选择性
共价键
三嗪
催化作用
光敏剂
化学
光化学
材料科学
戒指(化学)
组合化学
有机化学
作者
Xin Chen,Qiang Dang,Rongjian Sa,Liuyi Li,Jinhong Bi,Zizhong Zhang,Jinlin Long,Yan Yu,Zhigang Zou
出处
期刊:Chemical Science
[The Royal Society of Chemistry]
日期:2020-01-01
卷期号:11 (26): 6915-6922
被引量:77
摘要
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.
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