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WO1999049530A1 - Separateur pour element a combustible et son procede de production - Google Patents

Separateur pour element a combustible et son procede de production Download PDF

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Publication number
WO1999049530A1
WO1999049530A1 PCT/JP1999/001349 JP9901349W WO9949530A1 WO 1999049530 A1 WO1999049530 A1 WO 1999049530A1 JP 9901349 W JP9901349 W JP 9901349W WO 9949530 A1 WO9949530 A1 WO 9949530A1
Authority
WO
WIPO (PCT)
Prior art keywords
fuel cell
resin
conductive
molded body
cell separator
Prior art date
Application number
PCT/JP1999/001349
Other languages
English (en)
Japanese (ja)
Inventor
Hiroyuki Tajiri
Satoshi Yamaguchi
Naoto Yoshinaga
Yoshiteru Nakagawa
Original Assignee
Osaka Gas Company Limited
Kanebo, Ltd.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Osaka Gas Company Limited, Kanebo, Ltd. filed Critical Osaka Gas Company Limited
Publication of WO1999049530A1 publication Critical patent/WO1999049530A1/fr

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Classifications

    • 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
    • H01M8/0247—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form
    • H01M8/0256—Vias, i.e. connectors passing through the separator material
    • 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
    • H01M8/0213—Gas-impermeable carbon-containing 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
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0221—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
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204—Non-porous and characterised by the material
    • H01M8/0223—Composites
    • H01M8/0226—Composites in the form of mixtures
    • 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
    • H01M8/0223—Composites
    • H01M8/0228—Composites in the form of layered or coated products
    • 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 invention relates to separation in a fuel cell (particularly, a polymer electrolyte fuel cell) and a method for producing the same.
  • a fuel cell for example, a solid polymer fuel cell uses a solid polymer membrane (such as a Nafion membrane of DuPont or a Dow chemical of Dow Chemical) as an electrolyte membrane, and has a thickness of 0.1 on both sides of the electrolyte membrane.
  • a porous graphite paper of about 0.3 mm is provided, and a platinum alloy catalyst is supported as an electrode catalyst on the surface of the paper. Outside the graphite vapor, a porous graphite plate having a thickness of about 1 to 3 mm and a dense carbon plate having a thickness of about 0.5 mm are provided with grooves serving as gas flow paths.
  • a cell is constructed by sequentially arranging flat plate separators, or a separate carbon plate, which is a dense carbon plate with a thickness of about 1 to 3 mm with grooves formed as gas passages, Make up.
  • the plate separator is required to have gas impermeability to oxygen and hydrogen, electric conductivity, heat conductivity, mechanical strength, acid resistance and the like.
  • a grooved separator in addition to the performance required for a flat plate separator, it is required that the dimensional accuracy of the gas flow path be high.
  • Such separators are manufactured by forming a flat plate by carbonizing or graphitizing a molded plate of phenolic resin and graphite powder, or by forming grooves on the surface of the flat plate by cutting. It is also manufactured using petroleum or coal pitch instead of phenol resin.
  • an object of the present invention is to provide a fuel cell separator (particularly a solid polymer) having excellent properties such as gas impermeability, electrical conductivity, thermal conductivity, mechanical strength, and acid resistance without undergoing a carbonization step. And a method for manufacturing the same.
  • Another object of the present invention is to provide a fuel cell capable of forming grooves (gas flow paths) with high dimensional accuracy in addition to characteristics such as high electrical conductivity and thermal conductivity by molding without going through a carbonizing step and a cutting step. It is an object of the present invention to provide a method for producing a separator for a fuel cell (particularly a separator for a polymer electrolyte fuel cell). Disclosure of the invention
  • the inventors of the present invention have conducted intensive studies to achieve the above object, and as a result, have formed a non-carbonaceous resin (particularly, a combination of a resin and a specific conductive agent) or a resin molded body and a conductive member. When they were formed together, they found that a high-performance separator could be obtained without going through the carbonization and cutting steps, and completed the present invention.
  • the separator for a fuel cell of the present invention contains a non-carbonaceous resin and has a large thickness.
  • the thermal conductivity in the thickness direction of the separator may be about 2 to 60 WmK.
  • Such separations consist of (a) non-carbon resin, at least one conductive agent selected from spherical graphite, graphite powder with an aspect ratio of 2.0 or less, and conductive carbon black. Included is the separation of molded synthetic resin composites.
  • the separation includes a separation consisting of (b) a synthetic resin molded body and a conductive member integrated with the molded body. Separation (b) may have the same characteristics as described above.
