JP2007141704A - Separator for fuel cell, and its manufacturing method, as well as fuel cell using it - Google Patents
Separator for fuel cell, and its manufacturing method, as well as fuel cell using it Download PDFInfo
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- JP2007141704A JP2007141704A JP2005335426A JP2005335426A JP2007141704A JP 2007141704 A JP2007141704 A JP 2007141704A JP 2005335426 A JP2005335426 A JP 2005335426A JP 2005335426 A JP2005335426 A JP 2005335426A JP 2007141704 A JP2007141704 A JP 2007141704A
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- fuel cell
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- 239000000446 fuel Substances 0.000 title claims abstract description 78
- 238000004519 manufacturing process Methods 0.000 title abstract description 8
- 229920000139 polyethylene terephthalate Polymers 0.000 claims abstract description 52
- 239000005020 polyethylene terephthalate Substances 0.000 claims abstract description 52
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 37
- 239000000463 material Substances 0.000 claims abstract description 23
- 238000002156 mixing Methods 0.000 claims abstract description 6
- -1 polyethylene terephthalate Polymers 0.000 claims abstract description 6
- 239000003054 catalyst Substances 0.000 claims description 53
- 239000004020 conductor Substances 0.000 claims description 24
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 20
- 239000011347 resin Substances 0.000 claims description 20
- 229920005989 resin Polymers 0.000 claims description 20
- 229910052799 carbon Inorganic materials 0.000 claims description 19
- 239000012528 membrane Substances 0.000 claims description 16
- TXEYQDLBPFQVAA-UHFFFAOYSA-N tetrafluoromethane Chemical compound FC(F)(F)F TXEYQDLBPFQVAA-UHFFFAOYSA-N 0.000 claims description 16
- 239000005518 polymer electrolyte Substances 0.000 claims description 15
- 239000007787 solid Substances 0.000 claims description 15
- 239000002245 particle Substances 0.000 claims description 13
- 238000009792 diffusion process Methods 0.000 claims description 12
- 229910052697 platinum Inorganic materials 0.000 claims description 10
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 8
- 125000001174 sulfone group Chemical group 0.000 claims description 7
- LSNNMFCWUKXFEE-UHFFFAOYSA-M Bisulfite Chemical compound OS([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-M 0.000 claims description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 6
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims description 4
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 4
- 229910052737 gold Inorganic materials 0.000 claims description 4
- 239000010931 gold Substances 0.000 claims description 4
- 229910052741 iridium Inorganic materials 0.000 claims description 4
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 4
- 229910052763 palladium Inorganic materials 0.000 claims description 4
- 238000010298 pulverizing process Methods 0.000 claims description 4
- 229910052703 rhodium Inorganic materials 0.000 claims description 4
- 239000010948 rhodium Substances 0.000 claims description 4
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 4
- 229910052707 ruthenium Inorganic materials 0.000 claims description 4
- 239000000758 substrate Substances 0.000 claims description 4
- 239000004696 Poly ether ether ketone Substances 0.000 claims description 3
- 239000004695 Polyether sulfone Substances 0.000 claims description 3
- 239000004642 Polyimide Substances 0.000 claims description 3
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims description 3
- 239000004744 fabric Substances 0.000 claims description 3
- 229910052751 metal Inorganic materials 0.000 claims description 3
- 239000002184 metal Substances 0.000 claims description 3
- 229910052762 osmium Inorganic materials 0.000 claims description 3
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 claims description 3
- 229920006393 polyether sulfone Polymers 0.000 claims description 3
- 229920002530 polyetherether ketone Polymers 0.000 claims description 3
- 229920001721 polyimide Polymers 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- 235000012239 silicon dioxide Nutrition 0.000 claims description 3
- 150000002739 metals Chemical class 0.000 claims description 2
- 238000000034 method Methods 0.000 abstract description 9
- 238000010438 heat treatment Methods 0.000 abstract description 8
- 238000000465 moulding Methods 0.000 abstract description 7
- 238000004064 recycling Methods 0.000 abstract description 3
- 238000009825 accumulation Methods 0.000 abstract description 2
- 239000007789 gas Substances 0.000 description 13
- 239000002994 raw material Substances 0.000 description 8
- 239000000126 substance Substances 0.000 description 6
- 229910002804 graphite Inorganic materials 0.000 description 5
- 239000010439 graphite Substances 0.000 description 5
- 239000000203 mixture Substances 0.000 description 5
- 238000010248 power generation Methods 0.000 description 5
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 4
- 230000002378 acidificating effect Effects 0.000 description 4
- 238000005452 bending Methods 0.000 description 4
- 239000007800 oxidant agent Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 235000013361 beverage Nutrition 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 229910001882 dioxygen Inorganic materials 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 229910021382 natural graphite Inorganic materials 0.000 description 2
- 239000012299 nitrogen atmosphere Substances 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 239000008399 tap water Substances 0.000 description 2
- 235000020679 tap water Nutrition 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 150000001722 carbon compounds Chemical class 0.000 description 1
- 230000001413 cellular effect Effects 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 230000002354 daily effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 230000003203 everyday effect Effects 0.000 description 1
- 230000009477 glass transition Effects 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 235000011835 quiches Nutrition 0.000 description 1
- 238000007650 screen-printing Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 230000003068 static effect Effects 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 238000004659 sterilization and disinfection Methods 0.000 description 1
- 238000003911 water pollution Methods 0.000 description 1
Classifications
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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
-
- 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
Landscapes
- Fuel Cell (AREA)
- Separation Using Semi-Permeable Membranes (AREA)
- Casting Or Compression Moulding Of Plastics Or The Like (AREA)
- Catalysts (AREA)
- Inert Electrodes (AREA)
Abstract
Description
本発明は、使用済みＰＥＴボトルを原料とした燃料電池用セパレータおよびその製造方法、並びに、それを用いた燃料電池に関する。 The present invention relates to a fuel cell separator using a used PET bottle as a raw material, a method for producing the same, and a fuel cell using the same.
