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Abstract:
Polymeric or organic semiconductors are promising candidates for photocatalysis but mostly only show moderate activity owing to strongly bound excitons and insufficient optical absorption. Herein, we report a facile bottom-up strategy to improve the activity of a carbon nitride to a level in which a majority of photons are really used to drive photoredox chemistry. Co-condensation of urea and oxamide followed by post-calcination in molten salt is shown to result in highly crystalline species with a maximum - layer stacking distance of heptazine units of 0.292nm, which improves lateral charge transport and interlayer exciton dissociation. The addition of oxamide decreases the optical band gap from 2.74 to 2.56eV, which enables efficient photochemistry also with green light. The apparent quantum yield (AQY) for H-2 evolution of optimal samples reaches 57% and 10% at 420nm and 525nm, respectively, which is significantly higher than in most previous experiments.
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Source :
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN: 1433-7851
Year: 2017
Issue: 43
Volume: 56
Page: 13445-13449
1 2 . 1 0 2
JCR@2017
1 6 . 1 0 0
JCR@2023
ESI Discipline: CHEMISTRY;
ESI HC Threshold:226
JCR Journal Grade:1
CAS Journal Grade:2
Cited Count:
WoS CC Cited Count: 583
SCOPUS Cited Count: 581
ESI Highly Cited Papers on the List: 35 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 2
Affiliated Colleges: