WO2014119929A1 - Procédé de fabrication d'une cellule destinée à une batterie de piles à combustible - Google Patents

Procédé de fabrication d'une cellule destinée à une batterie de piles à combustible Download PDF

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Publication number
WO2014119929A1
WO2014119929A1 PCT/KR2014/000857 KR2014000857W WO2014119929A1 WO 2014119929 A1 WO2014119929 A1 WO 2014119929A1 KR 2014000857 W KR2014000857 W KR 2014000857W WO 2014119929 A1 WO2014119929 A1 WO 2014119929A1
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Prior art keywords
layer
electrolyte layer
electrolyte
forming
filling
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PCT/KR2014/000857
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English (en)
Korean (ko)
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권오웅
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지브이퓨얼셀 주식회사
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Publication of WO2014119929A1 publication Critical patent/WO2014119929A1/fr

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    • 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
    • H01M8/1286—Fuel cells applied on a support, e.g. miniature fuel cells deposited on silica supports
    • 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
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the 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
    • H01M2008/1293—Fuel cells with solid oxide electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a method for manufacturing a stack for a fuel cell, and more particularly, to a method for manufacturing a fuel cell for improving an electrolyte layer in which pinholes are generated in a solid oxide fuel cell.
  • Solid Oxide Fuel Cells operate at the highest temperatures (700–1000 ° C) of fuel cells, using solid oxides with oxygen or hydrogen ion conductivity as electrolytes.
  • solid oxide fuel cells have a simpler structure than other fuel cells because all components are solid, there is no problem of electrolyte loss, replenishment and corrosion, no precious metal catalyst, and fuel supply through direct internal reforming. This is easy.
  • it has the advantage that thermal combined cycle power generation using waste heat is possible because the high-temperature gas is discharged.
  • a typical solid oxide fuel cell is composed of a dense electrolyte layer of oxygen ion conductivity and a porous cathode and anode positioned on both sides thereof.
  • the operating principle is that oxygen permeates through the porous cathode and reaches the electrolyte surface. Oxygen ions generated by the oxygen reduction reaction move to the fuel electrode through the dense electrolyte and react with hydrogen supplied to the porous anode to generate water. At this time, since electrons are generated at the anode and electrons are consumed at the cathode, electricity flows when the two electrodes are connected to each other.
  • the solid oxide fuel cell generates electricity in one cell, but the amount of electricity is very small to be used in real life, so the cells are stacked and used as a large amount of electrical energy. The collection of several cells is called a stack.
  • Figure 1 is a photograph showing a cross-sectional view of a single cell of the anode-supported solid oxide fuel cell according to the prior art 1.
  • a unit cell includes a porous anode support, a cathode functional layer, an electrolyte layer, and a composite air electrode layer, and the composite air electrode layer is composed of a cathode functional layer, an air electrode, and a current collector layer.
  • the metal support-type metal oxide fuel cell of the related art 2 includes a metal support 101; A first electrode 103 formed on one surface of the metal support 101; An electrolyte 107 formed on one surface of the first electrode 103 and a second electrode 109 formed on one surface of the electrolyte 107 are formed in a stacked stack to supply and discharge fuel or air. It includes a manifold 110, the first electrode 103 and the second electrode 109 is composed of different electrodes of the air electrode or fuel electrode.
  • the electrolyte material flows through the pores in the process of forming the electrolyte on the porous support to form pinholes or the like.
  • a separate method is required.
  • the thin film fuel cell 100 based on the conventional porous substrate shown in FIG. 3 in common with the prior arts 1 and 2 has an electrolyte thin film under the influence of the rough electrode (mainly anode) surface during fabrication. Defects such as pinholes may occur in the 120, and these defects may cause problems such as shorting or leakage, which may adversely affect cell performance.
  • the rough electrode mainly anode
  • An object of the present invention is to solve the problems of the prior art as described above, to remove the top portion of the first electrolyte layer in which the pinhole is formed to planarize the surface, to a highly dense packed layer It is to provide a fuel cell cell manufacturing method that can prevent problems such as short (short) or leakage (leakage) through the improvement of the electrolyte layer by stacking the second electrolyte layer after filling the pin hole.
  • the present invention comprises the steps of forming a porous first electrode layer; Forming a first electrolyte layer on the first electrode layer; Removing the top of the first electrolyte layer to planarize the removal surface; Forming a filling layer on the planarized surface of the first electrolyte layer to fill pin holes formed in the first electrolyte layer; Removing the packed layer; Forming a second electrolyte layer on the first electrolyte layer from which the filling layer is removed; And forming a second electrode layer on the second electrolyte layer.
  • planarization of the first electrolyte layer and the formation of the packed layer may be performed in one step, or the planarization of the first electrolyte layer and the formation of the packed layer may be performed in several steps by dividing the entire height.
  • the second electrolyte layer in the present invention may be formed of the same material as the first electrolyte layer, or may be formed of a different material.
  • the second electrolyte layer in the present invention may be formed by the same process as the first electrolyte layer, or may be formed by a different process.
  • the filling layer in the filling layer forming step of the present invention may be formed in a highly dense structure.
  • the filling layer in the present invention may be formed of a non-conductive material including an electrolyte or aluminum oxide (Al 2 O 3 ).
  • the upper surface of the first electrolyte layer in which the pinholes are formed is partially removed to planarize the surface, and the pinholes are filled with a highly dense packed layer, followed by stacking the second electrolyte layer.
  • the improvement of the layer has an effect that can prevent problems such as short (short) or leakage (leakage).
  • FIG. 1 is a cross-sectional view of a single cell of a cathode support solid oxide fuel cell according to the related art.
