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铯铅溴钙钛矿介导的醇类可见光光催化高选择性氧化为羰基化合物

Visible-Light Photocatalytic Highly Selective Oxidation of Alcohols into Carbonyl Compounds by CsPbBr Perovskite.

作者信息

Fan Qiangwen, Liu Dawei, Xie Zongbo, Le Zhanggao, Zhu Haibo, Song Xiuqing

机构信息

Jiangxi Province Key Laboratory of Synthetic Chemistry, East China University of Technology, Nanchang 330013, China.

Large-scale Instruments and Equipment Sharing Platform, Beijing University of Technology, Beijing 100124, China.

出版信息

J Org Chem. 2023 Oct 20;88(20):14559-14570. doi: 10.1021/acs.joc.3c01573. Epub 2023 Sep 29.

Abstract

Conversion of alcohols into corresponding carbonyl compounds through an oxidation reaction with high conversion and selectivity simultaneously under mild conditions still remains a great challenge. Herein, a cost-effective and highly efficient photocatalytic protocol for selective oxidation of alcohols was developed using CsPbBr perovskite as a heterogeneous photocatalyst, which afforded aldehydes/ketones exclusively with a yield of 99% at ambient temperature under an air atmosphere. Moreover, the photocatalyst can be recycled at least 5 times without a significant decrease in catalytic activity. The detailed reaction mechanism was investigated by a series of quenching experiments, including Stern-Volmer experiments and electron paramagnetic resonance spectroscopy analysis as well as DFT calculations.

摘要

在温和条件下通过氧化反应将醇同时高转化率和高选择性地转化为相应的羰基化合物仍然是一个巨大的挑战。在此,开发了一种具有成本效益且高效的光催化方法用于醇的选择性氧化,使用CsPbBr钙钛矿作为多相光催化剂,在空气气氛下于室温下仅生成醛/酮,产率为99%。此外,该光催化剂可以循环使用至少5次而催化活性没有显著降低。通过一系列猝灭实验研究了详细的反应机理,包括斯特恩-沃尔默实验、电子顺磁共振光谱分析以及密度泛函理论计算。

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