WO2020059783A1 - Électrode - Google Patents

Électrode Download PDF

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Publication number
WO2020059783A1
WO2020059783A1 PCT/JP2019/036710 JP2019036710W WO2020059783A1 WO 2020059783 A1 WO2020059783 A1 WO 2020059783A1 JP 2019036710 W JP2019036710 W JP 2019036710W WO 2020059783 A1 WO2020059783 A1 WO 2020059783A1
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fine powder
alloy
electrode
metal
transition metal
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PCT/JP2019/036710
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Japanese (ja)
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正己 奥山
鈴木　健治
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株式会社グラヴィトン
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
    • 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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/24—Chromium, molybdenum or tungsten
    • B01J23/26—Chromium
    • 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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/72—Copper
    • 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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74—Iron group metals
    • B01J23/745—Iron
    • 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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74—Iron group metals
    • B01J23/755—Nickel
    • 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
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
    • B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F3/00—Manufacture of workpieces or articles from metallic powder characterised by the manner of compacting or sintering; Apparatus specially adapted therefor ; Presses and furnaces
    • B22F3/10—Sintering only
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F5/00—Manufacture of workpieces or articles from metallic powder characterised by the special shape of the product
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/08—Alloys with open or closed pores
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C19/00—Alloys based on nickel or cobalt
    • C22C19/03—Alloys based on nickel or cobalt based on nickel
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C30/00—Alloys containing less than 50% by weight of each constituent
    • C22C30/02—Alloys containing less than 50% by weight of each constituent containing copper
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C33/00—Making ferrous alloys
    • C22C33/02—Making ferrous alloys by powder metallurgy
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
    • C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to an electrode used as an anode or a cathode.
  • a fuel cell electrode including a platinum catalyst in which platinum is supported on nitrogen-doped carbon obtained by firing a porous metal complex (PCP / MOF) containing zinc as a low-boiling metal (see Patent Document 1). Since this fuel cell electrode uses a porous metal complex (PCP / MOF) containing zinc, which is a low boiling point metal, as a raw material for production, the catalyst carrier is an NDC having a large specific surface area and containing almost no metal derived from the raw material. And a highly active platinum catalyst can be obtained by supporting a small amount of platinum. Further, since no metal derived from a porous metal complex (PCP / MOF), which is a raw material for production, is contained, firing conditions can be freely set. That is, by changing the organic compound linker of the porous metal complex (PCP / MOF) used as a raw material and adjusting the firing temperature, it is possible to control the nitrogen content and crystallinity in the obtained NDC.
  • PCP / MOF porous metal complex
  • platinum-supported carbons are widely used as electrode catalysts for polymer electrolyte fuel cells.
  • the platinum group element is a noble metal and is a scarce resource with a limited production amount. Therefore, it is required to reduce the amount of the platinum group element used. Further, with the spread of polymer electrolyte fuel cells in the future, development of inexpensive electrodes having a non-platinum catalyst using a metal other than expensive platinum is required.
  • An object of the present invention is to provide an electrode which can be produced at low cost without using a platinum group element and which can exhibit substantially the same catalytic activity (catalysis) as an electrode containing a platinum group element, and an electrode of the electrode. It is to provide a manufacturing method. Another object of the present invention is to enable a fuel cell to generate sufficient electricity, supply sufficient electric energy to a load connected to the fuel cell, and efficiently perform electrolysis in a hydrogen gas generator. An object of the present invention is to provide an electrode which can be performed well and can generate a large amount of hydrogen gas, and a method for manufacturing the electrode.
  • a first premise of the present invention for solving the above problem is an electrode used as an anode or a cathode.
  • the feature of the electrode of the present invention on the first premise is that the electrode is an austenitic stainless steel, a ferroalloy, and Cu which are selected so that the work function of a predetermined metal is close to the work function of a platinum group element.
  • Alloy-metal transition metal fine powder mixture obtained by uniformly mixing and dispersing stainless alloy fine powder obtained by finely pulverizing austenitic stainless steel, ferroalloy fine powder obtained by finely pulverizing ferroalloy, and Cu metal fine powder obtained by finely pulverizing Cu.
  • This is a porous alloy-metal transition metal thin plate electrode in which a large number of fine channels are formed by compressing and compressing into a thin plate having a predetermined area.
  • the weight ratio of the stainless alloy fine powder to the total weight of the alloy / metal transition metal powder mixture is in the range of 47 to 49%, and the total weight of the alloy / metal transition metal powder mixture is The weight ratio of the ferroalloy fine powder to the alloy is in the range of 47 to 49%, and the weight ratio of the Cu metal fine powder to the total weight of the alloy-metal transition metal fine powder mixture is in the range of 2 to 6%.
  • the thickness of the alloy-metal transition metal sheet electrode having a porous structure is in the range of 0.03 mm to 0.3 mm.
  • the porosity of the alloy-metal transition metal sheet electrode having a porous structure is in the range of 15% to 30%.
  • the density of the porous metal-metal transition metal plate electrode having a porous structure is in the range of 5.0 g / cm 2 to 7.0 g / cm 2 .
  • the particle size of the stainless alloy fine powder, the ferroalloy fine powder, and the Cu metal fine powder is in the range of 10 ⁇ m to 200 ⁇ m.
  • a Cu metal fine powder having the lowest melting point during firing of an alloy-metal transition metal fine powder mixture compressed into a thin plate having a predetermined area is used.
  • the stainless alloy fine powder and the ferroalloy fine powder are joined with the melted and melted Cu metal fine powder as a binder.
  • the austenitic stainless steel is at least one of SUS304, SUS316, and SUS340
  • the stainless alloy fine powder is SUS304 alloy fine powder, SUS316 alloy fine powder, SUS340 alloy fine powder.
  • ferroalloy is ferronickel (FeNi), ferromolybdenum (FeMo), ferromanganese (FeMn), ferrochrome (FeCr), ferrosilicon (FeSi), ferrotitanium (FeTi), ferroboron (FeB ), Ferromagnesium (FeMg), ferroniobium (FeNb), ferropanadium (FeV), and ferrotungsten (FeW), wherein the ferroalloy fine powder is ferronickel fine powder, ferro nickel fine powder, At least one of fine particles of ribene, fine powder of ferromanganese, fine powder of ferrochrome, fine powder of ferrosilicon, fine powder of ferrotitanium, fine powder of ferroboron, fine powder of ferromagnesium, fine powder of ferroniobium, fine powder of ferropanadium, and fine powder of ferrotungsten One.
  • ferroalloy fine powder is
  • a second premise of the present invention for solving the above-mentioned problem is an electrode manufacturing method for manufacturing an electrode used as an anode or a cathode.
  • the feature of the electrode manufacturing method of the present invention based on the second premise is that the electrode manufacturing method is an austenitic stainless steel selected such that a composite work function of a work function of a predetermined metal is close to a work function of a platinum group element.
  • austenitic stainless steel is finely pulverized to produce fine stainless alloy powder
  • ferroalloy is finely pulverized to produce ferroalloy fine powder
  • Cu is finely pulverized to produce Cu metal fine powder.
  • a stainless steel alloy, a ferroalloy fine powder, and a work function of a Cu metal fine powder produced in the body preparation step and the metal fine powder preparation step are combined so that the work function of the stainless alloy is close to the work function of the platinum group element.
  • Fine powder weight ratio which determines the weight ratio of fine powder, ferroalloy fine powder and Cu metal fine powder Alloy / metal transition metal to form an alloy / metal transition metal powder mixture by mixing and dispersing stainless alloy fine powder, ferroalloy fine powder, and Cu metal fine powder in the weight ratio determined by the constant step and the fine powder weight ratio determining step.
  • the alloy metal transition metal fine powder compact is formed by pressing the alloy metal transition metal fine powder mixture produced by the fine powder mixture production process and the alloy metal transition metal fine powder mixture production process at a predetermined pressure. A number of fine channels were formed by firing the alloy metal transition metal fine powder compact produced by the transition metal fine powder compact production process and the alloy metal transition metal fine powder compact production process at a predetermined temperature. And forming an alloy-metal transition metal sheet electrode having a porous structure.
  • the weight ratio of the stainless alloy fine powder to the total weight of the alloy / metal transition metal fine powder mixture is determined in the range of 47 to 49%
  • the weight ratio of the ferroalloy fine powder to the total weight of the metal transition metal fine powder mixture is determined in the range of 47 to 49%
  • the weight ratio of the Cu metal fine powder to the total weight of the alloy / metal transition metal fine powder mixture is 2 to 50%. Determine in the range of 6%.
  • the alloy / metal transition metal fine powder preparation step includes finely pulverizing austenitic stainless steel to a particle size of 10 ⁇ m to 200 ⁇ m and finely pulverizing ferroalloy to a particle size of 10 ⁇ m to 200 ⁇ m.
  • Cu is finely pulverized to a particle size of 10 ⁇ m to 200 ⁇ m.
  • the alloy-metal transition metal fine powder compact creation step is a step in which the alloy-metal transition metal fine powder mixture created by the alloy-metal transition metal fine powder mixture creation step is 500 MPa.
  • a compressed alloy metal transition metal powder having a thickness of 0.03 mm to 0.3 mm and a large number of fine channels is formed by pressurizing at a pressure of 800 MPa.
  • the alloy metal transition metal thin plate electrode making step firing the alloy metal transition metal fine powder compact at a temperature to melt the lowest melting point Cu metal fine powder, The stainless alloy fine powder and the ferroalloy fine powder are joined with the molten Cu metal fine powder as a binder.
  • the austenitic stainless steel is at least one of SUS304, SUS316, and SUS340
  • the stainless alloy fine powder is SUS304 alloy fine powder, SUS316 alloy fine powder, SUS340 alloy.
  • ferroalloy is ferronickel (FeNi), ferromolybdenum (FeMo), ferromanganese (FeMn), ferrochrome (FeCr), ferrosilicon (FeSi), ferrotitanium (FeTi), ferroboron (FeB), ferromagnesium (FeMg), ferroniobium (FeNb), ferropanadium (FeV), and ferrotungsten (FeW), wherein the ferroalloy fine powder is ferronickel fine powder.
  • ferroalloy fine powder is ferronickel fine powder.
  • At least one of ferromolybdenum fine powder, ferromanganese fine powder, ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, ferropanadium fine powder, and ferrotungsten fine powder is at least one of ferromolybdenum fine powder, ferromanganese fine powder, ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, ferropanadium fine powder, and ferrotungsten fine powder.
  • an austenitic stainless steel, a ferroalloy, and Cu (copper), which are selected so that the composite work function of the work function of a predetermined metal is close to the work function of a platinum group element, are used as raw materials.
  • Alloy-metal transition metal fine powder mixture obtained by uniformly mixing and dispersing a stainless alloy fine powder made of austenitic stainless steel, a ferroalloy fine powder made of a ferroalloy, and a Cu metal fine powder made of Cu, into a thin plate having a predetermined area.
  • the electrode is a non-platinum electrode made of austenitic stainless steel, ferroalloy, and Cu, does not use expensive platinum group elements, and can be manufactured at low cost.
  • the electrode Since the electrode exhibits substantially the same catalytic activity (catalysis) as an electrode containing a platinum group element, by using the electrode for the fuel cell, it is possible to generate sufficient electricity in the fuel cell, It is possible to supply sufficient electric energy to the load connected to the battery, and to use the electrodes in the hydrogen gas generator to efficiently perform electrolysis in the hydrogen gas generator. Hydrogen gas can be generated.
  • the weight ratio of the fine stainless alloy powder to the total weight of the alloy / metal transition metal fine powder mixture is in the range of 47 to 49%, and the weight ratio of the fine ferroalloy powder to the total weight of the alloy / metal transition metal fine powder mixture is 47 to 49%.
  • An electrode in the range of 49% and the weight ratio of the Cu metal fine powder to the total weight of the alloy-metal transition metal fine powder mixture in the range of 2 to 6% is based on the total weight of the alloy-metal transition metal fine powder mixture.
  • the work of synthesizing the work function of the stainless alloy fine powder, the ferroalloy fine powder, and the Cu metal fine powder can be approximated to the work function of the platinum group element.
  • Electrodes in which the weight ratio of stainless alloy fine powder, the weight ratio of ferroalloy fine powder, and the weight ratio of Cu metal fine powder with respect to the total weight of the alloy / metal transition metal fine powder mixture are within the above-mentioned range are electrodes containing a platinum group element. Since the catalyst exhibits substantially the same catalytic activity (catalysis) as that of the fuel cell, sufficient electricity can be generated in the fuel cell by using the electrode in the fuel cell, and sufficient electric energy is supplied to the load connected to the fuel cell. By using the electrode in a hydrogen gas generator, electrolysis can be efficiently performed in the hydrogen gas generator, and a large amount of hydrogen gas can be generated in a short time.
  • the electric resistance of the electrode can be reduced by setting the thickness of the electrode in the above range.
  • a current can be smoothly passed through the electrode.
  • Electrodes have almost the same catalytic activity (catalysis) as electrodes containing platinum group elements, and current flows smoothly through them.
  • Catalysis catalytic activity
  • the porosity of the porous alloy-metal transition metal sheet electrode is in the range of 15% to 30%
  • the porosity of the alloy-metal transition metal sheet electrode is set in the above range
  • the porous metal-alloy transition metal sheet electrode has the above porosity.
  • the transition metal sheet electrode is formed into a porous body having a large number of fine channels (passage holes), and the specific surface area of the transition metal sheet electrode can be increased.
  • the liquid can be brought into wide contact with the contact surface of the alloy / metal transition metal thin plate electrode, and the catalyst activity (catalytic action) substantially similar to that of the platinum group element can be surely exhibited.
  • the electrode can be used as a non-platinum anode or cathode which can utilize its catalytic function sufficiently and reliably and has excellent catalytic activity (catalytic activity).
  • An electrode having a density of the porous metal-metal transition metal sheet electrode having a porous structure in the range of 5.0 g / cm 2 to 7.0 g / cm 2 is obtained by setting the density of the alloy-metal transition metal sheet electrode within the above range.
  • An alloy-metal transition metal sheet electrode having a porous structure is formed into a porous material having a large number of fine channels (passage holes), and the specific surface area of the transition metal sheet electrode can be increased. Allows the gas or liquid to come into wide contact with the contact surface of the alloy-metal transition metal thin plate electrode while flowing, and can reliably exhibit the same catalytic activity (catalytic action) as the platinum group element.
  • the electrode can be used as a non-platinum anode or cathode which can utilize its catalytic function sufficiently and reliably and has excellent catalytic activity (catalytic activity).
  • the particle size of the stainless alloy fine powder, the ferroalloy fine powder, and the Cu metal fine powder is in the range of 10 ⁇ m to 200 ⁇ m
  • the particle size of the stainless alloy fine powder, the ferroalloy fine powder, and the Cu metal fine powder is in the above range.
  • Gas and liquid can be brought into wide contact with the contact surface of the alloy / metal transition metal thin plate electrode while gas and liquid flow through the flow path, and the catalyst activity (catalytic action) almost similar to that of platinum group elements can be reliably exhibited. can do.
  • the electrode can be used as a non-platinum anode or cathode which can utilize its catalytic function sufficiently and reliably and has excellent catalytic activity (catalytic activity).
  • the Cu metal fine powder having the lowest melting point is melted during firing of the alloy-metal transition metal fine powder mixture compressed into a thin plate having a predetermined area, and the molten Cu metal fine powder is melted.
  • An electrode in which a stainless alloy fine powder and a ferroalloy fine powder are joined as a binder is formed by joining a stainless alloy fine powder and a ferroalloy fine powder with a Cu metal fine powder having the highest melting point as a binder, thereby forming a large number of fine flow paths.
  • the electrode has high strength and can maintain its shape.
