WO2018116875A1 - Ｐｅｆｃ型燃料電池の電極形成方法及び燃料電池 - Google Patents

Ｐｅｆｃ型燃料電池の電極形成方法及び燃料電池 Download PDF

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Publication number
WO2018116875A1
WO2018116875A1 PCT/JP2017/044287 JP2017044287W WO2018116875A1 WO 2018116875 A1 WO2018116875 A1 WO 2018116875A1 JP 2017044287 W JP2017044287 W JP 2017044287W WO 2018116875 A1 WO2018116875 A1 WO 2018116875A1
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WIPO (PCT)
Prior art keywords
electrode
electrolyte membrane
membrane
roll
fuel cell
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Application number
PCT/JP2017/044287
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English (en)
French (fr)
Japanese (ja)
Inventor
松永　正文
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エムテックスマート株式会社
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Application filed by エムテックスマート株式会社 filed Critical エムテックスマート株式会社
Priority to CN201780078210.4A priority Critical patent/CN110100341B/zh
Publication of WO2018116875A1 publication Critical patent/WO2018116875A1/ja

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05D—PROCESSES FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05D7/00—Processes, other than flocking, specially adapted for applying liquids or other fluent materials to particular surfaces or for applying particular liquids or other fluent materials
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05D—PROCESSES FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05D7/00—Processes, other than flocking, specially adapted for applying liquids or other fluent materials to particular surfaces or for applying particular liquids or other fluent materials
    • B05D7/24—Processes, other than flocking, specially adapted for applying liquids or other fluent materials to particular surfaces or for applying particular liquids or other fluent materials for applying particular liquids or other fluent materials
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D11/00—Inks
    • C09D11/52—Electrically conductive inks
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • 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
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
    • 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

Definitions

  • the present invention relates to a method of forming an electrode for a PEFC (Polymer Electrolyte Membrane Fuel Cell) type fuel cell, and a fuel cell manufactured by the method. More specifically, the present invention relates to a CCM (Catalyst coated membrane) type electrolyte membrane / electrode forming method.
  • coating by this invention Atomization (including fiberization) application including roll coating, die coating, screen printing, curtain coating, dispensing, inkjet, and spraying, electrostatic atomization (including fiberization) application Including a method of applying particles and fibers such as the above to an object to be coated, and also includes a micro curtain application.
  • a micro curtain is a wide-angle pattern airless spray nozzle that can be used to traverse the coating object and spray nozzle using the liquid film before spraying when liquid is sprayed at a relatively low pressure of around 0.3 MPa.
  • overspray particles are not generated on the coated surface. It changes to a mist when the distance increases after passing through the object.
  • atomization fibrosis
  • atomization is applied by a method of producing particles and fibers by spinning liquids and melts with ultrasonic waves, electrospinning spins, centrifugal force with rotating bodies, melt-blown methods, etc. If necessary, it refers to a method of attaching or applying them to an object with the aid of compressed air.
  • an electrolyte solution which is a kind of ionomer, and a fine powder composed of carbon particles or platinum supported on carbon fibers are mixed in an electrolyte membrane, applied as an electrode catalyst ink to GDL (Gas diffusion layer), and then pressed onto the electrolyte membrane. Or applied to a release film such as PTFE and transferred to an electrolyte membrane.
  • GDL Gas diffusion layer
  • a release film such as PTFE
  • Patent Document 1 is a method invented by the present inventor, in which an electrode ink is sprayed in a state in which an electrolyte membrane for roll-to-roll is unwound and adsorbed on a heated adsorption drum or adsorption belt.
  • a method of laminating and drying by the above has been proposed. Since the electrolyte membrane is adsorbed and heated by heating the adsorption drum or the like, it is laminated as a thin film by spraying or the like, so that the solvent volatilizes instantly when the spray particles are applied to the electrolyte membrane and leveled.
  • the electrolyte is not damaged and adhesion is increased, so that the interface resistance between the electrode and the electrolyte membrane can be lowered to the limit, so that an ideal CCM can be formed.
  • the electrolyte membrane is sucked between the adsorbing drum and the electrolyte by interposing a breathable paper or film wider than the electrolyte membrane, the entire surface of the electrolyte membrane should be kept without leaving adsorption marks on the porous body such as the adsorbing drum.
  • uniform suction has also been a proposal for uniform suction.
  • Patent Document 2 is also a method invented by the present inventor, in which a film as an electrode-shaped mask is bonded to both surfaces of an electrolyte film for roll-to-roll (Roll to Roll) to form electrode-shaped concave portions
  • a method in which electrode ink is laminated and wound up while being unwound and adsorbed by a heated adsorption roll or adsorption belt.
  • a method for forming an electrode by filling a catalyst-shaped recess in an electrode-shaped recess formed between a mask and an electrolyte membrane.
  • the electrolyte membrane is sensitive to moisture and the like, and when the electrode catalyst ink is applied, it is deformed in an instant. Therefore, as described above, the electrolyte membrane is adsorbed to a heating adsorption belt or a heating adsorption roll. Attempts have been made to apply with a spray nozzle or slot nozzle while moving without deformation. However, even if the adsorption roll was polished with a polishing apparatus to a roundness of several microns or less at room temperature, the roll was greatly deformed when heated, and the roundness was extremely poor.
  • the coating amount after drying of the catalyst is a thin film such as 0.1 milligram per square centimeter at the anode and 0.3 milligram at the cathode, so even if the roundness of the roll is 3 microns, the electrolyte membrane and the nozzle tip It is necessary to make the wet film thick so as not to be affected by the distance. Therefore, it can be expected that the solid content of the electrolyte solution and the catalyst needs to be, for example, 15% or less.
  • the electrolyte membrane is usually manufactured by a casting method, there is a back sheet of a supporting substrate, so that the coating for forming one electrode can be applied by spraying or slot nozzle without deforming the electrolyte membrane.
  • the electrolyte membrane is as thin as 25 microns or less, or even 15 microns or less, and stretches when pulled, and as described above, it is extremely difficult to form electrodes on the opposite side because of the extremely delicate substrate that easily deforms with moisture in the air. It was extremely difficult to wind up the electrolyte membrane with electrodes formed on both sides of the membrane.
  • the present invention has been made to solve the above-described problems, and an object of the present invention is to provide a high-quality and durable PEFC fuel cell membrane electrode assembly (MEA) manufacturing method and MEA. . More specifically, an electrode ink is directly applied to a roll-to-roll electrolyte membrane to produce a high-performance membrane / electrode assembly, and thus a high-performance fuel cell.
  • MEA PEFC fuel cell membrane electrode assembly
  • the present invention is a method for forming an electrode on one side of an electrolyte membrane by continuously or intermittently moving a long electrolyte membrane supported by a backsheet to apply an electrode ink, on the opposite side of the backsheet surface
  • a first step of attaching a reinforcing tape to both sides of the electrolyte membrane surface a second step of applying a first electrode ink to the electrolyte membrane on the surface of the reinforcing tape, and a first electrode ink
  • a method for producing a membrane / electrode assembly for a fuel cell characterized in that an electrolyte membrane / electrode assembly is produced using a sheet.
  • the present invention is a method of continuously or intermittently moving a long electrolyte membrane supported by a backsheet to apply electrode ink to form an electrode on one side of the electrolyte, on the opposite side of the backsheet surface.
  • Applying the first electrode ink; drying the first electrode ink to form the first electrode; preparing a breathable substrate that supports the first electrode; and the electrolyte membrane A step of bonding the electrode non-application portion on both sides of the application surface of the first electrode ink and the breathable substrate with an adhesive or an adhesive interposed therebetween, and a longitudinal section from the central portion other than the both sides
  • a fuel cell membrane characterized by producing an electrolyte membrane / electrode assembly using the composite sheet comprising a step of forming a gas-permeable base material, an electrode ink, an electrolyte membrane, and a composite sheet in close contact as a backsheet layer Electrode assembly To provide a process for the preparation of chromatography.
  • the present invention includes a step of adsorbing the air permeable substrate side of the composite sheet to a heat adsorbing roll or a heat adsorbing belt, a step of peeling the back sheet, and heat sucking the electrolyte membrane through the air permeable substrate.
  • the second electrode ink is applied to the electrolyte membrane on the opposite surface of the first electrode, and the second electrode ink is dried to form the second electrode.
  • a release-treated substrate for supporting the second electrode is laminated on the second electrode, or the breathable substrate is previously released.
  • a method of manufacturing a membrane / electrode assembly for a fuel cell is provided.
  • the present invention includes a step of superposing a breathable base material on the surface on which the reinforcing tape is pasted and forming the first electrode and sucking with a suction roll or a suction belt, a step of peeling a back sheet from the electrolyte surface,
  • the method includes a step of applying a second electrode ink while heating and adsorbing an electrolyte membrane on the opposite surface of the first electrode, and a step of drying the second electrode ink to form a second electrode.
  • the present invention is a method for producing a membrane / electrode assembly, characterized in that the adhesive or pressure-sensitive adhesive interposed on both sides of the breathable substrate is applied in a porous manner to the breathable substrate.
  • the adhesive or pressure-sensitive adhesive includes a slight pressure-sensitive adhesive and has at least solvent resistance.
  • the present invention uses a membrane / electrode assembly in which an anode electrode is formed on one side of a fuel cell electrolyte membrane moved by a roll to roll and an electrode containing a cathode electrode catalyst is formed on the opposite side of the anode electrode.
  • a first step in which a reinforcing film is applied to both ends of an electrolyte membrane provided with a back sheet, and the reinforcing film is adsorbed by a heating adsorption roll or a heating adsorption belt.
  • a fuel cell using a membrane / electrode assembly characterized by finally winding up an electrolyte membrane on which electrodes of both electrodes are formed.
  • the present invention relates to a fuel cell using a membrane / electrode assembly in which an anode electrode is formed on one side of a fuel cell electrolyte membrane that is moved by a roll-to-roll and an electrode containing a cathode electrode catalyst is formed on one side.
  • a step of forming a second electrode by applying a catalyst to the opposite surface of the first electrode, a step of drying or pressure bonding the electrode, and an electrolyte membrane on which electrodes of both electrodes are formed Provided is a fuel cell using a membrane / electrode assembly characterized by winding.
  • the catalyst is platinum and the support is carbon having mesoporous.
  • an electrode ink can be directly applied to each surface of an electrolyte membrane, even if it is a delicate and extremely thin electrolyte membrane of, for example, 15 microns or less. Furthermore, since the electrode ink applied to the electrolyte membrane by heating and sucking to reduce the load on the electrolyte membrane wets the electrolyte membrane, 99% or more of the solvent amount can be volatilized within 3 seconds, for example. This is ideal because the adhesion between the film and the electrode can be increased and the interface resistance can be lowered to the maximum.
  • the impact pulse method which is a pulsed spray belonging to the spray method and adds speed to the spray particles and is a registered trademark of MTEC Smart Co., Ltd., is adopted, the adhesion of the catalyst to the electrolyte membrane is Further increase.
  • the amount of one layer of electrode per square centimeter can be adjusted to 0.001 to 0.3 milligram by the spray method, particularly the impact pulse method, so that, for example, 2 to 30 layers of electrode ink can be laminated.
  • the coating amount per layer can be reduced by a combination of the spray method using an impact pulse and a heating adsorption drum.
