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Electrocatalytic nitrate reduction reaction (NO3−RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues. We report a CuO nanoparticles incorporated on nitrogen-doped porous carbon (CuO@NC) catalyst for NO3−RR. Part of Cu(II) is reduced to Cu(I) during the NO3−RR process to construct Cu(I)-Cu(II) pairs, confirmed by in situ X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Density functional theory (DFT) calculations indicated that the formation of Cu(I) could provide a reaction path with smaller energy barrier for NO3−RR, while Cu(II) effectively suppressed the competition of hydrogen evolution reaction (HER). As a result, CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at −0.49 V versus reversible hydrogen electrode (RHE), and a NH3 yield rate of 17.2 mg h−1 mgcat.−1 at −0.79 V vs. RHE, higher than the Haber-Bosch process (<3.4 g h−1 gcat.−1). This work may open a new avenue for effective NO3−RR by modulating oxidation states. © 2024 Science Press
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Journal of Energy Chemistry
ISSN: 2095-4956
Year: 2025
Volume: 100
Page: 106-113
1 4 . 0 0 0
JCR@2023
Cited Count:
SCOPUS Cited Count: 2
ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 6
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