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Photocatalytic overall water splitting on isolated semiconductor photocatalyst sites in an ordered mesoporous silica matrix: A multiscale strategy

DOI:10.1016/j.jcat.2018.12.020 期刊:Journal of Catalysis 出版年份:2019 更新时间:2025-09-23 15:23:52
摘要: Photocatalytic overall water splitting (OWS) in a stoichiometric ratio has attracted increasing attention for the realization of a sustainable, environmentally friendly future. However, this reaction exhibits sluggish kinetics due to efficiency limitations of the involved steps, including photon absorption, electron transfer, and the reactions that occur at triple-phase boundary regions. Herein, we report a general multiscale strategy to address this challenge by designing a model composite catalyst with a high loading density of isolated Bi0.5Y0.5VO4 nanocrystals, as building blocks, dispersed in a hexagonally ordered mesoporous silica matrix. In contrast to the well-recognized heterojunction formed between different semiconductors, we show that confined growth favours the formation of isolated quaternary solid-solution photocatalysts (Bi0.5Y0.5VO4), which can further interface with the insulating silica to overcome temperature limitations and exhibit enhanced photon absorption and electrochemical and mass transfer properties due to the transparent periodic porous structure of silica and the as-formed small nanocrystals with high crystallinity and a passivated surface. When the semiconductor photocatalyst is incorporated with the inert silica insulator, this nanoarchitecture does not inhibit the OWS activity but actually delivers a 10-fold higher OWS activity than bulk Bi0.5Y0.5VO4 prepared by the conventional solid-state method.
作者: Zhi Jiang,Zhengwen Huang,Weiqi Guo,Wenfeng Shangguan
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To address the sluggish kinetics and efficiency limitations in photocatalytic overall water splitting by developing a multiscale strategy using isolated Bi0.5Y0.5VO4 nanocrystals in a mesoporous silica matrix to enhance photon absorption, electron transfer, and mass transfer properties.

The hierarchical mesoporous composite structure with isolated Bi0.5Y0.5VO4 nanocrystals in silica significantly enhances photocatalytic overall water splitting activity by improving light harvesting, charge separation, and mass transfer. This multiscale strategy overcomes temperature limitations and provides a 10-fold increase in activity compared to bulk materials, demonstrating potential for sustainable solar fuel production.

The study is limited to specific photocatalysts (Bi0.5Y0.5VO4, SrTiO3, TiO2) and silica matrices; the method may not be universally applicable to all materials. High-temperature calcination can lead to pore collapse and impurity formation if not optimized. The back-reaction of H2 and O2 to form water was not fully addressed, and the strategy requires further optimization for real-world solar fuel applications.

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