近年、河川の水質汚染が進むに連れ、水道水の殺菌用塩素の量が増え、水道水の安全性が危惧されている。
それに伴い、ＰＥＴ（ポリエチレンテレフタレート）ボトルに入った飲料の普及が著しい。
（特許文献１参照）
In recent years, the amount of chlorine for sterilization of tap water has increased as the water pollution of rivers has progressed, and the safety of tap water is feared.
Accordingly, the spread of beverages in PET (polyethylene terephthalate) bottles is remarkable.
(See Patent Document 1)
しかし、現行法では、上述のＰＥＴ（ポリエチレンテレフタレート）ボトルを、飲料用途に再使用することは許されていない。
従って、多量の使用済みＰＥＴボトルが日々蓄積されていることが問題となっている。
However, the current method does not allow the above-mentioned PET (polyethylene terephthalate) bottle to be reused in beverage applications.
Therefore, there is a problem that a large amount of used PET bottles are accumulated every day.
本発明の課題は、使用済みＰＥＴボトルを原料とした燃料電池用セパレータおよびその製造方法、並びに、それを用いた燃料電池を提供するものである。 The subject of this invention is providing the separator for fuel cells which used the used PET bottle as a raw material, its manufacturing method, and a fuel cell using the same.
請求項１に記載の発明は、ＰＥＴ（ポリエチレンテレフタレート）樹脂と黒鉛粉の配合量が、前記ＰＥＴ樹脂１００重量部に対して前記黒鉛粉３００〜８００重量部であることを特徴とする燃料電池用セパレータである。 The invention according to claim 1 is characterized in that the blending amount of the PET (polyethylene terephthalate) resin and the graphite powder is 300 to 800 parts by weight of the graphite powder with respect to 100 parts by weight of the PET resin. It is a separator.
ＰＥＴ樹脂１００重量部に黒鉛粉３００重量部未満であると、燃料電池用セパレータの導電率は０．２Ｓ／ｃｍを下回ってしまう。
導電率０．２Ｓ／ｃｍは、燃料電池用セパレータの導電率の許容下限値である。
If the amount of the PET resin is less than 300 parts by weight of the graphite resin, the electrical conductivity of the fuel cell separator is less than 0.2 S / cm.
The conductivity of 0.2 S / cm is an allowable lower limit value of the conductivity of the fuel cell separator.
また、ＰＥＴ樹脂１００重量部に黒鉛粉８００重量部以上であると、燃料電池用セパレータの曲げ強度は４ｋｇｆ／ｍｍ2を下回ってしまう。
曲げ強度４ｋｇｆ／ｍｍ2は、燃料電池用セパレータの強度の許容下限値である。
On the other hand, when the graphite resin is 800 parts by weight or more with respect to 100 parts by weight of the PET resin, the bending strength of the fuel cell separator is less than 4 kgf / mm 2 .
The bending strength of 4 kgf / mm 2 is an allowable lower limit value of the strength of the fuel cell separator.
請求項２に記載の発明は、前記ＰＥＴ樹脂が、使用済みＰＥＴボトルを粉末状に粉砕した材料からなることを特徴とする請求項１に記載の燃料電池用セパレータである。 The invention according to claim 2 is the fuel cell separator according to claim 1, wherein the PET resin is made of a material obtained by pulverizing a used PET bottle into a powder form.
請求項３に記載の発明は、固体高分子電解質膜の表裏面に触媒層が設けられ、該触媒層の前記固体高分子電解質膜と反対側の面にガス拡散材が設けられ、該ガス拡散材の前記触媒層と反対側の面に、請求項１または請求項２に記載の燃料電池用セパレータを設けたことを特徴とする燃料電池である。 According to a third aspect of the present invention, a catalyst layer is provided on the front and back surfaces of a solid polymer electrolyte membrane, and a gas diffusion material is provided on the surface of the catalyst layer opposite to the solid polymer electrolyte membrane, A fuel cell comprising the separator for a fuel cell according to claim 1 or 2 provided on a surface of the material opposite to the catalyst layer.
請求項４に記載の発明は、前記固体高分子電解質膜がスルホン基含有パーフルオロカーボン、または、カルボキシル基含有パーフルオロカーボンであることを特徴とする請求項３に記載の燃料電池である。 The invention according to claim 4 is the fuel cell according to claim 3, wherein the solid polymer electrolyte membrane is a sulfone group-containing perfluorocarbon or a carboxyl group-containing perfluorocarbon.
請求項５に記載の発明は、前記触媒層が、プロトン伝導性物質、電子伝導性物質、および、触媒からなることを特徴とする請求項３または請求項４に記載の燃料電池である。 The invention according to claim 5 is the fuel cell according to claim 3 or 4, wherein the catalyst layer is made of a proton conductive material, an electron conductive material, and a catalyst.
