JP2005071851A - Manufacturing method of gas diffusion electrode - Google Patents

Manufacturing method of gas diffusion electrode Download PDF

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JP2005071851A
JP2005071851A JP2003301333A JP2003301333A JP2005071851A JP 2005071851 A JP2005071851 A JP 2005071851A JP 2003301333 A JP2003301333 A JP 2003301333A JP 2003301333 A JP2003301333 A JP 2003301333A JP 2005071851 A JP2005071851 A JP 2005071851A
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Prior art keywords
catalyst
exchange resin
ion exchange
gas diffusion
particles
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Japanese (ja)
Inventor
Yoshihiro Hori
Hideo Kasahara
Shinya Kosako
Makoto Uchida
Eiichi Yasumoto
Takeshi Yonamine
毅 与那嶺
誠 内田
慎也 古佐小
堀  喜博
栄一 安本
英男 笠原
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Matsushita Electric Ind Co Ltd
松下電器産業株式会社
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Priority to JP2003301333A priority Critical patent/JP2005071851A/en
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    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50Manufacturing or production processes characterised by the final manufactured product
    • Y02P70/56Manufacturing of fuel cells

Abstract

<P>PROBLEM TO BE SOLVED: To provide a gas diffusion electrode which is of superior electronic conductivity, gas diffusion characteristics and ion conductivity. <P>SOLUTION: This is a manufacturing method of the gas diffusion electrode for a fuel cell of polyelectrolyte type comprising (a) a process of preparing a catalyst composition of the shape of a floc composed of catalyst particles and ion exchange resin 5 covering the surface of the catalyst particles by giving centrifugal force and shearing force simultaneously to a mixture of the catalyst particles composed of a noble metal catalyst 3 and carbon particles 4 carrying the noble metal catalyst 3, and the ion exchange resin 5, and (b) a process in which a catalyst layer 2 is formed from the catalyst composition. <P>COPYRIGHT: (C)2005,JPO&NCIPI

Description

  The present invention mainly relates to a method for producing a gas diffusion electrode for a polymer electrolyte fuel cell.

The polymer electrolyte fuel cell includes an ion exchange membrane such as a proton conductive polymer electrolyte membrane as an electrolyte, supplies hydrogen as a fuel to an anode, supplies oxygen as an oxidant to a cathode, and the catalyst layer of a gas diffusion electrode The device generates electric power by electrochemically reacting a fuel and an oxidant.
An example of the electrochemical reaction at each electrode is shown below.
Anode: H 2 → 2H + + 2e
Cathode: 1 / 2O 2 + 2H + + 2e → H 2 O
Total reaction: H 2 + 1 / 2O 2 → H 2 O

The reaction at the anode and cathode shown in the above formula requires the supply of fuel and oxidant and the exchange of protons (H + ) and electrons (e ). All reactions proceed at the three-phase interface in the catalyst layer that satisfies these conditions.
In the catalyst layer, there are innumerable proton conduction paths formed by ion exchange resins such as proton conductive polymer electrolytes, electron conduction paths formed by carbon particles, and gas diffusion paths formed by pores. The three-phase interface is formed.

  A gas diffusion electrode for a polymer electrolyte fuel cell includes the above-described catalyst layer and a gas diffusion layer serving as a current collector. A conductive porous substrate is used for the gas diffusion layer. A joined body in which a polymer electrolyte membrane is sandwiched between a pair of gas diffusion electrodes serving as an anode and a cathode is called a membrane-electrode assembly (MEA). In order to obtain a high output fuel cell, it is necessary that the catalyst layer has both high proton conductivity, electron conductivity and gas diffusibility. For this purpose, it is necessary to continuously form the above-mentioned three paths in the catalyst layer.

  As described above, in order to obtain a high-power fuel cell, it is necessary that the catalyst layer has both high proton conductivity, electron conductivity, and gas diffusibility, but a polymer generally used as a proton conductor. The electrolyte exhibits good proton conductivity only in a water-containing state. Therefore, the fuel gas and oxidant gas supplied to the anode and cathode are humidified to prevent the polymer electrolyte from drying.