  • the electrode can maintain its shape, it can use its catalytic function sufficiently and reliably, and is suitably used as a non-platinum anode or cathode having excellent catalytic activity (catalytic activity). be able to.
  • the austenitic stainless steel is at least one of SUS304, SUS316 and SUS340
  • the stainless alloy fine powder is at least one of SUS304 alloy fine powder, SUS316 alloy fine powder and SUS340 alloy fine powder
  • the ferroalloy is ferronickel
  • ferroalloy fine powder is ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder, and ferrotungsten fine powder, wherein the ferroalloy fine powder is ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder,
  • the electrode which is at least one of ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, ferropanadium fine powder, and ferrotungsten fine powder, has a predetermined metal property.
  • SUS304, SUS316, and SUS340 selected so that the work function of the work function is close to the work function of the platinum group element, and ferronickel (FeNi), ferromolybdenum (FeMo), and ferromanganese (FeMn) , Ferrochrome (FeCr), ferrosilicon (FeSi), ferrotitanium (FeTi), ferroboron (FeB), ferromagnesium (FeMg), ferroniob (FeNb), ferropanadium (FeV), ferrotungsten (FeW) SUS304 alloy fine powder, SUS316 alloy fine powder, SUS340 alloy fine powder and at least one of ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder, ferrochrome fine powder, ferromagnetic powder An alloy in which at least one of silicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferronickel (F
  • -A metal alloy having a porous structure in which a metal transition metal fine powder mixture is compressed into a thin plate having a predetermined area and then fired to form a large number of fine channels.
  • -Metal transition metal thin plate electrodes, SUS304 alloy fine powder, SUS316 alloy fine powder Body, SUS340 alloy At least one of the fine powders, ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder, ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, The total alloy-metal transition metal powder mixture is adjusted so that the work function of the work function of at least one of ferropanadium fine powder and ferrotungsten fine powder and the Cu metal fine powder is close to the work function of the platinum group element.
  • the electrode Since the weight ratio of the fine powder of the stainless alloy, the weight ratio of the fine powder of the ferroalloy, and the weight ratio of the fine powder of Cu metal to the weight are determined, the electrode has substantially the same work function as the electrode containing the platinum group element. Can exhibit substantially the same catalytic activity (catalysis) as electrodes containing group-elements.
  • the medium functionality can be suitably used as an anode or a cathode of the non-platinum having a catalytic activity (catalytic) excellent be possible to utilize sufficiently and reliably.
  • austenitic stainless steel, ferroalloy, and Cu which are selected so that the work function of a predetermined metal is close to the work function of a platinum group element, are used as raw materials.
  • the weight ratio of the fine powder of the stainless alloy and the ferroalloy are adjusted so that the work function of the work function of the fine powder of the stainless alloy, the fine powder of the ferroalloy, and the fine powder of the Cu metal produced by the body forming process is close to the work function of the platinum group element.
  • Fine powder weight ratio determining step of determining the weight ratio of the fine powder and the weight ratio of the Cu metal fine powder, and determining the fine powder weight ratio An alloy-metal transition metal fine powder mixture producing step of mixing and dispersing a stainless alloy fine powder, a ferroalloy fine powder, and a Cu metal fine powder having a weight ratio determined by the above process, Pressing the alloy / metal transition metal fine powder mixture produced by the metal / transition metal fine powder mixture production process at a predetermined pressure to produce an alloy / metal transition metal fine powder compact; , Alloy-metal transition metal fine powder compacts produced by the process of making compressed metal-metal transition metal powder compacts are baked at a predetermined temperature to form a number of fine channels, forming a porous alloy-metal transition metal sheet.
  • the platinum group element is used.
  • a non-platinum electrode that is not used can be produced at low cost, and an electrode (anode or cathode) having excellent catalytic activity (catalysis) and capable of fully and reliably utilizing the catalytic function can be produced.
  • the method for manufacturing an electrode is to produce an electrode capable of generating sufficient electricity in a fuel cell because the electrode produced by the electrode exhibits substantially the same catalytic activity (catalysis) as an electrode containing a platinum group element.
  • a non-platinum electrode capable of efficiently performing electrolysis in a hydrogen gas generator and generating a large amount of hydrogen gas in a short time can be produced.
  • the weight ratio of the stainless alloy fine powder to the total weight of the alloy / metal transition metal fine powder mixture is determined in the range of 47 to 49%, and the alloy / metal transition metal fine powder mixture is determined.
  • the weight ratio of the Cu metal fine powder to the total weight of the alloy-metal transition metal fine powder mixture is determined in the range of 2 to 6%.
  • the electrode manufacturing method is to determine the weight ratio of the stainless alloy fine powder, the ferroalloy fine powder, the weight ratio of the Cu metal fine powder to the total weight of the alloy-metal transition metal fine powder mixture, and the weight ratio of the Cu metal fine powder within the above range.
  • the work function of the alloy fine powder, ferroalloy fine powder, and Cu metal fine powder Function and has almost the same work function as an electrode containing a platinum group element, and can exhibit almost the same catalytic activity (catalysis) as an electrode containing a platinum group element, and has excellent catalytic activity. It is possible to produce an electrode (anode or cathode) that has (catalysis) and can utilize the catalytic function sufficiently and reliably.
  • the method for manufacturing an electrode is to produce an electrode capable of generating sufficient electricity in a fuel cell because the electrode produced by the electrode exhibits substantially the same catalytic activity (catalysis) as an electrode containing a platinum group element.
  • a non-platinum electrode capable of efficiently performing electrolysis in a hydrogen gas generator and generating a large amount of hydrogen gas in a short time can be produced.
  • An electrode manufacturing method in which a metal fine powder preparation step pulverizes austenitic stainless steel to a particle size of 10 ⁇ m to 200 ⁇ m, finely pulverizes ferroalloy to a particle size of 10 ⁇ m to 200 ⁇ m, and finely pulverizes Cu to a particle size of 10 ⁇ m to 200 ⁇ m.
  • a metal alloy having a porous structure having a large specific surface area by finely pulverizing austenitic stainless steel, ferroalloy, or Cu to a particle diameter in the above range, thereby forming a porous body having a large number of fine channels (passage holes).
  • transition metal sheet electrodes It is possible to make transition metal sheet electrodes, and it is possible to make the gas and liquid flow widely through the flow path of the gas and liquid to the contact surface of the alloy / transition metal sheet electrode.
  • An electrode anode or cathode capable of reliably exhibiting substantially the same catalytic activity (catalytic action) can be produced, and excellent catalytic activity (catalytic action) can be obtained.
  • the catalytic function can make a non-platinum electrodes that can be utilized sufficiently and reliably with a use).
  • the alloy / transition metal fine powder compact creation step is performed by applying a pressure of 500 Mpa to 800 Mpa to the alloy / metal transition metal fine powder mixture produced in the alloy / transition metal fine powder mixture creation step, and applying a pressure of 0.03 mm to 0.3 mm.
  • the method for producing an alloy-metal transition metal fine powder compact having a large number of fine channels with a thickness dimension of the thickness is performed by pressurizing (compressing) the alloy-metal transition metal fine powder mixture under a pressure in the above range. ), It is possible to produce an alloy / metal transition metal fine powder compact having a thickness of 0.03 mm to 0.3 mm and a large number of fine channels (passage holes), using a platinum group element.
  • Non-platinum porous metal-metal transition metal electrode with non-platinum structure can be manufactured at low cost, has excellent catalytic activity (catalytic action), and uses the catalytic function sufficiently and reliably You can make the electrode (anode or cathode) capable.
  • the electrode manufacturing method an electrode having a thickness in the range of 0.03 mm to 0.3 mm can be formed, so that the electric resistance can be reduced and an electrode (anode or anode) capable of flowing a current smoothly can be obtained. Cathode).
  • the alloy / metal transition metal thin plate electrode making process involves firing the alloy / metal transition metal fine powder compact at a temperature at which the Cu metal fine powder having the lowest melting point is melted, and using the molten Cu metal fine powder as a binder to form a stainless alloy fine powder.
