化学
光化学
格式化
光催化
光谱学
超快激光光谱学
光致发光
卟啉
金属有机骨架
电子
光电子学
催化作用
材料科学
物理化学
有机化学
吸附
物理
量子力学
作者
Hai-Qun Xu,Jiahua Hu,Dengke Wang,Zhaohui Li,Qun Zhang,Yi Luo,Shu‐Hong Yu,Hai‐Long Jiang
摘要
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 CO2 into formate anion compared to the corresponding porphyrin ligand itself. This work provides important insights into the design of MOF-based materials for CO2 capture and photoreduction.
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