WO2014117950A1 - Catalytic converter units for a high-temperature fuel cell system - Google Patents

Catalytic converter units for a high-temperature fuel cell system Download PDF

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Publication number
WO2014117950A1
WO2014117950A1 PCT/EP2014/000286 EP2014000286W WO2014117950A1 WO 2014117950 A1 WO2014117950 A1 WO 2014117950A1 EP 2014000286 W EP2014000286 W EP 2014000286W WO 2014117950 A1 WO2014117950 A1 WO 2014117950A1
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WO
WIPO (PCT)
Prior art keywords
catalyst
reforming
oxidation
catalytic converter
unit
Prior art date
Application number
PCT/EP2014/000286
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German (de)
French (fr)
Other versions
WO2014117950A8 (en
Inventor
Jürgen RECHBERGER
Michael Reissig
Original Assignee
Avl List Gmbh
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Publication date
Application filed by Avl List Gmbh filed Critical Avl List Gmbh
Priority to DE112014000664.5T priority Critical patent/DE112014000664A5/en
Publication of WO2014117950A1 publication Critical patent/WO2014117950A1/en
Publication of WO2014117950A8 publication Critical patent/WO2014117950A8/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
    • H01M8/06—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
    • H01M8/0625—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 in a modular combined reactor/fuel cell structure
    • 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
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/248—Reactors comprising multiple separated flow channels
    • B01J19/2495—Net-type reactors
    • 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
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/248—Reactors comprising multiple separated flow channels
    • B01J19/249—Plate-type reactors
    • 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
    • B01J8/0242—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 the fluid flow within the bed being predominantly vertical
    • B01J8/025—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 the fluid flow within the bed being predominantly vertical in a cylindrical shaped bed
    • 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
    • B01J8/0285—Heating or cooling the reactor
    • 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
    • C01B3/323—Catalytic reaction of gaseous or liquid organic compounds other than 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
    • 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
    • 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
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00168—Controlling the temperature by indirect heat exchange with heat exchange elements outside the bed of solid particles
    • B01J2208/00212—Plates; Jackets; Cylinders
    • 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
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00309—Controlling the temperature by indirect heat exchange with two or more reactions in heat exchange with each other, such as an endothermic reaction in heat exchange with an exothermic reaction
    • 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
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00796—Details of the reactor or of the particulate material
    • B01J2208/00823—Mixing elements
    • B01J2208/00831—Stationary elements
    • B01J2208/0084—Stationary elements inside the bed, e.g. baffles
    • 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
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00796—Details of the reactor or of the particulate material
    • B01J2208/00938—Flow distribution elements
    • 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
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2451—Geometry of the reactor
    • B01J2219/2454—Plates arranged concentrically
    • 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
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2451—Geometry of the reactor
    • B01J2219/2456—Geometry of the plates
    • B01J2219/2459—Corrugated plates
    • 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
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2461—Heat exchange aspects
    • B01J2219/2465—Two reactions in indirect heat exchange with each other
    • 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
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2469—Feeding means
    • B01J2219/247—Feeding means for the reactants
    • 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
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2491—Other constructional details
    • B01J2219/2492—Assembling means
    • 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
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • 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
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/066—Integration with other chemical processes with fuel cells
    • 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
    • C01B2203/0822—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel the fuel containing hydrogen
    • 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
    • C01B2203/0827—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel at least part of the fuel being a recycle stream
    • 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
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M2008/1293—Fuel cells with solid oxide electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency

Definitions

  • the invention relates to a catalyst unit for a high-temperature fuel cell system with a reforming catalyst for treating a fuel for the fuel cell and an oxidation catalyst for the
  • the catalyst unit described above can be used, for example, in a compact power unit (APU) of a motor vehicle, where it serves to provide electrical and thermal energy.
  • APU compact power unit
  • High-temperature fuel cell system in which a cylindrical reforming catalyst is incorporated in an oxidation catalyst.
  • a cylindrical reforming catalyst is arranged in a combustion chamber for a flame burner, which is annularly surrounded by an oxidation catalyst.
  • the unused fuel components of the anode exhaust gas are fed together with the cathode exhaust gas into the combustion chamber and post-treated in the oxidation catalyst.
  • the gaseous products after the catalytic conversion reach via edge-side openings of the oxidation catalyst in a
  • the gases to be treated initially flow through a cylindrical, inner catalyst, are then deflected and passed in countercurrent to an annular, outer catalyst region. The two areas are separated by a cylindrical partition. Both the inner catalyst and the outer catalyst have a metallic carrier (mash) layer for the catalytic substance.
  • the object of the invention is to develop a catalyst unit for a high-temperature fuel cell system of the type mentioned in such a way that a compact unit, especially for use in an APU is given, with improvements in heat transfer and in the maintenance and care of the unit to be achieved ,
  • the catalyst tube receiving reforming catalyst metal tube are separated, wherein the metal tube has a sleeve which forms a housing for the reforming catalyst, and an inner tube which forms the inner wall of the annular oxidation catalyst.
  • the reforming catalyst is exchangeable used in the annular oxidation catalyst.
  • both catalysts are thus fixed in independent housings.
  • the reforming catalyst can thus be easily replaced if necessary.
  • the oxidation catalyst and / or the reforming catalyst have a metallic catalyst carrier, wherein the sleeve is in thermal contact with the catalyst carrier of the reforming catalyst and the inner tube with the catalyst carrier of the oxidation catalyst.
  • catalyst support of the oxidation catalyst and the catalyst support of the reforming catalyst are connected by welding to the respectively adjacent parts of the metal pipe.
  • Oxidation catalyst can account for a conventional sealing mat, the
  • a particular advantage of this embodiment is that due to the improved thermal conductivity of the temperature profile of the
  • Catalyst unit (axial and radial) can be homogenized.
  • the improved heat dissipation in particular hot zones (hot spots) can be prevented in the two catalysts.
  • the gas distributor housing (reformer manifold) arranged at the beginning of the reforming catalyst can have an annular space into which the supply line for the fuel-gas mixture to be treated opens, starting radially from the annular space
  • Access openings are arranged from the annular space to the inlet surface of the reforming catalyst.
  • the axial distance a of the tangential inlet of the supply line for the fuel-gas mixture from the inlet surface of the reforming catalyst to the diameter D of the reforming catalyst can have a ratio a: D in the range from 0.2 to 1, preferably from 0 , 3 to 0.6, resulting in a desired ring flow
  • the tangential inlet may open into a cylindrical or frusto-conical region of the gas distributor housing.
  • FIG. 1 shows a catalyst unit according to the invention for a high-temperature fuel cell system in a three-dimensional, partially cutaway representation
  • Fig. 2 is a schematic representation of the principle of operation and the
  • FIG. 3 is a sectional view of the catalyst unit of FIG. 1,
  • Fig. 4 shows a variant of the catalyst unit of FIG. 1 in a three-dimensional representation.
  • Fig. 5 shows a first embodiment of a gas distributor housing
  • FIG. 6 shows the gas distributor housing according to FIG. 5 in an axial plan view
  • FIG. 7 shows a second embodiment of a gas distributor housing
  • FIG. 1 shows a catalyst unit 10 according to the invention for a high-temperature fuel cell system (not further illustrated here) with a cylindrical reforming catalyst 11 and a reforming catalyst annular
  • the reforming catalyst 11 is used for the preparation of the fuel for the fuel cell BZ (see Fig. 2), which is supplied with an oxidizing agent via the supply line 23 and with a
  • frustoconical gas distributor housing or Reformermanifold 24 is distributed as homogeneously as possible over the inlet surface of the reforming catalyst 11.
  • the oxidation catalyst 12 is used for exhaust aftertreatment of a starter burner and the fuel cell system.
  • Reforming catalyst 11 forms, as well as an outer tube 15, which forms the inner wall of the annular oxidation catalyst 12.
  • the reforming catalyst 11 can thus be used interchangeably in the annular oxidation catalyst 12.
  • the oxidation catalyst 12 and / or the reforming catalyst 11 preferably have a metallic catalyst carrier 16, 17, wherein the sleeve 14 of the metal tube 13 is in thermal contact with the catalyst carrier 16 of the reforming catalyst 11 and the outer tube 15 with the catalyst carrier 17 of the oxidation catalyst 12.
  • the catalyst support 17 of the oxidation catalyst 12 and the catalyst support 16 of the reforming catalyst 11 consists of a metallic
  • Wire mesh or a metallic lamellar structure which are connected by welding to the respective adjacent parts 14, 15 of the metal tube 13.
  • the sleeve 14 of the reforming catalyst 11 can be interchangeable inserted into the inner tube 15 and the inner wall of the annular oxidation catalyst 12 by means of a clearance fit, for example in the range of 0.2 mm to 1.5 mm. It is in the end of the sleeve 14 on the part of the
  • a ring seal 25 for example, a swelling mat
  • a swelling mat for example, a swelling mat
  • FIG. 2 shows, in a schematic overview, the arrangement of the catalyst unit 10 according to the invention, including the cylindrical reforming catalyst 11 and the annular oxidation catalyst 12 in combination with a
  • the fuel F is supplied during the starting cycle by means of a fuel pump 35 to a starter burner 26, the exhaust gases in the annular
  • Oxidation catalyst 12 are guided and arranged centrally
  • Fuel pump 36 of the evaporation unit 37 is supplied and introduced into the anode exhaust gas of the recirculation line 27, and together with the required oxidant, for example, air L, by means of compressor 28 the
  • the compressor 29 serves to supply the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.g., air L) to the oxidizing agent (e.
  • Oxidation catalyst 12 is subjected to waste heat. In the starting phase will also the starter burner 26 supplied via the compressor 29 with the required air.
  • Fig. 3 shows a variant of the catalyst unit 10 according to the invention in an enlarged sectional view.
  • Oxidation catalyst 12 and the reforming catalyst 11 separates, consists essentially of the sleeve 14, which forms a housing for the reforming catalyst 11, and from the inner tube 15, which is the inner wall of the annular
  • Oxidation catalyst 12 forms.
  • the circumferential sealing flange 18 here has a ring seal 25 to the end face of the inner tube 15.
  • both the oxidation catalytic converter 12 and the reforming catalytic converter 11 have a metallic catalyst carrier 16, 17, the gas paths of the two catalytic converters 11 being separated by a metal tube 13 accommodating the reforming catalyst 11 are, which is in thermal contact with the catalyst support 17 of the oxidation catalyst 12 and the catalyst support 16 of the reforming catalyst 11, for example by welding.
  • FIGS. 5 to 7 show two alternative embodiments for the gas distributor housing 24, which is arranged on the input side of the reforming catalytic converter 11. It serves to process the fuel-gas mixture over the whole
  • Gas distributor housing 24 an annular space 32, in which the supply line 23 for the fuel-gas mixture, for example, opens radially, starting from the annular space 32 radial access openings 33 in the form of a perforated ring from
  • Annular space 32 are arranged to the inlet surface 30 of the reforming catalyst 11, so that the reforming catalyst 11 is applied as uniformly as possible with the mixture of anode exhaust gas, vaporized fuel and oxidant.
  • the Reformermanifold of FIG. 5 and Fig. 6 is characterized by a compact design with low axial height.
  • a measuring device for example a temperature sensor, can be introduced into the annular space 32 (see FIG. 6).
  • the oxidation catalyst 12 has a tubular outer wall 21 with exhaust outlet openings 22. In this case, the exhaust gas outlet openings 22 are located in an area protruding beyond the catalyst carrier 17 (see also FIGS. 1 and 4).
  • the gas distributor housing 24 may be integrally formed with the inner wall 15 of the annular oxidation catalyst 12 or connected thereto by welding.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Fluid Mechanics (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

The invention relates to a catalytic converter unit (10) for a high-temperature fuel cell system, having a reformer catalytic converter (11) for the treatment of a fuel for the fuel cell and having an oxidation catalytic converter (12) for the aftertreatment of the exhaust gas from the fuel cell, wherein the oxidation catalytic converter (12) is arranged annularly around the cylindrical reformer catalytic converter (11). According to the invention, the gas paths of the oxidation catalytic converter (12) and of the reformer catalytic converter (11) are separated by a metal pipe (13) that accommodates the reformer catalytic converter (11), wherein the metal pipe (13) has a sleeve (14), which forms a housing for the reformer catalytic converter (11), and an inner pipe (15), which forms the inner wall of the annular oxidation catalytic converter (12).

Description

Katalysatoreinheit für ein Hochtemperatur-Brennstoffzellensystem  Catalyst unit for a high temperature fuel cell system
Die Erfindung betrifft eine Katalysatoreinheit für ein Hochtemperatur- Brennstoffzellensystem mit einem Reformerkatalysator zur Aufbereitung eines Kraftstoffs für die Brennstoffzelle und einen Oxidationskatalysator für die The invention relates to a catalyst unit for a high-temperature fuel cell system with a reforming catalyst for treating a fuel for the fuel cell and an oxidation catalyst for the
Abgasnachbehandlung der Brennstoffzelle, wobei der Oxidationskatalysator ringförmig um den zylindrisch ausgeführten Reformerkatalysator angeordnet ist. Exhaust gas aftertreatment of the fuel cell, wherein the oxidation catalyst is arranged annularly around the cylindrically designed reforming catalyst.
Die oben beschriebene Katalysatoreinheit kann beispielsweise in einer kompakten Energieerzeugungseinheit (Auxiliary Power Unit APU) eines Kraftfahrzeuges zum Einsatz kommen, wo sie zur Bereitstellung von elektrischer und thermischer Energie dient. . The catalyst unit described above can be used, for example, in a compact power unit (APU) of a motor vehicle, where it serves to provide electrical and thermal energy. ,
So ist beispielsweise aus der AT 502 131 Bl eine Katalysatoreinheit für ein For example, from AT 502 131 Bl a catalyst unit for a
Hochtemperatur-Brennstoffzellensystem bekannt, bei welchem ein zylindrischer Reformerkatalysator in einen Oxidationskatalysator eingebaut ist. Dabei ist in einer Brennkammer für einen Flammenbrenner ein zylindrischer Reformerkatalysator angeordnet, der von einem Oxidationskatalysator ringförmig umfasst wird. Die nicht verbrauchten Brennstoffbestandteile des Anodenabgases werden zusammen mit dem Kathodenabgas in die Brennkammer geführt und im Oxidationskatalysator nachbehandelt. Die gasförmigen Produkte nach der katalytischen Umsetzung gelangen über randseitige Öffnungen des Oxidationskatalysators in eine High-temperature fuel cell system is known in which a cylindrical reforming catalyst is incorporated in an oxidation catalyst. In this case, a cylindrical reforming catalyst is arranged in a combustion chamber for a flame burner, which is annularly surrounded by an oxidation catalyst. The unused fuel components of the anode exhaust gas are fed together with the cathode exhaust gas into the combustion chamber and post-treated in the oxidation catalyst. The gaseous products after the catalytic conversion reach via edge-side openings of the oxidation catalyst in a
Ringkammer und verlassen unter Abgabe von Wärme an einem Plattenwärmetauscher die Energieerzeugungseinheit. Ring chamber and leave with the release of heat to a plate heat exchanger, the power generation unit.
Aus der EP 2 255 872 A2 ist ein Oxidationskatalysator mit mehreren From EP 2 255 872 A2 is an oxidation catalyst with several
Reaktionszonen bekannt. Die zu behandelnden Gase strömen zunächst durch einen zylindrischen, inneren Katalysator, werden dann umgelenkt und im Gegenstrom in einen ringförmigen, äußeren Katalysatorbereich geführt. Die beiden Bereiche sind durch eine zylindrische Trennwand getrennt. Sowohl der innere Katalysator, als auch der äußere Katalysator weisen ein metallisches Trägersubstrat (mash layer bzw. honeycomb layer) für die katalytische Substanz auf. Die dargestellte, serielle Hintereinanderschaltung mehrerer Oxidationsstufen eines Oxidationskatalysators soll den Wirkungsgrad der Vorrichtung erhöhen. Aufgabe der Erfindung ist es, eine Katalysatoreinheit für ein Hochtemperatur- Brennstoffzellensystem der eingangs genannten Art derart weiterzubilden, dass eine kompakte Baueinheit, insbesondere für die Anwendung in einer APU gegeben ist, wobei Verbesserungen beim Wärmeübergang sowie bei der Wartung und Pflege der Einheit erzielt werden sollen. Reaction zones known. The gases to be treated initially flow through a cylindrical, inner catalyst, are then deflected and passed in countercurrent to an annular, outer catalyst region. The two areas are separated by a cylindrical partition. Both the inner catalyst and the outer catalyst have a metallic carrier (mash) layer for the catalytic substance. The illustrated, series connection of several oxidation stages of an oxidation catalyst to increase the efficiency of the device. The object of the invention is to develop a catalyst unit for a high-temperature fuel cell system of the type mentioned in such a way that a compact unit, especially for use in an APU is given, with improvements in heat transfer and in the maintenance and care of the unit to be achieved ,
Diese Aufgabe wird erfindungsgemäß dadurch gelöst, dass die Gaspfade des This object is achieved in that the gas paths of the
Oxidationskatalysators und des Reformerkatalysators durch ein den Oxidation catalyst and the reforming catalyst by a the
Reformerkatalysator aufnehmendes Metallrohr getrennt sind, wobei das Metallrohr eine Hülse aufweist, die ein Gehäuse für den Reformerkatalysator bildet, sowie ein Innenrohr, das die Innenwand des ringförmigen Oxidationskatalysators bildet. The catalyst tube receiving reforming catalyst metal tube are separated, wherein the metal tube has a sleeve which forms a housing for the reforming catalyst, and an inner tube which forms the inner wall of the annular oxidation catalyst.
Insbesondere ist vorgesehen, dass der Reformerkatalysator austauschbar in den ringförmigen Oxidationskatalysator einsetzbar ist. Trotz kompakter Bauform sind somit beide Katalysatoren in voneinander unabhängigen Gehäusen fixiert. Der Reformerkatalysator kann somit bei Bedarf auf einfache Weise ausgewechselt werden. In particular, it is provided that the reforming catalyst is exchangeable used in the annular oxidation catalyst. Despite their compact design, both catalysts are thus fixed in independent housings. The reforming catalyst can thus be easily replaced if necessary.
Um den Wärmeaustausch innerhalb der Katalysatoreinheit zu beschleunigen und zu optimieren ist erfindungsgemäß vorgesehen, dass der Oxidationskatalysator und/oder der Reformerkatalysator einen metallischen Katalysatorträger aufweisen, wobei die Hülse mit dem Katalysatorträger des Reformerkatalysators und das Innenrohr mit dem Katalysatorträger des Oxidationskatalysators in thermischem Kontakt stehen. In order to accelerate and optimize the heat exchange within the catalyst unit, it is provided according to the invention that the oxidation catalyst and / or the reforming catalyst have a metallic catalyst carrier, wherein the sleeve is in thermal contact with the catalyst carrier of the reforming catalyst and the inner tube with the catalyst carrier of the oxidation catalyst.
Besonders vorteilhaft ist es, wenn der Katalysatorträger des Oxidationskatalysators und der Katalysatorträger des Reformerkatalysators durch Schweißen mit den jeweils benachbarten Teilen des Metallrohrs verbunden sind. Durch direktes It is particularly advantageous if the catalyst support of the oxidation catalyst and the catalyst support of the reforming catalyst are connected by welding to the respectively adjacent parts of the metal pipe. By direct
Anschweißen der Substrate im Gehäuse des Reformerkatalysators bzw. des Welding of the substrates in the housing of the reforming catalyst or the
Oxidationskatalysators kann eine sonst übliche Dichtmatte entfallen, die den Oxidation catalyst can account for a conventional sealing mat, the
Wärmeaustausch behindert. Ein besonderer Vorteil dieser Ausgestaltung liegt darin, dass durch die verbesserte Wärmeleitfähigkeit das Temperaturprofil der Heat exchange hindered. A particular advantage of this embodiment is that due to the improved thermal conductivity of the temperature profile of the
Katalysatoreinheit (axial und radial) homogenisiert werden kann. Durch die verbesserte Wärmeableitung können insbesondere heiße Zonen (hot spots) in den beiden Katalysatoren verhindert werden. Gemäß einer Ausführungsvariante der Erfindung kann das eingangs des Reformerkatalysators angeordnete Gasverteilergehäuse (Reformermanifold) einen Ringraum aufweisen, in welchen die Zuleitung für das aufzubereitende Kraftstoff- Gas-Gemisch einmündet, wobei ausgehend vom Ringraum radiale Catalyst unit (axial and radial) can be homogenized. The improved heat dissipation in particular hot zones (hot spots) can be prevented in the two catalysts. According to one embodiment variant of the invention, the gas distributor housing (reformer manifold) arranged at the beginning of the reforming catalyst can have an annular space into which the supply line for the fuel-gas mixture to be treated opens, starting radially from the annular space
Zugangsöffnungen vom Ringraum zur Eintrittsfläche des Reformerkatalysators angeordnet sind. Durch diese Maßnahme wird eine Homogenisierung des Gasstroms durch den Katalysator erreicht. Access openings are arranged from the annular space to the inlet surface of the reforming catalyst. By this measure, a homogenization of the gas flow through the catalyst is achieved.
Gemäß einer weiteren Ausführungsvariante des Gasverteilergehäuses kann der axiale Abstand a des tangentialen Einlasses der Zuleitung für das Kraftstoff-Gas- Gemisch von der Eintrittsfläche des Reformerkatalysators zum Durchmesser D des Reformerkatalysators ein Verhältnis a : D im Bereich von 0,2 bis 1, vorzugsweise von 0,3 bis 0,6, aufweisen, wodurch sich eine gewünschte Ringströmung According to a further embodiment variant of the gas distributor housing, the axial distance a of the tangential inlet of the supply line for the fuel-gas mixture from the inlet surface of the reforming catalyst to the diameter D of the reforming catalyst can have a ratio a: D in the range from 0.2 to 1, preferably from 0 , 3 to 0.6, resulting in a desired ring flow
eingangsseitig des Reformerkatalysators etabliert. Der tangentiale Einlass kann in einen zylindrischen oder kegelstumpfförmigen Bereich des Gasverteilergehäuses einmünden. established on the input side of the reforming catalyst. The tangential inlet may open into a cylindrical or frusto-conical region of the gas distributor housing.
Die Erfindung wird im Folgenden anhand von zum Teil schematischen Zeichnungen näher erläutert. Es zeigen : The invention will be explained in more detail below with reference to partly schematic drawings. Show it :
Fig. 1 eine erfindungsgemäße Katalysatoreinheit für ein Hochtemperatur- Brennstoffzellensystem in einer dreidimensionalen, teilweise aufgeschnittenen Darstellung, 1 shows a catalyst unit according to the invention for a high-temperature fuel cell system in a three-dimensional, partially cutaway representation,
Fig. 2 eine schematische Darstellung des Funktionsprinzips und der Fig. 2 is a schematic representation of the principle of operation and the
Einbaulage der Katalysatoreinheit gemäß Fig. 1,  Installation position of the catalyst unit according to FIG. 1,
Fig. 3 eine Schnittdarstellung der Katalysatoreinheit gemäß Fig. 1, 3 is a sectional view of the catalyst unit of FIG. 1,
Fig. 4 eine Ausführungsvariante der Katalysatoreinheit gemäß Fig. 1 in einer dreidimensionalen Darstellung. Fig. 4 shows a variant of the catalyst unit of FIG. 1 in a three-dimensional representation.
Fig. 5 eine erste Ausführungsvariante eines Gasverteilergehäuses Fig. 5 shows a first embodiment of a gas distributor housing
(Reformermanifold) für den Reformerkatalysator der Katalysatoreinheit in einer Schnittdarstellung gemäß Linie V-V in Fig. 6,  (Reformermanifold) for the reformer catalyst of the catalyst unit in a sectional view taken along line V-V in Fig. 6,
Fig. 6 das Gasverteilergehäuse gemäß Fig. 5 in einer axialen Draufsicht, 6 shows the gas distributor housing according to FIG. 5 in an axial plan view, FIG.
sowie Fig. 7 eine zweite Ausführungsvariante eines Gasverteilergehäusessuch as Fig. 7 shows a second embodiment of a gas distributor housing
(Reformermanifold) für den Reformerkatalysator der Katalysatoreinheit in einem Axialschnitt. (Reformermanifold) for the reforming catalyst of the catalyst unit in an axial section.
In Fig. 1 ist eine erfindungsgemäße Katalysatoreinheit 10 für ein hier nicht weiter dargestelltes Hochtemperatur-Brennstoffzellensystem mit einem zylindrischen Reformerkatalysator 11 und einen den Reformerkatalysator ringförmig FIG. 1 shows a catalyst unit 10 according to the invention for a high-temperature fuel cell system (not further illustrated here) with a cylindrical reforming catalyst 11 and a reforming catalyst annular
umschließenden Oxidationskatalysator 12 skizziert. Der Reformerkatalysator 11 dient zur Aufbereitung des Kraftstoffs für die Brennstoffzelle BZ (siehe Fig. 2), der mit einem Oxidationsmittel über die Zuleitung 23 zugeführt und mit einem delineating oxidizing catalyst 12 outlined. The reforming catalyst 11 is used for the preparation of the fuel for the fuel cell BZ (see Fig. 2), which is supplied with an oxidizing agent via the supply line 23 and with a
kegelstumpfförmigen Gasverteilergehäuse bzw. Reformermanifold 24 möglichst homogen über die Eintrittsfläche des Reformerkatalysators 11 verteilt wird. Der Oxidationskatalysator 12 dient der Abgasnachbehandlung eines Starterbrenners und des Brennstoffzellensystems. frustoconical gas distributor housing or Reformermanifold 24 is distributed as homogeneously as possible over the inlet surface of the reforming catalyst 11. The oxidation catalyst 12 is used for exhaust aftertreatment of a starter burner and the fuel cell system.
In der dargestellten Ausführungsvariante sind die Gaspfade des In the illustrated embodiment, the gas paths of the
Oxidationskatalysators 12 und des Reformerkatalysators 11 durch ein den Oxidation catalyst 12 and the reforming catalyst 11 by a the
Reformerkatalysator 11 aufnehmendes Metallrohr 13 getrennt, das zweiteilig gestaltet ist und eine Hülse 14 aufweist, die ein Gehäuse für den Reformer catalyst 11 receiving metal tube 13 separated, which is designed in two parts and a sleeve 14 which has a housing for the
Reformerkatalysator 11 bildet, sowie ein Außenrohr 15, das die Innenwand des ringförmigen Oxidationskatalysators 12 bildet. Der Reformerkatalysator 11 kann somit austauschbar in den ringförmigen Oxidationskatalysator 12 eingesetzt werden. Reforming catalyst 11 forms, as well as an outer tube 15, which forms the inner wall of the annular oxidation catalyst 12. The reforming catalyst 11 can thus be used interchangeably in the annular oxidation catalyst 12.