  • FIG. 2 is a cross-sectional view showing an example of a metal support-type solid oxide fuel cell according to the prior art 2.
  • FIG 3 is a reference diagram showing a state in which a pin hole is formed in the electrolyte layer in the prior art.
  • FIG. 4 is a block diagram of a fuel cell manufacturing method according to a first embodiment of the present invention.
  • 5A to 5G are flowcharts of a fuel cell manufacturing method according to a first embodiment of the present invention.
  • the present invention comprises the steps of forming a porous first electrode layer; Forming a first electrolyte layer on the first electrode layer; Removing the top of the first electrolyte layer to planarize the removal surface; Forming a filling layer on the planarized surface of the first electrolyte layer to fill pin holes formed in the first electrolyte layer; Removing the packed layer; Forming a second electrolyte layer on the first electrolyte layer from which the filling layer is removed; And forming a second electrode layer on the second electrolyte layer.
  • planarization of the first electrolyte layer and the formation of the packed layer may be performed in one step, or the planarization of the first electrolyte layer and the formation of the packed layer may be performed in several steps by dividing the entire height.
  • the second electrolyte layer in the present invention may be formed of the same material as the first electrolyte layer, or may be formed of a different material.
  • the second electrolyte layer in the present invention may be formed by the same process as the first electrolyte layer, or may be formed by a different process.
  • the filling layer in the filling layer forming step of the present invention may be formed in a highly dense structure.
  • the filling layer in the present invention may be formed of a non-conductive material including an electrolyte or aluminum oxide (Al 2 O 3 ).
  • FIG. 4 is a block diagram showing a fuel cell manufacturing method according to a first embodiment of the present invention
  • Figure 5a to 5g is a flowchart showing a fuel cell manufacturing method according to a first embodiment of the present invention. .
  • the fuel cell manufacturing method is a porous first electrode layer forming step (S200), the first electrolyte layer forming step (S210), the first electrolyte layer surface planarization step (S220), A filling layer forming step (S230), a filling layer removing step (S240), a second electrolyte layer forming step (S250), and a second electrode layer forming step (S260) are included.
  • the porous first electrode layer forming step (S200) is a step of forming the first electrode layer 310 to have a porous (porous). [See Fig. 5 (a)]
  • the first electrode layer forming step (S200) is made of a material such as platinum (platinum, Pt), palladium (Pd), nickel (Ni), ruthenium (Ru), etc., which is a high-performance catalyst, sputtering, pulsed laser deposition Anodes are deposited by chemical vapor deposition (CVD), such as physical vapor deposition (PVD), atomic layer deposition (ALD), etc. (Pulsed Laser Deposition, PLD).
  • CVD chemical vapor deposition
  • PVD physical vapor deposition
  • ALD atomic layer deposition
  • PLD Pulsed Laser Deposition
  • the first electrolyte layer forming step (S210) is a step of depositing and forming the first electrolyte layer 320 on the first electrode layer 310. At this time, in the first electrolyte layer forming step (S210), the first electrode layer 310 is formed to have a porosity, so that small pin-holes are formed under the influence of the uneven electrode surface. [See Fig. 5 (b)]
  • the first electrolyte layer 320 may include zirconium oxide (Zr x O y ), cerium oxide (Ce x O y ), lanthanum galate, barium cerate, and barium zirconate ( Choose from a wide range of ionic conductors, such as Barium Zirconate, bismuth-based oxides or Oxygen ion conducting materials such as various doping phases of these materials, or Proton conducting materials have.
  • the first electrolyte layer 320 may be applied with an electrolyte material such as Gd-doped CeO 2 (GDC) or Yttria-stabilized zirconia (YSZ), and may be sputtered or pulsed laser deposition (PLD). It is deposited by a method such as chemical vapor deposition (CVD) such as physical vapor deposition (PVD), atomic layer deposition (ALD).
  • CVD chemical vapor deposition
  • PVD physical vapor deposition
  • ALD atomic layer deposition
  • the first electrolyte layer surface planarization step (S220) is a step of removing and planarizing an upper end of the first electrolyte layer 320 to finish the surface of the first electrolyte layer 320 with the second electrolyte layer 330.
  • the first electrolyte layer surface planarization step (S220) may be performed by reactive ion etching (RIE). [See Fig. 5 (c)]
  • the filling layer 330 may be atomized to fill pin-holes formed in the first electrolyte layer 320 on the planarized surface of the first electrolyte layer 320. It is a step of depositing and forming by a method such as Chemical Vapor Deposition (CVD), such as Atomic Layer Deposition (ALD). [See Fig. 5 (d)]
  • CVD Chemical Vapor Deposition
  • ALD Atomic Layer Deposition
  • the filling layer 330 in the filling layer forming step (S230) is formed to have a highly dense structure to fill a defect space such as a pin hole when forming.
  • the filling layer 330 has a small fin in the first electrolyte layer 320 under the influence of the rough surface of the uneven first electrode layer 310 in the process of forming the first electrolyte layer 320. As holes are generated, a short circuit or leakage occurs in the fuel cell. To solve this problem, the inside of the pin hole is filled with the filling of the filling layer 330.
  • the filling layer 330 may be formed of a non-conductive material such as aluminum oxide (Al 2 O 3 ) as well as an electrolyte.
  • a non-conductive material such as aluminum oxide (Al 2 O 3 ) as well as an electrolyte.
  • Removing the filling layer (S240) is a step of removing the filling layer 330 through a process such as reactive ion etching (RIE), so that the filling of the filling layer 330 to fill only the pin hole. 1 This is a step of removing a portion in contact with the surface of the electrolyte layer 320. [See Fig. 5 (e)]
  • the first electrolyte layer is filled with the pinholes filled with the filling of the filling layer 330 while removing the upper end of the filling layer 330 in contact with the surface of the first electrolyte layer 320.
  • a second electrolyte layer 340 having a dense structure is formed by depositing a thin film on the planarized surface of the 320. [See Fig. 5 (f)]
  • the second electrolyte layer 340 may include zirconium oxide (Zr x O y ), cerium oxide (Ce x O y ), lanthanum galate, barium cerate, and barium zirconate ( Choose from a wide range of ionic conductors, such as Barium Zirconate, bismuth-based oxides or Oxygen ion conducting materials such as various doping phases of these materials, or Proton conducting materials have.
