WO2024143355A1 - Cellule électrochimique, dispositif de cellule électrochimique, module et dispositif de réception de module - Google Patents

Cellule électrochimique, dispositif de cellule électrochimique, module et dispositif de réception de module Download PDF

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Publication number
WO2024143355A1
WO2024143355A1 PCT/JP2023/046645 JP2023046645W WO2024143355A1 WO 2024143355 A1 WO2024143355 A1 WO 2024143355A1 JP 2023046645 W JP2023046645 W JP 2023046645W WO 2024143355 A1 WO2024143355 A1 WO 2024143355A1
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WO
WIPO (PCT)
Prior art keywords
conductive member
electrochemical cell
cell
electrode
module
Prior art date
Application number
PCT/JP2023/046645
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English (en)
Japanese (ja)
Inventor
雄一 堀
一成 宮▲崎▼
Original Assignee
京セラ株式会社
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 京セラ株式会社 filed Critical 京セラ株式会社
Publication of WO2024143355A1 publication Critical patent/WO2024143355A1/fr

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    • 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
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • 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
    • C25B9/70—Assemblies comprising two or more cells
    • 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
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0215—Glass; Ceramic materials
    • 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
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • 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
    • 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
    • Y02E60/10—Energy storage using batteries

Definitions

  • the electrochemical cell includes a first electrode, a first conductive member, and a second conductive member.
  • the first electrode contains a first material having ionic conductivity and a second material having electronic conductivity.
  • a first element is dissolved in the first material.
  • the first conductive member contains a second element different from the first element and the second material.
  • the second conductive member is located between the first electrode and the first conductive member, and contains the first element, the second element, and the second material.
  • the first element is one or more elements selected from Mg, Ca, and rare earth elements.
  • the second element is one or more elements selected from Mg, Ca, Ti, Al, Si, and rare earth elements.
  • the content of ZrO 2 , CeO 2 , BaMO 3 , SrMO 3 , etc., in which rare earth element oxides are dissolved, in the fuel electrode 5 may be in the range of 35 volume % to 65 volume %.
  • the content of Ni and/or NiO may be in the range of 65 volume % to 35 volume %.
  • the porosity of the fuel electrode 5 may be 15% or more, particularly in the range of 20% to 40%.
  • the thickness of the fuel electrode 5 may be 1 ⁇ m to 30 ⁇ m.
  • the solid electrolyte layer 6 may contain, for example, a perovskite-type compound such as BaZrO 3 or SrZrO 3 in which a rare earth element such as Sc, Y, La, Nd, Sm, Gd, Dy, or Yb is solid-dissolved.
  • a perovskite-type compound such as BaZrO 3 or SrZrO 3 in which a rare earth element such as Sc, Y, La, Nd, Sm, Gd, Dy, or Yb is solid-dissolved.
  • the material of the air electrode 8 may be, for example, a conductive ceramic such as a so-called ABO3 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 LaxSr1 - xCoyFe1 -yO3 , LaxSr1 - xMnO3 , LaxSr1 - xFeO3 , and LaxSr1 - xCoO3 , where x is 0 ⁇ x ⁇ 1 and y is 0 ⁇ y ⁇ 1.
  • the intermediate layer 7 functions as a diffusion suppression layer.
  • elements such as Sr (strontium) contained in the air electrode 8 diffuse into the solid electrolyte layer 6, a resistive layer such as SrZrO3 is formed in the solid electrolyte layer 6.
  • the intermediate layer 7 makes it difficult for Sr to diffuse, thereby making it difficult for SrZrO3 and other oxides having electrical insulation to be formed.
  • the material of the intermediate layer 7 is not particularly limited as long as it generally makes it difficult for elements to diffuse between the air electrode 8 and the solid electrolyte layer 6.
  • the material of the intermediate layer 7 may contain, for example, cerium oxide (CeO 2 ) in which a rare earth element other than Ce (cerium) is dissolved.
  • CeO 2 cerium oxide
  • a rare earth element for example, Gd (gadolinium), Sm (samarium), etc. may be used.
  • the interconnector 4 is dense, which makes it difficult for the fuel gas flowing through the gas flow passage 2a located inside the support substrate 2 and the oxygen-containing gas flowing outside the support substrate 2 to leak.
  • the interconnector 4 may have a relative density of 93% or more, particularly 95% or more.
  • the material of the interconnector 4 may be a lanthanum chromite-based perovskite oxide ( LaCrO3 -based oxide), a lanthanum strontium titanium-based perovskite oxide ( LaSrTiO3 -based oxide), or the like. These materials are conductive and are not easily reduced or oxidized even when in contact with a fuel gas such as a hydrogen-containing gas and an oxygen-containing gas such as air. In addition, a metal or an alloy may be used as the material of the interconnector 4.
  • the cell stack device 10 includes a cell stack 11 having a plurality of cells 1 arranged (stacked) in the thickness direction T of the cells 1 (see FIG. 1A), and a fixing member 12.
  • the fixing member 12 has a fixing material 13 and a support member 14.
  • the support member 14 supports the cell 1.
  • the fixing material 13 fixes the cell 1 to the support member 14.
  • the support member 14 also has a support 15 and a gas tank 16.