  • the separator (a) can be manufactured by injection molding or compression molding, and the separator (b) can be manufactured by integrating a synthetic resin molded body and a conductive member by molding.
  • Non-carbonaceous resin means a resin selected from thermosetting resin and thermoplastic resin, and is, for example, heat-treated at a temperature of 700 ° C. or less (particularly 500 ° * or less). Carbonized or graphitized resin fired at a temperature of 700 or more (especially 500 or more).
  • the synthetic resin molded product is a molded product of a non-carbonaceous resin, or a molded product composed of a non-carbonous resin and a conductive agent, and if necessary, carbon fibers.
  • FIG. 1 is a schematic sectional view showing an example of a fuel cell separator according to the present invention.
  • FIG. 2 is a schematic sectional view showing another example of the fuel cell separator of the present invention.
  • FIG. 3 is a schematic sectional view showing still another example of the fuel cell separator of the present invention.
  • FIG. 4 is a schematic sectional view showing another example of the fuel cell separator of the present invention.
  • FIG. 5 is a schematic sectional view showing still another example of the fuel cell separator according to the present invention.
  • FIG. 6 is a schematic sectional view showing another example of the fuel cell separator of the present invention.
  • the separator for a fuel cell of the present invention is characterized by having a small volume resistance in the thickness direction and a high bending strength without going through a carbonization or graphitization step.
  • the volume resistance in the thickness direction of the separator is 0.15 Qcm or less (e.g., 0.000 0 1 to 0.15 Qcm), preferably 0.00 0 1 to 0.1 Q. cm, more preferably about 0.001 to 0.08 ⁇ cm.
  • Flexural strength 3 ⁇ 2 0 kgf / mm 2 , preferably 5 ⁇ 2 0 kgf / mm 2, more preferably 1 0 ⁇ 2 0 kgi Z mm ⁇ extent.
  • the thermal conductivity in the thickness direction of the separator is 2 to 60 WmK, preferably 3 to 60 WZmK, and more preferably about 5 to 60 W / mK.
  • the thickness of the separator is, for example, 0.5 to 3 mm, preferably about 0.8 to 2.5 mm, and the bulk density is a range that does not impair the gas barrier properties, for example, 1.1 to 2. It is about 2 gZcm 3 .
  • thermosetting resins and thermoplastic resins are at least one type of resin selected from thermosetting resins and thermoplastic resins.
  • (Binder) is composed of non-carbonaceous resin.
  • the thermosetting resin include a phenol resin, a copna resin (a resin obtained by reacting an aromatic aldehyde and an aromatic compound), a furan resin, an epoxy resin, a polyimide, a resin, and an amino resin. (Melamine resin, urea resin, etc.) and unsaturated polyester resin. These thermosetting resins can be used alone or in combination of two or more.
  • thermosetting resins phenolic resins are excellent in heat resistance, acid resistance, strength, hot water resistance, and cost.
  • the phenolic resins include ordinary resole resins, novolak resins, phenolic resins formed by a specific reaction of phenols with aldehydes, and phenolic resins formed by the reaction of phenols with aldehydes and nitrogen-containing compounds.
  • Hue also includes phenolic resins (copolymerized phenolic resins).
  • the phenolic resin obtained by the specific reaction between the above phenols and aldehydes and a method for producing the same are disclosed in Japanese Patent Publication No. Sho 62-32111.
  • HCHO formaldehyde
  • hydrochloric acid and formaldehyde 15 to 40% by weight in a formaldehyde hydrochloride bath.
  • the phenols are brought into contact with each other while maintaining the phenols in a specific ratio.
  • the contact causes turbidity of the phenols, and then the contact is carried out so as to form a granular or powdery solid.
  • a granular or powdery resin By maintaining the temperature in the reaction system at 45 or less during this contact, a granular or powdery resin can be obtained.
  • the resin solid may be separated from the reaction mixture, washed with water, and neutralized with an aqueous alkali solution (aqueous solution containing a base such as alkali metal hydroxide and ammonia).
  • the obtained phenolic resin is (1) substantially composed of carbon, hydrogen, and oxygen atoms, and (2) a methylene group, a methylol group, and a phenol group residue having three functions as main binding units. Contained, the trifunctional phenolic residue binds to the methylene group at one of the 2, 4 and 6-positions, and at least one other to the methylene group and Z or the methylol group. are doing.
