Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions

Autor(es)

Sorribes, Ivan ^[1] ; Ventura-Espinosa, David ^[2] ; Assis, Marcelo ^[3] ; Martin, Santiago ^{[4, 5]} ; Concepcion, Patricia ^[6] ; Bettini, Jefferson ^[7] ; Longo, Elson ^[3] ; Mata, Jose A. ^[2] ; Andres, Juan ^[1]

Afiliação do(s) autor(es)

^[1] Univ Jaume 1, Dept Quim Fis & Analit, Castellon de La Plana 12071 - Spain

^[2] Univ Jaume 1, Inst Adv Mat INAM, Castellon de La Plana 12071 - Spain

^[3] Univ Fed Sao Carlos, Ctr Dev Funct Mat CDMF, BR-13565905 Sao Carlos, SP - Brazil

^[4] Univ Zaragoza, Inst Nanociencia & Mat Aragon INMA, CSIC, Zaragoza 50009 - Spain

^[5] Univ Zaragoza, Dept Quim Fis, Zaragoza 50009 - Spain

^[6] Univ Politecn Valencia, Inst Tecnol Quim, CSIC, Valencia 46022 - Spain

^[7] Brazilian Nanotechnol Natl Lab LNNano, BR-13083970 Campinas, SP - Brazil

• Tipo de documento: Artigo Científico
• Fonte: ACS SUSTAINABLE CHEMISTRY & ENGINEERING; v. 9, n. 7, p. 2912-2928, FEB 22 2021.
• Citações Web of Science: 0

Resumo

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 X-ray diffraction, X-ray photo-electron spectroscopy, inductively coupled plasma mass spectrometry, and high-resolution transmission electron microscopy (TEM) in combination with careful examination of the structure with Cs-corrected high-angle annular dark-field scanning TEM revealed that the catalyst AgCr@CN-800 comprises Ag- and CrN-aggregated particles, as well as highly dispersed Ag-N-x and Cr-N-x 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. (AU)

• Processo FAPESP: 13/07296-2 - CDMF - Centro de Desenvolvimento de Materiais Funcionais
• Beneficiário: Elson Longo da Silva
• Modalidade de apoio: Auxílio à Pesquisa - Centros de Pesquisa, Inovação e Difusão - CEPIDs