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Issue 12, 2018
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Direct evidence of charge separation in a metal–organic framework: efficient and selective photocatalytic oxidative coupling of amines via charge and energy transfer

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Abstract

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.

Graphical abstract: Direct evidence of charge separation in a metal–organic framework: efficient and selective photocatalytic oxidative coupling of amines via charge and energy transfer

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Supplementary files

Article information


Submitted
14 Dec 2017
Accepted
19 Feb 2018
First published
20 Feb 2018

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2018,9, 3152-3158
Article type
Edge Article

Direct evidence of charge separation in a metal–organic framework: efficient and selective photocatalytic oxidative coupling of amines via charge and energy transfer

C. Xu, H. Liu, D. Li, J. Su and H. Jiang, Chem. Sci., 2018, 9, 3152
DOI: 10.1039/C7SC05296K

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