JP4506252B2 - Manufacturing method of fuel cell and electrode substrate - Google Patents
Manufacturing method of fuel cell and electrode substrate Download PDFInfo
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- JP4506252B2 JP4506252B2 JP2004117411A JP2004117411A JP4506252B2 JP 4506252 B2 JP4506252 B2 JP 4506252B2 JP 2004117411 A JP2004117411 A JP 2004117411A JP 2004117411 A JP2004117411 A JP 2004117411A JP 4506252 B2 JP4506252 B2 JP 4506252B2
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- 239000000446 fuel Substances 0.000 title claims description 43
- 239000000758 substrate Substances 0.000 title claims description 33
- 238000004519 manufacturing process Methods 0.000 title claims description 20
- 239000003054 catalyst Substances 0.000 claims description 74
- 238000000034 method Methods 0.000 claims description 13
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 12
- 238000009792 diffusion process Methods 0.000 claims description 8
- 239000003792 electrolyte Substances 0.000 claims description 8
- 238000002156 mixing Methods 0.000 claims description 6
- 229910052697 platinum Inorganic materials 0.000 claims description 6
- 238000005507 spraying Methods 0.000 claims description 5
- 239000011248 coating agent Substances 0.000 claims description 3
- 238000000576 coating method Methods 0.000 claims description 3
- 239000011347 resin Substances 0.000 claims description 3
- 229920005989 resin Polymers 0.000 claims description 3
- 238000003892 spreading Methods 0.000 claims description 2
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims 2
- 229910052731 fluorine Inorganic materials 0.000 claims 2
- 239000011737 fluorine Substances 0.000 claims 2
- 238000010410 dusting Methods 0.000 claims 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 23
- 229910052799 carbon Inorganic materials 0.000 description 23
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 13
- 238000001035 drying Methods 0.000 description 12
- 239000007789 gas Substances 0.000 description 11
- 238000000859 sublimation Methods 0.000 description 7
- 230000008022 sublimation Effects 0.000 description 7
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 6
- 239000000463 material Substances 0.000 description 6
- 239000002904 solvent Substances 0.000 description 5
- 238000001291 vacuum drying Methods 0.000 description 5
- 238000007710 freezing Methods 0.000 description 4
- 230000008014 freezing Effects 0.000 description 4
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 3
- 239000012528 membrane Substances 0.000 description 3
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 3
- 239000004810 polytetrafluoroethylene Substances 0.000 description 3
- 230000006837 decompression Effects 0.000 description 2
- -1 polytetrafluoroethylene Polymers 0.000 description 2
- 238000010248 power generation Methods 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000002826 coolant Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 238000005304 joining Methods 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229920006254 polymer film Polymers 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 238000003672 processing method Methods 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 238000009777 vacuum freeze-drying Methods 0.000 description 1
- 230000037303 wrinkles Effects 0.000 description 1
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- 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
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Description
本発明は、触媒層用ペーストをカーボンペーパー上に塗布したのち乾燥する方法によって電極触媒層が形成される燃料電池セルの製造方法に関する。 The present invention relates to a method for producing a fuel cell in which an electrode catalyst layer is formed by a method of applying a catalyst layer paste on carbon paper and then drying.
りん酸型燃料電池の単位セルは、電解質膜を燃料極と空気極で挟んで構成されており、各電極は電極触媒層、ガス拡散層、ガス流路付き基材よりなる。このうち、ガス拡散層とガス流路付き基材にはガス拡散性、電気伝導性、耐食性が要求され、通常、ガス拡散層にはカーボンペーパーが、またガス流路付き基材には多孔質カーボンが用いられている。このように構成された単位セルで得られる発電電圧は1Vに満たない低電圧であるため、所望の電圧に対応して必要となる複数の単位セルを積層し、電気的に直列に接続した電池スタックが使用される。このとき積層された単位セルの間には、反応ガスとして供給される水素と空気の混合を防止するためのカーボン製のセパレーターが配置される。また、単位セルを5〜8個積層するごとに、発電反応に伴う発熱を除去し、電池スタックを所定の温度に保持するための冷却板が挿入される。 A unit cell of a phosphoric acid fuel cell is configured by sandwiching an electrolyte membrane between a fuel electrode and an air electrode, and each electrode is composed of an electrode catalyst layer, a gas diffusion layer, and a substrate with a gas flow path. Of these, the gas diffusion layer and the base material with gas flow path are required to have gas diffusibility, electrical conductivity, and corrosion resistance. Usually, carbon paper is used for the gas diffusion layer and porous base material is used for the base material with the gas flow path. Carbon is used. Since the generated voltage obtained by the unit cell configured as described above is a low voltage of less than 1 V, a battery in which a plurality of unit cells necessary for a desired voltage are stacked and electrically connected in series A stack is used. At this time, a carbon separator for preventing mixing of hydrogen and air supplied as a reaction gas is disposed between the unit cells stacked. Further, every time 5 to 8 unit cells are stacked, a cooling plate is inserted to remove heat generated by the power generation reaction and maintain the battery stack at a predetermined temperature.
