EP2013141A2 - Heat exchange reformer unit and reformer system - Google Patents
Heat exchange reformer unit and reformer systemInfo
- Publication number
- EP2013141A2 EP2013141A2 EP07734374A EP07734374A EP2013141A2 EP 2013141 A2 EP2013141 A2 EP 2013141A2 EP 07734374 A EP07734374 A EP 07734374A EP 07734374 A EP07734374 A EP 07734374A EP 2013141 A2 EP2013141 A2 EP 2013141A2
- Authority
- EP
- European Patent Office
- Prior art keywords
- reforming
- sections
- section
- heat exchange
- exchange reformer
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Withdrawn
Links
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- 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
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- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/0093—Microreactors, e.g. miniaturised or microfabricated reactors
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- 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
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- B01J2219/00783—Laminate assemblies, i.e. the reactor comprising a stack of plates
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B—PERFORMING OPERATIONS; TRANSPORTING
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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
- 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
- C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
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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
- 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
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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
- 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
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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
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/08—Methods of heating or cooling
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- 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
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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
- 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
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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
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
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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
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/14—Details of the flowsheet
- C01B2203/141—At least two reforming, decomposition or partial oxidation steps in parallel
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- 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 present invention relates to a heat exchange reformer unit in which reforming reactions are caused by which reformate gas that contains hydrogen is obtained from reformation material, such as hydrocarbon, with heat supplied from a heating section to a reforming section.
- the present invention also relates to a reformer system including such a heat exchange reformer unit.
- JP-A-2004-244230 describes a technology for setting a region in which catalyst is not supported between plates so that the distribution of heat generation caused by combustion reactions and the distribution of heat absorption by reforming reactions in the regions between the plates are adjusted to each other.
- the present invention provides a heat exchange reformer unit of which the efficiency of heat exchange between a heating section and a reforming section is excellent.
- the present invention also provides a heat exchange reformer unit and a reformer system, which make it possible to improve reforming efficiency.
- a heat exchange reformer unit includes: a reforming section, in which reforming catalyst for inducing reforming reactions is supported, for producing reformate gas, which contains hydrogen, from supplied reformation material through reforming reactions including steam-reforming reaction; a heating section, which is disposed adjacent to the reforming section with a separation wall interposed between the heating section and the reforming section so as to cause a gas flow in the same direction as that of a gas flow in the reforming section, and in which oxidizing catalyst for catalytic combustion is supported, for supplying, to the reforming section, heat generated by catalytically burning supplied fuel; a reformation material-introducing section, one end of which serves as a supply port of the reformation material, and the other end of which is integral with a reformation material inflow side of the reforming section; and a fuel-introducing section, one end of which serves as a supply port of the fuel, and the other end of which is integral with a fuel inflow side of the heating section, for introducing the
- reforming reactions are caused (promoted) in the reforming section by bringing supplied reformation material into contact with the reforming catalyst with heat supplied from the heating section, so that reformate gas that contains hydrogen is obtained.
- Reforming reactions create a highly endothermic region near the end portion on the upstream side (on the reformation material supply side) of the region in which the reforming catalyst is supported.
- Combustion reactions create a highly exothermic region near the end portion on the upstream side (on the fuel supply side) of the region in which the oxidizing catalyst is supported.
- the direction in which the reformation material (or the reformate gas) flows in the reforming section, and the direction in which the fuel or fuel gas flows in the heating section are the same.
- the heating section and the reforming section constitute a parallel-flow heat exchange reformer unit. Accordingly, it is possible to create the highly endothermic region, which is created by the combustion reactions in the heating section, and the highly exothermic region, which is created by the reforming reactions in the reforming section, on the same side (upstream side) of the regions, in which the catalysts are supported, in the gas flow direction.
- the reformation material-introducing section which is integral with the upstream side of the reforming section
- the fuel-introducing section which is integral with the upstream side of the heating section in which the gas flow direction is parallel to that in the reforming passage (that is, the gas inlet ports of the reforming section and the heating section of, so to speak, the heat exchanger are positioned at virtually the same position)
- the reformation material-introducing section and the fuel-introducing section constitute a quasi cross-flow section.
- the heat exchange reformer unit according to the first embodiment has excellent efficiency of heat exchange between the heating section and the reforming section.
- the stability (robustness) of operation is enhanced, and it is made possible to realize stable operation against fluctuations (variation in the temperature of the reformation material, for example).
- the entirety of the fuel-introducing section may be a region in which no oxidizing catalyst is supported
- oxidizing catalyst is not supported in the fuel-introducing section, and therefore, catalytic combustion does not occur in the fuel-introducing section.
- the situation is prevented in which heat generated by catalytic combustion is not used in the reforming section and causes local high-temperature regions to occur.
- local high-temperature regions can occur because the position of the highly endothermic region and the position of the highly exothermic region are not matched when oxidizing catalyst is supported in the fuel-introducing section, which, together with the reformation material-introducing section, forms a quasi cross-flow section described above.
- oxidizing catalyst is not supported in the fuel-introducing section, occurrence of local high-temperature regions is effectively prevented.
- a plurality of the reforming sections and a plurality of the heating sections may be provided, and may be stacked with at least part of the plurality of the reforming sections being adjacent to at least part of the plurality of the heating sections, the reformation material-introducing section may be provided for each of the reforming sections, and surface planes of the reformation material supply ports may be substantially on the same plane, and the fuel-introducing section may be provided for each of the heating sections, and surface planes of the fuel supply ports may be substantially on the same plane.
- the plurality of the reforming sections and the plurality of the heating sections are stacked, and at least part of the reforming sections are adjacent to at least part of the heating sections.
- the number of the heating sections provided may be equal to or less than that of the reforming sections, and every heating section may be adjacent to the reforming section on each side of the heating section in the stacking direction. Because the reformation material-introducing sections that are open on the same surface plane are provided in the respective layers of the reforming sections, and the fuel-introducing sections that are open on the same surface plane are provided in the respective layers of the reforming sections, it is possible to separately supply reformation material and fuel to the same side of the reforming sections and the heating sections. Thus, it is possible to construct a parallel-flow heat exchange reformer unit, in which the region in which a large amount of heat is generated is located close to the region in which endothermic demand is large, with a multilayer structure showing excellent heat exchange efficiency,
- the heat exchange reformer unit may be constructed by stacking a plurality of reforming section-forming plate members and a plurality of heating section-forming plate members in a predetermined pattern.
- Each of the reforming section-forming plate members includes: a first flat-shaped plate portion; and a first standing wall provided on the first fiat-shaped plate portion in a standing condition for guiding the reformation material in a predetermined direction, wherein a first heat exchanging section constituting the reforming section together with another plate portion is formed of part of the first flat-shaped plate portion, and wherein a reformation material guide section constituting the reformation material-introducing section together with another plate portion is formed 4 of part of the first flat-shaped plate portion and the first standing wall that is formed adjacent to a reformation material supply-side of the first heat exchanging section.
- Each of the heating section-forming plate members includes: a second flat-shaped plate portion; and a second standing wall provided on the second flat-shaped plate portion in a standing condition for guiding the fuel in a direction intersecting the predetermined direction, wherein a second heat exchanging section constituting the heating section together with another plate portion is formed of part of the second flat-shaped plate portion, and wherein a fuel guide section constituting the fuel-introducing section together with another plate portion is formed of part of the second flat-shaped plate portion and the second standing wall that is formed adjacent to a fuel supply-side of the second heat exchanging section.
- the reforming section-forming plate members and the heating section-forming plate members are stacked in a predetermined pattern, so that the reforming sections and the heating sections are formed between the heat exchanging sections in the plate portions, and the reformation material-introducing sections and the fuel-introducing sections are formed between the reformation material guide sections and the fuel guide sections in the plate portions.
- the reformation material-introducing sections and the fuel-introducing sections are integrally formed on the upstream side of the parallel-flow heat-exchanging sections, wherein the reformation material-introducing sections and the fuel-introducing sections have the reformation material supply ports and the fuel supply ports, respectively, which are open separately.
- the heat exchange reformer unit may further include: a reformation material manifold, defining a collection space to which the reformation material supply ports of the plurality of the reformation material-introducing sections are open, for distributing the reformation material to the plurality of the reformation material-introducing sections; and a fuel manifold, defining a collection space to which the fuel supply ports of the plurality of the fuel-introducing sections are open, for distributing the fuel to the plurality of the fuel-introducing sections.
- the supply ports of the reformation material-introducing sections for introducing reformation material into the reforming sections of the respective layers are open to the reformation material manifold, and the supply ports of the fuel-introducing sections for introducing fuel into the heating sections of the respective layers are open to the fuel manifold.
- the fuel manifold with a mixer for mixing fuel and combustion-supporting gas, it is made possible to supply mixed gas, which is previously mixed immediately upstream of the heating sections of the respective layers, to the heating sections of the respective layers. Ih this case, occurrence of the regions in which fuel concentration is locally high is prevented, and thus, occurrence of local high-temperature regions in the heating sections is prevented.
- the heat exchange reformer unit may further include: a reformate gas-discharging section, one end of which serves as a discharge port of the reformate gas, and the other end of which is integral with a reformate gas outflow side of the reforming section; and a combustion exhaust gas-discharging section, one end of which serves as a discharge port of combustion exhaust gas of the heating section, and the other end of which is integral with a combustion exhaust gas outflow side of the heating section, for introducing the combustion exhaust gas to the discharge port of the combustion exhaust gas in a flow direction different from a flow direction of the reformate gas in the reformate gas-discharging section.
- the reformate gas-discharging section which is integral with the downstream side of the reforming section
- the combustion exhaust gas-discharging section which is integral with the downstream side of the heating section in which the gas flow direction is parallel to that in the reforming passage (that is, the gas outlet ports of the reforming section and the heating section of, so to speak, the heat exchanger are positioned at virtually the same position)
- the reformate gas-discharging section and the combustion exhaust gas-discharging section constitute a quasi cross-flow section.
- the reformate gas-discharging sections may be provided for the reforming sections of the respective layers, and the combustion exhaust gas-discharging sections may be provided for the heating sections of the respective layers.
- the configuration as described below may be adopted.
- the reformate gas guide section is formed in the plate portion of the reforming section-forming plate member on the side of the heat-exchanging section opposed to the reformation material guide section.
- the standing walls for guiding reformate gas in another predetermined direction are provided in a standing condition, and the reformate gas guide section constitutes the reformate gas-discharging section together with another plate portion.
- the exhaust gas guide section is formed in the plate portion of the heating section-forming plate member on the side of the heat-exchanging section opposed to the fuel guide section.
- the standing walls for guiding combustion exhaust gas in a direction intersecting the another predetermined direction in the reforming section-forming plate member are provided in a standing condition, and the exhaust gas guide section constitutes the combustion exhaust gas-discharging section together with another plate portion.
