
Table DCCCLVI provides 782 compounds of formula Ibd wherein A\ is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R^R4* and R8
are given in Table 1.
Table DCCCLVII provides 782 compounds of formula Ibe wherein Aj is hydrogen, B( and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R45, R^R44 and
R8 are given in Table 1.
Table DCCCLVHI provides 782 compounds of formula Ibf wherein Ai is hydrogen, B\ and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R^'R44 and
R8 are given in Table 1.
Table DCCCL1X provides 782 compounds of formula Ibg wherein Ai is hydrogen, B| and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4*' R4b> R^R*1 and Rs
are given in Table 1.

Table DCCCLX provides 782 compounds of formula Ibh wherein Ai is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b' R4c* R4d and R8
are given in Table 1.
Table DCCCLXI provides 782 compounds of formula IB1 wherein At is hydrogen, B1 and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4bl R^R^and R8
are given in Table 1.
Table DCCCLXH provides 782 compounds of formula IB1 wherein Aj is hydrogen, B1 ami
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4*1 R45, R4*" R** and
R are given in Table 1.
Table DCCCLXIII provides 782 compounds of formula Ibk wherein A1is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R4c' R4d and
R8 are given in Table 1.
Table DCCCLXIV provides 782 compounds of formula Ibl wherein A\ is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R4c' R4d and
Q
R are given in Table 1.
Table DCCCLXV provides 782 compounds of formula Ibm wherein At is hydrogen, Bt and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R4c,R4d and
R8 are given in Table 1.
Table DCCCLXVI provides 782 compounds of formula Ibn wherein A\ is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b* R^R4* and
R8 are given in Table 1.
Table DCCCLXVII provides 782 compounds of formula Ibo wherein A1is hydrogen, B1 and
B2 are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4bt R^R44 and
R8 are given in Table 1.
Table C1-4I provides 782 compounds of formula la wherein A\ and B1 together form
a bond and B2) B3 and B4 are all hydrogen and the values of R4a> R4b* R4c' R4d and Rs are given
in Table 1.
Table C1-4II provides 782 compounds of formula lb wherein At and B\ together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R40, R4* and R* are given
in Table 1.
Table C1-4III provides 782 compounds of formula Ic wherein A1and B1 together form

a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4Cf R4d and R8 are given
in Table 1.
Table C1-4IV provides 782 compounds of formula Id wherein A\ and B1 together form
a bond and "B2, B3 and B4 are all hydrogen and-the values of R4a* R4b* R4c' R4d and R8 are given
in Table 1.
Table C1-4V provides 782 compounds of formula Ie wherein Ai and B1 together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R40, R*5 and Rf are given
in Table 1.
Table C1-4VI provides 782 compounds of formula If wherein Ai and B* together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4* and R8 are given
in Table 1.
Table C1-4 VII provides 782 compounds of formula Ig wherein A\ and B| together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a R4b' R4c* R4d and R8 are given
in Table 1.
Table C1-4VITI provides 782 compounds of formula Ih wherein A) and B| together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c> R4d and R8 are given
in Table 1.
Table C1-4IX provides 782 compounds of formula Ii wherein Ai and B1 together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R40, R4d and Rsare given
in Table 1.
Table C1-4X provides 782 compounds of formula Ij wherein Ai and B1 together farm
a bond and B2) B3 and B4 are all hydrogen and the values of R4a' R4b' R4Ct R4d and R* are given
in Table 1.
Table C1-4XI provides 782 compounds of formula Ik wherein A1and B1 together form
a bond and B2) B3 and B4 are all hydrogen and the values of R4a' R4b' R4Cf R4dand RS3re given
in Table 1.
Table C1-4XII provides 782 compounds of formula II wherein A( and B1 together ftsnn
a bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R40' K46 and R* are given
in Table 1.
Table C1-4XID provides 782 compounds of formula Im wherein A1and B\ together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4** R4b' R4^ Rw and R* are given
in Table 1.

Table C1-4XTV provides 782 compounds of formula In wherein A1and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c* R4d and R8 are given
in Table 1.
Table C1-4XV provides 782 compounds of formula Io wherein Aj and B| together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R*are given
in Table 1.
Table C1-4XVI provides 782 compounds of formula Ip wherein Aj and B[ together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4* and R€ are given
in Table 1.
Table C1-4XVII provides 782 compounds of formula Iq wherein A1and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a R4b' R4c R4d and R8 are given
in Table 1.
Table C1-4XVIII provides 782 compounds of formula Ir wherein A1and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c,R4d and R8 are given
in Table 1.
Table C1-4X1X provides 782 compounds of formula Is wherein A1and B1 together form a
bond and B2) B3 and B4 are all hydrogen and the values of R4a' R4b' R4c> R4d and R8 are given
in Table 1.
Table C1-4XX provides 782 compounds of formula It wherein At and B1 together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a> R4b* R4c,R4d and R8are given
in Table 1.
Table C1-4XXI provides 782 compounds of formula Iu wherein Ai and B1 together form a
bond and B2> B3 and B4 are all hydrogen and the values of R4a> R4b' R4c' R4*5 and R* are given
in Table 1.
Table C1-4XXII provides 782 compounds of formula Iv wherein A1and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c' R4d and R* are given
in Table 1.
Table C1-4XXIII provides 782 compounds of formula Iw wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R* are given
in Table 1.

Table C1-4XXIV provides 782 compounds of formula Ix wherein Ai and B( together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c,R4d and R8are given
in Table 1.
Table C1-4XXV provides 782 compounds of formula Iy wherein Ai andB1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4XXVI provides 782 compounds of formula Iz wherein Aj and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R43' R4b' R4* R4d and R8 are given
in Table 1.
Table C1-4XXVII provides 782 compounds of formula Iaa wherein Ai and B| together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R8 are given
in Table 1.
Table C1-4XXVID provides 782 compounds of formula lab wherein A\ and B1 together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4XXIX provides 782 compounds of formula lac wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4XXX provides 782 compounds of formula lad wherein Aj is hydrogen, B? and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a* R4b* R^'R^and R8
are given in Table 1.
Table C1-4XXXI provides 782 compounds of formula Iae wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R41, R4b' R4c> R4d and R8 are given
in Table 1.
Table C1-4XXXII provides 782 compounds of formula Iaf wherein Ai and Bt together form a
bond and B2, B3 and B4 are ail hydrogen and the values of R4*' R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4XXXIII provides 782 compounds of formula lag wherein Ai and B| together form
a bond and B2f B3 and B4 are all hydrogen and the values of R4* R4b' R^'R^and Rf are given
in Table 1.

Table C1-4XXXJV provides 782 compounds of formula Iah wherein Aj and B1 together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given
in Table 1.
Table C1-4XXXV provides 782 compounds of formula Iai wherein Ai and B1 together form a
bond and B2, B3 and B4are all hydrogen and the values of R4a* R4b' R4cR4dand R8 are given
in Table 1.
Table C1-4XXXVI provides 782 compounds of formula Iaj wherein Aj and B| together fonn
a bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4*' R4d and R* are given
in Table 1.
Table C1-4XXXVII provides 782 compounds of formula Iak wherein Ai and B| together form
a bond and 83. B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given
in Table 1.
Table C1-4XXXVIII provides 782 compounds of formula Ial wherein A1and B\ together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4XXX1X provides 782 compounds of formula lam wherein A1and B1 together fonn
a bond and B2, B3 and B4 are all hydrogen and the values of R4a' R46, R4c' R4d and R8 are given
in Table 1.
Table C1-4XL provides 782 compounds of formula Ian wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4XLI provides 782 compounds of formula Iao wherein A1and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a> R4b* R4c' R4d and R* are given
in Table 1.
Table C1-4XLII provides 782 compounds of formula lap wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4bf R*' R4d and R1 arc given
in Table 1.
Table C1-4XLIII provides 782 compounds of formula Iaq wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4**' R40* R^ ami R1 are given
in Table 1.

Table C1-4XLIV provides 782 compounds of formula Iar wherein Ai and B1 together form a
bond and B2> B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4XLV provides 782 compounds of formula las wherein A\ and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4^ and Re are given
in Table 1.
Table C1-4XLVI provides 782 compounds of formula Iat wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R8 are given
in Table 1.
Table C1-4XLVII provides 782 compounds of formula Iau wherein A1and B\ together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c* R4d and R8 are given
in Table 1.
Table C1-4XLVIII provides 782 compounds of formula lav wherein A\ and B\ together form
a bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given
in Table 1.
Table C1-4XLIX provides 782 compounds of formula law wherein A1and B| together form a
bond and B2, B3 and B4 are all hydrogen and the values of R43, R4b' R4c' R4d and R8 are given
in T?*bl? 1:
Table C1-4L provides 782 compounds of formula lax wherein Ai and B| together form a bond
and B2> B3 and B4 are all hydrogen and the values of R4a' R4b> R4c*R4d and R8 are given in
Table 1.
Table C1-4LI provides 782 compounds of formula lay wherein A) and B» together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4*' R*d and R8 arc given
in Table 1.
Table C1-4LII provides 782 compounds of formula Iaz wherein Aj and B1 together fern a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4Ct R4d and Rg are given
in Table I.
Table C1-4LID provides 782 compounds of formula Iba wherein A] and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4** R4b* R^'R441 and R1 are given
in Table 1.

Table C1-4LIV provides 782 compounds of formula Ibb wherein A1and Bf together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4LV provides 782 compounds of formula Ibc wherein A1arid B» together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a" R4b> R4c' R4d and R8 are given
in Table 1.
Table C1-4LVI provides 782 compounds of formula Ibd wherein Aj and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R40' R4d and R8 zrz given
in Table 1.
Table C1-4LVII provides 782 compounds of formula Ibe wherein A\ and B1 together foim a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table C1-4LVIII provides 782 compounds of formula Ibf wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b" R4c' R4d and R8 are given
in Table 1.
Table C1-4LIX provides 782 compounds of formula lbg wherein A1and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a in Table 1.
Table C1-4LX provides 782 compounds of formula Ibh wherein A] and B| together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given
in Table 1.
Table C1-4LXI provides 782 compounds of formula IB1 wherein Ai and B\ together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4d and R8 arc given
in Table 1.
Table C1-4LXI1 provides 782 compounds of formula IB1 wherein A1and Bt togetha* fenn a
bond and B2) B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given
in Table 1.
Table C1-4LXIII provides 782 compounds of formula Ibk wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4d and R1 arc given
in Table 1.

Table C1-4LXIV provides 782 compounds of formula Ibl wherein A» and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c* R4d and R8 are given
in Table 1.
Table C1-4LXV provides 782 compounds of formula Ibm wherein Ai and B| together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R40, R4d and R8 are given
in Table 1.
Table C1-4LXVI provides 782 compounds of formula Ibn wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c> R4d and R* are given
in Table 1.
Table C1-4LXVII provides 782 compounds of formula Ibo wherein Ai and B1 together form a
bond and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given
in Table 1.
Table MI provides 782 compounds of formula la wherein A1and B1 together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table Mil provides 782 compounds of formula lb wherein Aj and B| together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given
in Tahle 1.
Table Mill provides 782 compounds of formula Ic wherein Aj and B] together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1:
Table MIV provides 782 compounds of formula Id wherein Ai and B| together form
-CH2- and B2, B3 and B4 are all hydrogen and the .values of R4a* R4b' R4c' R4d and R8 are given
in Table 1.
Table MV provides 782 compounds of formula Ie wherein Aj and B1 together form
-CH2- and B2, B3 and B4are all hydrogen and the values of R4*' R4bf R4Cf R4dand R*are given
in Table 1.
Table MVI provides 782 compounds of formula If wherein Aj and B| together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R4* R4b' R4c* R*6 and R1 are given
in Table 1.

Table MVIl provides 782 compounds of formula Ig wherein Aj and B1 together form -CH2-
and B2, B3 and B4 are all hydrogen and the values of R4a' R4b) R4Cf R4d and R8 are given in
Table 1.
Table MVIII provides 782 compounds of formula Ih wherein At and B\ together form"-CH2-
and B2> B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table ].
Table MIX provides 782 compounds of formula Ii wherein Ai and B| together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c> R4d and R* are given
in Table 1.
Table MX provides 782 compounds of formula Ij wherein A1and B1 together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R4a> R4b* R4c> R4d and R8 are given
in Table 1.
Table MXI provides 782 compounds of formula Ik wherein Ai and B] together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c> R4d and R8 are given
in Table 1.
Table MXH provides 782 compounds of formula II wherein A1and B1 together form
-CH2- and B2, B3 and B4 are all hydrogen and the values of R43, R4b' R4c' R4d and R8 are given
in Table 1.
Table MXIII provides 782 compounds of formula Im wherein Aj and B| together form -CH2-
and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in
Table 1.
Table MXIV provides 782 compounds of formula In wherein Ai and B1 together form -CH2-
and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c'R4d and R8are given in
Table 1.
Table MXV provides 782 compounds of formula Io wherein A1and B| together form -CH2-
and B2, B3 and B4 are all hydrogen and the values of R4a' R4bl R4c* R4d and R8 are given in
Table L
Table MXV1 provides 782 compounds of formula Ip wherein Ai and B| together form -CHr
and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c'R4d and R8 are given in
Table 1.

Table MXVII provides 782 compounds of formula Iq wherein A1and B1 together form -CH2-and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c,R4d and R8 are given in Table 1. * Table MXVM provides 782 compounds of formula Ir wherein A1and B1 together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table MXIX provides 782 compounds of formula Is wherein A\ and B| together form -CH2-and B2, B3 and B4 are all hydrogen and the values of R4a' R4* R4*' R4^ and R8 are grvea m Table 1.
Table MXX provides 782 compounds of formula It wherein A1and B| together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table MXXI provides 782 compounds of formula Iu wherein A1and B1 together form -CH2-and B2, B3 and B4 are all hydrogen and the values of R4a* R4bt R4c* R4d and R8 are given in Table 1.
Table MXXII provides 782 compounds of formula Iv wherein A( and B} together form -CH2-and B2) B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1.
Table MXX1H provides 782 compounds of formula Iw wherein Ai and B1 together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c* R4d and R8 are given in Table 1.
Table MXXIV provides 782 compounds of formula Ix wherein Ai and B1 together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4*' R4c' R4d and R8 are given in Table 1.
Table MXXV provides 782 compounds of formula ly wherein Ai and B| together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4b( R4* R4d and R8 are given in Table 1.
Table MXXVI provides 782 compounds of formula Iz wherein Ai and B1 together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4c' R4a and R8 are given in Table 1.

Table MXXVII provides 782 compounds of formula Iaa wherein Ai and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b| R4c' R4d and R8 are given
in Table 1.
Table MXXVIII provides 782 compounds of formula lab wherein Ai and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and RB are given
in Table 1.
Table MXXIX provides 782 compounds of formula lac wherein A\ and B| together forr* -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4** and Rs are given
in Table 1.
Table MXXX provides 782 compounds of formula lad wherein Ai is hydrogen, B\ and B2
are together =0 and B3 and B4 are both hydrogen and the values of R4a' R4b' R4c,R4dand R8
are given in Table 1.
Table MXXXI provides 782 compounds of formula Iae wherein A\ and B| together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table MXXXII provides 782 compounds of formula Iaf wherein Ai and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table MXXXIII provides 782 compounds of formula lag wherein At and B1 together form -
CH2- and B2f B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table 1.
Table MXXXIV provides 782 compounds of formula lah wherein Ai and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 ^e given
in Table 1.
Table MXXXV provides 782 compounds of formula Iai wherein Ai and B\ together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4c> R4d and R8 are given
in Table 1.
Table MXXXVI provides 782 compounds of formula laj wherein A1and B| together form -
CH2- and B2> B3 and B4 are all hydrogen and the values of R4a' R4b' R^'R^ and R* arc given
in Table 1.

Table MXXXV1I provides 782 compounds of formula Iak wherein At and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4bl R4c' R4d and R8 are given
in Table 1.
Table MXXXVHhprovides 782 compounds of formula Ial^wherein Ai and B| together form J '"
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c* R4d and RB are given
in Table 1.
Table MXXXIX provides 782 compounds of formula lam wherein A1and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R4** R4d and R8 arc given
in Table 1.
Table MXL provides 782 compounds of formula Ian wherein Ai and B1 together form -CH2-
and B2> B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table MXLI provides 782 compounds of formula Iao wherein Aj and B1 together form -CH2-
and B2> B3 and B4 are all hydrogen and the values of R4a' R4bt R4c' R4d and R8 are given in
Table 1.
Table MXL1I provides 782 compounds of formula lap wherein Ai and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given
in Table 1.
Table MXLIII provides 782 compounds of formula Iaq wherein Aj and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a> R4b' R4c* R4d and R8 are given
in Table 1.
Table MXLIV provides 782 compounds of formula Iar wherein A) and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4*' R4b| R4Cf R4d and R8 are given
in Table 1.
Table MXLV provides 782 compounds of formula las wherein A\ and B| together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4b> R4cR4d and R8are given
in Table 1.
Table MXLVI provides 782 compounds of formula Iat wherein Aj and B| together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4i* R4b' R40, R4* and R8 are given
in Table I.

Table MXLVII provides 782 compounds of formula Iau wherein Ai and B| together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c' R4d and R8 are given in Table 1.
Table MXLVIII provides 782 compounds of formula lav wherein Aj and B1 together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1,
Table MXLIX provides 782 compounds of formula law wherein Ai and B1 together forr, -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1.
Table ML provides 782 compounds of formula lax wherein Ai and B1 together form -CH2-and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R4c* R4d and R8 are given in Table 1.
Table MLI provides 782 compounds of formula lay wherein Ai and B1 together form -CH?-and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given in Table 1.
Table MLII provides 782 compounds of formula laz wherein Ai and B1 together form -CH2-and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table MLHI provides 782 compounds of formula Iba wherein Aj and B» together form -CH2-and B2, B3 and B4 are all hydrogen and the values of R4a* R4b* R4c' R4d and R8 are given in Table 1.
Table MLIV provides 782 compounds of formula Ibb wherein A\ and B1 together form -CH2- and B2j B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in Table 1.
Table MLV provides 782 compounds of formula Ibc wherein Ai and B1 together fonn -CH2-and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R46' R4d and R8 are given in Table 1.
Table MLVI provides 782 compounds of formula Ibd wherein Ai and B| together form -CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R40' R4d and R8 are given in Table 1.

Table MLVII provides 782 compounds of formula Ibe wherein Aj and B1 together form -
CHr and B2? B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given
in Table I.
Table MLVUI provides 782 compounds of formula Ibf wherein A\ and B| together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4bt R4c> R4d and R8 are given
in Table 1.
Table MLIX provides 782 compounds of formula Ibg wherein Ai and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4*' R4*' R4* and R8 are given
in Table 1.
Table MLX provides 782 compounds of formula Ibh wherein Ai and B1 together form -CHr
and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and Rg are given in
Table 1.
Table MLXI provides 782 compounds of formula lB1 wherein Ai and B| together form -CH2-
and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c' R4d and R8 are given in
Table 1.
Table MLXII provides 782 compounds of formula IB1 wherein Ai and B1 together form -
CH2- and B2) B3 and B4 are all hydrogen and the values of R4a' R4b* R4c* R4d and R8 are given
in Table 1.
Table MLXIII provides 782 compounds of formula Ibk wherein Ai and B\ together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4c' R4d and R8 are given
in Table 1.
Table MLXIV provides 782 compounds of formula Ibl wherein Aj and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b> R4Cl R4d and R8 are given
in Table 1.
Table MLXV provides 782 compounds of formula Ibm wherein A\ and B\ together &>nn -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a* R4b' R40, R4d and R8 arc given
in Table 1.
Table MLXVI provides 782 compounds of formula Ibn wherein Ai and B1 together fc^m -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b* R^' R4d and R8 are given
in Table 1.

Table MLXVII provides 782 compounds of formula Ibo wherein A[ and B1 together form -
CH2- and B2, B3 and B4 are all hydrogen and the values of R4a' R4b' R4c* R4d and R8 are given
in Table 1.
Table MCI provides 782 compounds of formula la wherein A1is hydrogen, B\ and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a' R4b
R4c' R4d and R8 are given in Table 1.
Table MCII provides 782 compounds of formula lb wherein A1is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R**~ R4**'
R4c'R4d and R8 are given in Table 1.
Table MCIII provides 782 compounds of formula Ic wherein A1is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*' R4b'
R4c' R4d and Rs are given in Table 1.
Table MCIV provides 782 compounds of formula Id wherein A1is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a' R4b'
R4c' R4d and R8 are given in Table 1.
Table MCV provides 782 compounds of formula Ie wherein A1is hydrogen, B\ and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a' R4b'
R4c* R4d and R8 are given in Table ,.
Table MCVI provides 782 compounds of formula If wherein Ai is hydrogen, B| and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4^ R4**
R4c' R4d and R8 are given in Table 1.
Table MCVII provides 782 compounds of formula Ig wherein Ai is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R**" R4b*
R4Cl R4d and R8 are given in Table 1.
Table MCVEII provides 782 compounds of formula Ih wherein A1is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*" R4b*
R4c> R4d and R8 are given in Table I.
Table MCIX provides 782 compounds of formula Ii wherein A1is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4^ R4b*
R4c- R4d and R8 are given in Table 1.

Table MCX provides 782 compounds of formula Ij wherein A] is hydrogen, B] and B3
together form a group-Cfy-CH:-, and B2 and B4 are both hydrogen and the values of R4a* R4b'
R4c' R4d and R8 are given in Table 1.
Table MCXI provides 782 compounds of formula Dc wherein A] is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R43, R4**'
R4c* R4d and R8 are given in Table 1.
Table MCXII provides 782 compounds of formula II wherein Aj is hydrogen, B? and B»
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R^ R*Ct
R4c* R4d and R8 are given in Table 1.
Table MCXIE provides 782 compounds of formula Im wherein A\ is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4b'
R4c' R4d and R8 are given in Table 1.
Table MCXIV provides 782 compounds of formula In wherein A1is hydrogen, B» and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a' R4bt
R4c' R4d and R8 are given in Table 1.
Table MCXV provides 782 compounds of formula Io wherein Aj is hydrogen, B] and B3
together form a group-CH2-CH2-> and B2 and B4 are both hydrogen and the values ofR4*1 R4b'
R4c' R4d and R8 are given in Table 1.
Table MCXVI provides 782 compounds of formula Ip wherein Ai is hydrogen, B| and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4b*
R4c* R4d and R8 are given in Table 1.
Table MCXVII provides 782 compounds of formula Iq wherein Ai is hydrogen, B1 and B3
together form a group-CH2-CH2-» and B2 and B4 are both hydrogen and the values of R4** R4**'
R4c' R4d and R8 are given in Table 1.
Table MCXVID provides 782 compounds of formula Ir wherein At is hydrogen, B% and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R*** R4bt
R4c* R4d and R8 are given in Table 1.
Table MCXIX provides 782 compounds of formula Is wherein Aj is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R**" R4**
R4c> R4d and R8 are given in Table 1.

Table MCXX provides 782 compounds of formula It wherein Ai is hydrogen, Bt and B3
together form a group-CH2-CH2-, and B? and B4 are both hydrogen and the values of R4a' R4b'
R4c' R4d and R8 are given in Table 1.
Table MCXXI provides 782 compounds of formula Iu wherein Aj is hydrogen, B'J and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*' R4fc*
R4c'R4d and R8 are given in Table i.
Table MCXXII provides 782 compounds of formula Iv wherein Ai is hydrogen, B1 and 3 3
together form a group-CH2-CH2-> and B? and B4 are both hydrogen and the values of R^ R"**
R4c* R4d and R8 are given in Table 1.
Table MCXXIII provides 782 compounds of formula lw wherein Ai is hydrogen, B1 and B3
together form a group-CHs-CF^-, and B2 and B4 are both hydrogen and the values of R4a* R*b'
R4c* R4d and R8 are given in Table 1.
Table MCXXIV provides 782 compounds of formula Ix wherein Aj is hydrogen, &\ and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a> R4b'
R4Cl R4d and R8 are given in Table 1.
Table MCXXV provides 782 compounds of formula Iy wherein Aj is hydrogen, B\ and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a* R4bl
R4c* R4d and R8 are given in Table 1.
Table MCXXVI provides 782 compounds of formula Iz wherein Ai is hydrogen, B1 and B3
together form a group~CH2-CH2-, and B2 and B4 are both hydrogen and the values of R44, R4b(
R4C( R4d and R8 are given in Table 1.
Table MCXXVII provides 782 compounds of formula laa wherein A1 is hydrogen, B* and B3
together form a group-CH2-CH2-3 and B2 and B4 are both hydrogen and the values of R4*1 R4b'
R4c> R4d and R8 are given in Table 1.
Table MCXXVIU provides 782 compounds of formula lab wherein At is hydrogen, B] and
B3 together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4Cl R4d and R8 are given in Table 1.
Table MCXXIX provides 782 compounds of formula lac wherein A\ is hydrogen, &\ and B3 together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4b' R4c' R4d and R8 are given in Table 1.

Table MCXXX provides 782 compounds of formula lad wherein At is hydrogen, B1 and B3
together form a group-CH^-CHj-, and B2 and B4 are both hydrogen and the values of R4a' R4b*
R4c, R4d and R8 are given in Table 1.
Table MCXXXI provides 782 compounds of formula lae wherein Ai is hydrogen, B\ and B5
together form a group-CH:-CH2-, and B2 and B4 are both hydrogen and the values of R4*" R4fe*
R4c' R4d and R8 are given in Table 1.
Table MCXXXII provides 782 compounds of formula laf wherein A\ is hydrogen, B\ aad B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and (he values of R4* K*'
R4c'R4d and R8 are given in Table 1.
Table MCXXXIII provides 782 compounds of formula lag wherein Ai is hydrogen, B1 and
B3 together form a group-CH2-CH2-5 and B2 and B4 are both hydrogen and the values of R4** R4c, R4d and R8 are given in Table 1.
Table MCXXXIV provides 782 compounds of formula lah wherein Ai is hydrogen, B1 and
B3 together form a group-CHs-CHb-, and B2 and B4 are both hydrogen and the values of R4a* R4c, R4d and R8 are given in Table 1.
Table MCXXXV provides 782 compounds of formula lai wherein Ai is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4iU R4b*
R4c* R4d and R8 are given in Table 1.
Table MCXXXVI provides 782 compounds of formula laj wherein Ai is hydrogen, B\ and
B3 together form a group~CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*
R4b* R4c* R4d and R8 are given in Table 1.
Table MCXXXVH provides 782 compounds of formula Iak wherein Ai is hydrogen, Bx and
B3 together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R44,
R4c, R4d and R8 are given in Table 1.
Table MCXXXVHI provides 782 compounds of formula Ial wherein Ai is hydrogen, B* and B3 together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R44,
R4c, R4d and R8 are given in Table 1.
Table MCXXXIX provides 782 compounds of formula lam wherein Ai is hydrogen, B1 and
B3 together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4c, R4d and R8 are given in Table 1.

