Title of Invention	A PROCESS AND A REACTOR FOR THE PREPARATION OF A HYDROGEN AND CARBON MONOXIDE CONTAINING SYNTHESIS GAS
Abstract	The present invention relates to a process for the preparation of a hydrogen and carbon monoxide containing synthesis gas by catalytic partial oxidation of a hydrocarbon feed gas with a stoichiometric amount of oxygen, the process comprising a plUrality of sequential, separated steps, whereby in each step only a fraction of the stoichiometric amount of oxygen is added to the hydrocarbon feed gas forming a reaction mixture and the reaction mixture is then passed through a catalytic zone, so that substantially complete conversion of the added amount of oxygen by reaction with a portion of the reaction mixture is obtained in each step. The present invention also relates to a reactor for the preparation of hydrogen and carbon monoxide containing synthesis gas.

Title of Invention

A PROCESS AND A REACTOR FOR THE PREPARATION OF A HYDROGEN AND CARBON MONOXIDE CONTAINING SYNTHESIS GAS

Abstract

The present invention relates to a process for the preparation of a hydrogen and carbon monoxide containing synthesis gas by catalytic partial oxidation of a hydrocarbon feed gas with a stoichiometric amount of oxygen, the process comprising a plUrality of sequential, separated steps, whereby in each step only a fraction of the stoichiometric amount of oxygen is added to the hydrocarbon feed gas forming a reaction mixture and the reaction mixture is then passed through a catalytic zone, so that substantially complete conversion of the added amount of oxygen by reaction with a portion of the reaction mixture is obtained in each step. The present invention also relates to a reactor for the preparation of hydrogen and carbon monoxide containing synthesis gas.

Full Text	BACKGROUND OF THE INVENTION It is known to prepare synthesis gas compositions consisting of hydrogen and carbon monoxide and containing very low content of methane and carbon dioxide by passing over a catalyst of hydrocarbon substrate, usually natural gas or methane mixed with oxygen at preheated temperature in the range of, e.g. 300-400°C. The processes are typically performed in the presence! of a noble metal catalyst, such as rhodium, platinum, palladium, or iridium, or other metals like nickel, cobalt and iruthenium, arranged in a fixed bed reactor. The residence time of the gas in a catalytic bed thereby is very short. Catalytic material can furthermore be in form of a sponge, metal, a metal web or supported on ceramic porous bodies, for example. By the above process, it possible to obtain a sub-■'■ '. 'I. sstantial and complete conversion of hydrocarbon with high selectivity for carbon monoxide and hydrogen. In order to obtain high selectivity, the residence time is usually very low and the gas maintained at elevated temperature for the shortest time possible. Alternatively, selectivity is achieved by keeping the process temperature as low as possible. The main problem with the known process is to avoid ignition of the gas/oxygen mixture prior to contact with the catalyst. In particular, this is problematic when the process is carried out at elevated pressure. SUMMARY OP THE INVENTION This invention provides an improved process for catalytic partial oxidation of a hydrocarbon substrate of the above type. The improvement comprises carrying out the process in a number of separated steps, whereby in each step solely a small fraction of the stoichiometric amount of oxygen is added to the reaction. The gas is passed through a catalytic zone arranged in each step, so that complete conversion of oxygen is obtained in each step. The reaction is performed at substantially the same temperature in all steps by cooling the reaction mixture in each step with a suitable cooling medium during the total process cycle. BRIEF DESCRIPTION OF THE DRAWING The sole figure is a schematic cross-section of a reaction apparatus according to a preferred embodiment of the present invention. DESCRIPTION OF THE PREFERRED EMBODIMENT Referring to the sole figure, a reaction apparatus according to a specific embodiment of the invention is shown schematically in a representative cross-section. The process is performed on a hydrocarbon gas substrate 2 fed to a tubular reactor surrounded by a cooling medium, such as pressurized boiling water 4, contained between reactor wall 6 and jacket 8 provided in the form of concentric tubes. The reactor is further provided with static mixing zones 10 in the reaction volume. Toward the beginning of each mixing zone, oxygen 12 is provided through perforated rings 14. Catalyst bodies 16 are arranged at predetermined distances from the oxygen supply rings. Product 18 is generated after gas 2 has passed through a predetermined number of catalyst reaction zones. When carrying out the process of this invention as described above, excessive concentrations of oxygen will not be available in the reactor. As a result, a very high temperature in the reactor is prevented, all the catalyst material will be at a controlled temperature, and the selectivity of the process thereby is improved. The invention further is useful in partial oxidation of higher hydrocarbons and in oxidative coupling reactions. Although the present invention has been described in relation to particular embodiments thereof, many other variations and modifications and other uses will become apparent to those skilled in the art. It is preferred, therefore, that the present invention be limited not by the specific disclosure herein, but only by the appended claims. WE CLAIM 1. A process for the preparation of a hydrogen/carbon monoxide containing synthesis gas by catalytic partial oxidation of a hydrocarbon feed gas with a stoichiometric amount of oxygen, the process comprising a plurality of sequential, separated steps, whereby in each step only a small fraction of the stoichiometric amount of oxygen is added to the hydrocarbon feed gas and the feed gas is then passed through a catalytic zone, so that substantially complete conversion of the added amount of oxygen by reaction with a portion of the feed gas is obtained in each step. 2. The process of claim 1, wherein the oxidation reaction is performed at substantially the same temperature in each of the steps by cooling the reaction mixture in each step with a suitable cooling medium. 3. The process of claim 1, wherein each step includes mixing the added amount of oxygen with the feed gas prior to passage through each catalytic zone. 4. The reactor for use in the preparation of a hydro gen/carbon monoxide containing synthesis gas by catalytic partial oxidation of a hydrocarbon feed gas, the prepara tion being carried out in a number of sequential, separated steps, whereby in each step only a small fraction of the stoichiometric amount of oxygen is added to the feed gas and the feed gas is then passed through a catalytic zone, so that substantially complete conversion of the added amount of oxygen is obtained in each step, the apparatus comprising a reactor fed by a hydrocarbon gas, the reactor including a plurality of reaction zones through which the hydrocarbon gas passes sequentially, each reaction zone having an oxygen supply and a catalyst, each reaction zone being provided with a cooling medium. 5. The reactor of claim 4, wherein the cooling medium surrounds the reaction zones. 6. The reactor of claim 4, wherein the cooling medium is pressurized boiling water. 7. The reactor of claim 4, wherein the reaction zones are provided with static mixing zones between the oxygen supply and the catalyst body, each catalyst body being arranged at a predetermined distance from the oxygen sup-ply. 4. A process for the preparation of a hydrogen/carbon monoxide, substantially as herein described with reference to the accompanying drawings.

