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

被引:99
作者
Chen, Xin [1 ]
Dang, Qiang [1 ]
Sa, Rongjian [2 ]
Li, Liuyi [1 ]
Li, Lingyun [1 ]
Bi, Jinhong [1 ,3 ]
Zhang, Zizhong [3 ]
Long, Jinlin [3 ]
Yu, Yan [1 ]
Zou, Zhigang [1 ,4 ]
机构
[1] Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Ecomat Adv Technol, Fuzhou 350108, Peoples R China
[2] Minjiang Univ, Ocean Coll, Inst Oceanog, Fuzhou 350108, Fujian, Peoples R China
[3] Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
[4] Nanjing Univ, Coll Engn & Appl Sci, Ecomat & Renewable Energy Res Ctr, Nanjing 210093, Peoples R China
基金
中国国家自然科学基金;
关键词
PHOTOCATALYTIC HYDROGEN-PRODUCTION; H-2; EVOLUTION; REDUCTION; CONVERSION; CATALYST; HETEROJUNCTION; CRYSTALLINE; FABRICATION; BEARING; HYBRID;
D O I
10.1039/d0sc01747g
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:6915 / 6922
页数:8
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