請求項６に記載の発明は、前記プロトン伝導性物質が、パーフルオロカーボンスルホン酸、ポリエーテルスルフォン、スルホン化ポリエーテルエーテルケトン、または、スルホン化ポリイミドであることを特徴とする請求項５に記載の燃料電池である。 The invention according to claim 6 is characterized in that the proton conductive material is perfluorocarbon sulfonic acid, polyether sulfone, sulfonated polyether ether ketone, or sulfonated polyimide. It is a fuel cell.
請求項７に記載の発明は、前記電子伝導性物質が、二酸化珪素、または、炭素であることを特徴とする請求項５または請求項６に記載の燃料電池である。 The invention according to claim 7 is the fuel cell according to claim 5 or 6, wherein the electron conductive material is silicon dioxide or carbon.
請求項８に記載の発明は、前記触媒が、金、白金、パラジウム、ロジウム、ルテニウム、オスミニウムおよびイリジウムから選ばれた１種または２種以上の金属からなることを特徴とする請求項５乃至請求項７のいずれか１項に記載の燃料電池である。 The invention according to claim 8 is characterized in that the catalyst is made of one or more metals selected from gold, platinum, palladium, rhodium, ruthenium, osmium and iridium. 8. The fuel cell according to any one of items 7.
触媒の材料としては、酸素還元能力、水素酸化能力の高い１Ｂ族または８族の金属を用いることが好ましい。 As a catalyst material, it is preferable to use a Group 1B or Group 8 metal having high oxygen reduction ability and hydrogen oxidation ability.
請求項９に記載の発明は、前記触媒の平均粒径が１ｎｍ以上５ｎｍ以下であることを特徴とする請求項５乃至請求項８のいずれか１項に記載の燃料電池である。 The invention according to claim 9 is the fuel cell according to any one of claims 5 to 8, wherein the average particle diameter of the catalyst is 1 nm or more and 5 nm or less.
触媒となる金、白金、パラジウム、ロジウム、ルテニウムおよびイリジウムの最小粒径自体が１ｎｍ以上であり、触媒の平均粒径が５ｎｍを超える時は、触媒の単位重量当たりの表面積が非常に小さく、触媒活性も小さく、燃料電池の出力特性が悪い。 When the minimum particle size of gold, platinum, palladium, rhodium, ruthenium, and iridium serving as a catalyst is 1 nm or more and the average particle size of the catalyst exceeds 5 nm, the surface area per unit weight of the catalyst is very small. The activity is also small, and the output characteristics of the fuel cell are poor.
請求項１０に記載の発明は、前記電子伝導性物質の前記触媒の担持率が１％〜８０％であることを特徴とする請求項５乃至請求項９のいずれか１項に記載の燃料電池である。 The invention according to claim 10 is the fuel cell according to any one of claims 5 to 9, characterized in that the supporting rate of the catalyst of the electron conductive material is 1% to 80%. It is.
触媒の担持率が１％未満では燃料電池の出力特性が悪く、触媒の担持率が８０％を超える範囲では電池の出力は変わらず、触媒の無駄使いとなる。 When the catalyst loading is less than 1%, the output characteristics of the fuel cell are poor, and when the catalyst loading exceeds 80%, the battery output does not change and the catalyst is wasted.
請求項１１に記載の発明は、前記ガス拡散材が、導電性多孔性基材であることを特徴とする請求項３乃至請求項１０のいずれか１項に記載の燃料電池である。 The invention according to claim 11 is the fuel cell according to any one of claims 3 to 10, wherein the gas diffusion material is a conductive porous substrate.
請求項１２に記載の発明は、前記導電性多孔性基材が、カーボンペーパー、カーボンクロスであることを特徴とする請求項１１に記載の燃料電池である。 The invention according to claim 12 is the fuel cell according to claim 11, wherein the conductive porous substrate is carbon paper or carbon cloth.
本発明では、使用済みＰＥＴボトルを燃料電池のセパレータとしてリサイクルすることによって、多量の使用済みＰＥＴボトルが日々蓄積するのを抑制することができる。 In the present invention, by recycling used PET bottles as fuel cell separators, it is possible to suppress the daily accumulation of a large amount of used PET bottles.
まず、使用済みＰＥＴボトルを周知の破砕装置（図示せず）を用いて５〜７ｍｍ程度のフレーク状片に破砕する。 First, a used PET bottle is crushed into flaky pieces of about 5 to 7 mm using a known crushing device (not shown).
次に、ＰＥＴフレーク状片を、加熱温度１２０℃〜１７０℃で３時間〜４時間加熱処理する。
非結晶状態のＰＥＴフレーク状片は水分を吸収し易く、含水率が大きい。
加熱処理することによりＰＥＴフレーク状片は結晶化して、水分を殆ど吸収しなくなる。
Next, the PET flake-shaped piece is heat-treated at a heating temperature of 120 ° C. to 170 ° C. for 3 hours to 4 hours.
The amorphous PET flake-like piece is easy to absorb moisture and has a high water content.
By the heat treatment, the PET flake-like piece crystallizes and hardly absorbs moisture.
