JP7411533B2 - 酸素還元反応のための金属間L10-NiPtAg触媒 - Google Patents
酸素還元反応のための金属間L10-NiPtAg触媒 Download PDFInfo
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- JP7411533B2 JP7411533B2 JP2020190198A JP2020190198A JP7411533B2 JP 7411533 B2 JP7411533 B2 JP 7411533B2 JP 2020190198 A JP2020190198 A JP 2020190198A JP 2020190198 A JP2020190198 A JP 2020190198A JP 7411533 B2 JP7411533 B2 JP 7411533B2
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- 239000003054 catalyst Substances 0.000 title claims description 35
- 238000006722 reduction reaction Methods 0.000 title claims description 13
- 229910052760 oxygen Inorganic materials 0.000 title claims description 10
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 title claims description 9
- 239000001301 oxygen Substances 0.000 title claims description 9
- 239000002105 nanoparticle Substances 0.000 claims description 51
- 239000000956 alloy Substances 0.000 claims description 44
- 229910045601 alloy Inorganic materials 0.000 claims description 44
- 238000000034 method Methods 0.000 claims description 37
- 230000000694 effects Effects 0.000 claims description 32
- 238000000137 annealing Methods 0.000 claims description 20
- 230000014759 maintenance of location Effects 0.000 claims description 12
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 7
- 229910052799 carbon Inorganic materials 0.000 claims description 7
- 239000002184 metal Substances 0.000 claims description 7
- 229910052751 metal Inorganic materials 0.000 claims description 7
- 239000002243 precursor Substances 0.000 claims description 7
- 239000010411 electrocatalyst Substances 0.000 claims description 5
- 239000002245 particle Substances 0.000 claims description 5
- 230000002194 synthesizing effect Effects 0.000 claims description 5
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- 239000004332 silver Substances 0.000 claims description 3
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 28
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 15
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 15
- 239000000243 solution Substances 0.000 description 9
- 230000015572 biosynthetic process Effects 0.000 description 8
- 239000000446 fuel Substances 0.000 description 7
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 125000004429 atom Chemical group 0.000 description 6
- 239000012071 phase Substances 0.000 description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 4
- 238000010899 nucleation Methods 0.000 description 4
- 238000002360 preparation method Methods 0.000 description 4
- 229920006395 saturated elastomer Polymers 0.000 description 4
- 239000006104 solid solution Substances 0.000 description 4
- 238000003786 synthesis reaction Methods 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 238000002484 cyclic voltammetry Methods 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000001995 intermetallic alloy Substances 0.000 description 3
- 230000000670 limiting effect Effects 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- QGLWBTPVKHMVHM-KTKRTIGZSA-N (z)-octadec-9-en-1-amine Chemical compound CCCCCCCC\C=C/CCCCCCCCN QGLWBTPVKHMVHM-KTKRTIGZSA-N 0.000 description 2
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 2
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- 235000019253 formic acid Nutrition 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 2
- QWPPOHNGKGFGJK-UHFFFAOYSA-N hypochlorous acid Chemical compound ClO QWPPOHNGKGFGJK-UHFFFAOYSA-N 0.000 description 2
- 229910000765 intermetallic Inorganic materials 0.000 description 2
- 238000004502 linear sweep voltammetry Methods 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000005554 pickling Methods 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- 238000012430 stability testing Methods 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- VEJOYRPGKZZTJW-FDGPNNRMSA-N (z)-4-hydroxypent-3-en-2-one;platinum Chemical compound [Pt].C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O VEJOYRPGKZZTJW-FDGPNNRMSA-N 0.000 description 1
