Origin of the electrocatalytic oxygen reduction activity of graphene-based catalysts: a roadmap to achieve the best performance

Jiao, Yan, Zheng, Yao, Jaroniec, Mietek and Qiao, Shi Zhang (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, 136 11: 4394-4403. doi:10.1021/ja500432h


Author Jiao, Yan
Zheng, Yao
Jaroniec, Mietek
Qiao, Shi Zhang
Title Origin of the electrocatalytic oxygen reduction activity of graphene-based catalysts: a roadmap to achieve the best performance
Journal name Journal of the American Chemical Society   Check publisher's open access policy
ISSN 0002-7863
1520-5126
Publication date 2014-03-19
Year available 2014
Sub-type Article (original research)
DOI 10.1021/ja500432h
Open Access Status DOI
Volume 136
Issue 11
Start page 4394
End page 4403
Total pages 10
Place of publication Washington, DC, United States
Publisher American Chemical Society
Language eng
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.
Keyword Chemistry, Multidisciplinary
Chemistry
CHEMISTRY, MULTIDISCIPLINARY
Q-Index Code C1
Q-Index Status Confirmed Code
Grant ID DP130104459
Institutional Status UQ

Document type: Journal Article
Sub-type: Article (original research)
Collections: Official 2015 Collection
Australian Institute for Bioengineering and Nanotechnology Publications
 
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