次に、加熱処理したＰＥＴフレーク状片を、切断カッタ部を有する一対のカッタローラを備えた周知の粉砕装置（図示せず）で１００μｍ〜４ｍｍの大きさに粉砕する。
ＰＥＴ粒子の大きさが５〜７ｍｍであると、ＰＥＴ粒子を型内に密に充填することができない。
一方、ＰＥＴ粒子の大きさが１００μｍ未満の場合は、静電気によりＰＥＴ粒子が凝集し、セパレータに導電性を付与するための黒鉛粉とＰＥＴ樹脂を均一に混合できない。
このＰＥＴ粉砕片（結晶化物）は、リサイクル樹脂材料として市販されており、それを用いることもできる。
Next, the heat-treated PET flake-like piece is pulverized to a size of 100 μm to 4 mm by a known pulverization apparatus (not shown) provided with a pair of cutter rollers having a cutting cutter part.
When the size of the PET particles is 5 to 7 mm, the PET particles cannot be densely filled in the mold.
On the other hand, when the size of the PET particles is less than 100 μm, the PET particles aggregate due to static electricity, and the graphite powder and the PET resin for imparting conductivity to the separator cannot be mixed uniformly.
This PET pulverized piece (crystallized product) is commercially available as a recycled resin material, and can also be used.
次に、ＰＥＴ粉砕片に、黒鉛粉を添加した後に加熱加圧成型し、セパレータを作製する。 Next, after adding graphite powder to the PET pulverized piece, it is heated and pressed to prepare a separator.
黒鉛粉の材料としては、天然黒鉛、キッシュ黒鉛を用いることができる。
中でも、経済性を考慮すると天然黒鉛が好ましい。
Natural graphite and quiche graphite can be used as the material of the graphite powder.
Among these, natural graphite is preferable in consideration of economy.
黒鉛粉の製造方法としては、原料炭素を酸性物質及び酸化剤を含む溶液中に浸漬して炭素化合物を生成させ、粉砕する方法を用いることができる。 As a method for producing graphite powder, a method of pulverizing raw material carbon by immersing it in a solution containing an acidic substance and an oxidizing agent to produce a carbon compound can be used.
原料炭素を処理する酸性物質としては、酸濃度９０重量％以上の硫酸または硫酸と硝酸の混合液を用いることができる。 As an acidic substance for treating raw material carbon, sulfuric acid or a mixed solution of sulfuric acid and nitric acid having an acid concentration of 90% by weight or more can be used.
原料炭素と酸性物質の混合比は、原料炭素１００重量部に対して酸性物質１００重量部〜１０００重量部が好ましい。 The mixing ratio of the raw material carbon and the acidic substance is preferably 100 parts by weight to 1000 parts by weight of the acidic substance with respect to 100 parts by weight of the raw material carbon.
酸化剤としては、酸濃度１０重量％〜４０重量％の過酸化水素または塩酸を用いることができる。 As the oxidizing agent, hydrogen peroxide or hydrochloric acid having an acid concentration of 10 to 40% by weight can be used.
原料炭素と酸化剤の混合比は、原料炭素１００重量部に対して酸化剤１０重量部〜６０重量部が好ましい。 The mixing ratio of the raw material carbon and the oxidizing agent is preferably 10 to 60 parts by weight of the oxidizing agent with respect to 100 parts by weight of the raw material carbon.
黒鉛粉の粒径は、１０μｍ〜１０００μｍが好ましい。
粒径が１０μｍ未満の場合、セパレータの導電率は０．２Ｓ／ｃｍを下回ってしまう。
また、粒径が１０００μｍを超える場合、黒鉛粉とＰＥＴ樹脂との相溶性が悪く、セパレータの導電率は０．２Ｓ／ｃｍを下回ってしまう。
導電率０．２Ｓ／ｃｍは、燃料電池用セパレータの導電率の許容下限値である。
The particle size of the graphite powder is preferably 10 μm to 1000 μm.
When the particle size is less than 10 μm, the conductivity of the separator is less than 0.2 S / cm.
Moreover, when a particle size exceeds 1000 micrometers, the compatibility of graphite powder and PET resin is bad, and the electrical conductivity of a separator will be less than 0.2 S / cm.
The conductivity of 0.2 S / cm is an allowable lower limit value of the conductivity of the fuel cell separator.
ＰＥＴ樹脂と黒鉛粉との配合割合は、ＰＥＴ樹脂１００重量部に黒鉛粉３００〜８００重量部を用いることができる。 As for the blending ratio of PET resin and graphite powder, 300 to 800 parts by weight of graphite powder can be used for 100 parts by weight of PET resin.
ＰＥＴ樹脂１００重量部に黒鉛粉３００重量部未満であると、セパレータの導電率は０．２Ｓ／ｃｍを下回ってしまう。
導電率０．２Ｓ／ｃｍは、燃料電池用セパレータの導電率の許容下限値である。
If the amount of the PET resin is less than 300 parts by weight with respect to 100 parts by weight of the PET resin, the conductivity of the separator is less than 0.2 S / cm.
The conductivity of 0.2 S / cm is an allowable lower limit value of the conductivity of the fuel cell separator.
また、ＰＥＴ樹脂１００重量部に黒鉛粉８００重量部以上であると、セパレータの曲げ強度は４ｋｇｆ／ｍｍ2を下回ってしまう。
曲げ強度４ｋｇｆ／ｍｍ2は、燃料電池用セパレータの強度の許容下限値である。
Moreover, the bending strength of a separator will be less than 4 kgf / mm < 2 > that it is 800 weight part or more of graphite powder with respect to 100 weight part of PET resin.
