期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 34, 页码 11752-11756出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201905869
关键词
boron; carbon dioxide reduction; copper; nanocages; photocatalysis
资金
- NSFC [51772291, 21425102, 21773242, 21603226]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB20000000]
- National Key Research and Development Program of China [2018YFA0208600]
- Youth Innovation Promotion of CAS [2016276]
- NSF of Fujian province [2016J05052]
Photocatalytic reduction of CO2 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 CO2 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 CO2. 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 CO2 to CO with an evolution rate of 3334 mu mol g(-1) h(-1) and a high selectivity of 82.6 %.
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