CA1257478A - Process and equipment for the generation of a product gas containing hydrogen and carbon oxides - Google Patents
Process and equipment for the generation of a product gas containing hydrogen and carbon oxidesInfo
- Publication number
- CA1257478A CA1257478A CA000442092A CA442092A CA1257478A CA 1257478 A CA1257478 A CA 1257478A CA 000442092 A CA000442092 A CA 000442092A CA 442092 A CA442092 A CA 442092A CA 1257478 A CA1257478 A CA 1257478A
- Authority
- CA
- Canada
- Prior art keywords
- gas
- reaction tubes
- reactor
- lower chamber
- product gas
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired
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Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
- B01J8/06—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes
- B01J8/062—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes being installed in a furnace
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
- C01B3/384—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts the catalyst being continuously externally heated
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/08—Methods of heating or cooling
- C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
- C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Engineering & Computer Science (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
- Carbon And Carbon Compounds (AREA)
- Catalysts (AREA)
- Hydrogen, Water And Hydrids (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
- Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
Abstract
ABSTRACT
In a process for generating a product gas containing hydrogen and carbon oxides from a feed gas the improvement which comprises catalytic endothermic reforming of a part of the feed gas, to which steam is admixed, in the catalyst filled reaction tubes to obtain reformed gas, and mixing the reformed gas with the remaining part of the feed gas to obtain, by partial combustion, the product gas and leading the product gas around the catalyst-filled reaction tubes. Apparatus for implementing such a process comprises reaction tubes for containing catalyst installed in a reactor which is divided by a partition wall into an upper chamber for receiving feed gas with which the steam is admixed and a lower chamber in which further reactions take place, the reaction tubes being fixed to the partition wall by a gas-tight seal and each having an open upper end communicating with the upper chamber for the intake of feed gas and an open lower end communicating with the lower chamber and which comprises one or more intake nozzles for providing process fluids on the reactor wall or reactor bottom or both, at least one jet tube or at least one permeable ceramic plate or both for fluid passage into the free space of the lower chamber and at least one jet tube for a start-up burner.
In a process for generating a product gas containing hydrogen and carbon oxides from a feed gas the improvement which comprises catalytic endothermic reforming of a part of the feed gas, to which steam is admixed, in the catalyst filled reaction tubes to obtain reformed gas, and mixing the reformed gas with the remaining part of the feed gas to obtain, by partial combustion, the product gas and leading the product gas around the catalyst-filled reaction tubes. Apparatus for implementing such a process comprises reaction tubes for containing catalyst installed in a reactor which is divided by a partition wall into an upper chamber for receiving feed gas with which the steam is admixed and a lower chamber in which further reactions take place, the reaction tubes being fixed to the partition wall by a gas-tight seal and each having an open upper end communicating with the upper chamber for the intake of feed gas and an open lower end communicating with the lower chamber and which comprises one or more intake nozzles for providing process fluids on the reactor wall or reactor bottom or both, at least one jet tube or at least one permeable ceramic plate or both for fluid passage into the free space of the lower chamber and at least one jet tube for a start-up burner.
Description
~s~
This lnvention relates to a process ancl apparatus for the generation of a product gas containing hydrogen and carbon oxides from a feedgas consisting substantially of hydrocarbons, particularly natural gas with which steam is admixed. The process involves catalytic endothermic reforming of the feedgas in catalyst-containing reaction tubes and a partial combustion of the reformed gas, to obtain a product gas, with oxygen or an oxygen-bearing gas, for example air. The product gas may be subjected to further processing to produce synthesis gas for the manufacture of for example, methanol or ammonia.
For the catalytic endothermic reforming of the feedgas it is necessary to produce the amount of heat required for ~he reaction and to transfer this heat through the reaction tubes to the feed gas passing through the tubes. For this purpose, it is known to arrange a multitude of the catalyst-containing reaction tubes in vertical rows in what is called a primary reformer and to heat them by a multitude of gas- or oil-firing burners mounted on the reformer walls. The combustion chamber of the reformer is operated at atmospheric pressure. The combustion gas leaves the combustion chamber at a temperature of approximately 950C and is heat-exchanged against process fluids and utilities before it passes into the stack at a temperature of 120 to 160C.