  However, since the fuel gas and the oxidant gas are humidified, and water is generated by reaction at the cathode, if the operation of the polymer electrolyte fuel cell is continued at a high current density, the surface of the catalyst layer and the fine particles are reduced. Water stays in the pores, gas diffusibility is hindered, and output is significantly reduced. Therefore, in order to suppress water retention, polytetrafluoroethylene (PTFE) particles having water repellency are mixed into the catalyst particles constituting the catalyst layer, or PTFE is applied to the surface of the conductive porous substrate. Has been proposed (see, for example, Patent Document 1).

In addition, in order to impart proton conductivity to the entire catalyst layer, a catalyst layer is formed using a paste in which catalyst particles are mixed with a polymer electrolyte (see, for example, Patent Document 2), or a polymer electrolyte is formed on the catalyst layer. It has been proposed to impregnate solutions.
Further, in order to improve the utilization factor of the catalyst, it is proposed that after the polymer electrolyte is mixed with the catalyst support particles, a catalyst raw material compound is added to the mixture and the compound is reduced (for example, Patent Documents). 3).
JP 2001-319660 A JP 2000-208151 A JP 2000-12041 A

  In order to suppress the retention of water, in the proposal of mixing PTFE particles into the catalyst particles constituting the catalyst layer or adding PTFE to the surface of the conductive porous substrate, the inside of the electrode during high current density operation In order to prevent the water from staying there, it is necessary to use a considerable amount of PTFE. However, although PTFE has strong water repellency, it does not have electron conductivity, proton conductivity, and gas diffusibility. Therefore, the electron conduction path, the proton conduction path, and the gas diffusion path are blocked by PTFE, which causes a problem that the output of the fuel cell is lowered.

  In addition, in order to impart proton conductivity to the entire catalyst layer, a proposal that a catalyst particle is mixed with a polymer electrolyte or a catalyst layer is impregnated with a polymer electrolyte solution is a polymer having a certain viscosity. It is difficult to evenly distribute the electrolyte solution to the deep part of the electrode, and a sufficient three-phase interface is not formed in the deep part of the electrode, and the utilization factor of the catalyst is reduced.

  The present invention provides (a) a catalyst particle consisting of a noble metal catalyst and carbon particles carrying the noble metal catalyst, and a mixture of an ion exchange resin, and simultaneously applying a centrifugal force and a shearing force to the catalyst particle and its surface. A gas diffusion electrode for a polymer electrolyte fuel cell, comprising: a step of preparing an agglomerated particulate catalyst composition comprising the ion exchange resin covering the surface; and (b) a step of forming a catalyst layer from the catalyst composition. It relates to the manufacturing method.

In the step (a), the ion exchange resin is preferably softened by frictional heat. In the catalyst composition used in the step (b), it is preferable that 70% or more of the surface of the catalyst particles is covered with the ion exchange resin. The median diameter of the catalyst composition is preferably 1 to 30 μm.
The present invention also relates to a polymer electrolyte fuel cell comprising a gas diffusion electrode obtained by the above method.

  According to the present invention, the step of covering the surfaces of the catalyst particles with the ion exchange resin by simultaneously applying centrifugal force and shearing force to the mixture of the catalyst particles and the ion exchange resin is performed. A strong ion exchange resin coating can be formed on the catalyst particles. As a result, a catalyst layer having high gas diffusibility can be easily obtained, and water does not easily stay in the catalyst layer. Further, since the ion exchange resin coating is thin and strong, the electron conductivity between the catalyst particles can be maintained. Moreover, since the ion exchange resin can form a network ion channel in the catalyst layer, the ion conductivity of the catalyst layer can be increased. Therefore, a high output fuel cell can be provided. Particularly, since high gas diffusibility is ensured by preventing water from staying inside the catalyst layer, high performance can be obtained even in a fuel cell using air having a low oxygen partial pressure as an oxidant gas.

  In the present invention, first, an agglomerated particulate catalyst composition comprising catalyst particles and an ion exchange resin covering the surface of the catalyst particles is prepared. The catalyst composition is prepared by simultaneously applying centrifugal force and shear force to a mixture of catalyst particles and ion exchange resin. The median diameter of the catalyst composition is preferably 1 to 30 μm, more preferably 10 to 15 μm. The catalyst particles include a noble metal catalyst and carbon particles supporting the noble metal catalyst. The average particle size of the carbon particles is preferably 0.1 to 10 μm. As a method for supporting the noble metal catalyst on the carbon particles, a method similar to the conventional method can be employed. For the ion exchange resin, a proton conductive polymer electrolyte such as perfluorocarbon sulfonic acid is preferably used.

