Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (10): 1755-1762.DOI: 10.1016/S1872-2067(21)63795-6

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La-doped TiO2 nanorods toward boosted electrocatalytic N2-to-NH3 conversion at ambient conditions

Li Lia, Haijun Chena,b, Lei Lib, Baihai Lib, Qianbao Wua, Chunhua Cuia, Biao Denga, Yonglan Luoa, Qian Liua(), Tingshuai Lia, Fang Zhangc, Abdullah M. Asirid, Zhe-Sheng Fengb, Yan Wangb(), Xuping Suna()   

  1. aInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China
    bSchool of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China
    cNational Engineering Research Center for Nanotechnology, Shanghai 200241, China
    dChemistry Department, Faculty of Science & Center of Excellence for Advanced Materials Research, King Abdulaziz University, P.O. Box 80203, Jeddah 21589, Saudi Arabia
  • Received:2021-01-22 Accepted:2021-03-01 Online:2021-10-18 Published:2021-06-20
  • Contact: Qian Liu,Yan Wang,Xuping Sun
  • About author:First author contact:

    Contributed equally to this work.

  • Supported by:
    National Natural Science Foundation of China(22072015);Shanghai Scientific and Technological Innovation Project(18JC1410604)

Abstract:

Electrochemical N2 reduction provides a green and sustainable alternative to the Haber-Bosch technology for NH3 synthesis. However, the extreme inertness of N2 molecules is a formidable challenge, which requires the development of an active electrocatalyst to drive the N2 reduction reaction (NRR) for NH3 production at ambient conditions. Herein, we demonstrate the development of La-doped TiO2 nanorods as an efficient NRR electrocatalyst for ambient NH3 synthesis. The optimized La-TiO2 catalyst offers a large NH3 yield of 23.06 μg h-1 mgcat-1 and a high Faradaic efficiency of 14.54% at -0.70 V versus reversible hydrogen electrode in 0.1 M LiClO4, outperforming most La- and Ti-based catalysts reported before. Significantly, it also demonstrates high electrochemical stability and its activity decay is negligible after 48 h test. The mechanism is further revealed by density functional theory calculations.

Key words: La doping, Electrocatalytic N2 reduction, Oxygen vacancy, TiO2, Density functional theory