At the time of subsequent partial combustion, i.e. of further reduction of the CH4 content and admixture, if required, with nitrogen to obtain a synthesis gas for the manufacture of ammonia it is necessary to add oxygen or an oxygen-bearing gas, for example air, to the reformed gas. This is done in what is called a secondary reformer. l`he latter contains facilities for admission of the oxygen or air and a catalyst layer for further catalytic conversion of undesirable gaseous components contained in the - 1 - ."~.~
. ~
reformed gas.
For implementing the steam reforming process, the state of the art also includes processes and equipment which provide for indirect heating of the reaction tubes by means of combustion gas generated under pressure, the hot gas leaving the primary reformer being expanded in a gas turbine as outlined, for example in DAS 17 92 229 and DAS 20 55 439. The combustion gas is a flue gas which is discharged to the atmosphere after expansion and cooling and, consequently, contribu-tes to environ-mental pollution by emitting certain trace pollutants. Moreover,the recoverable heat content in the lower temperature range of the combustion gas or flue gas requires significant expenditure in terms of costly heat exchange surface for economical utiliz-ation.
An object of the invention is to simplify, and to reduce pollution by using processes and apparatus for the gener-ation of product gases containing hydrogen and carbon oxide.
The invention provides a process for the generation of a product gas containing hydrogen and carbon oxides Erom a feed gas consisting substantially of hydrocarbons comprising the steps of:
(a) catalytic endothermic reforming offeed gas in catalyst filled reaction tubes to obtain reformed gas;
(b) partial combustion of the reformed gas by means of the addition of an oxygen-bearing gas to the reformed gas to obtain a product gas; and
This lnvention relates to a process ancl apparatus for the generation of a product gas containing hydrogen and carbon oxides from a feedgas consisting substantially of hydrocarbons, particularly natural gas with which steam is admixed. The process involves catalytic endothermic reforming of the feedgas in catalyst-containing reaction tubes and a partial combustion of the reformed gas, to obtain a product gas, with oxygen or an oxygen-bearing gas, for example air. The product gas may be subjected to further processing to produce synthesis gas for the manufacture of for example, methanol or ammonia.
For the catalytic endothermic reforming of the feedgas it is necessary to produce the amount of heat required for ~he reaction and to transfer this heat through the reaction tubes to the feed gas passing through the tubes. For this purpose, it is known to arrange a multitude of the catalyst-containing reaction tubes in vertical rows in what is called a primary reformer and to heat them by a multitude of gas- or oil-firing burners mounted on the reformer walls. The combustion chamber of the reformer is operated at atmospheric pressure. The combustion gas leaves the combustion chamber at a temperature of approximately 950C and is heat-exchanged against process fluids and utilities before it passes into the stack at a temperature of 120 to 160C.
At the time of subsequent partial combustion, i.e. of further reduction of the CH4 content and admixture, if required, with nitrogen to obtain a synthesis gas for the manufacture of ammonia it is necessary to add oxygen or an oxygen-bearing gas, for example air, to the reformed gas. This is done in what is called a secondary reformer. l`he latter contains facilities for admission of the oxygen or air and a catalyst layer for further catalytic conversion of undesirable gaseous components contained in the - 1 - ."~.~
. ~
reformed gas.
For implementing the steam reforming process, the state of the art also includes processes and equipment which provide for indirect heating of the reaction tubes by means of combustion gas generated under pressure, the hot gas leaving the primary reformer being expanded in a gas turbine as outlined, for example in DAS 17 92 229 and DAS 20 55 439. The combustion gas is a flue gas which is discharged to the atmosphere after expansion and cooling and, consequently, contribu-tes to environ-mental pollution by emitting certain trace pollutants. Moreover,the recoverable heat content in the lower temperature range of the combustion gas or flue gas requires significant expenditure in terms of costly heat exchange surface for economical utiliz-ation.
An object of the invention is to simplify, and to reduce pollution by using processes and apparatus for the gener-ation of product gases containing hydrogen and carbon oxide.
The invention provides a process for the generation of a product gas containing hydrogen and carbon oxides Erom a feed gas consisting substantially of hydrocarbons comprising the steps of:
(a) catalytic endothermic reforming offeed gas in catalyst filled reaction tubes to obtain reformed gas;
(b) partial combustion of the reformed gas by means of the addition of an oxygen-bearing gas to the reformed gas to obtain a product gas; and
- 2 -~5~7~
(c) heating the reaction tubes by means of the product gas generated by the partial combustion;
the improvement which comprises catalytic endothermic reforming of a part of the feed gas, to which steam is admixed, in the catalyst filled reaction tubes to obtain reformed gas, and mixing the reformed gas with the remaining part of the feed gas and an oxygen-bearing gas to obtain, by partial combustion, the product gas and leading the product gas around the catalyst filled reaction tubes.