  FIG. 1 is a schematic view showing a cross section of a membrane-electrode assembly using a gas diffusion electrode produced by the production method of the present invention. The membrane-electrode assembly is composed of a polymer electrolyte membrane 11 sandwiched between an anode 9 and a cathode 10, and a current flows when the anode 9 and the cathode 10 are connected to a resistor 12. As schematically shown in FIG. 1, the gas diffusion electrode includes a gas diffusion layer 1 and a catalyst layer 2. The catalyst layer 2 includes a noble metal catalyst 3, catalyst particles composed of carbon particles 4 supporting the noble metal catalyst 3, and an ion exchange resin 5 that covers the surface of the catalyst particles. In the catalyst layer 2, the electron channel 6 formed by the carbon particles 4, the gas channel 7 formed by the gap between the catalyst particles, and the ion channel 8 formed by the ion exchange resin are sufficiently secured. Therefore, since it is excellent in electron conductivity, gas diffusibility, and ion conductivity, a high output fuel cell can be provided.

  By simultaneously applying centrifugal force and shearing force to the mixture of the catalyst particles and the ion exchange resin, the ion exchange resin is strongly pressed against the catalyst particles. As a result, the ratio of the catalyst particle surface coated with the ion exchange resin is increased to, for example, 70% or more. As a result, as shown in FIG. 2, the contact area between the noble metal catalyst 3 supported on the carbon particles 4 and the ion exchange resin 5 increases. In addition, when such particles are used, the ion exchange resin can form a network ion channel in the catalyst layer, so that the ion conductivity of the catalyst layer can be increased.

  When a centrifugal force and a shearing force are simultaneously applied to the mixture of the catalyst particles and the ion exchange resin, the ion exchange resin can be softened. By softening the ion exchange resin, a uniform, thin and firm coating can be formed on the catalyst particles. As a result, a catalyst layer having high gas diffusibility can be easily obtained, and water does not easily stay in the catalyst layer. Further, since the ion exchange resin coating is thin and strong, the electron conductivity between the catalyst particles can be maintained. The ion exchange resin not only provides uniform ion conductivity and high gas diffusibility to the details of the catalyst layer, but also plays a role in sufficiently binding the catalyst particles together. Since the catalyst particles are sufficiently bound together, the mechanical strength of the catalyst layer is increased.

  The ion exchange resin is preferably mixed in an amount of 50 to 80 parts by weight per 100 parts by weight of the catalyst particles. When there is too much quantity of ion exchange resin, there exists a tendency for the gas diffusibility of a catalyst layer to fall. On the other hand, if the amount of the ion exchange resin is too small, sufficient ion channels are not formed in the catalyst layer. Moreover, it is preferable that a catalyst particle consists of 100 weight part of carbon particles and 40-60 weight part of noble metal catalysts. The average particle diameter of the noble metal catalyst supported on the carbon particles is preferably 0.1 to 1 μm.

Next, an example of a method for simultaneously applying centrifugal force and shearing force to a mixture of catalyst particles and ion exchange resin will be described with reference to FIG.
First, the catalyst particles 33 and the ion exchange resin are sequentially put into the rotating container 31, and the rotating container 31 is rotated at high speed in the X direction. Due to the centrifugal force in the Y direction, the catalyst particles 33 and the ion exchange resin are pressed against and fixed to the inner wall surface of the rotating container 31 having a certain curvature. An inner piece 32 is installed near the inner wall surface of the rotating container 31. The curvature of the portion of the inner piece 32 that contacts the catalyst particles is larger than the inner wall surface of the rotating container 31. The catalyst particles 33 and the ion exchange resin receive a strong compression / shearing force between the inner wall surface of the rotating container 31 and the inner piece 32. By such a mechanism, the ion exchange resin is rubbed against the surface of the catalyst particles. The ion exchange resin forms a uniform, thin and strong film on the surface of the catalyst particles. The catalyst composition thus obtained forms agglomerated particles having a predetermined median diameter by the action of the ion exchange resin as a binder.