Der Oxidationskatalysator 12 und/oder der Reformerkatalysator 11 weisen bevorzugt einen metallischen Katalysatorträger 16, 17 auf, wobei die Hülse 14 des Metallrohrs 13 mit dem Katalysatorträger 16 des Reformerkatalysators 11 und das Außenrohr 15 mit dem Katalysatorträger 17 des Oxidationskatalysators 12 in thermischem Kontakt steht. Damit können für den Wärmeübergang weit bessere Werte erzielt werden, als bei der Verwendung keramischer Substrate, die The oxidation catalyst 12 and / or the reforming catalyst 11 preferably have a metallic catalyst carrier 16, 17, wherein the sleeve 14 of the metal tube 13 is in thermal contact with the catalyst carrier 16 of the reforming catalyst 11 and the outer tube 15 with the catalyst carrier 17 of the oxidation catalyst 12. Thus, far better values for the heat transfer can be achieved than with the use of ceramic substrates, the
üblicherweise mit einer Dichtmatte zum Gehäuse abgedichtet werden. Usually sealed with a sealing mat to the housing.
Bevorzugt besteht der Katalysatorträger 17 des Oxidationskatalysators 12 und der Katalysatorträger 16 des Reformerkatalysators 11 aus einem metallischen Preferably, the catalyst support 17 of the oxidation catalyst 12 and the catalyst support 16 of the reforming catalyst 11 consists of a metallic
Drahtgeflecht oder einer metallischen Lamellenstruktur, die durch Schweißen mit den jeweils benachbarten Teilen 14, 15 des Metallrohrs 13 verbunden sind. Die Hülse 14 des Reformerkatalysators 11 kann mittels einer Spielpassung, beispielsweise im Bereich von 0,2 mm bis 1,5 mm, auswechselbar in das Innenrohr 15 bzw. die Innenwand des ringförmigen Oxidationskatalysators 12 eingefügt werden. Dabei ist im Endbereich der Hülse 14 auf Seiten des Wire mesh or a metallic lamellar structure, which are connected by welding to the respective adjacent parts 14, 15 of the metal tube 13. The sleeve 14 of the reforming catalyst 11 can be interchangeable inserted into the inner tube 15 and the inner wall of the annular oxidation catalyst 12 by means of a clearance fit, for example in the range of 0.2 mm to 1.5 mm. It is in the end of the sleeve 14 on the part of the
Gasverteilungsgehäuses bzw. Reformermanifolds 24 ein Dichtelement 19 Gas distribution housing or Reformermanifolds 24 a sealing element 19th
angeordnet. arranged.
Erfindungsgemäß weist die Hülse 14 des Reformerkatalysators 11 oder das According to the invention, the sleeve 14 of the reforming catalyst 11 or the
Innenrohr 15 des Oxidationskatalysators 12 einen Dichtflansch 18 auf, wobei zwischen dem Dichtflansch 18 und dem Ende des Innenrohrs 15 in einer Inner tube 15 of the oxidation catalyst 12, a sealing flange 18, wherein between the sealing flange 18 and the end of the inner tube 15 in a
entsprechenden Ausnehmung eine Ringdichtung 25, beispielsweise eine Quellmatte, vorgesehen ist. Für Montage- und Demontagezwecke können an der Hülse 14 des Reformerkatalysators 11 Eingriffselemente oder Eingriffsöffnungen 20 für ein corresponding recess a ring seal 25, for example, a swelling mat, is provided. For assembly and disassembly purposes can on the sleeve 14 of the reforming catalyst 11 engaging elements or engaging holes 20 for a
Abzugwerkzeug ausgebildet sein. Pulling tool be formed.
Fig. 2 zeigt in einer schematischen Übersichtsdarstellung die Anordnung der erfindungsgemäßen Katalysatoreinheit 10 samt zylindrischem Reformerkatalysator 11 und ringförmigem Oxidationskatalysator 12 im Verbund mit einem FIG. 2 shows, in a schematic overview, the arrangement of the catalyst unit 10 according to the invention, including the cylindrical reforming catalyst 11 and the annular oxidation catalyst 12 in combination with a
Hochtemperatur-Brennstoffzellensystem BZ mit der Anodenseite A und der High-temperature fuel cell system BZ with the anode side A and the
Kathodenseite K. Cathode side K.
Der Kraftstoff F wird während des Startzyklus mit Hilfe einer Kraftstoffpumpe 35 einem Starterbrenner 26 zugeführt, dessen Abgase in den ringförmigen The fuel F is supplied during the starting cycle by means of a fuel pump 35 to a starter burner 26, the exhaust gases in the annular
Oxidationskatalysator 12 geführt werden und den zentral angeordneten Oxidation catalyst 12 are guided and arranged centrally
Reformerkatalysator 11 aufheizen. Weiters wird der Kraftstoff F mittels Heat reforming catalyst 11. Furthermore, the fuel F by means
Kraftstoffpumpe 36 der Verdampfungseinheit 37 zugeführt und in das Anodenabgas der Rezirkulationsleitung 27 eingebracht, sowie zusammen mit dem benötigten Oxidationsmittel, beispielweise Luft L, mittels Verdichter 28 dem Fuel pump 36 of the evaporation unit 37 is supplied and introduced into the anode exhaust gas of the recirculation line 27, and together with the required oxidant, for example, air L, by means of compressor 28 the
Gasverteilergehäuse bzw. Reformermanifold 24 des Reformerkatalysators 11 zugeführt. Gas manifold housing or Reformermanifold 24 of the reforming catalyst 11 is supplied.
Der Verdichter 29 dient für die Zufuhr des Oxidationsmittels (z.B. Luft L) zur The compressor 29 serves to supply the oxidizing agent (e.g., air L) to the
Kathodenseite K des Brennstoffzellensystems BZ, wobei das Oxidationsmittel über einen Wärmetauscher 38 geführt wird, der von den Abgasen des Cathode side K of the fuel cell system BZ, wherein the oxidizing agent is passed through a heat exchanger 38, the exhaust gases of the
Oxidationskatalysators 12 mit Abwärme beaufschlagt wird. In der Startphase wird auch der Starterbrenner 26 über den Verdichter 29 mit der benötigten Luft versorgt. Oxidation catalyst 12 is subjected to waste heat. In the starting phase will also the starter burner 26 supplied via the compressor 29 with the required air.
