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选择性渗透 FeOOH 非晶层包覆 CdS 以提高苯甲醇的光催化转化和选择性生成苯甲醛。

Selectively Permeable FeOOH Amorphous Layer Coating CdS for Enhancing Photocatalytic Conversion of Benzyl Alcohol and Selectivity to Benzaldehyde.

机构信息

International Joint Research Center for Photoresponsive Molecules and Materials, School of Chemical and Material Engineering, Jiangnan University, 214122, Wuxi, P. R. China.

Department of Chemistry, Tsinghua University, 100084, Beijing, P. R. China.

出版信息

ChemSusChem. 2023 May 5;16(9):e202202355. doi: 10.1002/cssc.202202355. Epub 2023 Mar 17.

Abstract

The development of new strategies to improve reaction efficiency and light utilization is one of the biggest challenges in photosynthetic chemistry. Dynamics control, particularly tuning the adsorption/desorption of reactants and products, is an ideal way to improve the conversion and selectivity in catalytic reactions, but it is rarely studied for photocatalytic organic synthesis. This study concerns the design of an amorphous FeOOH coating to decorate CdS photocatalyst to control the adsorption and desorption of reactants and products to improve reaction efficiency for the photocatalytic conversion of benzyl alcohol (BA) into benzaldehyde (BAD). The best conversion of the core-shell photocatalyst is 74.1 % in 2 h, together with >99.9 % selectivity to BAD, and the photocatalyst exhibits response above 600 nm, which is the longest active wavelength reported for the reaction. Further data illustrate that the amorphous FeOOH coating enables selective sorption of BA/BAD molecules by H-bonding interactions, which may result in the excellent performance. Construction of amorphous coating layers and understanding the selective permeability may provide a new strategy for the design of more efficient photocatalytic systems for organic synthesis.

摘要

开发新策略以提高反应效率和光利用效率是光合作用化学中的最大挑战之一。动力学控制,特别是调节反应物和产物的吸附/解吸,是提高催化反应转化率和选择性的理想方法,但很少用于光催化有机合成。本研究设计了一种非晶态 FeOOH 涂层来修饰 CdS 光催化剂,以控制反应物和产物的吸附和解吸,从而提高光催化转化苄醇(BA)为苯甲醛(BAD)的反应效率。核壳型光催化剂的最佳转化率为 2 h 内 74.1%,对 BAD 的选择性>99.9%,且光催化剂在 600nm 以上有响应,这是该反应报道的最长活性波长。进一步的数据表明,非晶态 FeOOH 涂层通过氢键相互作用实现了 BA/BAD 分子的选择性吸附,这可能是其优异性能的原因。非晶态涂层结构的构建和选择性渗透性的理解为设计用于有机合成的更高效光催化体系提供了新策略。

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