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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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 O2 adsorption must precede the ET step and thus that the active site must possess as good an O2 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.
Publisher
AMER CHEMICAL SOC
Issue Date
2014
Language
English
Article Type
Article
Keywords

PEM FUEL-CELLS; NITROGEN-DOPED GRAPHENE; CATHODE CATALYSTS; CARBON; ELECTROCATALYSTS; IRON; POLYANILINE; MECHANISM; PLATINUM; SITES

Citation

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.136, no.25, pp.9070 - 9077

ISSN
0002-7863
DOI
10.1021/ja5033474
URI
http://hdl.handle.net/10203/190019
Appears in Collection
EEW-Journal Papers(저널논문)CBE-Journal Papers(저널논문)
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