JP2008532732A - 炭素担持された白金合金触媒 - Google Patents
炭素担持された白金合金触媒 Download PDFInfo
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- JP2008532732A JP2008532732A JP2007541859A JP2007541859A JP2008532732A JP 2008532732 A JP2008532732 A JP 2008532732A JP 2007541859 A JP2007541859 A JP 2007541859A JP 2007541859 A JP2007541859 A JP 2007541859A JP 2008532732 A JP2008532732 A JP 2008532732A
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- catalyst
- carbon
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- transition metal
- carbon support
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- 239000003054 catalyst Substances 0.000 title claims abstract description 63
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 33
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 32
- 229910001260 Pt alloy Inorganic materials 0.000 title claims abstract description 19
- 238000009792 diffusion process Methods 0.000 claims abstract description 16
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 15
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 15
- 150000003624 transition metals Chemical class 0.000 claims abstract description 15
- YKIOKAURTKXMSB-UHFFFAOYSA-N adams's catalyst Chemical compound O=[Pt]=O YKIOKAURTKXMSB-UHFFFAOYSA-N 0.000 claims abstract description 11
- 229910052804 chromium Inorganic materials 0.000 claims abstract description 8
- 238000011065 in-situ storage Methods 0.000 claims abstract description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 8
- 238000006722 reduction reaction Methods 0.000 claims abstract description 7
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 5
- 229910052742 iron Inorganic materials 0.000 claims abstract description 4
- 229910052720 vanadium Inorganic materials 0.000 claims abstract description 4
- 229910000045 transition metal hydride Inorganic materials 0.000 claims abstract 2
- 238000000034 method Methods 0.000 claims description 28
- 239000002002 slurry Substances 0.000 claims description 16
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
- 239000007789 gas Substances 0.000 claims description 15
- 239000002253 acid Substances 0.000 claims description 13
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 12
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 8
- 239000006229 carbon black Substances 0.000 claims description 8
- 150000003839 salts Chemical class 0.000 claims description 8
- 229910021529 ammonia Inorganic materials 0.000 claims description 6
- 238000006243 chemical reaction Methods 0.000 claims description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 5
- 239000002243 precursor Substances 0.000 claims description 5
- 235000011121 sodium hydroxide Nutrition 0.000 claims description 5
- 229910002651 NO3 Inorganic materials 0.000 claims description 4
- 239000003513 alkali Substances 0.000 claims description 4
- 238000000137 annealing Methods 0.000 claims description 4
