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Jingwen Xu, Shengbo Zhang, Hengjie Liu, Shuang Liu, Yuan Yuan, Yahan Meng, Mingming Wang, Chunyue Shen, Qia Peng, Jinghao Chen and 4 more
The electrochemical conversion of nitrate pollutants into value‐added ammonia is a feasible way to achieve artificial nitrogen cycle. However, the development of electrocatalytic nitrate‐to‐ammonia reduction reaction (NO 3 − RR) has been hampered by high overpotential and low Faradaic efficiency. Here we develop an iron single‐atom catalyst coordinated with nitrogen and phosphorus on hollow carbon polyhedron (denoted as Fe−N/P−C) as a NO 3 − RR electrocatalyst. Owing to the tuning effect of phosphorus atoms on breaking local charge symmetry of the single‐Fe‐atom catalyst, it facilitates the adsorption of nitrate ions and enrichment of some key reaction intermediates during the NO 3 − RR process. The Fe−N/P−C catalyst exhibits 90.3 % ammonia Faradaic efficiency with a yield rate of 17980 μg h −1 mg cat −1 , greatly outperforming the reported Fe‐based catalysts. Furthermore, operando SR‐FTIR spectroscopy measurements reveal the reaction pathway based on key intermediates observed under different applied potentials and reaction durations. Density functional theory calculations demonstrate that the optimized free energy of NO 3 − RR intermediates is ascribed to the asymmetric atomic interface configuration, which achieves the optimal electron density distribution. This work demonstrates the critical role of atomic‐level precision modulation by heteroatom doping for the NO 3 − RR, providing an effective strategy for improving the catalytic performance of single atom catalysts in different electrochemical reactions.
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Xu, J., Zhang, S., Liu, H., Liu, S., Yuan, Y., Meng, Y., Wang, M., Shen, C., Peng, Q., Chen, J., Wang, X., Song, L., Li, K., & Chen, W. (2023). Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia. Angewandte Chemie International Edition, 62(39), e202308044. https://doi.org/10.1002/anie.202308044
Xu, Jingwen, et al. "Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia." Angewandte Chemie International Edition, vol. 62, no. 39, 2023, pp. e202308044, https://doi.org/10.1002/anie.202308044.
Xu, Jingwen, Shengbo Zhang, Hengjie Liu, Shuang Liu, Yuan Yuan, Yahan Meng, Mingming Wang, et al. "Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia." Angewandte Chemie International Edition 62, no. 39 (2023): e202308044. https://doi.org/10.1002/anie.202308044.
Xu J., Zhang S., Liu H. [и др.] Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia // Angewandte Chemie International Edition. — 2023. — Vol. 62, № 39. — P. e202308044. — URL: https://doi.org/10.1002/anie.202308044
@article{xu2023breaking,
title = {{Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia}},
author = {Jingwen Xu and Shengbo Zhang and Hengjie Liu and Shuang Liu and Yuan Yuan and Yahan Meng and Mingming Wang and Chunyue Shen and Qia Peng and Jinghao Chen and Xiaoyang Wang and Li Song and Ke Li and Wei Chen},
journal = {Angewandte Chemie International Edition},
year = {2023},
volume = {62},
number = {39},
pages = {e202308044},
doi = {10.1002/anie.202308044},
url = {https://doi.org/10.1002/anie.202308044}
}TY - JOUR AU - Xu, Jingwen AU - Zhang, Shengbo AU - Liu, Hengjie AU - Liu, Shuang AU - Yuan, Yuan AU - Meng, Yahan AU - Wang, Mingming AU - Shen, Chunyue AU - Peng, Qia AU - Chen, Jinghao AU - Wang, Xiaoyang AU - Song, Li AU - Li, Ke AU - Chen, Wei TI - Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia JO - Angewandte Chemie International Edition VL - 62 IS - 39 SP - e202308044 PY - 2023 DA - 2023/07/22 DO - 10.1002/anie.202308044 UR - https://doi.org/10.1002/anie.202308044 ER -
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