- a heat exchange reformer includes: a plurality of reforming sections for producing reformate gas, in which reforming catalyst for inducing reforming reactions is supported; and a plurality of heating sections, in which reforming catalyst for catalytic combustion is supported, for supplying heat, which is generated by catalytically burning supplied fuel, to the reforming sections, wherein the number of the heating sections is less than the number of the reforming sections.
- reformate gas is obtained by bringing supplied reformation material into contact with the reforming catalyst in the reforming section with combustion heat supplied from the heating section to cause (promote) reformation reactions-
- reforming reactions require a reaction space (volume) larger than that of combustion reactions.
- the number of layers of the reforming sections is greater than the number of layers of the heating sections, the difference in the amount of reaction per volume between the reforming passages and the combustion passages is compensated by the difference in the number of layers thereof (the volume of reaction space). That is, the amount of reaction is set according to the reaction field, and it is possible to increase the amount of reformate gas produced relative to the amount of reformation material supplied, or to the volume of the heat exchange reformer unit.
- the reforming section may be a reaction section for producing reformate gas that contains hydrogen from supplied reformation material through reforming reactions including the steam-reforming reaction, for example.
- a heat exchange reformer includes: a plurality of reforming sections for producing reformate gas, in which reforming catalyst for inducing reforming reactions is supported; and a plurality of heating sections, in which reforming catalyst for catalytic combustion is supported, for supplying heat, which is generated by catalytically burning supplied fuel, to the reforming reactions, wherein the plurality of the reforming sections and the plurality of the heating sections are stacked so that the surface area of the region in which the reforming catalyst is supported is greater than the surface area of the region in which the oxidizing catalyst is supported,
- reformate gas is obtained by bringing supplied reformation material into contact with the reforming catalyst in the reforming section with combustion heat supplied from the heating section to cause (promote) reformation reactions.
- the surface area of the region in which the reforming catalyst is supported is greater than the surface area of the region in which the oxidizing catalyst is supported. For this reason, the amount of reforming reaction relative to the amount of combustion reaction is increased, and therefore, the difference in the amount of reaction between the reforming sections and the combustion sections is reduced (the difference in the amount of reaction per volume is compensated). That is, the amount of reaction is set according to the reaction field, and it is possible to increase the amount of reformate gas produced relative to the amount of reformation material supplied, or to the volume of the heat exchange reformer unit.
- the reforming section may be a reaction section for producing reformate gas that contains hydrogen from supplied reformation material through reforming reactions including the steam-reforming reaction, for example.
- a heat exchange reformer includes: a plurality of reforming sections for producing reformate gas, in which reforming catalyst for inducing reforming reactions is supported; and a plurality of heating sections, in which reforming catalyst for catalytic combustion is supported, for supplying heat, which is generated by catalytically burning supplied fuel, to the reforming reactions, wherein the plurality of the reforming sections and the plurality of the heating sections are stacked so that the amount of the reforming catalyst supported is greater than the amount of the oxidizing catalyst supported.
- reformate gas is obtained by bringing supplied reformation material into contact with the reforming catalyst in the reforming section with combustion heat supplied from the heating section to cause (promote) reformation reactions.
- the amount of reforming catalyst supported is greater than the amount of oxidizing catalyst supported. For this reason, the amount of reforming reaction relative to the amount of combustion reaction is increased, and therefore, the difference in the amount of reaction between the reforming sections and the combustion sections is reduced (the difference in the amount of reaction per volume is compensated). That is, the amount of reaction is set according to the reaction field, and it is possible to increase the amount of reformate gas produced relative to the amount of reformation material supplied, or to the volume of the heat exchange reformer unit.
- the reforming section may be a reaction section for producing reformate gas that contains hydrogen from supplied reformation material through reforming reactions including the steam-reforming reaction, for example.
- a heat exchange reformer includes: a plurality of reforming sections for producing reformate gas, in which reforming catalyst for inducing reforming reactions is supported; and a plurality of heating sections, in which reforming catalyst for cataLytic combustion is supported, for supplying heat, which is generated by catalytically burning supplied fuel, to the reforming reactions, wherein the plurality of the reforming sections and the plurality of the heating sections are stacked so that the total volume of the plurality of the reforming sections is greater than the total volume of the plurality of heating sections,
- reformate gas is obtained by bringing supplied reformation material into contact with the reforming catalyst in the reforming section with combustion heat supplied from the heating section to cause (promote) reformation reactions.
- reaction velocity of reforming reactions is lower than that of combustion reactions
- reforming reactions require a reaction space (volume) larger than that of combustion reactions.
- the total volume of the plurality of the reforming sections is greater than the total volume of the plurality of the combustion sections.
- the difference in the amount of reaction per volume between the reforming passages and the combustion passages is compensated by the difference in the volume of the respective reaction spaces (volume ratio). That is, the amount of reaction is set according to the reaction field, and it is possible to increase the amount of reformate gas produced relative to the amount of reformation material supplied, or to the volume of the heat exchange reformer unit.
- the reforming section may be a reaction section for producing reformate gas that contains hydrogen from supplied reformation material through reforming reactions including the steam-reforming reaction, for example.
- the heat exchange reformer unit may include a part in which two layers of the reforming sections are stacked per one layer of the heating section.
- the heat exchange reformer unit includes a part in which the reforming sections and the heating sections are stacked so that the units are stacked in each of which two layers of the reforming sections are disposed on the same side of one layer of the heating section, or so that the units are stacked in each of which one layer of the heating section is sandwiched between a pair of layers of the reforming sections, for example.
- two layers of the reforming sections are disposed between a pair of the heating sections.
- at least one side of each reforming section is adjacent to a heating section.
- the volume of the reforming sections (the catalyst-supporting region surface area, or the amount of catalyst supported) with the heat transport distance between the heating sections and the reforming sections kept short as compared to that of the configuration in which the heating sections and the reforming sections are alternately stacked.
- the ratio of the volume of the reforming sections to the overall volume of the reformer unit is about 50% in the configuration in which the heating sections and the reforming sections are alternately stacked, it is possible to increase the ratio of the volume of the reforming sections to the overall volume of the reformer unit to about 67% in the above configuration.
- the heat exchange reformer unit may include a part in which three layers of the reforming sections are stacked per one layer of the heating section.
- the heat exchange reformer unit includes a part in which the reforming sections and the heating sections are stacked so that the units are stacked in each of which three layers of the reforming sections are disposed on the same side of one layer of the heating section, for example. Ih such a part, three layers of the reforming sections are disposed between a pair of the heating sections. In this way, while the ratio of the volume of the reforming sections to the overall volume of the reformer unit is about 50% in the configuration in which the heating sections and the reforming sections are alternately stacked, for example, it is possible to increase the ratio of the volume of the reforming sections to the overall volume of the reformer unit to about 75% in the above configuration.
- the heat exchange reformer unit may include a part in which four or more layers of the reforming sections are stacked per one layer of the heating section.
- the heat exchange reformer unit includes a part in which the reforming sections and the heating sections are stacked so that the units are stacked in each of which four layers of the reforming sections are disposed on the same side of one layer of the heating section, for example. In such a part, four layers of the reforming sections are disposed between a pair of the heating sections. In this way, while the ratio of the volume of the reforming sections to the overall volume of the reformer unit is about 50% in the configuration in which the heating sections and the reforming sections are alternately stacked, for example, it is possible to increase the ratio of the volume of the reforming sections to the overall volume of the reformer unit to about 80% or more in the above configuration.
- the heat exchange reformer unit according to this aspect may further include a heat transfer-promoting portion for promoting heat transfer from the heating section to the adjacent reforming section.
- thermal resistance between the heating sections and the reforming sections is reduced by the heat transfer-promoting portions, whereby the heat transport from the heating section to the reforming section is promoted.
- a connecting wall or the like connecting between the separation walls each separating the reforming section and the heating section may be used, for example.
- a reformer system includes: the heat exchange reformer unit according to the above aspect; and a water supply system for supplying water to the reforming section of the heat exchange reformer unit.
- the water supplied to the reforming section through the water supply system reacts with the reformation material in the reforming section, and reforms the reformation material into reformate gas that contains hydrogen.
- reforming reactions including the steam-reforming reaction, which is endothermic reaction, occur in the reforming sections, and the heat required to cause the steam-reforming reaction is supplied from the heating sections to the reforming sections.
- the reformer system includes the heat exchange reformer unit according to the above aspect, the difference in the amount of reaction per volume between the reforming passages (reforming sections) and the combustion ' passages (heating sections) is compensated, and the reformer system increases the amount of reformate gas produced relative to the amount of reformation material supplied, or to the volume of the heat exchange reformer unit, despite the configuration in which steam-reforming reaction is caused that has reaction velocities lower than those of combustion reactions.
- the heat exchange reformer unit and the reformer system according to the above aspects of the present invention have excellent efficiency of heat exchange between the heating sections and the reforming sections, and exhibit the advantageous effect that the reforming efficiency is enhanced.
- FIG. I is a schematic system flow diagram of a fuel cell system in which a heat exchange reformer unit according to any one of first to sixth embodiments of the present invention is used;
- FIG. 2 is an exploded perspective view showing a main part of the heat exchange reformer unit according to the first embodiment of the present invention
- FIG. 3 is a perspective view of the heat exchange reformer unit according to the first embodiment of the present invention.
- FIG. 4 is an exploded perspective view showing a catalyst-supporting region of the heat exchange reformer unit according to the first embodiment of the present invention
- FIGS. 5 A to 5C are diagrams showing a process in which catalyst is supported, in the heat exchange reformer unit according to the first embodiment of the present invention, wherein FIG. 5A is a schematic diagram showing a state in which a catalyst carrier is flowing into the heat exchange reformer unit, FIG. 5B is a schematic diagram showing a state in which the inflow of the catalyst carrier is stopped, and FIG. 5C is a schematic diagram, showing a state in which the catalyst is introduced; FIG. 6 is a diagram showing a temperature distribution in a combustion passage of the heat exchange reformer unit according to the first embodiment of the present invention;
- FIGS. 7 A to 7C are schematic diagrams showing examples that are defective in supporting the catalyst
- FIGS. 8 A and 8B are diagrams showing the heat exchange reformer unit according to the second embodiment of the present invention, wherein FIG. 8 A is a front view, and FIG. 8B is a partially enlarged front view;
- FIG. 9 is an exploded perspective view showing a main part of the heat exchange reformer unit according to the second embodiment of the present invention.
- FIG. 10 is a perspective view showing an external appearance of the heat exchange reformer unit according to the second embodiment of the present invention.
- FIG. 11 is a diagram schematically showing the reaction field of reforming reactions and the reaction field of combustion reactions in the heat exchange reformer unit according to the second embodiment of the present invention.
- FIG. 12 is a graph showing the ratio of the volume of the reforming passages to the volume of a multilayer core unit constituting the heat exchange reformer unit according to any one of the embodiments of the present invention.
- FIG. 13 is a graph showing the relation between the area of the region in which oxidizing catalyst is supported and the area of the region in which reforming catalyst is supported in the multilayer core unit constituting the heat exchange reformer unit according to any one of the embodiments of the present invention
- FIG. 14 is a diagram showing actually measured values of the conversion ratio of the reformation material versus the ratio of the volume of the reforming passages to the volume of the multilayer core unit of the heat exchange reformer unit according to any one of the embodiments of the present invention
- FIGS. 15A and 15B are diagrams showing the heat exchange reformer unit according to the third embodiment of the present invention, wherein FIG. 15A is a front view, and FIG. 15B is a partially enlarged front view;
- FIG. 16A and 16B are diagrams showing the heat exchange reformer unit according to the fourth embodiment of the present invention, wherein FIG. 16A is a front view, and FIG. 16B is apian view;
- FIG 17 is a schematic diagram in which the multilayer core unit constituting the heat exchange reformer unit according to the fourth embodiment of the present invention is modeled as a heat transfer fin unit;
- FIG. 18 is a graph showing fin efficiency of the multilayer core unit of the heat exchange reformer unit according to any one of embodiments of the present invention.
- FIGS. 19A and 19B are diagrams showing the heat exchange reformer unit according to the fifth embodiment of the present invention, wherein FIG. 19 A is a front view, and FIG. 19B is apian view;
- FIG. 20 is a front view showing the heat exchange reformer unit according to the sixth embodiment of the present invention.
- FIGS. 21 A and 2 IB are diagrams showing the heat exchange reformer unit according to the seventh embodiment of the present invention, wherein FIG. 21 A is a front view, and FIG. 21B is a partially enlarged front view; and
- FIGS. 22A and 22B are diagrams showing the heat exchange reformer unit according to a comparative example for comparison with the embodiments of the present invention, wherein FIG. 22A is a front view, and FIG. 22B is a partially enlarged front view;
- a heat exchange reformer unit 10 according to a first embodiment of the present invention will be described with reference to FIGS. 1 to 6. First, the overall system configuration of a fuel cell system 11, in which the heat exchange reformer unit 10 is used, will be described, and then the structural details of the heat exchange reformer unit 10 will be described.
- FIG. 1 shows a system configuration diagram (process flow sheet) of the fuel cell system 11.
- the fuel cell system 11 is constructed using, as main components, a fuel cell 12 that uses hydrogen to generate electricity, and the heat exchange reformer unit (reformer) 10 for producing reformate gas that contains hydrogen to be supplied to the fuel cell 12.
- the heat exchange reformer unit (reformer) 10 for producing reformate gas that contains hydrogen to be supplied to the fuel cell 12.
- the fuel cell 12 is constructed with electrolyte (not shown) interposed between an anode electrode (fuel electrode) 14 and a cathode electrode (air electrode) 16, and is configured so as to generate electricity mainly by electrochemically reacting the hydrogen that is supplied to the anode electrode 14, and the oxygen that is supplied to the cathode electrode 16.
- electrolyte not shown
- anode electrode fuel electrode
- cathode electrode air electrode
- various types of fuel cells may be used as the fuel cell 12
- a fuel cell having proton conductive electrolyte such as a solid polymer fuel cell and a hydrogen membrane fuel cell
- medium temperatures about 300 to 70O 0 C
- the heat exchange reformer unit 10 includes: a reforming passage 18, which constitutes a reforming section for producing the reformate gas, which contains hydrogen, to be supplied to the anode electrode 14 of the fuel cell 12; and a combustion passage 20, which constitutes a heating section for supplying heat that is used in the reforming passage 18 to cause reforming reactions.
- the reforming passage 18 supports reforming catalyst 22, so that reformate gas that contains hydrogen is produced (reforming reactions are caused) by catalytically reacting hydrocarbon gas (such as gasoline, methanol and natural gas) and reforming gas (steam), which are supplied.
- the reforming reactions in the reforming passage 18 includes reactions including the steam-reforming reaction expressed by the equation (1), as shown by the following equations (1) to (4). Accordingly, the reformate gas obtained through the reforming process contains combustible gas, such as hydrogen (H 2 ), carbon monoxide (CO), methane (CH f ) 5 decomposed hydrocarbon and unreacted hydrocarbon material (C x Hy), and incombustible gas, such as carbon dioxide (CO 2 ) and water (H 2 O).
- combustible gas such as hydrogen (H 2 ), carbon monoxide (CO), methane (CH f ) 5 decomposed hydrocarbon and unreacted hydrocarbon material (C x Hy)
- incombustible gas such as carbon dioxide (CO 2 ) and water (H 2 O).
- the combustion passage 20 supports oxidizing catalyst 24, and is disposed adjacent to the reforming passage 18, so that the combustion passage 20 is configured so as to bring the supplied fuel and oxygen into contact with the oxidizing catalyst 24 to cause catalytic combustion.
- the partial oxidation reaction expressed by the equation (2) is exothermic reaction.
- the heat generated by the partial oxidation reaction is used in the steam-reforming reaction together with the heat supplied from the combustion passage 20.
- the heat exchange reformer unit 10 is designed to supply the combustion heat obtained by catalytically burning fuel in the combustion passage 20 to the reforming passage 18 through a plate portion 52 described later.
- the heat exchange reformer unit 10 is configured so as to be able to directly supply heat to the reforming passage 18 without converting the heat into temperature as in the case of the configuration in which the reforming passage 18 is heated using heating medium (fluid), such as combustion gas.
- the fuel cell system 11 includes a material pump 26 for supplying hydrocarbon material to the reforming passage 18.
- the discharge port of the material pump 26 is connected to a material inlet port 18A of the reforming passage 18 through a material supply line 28.
- the hydrocarbon material includes a very small amount of sulfur ingredients (sulfur compounds), which do not contribute to the reforming reactions described above.
- the hydrocarbon material is supplied to the reforming passage 18 in a gas phase or in an atomized form by a vaporizing device or the like (not shown), such as a vaporizer and an injector.
- a reformate gas outlet 18B of the reforming passage 18 is connected to the upstream end of a reformate gas supply line 30, the downstream end of which is connected to a fuel inlet 14A of the anode electrode 14.
- the reformate gas produced in the reforming passage 18 is supplied to the anode electrode 14 of. the fuel cell 12.
- the upstream end of an anode off-gas line 32 is connected to an off-gas outlet 14B of the anode electrode 14.
- the downstream end of the anode off-gas line 32 is connected to a fuel inlet 33A of a gas mixer 33.
- the gas mixer 33 substantially homogeneously mixes the anode off-gas and the coolant off-gas supplied through a combustion-supporting gas supply line 46 described later.
- a mixed gas outlet 33B of the gas mixer 33 is connected to a fuel (mixed gas) inlet 2OA of the fuel passage 20.
- the fuel cell system 11 is designed so that hydrogen in the reformate gas produced in the reforming passage 18 is used in the fuel cell 12, the remaining components, other than the used hydrogen, are introduced into the combustion passage 20 as an anode off-gas, and the combustible components therein (H 2 , CO, HC and CH 4 ) are used as fuel in the combustion passage 20.
- An exhaust gas line 34 for discharging combustion exhaust gas out of the system is connected to an exhaust gas outlet 2OB.
- the fuel cell system 11 includes a cathode air pump 36 for supplying cathode air to the cathode electrode 16.
- a cathode air pump 36 for supplying cathode air to the cathode electrode 16.
- Connected to the discharge port of the cathode air pump 36 is the upstream end of a cathode air supply line 38, the downstream end of which is connected to an air inlet 16A of the cathode electrode 16.
- the upstream end of a steam supply line 40 is connected to an off-gas outlet 16B of the cathode electrode 16, and the downstream end of the steam supply line 40 is connected to a steam inlet 18C of the reforming passage 18.
- the cathode off-gas that contains steam produced by the cathode electrode 16 and oxygen that is not used on the cathode electrode 16 are supplied to the reforming passage 18.
- the steam in the cathode off-gas is used in the steam-reforming reaction expressed by the equation (1), and oxygen is used in the partial oxidation reaction expressed by the equation (2),
- the heat exchange reformer unit 10 according to the first embodiment is configured so as to be operated under particular conditions in which the O/C ratio that is the ratio of the amount of supplied oxygen to the amount of carbon in the hydrocarbon material is set to a particular ratio by supplying cathode off-gas that contains oxygen to the reforming passage 18.
- the fuel cell system 11 includes a cooling air pump 42 for supplying cooling air to the fuel cell 12,
- the discharge port of the cooling air pump 42 is connected to the upstream end of a cooling air supply line 44, the downstream end of which is connected to an inlet 12A of, the coolant passage (not shown) of the fuel cell 12.
- An outlet 12B of the coolant passage is connected to the upstream end of a combustion-supporting gas supply line 46.
- the combustion-supporting gas supply line 46 is connected to a combustion-supporting gas inlet 33C of the gas mixer 33 so as to supply coolant off-gas that contains oxygen as combustion-supporting gas to the gas mixer 33.
- the mixed gas that is obtained by mixing the anode off-gas supplied through the anode off-gas line 32 and the coolant off-gas supplied through the combustion-supporting gas supply line 46 in the gas mixer 33 is brought into contact with the oxidizing catalyst 24 that the combustion passage 20 has therein, thereby causing catalytic combustion.
- the gas mixer 33 instead of the configuration in which the gas mixer 33 is provided, a configuration may be adopted in which the downstream end of the anode off-gas line 32 and the downstream end of the combustion-supporting gas supply line 46 are individually connected to the combustion passage 20, for example.
- the fuel cell 12 (cathode electrode 16) and the steam supply line 40 may be regarded as the water supply device of the present invention
- the fuel cell system 11 (more specifically, the part of the fuel cell system 11, which includes the heat exchange reformer unit 10, the cathode electrode 16, and the steam supply line 40) may be regarded as the reformer system of the present invention.
- a configuration may be adopted in which the steam supply line 40 is provided with a separation membrane (a porous separation membrane made of polyimide and ceramic, for example) that selectively allows permeation of only the steam in the cathode off-gas, or in which the steam used in reforming is introduced from the outside of the system, so that oxygen is not supplied to the reforming passage 18, or that the ratio (O/C ratio) of the amount of supplied oxygen to the amount of carbon in the hydrocarbon material is small.
- the main reaction of the reforming reactions in the heat exchange reformer unit 10 is the steam-reforming reaction, and therefore, the partial oxidation reaction is not caused, or the amount of heat generated by the partial oxidation reaction becomes very small.
- FIG. 2 shows a multilayer core unit 65 of the heat exchange reformer unit 10 in an exploded perspective view.
- the reforming passages 18 constituting the reforming sections and the combustion passages 20 constituting the heating sections are formed in the form of separate gas passages between the unit plate members 50 and 51, which are provided as a plurality of reforming section-forming plate members and a plurality of heating section-forming plate members, which are stacked, wherein the reforming passages 18 and the combustion passages 20 are separated by the plate portions 52 as separation walls, which may be regarded as flat-shaped plate portions of the unit plate members 50 and 51.
- the reforming passages 18 and the combustion passages 20 are alternately stacked in the stacking direction (the thickness direction of the plate portion 52).
- the reforming passage 18 and the combustion passage 20 are adjacent to each other with the plate portion 52 interposed therebetween. Specific description will be given below.
- the unit plate member 50 includes the plate portion 52 formed in a flat shape.
- the plate portion 52 is formed by integrally providing, at both ends in the longitudinal direction of a parallel flow portion 52 constituting a heat exchanging section formed in a rectangular shape, flow direction-changing sections 52B and 52C, when viewed from above,
- the flow direction-changing sections 52B and 52C are formed in a triangular shape such that the bases thereof are made to coincide with the corresponding short sides of the parallel flow portion 52A (with a rectangular shape).
- the plate portion 52 as a whole is formed in a substantially hexagonal shape.
- Each unit plate member 50 includes outer walls 54, which are provided in a standing condition at edges of the plate portion 52 on the side thereof on which the reforming passages 18 are formed.
- the outer walls 54 are provided in a standing condition all around the plate portion 52 except one side portion of each of the direction-changing sections 52B and 52C, so that the outer walls 54 function as spacers that define the reforming passages 18 between the stacked unit plate members 50 and 51, and also function as outer walls that prevent the outflow of gas from the reforming passages 18, and, at the same time, create a gas inlet 5OA on the flow-directioh changing section 52B-side, and a gas outlet 5OB on the flow-direction changing section 52C-side.
- the gas inlet 5OA and the gas outlet 5OB are formed symmetrically with respect to the centroid of the plate portion 52, and the openings thereof are oriented in the directions indicated by the arrows Cl and C2 beside the flow-direction changing sections 52B and 52C, respectively, which are opposite to the direction of the parallel flow portion 52A 5 which extends along the longitudinal direction of the outer walls 54.
- a plurality of standing walls (partition walls) 56 that divide the reforming passage 18 into a plurality of parallel passages are provided in a standing condition on the reforming passage 18-formed-side of the plate portion 52 of the unit plate members 50.
- the standing walls 56 are made substantially parallel with the outer walls 54 from the gas inlet 50A to the gas outlet 5OB, and are configured so as to divide the reforming passage 18 into a plurality of divided passages (microchannels) 58.
- Each divided passage 58 is formed in a crank-like shape such that the length of the passages from the gas inlet 50A to the gas outlet 50B is substantially the same owing to the symmetrical arrangement of the gas inlet 50A and the gas outlet 5OB described above.
- the inlet guide walls 56B are part of the standing walls 56, and lie along the direction indicated by the arrow Cl.
- outlet guide walls 56C are part of the standing walls 56, and lie along the direction indicated by the arrow C2.
- the unit plate member 51 includes a plate portion 52 that has the same shape as that of the plate portion 52 constituting the unit plate member 50, and includes outer walls 60, which are provided in a standing condition at the periphery of the plate portion 52 on the side thereof on which the combustion passages 20 are formed.
- the outer walls 60 are provided in a standing condition all around the plate portion 52 except one side portion of each of the direction-changing sections 52B and 52C, so that the outer walls 60 function as spacers that form the combustion passages 20 between the stacked unit plate members 50 and 51, and also function as outer walls that prevent the outflow of gas from the combustion passages 20, and so that the outer walls 60 form a gas inlet 51A on the flow-direction changing section 52B-side, and a gas outlet 5 IB on the flow-direction changing section 52C-side.
- the gas inlet 51 A is formed on the same side of a parallel flow portion 52A in the longitudinal direction as the gas inlet 5OA of the unit plate member 50 (that is, on the side indicated by the arrow A in FIG. 2) so as to be open toward the direction indicated by the arrow Dl, which is different from the direction indicated by the arrow Cl (that is, which is symmetric with respect to the longitudinal axis of the parallel flow portion 52A) 5 toward which the gas inlet 5OA is open.
- the gas outlet 51B is formed on the same side of a parallel flow portion 52A in the longitudinal direction as the gas outlet 50B of the unit plate member 50 (that is, on the side indicated by the arrow B in FIG. 2) so as to be open toward the direction indicated by the arrow D2, which is different from the direction indicated by the arrow C2 (that is, which is symmetric with respect to the longitudinal axis of the parallel flow portion 52A), toward which the gas outlet 5OB is open.
- a plurality of standing walls (partition walls) 62 that divide the combustion passage 20 into a plurality of parallel passages are provided in a standing condition on the combustion passage 20-fbrmed-side of the plate portion 52 of the unit plate members 51.
- the standing walls 62 are made substantially parallel with the outer walls 60 from the gas inlet 5 IA to the gas outlet 5 IB, and are configured so as to divide the combustion passage 20 into a plurality of divided passages (microchannels) 64.
- Each divided passage 64 is formed in a crank-like shape such that the length of the passages from the gas inlet 51 A to the gas outlet 5 IB is substantially the same owing to the symmetrical arrangement of the gas inlet 51 A and the gas outlet 5 IB described above.
- the inlet guide walls 62B are part of the standing walls 62, and lie along the direction indicated by the arrow Dl.
- the part of the divided passages 64 between which outlet guide walls 62C are provided on the flow-direction changing section 52C in a standing condition serve as combustion exhaust gas guide passages 64C constituting a combustion exhaust gas guide section.
- the outlet guide walls 62C are part of the standing walls 62, and lie along the direction indicated by the arrow D2.
- the gas inlets 50A and 51A are positioned on the same side (that is, on the side indicated by the arrow A) of the parallel flow portion 52A (the heat-exchanging passages 58A and 64A) 5 and the gas outlets 50B and 51B are positioned on the same side (that is, on the side indicated by the arrow B) of the parallel flow portion 52A as described above, so that the directions in which gas flows in the heat-exchanging passages 58A and 64A on the respective layers are set to the same direction (the direction indicated by the arrow F).
- the portions are integrally formed of metallic materials, such as stainless steel, or solid (not porous) ceramics, for example.
- the plurality of the unit plate members 50 and the plurality of the unit plate members 51 constitute the multilayer core unit 65 of the heat exchange reformer unit 10, wherein the plate members 52 and the outer walls 54 and 60 (the standing walls 56 and 62) are airtightly joined by brazing using brazing filler or by diffusion bonding, for example.
- a flat-shaped plate portion 52 (cover) on which the outer walls 54 or the like are not provided in a standing condition is placed on the top of the heat exchange reformer unit 10 so as to close the reforming passage 18.
- a reformation inlet manifold 66 that defines a collection space to which the gas inlets 5OA of the respective layers are open is connected to the multilayer core unit 65.
- a reformation outlet manifold 68 that defines a collection space to which the gas outlets 5OB of the respective layers are open is connected to the multilayer core unit 65.
- a combustion inlet manifold 70 that defines a collection space to which the gas inlets 51 A of the respective layers are open is connected to the multilayer core unit 65.
- a combustion outlet manifold 72 that defines a collection space to which the gas outlets 5 IB of the respective layers are open is connected to the multilayer core unit 65.
- Each of the manifolds 66, 68, 70 and 72 is formed in a rectangular tube shape, and one open end thereof is joined to the end portions of the top and bottom plate portions 52, and the end portions of the outer walls 54 and 60 of the respective layers by brazing, for example.
- the material inlet 18A and the steam inlet 18C for introducing reformation material (hydrocarbon) and steam (cathode off-gas), respectively, are provided in the reformation inlet manifold 66, and the reformate gas outlet 18B for discharging reformate gas is provided in the reformation outlet manifold 68.
- the fuel inlet 2OA for introducing 1 mixed gas from the gas mixer 33 is provided in the combustion inlet manifold 70, and the exhaust gas outlet 2OB for discharging combustion exhaust gas is provided in the combustion outlet manifold 72.
- the reforming catalyst 22 is supported on the inner surface of the divided passages 58 on the unit plate member 50, and the oxidizing catalyst 24 is supported on the inner surface of the divided passages 64 on the unit plate member 51. As shown in FIG.
- the reforming catalyst 22 is supported in the divided passages 58 (reforming passage 18) in a predetermined region thereof that does not include part of the divided passages 58 on the gas inlet 50A-side, and the oxidizing catalyst 24 is supported in the divided passages 58 (combustion passage 20) in a predetermined region thereof that does not include part of the divided passages 64 on the gas inlet 51A-side.
- an upstream-side supporting region end 22A that is the end on the upstream side (that is, on the side indicated by the arrow A) in the gas flow direction in which the reformation material is supplied, substantially coincides with the border between the heat-exchanging passages 58A (parallel flow sections 52A) and the reformation material guide passages 58B (flow direction-changing sections 52B) of the divided passages 58.
- an upstream-side supporting region end 24A that is the end on the upstream side (that is, on the side indicated by the arrow A) in the gas flow direction in which the fuel is supplied, substantially coincides with the border between the heat-exchanging passages 64A (parallel flow sections 52A) and the mixed gas guide passages 64B (flow-direction changing sections 52B) of the divided passages 64.
- the upstream-side supporting region end 24A of the oxidizing catalyst 24 coincides with the upstream-side supporting region end 22A of the reforming catalyst 22, or is positioned a bit further downstream than the upstream-side supporting region end 22A.
- a catalyst carrier is applied on the divided passages 58 of the reforming passage 18 and the divided passages 64 of the combustion passage 20 by immersing the multilayer core unit 65, from the end thereof on the gas outlet 50B-side, or 51B-side, into a slurry-like catalyst carrier 75 stored in a storage tank 76. Then, the catalyst carrier 75 applied on the divided passages 58 and 64 is caused to support the reforming catalyst 22 and the oxidizing catalyst 24, respectively.
- the detection signal from a catalyst sensor or sensors 74 for detecting the catalyst carrier which are provided in representative ones of or all of the divided passages 58 and 64, is used.
- a method of producing the heat exchange reformer unit 10 will be specifically described below.
- the unit plate members 50 and 51 are alternately stacked, and the free edges of the outer walls 54 and 60 are bonded to the plate portions 52 of the adjacent unit plate members 51 and 50, respectively.
- the multilayer core unit 65 is formed.
- the catalyst-supporting region position sensors 74 are set on the divided passages 58 and 64 of the multilayer core unit 65,
- the catalyst-supporting region position sensor 74 is designed to output an ON signal to a notification device (not shown), such as a display device and notification sound-generating device, when the catalyst carrier is brought into contact with a slurry-detecting portion 74A provided on the tip of the sensor.
- the catalyst-supporting region position sensors 74 are inserted into representative ones of the divided passages 58 and 64 from the gas inlet 50A-side, or 51A-side so that the slurry-detecting portions 74A are positioned at the desired positions to which the upstream-side supporting region end 22A of the reforming catalyst 22 and the upstream-side supporting region end 24A of the oxidizing catalyst 24 on the divided passages 58 and 64 are controlled.
