In situ construction of Cu(I)-Cu(II) pairs for efficient electrocatalytic nitrate reduction reaction to ammonia - Details

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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　(−1　gcat.−1).　This　work　may　open　a　new　avenue　for　effective　NO3−RR　by　modulating　oxidation　states.　©　2024　Science　Press

Keyword：

Ammonia Electrolysis Electrolytic reduction Green Synthesis Nitrates Oxygen reduction reaction

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[ 1 ] [Zheng, Muyun]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 2 ] [Wan, Yuchi]Institute of New Energy Materials and Engineering, School of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou; 350108, China
[ 3 ] [Yang, Leping]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 4 ] [Ao, Shen]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 5 ] [Fu, Wangyang]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 6 ] [Fu, Wangyang]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 7 ] [Zhang, Zhengjun]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 8 ] [Zhang, Zhengjun]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 9 ] [Huang, Zheng-Hong]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 10 ] [Huang, Zheng-Hong]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 11 ] [Ling, Tao]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, Feiyu]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 13 ] [Kang, Feiyu]Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 14 ] [Lv, Ruitao]State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing; 100084, China
[ 15 ] [Lv, Ruitao]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

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SCOPUS Cited Count： 2

ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 4

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