  • the support member 14, which is made of a metal, has electrical conductivity.
  • the gas tank 16 has an opening for supplying reactive gas to the multiple cells 1 through the insertion holes 15a, and a groove 16a located around the opening.
  • the outer peripheral edge of the support 15 is joined to the gas tank 16 by a bonding material 21 filled in the groove 16a of the gas tank 16.
  • Hydrogen-rich fuel gas can be produced by, for example, steam reforming the raw fuel.
  • fuel gas is produced by steam reforming, the fuel gas contains water vapor.
  • 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. This bonds and fixes the inner wall of the insertion hole 15a to the lower ends of the multiple cells 1, and also bonds and fixes the lower ends of the cells 1 to each other.
  • the gas flow path 2a of each cell 1 communicates with the internal space 22 of the support member 14 at its lower end.
  • the fixing material 13 and the bonding material 21 may be made of a material with low electrical conductivity, such as glass.
  • Specific materials for the fixing material 13 and the bonding material 21 may include amorphous glass, and in particular, crystallized glass.
  • the content of the first element, the second element, the first material, and the second material can be confirmed by, for example, elemental analysis using EPMA. Specifically, for example, a cross section of the element portion 3 in the stacking direction is mirror-polished, and the first element, the second element, the first material, and the second material are each semi-quantitatively analyzed in a predetermined area, thereby calculating the content per unit area of each.
  • the content of the first element may be evaluated, for example, as the ratio of the first element to the sum of the first element, the second element, and the metal elements that make up the first material.
  • the content of the first element contained in the fuel electrode 5 may decrease as it approaches the support substrate 2 in a cross section of the element portion 3 in the stacking direction.
  • the content of the first element in the fuel electrode 5 may be distributed so as to decrease as it approaches the boundary between the fuel electrode 5 and the second conductive member 2b. This further improves the durability of the cell 1.
  • the fuel electrode 5, the second conductive member 2b and the support substrate 2 may have a portion in which the content of the first element is a maximum value and/or a minimum value in a cross section of the element portion 3 in the stacking direction.
  • a maximum value is a local maximum value
  • a minimum value is a local minimum value.
  • the boundary between the second conductive member 2b and the fuel electrode 5 is, for example, the portion closest to the solid electrolyte layer 6 among the portions where the content of the first element is at a minimum value.
  • the content of the first element contained in the boundary between the second conductive member 2b and the fuel electrode 5 may be, for example, 1/3 or less of the content of the first element in the vicinity of the solid electrolyte layer 6 of the fuel electrode 5.
  • the boundary between the second conductive member 2b and the support substrate 2 is, for example, a portion where the distance from the solid electrolyte layer 6 is greater than the distance to the boundary between the second conductive member 2b and the fuel electrode 5, and where the content of the first element is equal to the content of the first element at the boundary between the second conductive member 2b and the fuel electrode 5.
  • the second conductive member 2b may have a portion where the content of the first element is at a maximum value between the boundary between the second conductive member 2b and the fuel electrode 5 and the boundary between the second conductive member 2b and the support substrate 2.
  • the second conductive member 2b may contain a greater amount of the first material containing the first element in a portion closer to the fuel electrode 5 than in a portion farther from the fuel electrode 5. This makes the fuel electrode 5 less likely to peel off from the support substrate 2.
  • the second conductive member 2b may contain a greater amount of an oxide of the first element in a portion closer to the support substrate 2 than in a portion farther from the support substrate 2. This makes the fuel electrode 5 less likely to peel off from the support substrate 2.
  • the second conductive member 2b may contain a first material containing the second element in a portion closer to the fuel electrode 5.
  • the content of the second material in the fuel electrode 5, the support substrate 2, and the second conductive member 2b may be the same or different.
  • Fig. 4 is an external perspective view showing the module according to the first embodiment.
  • Fig. 4 shows a state in which the front and rear surfaces, which are part of the storage container 101, have been removed and the cell stack device 10 of the fuel cell stored inside has been removed to the rear.
  • the module 100 includes a storage container 101 and a cell stack device 10 stored in the storage container 101.
  • a reformer 102 is disposed above the cell stack device 10.
  • the reformer 102 reforms raw fuel such as natural gas or kerosene to generate fuel gas, which is then supplied to the cell 1.
  • the raw fuel is supplied to the reformer 102 through a raw fuel supply pipe 103.
  • the reformer 102 may also include a vaporizer 102a that vaporizes water, and a reformer 102b.
  • the reformer 102b includes 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 in the reformer 102 is then supplied to the gas flow path 2a (see Figure 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 approximately 500°C to 1000°C due to the combustion of gas and power generation by the cell 1.