The bending strength of 4 kgf / mm 2 is an allowable lower limit value of the strength of the fuel cell separator.
セパレータの成型方法としては、加圧加熱成型法を用いることができる。
成型温度は、２８０〜３００℃を用いることができる。
成型圧力は、１×１０１〜１．５×１０２ＭＰａを用いることができる。
As a method for molding the separator, a pressure heating molding method can be used.
The molding temperature can be 280 to 300 ° C.
As the molding pressure, 1 × 10 1 to 1.5 × 10 2 MPa can be used.
金型は、セパレータ７（燃料極側）およびセパレータ８（空気極側）の片面にガス流路を形成するための凹凸部を有する金型を用いることができる。 As the mold, a mold having an uneven portion for forming a gas flow path on one side of the separator 7 (fuel electrode side) and the separator 8 (air electrode side) can be used.
次に、ガス拡散材１またはガス拡散材５上に触媒層２または触媒層４を形成する。（図１（ａ）） Next, the catalyst layer 2 or the catalyst layer 4 is formed on the gas diffusion material 1 or the gas diffusion material 5. (Fig. 1 (a))
ガス拡散材１またはガス拡散材５の材料としては、カーボンペーパー、カーボンクロスを用いることができる。 As a material of the gas diffusion material 1 or the gas diffusion material 5, carbon paper or carbon cloth can be used.
触媒層２および触媒層４の材料としては、プロトン伝導性物質であるパーフルオロカーボンスルホン酸、ポリエーテルスルフォン、スルホン化ポリエーテルエーテルケトン、スルホン化ポリイミド等、および、電子伝導性物質である二酸化珪素、炭素等、および、触媒である金、白金、パラジウム、ロジウム、ルテニウム、オスミニウムおよびイリジウムを用いることができる。 Examples of the material of the catalyst layer 2 and the catalyst layer 4 include perfluorocarbon sulfonic acid, polyether sulfone, sulfonated polyether ether ketone, sulfonated polyimide, etc., which are proton conductive materials, and silicon dioxide, which is an electron conductive material, Carbon and the like, and catalysts such as gold, platinum, palladium, rhodium, ruthenium, osmium and iridium can be used.
触媒層２および触媒層４の製造方法としては、触媒を担持した電子伝導性物質とプロトン伝導性物質を、ＩＰＡやＮＰＡ等のアルコール、および、水に溶解して触媒インクを生成した後、触媒インクをガス拡散材１または５上に、バーコート、スプレー、または、スクリーン印刷する方法を用いることができる。 The catalyst layer 2 and the catalyst layer 4 are produced by dissolving a catalyst-supported electron conductive material and proton conductive material in alcohol such as IPA and NPA and water to produce a catalyst ink, A method of bar coating, spraying, or screen printing on the gas diffusion material 1 or 5 can be used.
触媒を担持した電子伝導性物質とプロトン伝導性物質は、重量比で１：１〜５０：１の範囲にすることが好ましい。 The weight ratio of the electron conductive material carrying the catalyst and the proton conductive material is preferably in the range of 1: 1 to 50: 1.
次に、触媒層２および触媒層４を向かい合わせにして、固体高分子電解質膜３を挟み込み、固体高分子電解質膜電極接合体６（以下ＭＥＡと記述する）を作製する。（図１（ｃ）） Next, with the catalyst layer 2 and the catalyst layer 4 facing each other, the solid polymer electrolyte membrane 3 is sandwiched to produce a solid polymer electrolyte membrane electrode assembly 6 (hereinafter referred to as MEA). (Fig. 1 (c))
固体高分子電解質膜３の材料としては、スルホン基含有パーフルオロカーボン、または、カルボキシル基含有パーフルオロカーボンを用いることができる。 As a material for the solid polymer electrolyte membrane 3, a sulfone group-containing perfluorocarbon or a carboxyl group-containing perfluorocarbon can be used.
ＭＥＡ６の製造方法としては、触媒層４（燃料極側）と触媒層２（空気極側）を向かい合わせにして固体高分子電解質膜３を挟み、熱圧着する方法を用いることができる。
加熱温度としては、触媒層２、触媒層４および固体高分子電解質膜３の樹脂の軟化温度やガラス転位温度を超える温度を用いることができる。
触媒層２、触媒層４および固体高分子電解質膜３の樹脂がパーフルオロカーボンスルホン酸の場合は、温度＝１００℃〜３００℃、圧力＝１ＭＰａ〜１５ＭＰａ、時間＝５秒〜４００秒の熱圧着条件を用いることができる。
As a method for producing the MEA 6, a method in which the solid polymer electrolyte membrane 3 is sandwiched with the catalyst layer 4 (fuel electrode side) and the catalyst layer 2 (air electrode side) facing each other and thermocompression bonded can be used.
As the heating temperature, a temperature exceeding the softening temperature of the resin of the catalyst layer 2, the catalyst layer 4, and the solid polymer electrolyte membrane 3 or the glass transition temperature can be used.
When the resin of catalyst layer 2, catalyst layer 4 and solid polymer electrolyte membrane 3 is perfluorocarbon sulfonic acid, thermocompression bonding conditions of temperature = 100 ° C. to 300 ° C., pressure = 1 MPa to 15 MPa, time = 5 seconds to 400 seconds Can be used.
