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WO2024143292A1 - Cellule électrochimique - Google Patents

Cellule électrochimique Download PDF

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Publication number
WO2024143292A1
WO2024143292A1 PCT/JP2023/046482 JP2023046482W WO2024143292A1 WO 2024143292 A1 WO2024143292 A1 WO 2024143292A1 JP 2023046482 W JP2023046482 W JP 2023046482W WO 2024143292 A1 WO2024143292 A1 WO 2024143292A1
Authority
WO
WIPO (PCT)
Prior art keywords
electrode layer
metal support
hydrogen electrode
layer
recess
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.)
Ceased
Application number
PCT/JP2023/046482
Other languages
English (en)
Japanese (ja)
Inventor
誠 大森
真司 藤崎
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
NGK Insulators Ltd
Original Assignee
NGK Insulators Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by NGK Insulators Ltd filed Critical NGK Insulators Ltd
Priority to JP2024567815A priority Critical patent/JPWO2024143292A1/ja
Publication of WO2024143292A1 publication Critical patent/WO2024143292A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • 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
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/02—Hydrogen or oxygen
    • C25B1/04—Hydrogen or oxygen by electrolysis of water
    • C25B1/042—Hydrogen or oxygen by electrolysis of water by electrolysis of steam
    • 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
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/23—Carbon monoxide or syngas
    • 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
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/052—Electrodes comprising one or more electrocatalytic coatings on a substrate
    • 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
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • 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
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C25B9/23—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms comprising ion-exchange membranes in or on which electrode material is embedded
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M8/1213—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material
    • 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