  • An electrode manufacturing method for joining ferroalloy fine powder is a method of joining a stainless alloy fine powder and a ferroalloy fine powder using a Cu metal fine powder having the highest melting point as a binder, thereby forming a porous material having a large number of fine channels (passage holes).
  • the austenitic stainless steel is at least one of SUS304, SUS316 and SUS340
  • the stainless alloy fine powder is at least one of SUS304 alloy fine powder, SUS316 alloy fine powder and SUS340 alloy fine powder
  • the ferroalloy is ferronickel
  • the electrode manufacturing method is at least one of ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, ferropanadium fine powder, and ferrotungsten fine powder.
  • SUS304, SUS316, and SUS340 selected so that the work function of the metal of the metal of the present invention is close to the work function of the platinum group element, and ferronickel (FeNi), ferromolybdenum (FeMo), and ferromanganese ( FeMn), ferrochrome (FeCr), ferrosilicon (FeSi), ferrotitanium (FeTi), ferroboron (FeB), ferromagnesium (FeMg), ferroniobium (FeNb), ferropanadium (FeV), ferrotungsten (Fe ) And Cu as raw materials, at least one of SUS304 alloy fine powder, SUS316 alloy fine powder, and SUS340 alloy fine powder as stainless alloy fine powder, and ferronickel fine powder as ferroalloy fine powder.
  • a metal fine powder preparation step a fine powder weight ratio determining step, an alloy / metal transition metal fine powder mixture preparation step, an alloy / metal transition metal fine powder compaction preparation step, an alloy / metal transition metal sheet
  • Electrode anode or cathode
  • FIG. 3 is a partially enlarged front view showing an example of an electrode.
  • FIG. 9 is a partially enlarged front view showing another example of an electrode.
  • FIG. 3 is an exploded perspective view showing an example of a cell using electrodes.
  • FIG. 4 is a side view of a cell using electrodes. The figure explaining the electric power generation of the polymer electrolyte fuel cell using the electrode. The figure which shows the result of the electromotive force test of an electrode. The figure which shows the result of the IV characteristic test of an electrode. The figure explaining the electrolysis of the hydrogen gas generator using an electrode.
  • FIG. 4 is a diagram illustrating a method for manufacturing an electrode.
  • FIG. 1 is a perspective view of the electrode 10 shown as an example.
  • FIG. 2 is a partially enlarged front view showing an example of the electrode 10
  • FIG. 3 is a partially enlarged front view shown as another example of the electrode 10.
  • the thickness direction is indicated by an arrow X
  • the radial direction is indicated by an arrow Y.
  • the electrode 10 is used as an anode (anode fuel electrode 21) or a cathode (cathode air electrode 22).
  • the electrode 10 has a front surface 11 and a rear surface 12, has a predetermined area and a predetermined thickness L1, and has a square planar shape.
  • the electrode 10 is an alloy-metal transition metal thin plate electrode 14 having a porous structure (porous) having a number of fine channels 13 (passage holes). Gas or liquid flows through the flow path 13 (passage hole).
  • the planar shape of the electrode 10 is not particularly limited, and can be formed into any other planar shape such as a circle, an ellipse, and a polygon according to the application in addition to a square.
  • the electrode 10 (alloy metal transition metal thin plate electrode 14 having a porous structure) has a work function of a predetermined metal (energy required for extracting electrons from a substance) having a work function of a platinum group element (5.65 eV). ) Are selected from austenitic stainless steel 42 (alloy transition metal), ferroalloy 43 (alloy iron), and Cu44 (copper) (metal transition metal).
  • austenitic stainless steel 42 at least one of SUS304, SUS316 and SUS340 is used.
  • SUS304 is preferably used, but any of SUS316, SUS340, SUS304 + SUS316, SUS304 + SUS340, SUS304 + SUS316 + SUS340 can also be used.
  • Ferroalloy 43 includes ferronickel (FeNi), ferromolybdenum (FeMo), ferromanganese (FeMn), ferrochrome (FeCr), ferrosilicon (FeSi), ferrotitanium (FeTi), ferroboron (FeB), and ferromagnesium (FeMg). , Ferroniobium (FeNb), ferropanadium (FeV), and ferrotungsten (FeW). As the ferroalloy 43, it is preferable to use ferronickel (FeNi) or ferromolybdenum (FeMo), but it is also possible to use another type or a combination thereof.
  • the electrode 10 is made of a stainless alloy fine powder 45 (fine austenitic stainless steel) obtained by finely pulverizing the austenitic stainless steel 42, a ferroalloy fine powder 46 (fine powdered ferroalloy) obtained by finely pulverizing the ferroalloy 43, and a Cu metal obtained by finely pulverizing Cu 44.
  • An alloy-metal transition metal fine powder mixture 48 in which fine powder 47 (fine powder Cu) is uniformly mixed and dispersed is compressed into a thin plate having a predetermined area to form an alloy-metal transition metal fine powder compressed product 49, and the alloy is formed.
  • -It is made by firing the compressed metal transition metal fine powder 49 (see FIG. 10).
  • the stainless alloy fine powder 45 at least one of SUS304 alloy fine powder, SUS316 alloy fine powder, and SUS340 alloy fine powder is used.
  • As the stainless alloy fine powder 45 it is preferable to use SUS304 alloy fine powder (fine powder SUS304) obtained by finely pulverizing SUS304.
  • SUS316 alloy fine powder fine SUS316 obtained by finely pulverizing SUS316 and SUS340 are preferably used. Any of crushed SUS340 alloy fine powder (fine SUS340), SUS304 alloy fine powder + SUS316 alloy fine powder, SUS304 alloy fine powder + SUS340 alloy fine powder, SUS304 alloy fine powder + SUS316 alloy fine powder + SUS340 alloy fine powder Can also.
  • Ferroalloy fine powder 46 includes ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder, ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, At least one of a fine powder of vanadium and a fine powder of ferrotungsten are used.
  • ferroalloy fine powder 46 it is preferable to use a ferronickel fine powder or a ferromolybdenum fine powder, but it is also possible to use another type or a combination thereof.
  • the Cu metal fine powder 47 having the lowest melting point is melted when the alloy metal fine powder mixture 48 compressed into a thin plate having a predetermined area is melted and melted.
  • the stainless alloy fine powder 45 and the ferroalloy fine powder 46 are joined using the obtained Cu metal fine powder 47 as a binder.
  • the melting point of Cu44 is 1084.5 ° C.
  • the work function of the stainless alloy fine powder 45 at least one of SUS304 alloy fine powder, SUS316 alloy fine powder, and SUS340 alloy fine powder
  • the ferroalloy fine powder Body 46 ferroalloy fine powder Body 46
  • ferroalloy fine powder body 46 ferroalloy fine powder Body 46
  • the alloy / metal transition metal fine powder mixture 48 so that the composite work function of the work function of at least one of the ferrotungsten fine powder) and the work function of the Cu metal fine powder 47 approximates the work function of the platinum group element.
  • the weight ratio of the fine powder 45 is determined, the weight ratio of the ferroalloy fine powder 46 to the total weight of the alloy-metal transition metal fine powder mixture 48 is determined, and the weight ratio of the alloy-metal transition metal fine powder mixture 48 to the total weight is determined.
  • the weight ratio of the Cu metal fine powder 47 is determined.
  • the weight ratio of the stainless alloy fine powder 45 to the total weight (100%) of the alloy / metal transition metal fine powder mixture 48 is in the range of 47 to 49%, and preferably 48%.
  • the weight ratio of the ferroalloy fine powder 46 to the total weight (100%) of the alloy / metal transition metal fine powder mixture 48 is in the range of 47 to 49%, preferably 48%.
  • the weight ratio of the Cu metal fine powder 47 to the total weight (100%) of the alloy-metal transition metal fine powder mixture 48 is in the range of 2 to 6%, preferably 4%.
  • the composite work function of the fine powders 45 to 47 becomes the work function of the platinum group element.
