4.8 Article

Photocatalytic Cascade Reaction Driven by Directed Charge Transfer over VS-Zn0.5Cd0.5S/GO for Controllable Benzyl Oxidation

期刊

ADVANCED SCIENCE
卷 10, 期 20, 页码 -

出版社

WILEY
DOI: 10.1002/advs.202207250

关键词

photocatalytic cascade reaction; proton-coupled electron transfer; singlet O-2; S vacancy

向作者/读者索取更多资源

This study reports a light-driven synergistic redox reaction for the selective oxidation of benzyl to phenylcarbinol using Zn0.5Cd0.5S/graphene oxide photocatalyst. The presence of S vacancies on the surface of the photocatalyst plays a crucial role in the adsorption and activation of oxygen, generating superoxide radicals and singlet oxygen. The pi-pi stacking effect between the photocatalyst and graphene oxide accelerates the transfer of photogenerated electrons and promotes the selective hydrogenation of aldehydes.
Photocatalysis is an important technique for synthetic transformations. However, little attention has been paid to light-driven synergistic redox reactions for directed synthesis. Herein, the authors report tunable oxidation of benzyl to phenylcarbinol with the modest yield (47%) in 5 h via singlet oxygen (O-1(2)) and proton-coupled electron transfer (PCET) over the photocatalyst Zn0.5Cd0.5S (ZCS)/graphene oxide (GO) under exceptionally mild conditions. Theoretical calculations indicate that the presence of S vacancies on the surface of ZCS/GO photocatalyst is crucial for the adsorption and activation of O-2, successively generating the superoxide radical (O-center dot(2)-) and O-1(2), attributing to the regulation of local electron density on the surface of ZCS/GO and photogenerated holes (h(+)). Meanwhile, accelerated transfer of photogenerated electrons (e(-)) to GO caused by the pi-pi stacking effect is conducive to the subsequent aldehyde hydrogenation to benzyl alcohol rather than non-selective oxidation of aldehyde to carboxylic acid. Anisotropic charge transport driven by the built-in electric field can further promote the separation of e(-) and h(+) for multistep reactions. Promisingly, one-pot photocatalytic conversion of p-xylene to 4-methylbenzyl alcohol is beneficial for reducing the harmful effects of aromatics on human health. Furthermore, this study provides novel insights into the design of photocatalysts for cascade reactions.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.8
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据