- the multilayer core unit 65 in which the catalyst-supporting region position sensors 74 are set is immersed into the catalyst carrier 75 in the storage tank 76 from the gas outlet-50B, or 5 IB-side.
- the multilayer core unit 65 is gradually (slowly) immersed into the catalyst carrier 75 until a notification is made by the notification device (until the catalyst-supporting region position sensor(s) 74 detects the catalyst carrier 75), as shown in FIGS. 5 A and 5B.
- the notification device until the catalyst-supporting region position sensor(s) 74 detects the catalyst carrier 75
- the multilayer core unit 65 is drawn out of the storage tank 76, and the surplus catalyst carrier 75 is removed from the divided passages 58 and 64 by blowing air thereinto through the gas inlets 5OA and 51A 5 for example.
- the reforming catalyst 22 is supplied into the divided passages 58 through the gas outlets 5OB to cause the catalyst carrier 75 in the divided passages 58 to support the reforming catalyst 22.
- the oxidizing catalyst 24 is supplied into the divided passages 64 through the gas outlets 5 IB to cause the catalyst carrier 75 in the divided passages 64 to support the oxidizing catalyst 24.
- the multilayer core unit 65 is constructed in which the reforming catalyst 22 is supported in the heat-exchanging passages 58A and the reformate gas guide passages 58C of the divided passages 58 but is not supported in the reformation material guide passages 58B, and in which the oxidizing catalyst 24 is supported in the heat-exchanging passages 64A and the combustion exhaust gas guide passages 64C of the divided passages 64 but is not supported in the mixed gas guide passages 64B.
- the reformation inlet manifold 66, the combustion inlet manifold 70, the reformation outlet manifold 68, and the combustion outlet manifold 72 are respectively joined to the opening portions of the gas inlets 5OA and 5 IA, and the gas outlets 5OB and 5 IB of the respective layers of the multilayer core unit 65.
- the production process of the heat exchange reformer unit 10 as shown in FIG. 3 is completed.
- the reformate gas produced in the reforming passages 18 is supplied to the anode electrode 14 through the fuel inlet 14A of the anode electrode 14. Ih the fuel cell 12, hydrogen in the reformate gas supplied to the anode electrode 14 is turned into protons, and the protons migrate to the cathode electrode 16 through the electrolyte to react with oxygen in the air introduced onto the cathode electrode 16. As the protons migrate in this way, electrons flow from the anode electrode 14 toward the cathode electrode 16 through the external conductor, so that electricity is generated.
- the generation of electricity uses hydrogen in the reformate gas supplied to the anode electrode 14 and oxygen in the cathode air supplied to the cathode electrode 16 in accordance with the amount of electricity generated (the electric power consumption of a load), and water (steam under operating temperature conditions) is produced at the cathode electrode 16.
- the gas that contains steam is expelled from the cathode electrode 16 to the steam supply line 40 as cathode off-gas as described above, and introduced into the reforming passage 18 through the steam inlet 18C.
- the gas resulting after hydrogen in the reformate gas is used according to the amount of generated electricity as electricity is generated, is discharged from the anode electrode 14 as anode off-gas.
- the anode off-gas is supplied to the combustion passages 20 of the heat exchange reformer unit 10 through the anode off-gas line 32.
- the coolant off-gas after cooling the fuel cell 12 is supplied to the combustion passages 20 through the combustion-supporting gas supply line 46.
- catalytic combustion is caused by bringing the combustible components in the anode off-gas, which is fuel, into contact with the oxidizing catalyst 24 together with the oxygen in the coolant off-gas as the combustion-supporting gas.
- the heat produced by the catalytic combustion is supplied to the reforming passages 18 through the plate' portions 52.
- the reforming reactions which are endothermic reactions, are maintained, and the operating temperature (reformate gas temperature) is maintained at a temperature required to bring about reforming reactions.
- the fuel cell system 11 supplies hydrocarbon material to the heat exchange reformer unit 10, and effectively uses various exhaust gases of the fuel cell 12 (the cathode off-gas that contains steam, the anode off-gas that contains combustible components, and the coolant off-gas that contains oxygen) to maintain the operation of the heat exchange reformer unit 10, which produces hydrogen that is supplied to the fuel cell 12.
- various exhaust gases of the fuel cell 12 the cathode off-gas that contains steam, the anode off-gas that contains combustible components, and the coolant off-gas that contains oxygen
- the reforming reactions in the reforming passages 18 have an endothermic peak on the reformation material inlet side, that is, on the upstream-side catalyst-supporting region 22A-side of the region in which the reforming catalyst 22 is supported.
- the burning reactions in the combustion passages 20 have an exothermic peak on the fuel inlet side, that is, on the upstream-side catalyst-supporting region 24A-side of the region in which the reforming catalyst 24 is supported.
- counter-flow heat exchange reformer units for example, an endothermic peak and an exothermic peak in a reforming section and a heating section occur at opposite end portions with respect to the gas flow direction in a heat exchanging section, and therefore, counter-flow heat exchange reformer units are not suitable for the heat exchangers in reformers.
- a parallel-flow heat exchanger in which the gas flow direction in the heat-exchanging passages 58 A of the reforming passage 18 and the gas flow direction in the heat-exchanging passages 64A of the combustion passage 20 are the same, is constructed, that is, it is possible to set an endothermic peak and an exothermic peak on the same side with respect to the gas flow direction, wherein, in the reforming reactions, the endothermic peak occurs on the gas inlet 50A-side to which reformation material is supplied, and, in the combustion reactions, the exothermic peak occurs on the gas inlet 51A-side to which fuel is supplied. Accordingly, the efficiency of heat exchange between the reforming passages 18 and the combustion passages 20 is enhanced.
- the reformation material guide passages 58B and the mixed gas guide passages 64B which are located on the upstream side of the heat-exchanging passages 58A and 64A substantially constituting a parallel-flow heat exchanger, constitute a cross-flow heat exchanging section, so that the heat exchange therein enables stable operation against fluctuation (robustness is enhanced).
- An experimental example is shown in FIG. 6. FIG.
- FIG. 6 is a diagram showing a temperature distribution at points along the gas flow direction in the divided passages 64 when the temperature of the mixed gas supplied is at a constant temperature of 400°C
- the solid line represents the case where the temperature of the reformation material supplied to the divided passages 58 is 600°C
- the dashed line represents the case where the temperature of the reformation material supplied to the divided passages 58 is 400°C. From this figure, it can be seen that, even when the temperature of the gas flowing into the divided passages 58 varies by 200°C, the increase in the highest temperature in the divided passages 64 is restricted to 30°C. That is, the heat exchange reformer unit 10 makes it possible to effectively suppress sharp variation in the temperature of the reaction field depending on the gas inlet temperature.
- the reforming catalyst 22 and the oxidizing catalyst 24 are not supported in the cross-flow heat exchanging section, which is constituted of the reformation material guide passages 58B and the mixed gas guide passages 64B, and therefore, neither a reforming reaction nor a combustion reaction occurs in the reformation material guide passages 58B and the mixed gas guide passages 64B. Accordingly, the occurrence of local high-temperature regions due to the unbalance between the positions of the endothermic region and the exothermic region is prevented, which is a problem arising when a cross-flow heat exchange reformer unit is used.
- the cross-flow heat exchanging section (quasi-cross-fiow section), which is constituted of the reformation material guide passages 58B and the mixed gas guide passages 64B, upstream of the parallel-flow heat-exchanging section, which is constituted of the heat-exchanging passages 58A and the heat-exchanging passages 64A, it is made possible to realize an ideal reaction field (thermal balance) in the reforming passages 18 and the combustion passages 20, and in addition, the improvement in the robustness of the system is achieved.
- the region in which the catalyst carrier 75 is provided is controlled using the catalyst-supporting region position sensor 74, it is possible to accurately form the upstream-side supporting region ends 22A and 24A of the reforming catalyst 22 and the oxidizing catalyst 24.
- the multilayer core unit 65 in which multiple unit plate members 50 and 51 are stacked it is infeasible to see the inside of the divided passages 58 and 64, it is possible to prevent the situation where catalyst is supported in the reformation material guide passages 58B and the mixed gas guide passages 64B as shown in FIG.
- the reformation material guide passages 58B and the mixed gas guide passages 64B which are positioned upstream of the heat-exchanging passages 58A and 64A substantially constituting a parallel-flow heat exchanger, constitute a cross-flow (quasi-cross-flow) section, so that it is possible to form the gas inlets 50A 5 whose surface planes in the respective layers are substantially on the same plane, and the gas inlet 51A, whose surface planes in the respective layers are substantially on the same plane, in the form of separate opening portions that are open toward different directions.
- the combustion inlet manifold 70 when the combustion inlet manifold 70 is provided, it is made possible to dispose the gas mixer 33, which supplies mixed gas to the divided passages 64 (combustion passages 20), immediately before the gas inlets 5 IA.
- a gas mixer 33 is structured in the form of a mixing space provided downstream of the microchannei structure, which is constructed by alternately stacking such unit plates as obtained by removing the flow direction-changing section 52C and the outlet guide walls 56C or 62C from the unit plate members 50 and 51, it is made possible to dispose, or form, the gas mixer 33 in the combustion inlet manifold 70 (or in a pipe with a rectangular cross-section connected to the combustion inlet manifold 70).
- the reformate gas guide passages 58C and the combustion exhaust gas guide passages 64C which are positioned downstream of the heat-exchanging passages 58A and 64A substantially constituting a parallel-flow heat exchanger, constitute a cross-flow (quasi -cross-flow) section, so that it is possible to form the gas outlets 5OB and 5 IB in the form of separate opening portions that, are open toward different directions.
- FIG. 8A shows the multilayer core unit 65, which is a main component of the heat exchange reformer unit 10, in a front view in section.
- FIG. 9 shows the multilayer core unit 65 in an exploded perspective view.
- the reforming passages 18 as the reforming sections, and the combustion passages 20 as the heating sections are formed in the form of separate gas passages between the unit plate members 50 and 51, which are provided as a plurality of reforming section-forming plate members and a plurality of heating section-forming plate members, which are stacked, wherein the reforming passages 18 and the combustion passages 20 are separated by the plate portions 52 as separation walls, which may be regarded as flat-shaped plate portions of unit plate members 50 and 51.
- the multilayer core unit 65 has a configuration in which the number of layers of the reforming passages 18 and the number of layers of the combustion passages 20 differ from each other. Specific description will be given below.
- the unit plate member 50 includes the plate portion 52 formed in a flat shape. As shown in FIG. 9, the plate portion 52 is formed by providing, at both ends in the longitudinal direction of the parallel flow portion 52 as the heat exchanging section, which is formed in the rectangular shape, the flow direction-changing sections 52B and 52C, individually, in a continuous manner, when viewed from above. In this embodiment, the flow direction-changing sections 52B and 52C are formed in a triangular shape such that the bases thereof are made to coincide with the corresponding short sides of the parallel flow portion 52A (with a rectangular shape). Accordingly, the plate portion 52 as a whole is formed in a substantially hexagonal shape. Each unit plate member 50 includes the outer walls 54, which are provided in a standing condition at edges of the plate portion 52 on the side thereof on which the reforming passages 18 are formed.
