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Qikun Hu, Ke Yang, Ouwen Peng, Minzhang Li, Lu Ma, Songpeng Huang, Yonghua Du, Zong‐Xiang Xu, Qing Wang, Zhongxin Chen, Ming Yang, Kian Ping Loh
Electrochemical synthesis of ammonia via the nitrate reduction reaction (NO3RR) has been intensively researched as an alternative to the traditional Haber–Bosch process. Most research focuses on the low concentration range representative of the nitrate level in wastewater, leaving the high concentration range, which exists in nuclear and fertilizer wastes, unexplored. The use of a concentrated electrolyte (≥1 M) for higher rate production is hampered by poor hydrogen transfer kinetics. Herein, we demonstrate that a cocatalytic system of Ru/Cu 2 O catalyst enables NO3RR at 10.0 A in 1 M nitrate electrolyte in a 16 cm 2 flow electrolyzer, with 100% faradaic efficiency toward ammonia. Detailed mechanistic studies by deuterium labeling and operando Fourier transform infrared (FTIR) spectroscopy allow us to probe the hydrogen transfer rate and intermediate species on Ru/Cu 2 O. Ab initio molecular dynamics (AIMD) simulations reveal that adsorbed hydroxide on Ru nanoparticles increases the density of the hydrogen-bonded water network near the Cu 2 O surface, which promotes the hydrogen transfer rate. Our work highlights the importance of engineering synergistic interactions in cocatalysts for addressing the kinetic bottleneck in electrosynthesis.
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Hu, Q., Yang, K., Peng, O., Li, M., Ma, L., Huang, S., Du, Y., Xu, Z., Wang, Q., Chen, Z., Yang, M., & Loh, K. P. (2023). Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study. Journal of the American Chemical Society, 146(1), 668–676. https://doi.org/10.1021/jacs.3c10516
Hu, Qikun, et al. "Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study." Journal of the American Chemical Society, vol. 146, no. 1, 2023, pp. 668–676, https://doi.org/10.1021/jacs.3c10516.
Hu, Qikun, Ke Yang, Ouwen Peng, Minzhang Li, Lu Ma, Songpeng Huang, Yonghua Du, et al. "Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study." Journal of the American Chemical Society 146, no. 1 (2023): 668–676. https://doi.org/10.1021/jacs.3c10516.
Hu Q., Yang K., Peng O. [и др.] Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study // Journal of the American Chemical Society. — 2023. — Vol. 146, № 1. — P. 668–676. — URL: https://doi.org/10.1021/jacs.3c10516
@article{hu2023ammonia,
title = {{Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study}},
author = {Qikun Hu and Ke Yang and Ouwen Peng and Minzhang Li and Lu Ma and Songpeng Huang and Yonghua Du and Zong‐Xiang Xu and Qing Wang and Zhongxin Chen and Ming Yang and Kian Ping Loh},
journal = {Journal of the American Chemical Society},
year = {2023},
volume = {146},
number = {1},
pages = {668--676},
doi = {10.1021/jacs.3c10516},
url = {https://doi.org/10.1021/jacs.3c10516}
}TY - JOUR AU - Hu, Qikun AU - Yang, Ke AU - Peng, Ouwen AU - Li, Minzhang AU - Ma, Lu AU - Huang, Songpeng AU - Du, Yonghua AU - Xu, Zong‐Xiang AU - Wang, Qing AU - Chen, Zhongxin AU - Yang, Ming AU - Loh, Kian Ping TI - Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study JO - Journal of the American Chemical Society VL - 146 IS - 1 SP - 668 EP - 676 PY - 2023 DA - 2023/12/28 DO - 10.1021/jacs.3c10516 UR - https://doi.org/10.1021/jacs.3c10516 ER -
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