Full Text

BACKGROUND OF THE INVENTION
It is known to prepare synthesis gas compositions consisting of hydrogen and carbon monoxide and containing very low content of methane and carbon dioxide by passing over a catalyst of hydrocarbon substrate, usually natural gas or methane mixed with oxygen at preheated temperature in the range of, e.g. 300-400°C.
The processes are typically performed in the presence! of a noble metal catalyst, such as rhodium, platinum, palladium, or iridium, or other metals like nickel, cobalt and iruthenium, arranged in a fixed bed reactor. The residence time of the gas in a catalytic bed thereby is very short. Catalytic material can furthermore be in form of a sponge, metal, a metal web or supported on ceramic porous bodies, for example.
By the above process, it possible to obtain a sub-■'■ '. 'I. sstantial and complete conversion of hydrocarbon with high
selectivity for carbon monoxide and hydrogen. In order to obtain high selectivity, the residence time is usually very low and the gas maintained at elevated temperature for the shortest time possible.
Alternatively, selectivity is achieved by keeping the process temperature as low as possible. The main problem with the known process is to avoid ignition of the gas/oxygen mixture prior to contact with the catalyst. In particular, this is problematic when the process is carried out at elevated pressure.
SUMMARY OP THE INVENTION
This invention provides an improved process for catalytic partial oxidation of a hydrocarbon substrate of the above type. The improvement comprises carrying out the process in a number of separated steps, whereby in each step solely a small fraction of the stoichiometric amount

