Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia

Shuo Zhang, Jianghua Wu, Mengting Zheng, Xin Jin, Zihan Shen, Zhonghua Li, Yanjun Wang, Quan Wang, Xuebin Wang, Hui Wei, Jiangwei Zhang, Peng Wang, Shanqing Zhang, Liyan Yu, Lifeng Dong, Qingshan Zhu (), Huigang Zhang () and Jun Lu ()
Additional contact information
Shuo Zhang: Institute of Process Engineering, Chinese Academy of Sciences
Jianghua Wu: Nanjing University
Mengting Zheng: Griffith University
Xin Jin: Nanjing University
Zihan Shen: Institute of Process Engineering, Chinese Academy of Sciences
Zhonghua Li: Nanjing University
Yanjun Wang: Nanjing University
Quan Wang: Nanjing University
Xuebin Wang: Nanjing University
Hui Wei: Nanjing University
Jiangwei Zhang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences (CAS)
Peng Wang: Nanjing University
Shanqing Zhang: Griffith University
Liyan Yu: Qingdao University of Science and Technology
Lifeng Dong: Qingdao University of Science and Technology
Qingshan Zhu: Institute of Process Engineering, Chinese Academy of Sciences
Huigang Zhang: Institute of Process Engineering, Chinese Academy of Sciences
Jun Lu: Zhejiang University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO3− adsorption on cathode surfaces. Here, we report a Fe/Cu diatomic catalyst on holey nitrogen-doped graphene which exhibits high catalytic activities and selectivity for ammonia production. The catalyst enables a maximum ammonia Faradaic efficiency of 92.51% (−0.3 V(RHE)) and a high NH3 yield rate of 1.08 mmol h−1 mg−1 (at − 0.5 V(RHE)). Computational and theoretical analysis reveals that a relatively strong interaction between NO3− and Fe/Cu promotes the adsorption and discharge of NO3− anions. Nitrogen-oxygen bonds are also shown to be weakened due to the existence of hetero-atomic dual sites which lowers the overall reaction barriers. The dual-site and hetero-atom strategy in this work provides a flexible design for further catalyst development and expands the electrocatalytic techniques for nitrate reduction and ammonia synthesis.

Date: 2023
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DOI: 10.1038/s41467-023-39366-9

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