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Electrochemical nitrate reduction reaction (NO3RR) is a promising means for generating the energy carrier ammonia. Herein, we report the synthesis of heterostructure copper-nickel phosphide electrocatalysts via a simple vapor-phase hydrothermal method. The resultant catalysts were evaluated for electrocatalytic nitrate reduction to ammonia (NH3) in three-type electrochemical reactors. In detail, the regulation mechanism of the heterogeneous Cu3P-Ni2P/CP-x for NO3RR performance was systematically studied through the H-type cell, rotating disk electrode setup, and membrane-electrode-assemblies (MEA) electrolyzer. As a result, the Cu3P-Ni2P/CP-0.5 displays the practicability in an MEA system with an anion exchange membrane, affording the largest ammonia yield rate (RNH3) of 1.9 mmol·h−1·cm−2, exceeding most of the electrocatalytic nitrate reduction electrocatalysts reported to date. The theoretical calculations and in-situ spectroscopy characterizations uncover that the formed heterointerface in Cu3P-Ni2P/CP is beneficial for promoting nitrate adsorption, activation, and conversion to ammonia through the successive hydrodeoxygenation pathway.

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Acknowledgements

Publication history

Received: 16 November 2023
Revised: 21 December 2023
Accepted: 06 January 2024
Published: 08 February 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This work was financially supported by the postdoctoral researcher funding project of Anhui Province (No. 2022B585), the HFIPS Director’s Fund (No. YZJJ2023QN29), the National Natural Science Foundation of China (No. 52172106), and the Special Research Assistant Program, Chinese Academy of Sciences.

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