  • the highly durable cell stack device 10 is housed and configured, thereby making the module 100 highly durable.
  • Fig. 5 is an exploded perspective view showing an example of a module housing device according to the first embodiment.
  • the module housing device 110 according to this embodiment includes an outer case 111, the module 100 shown in Fig. 4, and auxiliary equipment (not shown).
  • the auxiliary equipment operates the module 100.
  • the module 100 and the auxiliary equipment are housed in the outer case 111. Note that some components are omitted in Fig. 5.
  • the exterior case 111 of the module accommodating device 110 shown in Figure 5 has support posts 112 and an exterior plate 113.
  • a partition plate 114 divides the interior of the exterior case 111 into upper and lower sections.
  • the space above the partition plate 114 in the exterior case 111 is a module accommodating chamber 115 that accommodates the module 100, and the space below the partition plate 114 in the exterior case 111 is an auxiliary equipment accommodating chamber 116 that accommodates the auxiliary equipment that operates the module 100. Note that in Figure 5, the auxiliary equipment accommodated in the auxiliary equipment accommodating chamber 116 is omitted.
  • the partition plate 114 also has an air flow port 117 for allowing air from the auxiliary equipment housing chamber 116 to flow toward the module housing chamber 115.
  • the exterior plate 113 that constitutes the module housing chamber 115 has an exhaust port 118 for exhausting air from within the module housing chamber 115.
  • a highly durable module 100 is provided in the module storage chamber 115, thereby making the module storage device 110 highly durable.
  • a hollow flat support substrate is used, but the present invention can also be applied to a cell stack device that uses a cylindrical support substrate.
  • a so-called “vertical stripe type” in which only one element part including a fuel electrode layer, a solid electrolyte layer, and an air electrode layer is provided on the surface of the support substrate is exemplified, but the present invention can also be applied to a horizontal stripe type electrochemical cell device in which so-called “horizontal stripe type” electrochemical cells are arranged in which element parts are provided at multiple locations spaced apart from each other on the surface of the support substrate and adjacent element parts are electrically connected.
  • FIG. 6 is a cross-sectional view of an electrochemical cell device according to the second embodiment.
  • FIG. 7 is a cross-sectional view showing an example of an electrochemical cell according to the second embodiment.
  • the cell 1A includes a support substrate 2, a pair of element portions 3, and a sealing portion 30.
  • the support substrate 2 is columnar, having a pair of opposing flat surfaces, a first surface n1 and a second surface n2, and a pair of arc-shaped side surfaces m connecting the first surface n1 and the second surface n2.
  • Cell 1A may have a symmetrical shape with respect to a plane that passes through the center of the thickness direction T and is parallel to the first surface n1 and the second surface n2 of the support substrate 2.
  • the element section 3 includes a fuel electrode 5, a solid electrolyte layer 6, and an air electrode 8.
  • the element section 3 may include an intermediate layer 7 between the solid electrolyte layer 6 and the air electrode 8.
  • FIG. 8 is an enlarged cross-sectional view of region R2 shown in FIG. 7.
  • cell 1A includes a solid electrolyte layer 6, a fuel electrode 5, and an insulating support substrate 2.
  • the solid electrolyte layer 6 contains a first material in which a first element is dissolved.
  • the first element is one or more elements selected from Mg, Ca, and rare earth elements.
  • the first material may include, for example, stabilized zirconia containing Sc, Y, Yb, or the like.
  • the fuel electrode 5 includes a fuel electrode functional layer 5a as a first electrode, a fuel electrode current collecting layer 5b as a first conductive member, and a second conductive member 5c.
  • the fuel electrode functional layer 5a contains a first material having ionic conductivity and a second material having electronic conductivity.
  • the fuel electrode current collecting layer 5b is a first conductive member and contains a second element and a second material.
  • the second element is one or more elements selected from Mg, Ca, Ti, Al, Si, and rare earth elements, and is an element different from the first element.
  • the fuel electrode current collecting layer 5b may contain, for example, stabilized zirconia containing Sc, Y, Yb, or the like.
  • the insulating support substrate 2 may or may not contain stabilized zirconia containing, for example, Sc, Y, Yb, or the like.
  • the second conductive member 5c is located between the fuel electrode functional layer 5a as the first electrode and the fuel electrode current collecting layer 5b as the first conductive member.
  • the second conductive member 5c contains a first element, a second element, and a second material.
  • the gas flow path 2a of the support substrate 2 may also be formed by a member 120 having projections and recesses as shown in FIG. 9C.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Metallurgy (AREA)
  • Materials Engineering (AREA)
  • Sustainable Energy (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
  • Ceramic Engineering (AREA)
  • Conductive Materials (AREA)
  • Battery Mounting, Suspending (AREA)
  • Secondary Cells (AREA)

