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
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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Cites
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High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
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Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
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Varcoe, J. R., Atanassov, P., Dekel, D. R., Herring, A. M., Hickner, M. A., Kohl, P. A., Kucernak, A. R., Mustain, W. E., Nijmeijer, K., Scott, K., et al. (2014) · Energy Environ. Sci. · doi:10.1039/c4ee01303d · Cited by 2,051
Wu, G., Santandreu, A., Kellogg, W., Gupta, S., Ogoke, O., Zhang, H., Wang, H.-L., & Dai, L. (2016) · Nano Energy · doi:10.1016/j.nanoen.2015.12.032 · Cited by 744
Single atom electrocatalysts supported on graphene or graphene-like carbons
Fei, H., Dong, J., Chen, D., Hu, T., Duan, X., Shakir, I., Huang, Y., & Duan, X. (2019) · Chemical Society Reviews · doi:10.1039/c9cs00422j · Cited by 673
Design Strategies toward Advanced MOF‐Derived Electrocatalysts for Energy‐Conversion Reactions
Liu, J., Zhu, D., Guo, C., Vasileff, A., & Qiao, S. (2017) · Advanced Energy Materials · doi:10.1002/aenm.201700518 · Cited by 668
Reactivity Descriptors for the Activity of Molecular MN4 Catalysts for the Oxygen Reduction Reaction
Zagal, J. H., & Koper, M. T. M. (2016) · Angewandte Chemie International Edition · doi:10.1002/anie.201604311 · Cited by 587
Metadata
- Authors
- Ramaswamy, N., Tylus, U., Jia, Q., & Mukerjee, S.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- 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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