  • the solid content of the electrode ink made of alcohol can even be 10% or less, for example, 3% or less by weight.
  • the merit of making the solid content concentration as described above is that the thinner the film is laminated, the less the load on the electrolyte membrane and the more uniform the coating amount per unit area, leading to improved fuel cell performance.
  • the present invention is heated at, for example, 50 to 120 ° C. through a microporous air-permeable substrate, for example, dust-free paper, and can be sucked with, for example, a commercially available vacuum pump having a vacuum degree of 60 KPa or more, so that the electrolyte membrane is damaged Membrane / electrode assemblies that are not only defect-free can be manufactured.
  • the adhesive can be applied to both sides of the breathable base material by using a gravure roll or the like to interspers the adhesive to make it porous. A slight pressure-sensitive adhesive that can be easily removed in the process can be used.
  • the vacuum pump may be selected from Orion's KRF, KHA, KHH, etc., which have been adopted in commercially available CCM applications in the fuel cell industry since around 2002, for example.
  • the electrode ink is directly laminated on the electrolyte membrane which is easily deformed and difficult to handle with an extremely thin film which is not expected at the time of the patent application of the liquid coating and drying method disclosed in Japanese Patent Application Laid-Open No. 2004-351413. It is to produce a stable membrane / electrode assembly.
  • FIG. 1 is a schematic cross-sectional view of a membrane / electrode assembly according to an embodiment of the present invention. It is this schematic of unwinding, 1st electrode ink application
  • a reinforcing tape 3 is attached to the electrolyte membrane 1 provided with the back sheet 2.
  • the reinforcing tape can be made of any material as long as it can withstand heating and a solvent atmosphere and does not leave a residue when peeled off.
  • FIG. 2 shows a structure in which the first electrode 4 is formed by applying the first electrode ink to the electrolyte membrane at a location other than the reinforcing tape attached to the electrolyte membrane in the configuration of FIG.
  • first electrode 4 is formed by applying the first electrode ink to the electrolyte membrane at a location other than the reinforcing tape attached to the electrolyte membrane in the configuration of FIG.
  • FIG. 3 is a view in which FIG. 2 is reversed and the breathable base material 2 is laminated on the first electrode surface 4.
  • an adhesive such as a slight adhesive is applied to the surface of the reinforcing tape 3 in advance, the electrolyte membrane can be bonded.
  • FIG. 4 is a diagram in which the first electrode is formed on the electrolyte membrane 1 supported by the back sheet 2 without attaching the reinforcing tape.
  • FIG. 5 is a view in which the breathable substrate 6 to which the adhesive 7 has been applied in advance on both sides of the breathable substrate 6 is attached to a portion of the electrolyte membrane 1 where no electrode is formed.
  • a back sheet 2 is left on top of the electrolyte membrane 1. The back sheet 2 may be adsorbed when an air-permeable substrate is adsorbed on an adsorption roll described later.
  • FIG. 6 shows a state in which the back electrode of FIG. 5 is peeled off, and the second electrode is dried by applying the second electrode ink to the electrolyte membrane adsorbed through the air-permeable sheet 6 on the heating adsorption roll described later.
  • FIG. 7 is a diagram of a membrane / electrode assembly manufactured according to the present invention. It is obtained by peeling the breathable sheet 6 of FIG. 6 from the electrolyte membrane 1. A first electrode 4 and a second electrode are formed on the electrolyte membrane 1.
  • the electrolyte film supported by the back sheet is fed out from the unwinding roll stock 10 and sent to the suction heating roll 20 while being pressed by the guide roll 1 and sucked and heated, and then the electrode ink is spray coated from the coating head 21. After being sufficiently dried, it is detached from the adsorbing roll and the guide roll and wound up as a winding roll stock 11.
  • the application method is not limited to spraying. Further, when the drying process is in a subsequent process, the drying here may not be sufficient.
  • the adsorption heating roll may be an adsorption heating belt. Further, the adsorption heating may be performed by using only the adsorption drum or the adsorption belt, and the heating of the electrolyte membrane may be performed only by the steps after the application.
  • FIG. 9 is a system having multiple functions as shown in FIG. 8.
  • the air-permeable base 6 is fed together with the unwinding roll stock 10, and the back sheet 2 is peeled off while being pressed and adsorbed by the guide roll and the suction heating roll 20. Then, the electrolyte membrane moves while being adsorbed by heating, and after the second electrode ink is applied with a coating head and dried to form the second electrode, it is detached from the guide roll and wound up.
  • the breathable substrate 6 is peeled off and wound up separately. In that case, another electrode support base material 8 can be moved and wound up, laminating
  • a membrane / electrode assembly for a PEFC fuel cell can be manufactured with high quality by the CCM method.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Wood Science & Technology (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Fuel Cell (AREA)
  • Application Of Or Painting With Fluid Materials (AREA)
  • Inks, Pencil-Leads, Or Crayons (AREA)
  • Inert Electrodes (AREA)
PCT/JP2017/044287 2016-12-21 2017-12-11 Ｐｅｆｃ型燃料電池の電極形成方法及び燃料電池 WO2018116875A1 (ja)

