WO2014189177A1 - Séparateur de type maille pour pile à combustible et son procédé de fabrication - Google Patents

Séparateur de type maille pour pile à combustible et son procédé de fabrication Download PDF

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Publication number
WO2014189177A1
WO2014189177A1 PCT/KR2013/007899 KR2013007899W WO2014189177A1 WO 2014189177 A1 WO2014189177 A1 WO 2014189177A1 KR 2013007899 W KR2013007899 W KR 2013007899W WO 2014189177 A1 WO2014189177 A1 WO 2014189177A1
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Prior art keywords
resin
mesh
fuel cell
separator
mold
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PCT/KR2013/007899
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English (en)
Korean (ko)
Inventor
이용헌
이혁상
서준택
서정혁
유승을
구영모
김명환
김종학
Original Assignee
에이스산업 주식회사
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Publication of WO2014189177A1 publication Critical patent/WO2014189177A1/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
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/023—Porous and characterised by the material
    • H01M8/0239—Organic resins; Organic polymers
    • 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
    • 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
    • H01M8/023—Porous and characterised by the material
    • H01M8/0241—Composites
    • H01M8/0243—Composites in the form of mixtures
    • 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 mesh type separator for fuel cells and a method of manufacturing the same. More specifically, both the bending strength and the electrical conductivity are mainly composed of two kinds of blends having different mixing ratios of thermoplastic resins or thermosetting resins and conductive carbon materials.
  • the present invention relates to a separator for a fuel cell having an excellent mesh structure and a method of manufacturing the same.
  • a fuel cell is an electrochemical device that directly converts chemical energy of hydrogen and oxygen contained in hydrocarbon-based materials such as methanol, ethanol, and natural gas into electrical energy.
  • hydrocarbon-based materials such as methanol, ethanol, and natural gas
  • the energy conversion process of a fuel cell is very efficient and environmentally friendly. Because of this, interest continues to be in recent years.
  • the fuel cell is a phosphoric acid fuel cell (PAFC), molten carbonate fuel cell (MCFC), solid oxide fuel cell (SOFC), polymer electrolyte fuel cell (PEMFC) and alkali type depending on the type of electrolyte used It is classified into a fuel cell (AFC) and the like.
  • PAFC phosphoric acid fuel cell
  • MCFC molten carbonate fuel cell
  • SOFC solid oxide fuel cell
  • PEMFC polymer electrolyte fuel cell
  • alkali type depending on the type of electrolyte used It is classified into a fuel cell (AFC) and the like.
  • AFC fuel cell
  • Each of these fuel cells operates on essentially the same principle, but differs in the type of fuel used, operating temperature, catalyst, and electrolyte.
  • the polymer electrolyte fuel cell is known to be most promising not only for small stationary power generation equipment but also for transportation systems, and membrane electrode assemblies and separators including the polymer electrolyte membrane are the core parts. Is actively underway.
  • a membrane electrode assembly including a polymer electrolyte membrane provided between an anode and a cathode is interposed therebetween, and a separator plate having a hydrogen flow path and a separator plate having an oxygen flow path are disposed on both sides thereof.
  • the unit cell is formed, and the unit cells are formed by stacking dozens or hundreds of unit cells.
  • the separator plate must have excellent electrical conductivity as well as gas impermeability such as hydrogen and oxygen. When used for transportation, such as fuel cells, it must have high mechanical strength to withstand various shocks and vibrations. In addition, it is also known to realize a low cost process through low weight thinning of the separator, which accounts for about 80% of the weight of the fuel cell.
  • a content of a fuel cell separator is molded from a conductive curable resin composition composed of a hydrocarbon compound having several carbon-carbon double bonds, an elastomer and a carbonaceous material (Patent Document 3).
  • a conductive resin composition in which powder, fiber, or a conductive material mixed with powder and fiber is mixed with a multicomponent polymer resin binder having a number average particle size of 0.1 to 2 ⁇ m in a dispersed phase.
  • Patent Document 4 Although a technique for manufacturing a separator for a battery is also known (Patent Document 4), all of these prior arts not only select a specific polymer resin as a molding material of a thin plate separator, but also carbon fine powder, carbon nanotubes, and usually 10-20. A conductive material in the form of microparticles such as carbon fiber having a length of ⁇ m is selected. It is not easy to select the molecular material, and sufficient bending strength cannot be obtained by using only a microm fine conductive material, and when the thin plate is manufactured, the fine powder conductive material itself is expensive, so Due to the rise, there is a problem that it is difficult to realize a low-cost process.
