Integrating single Ni sites into biomimetic networks of covalent organic frameworks for selective photoreduction of CO2

Selective photoreduction of CO2 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...

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Bibliographic Details
Published in:Chemical science (Cambridge) 2020-07, Vol.11 (26), p.6915-6922
Main Authors: Chen, Xin, Dang, Qiang, Sa, Rongjian, Li, Liuyi, Li, Lingyun, Bi, Jinhong, Zhang, Zizhong, Long, Jinlin, Yu, Yan, Zou, Zhigang
Format: Article
Language:English
Subjects:
Biomimetics
Carbon dioxide
Charge transfer
Current carriers
Diimide
Nickel
Photosynthesis
Selectivity
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Summary:Selective photoreduction of CO2 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 CO2 to CO. The single Ni sites in the hexagonal pores of the COFs serve as active sites for CO2 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.
ISSN:2041-6520
2041-6539
DOI:10.1039/d0sc01747g