- NHNBFGGVMKEFGY-UHFFFAOYSA-N nitrate group Chemical group [N+](=O)([O-])[O-] NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 4
- 229910052786 argon Inorganic materials 0.000 claims description 3
- 239000003014 ion exchange membrane Substances 0.000 claims description 3
- 239000007864 aqueous solution Substances 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims description 2
- 238000004320 controlled atmosphere Methods 0.000 claims 3
- 239000012298 atmosphere Substances 0.000 claims 2
- 239000012300 argon atmosphere Substances 0.000 claims 1
- 239000012299 nitrogen atmosphere Substances 0.000 claims 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 abstract description 35
- 239000011651 chromium Substances 0.000 abstract description 11
- 239000012528 membrane Substances 0.000 abstract description 7
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 abstract description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 abstract description 4
- 229910017052 cobalt Inorganic materials 0.000 abstract description 4
- 239000010941 cobalt Substances 0.000 abstract description 4
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 abstract description 4
- 239000010411 electrocatalyst Substances 0.000 abstract description 2
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 abstract description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 46
- 229910052697 platinum Inorganic materials 0.000 description 20
- 239000000243 solution Substances 0.000 description 15
- 230000015572 biosynthetic process Effects 0.000 description 13
- 239000000446 fuel Substances 0.000 description 10
- 229910052751 metal Inorganic materials 0.000 description 10
- 239000002184 metal Substances 0.000 description 10
- 239000002245 particle Substances 0.000 description 8
- 238000005275 alloying Methods 0.000 description 7
- 229910045601 alloy Inorganic materials 0.000 description 6
- 239000000956 alloy Substances 0.000 description 6
- 238000010438 heat treatment Methods 0.000 description 6
- 238000003756 stirring Methods 0.000 description 6
- 239000008367 deionised water Substances 0.000 description 5
- 229910021641 deionized water Inorganic materials 0.000 description 5
- 239000001257 hydrogen Substances 0.000 description 5
- 229910052739 hydrogen Inorganic materials 0.000 description 5
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 229910019026 PtCr Inorganic materials 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 229920000554 ionomer Polymers 0.000 description 3
- 229910044991 metal oxide Inorganic materials 0.000 description 3
- 150000004706 metal oxides Chemical class 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- 229910002844 PtNi Inorganic materials 0.000 description 2
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 description 2
- 229910001981 cobalt nitrate Inorganic materials 0.000 description 2
- 239000000084 colloidal system Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000011109 contamination Methods 0.000 description 2
