WO2023074807A1 - Élément électroconducteur, cellule électrochimique, dispositif à cellule électrochimique, module et dispositif de stockage de module - Google Patents

Élément électroconducteur, cellule électrochimique, dispositif à cellule électrochimique, module et dispositif de stockage de module Download PDF

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Publication number
WO2023074807A1
WO2023074807A1 PCT/JP2022/040193 JP2022040193W WO2023074807A1 WO 2023074807 A1 WO2023074807 A1 WO 2023074807A1 JP 2022040193 W JP2022040193 W JP 2022040193W WO 2023074807 A1 WO2023074807 A1 WO 2023074807A1
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WIPO (PCT)
Prior art keywords
conductive member
cell
electrochemical cell
polycrystalline film
module
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PCT/JP2022/040193
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English (en)
Japanese (ja)
Inventor
章洋 原
和輝 平尾
篤輝 山口
貴弘 小見山
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京セラ株式会社
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Priority to JP2023556640A priority Critical patent/JPWO2023074807A1/ja
Publication of WO2023074807A1 publication Critical patent/WO2023074807A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
    • C01F17/00—Compounds of rare earth metals
    • C01F17/20—Compounds containing only rare earth metals as the metal element
    • C01F17/206—Compounds containing only rare earth metals as the metal element oxide or hydroxide being the only anion
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G25/00—Compounds of zirconium
    • C01G25/02—Oxides
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G37/00—Compounds of chromium
    • C01G37/02—Oxides or hydrates thereof
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C26/00—Coating not provided for in groups C23C2/00 - C23C24/00
    • 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
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465—Details of groupings of fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01R—ELECTRICALLY-CONDUCTIVE CONNECTIONS; STRUCTURAL ASSOCIATIONS OF A PLURALITY OF MUTUALLY-INSULATED ELECTRICAL CONNECTING ELEMENTS; COUPLING DEVICES; CURRENT COLLECTORS
    • H01R11/00—Individual connecting elements providing two or more spaced connecting locations for conductive members which are, or may be, thereby interconnected, e.g. end pieces for wires or cables supported by the wire or cable and having means for facilitating electrical connection to some other wire, terminal, or conductive member, blocks of binding posts
    • H01R11/01—Individual connecting elements providing two or more spaced connecting locations for conductive members which are, or may be, thereby interconnected, e.g. end pieces for wires or cables supported by the wire or cable and having means for facilitating electrical connection to some other wire, terminal, or conductive member, blocks of binding posts characterised by the form or arrangement of the conductive interconnection between the connecting locations
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01R—ELECTRICALLY-CONDUCTIVE CONNECTIONS; STRUCTURAL ASSOCIATIONS OF A PLURALITY OF MUTUALLY-INSULATED ELECTRICAL CONNECTING ELEMENTS; COUPLING DEVICES; CURRENT COLLECTORS
    • H01R13/00—Details of coupling devices of the kinds covered by groups H01R12/70 or H01R24/00 - H01R33/00
    • H01R13/02—Contact members
    • H01R13/03—Contact members characterised by the material, e.g. plating, or coating materials
    • 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

  • the present disclosure relates to conductive members, electrochemical cells, electrochemical cell devices, modules, and module housing devices.
  • a fuel cell is a type of electrochemical cell that can obtain electric power using a fuel gas such as a hydrogen-containing gas and an oxygen-containing gas such as air.
  • a conductive member has a base material and a polycrystalline film.
  • the substrate contains chromium.
  • a polycrystalline film includes a plurality of chromium oxide particles and is located on the substrate.
  • the polycrystalline film contains a first element. The first element is located between the chromium oxide particles and has a first ionization energy and a free energy of oxide formation per mole of oxygen smaller than those of chromium.
  • an electrochemical cell of the present disclosure includes an element portion and the conductive member described above.
  • a conductive member is connected to the element portion.
  • the electrochemical cell device of the present disclosure has a cell stack including the electrochemical cell described above.
  • the module of the present disclosure includes the electrochemical cell device described above and a storage container that stores the electrochemical cell device.
  • the module housing device of the present disclosure includes the module described above, an accessory for operating the module, and an exterior case that accommodates the module and the accessory.
  • FIG. 1A is a cross-sectional view showing an example of an electrochemical cell according to a first embodiment
  • FIG. FIG. 1B is a side view of an example of the electrochemical cell according to the first embodiment, viewed from the air electrode side.
  • FIG. 1C is a side view of an example of the electrochemical cell according to the first embodiment, viewed from the interconnector side.
  • 2A is a perspective view showing an example of an electrochemical cell device according to the first embodiment;
  • FIG. FIG. 2B is a cross-sectional view taken along line XX shown in FIG. 2A.
  • 2C is a top view showing an example of the electrochemical cell device according to the first embodiment;
  • FIG. 3 is a cross-sectional view showing an example of a conductive member according to the embodiment; 4A is a cross-sectional view taken along line AA shown in FIG. 3.
  • FIG. 4B is an enlarged view of area B shown in FIG. 4A.
  • FIG. 4C is an enlarged view of the polycrystalline film shown in FIG. 4B.
  • FIG. 5 is an external perspective view showing an example of the module according to the first embodiment.
  • FIG. 6 is an exploded perspective view schematically showing an example of the module housing device according to the first embodiment.
