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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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Publication details

The article was received on 14 Dec 2017, accepted on 19 Feb 2018 and first published on 20 Feb 2018


Article type: Edge Article
DOI: 10.1039/C7SC05296K
Citation: Chem. Sci., 2018,9, 3152-3158
  • Open access: Creative Commons BY license
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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

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

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