- 239000004744 fabric Substances 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- NBVXSUQYWXRMNV-UHFFFAOYSA-N fluoromethane Chemical compound FC NBVXSUQYWXRMNV-UHFFFAOYSA-N 0.000 description 2
- 239000008187 granular material Substances 0.000 description 2
- 238000010348 incorporation Methods 0.000 description 2
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical group [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 description 2
- 229910017604 nitric acid Inorganic materials 0.000 description 2
- 239000012071 phase Substances 0.000 description 2
- 239000004810 polytetrafluoroethylene Substances 0.000 description 2
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 238000000527 sonication Methods 0.000 description 2
- 239000000725 suspension Substances 0.000 description 2
- 229910000314 transition metal oxide Inorganic materials 0.000 description 2
- LBLYYCQCTBFVLH-UHFFFAOYSA-N 2-Methylbenzenesulfonic acid Chemical compound CC1=CC=CC=C1S(O)(=O)=O LBLYYCQCTBFVLH-UHFFFAOYSA-N 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- 229910002845 Pt–Ni Inorganic materials 0.000 description 1
- 230000010757 Reduction Activity Effects 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 239000008346 aqueous phase Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 239000013043 chemical agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000001143 conditioned effect Effects 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 230000034964 establishment of cell polarity Effects 0.000 description 1
- 229920002313 fluoropolymer Polymers 0.000 description 1
- 238000007756 gravure coating Methods 0.000 description 1
- QWPPOHNGKGFGJK-UHFFFAOYSA-N hypochlorous acid Chemical compound ClO QWPPOHNGKGFGJK-UHFFFAOYSA-N 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910001960 metal nitrate Inorganic materials 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 125000000896 monocarboxylic acid group Chemical group 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 229910002059 quaternary alloy Inorganic materials 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 238000007761 roller coating Methods 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 239000012266 salt solution Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 238000010561 standard procedure Methods 0.000 description 1
- 229910002058 ternary alloy Inorganic materials 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- ITMCEJHCFYSIIV-UHFFFAOYSA-N triflic acid Chemical compound OS(=O)(=O)C(F)(F)F ITMCEJHCFYSIIV-UHFFFAOYSA-N 0.000 description 1
- 239000002759 woven fabric Substances 0.000 description 1
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Abstract
【選択図】なし
Description
触媒、より詳細には、ガス拡散電極又は触媒被覆膜構造への組み込みに適した炭素担持された白金合金電極触媒。