  • the electrode 10 formed by compressing and firing the alloy / metal transition metal fine powder mixture 48 exhibits substantially the same catalytic activity (catalysis) as an electrode containing a platinum group element. Can not.
  • a large number of fine channels 13 (passage holes) having different diameters are formed in the electrode 10 (porous structure alloy / metal transition metal thin plate electrode 14).
  • the electrode 10 has a large specific surface area because a large number of fine channels 13 (passage holes) are formed.
  • Each of the flow paths 13 (passage holes) has a plurality of flow openings 15 opening to the front surface 11 and a plurality of flow openings 17 opening to the rear surface 12.
  • the electrode 10 penetrates from the front surface 11 toward the rear surface 12 between the electrode 10 and the twelve flow openings 17.
  • the flow paths 13 extend between the front surface 11 and the rear surface 12 of the electrode 10 while bending irregularly in the thickness direction of the electrode 10, and extend from the outer peripheral edge 16 of the electrode 10 toward the center. It extends while bending in the direction irregularly.
  • the flow paths 13 that are adjacent to each other in the radial direction and that bend in the thickness direction are partially connected in the radial direction, and the one flow path 13 and the other flow path 13 communicate with each other.
  • the flow paths 13 that are adjacent to each other in the thickness direction and bent in the radial direction are partially connected in the thickness direction, and one flow path 13 and the other flow path 13 communicate with each other.
  • the opening areas (opening diameters) of the flow paths 13 are not uniform in the thickness direction, are irregularly changed in the thickness direction, and are not uniform in the radial direction. , Changing irregularly in the radial direction.
  • the channels 13 are irregularly opened in the thickness direction and the radial direction while the opening area (opening diameter) is increased or decreased. Further, the opening area (opening diameter) of the opening 15 on the front surface 11 and the opening 15 on the rear surface 12 are not uniform, and the areas are all different.
  • the opening diameters of the flow paths 13 (passage holes) and the opening diameters of the flow openings 15 on the front and rear surfaces 11 and 12 are in the range of 1 ⁇ m to 100 ⁇ m.
  • the electrode 10 (porous structure alloy / metal transition metal sheet electrode 14) has a thickness L1 in the range of 0.03 mm to 0.3 mm, preferably in the range of 0.05 mm to 0.1 mm. If the thickness L1 of the electrode 10 is less than 0.03 mm, the strength is reduced, and the electrode 10 may be easily damaged or damaged when an impact is applied, and the shape may not be maintained. When the thickness L1 of the electrode 10 exceeds 0.3 mm, the electric resistance of the electrode 10 increases, the current does not flow smoothly to the electrode 10, and when the electrode 10 is used in the polymer electrolyte fuel cell 18, Sufficient electricity cannot be generated in the battery 18, and sufficient electric energy cannot be supplied to the load 30 connected to the fuel cell 18. In addition, when the electrode 10 is used in the hydrogen gas generator 31, electrolysis cannot be performed efficiently, and the hydrogen gas generator 31 cannot generate a large amount of hydrogen gas in a short time.
  • the thickness of the electrode 10 is in the range of 0.03 mm to 0.3 mm, preferably 0.05 mm to 0.1 mm. Has high strength and can maintain its shape, and can prevent damage or damage to the electrode 10 when an impact is applied to the electrode 10. Further, the electric resistance of the electrode 10 can be reduced, the current flows smoothly through the electrode 10, and the fuel cell 18 generates sufficient electricity when the electrode 10 ⁇ / b> A is used in the polymer electrolyte fuel cell 18. Thus, sufficient electric energy can be supplied to the load 30 connected to the fuel cell 18. Further, when the electrode 10 is used in the hydrogen gas generator 31, electrolysis can be efficiently performed, and the hydrogen gas generator 31 can generate a large amount of hydrogen gas in a short time.
  • the porosity of the electrode 10 is in the range of 15% to 30%, preferably 20% to 25%, and the relative density thereof is 70% to 85%. %, Preferably in the range of 75% to 80%. If the porosity of the electrode 10 is less than 15% and the relative density exceeds 85%, a large number of fine channels 13 (passage holes) are not formed in the electrode 10, and the specific surface area of the electrode 10 may be increased. Can not.
  • the porosity of the electrode 10 exceeds 30% and the relative density is less than 70%, the opening area (opening diameter) of the flow path 13 (passage hole) and the opening area (opening) of the flow opening 15 of the front and rear surfaces 11 and 12 are increased. The diameter of the electrode 10 becomes larger than necessary, the strength of the electrode 10 is reduced, and the electrode 10 may be easily damaged or damaged when an impact is applied, and the shape may not be maintained.
  • the electrode 10 Since the porosity and the relative density of the electrode 10 (alloy-metal transition metal thin plate electrode 14 having a porous structure) are within the above-mentioned ranges, the electrode 10 has a large number of fine channels 13 (passages) having different opening areas (opening diameters). (Pores) and a large number of fine front and rear surfaces 11, 12 having different opening areas (opening diameters).
  • the gas or the liquid can be brought into wide contact with the contact surfaces of the flow path 13 of the electrode 10 while the gas or the liquid flows through the passage hole).
  • the electrode 10 (alloy metal transition metal thin plate electrode 14 having a porous structure) has a density in the range of 5.0 g / cm 2 to 7.0 g / cm 2 , preferably 5.5 g / cm 2 to 6.5 g / cm 2. cm 2 .
  • the density of the electrode 10 is less than 5.0 g / cm 2 , the strength of the electrode 10 is reduced, and the electrode 10 is easily damaged or damaged when an impact is applied, and the shape may not be maintained. . If the density of the electrode 10 exceeds 7.0 g / cm 2 , a large number of fine channels 13 (passage holes) are not formed in the electrode 10 and the specific surface area of the electrode 10 cannot be increased.
  • the electrode 10 (alloy-metal transition metal thin plate electrode 14 having a porous structure) has a density within the above range, the electrode 10 has a large number of fine channels 13 (passage holes) and openings having different opening areas (opening diameters).
  • the electrode 10 is formed into a porous shape having a large number of fine front and rear surfaces 11 and 12 having different areas (opening diameters), and the specific surface area of the electrode 10 can be increased.
  • the gas or liquid can be brought into wide contact with the contact surface of the electrode 10 in the flow path 13 while the gas or liquid flows.
  • the particle size of the stainless alloy fine powder 45 (at least one of SUS304 alloy fine powder, SUS316 alloy fine powder and SUS340 alloy fine powder) and ferroalloy fine powder 46 (ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder) Body, ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, ferropanadium fine powder, ferrotungsten fine powder), particle size of Cu)
  • the particle size of the metal fine powder 47 is in the range of 10 ⁇ m to 200 ⁇ m.
  • the flow path 13 (passage hole) is closed by the fine powders 45 to 47, and the electrode 10 has many fine particles.
  • the flow path 13 cannot be formed, and the specific surface area of the electrode 10 (porous alloy / metal transition metal thin plate electrode 14) cannot be increased. If the particle diameter of the stainless alloy fine powder 45, the ferroalloy fine powder 46, or the Cu metal fine powder 47 exceeds 200 ⁇ m, the opening area (opening diameter) of the flow passage 13 (passage hole) and the flow openings 15 of the front and rear surfaces 11, 12 are increased.
  • the opening area (opening diameter) of the electrode 10 becomes unnecessarily large, so that a large number of fine channels 13 cannot be formed in the electrode 10, and the specific surface area of the electrode 10 (alloy / metal transition metal thin plate electrode 14 having a porous structure) Cannot be increased.
  • the electrode 10 has an opening area (open area). It is molded into a porous structure having a large number of fine flow paths 13 (passage holes) having different diameters and a large number of fine front and rear surfaces 11 and 12 having different opening areas (opening diameters). The surface area can be increased, and the gas and the liquid can be brought into wide contact with the contact surface of the electrode 10 in the flow channel 13 while the gas and the liquid flow through the flow channel.