The feedgas for the process consists substantially of hydrocarbons, particularly natural gas with which steam is admixed. It may also contain hydrogen, or an oxide of carbon, or both.
The process may include the adding of a fuel gas to supplement the partial combustion of the reformed gas. The fuel gas may be hydrogen, hydrocarbons, or a mixture of hydrogen and hydrocarbons.
- 2a -~Z~ 78 The process mav also be carried out at elevated pressure, preferably at a pressure exceeding 3 bar.
The invention also provides an apparatus for implement-ing the above process which comprises reaction tubes for filling with catalyst installed in a reactor which is divided by a part~
ition wall into an upper chamber Eor receiving feedgas consisting substantially of hydrocarbons with which steam is admixed and a lower chamber in which further reactions can take place, the reaction tubes being fixed to the partition wall through a gas-tight seal and each having an open upper end communicating withthe upper chamber for the intake of the feedgas and an open lower end communicating with the lower chamber and comprises one or more intake nozzles for providing process fluid on thereactor wall or reactor bottom or both, at least one jet tube or at least one permeable ceramic plate or both for fluid passage into a free space of the lower chamber and at least one jet tube for a start-up burner.
Preferably, the apparatus comprises baffles for aiding heat transfer from a hot, combustion gas side of the lower chamber.
The baffles, in such case, are connected to the partition wall, one or more of the reaction tubes, or both.
The apparatus also preferably comprises the reaction tubes connected to the partition wall, such connection being detachable but gas tight.
The apparatus may also comprise at least one of the reaction tubes having a central tube of smaller diameter through which at least part of an oxidation agent can be supplied to the free space of the lower chamber.
(c) heating the reaction tubes by means of the product gas generated by the partial combustion;
the improvement which comprises catalytic endothermic reforming of a part of the feed gas, to which steam is admixed, in the catalyst filled reaction tubes to obtain reformed gas, and mixing the reformed gas with the remaining part of the feed gas and an oxygen-bearing gas to obtain, by partial combustion, the product gas and leading the product gas around the catalyst filled reaction tubes.
The feedgas for the process consists substantially of hydrocarbons, particularly natural gas with which steam is admixed. It may also contain hydrogen, or an oxide of carbon, or both.
The process may include the adding of a fuel gas to supplement the partial combustion of the reformed gas. The fuel gas may be hydrogen, hydrocarbons, or a mixture of hydrogen and hydrocarbons.
- 2a -~Z~ 78 The process mav also be carried out at elevated pressure, preferably at a pressure exceeding 3 bar.
The invention also provides an apparatus for implement-ing the above process which comprises reaction tubes for filling with catalyst installed in a reactor which is divided by a part~
ition wall into an upper chamber Eor receiving feedgas consisting substantially of hydrocarbons with which steam is admixed and a lower chamber in which further reactions can take place, the reaction tubes being fixed to the partition wall through a gas-tight seal and each having an open upper end communicating withthe upper chamber for the intake of the feedgas and an open lower end communicating with the lower chamber and comprises one or more intake nozzles for providing process fluid on thereactor wall or reactor bottom or both, at least one jet tube or at least one permeable ceramic plate or both for fluid passage into a free space of the lower chamber and at least one jet tube for a start-up burner.
Preferably, the apparatus comprises baffles for aiding heat transfer from a hot, combustion gas side of the lower chamber.
The baffles, in such case, are connected to the partition wall, one or more of the reaction tubes, or both.
The apparatus also preferably comprises the reaction tubes connected to the partition wall, such connection being detachable but gas tight.
The apparatus may also comprise at least one of the reaction tubes having a central tube of smaller diameter through which at least part of an oxidation agent can be supplied to the free space of the lower chamber.
3 -,~
;
'' :, , ' ~;7~7:~3 The inven-tion offers the particular advan-tage that the process used for ob-taining product gas yields no flue gas so that no complex heat - 3a -~5'7~'78 exchangers are needed. There is a consequent recluction of capital cost.
