Journal
CHEMICAL SCIENCE
Volume 11, Issue 26, Pages 6915-6922Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc01747g
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Funding
- National Natural Science Foundation of China [U1905215, 51672046, 51672047]
- Natural Science Foundation of Fujian Province of China [2019J01226, 2019J01648]
- Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment [SKLPEE-KF201815, SKLPEE-KF201813]
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Selective photoreduction of CO(2)into a given product is a great challenge but desirable. Inspired by natural photosynthesis occurring in hierarchical networks over non-precious molecular metal catalysts, we demonstrate an integration of single Ni sites into the hexagonal pores of polyimide covalent organic frameworks (PI-COFs) for selective photoreduction of CO(2)to CO. The single Ni sites in the hexagonal pores of the COFs serve as active sites for CO(2)activation and conversion, while the PI-COFs not only act as a photosensitizer to generate charge carriers but also exert a promoting effect on the selectivity. The optimized PI-COF with a triazine ring exhibits excellent activity and selectivity. A possible intra- and inter-molecular charge-transfer mechanism was proposed, in which the photogenerated electrons in PI-COFs are efficiently separated from the central ring to the diimide linkage, and then transferred to the single Ni active sites, as evidenced by theoretical calculations.
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