Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution - Details

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The　integration　of　electron　donor　(D)　and　acceptor　(A)　units　into　covalent　organic　frameworks　(COFs)　has　received　increasing　interest　due　to　its　potential　for　efficient　photocatalytic　hydrogen　(H2)　evolution　from　water.　Nevertheless,　the　advancement　of　D–A　COFs　is　still　constrained　by　the　limited　investigations　on　acceptor　engineering,　which　enables　the　highly　effective　charge　transfer　pathways　in　COFs　to　deliver　photoexcited　electrons　in　a　preferential　orientation　to　enhance　photocatalytic　performance.　Herein,　two　systems　with　D–A　and　D–A–A　configurations　based　on　the　acceptor　molecular　engineering　strategy　are　proposed　to　construct　three　distinct　COFs.　Specifically,　TAPPy-DBTDP-COF　merging　one　pyrene-based　donor　and　two　benzothiadiazole　acceptors　realized　an　average　H2　evolution　rate　of　12.7 mmol　h−1　g−1　under　visible　light,　among　the　highest　ever　reported　for　typical　D–A-type　COF　systems.　The　combination　of　experimental　and　theoretical　analysis　signifies　the　crucial　role　of　the　dual-acceptor　arrangement　in　promoting　exciton　dissociation　and　carrier　migration.　These　findings　underscore　the　significant　potential　of　D–A–A　structural　design,　which　is　conducive　to　the　efficient　separation　of　photoexcited　electrons　and　holes　resulting　in　superior　photocatalytic　activities.　©　2024　Wiley-VCH　GmbH.

Keyword：

covalent organic frameworks donor-acceptor COFs H2 evolution photocatalysis

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[ 1 ] [Liu N.]State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 2 ] [Xie S.]Department of Chemistry, Faculty of Science, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore
[ 3 ] [Huang Y.]State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 4 ] [Lu J.]State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 5 ] [Shi H.]State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 6 ] [Xu S.]State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 7 ] [Zhang G.]State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 8 ] [Chen X.]State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou, 350116, China

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Advanced Energy Materials

ISSN： 1614-6832

Year： 2024

Issue： 40

Volume： 14

2 4 . 4 0 0

JCR@2023

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SCOPUS Cited Count： 1

ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 1

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