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Cyanide-based Covalent Organic Frameworks for Enhanced Overall Photocatalytic Hydrogen Peroxide Production.
Zhou, Enbo; Wang, Futong; Zhang, Xiang; Hui, Yangdan; Wang, Yaobing.
Afiliación
  • Zhou E; CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, Fujian, P. R. China.
  • Wang F; University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
  • Zhang X; CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, Fujian, P. R. China.
  • Hui Y; University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
  • Wang Y; CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, Fujian, P. R. China.
Angew Chem Int Ed Engl ; 63(19): e202400999, 2024 May 06.
Article en En | MEDLINE | ID: mdl-38489230
ABSTRACT
Photocatalytic oxygen reduction to produce hydrogen peroxide (H2O2) is a promising route to providing oxidants for various industrial applications. However, the lack of well-designed photocatalysts for efficient overall H2O2 production in pure water has impeded ongoing research and practical thrusts. Here we present a cyanide-based covalent organic framework (TBTN-COFs) combining 2,4,6-trimethylbenzene-1,3,5-tricarbonitrile (TBTN) and benzotrithiophene-2,5,8-tricarbaldehyde (BTT) building blocks with water-affinity and charge-separation. The ultrafast intramolecular electron transfer (<500 fs) and prolonged excited state lifetime (748 ps) can be realized by TBTN-COF, resulting in a hole accumulated BTT and electron-rich TBTN building block. Under one sun, the 11013 µmol h-1 g-1 yield rate of H2O2 can be achieved without any sacrificial agent, outperforming most previous reports. Furthermore, the DFT calculation and in situ DRIFTS spectrums suggesting a Yeager-type absorption of *O2⋅- intermediate in the cyanide active site, which prohibits the formation of superoxide radical and revealing a favored H2O2 production pathway.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article Pais de publicación: Alemania