The curvature r of the inner wall surface of the rotating container 31 is preferably 0.005 to 1 mm −1 , and the curvature R of the portion of the inner piece 32 that is in contact with the catalyst particles is preferably 0.5 to 1 mm −1 . Further, the ratio r / R is preferably 1 to 200. The rotation speed of the rotating container 31 is preferably 30 to 180 rpm. The inner piece 32 is preferably rotated at 30 to 180 rpm in the opposite direction to the rotating container 1.
EXAMPLES Hereinafter, although this invention is demonstrated concretely based on an Example, this invention is not limited to these.

(I) Preparation of Aggregated Particle Catalyst Composition As catalyst particles, platinum is supported on 100 parts by weight of carbon particles carrying platinum (TEC-10V-30E: Valcan XC-72 (carbon particles) manufactured by Tanaka Kikinzoku Co., Ltd.). 30 parts by weight supported) was used. The average particle diameter of carbon particles (Valcan XC-72) is 0.3 μm, and the average particle diameter of platinum is 0.1 μm.

  100 parts by weight of catalyst particles were put into a rotating container having an inner wall surface with a curvature of 0.025 (curvature radius of 40 mm), and the rotating container was rotated at a rotation speed of 120 rpm to give centrifugal force to the catalyst particles. When 10 minutes passed in that state, 90 parts by weight of ion exchange resin (Nafion) powder (manufactured by Aldrich) was charged into the inside of the rotating container. And the inner piece which has a curvature 3 times the inner wall surface of a rotation container was rotated with the rotation speed of 30 rpm in the opposite direction to a rotation container, and the shear force was provided to the catalyst particle | grains and ion exchange resin. The gap between the tip of the inner piece and the inner wall surface of the rotating container was 0.1 mm.

  The temperature in the rotating container was kept at 120 ° C. When 8 minutes passed in that state, the catalyst composition composed of the catalyst particles and the ion exchange resin was taken out of the rotating container. The resulting catalyst composition A had a median diameter of 8 μm. Moreover, the ratio (coverage) of the area covered with the ion exchange resin in the surface area of the catalyst particles was 90%. The coverage was determined from the amount of change in surface area by measuring the surface area of the catalyst particles before coating with the ion exchange resin and the surface area of the catalyst particles after coating with the ion exchange resin with a mercury porosimeter.

  Further, except that the weight ratio of the catalyst particles to the ion exchange resin powder was 100: 80, a catalyst composition B having a median diameter of 7 μm and a coverage of 70% was obtained in the same manner as in the case of the catalyst composition A. Prepared.

  Further, the median is the same as in the case of the catalyst composition A except that the weight ratio of the catalyst particles to the ion exchange resin powder is 100: 70 and the rotation speed of the inner piece is changed in the range of 20 to 30 rpm. A catalyst composition C having a diameter of 9.5 μm and a coverage of 60% was prepared.

  Further, the median diameter was 12 μm and the coverage was 90 μm in the same manner as in the case of the catalyst composition A, except that the rotation speed of the rotating container was 100 rpm and the rotation speed of the inner piece was changed in the range of 20 to 30 rpm. % Catalyst composition A-1.

  Further, except that the weight ratio of the catalyst particles and the ion exchange resin powder was 100: 85, the rotation speed of the rotating container was 140 rpm, and the rotation speed of the inner piece was changed in the range of 20 to 30 rpm. A catalyst composition A-2 having a median diameter of 10 μm and a coverage of 90% was prepared in the same manner as described above.

  Further, the same method as in the case of the catalyst composition A, except that the weight ratio of the catalyst particles and the ion exchange resin powder is 100: 85, the rotation speed of the rotating container is 140 rpm, and the rotation speed of the inner piece is 40 rpm. Thus, a catalyst composition A-3 having a median diameter of 5 μm and a coverage of 90% was prepared.