  • FIG. 7A is a cross-sectional view showing an electrochemical cell according to a second embodiment;
  • FIG. 7B is an enlarged cross-sectional view of a conductive member according to the second embodiment;
  • FIG. 8A is a perspective view showing an electrochemical cell according to a third embodiment
  • FIG. FIG. 8B is a partial cross-sectional view of the electrochemical cell shown in FIG. 8A.
  • FIG. 8C is a partial cross-sectional view of the electrochemical cell shown in FIG. 8A.
  • FIG. 9A is a cross-sectional view showing an example of an electrochemical cell according to a fourth embodiment
  • FIG. 9B is a cross-sectional view showing another example of the electrochemical cell according to the fourth embodiment
  • FIG. 9C is a cross-sectional view showing another example of the electrochemical cell according to the fourth embodiment
  • FIG. 9D is an enlarged cross-sectional view of region C shown in FIG. 9A.
  • An electrochemical cell arrangement may comprise a cell stack having a plurality of electrochemical cells.
  • An electrochemical cell device having multiple electrochemical cells is simply referred to as a cell stack device.
  • FIG. 1A is a cross-sectional view showing an example of an electrochemical cell according to the first embodiment
  • FIG. 1B is a side view of the example of the electrochemical cell according to the first embodiment as seen from the air electrode side
  • 1C is a side view of an example of the electrochemical cell according to the first embodiment, viewed from the interconnector side; FIG. Note that FIGS. 1A to 1C show enlarged portions of each configuration of the electrochemical cell.
  • the electrochemical cell may be simply called a cell.
  • the cells 1 are hollow flat plate-shaped and elongated plates.
  • the shape of the entire cell 1 seen from the side is, for example, the length of the side in the length direction L is 5 cm to 50 cm, and the length of the width direction W orthogonal to the length direction L is is, for example, a rectangle of 1 cm to 10 cm.
  • the thickness of the entire cell 1 in the thickness direction T is, for example, 1 mm to 5 mm.
  • the cell 1 includes a conductive support substrate 2, an element section 3, and an interconnector 4.
  • the support substrate 2 has a columnar shape having a pair of opposing first and second surfaces n1 and n2, and a pair of arcuate side surfaces m connecting the first and second surfaces n1 and n2.
  • the element section 3 is located on the first surface n1 of the support substrate 2.
  • the element section 3 has a fuel electrode 5 , a solid electrolyte layer 6 and an air electrode 8 .
  • the interconnector 4 is positioned on the second surface n2 of the cell 1 .
  • the cell 1 may have an intermediate layer 7 between the solid electrolyte layer 6 and the air electrode 8 .
  • the air electrode 8 does not extend to the lower end of the cell 1.
  • the air electrode 8 does not extend to the lower end of the cell 1.
  • the interconnector 4 may extend to the lower end of the cell 1.
  • FIG. 1A the solid electrolyte layer 6 is exposed on the surfaces of the pair of arc-shaped side surfaces m of the cell 1 .
  • Interconnector 4 does not have to extend to the bottom end of cell 1 .
  • the support substrate 2 has inside a gas flow path 2a through which gas flows.
  • the example of the support substrate 2 shown in FIG. 1A has six gas channels 2a.
  • the support substrate 2 has gas permeability and allows the gas flowing through the gas flow path 2a to permeate up to the fuel electrode 5 .
  • the support substrate 2 may have conductivity.
  • the support substrate 2 having conductivity collects the electricity generated in the element section 3 to the interconnector 4 .
  • the material of the support substrate 2 includes, for example, iron group metal components and inorganic oxides.
  • the iron group metal component may be Ni (nickel) and/or NiO, for example.
  • Inorganic oxides may be, for example, certain rare earth element oxides.
  • the rare earth element oxide may contain one or more rare earth elements selected from, for example, Sc, Y, La, Nd, Sm, Gd, Dy and Yb.
  • the fuel electrode 5 may be a porous conductive ceramic containing an electronically conductive material and an ionic conductive material.
  • conductive ceramics for example, ceramics containing ZrO 2 in which calcium oxide, magnesium oxide, or rare earth element oxides are solid-dissolved, and Ni and/or NiO may be used.
  • This rare earth element oxide may include a plurality of rare earth elements selected from, for example, Sc, Y, La, Nd, Sm, Gd, Dy and Yb.
  • ZrO 2 in which calcium oxide, magnesium oxide, or oxides of rare earth elements are solid-dissolved is sometimes called stabilized zirconia. Stabilized zirconia also includes partially stabilized zirconia.
  • the solid electrolyte layer 6 is an electrolyte, and transfers ions between the fuel electrode 5 and the air electrode 8. At the same time, the solid electrolyte layer 6 has gas barrier properties and makes it difficult for fuel gas and oxygen-containing gas to leak.
  • the material of the solid electrolyte layer 6 may be, for example, ZrO 2 in which 3 mol % to 15 mol % of rare earth element oxide is solid-dissolved.
  • the rare earth element oxide may contain one or more rare earth elements selected from, for example, Sc, Y, La, Nd, Sm, Gd, Dy and Yb.
  • the solid electrolyte layer 6 may contain, for example, ZrO 2 in which Yb, Sc or Gd is dissolved, CeO 2 in which La, Nd or Yb is dissolved, or BaZrO 3 in which Sc or Yb is dissolved. BaCeO 3 in which Sc or Yb is solid-dissolved may be included.
  • the air electrode 8 has gas permeability.
  • the open porosity of the cathode 8 may be, for example, in the range from 20% to 50%, especially from 30% to 50%.
  • the open porosity of the air electrode 8 may also be referred to as the air electrode 8 porosity.
  • the material of the air electrode 8 is not particularly limited as long as it is generally used for air electrodes.
  • the material of the air electrode 8 may be, for example, a conductive ceramic such as a so-called ABO 3 type perovskite oxide.
  • the material of the air electrode 8 may be, for example, a composite oxide in which Sr (strontium) and La (lanthanum) coexist at the A site.
  • composite oxides include La x Sr 1-x Co y Fe 1-y O 3 , La x Sr 1-x MnO 3 , La x Sr 1-x FeO 3 , La x Sr 1-x CoO3 and the like. Note that x satisfies 0 ⁇ x ⁇ 1 and y satisfies 0 ⁇ y ⁇ 1.
  • the intermediate layer 7 functions as a diffusion suppressing layer.
  • Sr (strontium) contained in the air electrode 8 diffuses into the solid electrolyte layer 6 , a resistance layer of SrZrO 3 is formed on the solid electrolyte layer 6 .
  • the intermediate layer 7 makes SrZrO 3 less likely to be formed by making Sr less likely to diffuse.
  • the material of the intermediate layer 7 is not particularly limited as long as it is generally used for an element diffusion suppression layer between the air electrode 8 and the solid electrolyte layer 6 .
  • the material of the intermediate layer 7 may include, for example, cerium oxide (CeO 2 ) in which rare earth elements other than Ce (cerium) are solid-dissolved.
  • CeO 2 cerium oxide
  • rare earth elements for example, Gd (gadolinium), Sm (samarium), etc. may be used.
  • the interconnector 4 is dense and makes it difficult for the fuel gas flowing through the gas flow path 2a located inside the supporting substrate 2 and the oxygen-containing gas flowing outside the supporting substrate 2 to leak.
  • the interconnector 4 may have a relative density of 93% or more, in particular 95% or more.
  • a lanthanum chromite-based perovskite-type oxide (LaCrO 3 -based oxide), a lanthanum strontium titanium-based perovskite-type oxide (LaSrTiO 3 -based oxide), or the like may be used. These materials are electrically conductive and are less likely to be reduced or oxidized when in contact with a fuel gas such as a hydrogen-containing gas and an oxygen-containing gas such as air.
  • FIGS. 2A to 2C are perspective views showing an example of an electrochemical cell device according to the first embodiment
  • FIG. 2B is a cross-sectional view taken along line XX shown in FIG. 2A
  • FIG. It is a top view which shows an example of the electrochemical cell apparatus which concerns on a form.
  • the cell stack device 10 includes a cell stack 11 having a plurality of cells 1 arranged (stacked) in the thickness direction T (see FIG. 1A) of the cells 1, and a fixing member 12.
  • the fixing member 12 has a fixing member 13 and a support member 14 .
  • Support member 14 supports cell 1 .
  • the fixing member 13 fixes the cell 1 to the support member 14 .
  • the support member 14 has a support 15 and a gas tank 16 .
  • the support 15 as the support member 14 and the gas tank 16 are made of metal and have electrical conductivity.
  • the support 15 has insertion holes 15a into which the lower ends of the plurality of cells 1 are inserted.
  • the lower ends of the cells 1 and the inner wall of the insertion hole 15a are joined with a fixing member 13. As shown in FIG. 2B, the support 15 has insertion holes 15a into which the lower ends of the plurality of cells 1 are inserted.
  • the lower ends of the cells 1 and the inner wall of the insertion hole 15a are joined with a fixing member 13. As shown in FIG.
  • the gas tank 16 has openings for supplying reaction gas to the plurality of cells 1 through the insertion holes 15a, and grooves 16a located around the openings.
  • the end of the outer periphery of the support 15 is joined to the gas tank 16 by a joining material 21 filled in the groove 16a of the gas tank 16. As shown in FIG.
  • the fuel gas is stored in the internal space 22 formed by the support 15 which is the support member 14 and the gas tank 16 .
  • a gas distribution pipe 20 is connected to the gas tank 16 .
  • the fuel gas is supplied to the gas tank 16 through this gas flow pipe 20, and supplied from the gas tank 16 to the gas flow path 2a (see FIG. 1A) inside the cell 1.
  • the fuel gas supplied to the gas tank 16 is generated by a reformer 102 (see FIG. 5), which will be described later.
  • Hydrogen-rich fuel gas can be generated by steam reforming the raw fuel.
  • the fuel gas contains steam.
  • FIG. 2A includes two rows of cell stacks 11, two supports 15, and a gas tank 16.
  • Each of the two columns of cell stacks 11 has a plurality of cells 1 .
  • Each cell stack 11 is fixed to each support 15 .
  • the gas tank 16 has two through holes on its upper surface.
  • Each support 15 is arranged in each through-hole.
  • the internal space 22 is formed by one gas tank 16 and two supports 15 .
  • the shape of the insertion hole 15a is, for example, an oval shape when viewed from above.
  • the insertion hole 15 a may have a length in the cell 1 arrangement direction, that is, in the thickness direction T, longer than the distance between the two end collector members 17 located at both ends of the cell stack 11 .
  • the width of the insertion hole 15a may be, for example, greater than the length of the cell 1 in the width direction W (see FIG. 1A).
  • the joint between the inner wall of the insertion hole 15a and the lower end of the cell 1 is filled with a fixing material 13 and solidified.
  • the inner wall of the insertion hole 15a and the lower end portions of the plurality of cells 1 are respectively joined and fixed, and the lower end portions of the cells 1 are joined and fixed.