of oxygen is added to the reaction. The gas is passed through a catalytic zone arranged in each step, so that complete conversion of oxygen is obtained in each step. The reaction is performed at substantially the same temperature in all steps by cooling the reaction mixture in each step with a suitable cooling medium during the total process cycle.
BRIEF DESCRIPTION OF THE DRAWING
The sole figure is a schematic cross-section of a reaction apparatus according to a preferred embodiment of the present invention.
DESCRIPTION OF THE PREFERRED EMBODIMENT
Referring to the sole figure, a reaction apparatus according to a specific embodiment of the invention is shown schematically in a representative cross-section. The process is performed on a hydrocarbon gas substrate 2 fed to a tubular reactor surrounded by a cooling medium, such as pressurized boiling water 4, contained between reactor wall 6 and jacket 8 provided in the form of concentric tubes.
The reactor is further provided with static mixing zones 10 in the reaction volume. Toward the beginning of each mixing zone, oxygen 12 is provided through perforated rings 14. Catalyst bodies 16 are arranged at predetermined distances from the oxygen supply rings. Product 18 is generated after gas 2 has passed through a predetermined number of catalyst reaction zones.
When carrying out the process of this invention as described above, excessive concentrations of oxygen will not be available in the reactor. As a result, a very high temperature in the reactor is prevented, all the catalyst material will be at a controlled temperature, and the selectivity of the process thereby is improved.

The invention further is useful in partial oxidation of higher hydrocarbons and in oxidative coupling reactions.
Although the present invention has been described in relation to particular embodiments thereof, many other variations and modifications and other uses will become apparent to those skilled in the art. It is preferred, therefore, that the present invention be limited not by the specific disclosure herein, but only by the appended claims.

WE CLAIM
1. A process for the preparation of a hydrogen/carbon
monoxide containing synthesis gas by catalytic partial
oxidation of a hydrocarbon feed gas with a stoichiometric amount of oxygen, the process comprising a plurality of
sequential, separated steps, whereby in each step only a
small fraction of the stoichiometric amount of oxygen is added to the hydrocarbon feed gas and the feed gas is then passed through a catalytic zone, so that substantially complete conversion of the added amount of oxygen by reaction with a portion of the feed gas is obtained in each step.
2. The process of claim 1, wherein the oxidation reaction is performed at substantially the same temperature in each of the steps by cooling the reaction mixture in each step with a suitable cooling medium.
3. The process of claim 1, wherein each step includes mixing the added amount of oxygen with the feed gas prior to passage through each catalytic zone.

4. The reactor for use in the preparation of a hydro
gen/carbon monoxide containing synthesis gas by catalytic
partial oxidation of a hydrocarbon feed gas, the prepara
tion being carried out in a number of sequential, separated
steps, whereby in each step only a small fraction of the
stoichiometric amount of oxygen is added to the feed gas
and the feed gas is then passed through a catalytic zone,
so that substantially complete conversion of the added
amount of oxygen is obtained in each step, the apparatus
comprising a reactor fed by a hydrocarbon gas, the reactor
including a plurality of reaction zones through which the
hydrocarbon gas passes sequentially, each reaction zone having an oxygen supply and a catalyst, each reaction zone being provided with a cooling medium.
5. The reactor of claim 4, wherein the cooling medium
surrounds the reaction zones.
6. The reactor of claim 4, wherein the cooling medium
is pressurized boiling water.
7. The reactor of claim 4, wherein the reaction zones are provided with static mixing zones between the oxygen supply and the catalyst body, each catalyst body being arranged at a predetermined distance from the oxygen sup-ply.

4. A process for the preparation of a hydrogen/carbon monoxide, substantially as herein described with reference to the accompanying drawings.

Documents:

2571-mas-1997-abstract.pdf

2571-mas-1997-claims duplicate.pdf

2571-mas-1997-claims original.pdf

2571-mas-1997-correspondence others.pdf

2571-mas-1997-correspondence po.pdf

2571-mas-1997-description complete duplicate.pdf

2571-mas-1997-description complete original.pdf

2571-mas-1997-drawings.pdf

2571-mas-1997-form 1.pdf

2571-mas-1997-form 26.pdf

2571-mas-1997-form 3.pdf

2571-mas-1997-form 4.pdf

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Patent Number

208023

Indian Patent Application Number

2571/MAS/1997

PG Journal Number

27/2007

Publication Date

06-Jul-2007

Grant Date

06-Jul-2007

Date of Filing

12-Nov-1997

Name of Patentee

HALDOR TOPSOE A/S

Applicant Address

NYMOLLEVEJ 55, DK-2800 LYNGBY.

Inventors:

#	Inventor's Name	Inventor's Address
1	IVAR IVARSEN PRIMDAHL	DALMOSEVEJ 6-8, DK-2400 COPENHAGEN NV.

PCT International Classification Number

C01B03/38

PCT International Application Number

N/A

PCT International Filing date

PCT Conventions:

#	PCT Application Number	Date of Convention	Priority Country
1	60/030,847	1996-11-15	U.S.A.