(Ii) Production of membrane-electrode assembly Gas diffusion electrodes were produced using the obtained catalyst compositions A, B, C, A-1, A-2, and A-3. Specifically, each catalyst composition was applied to both surfaces of a proton conductive polymer electrolyte membrane (Nafion made by DuPont, film thickness 150 μm), and both were joined by hot pressing (95 ° C.). And the proton conductive polymer electrolyte membrane which has the catalyst layer which consists of a catalyst composition on both surfaces was pinched | interposed with the carbon paper (thickness 20 micrometers) used as a gas diffusion layer, and the membrane-electrode assembly was obtained. Gas diffusion electrodes produced using the catalyst compositions A, B, C, A-1, A-2 and A-3 were prepared as membrane-electrode assemblies A, B, C, A-1, A, respectively. -2 and A-3. Using the membrane-electrode assemblies A, B, C, A-1, A-2, and A-3, the single-cell fuel cells A, B, C, A-1, A-2, and A-3, respectively, Assembled.
The amount of the catalyst composition applied to the proton conductive polymer electrolyte membrane was adjusted so that the amount of platinum contained in the catalyst layer of each membrane-electrode assembly was about 1.0 mg / cm 2 .

Comparative Example 1

A catalyst composition D was obtained in the same manner as the catalyst composition A except that the catalyst particles and the ion exchange resin were simply mixed to coat the surface of the catalyst particles with the ion exchange resin. The catalyst particles and the ion exchange resin were the same as the catalyst composition A. Then, using the catalyst composition D, a membrane-electrode assembly D was produced in the same manner as in Example 1, and a single-cell fuel cell D was assembled.
Again, the amount of the catalyst composition D applied to the proton conductive polymer electrolyte membrane is adjusted so that the amount of platinum contained in the catalyst layer of the membrane-electrode assembly D is about 1.0 mg / cm 2. It was adjusted.

[Evaluation of fuel cell]
The current-voltage characteristics of single cell fuel cells A, B, C, D, A-1, A-2 and A-3 were examined. FIG. 4 shows current-voltage characteristics when hydrogen is supplied to the anode side and oxygen is supplied to the cathode side of each fuel cell. FIG. 5 shows current-voltage characteristics when hydrogen is supplied to the anode side and air is supplied to the cathode side of each fuel cell.
The supply gas pressure was 1 atm. Each was humidified by bubbling in a sealed water bath at 70 ° C. The operating temperature of the fuel cell was 60 ° C., and the holding time during voltage measurement at each current value was 2 minutes.

  As is apparent from FIGS. 4 and 5, the fuel cells A, B and C according to the manufacturing method of the present invention can obtain a higher output voltage at each current density than the fuel cell D according to the conventional manufacturing method. It was. In particular, as seen in FIG. 5, the difference was remarkable when air was supplied to the cathode side. Since the fuel cells A and B have a higher output voltage than the fuel cell C, it can be said that the coverage of the catalyst particles with the ion exchange resin is preferably 70% or more. Further, the fuel cell A-2 was further improved in output as compared with the fuel cells A and B.

  In the fuel cell D according to the conventional manufacturing method, although the catalyst layer contains an ion exchange resin, the ion conduction path, the electron conduction path, and the gas diffusion path are cut off, and the output is considered to be reduced. . Further, the fuel cells A and B according to the production method of the present invention maintain better gas diffusibility, electron conductivity and proton conductivity than the fuel cell C. In the fuel cells A and B, the gas diffusion It is considered that the retention of water in the electrode is best suppressed. Further, the improvement in gas diffusivity is considered to sufficiently supply oxygen even when air having a low oxygen partial pressure is used as an oxidant gas, thereby greatly improving the output.

  The catalyst composition A-2 not only has high gas diffusibility and proton conductivity, but also has a significantly increased utilization rate of platinum because the platinum particles are reliably supported on the three-phase interface of the electrode. Thus, a higher performance electrode than the conventional one was obtained. In the catalyst composition A-2, the platinum particles were surely supported on the three-phase interface of the electrode because the relationship between the average particle diameter and the median diameter of the carbon particles and the ratio of the ion exchange resin were appropriate. It is done.

  ADVANTAGE OF THE INVENTION According to this invention, the gas diffusion electrode excellent in electronic conductivity, gas diffusibility, and ion conductivity can be provided.

