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Electrocatalytic ammonia oxidation reaction (EAOR) provides an ideal solution for on-board hydrogen supply for fuel cells, while the lack of efficient and durable EAOR catalysts has been a long-standing obstacle for its practical application. Herein, we reported that the defect engineering via in-situ electrochemically introducing oxygen vacancies (Vo) not only turns the inactive CuO into efficient EAOR catalyst but also achieves a high stability of over 400 h at a high current density of ~ 200 mA·cm−2. Theoretical simulation reveals that the presence of Vo on the CuO surface induces a remarkable upshift of the d-band center of active Cu site closer to the Fermi level, which significantly stabilizes the reaction intermediates (*NHx) and efficiently oxidizes NH3 into N2. This Vo-modulated CuO shows a different catalytic mechanism from that on the conventional Pt-based catalysts, paving a new avenue to develop inexpensive, efficient, and robust catalysts, not limited to EAOR.

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Publication history
Copyright
Acknowledgements

Publication history

Received: 01 January 2022
Revised: 26 February 2022
Accepted: 27 February 2022
Published: 30 April 2022
Issue date: July 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by Westlake Education Foundation. The authors thank Prof. Qiyang Lu for his useful suggestions on characterization of oxygen vacancies. The authors thank Micro/Nano Fabrication Center, the Instrumentation and Service Center for Physical Sciences (ISCPS) Center and the Instrumentation and Service Center for Molecular Sciences (ISCMS) Center of Westlake University for characterization support, and Westlake High-Performance Computing Center (Westlake HPC Center) for computation support.

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