WO2002085509A1 - Reacteur - Google Patents

Reacteur Download PDF

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Publication number
WO2002085509A1
WO2002085509A1 PCT/US2002/012897 US0212897W WO02085509A1 WO 2002085509 A1 WO2002085509 A1 WO 2002085509A1 US 0212897 W US0212897 W US 0212897W WO 02085509 A1 WO02085509 A1 WO 02085509A1
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WO
WIPO (PCT)
Prior art keywords
reactor
flat plate
integrated reactor
gas
integrated
Prior art date
Application number
PCT/US2002/012897
Other languages
English (en)
Inventor
Richard R. Woods
Kandaswamy Duraiswamy
Jeffrey S. Pickles
Original Assignee
Hydrogen Burner Technology, Inc.
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Hydrogen Burner Technology, Inc. filed Critical Hydrogen Burner Technology, Inc.
Publication of WO2002085509A1 publication Critical patent/WO2002085509A1/fr

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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
    • 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
    • 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
    • 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
    • C01B3/382—Multi-step processes
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F28—HEAT EXCHANGE IN GENERAL
    • F28D—HEAT-EXCHANGE APPARATUS, NOT PROVIDED FOR IN ANOTHER SUBCLASS, IN WHICH THE HEAT-EXCHANGE MEDIA DO NOT COME INTO DIRECT CONTACT
    • F28D9/00—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall
    • 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
    • B01J2219/00074—Controlling the temperature by indirect heating or cooling employing heat exchange fluids
    • B01J2219/00076—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements inside the reactor
    • B01J2219/00085—Plates; Jackets; Cylinders
    • 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
    • B01J2219/02—Apparatus characterised by their chemically-resistant properties
    • B01J2219/025—Apparatus characterised by their chemically-resistant properties characterised by the construction materials of the reactor vessel proper
    • B01J2219/0254—Glass
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J2219/0277—Metal based
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    • B01J2219/02—Apparatus characterised by their chemically-resistant properties
    • B01J2219/025—Apparatus characterised by their chemically-resistant properties characterised by the construction materials of the reactor vessel proper
    • B01J2219/0277—Metal based
    • B01J2219/0281—Metal oxides
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    • B01J2219/0295—Synthetic organic materials
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    • B01J2219/2458—Flat plates, i.e. plates which are not corrugated or otherwise structured, e.g. plates with cylindrical shape
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    • B01J2219/2461—Heat exchange aspects
    • B01J2219/2462—Heat exchange aspects the reactants being in indirect heat exchange with a non reacting heat exchange medium
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2219/2477—Construction materials of the catalysts
    • B01J2219/2479—Catalysts coated on the surface of plates or inserts
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2219/2492—Assembling means
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    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
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    • C01B2203/0244—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being an autothermal reforming step, e.g. secondary reforming processes
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    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0838—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel
    • C01B2203/0844—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
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    • C01B2203/80—Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
    • C01B2203/82—Several process steps of C01B2203/02 - C01B2203/08 integrated into a single apparatus

Definitions

  • the field of the invention is the production of hydrogen-rich reformer gas for use in fuel- cells for the generation of electricity.
  • the present invention is aimed at a simple, inexpensive fuel processor for the production of a hydrogen-rich gas-stream from a feed-gas mixture of hydrocarbon fuel, oxidant, and steam.
  • the present invention uses simple structural elements such as flat plates and square bars to assemble an integrated fuel processor, which combines an Anode Offgas Oxidizer (AGO) and an Auto-Thermal Reactor (ATR) in a single module. Further, the structural elements of the module are arranged so that heat generated by the combustion of the anode off-gas in the AGO is efficiently transferred to the ATR for sustaining the endothermic SMR reaction in the ATR. Further, the structural elements are also arranged so that the sensible heat in the hot reformer gas in the ATR and the sensible heat of the hot oxidized anode off-gas is transferred to the incoming cold feed gas to provide a highly energy-efficient fuel-processor.
  • the single module can be easily made in small flow units and can be easily assembled into multiple module assemblies to satisfy any increase in reformer gas requirements. Thus an almost infinitesimal increase in reformer gas requirement can be accommodated by the use of additional modules.
  • the assembly is also configured so as to provide flow channels for the AGO gas and the ATR gas.
  • the configuration of the assembly is such that these flow channels are separated by common walls which function as heat-transfer surfaces to easily and efficiently transfer heat between the hot combusted AGO gas and the incoming cold ATR feed-gas.
  • the assembly also provides a common wall between the AGO and the ATR through which the hot combusted AGO gas can transfer heat to sustain the endothermic SMR reaction which takes place in the ATR.
  • flat plates and square bars are used to create an integrated reactor module consisting of an AGO, a feed-gas preheater, and an ATR.
  • This embodiment has the advantage that complex punching, shearing, and bending of the plate is not required to create the assembly.
  • Figure 1 shows a single module of an integrated reactor according to the present invention.
  • Figures 2A, 2B, 2C, and 2D show the configuration of the flat plates used to form a single module of the integrated reactor of Fig 1.
  • Fig 3 A, 3B, 3C, and 3D show an exploded view showing the assembly of a single module of an integrated reactor of Fig 1 using the flat plates of Fig 2.
  • Fig 4(a) shows a scaleable integrated reactor using two of the modules shown in Fig 1
  • Fig 4(b) shows a scaleable integrated reactor in another embodiment using two of the modules shown in Fig 1.
  • Fig 5 shows a single module of an integrated reactor according to another embodiment of the present invention.
  • Fig 6 shows an exploded view showing the assembly of a single module of the integrated reactor of Fig 5 using simple structural elements such as flat plates and square bars.
  • Fig. 1 shows a single module 2 of an integrated reactor according to the present invention.
  • Module 2 consists of an Anodizer Offgas Assembly 10 and an Auto-Thermal Reactor Assembly 60, which are separated by a common wall 22, which will be described further below.
  • an AGO reactor is a device within which the unreacted hydrogen-rich fuel-gas from the anode of the fuel is oxidized to water-vapor by reacting with air or oxygen from the cathode side of the fuel-cell to meet regulatory or safety requirements.
  • the hydrogen- rich fuel-cell gas from the anode of the fuel-cell is termed the anode off-gas.
  • the oxygen- depleted air from the cathode of the fuel cell is termed the cathode off-gas.
  • an ATR is a device wherein a mixture of a hydrocarbon fuel, air, and steam is converted to a hydrogen rich reformer gas stream through reaction mechanisms such as catalytic partial oxidation and steam methane reforming.
  • the hydrocarbon fuel is generally a hydrocarbon gas such as methane, propane, and butane. However, other hydrocarbons such as benzene can also be used. Further, mixtures of hydrocarbons similar to those found in liquid fuels such as kerosene or gasoline can also be used. Yet further, oxygenated hydrocarbons such as methanol or ethanol can also be used.
  • An ATR generally consists of a reactor vessel within which is located a CPO catalyst and a SMR catalyst.
  • an advanced SMR catalyst which combines both the CPO and the SMR catalyst functions can also be used instead of the CPO and the SMR catalysts.
  • the material of construction of the ATR's reactor vessel can be a suitable metal such as carbon or stainless steel or any other suitable metallic alloy or even a non-metallic substance such as glass or synthetic composite material.
  • the CPO catalyst is arranged such that the mixture of reactant gases described above can flow uniformly through the catalyst layer without much stratification of the flow.
  • a CPO catalyst is a partial oxidation catalyst, which partially oxidizes a hydrocarbon to hydrogen, carbon-monoxide, and other products of partial combustion according to the chemical reaction equation
  • methane is indicated as the partially oxidizing hydrocarbon, but other hydrocarbons such as propane, butane, pentane, etc. could also be used to provide a partially oxidized gas stream mixture consisting mainly of carbon-monoxide and hydrogen.
  • Liquid hydrocarbon fuels such as kerosene or gasoline could also be used in the CPO reactor.
  • Partial oxidation catalysts are generally precious metal-based and are well known in the art. These catalysts are readily available in the USA from manufacturers such as Engelhard Corporation.
  • the active-catalyst material which is generally platinum or palladium is usually coated on a high-surface area, highly porous, non-catalytic substrate material such as a ceramic base to provide a very large number of active catalyst sites per unit volume of the catalyst.
  • the catalyst can be configured in a granulated or pellet form for economical reasons or can be configured in a monolithic form to provide a low operating pressure drop. Yet further, the catalyst can be configured as a fixed packed bed or as a fluidized bed without substantially deviating from its function of partially oxidizing the hydrocarbons in the mixture of reactants that are passed through the CPO reactor.
  • the SMR catalyst is also arranged within the reactor vessel and is located downstream of the CPO catalyst so that the mixture of reactant gases which leave the CPO catalyst can flow uniformly through the catalyst layer without much stratification of the flow.
  • the SMR catalyst consists of steam reforming catalysts.
  • a steam methane reforming catalyst is a catalyst, which converts the methane and steam in the partially oxidized gas stream described above to carbon-monoxide and hydrogen according to the chemical reaction equation:
  • the SMR catalyst also converts the carbon monoxide and steam in the reactants to hydrogen and carbon dioxide according to the chemical reaction equation, commonly known as water-gas-shift reaction:
  • steam methane reforming catalyst further increases the yield of hydrogen from the autothermal reactor.
  • Conventional steam methane reforming catalysts are generally metal-oxide based and are well known in the art. Steam methane reforming catalysts made of nickel on alumina with certain promoters and are readily available in the US from manufacturers such as United Catalyst.
  • the active SMR catalyst material is generally coated on a high-surface area, highly porous, non-catalytic substrate material such as a ceramic base to provide a very large amount of active catalyst sites per unit volume of the catalyst.
  • the SMR catalyst can be configured in a granulated or pellet form for economical reasons or can be configured in a monolithic form to provide a low operating pressure drop. Yet further, the SMR catalyst can be configured as a fixed packed bed or a fluidized bed without substantially deviating from its function of converting the feed gas-stream to a hydrogen-rich reformer gas.
  • an ASMR catalyst In the presence of sub-stochio etric quantities of oxygen, an ASMR catalyst will partially oxidize a hydrocarbon to hydrogen and carbon- monoxide while in the presence of steam, the ASMR catalyst will the oxidize hydrocarbon and the carbon-monoxide to hydrogen according to the shift reaction and water-gas shift mechanisms shown above.
  • Advanced SMR catalysts are generally made up of noble metals such as platinum, palladium or rhodium and are supplied by Engelhard Corporation.
  • AGO 10 consists of a rectangular cross-sectioned duct formed by the bending and positioning of flat plates 12 and 22 respectively. Further details of flat plates 12 and 22 will be given below.
  • the mixture of anode off-gas and cathode off-gas and additional air or oxygen, if required, is shown entering AGO 10 from the left and flowing through AGO 10 from left to right.
  • the oxidized gases are shown exiting AGO 10 from the left.
  • inlet and outlet transitions which are shown in phantom, may be provided to provide an uniform entry of the reactant gases into AGO 10 and to remove the oxidized gases from AGO 10.
  • ATR assembly 60 is formed by the bending and/or positioning of plates 22, 32, and 42. Further details of plates 22, 32, and 42 will be provided below.
  • ATR 60 houses CPO catalyst 70 and SMR catalyst 72 in the path of flow of the reactant mixture of hydrocarbon fuel, air, and steam.
  • the bending and positioning of plates 12, 22, 32, and 42 also create flow and heat transfer channels within which the reactant mixture flows to the ATR chamber for conversion by the catalysts to a reformer gas. Further heat transfer between the AGO products of reaction and the reactant gases within the flow channels and CPO 70 and SMR 70 is also facilitated between the common wall formed by plate 22.
  • the above details will be more clearly understood by a discussion of Figure 2A, 2B, 2C, 2D, 3 A, 3B, 3C, and 3D wherein the constructional details and the configurations of plates 12, 22, 32, and 42 are described.
  • plate 12 is made of steel or aluminum or stainless steel or other suitable material which can withstand the temperature, pressure and corrosive environment within AGO 10.
  • plate 12 could be made of thin rolled steel such as 24 gauge carbon steel to facilitate shearing and bending and other production operations.
  • Plate 12 is cut or sheared or punched out in the form shown in Fig 2 A to form a generally cross-shaped flat piece having zones rectangular 12A, 12B, 12C, 12D, 12G, 12H, 121, and 12 J.
  • Zones 12B and 12C have identical widths L and heights H while zone 12D has a width D and a height, which is equal to width L of zone 12B.
  • Zones 12G, 12H, 121 and 12J have widths, which are equal to width D of zone 12D. Further zones 12G and 121 have identical heights X and zones 12H and 12J have identical heights Y. Further punched into plate 12 are cutouts 12E, 12F, 12K, 12L, 12 M, and 12N. Cutouts 12K and 12L are located in the right and the left arm respectively of the cross-shaped configuration formed by plate 12 and are close to zone 12 A. When assembled, cutout 12L forms the opening in FPIR 2 for the entry of the anode off-gas into AGO 10 and cutout 12K forms the opening in FPIR 2 for the removal of the oxidized anode off-gas from AGO 10.
  • cutouts 12K and 12L are generally but not necessarily designed to be identical in dimensions.
  • cutout 12E forms the opening in FPIR 2 for the entry of the ATR fuel-gas into CPO 70 through fluid flow channel 80 which will be described below.
  • cutout 12N forms the opening in FPIR 2 for the removal of the ATR fuel-gas from fluid flow channel 80 and its transfer into channel 82 which will be described below.
  • Cutouts 12M and 12F are narrow slits, which are cut into plate 22 to facilitate bending and forming operations.
  • plate 12 is bent along fold-lines 14A, 14B, 14C, 14D, 14E, 14F, and 14G as shown in Figure 3 A, which shows formed plate 22 after it is bent along the above fold- lines.
  • Plate 22 is first bent at a right angle at fold-line 14D so that zone 12G is pivoted towards zone 12 A.
  • Plate 22 is next bent at a right angle at fold-line 14E so that zone 12H is pivoted away from zone 12A.
  • Plate 22 is again bent at a right angle at fold-line 14F to cause zone 121 to move towards zone 12G.
  • Plate 22 is next bent at a right angle at fold-line 14G to move zone 12J towards zone 12H.
  • a rectangular flow channel 80 having height Y and width X is created by bending zones 12G, 12H, 121, and 12J along fold-lines 14D, 14E, 14F, and 14G. It will be obvious that flow channel 80 will be square in cross-section if X equals Y.
  • Plate 12 is further bent at a right angle at fold-line 14A to move zone 12B towards zone 12 A.
  • Plate 12 is next bent at a right angle at fold-line 14C to move zone 12C towards zone 12 A.
  • plate 12 is next bent at a right angle at fold-line 14B to move zone 12D towards zone 12 A.
  • a cavity is created by zones 12 A, 12B, 12C, 12D, and 12G within which AGO 10 is located as will be described below.
  • plate 22 is used in conjunction with formed plate 12.
  • Figure 2B shows the configuration of plate 22 before it is bent.
  • the dimensions of plate 22 are selected so that plate 22 can fit in the cavity formed by plate 12 as described above after being bent into the configuration shown in Figure 3B. Thus adjustments to the dimensions for the thickness of plates 12 and 22 should be made when shearing or cutting plate 22.
  • Plate 22 has zones 22 A and 22D. Cutouts 22B and 22C are punched in plate 22 as shown in Figure 2B.
  • the location and dimensions of cutout 22B is selected so that cutout 22B overlaps cutout 12N of plate 12.
  • Cutout 22C is located in zone 22C and is sized to accommodate the flow of the reformer gas which is formed in the SMR catalyst as will be described below. However, the dimensions of cutout 22C are selected so that there is no overlap with cutout 22B.
  • plate 22 is bent at fold-line 24A to form a generally L-shaped structure.
  • Formed plate 22 is next inserted into the cavity formed in plate 12 so that the cut-out 22B of plate 22 overlaps cutout 12N of plate 12.
  • the zone 22A of plate 22 cooperates with zones 12 A, 12C, 12D, and 12G of plate 12 to form a rectangular cross-sectioned flow channel 88 which functions as a reaction chamber for the AGO reaction.
  • the inlet to the reaction chamber is provided by cut-out 12L and the outlet from the reaction chamber is provided by cutout 12K.
  • Formed plate 22 now has an outlet opening defined by zone 22C in the lower portion of the L-shape adjacent to rectangular tube 80 formed in plate 12.
  • ATR 60 in FPIR 2 is formed by the cooperation of plate 22 with plates 32 and 42 which are shown in figures 2C, 3C, 2D and 3D.
  • Plate 32 is a thin rectangular strip defined by zone 32A. The width dimension of plate 32 is selected so that when plate 32 is held perpendicularly by its long edge against zone 22 A of plate 22 (when partially assembled with plate 12 as shown by combining Figure 3 A and 3B), the width edge of plate 32 does not protrude past the edges of zones 12B and 12C.
  • the height of plate 32 is selected to be less than the height of zone 12A of plate 12 so that a window 74 is created by the upper edge of plate 32 and zone 12D of plate 12 when plate 32 is held perpendicularly by its long edge against zone 22 A of plate 22 (when partially assembled with plate 12 as shown by combining Figure 3A and 3B.)
  • Plate 42 is an endplate whose dimensions are selected so it closes the cavity created in plate 12 as described above.
  • plate 32 is attached by its long edge in a vertical orientation to zone 22A of formed plate 22 so that its width dimension is perpendicular to the zone 22 A and its length dimension is perpendicular to zone 22D. Any method of attachment such as welding, soldering, brazing or riveting can be used to attach plate 32 to plate 22 as long as an air-tight seal is formed between plate 32 and zones 22A and zones 22D.
  • Plate 42 is then attached to the frame created by the edges of zones 12B, 12C, 12D and 22D using any of the attachment methods described above. An air-tight seal is also created between the long edge of plate 32 and zone 42A.
  • plates 12, 22, 32, and 42 cooperate to create flow channels 82, 84, and 86.
  • CPO catalyst 70 and SMR catalyst 72 are installed in flow channel 86 before endplate 42 is installed.
  • the feed-gas from flow channel 80 which was formed as described above by bending plate 12 exits flow channel 80 through cutout 12N in plate 12 and enters flow channel 82 through cutout 22B in plate 22.
  • the feed-gas then flows upwards in channel 82 and enters flow channel 84 through window 74 created by the upper edge of zone 32A and zone 12D as described above.
  • the feed-gas then enters flow-channel 86 wherein CPO catalyst 70 and SMR catalyst 72 are located.
  • the feed-gas then flows downwards first through CPO catalyst 70 and then through SMR catalyst 72 and then out of flow channel 86 through the gas-exit opening defined by zone 22C.
  • Anode off-gas and cathode offgas along with any required oxygen in the form of ambient air to provide complete oxidation of the hydrogen in the offgases is introduced into the AGO reaction chamber defined by flow channel 88 through the offgas inlet defined by cutout 12L.
  • An ignition source which is not shown in the figures is used to provide ignition of the combustible offgas mixture within flow channel 88.
  • the ignition source can be source of high temperature such as a spark plug, a glow-bar or other such means to increasing the temperature of a portion of the combustible offgas mixture to a temperature at which auto-ignition can take place.
  • the ignition of the portion of the combustible offgases provides enough energy to the rest of the combustible offgases to combust in a sustained manner.
  • the combustion of the offgases in channel 88 creates excess heat energy which is transferred across zones 12G and 22A as will be described below.
  • Feed gas for the ATR reaction consisting of a mixture of hydrocarbon fuel, air and steam as described above is introduced into flow channel 80 through the gas inlet defined by cutout 12E of plate 12.
  • This gas flows in channel 80 in a countercurrent direction to the flow of the offgases in channel 88.
  • This gas also picks up heat, which is transferred from the combusting offgases in channel 88 as described above through zone 12G.
  • the feed gas is preheated by the heat from the combusting offgases in channel 88 as the feed gas flows through channel 80.
  • the preheated feed gas exits channel 80 through the side exit defined by cutout 12N in plate 12 and enters channel 82 through the entrance defined by cutout 22B which is designed to overlap cutout 12N as described previously.
  • the preheated gas flows upward in flow channel 82 and is further preheated by the combusting offgases in channel 88 which release heat through zone 22A as described previously.
  • the further preheated feed gas then exits channel 82 through window 74 and enters channel 84 where it is further heated by the combusting offgases in channel 88 which release heat through zone 22 A.
