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Imine-linked covalent organic frameworks (COFs) are popular candidates for photocatalytic CO2 reduction, but high polarization of the imine bond is less efficient for pi-electron delocalization between the linked building units, leading to low intramolecular electron transfer and poor photocatalytic efficiency. Herein, we present a structural and electronic engineering strategy through integrating the imine-linked COF consisting of Zn-porphyrin and Co-bipyridyl units with cadmium sulfide (CdS) nanowires to form a CdS@COF core-shell structure. The experimental and theoretical results have validated that CdS serves as the electron transfer channel through the interfacial electron effects, which induces photoelectron transfer from Zn-porphyrin to CdS and subsequent injection into Co-bipyridyl units for CO2 reduction. The as-prepared CdS@COF generates 4057 mu mol g(-1) CO in 8 h under visible-light irradiation, which is considerably higher than those of its neat CdS and imine-linked COF counterparts. This work provides protocols to tackle intramolecular charge transfer across polar linkages between photosensitizers and active sites for solar-to-chemical energy conversion.
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ACS CATALYSIS
ISSN: 2155-5435
Year: 2022
Issue: 6
Volume: 12
Page: 3550-3557
1 2 . 9
JCR@2022
1 1 . 7 0 0
JCR@2023
ESI Discipline: CHEMISTRY;
ESI HC Threshold:74
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 124
SCOPUS Cited Count: 127
ESI Highly Cited Papers on the List: 11 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 2
Affiliated Colleges: