Chinese Journal of Catalysis

Chinese Journal of Catalysis ›› 2023, Vol. 52: 196-206.DOI: 10.1016/S1872-2067(23)64506-1

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In situ constructed dynamic Cu/Ce(OH)x interface for nitrate reduction to ammonia with high activity, selectivity and stability

Yong Liua,b, Xiaoli Zhaoa,c, Chang Longd, Xiaoyan Wanga, Bangwei Denga, Kanglu Lie,f, Yanjuan Suna,c, Fan Donga,e,*()   

  1. aYangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313000, Zhejiang, China
    bCollege of Optoelectronic Engineering, Chengdu University of Information Technology, Chengdu 610225, Sichuan, China
    cSchool of Resources and Environment, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China
    dMolecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China
    eResearch Center for Carbon-Neutral Environmental & Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China
    fCollege of Architecture and Environment, Sichuan University, Chengdu 610065, Sichuan, China
  • Received:2023-05-03 Accepted:2023-08-21 Online:2023-09-18 Published:2023-09-25
  • Contact: *E-mail: dfctbu@126.com,dongfan@uestc.edu.cn (F. Dong).
  • Supported by:
    National Key R&D Program of China(2020YFA0710000);National Natural Science Foundation of China(22225606);National Natural Science Foundation of China(22176029);Sichuan Natural Science Foundation for Distinguished Scholars(2021JDJQ0006)

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Abstract:

Electrocatalytic nitrate reduction (NO3‒RR) offers a promising technique for the removal and utilization of nitrate in water. However, the performance of current catalysts is still limited mainly due to the unfavorable interface that largely determines the reaction efficiency and selectivity. Here we present an in situ dynamic reconstruction strategy to enhance the NO3‒RR by constructing Cu/Ce(OH)x catalyst with abundant interfacial active sites. The Cu/Ce(OH)x catalyst was in situ formed through dynamic reconstruction of Cu2Cl(OH)3/Ce(OH)x heterostructure during electrochemical NO3‒RR process. The catalyst exhibits high performance with NO3‒ conversion of 100.0%, NH3 selectivity of 97.8%, NH3 Faradaic efficiency of 99.2% and long stability, which is among the state-of-the-art catalysts in neutral media. Both experimental and theoretical results demonstrate that the Cu and Ce sites at the interface can operate cooperatively to promote the adsorption and activation of NO3‒, and lower the formation energy of key intermediate *HNO. Meanwhile, the hydrogen evolution reaction is also greatly suppressed due to the high H* binding strength at the interface. The strategy can be extended to other catalytic systems and opens a new avenue for the design of efficient electrocatalysts.

Key words: Metal/hydroxide interface, In situ construction, Electrocatalytic nitrate reduction, Ammonia synthesis, Selectivity