  • the preheated feed-gas then flows into channel 86 wherein it first contacts CPO catalyst 70 wherein the hydrocarbon fuel in the feed-gas is partially oxidized by the sub-stochiometric oxygen in the feed-gas to provide hydrogen and carbon-monoxide as described previously with respect to the various reaction mechanisms in an ATR.
  • the partially reformed feed gas then exits CPO catalyst 70 and enters SMR catalyst 72 wherein the steam in the feed-gas further converts the unreacted hydrocarbon fuel and the carbon-monoxide to hydrogen as described previously with respect to the various reaction mechanisms in an ATR. Since the SMR reaction is endothermic, additional heat for the optimum conversion of the reactants is provided by heat transfer though zone 22 A from the combusting offgases in channel 88.
  • the reformed gas which contains a high proportion of hydrogen along with carbon- monoxide and nitrogen then exits flow channel 86 through the gas outlet defined by cutout 22C in plate 22.
  • the reformed gas can be used directly in a fuel-cell or can be processed further to reduce the carbon-monoxide concentration prior to its use in a fuel-cell.
  • a single catalyst known as an advanced SMR catalyst can be used instead of CPO catalyst 70 and SMR catalyst 72 described above to effect the CPO and SMR reactions in a single stage.
  • the ASMR catalyst can be located in flow chamiel 82 for contact with the preheated feed-gas.
  • the single module FPIR described in Figures 1, 2A, 2B, 2C, 2d, 3A, 3B, 3C, and 3D can be stacked to provide fuel-processors of increased reformer gas generation capacity.
  • Fig 4 shows an embodiment of such a fuel -processor which uses two of the single modules described above. It will be apparent that any number of such modules could be stacked to meet fuel-processor fuel-gas requirements in a practical and economical manner.
  • FIG. 5 shows a FPIR 90 which is constructed from simple structural members such as flat plates and square bars.
  • Fig 6 shows an exploded view of the FPIR of Fig. 5.
  • Central frame 100 consists of horizontal structural members 104A and 104B of equal length which are positioned generally parallel to each other.
  • a vertical member 102 connects one end of members 104A and 104B to form a C-shape.
  • a shorter vertical member 108 is connected to the second end of member 104B and is positioned generally parallel to first vertical member 102.
  • a fifth structural member is connected to the second unconnected end of member 108 generally parallel to first horizontal member 104A.
  • the structural members generally form a lower case alphabet "e" shaped frame.
  • ASMR catalyst 200 is placed within the space created by members 106 and 104B .
  • ASMR 200 can be configured in the form of a ceramic matrix on which active catalytic material is coated or it can be configured in the form of a cartridge which contains the catalyst in a granular form and which is open to flow in the horizontal direction from right to left.
  • the width of ASMR 200 is selected to be smaller than the width of horizontal member 106.
  • ASMR 200 is positioned such that its lower left corner is aligned with the unconnected end of horizontal member 106 so that a space 110 is left between ASMR 200 and vertical member 108.
  • the various members along with ASMR 200 create a flow path for the flow of the feed gas for conversion into a hydrogen rich reformer gas in ASMR 200.
  • the flow path starts at space 110 and goes on through ASMR 200 and exits into space 112 created between ASMR 200 and vertical member 102.
  • the reformer gas then exits space 112 through opening 116 created between the unconnected end of member 106 and the vertical member 102. It then enters space 114 created between the horizontal members 104 A and 106.
  • the reformer gas then exits FPIR 90 through opening 118 created between the connected end of member 106 and the unconnected end of horizontal member 104 A.
  • the casing of the ATR in FPIR 90 is formed by 2 identical flat plates shown as 120 which sandwich ATR frame 100 to create the ATR.
  • Flat plate 120 is generally rectangular in dimension.
  • the horizontal dimension of plate 120 is equal to the length of horizontal member 104 A.
  • the vertical dimension of plate 120 is equal to the length of vertical member 102.
  • Flat plate 120 has a solid zone 122 in which a flow opening 124 is punched. Flow opening 124 is located so that it opens into space 110 described above.
  • FPIR 90 has two identical feed pre-heater, which sandwich the ATR section described above.
  • the first feed pre-heater section of FPIR 90 is formed by structural member assembly 130 and flat end plate 150.
  • the second feed preheater section of FPIR 90 is formed by a second structural member assembly 130 and a second flat end plate 150.
