Origin of the Electrocatalytic Oxygen Reduction Activity of Graphene-Based Catalysts: A Roadmap to Achieve the Best Performance.
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...
| Publicado en: | Journal of the American Chemical Society Vol. 136; no. 11; pp. 4394 - 4404 |
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| Autores principales: | , , , |
| Formato: | Artículo |
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American Chemical Society
3/19/2014
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| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=95469694&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 95469694 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 3/19/2014 vid: 136 iid: 11 pid: 997 pub: American Chemical Society artinfo: ui: 95469694 10.1021/ja500432h ppf: 4394 ppct: 10 formats: tig: atl: Origin of the Electrocatalytic Oxygen Reduction Activity of Graphene-Based Catalysts: A Roadmap to Achieve the Best Performance. aug: au: Yan Jiao Yao Zheng Jaroniec, Mietek Shi Zhang Qiao affil: School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, Australia Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane,Queensland 4067, Australia Department of Chemistry and Biochemistry, Kent State University, Kent, Ohio 44242, United States su: Electrochemical research Density functional theory Graphene Electrocatalysts Oxygen reduction Catalysts Chemical research sug: subj: Electrochemical research Density functional theory Graphene Electrocatalysts Oxygen reduction Catalysts Chemical research ab: 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. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2014 holdings: @attributes: islocal: N |
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