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The DOI matches its Crossref record; 6 of the 6 references it cites were found in a registry or an index.

Activity Descriptor Identification for Oxygen Reduction on Nonprecious Electrocatalysts: Linking Surface Science to Coordination Chemistry

Ramaswamy, Nagappan, Tylus, Urszula, Jia, Qingying, Mukerjee, Sanjeev·2013·Journal of the American Chemical Society

Abstract

Developing nonprecious group metal based electrocatalysts for oxygen reduction is crucial for the commercial success of environmentally friendly energy conversion devices such as fuel cells and metal-air batteries. Despite recent progress, elegant bottom-up synthesis of nonprecious electrocatalysts (typically Fe-N(x)/C) is unavailable due to lack of fundamental understanding of molecular governing factors. Here, we elucidate the mechanistic origin of oxygen reduction on pyrolyzed nonprecious catalysts and identify an activity descriptor based on principles of surface science and coordination chemistry. A linear relationship, depicting the ascending portion of a volcano curve, is established between oxygen-reduction turnover number and the Lewis basicity of graphitic carbon support (accessed via C 1s photoemission spectroscopy). Tuning electron donating/withdrawing capability of the carbon basal plane, conferred upon it by the delocalized π-electrons, (i) causes a downshift of e(g)-orbitals (d(z(2))) thereby anodically shifting the metal ion's redox potential and (ii) optimizes the bond strength between the metal ion and adsorbed reaction intermediates thereby maximizing oxygen-reduction activity.

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Crossref · 10.1021/ja405149m

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Metadata

Authors
Ramaswamy, N., Tylus, U., Jia, Q., & Mukerjee, S.
Venue
Journal of the American Chemical Society
Published
2013-10-02
Volume
135
Issue
41
Pages
15443-15449
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
OpenAlex
W2329247413
Cited by
882
References
6
FWCI
15.39
Type
journal article
Language
en
Open access
closed

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Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).

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