  • the gas channel 2a of each cell 1 communicates with the internal space 22 of the support member 14 at its lower end.
  • materials with low conductivity such as glass can be used.
  • a specific material for the fixing material 13 and the bonding material 21 amorphous glass or the like may be used, and in particular, crystallized glass or the like may be used.
  • crystallized glass examples include SiO 2 —CaO system, MgO—B 2 O 3 system, La 2 O 3 —B 2 O 3 —MgO system, La 2 O 3 —B 2 O 3 —ZnO system, and SiO 2 .
  • -CaO-ZnO based materials may be used, and in particular SiO 2 -MgO based materials may be used.
  • conductive members 18 are interposed between adjacent cells 1 among the plurality of cells 1 .
  • the conductive member 18 electrically connects the fuel electrode 5 of one adjacent cell 1 and the air electrode 8 of the other adjacent cell 1 in series. More specifically, the interconnector 4 electrically connected to the fuel electrode 5 of one adjacent cell 1 and the air electrode 8 of the other cell 1 are connected. Details of the conductive member 18 connected to the adjacent cell 1 will be described later.
  • the end current collecting member 17 is electrically connected to the cell 1 located on the outermost side in the arrangement direction of the plurality of cells 1 .
  • the end collector member 17 is connected to a conductive portion 19 protruding outside the cell stack 11 .
  • the conductive portion 19 collects the electricity generated by the power generation of the cell 1 and extracts it to the outside. It should be noted that illustration of the end collector member 17 is omitted in FIG. 2A.
  • the cell stack device 10 has two cell stacks 11A and 11B connected in series and functions as one battery. Therefore, the conductive portion 19 of the cell stack device 10 is divided into a positive terminal 19A, a negative terminal 19B, and a connection terminal 19C.
  • the positive electrode terminal 19A is a positive electrode when the power generated by the cell stack 11 is output to the outside, and is electrically connected to the positive electrode-side end collector member 17 in the cell stack 11A.
  • the negative electrode terminal 19B is a negative electrode when the power generated by the cell stack 11 is output to the outside, and is electrically connected to the negative electrode-side end current collecting member 17 in the cell stack 11B.
  • connection terminal 19C electrically connects the negative electrode-side end collector member 17 in the cell stack 11A and the positive electrode-side end collector member 17 in the cell stack 11B.
  • FIG. 3 is a cross-sectional view showing an example of a conductive member according to the embodiment.
  • the conductive member 18 has a connecting portion 18a connected to one adjacent cell 1 and a connecting portion 18b connected to the other adjacent cell 1. As shown in FIG. In addition, the conductive member 18 has connecting portions 18c at both ends in the width direction W to connect the connecting portions 18a and 18b. Thereby, the conductive member 18 can electrically connect the cells 1 adjacent to each other in the thickness direction T. As shown in FIG. In addition, in FIG. 3, the shape of the cell 1 is simplified and illustrated.
  • connection portions 18a and 18b have a first surface 181 facing the cell 1 and a second surface 182 facing the connection portions 18b and 18a.
  • FIG. 4A is a cross-sectional view along line AA shown in FIG.
  • FIG. 4B is an enlarged view of area B shown in FIG. 4A.
  • the conductive member 18 extends in the length direction L of the cell 1. As shown in FIG. 4A , a plurality of connection portions 18 a and 18 b of the conductive member 18 are alternately positioned along the length direction L of the cell 1 . The conductive member 18 is in contact with the cell 1 at respective connecting portions 18a and 18b.
  • the conductive member 18 has a base material 41, a polycrystalline film 42, and a coating layer 43. Also, the conductive member 18 has a first surface 181 and a second surface 182 positioned at both ends in the thickness direction T of the cell 1 . Also, the conductive member 18 has third surfaces 183 and 184 connecting the first surface 181 and the second surface 182 .
  • the conductive member 18 (connecting portion 18b) is joined to the cell 1 via a joining material 50.
  • the bonding material 50 is positioned between the first surface 181 of the conductive member 18 and the cell 1 and bonds the conductive member 18 and the cell 1 .
  • the second surface 182 and the third surfaces 183, 184 are exposed to an oxidizing atmosphere such as air.
  • the base material 41 has electrical conductivity and heat resistance.
  • Base material 41 contains chromium.
  • Base material 41 is, for example, stainless steel.
  • Base material 41 may contain, for example, a metal oxide.
  • FIG. 4C is an enlarged view of the polycrystalline film shown in FIG. 4B.
  • Polycrystalline film 42 is located on substrate 41 .
  • polycrystalline film 42 includes a plurality of chromium oxide particles 421 and first particles 422 .
  • Chromium oxide particles 421 contain, for example, chromium oxide (Cr 2 O 3 ). By including the chromium oxide particles 421 in the base material 41 in this way, the durability of the conductive member 18 is enhanced.
  • the chromium oxide particles 421 may have an average particle diameter (equivalent circle diameter) of, for example, 500 nm or less, particularly 100 nm or more and 350 nm or less. Also, the chromium oxide particles 421 may contain components other than chromium oxide. Chromium oxide particles 421 may not contain the first element. Details of the first element will be described later.
  • the first particles 422 are located between the chromium oxide particles 421 .
  • First particles 422 contain a first element.
  • the first element has a first ionization energy and a free energy of oxide formation per mole of oxygen smaller than those of chromium.