Table MCXL provides 782 compounds of formula Ian wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH:-, and B2 and B4 are both hydrogen and the values of R4a* R4b'
R4c> R4d and R8 are given in Table 1.
Table MCXLI provides 782 compounds of formula Iao wherein A1is hydrogen, B1 and B3 -
together form a group~CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a* R4**'
R4c' R4d and R8 are given in Table 1.
Table MCXLII provides 782 compounds of formula lap wherein Aj is hydrogen, B\ and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R^ R*5,
R4c' R4d and R8 are given in Table 1.
Table MCXLI1I provides 782 compounds of formula Iaq wherein Ai is hydrogen, B| and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a* R4b*
R40, R4d and R8 are given in Table 1.
Table MCXLIV provides 782 compounds of formula Iar wherein Aj is hydrogen, B\ and B3
together form a group-CH2-CH2-» and B2 and B4 are both hydrogen and the values of R4a' R4b'
R4c> R4d and R8 are given in Table 1.
Table MCXLV provides 782 compounds of formula las wherein Aj is hydrogen, B1 and B3
together form a group-CH2-CH2-s and B2 and B4 are both hydrogen and the values of R4a* R4bt
R4c' R4d and R8 are given in Table 1.
Table MCXLVI provides 782 compounds of formula lat wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*' R4^
R4c' R4d and R8 are given in Table 1,
Table MCXLVI1 provides 782 compounds of formula Iau wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2:-, and B2 and B4 are both hydrogen and the values of R4* R4b
R4c' R4d and R8 are given in Table 1.
Table MCXLVEQ provides 782 compounds of formula lav wherein A1 is hydrogen, B1 and
B3 together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a R4c,R4d,and R8 are given in Table 1.
Table MCXLLX provides 782 compounds of formula law wherein Aj is hydrogen, B1and B3 together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a R4b R4c' R4d and R8 are given in Table 1.

Table MCL provides 782 compounds of formula lax wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a* R4b"
R4c' R4d and R8 are given in Table 1.
Table MCLI provides 782 compounds of formula lay wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*' R4*'
R4c' R4d and R8 are given in Table 1.
Table MCLI1 provides 782 compounds of formula laz wherein A1 is hydrogen, B1 and 3:,
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*" R4*
R4c- R4d and R8 are given in Table 1.
Table MCLIII provides 782 compounds of formula Iba wherein Aj is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a* R4**
R4c* R4d and R8 are given in Table 1.
Table MCLIV provides 782 compounds of formula Ibb wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a% R4b*
R4c' R4d and R8 are given in Table 1.
Table MCLV provides 782 compounds of formula Ibc wherein A1 is hydrogen, B1 and B3
together form a group-CH?-CH2-, and B2 and B4 are both hydrogen and the values of R4a' R4b'
R4c' R4d and R8 are given in Table 1.
Table MCLVI provides 782 compounds of formula Ibd wherein A1 is hydrogen, B\ and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4**
R4c' R4d and R8 are given in Table 1.
Table MCLVII provides 782 compounds of formula Ibe wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4b*
R4c- R4d and R8 are given in Table 1.
Table MCLVIII provides 782 compounds of formula Ibf wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R4**'
R4c' R4d and R8 are given in Table 1.
Table MCLIX provides 782 compounds of formula Ibg wherein Aj is hydrogen, B) and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4*" R*"
R4c^ R4d and R8 are given in Table 1.

Table MCLX provides 782 compounds of formula Ibh wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a R4c' R4d and R8 are given in Table 1.
Table MCLXI provides 782 compounds of formula fB1 Wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4a R4b* .
R4c'R4d and R8 are given in Table 1.
Table MCLXII provides 782 compounds of formula IB1 wherein Aj is hydrogen, B1 and B3
together form a group-CH2CH2-, and B2 and BA are both hydrogen and the values of R** R4*
R4c' R4d and R8 are given in Table 1.
Table MCLXI1I provides 782 compounds of formula Ibk wherein At is hydrogen, Bt and B3
together form a group-CHrCHs-, and B2 and B4 are both hydrogen and the values of R4a, R4*'
R4c' R4d and R8 are given in Table 1.
Table MCLXIV provides 782 compounds of formula Ibl wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CHr, and B2 and B4 are both hydrogen and the values of R4a' R4t>)
R4c' R4d and R8 are given in Table 1.
Table MCLXV provides 782 compounds of formula Ibm wherein A1 is hydrogen, B1 and B3
together form a group-CHrCH2-, and B2 and B4 are both hydrogen and the values of R4a' R4b'
R4c' R4d and R8 are given in Table 1.
Table MCLXVI provides 782 compounds of formula Ibn wherein A1 is hydrogen, B\ and B3
together form a group-CHrCH2-s and B2 and B4 are both hydrogen and the values of R4** R4^
R4c' R4d and R8 are given in Table 1.
Table MCLXVTI provides 782 compounds of formula Ibo wherein A1 is hydrogen, B1 and B3
together form a group-CH2-CH2-, and B2 and B4 are both hydrogen and the values of R4** R45,
R4c' R4d and R8 are given in Table 1.
Mass spectra data were obtA1ned for selected compounds of Tables I to MCLXVTI using LC1-4S: LC5: 254nm - gradient 10% A to 100% B A=H2O+0.01%HCOOH B<:h3cn positive electrospray m the data are shown in table>
Table 2

The compounds of the invention may be synthesised by various methods. For example the compounds of formula 1 may be synthesised as described in Scheme 1.
Thus a compound of formula 1 may be synthesised from a compound of formula 2 by reaction with an acid such as trifluoroacetic acid at amB1ent temperature in an organic solvent such as dichloromethane, chloroform or 1,2-dichloroethane followed by neutralisation of the reaction mixture with an aqueous solution of an iC1-4rganic base such as sodium carbonate, sodium B1carbonate or similar compound. The intermediate thus formed the reacts with an alkylating agent of the formula R8-L, where L is chloride, bromide, iodide or a sulfonate (e.g. mesylate or tosylate) or similar leaving group at a temperature of between amB1ent temperature and 100°C, typically amB1ent temperature, in an organic solvent such as acetonitrile, dimethylformamide, dichloromethane, chloroform or 1,2-dichloroethane in the presence of a tertiary amine base such as triethylamine or diisopropylethylarnine and optionally catalysed by halide salts such as sodium iodide, potassium iodide or tetrabutylammonium iodide.
Alternatively a compound of formula 2, after removal of the t-butoxycarbonyl protecting group as described above, may be reacted with an aldehyde of the formula RCHO at a temperature between amB1ent temperature and 100°C in an organic solvent such as tetrahydrofuran or ethaC1-4l or mixtures of solvents in the presence of a reducing agent such as borane-pyridine complex, sodium borohydride, sodium (triacetoxy)borohydride, sodium cyaC1-4borohydride or such like, to produce a compound of formula 1 where R8 is CH2R-
In an alternative method compounds of formula 1 maybe obtA1ned from compounds of formula 6 by reaction with a suitable electrophilic species. Compounds of formula 1 where

Y is a carbonyl group may be formed by the reaction of compounds of formula 6 with a carboxylic acid derivative of formula R1-C(0)-Z where Z is chloride, hydroxy, alkoxy or acyloxy at a temperature between 0°C and 150°C optionally in an organic solvent such as dichloromethane, chloroform or 1,2-dichloroethane, optionally in the presence of a tertiary amine base such as triethylamine or diisopropylethylamine and optionally in the presence of a coupling agent such as dicyclohexylcarbodiimide. Compounds of formula 1 where Y is a carbonyl group and Rl is an amiC1-4 substituent of formula R'-NH- may be formed by the reaction of compounds of formula 6 with an isocyanate of formula R'-N=C=0 under similar conditions. Compounds of formula 1 where Y is a group of formula S(0)q maybe formed from compounds of formula 6 by treatment with compounds of formula of Rl-S(0)q-CI under similar conditions. Compounds of formula 1 where Y is a thiocarbonyl group and Rl is an amiC1-4 substituent of formula R'-NH- may be formed by the reaction of compounds of formula 6 with an isothiocyanate of formula R'-N=C=S under similar conditions. Alternatively compounds of formula 1 where Y is a thiocarbonyl group and Rl is a carbon substituent may be formed by treatment of compounds of formula 1 where Y is a carbonyl group and Rl is a carbon substituent with a suitable thionating agent such as Lawesson's reagent.
In the above procedures, acid derivatives of the formula R1-C(0)-Z, isocyanates of formula R'-N=C=0, isothiocyanates of formula R'-N=C=S and sulfur electrophiles of formula Rl-S(0)q-Cl are either kC1-4wn compounds or may be formed from kC1-4wn compounds by kC1-4wn methods by a person skilled in the art.
A compound of formula 2 may be obtA1ned from a compound of formula 3 by reaction with a suitable electrophilic species, as described above.
Compounds of formula 3 may be obtA1ned by reacting compounds of formula 4 with compounds of formula 10 at a temperature of between 0°C and 100°C in an organic solvent such as dichloromethane, chloroform or 1,2-dichloroethane in the presence of an acid such as hydrochloric acid or trifluoroacetic acid and optionnally a co-solvent such as water, methaC1-4l or ethaC1-4l. The intermediates formed are subsequently treated with a reducing agent such as sodium borohydride, sodium (triacetoxy)borohydride, sodium cyaC1-4borohydride, triethylsilane or similar at amB1ent temperature in organic solvent such as ethaC1-4l or chloroform or with a nucleophile R3-M (where M is a metallic species; R3-M is for example

a Grignard reagent). The basic procedure is described in Tetrahedron (1997), 53, 10983-10992.
Similarly, compounds of formula 6 may be synthesised by reacting compounds of formula 7 with compounds of formula 10 using the conditions described above.
Compounds of formula 4 may be obtA1ned from compounds of formula 5 by reaction with a 1-alkoxy substituted phosphonium salt of formula 9 such as
methoxymethyl(triphenyl)phosphonium chloride and a base such as potassium tert-butoxide at a temperature of 0°C to 80°C in tetrahydrofuran.
Similarly, compounds of formula 7 may be synthesised from compounds of formula S using the conditions described above.
Compounds of formula 5, 8 and 10 are either kC1-4wn compounds or may be formed from kC1-4wn compounds by kC1-4wn methods by a person skilled in the art.
CertA1n compounds of formula 2, 3 and 6 are C1-4vel and as such form a further aspect of the invention.



In an alternative melhod a compound of formula 1 wherein Al, A2, A3, A4, B2, B3 and B4 are H and B1 is OH may be obtA1ned from a compound of formula 12 by removal of the t-butoxycarbonyi protecting group and reaction with an alkylating agent R8-L as described previously. A Compound of formula 12 maybe obtA1ned from an intermediate of formula 11 by reaction with an hydroborating agent such as borane in an organic solvent such as dichloromethane or tetrahydrofuran at a temperature of between 0°C to 80°C, followed by treatment with an oxidising agent such as hydrogen peroxide in the presence of water and a base such as sodium hydroxide at a temperature of between 0°C to 100°C (Scheme 2).
The skilled person will readily recognise that it is possible to convert one compound of formula 12 to other compounds of formula 1.

In aC1-4ther alternative method, a compound of formula 11 may be reacted with a suitable fluorinating species, such as Selectfluor®, followed by reaction with a reducing agent such as triethylsilane in the presence of an acid such as trifluoroacetic acid to provide a compound of formula 13 or a compound of formula 14. Compounds of formula 13 (or 14) may be converted into compounds of formula 1 wherein A1, A2, A3, A4, B2, B3 and B4 are H and B1 is F (i.e. A1, A2, A3, A4, B3 and B4 are H, B1 and B2 are F) by reaction with an alkylating agent of the formula R8-L as described previously (Scheme 3).


