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Origin of the Electrocatalytic Oxygen Reduction Activity of Graphene-Based Catalysts: A Roadmap to Achieve the Best Performance

Open access
Jiao, Yan, Zheng, Yao, Jaroniec, Mietek, Qiao, Shi Zhang·2014·Journal of the American Chemical Society

Abstract

The mutually corroborated electrochemical measurements and density functional theory (DFT) calculations were used to uncover the origin of electrocatalytic activity of graphene-based electrocatalysts for oxygen reduction reaction (ORR). A series of graphenes doped with nonmetal elements was designed and synthesized, and their ORR performance was evaluated in terms of four electrochemical descriptors: exchange current density, on-set potential, reaction pathway selectivity and kinetic current density. It is shown that these descriptors are in good agreement with DFT calculations, allowing derivation of a volcano plot between the ORR activity and the adsorption free energy of intermediates on metal-free materials, similarly as in the case of metallic catalysts. The molecular orbital concept was used to justify this volcano plot, and to theoretically predict the ORR performance of an ideal graphene-based catalyst, the ORR activity of which is comparable to the state-of-the-art Pt catalyst. Moreover, this study may stimulate the development of metal-free electrocatalysts for other key energy conversion processes including hydrogen evolution and oxygen evolution reactions and largely expand the spectrum of catalysts for energy-related electrocatalysis reactions.

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Metadata

Authors
Jiao, Y., Zheng, Y., Jaroniec, M., & Qiao, S. Z.
Venue
Journal of the American Chemical Society
Published
2014-03-11
Volume
136
Issue
11
Pages
4394-4403
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
OpenAlex
W1979396951
Cited by
1,104
References
7
FWCI
34.93
Type
journal article
Language
en
Open access
hybrid

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CoChat. (2026). Citation check: Origin of the Electrocatalytic Oxygen Reduction Activity of Graphene-Based Catalysts: A Roadmap to Achieve the Best Performance. https://app.cochat.ai/papers/10.1021/ja500432h
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Jiao, Y., Zheng, Y., Jaroniec, M., & Qiao, S. Z. (2014). Origin of the Electrocatalytic Oxygen Reduction Activity of Graphene-Based Catalysts: A Roadmap to Achieve the Best Performance. Journal of the American Chemical Society. https://doi.org/10.1021/ja500432h

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