上記の単位セルにおいて、発電反応に重要な役割を果す電極触媒層は、白金触媒とフッ素樹脂を混合して調整した触媒層用ペーストを多孔質のカーボンペーパーよりなる電極基板上に塗布あるいは散布したのち、溶媒や水分を乾燥除去し、さらに、適度な撥水性とカーボンペーパーの結着性を高めるために、フッ素樹脂の溶融温度、例えばポリテトラフルオロエチレン(PTFE)の場合には約330℃で、プレス等によって熱圧着する方法によって形成されている。特許文献1に見られる真空乾燥装置は、この種の燃料電池の電極膜の製造に際し、電極基板上に塗布あるいは散布された触媒層用ペーストの溶媒や水分の乾燥除去に用いられる真空乾燥装置の一例である。この装置では、真空容器内部にヒーターや、冷却用媒体を通流させる配管、加熱用媒体を通流させる配管を備えることによって、電極膜の温度を均一に保持し、しわや亀裂を生じることなく乾燥処理ができるように構成されている。 In the above unit cell, the electrode catalyst layer that plays an important role in the power generation reaction was applied or dispersed on an electrode substrate made of porous carbon paper with a catalyst layer paste prepared by mixing a platinum catalyst and a fluororesin. After that, in order to dry and remove the solvent and moisture, and further increase the water repellency and carbon paper binding properties, the melting temperature of the fluororesin, for example, about 330 ° C. in the case of polytetrafluoroethylene (PTFE) It is formed by a method of thermocompression bonding using a press or the like. The vacuum drying apparatus found in Patent Document 1 is a vacuum drying apparatus used for drying and removing the solvent and moisture of the catalyst layer paste applied or dispersed on the electrode substrate in the production of this type of fuel cell electrode membrane. It is an example. In this equipment, the temperature of the electrode film is maintained uniformly without causing wrinkles or cracks by providing a heater, piping for passing a cooling medium, and piping for passing a heating medium inside the vacuum vessel. It is configured so that it can be dried.
なお、この種の燃料電池の電極膜は、上記のごとき製造方法のほかに、触媒ペーストをポリマーフィルム上に塗布したのち、電極基材を重ねて接合し、真空凍結乾燥、プレス加工を行って電極基材に触媒層を転写形成する方法(特許文献2参照)等の製造方法によっても製造されている。
上記のように、りん酸型燃料電池の単位セルの電極触媒層を形成する際には、触媒層用ペーストをカーボンペーパーよりなる電極基材上に塗布あるいは散布したのち、溶媒や水分を乾燥除去し、さらに、適度な撥水性を付与し、カーボンペーパーの結着性を高めるために熱圧着する方法が採られており、触媒層用ペーストを塗布あるいは散布して電極膜として成型した基材を複数個まとめて乾燥機中に投入して溶媒や水分を除去し、続いてプレス装置あるいは連続焼成炉により溶着させている。本製造方法では、層内に残存する水分に起因する電極触媒層のひび割れの発生を防止するために、通常、真空乾燥機が用いられており、水分は凍結され昇華により除去されている。
しかしながら、効率的に乾燥処理を行うために、真空乾燥機には触媒層用ペーストを塗布あるいは散布した電極基板が複数個まとめて投入されるので、各電極基板の塗布あるいは散布完了から乾燥処理開始までの放置時間が異なり、放置時の水分の蒸発量に差が生じる。したがって、真空乾燥機に投入される各電極基板の水分保持量には、乾燥処理開始時に既に差があるので、同一時間の真空乾燥処理では、水分の凍結、昇華量が不足して、形成した電極触媒層にひび割れが生じる電極基板の発生を回避できないという問題点があった。
As described above, when forming the electrode catalyst layer of the unit cell of a phosphoric acid fuel cell, the catalyst layer paste is applied or dispersed on the electrode substrate made of carbon paper, and then the solvent and moisture are removed by drying. In addition, a method of thermocompression bonding has been adopted in order to impart appropriate water repellency and enhance the binding properties of carbon paper, and a base material molded as an electrode film by applying or spraying a catalyst layer paste A plurality of them are put together in a dryer to remove the solvent and moisture, and subsequently welded by a press device or a continuous firing furnace. In this production method, a vacuum dryer is usually used to prevent the electrode catalyst layer from cracking due to moisture remaining in the layer, and the moisture is frozen and removed by sublimation.
