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用于在类三明治结构的Pd@TiO₂@ZnIn₂S₄纳米盒上协同析氢与苄胺氧化偶联的双功能光催化

Dual-Functional Photocatalysis for Cooperative Hydrogen Evolution and Benzylamine Oxidation Coupling over Sandwiched-Like Pd@TiO @ZnIn S Nanobox.

作者信息

She Ping, Qin Jun-Sheng, Sheng Jiyao, Qi Yuanyuan, Rui Hongbang, Zhang Wei, Ge Xin, Lu Geyu, Song Xiaowei, Rao Heng

机构信息

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Key Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun, 130012, P. R. China.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, International Center of Future Science, College of Chemistry, Jilin University, Changchun, 130012, P. R. China.

出版信息

Small. 2022 Mar;18(10):e2105114. doi: 10.1002/smll.202105114. Epub 2022 Jan 5.

Abstract

Photocatalytic hydrogen evolution (PHE) over semiconductor photocatalysts is usually constrained by the limited light-harvesting and separation of photogenerated electron-hole pairs. Most of the reported systems focusing on PHE are facilitated by consuming the photoinduced holes with organic sacrificial electron donors (SEDs). The introduction of the SEDs not only causes the environmental problem, but also increases the cost of the reaction. Herein, a dual-functional photocatalyst is developed with the morphology of sandwiched-like hollowed Pd@TiO @ZnIn S nanobox, which is synthesized by choosing microporous zeolites with sub-nanometer-sized Pd nanoparticles (Pd NPs) embedded as the sacrificial templates. The ternary Pd@TiO @ZnIn S photocatalyst exhibits a superior PHE rate (5.35 mmol g h ) and benzylamine oxidation conversion rate (>99%) simultaneously without adding any other SEDs. The PHE performance is superior to the reported composites of TiO and ZnIn S , which is attributed to the elevated light capture ability induced by the hollow structure, and the enhanced charge separation efficiency facilitated by the ultrasmall sized Pd NPs. The unique design presented here holds great potential for other highly efficient cooperative dual-functional photocatalytic reactions.

摘要

半导体光催化剂上的光催化析氢(PHE)通常受到光捕获有限和光生电子-空穴对分离的限制。大多数报道的专注于PHE的体系是通过有机牺牲电子供体(SEDs)消耗光生空穴来实现的。SEDs的引入不仅会引发环境问题,还会增加反应成本。在此,开发了一种具有夹心状中空Pd@TiO₂@ZnIn₂S₄纳米盒形态的双功能光催化剂,它是通过选择嵌入亚纳米尺寸钯纳米颗粒(Pd NPs)的微孔沸石作为牺牲模板合成的。三元Pd@TiO₂@ZnIn₂S₄光催化剂在不添加任何其他SEDs的情况下,同时展现出优异的PHE速率(5.35 mmol g⁻¹ h⁻¹)和苄胺氧化转化率(>99%)。其PHE性能优于报道的TiO₂和ZnIn₂S₄复合材料,这归因于中空结构诱导的光捕获能力提升,以及超小尺寸Pd NPs促进的电荷分离效率增强。这里提出的独特设计在其他高效协同双功能光催化反应方面具有巨大潜力。

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