In Situ Integration of Metallic Catalytic Sites and Photosensitive Centers within Covalent Organic Frameworks for the Enhanced Photocatalytic Reduction of CO2 - Details

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Covalent　organic　frameworks　(COFs)　are　a　promising　platform　for　heterogeneous　photocatalysis　due　to　their　stability　and　design　diversity,　but　their　potential　is　often　restricted　by　unmanageable　targeted　excitation　and　charge　transfer.　Herein,　a　bimetallic　COF　integrating　photosensitizers　and　catalytic　sites　is　designed　to　facilitate　locally　ultrafast　charge　transfer,　aiming　to　improve　the　photocatalytic　reduction　of　CO2.　The　strategy　uses　a　“one-pot”　method　to　synthesize　the　bimetallic　COF　(termed　PBCOFRuRe)　through　in　situ　Schiff-base　condensation　of　Pyrene　with　MBpy　(M　=　Ru,　Re)　units.　In　this　structure,　Ru　and　Re　are　anchored　within　bipyridine　as　the　photosensitive　center　and　catalytic　site,　respectively.　The　bimetallic　architecture　of　PBCOFRuRe　significantly　boosts　the　photocatalytic　efficiency　for　CO2　reduction,　achieving　an　impressive　CO　yield　of　8306.6 µmol　g−1 h−1　with　99.8%　selectivity,　surpassing　most　reported　COF　materials.　This　improvement　is　attributed　to　the　localized　ultrafast　charge　transfer　(0.23 ps)　from　Ru　to　Re,　as　demonstrated　by　femtosecond　transient　absorption　spectroscopy　(TAS).　Further　investigations　demonstrate　its　heterogeneous　feature,　showcasing　exceptional　long-term　stability　and　recyclability.　This　study　represents　a　versatile　approach　for　designing　bimetallic　COFs　with　ultrafast　charge　transfer,　paving　the　pathway　for　advancements　in　artificial　photosynthesis.　©　2025　Wiley-VCH　GmbH.

Keyword：

charge transfer CO2 photoreduction covalent organic frameworks heterogeneous photocatalyst

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[ 1 ] [Liu J.]State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 2 ] [Liu J.]College of Chemistry, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 3 ] [Liu J.]University of Chinese Academy of Science, Beijing, 100049, China
[ 4 ] [Li J.]State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 5 ] [Li J.]University of Chinese Academy of Science, Beijing, 100049, China
[ 6 ] [Li J.]College of Life Science, Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fujian, Fuzhou, 350108, China
[ 7 ] [Lin Z.]College of Life Science, Fujian Agriculture and Forestry University, Fujian, Fuzhou, 350002, China
[ 8 ] [Ye S.]State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 9 ] [Ye S.]University of Chinese Academy of Science, Beijing, 100049, China
[ 10 ] [Lin W.]State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 11 ] [Lin W.]University of Chinese Academy of Science, Beijing, 100049, China
[ 12 ] [Yang X.]State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 13 ] [Yang X.]University of Chinese Academy of Science, Beijing, 100049, China
[ 14 ] [Gao S.-Y.]State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 15 ] [Gao S.-Y.]College of Chemistry, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 16 ] [Gao S.-Y.]University of Chinese Academy of Science, Beijing, 100049, China
[ 17 ] [Cao R.]State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 18 ] [Cao R.]College of Chemistry, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 19 ] [Cao R.]University of Chinese Academy of Science, Beijing, 100049, China
[ 20 ] [Cao R.]College of Life Science, Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fujian, Fuzhou, 350108, China

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ISSN： 1613-6810

Year： 2025

Issue： 7

Volume： 21

1 3 . 0 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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