However, in order to efficiently perform the drying process, a plurality of electrode substrates coated with or sprayed with catalyst layer paste are put together in the vacuum dryer, so the drying process starts after the application or spraying of each electrode substrate is completed. The leaving time until is different, and there is a difference in the amount of water evaporated when left. Therefore, since the moisture retention amount of each electrode substrate put into the vacuum dryer is already different at the start of the drying process, the moisture drying and sublimation amount were insufficient in the vacuum drying process for the same time. There has been a problem that it is impossible to avoid the generation of an electrode substrate in which the electrode catalyst layer cracks.
本発明は、このような従来技術の問題点を顧慮してなされたもので、本発明の目的は、触媒層用ペーストを電極基板上に塗布あるいは散布したのち、溶媒や水分を乾燥除去し、さらに、適度な撥水性を付与し、カーボンペーパーの結着性を高めるために熱圧着して電極触媒層を形成する燃料電池セルの製造方法において、塗布あるいは散布完了から乾燥処理開始までの放置時間が異なる複数の電極基板を乾燥処理する場合にも、各基材に形成された電極触媒層に残存水分に起因するひび割れを引起す恐れがなく、安定した特性で運転可能な燃料電池セルの製造方法を提供することにある。 The present invention has been made in view of such problems of the prior art, and the object of the present invention is to apply or spray the catalyst layer paste on the electrode substrate, and then remove the solvent and moisture by drying. Furthermore, in the method of manufacturing a fuel cell in which an electrode catalyst layer is formed by thermocompression bonding in order to provide appropriate water repellency and enhance the binding property of carbon paper, the standing time from the completion of coating or spraying to the start of drying treatment Manufacturing of fuel cells that can be operated with stable characteristics without causing cracks due to residual moisture in the electrode catalyst layer formed on each substrate even when drying multiple electrode substrates with different It is to provide a method.
上記の目的を達成するために、本発明においては、
電解質層と、この電解質層を挟持する燃料極触媒層および空気極触媒層と、これらの触媒層の外面に接して配されるガス拡散層と、これらのガス拡散層の外面に接して配されるガス流路付き基材とにより構成される燃料電池セルの製造方法であって、白金触媒とフッ素樹脂を混合して調整した触媒層用ペーストを電極基板に塗布または散布したのち、乾燥して水分を除去することによって前記の燃料極触媒層および空気極触媒層を形成するものにおいて、
(1)前記触媒層用ペーストの塗布または散布の完了からの経過時間の異なる複数の電極基板を収容した装置内の温度と湿度を一定に保持したのち、前記複数の電極基板を同時に同一時間、真空乾燥することとする。
(2)さらに、上記(1)において、前記複数の電極基板を収容した装置として、温度と湿度を一定に保持することが可能な真空乾燥機を用いることとする。
(3)さらに、上記(1)または(2)の前記複数の燃料電池セルは、同一の電池スタックを構成する際に用いられるものとする。
In order to achieve the above object, in the present invention,
An electrolyte layer, a fuel electrode catalyst layer and an air electrode catalyst layer sandwiching the electrolyte layer, a gas diffusion layer disposed in contact with the outer surfaces of these catalyst layers, and a contact with the outer surfaces of these gas diffusion layers. And a catalyst layer paste prepared by mixing a platinum catalyst and a fluororesin and applying or spraying on the electrode substrate and then drying. In forming the fuel electrode catalyst layer and the air electrode catalyst layer by removing moisture,
(1) After maintaining a constant temperature and humidity in an apparatus containing a plurality of electrode substrates having different elapsed times from the completion of application or spreading of the catalyst layer paste, the plurality of electrode substrates are simultaneously held for the same time, Let it be vacuum dried.
(2) Furthermore, in the above (1), a vacuum dryer capable of maintaining a constant temperature and humidity is used as the device containing the plurality of electrode substrates.
(3) Further, the plurality of fuel cells of (1) or (2) are used when configuring the same battery stack.
(3)さらに、上記(1)または(2)において、電極基板を同一の水分量に保持する処理を実施する複数の燃料電池セルを、同一の電池スタックを構成する燃料電池セルよりなるものとする。 (3) Further, in the above (1) or (2), the plurality of fuel cells that perform the process of holding the electrode substrate at the same water content are composed of the fuel cells constituting the same battery stack. To do.