  • FIG. 4 is an exploded perspective view showing an example of the cell 17 using the electrode 10
  • FIG. 5 is a side view of the cell 17 using the electrode 10.
  • FIG. 6 is a diagram illustrating the power generation of the polymer electrolyte fuel cell 18 using the electrode 10
  • FIG. 7 is a diagram illustrating the result of an electromotive force test of the electrode 10.
  • FIG. 8 is a diagram showing a result of an IV characteristic test of the electrode 10.
  • a fuel electrode 19 (anode) using the electrode 10
  • an air electrode 20 (cathode) using the electrode 10
  • a fuel electrode 19 and air A solid polymer electrolyte membrane 21 interposed between the poles 20 (a pole assembly membrane) (fluorine-based ion exchange membrane), a separator 22 (bipolar plate) positioned outside the fuel electrode 19 in the thickness direction, and a thickness outside the air electrode 20
  • a separator 23 (bipolar plate) positioned at A supply channel for a reaction gas (hydrogen, oxygen, or the like) is formed (engraved) in the separators 22 and 23.
  • the fuel electrode 19, the air electrode 20, and the solid polymer electrolyte membrane 21 are overlapped and integrated in the thickness direction to form a membrane / electrode assembly 24 (Membrane Electrode Assembly, MEA).
  • MEA Membrane Electrode Assembly
  • the membrane / electrode assembly 24 is sandwiched between the separators 22 and 23.
  • a plurality of cells 17 overlap in one direction and are connected in series to form a cell stack (fuel cell stack).
  • the solid polymer electrolyte membrane 21 has proton conductivity and does not have electronic conductivity.
  • a gas diffusion layer 25 is formed between the fuel electrode 19 and the separator 22, and a gas diffusion layer 26 is formed between the air electrode 20 and the separator 23.
  • a gas seal 27 is provided between the fuel electrode 19 and the separator 22 and above and below the gas diffusion layer 26.
  • a gas seal 28 is provided between the air electrode 20 and the separator 23 and above and below the gas diffusion layer 26.
  • hydrogen (fuel) is supplied to the fuel electrode 19 (electrode 10), and air (oxygen) is supplied to the air electrode 20 (electrode 10).
  • hydrogen is decomposed into protons (hydrogen ions, H + ) and electrons by a reaction (catalysis) of H 2 ⁇ 2H + + 2e ⁇ .
  • the protons move to the air electrode 20 (electrode 10) through the solid polymer electrolyte membrane 21, and the electrons move to the air electrode 20 through the conductive wire 29.
  • Protons generated at the fuel electrode 19 flow through the solid polymer electrolyte membrane 21.
  • the protons transferred from the solid polymer electrolyte membrane 21 and the electrons transferred on the conductive wire 29 react with oxygen in the air, and water is generated by the reaction of 4H + + O 2 + 4e ⁇ 2H 2 O.
  • the fuel electrode 19 (electrode 10) and the air electrode 20 (electrode 10) are made of an austenitic stainless steel 42 (alloy transition metal) and a ferroalloy 43, which are selected so that the composite work function of the work function is close to the work function of a platinum group element.
  • stainless steel fine powder 45 at least one of SUS304 alloy fine powder, SUS316 alloy fine powder, SUS340 alloy fine powder
  • ferroalloy fine powder 46 Ferronickel fine powder, Ferromolybdenum fine powder, Ferromanganese fine powder, Ferrochrome fine powder, Ferrosilicon fine powder, Ferrotitanium fine powder, Ferroboron fine powder, Ferromagnesium fine powder, Ferroniob fine powder, Ferropanadium fine powder, Ferrotungsten fine powder At least one of the bodies
  • the weight ratio of the stainless alloy fine powder 45 to the total weight of the alloy-metal transition metal fine powder mixture 48 and the ferroalloy fine powder are set such that the work function of the work function with the u-metal fine powder 47 is close to the work function of the platinum group element.
  • the fuel electrode 19 and the air electrode 20 have substantially the same work function as the electrode containing the platinum group element and contain the platinum group element.
  • the catalyst exhibits catalytic activity (catalysis) substantially similar to that of an electrode, and hydrogen is efficiently decomposed into protons and electrons.
  • the electrode 10 is made of an austenitic stainless steel 42 (at least one of SUS304, SUS316, and SUS340) (alloy transition) selected such that the work function of a predetermined metal is close to the work function of a platinum group element.
  • Metal and ferroalloy 43 (ferronickel (FeNi), ferromolybdenum (FeMo), ferromanganese (FeMn), ferrochrome (FeCr), ferrosilicon (FeSi), ferrotitanium (FeTi), ferroboron (FeB), ferromagnesium (FeMg) ), Ferroniobium (FeNb), ferropanadium (FeV), and ferrotungsten (FeW)) (alloy iron) and Cu44 (metal transition metal) as raw materials, and stainless steel made from austenitic stainless steel 42.
  • ferroalloy 43 ferrronickel (FeNi), ferromolybdenum (
  • a B Fine powder 45 (at least one of SUS304 alloy fine powder, SUS316 fine powder and SUS340 fine powder) and ferroalloy fine powder 46 (ferronickel fine powder, ferromolybdenum fine powder, ferroalloy fine powder) made of ferroalloy 43 At least one of manganese fine powder, ferrochrome fine powder, ferrosilicon fine powder, ferrotitanium fine powder, ferroboron fine powder, ferromagnesium fine powder, ferroniob fine powder, ferropanadium fine powder, ferrotungsten fine powder) and Cu44 ( An alloy / metal transition metal fine powder mixture 48 in which a Cu metal fine powder 47 made of copper) is uniformly mixed and dispersed, is compressed into a thin plate having a predetermined area, and then fired to form a large number of fine channels 13.
  • the alloy / metal transition metal fine powder mixture 48 is prepared such that the work function of the stainless steel alloy fine powder 45, the ferroalloy fine powder 46, and the Cu metal fine powder 47 is close to the work function of the platinum group element. Since the weight ratio of the stainless alloy fine powder 45, the weight ratio of the ferroalloy fine powder 46, and the weight ratio of the Cu metal fine powder 47 to the total weight are determined, the electrode 10 has substantially the same work as the electrode containing the platinum group element. It has a function and can exhibit almost the same catalytic activity (catalytic action) as an electrode containing a platinum group element. ) Can be suitably used as a non-platinum anode or cathode.
  • the electrode 10 (alloy-metal transition metal thin plate electrode 14 having a porous structure) exhibits almost the same catalytic activity (catalysis) as an electrode containing a platinum group element
  • the electrode 10 is formed of a polymer electrolyte fuel cell 21. In this case, sufficient electricity can be generated in the fuel cell 21, and sufficient electric energy can be supplied to the load 30 connected to the fuel cell 21.
  • the electrode 10 is made of austenitic stainless steel, ferroalloy, and Cu, does not use an expensive platinum group element, and has a non-platinum fuel electrode 19 (anode) used for the polymer electrolyte fuel cell 21.
  • the cathode 20 (cathode) can be manufactured at low cost.
  • FIG. 9 is a diagram for explaining the electrolysis of the hydrogen gas generator 31 using the electrode 10.
  • an anode 32 anode
  • a cathode 33 cathode
  • an anode 32 and a cathode 33 a solid polymer electrolyte membrane 34 (electrode assembly membrane) (fluorine-based ion exchange membrane)
  • anode power supply member 35 and a cathode power supply member 36 an anode water reservoir 37 and a cathode water reservoir 38
  • An anode main electrode 39 and a cathode main electrode 40 An anode main electrode 39 and a cathode main electrode 40.
  • the anode 32, the cathode 33, and the solid polymer electrolyte membrane 34 are overlapped and integrated in the thickness direction to form a membrane / electrode assembly 41 (Membrane Electrode Assembly, MEA). 41 is sandwiched between an anode power supply member 35 and a cathode power supply member 36.
  • the solid polymer electrolyte membrane 34 has proton conductivity and does not have electron conductivity.