最後に、セパレータ７（燃料極側）およびセパレータ８（空気極側）のガス流路形成面どうしを向かい合わせにして、ＭＥＡ６を挟み込み、その両側に集電板９（燃料極側）およびセパレータ１０（空気極側）を配置してロッドで締結して燃料電池を得た。（図１（ｄ）） Finally, the gas flow path forming surfaces of the separator 7 (fuel electrode side) and the separator 8 (air electrode side) face each other and the MEA 6 is sandwiched between the current collector plate 9 (fuel electrode side) and the separator 10 on both sides thereof. (Air electrode side) was placed and fastened with a rod to obtain a fuel cell. (Fig. 1 (d))
集電板９（燃料極側）およびセパレータ１０（空気極側）の材料としては、ＳＵＳを用いることができる。 SUS can be used as the material for the current collector plate 9 (fuel electrode side) and the separator 10 (air electrode side).
まず、ＰＥＴボトルを、破砕装置を用いて５〜７ｍｍ程度のフレーク状片に破砕した。 First, the PET bottle was crushed into flaky pieces of about 5 to 7 mm using a crushing apparatus.
次に、ＰＥＴのフレーク状片を、加熱温度１５０℃で３．５時間加熱処理した。 Next, the PET flake-shaped piece was heat-treated at a heating temperature of 150 ° C. for 3.5 hours.
次に、ＰＥＴのフレーク状片を、切断カッタ部を有する一対のカッタローラを備えた周知の粉砕装置で１００μｍ〜４ｍｍの大きさに粉砕した。 Next, the PET flake-like piece was pulverized to a size of 100 μm to 4 mm by a known pulverizer equipped with a pair of cutter rollers having a cutting cutter part.
次に、以下の組成になるように、平均粒径が３ｎｍの白金を担持した電子伝導性物質（白金：電子伝導性物質＝１：１（重量比））、プロトン伝導性物質を溶媒に溶解した触媒インクを調整した。
・白金を担持したカーボン（電子伝導性物質） ７．５重量％
・パーフロロカーボンスルホン酸（プロトン伝導性物質） ２．５重量％
・水 ３０．０重量％
・ＩＰＡ ３０．０重量％
・ＮＰＡ ３０．０重量％
Next, an electron conductive material carrying platinum having an average particle diameter of 3 nm (platinum: electron conductive material = 1: 1 (weight ratio)) and proton conductive material are dissolved in a solvent so as to have the following composition. The prepared catalyst ink was prepared.
-Carbon carrying platinum (electron-conducting substance) 7.5% by weight
・ Perfluorocarbon sulfonic acid (proton conductive material) 2.5% by weight
・ Water 30.0% by weight
・ IPA 30.0% by weight
・ NPA 30.0% by weight
次に、この触媒インクを、バーコーターを使用して、２００ｍｍ×２００ｍｍのサイズに断裁した厚さ１９０μｍのカーボンペーパー上に塗布した。 Next, this catalyst ink was applied onto carbon paper having a thickness of 190 μm cut into a size of 200 mm × 200 mm using a bar coater.
次に、窒素雰囲気中、１２０℃、１時間の熱処理を施した後、３０分間放冷し、燃料電池用触媒電極を作製した。 Next, after heat treatment at 120 ° C. for 1 hour in a nitrogen atmosphere, the mixture was allowed to cool for 30 minutes to produce a fuel cell catalyst electrode.
次に、上記の方法で作製した２枚の燃料電池用触媒電極の触媒層どうしを向かい合わせにして、厚さ５０μｍのスルホン基含有パーフルオロカーボンを挟んで、１３０℃、３０分、３ＭＰａの条件で加熱成型しＭＥＡを作製した。 Next, the catalyst layers of the two fuel cell catalyst electrodes produced by the above method are face to face, and a sulfone group-containing perfluorocarbon having a thickness of 50 μm is sandwiched between 130 ° C., 30 minutes, and 3 MPa. MEA was produced by heat molding.
次に、上記１００μｍ〜４ｍｍの大きさに粉砕したＰＥＴ（ポリエチレンテレフタレート）１００重量部に対して黒鉛粉３００〜８００重量部の混合物を、面中央の１１ｃｍ×１１ｃｍの領域に２０本の並行した溝（幅：２ｍｍ、長さ：１０ｃｍ、深さ：３ｍｍ、溝間隔：２ｍｍ）が刻んであるオスメス金型を用い、温度２９０℃、成型圧力５×１０１ＭＰａで加圧加熱成型して、厚さ３ｍｍのセパレータを作製した。 Next, a mixture of 300 to 800 parts by weight of graphite powder with respect to 100 parts by weight of PET (polyethylene terephthalate) pulverized to a size of 100 μm to 4 mm, and 20 parallel grooves in an area of 11 cm × 11 cm in the center of the surface. Using a male-female mold in which (width: 2 mm, length: 10 cm, depth: 3 mm, groove interval: 2 mm) is engraved, the thickness is press-heated and molded at a temperature of 290 ° C. and a molding pressure of 5 × 10 1 MPa. A separator having a thickness of 3 mm was produced.
最後に、２つのセパレータのガス流路形成面どうしを向かい合わせにして、ＭＥＡを挟み込み、その両側にＳＵＳ製の厚さ０．３ｍｍの集電板を配置して、ロッドで締結して、燃料電池を得た。 Finally, the gas flow path forming surfaces of the two separators face each other, the MEA is sandwiched between them, SUS-made current collector plates with a thickness of 0.3 mm are arranged on both sides, and fastened with rods. A battery was obtained.