燃料電池スタックを構成する複数の燃料電池セルの燃料極触媒層、空気極触媒層を上記の(1)のごとく形成して燃料電池セルを製造することとすれば、触媒層用ペーストを塗布した後の放置時間の長さ如何にかかわらず、真空乾燥処理に供されるすべての電極基板はほぼ同一の水分量に保持されるので、凍結、昇華を同一条件で実施でき、乾燥条件の不具合によるひび割れの発生を防止できる。特に上記の(2)のごとき方法を用いれば、同一装置内で、電極基板を同一の水分量に保持し、真空乾燥処理できるので、水分の凍結、昇華処理が効果的に制御され、効率的に行われることとなる。また、同一の電池スタックを構成する複数の燃料電池セルにおいては同一の燃料極触媒層、空気極触媒層が用いられるので、上記の(3)のごとくとすれば、特に効果的である。 If a fuel cell is manufactured by forming the fuel electrode catalyst layer and air electrode catalyst layer of a plurality of fuel cells constituting the fuel cell stack as described in (1) above, the catalyst layer paste is applied. Regardless of the length of the subsequent standing time, all the electrode substrates subjected to the vacuum drying process are kept at almost the same moisture content, so that freezing and sublimation can be performed under the same conditions, due to problems with the drying conditions. Cracks can be prevented from occurring. In particular, if the method (2) above is used, the electrode substrate can be kept at the same moisture content and vacuum dried in the same apparatus, so that moisture freezing and sublimation can be effectively controlled and efficient. Will be done. Further, since the same fuel electrode catalyst layer and air electrode catalyst layer are used in a plurality of fuel cells constituting the same battery stack, the above (3) is particularly effective.
本発明の燃料電池セルの製造方法の最良の実施形態は、
電解質層と、これを挟持する燃料極触媒層および空気極触媒層と、これらの触媒層の外面に順次配されるガス拡散層とガス流路付き基材とにより構成される燃料電池セルで、上記の各触媒層が、白金触媒とフッ素樹脂を混合して調整した触媒層用ペーストを電極基板に塗布し、水分を除去することによって形成されるものにおいて、触媒層用ペーストを塗布した、複数の燃料電池セルの電極基板を、温度と湿度を一定に保持することが可能な真空乾燥機内に収納し、同一の水分量に保持したのち、真空乾燥して水分を除去し、各触媒層を形成する燃料電池セルの製造方法にある。
The best embodiment of the method for producing a fuel cell of the present invention is:
A fuel cell comprising an electrolyte layer, a fuel electrode catalyst layer and an air electrode catalyst layer sandwiching the electrolyte layer, a gas diffusion layer and a base material with a gas flow path sequentially arranged on the outer surface of these catalyst layers, Each of the above catalyst layers is formed by applying a catalyst layer paste prepared by mixing a platinum catalyst and a fluororesin to an electrode substrate and removing moisture. The electrode substrate of the fuel cell is housed in a vacuum dryer capable of maintaining a constant temperature and humidity, and after maintaining the same moisture content, the moisture is removed by vacuum drying, and each catalyst layer is removed. It exists in the manufacturing method of the fuel cell formed.
以下、本発明の燃料電池セルの製造方法による触媒層の形成処理の一実施例を示す。
まず、白金触媒とポリテトラフルオロエチレン樹脂を混合、調整して触媒層用ペーストを作製する。次いで、この触媒層用ペーストを電極基板となるカーボンペーパーの一方の面の上に塗布し、反対面側から吸引することによって、カーボンペーパーの一方の面に触媒層を形成する。燃料電池スタックに組込まれる燃料電池セルの個数を加味して、このカーボンペーパーへの触媒層の形成作業を、数十枚のカーボンペーパーに対して実施する。触媒層が形成されたカーボンペーパーは真空乾燥機内に設置された棚へと収納される。
図1は、この真空乾燥機の基本構成を示す縦断面図である。図において、1は真空乾燥機、2は触媒層が形成されたカーボンペーパーが収納される棚、3はヒーター、4は温度センサー、5は湿度センサーである。また、6は、真空乾燥機1の内部の湿度、温度を調整する加湿・温度制御装置、7は開閉バルブであり、8は真空排気装置、9は開閉バルブである。触媒層が形成されたカーボンペーパーを真空乾燥機1に収納する際には、真空乾燥機1の内部はヒーター3で加熱され、加湿・温度制御装置6より送られる水蒸気により加湿されて、温度が約25℃、湿度が70〜90%に設定されている。したがって、棚2に収納された触媒層付きカーボンペーパー10は、高温多湿条件下に置かれることによって含有水分量が増大する。このため、触媒層付きカーボンペーパー10をすべて棚2に収納したのち、30分から1時間にわたってこの高温多湿条件下におくことにより、全ての触媒層付きカーボンペーパー10はほぼ同一の水分量に、望ましくは同一の水分量に保持されることとなる。
Hereinafter, an example of the formation process of the catalyst layer by the manufacturing method of the fuel cell of the present invention will be shown.