Fig. 3 zeigt eine Variante der erfindungsgemäßen Katalysatoreinheit 10 in einer vergrößerten Schnittdarstellung. Das Metallrohr 13, das die Gaspfade des Fig. 3 shows a variant of the catalyst unit 10 according to the invention in an enlarged sectional view. The metal tube 13, which is the gas paths of the
Oxidationskatalysators 12 und des Reformerkatalysators 11 trennt, besteht im Wesentlichen aus der Hülse 14, die ein Gehäuse für den Reformerkatalysator 11 bildet, sowie aus dem Innenrohr 15, das die Innenwand des ringförmigen Oxidation catalyst 12 and the reforming catalyst 11 separates, consists essentially of the sleeve 14, which forms a housing for the reforming catalyst 11, and from the inner tube 15, which is the inner wall of the annular
Oxidationskatalysators 12 bildet. Der umlaufende Dichtflansch 18 weist hier eine Ringdichtung 25 zur Stirnseite des Innenrohrs 15 auf. Oxidation catalyst 12 forms. The circumferential sealing flange 18 here has a ring seal 25 to the end face of the inner tube 15.
Fig. 4 zeigt eine Ausführungsvariante der Vorrichtung gemäß Fig. 1, bei welcher sowohl der Oxidationskatalysator 12, als auch der Reformerkatalysator 11 einen metallischen Katalysatorträger 16, 17 aufweisen, wobei die Gaspfade der beiden Katalysatoren 11, durch ein den Reformerkatalysator 11 aufnehmendes Metallrohr 13 getrennt sind, welches mit dem Katalysatorträger 17 des Oxidationskatalysators 12 und dem Katalysatorträger 16 des Reformerkatalysators 11, beispielsweise durch Schweißen, in thermischem Kontakt steht. 1, in which both the oxidation catalytic converter 12 and the reforming catalytic converter 11 have a metallic catalyst carrier 16, 17, the gas paths of the two catalytic converters 11 being separated by a metal tube 13 accommodating the reforming catalyst 11 are, which is in thermal contact with the catalyst support 17 of the oxidation catalyst 12 and the catalyst support 16 of the reforming catalyst 11, for example by welding.
In den Fig. 5 bis Fig. 7 sind zwei Ausführungsvarianten für das Gasverteilergehäuse 24 dargestellt, das eingangsseitig des Reformerkatalysators 11 angeordnet ist. Es dient dazu, das aufzubereitende Kraftstoff-Gas-Gemisch über die gesamte FIGS. 5 to 7 show two alternative embodiments for the gas distributor housing 24, which is arranged on the input side of the reforming catalytic converter 11. It serves to process the fuel-gas mixture over the whole
Eintrittsfläche 30 des Reformerkatalysators 11 zu verteilen, wobei die Zuleitung 23 für das Kraftstoff-Gas-Gemisch radial oder tangential in Bezug auf die Achse 11' des Reformerkatalysators 11 in das Gasverteilergehäuse 24 einmündet. Dispense inlet surface 30 of the reforming catalyst 11, wherein the feed line 23 for the fuel-gas mixture opens radially or tangentially with respect to the axis 11 'of the reforming catalyst 11 in the gas distributor housing 24.
Bei der in den Fig. 5 und Fig. 6 dargestellten Ausführungsvariante weist das In the embodiment variant shown in FIGS. 5 and 6, the
Gasverteilergehäuse 24 einen Ringraum 32 auf, in welchen die Zuleitung 23 für das Kraftstoff-Gas-Gemisch beispielsweise radial einmündet, wobei ausgehend vom Ringraum 32 radiale Zugangsöffnungen 33 in Form eines Lochkranzes vom Gas distributor housing 24 an annular space 32, in which the supply line 23 for the fuel-gas mixture, for example, opens radially, starting from the annular space 32 radial access openings 33 in the form of a perforated ring from
Ringraum 32 zur Eintrittsfläche 30 des Reformerkatalysators 11 angeordnet sind, sodass der Reformerkatalysators 11 möglichst gleichmäßig mit dem Gemisch aus Anodenabgas, verdampftem Kraftstoff und Oxidationsmittel beaufschlagt wird. Das Reformermanifold gemäß Fig. 5 und Fig. 6 zeichnet sich durch eine kompakte Bauweise mit geringer axialer Bauhöhe aus. Im Rohr 34 kann eine Messeinrichtung, z.B. ein Temperatursensor, in den Ringraum 32 eingebracht werden (siehe Fig. 6). Der Oxidationskatalysator 12 weist eine rohrförmige Außenwand 21 mit Abgas- Auslassöffnungen 22 auf. Die Abgas-Auslassöffnungen 22 befinden sich dabei in einem über den Katalysatorträger 17 ragenden Bereich (siehe dazu auch Fig. 1 und 4). Annular space 32 are arranged to the inlet surface 30 of the reforming catalyst 11, so that the reforming catalyst 11 is applied as uniformly as possible with the mixture of anode exhaust gas, vaporized fuel and oxidant. The Reformermanifold of FIG. 5 and Fig. 6 is characterized by a compact design with low axial height. In the pipe 34, a measuring device, for example a temperature sensor, can be introduced into the annular space 32 (see FIG. 6). The oxidation catalyst 12 has a tubular outer wall 21 with exhaust outlet openings 22. In this case, the exhaust gas outlet openings 22 are located in an area protruding beyond the catalyst carrier 17 (see also FIGS. 1 and 4).
In der Ausführungsvariante gemäß Fig. 7 weist der axiale Abstand a des In the embodiment according to FIG. 7, the axial distance a of
tangentialen Einlasses 31 der Zuleitung 23 für das Kraftstoff-Gas-Gemisch von der Eintrittsfläche 30 des Reformerkatalysators 11 zum Durchmesser D des Tangential inlet 31 of the supply line 23 for the fuel-gas mixture from the inlet surface 30 of the reforming catalyst 11 to the diameter D of
Reformerkatalysators 11 ein Verhältnis a : D im Bereich von 0,2 bis 1, Reformer catalyst 11 a ratio a: D in the range of 0.2 to 1,
vorzugsweise von 0,3 bis 0,6, auf, sodass sich eine optimale Ringströmung im Inneren des Reformermanifolds 24 ausbilden kann, die eine homogene Preferably, from 0.3 to 0.6, so that an optimal ring flow can form inside the Reformermanifolds 24, which is a homogeneous
Gasverteilung an der Eintrittsfläche 30 des Reformerkatalysators 11 erzeugt. Gas distribution at the entrance surface 30 of the reforming catalyst 11 is generated.
Vorteile sind ein kompaktes Design und geringe Druckverluste. Advantages are a compact design and low pressure losses.
Bevorzugt kann das Gasverteilergehäuse 24 einstückig mit der Innenwand 15 des ringförmigen Oxidationskatalysators 12 hergestellt oder durch Schweißen mit dieser verbunden sein. Preferably, the gas distributor housing 24 may be integrally formed with the inner wall 15 of the annular oxidation catalyst 12 or connected thereto by welding.