  • an electrolyte material such as Gd-doped CeO 2 (GDC) or Yttria-stabilized zirconia (YSZ) may be applied to the second electrolyte layer 340. It is deposited by a method such as chemical vapor deposition (CVD) such as physical vapor deposition (PVD), atomic layer deposition (ALD).
  • CVD chemical vapor deposition
  • PVD physical vapor deposition
  • ALD atomic layer deposition
  • the second electrolyte layer forming step (S250) is to finish the upper surface of the first electrolyte layer 320 with the second electrolyte layer 330.
  • first electrolyte layer surface planarization step S220 and the filling layer forming step S230 may be performed at a time by a height corresponding to the removal height of the first electrolyte layer 320 and the formation height of the filling layer 330.
  • the total height corresponding to the removal height of the first electrolyte layer 320 and the formation height of the filling layer 330 may be divided into a plurality of steps by the divided heights, and the steps may be sequentially performed.
  • the electrolyte materials forming the first electrolyte layer 320 and the second electrolyte layer 340 are the same material. It may be formed of or made of different materials.
  • the process of forming the first electrolyte layer 320 and the second electrolyte layer 340 is the same. It may be carried out in a process or in a different process.
  • the first electrolyte layer 320 and the second electrolyte layer 340 are the same material (for example, YSZ), but may be an application using a different material (for example, GDC), the first electrolyte layer in the deposition process
  • the chemical vapor deposition method 320 may include chemical vapor deposition (CVD) such as physical vapor deposition (PVD), atomic layer deposition (ALD), and the like, such as sputtering and pulsed laser deposition (PLD). Chemical Vapor Deposition) and the second electrolyte layer 340 may be performed by a chemical vapor deposition (CVD) process, such as atomic layer deposition (ALD). Can be.
  • CVD chemical vapor deposition
  • ALD atomic layer deposition
  • the second electrode layer forming step S260 is a step of forming the second electrode layer 350 on the second electrolyte layer 340. (See Fig. 5 (g))
  • the second electrode layer forming step (S260) is made of a high performance catalyst such as platinum (platinum, Pt), palladium (Pd), nickel (Ni), ruthenium (Ru), sputtering, pulsed laser deposition method Cathode is deposited by a method such as chemical vapor deposition (CVD) such as physical vapor deposition (PVD), atomic layer deposition (ALD), etc. (Pulsed Laser Deposition, PLD), etc. In this step, the second electrode layer 350 is formed as an electrode.
  • CVD chemical vapor deposition
  • PVD physical vapor deposition
  • ALD atomic layer deposition
  • PLD Pulsed Laser Deposition
  • the fuel cell 300 manufactured by the fuel cell manufacturing method of the present invention includes a first electrode layer 310, a first electrolyte layer 320, a second electrolyte layer 340, and a second electrode layer 350. do.
  • first and second electrolyte layers 320 and 340 provide a passage for the movement of ions between the electrodes but block the movement of electrons and separate fuel and oxygen, and are formed by the catalyst.
  • the 310 and the second electrode layer 350 serve to provide a large surface area for the electrochemical reaction to occur and to provide a movement path for electrons generated at this time.
  • the first electrode layer 310 is an anode electrode and is made of a material such as platinum (platinum, Pt), palladium (Pd), nickel (Ni), ruthenium (Ru), etc., which is a high-performance catalyst, and is formed by sputtering and pulse laser deposition ( Physical vapor deposition (PVD) such as Pulsed Laser Deposition (PLD), etc., is deposited by chemical vapor deposition (CVD) such as Atomic Layer Deposition (ALD). .
  • PVD Physical vapor deposition
  • PLD Pulsed Laser Deposition
  • CVD chemical vapor deposition
  • ALD Atomic Layer Deposition
  • the first electrode layer 310 is formed to have a porous (porous) for gas infiltration and expansion of the reaction area.
  • the first electrolyte layer 320 is formed on the first electrode layer 310, and includes zirconium oxide (Zr x O y ), cerium oxide (Ce x O y ), lanthanum galate, and barium cerate.
  • Ion conductors such as oxygen ion conducting materials, such as Cerate, Barium Zirconate, bismuth-based oxides or various doping phases of these materials, or Proton conducting materials You can choose from a wide range of categories.
  • an electrolyte material such as Gd-doped CeO 2 (GDC) or Yttria-stabilized zirconia (YSZ) may be applied to the first electrolyte layer 320.
  • GDC Gd-doped CeO 2
  • YSZ Yttria-stabilized zirconia
  • the first electrolyte layer 320 is formed such that the first electrode layer 310 has a porosity, and small pin-holes are formed therein under the influence of the uneven surface of the first electrode layer 310. .
  • the pinhole formed in the first electrolyte layer 320 is filled with the filling layer 330.
  • the second electrolyte layer 340 is formed to have a dense structure on the first electrolyte layer 320 having a flat surface, so that the pin holes of the first electrolyte layer 320 are filled with the filling material of the filling layer 330. While filling, the upper surface of the first electrolyte layer 320 is closed to prevent cracks.
  • the second electrolyte layer 340 may be formed of the same material or different materials from the first electrolyte layer 320 and the electrolyte material.
  • the first electrolyte layer 320 and the second electrolyte layer 340 are the same material (for example, YSZ), an application using another material (for example, GDC) is possible.
  • the second electrode layer 350 is a cathode electrode formed on the second electrolyte layer 340, and is made of a high performance catalyst such as platinum (platinum, Pt), palladium (Pd), nickel (Ni), ruthenium (Ru), or the like.
  • Chemical vapor deposition Chemical Vapor
  • PVD physical vapor deposition
  • ALD atomic layer deposition
  • PLD pulsed laser deposition
  • It is formed by vapor deposition by a method such as Deposition).
  • the present invention relates to a fuel cell manufacturing method, the present invention comprises the steps of forming a porous first electrode layer; Forming a first electrolyte layer on the first electrode layer; Removing the top of the first electrolyte layer to planarize the removal surface; Forming a filling layer on the planarized surface of the first electrolyte layer to fill pin holes formed in the first electrolyte layer; Removing the packed layer; Forming a second electrolyte layer on the first electrolyte layer from which the filling layer is removed; And forming a second electrode layer on the second electrolyte layer.
  • the upper surface of the first electrolyte layer in which the pinholes are formed is partially removed to planarize the surface, and the pinholes are filled with a highly dense packed layer, followed by stacking the second electrolyte layer.
  • the improvement of the layer has an effect that can prevent problems such as short (short) or leakage (leakage).