- the outer walls 54 are provided in a standing condition all around the plate portion 52 except one side portion of each of the direction-changing sections 52B and 52C, so that the outer walls 54 function as spacers that define the reforming passages 18 between the stacked unit plate members 50 and 51, and also function as outer walls that prevent the outflow of gas from the reforming passages 18, and, at the same time, create the gas inlet 5OA on the flow-direction changing section 52B-side, and the gas outlet 5OB on the flow-direction changing section 52C-side.
- the gas inlet 5OA and the gas outlet 5OB are formed symmetrically with respect to the centroid of the plate portion 52, and the openings thereof are oriented in the directions indicated by the arrows Cl and C2, respectively, which are opposite to the direction of the parallel flow portion 52A, which extends along the longitudinal direction of the outer walls 54, in the flow-direction changing sections 52B and 52C.
- a plurality of standing walls (partition walls) 56 that divide the reforming passage 18 into a plurality of parallel passages are provided in a standing condition on the side of the plate portion 52 of the unit plate members 50 on which the reforming passage 18 is formed.
- the standing walls 56 are made substantially parallel with the outer walls 54 from the gas inlet 5OA to the gas outlet 50B, and are configured so as to divide the reforming passage 18 into the plurality of divided passages (microchannels) 58.
- Each divided passage 58 is formed in a crank-like shape such that the length of the passages from the gas inlet 5OA to the gas outlet 5OB is substantially the same owing to the symmetrical arrangement of the gas inlet 50A and the gas outlet 5OB described above.
- the inlet guide walls 56B are part of the standing walls 56, and lie along the direction indicated by the arrow Cl.
- the unit plate member 51 includes the plate portion 52 that has the same shape as that of the plate portion 52 constituting the unit plate member 50, and includes the outer walls 60, which are provided in a standing condition at the periphery of the plate portion 52 on the side thereof on which the combustion passages 20 are formed.
- the outer walls 60 are provided in a standing condition all around the plate portion 52 except one side portion of each of the direction-changing sections 52B and 52C, so that the outer walls 60 function as spacers that form the combustion passages 20 between the stacked unit plate members 50 and 51, and also function as outer walls that prevent the outflow of gas from the combustion passages 20, and so that the outer walls 60 form the gas inlet 51A on the flow-direction changing section 52B-side, and the gas outlet 51B on the flow-direction changing section 52C-side.
- the gas inlet 5 IA is formed on the same side of a parallel flow portion 52A in the longitudinal direction as the gas inlet 5OA of the unit plate member 50 (that is, on the side indicated by the arrow A in FIG. 9) so as to be open toward the direction indicated by the arrow Dl, which is different from the direction indicated by the arrow Cl (that is, which is symmetric with respect to the longitudinal axis of the parallel flow portion 52A).
- the gas outlet 5 IB is formed on the same side of a parallel flow portion 52A in the longitudinal direction as the gas inlet 5OA of the unit plate member 50 (that is, on the side indicated by the arrow B in FIG.
- the plurality of standing walls (partition walls) 62 that divide the combustion passage 20 into a plurality of parallel passages are provided in a standing condition on the combustion passage 20-formed-side of the plate portion 52 of the unit plate members 51.
- the standing walls 62 are made substantially parallel with the outer walls 60 from the gas inlet 51 A to the gas outlet 5 IB, and are configured so as to divide the combustion passage 20 into the plurality of divided passages (microchannels) 64.
- Each divided passage 64 is formed in a crank-like shape such that the length of the passages from the gas inlet 51 A to the gas outlet 5 IB is substantially the same owing to the symmetrical arrangement of the gas inlet 51A and the gas outlet 51B described above.
- the portions in the parallel flow portion 52A that are separated by partition wall portions 62A of the standing walls 62 lying along the longitudinal direction of the parallel flow portions 52A are made to serve as heat-exchanging passages 64A.
- the part of the divided passages 64 that are created by providing, as part of the standing walls 62, inlet guide walls 62B on the flow-direction changing section 52B in a standing condition that lie along the direction indicated by the arrow Dl are made to serve as mixed gas guide passages 64B constituting a fuel guide section.
- part of the divided passages 64 that are created by providing, as part of the standing walls 62, outlet guide walls 62C on a ' flow-direction changing section 52C in a standing condition that lie along the direction indicated by the arrow D2, are made to serve as combustion exhaust gas guide passages 64C constituting a combustion exhaust gas guide section.
- the multilayer core unit 65 is constructed by stacking the unit plate members 50 and 51 in the following manner: the gas inlets 5OA and 51A are positioned on the same side (that is, on the side indicated by the arrow A) of the parallel flow portion 52A (the heat-exchanging passages 58A and 64A), and the gas outlets 5OB and 5 IB are positioned on the same side (that is, on the side indicated by the arrow B) of the parallel flow portion 52A as described above, so that the directions in which gas flows in the heat-exchanging passages 58A and 64A on the respective layers are set to the same direction (the direction indicated by the arrow F).
- the multilayer core unit 65 is constructed by stacking two unit plate members 50 (two layers of the reforming passages 18) per one unit plate member 51 (one layer of the combustion passage 20). Specifically, in the multilayer core unit 65, by stacking the units, in each of which two unit plate members 50 are stacked on the same side of one unit plate member 51, or the units, in each of which one unit plate member 51 is sandwiched between the unit plate members 50 in the stacking direction, two layers of the reforming passages 18 are disposed between a pair of the combustion passages 20 such that a combustion passage 20 is not adjacent to another combustion passage 20 in the stacking direction, as shown in FIG. 8B. Accordingly, in the multilayer core unit 65, the reforming passage 18 of each layer is, on any one side thereof, adjacent to a combustion passage 20 with a plate portion 52 interposed therebetween.
- the portions are integrally formed of metallic materials, such as stainless steel, or solid (not porous) ceramics, for example.
- the plurality of the unit plate members 50 and the plurality of the unit plate members 51 constitute the multilayer core unit 65 of the heat exchange reformer unit 10, wherein the plate members 52 and the outer walls 54 and 60 (the standing walls 56 and 62) are airtightly joined by brazing using brazing filler or by diffusion bonding, for example.
- a flat-shaped plate portion 52 (cover) on which the outer walls 54 or the like are not provided in a standing condition is placed on the top of the heat exchange reformer unit 10 so as to close the reforming passage 18.
- a reformation inlet manifold 66 that defines a collection space to which the gas inlets 50A of the respective layers are open is connected to the multilayer core unit 65.
- a reformation outlet manifold 68 that defines a collection space to which the gas outlets 50B of the respective layers are open is connected to the multilayer core unit 65.
- a combustion inlet manifold 70 that defines a collection space to which the gas inlets 5 IA of the respective layers are open is connected to the multilayer core unit 65.
- a combustion outlet manifold 72 that defines a collection space to which the gas outlets 5 IB of the respective layers are open is connected to the multilayer core unit 65.
- Each of the manifolds 66, 68, 70 and 72 is formed in a rectangular tube shape, and one open end thereof is joined to the end portions of the top and bottom plate portions 52, and the end portions of the outer walls 54 and 60 of the respective layers by brazing, for example.
- the material inlet 18A and the steam inlet 18C for introducing reformation material (hydrocarbon) and steam (cathode off-gas), respectively, are provided in the reformation inlet manifold 66, and the reformate gas outlet 18B for discharging reformate gas is provided in the reformation outlet manifold 68.
- the fuel inlet 2OA for introducing mixed gas from the gas mixer 33 is provided in the combustion inlet manifold 70 ? and the exhaust gas outlet 2OB for discharging combustion exhaust gas is provided in the combustion outlet manifold 72.
- the reforming catalyst 22 is supported on the inner surface of the divided passages 58 on the unit plate member 50, and the oxidizing catalyst 24 is supported on the inner surface of the divided passages 64 on the unit plate member 51. As shown in FIG.
- the reforming catalyst 22 is supported in the divided passages 58 (reforming passage 18) in a predetermined region thereof that does not include part of the divided passages 58 on the gas inlet 5OA -side, and the oxidizing catalyst 24 is supported in the divided passages 58 (combustion passage 20) in a predetermined region thereof that does not include part of the divided passages 64 on the gas inlet 51 A-side.
- an upstream-side supporting region end 22A that is the end on the upstream side (that is, on the side indicated by the arrow A) in the gas flow direction in which the reformation material is supplied, substantially coincides with the border between the heat-exchanging passages 58A (parallel flow section 52A) and the reformation material guide passages 58B (flow direction-changing section 52B) of the divided passages 58.
- an upstream-side supporting region end 24A that is the end on the upstream side (that is, on the side indicated by the arrow A) in the gas flow direction, in which the fuel is supplied, substantially coincides with the border between the heat-exchanging passages 64A (parallel flow section 52A) and the mixed gas guide passages 64B (flow-direction changing section 52B) of the divided passages 64.
- the upstream-side supporting region end 24A of the oxidizing catalyst 24 coincides with the upstream-side supporting region end 22A of the reforming catalyst 22, or is positioned a bit further downstream than the upstream-side supporting region end 22A.
- the reformate gas produced in the reforming passages 18 is supplied to the anode electrode 14 through the fuel inlet 14A of the anode electrode 14.
- hydrogen in the reformate gas supplied to the anode electrode 14 is turned into protons, and the protons migrate to the cathode electrode 16 through the electrolyte to react with oxygen in the air introduced onto the cathode electrode 16.
- the protons migrate in this way, electrons flow from the anode electrode 14 toward the cathode electrode 16 through the external conductor, so that electricity is generated.
- the generation of electricity uses hydrogen in the reformate gas supplied to the anode electrode 14 and oxygen in the cathode air supplied to the cathode electrode 16 in accordance with the amount of electricity generated (the electric power consumption of a load), and water (steam under operating temperature conditions) is produced at the cathode electrode 16.
- the gas that contains steam is expelled from the cathode electrode 16 to the steam supply line 40 as cathode off-gas as described above, and introduced into the reforming passage 18 through the steam inlet 18C.
- the gas resulting after hydrogen in the reformate gas is used according to the amount of generated electricity as electricity is generated, is discharged from the anode electrode 14 as anode off-gas.
- the anode off-gas is supplied to the combustion passages 20 of the heat exchange reformer unit 10 through the anode off-gas line 32.
- the coolant off- gas after cooling the fuel cell 12 is supplied to the combustion passages 20 through the combustion-supporting gas supply line 46, Ih the combustion passages 20, catalytic combustion is caused by bringing the combustible components in the anode off-gas, which is fuel, into contact with the oxidizing catalyst 24 together with the oxygen in the coolant off-gas as the combustion-supporting gas.