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CN201780078210.4A CN110100341B (zh) 2016-12-21 2017-12-11 Pefc型燃料电池的电极形成方法和燃料电池

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JP2016-248157 2016-12-21
JP2016248157A JP6903910B2 (ja) 2016-12-21 2016-12-21 燃料電池の製造方法、膜・電極アッセンブリー、燃料電池

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112585798A (zh) * 2018-08-21 2021-03-30 玛太克司马特股份有限公司 全固体电池的制造方法
US20230246203A1 (en) * 2018-08-01 2023-08-03 Toray Industries, Inc. Method of manufacturing and device for manufacturing membrane-catalyst assembly

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP7395127B2 (ja) * 2019-08-23 2023-12-11 エムテックスマート株式会社 電池の製造方法及び電池
CN112803050A (zh) * 2021-01-29 2021-05-14 山东魔方新能源科技有限公司 一种膜电极制备装置及其制备方法
JP2022172677A (ja) * 2021-05-06 2022-11-17 エムテックスマート株式会社 膜電極アッセンブリーと通気性基材の積層体の製造方法、膜電極アッセンブリーと通気性基材の積層体、燃料電池の製造方法
JP2022178501A (ja) * 2021-05-20 2022-12-02 エムテックスマート株式会社 膜電極アッセンブリーの製造方法、膜電極アッセンブリーと通気性基材の積層体の製造方法、膜電極アッセンブリーと通気性基材の積層体、燃料電池の製造方法、燃料電池

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JP2010129247A (ja) * 2008-11-26 2010-06-10 Nissan Motor Co Ltd 燃料電池電極積層体の製造方法
JP2012074315A (ja) * 2010-09-29 2012-04-12 Toppan Printing Co Ltd 固体高分子形燃料電池の膜電極接合体およびその製造方法
JP2013084427A (ja) * 2011-10-07 2013-05-09 Panasonic Corp 膜−触媒層接合体の製造方法及び膜電極接合体の製造方法
JP2013161557A (ja) * 2012-02-02 2013-08-19 Panasonic Corp 膜−触媒層接合体の製造方法および膜−触媒層接合体の製造装置

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JP5928030B2 (ja) * 2012-03-15 2016-06-01 凸版印刷株式会社 固体高分子形燃料電池用膜電極接合体の製造装置
JP2014229370A (ja) * 2013-05-20 2014-12-08 大日本スクリーン製造株式会社 複合膜の製造装置および製造方法
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JP2010129247A (ja) * 2008-11-26 2010-06-10 Nissan Motor Co Ltd 燃料電池電極積層体の製造方法
JP2012074315A (ja) * 2010-09-29 2012-04-12 Toppan Printing Co Ltd 固体高分子形燃料電池の膜電極接合体およびその製造方法
JP2013084427A (ja) * 2011-10-07 2013-05-09 Panasonic Corp 膜−触媒層接合体の製造方法及び膜電極接合体の製造方法
JP2013161557A (ja) * 2012-02-02 2013-08-19 Panasonic Corp 膜−触媒層接合体の製造方法および膜−触媒層接合体の製造装置

Cited By (3)

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Publication number Priority date Publication date Assignee Title
US20230246203A1 (en) * 2018-08-01 2023-08-03 Toray Industries, Inc. Method of manufacturing and device for manufacturing membrane-catalyst assembly
US12040497B2 (en) * 2018-08-01 2024-07-16 Toray Industries, Inc. Method of manufacturing and device for manufacturing membrane-catalyst assembly
CN112585798A (zh) * 2018-08-21 2021-03-30 玛太克司马特股份有限公司 全固体电池的制造方法

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