  • the anode power supply member 35 is located outside the anode 32 and is in close contact with the anode 32, and supplies a positive current to the anode 32.
  • the anode water storage tank 37 is located outside the anode power supply member 35 and is in close contact with the anode power supply member 35.
  • the anode main electrode 39 is located outside the anode water storage tank 37 and supplies a positive current to the anode power supply member 35.
  • the cathode power supply member 36 is located outside the cathode 33 and is in close contact with the cathode 33, and supplies a negative current to the cathode 33.
  • the cathode water tank 38 is located outside the cathode power supply member 36 and is in close contact with the cathode power supply member 36.
  • the cathode main electrode 40 is located outside the cathode water storage tank 38 and supplies a negative current to the cathode power supply member 36.
  • water H 2 O
  • cathode water storage tank 38 water (H 2 O) is supplied to the anode water storage tank 37 and the cathode water storage tank 38 as shown by arrows in FIG.
  • a negative current is supplied from the power supply to the cathode main electrode 40.
  • the + current supplied to the anode main electrode 39 is supplied from the anode power supply member 35 to the anode 32 (anode), and the-current supplied to the cathode main electrode 40 is supplied from the cathode power supply member 36 to the cathode 33 (cathode). Is done.
  • the electrode 10 is made of an austenitic stainless steel 42 using austenitic stainless steel 42, ferroalloy 43, and Cu 44, which are selected so that the work function of the work function of a predetermined metal is close to the work function of a platinum group element.
  • An alloy / transition metal fine powder mixture 48 in which a ferroalloy fine powder 46 made of ferroalloy 43 and a ferroalloy fine powder 46 made of ferroalloy 43 and a Cu metal fine powder 47 made of Cu44 (copper) are uniformly mixed and dispersed to a predetermined area.
  • the electrode 10 is an electrode containing a platinum group element. It has substantially the same work function as that of an electrode containing a platinum group element and can exhibit substantially the same catalytic activity (catalysis) as that of an electrode containing a platinum group element. It can be suitably used as the non-platinum anode 32 or cathode 33 having catalytic activity (catalytic action).
  • the electrode 10 (alloy / transition metal thin plate electrode 14 having a porous structure) exhibits substantially the same catalytic activity (catalysis) as an electrode containing a platinum group element, the electrode 10 is used for the hydrogen gas generator 31.
  • electrolysis can be efficiently performed in the hydrogen gas generator 31, and a large amount of hydrogen gas can be generated in a short time.
  • the electrode 10 is made of an austenitic stainless steel 42, a ferroalloy 43, and Cu44, does not use an expensive platinum group element, and uses a non-platinum anode 32 and a cathode 33 used for the hydrogen gas generator 31 at low cost. Can be made.
  • FIG. 10 is a view for explaining a method of manufacturing the electrode 10.
  • the electrode 10 includes a metal fine powder forming step S1, a fine powder weight ratio determining step S2, an alloy / metal transition metal fine powder mixture forming step S3, and an alloy / metal transition metal fine powder compact forming step S4.
  • the electrode manufacturing method includes an austenitic stainless steel 42 (at least one of SUS304, SUS316 and SUS340) (alloy) selected such that the work function of a predetermined metal is close to the work function of a platinum group element.
  • the electrode 10 is manufactured using at least one of FeMg), ferroniobium (FeNb), ferropanadium (FeV), and ferrotungsten (FeW) (alloy iron) and Cu44 (metal transition metal) as raw materials.
  • the austenitic stainless steel 42 is finely pulverized and finely divided into stainless alloy fine powder 45 (SUS304 alloy fine powder (fine powder SUS304), SUS316 alloy fine powder (fine powder SUS316), and SUS340 alloy fine powder ( At least one of finely powdered SUS 340), and ferroalloy 43 is finely pulverized to obtain a ferroalloy fine powder 46 (ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder, ferrochrome fine powder, ferrosilicon fine powder).
  • stainless alloy fine powder 45 SUS304 alloy fine powder (fine powder SUS304), SUS316 alloy fine powder (fine powder SUS316), and SUS340 alloy fine powder ( At least one of finely powdered SUS 340)
  • ferroalloy 43 is finely pulverized to obtain a ferroalloy fine powder 46 (ferronickel fine powder, ferromolybdenum fine powder, ferromanganese fine powder, fer
  • the austenitic stainless steel 42 (at least one of SUS304, SUS316 and SUS340) is finely pulverized to a particle size of 10 ⁇ m to 200 ⁇ m by a fine pulverizer, and the ferroalloy 43 (ferronickel) is pulverized by the fine pulverizer.
  • FeNi ferromolybdenum
  • FeMn ferromanganese
  • FeCr ferrosilicon
  • FeSi ferrrotitanium
  • FeB ferroboron
  • FeMg ferroboron
  • FeMg ferroboron
  • FeNb ferro
  • At least one of panadium (FeV) and ferrotungsten (FeW)) is finely pulverized to a particle size of 10 ⁇ m to 200 ⁇ m
  • Cu44 is finely pulverized by a fine pulverizer to a particle size of 10 ⁇ m to 200 ⁇ m.
  • the electrode is manufactured by finely pulverizing austenitic stainless steel 42, ferroalloy 43, and Cu44 to a particle diameter of 10 ⁇ m to 200 ⁇ m, thereby forming a porous body having a large number of fine channels 13 (passage holes) and a specific surface area.
  • An alloy-metal transition metal thin plate electrode 14 having a large porous structure can be formed, and gas or liquid flows through the flow passages 13 while the gas or liquid flows through the flow passages 13 of the electrode 10 (alloy-transition metal thin plate electrode 14).
  • the electrode 10 that can be brought into wide contact with the contact surface in can be manufactured.
  • the work function of the work function of the austenitic alloy fine powder 45, the ferroalloy fine powder 46, and the Cu metal fine powder 47 produced in the fine metal powder preparation step is changed to the work function of the platinum group element.
  • the weight ratio of the austenitic alloy fine powder 45 to the total weight of the alloy / metal transition metal fine powder mixture 48 was determined, and the weight ratio of the ferroalloy fine powder 46 to the total weight of the alloy / metal transition metal fine powder mixture 48 was determined.
  • the weight ratio of the Cu metal fine powder 47 to the total weight of the alloy / metal transition metal fine powder mixture 48 is determined.
  • the weight ratio of the stainless alloy fine powder 45 to the total weight (100%) of the alloy / metal transition metal fine powder mixture 48 is determined in the range of 47 to 49% (preferably 48%),
  • the weight ratio of the ferroalloy fine powder 46 to the total weight (100%) of the alloy / metal transition metal fine powder mixture 48 is determined in the range of 47 to 49% (preferably 48%), and the alloy / metal transition metal fine powder mixture is determined.
  • the weight ratio of the Cu metal fine powder 47 to the total weight (100%) of the 48 is determined in the range of 2 to 6% (preferably 2%).
  • the weight ratio of the stainless alloy fine powder 45, the weight ratio of the ferroalloy fine powder 46, and the weight ratio of the Cu metal fine powder 47 to the total weight of the alloy / metal transition metal fine powder mixture 48 are determined within the above ranges.
  • the work function of the stainless alloy fine powder 45, the ferroalloy fine powder 46, and the Cu metal fine powder 47 can be approximated to the work function of the platinum group element, and is substantially the same as the electrode containing the platinum group element. It has a work function, can exhibit almost the same catalytic activity (catalytic action) as an electrode containing a platinum group element, has excellent catalytic activity (catalytic action), and uses the catalytic function sufficiently and reliably.
  • the electrode 10 anode or cathode that can be manufactured can be produced.
  • the stainless alloy fine powder 45 having the weight ratio determined in the fine powder weight ratio determining step, the ferroalloy fine powder 46 having the weight ratio determined in the fine powder weight ratio determining step, and the fine powder are used.
  • the Cu metal fine powder 47 having the weight ratio determined in the weight ratio determining step is put into a mixer, and the stainless alloy fine powder 45, the ferroalloy fine powder 46, and the Cu metal fine powder 47 are stirred and mixed by the mixer to form a stainless alloy.