  • the powdery phenol resin contains ( ⁇ ) spherical primary particles having an average particle diameter of 0.1 to 150 and secondary clots, and (B) at least 50% by weight of (C)
  • the free phenol content by liquid chromatography is 50 to 500 ppm (preferably 400 ppm or less, more preferably 300 ppm or less). ppm or less).
  • the solubility of the resin in methanol is 20% by weight or more (preferably 30% by weight or more, more preferably 40% by weight or more).
  • a polyolefin-based resin polypropylene
  • polyester-based resin polyalkylene terephthalate, polyalkylene naphthate or their copolyester, polyarylate, etc.
  • polycarbonate resin bisphenol A-type polycarbonate
  • Styrene-based resin such as styrene alone or copolymer
  • acrylic resin alone or copolymerized with acryl-based monomer such as methyl methacrylate.
  • Polyamide resin Polyamide 6, Polyamide 66, Polyamide 610, etc.
  • Polyamide resin Polyamide 6, Polyamide 66, Polyamide 610, etc.
  • examples include phenylene ether resin, polyphenylene sulfide resin, polyester terketone resin, polysulfone resin (polysulfone resin, polyethersulfone resin, etc.) These thermoplastic resins may be used alone or Two or more can be used in combination.
  • conductive agent at least one selected from spherical graphite, graphite powder having an aspect ratio of 2.0 or less, and conductive carbon black (such as furnace black) can be used.
  • spheroidal graphite examples include graphitized mesocarbon microbeads, spheroidized natural and artificial graphite, Flutcox, and Gilsonie. And tocokes.
  • MCMB mesocarbon microbeads
  • the average particle size of the spherical MCMB is usually 5 to 50 m (e.g., 5 to 25 m), preferably 10 to 40 m (e.g., 10 to 25 tim), particularly 10 to 50 m. It is about 30 Aim.
  • MCM B is formed by heating bituminous substances such as coal tar, coal rubbit, and heavy oil at a temperature of about 300-500. Such a method for producing MCMB is described in, for example, Japanese Patent Publication No. 11-27968 and Japanese Patent Publication No. Hei 1-264691.
  • Graphitized MCMB is a graphitized version of MCMB in the usual way.
  • Examples of the graphite powder include natural and artificial graphite powder having an aspect ratio of 2.0 or less (1 to 2.0).
  • the average particle size of the graphite powder is, for example, 2 to 35 / zm, preferably It is about 5 to 30 m.
  • Artificial graphite powder is obtained by using petroleum coke or the like as a raw material, molding, firing, and further graphitizing at a high temperature of 2000 or more.
  • the composite material composed of the resin and the conductive agent may further contain carbon fibers.
  • the type of carbon fiber is not limited, and petroleum-based or coal-based pitch-based carbon fiber, PAN (polyacrylonitrile) -based carbon fiber, rayon-based carbon fiber, phenol resin-based carbon fiber, and the like can be used.
  • the average fiber diameter of the carbon fibers can be selected from the range of, for example, 0.5 to 50 zm, preferably 1 to 30 um., And more preferably 5 to 20 m.
  • the average fiber length of the carbon fibers can be appropriately selected and is, for example, about 10 m to 5 mm, and preferably about 20 m to 3 mm.
  • the amount of carbon fiber used can be selected from the range of about 1 to 10% by weight of the whole composite material constituting Separé. If the carbon fiber content exceeds 10% by weight, the airtightness is reduced and the gas permeability is increased.
  • a synthetic resin composite material composed of a resin, a conductive agent, and, if necessary, carbon fiber, etc.
  • a coupling agent a release agent, a lubricant, a plasticizer, a curing agent, a curing aid, if necessary.
  • a stabilizer and the like may be appropriately blended.
  • Such a separator (a) can be produced by a conventional molding method for a composite material, for example, injection molding or compression molding.
  • injection molding the resin, the conductive agent, and if necessary, a composite material component composed of carbon fiber are melt-kneaded (prepared as necessary and melt-kneaded), and injection-molded into a predetermined mold.
  • a flat plate separator can be manufactured.
  • a thermosetting resin used in the compression molding, for example, at a pressure of about 20 to 100 kg / cm 2 and a temperature of about 100 to 300, the composite material component is placed in a mold. By heating and pressing under pressure, a flat separator can be manufactured.
  • the separation (b) of the separation for the fuel cell is composed of a synthetic resin molded body and a conductive member integrated with the molded body.
