期刊
CHEMSUSCHEM
卷 13, 期 7, 页码 1725-1729出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201903545
关键词
carbazole; CO2 reduction; covalent organic framework; donor-acceptor; photocatalysis
资金
- National Natural Science Foundation of China [21476108, 51872147] Funding Source: Medline
Visible-light-driven CO2 reduction to valuable chemicals without sacrificial agents and cocatalysts remains challenging, especially for metal-free photocatalytic systems. Herein, a novel donor-acceptor (D-A) covalent organic framework (CT-COF) was constructed by the Schiff-base reaction of carbazole-triazine based D-A monomers and possessed a suitable energy band structure, strong visible-light-harvesting, and abundant nitrogen sites. CT-COF as a metal-free photocatalyst could reduce CO2 with gaseous H2O to CO as the main carbonaceous product with approximately stoichiometric O-2 evolution under visible-light irradiation and without cocatalyst. The CO evolution rate (102.7 mu mol g(-1) h(-1)) was 68.5 times that of g-C3N4 under the same conditions. In situ Fourier-transform (FT)IR analysis indicated that CT-COF could adsorb and activate the CO2 and H2O molecules and that COOH* species may be a key intermediate. DFT calculations suggested that nitrogen atoms in the triazine rings may be photocatalytically active sites.
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