WO2015069836A4 - Gaseous fuel cpox reformers and methods of cpox reforming - Google Patents

Gaseous fuel cpox reformers and methods of cpox reforming Download PDF

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Publication number
WO2015069836A4
WO2015069836A4 PCT/US2014/064239 US2014064239W WO2015069836A4 WO 2015069836 A4 WO2015069836 A4 WO 2015069836A4 US 2014064239 W US2014064239 W US 2014064239W WO 2015069836 A4 WO2015069836 A4 WO 2015069836A4
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WO
WIPO (PCT)
Prior art keywords
cpox
reactor unit
gaseous
cpox reactor
reformer
Prior art date
Application number
PCT/US2014/064239
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French (fr)
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WO2015069836A2 (en
WO2015069836A3 (en
Inventor
Caine M. FINNERTY
Paul DEWALD
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Watt Fuel Cell Corp.
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Application filed by Watt Fuel Cell Corp. filed Critical Watt Fuel Cell Corp.
Priority to JP2016553235A priority Critical patent/JP6253795B2/en
Priority to CA2929546A priority patent/CA2929546C/en
Priority to MX2016004681A priority patent/MX352220B/en
Priority to AU2014346741A priority patent/AU2014346741B2/en
Priority to CN201480060614.7A priority patent/CN105706282B/en
Priority to KR1020167012056A priority patent/KR101796495B1/en
Priority to EP14803010.9A priority patent/EP3065856B1/en
Publication of WO2015069836A2 publication Critical patent/WO2015069836A2/en
Publication of WO2015069836A3 publication Critical patent/WO2015069836A3/en
Publication of WO2015069836A4 publication Critical patent/WO2015069836A4/en

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J12/00—Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor
    • B01J12/007—Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor in the presence of catalytically active bodies, e.g. porous plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J19/2425—Tubular reactors in parallel
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    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J4/00—Feed or outlet devices; Feed or outlet control devices
    • B01J4/001—Feed or outlet devices as such, e.g. feeding tubes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J4/00—Feed or outlet devices; Feed or outlet control devices
    • B01J4/001—Feed or outlet devices as such, e.g. feeding tubes
    • B01J4/002—Nozzle-type elements
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J4/00—Feed or outlet devices; Feed or outlet control devices
    • B01J4/001—Feed or outlet devices as such, e.g. feeding tubes
    • B01J4/005—Feed or outlet devices as such, e.g. feeding tubes provided with baffles
    • C—CHEMISTRY; METALLURGY
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    • 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
    • C01B3/323—Catalytic reaction of gaseous or liquid organic compounds other than hydrocarbons with gasifying agents
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    • 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
    • C01B3/386—Catalytic partial combustion
    • H—ELECTRICITY
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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • H01M8/0618—Reforming processes, e.g. autothermal, partial oxidation or steam reforming
    • 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
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00002—Chemical plants
    • B01J2219/00004—Scale aspects
    • B01J2219/00006—Large-scale industrial plants
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    • B01J2219/00051—Controlling the temperature
    • B01J2219/00054—Controlling or regulating the heat exchange system
    • B01J2219/00056—Controlling or regulating the heat exchange system involving measured parameters
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    • B01J2219/0006—Temperature measurement of the heat exchange medium
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    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00054—Controlling or regulating the heat exchange system
    • B01J2219/00056—Controlling or regulating the heat exchange system involving measured parameters
    • B01J2219/00069—Flow rate measurement
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00132—Controlling the temperature using electric heating or cooling elements
    • B01J2219/00135—Electric resistance heaters
    • 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
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00159—Controlling the temperature controlling multiple zones along the direction of flow, e.g. pre-heating and after-cooling
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
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    • B01J2219/00191—Control algorithm
    • B01J2219/00193—Sensing a parameter
    • B01J2219/00195—Sensing a parameter of the reaction system
    • B01J2219/002—Sensing a parameter of the reaction system inside the reactor
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00191—Control algorithm
    • B01J2219/00222—Control algorithm taking actions
    • B01J2219/00227—Control algorithm taking actions modifying the operating conditions
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    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
    • C01B2203/0261—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a catalytic partial oxidation step [CPO]
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    • C01—INORGANIC CHEMISTRY
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1005—Arrangement or shape of catalyst
    • C01B2203/1035—Catalyst coated on equipment surfaces, e.g. reactor walls
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
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    • C01B2203/1223—Methanol
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
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    • C01B2203/1229—Ethanol
    • C—CHEMISTRY; METALLURGY
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    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
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    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1241—Natural gas or methane
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1247—Higher hydrocarbons
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/14—Details of the flowsheet
    • C01B2203/141—At least two reforming, decomposition or partial oxidation steps in parallel
    • 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
    • C01B2203/16—Controlling the process
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    • C01B2203/16—Controlling the process
    • C01B2203/1604—Starting up the process