In addition, and as compered with the conventional process, heat economy is significant because of the complete absence of the substantial volume of flue gas with its unrecoverable heat content at low ~emperature.
In drawings which illustrate, by way of example, embodiments of the invention:
Figure 1 shows a flowsheet of one embodiment of the process according to the invention with natural gas serving as feedgas, the product gas being used in a methanol synthesis plant;
Figure 2 is a cross-sectional view of an apparatus for implementing the process shown in Figure l;
Figure 3 is a cross-sectional view of the lower part of a reaction tube.
Referring to Figure 1, a natural gas/steam mixture used as feedstock enters at 1 into reactor 2. In an upper chamber 3, the mixture is distributed to catalyst-containing reaction tubes ~; while passing through the tubes, it absorbs heat and undergoes conversion to a preconditioned reformed gas. The preconditioned reformed gas leaves the reaction tubes ~
at tube ends 5 and mixes in free space 6 with an oxidation agent, for example oxygen, admitted to the free space through line 7. ~atural gas and recycle gas, if any, are admitted through lines 8 and 9, and further reaction occurs with continued temperature rise. The heat produced by this reaction is utilized for heating the reaction tubes 4. As indicated by arrows at 10, the hot product gas passes through the free space of the reactor 2, in a direction opposite to the direction of flow inside the reaction tubes 4 and leaves reactor 2 at outlet 11.
~2~7~k7~
The gas then goes to a cooling loop 12 which serves especially for condensing water vapour, the condensate being drained through line 13. The heat liberated in the cooling loop can be utili~ed in various ways, especially for preheating and superheating the starting materials, viz~ natural gas and steam which are emitted through line 1~ to cooling loop 12.
For final cooling, any suitable coolant, for example water, air or OXygen admitted through line 15 can be used if it must undergo preheating from a relatively low temperature.
The near-anhydrous product gas can now be processed in a synthesis plant, for example in the manufacture of methanol. A defined quantity of the gas with inert components must be withdrawn from the synthesis loop through line 17 because any product gas will contain inert components. Another portion, called recycle gas, is returned through line 9 to reactor 2. The quantity of recycle gas depends on the composition of the feedgas in reactor 2 and the reaction conditions prevailing in free space 6. Moreover, provision is made for adding the recycle gas or part thereof through line 18 to the feed mixture. The crude methanol leaves the synthesis loop through line 19.
For the conventional process, heat requirements amount to approximately 7.9 Gcal/ton of methanol. For the process according to the invention, heat requirements are less than 7.1 Gcal/ton of methanol.
Figure 2 shows apparatus for implementing the process illustrated in Figure 1. Reactor 2 contains a multitude of reaction tubes 4 filled with catalyst 20. Reaction tubes ~ are sealed into partition wall 21. The upper end 22 is open and communicates with the upper chamber while the lower end 23 is also open for communicating with the lower chamber 2~. In this way, the assembly comprising partitionwas 11 21 and reaction tubes ~ is released from ~z~74~
pressure. The upper parts of reaction tubes 4 are provided with baffles 25 jacketing the reaction tubes so that the hot product gas passes through annular spaces. This gas leaves reactor 2 through nozzle 26. Because of the prevailing high temperature, the lower chamber 24 of reactor 2 including the underside of the partition wall is provided with refractory insulation or brick lining 27. For improving the heat transfer on the hot combustion gas side of the lower chamber 24, provision may be made for installing baffles 25 of different configuration, exemplified by jacket tubes, between the reaction tubes. These baffles should be connected to the reaction tubes or the partition wall or both so that they can be installed and removed jointly with the reaction tubes. ~e enclosing walls of free space 6 contain feed connections or oxidation agent and hydrocarbon, said connections comprising both simple jet tubes 28 especially for the admission of hydrocarbons, and permeable porous ceramic plates 29, especially for the admission of oxidation agents. Moreover, jet tube 28 is designed to permit the admission of oxidation agent for preheating and commissioning the reactor.
Figure 3 refers to another design of the reaction tube, the ~igure illustrating only the lower end of the tube. This design provides for admitting at least part of the oxidation agent to space 6 through tube 30 arranged in the center of the reaction tube. Referring to reactors of large diameter~ this design offers the advantage of improved mixing conditions in free space 6. However, it is not absolutely necessary that each reaction tube 4 be provided with a tube 30 for the passage/admission of oxidation agent.
