Efficient Visible‐Light‐Driven Carbon Dioxide Reduction by a Single‐Atom Implanted Metal–Organic Framework |
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| Authors: | Dr Huabin Zhang Dr Jing Wei Dr Juncai Dong Dr Guigao Liu Li Shi Dr Pengfei An Dr Guixia Zhao Dr Jintao Kong Dr Xiaojun Wang Dr Xianguang Meng Prof Jing Zhang Prof Jinhua Ye |
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| Affiliation: | 1. International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), Ibaraki, Japan;2. Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, P.R. China;3. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, P.R. China;4. TU-NIMS Joint Research Center, School of Material Science and Engineering, Tianjin University, Tianjin, P.R. China;5. Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, P.R. China |
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| Abstract: | 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 μmol g?1 h?1) and a 5.93‐fold enhancement in CH4 generation rate (36.67 μmol g?1 h?1) compared to the parent MOF. |
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| Keywords: | active sites CO2 reduction heterogeneous catalysis photocatalysis solar-energy conversion |
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