  • the synthetic resin molded body may be formed of the resin alone, and as in the case of the separator (a), a synthetic resin composite material (conductive composite) composed of a resin, a conductive agent, and, if necessary, carbon fiber. Material).
  • the type and form of the conductive member are not particularly limited, and a coating (such as a conductive coating film), a fibrous conductive member (a conductive fiber such as a metal fiber or a carbon fiber, or a strand thereof) may be used.
  • the volume resistivity of the conductive member for example, as a 1 0 _ 5 to 1 0 "may be about 2 Omega cm.
  • the conductive member a metal, e.g., Al Miniumu, copper, gold, silver, and platinum .
  • the separation (b) includes various aspects, for example, (b-1) a separation for a fuel cell in which at least one surface of a synthetic resin molded body is covered with a conductive member; (b-2) At least one side or inside of the synthetic resin molded body includes a separator for a fuel cell having a closely adhered or embedded conductive member.
  • the conductive member is often a conductive film or a thin-film conductive member.
  • the conductive member is a flat conductive member ⁇ rod-shaped conductive member. It is often a member, and the conductive member may be at least partially embedded in the synthetic resin molded body.
  • the fuel cell separator (b) can be manufactured by integrating a synthetic resin molded body and a conductive member by molding. More specifically, molding is performed using a compression molding machine including a flat mold (female mold) having a cavity and a mold (male or core) corresponding to the cavity and having an uneven portion. At this time, a step of disposing a conductive member (such as a conductive sheet) on a portion of the mold corresponding to at least one side (one side or both sides) of the molded body; By performing the pressing step, a separator having at least one surface covered with a conductive member or a separator having at least one surface closely adhered to a conductive member can be manufactured.
  • a conductive member such as a conductive sheet
  • the conductive member may be provided so as to be peelable from the mold, and may be provided (or adhered) using an adhesive if necessary. Further, the conductive member can be disposed on the cavity side and the Z or core side of the mold. . Further, instead of disposing the conductive member, a step of applying a conductive member (such as a conductive resin composition) to at least a portion of the mold corresponding to one side (one side or both sides) of the molded body is adopted, It is also possible to manufacture a fuel cell separator by passing a synthetic resin or the above composite material into the cavity and pressurizing the same.
  • the conductive resin composition may be in the form of a conductive paint or the like, and may be releasably applied to the cavity side and / or the core side of the mold.
  • a step of previously setting a conductive member such as a conductive metal plate
  • a conductive member such as a conductive metal plate
  • a member such as a metal plate
  • the pressure molding can be performed according to a conventional method according to the type of the resin, for example, when a thermosetting resin is used, at a pressure of S O L O O O K g Z cm at a temperature of about 100 to 300.
  • compression molding, transfer molding, and the like can be used for pressure molding, and insert molding can also be applied to these molding methods.
  • a conductive member is disposed on at least one of the mold side and the core side (usually, the cavity side), and the mold is made of a synthetic resin or the composite material. And insert the conductive insert (insert pin, insert plate, etc.) into one of the mold side (usually the core side) and the other side (usually the cavity side).
  • the conductive insert may be buried in the thickness direction of the separator.
  • FIG. 1 is a schematic sectional view showing an example of a fuel cell separator according to the present invention.
  • the fuel cell separator is provided with a conductive metal foil 3 having an uneven cross section and a conductive insert bin 2 standing up at predetermined intervals in a plurality of recesses of the conductive metal foil.
  • the conductive metal foil 3 and the conductive insert bin 2 are integrated with the resin molded body 1.
  • One end face of the conductive insert pin 2 is electrically connected to the conductive metal foil 3, and the other end face is exposed on the flat surface of the resin molding 1.
  • conductive metal foil (aluminum foil, platinum foil, etc.) 3 is temporarily fixed along the concave / convex grooves on the core side of the mold in a concave / convex section, and a plurality of conductive inserts are used.
  • a pin (such as an aluminum insert bin) 2 can be obtained by inserting the resin 1 into a plurality of projections on the core side of the mold at predetermined intervals, standing up, and then putting the resin 1 into the mold and molding.
  • the resin 1 may be a thermosetting resin or a thermoplastic resin, and is typically a phenol resin.
  • the molding is performed by filling the resin 1 with the conductive metal foil (aluminum foil, platinum foil, etc.) 3 present on either the cavity side or the core side of the mold, and then performing pressure molding. be able to.
  • the conductive insert pin (aluminum insert pin) 2 can be inserted in the thickness direction of the separator by contacting the conductive metal foil 3 to impart conductivity in the thickness direction.
  • FIG. 2 is a schematic sectional view showing another example of the fuel cell separator of the present invention.
  • This fuel cell separator is the same as the separator shown in FIG. 1 except that the sheet-shaped conductive metal foil 3 is located on the surface opposite to the conductive metal foil 3 having the uneven cross section. Both end surfaces of the pin 2 are in contact with the conductive gold foil 3 on both sides, and the conductive gold foil 3 on both sides and the conductive insert pin 2 are integrated with the resin molding 1.
  • Such fuel cell separators are located on the core and cavity sides of the mold.
  • a conductive metal foil with an uneven cross section and a sheet-shaped conductive metal foil (aluminum foil, platinum foil, etc.) 3 are fixed, and an aluminum insert bin 2 is inserted into the convex part of the core, and the resin It can be obtained by molding by adding 1.
  • the conductive metal foil 3 can be integrated on both sides of the separator as it is formed.
  • FIG. 3 is a schematic sectional view showing still another example of the fuel cell separator of the present invention.
  • This fuel cell separator has a plate-shaped resin molded product 1 having an uneven groove formed on one surface, a conductive paint 4 formed on the uneven surface of the resin molded product, It is composed of a conductive insert pin 2 that extends in the thickness direction upon contact, and a resin molded body 1, a conductive paint 4, and a conductive insert bin 2 are integrated. Further, the conductive insert bins 2 are respectively arranged in adjacent grooves of the resin molded body 1.
  • One end face of the conductive insert pin 2 is arranged on the bottom of the adjacent concave groove of the resin molded body 1 in contact with the conductive paint 4, and the end face of the insert bin 2 is formed of the resin molded body. It is exposed on 1 flat surface.
  • a separator for fuel cells is prepared by applying a conductive paint (Dohite, manufactured by Fujikura Kasei Co., Ltd., etc.) 4 to the core of the mold by brushing or the like in a releasable manner. It can be obtained by inserting a conductive insert pin (aluminum insert pin) 2 in the thickness direction and adding resin 1 and molding. The molding was performed in the same manner as the fuel cell separator shown in Fig.
  • the conductive insert pins 2 are erected in the mold to form the resin molded body 1 having the concave and convex grooves on one surface, and the conductive paint 4 is coated on the concave and convex surface of the obtained resin molded body 1. By coating, a separator for a fuel cell having the above structure can be obtained.
  • FIG. 4 is a schematic sectional view showing another example of the fuel cell separator of the present invention.
  • This fuel cell separator is the same as the fuel cell separator shown in FIG. 3 except that a resin molded body 1 having an uneven groove on one surface is provided.
  • Such a fuel cell separator having conductivity on both sides is coated with a conductive paint (such as a metal sheet) 4 on the mold side and the core side in a releasable manner.
  • Insert the resin by inserting the conductive insert pin into the mold, and insert the resin 1 into the mold, and then raise the conductive insert bin 2 in the mold to form a resin with an uneven groove on one surface. It can be obtained by molding the body 1 and applying the conductive paint 4 to both sides of the obtained resin molded body 1.
  • FIG. 5 is a schematic sectional view showing still another example of the fuel cell separator of the present invention.
  • This fuel cell separator is composed of a conductive resin molded body 5 having an uneven groove formed on one surface, and a conductive plate material (eg, an aluminum plate) 6 integrated with a flat surface of the molded body.
  • a conductive plate material eg, an aluminum plate
  • Separators having such a structure can be obtained by temporarily fixing a conductive plate material (such as an aluminum plate) 6 to the mold cavity side, placing conductive resin 5 in the mold, and molding.
  • the resin constituting the conductive resin 5 either a thermosetting resin or a thermoplastic resin can be used, and a phenol resin is a typical example.
  • the molding can be performed by arranging the conductive plate material 6 in a mold, filling the mold with the conductive resin 5, and performing pressure molding.
  • FIG. 6 is a schematic sectional view showing another example of the fuel cell separator of the present invention.
  • This separator has the same structure as that of the conductive resin molding 5 except that the conductive insert bin 2 extends in the thickness direction on the other uneven surface in order to increase the conductivity in the thickness direction. It has the same structure as the separator shown in Figure 5.
  • the separator with such a structure has a conductive plate (aluminum plate, etc.) 6 temporarily fixed on the mold cavity side, and a plurality of conductive insert pins (aluminum insert pins) on the core side protrusion. Etc.) 2 can be obtained by inserting the conductive resin 5 into the mold and press-molding.