Abstract

L'invention concerne une cellule électrochimique comprenant une première électrode, un premier élément conducteur et un second élément conducteur. La première électrode contient un premier matériau ayant une conductivité ionique dans laquelle un premier élément est solubilisé à l'état solide, et un second matériau ayant une conductivité électronique. Un premier élément est solubilisé à l'état solide dans le premier matériau. Le premier élément conducteur contient un second élément différent du premier élément, et un second matériau. Un second élément conducteur est situé entre la première électrode et le premier élément conducteur, et contient un premier élément, un second élément et un second matériau. Le premier élément est au moins un élément choisi parmi Mg, Ca et des éléments des terres rares. Le second élément est au moins un élément choisi parmi Mg, Ca, Ti, Al, Si et des éléments des terres rares.
PCT/JP2023/046645 2022-12-26 2023-12-26 Cellule électrochimique, dispositif de cellule électrochimique, module et dispositif de réception de module WO2024143355A1 (fr)

Applications Claiming Priority (2)

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JP2022209058 2022-12-26
JP2022-209058 2022-12-26

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WO2024143355A1 true WO2024143355A1 (fr) 2024-07-04

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2004152585A (ja) * 2002-10-30 2004-05-27 Kyocera Corp 燃料電池セル及び燃料電池
JP2005346991A (ja) * 2004-05-31 2005-12-15 Kyocera Corp 固体電解質形燃料電池セルスタック、バンドル及び燃料電池並びに燃料電池セルスタックの製造方法
JP2013110093A (ja) * 2011-10-25 2013-06-06 Ngk Insulators Ltd 燃料電池の構造体
JP2013110090A (ja) * 2011-10-25 2013-06-06 Ngk Insulators Ltd 燃料電池の構造体

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2004152585A (ja) * 2002-10-30 2004-05-27 Kyocera Corp 燃料電池セル及び燃料電池
JP2005346991A (ja) * 2004-05-31 2005-12-15 Kyocera Corp 固体電解質形燃料電池セルスタック、バンドル及び燃料電池並びに燃料電池セルスタックの製造方法
JP2013110093A (ja) * 2011-10-25 2013-06-06 Ngk Insulators Ltd 燃料電池の構造体
JP2013110090A (ja) * 2011-10-25 2013-06-06 Ngk Insulators Ltd 燃料電池の構造体

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