Long-Range Electron Transfer over Graphene-Based Catalyst for High-Performing Oxygen Reduction Reactions: Importance of Size, N-doping, and Metallic Impurities
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作者:
Choi, Chang Hyuck
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Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South KoreaKorea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Choi, Chang Hyuck
[1
]
Lim, Hyung-Kyu
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Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South KoreaKorea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Lim, Hyung-Kyu
[2
]
Chung, Min Wook
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Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South KoreaKorea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Chung, Min Wook
[2
]
Park, Jong Cheol
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Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
GS Caltex, Connect & Dev Team 1, Taejon 305380, South KoreaKorea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Park, Jong Cheol
[1
,3
]
Shin, Hyeyoung
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Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South KoreaKorea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Shin, Hyeyoung
[2
]
Kim, Hyungjun
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Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South KoreaKorea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Kim, Hyungjun
[2
]
Woo, Seong Ihl
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Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South KoreaKorea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
Woo, Seong Ihl
[1
,2
]
机构:
[1] Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
[2] Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South Korea
[3] GS Caltex, Connect & Dev Team 1, Taejon 305380, South Korea
N-doped carbon materials are considered as next-generation oxygen reduction reaction (ORR) catalysts for fuel cells due to their prolonged stability and low cost. However, the underlying mechanism of these catalysts has been only insufficiently identified, preventing the rational design of high-performing catalysts. Here, we show that the first electron is transferred into O-2 molecules at the outer Helmholtz plane (ET-OHP) over a long range. This is in sharp contrast to the conventional belief that O-2 adsorption must precede the ET step and thus that the active site must possess as good an O-2 binding character as that which occurs on metallic catalysts. Based on the ET-OHP mechanism, the location of the electrode potential dominantly characterizes the ORR activity. Accordingly, we demonstrate that the electrode potential can be elevated by reducing the graphene size and/or including metal impurities, thereby enhancing the ORR activity, which can be transferred into single-cell operations with superior stability.
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页码:9070 / 9077
页数:8
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Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Ferrandon, Magali
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Kropf, A. Jeremy
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Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Kropf, A. Jeremy
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Myers, Deborah J.
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Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Myers, Deborah J.
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Artyushkova, Kateryna
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Univ New Mexico, Dept Chem & Nucl Engn, Farris Engn Ctr 209, Albuquerque, NM 87131 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Artyushkova, Kateryna
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Kramm, Ulrike
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Helmholtz Ctr Berlin Mat & Energy, Dept Solar Fuels & Energy Storage E I6, D-14109 Berlin, GermanyArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Kramm, Ulrike
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Bogdanoff, Peter
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Helmholtz Ctr Berlin Mat & Energy, Dept Solar Fuels & Energy Storage E I6, D-14109 Berlin, GermanyArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Bogdanoff, Peter
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Wu, Gang
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Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Wu, Gang
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Johnston, Christina M.
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Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Johnston, Christina M.
;
Zelenay, Piotr
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Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
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Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Ferrandon, Magali
;
Kropf, A. Jeremy
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Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Kropf, A. Jeremy
;
Myers, Deborah J.
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Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Myers, Deborah J.
;
Artyushkova, Kateryna
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Univ New Mexico, Dept Chem & Nucl Engn, Farris Engn Ctr 209, Albuquerque, NM 87131 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Artyushkova, Kateryna
;
Kramm, Ulrike
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Helmholtz Ctr Berlin Mat & Energy, Dept Solar Fuels & Energy Storage E I6, D-14109 Berlin, GermanyArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Kramm, Ulrike
;
Bogdanoff, Peter
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Helmholtz Ctr Berlin Mat & Energy, Dept Solar Fuels & Energy Storage E I6, D-14109 Berlin, GermanyArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Bogdanoff, Peter
;
Wu, Gang
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Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Wu, Gang
;
Johnston, Christina M.
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Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
Johnston, Christina M.
;
Zelenay, Piotr
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Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USAArgonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA