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Efficient Visible‐Light‐Driven Carbon Dioxide Reduction by a Single‐Atom Implanted Metal–Organic Framework
Author(s) -
Zhang Huabin,
Wei Jing,
Dong Juncai,
Liu Guigao,
Shi Li,
An Pengfei,
Zhao Guixia,
Kong Jintao,
Wang Xiaojun,
Meng Xianguang,
Zhang Jing,
Ye Jinhua
Publication year - 2016
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201608597
Subject(s) - metal organic framework , porphyrin , photochemistry , catalysis , photocatalysis , molecule , metal , materials science , adsorption , chemistry , organic chemistry , metallurgy
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 CO 2 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 CO 2 molecules adsorbed on Co centers. As a direct result, porphyrin MOF comprising atomically dispersed catalytic centers exhibits significantly enhanced photocatalytic conversion of CO 2 , 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 CH 4 generation rate (36.67 μmol g −1 h −1 ) compared to the parent MOF.