炭素担持白金(Carbon−supported platinum)は、例えば、燃料電池、電気分解及びセンサー用途において、ガス拡散電極及び触媒被覆膜構造(catalyst−coated membrane structures)への組み込みのためによく知られた触媒である。場合によっては、異なる目的のために白金と他の遷移金属を合金するのが望ましい;例えば他の貴金属(例えばルテニウム)との白金合金の場合は、一酸化炭素耐性アノード触媒及び直接メタノール燃料電池(または他の直接酸化燃料電池)のためのガス拡散アノードの分野ではよく知られている。炭素担持された、非貴の遷移金属(non−noble transition metals)との白金合金は、燃料電池の分野、特にガス拡散カソードのために有用であることも知られている。ニッケル、クロム又はコバルトとの白金合金は、通常酸素還元に対して優れた活性を示す。これらの合金は、直接酸化燃料電池カソードのためにより有用であり得る。なぜなら、それらの高い活性に加えて、それらはまた、アルコール燃料(これらはセパレーターとして使用される半透膜を超えてある程度拡散し、一般的にこれらの電池のカソードコンポーネントを重要なほどに汚染する)によって、より汚染されにくいからである。
これは、なぜ合金化の程度が、個々の元素の大きなドメインと限定された合金相(limited alloyed phase)の形成を伴って重要な程度まで凝離が起こることを示すXRDスキャンによって証明されたように、相当低いのかを、説明する。
いくつかの適当な白金触媒としての望ましい電気化学的特質が失われるのに加えて、この構造均一性の欠如はまた、不満足な平均粒度及びその分布をもたらす。そのうえ、塩化白金酸の使用は系中に、完全に除去するのが困難で、かつ触媒毒として働き得、その活性を低下させる塩化物イオンを導入する。
本発明の目的は、高度の合金化及び微少で均質な粒度により特徴付けられる炭素担持白金合金触媒を提供することである。
第1の局面において、本発明は、炭素担体上の二酸化白金及び少なくとも1つの遷移金属水和酸化物MOX−YH2O(ここでMは任意の遷移金属であり、より有利にはニッケル、コバルト、クロム、バナジウム及び鉄の中から選択される)の同時の化学的還元により得られる炭素担持白金合金触媒からなる。好ましい実施形態において、二酸化白金は、白金酸としてもまた知られたヘキサヒドロキソ白金(IV)酸(dihydrogen hexahydroxyplatinate:H2Pt(OH)6)から沈殿し、遷移金属水和酸化物は可溶遷移金属塩、好ましくは硝酸塩の転化により得られる。1を超える遷移金属水和酸化物は、例えば炭素担持された3成分系又は4成分系合金の形成のために、二酸化白金と同時に還元され得る。
実施例1
Vulcan XC−72カーボンブラック上の30重量%Pt−Ni触媒(Pt:Ni 1:1、原子ベース)100gを、つぎの手順に従って調製した:
70gのCabot Corp./アメリカ合衆国 社製のVulcan XC−72を4リットルビーカー中で2.5リットルのイオン化水(ionized water)により懸濁した。5分間の超音波処理により炭素を微細に分散させ、そしてスラリーをマグネチックスターラーにより撹拌し、そして87mlの濃HNO3(〜69%)をそこへ加えた。
実施例2
実施例1の手順を、Vulcan XC−72上の30重量%のPt:Ni 2:1触媒を得るため、改変した。この目的のために、PTAの量を40.75g(トータル26.08gのPt)に増やし、一方スラリーに加えるNi(NO3)2・6H2Oの量は19.43g(20.19%Ni、トータルで3.92gのNi)に減らした。
実施例3
実施例1の手順を、Vulcan XC−72上の30重量%のPt:Ni 3:1触媒を得るため、改変した。この目的のために、PTAの量を42.60g(トータル27.27gのPt)に増やし、一方スラリーに加えるNi(NO3)2・6H2Oの量は13.54g(20.19%Ni、トータルで2.73gのNi)に減らした。
実施例4
実施例1の手順を、Vulcan XC−72上の30重量%のPt:Ni 4:1触媒を得るため、改変した。この目的のために、PTAの量を43.60g(トータル27.90gのPt)に増やし、一方スラリーに加えるNi(NO3)2・6H2Oの量は10.39g(20.19%Ni、トータルで2.10gのNi)に減らした。
実施例5
実施例3の手順を、Vulcan XC−72上の30重量%のPt:Co 3:1触媒を得るため、改変した。この目的のために、硝酸ニッケルをモル当量の硝酸コバルトへと置き換えた。
実施例6
Vulcan XC−72カーボンブラック上の30重量%Pt−Cr触媒(Pt:Cr 3:1)100gを、つぎの手順に従って調製した:
4リットルビーカー中で2.5リットルの脱イオン化水(deionized water)に70gのCabot Corp./アメリカ合衆国 社製のVulcan XC−72を懸濁し、そして15分間の超音波処理により該カーボンを微細に分散させた。さらにスラリーをマグネチックスターラーにより撹拌し、そして87mlの濃HNO3(〜69%)をそこへ加えた。
実施例7
グラビア/ローラーコーティング機を用いてテキストロン(Textron)カーボンクロス上のインク溶液からShawiniganアセチレンブラック(SAB)/PTFE層(60/40wt)を第1層に適用し、そしてVulcan XC−72/PTFEを第2層に適用することによって、ガス拡散電極を調製した。被覆カーボンクロスは340℃で焼結した。このようにして得られた焼結させたガス拡散層を重量2:1の触媒/アイオノマー懸濁インクに対し支持体として使用し、一方で、触媒は実施例6のPtCr/Cであり、フルオロカーボンポリマーアイオノマー懸濁液はアルコール中で9%の市販フルオロカーボン材料から調製した。約0.4―0.5 mg/cm2でロードされたPtが幾つかの被膜中に得られた。所望の白金充填に達した後、100−130℃で最終アニーリングを行った。
比較例1
ガス拡散電極を、使用した触媒が、実施例1の手順(但し硝酸ニッケルの添加及びその後の転化を省略)に従って白金酸を用いて調製した30%Pt/Cであることを除いては、実施例7に記載の手順に従って調製した。
実施例8
膜−電極接合体(MEA)を、実施例7で調製したガス拡散電極をカソードとして、そして標準的な機械製品の30%PT/Cガス拡散電極(公知技術として知られたフルオロカーボンポリマーアイオノマーで含浸され、標準的な手順に従って市販膜の反対側にホットプレスされたもの)を、アノードとして組み込むことにより作製した。他のMEAを同じ手順(但し比較例1のガス拡散電極をカソードとして使用)で作製した。どちらのMEAも実験燃料電池へ導入し、70℃、100%に調湿の反応ガス(空気/純粋(pure)H2)で作動させた。圧力は、カソード側に4バール絶対圧、アノード側3.5バール絶対圧の一定のフローレート(flow−rates)とし、1.2A/cm2の空気2、水素1.5の化学量論の比率に相当する。
実施例9
