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Modifying the Charge-Density of Tetrahedral Cobalt(II) Centers through Carbon-Layer Modulation Promotes C-H Activation in the Propane Dehydrogenation Reaction (PDH).
Huang, Zijun; He, Dedong; Lu, Jichang; Han, Lanfang; Li, Kongzhai; Chen, Dingkai; Cao, Xiaohua; Li, Tan; Luo, Yongming.
Afiliación
  • Huang Z; Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming, 650500, China.
  • He D; Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500, China.
  • Lu J; The Innovation Team for Volatile Organic Compounds Pollutants Control and Resource Utilization of, Yunnan Province, Kunming, 650500, China.
  • Han L; The Higher Educational Key Laboratory for Odorous Volatile Organic Compounds Pollutants Control of Yunnan Province, Kunming, 650500, China.
  • Li K; Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming, 650500, China.
  • Chen D; Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500, China.
  • Cao X; The Innovation Team for Volatile Organic Compounds Pollutants Control and Resource Utilization of, Yunnan Province, Kunming, 650500, China.
  • Li T; The Higher Educational Key Laboratory for Odorous Volatile Organic Compounds Pollutants Control of Yunnan Province, Kunming, 650500, China.
  • Luo Y; Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500, China.
Angew Chem Int Ed Engl ; 63(36): e202408391, 2024 Sep 02.
Article en En | MEDLINE | ID: mdl-39031836
ABSTRACT
The electronic structure of active metal centers plays an indispensable role in regulating catalytic reactivity in heterogeneous catalysis, developing other metals as promoters to decorate electronic state is a common strategy, while non-metal component of carbon as electronic additives to regulate d-band center has rarely been studied in thermal-catalysis field. Herein, we report electron-deficient tetrahedral Co(II) (Td-cobalt(II)) centers through carbon-layer modulation for propane dehydrogenation (PDH). It is indicated that bifunctional sites of both Td-cobalt(II) and metallic-cobalt are designed, and the in situ generated carbon through the disproportionation of CO on metallic-cobalt can cover the inactive metallic-cobalt and tailor d-band of active Td-cobalt(II) simultaneously. More importantly, the pre-deposited carbon-layer is proposed to decrease electron density of Td-cobalt(II) and make d-band center closer to Fermi level, consequently promotes C-H activation in PDH reaction. This study provides new perspective for the utilization of inactive carbon as electronic promoters and unlocks new opportunity to fabricate efficient PDH and other heterogeneous catalysts.
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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 País de afiliación: China 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 País de afiliación: China Pais de publicación: Alemania