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Ji Yang, Haifeng Qi, Anqi Li, Xiaoyan Liu, Xiaofeng Yang, Shengxin Zhang, Qiao Ling Zhao, Qike Jiang, Yang Su, Leilei Zhang and 5 more
Restructuring is ubiquitous in thermocatalysis and of pivotal importance to identify the real active site, yet it is less explored in electrocatalysis. Herein, by using operando X-ray absorption spectroscopy in conjunction with advanced electron microscopy, we reveal the restructuring of the as-synthesized Cu–N 4 single-atom site to the nanoparticles of ∼5 nm during the electrochemical reduction of nitrate to ammonia, a green ammonia production route upon combined with the plasma-assisted oxidation of nitrogen. The reduction of Cu 2+ to Cu + and Cu 0 and the subsequent aggregation of Cu 0 single atoms is found to occur concurrently with the enhancement of the NH 3 production rate, both of them are driven by the applied potential switching from 0.00 to −1.00 V versus RHE. The maximum production rate of ammonia reaches 4.5 mg cm –2 h –1 (12.5 mol NH 3 g Cu –1 h –1 ) with a Faradaic efficiency of 84.7% at −1.00 V versus RHE, outperforming most of the other Cu catalysts reported previously. After electrolysis, the aggregated Cu nanoparticles are reversibly disintegrated into single atoms and then restored to the Cu–N 4 structure upon being exposed to an ambient atmosphere, which masks the potential-induced restructuring during the reaction. The synchronous changes of the Cu 0 percentage and the ammonia Faradaic efficiency with the applied potential suggests that the Cu nanoparticles are the genuine active sites for nitrate reduction to ammonia, which is corroborated with both the post-deposited Cu NP catalyst and density functional theory calculations.
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Yang, J., Qi, H., Li, A., Liu, X., Yang, X., Zhang, S., Zhao, Q. L., Jiang, Q., Su, Y., Zhang, L., Li, J., Tian, Z., Liu, W., Wang, A., & Zhang, T. (2022). Potential-Driven Restructuring of Cu Single Atoms to Nanoparticles for Boosting the Electrochemical Reduction of Nitrate to Ammonia. Journal of the American Chemical Society, 144(27), 12062–12071. https://doi.org/10.1021/jacs.2c02262
Yang, Ji, et al. "Potential-Driven Restructuring of Cu Single Atoms to Nanoparticles for Boosting the Electrochemical Reduction of Nitrate to Ammonia." Journal of the American Chemical Society, vol. 144, no. 27, 2022, pp. 12062–12071, https://doi.org/10.1021/jacs.2c02262.
Yang, Ji, Haifeng Qi, Anqi Li, Xiaoyan Liu, Xiaofeng Yang, Shengxin Zhang, Qiao Ling Zhao, et al. "Potential-Driven Restructuring of Cu Single Atoms to Nanoparticles for Boosting the Electrochemical Reduction of Nitrate to Ammonia." Journal of the American Chemical Society 144, no. 27 (2022): 12062–12071. https://doi.org/10.1021/jacs.2c02262.
Yang J., Qi H., Li A. [и др.] Potential-Driven Restructuring of Cu Single Atoms to Nanoparticles for Boosting the Electrochemical Reduction of Nitrate to Ammonia // Journal of the American Chemical Society. — 2022. — Vol. 144, № 27. — P. 12062–12071. — URL: https://doi.org/10.1021/jacs.2c02262
@article{yang2022potentialdriven,
title = {{Potential-Driven Restructuring of Cu Single Atoms to Nanoparticles for Boosting the Electrochemical Reduction of Nitrate to Ammonia}},
author = {Ji Yang and Haifeng Qi and Anqi Li and Xiaoyan Liu and Xiaofeng Yang and Shengxin Zhang and Qiao Ling Zhao and Qike Jiang and Yang Su and Leilei Zhang and Jian‐Feng Li and Zhong‐Qun Tian and Wei Liu and Aiqin Wang and Tao Zhang},
journal = {Journal of the American Chemical Society},
year = {2022},
volume = {144},
number = {27},
pages = {12062--12071},
doi = {10.1021/jacs.2c02262},
url = {https://doi.org/10.1021/jacs.2c02262}
}TY - JOUR AU - Yang, Ji AU - Qi, Haifeng AU - Li, Anqi AU - Liu, Xiaoyan AU - Yang, Xiaofeng AU - Zhang, Shengxin AU - Zhao, Qiao Ling AU - Jiang, Qike AU - Su, Yang AU - Zhang, Leilei AU - Li, Jian‐Feng AU - Tian, Zhong‐Qun AU - Liu, Wei AU - Wang, Aiqin AU - Zhang, Tao TI - Potential-Driven Restructuring of Cu Single Atoms to Nanoparticles for Boosting the Electrochemical Reduction of Nitrate to Ammonia JO - Journal of the American Chemical Society VL - 144 IS - 27 SP - 12062 EP - 12071 PY - 2022 DA - 2022/06/29 DO - 10.1021/jacs.2c02262 UR - https://doi.org/10.1021/jacs.2c02262 ER -
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