Compounds of formula 11 may be synthesised by the method outlined on Scheme 4.
Thus a compound of formula 11 may be synthesised from a compound of formula 15 by reacting with an electrophilic species as described previously.
A compound of formula 15 may be prepared from a compound of formula 16 by treatment with a suitable base such as potassium carbonate at a temperature of between 0°C to 80°C in an organic solvent such as methaC1-4l or ethaC1-4l in comB1nation with water.
A compound of formula 16 may be synthesised by cyclising a compound of formula 17 under Heck conditions, typically in the presence of a catalyst such as palladium(II) acetate, optionally a ligand such as triphenylphosphine or/and an additive such as tetrabutylammonium bromide and a base such as triethylamine in an organic solvent such as tetrahydrofuran, acetonitrile, dimethylformamide, N-methyl-pyrrolidiC1-4ne or dimethylacetamide at a temperature of between 20°C to 140°C
Compounds of formula 17 may be synthesised by coupling compounds of formula IS with the kC1-4wn alcohol 19 {J. Org. Chem. 2001,66, 5545-5551) under MitsuC1-4bu conditions, typically using a phosphine such as triphenylphosphine and an azo compound such as diethylazodicarboxylate or diisopropylazodicarboxylate in an organic solvent such as tetrahydrofuran or toluene at a temperature of between 0°C to 80°C.
Compounds of formula 18 are either kC1-4wn compounds or may be formed from kC1-4wn compounds by kC1-4wn methods by a person skilled in the art.



The compounds of formula (I) can be used to combat and control infestations of insect pests such as Lepidoptera, Diptera, Hemiptera, ThysaC1-4ptera, Orthoptera, Dictyoptera, Coleoptera, Siphonaptera, HymeC1-4ptera and Isoptera and also other invertebrate pests, for example, acarine, nematode and mollusc pests. Insects, acarines, nematodes and molluscs are hereinafter collectively referred to as pests. The pests which may be combated and controlled by the use of the invention compounds include those pests associated with agriC1-4lture (which term includes the growing of crops for food and fibre products), hortiC1-4lture and animal husbandry, companion animals, forestry and the storage of products of vegetable origin (such as fruit, grA1n and timber); those pests associated with the damage of man-made structures and the transmission of diseases of man and animals; and also nuisance pests (such as flies).
Examples of pest species which may be controlled by the compounds of formula (I) include: Myzus persicae (aphid), Aphis gossypii (aphid), Aphis fabae (aphid), Lygus spp. (capsids), DysderC1-4s spp. (capsids), Nilaparvata lugens (planthopper), Nephotettixc incticeps (leafhopper), Nezara spp. (stinkbugs), Euschistus spp. (stinkbugs), Leptocorisa spp. (stinkbugs), Frankliniella occidentalis (thrip), Thrips spp. (thrips), LeptiC1-4tarsa decemlineA1a (Colorado potato beetle), AnthoC1-4mus grandis (boll weevil), Aonidiella spp. (scale insects), Trialeurodes spp. (white flies), Bemisia tabaci (white fly), Ostrinia nuB1lalis (European corn borer), Spodoptera littoralis (cotton leafworm), Heliothis virescens (tobacco budworm), Helicoverpa armigera (cotton bollworm), Helicoverpa zea (cotton bollworm), Sylepta derogata (cotton leaf roller), Pieris brassicae (white butterfly), Plutella xylostella (diamond back moth), Agrotis spp. (C1-4tworms), Chilo suppressalis (rice stem borer), LoC1-4sta migratoria (loC1-4st), Chortiocetes terminifera (loC1-4st), Diabrotica spp. (rootworms), PaC1-4nychus ulmi (European red mite), PaC1-4nychus citri (citrus red mite), Tetranychus urticae (two-spotted spider mite), Tetranychus cinnabarinus (carmine spider mite), Phyllocoptruta oleivora (citrus rust mite), Polyphagotarsonemus latus (broad mite), Brevipalpus spp. (flat mites), Boophilus microplus (cattle tick), Dermacentor variaB1lis (American dog tick), CteC1-4cephalides felis (cat flea), Liriomyza spp. (leaftniner), Musca domestica (housefly), Aedes aegypti (mosquito), AC1-4pheles spp. (mosquitoes), C1-4lex spp. (mosquitoes), Lucillia spp. (blowflies), Blatiella germanica (cockroach), Periplaneia americana (cockroach), Blatta orientalis (cockroach), termites of the Mastotermitidae (for example Mastotermes spp.), the Kalotermitidae (for example Neotermes spp.), the

RhiC1-4termitidae (for example Coptotermes formosanus, RetiC1-4litermes flavipes, R. speratu, R. virginicas, R. hesperus, and R. santonensis) and the Termitidae (for example GloB1termes sulphnreus), SoleC1-4psis geminata (fire ant), MoC1-4mohum pharaonis (pharaoh's ant), Damalinia spp. and Liriognalhus spp. (B1ting and sucking lice), Meloidogyne spp. (root kC1-4t nematodes), Globodera spp. and Heterodera spp. (cyst nematodes), Pratylenchus spp. (lesion nematodes), Rhodopholus spp. (banana burrowing nematodes), Tylenchulus spp.(citrus nematodes), Haemonchus conforms (barber pole worm), CaeC1-4rhabditis elegans(vinigar eelworm), Trichostrongylus spp. (gastro intestinal nematodes) and Deroceras retiC1-4latum (slug).
The invention therefore provides a method of combating and controlling insects, acarines, nematodes or molluscs which comprises applying an insecticidally, acaricidally, nematicidally or molluscicidally effective amount of a compound of formula (I), or a composition contA1ning a compound of formula (I), to a pest, a loC1-4s of pest, or to a plant susceptible to attack by a pest, The compounds of formula (I) are preferably used agA1nst insects, acarines or nematodes.
The term "plant" as used herein includes seedlings, bushes and trees.
In order to apply a compound of formula (I) as an insecticide, acaricide, nematicide or molluscicide to a pest, a loC1-4s of pest, or io a piani susceptiB1e to attack by a pest, a compound of formula (I) is usually formulated into a composition which includes, in addition to the compound of formula (I), a suitable inert diluent or carrier and, optionally, a surface active agent (SFA). SFAs are chemicals which are able to modify the properties of an interface (for example, liquid/solid, liquid/A1r or liquid/liquid interfaces) by lowering the interfacial tension and thereby leading to changes in other properties (for example dispersion, emulsification and wetting). It is preferred that A1l compositions (both solid and liquid formulations) comprise, by weight, 0.0001 to 95%, more preferably 1 to 85%, for example 5 to 60%, of a compound of formula (I). The composition is generally used for the control of pests such that a compound of formula (I) is applied at a rate of from 0,1 g to 10kg per hectare, preferably from lg to 6kg per hectare, more preferably from 1 g to 1kg per hectare.
When used in a seed dressing, a compound of formula (I) is used at a rate of O.OOOIg to 1 Og (for example 0.001 g or 0.05g), preferably 0.005g to 1 Og, more preferably 0.005g to 4g. per kilogram of seed.

In aC1-4ther aspect the present invention provides an insecticidal, acaricidal, nematicidal or molluscicidal composition comprising an insecticidally, acaricidally, nematicidally or molluscicidally effective amount of a compound of formula (I) and a suitable carrier or diluent therefor. The composition is preferably an insecticidal, acaricidal, nematicidal or molluscicidal composition.
In a still further aspect the invention provides a method of combating and controlling pests at a loC1-4s which comprises treating the pests or the loC1-4s of the pests with an insecticidally, acaricidally, nematicidally or molluscicidally effective amount of a composition comprising a compound of formula (I). The compounds of formula (I) are preferably used agA1nst insects, acarines or nematodes.
The compositions can be chosen from a number of formulation types, including dustable powders (DP), soluble powders (SP), water soluble granules (SG), water dispersible granules (WG), wettable powders (WP), granules (GR) (slow or fast release), soluble concentrates (SL), oil miscible liquids (OL), ultra low volume liquids (UL), emulsifiable concentrates (EC), dispersible concentrates (DC), emulsions (both oil in water (EW) and water in oil (EO)), micro-emulsions (ME), suspension concentrates (SC), aerosols, fogging/smoke formulations, capsule suspensions (CS) and seed treatment formulations. The formulation type chosen in any instance will depend upon the partiC1-4lar purpose envisaged and the physical, chemical and B1ological properties of the compound of formula (I).
Dustable powders (DP) may be prepared by mixing a compound of formula (I) with one or more solid diluents (for example natural clays, kaolin, pyrophyllite, bentonite, alumina, montmorillonite, kieselguhr, chalk, diatomaceous earths, calcium phosphates, calcium and magnesium carbonates, sulphur, lime, flours, talc and other organic and iC1-4rganic solid carriers) and mechanically grinding the mixture to a fine powder.
Soluble powders (SP) may be prepared by mixing a compound of formula (I) with one or more water-soluble iC1-4rganic salts (such as sodium B1carbonate, sodium carbonate or magnesium sulphate) or one or more water-soluble organic solids (such as a polysaccharide) and, optionally, one or more wetting agents, one or more dispersing agents or a mixture of sA1d agents to improve water dispersiB1lity/soluB1lity. The mixture is then ground to a fine powder. Similar compositions may also be granulated to form water soluble granules (SG).
Wettable powders (WP) may be prepared by mixing a compound of formula (I) with one or more solid diluents or carriers, one or more wetting agents and, preferably, one or

more dispersing agents and, optionally, one or more suspending agents to facilitate the dispersion in liquids. The mixture is then ground to a fine powder. Similar compositions may also be granulated to form water dispersible granules (WG).
Granules (GR) may be formed either by granulating a mixture of a compound of formula (I) and one or more powdered solid diluents or carriers, or from pre-formed blank granules by absorB1ng a compound of formula (I) (or a solution thereof, in a suitable agent) in a porous granular material (such as pumice, attapulgite clays, fuller's earth, kieselguhr, diatomaceous earths or ground corn cobs) or by adsorB1ng a compound of formula (I) (or a solution thereof, in a suitable agent) on to a hard core material (such as sands, silicates, mineral carbonates, sulphates or phosphates) and drying if necessary. Agents which are commonly used to A1d absorption or adsorption include solvents (such as aliphatic and aromatic petroleum solvents, alcohols, ethers, ketones and esters) and sticking agents (such as polyvinyl acetates, polyvinyl alcohols, dextrins, sugars and vegetable oils). One or more other additives may also be included in granules (for example an emulsifying agent, wetting agent or dispersing agent).
Dispersible Concentrates (DC) may be prepared by dissolving a compound of formula (I) in water or an organic solvent, such as a ketone, alcohol or glycol ether. These solutions may contA1n a surface active agent (for example to improve water dilution or prevent crystallisation in a spray tank).
Emulsifiable concentrates (EC) or oil-in-water emulsions (EW) may be prepared by dissolving a compound of formula (I) in an organic solvent (optionally contA1ning one or more wetting agents, one or more emulsifying agents or a mixture of sA1d agents).. Suitable organic solvents for use in ECs include aromatic hydrocarbons (such as alkylbenzenes or alkylnaphthalenes, exemplified by SOLVESSO 100, SOLVESSO 150 and SOLVESSO 200; SOLVESSO is a Registered Trade Mark), ketones (such as cyclohexaC1-4ne or methylcyclohexaC1-4ne) and alcohols (such as benzyl alcohol, furfuryl alcohol or butaC1-4l), N-alkylpyrrolidones (such as N-methylpyrrolidone or N-octylpyrrolidone), dimethyl amides of fatty acids (such as C8-C10 fatty acid diethylamide) and chlorinated hydrocarbons. An EC product may spontaneously emulsify on addition to water, to produce an emulsion with sufficient staB1lity to allow spray application through appropriate equipment. Preparation of an EW involves obtA1ning a compound of formula (I) either as a liquid (if it is C1-4t a liquid at room temperature, it may be melted at a reasonable temperature, typically below 70°C) or hi

solution (by dissolving it in an appropriate solvent) and then emulsifiying the resultant liquid or solution into water contA1ning one or more SFAs, under high shear, to produce an emulsion. Suitable solvents for use in EWs include vegetable oils, chlorinated hydrocarbons (such as chlorobenzenes), aromatic solvents (such as alkylbenzenes or alkylnaphtfialenes) and other appropriate organic solvents which have a low soluB1lity in water.
Microemulsions (ME) may be prepared by mixing water with a blend of one or more solvents with one or more SFAs, to produce spontaneously a thermodynamically stable isotropic liquid formulation. A compound of formula (I) is present initially in either the water or the solvent/SFA blend. Suitable solvents for use in MEs include those hereinbefore described for use in in ECs or in EWs. An ME may be either an oil-in-water or a water-in-oil system (which system is present may be determined by conductivity measurements) and may be suitable for mixing water-soluble and oil-soluble pesticides in the same formulation. An ME is suitable for dilution into water, either remA1ning as a microemulsion or forming a conventional oil-in-water emulsion.
Suspension concentrates (SC) may comprise aqueous or C1-4n-aqueous suspensions of finely divided insoluble solid particles of a compound of formula (I). SCs may be prepared by ball or bead milling the solid compound of formula (I) in a suitable medium, optionally with one or more dispersing agents, to produce a fine particle suspension of the compound. One or more wetting agents may be included in the composition and a suspending agent may be included to reduce the rate at which the particles settle. Alternatively, a compound of formula (I) may be dry milled and added to water, contA1ning agents hereinbefore described, to produce the desired end product.
Aerosol formulations comprise a compound of formula (I) and a suitable propellant (for example n-butane). A compound of formula (I) may also be dissolved or dispersed in a suitable medium (for example water or a water miscible liquid, such as n-propaC1-4l) to provide compositions for use in C1-4n-pressurised, hand-actuated spray pumps.
A compound of formula (I) may be mixed in the dry state with a pyrotechnic mixture to form a composition suitable for generating, in an enclosed space, a smoke contA1ning the compound.
Capsule suspensions (CS) may be prepared in a manner similar to the preparation of EW formulations but with an additional polymerisation stage such that an aqueous dispersion of oil droplets is obtA1ned, in which each oil droplet is encapsulated by a polymeric shell and