  • Patent Document 1 Japanese Patent Application Laid-Open No. 2001-335695
  • Patent Document 2 Korea Patent Registration No. 10-0485285
  • Patent Document 3 Korean Patent Publication No. 10-2007-0110531
  • Patent Document 4 Korean Patent No. 10-0798121
  • the present invention has been devised in view of the above problems, and an object of the present invention is to realize low-cost thin weight thinning without using a specific polymer material and expensive conductive carbon material, and to have excellent flexural strength and electrical conductivity.
  • the present invention is to provide a separator plate for a fuel cell having a mesh structure and a method of manufacturing the same, comprising two kinds of blends having different blending ratios of thermoplastic resins or thermosetting resins and conductive carbon materials.
  • a mesh-type separator for fuel cells comprising a thermoplastic resin or a thermosetting resin, and two kinds of blends different in the mixing ratio of the conductive carbon material.
  • thermoplastic resin is polyethylene, polypropylene, polymethyl methacrylate, polybutylene terephthalate, polyamide, polyimide, polycarbonate, polyvinylidene fluoride, polyether sulfone, polyether ether ketone, polyphenylene sulfide, And it is characterized in that any one selected from the group consisting of polybenzimidazole.
  • thermosetting resin is characterized in that any one selected from the group consisting of phenol resin, epoxy resin, urea resin, melamine resin, unsaturated polyester resin, polycarbodiimide resin, perryl alcohol resin, and alkyd resin.
  • the conductive carbon material is characterized in any one selected from the group consisting of natural graphite, artificial graphite, expanded graphite, carbon black, carbon fiber, carbon nanotubes, amorphous carbon, and mixtures thereof.
  • thermoplastic resin or the thermosetting resin and the conductive carbon material is characterized in that 10:90 ⁇ 60:40.
  • the present invention comprises the steps of: i) kneading each of the two kinds of raw materials differing in the mixing ratio of the thermoplastic resin or the thermosetting resin and the conductive carbon material; ii) injecting two kinds of raw materials having different mixing ratios in step i) into a mold in a mesh form and pressing to form a sheet; And iii) inserting the sheet formed in step ii) into a mold having a flow path and compressing the sheet.
  • the process of putting in the mold is characterized in that it is carried out in a width of 5 ⁇ 20 mm in the form of a mesh using an automatic powder injection device.
  • the sheet formed in step ii) is characterized in that the thickness of 0.05 ⁇ 1.5 mm.
  • the sheet formed in step ii) is characterized in that the laminated structure of 2-3 layers.
  • the mold of step iii) is characterized in that a wavy flow path having a concave portion and a convex portion is formed by a stamping process.
  • Compression molding of step iii) is characterized in that it is carried out for 1 to 5 minutes at a pressure of 1,000 ⁇ 2,000 kgf / cm 2 , a temperature of 150 ⁇ 170 °C.
  • a fuel cell mesh separation plate for fuel cell which realizes low-cost low-weight thinning and excellent flexural strength and electrical conductivity without using a specific polymer material and expensive conductive carbon material.
  • FIG. 1 is a conceptual diagram of a mesh type separator for fuel cells according to the present invention.
  • FIG. 2 is an explanatory diagram of (a) surface direction and (b) vertical direction of a mesh type separator for fuel cell according to the present invention
  • Figure 3 is a mesh separator for a fuel cell prepared from Example 1 of the present invention.
  • Figure 4 is a graph showing the electrical conductivity average value, maximum value, minimum value of the mesh type separator for fuel cells prepared from Example 2 of the present invention and the separators prepared from Comparative Examples 1 and 2 [(a) Comparative Example 1 average value, (b) Example 2 maximum value, (c) Example 2 average value, (d) Example 2 minimum value, (e) Comparative example 2 average value].
  • Figure 5 is a graph showing the electrical conductivity characteristics of 17 parts of the surface of the separator plate prepared from the fuel cell mesh separator and Comparative Examples 1, 2 prepared from Example 2 of the present invention.
  • a separator for a fuel cell is formed by mixing a polymer resin and graphite particles.
  • a polymer resin is mixed to reinforce flexural strength, the flexural strength is excellent, but electrical conductivity and thermal conductivity tend to be inferior.
