量子点
氧化还原
催化作用
光化学
量子产额
化学
半导体
异质结
光催化
电子转移
光催化
偶联反应
纳米技术
材料科学
光电子学
无机化学
物理
有机化学
量子力学
荧光
作者
Lin-Xing Zhang,Ming‐Yu Qi,Zi‐Rong Tang,Yi‐Jun Xu
出处
期刊:Research
[AAAS00]
日期:2023-01-01
卷期号:6
被引量:3
标识
DOI:10.34133/research.0073
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 H 2 . 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.
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