contA1ns a compound of formula (I) and, optionally, a carrier or diluent therefor. The polymeric shell may be produced by either an interfacial polycondensation reaction or by a coacervation procedure. The compositions may provide for controlled release of the compound of formula (I) and they may be used for seed treatment. A compound of formula (I) may also be formulated in a B1odegradable polymeric matrix to provide a slow, controlled release of the compound.
A composition may include one or more additives to improve the B1ological performance of the composition (for example by improving wetting, retention or distribution on surfaces; resistance to rA1n on treated surfaces; or uptake or moB1lity of a compound of formula (I)). Such additives include surface active agents, spray additives based on oils, for example certA1n mineral oils or natural plant oils (such as soy bean and rape seed oil), and blends of these with other B1o-enhancing adjuvants (ingredients which may A1d or modify the action of a compound of formula (I)).
A compound of formula (I) may also be formulated for use as a seed treatment, for example as a powder composition, including a powder for dry seed treatment (DS), a water soluble powder (SS) or a water dispersible powder for slurry treatment (WS), or as a liquid composition, including a flowable concentrate (FS), a solution (LS) or a capsule suspension (CS). The preparations of DS, SS? WS. FS and LS compositions are very similar to those of, respectively, DP, SP, WP, SC and DC compositions described above. Compositions for treating seed may include an agent for assisting the adhesion of the composition to the seed (for example a mineral oil or a film-forming barrier).
Wetting agents, dispersing agents and emulsifying agents may be surface SFAs of the cationic, anionic, amphoteric or C1-4n-ionic type.
Suitable SFAs of the cationic type include quaternary ammonium compounds (for example cetyltrimethyl ammonium bromide), imidazolines and amine salts.
Suitable anionic SFAs include alkali metals salts of fatty acids, salts of aliphatic moC1-4esters of sulphuric acid (for example sodium lauryl sulphate), salts of sulphonated aromatic compounds (for example sodium dodecylbenzenesulphonate, calcium dodecylbenzenesulphonate, butylnaphthalene sulphonate and mixtures of sodium di-isopropyl- and tri-isopropyl-naphthalene sulphonates), ether sulphates, alcohol ether sulphates (for example sodium laureth-3-sulphate), ether carboxylates (for example sodium laureth-3-carboxylate), phosphate esters (products from the reaction between one or more

fatty alcohols and phosphoric acid (predominately moC1-4-esters) or phosphorus pentoxide (predominately di-esters), for example the reaction between lauryl alcohol and tetraphosphoric acid; additionally these products may be ethoxylated), sulphosuccinamates, paraffin or olefme sulphonates, taurates and ligC1-4sulphonates.
Suitable SFAs of the amphoteric type include betA1nes, propionates and glycinates.
Suitable SFAs of the C1-4n-ionic type include condensation products of alkylene oxides, such as ethylene oxide, propylene oxide, butylene oxide or mixtures thereof, with fatty alcohols (such as oleyl alcohol or cetyl alcohol) or with alkylpheC1-4ls (such as octylpheC1-4l, C1-4nylpheC1-4l or octylcresol); partial esters derived from long chA1n fatty acids or hexitol anhydrides; condensation products of sA1d partial esters with ethylene oxide; block polymers (comprising ethylene oxide and propylene oxide); alkaC1-4lamides; simple esters (for example fatty acid polyethylene glycol esters); amine oxides (for example lauryl dimethyl amine oxide); and lecithins.
Suitable suspending agents include hydrophilic colloids (such as polysaccharides, polyvinylpyrrolidone or sodium carboxymethylcellulose) and swelling clays (such as bentonite or attapulgite).
A compound of formula (I) may be applied by any of the kC1-4wn means of applying pesticidal compounds. For example, it may be applied, formulated or unformulated, to the pests or to a loC1-4s of the pests (such as a haB1tat of the pests, or a growing plant liable to infestation by the pests) or to any part of the plant, including the foliage, stems, branches or roots, to the seed before it is planted or to other media in which plants are growing or are to be planted (such as soil surrounding the roots, the soil generally, paddy water or hydroponic C1-4lture systems), directly or it may be sprayed on, dusted on, applied by dipping, applied as a cream or paste formulation, applied as a vapour or applied through distribution or incorporation of a composition (such as a granular composition or a composition packed in a water-soluble bag) in soil or an aqueous environment.
A compound of formula (I) may also be injected into plants or sprayed onto
vegetation using electrodynamic spraying techniques or other low volume methods, or
applied by land or aerial irrigation systems.
Compositions for use as aqueous preparations (aqueous solutions or dispersions) are
generally supplied in the form of a concentrate contA1ning a high proportion of the active ingredient, the concentrate being added to water before use. These concentrates, which may

include DCs, SCs, ECs, EWs, MEs SGs, SPs, WPs, WGs and CSs, are often required to withstand storage for prolonged periods and, after such storage, to be capable of addition to water to form aqueous preparations which remA1n homogeneous for a sufficient time to enable them to be applied by conventional spray equipment. Such aqueous preparations may contA1n varying amounts of a compound of formula (I) (for example 0.0001 to 10%, by weight) depending upon the purpose for which they are to be used.
A compound of formula (I) may be used in mixtures with fertilisers (for example nitrogen-, potassium- or phosphorus-contA1ning fertilisers). Suitable formulation types include granules of fertiliser. The mixtures suitably contA1n up to 25% by weight of the compound of formula (I).
The invention therefore also provides a fertiliser composition comprising a fertiliser and a compound of formula (I).
The compositions of this invention may contA1n other compounds having B1ological activity, for example micronutrients or compounds having fungicidal activity or which possess plant growth regulating, herB1cidal, insecticidal, nematicidal or acaricidal activity.
The compound of formula (I) may be the sole active ingredient of the composition or it may be admixed with one or more additional active ingredients such as a pesticide, fungicide, synergist, herB1cide or plant growth regulator where appropriate. An additional active ingredient may: provide a composition having a broader spectrum of activity or increased persistence at a loC1-4s; synergise the activity or complement the activity (for example by increasing the speed of effect or overcoming repellency) of the compound of formula (I); or help to overcome or prevent the development of resistance to individual components. The partiC1-4lar additional active ingredient will depend upon the intended utility of the composition. Examples of suitable pesticides include the following:
a) Pyrethroids, such as permethrin, cypermethrin, fenvalerate, esfenvalerate, deltamethrin, cyhalothrin (in partiC1-4lar lambda-cyhalothrin), B1fenthrin, fenpropathrin, cyfluthrin, tefluthrin, fish safe pyrethroids (for example ethofenprox), natural pyrethrin, tetramethrin, s-B1oallethrin, fenfluthrin, prallethrin or 5-benzyl-3-furylmethyl-(E)-(lR,3S)-2,2-dimethyl-3-(2-oxothiolan-3-ylidenemethyl)cyclopropanecarboxyIate;
b) OrgaC1-4phosphates, such as, profeC1-4fos, sulprofos, acephate, methyl parathton, azinphos-methyl, demeton-s-methyl, hepteC1-4phos, thiometon, fenamiphos, moC1-4crotophos, profeC1-4fos, triazophos, methamidophos, dimethoate, phosphamidon, malathion, chlorpyrifos,

phosalone, terbufos, fensulfothion, foC1-4fos, phorate, phoxim, pirimiphos-methyl, pirimiphos-ethyl, fenitrothion, fosthiazate or diaziC1-4n;
c) Carbamates (including aryl carbamates), such as pirimicarb, triazamate, cloelhocarb, carbofuran, furathiocarb, ethiofencarb, aldicarb, thiofiirox, carbosulfan, bendiocarb, feC1-4bucarb, propoxur, methomyl or oxamyl;
d) Benzoyl ureas, such as diflubenzuron, triflumuron, hexaflumuron, flufeC1-4xuron or chlorfluazuron;
e) Organic tin compounds, such as cyhexatin, fenbutatin oxide or azocyclotin;
f) Pyrazoles, such as tebufenpyrad and fenpyroximate;
g) Macrolides, such as avermectins or milbemycins, for example abamectin, emamectin benzoate, ivermectin, milbemycin, spiC1-4sad or azadirachtin;
h) Hormones or pheromones;
i) OrgaC1-4chlorine compounds such as endosulfan, benzene hexachloride, DDT, chlordane or
dieldrin;
j) Amidines, such as chlordimeform or amitraz;
k) Fumigant agents, such as chloropicrin, dichloropropane, methyl bromide or metam;
1) Chloronicotinyl compounds such as imidacloprid, thiacloprid, acetamiprid, nitenpyram or
thiamethoxam;
m) Diacylhydrazines, such as tebufeC1-4zide, chromafeC1-4zide or methoxyfeC1-4zide;
n) Diphenyl ethers, such as diofeC1-4lan or pyriproxifen;
o) Indoxacarb;
p) Chlorfenapyr; or
q) Pymetrozine.
In addition to the major chemical classes of pesticide listed above, other pesticides having partiC1-4lar targets may be employed in the composition, if appropriate for the intended utility of the composition. For instance, selective insecticides for partiC1-4lar crops, for example stemborer specific insecticides (such as cartap) or hopper specific insecticides (such as buprofezin) for use in rice may be employed. Alternatively insecticides or acaricides specific for partiC1-4lar insect species/stages may also be included in the compositions (for example acaricidal ovo-larvicides, such as clofentezine, flubenzimine, hexythiazox or tetradifon; acaricidal motilicides, such as dicofol or propargite; acaricides, such as

bromopropylate or chlorobenzilate; or growth regulators, such as hydramethylC1-4n, cyromazine, methoprene, chiorfluazuron or diflubenzuron).
Examples of fungicidal compounds which may be included in the composition of the invention are (£}-//-methyI-2-[2-(2,5-dimethylpheC1-4xymethyl)phenyI]-2-methoxy-imiC1-4acetamide (SSF-129), 4-bromo-2-cyaC1-4-N,N-dimethyl-6-trifluoromethyIbenzimidazole* 1 -sulphonamide, a-[N-(3-chloro-2,6-xylyl)-2-methoxyacetamido]-y-butyrolactone, 4-chloro-2-cyaC1-4-JV^-dimethyl-5-p-tolyhmidazole-l -sulfonamide (DCF-916, cyamidazosulfamid), 3-5-dichloro-Af-(3-chloro-l -ethyl-1 -roethyI~2-oxopropyl)-4-methylbenzamide (RH-7281, zoxamide), N-ally]-4,5,-dimethyl-2-trimethylsilylthiophene-3-carboxamide (MON65500), N-(l-cyaC1-4-l,2-dimethylpropyI)-2-(2,4-dichloropheC1-4xy)propionamide(AC382042)> N-(2-methoxy-5-pyridyl)-cyclopropane carboxamide, acibenzolar (CGA245704), alanycarb, aldimorph, anilazine, azaconazole, azoxystroB1n, benalaxyl, beC1-4myl, B1loxazol, B1tertaC1-4l, blasticidin S, bromuconazole, bupirimate, captafol, captan, carbendazim, carbendazim chlorhydrate, carboxin, carpropamid, carvone, CGA41396, CGA41397, chiC1-4methionate, chlorothalonil, chlorozolinate, clozylacon, copper contA1ning compounds such as copper oxychloride, copper oxyquiC1-4late, copper sulphate, copper tallate and Bordeaux mixture, cymoxanil, cyproconazole, cyprodinil, debacarb, di-2-pyridyl disulphide l,l'-dioxide, dichlofluanid, diclomezine, diclcrar., diethcfencarb, difeC1-4conazole, difenzoquA1, diflumetorirn, O,O-di-iso-propyl-S-benzyl thiophosphate, dimefluazole, dimetconazole, dimethomorph, dimethirimol, diniconazole, diC1-4cap, dithiaC1-4n, dodecyl dimethyl ammonium chloride, dodemorph, dodine, doguadine, edifenphos, epoxiconazole, ethirimol, ethyl(Z)-N-benzyl-N([methyl(methyl-thioethylideneamiC1-4oxycarbonyl)amiC1-4]thio)-p -alaninate, etridiazole, famoxadone, fenamidone (RPA407213), fenarimol, fenbuconazole, fenfuram, fenhexamid (KBR2738), fenpiclonil, fenpropidin, fenpropimorph, fentin acetate, fentin hydroxide, ferbam, ferimzone, fluazinam, fludioxonil, flumetover, fluoroimide, fluquinconazole, flusilazole, flutolanil, flutriafol, folpet, fuberidazole, fiiralaxyl, fiirametpyr, guazatine, hexaconazole, hydroxyisoxazole, hymexazole, imazalil, imibenconazole, imiC1-4ctadine, imiC1-4ctadine triacetate, ipconazole, iprobenfos, iprodione, iprovalicarb (SZX0722), isopropanyl butyl carbamate, isoprothiolane, kasugamycin, kresoxim-methyl, LY186054, LY211795, LY248908, mancozeb, maneb, mefeC1-4xam, mepanipyrim, mepronil, metalaxyl, metconazole, metiram, metiram-zinc, metomiC1-4stroB1n, myclobutanil, neoasozin, nickel dimethyldithiocarbamate, nitrothal-isopropyl, nuarimol, ofurace, orgaC1-4merC1-4ry