次に、燃料電池の出力を、エレクトロケミカルインターフェース（ソーラトロン社製ＳＩ−１２８７）、周波数応答アナライザー（ソーラトロン社製ＳＩ−１２６０）、電子負荷器（スクリブナー社製８９０ＣＬ）が用いられている燃料電池測定システムＧＦＴ−ＳＧ１（株式会社東陽テクニカ製）を用いて、以下のように測定した。 Next, the output of the fuel cell is measured by a fuel cell using an electrochemical interface (Solaron SI-1287), a frequency response analyzer (Solartron SI-1260), and an electronic loader (Scribner 890CL). Using system GFT-SG1 (manufactured by Toyo Corporation), the measurement was performed as follows.
まず、上記の燃料電池をグラファイト製の発電セルに装着後、４０℃、相対湿度１００％の条件にて１時間保管した。
この間、厚さ５０μｍのスルホン基含有パーフルオロカーボン膜を十分に湿潤させる目的で、燃料電池には１Ａ／ｃｍ２の直流電流を発電モードで流し続けた。
First, after mounting the fuel cell on a power generation cell made of graphite, it was stored for 1 hour under the conditions of 40 ° C. and relative humidity of 100%.
During this time, a direct current of 1 A / cm 2 was continuously supplied to the fuel cell in the power generation mode in order to sufficiently wet the sulfone group-containing perfluorocarbon membrane having a thickness of 50 μm.
次に、セル温度を８０℃、アノード加湿器温度を８０℃、カソード加湿器温度を８０℃、配管温度を１２０℃、アノードの水素ガス流量を０．３リットル／分、カソードの酸素ガス流量を１．０リットル／分の条件で燃料電池の出力を測定した。
燃料電池の出力は１．０Ｗ／ｃｍ２であり、良好な発電特性を示した。
Next, the cell temperature is 80 ° C., the anode humidifier temperature is 80 ° C., the cathode humidifier temperature is 80 ° C., the piping temperature is 120 ° C., the anode hydrogen gas flow rate is 0.3 liter / min, and the cathode oxygen gas flow rate is The output of the fuel cell was measured under the condition of 1.0 liter / min.
The output of the fuel cell was 1.0 W / cm 2 , indicating good power generation characteristics.
＜比較例＞
まず、以下の組成になるように、平均粒径が３ｎｍの白金を担持した電子伝導性物質（白金：電子伝導性物質＝１：１（重量比））、プロトン伝導性物質を溶媒に溶解した触媒インクを調整した。
・白金を担持したカーボン（電子伝導性物質） ７．５重量％
・パーフロロカーボンスルホン酸（プロトン伝導性物質） ２．５重量％
・水 ３０．０重量％
・ＩＰＡ ３０．０重量％
・ＮＰＡ ３０．０重量％
<Comparative example>
First, an electron conductive material carrying platinum having an average particle diameter of 3 nm (platinum: electron conductive material = 1: 1 (weight ratio)) and a proton conductive material were dissolved in a solvent so as to have the following composition. A catalyst ink was prepared.
-Carbon carrying platinum (electron-conducting substance) 7.5% by weight
・ Perfluorocarbon sulfonic acid (proton conductive material) 2.5% by weight
・ Water 30.0% by weight
・ IPA 30.0% by weight
・ NPA 30.0% by weight
次に、この触媒インクを、バーコーターを使用して、２００ｍｍ×２００ｍｍのサイズに断裁した厚さ１９０μｍのカーボンペーパー上に塗布した。 Next, this catalyst ink was applied onto carbon paper having a thickness of 190 μm cut into a size of 200 mm × 200 mm using a bar coater.
次に、窒素雰囲気中、１２０℃、１時間の熱処理を施した後、３０分間放冷し、燃料電池用触媒電極を作製した。 Next, after heat treatment at 120 ° C. for 1 hour in a nitrogen atmosphere, the mixture was allowed to cool for 30 minutes to produce a fuel cell catalyst electrode.
次に、上記の方法で作製した２枚の燃料電池用触媒電極の触媒層どうしを向かい合わせにして、厚さ５０μｍのスルホン基含有パーフルオロカーボンを挟んで、１３０℃、３０分、３ＭＰａの条件で熱圧着し平板状のＭＥＡを作製した。 Next, the catalyst layers of the two fuel cell catalyst electrodes produced by the above method are face to face, and a sulfone group-containing perfluorocarbon having a thickness of 50 μm is sandwiched between 130 ° C., 30 minutes, and 3 MPa. A plate-like MEA was produced by thermocompression bonding.
最後に、面中央の１１ｃｍ×１１ｃｍの領域に２０本の並行した溝（幅：２ｍｍ、長さ：１０ｃｍ、深さ：３ｍｍ、溝間隔：２ｍｍ）が刻んである厚さ３ｍｍの銅製のセパレータを２組用意し、２つのセパレータのガス流路形成面どうしを向かい合わせにして、ＭＥＡを挟み込み、その両側にＳＵＳ製の厚さ０．３ｍｍの集電板を配置して、ロッドで締結して、燃料電池を得た。 Finally, a 3 mm thick copper separator with 20 parallel grooves (width: 2 mm, length: 10 cm, depth: 3 mm, groove spacing: 2 mm) in an 11 cm × 11 cm region in the center of the surface Two sets are prepared, the gas flow path forming surfaces of the two separators face each other, the MEA is sandwiched, SUS current collector plates with a thickness of 0.3 mm are arranged on both sides, and fastened with rods A fuel cell was obtained.