- 241000473391 Archosargus rhomboidalis Species 0.000 description 1
- 229910002441 CoNi Inorganic materials 0.000 description 1
- 229910018979 CoPt Inorganic materials 0.000 description 1
- 229910005335 FePt Inorganic materials 0.000 description 1
- 235000008331 Pinus X rigitaeda Nutrition 0.000 description 1
- 235000011613 Pinus brutia Nutrition 0.000 description 1
- 241000018646 Pinus brutia Species 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 238000010306 acid treatment Methods 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000005119 centrifugation Methods 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 239000013256 coordination polymer Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000002848 electrochemical method Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 230000002452 interceptive effect Effects 0.000 description 1
- 229920000554 ionomer Polymers 0.000 description 1
- 239000003273 ketjen black Substances 0.000 description 1
- 238000002386 leaching Methods 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 230000001404 mediated effect Effects 0.000 description 1
- 229910001092 metal group alloy Inorganic materials 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- BMGNSKKZFQMGDH-FDGPNNRMSA-L nickel(2+);(z)-4-oxopent-2-en-2-olate Chemical compound [Ni+2].C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O BMGNSKKZFQMGDH-FDGPNNRMSA-L 0.000 description 1
- 230000008520 organization Effects 0.000 description 1
- VLTRZXGMWDSKGL-UHFFFAOYSA-N perchloric acid Chemical compound OCl(=O)(=O)=O VLTRZXGMWDSKGL-UHFFFAOYSA-N 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000002829 reductive effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000000717 retained effect Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000012552 review Methods 0.000 description 1
- 238000010532 solid phase synthesis reaction Methods 0.000 description 1
- 238000000527 sonication Methods 0.000 description 1
- 238000013112 stability test Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000001629 suppression Effects 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 238000009210 therapy by ultrasound Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22F—CHANGING THE PHYSICAL STRUCTURE OF NON-FERROUS METALS AND NON-FERROUS ALLOYS
- C22F1/00—Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working
- C22F1/14—Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working of noble metals or alloys based thereon
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F1/05—Metallic powder characterised by the size or surface area of the particles
- B22F1/054—Nanosized particles
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F1/17—Metallic particles coated with metal
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F9/00—Making metallic powder or suspensions thereof
- B22F9/16—Making metallic powder or suspensions thereof using chemical processes
- B22F9/18—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds
- B22F9/24—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds starting from liquid metal compounds, e.g. solutions
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/04—Making non-ferrous alloys by powder metallurgy
- C22C1/0433—Nickel- or cobalt-based alloys
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/04—Making non-ferrous alloys by powder metallurgy
- C22C1/0466—Alloys based on noble metals
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C5/00—Alloys based on noble metals
- C22C5/04—Alloys based on a platinum group metal
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
- H01M4/921—Alloys or mixtures with metallic elements
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F2301/00—Metallic composition of the powder or its coating
- B22F2301/25—Noble metals, i.e. Ag Au, Ir, Os, Pd, Pt, Rh, Ru