compounds, oxadixyl, oxasulfuron, oxolinic acid, oxpoconazole, oxycarboxin, pefurazoate, penconazole, pencyC1-4ron, phenazin oxide, phosetyl-Al, phosphorus acids, phthalide, picoxystroB1n (ZA1963), polyoxin D, polyram, probenazole, prochloraz, procymidone, propamocarb, propiconazole, propineb, propionic acid, pyrazophds, pyriferiox, pyrimethanil, pyroquilon, pyroxyfur, pyrrolnitrin, quaternary ammonium compounds, quiC1-4methionate, quiC1-4xyfen, quintozene, sipconazole (F-155), sodium pentachlorophenate, spiroxamine, streptomycin, sulphur, tebuconazole, tecloftalam, tecnazene, tetraconazole, thiabendazole, thifluzamid, 2-(thiocyaC1-4methylthio)benzothiazole, thiophanate-methyl, thiram, timibenconazole, tolclofos-methyl, tolylfluanid, triadimefon, triadimeC1-4l, triazbutil, triazoxide, tricyclazole, tridemorph, trifloxystroB1n (CGA279202), triforine, triflumizole, triticonazole, validamycin A, vapam, vinclozolin, zineb and ziram.
The compounds of formula (I) may be mixed with soil, peat or other rooting media for the protection of plants agA1nst seed-borne, soil-borne or foliar fungal diseases.
Examples of suitable synergists for use in the compositions include piperonyl butoxide, sesamex, safroxan and dodecyl imidazole.
Suitable herB1cides and plant-growth regulators for inclusion in the compositions will depend upon the intended target and the effect required.
An example of a rice selective herB1cide which may be included is propanil. An
example of a plant growth regulator for use in cotton is PIX™.
Some mixtures may comprise active ingredients which have significantly different
physical, chemical or B1ological properties such that they do C1-4t easily lend themselves to the same conventional formulation type. In these cirC1-4mstances other formulation types may be prepared. For example, where one active ingredient is a water insoluble solid and the other a water insoluble liquid, it may nevertheless be possible to disperse each active ingredient in the same continuous aqueous phase by dispersing the solid active ingredient as a suspension (using a preparation analogous to that of an SC) but dispersing the liquid active ingredient as an emulsion (using a preparation analogous to that of an EW). The resultant composition is a suspoemulsion (SE) formulation.

The invention is illustrated by the following Examples:
EXAMPLE 1 This Example illustrates the preparation of compound 111,49; 5-chloro-l-(2-
chloropyridin-4-yl)carbonyl-1'-(trans-3-(4-chlorophenyl)allyl)-3'-methyl-spiro(indoline-3,4'-piperidine]
Step A: Potassium t-butoxide (1.56 g) was added portionwise to a stirred suspension of methoxymethyltriphenylphosphonium chloride (4.76 g) in tetrahydrofuran (30 ml) at 0°C under argon. The resulting orange mixture was stirred at 0°C for 30 min., then l-(4-chlorocinnamyl)-3-methyl-piperidin-4-one (1.83 g, prepared by alkylation of 3-methyl-piperidin-4-one [CAS C1-4 5773-58-0] with 4-chloro-cinnamyl chloride) dissolved in a minimum volume of tetrahydrofuran was added dropwise and the resulting solution was stirred at room temperature for I hour, poured into water and extracted twice with ether. The comB1ned organic layers were dried over sodium sulphate and concentrated in vaC1-4o. The residue was purified by silica gel chromatography (cyclohexaneiethyl acetate 75:25) to afford l-(4-chlorocinnamyl)-4-[l-methoxy-methylidene]-3-methyl-piperidine as a mixture of diastereoisomers. MS (ES+) 292/294 (M+H+).
Step B: A mixture of l-(4-chlorocinnamyl)-4-[l-methoxy-methylidene]-3-methyl-piperidine (1.25 g) and 4-chlorophenylhydrazine hydrochloride (0.85 g) in chloroform (43 ml) was treated with trifluoroacetic acid (4.3 m!) and heated at reflux under argon for 12 hours. The reaction mixture was cooled to room temperature, triethylsilane (3.1 ml) was

added and the solution refluxed for 2 hours. The reaction mixture was cooled to room temperature, diluted with dichloromethane, neutralised with aqueous ammonium hydroxide, washed with brine, dried (sodium sulphate) and concentrated. The dark residue was purified by silica gel chromatography (cyclohexane;ethyl acetate 1:1+ 0.5% triethylamine) to afford 5-chloro-1'-[trans-3-(4--chlorophenyl)allyl)-3'-methyl-spiroJindoline-3,4'-piperidine] (1.63 g). 'H NMR (600 MHz, CDC13) 0.69 (d, J = 9 Hz, 3H), 1.89 (m, 2H), 2.0 (m, 3H), 2.86 (dd, 1H), 2.95 (m, 1H), 3.17 (d, J = 7.2 Hz, 2H), 3.31 (d, J = 12 Hz, 1H), 3.58 (d, J = 12 Hz, 1H), 3.65 (m, 1H), 6.30 (dt, J = 7.2, 18.0 Hz, 1H), 6.49 (dt J = 8.0 Hz, 1H), 6.50 (d, J = 7.0 Hz, 1H), 2H), 6.94 (d, J = 0.9 Hz, 1H), 6.97 (dd, J = 7.0,0.9 Hz, 1H), 7.25-7.33 (m, 4H); MS (ES+) 387/389 (M+H+).
Step C: To a solution of 5-chloro-l '-[trans-3-(4-chlorophenyl)allyl]-3,-methyl-spiro[indoline-3,4'-piperidine] obtA1ned in Step B (210 mg) and triethylamine (0.23 ml) in dichloromethane (10 ml) at 0°C was added 2-chloro-isonicotiC1-4yl chloride (176 mg) and the resulting solution was kept at 0°C for 30 min., diluted with dichloromethane, washed with diluted aqueous sodium B1carbonate, dried (sodium sulphate) and concentrated. Silica gel chromatography of the residue (cyclohexane:ethyl acetate 1:1) afforded the title compound as a slight yellow solid (200 mg); M.p. 91-93°C; MS (ES+) 526/528 (M+H+)
EXAMPLE 2 This Example illustrates the preparation of 5-chloro-l-(2-chloropyridin-4-yOcarbonyl-spirofindoline-3,4'-(1',2',3',4'-tetrahydropyridine)]-!' carboxylic acid tert-butyl ester


Step A: Triphenylphosphine (5.16 g) was dissolved in tetrahydrofuran (130 ml) and the solution was cooled to 0°C under argon. Diisopropylazodicarboxylate (3.82 ml) was added dropwise over 10 min and the resulting mixture was stirred at 0°C for 20 min (formation of a white precipitate). N-(4-Chloro-2-iodo-phenyl)-2,2,2-trifluoro-acetamide (5.5 g) was added as a solid, followed by 4-hydroxymethyl-3,6-dihydro-2H-pyridine-l-carboxylic acid tert-butyl ester (J. Org. Chem. 2001, 66, 5545-5551, 3.4 g) dissolved in a minimum volume of tetrahydrofuran. The reaction mixture was allowed to warm to room temperature and stirred for 12 hours. The solution was then concentrated in vaC1-4o and the residue suB1ected to silica gel chromatography (cyclohexane:ethyl acetate 9:1) to afford 4-{[(4-chloro-2-iodo-phenyl)-(2,2,2-trifluoro-acetyl)-amiC1-4]-methyl}-3,6-dihydro-2H-pyridine-l-carboxylic acid tert-butyl ester (4.7 g), !H NMR (600 MHz, CDC13) 1.5 (s, 9H), 2.20 (m, 2H), 3.49 (m, 1H), 3.50 (d, J = 17 Hz, 1H), 3.55 (m, 1H), 3.8-3.9 (m, 2H), 5.02 (d, J = 17 Hz, 1H), 5,40 (s, 1H), 7.0 (m, 1H), 738 (dd, 1H), 7.92 (d, 1H); MS (ES+) 445/447 (M+H+-C02-isobutene), 486/488 (M+H+-isobutene).
Step B: In a dried, argon purged flask, 4-{[(4-chloro-2-iodo-phenylH2,2,2-trifluoro-acetyl)-amiC1-4]-methyl}-3,6-dihydro-2H-pyridine-l-carboxylic acid tert-butyl ester obtA1ned in Step A (3.55 g) was dissolved in dimethylformamide (55 ml); triethylamine (2.3 ml), tetrabutylammonium bromide (2.5 g) and palladium(II) acetate (0.22 g) were successively added and the solution was heated at 80°C for 3 hours. After cooling to room temperature, the reaction mixture was diluted with ethyl acetate, washed with brine, dried over sodium sulphate and concentrated in vaC1-4o. The crude residue was dissolved in methaC1-4l (140 ml)

and water (30 mi), placed under argon and potassium carbonate (6.8 g) was added. The reaction mixture was stirred for 1 hour at room temperature, the mixture was filtered and the filtrate concentrated in vaC1-4o. The residue was diluted with ethyl acetate, washed with brine, dried (sodium sulphate) and concentrated in vaC1-4o. Silica gel chromatography of the residue (cyclohexane:ethyl acetate 8:2) afforded S-chloro-spirofindoline-3,4'-(1',2',3',4'-tetrahydropyridine)]-r carboxylic acid tert-butyl ester (1.3 g) as a a pale yellow powder. M.p. 50-51°C; ]H NMR (600 MHz, CDC12CDC12, 80°C) 1.54 (s, 9H), 1.83 (m, 1H), 1.99 (m, 1H), 3.36 (d, J = 11.4 Hz, 1H), 3.50 (d, J = 11.4 Hz, 1H), 3.51 (m, 1H), 3.75 (brs, 1H, NH), 3.78 (m, 1H), 4.81 (d, J = 8.6 Hz, 1H), 6.57 (d, J = 10.2 Hz, 1H), 6.98 (d, J = 2.4 Hz,lH), 7.02 (m, 1H), 7.03 (dd, J = 10.2, 2.4 Hz, 1H); nC NMR (125 MHz, CDC12CDC12, SOX) selected data 28.2, 33.2, 39.1, 60.6, 108.5, 110.2, 123.5, 126.4, 127.5; MS (ES+) 221/223 (M+H+-C02-isobutene), 265/267 (M+H+-isobutene); 321/323 (M+H+).
StepC: 5-Chloro-spirofindoline-3,4'-(1',2',3',4'--tetrahydropyridine)]-1' carboxylic acid tert-butyl ester (274 mg) was acylated in dichloromethane (10 ml) with 2-chloroisonicotiC1-4yl chloride (250 mg) in the presence of triethylamine (0.48 ml) using the method described in Example 1 Step C to give the title compound (360 mg). MS (ES+) 360/362 (M+H+-C02-isobutene), 404/406 (M+H+-isobutene).
EXAMPLE 3 This Example illustrates the preparation of compound CHI.49, 5-chloro-l-(2-chloropyridin-4-yl)carbonyl-1'-[trans-3-(4-chlorophenyl)allyl)-3'-hydroxy-spiro(indoline-3,4'-piperidine]


Borane-methylsulfide complex (1M in dichioromethane, 1.05 ml) was added dropwise under argon to a solution of 5-chloro-l-(2-chloropyridin-4-yl)carbonyl-spiro[indoline-3,4'-(l',2',3,,4,-tetrahydropyridine)]-1' carboxylic acid tert-butyl ester (Example 2, 350 mg) in tetrahydrofuran (15 ml) at room temperature and the resulting solution was stirred at room temperature for 18 hours. 3N NaOH (0.9 ml) was added, followed by 30% aqueous hydrogen peroxide (0.9 ml) and the resulting mixture was stirred at room temperature for 1 hour, poured into water, extracted twice with ethyl acetate, dried (sodium sulphate) and concentrated in vaC1-4o. The major product was isolated by silica gel chromatography (cyclohexane:ethyl acetate 7:3) to give 125 mg of a solid. The latter was dissolved in dichioromethane (10 ml) and treated with trifluoroacetic acid (1 ml) at room temperature for 2 hours. The solution was partitioned between water and dichioromethane, the organic layer was neutralised with saturated aqueous sodium B1carbonate, dried (sodium sulphate) and concentrated in vaC1-4o. The residue was dissolved in acetonitrile (5 ml) and treated with diisopropylethylamine (0.065 ml) and 4-chlorocinnamyl bromide (58 mg) for 12 hours at room temperature under argon. Standard aqueous work-up afforded a residue which was purified by flash chromatography (silica gel, ethyl acetate:methaC1-4l 98:2) to give the title product (51 mg) as a colorless solid. M.p. 110°C; MS (ES+) 528/530/532/533 (M+H+).