  • Examples of the first element include Y, Ce, Eu, Gd, Pr, Yb and Zr.
  • the free energy of formation is also called the Gibbs energy of formation.
  • the free energy of formation can be confirmed in a thermodynamic database such as the "Nuclear Fuel/Nuclear Material Thermodynamics Database".
  • the first element may in particular be one of Ce, Eu, Pr and Zr.
  • the first element may be located in the first particles 422 as an oxide of such element. Examples of oxides of the first element include Y 2 O 3 , CeO 2 , EuO, Gd 2 O 3 , PrO 2 , Yb 2 O 3 and ZrO 2 .
  • the first particles 422 may contain, for example, one or more of the first elements.
  • the first particles 422 may contain elements other than the first element.
  • the first particles 422 may contain, for example, CeO 2 in which Sm (samarium) and Gd (gadolinium) are solid-dissolved, or ZrO 2 in which Sc (scandium), Y (yttrium), Yb (ytterbium), etc. are solid-dissolved. 2. May contain so-called stabilized zirconia or partially stabilized zirconia.
  • first particles 422 may contain a composite oxide containing a first element such as Ce 2 Ti 2 O 7 .
  • the polycrystalline film 42 may have grain boundary phases containing the first element between the chromium oxide grains 421, for example.
  • the grain boundary phase containing the first element may contain, for example, 0.1 atomic % or more of the first element.
  • the polycrystalline film 42 may have a flat interface with the base material 41 or may have unevenness and undulations at the interface with the base material 41 .
  • the polycrystalline film 42 may contain Si, for example.
  • Si may be located at the tip of the projection projecting toward the base material 41 .
  • the polycrystalline film 42 of the conductive member 18 contains the first element, it becomes difficult for Cr in the base material 41 to diffuse, so that the polycrystalline film 42 is difficult to grow. Thereby, deterioration of the power generation performance of the cell 1 can be reduced.
  • the thickness of the polycrystalline film 42 may be, for example, 20 nm or more and 5 ⁇ m or less, or further 200 nm or more and 1.5 ⁇ m or less.
  • the effect of the polycrystalline film 42 on the internal resistance is reduced, so that the conductive member 18 is less likely to increase in internal resistance. Thereby, deterioration of the power generation performance of the cell 1 can be reduced.
  • the conductive member 18 may have an oxide of the first element located on the polycrystalline film 42 .
  • the oxide of the first element may be Y2O3 , CeO2 , EuO , Gd2O3 , PrO2 , Yb2O3 , ZrO2 , for example.
  • the presence or absence of the first element and the size of the first particles 422 containing the first element can be determined, for example, in the cross section of the conductive member 18 by HAADF-STEM (high angle annular dark field scanning transmission electron microscope), FIB-SEM (focusing It can be confirmed by mapping the first element using an ion beam scanning electron microscope) or an EPMA (electron probe microanalyzer). Further, the average thickness of the polycrystalline film 42 is determined by mapping chromium and the first element on the cross section of the conductive member 18 at a magnification of 1,000,000 times using, for example, HAADF-STEM with an acceleration voltage of 200 kV. is obtained by measuring the thickness of the portion where is detected at 10 or more points and calculating the average value.
  • Such a conductive member 18 is obtained by forming a film containing the first element on the surface of the base material 41 containing chromium, and heat-treating the film containing the first element and the base material 41 .
  • the coating containing the first element may be, for example, an oxide coating of the first element.
  • the film containing the first element may be formed, for example, by a physical vapor deposition method such as IAD (Ion Assisted Deposition), application of a slurry containing the oxide of the first element, or the like.
  • the thickness of the film containing the first element may be, for example, 1 nm or more and 1000 nm or less.
  • the thickness of the film containing the first element may be 5 nm or more and 150 nm or less, further 10 nm or more and 100 nm or less.
  • the coating containing the first element may contain oxide particles of the first element having a diameter of, for example, 30 nm or less.
  • the coating containing the first element may contain, for example, acicular or dendritic oxide particles of the first element.
  • the acicular or dendritic oxide particles of the first element may have a short diameter of 30 nm or less.
  • the oxide particles of the first element having such a diameter or minor axis are likely to be arranged between the particles of the polycrystalline film 42 by the heat treatment.
  • the heat treatment of the coating containing the first element and the substrate 41 may be performed at a temperature of 50° C. to 1100° C. in air, for example.
  • the base material 41 may not contain the first element.
  • the covering layer 43 is located on the polycrystalline film 42 .
  • the covering layer 43 covers the polycrystalline film 42 over the entire thickness direction T and length direction L of the cell 1 .
  • the coating layer 43 contains elements different from those of the polycrystalline film 42 .
  • Covering layer 43 has conductivity, for example.
  • the coating layer 43 may contain an oxide containing, for example, Mn (manganese) and Co (cobalt). Moreover, the coating layer 43 may be porous. The coating layer 43 may have a laminated structure containing different elements.
  • FIG. 5 is an external perspective view showing the module according to the first embodiment.
  • FIG. 5 shows a state in which the front surface and the rear surface, which are part of the storage container 101, are removed, and the cell stack device 10 of the fuel cell housed therein is taken out rearward.
  • the module 100 includes a storage container 101 and a cell stack device 10 housed in the storage container 101. As shown in FIG. A reformer 102 is arranged above the cell stack device 10 .
  • the reformer 102 reforms raw fuel such as natural gas and kerosene to generate fuel gas and supplies it to the cell 1 .