It is a schematic diagram which shows the cross section of the membrane-electrode assembly using the gas diffusion electrode produced with the manufacturing method of this invention. It is a schematic diagram which shows the catalyst particle | grains coat | covered with the ion exchange resin contained in the catalyst composition which concerns on the manufacturing method of this invention. It is a schematic diagram which shows an example of the apparatus which provides a centrifugal force and a shearing force simultaneously to the mixture of a catalyst particle and ion exchange resin. It is a current-voltage characteristic diagram of a fuel cell when hydrogen is supplied to the anode and oxygen is supplied to the cathode. It is a current-voltage characteristic view of a fuel cell when hydrogen is supplied to the anode and air is supplied to the cathode.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Gas diffusion layer 2 Catalyst layer 3 Noble metal catalyst 4 Carbon particle 5 Ion exchange resin 6 Electron channel 7 Gas channel 8 Ion channel 9 Anode 10 Cathode 11 Polymer electrolyte membrane 12 Resistance 31 Rotating vessel 32 Inner piece 33 Catalyst particle

Claims (5)

  1. (A) Applying centrifugal force and shearing force simultaneously to a mixture of a noble metal catalyst and catalyst particles composed of carbon particles supporting the noble metal catalyst and an ion exchange resin, thereby covering the catalyst particles and the ions thereof. A step of preparing an agglomerated particulate catalyst composition comprising an exchange resin, and
    (B) A method for producing a gas diffusion electrode for a polymer electrolyte fuel cell, comprising the step of forming a catalyst layer from the catalyst composition.
  2.   The method for producing a gas diffusion electrode for a polymer electrolyte fuel cell according to claim 1, wherein in the step (a), the ion exchange resin is softened by frictional heat.
  3.   The method for producing a gas diffusion electrode for a polymer electrolyte fuel cell according to claim 1 or 2, wherein 70% or more of the surface of the catalyst particle is coated with the ion exchange resin.
  4.   The method for producing a gas diffusion electrode for a polymer electrolyte fuel cell according to any one of claims 1 to 3, wherein the catalyst composition has a median diameter of 1 to 30 µm.
  5.   A polymer electrolyte fuel cell comprising a gas diffusion electrode obtained by the method according to claim 1.
JP2003301333A 2003-08-26 2003-08-26 Manufacturing method of gas diffusion electrode Pending JP2005071851A (en)

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR100684836B1 (en) 2005-03-28 2007-02-20 삼성에스디아이 주식회사 Catalyst complex for fuel cell, method for preparing the same, membrane-electrode assembly comporising the same, and fuel cell system comprising the same
WO2011036749A1 (en) * 2009-09-24 2011-03-31 株式会社 東芝 Collector member, power generation device, and method for producing collector member for power generation device
JP2013164896A (en) * 2012-01-13 2013-08-22 Aisin Chemical Co Ltd Paste composition for micro porous layer formation and manufacturing method thereof
JP2016146305A (en) * 2015-02-09 2016-08-12 株式会社キャタラー Electrode for fuel cell

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR100684836B1 (en) 2005-03-28 2007-02-20 삼성에스디아이 주식회사 Catalyst complex for fuel cell, method for preparing the same, membrane-electrode assembly comporising the same, and fuel cell system comprising the same
US8512915B2 (en) 2005-03-28 2013-08-20 Samsung Sdi Co., Ltd. Catalyst composite material fuel cell, method for preparing the same, membrane-electrode assembly comprising the same, and fuel cell system comprising the same
WO2011036749A1 (en) * 2009-09-24 2011-03-31 株式会社 東芝 Collector member, power generation device, and method for producing collector member for power generation device
JP5562968B2 (en) * 2009-09-24 2014-07-30 株式会社東芝 Current collecting member, power generation device, and method of manufacturing current collecting member for power generation device
US9972849B2 (en) 2009-09-24 2018-05-15 Kabushiki Kaisha Toshiba Collector member, power generator, and method of manufacturing collector member for power generator
JP2013164896A (en) * 2012-01-13 2013-08-22 Aisin Chemical Co Ltd Paste composition for micro porous layer formation and manufacturing method thereof
JP2016146305A (en) * 2015-02-09 2016-08-12 株式会社キャタラー Electrode for fuel cell

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