  • An alloy-metal transition metal fine powder mixture 48 in which the fine powder 45, the ferroalloy fine powder 46, and the Cu metal fine powder 47 are uniformly mixed and dispersed is prepared.
  • the alloy / metal transition metal fine powder compressed material producing step S4 the alloy / metal transition metal fine powder mixture 48 produced in the alloy / metal transition metal fine powder mixture producing step S3 is pressurized at a predetermined pressure, and the alloy / metal transition metal A compressed alloy / metal transition metal powder 49 is prepared by compressing the fine powder mixture 48 into a thin plate having a predetermined area.
  • the alloy / metal transition metal fine powder compressed material preparation step S4 the alloy / metal transition metal fine powder mixture 48 is put into a mold, and the metal / metal transition metal fine powder is pressed by a press machine. A compressed body 49 is made.
  • the press pressure (pressure) during the press working is in the range of 500 MPa to 800 MPa.
  • the opening area (opening diameter) of the flow channel 13 (passage hole) formed in the compressed alloy-metal transition metal fine powder 49 (alloy-metal transition metal thin plate electrode 14) is large.
  • the opening diameter of the compressed alloy-metal transition metal fine powder 49 (alloy-metal transition metal thin plate electrode 14) is set to a thickness L1 of 0.03 mm to 0.3 mm (preferably 0.05 mm to 0.1 mm).
  • a large number of fine channels 13 (passage holes) in the range of 1 ⁇ m to 100 ⁇ m cannot be formed in the compressed alloy-metal transition metal fine powder 49 (alloy-metal transition metal sheet electrode 14).
  • the opening area (opening diameter) of the flow path 13 (passage hole) formed in the compressed alloy-metal transition metal fine powder 49 (alloy-metal transition metal thin plate electrode 14) is reduced.
  • the thickness L1 of the compressed alloy / metal transition metal fine powder 49 (alloy / metal transition metal thin plate electrode 14) becomes 0.03 mm to 0.3 mm (preferably 0.05 mm to 0.1 mm).
  • a large number of fine channels 13 (passage holes) having an opening diameter in the range of 1 ⁇ m to 100 ⁇ m cannot be formed in the alloy-metal transition metal fine powder compact 49 (alloy-metal transition metal thin plate electrode 14).
  • the alloy / metal transition metal fine powder mixture 48 is pressurized (compressed) at a pressure within the above range to form the alloy / metal transition metal fine powder compressed material 49 (alloy / metal transition metal thin plate electrode 14).
  • the compressed metal transition metal powder 49 (alloy / metal transition metal thin plate electrode 14) can be formed.
  • the electrode manufacturing method since the electrode 10 having a thickness L1 in the range of 0.03 mm to 0.3 mm (preferably in the range of 0.05 mm to 0.1 mm) can be produced, the electric resistance can be reduced. Thus, the electrode 10 (anode or cathode) capable of flowing a current smoothly can be manufactured.
  • the alloy / metal transition metal fine powder compact 49 produced in the alloy / metal transition metal fine powder compact forming step is charged into a furnace (electric furnace), The transition metal fine powder compact 49 is fired (sintered) at a predetermined temperature in a furnace to form an alloy metal transition metal thin plate electrode 14 (electrode 10) having a porous structure in which a number of fine channels 13 (passage holes) are formed. create.
  • the alloy / metal transition metal thin plate electrode forming step S5 the alloy / metal transition metal fine powder compact 49 is fired for a long time at a temperature at which the Cu metal fine powder 47 having the lowest melting point is melted.
  • the firing (sintering) time is 3 hours to 6 hours.
  • the Cu metal fine powder 47 having the lowest melting point was melted and melted when the pressed alloy / metal transition metal fine powder 49 compressed into a thin plate having a predetermined area was fired.
  • the stainless alloy fine powder 45 and the ferroalloy fine powder 46 are joined (fixed) using the Cu metal fine powder 47 as a binder.
  • the electrode manufacturing method includes a metal fine powder preparation step S1, a fine powder weight ratio determination step S2, an alloy / metal transition metal fine powder mixture preparation step S3, an alloy / metal transition metal fine powder compressed product preparation step S4, an alloy / metal transition metal
  • the thickness L1 is in the range of 0.03 mm to 0.3 mm (preferably in the range of 0.05 mm to 0.1 mm) due to each step of the thin plate electrode forming step S5, and a large number of fine channels 13 (passage holes).
  • a non-platinum electrode 10 anode or cathode
  • the catalyst has excellent catalytic activity (catalytic action).
  • the electrode 10 (anode or cathode) that can use the function sufficiently and reliably can be manufactured.
  • the electrode 10 produced thereby exhibits substantially the same catalytic activity (catalysis) as the electrode containing the platinum group element, it is possible to generate sufficient electricity in the polymer electrolyte fuel cell 18.
  • a non-platinum electrode 10 capable of supplying sufficient electric energy to a load 30 connected to the polymer electrolyte fuel cell 18 can be produced, and the hydrogen gas generator 31 can efficiently perform electrolysis.
  • a non-platinum electrode 10 that can be performed well and can generate a large amount of hydrogen gas in a short time can be manufactured.
  • the electrode manufacturing method is a method of joining a stainless alloy fine powder 45 and a ferroalloy fine powder 46 using a Cu metal fine powder 47 having the highest melting point as a binder to form a porous alloy having a large number of fine flow channels 13 (passage holes).
  • Non-platinum that can make the metal transition metal sheet electrode 14 (electrode 10), maintain its shape with high strength, and prevent breakage and damage when subjected to impact Electrode 10 can be made.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Inert Electrodes (AREA)
  • Powder Metallurgy (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Fuel Cell (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)

Abstract

L'invention aborde le problème de la fourniture d'une électrode qui peut être produite à faible coût sans utiliser d'élément du groupe du platine mais qui peut démontrer sensiblement la même activité catalytique (effet catalytique) qu'une électrode contenant un élément du groupe du platine. La solution selon l'invention porte sur une électrode 10 qui est une électrode en feuille mince de métal de transition métal-alliage d'une structure poreuse dans laquelle de l'acier inoxydable austénitique, un ferro-alliage, et du Cu sélectionnés de telle sorte que la fonction de travail combinée s'approche de la fonction de travail d'un élément du groupe du platine qui sont utilisés en tant que matières premières. Un mélange de poudre fine de métal de transition métal-alliage obtenu par mélange et dispersion uniformes d'une poudre fine d'alliage d'acier inoxydable, d'une poudre fine de ferro-alliage, et d'une poudre fine métallique de Cu est comprimé sous la forme d'une plaque mince de zone prescrite, puis cuit pour former un grand nombre de canaux fins. Avec cette électrode 10, le rapport en poids de la poudre fine d'alliage d'acier inoxydable, le rapport en poids de la poudre fine de ferro-alliage, et le rapport en poids de la poudre fine métallique de Cu au poids total du mélange de poudre fine de métal de transition métal-alliage sont déterminés de telle sorte que la fonction de travail combinée de la poudre fine d'alliage d'acier inoxydable, de la poudre fine de ferro-alliage, et de la poudre fine métallique de Cu se rapproche de la fonction de travail de l'élément du groupe platine.
PCT/JP2019/036710 2018-09-19 2019-09-19 Électrode WO2020059783A1 (fr)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS5724633B2 (fr) * 1974-07-26 1982-05-25
JP2017095746A (ja) * 2015-11-20 2017-06-01 鈴木　健治 水素生成装置および給湯システム
JP2017098004A (ja) * 2015-11-20 2017-06-01 株式会社健明 燃料電池用電極材料、およびその製造方法

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS5724633B2 (fr) * 1974-07-26 1982-05-25
JP2017095746A (ja) * 2015-11-20 2017-06-01 鈴木　健治 水素生成装置および給湯システム
JP2017098004A (ja) * 2015-11-20 2017-06-01 株式会社健明 燃料電池用電極材料、およびその製造方法

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