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Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature

Jia-Yi Fang, Qi-Zheng Zheng, Yao-Yin Lou (), Kuang-Min Zhao, Sheng-Nan Hu, Guang Li, Ouardia Akdim, Xiao-Yang Huang and Shi-Gang Sun ()
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Jia-Yi Fang: Xiamen University
Qi-Zheng Zheng: Xiamen University
Yao-Yin Lou: Xiamen University
Kuang-Min Zhao: Xiamen University
Sheng-Nan Hu: Xiamen University
Guang Li: Xiamen University
Ouardia Akdim: Cardiff University
Xiao-Yang Huang: Xiamen University
Shi-Gang Sun: Xiamen University

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

Abstract: Abstract The development of electrocatalysts capable of efficient reduction of nitrate (NO3−) to ammonia (NH3) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO2− via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NOx− adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm−2 at −0.2 V vs. Reversible Hydrogen Electrode. The NH3 production rate reaches a high activity of 4.8 mmol cm−2 h−1 (960 mmol gcat−1 h−1). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO3− to NH3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO3 led simultaneously to high NH3 selectivity and yield.

Date: 2022
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DOI: 10.1038/s41467-022-35533-6

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