Definitions

  • electrochemical cells electrolysis cells, fuel cells, etc.
  • the electrochemical cell described in Patent Document 1 has a cell body in which a first electrode layer, an electrolyte layer, and a second electrode layer are laminated in this order on the main surface of a metal support.
  • the metal support has a plurality of supply holes formed therein for supplying raw material gas to the first electrode layer.
  • the electrochemical cell according to the first aspect of the present invention comprises a metal support and a cell body.
  • the metal support has a first main surface, a second main surface, and a plurality of supply holes.
  • the cell body is supported by the metal support and has a first electrode layer, a second electrode layer, and an electrolyte layer disposed between the first electrode layer and the second electrode layer.
  • the first electrode layer has a contact surface that contacts the electrolyte layer. In a cross section along the thickness direction of the first electrode layer, the contact surface is curved in a convex shape toward the metal support.
  • the electrochemical cell according to the second aspect of the present invention is the same as the first aspect, and in the cross section, the closest point of the contact surface to the metal support in the thickness direction is located at the center of the first electrode layer in the surface direction.
  • the electrochemical cell according to the third aspect of the present invention is the electrochemical cell according to the first or second aspect, in which the metal support has a recess formed in the first main surface, and at least a portion of the first electrode layer is disposed within the recess.
  • the electrochemical cell according to the fourth aspect of the present invention is the same as the third aspect, and in a cross section along the thickness direction of the metal support, the boundary between the side peripheral surface and the bottom surface of the recess is rounded.
  • the electrochemical cell according to the fifth aspect of the present invention is the electrochemical cell according to the third or fourth aspect, and the cell body has a catalyst layer disposed in at least one of the multiple supply holes and connected to the first electrode layer.
  • the present invention provides an electrochemical cell that can improve the durability of the first electrode layer.
  • FIG. 1 is a plan view of an electrolysis cell according to an embodiment.
  • FIG. 2 is a cross-sectional view taken along line AA of FIG.
  • FIG. 3 is a cross-sectional view of an electrolysis cell according to the first modification.
  • FIG. 4 is a cross-sectional view of an electrolysis cell according to the second modification.
  • FIG. 1 is a plan view of an electrolysis cell 100 according to an embodiment.
  • Fig. 2 is a cross-sectional view taken along line AA in Fig. 1.
  • Line AA in Fig. 2 is a line passing through the center of the hydrogen electrode layer 1 in a plan view.
  • the electrolytic cell 100 is a so-called metal-supported electrolytic cell.
  • the electrolytic cell 100 is an example of an "electrochemical cell" according to the present invention.
  • the electrolytic cell 100 is formed in a plate shape extending in the X-axis and Y-axis directions.
  • the electrolytic cell 100 is formed in a rectangular shape extending in the Y-axis direction in a plan view, but the planar shape of the electrolytic cell 100 is not particularly limited, and may be a polygon other than a rectangle, an ellipse, a circle, etc.
  • the electrolysis cell 100 includes a metal support 10, a cell body 20, and a flow path member 30.
  • the metal support 10 supports the cell main body 20.
  • the metal support 10 is formed in a plate shape.
  • the metal support 10 may be in a flat plate shape or a curved plate shape.
  • the metal support 10 may have any thickness as long as it can maintain the strength of the electrolysis cell 100, and the thickness is not particularly limited, but may be, for example, 0.1 mm or more and 2.0 mm or less.
  • the metal support 10 has a first main surface 11, a second main surface 12, a recess 13, and a plurality of supply holes 14.
  • the first main surface 11 is the main surface on the cell main body 20 side.
  • the first main surface 11 is formed in a planar shape.
  • the cell main body 20 is joined to the first main surface 11.
  • a recess 13 is formed in the first main surface 11. Therefore, the first main surface 11 is formed in a ring shape when viewed in a plane.
  • the second main surface 12 is the main surface opposite the cell body 20, and is provided on the opposite side of the first main surface 11.
  • the second main surface 12 is formed in a planar shape.
  • a flow path member 30 is joined to the second main surface 12.
  • the recess 13 is formed in the first main surface 11.
  • the recess 13 opens to the first main surface 11.
  • the recess 13 is a so-called bottomed recess.
  • the hydrogen electrode layer 1, which will be described later, is disposed within the recess 13.
  • the recess 13 has a bottom surface S1 and a peripheral side surface S2.
  • the side peripheral surface S2 is connected to the outer edge of the bottom surface S1 and the inner edge of the first main surface 11.
  • the side peripheral surface S2 is formed in an annular shape.
  • the side peripheral surface S2 contacts the hydrogen electrode layer 1.
  • the side peripheral surface S2 covers the side circumference of the hydrogen electrode layer 1.
  • the depth of the recess 13 in the Z-axis direction is not particularly limited, but can be 1% or more and 50% or less of the thickness of the metal support 10 in the Z-axis direction.
  • the metal support 10 may contain Ti (titanium) and Zr (zirconium).
  • the Ti content in the metal support 10 is not particularly limited, but may be 0.01 mol% or more and 1.0 mol% or less.
  • the Al content in the metal support 10 is not particularly limited, but may be 0.01 mol% or more and 0.4 mol% or less.
  • the metal support 10 may contain Ti as TiO2 (titania) and may contain Zr as ZrO2 (zirconia).
  • the metal support 10 may have an oxide film on its surface that is formed by oxidation of the constituent elements of the metal support 10.
  • a typical example of the oxide film is a chromium oxide film.
  • the chromium oxide film covers at least a portion of the surface of the metal support 10.
  • the chromium oxide film may cover at least a portion of the inner circumferential surface of each supply hole 14.
  • the center of the surface direction of the hydrogen electrode layer 1 is the part located in the center when the hydrogen electrode layer 1 is divided into three equal parts in the surface direction.
  • the outer peripheral part of the surface direction of the hydrogen electrode layer 1 is the part located on both sides of the center when the hydrogen electrode layer 1 is divided into three equal parts in the surface direction.
  • the hydrogen electrode layer 1 fills the recess 13. That is, the entire hydrogen electrode layer 1 is disposed within the recess 13. Therefore, as shown in FIG. 2, the hydrogen electrode layer 1 is formed to follow the contour of the recess 13.
  • the hydrogen electrode layer 1 When the source gas contains CO 2 in addition to H 2 O, the hydrogen electrode layer 1 produces H 2 , CO, and O 2 ⁇ from the source gas in accordance with the co-electrochemical reactions shown in the following formulas (2), (3), and (4).
  • Hydrogen electrode layer 1 CO 2 + H 2 O + 4e ⁇ ⁇ CO + H 2 + 2O 2 ⁇ (2)
  • Electrochemical reaction of CO2 CO2 + 2e- ⁇ CO + O2 -... (4)
  • the hydrogen electrode layer 1 is made of a porous material having electronic conductivity.
  • the hydrogen electrode layer 1 may have oxide ion conductivity.
  • the hydrogen electrode layer 1 may be made of, for example, yttria-stabilized zirconia (YSZ), calcia-stabilized zirconia (CSZ), scandia-stabilized zirconia (ScSZ), gadolinium-doped ceria (GDC), samarium-doped ceria (SDC), (La,Sr)(Cr,Mn) O3 , (La,Sr) TiO3 , Sr2 (Fe,Mo) 2O6 , ( La,Sr) VO3 , (La,Sr) FeO3 , a mixed material of two or more of these, or a composite of one or more of these and NiO.
  • YSZ yttria-stabilized zirconia
  • CSZ calcia-stabilized zirconia
  • the method for forming the hydrogen electrode layer 1 is not particularly limited, and may be a sintering method, a spray coating method (thermal spraying, aerosol deposition, aerosol gas deposition, powder jet deposition, particle jet deposition, cold spray, etc.), a PVD method (sputtering, pulsed laser deposition, etc.), a CVD method, etc.
  • Each of the plurality of catalyst layers 2 is disposed in a corresponding supply hole 14 and is continuous with the hydrogen electrode layer 1.
  • Each catalyst layer 2 is engaged with the opening of each supply hole 14 on the bottom surface S1 side in the planar direction.
  • Each catalyst layer 2 may contain an oxide ion conductive material.
  • oxide ion conductive material those listed as the oxide ion conductive materials for the hydrogen electrode layer 1 can be used.
  • each catalyst layer 2 is not particularly limited, but can be, for example, 5% to 70%.
  • the depth of each catalyst layer 2 in the Z-axis direction is not particularly limited, but can be 10% to 100% of the length of each supply hole 14 in the Z-axis direction.
  • the electrolyte layer 3 covers the contact surface S3 of the hydrogen electrode layer 1.
  • the hydrogen electrode layer 1 is filled in the recess 13 of the metal support 10, so the electrolyte layer 3 is positioned outside the recess 13.
  • the outer edge of the electrolyte layer 3 is connected to the first main surface 11 of the metal support 10.
  • a portion of the first main surface 11 is exposed from the electrolyte layer 3, but the entire first main surface 11 may be covered by the electrolyte layer 3.
  • reaction prevention layer 4 The reaction prevention layer 4 is disposed between the electrolyte layer 3 and the oxygen electrode layer 5. The reaction prevention layer 4 is disposed on the opposite side of the electrolyte layer 3 from the hydrogen electrode layer 1. The reaction prevention layer 4 prevents the constituent elements of the electrolyte layer 3 from reacting with the constituent elements of the oxygen electrode layer 5 to form a layer with high electrical resistance.
  • Oxygen electrode layer 5 2O 2 ⁇ ⁇ O 2 +4e ⁇ (5)
  • the oxygen electrode layer 5 is made of a porous material having oxide ion conductivity and electron conductivity, and may be made of a composite material of one or more of (La,Sr)(Co,Fe) O3 , (La,Sr) FeO3 , La(Ni,Fe) O3 , (La,Sr) CoO3 , and (Sm,Sr) CoO3 and an oxide ion conductive material (such as GDC).
  • the flow path member 30 can be made of, for example, an alloy material.
  • the flow path member 30 may be made of the same material as the metal support 10. In this case, the flow path member 30 may be substantially integral with the metal support 10.
  • the flow path member 30 has a frame body 31 and an interconnector 32.
  • the frame body 31 is an annular plate member that surrounds the side circumference of the flow path 30a.
  • the frame body 31 is joined to the second main surface 12 of the metal support body 10.
  • the interconnector 32 is a plate member for electrically connecting an external power source or another electrolytic cell in series with the electrolytic cell 100.
  • the interconnector 32 is joined to the frame body 31.
  • the frame body 31 and the interconnector 32 are separate components, but the frame body 31 and the interconnector 32 may be an integrated component.
  • the proximity point S4 of the contact surface S3 is located in the center of the hydrogen electrode layer 1 in the surface direction. Therefore, the source gas can be diffused in a balanced manner from the center to the outer periphery in the surface direction, further mitigating the current distribution in the surface direction of the hydrogen electrode layer 1.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)