  • the raw fuel is supplied to the reformer 102 through the raw fuel supply pipe 103 .
  • the reformer 102 may include a vaporization section 102a for vaporizing water and a reforming section 102b.
  • the reformer 102b has a reforming catalyst (not shown) and reforms the raw fuel into fuel gas.
  • Such a reformer 102 can perform steam reforming, which is a highly efficient reforming reaction.
  • the fuel gas generated by the reformer 102 is supplied to the gas flow path 2a (see FIG. 1A) of the cell 1 through the gas flow pipe 20, the gas tank 16, and the support member 14.
  • the temperature inside the module 100 during normal power generation is about 500° C. to 1000° C. due to the combustion of gas and the power generation of the cell 1 .
  • the module 100 can reduce deterioration in power generation performance by accommodating the cell stack device 10 including a plurality of cells 1 whose internal resistance is less likely to increase. can be done.
  • FIG. 6 is an exploded perspective view showing an example of the module housing device according to the first embodiment.
  • a module housing device 110 according to this embodiment includes an exterior case 111, the module 100 shown in FIG. 5, and an auxiliary machine (not shown).
  • the accessory drives the module 100 .
  • the module 100 and auxiliary equipment are housed inside an exterior case 111 .
  • FIG. 6 a part of the configuration is omitted.
  • the partition plate 114 divides the inside of the outer case 111 into upper and lower parts.
  • the space above the partition plate 114 in the exterior case 111 is a module storage chamber 115 that stores the module 100, and the space below the partition plate 114 in the exterior case 111 stores auxiliary equipment that operates the module 100. It is the auxiliary machine accommodation room 116 which carries out.
  • the auxiliary equipment accommodated in the auxiliary equipment accommodation chamber 116 is omitted.
  • the partition plate 114 has an air circulation port 117 for flowing the air in the accessory storage chamber 116 to the module storage chamber 115 side.
  • the exterior plate 113 forming the module storage chamber 115 has an exhaust port 118 for exhausting the air inside the module storage chamber 115 .
  • the module housing chamber 115 is provided with the module 100 that reduces the deterioration of the power generation performance, thereby reducing the deterioration of the power generation performance. can be done.
  • the so-called “vertical stripe type” in which only one element portion including the fuel electrode, the solid electrolyte layer and the air electrode is provided on the surface of the support substrate is exemplified.
  • the present invention can be applied to a horizontal-striped electrochemical cell device in which so-called “horizontal-striped” electrochemical cells are arranged in which element portions are provided at respective locations and adjacent element portions are electrically connected.
  • FIG. 7A is a cross-sectional view showing an electrochemical cell according to the second embodiment.
  • the cell stack device 10A has a plurality of cells 1A extending in the length direction L from a pipe 73 for circulating fuel gas.
  • the cell 1A has a plurality of element portions 3A on the support substrate 2. As shown in FIG. Inside the support substrate 2, a gas flow path 2a through which gas from the pipe 73 flows is provided. Each element portion 3A on the support substrate 2 is electrically connected by a connection layer (not shown).
  • a plurality of cells 1A are electrically connected to each other via conductive members 18 .
  • the conductive member 18 is positioned between the element portions 3A of the cells 1A and electrically connects the adjacent cells 1A.
  • the current collector or interconnector electrically connected to the air electrode of the element portion 3A of one cell 1A among the adjacent cells 1A and the fuel electrode of the element portion 3A of the other cell 1A are electrically connected to each other. electrically connected to the electrically connected current collectors or interconnectors.
  • FIG. 7B is an enlarged cross-sectional view of a conductive member according to the second embodiment.
  • the conductive members 18 are joined to the adjacent cells 1A via the joining material 50, respectively.
  • the conductive member 18 has a first surface 181 and a second surface 182 facing each other with the base material 41 interposed therebetween.
  • the conductive member 18 has third surfaces 183 and 184 connecting the first surface 181 and the second surface 182 .
  • the conductive member 18 is joined to the cell 1A via a joining material 50.
  • the bonding material 50 is positioned between the first surface 181 of the conductive member 18 and the element portion 3A of one cell 1A, and between the second surface 182 of the conductive member 18 and the element portion 3A of the other cell 1A.
  • a pair of cells 1A and the conductive member 18 facing each other with the conductive member 18 interposed therebetween are joined.
  • the third surfaces 183 and 184 are exposed to an oxidizing atmosphere such as air.
  • the conductive member 18 has a base material 41 , a polycrystalline film 42 and a coating layer 43 .
  • Each part constituting the conductive member 18 can be made of a material similar to that of the conductive member 18 according to the first embodiment, for example.
  • the polycrystalline film 42 is located on the base material 41 .
  • Polycrystalline film 42 is located between substrate 41 and coating layer 43 .
  • Polycrystalline film 42 includes a plurality of chromium oxide particles 421 and a first element (see FIG. 4C).
  • the first element is located between the chromium oxide particles 421 and has a lower first ionization energy and free energy of oxide formation per 1 mol of oxygen than chromium.
  • the conductive member 18 Since the conductive member 18 has the first element at a specific position of the polycrystalline film 42 in this manner, the polycrystalline film 42 is difficult to grow. An increase in internal resistance is less likely to occur. As a result, it is possible to reduce the deterioration of the power generation performance of the cell 1A, thereby reducing the deterioration of the power generation performance of the cell stack device 10A.
  • FIG. 8A is a perspective view showing an electrochemical cell according to a third embodiment
  • FIG. 8B is a partial cross-sectional view of the electrochemical cell shown in FIG. 8A.