  • a high-performance separator can be produced by molding without going through a carbonizing or graphitizing step and a cutting step. Therefore, a grooved separator can be obtained with high precision by using a mold having a convex portion (protrusion) or a groove formed on at least one of the cavity side and the core side (particularly, the core side). be able to.
  • the separator of the present invention is excellent in various properties such as gas impermeability, electric conductivity, heat conductivity, mechanical strength, and acid resistance without undergoing a carbonization step or a cutting step, and is excellent in a fuel cell, particularly a solid state. It is useful as a separator for polymer electrolyte fuel cells using a polymer membrane as the electrolyte membrane. In particular, when a phenolic resin is used, it is excellent in heat resistance, acid resistance, strength, hot water resistance, and cost. According to the method of the present invention, a groove (gas flow path) having high dimensional accuracy can be formed by molding without going through the carbonizing step and the cutting step, in addition to the properties such as high conductivity and thermal conductivity. Therefore, the present invention can be effectively applied to a fuel cell separator (particularly, a polymer electrolyte fuel cell separator using a solid polymer membrane as an electrolyte membrane).
  • Example 1 Example 1
  • Phenol resin manufactured by Kanebo Co., Ltd .: Bellpearl S890
  • graphitized MCMB manufactured by Osaka Gas Co., Ltd., average particle size: 10 jm and 25 ⁇ m
  • artificial graphite powder Choetsu Graphite Co., Ltd.
  • RA 15 aspect ratio 1.3 average particle size 5 m
  • Table 1 33. 3: 6.6.7 or 25.0: 75.0
  • This powder mixture was charged into a mold and molded under the conditions of a molding pressure of 5 O kg / cm 2 and 160 ⁇ 20 minutes.
  • 2 parts by weight of carbon fiber was used per 100 parts by weight. The results are shown in Table 1.
  • Polyphenylene ether resin manufactured by Mitsubishi Engineering-Plastics Co., Ltd .: Upies NX-700N
  • graphitized MCM B Osaka Gas Co., Ltd., average particle size 1 0 m and 25 m
  • artificial graphite powder manufactured by Chuetsu Graphite Co., Ltd., RA 15, aspect ratio 1.3, average particle size 5 / zm
  • Table 2 25 parts by weight ratio
  • the powder mixture was supplied to an extruder to prepare a pellet.
  • Flat plates were formed by injection molding using the prepared pellets. The results are shown in Table 2.
  • An aluminum foil (thickness: 30 m) or a platinum foil (thickness: 30 m) is set on the cavity side or both sides of the flat mold with a small amount of adhesive, and on the core side to impart conductivity in the thickness direction.
  • a plurality of aluminum insert bins (2 ⁇ ⁇ 1.5 mm x 4) in the thickness direction the phenolic resin used in Examples 1-4 (manufactured by Kanebo Co., Ltd.) was inserted into the mold. : Only Bellpearl S890) was added and molded under the same molding conditions as in Examples 1 to 5. The results are shown in Table 3.
  • Conductive paint (Fujikura Kasei Co., Ltd., Doyu It) is brush-coated on the core side.
  • an aluminum insert plate (thickness: 1.0 mm) having a plurality of protrusions (pins) is inserted on the cavity side, fixed, and then inserted into the mold.
  • Only the phenolic resin (manufactured by Kanebo Co., Ltd .: Bellpearl S890) used in Examples 1 to 4 was put into the mold, and molded under the same molding conditions as in Examples 1 to 5. The results are shown in Table 3.
  • Phenolic resin manufactured by Kanebo Co., Ltd .: Bell Pearl S890
  • graphitized MCMB manufactured by Osaka Gas Co., Ltd., average particle size: 10 m
  • artificial A molded product was obtained in the same manner as in Example 1 except that graphite powder (manufactured by Chuetsu Graphite Co., Ltd., RA 15, aspect ratio 1.3, average particle diameter 5 ⁇ ) 16.7 parts by weight was used. .
  • This compact has a thickness of 1.20 mm, a bulk density of 1.82 g / cm 3 , a volume resistivity in the thickness direction of 0.07 ⁇ cm, a bending strength of 9.2 kg / mm 2 , and an apparent
  • the thermal conductivity in the thickness direction was 6.0 W / mk, and the surface condition was good.
  • the thickness of this molded body is 1.22 mm, the bulk density is 1.85 gcm 3 , the volume resistivity in the thickness direction is 0.04 Qcm, and the bending strength is 8.6 kg / mm
  • the apparent thermal conductivity in the thickness direction was 7.0 W Zmk, and the surface condition was good.

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  • Fuel Cell (AREA)

Abstract

L'invention concerne un séparateur contenant une résine non carbonée et présentant une résistance transversale dans le sens de l'épaisseur de 0,15 Φcm ou moins, une résistance à la flexion de 3 à 20 kgf/mm2 et une conductivité thermique dans le sens de l'épaisseur de 2 à 60 W/mK. Ledit séparateur peut être produit par un procédé (a) dans lequel un mélange d'une résine et d'un agent électroconducteur consistant en de la poudre de graphite à grains sphériques ou en une poudre de graphite ayant un rapport de forme de 2,0 ou moins, est moulé par injection ou moulé par compression ; ou par un procédé (b) dans lequel une pièce moulée en résine synthétique et un élément électroconducteur sont moulés d'une pièce. Ainsi, sans passer par une étape de carbonisation et de coupe, on produit par moulage un séparateur possédant d'excellentes propriétés de conductivité électrique, de conductivité thermique, de résistance mécanique et ainsi qu'une rainure de dimensions précises.
PCT/JP1999/001349 1998-03-20 1999-03-18 Separateur pour element a combustible et son procede de production WO1999049530A1 (fr)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
JP7164398 1998-03-20
JP10/71643 1998-03-20
JP10/194691 1998-07-09
JP19469198 1998-07-09

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WO1999049530A1 true WO1999049530A1 (fr) 1999-09-30

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Cited By (18)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2001325967A (ja) * 2000-05-15 2001-11-22 Nisshinbo Ind Inc 燃料電池セパレータの製造方法、燃料電池セパレータ及び固体高分子型燃料電池
JP2001351645A (ja) * 2000-06-09 2001-12-21 Kawasaki Steel Corp 燃料電池用セパレータおよび燃料電池
JP2001351644A (ja) * 2000-06-07 2001-12-21 Kawasaki Steel Corp 燃料電池用セパレータおよび燃料電池
WO2002001660A1 (fr) * 2000-06-29 2002-01-03 Osaka Gas Company Limited Composition conductrice pour separateur de pile a combustible de type a polymere solide, separateur de pile a combustible de type a polymere solide, pile a combustible de type a polymere solide et systeme de pile a combustible de type a polymere solide utilisant ce separateur
JP2002063913A (ja) * 2000-08-22 2002-02-28 Tokai Carbon 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
JP2002134135A (ja) * 2000-10-20 2002-05-10 Sony Corp 燃料電池用セパレータ
JP2002141084A (ja) * 2000-05-08 2002-05-17 Honda Motor Co Ltd 燃料電池
JP2003068316A (ja) * 2001-03-06 2003-03-07 Toray Ind Inc 燃料電池用セパレーターおよびその製造方法
WO2005038969A1 (fr) * 2003-10-21 2005-04-28 Compotec S.P.A. Materiau de fabrication de plaques bipolaires pour piles a combustible, plaque bipolaire a base de ce materiau et pile a combustible comportant cette plaque
JP2005521194A (ja) * 2001-11-02 2005-07-14 フラウンホッファー−ゲゼルシャフト・ツァー・フォデラング・デル・アンゲワンテン・フォーシュング・エー．ファウ． マイクロ燃料電池システム
JP2006092773A (ja) * 2004-09-21 2006-04-06 Honda Motor Co Ltd 燃料電池用セパレータの製造方法
JP2007324146A (ja) * 2007-09-07 2007-12-13 Mitsubishi Plastics Ind Ltd 燃料電池用セパレータ
DE10216306B4 (de) * 2002-04-14 2008-06-12 Sgl Carbon Ag Verfahren zur Herstellung einer Kontaktplatte für eine elektrochemische Zelle sowie deren Verwendungen
JP2008243513A (ja) * 2007-03-27 2008-10-09 Equos Research Co Ltd 集電体、その製造方法及び燃料電池
FR2944915A1 (fr) * 2009-04-27 2010-10-29 Air Liquide Plaque de pile a combustible, son procede de fabrication et pile a combustible correspondante.
