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使用无铅金属卤化物钙钛矿进行可见光驱动的分子氧活化用于醇的氧化酰胺化反应

Visible light-driven molecular oxygen activation for oxidative amidation of alcohols using lead-free metal halide perovskite.

作者信息

Kumar Vishesh, Vyas Ved, Kumar Deepak, Kushwaha Ashish Kumar, Indra Arindam

机构信息

Department of Chemistry, Indian Institute of Technology (BHU) Varanasi UP 221005 India

Department of Chemistry, Banaras Hindu University Varanasi UP 221005 India.

出版信息

Chem Sci. 2024 Aug 29;15(37):15448-55. doi: 10.1039/d4sc03796k.

Abstract

Herein, we report the modulation of the band structures of halide perovskite CsCuBr by tuning the synthesis methods. The photocatalyst PC-1, synthesized by the hot injection method, has a more negative conduction band minima (CBM) than the photocatalyst PC-2, synthesized at room temperature. As a result, PC-1 can activate molecular O more efficiently to initiate the radical-mediated dehydrogenation of alcohols. The more positive valence band maxima (VBM) of PC-1 also facilitates amine oxidation to the corresponding radical. Further, improved charge separation and transport and a decrement in the photogenerated charge carrier recombination have been detected for PC-1 to enhance photocatalytic activity. PC-1 showed improved yields for a series of structurally diverse amides (highest yield = 98%) by oxidative amidation of alcohols under visible light irradiation.

摘要

在此,我们报告了通过调整合成方法对卤化物钙钛矿CsCuBr能带结构的调控。通过热注入法合成的光催化剂PC-1,其导带最小值(CBM)比在室温下合成的光催化剂PC-2更负。因此,PC-1能够更有效地激活分子氧,以引发自由基介导的醇脱氢反应。PC-1更正的价带最大值(VBM)也有利于胺氧化为相应的自由基。此外,已检测到PC-1的电荷分离和传输得到改善,光生电荷载流子复合减少,从而提高了光催化活性。在可见光照射下,PC-1通过醇的氧化酰胺化反应,对一系列结构多样的酰胺表现出更高的产率(最高产率 = 98%)。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01f5/11423617/090caa3fd13c/d4sc03796k-s1.jpg

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