;
'' :, , ' ~;7~7:~3 The inven-tion offers the particular advan-tage that the process used for ob-taining product gas yields no flue gas so that no complex heat - 3a -~5'7~'78 exchangers are needed. There is a consequent recluction of capital cost.
In addition, and as compered with the conventional process, heat economy is significant because of the complete absence of the substantial volume of flue gas with its unrecoverable heat content at low ~emperature.
In drawings which illustrate, by way of example, embodiments of the invention:
Figure 1 shows a flowsheet of one embodiment of the process according to the invention with natural gas serving as feedgas, the product gas being used in a methanol synthesis plant;
Figure 2 is a cross-sectional view of an apparatus for implementing the process shown in Figure l;
Figure 3 is a cross-sectional view of the lower part of a reaction tube.
Referring to Figure 1, a natural gas/steam mixture used as feedstock enters at 1 into reactor 2. In an upper chamber 3, the mixture is distributed to catalyst-containing reaction tubes ~; while passing through the tubes, it absorbs heat and undergoes conversion to a preconditioned reformed gas. The preconditioned reformed gas leaves the reaction tubes ~
at tube ends 5 and mixes in free space 6 with an oxidation agent, for example oxygen, admitted to the free space through line 7. ~atural gas and recycle gas, if any, are admitted through lines 8 and 9, and further reaction occurs with continued temperature rise. The heat produced by this reaction is utilized for heating the reaction tubes 4. As indicated by arrows at 10, the hot product gas passes through the free space of the reactor 2, in a direction opposite to the direction of flow inside the reaction tubes 4 and leaves reactor 2 at outlet 11.
~2~7~k7~
The gas then goes to a cooling loop 12 which serves especially for condensing water vapour, the condensate being drained through line 13. The heat liberated in the cooling loop can be utili~ed in various ways, especially for preheating and superheating the starting materials, viz~ natural gas and steam which are emitted through line 1~ to cooling loop 12.
For final cooling, any suitable coolant, for example water, air or OXygen admitted through line 15 can be used if it must undergo preheating from a relatively low temperature.
The near-anhydrous product gas can now be processed in a synthesis plant, for example in the manufacture of methanol. A defined quantity of the gas with inert components must be withdrawn from the synthesis loop through line 17 because any product gas will contain inert components. Another portion, called recycle gas, is returned through line 9 to reactor 2. The quantity of recycle gas depends on the composition of the feedgas in reactor 2 and the reaction conditions prevailing in free space 6. Moreover, provision is made for adding the recycle gas or part thereof through line 18 to the feed mixture. The crude methanol leaves the synthesis loop through line 19.
For the conventional process, heat requirements amount to approximately 7.9 Gcal/ton of methanol. For the process according to the invention, heat requirements are less than 7.1 Gcal/ton of methanol.
Figure 2 shows apparatus for implementing the process illustrated in Figure 1. Reactor 2 contains a multitude of reaction tubes 4 filled with catalyst 20. Reaction tubes ~ are sealed into partition wall 21. The upper end 22 is open and communicates with the upper chamber while the lower end 23 is also open for communicating with the lower chamber 2~. In this way, the assembly comprising partitionwas 11 21 and reaction tubes ~ is released from ~z~74~
pressure. The upper parts of reaction tubes 4 are provided with baffles 25 jacketing the reaction tubes so that the hot product gas passes through annular spaces. This gas leaves reactor 2 through nozzle 26. Because of the prevailing high temperature, the lower chamber 24 of reactor 2 including the underside of the partition wall is provided with refractory insulation or brick lining 27. For improving the heat transfer on the hot combustion gas side of the lower chamber 24, provision may be made for installing baffles 25 of different configuration, exemplified by jacket tubes, between the reaction tubes. These baffles should be connected to the reaction tubes or the partition wall or both so that they can be installed and removed jointly with the reaction tubes. ~e enclosing walls of free space 6 contain feed connections or oxidation agent and hydrocarbon, said connections comprising both simple jet tubes 28 especially for the admission of hydrocarbons, and permeable porous ceramic plates 29, especially for the admission of oxidation agents. Moreover, jet tube 28 is designed to permit the admission of oxidation agent for preheating and commissioning the reactor.
Figure 3 refers to another design of the reaction tube, the ~igure illustrating only the lower end of the tube. This design provides for admitting at least part of the oxidation agent to space 6 through tube 30 arranged in the center of the reaction tube. Referring to reactors of large diameter~ this design offers the advantage of improved mixing conditions in free space 6. However, it is not absolutely necessary that each reaction tube 4 be provided with a tube 30 for the passage/admission of oxidation agent.
Claims (13)
PROPERTY OR PRIVILEGE IS CLAIMED ARE DEFINED AS FOLLOWS:
1. In a process for the generation of a product gas contain-ing hydrogen and carbon oxides from a feed gas consisting sub-stantially of hydrocarbons comprising the steps of:
(a) catalytic endothermic reforming of feed gas in catalyst filled reaction tubes to obtain reformed gas;
(b) partial combustion of the reformed gas by means of the addition of an oxygen-bearing gas to the reformed gas to obtain a product gas; and (c) heating the reaction tubes by means of the product gas generated by the partial combustion;
the improvement which comprises catalytic endothermic reforming of a part of the feed gas, to which steam is admixed, in the catalyst filled reaction tubes to obtain reformed gas, and mixing the reformed gas with the remaining part of the feed gas and an oxygen-bearing gas to obtain, by partial combustion, the product gas and leading the product gas around the catalyst filled reaction tubes.
(a) catalytic endothermic reforming of feed gas in catalyst filled reaction tubes to obtain reformed gas;
(b) partial combustion of the reformed gas by means of the addition of an oxygen-bearing gas to the reformed gas to obtain a product gas; and (c) heating the reaction tubes by means of the product gas generated by the partial combustion;
the improvement which comprises catalytic endothermic reforming of a part of the feed gas, to which steam is admixed, in the catalyst filled reaction tubes to obtain reformed gas, and mixing the reformed gas with the remaining part of the feed gas and an oxygen-bearing gas to obtain, by partial combustion, the product gas and leading the product gas around the catalyst filled reaction tubes.
2. A process-as defined in claim 1 wherein the feedgas consists substantially of natural gas.
3. A process as defined in claim 1 wherein the oxygen for the partial combustion of the reformed gas is provided by air.
4. A process as defined in claim 1 wherein the feedgas contains hydrogen or an oxide of carbon or both.
5. A process as defined in claim 1 wherein a fuel gas is added to supplement the partial combustion of the reformed gas.
6. A process as defined in claim 5 wherein the fuel gas is one of hydrogen, hydrocarbons and a mixture of hydrogen and hydrocarbons.
7. A process as defined in claim 1 wherein the reaction is carried out at elevated pressure.
8. A process as defined in claim 7 wherein the elevated pressure exceeds 3 bar.
9. An apparatus for implementing the process as defined in claim 1 which apparatus comprises reaction tubes for containing catalyst installed in a reactor which is divided by a partition wall into an upper chamber for receiving feedgas consisting sub-stantially of hydrocarbons with which steam is admixed and a lower chamber in which further reactions take place, the reaction tubes being fixed to the partition wall through a gastight seal and each having an open upper end communicating with the upper chamber for the intake of the feedgas and an open lower end communicating with the lower chamber and which comprises one or more intake nozzles for providing process fluids on the reactor wall or reactor bottom or both, at least one jet tube or at least one permeable ceramic plate or both for fluid passage into the free space of the lower chamber and at least one jet tube for a start-up burner.
10. An apparatus as defined in claim 9 which comprises one or more jet tubes in the lower reactor wall or reactor bottom for admission of hydrocarbons and admission of oxidation agents.
11. An apparatus as defined in claim 9 wherein an inside surface of the lower chamber of the reactor is provided with a refractory insulation or brick lining.
12. An apparatus as defined in claim 9 comprising baffles for aiding heat transfer from the hot, combustion gas side of the lower chamber, said baffles being connected to the partition wall, or one or more reaction tubes, or both.
