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

[EN] 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 sila...

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Autores: Sorribes-Terrés, Iván, Ventura-Espinosa, David, Assis, Marcelo, Martin, Santiago, Bettini, Jefferson, Longo, Elson, Mata, Jose A., Andrés, Juan, Concepción Heydorn, Patricia|||0000-0003-2058-3103
Tipo de recurso: artículo
Fecha de publicación:2021
País:España
Institución:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:riunet.upv.es:10251/201121
Acceso en línea:https://riunet.upv.es/handle/10251/201121
Access Level:acceso abierto
Palabra clave:Chitosan
Silanes
Alcohols
Dehydrogenative coupling
Silyl ethers
Oxygen activation
In situ Raman spectroscopy
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dc.title.none.fl_str_mv Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
title Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
spellingShingle Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
Sorribes-Terrés, Iván
Chitosan
Silanes
Alcohols
Dehydrogenative coupling
Silyl ethers
Oxygen activation
In situ Raman spectroscopy
title_short Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
title_full Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
title_fullStr Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
title_full_unstemmed Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
title_sort Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic Conditions
dc.creator.none.fl_str_mv Sorribes-Terrés, Iván
Ventura-Espinosa, David
Assis, Marcelo
Martin, Santiago
Bettini, Jefferson
Longo, Elson
Mata, Jose A.
Andrés, Juan
Concepción Heydorn, Patricia|||0000-0003-2058-3103
author Sorribes-Terrés, Iván
author_facet Sorribes-Terrés, Iván
Ventura-Espinosa, David
Assis, Marcelo
Martin, Santiago
Bettini, Jefferson
Longo, Elson
Mata, Jose A.
Andrés, Juan
Concepción Heydorn, Patricia|||0000-0003-2058-3103
author_role author
author2 Ventura-Espinosa, David
Assis, Marcelo
Martin, Santiago
Bettini, Jefferson
Longo, Elson
Mata, Jose A.
Andrés, Juan
Concepción Heydorn, Patricia|||0000-0003-2058-3103
author2_role author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Instituto Universitario Mixto de Tecnología Química
Gobierno de Aragón
Universitat Jaume I
Diputación General de Aragón
Agencia Estatal de Investigación
European Regional Development Fund
Financiadora de Estudos e Projetos, Brasil
Ministerio de Educación, Cultura y Deporte
Ministerio de Ciencia, Innovación y Universidades
Fundação de Amparo à Pesquisa do Estado de São Paulo
Coordenaçao de Aperfeiçoamento de Pessoal de Nível Superior, Brasil
Repositorio Institucional de la Universitat Politècnica de València Riunet
dc.subject.none.fl_str_mv Chitosan
Silanes
Alcohols
Dehydrogenative coupling
Silyl ethers
Oxygen activation
In situ Raman spectroscopy
topic Chitosan
Silanes
Alcohols
Dehydrogenative coupling
Silyl ethers
Oxygen activation
In situ Raman spectroscopy
description [EN] 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.
publishDate 2021
dc.date.none.fl_str_mv 2021
2021-02-22
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
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dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://riunet.upv.es/handle/10251/201121
url https://riunet.upv.es/handle/10251/201121
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 PGC2018-094417-B-I00 APROXIMACIONES RACIONALES PARA EL DISEÑO DE NUEVOS MATERIALES MEDIANTE LA COMBINACION DE TEORIA Y EXPERIMENTO
Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 RTI2018-098237-B-C22 FUNCIONALIZACION DE GRAFENO CON COMPLEJOS METALICOS DEFINIDOS EN TRANSFORMACIONES CATALITICAS SOSTENIBLES: ALMACENAMIENTO DE HIDROGENO Y CONVERSION DE BIOMASA
Ministerio de Educación y Cultura http://dx.doi.org/10.13039/501100003176 FPU15%2F03011 FPU15%2F03011
Diputación General de Aragón DGA E31_17R
Fundação de Amparo à Pesquisa do Estado de São Paulo https://doi.org/10.13039/501100001807 2013%2F07296-2
Ministerio de Ciencia, Innovación y Universidades https://doi.org/10.13039/100014440 IJCI-2016-30590
Ministerio de Ciencia, Innovación y Universidades https://doi.org/10.13039/100014440 CAS19%2F00339
Universitat Jaume I https://doi.org/10.13039/501100004834 RTI2018-098237-B-C22
Universitat Jaume I https://doi.org/10.13039/501100004834 UJI-B2018-23
Universitat Jaume I https://doi.org/10.13039/501100004834 UJI-B2019-30
Universitat Jaume I https://doi.org/10.13039/501100004834 UJI-A2019-16
Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 PGC2018-094417-B-I00 APROXIMACIONES RACIONALES PARA EL DISEÑO DE NUEVOS MATERIALES MEDIANTE LA COMBINACION DE TEORIA Y EXPERIMENTO
