电荷(物理)
光诱导电荷分离
电子转移
催化作用
材料科学
金属有机骨架
无机化学
化学工程
电化学
金属
作者
Caiyun Xu,Hang Liu,Dandan Li,Ji-Hu Su,Hai-Long Jiang
出处
期刊:Chemical Science
[The Royal Society of Chemistry]
日期:2018-03-21
卷期号:9 (12): 3152-3158
被引量:107
摘要
The selective aerobic oxidative coupling of amines under mild conditions is an important laboratory and commercial procedure yet a great challenge. In this work, a porphyrinic metal–organic framework, PCN-222, was employed to catalyze the reaction. Upon visible light irradiation, the semiconductor-like behavior of PCN-222 initiates charge separation, evidently generating oxygen-centered active sites in Zr-oxo clusters indicated by enhanced porphyrin π-cation radical signals. The photogenerated electrons and holes further activate oxygen and amines, respectively, to give the corresponding redox products, both of which have been detected for the first time. The porphyrin motifs generate singlet oxygen based on energy transfer to further promote the reaction. As a result, PCN-222 exhibits excellent photocatalytic activity, selectivity and recyclability, far superior to its organic counterpart, for the reaction under ambient conditions via combined energy and charge transfer.
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