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Citation: Ruiyun Liu, Ping Wang, Xuefei Wang, Feng Chen, Huogen Yu. Work-function-engineered Mo 4d electronic structure modulation in Mo2C MXene cocatalyst for efficient photocatalytic H2 evolution[J]. Acta Physico-Chimica Sinica, ;2025, 41(11): 100137. doi: 10.1016/j.actphy.2025.100137 shu

Work-function-engineered Mo 4d electronic structure modulation in Mo2C MXene cocatalyst for efficient photocatalytic H2 evolution

  • 1.

    School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, Hubei Province, China

  • 2.

    Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, Hubei Province, China

  • Corresponding author: Ping Wang, wangping0904@whut.edu.cn Huogen Yu, yuhuogen@cug.edu.cn
  • Received Date: 29 June 2025
    Revised Date: 22 July 2025
    Accepted Date: 24 July 2025

    Fund Project: the National Natural Science Foundation of China 22472127the National Natural Science Foundation of China 22178275the National Natural Science Foundation of China U22A20147the Natural Science Foundation of Hubei Province of China 2022CFA001

  • Mo2C MXene (Mo2CTx) exhibits exceptional hydrogen-evolution potential in photocatalysis due to the Pt-like electronic structure of surface Mo active sites. However, the Mo sites in Mo2CTx usually show excessively strong H-adsorption during HER, significantly limiting the intrinsic catalytic activity of Mo2CTx. To weaken the H-adsorption capacity of Mo active sites, a strategy of modulating d-orbital electron is implemented via in-situ constructing MoC-Mo2C MXene heterojunction by a work-function-induced effect. The MoC-Mo2CTx heterojunction was synthesized by in situ conversion of Mo2C MXene into MoC via a Co-induced molten salt method, followed by coupling with TiO2 through a simple ultrasonication-assisted method to prepare the MoC-Mo2CTx/TiO2 photocatalyst. Photocatalytic tests showed that the optimal MoC-Mo2CTx/TiO2 sample achieves an excellent hydrogen production rate of 1886 μmol∙h−1∙g−1, representing 117.9 and 3.9 fold enhancements over TiO2 and Mo2CFX/TiO2 (Mo2CF2 prepared by a conventional etchant NH4F+HCl), respectively. Experimental and theoretical calculations substantiate that the work-function gradient between MoC and Mo2C MXene induces electron transfer from MoC to Mo2C MXene to weaken the H-adsorption of Mo active sites in Mo2CTx cocatalyst, thereby enhancing its HER activity. This research provides a new strategy of in situ constructing Mo2C MXene-based heterojunction for adjusting the H-adsorption capacity of Mo active sites.
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