Indexed by:
Abstract:
The efficient polymeric semiconducting photocatalyst for solar -driven sluggish kinetics with multielectron transfer oxygen evolution has spurred scientific interest. However, existing photocatalysts limited by pi-conjugations, visible-light harvest, and charge transfer often compromise the O-2 production rate. Herein, we introduced an alternative strategy involving a boranil functionalized-based fully pi-conjugated ordered donor and acceptor (D-A) covalent organic frameworks (Ni-TAPP-COF-BF2) photocatalyst. The co-catalystfree Ni-TAPP-COF-BF2 exhibits an excellent similar to 11-fold photocatalytic water oxidation rate, reaching 1404 mu mol g(-1)h(-1)under visible light irradiation compared to pristine Ni-TAPP-COF (123 mu mol g(-1) h(- 1)) alone and surpasses to reported organic frameworks counterpart. Both experimental and theoretical results demonstrate that the push/pull mechanism (metalloporphyrin/BF2) is responsible for the appropriate light-harvesting properties and extending pi-conjugation through chelating BF2 moieties. This strategy benefits in narrowing band structure, improving photo-induced charge separation, and prolonged charge recombination. Further, the lower spin magnetic moment of M-TAPP-COF-BF2 and the closer d-band center of metal sites toward the Fermi level lead to a lower energy barrier for *O intermediate. Reveal the potential of the functionalization strategy and opens up an alternative approach for engineering future photocatalysts in energy conversion applications.
Keyword:
Reprint 's Address:
Email:
Version:
Source :
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN: 1433-7851
Year: 2024
Issue: 13
Volume: 63
1 6 . 1 0 0
JCR@2023
Cited Count:
WoS CC Cited Count: 18
SCOPUS Cited Count: 21
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1
Affiliated Colleges: