WO2017188059A1 - Composition de caoutchouc de silicone liquide, et constituant d'étanchéité pour séparateur de pile à combustible à polymère solide - Google Patents

Composition de caoutchouc de silicone liquide, et constituant d'étanchéité pour séparateur de pile à combustible à polymère solide Download PDF

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Publication number
WO2017188059A1
WO2017188059A1 PCT/JP2017/015577 JP2017015577W WO2017188059A1 WO 2017188059 A1 WO2017188059 A1 WO 2017188059A1 JP 2017015577 W JP2017015577 W JP 2017015577W WO 2017188059 A1 WO2017188059 A1 WO 2017188059A1
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WO
WIPO (PCT)
Prior art keywords
silicone rubber
liquid silicone
rubber composition
fuel cell
talc
Prior art date
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Ceased
Application number
PCT/JP2017/015577
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English (en)
Japanese (ja)
Inventor
昭寛 鈴木
秀人 小紫
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Nok Corp
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Nok Corp
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Priority to JP2018514512A priority Critical patent/JPWO2017188059A1/ja
Publication of WO2017188059A1 publication Critical patent/WO2017188059A1/fr
Anticipated expiration legal-status Critical
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Classifications

    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J3/00—Processes of treating or compounding macromolecular substances
    • C08J3/24—Crosslinking, e.g. vulcanising, of macromolecules
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/34—Silicon-containing compounds
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L83/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers
    • C08L83/04—Polysiloxanes
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K3/00—Materials not provided for elsewhere
    • C09K3/10—Materials in mouldable or extrudable form for sealing or packing joints or covers
    • 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
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • 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
    • 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 liquid silicone rubber composition and a sealing component for a polymer electrolyte fuel cell separator using the same.
  • polymer electrolyte fuel cells operate at lower temperatures than other types of fuel cells, so there is no risk of material corrosion of the components that make up the cells, and they are relatively large for low-temperature operation. It has the feature of being able to discharge current, and is attracting attention as an alternative power source for in-vehicle internal combustion engines as well as for home cogeneration.
  • the separator is generally formed by forming a plurality of parallel grooves on both sides or one side of a flat plate, and power is generated by a gas diffusion electrode in the fuel cell. In addition to transmitting the electrodes to the outside, it plays a role of draining the water generated in the groove during the power generation process and securing the groove as a flow path for the reaction gas flowing out to the fuel cell.
  • a battery separator further downsizing is required, and a separator sealing material that is excellent in durability and can be used for a long time is required because a large number of separators are used in an overlapping manner.
  • a liquid silicone rubber excellent in heat resistance, elasticity and high-speed moldability is suitably used (Patent Document 1).
  • the rubber composition using such a liquid silicone rubber may have poor acid resistance after crosslinking.
  • the present invention has been made in view of the above circumstances, and provides a liquid silicone rubber composition from which a sealing part for a polymer electrolyte fuel cell separator having sufficient heat resistance and excellent acid resistance can be obtained. Objective.
  • the present inventors have realized sufficient heat resistance after crosslinking and further improved acid resistance by combining liquid silicone rubber and a predetermined amount of talc. It has been found that a liquid silicone rubber composition can be obtained, and the present invention has been completed based on this finding.
  • the gist configuration of the present invention is as follows. [1] It contains liquid silicone rubber and talc, The content of the talc is 0.5 to 15 parts by weight with respect to 100 parts by weight of the liquid silicone rubber, A liquid silicone rubber composition used for producing a sealing part for a polymer electrolyte fuel cell separator. [2] The liquid silicone rubber composition according to the above [1], which is subjected to addition crosslinking. [3] A sealing component for a polymer electrolyte fuel cell separator, which is a product obtained by crosslinking and molding the liquid silicone rubber composition according to [1] or [2].
  • liquid silicone rubber composition used for producing the sealing part for a polymer electrolyte fuel cell separator of the present invention contains liquid silicone rubber [A] and talc [B] as essential components, but is necessary. Depending on the type, various additives [C] can be contained.
  • liquid silicone rubber is not particularly limited, and for example, a low-viscosity liquid silicone rubber having self-fluidity at room temperature (25 ° C.) can be used.
  • a low-viscosity liquid silicone rubber having self-fluidity at room temperature (25 ° C.) can be used.
  • commercially available products such as the KE-1950 series, which is a liquid silicone rubber manufactured by Shin-Etsu Chemical Co., Ltd., and the LR3004 series manufactured by WACKER can be used as they are.
  • liquid silicone rubber as the LIM molding material preferably has a viscosity at 25 ° C. of 1 to 1000 Pa ⁇ s.
  • the viscosity value can be measured with a rotational viscometer.
  • Talc Talc is used to suppress a decrease in compression set under acidic conditions, and can be used regardless of the presence or absence of firing. From the viewpoint of improving acid resistance, in particular, using fired talc. Is preferred.
