Interfacial Water Structure Modulation on Unconventional Phase Non‐Precious Metal Alloy Nanostructures for Efficient Nitrate Electroreduction to Ammonia in Neutral Media

Abstract Electrocatalytic nitrate reduction reaction (NO 3 RR) has been recognized as a sustainable route for nitrate removal and value‐added ammonia (NH 3 ) synthesis. Regulating the surface active hydrogen (*H) behavior is crucial but remains a formidable challenge, especially in neutral electrolytes, greatly limiting the highly selective NH 3 formation. Herein, we report the controlled synthesis of heterophase hcp/fcc non‐precious CuNi alloy nanostructures for efficient NH 3 electrosynthesis in neutral media. Significantly, hcp/fcc Cu 10 Ni 90 exhibits excellent performance with NH 3 Faradaic efficiency and yield rate of 98.1% and 57.4 mg h −1 mg cat −1 , respectively. In situ studies suggest that the high proportion of interfacial K + ion hydrated water (K + –H 2 O) on hcp/fcc Cu 10 Ni 90 creates high *H coverage via boosting interfacial water dissociation, enabling the rapid hydrogenation kinetics for NH 3 synthesis. Theoretical calculations reveal that the superior NO 3 RR performance of hcp/fcc Cu 10 Ni 90 originates from both the existence of hcp phase to improve the electroactivity and the high Ni content to guarantee an efficient active hydrogen supply. The strong interaction between Ni and Cu also optimizes the electronic structures of Cu sites to realize fast intermediate conversions with low energy barriers. This work provides a novel strategy to optimize surface *H behavior via tuning interfacial water structure by crystal phase control.

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Publication Details

Journal
Angewandte Chemie
Published
2025-05-05
DOI
https://doi.org/10.1002/ange.202508617
Citations
5
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
Field-Weighted Citation Impact
1.94
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article

Interfacial Water Structure Modulation on Unconventional Phase Non‐Precious Metal Alloy Nanostructures for Efficient Nitrate Electroreduction to Ammonia in Neutral Media

Yuecheng Xiong, Bolong Huang, Wenxin Niu, Jingwen Zhou et al.
5 citations
Angewandte Chemie
Ammonia Synthesis and Nitrogen Reduction
1.94
article

Interfacial Water Structure Modulation on Unconventional Phase Non‐Precious Metal Alloy Nanostructures for Efficient Nitrate Electroreduction to Ammonia in Neutral Media

Yuecheng Xiong, Bolong Huang, Wenxin Niu, Jingwen Zhou, Yubing Hu, Shibo Xi, Chenliang Ye, Fengkun Hao, Yunhao Wang, Zhanxi Fan, Minhua Shao, Mingzi Sun, Guozhi Wang, Jinwen Yin, Yangbo Ma, Pengyi Lu, Qinghua Zhang, Juan Wang, Xiang Meng, Chaohui Wang, Liang Guo, Xixi Wang, Hongming Xu, Fu Liu, Mingzheng Shao, Jie Wang
article en
5 citations

Abstract

Abstract Electrocatalytic nitrate reduction reaction (NO 3 RR) has been recognized as a sustainable route for nitrate removal and value‐added ammonia (NH 3 ) synthesis. Regulating the surface active hydrogen (*H) behavior is crucial but remains a formidable challenge, especially in neutral electrolytes, greatly limiting the highly selective NH 3 formation. Herein, we report the controlled synthesis of heterophase hcp/fcc non‐precious CuNi alloy nanostructures for efficient NH 3 electrosynthesis in neutral media. Significantly, hcp/fcc Cu 10 Ni 90 exhibits excellent performance with NH 3 Faradaic efficiency and yield rate of 98.1% and 57.4 mg h −1 mg cat −1 , respectively. In situ studies suggest that the high proportion of interfacial K + ion hydrated water (K + –H 2 O) on hcp/fcc Cu 10 Ni 90 creates high *H coverage via boosting interfacial water dissociation, enabling the rapid hydrogenation kinetics for NH 3 synthesis. Theoretical calculations reveal that the superior NO 3 RR performance of hcp/fcc Cu 10 Ni 90 originates from both the existence of hcp phase to improve the electroactivity and the high Ni content to guarantee an efficient active hydrogen supply. The strong interaction between Ni and Cu also optimizes the electronic structures of Cu sites to realize fast intermediate conversions with low energy barriers. This work provides a novel strategy to optimize surface *H behavior via tuning interfacial water structure by crystal phase control.

Angewandte ChemieVol. 137(28)
Xihua University (CN), Agency for Science, Technology and Research (SG), Hong Kong Polytechnic University (HK), Applied Science and Technology Research Institute (CN), North China Electric Power University (CN), Tianjin University (CN), City University of Hong Kong (HK), Chinese Academy of Sciences (CN), Hong Kong University of Science and Technology (HK), Changchun Institute of Applied Chemistry (CN), Singapore Institute for Clinical Sciences (SG), City University of Hong Kong, Shenzhen Research Institute (CN), FZU ‒ Institute of Physics of the Academy of Sciences of the Czech Republic (CZ), Guangzhou HKUST Fok Ying Tung Research Institute (CN), Institute of Physics (CN), National Laboratory for Superconductivity (CN), State Key Laboratory of Electroanalytical Chemistry
Openalex Percentile: Top 14%
Ammonia Synthesis and Nitrogen Reduction
1.94
DOISourceOpenAlex
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