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Insight into the Molecular Mechanism for Enhanced Longevity of Supramolecular Vesicular Photocatalysts.
Liu, Yannan; Zheng, Fulu; Dai, Haojie; Chen, Chuanshuang; Chen, Yajing; Wu, Haolin; Yu, Chunyang; Mai, Yiyong; Frauenheim, Thomas; Zhou, Yongfeng.
  • Liu Y; School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, P. R. China.
  • Zheng F; Center for Advancing Electronics Dresden (cfaed), Technische Universität Dresden, 01062, Dresden, Germany.
  • Dai H; Bremen Center for Computational Materials Science, University of Bremen, Am Fallturm 1, 28359, Bremen, Germany.
  • Chen C; School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, P. R. China.
  • Chen Y; School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, P. R. China.
  • Wu H; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing, 100190, P. R. China.
  • Yu C; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing, 100190, P. R. China.
  • Mai Y; School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, P. R. China.
  • Frauenheim T; School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, P. R. China.
  • Zhou Y; Shenzhen JL Computational Science and Applied Research Institute, Shenzhen, 518110, China.
Angew Chem Int Ed Engl ; 62(23): e202302126, 2023 Jun 05.
Article en En | MEDLINE | ID: mdl-37051748
ABSTRACT
Supramolecular self-assembly is a promising strategy for stabilizing the photo-sensitive components in photocatalysis. However, the underlying correlation between the enhanced photostability and supramolecular structure at the molecular level has not yet been fully understood. Herein, we develop a biomimetic vesicular membrane-based polyporphyrin photocatalyst exhibiting excellent photocatalytic stability with at least activity time of 240 h in hydrogen generation. Time-domain ab initio modelling together with transient absorption spectroscopy, visual frontier orbitals and Gibbs free energy calculation disclose that the ordered aggregation of porphyrin units in the vesicle membrane facilitates "hot" electron relaxation and the rapid dissipation of photo-generated charges, thereby contributing to the longevity. This work deepens the molecular-level understanding on photostability and photocatalytic mechanism of supramolecular photocatalysts.
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Texto completo: 1 Banco de datos: MEDLINE Idioma: En Año: 2023 Tipo del documento: Article
Texto completo
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PubMed Links
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Texto completo: 1 Banco de datos: MEDLINE Idioma: En Año: 2023 Tipo del documento: Article