The DOI matches its Crossref record; 53 of the 53 references it cites were found in a registry or an index.
Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N3 as an Active Site for the Oxygen Reduction Reaction
Abstract
Atomically dispersed M-N-C (M refers to transition metals) materials represent the most promising catalyst alternatives to the precious metal Pt for the electrochemical reduction of oxygen (ORR), yet the genuine active sites in M-N-C remain elusive. Here, we develop a two-step approach to fabricate Cu-N-C single-atom catalysts with a uniform and well-defined Cu 2+ -N 4 structure that exhibits comparable activity and superior durability in comparison to Pt/C. By combining operando X-ray absorption spectroscopy with theoretical calculations, we unambiguously identify the dynamic evolution of Cu-N 4 to Cu-N 3 and further to HO-Cu-N 2 under ORR working conditions, which concurrently occurs with reduction of Cu 2+ to Cu + and is driven by the applied potential. The increase in the Cu + /Cu 2+ ratio with the reduced potential indicates that the low-coordinated Cu + -N 3 is the real active site, which is further supported by DFT calculations showing the lower free energy in each elemental step of the ORR on Cu + -N 3 than on Cu 2+ -N 4 . These findings provide a new understanding of the dynamic electrochemistry on M-N-C catalysts and may guide the design of more efficient low-cost catalysts.
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Cites
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Self-citationHigh-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
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Self-citationReview of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)
Song, W., Xiao, C., Ding, J., Huang, Z., Yang, X., Zhang, T., Mitlin, D., & Hu, W. (2024) · Advanced Materials · doi:10.1002/adma.202301477 · Cited by 373
Self-citationHu, X., Chen, S., Chen, L., Tian, Y., Yao, S., Lu, Z., Zhang, X., & Zhou, Z. (2022) · Journal of the American Chemical Society · doi:10.1021/jacs.2c08743 · Cited by 322
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Metadata
- Authors
- Yang, J., Liu, W., Xu, M., Liu, X., Qi, H., Zhang, L., Yang, X., Niu, S., Zhou, D., Liu, Y., Su, Y., Li, J.-F., Tian, Z.-Q., Zhou, W., Wang, A., & Zhang, T.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2021-08-31
- Volume
- 143
- Issue
- 36
- Pages
- 14530-14539
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W3197855596
- Cited by
- 512
- References
- 53
- FWCI
- 14.37
- Type
- journal article
- Language
- en
- Open access
- closed
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- Yang, J., Liu, W., Xu, M., Liu, X., Qi, H., Zhang, L., Yang, X., Niu, S., Zhou, D., Liu, Y., Su, Y., Li, J.-F., Tian, Z.-Q., Zhou, W., Wang, A., & Zhang, T. (2021). Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N3 as an Active Site for the Oxygen Reduction Reaction. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.1c03788
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