  • the content of talc is 0.5 to 15 parts by weight, preferably 1 to 10 parts by weight, more preferably 2 to 5 parts by weight with respect to 100 parts by weight of the liquid silicone rubber [A]. By setting it as the said range, it has sufficient heat resistance and can improve especially acid resistance. On the other hand, when the content of talc is less than 0.5 parts by weight, the effect of improving acid resistance is not sufficiently exhibited. Further, if the content of talc exceeds 15 parts by weight, sufficient heat resistance cannot be obtained.
  • reinforcing agents such as carbon black and silica generally used as a rubber compounding agent, clay, graphite, calcium silicate Fillers such as zinc oxide and magnesium oxide, hydrosilylation reaction control agents, colorants, heat resistance improvers, flame retardant improvers, heat conduction improvers, internal mold release agents, adhesion imparting agents, A thixotropic agent or the like is appropriately added and used as necessary.
  • reinforcing agents such as carbon black and silica generally used as a rubber compounding agent, clay, graphite, calcium silicate Fillers such as zinc oxide and magnesium oxide, hydrosilylation reaction control agents, colorants, heat resistance improvers, flame retardant improvers, heat conduction improvers, internal mold release agents, adhesion imparting agents, A thixotropic agent or the like is appropriately added and used as necessary.
  • the liquid silicone rubber composition can be prepared by mixing the above-mentioned [A] and [B] components and, if necessary, the [C] component by a known mixing method. For example, it can be prepared by kneading the predetermined components using a kneader such as an intermix or a three roll.
  • a kneader such as an intermix or a three roll.
  • the liquid silicone rubber composition according to the present invention is a low viscosity silicone rubber composition having self-fluidity at room temperature (25 ° C.), and in particular, a polymer electrolyte fuel cell separator by rim molding (Liquid Injection Molding). It is suitably used when manufacturing a sealing part for a machine.
  • the method for producing a sealing part for a polymer electrolyte fuel cell separator according to the present invention selectively uses a specific liquid silicone rubber composition containing the above-described components [A] and [B]. Preferably, it is subjected to addition crosslinking to form an elastic seal layer made of a crosslinked silicone rubber at the peripheral portion of at least one surface of the polymer electrolyte fuel cell separator component.
  • the crosslinking of the liquid silicone rubber composition can be generally performed by pressure crosslinking at about 100 to 300 ° C. for about 10 seconds to 30 minutes using an injection molding machine or the like.
  • secondary crosslinking post-cure
  • Secondary crosslinking can be performed by oven heating generally at about 100-250 ° C. for about 1-10 hours.
  • the thickness of the elastic seal layer obtained by crosslinking and molding the liquid silicone rubber composition is usually 0.05 to 5 mm, particularly preferably about 0.1 to 2 mm.
  • Example 1 First, 100 parts by weight of liquid silicone rubber (KE-1950-50A / B, manufactured by Shin-Etsu Chemical Co., Ltd.) and 0.6 parts by weight of calcined talc (Enstack 24, manufactured by Asada Flour Milling Co., Ltd.), a volume of 2 liters Kneading with a planetary mixer (PLM-2 type, manufactured by Inoue Seisakusho Co., Ltd.), and this is further passed once through a 3-inch ⁇ 3-roll (3-roll mill, Kodaira Seisakusho Co., Ltd.) A silicone rubber composition was obtained.
  • liquid silicone rubber KE-1950-50A / B, manufactured by Shin-Etsu Chemical Co., Ltd.
  • calcined talc Engelhardenetack 24, manufactured by Asada Flour Milling Co., Ltd.
  • PLM-2 type manufactured by Inoue Seisakusho Co., Ltd.
  • Example 2 to 5 and Comparative Examples 1 to 3 liquid silicone rubber compositions were obtained in the same manner as in Example 1, except that the amount of calcined talc was changed as shown in Table 1.
  • Example 6 a liquid silicone rubber composition was obtained in the same manner as in Example 3 except that unsintered talc (Mistrone Vapor, Imeris Specialties Japan Co., Ltd.) was used instead of calcined talc. .
  • the compression set means that the smaller the value, the better the heat resistance (sealability) and the longer the seal life.
  • the compression set in hydrofluoric acid means that the smaller the value, the higher the acid resistance.
  • a product having a compression set of 25% or less in air, 34% or less in water, and 50% or less in hydrofluoric acid was determined as an acceptable level.
  • the talc content is particularly in the range of 0.5 to 15 parts by weight with respect to 100 parts by weight of the liquid silicone rubber. It was confirmed that a molded article having a sufficient heat resistance and an excellent acid resistance having a small compression set in air, water and hydrofluoric acid can be produced.
  • the liquid silicone compositions according to Comparative Examples 1 and 2 were manufactured using these because the talc content was less than 0.5 parts by weight with respect to 100 parts by weight of the liquid silicone rubber.
  • the molded articles have particularly large compression set in hydrofluoric acid, and sufficient acid resistance can be obtained. Not confirmed.
  • the content of talc in the liquid silicone composition according to Comparative Example 3 exceeds 15 parts by weight with respect to 100 parts by weight of the liquid silicone rubber, a molded product manufactured using the talc is obtained by the present invention. It was confirmed that the compression set in air and water was large and sufficient heat resistance could not be obtained as compared with molded articles produced using the liquid silicone compositions (Examples 1 to 6).
  • liquid silicone composition according to the present invention a rubber molded article excellent in heat resistance and acid resistance can be obtained, and therefore, it is suitable for producing a sealing part for a polymer electrolyte fuel cell separator. It was confirmed.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Polymers & Plastics (AREA)
  • Medicinal Chemistry (AREA)
  • Sustainable Energy (AREA)
  • General Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Fuel Cell (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Sealing Material Composition (AREA)

