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Abstract:
Covalent organic frameworks (COFs)-based photocatalysts have received growing attention for photocatalytic hydrogen (H-2) production. One of the big challenges in the field is to find ways to promote energy/electron transfer and exciton dissociation. Addressing this challenge, herein, a series of olefin-linked 2D COFs is fabricated with high crystallinity, porosity, and robustness using a melt polymerization method without adding volatile organic solvents. It is found that regulation of the spatial distances between the acceptor units (triazine and 2, 2'-bipyridine) of COFs to match the charge carrier diffusion length can dramatically promote the exciton dissociation, hence leading to outstanding photocatalytic H-2 evolution performance. The COF with the appropriate acceptor distance achieves exceptional photocatalytic H-2 evolution with an apparent quantum yield of 56.2% at 475 nm, the second highest value among all COF photocatalysts and 70 times higher than the well-studied polymer carbon nitride. Various experimental and computation studies are then conducted to in-depth unveil the mechanism behind the enhanced performance. This study will provide important guidance for the design of highly efficient organic semiconductor photocatalysts.
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Source :
ADVANCED SCIENCE
Year: 2022
Issue: 29
Volume: 9
1 5 . 1
JCR@2022
1 5 . 1 0 0
JCR@2022
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 62
SCOPUS Cited Count: 64
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 9
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