Chemical Research in Chinese Universities ›› 2022, Vol. 38 ›› Issue (5): 1243-1250.doi: 10.1007/s40242-022-2194-7

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Anchoring Single Nickel Atoms on Carbon-vacant Carbon Nitride Nanosheets for Efficient Photocatalytic Hydrogen Evolution

LIN Zhi1, ZHANG Zhengqi1, WANG Yiqing1, PENG Zhiming1, WANG Xinxin1, WANG Ruizhe1, HUANG Yu-Cheng2, MENG Fanqi3, LI Mingtao1, DONG Chung-Li2, ZHANG Qinghua3, GU Lin3, SHEN Shaohua1   

  1. 1. International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an 710049, P. R. China;
    2. Department of Physics, Tamkang University, New Taipei City 25137, Taiwan, P. R. China;
    3. Institute of Physics, Chinese Academy of Sciences, Beijing 100190, P. R. China
  • Received:2022-06-10 Online:2022-10-01 Published:2022-10-08
  • Contact: SHEN Shaohua E-mail:shshen_xjtu@mail.xjtu.edu.cn
  • Supported by:
    This work was supported by the National Key Research and Development Program of China(No.2018YFB1502003), the National Natural Science Foundation of China(No.21875183), the Natural Science Basic Research Program of Shaanxi Province, China(No.2019JCW-10), the Fundamental Research Funds for the Central Universities, China and the Youth Innovation Team of Shaanxi Universities, China.

Abstract: Polymeric carbon nitride(PCN) has emerged as a promising candidate for photocatalytic hydrogen evolution, but its dependence on scarce and high-cost noble metal co-catalysts severely limits its extensive application. It will be of great promise to develop non-noble metal single-atom co-catalysts with low-cost and high atom utilization to improve the photocatalytic performance over PCN. Herein, single Ni atoms are successfully anchored onto carbon-vacant PCN nanosheets(CCN-SANi) via a two-step ammonia thermal treatment and photo-deposition process. Theoretical calculations and experimental results demonstrate that the optical absorption property and the charge transfer ability of CCN-SANi have been significantly improved with the introduction of single Ni atoms to form Ni-N3 sites. In comparison to carbon-vacant PCN(CCN) loaded with Ni clusters, the obtained CCN-SANi exhibits 11.4 times increased photocatalytic performance, with the highest hydrogen evolution rate reaching 511 μmol/(g·h), which is even 1.7 times higher than that of CCN loaded with Pt clusters. This research proposes an inspiring and reliable strategy to design novel single-atom semiconducting polymers with electronic structures manipulated for efficient photocatalysis.

Key words: Photocatalytic hydgogen evolution, Single metal atom, Polymeric carbon nitride