- the heat produced by the catalytic combustion is supplied to the reforming passages 18 through the plate portions 52.
- the reforming reactions which are endothermic reactions, are maintained, and the operating temperature (reformate gas temperature) is maintained at a temperature required to bring about reforming reactions.
- the fuel cell system 11 supplies hydrocarbon material to the heat exchange reformer unit 10, and effectively uses various exhaust gases of the fuel cell 12 (the cathode off-gas that contains steam, the anode off-gas that contains combustible components, and the coolant off-gas that contains oxygen) to maintain the operation of the heat exchange reformer unit 10, which produces hydrogen that is supplied to the fuel cell 12.
- various exhaust gases of the fuel cell 12 the cathode off-gas that contains steam, the anode off-gas that contains combustible components, and the coolant off-gas that contains oxygen
- the number of the stacked layers (channels) of the reforming passages 18 is larger than the number of the stacked layers of the combustion passages 20,
- the increase in the volume (ratio) of the reforming passage 18 (divided passages 58) is achieved while keeping the overall volume (the sum of the total volume of the reforming passages 18 and the total volume of the combustion passages 20) unchanged.
- the total amount of the reforming reaction in the reforming passages 18 and the total amount of the combustion reaction in the combustion passages 20 are matched (the amount of reforming reaction and the amount of combustion reaction are set according to the reforming reaction field), which realizes the operation at high space velocities.
- a heat exchange reformer unit 200 according to the comparative example shown in FIGS. 22A and 22B is constructed by alternately stacking reforming passages 18 and combustion passages 20. Accordingly, in the heat exchange reformer unit 200, the ratio of the volume of the reforming passages 18 to the volume of the heat exchange reformer unit 200 (overall volume) is about 50% (see the "1/1" (layer ratio) bar in the graph of FIG. 12). Meanwhile, the reforming reactions, which have low reaction velocities as mentioned above, require a certain reaction space. Accordingly, it is difficult to achieve a high space velocity for reformation material by using the heat exchange reformer unit 200.
- the inner surface area of the reforming passages 18, that is, the area of the region, in which the reforming catalyst 22 is supported, that is, the amount of catalyst supported increases by about 34% as compared to the heat exchange reformer unit 200 that has the layer ratio of 1/1 (see the "1/1" (layer ratio) bar in the graph of FIG. 13), as shown in FIG. 13 (see the "2/1" (layer ratio) bar in the graph).
- FIG. 14 shows a relation between the proportion of the region occupied by the reforming passages 18 (volume, or the surface area of the region in which the reforming catalyst 22 is supported) and the conversion ratio (reformation ratio) when the space velocity is constant (about 50000/h).
- the conversion ratio represents the proportion in which the hydrocarbon, which is reformation material, is converted into carbon monoxide, carbon dioxide, or methane.
- the conversion ratio of the heat exchange reformer unit 10 (in which the ratio of the volume occupied by the reforming passages 18 is 67 %) is improved by about 10% as compared to that of the heat exchange reformer unit 200 (in which the same volume ratio is 50%).
- the heat exchange reformer unit 10 according to the second embodiment improves the reforming efficiency.
- FIG. 15 A shows a heat exchange reformer unit 80 according to a third embodiment in a front view in section corresponding to FIG. 8 A.
- the heat exchange reformer unit 80 differs from the heat exchange reformer unit 10, which includes the multilayer core unit 65 in which two layers of the reforming passages 18 are stacked per one layer of the combustion passage 20, in that the heat exchange reformer unit 80 includes a multilayer core unit 82 in which three unit plate members 50 (three layers of the reforming passages 18) are stacked per one unit plate member 51 (one layer of the combustion passage 20).
- the multilayer core unit 82 three layers of the reforming passages 18 are disposed between a pair of the combustion passages 20, as shown in FIG. 15B, by stacking the units, in each of which three unit plate members 50 are stacked on the same side of one unit plate member 51. Accordingly, in the multilayer core unit 82, one layer of the reforming passage 18 is disposed so as to be sandwiched between two layers of the reforming passages 18 each of which is, on any one side thereof, adjacent to a combustion passage 20 with a plate portion 52 interposed therebetween, that is, so as not to be adjacent to the combustion passage 20 on either side of the reforming passage 18.
- the ratio of the volume of the reforming passages 18 to the overall volume is about 75% as shown in FIG. 12 (see the "3/1 " bar in the graph).
- the inner surface area, that is, the catalyst-supporting region area (supporting amount) of the combustion passages 20 is increased by about 50% as compared to that of the heat exchange reformer unit 200 (see the "1/1" bar (layer ratio) in the graph).
- the configuration of the heat exchange reformer unit 80 is the same as that of the heat exchange reformer unit 10. Accordingly, as in the case of the heat exchange reformer unit 10 according to the second embodiment, the heat exchange reformer unit 80 according to the third embodiment also makes it possible to match the total amount of the reforming reaction in the reforming passages 18 and the total amount of the combustion reaction in the combustion passages 20 (that is, to set the amount of reforming reaction and the amount of combustion reaction according to the reforming reaction field), and high space velocities are therefore achieved. That is, it is possible to improve reforming efficiency.
- FIG, 16A shows a front view in section of a heat exchange reformer unit 90 according to a fourth embodiment.
- FIG. 16B shows a plan view of the reforming passage 18 (combustion passage 20) constituting the heat exchange reformer unit 90.
- the heat exchange reformer unit 90 differs from the heat exchange reformer unit 80 in including a multilayer core unit 94 in which such unit plate members 50 and 51 as described below are stacked.
- heat transfer-supporting ribs 92 which constitutes heat transfer-promoting portions, are provided in a standing condition between the end portions of the standing walls 56 on the gas inlet 50A-side thereof, and in unit plate members 51, heat transfer-supporting ribs 92, which constitutes heat transfer-promoting portions, are provided in a standing condition between the end portions of the standing walls 62 on the gas inlet 51 A-side thereof.
- the heat transfer-supporting ribs 92 are provided on the plate portions 52 in twos between the adjacent standing walls 56 (including between an outer wall 54 and the adjacent standing wall 56) and between the adjacent standing walls 62 (including between an outer wall 60 and the adjacent standing wall 62) in a standing condition so that the height of the standing walls 56 and 62 are equal to each other.
- the portions at which the heat transfer-supporting ribs 92 are provided in a standing condition are set substantially corresponding to the reaction field in which the combustion reactions mainly occur in the combustion passages 20, that is, the region in which a large amount of heat is generated.
- the plate portions 52 between the layers are regarded as heat transfer fins, wherein the width of the fin is W, the thickness of the connecting portions (the standing wall 56, the standing wall 64 and the heat transfer-supporting rib 92) is d, and the thermal conductivity is ?, as shown in FIG. 17, providing the heat transfer-supporting ribs 92 causes the multilayer core unit 94 to have a configuration in which the width W is reduced as compared to that of the third embodiment.
- the fin efficiency of the multilayer core unit 82 of the heat exchange reformer unit 80 is 0.89
- the fin efficiency of the multilayer core unit 94 of the heat exchange reformer unit 90 is enhanced to 0.98.
- the arrows in FIG. 17 show heat transfer paths.
- the configuration of the heat exchange reformer unit SO is the same as that of the heat exchange reformer unit 10. Accordingly, as in the case of the heat exchange reformer unit 10 according to the second embodiment, the heat exchange reformer unit 90 according to the fourth embodiment also makes it possible to match the total amount of the reforming reaction in the reforming passages 18 and the total amount of the combustion reaction in the combustion passages 20 (that is, to set the amount of reforming reaction and the amount of combustion reaction according to the reforming reaction field), and high space velocities are therefore achieved. That is, it is possible to improve reforming efficiency.
- the heat transfer-supporting ribs 92 promote heat transfer from the combustion passages 20 to the reforming passages 18, especially to the reforming passages 18 that are not adjacent to the combustion passages 20 on either side of each reforming passage 18, which cancels out the reduction in the thermal efficiency (heat-transfer controlled effect) caused in the case of the third embodiment.
- the heat exchange reformer unit 90 in which the ratio of the volume occupied by the reforming passages 18 is 75%), the conversion ratio exceeding that of the heat exchange reformer unit 10 is achieved under the operating conditions in which the space velocity is high and the temperature of the reformate gas is 650 ° C, as shown by the solid symbols in FIG. 14.
- the heat transfer-supporting ribs 92 by virtue of the promotion of heat transfer by the heat transfer-supporting ribs 92, it is achieved to make the increase in the volume of the reforming passages 18 (the surface area of the region in which the reforming catalyst 22 is supported) contribute to the improvement in the conversion ratio, in addition, because the region in which the heat transfer-supporting ribs 92 are disposed is limited to the end portions on the gas inlet 50A-side, or 5lA-side, it is made possible to minimize the increase in the pressure loss relative to that of the heat exchange reformer unit 80.
- FIG. 19A shows a heat exchange reformer unit 100 according to a fifth embodiment in a front view in section.
- FIG. 19B shows the reforming passages 18 (combustion passages 20) constituting the heat exchange reformer unit 100 in a plan view.
- the heat exchange reformer unit 100 differs from the heat exchange reformer unit 80 in including a multilayer core unit 104 in which such unit plate members 50 and 51 as described below are stacked.
- end portions of the standing walls 56 on the gas inlet 50A-side, and end portions of the standing walls 62 on the gas inlet 51A-side are formed into heat transfer-supporting thick portions 102 as heat transfer-promoting portions, which are thicker than the remaining portions of the standing walls 56 and 62.
- the heat transfer-supporting thick portions 102 are set substantially corresponding to the reaction field in which the combustion reactions mainly occur in the combustion passages 20, that is, the region in which a large amount of heat is generated.
- the multilayer core unit 94 is rendered to have a configuration in which the thickness d of the connecting portions between the plate portions 52 are increased as compared to that of the third embodiment, by'providing the heat transfer-supporting thick portions 102.
- the fin efficiency of the multilayer core unit 82 of the heat exchange reformer unit 80 is 0.89
- the fin efficiency of the multilayer core unit 104 of the heat exchange reformer unit 100 is enhanced to 0.99.
- the configuration of the heat exchange reformer unit 100 is the same as that of the heat exchange reformer unit 80. Accordingly, as in the case of the heat exchange reformer unit 10 according to the second embodiment, the heat exchange reformer unit 100 according to the fifth embodiment also makes it possible to match the total amount of the reforming reaction in the reforming passages 18 and the total amount of the combustion reaction in the combustion passages 20 (that is, to set the amount of reforming reaction and the amount of combustion reaction according to the reforming reaction field), and high space velocities are therefore achieved. That is, it is possible to improve reforming efficiency.
- the heat transfer-supporting thick portions 102 promote heat transfer from the combustion passages 20 to the reforming passages 18, especially to the reforming passages 18 that are not adjacent to the combustion passages 20 on either side of each reforming passage 18, which cancels out the reduction in the thermal performance (heat-transfer controlled effect) caused in the case of the third embodiment.