Abstract

Dans la présente invention, une cellule électrolytique (100) comprend un support métallique (10) et un corps de cellule (20). Le corps de cellule (20) est supporté par le support métallique (10). Le corps de cellule (20) comprend une couche d'électrode à hydrogène (1), une couche d'électrolyte (3) et une couche d'électrode à oxygène (5). La couche d'électrode à hydrogène (1) comprend une surface de contact (S3) qui est en contact avec la couche d'électrolyte (3). La surface de contact (S3) est incurvée de façon à faire saillie vers le support métallique (10) dans la section transversale dans le sens de l'épaisseur de la couche d'électrode à hydrogène (1).
PCT/JP2023/046482 2022-12-27 2023-12-25 Cellule électrochimique Ceased WO2024143292A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP2024567815A JPWO2024143292A1 (fr) 2022-12-27 2023-12-25

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2022209931 2022-12-27
JP2022-209931 2022-12-27

Publications (1)

Publication Number Publication Date
WO2024143292A1 true WO2024143292A1 (fr) 2024-07-04

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WO (1) WO2024143292A1 (fr)

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2009099562A (ja) * 2007-09-28 2009-05-07 Dainippon Printing Co Ltd 固体酸化物形燃料電池及びその製造方法
JP2019046570A (ja) * 2017-08-30 2019-03-22 学校法人東京理科大学 膜電極接合体、燃料電池および膜電極接合体用電解質膜
JP2019210543A (ja) * 2018-06-04 2019-12-12 パナソニックＩｐマネジメント株式会社 電気化学式ポンプ

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2009099562A (ja) * 2007-09-28 2009-05-07 Dainippon Printing Co Ltd 固体酸化物形燃料電池及びその製造方法
JP2019046570A (ja) * 2017-08-30 2019-03-22 学校法人東京理科大学 膜電極接合体、燃料電池および膜電極接合体用電解質膜
JP2019210543A (ja) * 2018-06-04 2019-12-12 パナソニックＩｐマネジメント株式会社 電気化学式ポンプ

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