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Isolated Square‐Planar Copper Center in Boron Imidazolate Nanocages for Photocatalytic Reduction of CO 2 to CO
Author(s) -
Zhang HaiXia,
Hong QinLong,
Li Jing,
Wang Fei,
Huang Xinsong,
Chen Shumei,
Tu Wenguang,
Yu Dingshan,
Xu Rong,
Zhou Tianhua,
Zhang Jian
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201905869
Subject(s) - photocatalysis , copper , selectivity , imidazolate , nanocages , photochemistry , catalysis , materials science , chemistry , zeolitic imidazolate framework , adsorption , inorganic chemistry , metal organic framework , biochemistry , metallurgy
Photocatalytic reduction of CO 2 to value‐added fuel has been considered to be a promising strategy to reduce global warming and shortage of energy. Rational design and synthesis of catalysts to maximumly expose the active sites is the key to activate CO 2 molecules and determine the reaction selectivity. Herein, we synthesize a well‐defined copper‐based boron imidazolate cage (BIF‐29) with six exposed mononuclear copper centers for the photocatalytic reduction of CO 2 . Theoretical calculations show a single Cu site including weak coordinated water delivers a new state in the conduction band near the Fermi level and stabilizes the *COOH intermediate. Steady‐state and time‐resolved fluorescence spectra show these Cu sites promote the separation of electron–hole pairs and electron transfer. As a result, the cage achieves solar‐driven reduction of CO 2 to CO with an evolution rate of 3334 μmol g −1 h −1 and a high selectivity of 82.6 %.