- the heat exchange reformer unit 100 in which the ratio of the volume occupied by the reforming passages 18 is 75%), the conversion ratio exceeding that of the heat exchange reformer unit 10 is achieved under the operating conditions in which the space velocity is high and the temperature of the reformate gas is 650 0 C 5 as shown by the solid symbols in FIG. 14.
- the heat transfer-supporting thick portions 102 by virtue of the promotion of heat transfer by the heat transfer-supporting thick portions 102, it is achieved to make the increase in the volume of the reforming passages 18 (the surface area of the region in which the reforming catalyst 22 is supported) contribute to the improvement in the conversion ratio.
- the region in which the heat transfer-supporting thick portions 102 are provided is limited to the end portions on the gas inlet 50A-side, or 51A-side, it is made possible to minimize the increase in the pressure loss relative to that of the heat exchange reformer unit 80.
- FIG. 20 shows a heat exchange reformer unit 110 according to a sixth embodiment in a front view in section.
- the heat exchange reformer unit 110 differs from the heat exchange reformer unit 80 in including a multilayer core unit 116 that has, instead of part of the plate portions 52 and the standing walls 56 constituting the unit plate member 50, plate portions 112 and standing walls 114 both constituting heat transfer-promoting portions made of material (highly heat-conductive steel) having a thermal conductivity higher than that of the plate portions 52 and the standing walls 56.
- the plate portion 112 is disposed except at the portions constituting the combustion passages 20, in other words, so as to separate the reforming passages 18 that are adjacent to each other in the stacking direction.
- the standing walls 114 are disposed at the positions such that the reforming passage 18 that is adjacent to a combustion passage 20 is divided into the divided passages 58. In FIG. 20, only the plate portions 112 and the standing walls 114 out of the components of the unit plate members 50 and 51 are hatched.
- the multilayer core unit 116 is rendered to have a configuration in which the thermal conductivity ? of each separation wall between the reforming passages 18 that are adjacent to each other in the stacking direction, and connecting portions having the thickness d is increased as compared to that of the third embodiment, by providing the plate portions 112 and the standing walls 114.
- the fin efficiency of the multilayer core unit 82 of the heat exchange reformer unit 80 is 0.89
- the fin efficiency of the multilayer core unit 116 of the heat exchange reformer unit 110 is enhanced to 0.99.
- the configuration of the heat exchange reformer unit 110 is the same as that of the heat exchange reformer unit 80. Accordingly, as in the case of the heat exchange reformer unit 10 according to the second embodiment, the heat exchange reformer unit 110 according to the sixth embodiment also makes it possible to match the total amount of the reforming reaction in the reforming passages 18 and the total amount of the combustion reaction in the combustion passages 20 (that is, to set the amount of reforming reaction and the amount of combustion reaction according to the reforming reaction field), and high space velocities are therefore achieved.
- the plate portions 112 and the standing walls 114 promote heat transfer from the combustion passages 20 to the reforming passages 18, especially to the reforming passages 18 that are not adjacent to the combustion passages 20 on either side of each reforming passage 18, which cancels out the reduction in the thermal efficiency (heat-transfer controlled effect) caused in the case of the third embodiment,
- the heat exchange reformer unit 110 in which the ratio of the volume occupied by the reforming passages 18 is 75%), the conversion ratio exceeding that of the heat exchange reformer unit 10 is achieved under the operating conditions in which the space velocity is high and the temperature of the reformate gas is 650° C, as shown by the solid symbols in FIG, 14.
- the plate portions 112 and the standing walls 114 by virtue of the promotion of heat transfer by the plate portions 112 and the standing walls 114, it is achieved to make the increase in the volume of the reforming passages 18 (the surface area of the region in which the reforming catalyst 22 is supported) contribute to the improvement in the conversion ratio.
- the plate portions 112 and the standing walls 114 do not change of the cross-sectional area of the reforming passages 18, the increase in the pressure loss relative to that of the heat exchange reformer unit 80 is avoided.
- FIG. 21A shows a heat exchange reformer unit 120 according to a seventh embodiment in a front view in section corresponding to FIG. 8A.
- the heat exchange reformer unit 120 differs from the heat exchange reformer unit 10 that includes the multilayer core unit 65 in which two layers of the reforming passages 18 are stacked per one unit plate member 50, in including a multilayer core unit 122 in which four unit plate members 50 (four layers of the reforming passages 18) are stacked per one unit plate member 51 (one layer of the combustion passage 20).
- the multilayer core unit 122 four layers of the reforming passages 18 are disposed between a pair of the combustion passages 20, as shown in FIG.
- two layer of the reforming passages 18 are disposed so as to be sandwiched between two layers of the reforming passages 18, each of which is, on any one side thereof, adjacent to a combustion passage 20 with a plate portion 52 interposed therebetween in the stacking direction, that is, so as not to be adjacent to the combustion passage 20 on either side of the concerned reforming passage 18.
- the ratio of volume of the reforming passages 18 to the overall volume is about 80%.
- the inner surface area, that is, the catalyst-supporting region area (supporting amount) of the combustion passages 20 is increased by about 60% as compared to that of the heat exchange reformer unit 200.
- the configuration of the heat exchange reformer unit 120 is the same as that of the heat exchange reformer unit 10. Accordingly, as in the case of the heat exchange reformer unit 10 according to the second embodiment, the heat exchange reformer unit 120 according to the seventh embodiment also makes it possible to match the total amount of the reforming reaction in the reforming passages 18 and the total amount of the combustion reaction in the combustion passages 20 (that is, to set the amount of reforming reaction and the amount of combustion reaction according to the reforming reaction field), and high space velocities are therefore achieved. That is, it is possible to improve reforming efficiency.
- the heat transfer-supporting ribs 92, the heat transfer-supporting thick portion 102, or both of the plate portions 112 and the standing walls 114 may be provided.
- the present invention is not limited to these embodiments.
- the present invention is not limited by applications as long as the heat exchange reformer unit is one of various heat exchange reformer units for obtaining gas that contains hydrogen from reformation material.
- the present invention is not limited by the configuration of the water supply system. For example, a configuration in which a water tank, water pipes, water vaporizer etc. are provided as a water supply system may be adopted.
- heat exchange reformer units 10, 80, 90, 100, 110 and 120 are each a parallel-flow heat exchange reformer unit
- present invention is not limited to the embodiments.
- the present invention may be applied to a cross-flow heat exchange reformer unit, for example.
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Engineering & Computer Science (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
Description
Claims
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP2006119751A JP4809113B2 (en) | 2006-04-24 | 2006-04-24 | Heat exchange type reformer |
JP2006126407A JP4809117B2 (en) | 2006-04-28 | 2006-04-28 | Heat exchange type reformer and reformer |
PCT/IB2007/001056 WO2007122497A2 (en) | 2006-04-24 | 2007-04-24 | Heat exchange reformer unit and reformer system |
Publications (1)
Publication Number | Publication Date |
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EP2013141A2 true EP2013141A2 (en) | 2009-01-14 |
Family
ID=38537793
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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EP07734374A Withdrawn EP2013141A2 (en) | 2006-04-24 | 2007-04-24 | Heat exchange reformer unit and reformer system |
Country Status (3)
Country | Link |
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US (1) | US20090064579A1 (en) |
EP (1) | EP2013141A2 (en) |
WO (1) | WO2007122497A2 (en) |
Families Citing this family (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US8268028B2 (en) * | 2007-03-26 | 2012-09-18 | Protonex Technology Corporation | Compositions, devices and methods for hydrogen generation |
FR2927323A3 (en) * | 2008-02-08 | 2009-08-14 | Renault Sas | System for the production of hydrogen loaded at an edge of a motor vehicle, comprises a catalytic reactor equipped with a subset comprising first and second coupled plates, a supply chamber, and an evacuation chamber |
KR101422630B1 (en) * | 2011-12-30 | 2014-07-23 | 두산중공업 주식회사 | Heat exchange type prereformer |
US11607657B2 (en) | 2012-02-06 | 2023-03-21 | Helbio S.A. | Heat integrated reformer with catalytic combustion for hydrogen production |
WO2013117948A1 (en) | 2012-02-06 | 2013-08-15 | Helbio Societé Anonyme Hydrogen And Energy Production Systems | Heat integrated reformer with catalytic combustion for hydrogen production |
CA3137624C (en) * | 2012-03-08 | 2023-06-20 | Helbio Societe Anonyme Hydrogen And Energy Production Systems | Catalytically heated fuel processor with replaceable structured supports bearing catalyst for fuel cell |
JP6192564B2 (en) * | 2014-02-18 | 2017-09-06 | 日新製鋼株式会社 | Plate heat exchanger and manufacturing method thereof |
US20170146305A1 (en) * | 2015-11-24 | 2017-05-25 | Hamilton Sundstrand Corporation | Header for heat exchanger |
JP6728751B2 (en) | 2016-02-23 | 2020-07-22 | 株式会社Ihi | Reactor and reaction system |
SE541284C2 (en) * | 2016-05-30 | 2019-06-11 | Alfa Laval Corp Ab | A plate heat exchanger |
Family Cites Families (8)
Publication number | Priority date | Publication date | Assignee | Title |
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US3926251A (en) * | 1973-02-16 | 1975-12-16 | Owens Illinois Inc | Recuperator structures |
AU2001212349B2 (en) * | 2000-10-27 | 2007-01-04 | Uop Llc | Process and apparatus using plate arrangement for reactant heating and preheating |
DE60203018T2 (en) * | 2001-10-12 | 2005-07-07 | Gtl Microsystems Ag | CATALYTIC REACTOR |
GB0124999D0 (en) * | 2001-10-18 | 2001-12-05 | Accentus Plc | Catalytic reactor |
GB0125035D0 (en) * | 2001-10-18 | 2001-12-12 | Accentus Plc | Catalytic reactor |
US7179313B2 (en) * | 2002-08-02 | 2007-02-20 | Catacel Corp. | Regenerative autothermal catalytic steam reformer |
KR100542201B1 (en) * | 2004-03-03 | 2006-01-10 | 삼성에스디아이 주식회사 | Reformer for fuel cell system and fuel cell system having thereof |
JP4254770B2 (en) * | 2005-09-08 | 2009-04-15 | カシオ計算機株式会社 | Reactor |
-
2007
- 2007-04-24 EP EP07734374A patent/EP2013141A2/en not_active Withdrawn
- 2007-04-24 WO PCT/IB2007/001056 patent/WO2007122497A2/en active Application Filing
- 2007-04-24 US US12/297,653 patent/US20090064579A1/en not_active Abandoned
Non-Patent Citations (1)
Title |
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See references of WO2007122497A2 * |
Also Published As
Publication number | Publication date |
---|---|
WO2007122497A3 (en) | 2008-01-17 |
US20090064579A1 (en) | 2009-03-12 |
WO2007122497A2 (en) | 2007-11-01 |
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