次に、燃料電池の出力を、エレクトロケミカルインターフェース（ソーラトロン社製ＳＩ−１２８７）、周波数応答アナライザー（ソーラトロン社製ＳＩ−１２６０）、電子負荷器（スクリブナー社製８９０ＣＬ）が用いられている燃料電池測定システムＧＦＴ−ＳＧ１（株式会社東陽テクニカ製）を用いて、以下のように測定した。 Next, the output of the fuel cell is measured by a fuel cell using an electrochemical interface (Solaron SI-1287), a frequency response analyzer (Solartron SI-1260), and an electronic loader (Scribner 890CL). Using system GFT-SG1 (manufactured by Toyo Corporation), the measurement was performed as follows.
まず、上記の燃料電池をグラファイト製の発電セルに装着後、４０℃、相対湿度１００％の条件にて１時間保管した。
この間、厚さ５０μｍのスルホン基含有パーフルオロカーボン膜を十分に湿潤させる目的で燃料電池には１Ａ／ｃｍ２の直流電流を発電モードで流し続けた。
First, after mounting the fuel cell on a power generation cell made of graphite, it was stored for 1 hour under the conditions of 40 ° C. and relative humidity of 100%.
During this time, a direct current of 1 A / cm 2 was continuously supplied to the fuel cell in the power generation mode in order to sufficiently wet the sulfone group-containing perfluorocarbon membrane having a thickness of 50 μm.
次に、セル温度を８０℃、アノード加湿器温度を８０℃、カソード加湿器温度を８０℃、配管温度を１２０℃、アノードの水素ガス流量を０．３リットル／分、カソードの酸素ガス流量を１．０リットル／分の条件で燃料電池の出力を測定した。
固体高分子型燃料電池の出力は１．０Ｗ／ｃｍ２であった。
Next, the cell temperature is 80 ° C., the anode humidifier temperature is 80 ° C., the cathode humidifier temperature is 80 ° C., the piping temperature is 120 ° C., the anode hydrogen gas flow rate is 0.3 liter / min, and the cathode oxygen gas flow rate is The output of the fuel cell was measured under the condition of 1.0 liter / min.
The output of the polymer electrolyte fuel cell was 1.0 W / cm 2 .
本発明のセパレータを使用した燃料電池は、従来使用されている銅製のセパレータを使用した燃料電池と同等の出力特性が有ることが確認された。 It has been confirmed that the fuel cell using the separator of the present invention has output characteristics equivalent to those of a fuel cell using a copper separator that has been conventionally used.
本発明の、燃料電池用セパレータおよびその製造方法、並びに、それを用いた燃料電池は、ＰＥＴボトルのリサイクルに利用できる。
また、電気自動車用電源、携帯電話用電源等に用いるＰＡＦＣ（リン酸型）、ＰＥＦＣ（固体高分子型）燃料電池に利用できる。
The separator for a fuel cell, the method for producing the same, and the fuel cell using the same of the present invention can be used for recycling PET bottles.
Further, it can be used for PAFC (phosphoric acid type) and PEFC (solid polymer type) fuel cells used for power sources for electric vehicles, cellular phones and the like.
１・・・・ガス拡散材（空気極側）
２・・・・触媒層（空気極側）
３・・・・固体高分子電解質膜
４・・・・触媒層（燃料極側）
５・・・・ガス拡散材（燃料極側）
６・・・・ＭＥＡ（固体高分子電解質膜電極接合体）
７・・・・セパレータ（燃料極側）
８・・・・セパレータ（空気極側）
９・・・・集電板（燃料極側）
１０・・・集電板（空気極側）
1. Gas diffusion material (air electrode side)
2 .... Catalyst layer (Air electrode side)
3 ... Solid polymer electrolyte membrane 4 ... Catalyst layer (fuel electrode side)
5. Gas diffusion material (fuel electrode side)
6 ... MEA (Solid polymer electrolyte membrane electrode assembly)
7 ... Separator (fuel electrode side)
8 ... Separator (air electrode side)
9 ... Current collector (fuel electrode side)
10 ... collector plate (air electrode side)
Claims (12)
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2005335426A JP2007141704A (en) | 2005-11-21 | 2005-11-21 | Separator for fuel cell, and its manufacturing method, as well as fuel cell using it |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2005335426A JP2007141704A (en) | 2005-11-21 | 2005-11-21 | Separator for fuel cell, and its manufacturing method, as well as fuel cell using it |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JP2007141704A true JP2007141704A (en) | 2007-06-07 |
Family
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2005335426A Pending JP2007141704A (en) | 2005-11-21 | 2005-11-21 | Separator for fuel cell, and its manufacturing method, as well as fuel cell using it |
Country Status (1)
| Country | Link |
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| JP (1) | JP2007141704A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009117069A (en) * | 2007-11-02 | 2009-05-28 | Equos Research Co Ltd | Paste for electrode of fuel cell, membrane electrode assembly, and method of manufacturing paste for electrode |
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2005
- 2005-11-21 JP JP2005335426A patent/JP2007141704A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009117069A (en) * | 2007-11-02 | 2009-05-28 | Equos Research Co Ltd | Paste for electrode of fuel cell, membrane electrode assembly, and method of manufacturing paste for electrode |
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