Steering the catalyst structure and intermediates adsorption configuration during pulsed nitrate electroreduction

Limin Wu, Shunhan Jia, Ruhan Wang, Jiaqi Feng, Libing Zhang, Hanle Liu, Xing Tong, Rongjuan Feng, Xinchen Kang, Qinggong Zhu, Qingli Qian, Liang Xu (), Xiaofu Sun () and Buxing Han ()
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Limin Wu: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Shunhan Jia: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Ruhan Wang: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Jiaqi Feng: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Libing Zhang: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Hanle Liu: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Xing Tong: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Rongjuan Feng: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Xinchen Kang: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Qinggong Zhu: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Qingli Qian: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Liang Xu: Beijing University of Chemical Technology, College of Chemical Engineering
Xiaofu Sun: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry
Buxing Han: Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract The electroreduction of nitrate (NO3−) offers a promising pathway for carbon−free NH3 production and nitrogen cycle management. Pulsed NO3− electroreduction has demonstrated to enable the improvement of catalytic performance, but the underlying mechanisms remain little understood. Herein, we tune the Cu catalyst structure and steer the key N−containing intermediate adsorption configuration during pulsed NO3− electroreduction. By applying different positive and negative potentials, in situ dynamic restructuring of the Cu catalyst and the regulation of local microenvironment have been revealed. According to detailed in situ characterizations and theoretical calculations, periodic Cu oxidation occurs within specific potential ranges from −0.2 V to 0.2 V vs. saturated Ag/AgCl, facilitating the transition of *NO adsorption configuration and thereby enhancing NH3 formation. It can also increase NO2− coverage on Cu surface and inhibit side reactions. Conversely, the enhanced catalytic preformation in potential ranges from −1.2 V to −0.2 V was only attributed to the intrinsic characteristics of pulsed electrolysis. This study not only reveals the in−depth understanding of pulsed NO3− electrolysis, but also offers a general way of optimizing other electrocatalytic reactions.

Date: 2025
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DOI: 10.1038/s41467-025-65391-x

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