Abstract

A gaseous fuel catalytic partial oxidation (CPOX) reformer can include a plurality or an array of spaced-apart CPOX reactor units (408), each reactor unit including an elongate tube having a wall with internal and external surfaces, the wall enclosing an open gaseous flow passageway with at least a portion of the wall having CPOX catalyst disposed therein and/or comprising its structure. The catalyst-containing wall structure and open gaseous flow passageway enclosed thereby define a gaseous phase CPOX reaction zone (409), the catalyst-containing wall section being gas-permeable to allow gaseous CPOX reaction mixture to diffuse therein and hydrogen- rich product reformate to diffuse therefrom. At least the exterior surface of a CPOX reaction zone of a CPOX reactor unit can include a hydrogen barrier. The gaseous fuel CPOX reformer also can include one or more igniters, and a source of gaseous reformable fuel.

Claims

AMENDED CLAIMS received by the International Bureau on 25 August 2015 (25.08.2015)
1. A gaseous fuel CPOX reformer comprising: an array of spaced-apart CPOX reactor units, each CPOX reactor unit comprising an elongate tube having a gas-permeable wall with an internal surface and an external surface, the gas-permeable wall enclosing an open gaseous flow passageway and defin ing an inlet and an outlet of the CPOX reactor unit, wherein a CPOX reactor unit is in thermal communication with at least an adjacent CPOX reactor unit(s) in the array.. at least a section of the gas-permeable wall comprises a CPOX catalyst, and an igniter in thermal communication with at least a section of the gas permeable wail comprising a CPOX catalyst of at least one CPOX reactor unit.
2. The gaseous fuel CPOX reformer of claim 1 , wherein a hydrogen barrier is associated with the external surface of at least the CPOX catalyst-containing wall section of a CPOX reactor unit.
3. The gaseous fuel CPOX reformer of claims 1 or 2, wherein the maximum distance between adjacent CPOX reactor units is that distance beyond which a CPOX reaction fails to be initiated in an adjacent CPOX reactor unit by the heat from a CPOX reaction in an operating CPOX reactor unit and/or during a steady-state mode of operation, the temperature of the array of spaced-apart CPOX reactor uni ts falls below a predetermined minimum array temperature; and the minimum distance between adjacent CPOX reactor units is that distance below which the temperature at an outlet of a CPOX reactor unit is greater than a predetermined maximum temperature.
4. The gaseous fuel CPOX reformer of any one of claims 1 -3, wherein the predetermined maximum temperature is a temperature that is tolerable by an inlet of a fuel cell stack in thermal and fluid communication with an outlet of a CPOX reactor unit.
5. The gaseous fuel CPOX reformer of any one of claims 1 -4, comprising more than one igniter, wherein each igniter is positioned in thermal communication with at least a section of the gas-permeable wall comprising a CPOX catalyst of at least one CPOX reactor unit.
6. The gaseous fuel CPOX reformer of any one of claims 1 -5, wherein the CPOX catalyst is disposed within the wall of the CPOX reactor unit, disposed on an internal surface of the wall of the CPOX reactor unit, partially or completely forms the structure of the wall of the CPOX reactor unit, and combinations thereof.
7. The gaseous fuel CPOX reformer of any one of claims 1 -6, wherein the CPOX catalyst-containing wall section comprises a ceramic.
8. The gaseous fuel CPOX reformer of any one of claims 2-7, wherein the hydrogen barrier comprises pressurized fluid.
9. A method of CPOX reforming a gaseous reformable fuel to a hydrogen-rich reformate employing the gaseous fuel CPOX reformer of claim 1 , the method comprising: introducing a gaseous CPOX reaction mixture comprising a gaseous reformable fuel into inlets of CPOX reactor units of the reformer; initiating catalytic partial oxidation of the gaseous CPOX reaction mixture to begin production of a hydrogen-rich reformate in at least one CPOX reactor unit, the gas-permeable CPOX catalyst-containing wall section of the at least one CPOX reactor unit allowing gaseous CPOX reaction mixture to diffuse therein and product hydrogen-rich reformate to diffuse therefrom; and, maintaining catalytic partial oxidation of the gaseous CPOX reaction mixture in the at least one CPOX reactor unit.
10. The method of claim 9, wherein a hydrogen barrier is associated with the external surface of at least the CPOX catalyst-containing wall section of a CPOX reactor unit.
1 1. The method of claim 9 or 10, wherein in the step of initiating catalytic partial oxidation, the molar ratio of oxygen to carbon of the gaseous CPOX reaction mixture
corresponds to that of a fuel-lean CPOX reaction mixture and in the step of maintaining catalytic partial oxidation of gaseous CPOX reaction mixture, the molar ratio of oxygen to carbon of the gaseous CPOX reaction mixture corresponds to that of a fuel-rich CPOX reaction mixture.
12. The method of any one of claims 9-11, wherein the maximum distance between adjacent CPOX reactor units is that distance beyond which a CPOX reaction fails to be initiated in an adjacent CPOX reactor unit by the heat from a CPOX reaction in an operating CPOX reactor unit and/or during a steady-state mode of operation, the temperature of a CPOX reactor unit falls below a predetermined minimum array temperature; and the minimum distance between adjacent CPOX reactor units is that distance below which the temperature at an outlet of a CPOX reactor unit is greater than a predetermined maximum temperature.
13. The method of any one of claims 9-12, wherein initiating catalytic partial oxidation comprises: initiating a CPOX reaction in at least one CPOX reactor unit; and transferring heat from the CPOX reaction in the at least one CPOX reactor unit to at least one other CPOX reactor unit to initiate a CPOX reaction therein.
14. The method of any one of claims 9-13, wherein initiating the CPOX reaction comprises initiating more than a single igniter to initiate catalytic partial oxidation of the gaseous CPOX reaction mixture in each of the CPOX reactor units, wherein the number of igni ters is less than the number of CPOX reactor units,
15. The method of any one of claims 9-14, comprising varying the oxygen to carbon ratio of the gaseous CPOX reaction mixture during operation of the gaseous fuel CPOX reformer.
PCT/US2014/064239 2013-11-06 2014-11-06 Gaseous fuel cpox reformers and methods of cpox reforming WO2015069836A2 (en)