  • electrical conductivity and thermal conductivity tend to be inferior.
  • conductive carbon materials such as black string particles are mixed, the electric conductivity and the thermal conductivity are excellent, but the flexural strength is reduced, so that when the external shock or vibration is broken or cracks are generated, hydrogen or oxygen leaks.
  • thermoplastic resin or thermosetting resin and conductive carbon material have different mixing ratios.
  • the above problem that is, the trade-off relationship between bending strength and electrical conductivity, was solved by forming a separator using a blend of as a raw material and having the mesh structure.
  • 1 is a conceptual diagram of a mesh type separator for fuel cells according to the present invention, and two kinds of raw materials A having different mixing ratios (higher carbon materials than B) and B (lower carbon contents than A) ), And the blend is capable of forming a mesh-type separator plate in which A and B mesh structures are combined by inputting A and B raw materials in a mesh form into a mold prepared in advance.
  • the present invention provides a mesh type separator for fuel cell comprising a thermoplastic resin or a thermosetting resin and two blends having different blending ratios of conductive carbon materials.
  • a thermoplastic resin or a thermosetting resin can be used as the polymer resin that is the main raw material of the separator for fuel cell.
  • thermoplastic resin examples include polyethylene, polypropylene, polymethyl methacrylate, polybutylene terephthalate, polyamide, polyimide, polycarbonate, polyvinylidene fluoride, polyether sulfone, polyether ether ketone, polyphenylene sulfide, And polybenzimidazole, any one selected from the group consisting of can be used without limitation.
  • thermosetting resin may be any one selected from the group consisting of phenol resins, epoxy resins, urea resins, melamine resins, unsaturated polyester resins, polycarbodiimide resins, perperyl alcohol resins, and alkyd resins.
  • the phenol resin usually used in the production of separator plates for fuel cells can be used more preferably.
  • the conductive carbon material may be used without particular limitation as long as the carbon material exhibits conductivity.
  • graphite is easily available and inexpensive, and may be used regardless of the type of graphite. Any one of graphite or expanded graphite may be used, and any one selected from the group consisting of carbon black, carbon fiber, carbon nanotubes, amorphous carbon, and mixtures thereof may be used.
  • thermoplastic resin or the thermosetting resin and the conductive carbon material When the blending ratio of the thermoplastic resin or the thermosetting resin and the conductive carbon material is 10:90 to 60:40, when the two kinds of blends having different blending ratios within the range are used as raw materials, both the electrical conductivity and the flexural strength are used. It is preferable to obtain an excellent separator, and the mixing ratio can be adjusted in consideration of the characteristics of the separator within the above range.
  • Figure 2 is a diagram illustrating the electrical flow in the (a) surface direction and (b) vertical direction of the mesh type separator for fuel cell according to the present invention, the content of the carbon material compared to the two kinds of raw materials A (B) different in the mixing ratio High), B (lower carbon content than A) into mesh form, and then into the mold to form a mesh-type separating plate in which A and B mesh structures are combined. It shows that the electrical conductivity is high in the part with the raw material A, and also excellent in the conductivity with the raw material A in the vertical direction.
  • the present invention comprises the steps of: i) kneading each of the two kinds of raw materials differing in the mixing ratio of the thermoplastic resin or the thermosetting resin and the conductive carbon material; ii) injecting two kinds of raw materials having different mixing ratios in step i) into a mold in a mesh form and pressing to form a sheet; And iii) inserting the sheet formed in step ii) into a mold having a flow path and compressing the sheet.
  • thermoplastic resin or thermosetting resin, the conductive carbon material, and the blending ratio of step i) are as described above, and as the raw material of the separator, other than the thermoplastic resin or the thermosetting resin, and the conductive carbon material, glass fibers, etc. Reinforcing materials and release agents may also be added.
  • step ii) two kinds of raw materials kneaded in step i) are added in a mesh form using an automatic powder input device, and the width of the powder is preferably 5-20 mm. If the width is less than 5 mm, it is difficult to maintain the mesh form made of two kinds of raw materials in which the raw materials are mixed with each other and the mixing ratio is different. If the width exceeds 20 mm, the compatibility is inferior.
