Silvestre Albero, J.; Domine ., ME.; Jorda Moret, JL.; Navarro Villalba, MT.; Rey Garcia, F.; Rodriguez-Reinoso, F.; Corma Canós, A. (2015). Spectroscopic, calorimetric, and catalytic evidences of hydrophobicity on Ti-MCM-41 silylated materials for olefin epoxidations. Applied Catalysis A: General. 507:14-25. https://doi.org/10.1016/j.apcata.2015.09.029
Por favor, use este identificador para citar o enlazar este ítem: http://hdl.handle.net/10251/71399
Título:
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Spectroscopic, calorimetric, and catalytic evidences of hydrophobicity on Ti-MCM-41 silylated materials for olefin epoxidations
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Autor:
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Silvestre Albero, Joaquin
Domine ., Marcelo Eduardo
Jorda Moret, Jose Luis
Navarro Villalba, Mª Teresa
Rey Garcia, Fernando
Rodriguez-Reinoso, Francisco
Corma Canós, Avelino
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Entidad UPV:
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Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química
Universitat Politècnica de València. Departamento de Química - Departament de Química
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Fecha difusión:
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Resumen:
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tHydrophobic Ti-MCM-41 samples prepared by post-synthesis silylation treatment demonstrate to behighly active and selective catalysts in olefins epoxidation by using organic hydroperoxides as oxidizingagents in liquid phase ...[+]
tHydrophobic Ti-MCM-41 samples prepared by post-synthesis silylation treatment demonstrate to behighly active and selective catalysts in olefins epoxidation by using organic hydroperoxides as oxidizingagents in liquid phase reaction systems. Epoxide yields show important enhancements with increasedsilylation degrees of the Ti-mesoporous samples. Catalytic studies are combined and correlated withspectroscopic techniques (e.g. XRD, XANES, UV-Visible,29Si MAS-NMR) and calorimetric measurementsto better understand the changes in the surface chemistry of Ti-MCM-41 samples due to the post-synthesis silylation treatment and to ascertain the role of these trimethylsilyl groups incorporated inolefin epoxidation. In such manner, the effect of the organic moieties on solids, and both water and gly-col molecules contents on the catalytic activity and selectivity are analyzed in detail. Results show thatthe hydrophobicity level of the samples is responsible for the decrease in water adsorption and, conse-quently, the negligible formation of the non-desired glycol during the catalytic process. Thus, catalystdeactivation by glycol poisoning of Ti active sites is greatly diminished, this increasing catalyst stabilityand leading to practically quantitative production of the corresponding epoxide. The extended use ofthese hydrophobic Ti-MCM-41 catalysts together with organic hydroperoxides for the highly efficientand selective epoxidation of natural terpenes is also exemplified.
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Palabras clave:
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Hydrophobic materials
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Ti-MCM-41 catalyst
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Silylation treatment
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Immersion calorimetry
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Catalytic epoxidation
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Derechos de uso:
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Reconocimiento - No comercial - Sin obra derivada (by-nc-nd)
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Fuente:
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Applied Catalysis A: General. (issn:
0926-860X
) (eissn:
1873-3875
)
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DOI:
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10.1016/j.apcata.2015.09.029
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Editorial:
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Elsevier
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Versión del editor:
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http://dx.doi.org/10.1016/j.apcata.2015.09.029
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Código del Proyecto:
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info:eu-repo/grantAgreement/MINECO//MAT2012-38567-C02-01/ES/MATERIALES ZEOLITICOS COMO ESTRUCTURAS ANFITRIONAS DE NANOPARTICULAS. SINTESIS Y APLICACIONES NANOTECNOLOGICAS, CATALITICAS Y MEDIOAMBIENTALES/
...[+]
info:eu-repo/grantAgreement/MINECO//MAT2012-38567-C02-01/ES/MATERIALES ZEOLITICOS COMO ESTRUCTURAS ANFITRIONAS DE NANOPARTICULAS. SINTESIS Y APLICACIONES NANOTECNOLOGICAS, CATALITICAS Y MEDIOAMBIENTALES/
info:eu-repo/grantAgreement/CSIC//2009801063/
info:eu-repo/grantAgreement/MINECO//MAT2013-45008-P/ES/NANOMATERIALES NOVEDOSOS PARA LA CAPTURA Y CONVERSION DE CO2/
info:eu-repo/grantAgreement/MINECO//PCIN-2013-057/ES/ADSORBENTES EQUIPADOS CON NANORADIADORES PARA ALMACENAMIENTO EFICIENTE Y SEGURO DE METANO/
info:eu-repo/grantAgreement/GVA//PROMETEO09%2F2009%2F002/ES/Desarrollo de nanomateriales para aplicaciones energéticas y medioambientales/
info:eu-repo/grantAgreement/MICINN//CSD2009-00050/ES/Desarrollo de catalizadores más eficientes para el diseño de procesos químicos sostenibles y produccion limpia de energia/
info:eu-repo/grantAgreement/MINECO//SEV-2012-0267/ES/SEV-2012-0267/
info:eu-repo/grantAgreement/MICINN//CTQ2011-27550/ES/TRANSFORMACION CATALITICA DE BIOMASA EN DIESEL Y EN PRODUCTOS QUIMICOS/
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Agradecimientos:
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The authors gratefully acknowledge financial support of Spanish Government (MAT2012-38567-C02-01, Consolider-Ingenio 2010-Multicat CSD-2009-00050 and Severo Ochoa SEV-2012-0267) and Generalitat Valenciana (Project Prometeo). ...[+]
The authors gratefully acknowledge financial support of Spanish Government (MAT2012-38567-C02-01, Consolider-Ingenio 2010-Multicat CSD-2009-00050 and Severo Ochoa SEV-2012-0267) and Generalitat Valenciana (Project Prometeo). M.E.D. also thanks funds from Spanish Government (CTQ-2011-27550) and CSIC (PIE 2009801063). J.S.A. and F.R.R. acknowledge financial support from MINECO (Projects MAT2013-45008-p and CONCERT Project-NASEMS (PCIN-2013-057), and from Generalitat Valenciana (PROMETEO2009/002).
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Tipo:
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Artículo
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