EXAMPLE 4 This Example illustrates the preparation of compound CCIII.49, 5-chloro-l-(2-chloropyridin-4-yl)carbonyl-1'-(trans-3-(4-chlorophenyl)allyl)-3'-fluoro-spiro(indoline-3,4'-piperidine]
[l-(Chloromethyl)-4-fluoro-l,4-diazoniaB1cyclo[2.2.2]octaneB1s(tetrafluoroborate)] (Selectfluor™, 266 mg) was added to a solution of 5-chloro-l-(2-chloropyridin-4-yOcarbonyl-spirofindoline-3,4'-(1',2',3',4'-tetrahydropyridine)]-1' carboxylic acid tert-butyl ester (Example 2, 345 mg) in dimethylformamide (20 ml) at room temperature and the resulting solution was stirred at 70°C for 1 hour, cooled to room temperature, poured into water (50 ml) and extracted twice with ethyl acetate; the comB1ned organic layers were washed with brine, dried (sodium sulphate), concentrated in vaC1-4o and the residue purified by silica gel chromatography (cyclohexane:ethyl acetate 8.2) to afford 5-chloro-l-(2-chloropyridin-4-yl)carbonyl-3'-fluoro-2'-hydroxy-spiro[indoline-3,4,-piperidine] 1' carboxylic acid tert-butyl ester (200 mg) as a colorless solid; MS (ES+) 496/498 (M+H+). This product was dissolved in dichloromethane (10 ml) and treated successively with triethylsilane (0.3 ml) and trifluoroacetic acid (0.57 ml); the solution was stirred under argon for 12 hrs, diluted with dichloromethane, neutralised with aqueous sodium B1carbonate, dried (sodium sulphate) and concentrated in vaC1-4o. The residue was dissolved in acetonitrile (10 ml) and treated with diisopropylethylamine (0.1 ml) and 4-chlorocinnamyl chloride (71 mg) for 12 hours at reflux under argon. Standard aqueous work-up afforded a residue which was

purified by flash chromatography (silica gel, cyclohexane:ethyl acetate 7:3) to give the title product (111 mg) as a colorless solid. M.p. 96-97°C; MS (ES+) 530/532/534 (M+H+).
EXAMPLE 5 This Example illustrates the preparation of compound CCCIII.49, 5-chloro-l-(2-chloropyrridin-4-yl)carbonyl-r-[trans-3-(4-chlorophenyl)allyl]-3,,3,--difluoro-spiro[indoline-3,4'-piperidine]
{1 -(Chloromethyl)-4-fluoro-1,4-diazoniaB1cyclo[2.2.2]octane B1s(tetrafluoroborate)] (Selectfluor™, 1.05 g) was added to a solution of 5-chloro-l-(2-chloropyridin-4-yl)carbonyl-spiro[indoline-3,4,-(1',2',3,,4'-tetrahydropyridine)]-r carboxylic acid tert-butyl ester (Example 2, 345 mg) in dimethylformamide (15 ml) at room temperature and the resulting solution was stirred at 80°C for 2 hours, cooled to room temperature, poured into water and extracted twice with ethyl acetate; the comB1ned organic layers were washed with brine, dried (sodium sulphate), concentrated in vaC1-4o and the residue purified by silica gel chromatography (cyclohexane:ethyl acetate 65.35) to afford 5-chloro-l-(2-chloropyridin-4-yOcarbonyl-3',3'-difluoro-2'-hydroxy-spirotindoline-3,4'-piperidine] V carboxylic acid tert-butyl ester (217 mg) as a colorless solid; MS (ES+) 514/516 (M+H+). This product was dissolved in dichloromethane (14 ml) and treated successively with triethylsilane (0.34 ml) and trifluoroacetic acid (0.64 ml); the solution was stirred under argon for 12 hrs, diluted with dichloromethane, neutralised with aqueous sodium B1carbonate, dried (sodium sulphate)

and concentrated in vaC1-4o. The residue was dissolved in acetonitrile (10 m!) and treated with diisopropylethylamine (0.1 ml) and 4-chlorocinnamyl chloride (71 mg) for 10 hours at reflux under argon. Standard aqueous work-up afforded a residue which was purified by flash chromatography (silica gel, cyclohexane:ethyl acetate 7:3) to give the title product 1.4 (118 mg) as a colorless solid. M.p. 100-101°C; 1H NMR (600 MHz, CDCI2CDCI2, 80°C) 1.86 (m, 1H), 2.20 (m, IH), 2.41 (m, IH), 2.45 (m, 1H), 3.02 (d, J = 12 Hz, IH), 3.24 (m, 3H), 3.85 (d, J = 12 Hz, IH), 4.24 (m, IH), 6.24 (dd, J = 12 Hz, 7.2 Hz, IH), 6.6 (d, J - 12 Hz,lH), 7.27-7.47 (m, 9H), 8.57 (d, J = 6 Hz, IH); I3C NMR (125 MHz, CDCI2CDCI2, 80°C) selected data 34.5,48.4, 55.5, 56.8, 59.3, 119.4, 120.3, 121.5, 125.9, 126.1, 127.5, 128.6, 128.9, 129.9, 132.2, 150.6; MS (ES+) 548 (M+H+).
EXAMPLE 6 This Example illustrates the pesticidal/insecticidal properties of compounds of formula (I). . Test agA1nst were performed as follows: Spodoptera littoralis (Egyptian cotton leafwomi)
Cotton leaf discs were placed on agar in a 24-well microtiter plate and sprayed with test solutions at an application rate of 200 ppm. After drying, the leaf discs were infested with 5 Lj larvae. The samples were checked for mortality, repellent effect, feeding behaviour, and growth regulation 3 days after treatment (DAT). The following compounds gave at least 80% control of Spodoptera littoralis:
cIII-49.
Heliothis virescens (Tobacco budworm):
Eggs (0-24 h old) were placed in 24-well microtiter plate on artificial diet and treated with
test solutions at an application rate of 200 ppm by pipetting. After an inC1-4bation period of 4
days, samples were checked for egg mortality, larval mortality, and growth regulation. The
following compounds gave at least 80% control of Heliothis virescen:
HI-49, CIII-49, CCin-49, CCCIII-49.
Plutella xylostella (Diamond back moth):

24-well microtiter plate (MTP) with artificial diet was treated with test solutions at an application rate of 18.2 ppm by pipetting. After drying, the MTP's were infested with larvae (L2)(10-15 per well). After an inC1-4bation period of 5 days, samples were checked for larval mortality, antifeedant and growth regulation. The following compounds gave at least 80% control of Pluiella xylostella: Cni-49, CC1-4-49, CCCIII-49.
Aedes aegypti (Yellow fever mosquito):
10-15 Aedes larvae (L2) together with a nutrition mixture are placed in 96-well microtiter
plates. Test solutions at an application rate of 2ppm are pipetted into the wells. 2 days later,
insects were checked for mortality and growth inhiB1tion. The following compounds gave at
least 80% control of Aedes aegypti
111-49, CIII-49, CCI1I-49.

CLAIMS 1. A compound of formula I

wherein Y is a single bond, C=0, C=S or S(0)m where m is 0, 1 or 2; R1 is hydrogen, optionally substituted alkyl, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbonyl, aminocarbonyl, optionally substituted alkylaminocarbonyl, optionally substituted dialkylaminocarbonyl, optionally substituted aryl, optionally substituted heteroaryl, optionally substituted alkoxy, optionally substituted aryloxy, optionally substituted heteroaryloxy, optionally substituted heterocyclyloxy, cyano, optionally substituted alkenyl, optionally substituted alkynyl, optionally substituted cycloalkyl, optionally substituted cycloalkenyl, formyl, optionally substituted heterocyclyl, optionally substituted alkylthio, NO or NR13R14 where R!3 and Ru are independently hydrogen, COR15, optionally substituted alkyl, optionally substituted aryl, optionally substituted heteroaryl, optionally substituted heterocyclyl or R!3 and Ru together with the N atom to which they are attached form a group -N=C(R16)-NR17R18; Ri5 is H, optionally substituted alkyl, optionally substituted alkoxy, optionally substituted aryl, optionally substituted aryloxy optionally substituted heteroaryl, optionally substituted heteroaryloxy or NR19R20; R16, R17 and R!8 are each independently H or lower alkyl; R19 and R20 are independently optionally substituted alkyl, optionally substituted aryl or optionally substituted heteroaryl; R2 and R3 are independently hydrogen, halogen, cyano, optionally substituted alkyl, optionally substituted alkoxy or optionally substituted aryl;
each R4 is independently halogen, nitro, cyano, optionally substiiuted C1-8 alkyl, optionally substituted C1-6 alkenyl, optionally substituted C2-6 alkynyl, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbonyl, optionally substituted alkylaminocarbonyl, optionally substituted dialkylaminocarbonyl, optionally substituted C3.7 cycloalkyl, optionally substituted aryl, optionally substituted heteroaryl, optionally substituted heterocyclyl, optionally substituted alkoxy, optionally substituted aryloxy, optionally substituted heteroaryloxy, optionally substituted alkylthio or R2IR22N where R21 and R22 are, independently, hydrogen, C1-8 alkyl, C3-7 cycloalkyl, C3-6 alkenyl, C3-6 alkynyl, C3-7 cycloalkyl(Ci-4)alkyl, C2-6 haloalkyl, Cj.6 alkoxy(C1-6)alkyl, C1-6 alkoxycarbonyl or R21 and R22 together with the N atom to which they are attached form a five, six or seven-membered heterocyclic ring which may contain one or two further heteroatoms selected from 0, N or S and which may be optionally substituted by one or two Chalky! groups, or 2 adjacent groups R4 together with the carbon atoms to which they are attached form a 4, 5, 6,or 7 membered carbocyclic or heterocyclic ring which may be optionally substituted by halogen; n is 0,1, 2, 3 or 4; R8 is optionally substituted alkyl, optionally substituted alkenyl, optionally substituted
alkanyl,optionally substituted cycloalkyl,optionally substituted aryl,optionally
substituted alkoxy, optionally substituted aryloxy, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbonyl or optionally substituted alkenylcarbonyl;A1, A2, A3, A4, B1, B2, B3 and B4 are independently hydrogen, halogen, hydroxy, cyano, optionally substituted C1-8 alkyl, optionally substituted C2-6 alkenyl, optionally substituted C2-6 alkynyl, optionally substituted alkoxycarbonyl, optionally substituted alkylcarbonyl, optionally substituted alkylaminocarbonyl, optionally substituted dialkylaminocarbonyl, optionally substituted C3.7 cycloalkyl, optionally substituted aryl, optionally substituted heteroaryl, optionally substituted heterocyclyl, optionally substituted alkoxy, optionally substituted aryloxy, optionally substituted heteroaryloxy, optionally substituted alkylthio, optionally substituted arylthio or R23R24N where R23 and R24 are, independently, hydrogen, C1-8 alkyl, C3.7 cycloalkyl, C3-6 alkenyl, C3-6 alkynyl, C3.7 cycIoalkyl(C1-4)alkyI, C2-6 haloalkyl, C1-6 aDcoxy(C1. 6)alkyl, C1-6 alkoxycarbonyl or R23 and R24 together with the N atom to which they are