Coordenaçao de Aperfeiçoamento de Pessoal de Nível Superior, Brasil https://doi.org/10.13039/501100002322 166281%2F2017-4
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reserva de todos los derechos
http://rightsstatements.org/vocab/InC/1.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reserva de todos los derechos
http://rightsstatements.org/vocab/InC/1.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
instname:Universitat Politècnica de València (UPV)
instname_str Universitat Politècnica de València (UPV)
reponame_str RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
collection RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
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spelling Unraveling a Biomass-Derived Multiphase Catalyst for the Dehydrogenative Coupling of Silanes with Alcohols under Aerobic ConditionsSorribes-Terrés, IvánVentura-Espinosa, DavidAssis, MarceloMartin, SantiagoBettini, JeffersonLongo, ElsonMata, Jose A.Andrés, JuanConcepción Heydorn, Patricia|||0000-0003-2058-3103ChitosanSilanesAlcoholsDehydrogenative couplingSilyl ethersOxygen activationIn situ Raman spectroscopy[EN] 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.The authors thank the financial support from MICIU/AEI/FEDER (PGC2018-094417-B-I00 and RTI2018-098237-B-C22) and Universitat Jaume I (UJI-A2019-16, UJI-B2019-30, and UJI-B2018-23). I.S. thanks the Spanish Ministerio de Economia, Industria y Competitividad (MINECO) for a postdoctoral "Juan de la Cierva-Incorporacion" fellowship (IJCI-2016-30590), and the financial support from the "Jose Castillejo" Mobility Program (CAS19/00339) of the Ministerio de Ciencia, Innovacion y Universidades (MICIU). S.M. acknowledges DGA/fondos FEDER (construyendo Europa desde Aragon) for funding the research group Platon (E31_17R). D.V.-E. thanks the MICIU for a FPU grant (FPU15/03011). E.L. and M.A. thank the financial support from FAPESP (2013/07296-2), CNPq (166281/2017-4), CAPES, and FINEP. The authors also thank the "Servei Central d'Instrumentacio Cientifica (SCIC)" of the Universitat Jaume I, as well as Dr. G. Antorrena for technical support in XPS studies.American Chemical SocietyInstituto Universitario Mixto de Tecnología QuímicaGobierno de AragónUniversitat Jaume IDiputación General de AragónAgencia Estatal de InvestigaciónEuropean Regional Development FundFinanciadora de Estudos e Projetos, BrasilMinisterio de Educación, Cultura y DeporteMinisterio de Ciencia, Innovación y UniversidadesFundação de Amparo à Pesquisa do Estado de São PauloCoordenaçao de Aperfeiçoamento de Pessoal de Nível Superior, BrasilRepositorio Institucional de la Universitat Politècnica de València Riunet20212021-02-22journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfapplication/pdfhttps://riunet.upv.es/handle/10251/201121reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valénciainstname:Universitat Politècnica de València (UPV)InglésengAgencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 PGC2018-094417-B-I00 APROXIMACIONES RACIONALES PARA EL DISEÑO DE NUEVOS MATERIALES MEDIANTE LA COMBINACION DE TEORIA Y EXPERIMENTOAgencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 RTI2018-098237-B-C22 FUNCIONALIZACION DE GRAFENO CON COMPLEJOS METALICOS DEFINIDOS EN TRANSFORMACIONES CATALITICAS SOSTENIBLES: ALMACENAMIENTO DE HIDROGENO Y CONVERSION DE BIOMASAMinisterio de Educación y Cultura http://dx.doi.org/10.13039/501100003176 FPU15%2F03011 FPU15%2F03011Diputación General de Aragón DGA E31_17RFundação de Amparo à Pesquisa do Estado de São Paulo https://doi.org/10.13039/501100001807 2013%2F07296-2Ministerio de Ciencia, Innovación y Universidades https://doi.org/10.13039/100014440 IJCI-2016-30590Ministerio de Ciencia, Innovación y Universidades https://doi.org/10.13039/100014440 CAS19%2F00339Universitat Jaume I https://doi.org/10.13039/501100004834 RTI2018-098237-B-C22Universitat Jaume I https://doi.org/10.13039/501100004834 UJI-B2018-23Universitat Jaume I https://doi.org/10.13039/501100004834 UJI-B2019-30Universitat Jaume I https://doi.org/10.13039/501100004834 UJI-A2019-16Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 PGC2018-094417-B-I00 APROXIMACIONES RACIONALES PARA EL DISEÑO DE NUEVOS MATERIALES MEDIANTE LA COMBINACION DE TEORIA Y EXPERIMENTOCoordenaçao de Aperfeiçoamento de Pessoal de Nível Superior, Brasil https://doi.org/10.13039/501100002322 166281%2F2017-4open accesshttp://purl.org/coar/access_right/c_abf2Reserva de todos los derechoshttp://rightsstatements.org/vocab/InC/1.0/info:eu-repo/semantics/openAccessoai:riunet.upv.es:10251/2011212026-06-13T07:49:27Z
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