Active hydrogen boosts electrochemical nitrate reduction to ammonia

Kui Fan, Wenfu Xie, Jinze Li, Yining Sun, Pengcheng Xu, Yang Tang, Zhenhua Li and Mingfei Shao ()
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Kui Fan: Beijing University of Chemical Technology
Wenfu Xie: Beijing University of Chemical Technology
Jinze Li: Beijing University of Chemical Technology
Yining Sun: Beijing University of Chemical Technology
Pengcheng Xu: Beijing University of Chemical Technology
Yang Tang: Beijing University of Chemical Technology
Zhenhua Li: Beijing University of Chemical Technology
Mingfei Shao: Beijing University of Chemical Technology

Nature Communications, 2022, vol. 13, issue 1, 1-13

Abstract: Abstract Electrochemical nitrate reduction to ammonia is a promising alternative strategy to the traditional Haber-Bosch process but suffers from a low Faradaic efficiency and limited ammonia yield due to the sluggish multi-electron/proton-involved steps. Herein, we report a typical hollow cobalt phosphide nanosphere electrocatalyst assembled on a self-supported carbon nanosheet array synthesized with a confinement strategy that exhibits an extremely high ammonia yield rate of 8.47 mmol h−1 cm−2 through nitrate reduction reaction, which is highly superior to previously reported values to our knowledge. In situ experiments and theoretical investigations reveal that the dynamic equilibrium between the generation of active hydrogen on cobalt phosphide and its timely consumption by nitrogen intermediates leads to a superior ammonia yield with a high Faradaic efficiency. This unique insight based on active hydrogen equilibrium provides new opportunities for large-scale ammonia production through electrochemical techniques and can be further used for carbon dioxide capture.

Date: 2022
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DOI: 10.1038/s41467-022-35664-w

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