attached form a five, six or seven-membered heterocyclic ring which may contA1n one
or two further heteroatoms selected from O, N or S and which may be optionally
substituted by one or two C1-6 alkyl groups,
or A1 and A2 together are =0,
or A3 and A4 together are =0,
or B1 and B2 together are =0,
or B3 and B4 together are =0,
or A1 together with B\ is a bond,
or A3 together with B3 is a bond,
or A1 together with A2 form with the carbon to which they are bound a three- to
seven-membered ring, and may be saturated or unsaturated, and that may contA1n one
or two hetero atoms selected from the group consisting of N, O and S, and which may
be optionally substituted by one or two C1-6 alkyl groups;
or A1 together with B1 form with the carbon to which they are bound a three- to
seven-membered ring, and may be saturated or unsaturated, and that may contA1n one
or two hetero atoms selected from the group consisting of N, O and S, and which may
be optionally substituted by one or two C1-6 alkyl groups;
or B1 together with B2 form with the carbon to which they are bound a three- to
seven-membered ring, and may be saturated or unsaturated, and that may contA1n one
or two hetero atoms selected from the group consisting of N, O and S, and which may
be optionally substituted by one or two C1-6 alkyl groups;
or A1 together with A3 form a group -CH2-, -CH=CH- or -CH2CH2;
or B1 together with B3 form a group -CH2-, -CH=CH- or -CH2CH2;
or salts or N-oxides thereof provided that when B1, B2, B3 and B4 are all H, either
both A1 and A2 are different from H or both A3 and A4 are different from H.
2. A compound according to clA1m 1 wherein Y is a single bond or C=0.
3. A compound according to clA1m 1 or clA1m 2 wherein R2 and R3 are each independently hydrogen, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy or cyano.4. A compound according to any preceeding clA1m wherein R1 is hydrogen, C1-6 alky], C1-6 cyanoalkyl, C1-6 haloalkyl, C3.7 cycloalkyI(C1-4)alkyl, C1-6 a1koxy(C1-6)alkyl, heteroaryl(C1-6)alkyl (wherein the heteroaryl group may be optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy, C1-6 haloalkoxy, C1-6 alkylsulfonyl, C1-6 alkylsulfmyl, C1-6 alkylthio, C1-6 alkoxycarbonyl, C1-6 alkylcarbonylamino, arylcarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5,6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), aryl(C1-6)alkyl (wherein the aryl group maybe optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy, d-6 haloalkoxy, C1-6 alkylsulfonyl, C1-6 alkylsulfinyl, C1-6 alkylthio, C1-6 alkoxycarbonyl, C1-6 alkylcarbonylamino, arylcarbonyl, or two adjacent positions on the aryl system may be cyclised to form a 5,6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), C1-6 alkylcarbonylamino(C1-6)alkyl, aryl (which may be optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy, C1-6 haloalkoxy, C1-6 alkylsulfonyl, C1-6 alkylsulfmyl, C1-6 alkylthio, C1-6 alkoxycarbonyl, C1-6 alkylcarbonylamino, arylcarbonyl, or two adjacent positions on the aryl system may be cyclised to form a 5. 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), heteroaryl (which may be optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy, C1-6 haloalkoxy, C1-6 alkylsulfonyl, C1-6 alkylsulfmyl, C1-6 alkylthio, C1-6 alkoxycarbonyl, C1-6 alkylcarbonylamino, arylcarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), C1-6 alkoxy, C1-6 haloalkoxy, phenoxy (wherein the phenyl group is optionally substituted by halogen, C1-6 alkyl, C1-6 alkoxy, C1-6 haloalkyl, C1-6 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino), heteroaryloxy (optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy or C1-6 haloalkoxy), heterocyclyloxy (optionally substituted by halo, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy or C1-6 haloalkoxy), cyano, C2-6 alkenyl, C2-6 alkynyl, C1-6 cycloalkyl, C5.7 cycloalkenyl, heterocyclyl (optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy or C1-6 haloalkoxy), C1-6 alkylthio, C1-6haloalkylthio or NRI3R14 where R13 and R14 are independently hydrogen, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy(C1-6)alkyl, phenyl (which may be optionally substituted by halogen, C1-6 alkyl. C1-6 alkoxy, C1-6 haloalkyl, C1-6 haloalkoxy, CN, NO2, aryl, heteroaryl, amino, dialkylamino or C 1-4 alkoxycarbonyl), phenyl (C1-6)alkyl (wherein the phenyl group may be optionally substituted by halogen, C1-6 alkyl, C1-6 alkoxy, C1-6 haloalkyl, C1-6 haloalkoxy, CN, NO2, aryl, heteroaryl, amino, dialkylamino, C1-6 alkylsulfonyl, C1-6 alkoxycarbonyl, or two adjacent positions on the phenyl ring may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen), heteroaryl (C1-6)alkyl (wherein the heteroaryl group may be optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy, C1-6 haloalkoxy, C1-6 alkylsulfonyl, C1-6 alkylsulfinyl, C1-6 alkylthio, C1-6 alkoxycarbonyl, C1-6 alkylcarbonylamino, arylcarbonyl, or two adjacent positions on the heteroaryl system may be cyclised to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring, itself optionally substituted with halogen) or heteroaryl (which may be optionally substituted by halo, nitro, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy or C1-6 haloalkoxy, C1-6 alkoxycarbonyl C1-6 alkylcarbonylamino, phenyloxycarbonylamifto (wherein the phenyl group is optionally substituted by halogen, C1-6 alkyl, C1-6 alkoxy, C1-6 haloalkyl, C1-6 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino), amino, C1-6 A1kylamino or phenylamino (wherein the phenyl group is optionally substituted halogen, C1-6 alkyl, C1-6 alkoxy, C1-6 haloalkyl, C1-6 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino)).A compound according to any preceeding clA1m wherein each R4 is independently halogen, cyano, C1-6 alkyl, C1-6 haloalkyl, C1-6 cyanoalkyl, C1-6 alkoxy(C1-6)alkyl, C3.7 cycloalkyl(Ci.6)alkyl, C5.6 cycloalkenyl(C1-6)alkyl, C3-6 alkenyloxy(C1-6)alkyl, C3.6 a!kynyloxy(C|-6)alkyl, aryloxy(C1-6)alkyl, C1-6 carboxyalkyl, C1-6 alkylcarbonyKQ. 6)alkyl, C2-6 alkenylcarbonyl(Ci.6)alkyl, C2-6 alkynylcarbonyl(Cu)-alkyl, C1-6 alkoxycarbonyl(C1-6)alkyl, C3-6 a!kenyloxycarbonyl(C1-6)alkyl, C3-6 alkynyloxycarbonyl(C|-6)alkyl, aryloxycarbonyl(Ci-e)alkyl, C1-6 alkylthio(C1-6)alkyl, C1-6 alkylsulfinyl(C1-6)alkyl, C1-6 alkylsulfonyl(C1-6)alkyl, aminocarbonyl(C1-6)alkyl, C1-6alkylaminocarbonyl(C1-6)alkyl, di(C1-6)alkylaminocarbonyl(C1-6)alkyl, phenyl(C1-4)alkyl (wherein the phenyl group is optionally substituted by halogen, C1-6
alky], C1-4 alkoxy, C1.4 haloalkyl, C1-4 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino), heteroaryl(C1-4)alkyl (wherein the heteroaryl group is optionally substituted by halo, nitro, cyano, C1-4 alkyl, C1-4 haloalkyl, C1-4 alkoxy or C1-4 haloalkoxy), heterocyclyl(C1-4)alkyl (wherein the heterocyclyl group is optionally substituted by halo, nitro, cyano,C1-6 alkyl, C1-6 haloalkyl, C1-6 alkoxy orC1-6 haloalkoxy), C2-6 alkenyl, aminocarbonyl(C2-6)A1kenyl, C1-6alkylaminocarbonyKCi. 6)alkenyl, di(C1-6)alkylaminocarbonyl(C2-6)alkenyl, phenyl(C2-4)-alkenyl, (wherein the phenyl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino), C2-6 alkynyl, trimethylsilyl(C2-6)alkynyl, aminocarbonyl(C2.6)alkynyl, C1-4 alkylaminocarbonyl(C2-6)alkynyI, di(C1-4)alkylaminocarbonyl(C2-6)a!kynyl, C1-4 alkoxycarbonyl, C3-7 cycloalkyl, C3.7 halocycloalkyl, C3.7 cyanocycloalkyl, C1-4 alkyl(C3.7)-cycloalkyl, C1-3 alkyl(C3_7)halocycloalkyl,phenyl (optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino), heteroaryl (optionally substituted by halo, nitro, cyano, C1-4 alkyl, C1-4 haloalkyl, C1-4 alkoxy or C1-4 haloalkoxy), heterocyclyl (wherein the heterocyclyl group is optionally substituted by halo, nitro, cyano, C1-4 alkyl, C1-4 haloalkyl, C1-4 alkoxy or C1-4 haloalkoxy), or 2 adjacent groups R4 together with the carbon atoms to which they are attached form a 4, 5,6 or 7 membered carbocylic or heterocyclic ring which may be optionally substituted by halogen, C1-4 alkoxy,C1-6 haloalkoxy, phenoxy (optionally substituted by halo, nitro, cyano, C1-4 alkyl, C1-4 haloalkyl, C1-4 alkoxy or C1-6 haloalkoxy), heteroaryloxy (optionally substituted by halo, nitro, cyano, C1-4 alkyl, C1-4 haloalkyl,C1-6 alkoxy or C1-4 haloalkoxy), C1-4 alkylthio or RI9R20N where R19 and R20 are, independently, hydrogen, C1-4 alkyl, C3-7 cycloalkyl, C3-6 alkenyl, C3-6 alkynyl, C2-6 haloalkyl, C1-4 alkoxycarbonyl or R19 and R20 together with the N atom to which they are attached form a five, six or seven-membered heterocyclic ring which may contA1n one or two further heteroatoms selected from O, N or S and which may be optionally substituted by one or two C1-4 alkyl groups; and n is 0, 1, 2 or 3.
A compound according to any preceeding clA1m wherein R is C1-4O alkyl, C1-4O haloalkyl, aryl(C1-6)alkyl (wherein the aryl group is optionally substituted by halogen,
C1-4 alkyl, C1.4 alkoxy, C1-4 haloalkyl, C1.4 haloalkoxy, CN, N02, aryl, heteroaryl, amino or dialkylamino), heteroaryl(C1-6)alkyl (wherein the heteroaryl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl. C1-4 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino), arylcarbonyl-(Ci-6)alkyl (wherein the aryl group may be optionally substituted by halogen, C1-4 alkyl. C1-4 alkoxy, C1-4 haloalkyl. C1-4 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino and the alkyl group may be optionally substituted by aryl), C2-8 alkenyl, C2-8 haloalkenyl, aryl(C2-6)-alkenyl (wherein the aryl group is optionally substituted halogen, C1-4 alkyl, C1-4.alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, N02, aryl, heteroaryl, amino or dialkylamino, C1-6 alkoxycarbonyl, or two adjacent substituents can cyclise lo form a 5,6 or 7 membered carbocyclic or heterocyclic ring), heteroaryl(C2-6)-alkenyl (wherein the heteroaryl group is optionally substituted halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino, C1-4 alkoxycarbonyl, or two adjacent substituents can cyclise to form a 5, 6 or 7 membered carbocyclic or heterocyclic ring), C2-6 alkynyl, phenyl(C2-6)alkynyl (wherein the phenyl group is optionally substituted by halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, NO:, aryl, heteroaryl, amino or dialkylamino), C3.7 cycloalkyl, Cut, alkoxycarbonyl, C1-6 alkylcarbonyl, C1-6 haloalkylcarbonyl or aryl(C2-6)alkenylcarbonyl (wherein the aryl group may be optionally substituted halogen, C1-4 alkyl, C1-4 alkoxy, C1-4 haloalkyl, C1-4 haloalkoxy, CN, NO2, aryl, heteroaryl, amino or dialkylamino), or -C(R51)(R52)-[CR53=CR 54]z-R55 where z is 1 or 2, R51 and R52 are each independently H, halo or C1-2 alkyl, R53 and R54 are each independently H, halogen, C1.4 alkyl or C1-4 haloalkyl and R55 is optionally substituted aryl or optionally substituted heteroaryl.
7. A compound according to any preceeding clA1m wherein A1, A2, A3, A4, B1 B2, B3 and B4 are independently each hydrogen, halo, cyano, C1-3 alkyl, hydroxy or two groups attached to the same carbon atom together with the carbon atom form a carbonyl group.
8. A compound of formula (II)

wherein Y, n, R1, R2, R\ R4, A1, A2, A3, A4, B1, B2, B3 and B4 are as defined in clA1m 1 and R8 is hydrogen or tert:butoxycarbonyl.
An Insecticidal acaricidal and nematicidal composition comprising an insecticidally, acaricidally or nematicidally effective amount of a compound of formula I as defined in clA1m 1.
A a method of combating and controlling insects, acarines, nematodes or molluscs which comprises applying to a pest, to a locus of a pest, or to a plant susceptible to attack by a pest an insecticidally, acaricidally, nematicidally or molluscicidally effective amount of a compound of formula I.
Dated this 12 day of June 2006


Documents:

2089-CHENP-2006 AMENDED PAGES OF SPECIFICATION 27-07-2011.pdf

2089-CHENP-2006 AMENDED CLAIMS 27-07-2011.pdf

2089-chenp-2006 form-3 27-07-2011.pdf

2089-CHENP-2006 OTHER PATENT DOCUMENT 27-07-2011.pdf

2089-CHENP-2006 POWER OF ATTORNEY 27-07-2011.pdf

2089-CHENP-2006 AMENDED CLAIMS 03-10-2011.pdf

2089-CHENP-2006 CORRESPONDENCE OTHERS 01-12-2010.pdf

2089-CHENP-2006 CORRESPONDENCE OTHERS 03-10-2011.pdf

2089-CHENP-2006 EXAMINATION REPORT REPLY RECEIVED 27-07-2011.pdf

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2089-chenp-2006-description(complete).pdf

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2089-chenp-2006-pct.pdf


Patent Number 252964
Indian Patent Application Number 2089/CHENP/2006
PG Journal Number 24/2012
Publication Date 15-Jun-2012
Grant Date 12-Jun-2012
Date of Filing 12-Jun-2006
Name of Patentee SYNGENTA PARTICIPATIONS AG
Applicant Address Schwarzwaldallee 215, CH-4058 Basel
Inventors:
# Inventor's Name Inventor's Address
1 CASSAYRE, Jerome Syngenta Crop Protection AG, Werk Rosental, Schwarzwaldallee 215, CH-4058 Basel
2 MOLLEYRES, Louis-Pierre Syngenta Crop Protection AG, Werk Rosental, Schwarzwaldallee 215, CH-4058 Basel
3 MAIENFISCH, Peter Syngenta Crop Protection AG, Werk Rosental, Schwarzwaldallee 215, CH-4058 Basel
4 CEDERBAUM, Fredrik Syngenta Crop Protection AG, Werk Rosental, Schwarzwaldallee 215, CH-4058 Basel
PCT International Classification Number C07D471/10,A61K31/438,A01N43/40
PCT International Application Number PCT/IB2004/004114
PCT International Filing date 2004-12-09
PCT Conventions:
# PCT Application Number Date of Convention Priority Country
1 0328908.9 2003-12-12 U.K.