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author:

Zheng, M. (Zheng, M..) [1] | Wan, Y. (Wan, Y..) [2] | Yang, L. (Yang, L..) [3] | Ao, S. (Ao, S..) [4] | Fu, W. (Fu, W..) [5] | Zhang, Z. (Zhang, Z..) [6] | Huang, Z.-H. (Huang, Z.-H..) [7] | Ling, T. (Ling, T..) [8] | Kang, F. (Kang, F..) [9] | Lv, R. (Lv, R..) [10]

Indexed by:

EI Scopus SCIE

Abstract:

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

Keyword:

Ammonia synthesis Cu oxidation state Electrochemistry In situ XPS Nitrate reduction

Community:

  • [ 1 ] [Zheng M.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 2 ] [Wan Y.]Institute of New Energy Materials and Engineering, School of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
  • [ 3 ] [Yang L.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 4 ] [Ao S.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 5 ] [Fu W.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 6 ] [Fu W.]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 7 ] [Zhang Z.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 8 ] [Zhang Z.]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 9 ] [Huang Z.-H.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 10 ] [Huang Z.-H.]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 11 ] [Ling T.]Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin Key Laboratory of Composite and Functional Materials, School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, China
  • [ 12 ] [Kang F.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 13 ] [Kang F.]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 14 ] [Lv R.]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China
  • [ 15 ] [Lv R.]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China

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Source :

Journal of Energy Chemistry

ISSN: 2095-4956

Year: 2025

Volume: 100

Page: 106-113

1 4 . 0 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 2

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 6

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