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Kaiwen Yang, Shuhe Han, Chuanqi Cheng, Chengying Guo, Tieliang Li, Yifu Yu
Electrocatalytic reduction of nitrate to ammonia (NRA) has emerged as an alternative strategy for sewage treatment and ammonia generation. Despite excellent performances having been achieved over cobalt-based electrocatalysts, the reaction mechanism as well as veritable active species across a wide potential range are still full of controversy. Here, we adopt CoP, Co, and Co 3 O 4 as model materials to solve these issues. CoP evolves into a core@shell structured CoP@Co before NRA. For CoP@Co and Co catalysts, a three-step relay mechanism is carried out over superficial dynamical Co δ+ active species under low overpotential, while a continuous hydrogenation mechanism from nitrate to ammonia is unveiled over superficial Co species under high overpotential. In comparison, Co 3 O 4 species are stable and steadily catalyze nitrate hydrogenation to ammonia across a wide potential range. As a result, CoP@Co and Co exhibit much higher NRA activity than Co 3 O 4 especially under a low overpotential. Moreover, the NRA performance of CoP@Co is higher than Co although they experience the same reaction mechanism. A series of characterizations clarify the reason for performance enhancement highlighting that CoP core donates abundant electrons to superficial active species, leading to the generation of more active hydrogen for the reduction of nitrogen-containing intermediates.
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Yang, K., Han, S., Cheng, C., Guo, C., Li, T., & Yu, Y. (2024). Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts. Journal of the American Chemical Society, 146(19), 12976–12983. https://doi.org/10.1021/jacs.3c13517
Yang, Kaiwen, et al. "Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts." Journal of the American Chemical Society, vol. 146, no. 19, 2024, pp. 12976–12983, https://doi.org/10.1021/jacs.3c13517.
Yang, Kaiwen, Shuhe Han, Chuanqi Cheng, Chengying Guo, Tieliang Li, and Yifu Yu. "Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts." Journal of the American Chemical Society 146, no. 19 (2024): 12976–12983. https://doi.org/10.1021/jacs.3c13517.
Yang K., Han S., Cheng C. [и др.] Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts // Journal of the American Chemical Society. — 2024. — Vol. 146, № 19. — P. 12976–12983. — URL: https://doi.org/10.1021/jacs.3c13517
@article{yang2024unveiling,
title = {{Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts}},
author = {Kaiwen Yang and Shuhe Han and Chuanqi Cheng and Chengying Guo and Tieliang Li and Yifu Yu},
journal = {Journal of the American Chemical Society},
year = {2024},
volume = {146},
number = {19},
pages = {12976--12983},
doi = {10.1021/jacs.3c13517},
url = {https://doi.org/10.1021/jacs.3c13517}
}TY - JOUR AU - Yang, Kaiwen AU - Han, Shuhe AU - Cheng, Chuanqi AU - Guo, Chengying AU - Li, Tieliang AU - Yu, Yifu TI - Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts JO - Journal of the American Chemical Society VL - 146 IS - 19 SP - 12976 EP - 12983 PY - 2024 DA - 2024/04/03 DO - 10.1021/jacs.3c13517 UR - https://doi.org/10.1021/jacs.3c13517 ER -
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