  • a cell 1B which is a plate-type electrochemical cell, has an element part 3B in which a fuel electrode 5, a solid electrolyte layer 6 and an air electrode 8 are laminated.
  • a plurality of cells 1B are electrically connected by conductive members 91 and 92 which are adjacent metal layers.
  • the conductive members 91 and 92 electrically connect adjacent cells 1B and have gas flow paths for supplying gas to the fuel electrode 5 or the air electrode 8 .
  • the conductive member 92 has a gas flow path 94 that supplies gas to the air electrode 8 .
  • the conductive member 92 is joined to the element portion 3B (air electrode 8) via the joining material 50.
  • the conductive member 92 may be in direct contact with the element portion 3B without the bonding material 50 interposed therebetween. In other words, in this embodiment, the conductive member 92 may be directly connected to the element portion 3B without using the bonding material 50 .
  • the conductive member 92 has a base material 41 , a polycrystalline film 42 and a coating layer 43 . Each part constituting the conductive member 92 can be made of a material such as the conductive member 18 described above, for example.
  • the polycrystalline film 42 is located on the base material 41 .
  • Polycrystalline film 42 is located between substrate 41 and coating layer 43 .
  • Polycrystalline film 42 includes a plurality of chromium oxide particles 421 and a first element (see FIG. 4C).
  • the first element is located between the chromium oxide particles 421 and has a lower first ionization energy and free energy of oxide formation per 1 mol of oxygen than chromium.
  • the conductive member 18 Since the conductive member 18 has the first element at a specific position of the polycrystalline film 42 in this manner, the polycrystalline film 42 is difficult to grow. An increase in internal resistance is less likely to occur. As a result, it is possible to reduce the deterioration of the power generation performance of the cell 1B, so that it is possible to reduce the deterioration of the power generation performance of the cell stack device having a plurality of cells 1B.
  • the conductive member 91 has a gas flow path 93 for supplying fuel gas to the fuel electrode 5.
  • the conductive member 91 is joined to the element portion 3B (fuel electrode 5) via the joining material 50.
  • the conductive member 91 may be in direct contact with the element portion 3B without the bonding material 50 interposed therebetween. In other words, the conductive member 91 may be directly connected to the element portion 3B without using the bonding material 50 .
  • the conductive member 91 has a base material 41 , a polycrystalline film 42 and a coating layer 43 . Each part constituting the conductive member 91 can be made of a material such as the conductive member 92 (conductive member 18) described above, for example.
  • the polycrystalline film 42 is located on the base material 41 .
  • Polycrystalline film 42 is located between substrate 41 and coating layer 43 .
  • Polycrystalline film 42 includes a plurality of chromium oxide particles 421 and a first element (see FIG. 4C).
  • the first element is located between the chromium oxide particles 421 and has a lower first ionization energy and free energy of oxide formation per 1 mol of oxygen than chromium.
  • the conductive member 91 Since the conductive member 91 has the first element at a specific position of the polycrystalline film 42 in this manner, the polycrystalline film 42 is difficult to grow. An increase in internal resistance is less likely to occur. As a result, it is possible to reduce the deterioration of the power generation performance of the cell 1B, so that it is possible to reduce the deterioration of the power generation performance of the electrochemical cell device having a plurality of cells 1B.
  • the conductive members 91 and 92 have the coating layer 43 in FIGS. 8B and 8C, one or both of the conductive members 91 and 92 may not have the coating layer 43 . That is, the polycrystalline film 42 may come into contact with the gas supplied to the fuel electrode 5 or air electrode 8 . Further, in the present embodiment, both the conductive members 91 and 92 are described as having the polycrystalline film 42 , but one of the conductive members 91 and 92 may not have the polycrystalline film 42 .
  • FIG. 9A is a cross-sectional view showing an example of an electrochemical cell according to a fourth embodiment
  • 9B and 9C are cross-sectional views showing another example of the electrochemical cell according to the fourth embodiment.
  • FIG. 9D is an enlarged view of area C shown in FIG. 9A. Note that FIG. 9D can also be applied to the examples of FIGS. 9B and 9C.
  • the cell 1C has an element portion 3C in which a fuel electrode 5, a solid electrolyte layer 6, and an air electrode 8 are laminated, and a support substrate 2.
  • the support substrate 2 has a through hole or a pore at a portion of the element section 3 that contacts the fuel electrode 5, and has a member 120 located outside the gas flow path 2a.
  • the support substrate 2 allows gas to flow between the gas flow path 2a and the element portion 3C.
  • Support substrate 2 may be composed of, for example, one or more metal plates.
  • the material of the metal plate may contain chromium.
  • the metal plate may have a conductive coating layer.
  • the support substrate 2 is a conductive member that electrically connects adjacent cells 1C.
  • the element portion 3C may be formed directly on the support substrate 2, or may be bonded to the support substrate 2 with a bonding material.
  • the side surface of the fuel electrode 5 is covered with the solid electrolyte layer 6 to airtightly seal the gas flow path 2a through which the fuel gas flows.
  • the sides of the fuel electrode 5 may be covered and sealed with a dense encapsulant 9 .
  • the sealing material 9 covering the side surface of the fuel electrode 5 may have electrical insulation.
  • the material of the sealing material 9 may be glass or ceramics, for example.
  • the gas flow path 2a of the support substrate 2 may be formed by a member 120 having unevenness.