EP1521320A3 (fr) * 2003-09-30 2011-03-16 Nichias Corporation Séparateur pour pile à combustible
JP2013093099A (ja) * 2011-10-24 2013-05-16 Panasonic Corp 燃料電池セパレータ成形材料、燃料電池セパレータ、及び燃料電池
WO2024121240A1 (fr) * 2022-12-08 2024-06-13 Leonhardt e. K. Procédé pour produire des composants de pile à combustible sous la forme de plaques, en particulier des plaques bipolaires, et composant de pile à combustible produit selon ce procédé

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JPS5048435A (fr) * 1973-07-02 1975-04-30
JPS6230211B2 (fr) * 1981-12-25 1987-07-01 Kanebo Ltd
JPS59213610A (ja) * 1983-05-18 1984-12-03 Showa Denko Kk 炭素成形体及びその製造法
JPS60246568A (ja) * 1984-05-22 1985-12-06 Fuji Electric Corp Res & Dev Ltd 燃料電池用リブ付セパレ−タの製造方法
JPS62260709A (ja) * 1986-05-07 1987-11-13 Kawasaki Steel Corp 炭素成形体及びその製造方法
JPH1012246A (ja) * 1996-06-25 1998-01-16 Du Pont Kk 固体高分子電解質型燃料電池
JPH1079260A (ja) * 1996-09-03 1998-03-24 Sanyo Electric Co Ltd 燃料電池

Cited By (19)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2002141084A (ja) * 2000-05-08 2002-05-17 Honda Motor Co Ltd 燃料電池
JP2001325967A (ja) * 2000-05-15 2001-11-22 Nisshinbo Ind Inc 燃料電池セパレータの製造方法、燃料電池セパレータ及び固体高分子型燃料電池
JP2001351644A (ja) * 2000-06-07 2001-12-21 Kawasaki Steel Corp 燃料電池用セパレータおよび燃料電池
JP2001351645A (ja) * 2000-06-09 2001-12-21 Kawasaki Steel Corp 燃料電池用セパレータおよび燃料電池
WO2002001660A1 (fr) * 2000-06-29 2002-01-03 Osaka Gas Company Limited Composition conductrice pour separateur de pile a combustible de type a polymere solide, separateur de pile a combustible de type a polymere solide, pile a combustible de type a polymere solide et systeme de pile a combustible de type a polymere solide utilisant ce separateur
US7049021B2 (en) 2000-06-29 2006-05-23 Osaka Gas Company Limited Conductive composition for solid polymer type fuel cell separator, solid polymer type fuel cell separator, solid polymer type fuel cell and solid polymer type fuel cell system using the separator
JP2002063913A (ja) * 2000-08-22 2002-02-28 Tokai Carbon 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
JP2002134135A (ja) * 2000-10-20 2002-05-10 Sony Corp 燃料電池用セパレータ
JP2003068316A (ja) * 2001-03-06 2003-03-07 Toray Ind Inc 燃料電池用セパレーターおよびその製造方法
JP2005521194A (ja) * 2001-11-02 2005-07-14 フラウンホッファー−ゲゼルシャフト・ツァー・フォデラング・デル・アンゲワンテン・フォーシュング・エー．ファウ． マイクロ燃料電池システム
DE10216306B4 (de) * 2002-04-14 2008-06-12 Sgl Carbon Ag Verfahren zur Herstellung einer Kontaktplatte für eine elektrochemische Zelle sowie deren Verwendungen
EP1521320A3 (fr) * 2003-09-30 2011-03-16 Nichias Corporation Séparateur pour pile à combustible
WO2005038969A1 (fr) * 2003-10-21 2005-04-28 Compotec S.P.A. Materiau de fabrication de plaques bipolaires pour piles a combustible, plaque bipolaire a base de ce materiau et pile a combustible comportant cette plaque
JP2006092773A (ja) * 2004-09-21 2006-04-06 Honda Motor Co Ltd 燃料電池用セパレータの製造方法
JP2008243513A (ja) * 2007-03-27 2008-10-09 Equos Research Co Ltd 集電体、その製造方法及び燃料電池
JP2007324146A (ja) * 2007-09-07 2007-12-13 Mitsubishi Plastics Ind Ltd 燃料電池用セパレータ
FR2944915A1 (fr) * 2009-04-27 2010-10-29 Air Liquide Plaque de pile a combustible, son procede de fabrication et pile a combustible correspondante.
JP2013093099A (ja) * 2011-10-24 2013-05-16 Panasonic Corp 燃料電池セパレータ成形材料、燃料電池セパレータ、及び燃料電池
WO2024121240A1 (fr) * 2022-12-08 2024-06-13 Leonhardt e. K. Procédé pour produire des composants de pile à combustible sous la forme de plaques, en particulier des plaques bipolaires, et composant de pile à combustible produit selon ce procédé

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