-
- 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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- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- General Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Thermal Sciences (AREA)
- Physics & Mathematics (AREA)
- Crystallography & Structural Chemistry (AREA)
- Electrochemistry (AREA)
- Inorganic Chemistry (AREA)
- Nanotechnology (AREA)
- Catalysts (AREA)
- Inert Electrodes (AREA)
- Hybrid Cells (AREA)
- Fuel Cell (AREA)
Description
本願は更に以下の態様を含んでいる:
《態様1》
1000A/g Pt を超える質量活性(MA)を有する金属間L1 0 -NiPtAg合金ナノ粒子を含む、酸素還元反応のための電極触媒。
《態様2》
前記金属間L1 0 -NiPtAg合金ナノ粒子が、1100A/g Pt を超える質量活性(MA)を有する、態様1に記載の触媒。
《態様3》
前記金属間L1 0 -NiPtAg合金ナノ粒子が、40%を超える質量活性(MA)保持率を有する、態様1に記載の触媒。
《態様4》
前記金属間L1 0 -NiPtAg合金ナノ粒子が、45%を超える質量活性(MA)保持率を有する、態様1に記載の触媒。
《態様5》
前記金属間L1 0 -NiPtAg合金ナノ粒子は、式Ni x Pt y Ag z で表され、ここで0.4≦x≦0.6、0.4≦y≦0.6、及びz≦0.1である、態様1に記載の触媒。
《態様6》
式Ni x Pt y Ag z 、ここで、0.4≦x≦0.6、0.4≦y≦0.6、及びz≦0.1、で表される金属間L1 0 -NiPtAg合金ナノ粒子を含む触媒の合成方法であって、
還元性の金属前駆体の共還元によってNiPt合金系を形成すること;
前記NiPt合金系に銀(Ag)をドープして、NiPtAg合金ナノ粒子を形成すること;
前記NiPtAg合金ナノ粒子を、カーボン担体上に担持し、300℃~約630℃で少なくとも6時間焼鈍して、L1 0 -NiPtAg金属間構造体を形成すること、
を含む、方法。
《態様7》
前記焼鈍が、約500℃~約600℃の範囲の温度で行われる、態様6に記載の方法。
《態様8》
前記焼鈍が、約550℃~約600℃の範囲の温度で行われる、態様6に記載の方法。
《態様9》
前記焼鈍が、約550℃の温度で行われる、態様6に記載の方法。
《態様10》
前記金属間L1 0 -NiPtAg合金ナノ粒子が、1100A/g Pt を超える質量活性(MA)を有する、態様6に記載の方法。
《態様11》
前記金属間L1 0 -NiPtAg合金ナノ粒子が、40%を超える質量活性(MA)保持率を有する、態様6に記載の方法。
《態様12》
前記金属間L1 0 -NiPtAg合金ナノ粒子が、45%を超える質量活性(MA)保持率を有する、態様6に記載の方法。
Claims (12)
- 1000A/gPtを超える質量活性(MA)を有する金属間L10-NiPtAg合金ナノ粒子を含む、酸素還元反応のための電極触媒。
- 前記金属間L10-NiPtAg合金ナノ粒子が、1100A/gPtを超える質量活性(MA)を有する、請求項1に記載の触媒。
- 前記金属間L10-NiPtAg合金ナノ粒子が、40%を超える質量活性(MA)保持率を有する、請求項1に記載の触媒。
- 前記金属間L10-NiPtAg合金ナノ粒子が、45%を超える質量活性(MA)保持率を有する、請求項1に記載の触媒。
- 前記金属間L10-NiPtAg合金ナノ粒子は、式NixPtyAgzで表され、ここで0.4≦x≦0.6、0.4≦y≦0.6、及びz≦0.1である、請求項1に記載の触媒。
- 式NixPtyAgz、ここで、0.4≦x≦0.6、0.4≦y≦0.6、及びz≦0.1、で表される金属間L10-NiPtAg合金ナノ粒子を含む触媒の合成方法であって、
還元性の金属前駆体の共還元によってNiPt合金系を形成すること;
前記NiPt合金系に銀(Ag)をドープして、NiPtAg合金ナノ粒子を形成すること;
前記NiPtAg合金ナノ粒子を、カーボン担体上に担持し、300℃~630℃で少なくとも6時間焼鈍して、L10-NiPtAg金属間構造体を形成すること、
を含む、方法。 - 前記焼鈍が、500℃~600℃の範囲の温度で行われる、請求項6に記載の方法。
- 前記焼鈍が、550℃~600℃の範囲の温度で行われる、請求項6に記載の方法。
- 前記焼鈍が、550℃の温度で行われる、請求項6に記載の方法。
- 前記金属間L10-NiPtAg合金ナノ粒子が、1100A/gPtを超える質量活性(MA)を有する、請求項6に記載の方法。
- 前記金属間L10-NiPtAg合金ナノ粒子が、40%を超える質量活性(MA)保持率を有する、請求項6に記載の方法。
- 前記金属間L10-NiPtAg合金ナノ粒子が、45%を超える質量活性(MA)保持率を有する、請求項6に記載の方法。
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US16/716,127 | 2019-12-16 |
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JP2017045625A (ja) | 2015-08-27 | 2017-03-02 | 株式会社ノリタケカンパニーリミテド | 電極用材料 |
JP2019534145A (ja) | 2016-10-26 | 2019-11-28 | スリーエム イノベイティブ プロパティズ カンパニー | 触媒 |
JP2020168588A (ja) | 2019-04-01 | 2020-10-15 | 国立大学法人 東京大学 | 担持バイメタル合金の製造方法 |
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US9005331B2 (en) | 2004-12-22 | 2015-04-14 | Brookhaven Science Associates, Llc | Platinum-coated non-noble metal-noble metal core-shell electrocatalysts |
US9680161B2 (en) | 2013-07-15 | 2017-06-13 | The Board Of Trustees Of The University Of Illinois | Noble metal-based electrocatalyst and method of treating a noble metal-based electrocatalyst |
US10680249B2 (en) | 2013-11-27 | 2020-06-09 | Brookhaven Science Associates, Llc | Nitride stabilized core/shell nanoparticles |
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Patent Citations (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20130133483A1 (en) | 2010-03-08 | 2013-05-30 | University Of Rochester | Synthesis of Nanoparticles Using Reducing Gases |
JP2017045625A (ja) | 2015-08-27 | 2017-03-02 | 株式会社ノリタケカンパニーリミテド | 電極用材料 |
JP2019534145A (ja) | 2016-10-26 | 2019-11-28 | スリーエム イノベイティブ プロパティズ カンパニー | 触媒 |
JP2020168588A (ja) | 2019-04-01 | 2020-10-15 | 国立大学法人 東京大学 | 担持バイメタル合金の製造方法 |
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JP2021097037A (ja) | 2021-06-24 |
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