13. An apparatus as defined in claim 9 wherein the reaction tubes are connected to the partition wall, the connection being detachable but gastight.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE19823244252 DE3244252A1 (en) | 1982-11-30 | 1982-11-30 | METHOD AND DEVICE FOR GENERATING PRODUCT GAS WITH HYDROGEN AND CARBON OXYDE CONTENT |
| DEP3244252.1 | 1982-11-30 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CA1257478A true CA1257478A (en) | 1989-07-18 |
Family
ID=6179426
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA000442092A Expired CA1257478A (en) | 1982-11-30 | 1983-11-28 | Process and equipment for the generation of a product gas containing hydrogen and carbon oxides |
Country Status (9)
| Country | Link |
|---|---|
| EP (1) | EP0110093B1 (en) |
| JP (1) | JPS59107901A (en) |
| AT (1) | ATE44717T1 (en) |
| AU (1) | AU579990B2 (en) |
| CA (1) | CA1257478A (en) |
| DE (2) | DE3244252A1 (en) |
| DK (1) | DK162935C (en) |
| MX (1) | MX161814A (en) |
| NO (1) | NO163732C (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105143099A (en) * | 2014-01-13 | 2015-12-09 | 气体化学技术有限责任公司 | Reactor for partial oxidation of hydrocarbon gases |
Families Citing this family (19)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0124226B1 (en) * | 1983-03-25 | 1989-10-18 | Imperial Chemical Industries Plc | Steam reforming |
| US4666680A (en) * | 1984-01-30 | 1987-05-19 | Fluor Corporation | Autothermal production of synthesis gas |
| GB2163449B (en) * | 1984-07-18 | 1988-06-02 | Shell Int Research | Production of gas mixtures containing hydrogen and carbon monoxide |
| US4919844A (en) * | 1984-08-16 | 1990-04-24 | Air Products And Chemicals, Inc. | Enhanced heat transfer reformer and method |
| DK165946C (en) * | 1985-03-21 | 1993-07-05 | Haldor Topsoe As | REFORMING PROCESS DURING HEAT EXCHANGE AND REACTOR THEREOF |
| DE3532413A1 (en) * | 1985-09-11 | 1987-03-12 | Uhde Gmbh | DEVICE FOR GENERATING SYNTHESIS GAS |
| DE3605811A1 (en) * | 1986-02-22 | 1987-08-27 | Uhde Gmbh | DEVICE FOR USE IN A METHOD FOR PRODUCING PRODUCT GAS WITH HYDROGEN AND CARBON OXIDE CONTENT |
| DE3719780A1 (en) * | 1987-06-13 | 1988-12-22 | Uhde Gmbh | METHOD FOR PRODUCING AMMONIA FROM NATURAL GAS |
| DE8816548U1 (en) * | 1988-02-03 | 1989-10-26 | Uhde Gmbh, 4600 Dortmund | Device for carrying out multi-stage synthesis gas production |
| DE3806408A1 (en) * | 1988-02-29 | 1989-09-07 | Uhde Gmbh | METHOD AND DEVICE FOR GENERATING AN H (ARROW DOWN) 2 (ARROW DOWN) AND CO-CONTAINING SYNTHESIS GAS |
| JPH01261201A (en) * | 1988-04-12 | 1989-10-18 | Mitsubishi Gas Chem Co Inc | Hydrocarbon reforming reactor |
| DE3813861C1 (en) * | 1988-04-23 | 1989-09-28 | Uhde Gmbh, 4600 Dortmund, De | |
| DE3813863A1 (en) * | 1988-04-23 | 1989-11-02 | Uhde Gmbh | DEVICE FOR RECEIVING CATALYSTS, ESPECIALLY IN THE PRODUCTION OF SYNTHESIS GAS |
| DE3813864A1 (en) * | 1988-04-23 | 1989-11-02 | Uhde Gmbh | Apparatus, in particular for producing synthesis gas in a reformer |
| GB2217728B (en) * | 1988-04-28 | 1992-02-26 | Humphreys & Glasgow Ltd | Combined reformer |
| DE4221837C1 (en) * | 1992-07-03 | 1993-08-19 | Uhde Gmbh, 4600 Dortmund, De | Shrouded catalytic reformer tube - with partially enclosed gas mixing zone, for prodn. of synthesis gas |
| MY139324A (en) * | 2001-06-25 | 2009-09-30 | Shell Int Research | Integrated process for hydrocarbon synthesis |
| JP2006523598A (en) * | 2003-04-15 | 2006-10-19 | シエル・インターナシヨネイル・リサーチ・マーチヤツピイ・ベー・ウイ | Syngas production method |