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
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Abstract

La présente invention concerne un procédé de fabrication d'une cellule destinée à une batterie de piles à combustible. Le procédé selon la présente invention comprend les étapes consistant à former une première couche d'électrode poreuse ; à former une première couche électrolytique sur la première couche d'électrode ; à aplanir la surface obtenue par la suppression de l'extrémité supérieure de la première couche électrolytique ; à former une couche de charge sur la surface aplanie de la première couche électrolytique, de façon à remplir les trous d'épingle existant dans la première couche électrolytique ; à retirer la couche de charge ; à former une seconde couche électrolytique sur la première couche électrolytique débarrassée de la couche de charge ; et à former une seconde couche d'électrode sur la seconde couche électrolytique. Selon la présente invention, la surface obtenue par le retrait de la partie extrémité supérieure de la première couche électrolytique comportant des trous d'épingle est aplanie, une couche de charge d'une densité élevée est appliquée de façon à remplir les trous d'épingle, puis la seconde couche électrolytique est appliquée de sorte que la couche électrolytique est améliorée, de façon à prévenir des problèmes tels qu'un court-circuit ou une fuite.
PCT/KR2014/000857 2013-01-29 2014-01-29 Procédé de fabrication d'une cellule destinée à une batterie de piles à combustible WO2014119929A1 (fr)