First, a catalyst layer paste is prepared by mixing and adjusting a platinum catalyst and a polytetrafluoroethylene resin. Next, this catalyst layer paste is applied onto one surface of carbon paper to be an electrode substrate, and sucked from the opposite surface side, thereby forming a catalyst layer on one surface of the carbon paper. In consideration of the number of fuel cells to be incorporated into the fuel cell stack, the catalyst layer forming operation on the carbon paper is performed on several tens of carbon papers. The carbon paper on which the catalyst layer is formed is stored in a shelf installed in the vacuum dryer.
FIG. 1 is a longitudinal sectional view showing the basic configuration of this vacuum dryer. In the figure, 1 is a vacuum dryer, 2 is a shelf for storing carbon paper on which a catalyst layer is formed, 3 is a heater, 4 is a temperature sensor, and 5 is a humidity sensor. Further, 6 is a humidification / temperature control device for adjusting the humidity and temperature inside the
このように棚2に収納した触媒層付きカーボンペーパー10をすべて同一の水分量に保持したのち、開閉バルブ7を閉じて加湿・温度制御装置6からの水蒸気の供給を停止するとともに、真空排気装置8を作動させ、開閉バルブ9を開けて真空乾燥機1の内部を排気し、0.1 〜 0.5 kPa程度の真空度まで急激に減圧する。この減圧処理によって触媒層内の水分は均一に凍結し、昇華現象によって外部へと放出され、触媒層内の水分が除去される。この処理方法においては、触媒層付きカーボンペーパー10をすべて同一の水分量に保持して処理されるので、減圧処理による水分の凍結、昇華条件がすべての触媒層付きカーボンペーパー10について同一となる。したがって、触媒層にひび割れをもたらす条件を回避して水分の凍結、昇華処理を行うことが容易となり、優れた特性の燃料極触媒層および空気極触媒層が得られる。
After all the carbon paper with
以上述べたように、本発明の請求項1、さらには請求項2のごとき製造方法を用いて燃料電池セルを製造することとすれば、多数の燃料電池セルの電極触媒層をひび割れを生じることなく形成できるので、この種のりん酸型燃料電池を構成する燃料電池セルの製造方法として有効である。また、請求項3のごとく製造することとすれば、燃料電池スタックを構成する全ての燃料電池セルの電極触媒層が均質に製造でき、ひび割れが回避されるので、燃料電池セルの製造方法として極めて有効である。 As described above, if the fuel cell is manufactured by using the manufacturing method according to claim 1 or 2 of the present invention, the electrode catalyst layer of many fuel cells is cracked. Therefore, it is effective as a method of manufacturing a fuel cell constituting this type of phosphoric acid fuel cell. Further, if manufactured as in claim 3, the electrode catalyst layers of all the fuel cells constituting the fuel cell stack can be manufactured uniformly, and cracks are avoided. It is valid.
1 真空乾燥機
2 棚
3 ヒーター
6 加湿・温度制御装置
8 真空排気装置
10 触媒層付きカーボンペーパー
1 Vacuum dryer
2 shelves
3 Heater
6 Humidification / temperature control device
8
Claims (4)
前記触媒層用ペーストの塗布または散布の完了からの経過時間の異なる複数の電極基板を収容した装置内の温度と湿度を一定に保持したのち、前記複数の電極基板を同時に同一時間、真空乾燥することを特徴とする電極基板の製造方法。 An electrolyte layer to a method of manufacturing an electrode substrate for fuel electrode catalyst layer or cathode catalyst layer that Soo nip, coating or a platinum catalyst and a fluorine resin mixed to adjust catalyst layer paste before Symbol electrodes substrate After spraying, in what dried to remove moisture,
After maintaining a constant temperature and humidity in an apparatus containing a plurality of electrode substrates with different elapsed times from the completion of the application or spreading of the catalyst layer paste, the plurality of electrode substrates are simultaneously vacuum dried for the same time. An electrode substrate manufacturing method characterized by the above.
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