  • the ATR in FPIR 90 is sandwiched between the first and the second AGO/preheater assemblies as will be described below.
  • Structural assembly 130 consists of a first horizontal structural member 104C, which is equal in length to member 104A of the ATR assembly.
  • a second horizontal member 104D which is equal in length to member 104C, is positioned so that it is above the opening 124 of plate 120.
  • a third horizontal member 136 which is shorter in length than member 104C is located in the same position as horizontal member 106 of the ATR assembly.
  • horizontal members 104C, 136, and 104D are positioned generally parallel to each other.
  • the first end of member 136 is located so that it is inline with the first ends of members 104E and 104C.
  • the first ends of member 136 and 104D are connected at a right angle by vertical structural member 134.
  • the second end of members 104C and 104D are connected at right angles by vertical structural member 132 to form a frame that is shaped similar to a mirror-image of the lower case alphabet "e".
  • the AGO section of FPIR 90 is created by positioning a horizontal member 104E, which is equal in length to member 104D, generally parallel to horizontal member 104D to create a space 160 which defines the AGO reactor volume.
  • Flow of the AGO gases to the AGO reactor volume is facilitated by inlet opening 162 which is defined by the first ends of horizontal members 104E and 104D.
  • Flow of the AGO gases out of the AGO reactor volume is facilitated by outlet opening 164 which is defined by the second ends of horizontal members 104E and 104D.
  • the casing of the feed preheater and the AGO is formed by plate 122, which also forms the case of the ATR, and by endplate 150.
  • Endplate 150 is identical in dimensions to plate 120.
  • Figure 5 and 6 shows a configuration wherein a FPIR 90 is created by stacking a first plate 150, a structural assembly 130, a first flat plate 120, a structural assembly 100, a second flat plate 120,another structural assembly 130, and a second flat plate 150 to create a FPIR which consists of an ATR which is sandwiched between two AGOs.
  • a FPIR which consists of an ATR which is sandwiched between two AGOs.
  • Such an assembly is designated as a 1-2 FPIR to indicate that there is 1 ATR and 2 AGOs in the fuel-processor.
  • the AGO offgas is introduced into AGO volume 160 through AGO inlet 162.
  • the AGO offgas is oxidized in volume 160 and heat energy is generated which is transferred tlirough reactor casing walls 122 and 150 and tlirough members 104E and 104D.
  • the oxidized anode offgas leaves reactor 160 through outlet opening 164.
  • the feed gas for the ATR is introduced through opening 144 and flows through space 140.
  • the feed gas then leaves space 140 tlirough opening 142 and enters space 138.
  • space 138 the feed gas is heated by the heat generated on the other side of plate 122 by the oxidation of the AGO off-gas in AGO volume 160.
  • the preheated feed gas then leaves space 138 through opening 124 in plate 122 and enters space 110 in frame assembly 100.
  • the feed gas is further preheated by the hot oxidized AGO offgas in volume 160.
  • the preheated feed-gas then enters ASMR 200 wherein it is converted to a hydrogen-rich reformer gas by the water-gas shift reaction and the shift reactions described previously.
  • the hot converted gas then exits ASMR 200 into space 112 wherein it gives up some of its sensible heat to the cooler feed gas in space 138.
  • the hot converted gas then exits space 112 through opening 116 and enters space 114 wherein it gives up some more of its sensible heat to the cold feed gas in space 140.
  • the cooled converted gas then exits space 114 through opening 118 and exits FPIR 90 for further post processing before use in a fuel cell.
  • a 2-3 FPIR wherein there are two ATRs and 3 AGOs can be easily created by stacking parts/subassemblies 150, 130, 120, 100, 120, 130, 120, 100, 120, 130, and 150.
  • Other configurations such as a 3-4 FPIR, a 4-5 FPIR, a 5-6 FPIR can be easily created by adopting the fabrication and stacking techniques described above.
  • a FPIR with a single ATR and a single AGO can be created by stacking flat plate 150, a ATR assembly 100, flat plate 120, a AGO assembly 130 and a second flat plate 150.
  • Such a configuration would not be as energy-efficient as the configuration shown in Figure 6.
  • FPIRs containing any number of ATRs and AGO can be a created by simply stacking the basic modules described above.
