Citation: Xinyu Yin, Haiyang Shi, Yu Wang, Xuefei Wang, Ping Wang, Huogen Yu. Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production[J]. Acta Physico-Chimica Sinica, ;2024, 40(10): 231200. doi: 10.3866/PKU.WHXB202312007 shu

Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production

Xinyu Yin ¹ ,
Haiyang Shi ¹ ,
Yu Wang ¹ ,
Xuefei Wang ^1,, ,
Ping Wang ¹ ,
Huogen Yu ^2,,

1.
School of Materials Science and Engineering, and School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, China;
2.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, China

Corresponding author: Xuefei Wang, Huogen Yu,
Received Date: 6 December 2023
Revised Date: 10 January 2024
Accepted Date: 10 January 2024

Fund Project: This work was supported by the National Natural Science Foundation of China (22178276, U22A20147, 52073263) and the Natural Science Foundation of Hubei Province of China (2022CFA001).

Transitional metal oxyhydroxides have been demonstrated to be the reliable cocatalysts for water oxidation reaction. However, their insufficient adsorption ability for H₂O and its intermediate products during water oxidation greatly restricts the improvement of water oxidation rate. In this study, a spontaneously improved adsorption of H₂O and its intermediates on the electron-deficient Mn^(3+δ)+ of MnOOH cocatalyst can greatly promote the rapid water oxidation to realize the efficient photocatalytic H₂O₂ production in a pure water system. In this case, amorphous MnOOH is selectively deposited on the (110) facet of AuPd-modified single-crystal BiVO₄ photocatalyst via the directionally photoinduced oxidation approach to produce AuPd/BiVO₄/MnOOH photocatalyst. Photocatalytic experiments exhibit that the as-prepared AuPd/BiVO₄/MnOOH (0.5%) photocatalyst obtains the boosted H₂O₂-evolution rate of 214 μmol·L^-1 as well as exhibits an outstanding stability and reproducibility. Density functional theory calculations and X-ray photoelectron spectroscopy (XPS) characterization reveal that the free electrons of MnOOH can effectively transfer to BiVO₄ to induce the generation of electron-deficient Mn sites (Mn^(3+δ)+), which spontaneously promotes the adsorption of H₂O and its intermediates for enhancing 4-electron water oxidation reaction, resulting in an efficient H₂O₂ production. The present work about the strong interaction between cocatalyst and bulk catalyst provides a fresh idea for the rational design of highly efficient catalytic materials.
- Photocatalysis,
- H₂O₂-production,
- MnOOH cocatalyst,
- Single-crystal BiVO₄,
- H₂O-adsorption
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Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production