Claims

PATE NTAN S PRÜ C H E PATE NTAN S CHECK
1. Katalysatoreinheit (10) für ein Hochtemperatur-Brennstoffzellensystem mit einem Reformerkatalysator (11) zur Aufbereitung eines Kraftstoffs für die Brennstoffzelle und einen Oxidationskatalysator (12) für die A catalyst unit (10) for a high-temperature fuel cell system having a reforming catalyst (11) for treating a fuel for the fuel cell and an oxidation catalyst (12) for the
Abgasnachbehandlung der Brennstoffzelle, wobei der Oxidationskatalysator (12), insbesondere ringförmig, um den, insbesondere zylindrisch  Exhaust gas aftertreatment of the fuel cell, wherein the oxidation catalyst (12), in particular annular, to the, in particular cylindrical
ausgeführten, Reformerkatalysator (11) angeordnet ist,  arranged, reformer catalyst (11) is arranged,
dadurch gekennzeichnet, dass  characterized in that
die Gaspfade des Oxidationskatalysators (12) und des Reformerkatalysators (11) durch ein den Reformerkatalysator (11) aufnehmendes Rohr (13), insbesondere ein Metallrohr, insbesondere gasdicht, getrennt sind,  the gas paths of the oxidation catalytic converter (12) and of the reforming catalytic converter (11) are separated by a tube (13) receiving the reforming catalytic converter (11), in particular a metal tube, in particular gas-tight
wobei das Rohr (13) eine Hülse (14) aufweist, die ein Gehäuse für den  the tube (13) having a sleeve (14) defining a housing for the
Reformerkatalysator (11) bildet, sowie ein Innenrohr (15), das die Innenwand des, insbesondere ringförmigen, Oxidationskatalysators (12) bildet.  Forming reformer catalyst (11), and an inner tube (15) which forms the inner wall of the, in particular annular, oxidation catalyst (12).
2. Katalysatoreinheit (10) nach Anspruch 1, dadurch gekennzeichnet, dass der Reformerkatalysator (11) austauschbar in den Oxidationskatalysator (12) einsetzbar ist. Second catalyst unit (10) according to claim 1, characterized in that the reforming catalyst (11) is interchangeable in the oxidation catalyst (12) can be used.
3. Katalysatoreinheit (10) nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass der Oxidationskatalysator (12) und/oder der Reformerkatalysator (11) einen, insbesondere metallischen, Katalysatorträger (16, 17) aufweisen, wobei die Hülse (14) mit dem Katalysatorträger (16) des Reformerkatalysators (11) und das Innenrohr (15) mit dem Katalysatorträger (17) des 3. catalyst unit (10) according to claim 1 or 2, characterized in that the oxidation catalyst (12) and / or the reforming catalyst (11) one, in particular metallic, catalyst carrier (16, 17), wherein the sleeve (14) with the Catalyst support (16) of the reforming catalyst (11) and the inner tube (15) with the catalyst support (17) of the
Oxidationskatalysators (12) in Kontakt stehen, insbesondere in thermisch leitenden Kontakt stehen.  Oxidation catalyst (12) are in contact, in particular in thermally conductive contact.
4. Katalysatoreinheit (10) nach Anspruch 3, dadurch gekennzeichnet, dass der Katalysatorträger (17) des Oxidationskatalysators (12) und der 4. catalyst unit (10) according to claim 3, characterized in that the catalyst carrier (17) of the oxidation catalyst (12) and the
Katalysatorträger (16) des Reformerkatalysators (11) stoffschlüssig,  Catalyst support (16) of the reforming catalyst (11) cohesively,
insbesondere durch Schweißen, Löten oder Kleben, mit den jeweils  in particular by welding, soldering or gluing, with the respectively
benachbarten Teilen des Rohrs (13) verbunden sind.  adjacent parts of the tube (13) are connected.
5. Katalysatoreinheit (10) nach Anspruch 3 oder 4, dadurch gekennzeichnet, dass der Katalysatorträger (17) des Oxidationskatalysators (12) und der Katalysatorträger (16) des Reformerkatalysators (11) wenigstens teilweise oder vollständig aus einem, insbesondere metallischen, Geflecht, insbesondere Drahtgeflecht, oder einer, insbesondere metallischen, Lamellenstruktur bestehen. 5. Catalyst unit (10) according to claim 3 or 4, characterized in that the catalyst carrier (17) of the oxidation catalyst (12) and the Catalyst support (16) of the reforming catalyst (11) consist at least partially or completely of a, in particular metallic, braid, in particular wire mesh, or one, in particular metallic, lamellar structure.
6. Katalysatoreinheit (10) nach einem der Ansprüche 1 bis 5, dad u rch 6. catalyst unit (10) according to one of claims 1 to 5, dad u rch
ge ken nze ich net, dass die Hülse (14) des Reformerkatalysators (11) mittels einer Spielpassung, beispielsweise im Bereich von 0,2 mm bis 1,5 mm, in das Innenrohr (15) des Oxidationskatalysators (12) eingefügt ist.  I net net, that the sleeve (14) of the reforming catalyst (11) by means of a clearance, for example in the range of 0.2 mm to 1.5 mm, in the inner tube (15) of the oxidation catalyst (12) is inserted.
7. Katalysatoreinheit (10) nach einem der Ansprüche 1 bis 6, da d u rch 7. Catalyst unit (10) according to any one of claims 1 to 6, since d u rch
geken nzeichnet, dass die Hülse (14) des Reformerkatalysators (11) oder das Innenrohr (15) des Oxidationskatalysators (12) einen Dichtflansch ( 18) aufweist, und zwischen dem Dichtflansch (18) und dem Ende des Innenrohrs (15) eine Ringdichtung (25), beispielsweise eine Quellmatte, vorgesehen ist.  that the sleeve (14) of the reforming catalytic converter (11) or the inner tube (15) of the oxidation catalytic converter (12) has a sealing flange (18), and between the sealing flange (18) and the end of the inner tube (15) an annular seal ( 25), for example a swelling mat, is provided.
8. Katalysatoreinheit (10) nach einem der Ansprüche 1 bis 7, da d u rch 8. catalyst unit (10) according to any one of claims 1 to 7, since d u rch
geke n nzei ch net, dass an der Hülse ( 14) des Reformerkatalysators (11) Eingriffselemente oder Eingriffsöffnungen (20), insbesondere für ein  net that on the sleeve (14) of the reforming catalyst (11) engaging elements or engagement openings (20), in particular for a
Abzugwerkzeug, ausgebildet sind.  Trigger tool, are formed.
9. Katalysatoreinheit (10) nach einem der Ansprüche 1 bis 8, da d u rch 9. catalyst unit (10) according to any one of claims 1 to 8, since d u rch
ge ken nze ich net, dass der Oxidationskatalysator (12) eine rohrförmige Außenwand (21) mit Abgas-Auslassöffnungen (22) in einem über den  I net net, that the oxidation catalyst (12) has a tubular outer wall (21) with exhaust outlet openings (22) in one over the
Katalysatorträger (17) ragenden Bereich aufweist.  Catalyst support (17) has projecting region.