  • the 1-1 FPIR described above can itself be stacked to provide a 2-2 FPIR, a 3-3 FPIR, a 4-4 FPIR and so forth.
  • Such an arrangement provides easy and convenient means of scaling up the capacity of the fuel-processor to meet fuel-cell requirements.
  • the basic modules can be created in a small capacity and can be stacked to provide a wide coverage of a range of fuel-cell requirements without large stepwise increases in capacity between models.
  • CPO and SMR catalyst can also be used instead of the ASMR catalyst described above. Such an arrangement may be necessary for economical reasons related to the relative costs of the CPO, SMR and ASMR catalyst.
  • the channels defined by the members in member sub-assemblies 100 and 120 in FPIR 90 could be incorporated into plates 120 and 150 themselves by impressing these flow patterns in the plates using dies.
  • Such an arrangement would be similar to those used in the fabrication of flat-plate heat-exchangers wherein flow patterns for the flow of the fluids is formed in the plates by subj ect the plates to metal-processing steps using a die. Examples of such plates are shown in standard engineering references such as Perry's Chemical Engineer's Handbook. Such plates can then be stacked together similar to the stacking in flat plate heat-exchanger to form the fuel-processor.
  • the plates can be made of a moldable substance such as ceramic and the flow patterns can be formed in the plates at the time of molding the plates.
  • the flow-pattern containing ceramic plates can then be stacked together to form the fuel-processor described above.

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Abstract

L'invention concerne un réacteur intégré (2) qui comprend une première plaque plate (12) découpée de manière sélective, et pliée de manière à présenter une paroi arrière, une paroi supérieure, deux parois latérales et une partie de base, et une deuxième plaque plate (22) pliée pour présenter une paroi intermédiaire et une paroi de base. La deuxième plaque plate (22) est placée dans la plaque supérieure et les parois latérales de la première plaque plate (12) de manière à définir avec la première plaque plate (12) une partie (10) de l'oxydant des gaz du compartiment anodique du réacteur intégré (2). Une troisième plaque plate (32) comprend une paroi avant et est placée à l'intérieur de la paroi supérieure et des parois latérales de la première plaque plate (12). La paroi intermédiaire de la deuxième plaque plate (22) et la paroi avant de la troisième plaque plate (32) sont espacées l'une de l'autre et définissent entre elles une partie (60) du réacteur autothermique du réacteur intégré (2). Une première trajectoire d'écoulement (88) est formée dans la partie (10) de l'oxydant des gaz du compartiment anodique pour permettre l'écoulement du gaz dans cette dernière et une deuxième trajectoire d'écoulement (80, 82, 84, 86) est formée dans la partie de réacteur autothermique (60) pour permettre l'écoulement du gaz dans cette dernière. Les première et deuxième trajectoires d'écoulement sont séparées par la deuxième plaque plate (22) et un échange de chaleur se produit entre les gaz dans l'écoulement.
PCT/US2002/012897 2001-04-24 2002-04-24 Reacteur WO2002085509A1 (fr)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006131094A1 (fr) * 2005-06-10 2006-12-14 Forschungszentrum Jülich GmbH Dispositif de reformage autotherme

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US4933242A (en) * 1989-02-28 1990-06-12 Ishikawajima-Harima Heavy Industries Co., Ltd. Power generation system with use of fuel cell
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US4933242A (en) * 1989-02-28 1990-06-12 Ishikawajima-Harima Heavy Industries Co., Ltd. Power generation system with use of fuel cell
US5077148A (en) * 1989-05-03 1991-12-31 Institute Of Gas Technology Fully internal manifolded and internal reformed fuel cell stack
US5180561A (en) * 1989-11-27 1993-01-19 Ishikawajima-Harima Heavy Industries Co., Ltd. Plate type reformer assembly
US5470670A (en) * 1993-03-01 1995-11-28 Matsushita Electric Industrial Co., Ltd. Fuel cell
US6069286A (en) * 1998-07-16 2000-05-30 Phillips Petroleum Company Hydrocarbon conversion process employing promoted zeolite catalyst

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WO2006131094A1 (fr) * 2005-06-10 2006-12-14 Forschungszentrum Jülich GmbH Dispositif de reformage autotherme

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