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Efficient selective aerobic oxidation of sulfides by molecular dipole modulation in methylphosphate-substituted perylene diimide supramolecular polarization photocatalyst.
Liu, Lin; Song, Ru; Wu, Yan; Song, Xiaoming; Song, Jiarui; Chen, Mo; Nie, Yina; Wang, Chengming; Wan, Jun.
Afiliación
  • Liu L; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China. Electronic address: liulin_0731@163.com.
  • Song R; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China.
  • Wu Y; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China.
  • Song X; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China.
  • Song J; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China.
  • Chen M; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China.
  • Nie Y; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China.
  • Wang C; Instruments Center for Physical Science, University of Science and Technology of China, Hefei, Anhui 230026, China.
  • Wan J; College of Chemistry & Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Yan'an University, Yan'an 716000, China. Electronic address: wjun1217@163.com.
J Colloid Interface Sci ; 663: 775-786, 2024 Jun.
Article en En | MEDLINE | ID: mdl-38442519
ABSTRACT
Photocatalytic aerobic oxidation is a promising sustainable strategy for the selective organic synthesis of industrially valuable chemicals. However, the poor charge separation and insufficient molecular activation restrict the overall photocatalytic efficiency. To address these issues, we have developed a novel approach involving molecular dipole modulation and polar molecular self-assembly to modulate the built-in electric field (BEF) in perylene diimide (PDI) supramolecular polarization photocatalysts by adjusting the electronegativity of terminal substituents. The optimized methylphosphate-substituted PDI (P-PDIP) supramolecular system features the strongest BEF induced by its large molecular dipole, with an intensity 3.89 times higher than that observed in methylcarboxy-substituted PDI (P-PDIC) and 5.64 times higher than that observed in P-PDI. This significant enhancement in BEF generates a powerful driving force within P-PDIP, facilitating directional charge separation toward active sites. Additionally, the incorporation of methylphosphate groups improves the activation efficiency of O2 and thioether molecules, resulting in a remarkable photocatalytic performance for selective aerobic oxidation of sulfides into sulfoxide (up to 99.9% conversion and 99.8% selectivity). This study highlights that enhancing BEF through manipulating molecular dipoles can significantly improve photocatalytic activity, offering great potential for constructing efficient organic polarization photocatalysts in green chemistry and sustainable production.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Colloid Interface Sci Año: 2024 Tipo del documento: Article Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Colloid Interface Sci Año: 2024 Tipo del documento: Article Pais de publicación: Estados Unidos