10. Katalysatoreinheit (10) für ein Hochtemperatur-Brennstoffzellensystem mit einem Reformerkatalysator (11) zur Aufbereitung eines Kraftstoffs für die Brennstoffzelle und einen Oxidationskatalysator (12) für die Abgasbehandlung der Brennstoffzelle, wobei der Oxidationskatalysator (12), insbesondere ringförmig, um den, insbesondere zylindrisch ausgeführten, 10. Catalyst unit (10) for a high-temperature fuel cell system with a reforming catalyst (11) for processing a fuel for the fuel cell and an oxidation catalyst (12) for the exhaust gas treatment of the fuel cell, wherein the oxidation catalyst (12), in particular annularly to the, in particular cylindrically executed,
Reformerkatalysator ( 11) angeordnet ist,  Reformer catalyst (11) is arranged,
dad u rch ge ken nzei ch net, dass  I can not say that
sowohl der Oxidationskatalysator (12), als auch der Reformerkatalysator (11) einen, wenigstens abschnittsweise insbesondere metallischen,  both the oxidation catalyst (12), and the reforming catalyst (11) one, at least in sections, in particular metallic,
Katalysatorträger ( 16, 17) aufweisen, wobei die Gaspfade des  Catalyst support (16, 17), wherein the gas paths of the
Oxidationskatalysators (12) und des Reformerkatalysators (11) durch ein den Reformerkatalysator ( 11) aufnehmendes Rohr (13), insbesondere ein Oxidation catalyst (12) and the reforming catalyst (11) by a den Reformer catalyst (11) receiving tube (13), in particular a
Metallrohr (13), getrennt sind, welches mit dem Katalysatorträger (17) des Oxidationskatalysators (12) und dem Katalysatorträger (16) des  Metal tube (13) are separated, which with the catalyst support (17) of the oxidation catalyst (12) and the catalyst support (16) of the
Reformerkatalysators (11) in Kontakt steht, insbesondere in thermisch leitenden Kontakt.  Reforming catalyst (11) is in contact, especially in thermally conductive contact.
11. Katalysatoreinheit (10) nach einem der vorhergehenden Ansprüche, dad u rch g eken nzei ch net, dass der Katalysatorträger (17) des Oxidationskatalysators (12) und der Katalysatorträger (16) des Reformerkatalysators (11) 11. Catalyst unit according to claim 1, characterized in that the catalyst support (17) of the oxidation catalytic converter (12) and the catalyst support (16) of the reforming catalytic converter (11)
stoffschlüssig, insbesondere durch Schweißen, Löten oder Kleben, mit dem Rohr (13) verbunden sind.  cohesively, in particular by welding, soldering or gluing, with the tube (13) are connected.
12. Katalysatoreinheit (10) nach einem der Ansprüche 1 bis 11, d a d u rch 12. catalyst unit (10) according to one of claims 1 to 11, d a d u rch
ge ken nzeich net, dass der Reformerkatalysator (11) eingangsseitig ein Gasverteilergehäuse (24) aufweist, dass das aufzubereitende Kraftstoff-Gas- Gemisch über eine Eintrittsfläche (30), insbesondere die gesamte  ge ken nzeich net, that the reforming catalyst (11) on the input side a gas distributor housing (24), that the fuel-gas mixture to be reprocessed via an inlet surface (30), in particular the entire
Eintrittsfläche (30), des Reformerkatalysators (11) verteilt, wobei die  Entrance surface (30), the reforming catalyst (11) distributed, wherein the
Zuleitung (23) für das Kraftstoff-Gas-Gemisch im Wesentlichen radial oder im Wesentlichen tangential in Bezug auf die Achse (11') des Reformerkatalysators (11) in das Gasverteilergehäuse (24) einmündet.  Supply line (23) for the fuel-gas mixture opens substantially radially or substantially tangentially with respect to the axis (11 ') of the reforming catalyst (11) in the gas distributor housing (24).
13. Katalysatoreinheit (10) nach Anspruch 12, dad u rch ge ke n nze i ch net, dass das Gasverteilergehäuse (24) einen Raum (32), insbesondere einen Ringraum (32), aufweist, in welchen die Zuleitung (23) für das Kraftstoff-Gas-Gemisch einmündet, wobei ausgehend vom Raum (32) Zugangsöffnungen (33), insbesondere radiale Zugangsöffnungen (33) vom Raum (32) zur 13. Catalyst unit (10) according to claim 12, characterized in that the gas distributor housing (24) has a space (32), in particular an annular space (32), in which the supply line (23) for the fuel-gas mixture opens, starting from the space (32) access openings (33), in particular radial access openings (33) from the space (32)
Eintrittsfläche (30) des Reformerkatalysators (11) angeordnet sind.  Entry surface (30) of the reforming catalyst (11) are arranged.
14. Katalysatoreinheit (10) nach Anspruch 12 oder 13, d ad u rch 14. Catalyst unit (10) according to claim 12 or 13, ad d u rch
ge ken nzeich net, dass der axiale Abstand a des tangentialen Einlasses (31) der Zuleitung (23) für das Kraftstoff-Gas-Gemisch von der Eintrittsfläche (30) des Reformerkatalysators (11) zum Durchmesser D des Reformerkatalysators (11) ein Verhältnis a : D aufweist und dass dieses Verhältnis vorzugsweise größer ist als 0,2, bevorzugt größer als 0,3 und vorzugsweise kleiner ist als 1 und bevorzugt kleiner ist als 0,6. Katalysatoreinheit (10) nach einem der Ansprüche 12 bis 14, d ad u rch geken nzeich n et, dass das Gasverteilergehäuse (24) mit der Innenwand des, insbesondere ringförmigen, Oxidationskatalysators (12) einstückig hergestellt oder stoffschlüssig, insbesondere durch Kleben, Löten oder Schweißen, verbunden ist. that the axial distance a of the tangential inlet (31) of the feed line (23) for the fuel-gas mixture from the inlet surface (30) of the reforming catalyst (11) to the diameter D of the reforming catalyst (11) is a ratio a : D and that this ratio is preferably greater than 0.2, preferably greater than 0.3 and preferably less than 1 and preferably less than 0.6. Catalyst unit (10) according to any one of claims 12 to 14, d ad u rch nken nzeich n et that the gas distributor housing (24) with the inner wall of the, in particular annular, oxidation catalyst (12) made in one piece or cohesively, in particular by gluing, soldering or Welding, is connected.
PCT/EP2014/000286 2013-02-04 2014-02-04 Catalytic converter units for a high-temperature fuel cell system WO2014117950A1 (en)

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