Abstract

Le but de la présente invention est de pourvoir à une composition de caoutchouc de silicone liquide à partir de laquelle un constituant d'étanchéité pour séparateurs de pile à combustible à polymère solide qui présente une stabilité thermique suffisante et une résistance aux acides supérieure peut être obtenu. La composition de caoutchouc de silicone liquide comprend du caoutchouc de silicone liquide et du talc, et la teneur en talc est de 0,5 à 15 parties en poids pour 100 parties en poids du caoutchouc de silicone liquide. La composition de caoutchouc de silicone liquide est utilisée pour fabriquer le constituant d'étanchéité pour séparateurs de pile à combustible à polymère solide.
PCT/JP2017/015577 2016-04-28 2017-04-18 Composition de caoutchouc de silicone liquide, et constituant d'étanchéité pour séparateur de pile à combustible à polymère solide Ceased WO2017188059A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP2018514512A JPWO2017188059A1 (ja) 2016-04-28 2017-04-18 液状シリコーンゴム組成物およびこれを用いた固体高分子型燃料電池セパレータ用シール部品

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JP2016089982 2016-04-28
JP2016-089982 2016-04-28

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPWO2021054113A1 (fr) * 2019-09-18 2021-03-25

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2001335654A (ja) * 2000-05-26 2001-12-04 Otsuka Chem Co Ltd シリコーン用発泡剤、発泡性シリコーン組成物及びシリコーン発泡体
JP2003257456A (ja) * 2002-02-28 2003-09-12 Shin Etsu Chem Co Ltd 固体高分子型燃料電池セパレータシール用ゴム組成物及びこれを用いたシール材並びに固体高分子型燃料電池セパレータ
WO2009122487A1 (fr) * 2008-03-31 2009-10-08 Nok株式会社 Composition de caoutchouc et son utilisation
JP2014209438A (ja) * 2013-03-29 2014-11-06 本田技研工業株式会社 燃料電池用セパレータ及びその製造方法
JP2015022800A (ja) * 2013-07-16 2015-02-02 信越化学工業株式会社 固体高分子型燃料電池セパレータ用シールの製造方法及び該方法に用いるシリコーンゴム組成物

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2001335654A (ja) * 2000-05-26 2001-12-04 Otsuka Chem Co Ltd シリコーン用発泡剤、発泡性シリコーン組成物及びシリコーン発泡体
JP2003257456A (ja) * 2002-02-28 2003-09-12 Shin Etsu Chem Co Ltd 固体高分子型燃料電池セパレータシール用ゴム組成物及びこれを用いたシール材並びに固体高分子型燃料電池セパレータ
WO2009122487A1 (fr) * 2008-03-31 2009-10-08 Nok株式会社 Composition de caoutchouc et son utilisation
JP2014209438A (ja) * 2013-03-29 2014-11-06 本田技研工業株式会社 燃料電池用セパレータ及びその製造方法
JP2015022800A (ja) * 2013-07-16 2015-02-02 信越化学工業株式会社 固体高分子型燃料電池セパレータ用シールの製造方法及び該方法に用いるシリコーンゴム組成物

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPWO2021054113A1 (fr) * 2019-09-18 2021-03-25
WO2021054113A1 (fr) * 2019-09-18 2021-03-25 Nok株式会社 Procédé de fabrication de joint d'étanchéité de séparateur d'élément de batterie à combustible
CN113767490A (zh) * 2019-09-18 2021-12-07 Nok株式会社 燃料电池单元用分隔件的垫片制造方法
JP7385668B2 (ja) 2019-09-18 2023-11-22 Nok株式会社 燃料電池用セパレータのガスケット製造方法
US11973246B2 (en) 2019-09-18 2024-04-30 Nok Corporation Method for manufacturing fuel battery cell separator gasket

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