| DE10345902B4 (en) * | 2003-10-02 | 2005-07-07 | Lurgi Ag | Production of synthesis gas from natural gas involves effecting both the reforming of a natural gas/steam mixture and also cooling of the obtained synthesis gas in a closed vertical reactor |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US2529630A (en) * | 1947-04-25 | 1950-11-14 | Stanolind Oil & Gas Co | Process for the manufacture of synthesis gases |
| US2579843A (en) * | 1947-12-10 | 1951-12-25 | Method foe the manufacture of | |
| DE1021121B (en) * | 1955-06-07 | 1957-12-19 | Max Gerhold Dipl Ing Dr Techn | Process for the thermal-catalytic conversion of high and high molecular weight, gaseous or liquid hydrocarbons into gases consisting essentially of low molecular weight carbon compounds and hydrogen |
| GB845401A (en) * | 1955-07-15 | 1960-08-24 | Gas Council | Improved process for the production of gases containing hydrogen |
| US3030092A (en) * | 1958-04-10 | 1962-04-17 | Degussa | Device for a gastight fixing of ceramic tubes in high temperature furnaces |
| DE1667573B2 (en) * | 1967-08-10 | 1976-10-21 | Krupp-Koppers Gmbh, 4300 Essen | METHOD AND DEVICE FOR GENERATING A HYDROGEN-RICH GAS BY THE SPREAD OF A MIXTURE OF GASEOUS AND / OR LIQUID HYDROCARBONS AND WATER VAPOR |
| US3751228A (en) * | 1970-12-16 | 1973-08-07 | V Semenov | Apparatus for reforming hydrocarbons under pressure |
| DE2412841C2 (en) * | 1974-03-18 | 1982-11-11 | Metallgesellschaft Ag, 6000 Frankfurt | Reactor for splitting hydrocarbons on an indirectly heated catalyst |
| JPS52112607A (en) * | 1976-03-09 | 1977-09-21 | Agency Of Ind Science & Technol | Reformers |
| JPS5382691A (en) * | 1976-12-29 | 1978-07-21 | Chiyoda Chem Eng & Constr Co Ltd | Preparation of synthetic gas for ammonia without using external heat type steam modifying device |
| FR2372116A1 (en) * | 1977-03-22 | 1978-06-23 | Banquy David | SYNTHESIS GAS PRODUCTION PROCESS |
-
1982
- 1982-11-30 DE DE19823244252 patent/DE3244252A1/en active Granted
-
1983
- 1983-10-18 DE DE8383110367T patent/DE3380212D1/en not_active Expired
- 1983-10-18 AT AT83110367T patent/ATE44717T1/en not_active IP Right Cessation
- 1983-10-18 EP EP83110367A patent/EP0110093B1/en not_active Expired
- 1983-11-18 NO NO834244A patent/NO163732C/en unknown
- 1983-11-23 AU AU21604/83A patent/AU579990B2/en not_active Expired
- 1983-11-28 CA CA000442092A patent/CA1257478A/en not_active Expired
- 1983-11-29 DK DK546683A patent/DK162935C/en not_active IP Right Cessation
- 1983-11-30 JP JP58224594A patent/JPS59107901A/en active Granted
- 1983-11-30 MX MX199586A patent/MX161814A/en unknown
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105143099A (en) * | 2014-01-13 | 2015-12-09 | 气体化学技术有限责任公司 | Reactor for partial oxidation of hydrocarbon gases |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0450245B2 (en) | 1992-08-13 |
| DE3244252A1 (en) | 1984-05-30 |
| DE3380212D1 (en) | 1989-08-24 |
| DK546683D0 (en) | 1983-11-29 |
| EP0110093A2 (en) | 1984-06-13 |
| ATE44717T1 (en) | 1989-08-15 |
| DK162935B (en) | 1991-12-30 |
| NO163732B (en) | 1990-04-02 |
| DK162935C (en) | 1992-05-25 |
| DK546683A (en) | 1984-05-31 |
| DE3244252C2 (en) | 1990-10-31 |
| MX161814A (en) | 1990-12-28 |
| AU2160483A (en) | 1984-06-07 |
| JPS59107901A (en) | 1984-06-22 |
| EP0110093A3 (en) | 1986-07-02 |
| NO834244L (en) | 1984-06-01 |
| EP0110093B1 (en) | 1989-07-19 |
| AU579990B2 (en) | 1988-12-22 |
| NO163732C (en) | 1990-07-11 |
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