  • the member 120 is joined to the air electrode 8 of another adjacent cell 1C via other conductive members such as the inter-cell connection member 60 and the joining material 50 . Note that the member 120 may be in direct contact with the air electrode 8 of another cell 1C without any other conductive member.
  • the member 120 has a base material 41, a polycrystalline film 42, and a coating layer 43.
  • Each part constituting the member 120 can be made of a material such as the conductive member 18 described above, for example.
  • the inter-cell connection member 60 may also be the conductive member 18 having the base material 41 , the polycrystalline film 42 , and the coating layer 43 .
  • the polycrystalline film 42 is located on the base material 41 .
  • Polycrystalline film 42 is located between substrate 41 and coating layer 43 .
  • Polycrystalline film 42 includes a plurality of chromium oxide particles 421 and a first element (see FIG. 4C).
  • the first element is located between the chromium oxide particles 421 and has a lower first ionization energy and free energy of oxide formation per 1 mol of oxygen than chromium.
  • the member 120 since the member 120 has the first element at a specific position of the polycrystalline film 42, the polycrystalline film 42 is difficult to grow. increase is less likely to occur. As a result, it is possible to reduce the deterioration of the power generation performance of the cell 1C, so that it is possible to reduce the deterioration of the power generation performance of the electrochemical cell device having a plurality of cells 1C.
  • the polycrystalline film 42 may be formed only on a part of the member 120 in this embodiment.
  • the first portion 120a facing the air electrode 8 of another cell 1C and the second portion 120b facing the support substrate 2 have the polycrystalline film 42 and the coating layer 43. good too.
  • the support substrate 2 may have a polycrystalline film 42 on the portion facing the fuel electrode 5 of the cell 1C.
  • fuel cells, fuel cell stack devices, fuel cell modules, and fuel cell devices are shown as examples of “electrochemical cells,” “electrochemical cell devices,” “modules,” and “module housing devices.”
  • electrolysis cells electrolysis cell stack devices, electrolysis modules and electrolysis devices, respectively.
  • the electrolysis cell has a first electrode layer and a second electrode layer, and decomposes water vapor into hydrogen and oxygen or carbon dioxide into carbon monoxide and oxygen when supplied with power.
  • an oxide ion conductor or a hydrogen ion conductor was shown as an example of the electrolyte material of the electrochemical cell, but a hydroxide ion conductor may be used. According to such electrolytic cell, electrolytic cell stack device, electrolytic module and electrolytic device, the electrolytic performance can be improved.
  • the conductive member 18 has the base material 41 and the polycrystalline film 42 containing a plurality of chromium oxide particles 421 and located on the base material 41 .
  • Base material 41 contains chromium.
  • the polycrystalline film 42 contains the first element. The first element is located between the chromium oxide particles 421 and has a lower first ionization energy and free energy of oxide formation per 1 mol of oxygen than chromium. Thereby, an increase in the internal resistance of the conductive member 18 can be reduced.
  • the electrochemical cell according to the embodiment includes the element portion 3 and the conductive member 18 described above.
  • the conductive member 18 is connected to the element section 3 .
  • the electrochemical cell device according to the embodiment has a cell stack 11 including a plurality of the electrochemical cells described above. As a result, it is possible to provide an electrochemical cell device that reduces deterioration in performance due to an increase in internal resistance.
  • the module 100 includes the electrochemical cell device described above and a storage container 101 that stores the electrochemical cell device. As a result, the module 100 can reduce deterioration in performance due to an increase in internal resistance.
  • the module housing device 110 includes the module 100 described above, auxiliary equipment for operating the module 100, and an exterior case for housing the module 100 and the auxiliary equipment. By this.
  • the module housing device 110 can reduce deterioration in performance due to an increase in internal resistance.

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Abstract

Cet élément électroconducteur comprend un substrat et un film polycristal. Le substrat contient du chrome. Le film polycristal contient une pluralité de particules d'oxyde chromique, et est disposé sur le substrat. Le film polycristal contient un premier élément. Le premier élément est disposé entre des particules d'oxyde chromique, qui présente une première énergie d'ionisation et une énergie libre de formation d'oxyde par mole d'oxygène inférieures à celles du chrome.
PCT/JP2022/040193 2021-10-27 2022-10-27 Élément électroconducteur, cellule électrochimique, dispositif à cellule électrochimique, module et dispositif de stockage de module WO2023074807A1 (fr)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007016297A (ja) * 2005-07-11 2007-01-25 Hitachi Metals Ltd 固体酸化物型燃料電池セパレータ用鋼
JP2008522037A (ja) * 2004-11-30 2008-06-26 サンドビック インテレクチュアル プロパティー アクティエボラーグ 電気接点用のペロブスカイトまたはスピネルの表面被膜を形成するストリップ製品
JP2010013727A (ja) * 2008-02-06 2010-01-21 Hitachi Metals Ltd 耐酸化性の優れたフェライト系ステンレス鋼

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008522037A (ja) * 2004-11-30 2008-06-26 サンドビック インテレクチュアル プロパティー アクティエボラーグ 電気接点用のペロブスカイトまたはスピネルの表面被膜を形成するストリップ製品
JP2007016297A (ja) * 2005-07-11 2007-01-25 Hitachi Metals Ltd 固体酸化物型燃料電池セパレータ用鋼
JP2010013727A (ja) * 2008-02-06 2010-01-21 Hitachi Metals Ltd 耐酸化性の優れたフェライト系ステンレス鋼

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