4.6 Article

Hydrogenated Oxide as Novel Quasi-metallic Cocatalyst for Efficient Visible-Light Driven Photocatalytic Water SplittingN

期刊

JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 23, 页码 12672-12681

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c02991

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资金

  1. National Key Research and Development Program of China [2016YFA0200602, 2018YFA0208603, 2017YFA0303500, 2018YFA0208702]
  2. National Natural Science Foundation of China [22025304, 22033007, 21790350, 21573211, 21633007, 21803067, 91950207, U2004214]
  3. DNL Cooperation Fund of Chinese Academy of Sciences [DNL201913]
  4. Anhui Initiative in Quantum Information Technologies [AHY090200]
  5. USTC-NSRL Joint Funds
  6. USTC Center for Micro-and Nanoscale Research and Fabrication
  7. Steady High Magnetic Field Facilities
  8. High Magnetic Field Laboratory
  9. Fundamental Research Funds for Central Universities of China

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This study demonstrates the potential of hydrogenated MoO3 (HMO) as an excellent cocatalyst for the ZnIn2S4 photocatalyst, significantly improving the H-2 production rate. The efficient charge transfer from ZnIn2S4 to HMO and the lowered overpotential of the H-2 evolution reaction contribute to this enhancement.
The frequent use of noble metals such as Pt as a cocatalyst to improve photocatalytic performance has stimulated an extensive search for cost-effective materials as alternative cocatalysts. Here we report the use of hydrogenated MoO3 (HMO) with a unique quasi-metallic property as an excellent cocatalyst for the ZnIn2S4 photocatalyst. The HMO-ZnIn2S4 composite with an optimized ratio realizes a H-2 production rate of 1564 mu mol h(-1) g(-1) under visible light (lambda >= 420 nm) excitation. It not only significantly surpasses the performance of pristine ZnIn2S4 (327 mu mol h(-1) g(-1)), but also outperforms the 1 wt % Pt-decorated ZnIn2S4 (1308 mu mol h(-1) g(-1)). The reasons for this improvement, as disclosed by photoelectrochemical characterization, ultrafast laser spectroscopy, and density functional calculation, is that the efficient charge transfer from ZnIn2S4 to HMO facilitates electron-hole separation after photoexcitaiton, and HMO substantially lowers the overpotential of the H-2 evolution reaction. This work thus demonstrates the potential of quasi-metallic hydrogenated metal oxide as an alternative to noble metal cocatalyst for photocatalytic application.

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