  • the sheet formed in step ii) has a thickness of 0.05 to 1.5 mm, and whether or not the final object can be formed into a thin plate-shaped separation plate is determined by the thickness of the sheet formed in step ii). Because it is determined according to the thickness can be adjusted well to reduce the thickness variation, it is possible to obtain a mesh-shaped separator plate. If the thickness of the sheet is less than 0.05 mm, there is a disadvantage that the mechanical strength is lowered, and if the thickness exceeds 1.5 mm, it is impossible to manufacture a mesh-type separation plate into a thin plate.
  • the sheet of step ii) has a multilayer structure, it is advantageous in terms of improving the performance and precision of the separator, but a sheet having a multilayer structure of more than three layers becomes so thick that the separator, which is the final object, is thinned. Since it becomes difficult to manufacture, it is preferable to have a laminated structure of 2-3 layers.
  • step iii) can be used to produce a separation plate of better performance by using a wavy channel having a concave portion and a convex portion formed by the stamping process.
  • the pressure of 1,000 to 2,000 kgf / cm 2 and the pressure of 150 to 170 are used in the compression molding of step iii).
  • the pressure of 1,000 to 2,000 kgf / cm 2 and the pressure of 150 to 170 are used in the compression molding of step iii).
  • a raw material consisting of 15 parts by weight of phenol resin and 85 parts by weight of graphite having an average particle diameter of 20 ⁇ m was kneaded, and B raw material consisting of 40 parts by weight of phenol resin and 60 parts by weight of graphite having an average particle diameter of 20 ⁇ m was kneaded, and then kneaded A, B
  • the raw material was fed into a mold in the form of a mesh of 10 mm in width using an automatic powder feeding device, and the sheet was formed by simply pressing without heating.
  • the molded sheet was introduced into a mold having a flow path and compression molded at 170 ° C. for 2 minutes and 30 seconds at a pressure of 1,000 kgf / cm 2 to prepare a mesh separator plate for a fuel cell having a thickness of 1.2 mm.
  • a thin-walled fuel cell mesh separator of 1.2 mm in thickness was manufactured in the same manner as in Example 1, except that 25 parts by weight of a phenol resin and 75 parts by weight of graphite having an average particle diameter of 20 m were used as B materials.
  • a separator for a conventional fuel cell was manufactured in the same manner as in Example 1, except that only A was added to a mold.
  • a separator for a conventional fuel cell was manufactured in the same manner as in Example 1, except that only B was added to a mold.
  • Figure 3 shows a real picture of the fuel cell mesh separator prepared from Example 1 of the present invention
  • Table 1 is a fuel cell mesh separator prepared according to Examples 1, 2 of the present invention and Electrical conductivity and flexural strength of conventional fuel cell separators prepared according to Comparative Examples 1 and 2 are shown.
  • the conventional fuel cell separators prepared according to Comparative Examples 1 and 2 use only one raw material A or one raw material B as raw materials. Therefore, electrical conductivity and flexural strength are typical according to the mixing ratio of phenol resin and graphite. While it can be seen that there is a trade-off relationship, the mesh type separator for fuel cells of thin plates manufactured according to Examples 1 and 2 of the present invention has the electrical conductivity and flexural strength without having a typical trade-off relationship. It can be confirmed that the eggplant properties are all excellent.
  • Figure 4 is a graph showing the electrical conductivity average value, maximum value, minimum value of the fuel cell mesh separator of the thin plate prepared from Example 2 of the present invention and the conventional fuel cell separator prepared from Comparative Examples 1, 2 [ (a) Comparative Example 1 average value, (b) Example 2 maximum value, (c) Example 2 average value, (d) Example 2 minimum value, (e) Comparative example 2 average value].
  • FIG. 5 shows the results of the random measurement of the electrical conductivity of 17 parts of the surface of the separator plate in order to more reliably confirm the electrical conductivity characteristics of the mesh type separator for fuel cell thin plate prepared from Example 2 of the present invention
  • the thin plate fuel cell separator prepared from Example 2 of the present invention has a mesh-like structure, and thus, two kinds of A and B raw materials having different blending ratios exhibit blended electrical conductivity characteristics.
  • the mesh separator of the thin plate manufactured according to the present invention has excellent electrical conductivity and flexural strength, and can be applied as a separator of a fuel cell.