Priority Applications (7)

Application Number Priority Date Filing Date Title
JP2016553235A JP6253795B2 (en) 2013-11-06 2014-11-06 Gaseous fuel CPOX reformer and CPOX reforming method
CA2929546A CA2929546C (en) 2013-11-06 2014-11-06 Gaseous fuel cpox reformers and methods of cpox reforming
MX2016004681A MX352220B (en) 2013-11-06 2014-11-06 Gaseous fuel cpox reformers and methods of cpox reforming.
AU2014346741A AU2014346741B2 (en) 2013-11-06 2014-11-06 Gaseous fuel CPOX reformers and methods of CPOX reforming
CN201480060614.7A CN105706282B (en) 2013-11-06 2014-11-06 Fuel gas CPOX reformers and CPOX reforming methods
KR1020167012056A KR101796495B1 (en) 2013-11-06 2014-11-06 Gaseous fuel cpox reformers and methods of cpox reforming
EP14803010.9A EP3065856B1 (en) 2013-11-06 2014-11-06 Gaseous fuel cpox reformers and methods of cpox reforming

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US201361900543P 2013-11-06 2013-11-06
US61/900,543 2013-11-06

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WO2015069836A2 (en) 2015-05-14
JP2016537297A (en) 2016-12-01
JP6253795B2 (en) 2017-12-27
CA2929546C (en) 2019-03-05
EP3065856B1 (en) 2022-06-08
US9627699B2 (en) 2017-04-18
KR20160083000A (en) 2016-07-11
MX2016004681A (en) 2016-07-26
CN105706282B (en) 2018-05-01
EP3065856A2 (en) 2016-09-14
WO2015069836A3 (en) 2015-08-27
US20150144841A1 (en) 2015-05-28
MX352220B (en) 2017-11-15
CA2929546A1 (en) 2015-05-14
AU2014346741A1 (en) 2016-03-17
CN105706282A (en) 2016-06-22
KR101796495B1 (en) 2017-11-10
AU2014346741B2 (en) 2017-01-19

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