期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 46, 页码 14308-14312出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201608597
关键词
active sites; CO2 reduction; heterogeneous catalysis; photocatalysis; solar-energy conversion
资金
- World Premier International Research Center Initiative (WPI Initiative) on Materials Nanoarchitectonics (MANA), MEXT (Japan)
- National Basic Research Program of China (973 Program) [2014CB239301, NSFC11605225]
- Jianlin Xie Foundation of the Institute of High Energy Physics, Chinese Academy of Sciences
Modular optimization of metal-organic frameworks (MOFs) was realized by incorporation of coordinatively unsaturated single atoms in a MOF matrix. The newly developed MOF can selectively capture and photoreduce CO2 with high efficiency under visible-light irradiation. Mechanistic investigation reveals that the presence of single Co atoms in the MOF can greatly boost the electron-hole separation efficiency in porphyrin units. Directional migration of photogenerated excitons from porphyrin to catalytic Co centers was witnessed, thereby achieving supply of long-lived electrons for the reduction of CO2 molecules adsorbed on Co centers. As a direct result, porphyrin MOF comprising atomically dispersed catalytic centers exhibits significantly enhanced photocatalytic conversion of CO2, which is equivalent to a 3.13-fold improvement in CO evolution rate (200.6 mu mol g(-1) h(-1)) and a 5.93-fold enhancement in CH4 generation rate (36.67 mu mol g(-1) h(-1)) compared to the parent MOF.
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