図2は、実施例6の3:1 PtCr触媒(3)及び米国特許番号5876867の教示に従って調製した3:1 PtCr触媒(4)のXRDスペクトルを示す。Pt220ピーク(2θ=68−69)は実施例6のより高い値を示すものであり、合金化の優れた程度を示すものである。その上、2θ=40から48の間に、より顕著な実施例6の触媒の“超格子ピーク”がみられる。これらのピークは、良好なO2還元活性と関連する。実施例6の触媒はまた、公知技術の触媒のXRDサイズ(53Å)と比較して、より小さいXRDサイズ(37Å)を有する。これは、実施例6の触媒が、より良好な性能と関連するより高い表面積を有することを示す。
Claims (24)
- インサイチュで形成された(in situ―formed)二酸化白金及び炭素担体上の少なくとも1つの遷移金属水和酸化物(transition metal hydrous oxide)の同時の化学的還元により得られ得る、炭素担持された白金合金触媒。
- 前記炭素担体が、少なくとも50m2/gのアクティブエリア(active area)を有するカーボンブラックである、請求項1の触媒。
- 前記インサイチュで形成された二酸化白金が、前記炭素担体上でのヘキサヒドロキソ白金(IV)酸(dihydrogen hexahydroxyplatinate)の転化により得られる、請求項1の触媒。
- 前記少なくとも1つの遷移金属水和酸化物が、前記炭素担体上での可溶性塩の転化によって得られる、請求項1の触媒。
- 前記可溶性塩が硝酸塩である、請求項4の触媒。
- 前記遷移金属が、Ni、Cr、Co、V及びFeからなる群より選択される、請求項1の触媒。
- 前記化学的還元が、少なくとも300℃の温度において水素ガスにより行われる、請求項1の触媒。
- さらに、少なくとも600℃の温度に制御された雰囲気中でアニーリング処理に供される、請求項1の触媒。
- 前記制御された雰囲気が、不活性なアルゴン又は窒素雰囲気である、請求項8の触媒。
- 導電性ウェブ、及びその中に組み込まれた請求項1の触媒を含む、ガス拡散電極。
- イオン交換膜及び少なくとも1つのその中に組み込まれた請求項10のガス拡散電極を含む、膜−電極接合体。
- インサイチュで形成された二酸化白金及び少なくとも1つの遷移金属水和酸化物を炭素担体上で同時に還元すること含む、炭素担持された白金合金触媒の製造方法。
- 前記インサイチュで形成された二酸化白金が、pH及び/又は温度の変化により、前記炭素担体上のヘキサヒドロキソ白金(IV)酸前駆体を転化することで得られる、請求項12の方法。
- 前記少なくとも1つの遷移金属水和酸化物が、pH及び/又は温度の変化により、前記二酸化白金を含む炭素担体上の可溶性塩を転化することで得られる、請求項12の方法。
- 前記pHの変化が、アルカリ、必要に応じて苛性ソーダ、又はアンモニアの添加により得られる、請求項13の方法。
- 前記アルカリ又はアンモニアの添加により、pHを2と9の間にする、請求項15の方法。
- 前記温度の変化が、前記水溶液を、室温から、30から100℃の終温度にすることからなる、請求項13の方法。
- 前記炭素担体が、50m2/g以上のアクティブエリアを有するカーボンブラックである、請求項12の方法。
- 前記カーボンブラックが、強酸中のスラリーである、請求項18の方法。
- 前記遷移金属が、Ni、Cr、Co、V及びFeからなる群より選択される、請求項12の方法。
- 前記遷移金属の可溶性塩が硝酸塩である、請求項14の方法。
- 前記化学的還元が、少なくとも300℃の温度において水素ガスで行われる、請求項12の方法。
- さらに、少なくとも600℃の温度において制御された雰囲気中でのアニーリング処理を含む、請求項22の方法。
- 前記制御された雰囲気が不活性雰囲気である、請求項23の方法。
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PCT/EP2005/012676 WO2006056470A1 (en) | 2004-11-29 | 2005-11-28 | Platinum alloy carbon-supported catalysts |
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US10454114B2 (en) | 2016-12-22 | 2019-10-22 | The Research Foundation For The State University Of New York | Method of producing stable, active and mass-producible Pt3Ni catalysts through preferential co etching |
CN111151279B (zh) * | 2019-12-27 | 2021-01-29 | 宁波工程学院 | 一种N,P掺杂碳纤维负载FeCo/Co2 P的复合催化剂及其制备方法 |
CN113398951B (zh) * | 2021-06-16 | 2022-10-28 | 中国科学技术大学 | 金属间化合物催化剂及采用双金属络合物制备金属间化合物催化剂的方法 |
CN113430567B (zh) * | 2021-06-28 | 2022-12-09 | 哈尔滨工业大学 | 一种碳纳米管负载的金纳米簇催化剂的制备方法及其应用 |
CN114497583B (zh) * | 2022-01-12 | 2024-05-07 | 青岛创启新能催化科技有限公司 | 一种燃料电池用PtRu/CN催化剂的制备方法 |
CN115106100A (zh) * | 2022-06-08 | 2022-09-27 | 青岛科技大学 | 一种Pt-Ni合金多孔碳复合材料及其制备方法和应用 |
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CA2589747A1 (en) | 2006-06-01 |
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US20080305946A1 (en) | 2008-12-11 |
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KR101270809B1 (ko) | 2013-06-05 |
JP5014146B2 (ja) | 2012-08-29 |
US20060116285A1 (en) | 2006-06-01 |
WO2006056470A1 (en) | 2006-06-01 |
KR20070085541A (ko) | 2007-08-27 |
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