Selective electrosynthesis of hydroxylamine from aqueous nitrate/nitrite by suppressing further reduction

Yirong Tang, Zhan Jiang (), Yubo Yuan, Li Xu, Chuyao Jin, Bulin Chen, Zhichao Lin, Jie Zao, Jianwei Du, Xiao Zhang (), Xiang Gao () and Yongye Liang ()
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Yirong Tang: Southern University of Science and Technology
Zhan Jiang: Southern University of Science and Technology
Yubo Yuan: Southern University of Science and Technology
Li Xu: State Environmental Protection Center for Coal-Fired Air Pollution Control
Chuyao Jin: State Environmental Protection Center for Coal-Fired Air Pollution Control
Bulin Chen: Southern University of Science and Technology
Zhichao Lin: Southern University of Science and Technology
Jie Zao: Southern University of Science and Technology
Jianwei Du: Ministry of Ecology and Environment
Xiao Zhang: State Environmental Protection Center for Coal-Fired Air Pollution Control
Xiang Gao: State Environmental Protection Center for Coal-Fired Air Pollution Control
Yongye Liang: Southern University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract The electrocatalytic reduction of nitrogenous waste offers a sustainable approach to producing nitrogen-containing chemicals. The selective synthesis of high-value hydroxylamine (NH2OH) is challenging due to the instability of NH2OH as an intermediate. Here, we present a rational electrocatalyst design strategy for promoting NH2OH electrosynthesis by suppressing the competing pathways of further reduction. We screen zinc phthalocyanines (ZnPc) with a high energy barrier for NH2OH reduction by regulating their intrinsic activity. Additionally, we discover that carbon nanotube substrates exhibit significant NH3-producing activity, which can be effectively inhibited by the high coverage of ZnPc molecules. In-situ characterizations reveal that NH2OH and HNO are generated as intermediates in nitrate reduction to NH3, and NH2OH can be enriched in the ZnPc electrode. In the H-cell, the optimized ZnPc catalyst demonstrates a Faradaic efficiency (FE) of 53 ± 1.7% for NH2OH with a partial current density exceeding 270 mA cm−2 and a turnover frequency of 7.5 ± 0.2 s−1. It also enables the rapid electrosynthesis of cyclohexanone oxime from nitrite with a FE of 64 ± 1.0%.

Date: 2024
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DOI: 10.1038/s41467-024-54204-2

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