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Structural Conjugation Tuning in Covalent Organic Frameworks Boosts Charge Transfer and Photocatalysis Performances.
Lin, Qihan; Yusran, Yusran; Xing, Jiabin; Li, Yongsheng; Zhang, Jiangshan; Su, Tianhui; Yang, Lingyi; Suo, Jinquan; Zhang, Liming; Li, Qiaowei; Wang, Hui; Fang, Qianrong; Li, Zhan-Ting; Zhang, Dan-Wei.
Afiliação
  • Lin Q; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Yusran Y; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Xing J; Department of Chemistry, State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.
  • Li Y; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Zhang J; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Su T; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Yang L; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Suo J; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Zhang L; Department of Chemistry, State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.
  • Li Q; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Wang H; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Fang Q; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
  • Li ZT; Department of Chemistry, State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.
  • Zhang DW; Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
ACS Appl Mater Interfaces ; 16(5): 5869-5880, 2024 Feb 07.
Article em En | MEDLINE | ID: mdl-38277475
ABSTRACT
Structural conjugation greatly affects the optical and electronic properties of the COF photocatalyst. Herein, we show that 2D hydrazone COFs with either π-extended biphenyl (BPh-COF) or acetylene (AC-COF) frameworks demonstrated distinct charge transfer and photocatalytic performances. The two COFs show good crystallinity and decent porosity as their frameworks are enforced by intra/interlayers hydrogen bonding. However, computational and experimental data reveal that AC-COF managed broader visible-light absorption and narrower optical bandgaps and performed efficient photoinduced charge separation and transfer in comparison with BPh-COF, meaning that the ethynyl skeleton with enhanced planarity better improves the π-conjugation of the whole structure. As a result, AC-COF exhibited an ideal bandgap for rapid oxidative coupling of amines under visible-light irradiation. Furthermore, taking advantage of its better charge transfer properties, AC-COF demonstrated considerable enhanced product conversion and notable functional tolerance for metallaphotocatalytic C-O cross-coupling of a wide range of both aryl bromides and chlorides with alcohols. More importantly, besides being recoverable, AC-COF showcased the previously inaccessible etherification of dihaloarene. This report shows a facile approach for manipulating the structure-activity relationship and paves the way for the development of a COF photocatalyst for solar-to-chemical energy conversion.
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article