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Atomic Tuning of Single-Atom Fe–N–C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction

Li, Ke, Zhang, Shengbo, Zhang, Xiuli, Liu, Shuang, Jiang, Haosong, Jiang, Taoli, Shen, Chunyue, Yu, Yi, Chen, Wei·2022·Nano Letters

Abstract

The electrochemical reduction of CO 2 to produce carbon-based fuels and chemicals possesses huge potentials to alleviate current environmental problems. However, it is confronted by great challenges in the design of active electrocatalysts with low overpotentials and high product selectivity. Here we report the atomic tuning of a single-Fe-atom catalyst with phosphorus (Fe–N/P–C) on commercial carbon black as a robust electrocatalyst for CO 2 reduction. The Fe–N/P–C catalyst exhibits impressive performance in the electrochemical reduction of CO 2 to CO, with a high Faradaic efficiency of 98% and a high mass-normalized turnover frequency of 508.8 h –1 at a low overpotential of 0.34 V. On the basis of ex-situ X-ray absorption spectroscopy measurements and DFT calculations, we reveal that the tuning of P in single-Fe-atom catalysts reduces the oxidation state of the Fe center and decreases the free-energy barrier of *CO intermediate formation, consequently maintaining the electrocatalytic activity and stability of single-Fe-atom catalysts.

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Metadata

Authors
Li, K., Zhang, S., Zhang, X., Liu, S., Jiang, H., Jiang, T., Shen, C., Yu, Y., & Chen, W.
Venue
Nano Letters
Published
2022-02-01
Volume
22
Issue
4
Pages
1557-1565
ISSN
  • 1530-6984 (ISSN-L)
  • 1530-6992
OpenAlex
W4210407942
Cited by
278
References
7
FWCI
10.52
Type
journal article
Language
en
Open access
closed

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CoChat. (2026). Citation check: Atomic Tuning of Single-Atom Fe–N–C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction. https://app.cochat.ai/papers/10.1021/acs.nanolett.1c04382
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Li, K., Zhang, S., Zhang, X., Liu, S., Jiang, H., Jiang, T., Shen, C., Yu, Y., & Chen, W. (2022). Atomic Tuning of Single-Atom Fe–N–C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction. Nano Letters. https://doi.org/10.1021/acs.nanolett.1c04382

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