摘要
Semiconductor quantum dots have been emerging as one of the most ideal materials for artificial photosynthesis.Here,we report the assembled ZnS-CdS hybrid heterostructure for efficient coupling cooperative redox catalysis toward the oxidation of 1-phenylethanol to acetophenone/2,3-diphenyl-2,3-butanediol(pinacol)integrated with the reduction of protons to H2.The strong interaction and typical type-I band-position alignment between CdS quantum dots and ZnS quantum dots result in efficient separation and transfer of electron-hole pairs,thus distinctly enhancing the coupled photocatalyzed-redox activity and stability.The optimal ZnS-CdS hybrid also delivers a superior performance for various aromatic alcohol coupling photoredox reaction,and the ratio of electrons and holes consumed in such redox reaction is close to 1.0,indicating a high atom economy of cooperative coupling catalysis.In addition,by recycling the scattered light in the near field of a SiO_(2)sphere,the SiO_(2)-supported ZnS-CdS(denoted as ZnS-CdS/SiO_(2))catalyst can further achieve a 3.5-fold higher yield than ZnS-CdS hybrid.Mechanistic research clarifies that the oxidation of 1-phenylethanol proceeds through the pivotal radical intermediates of•C(CH_(3))(OH)Ph.This work is expected to promote the rational design of semiconductor quantum dots-based heterostructured catalysts for coupling photoredox catalysis in organic synthesis and clean fuels production.
出处
《Research》
SCIE
EI
CSCD
2023年第4期207-217,共11页
研究（英文）
基金
The support from the NSFC(22072023,22172030,21872029,U1463204,and 21173045)
the Program for National Science and Technology Innovation Leading Talents(00387072)
the Award Program for Minjiang Scholar Professorship,the Program for Leading Talents of Fujian Universities,the First Program of Fujian Province for Top Creative Young Talents,and the NSF of Fujian Province(2019J01631 and 2017J07002)is gratefully acknowledged.
作者简介
Address correspondence to:Zi-Rong Tang,zrtang@fzu.edu.cn;Address correspondence to:Yi-Jun Xu,yjxu@fzu.edu.cn。
