期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 137, 期 42, 页码 13440-13443出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b08773
关键词
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资金
- 973 program [2014CB931803, 2010CB923300, 2014CB239303]
- NSFC [21371162, 21521001, 21173205, 91127042, 21273035]
- CAS [XDB01020000]
- Recruitment Program of Global Youth Experts
- Fundamental Research Funds for the Central Universities [WK2060190026, WK2340000063]
It is highly desirable to convert CO2 to valuable fuels or chemicals by means of solar energy, which requires CO2 enrichment around photocatalysts from the atmosphere. Here we demonstrate that a porphyrin-involved metal organic framework (MOF), PCN-222, can selectively capture and further photoreduce CO2 with high efficiency under visible-light irradiation. Mechanistic information gleaned from ultrafast transient absorption spectroscopy (combined with time-resolved photoluminescence spectroscopy) has elucidated the relationship between the photocatalytic activity and the electron hole separation efficiency. The presence of a deep electron trap state in PCN-222 effectively inhibits the detrimental, radiative electron hole recombination. As a direct result, PCN-222 significantly enhances photocatalytic conversion of CO, into formate anion compared to the corresponding porphyrin ligand itself. This work provides important insights into the design of MOP-based materials for CO2 capture and photoreduction.
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