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

Abstract

La présente invention concerne un séparateur de type maille pour une pile à combustible et son procédé de fabrication, et plus précisément, un séparateur de type maille pour une pile à combustible, ayant une excellente résistance à la flexion et une excellente conductivité électrique, comprenant, en tant que constituants principaux, deux types de mélanges dans différentes proportions de mélange d'une résine thermoplastique ou d'une résine thermodurcissable à un matériau de carbone conducteur et son procédé de fabrication. La présente invention concerne un séparateur de type maille pour pile à combustible, présentant une excellente résistance à la flexion et une excellente conductivité électrique, ce qui peut consister en une plaque mince de faible poids à faible coût sans utiliser un matériau en polymère particulier et une matière carbonée conductrice chère.
PCT/KR2013/007899 2013-05-24 2013-09-02 Séparateur de type maille pour pile à combustible et son procédé de fabrication WO2014189177A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KR10-2013-0058699 2013-05-24
KR1020130058699A KR101316006B1 (ko) 2013-05-24 2013-05-24 연료전지용 망사형 분리판 및 그 제조방법

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WO2014189177A1 true WO2014189177A1 (fr) 2014-11-27

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Publication number Priority date Publication date Assignee Title
KR101932424B1 (ko) * 2014-12-24 2018-12-27 (주)엘지하우시스 연료전지 분리판용 복합재, 연료전지 분리판 및 이의 제조방법
KR101764383B1 (ko) 2015-07-28 2017-08-02 서준택 유리섬유 부직포를 포함하는 연료전지용 박판형 분리판 및 그 제조방법

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2000067882A (ja) * 1998-08-26 2000-03-03 Mitsubishi Plastics Ind Ltd 燃料電池セル用セパレータとその製造方法
JP2002158017A (ja) * 2000-11-20 2002-05-31 Sanyo Electric Co Ltd 燃料電池用基板の製造方法及び燃料電池
JP2003323899A (ja) * 2002-02-28 2003-11-14 Sumitomo Bakelite Co Ltd 固体高分子型燃料電池用セパレータおよびその製造方法
KR20090072709A (ko) * 2007-12-28 2009-07-02 한국과학기술연구원 연료전지용 고분자 복합재료 분리판 제조방법
KR20120114511A (ko) * 2011-04-07 2012-10-17 에이스산업 주식회사 분쇄된 탄소섬유로 강화시킨 박판형 연료전지용 세퍼레이터 및 그 제조방법

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2000067882A (ja) * 1998-08-26 2000-03-03 Mitsubishi Plastics Ind Ltd 燃料電池セル用セパレータとその製造方法
JP2002158017A (ja) * 2000-11-20 2002-05-31 Sanyo Electric Co Ltd 燃料電池用基板の製造方法及び燃料電池
JP2003323899A (ja) * 2002-02-28 2003-11-14 Sumitomo Bakelite Co Ltd 固体高分子型燃料電池用セパレータおよびその製造方法
KR20090072709A (ko) * 2007-12-28 2009-07-02 한국과학기술연구원 연료전지용 고분자 복합재료 분리판 제조방법
KR20120114511A (ko) * 2011-04-07 2012-10-17 에이스산업 주식회사 분쇄된 탄소섬유로 강화시킨 박판형 연료전지용 세퍼레이터 및 그 제조방법

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