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KR20130009596 2013-01-29

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20040099149A (ko) * 2003-05-16 2004-11-26 산요덴키가부시키가이샤 연료 전지
JP2007087747A (ja) * 2005-09-21 2007-04-05 Dainippon Printing Co Ltd 固体酸化物形燃料電池
KR20100084322A (ko) * 2009-01-16 2010-07-26 삼성전자주식회사 연료전지 스택
KR20120008390A (ko) * 2010-07-16 2012-01-30 한국과학기술연구원 치밀성 박막과 이를 이용한 연료전지 및 그 제조방법
KR20120031036A (ko) * 2012-02-09 2012-03-29 한국과학기술원 금속폼 지지체를 사용하는 고체산화물 연료전지 및 그 제조방법

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20040099149A (ko) * 2003-05-16 2004-11-26 산요덴키가부시키가이샤 연료 전지
JP2007087747A (ja) * 2005-09-21 2007-04-05 Dainippon Printing Co Ltd 固体酸化物形燃料電池
KR20100084322A (ko) * 2009-01-16 2010-07-26 삼성전자주식회사 연료전지 스택
KR20120008390A (ko) * 2010-07-16 2012-01-30 한국과학기술연구원 치밀성 박막과 이를 이용한 연료전지 및 그 제조방법
KR20120031036A (ko) * 2012-02-09 2012-03-29 한국과학기술원 금속폼 지지체를 사용하는 고체산화물 연료전지 및 그 제조방법

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