Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
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INVESTIGACIONMetadades
Títol
Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic ConditionsAutoria
Data de publicació
2021Editor
American Chemical SocietyISSN
2168-0485Cita bibliogràfica
Sorribes, I., Ventura-Espinosa, D., Assis, M., Martín, S., Concepción, P., Bettini, J., Longo, E., Mata, J.A., Andrés, J. Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions. ACS Sustainable Chemistry and Engineering, 2021, 9, 7, 2912–2928Tipus de document
info:eu-repo/semantics/articleVersió
info:eu-repo/semantics/submittedVersionParaules clau / Matèries
Resum
Herein, a novel silver and chromium nanostructured N-doped carbonaceous material has been synthesized by a biomass-annealing approach using readily available chitosan as a raw material. The resulting catalyst AgCr@CN-800 ... [+]
Herein, a novel silver and chromium nanostructured N-doped carbonaceous material has been synthesized by a biomass-annealing approach using readily available chitosan as a raw material. The resulting catalyst AgCr@CN-800 has been applied for the dehydrogenative coupling reaction of various silanes with different alcohols to obtain the corresponding silyl ethers under aerobic and mild conditions. Besides excellent activity and selectivity, the as-prepared catalyst exhibits good stability and reusability. Characterization by XRD, XPS, ICP-MS, HRTEM, in combination with careful examination of the structure with Cs-corrected HAADF-STEM revealed that catalyst AgCr@CN-800 comprises Ag and CrN aggregated particles, as well as highly dispersed Ag-Nx and Cr-Nx sites embedded in N-doped graphitic structures. A comparative catalytic study using structure-related catalysts in combination with acid-leaching treatments has shown that the most active species are the Ag particles, and that their activity is boosted by the presence of Cr-derived species. By in-situ Raman spectroscopy experiments, it has been found that the dehydrogenative coupling of silanes with alcohols in the presence of catalyst AgCr@CN-800 takes place through an oxygen-assisted mechanism. [-]
Publicat a
ACS Sustainable Chemistry and Engineering, 2021Entitat finançadora
MICIU/AEI/FEDER: PGC2018-094417-B-I00 and RTI2018-098237-B-C22; Universitat Jaume I: UJI-A2019-16, UJI-B2019-30, and UJI-B2018-23; Spanish Ministerio de Economía, Industria y Competitividad (MINECO) for a postdoctoral “Juan de la Cierva-Incorporación”: IJCI-2016-30590; “José Castillejo” Mobility Program: CAS19/00339) of the Ministerio de Ciencia, Innovación y Universidades (MICIU); DGA/fondos FEDER (construyendo Europa desde Aragón) for funding the research group Platón (E31_17R); MICIU for a FPU grant: FPU15/03011; FAPESP: 2013/07296-2; CNPq: 166281/2017-4; CAPES; FINEP
Drets d'accés
http://rightsstatements.org/vocab/CNE/1.0/
info:eu-repo/semantics/openAccess
info:eu-repo/semantics/openAccess
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