Structure and Reactivity of sol–gel V/SiO2 Catalysts for the Direct Conversion of Methane to Formaldehyde

[EN] Vanadium oxide-silica catalysts prepared by the sol–gel method were characterized by different techniques (nitrogen adsorption–desorption isotherms, scanning electron microscopy, X-ray diffraction, temperature-programmed reduction, Raman spectroscopy and X-ray photoelectron spectroscopy) and ap...

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Detalles Bibliográficos
Autores: Loricera, Cristina V., Álvarez Galván, María Consuelo, Guil López, Ruth, Ismail, A. A., Al-Sayari, S. A., García Fierro, José Luis
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2017
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/202757
Acceso en línea:http://hdl.handle.net/10261/202757
Access Level:acceso abierto
Palabra clave:Vanadium catalysts
Methane/formaldehyde
Methane conversion
Sol-gel
Direct processes
Descripción
Sumario:[EN] Vanadium oxide-silica catalysts prepared by the sol–gel method were characterized by different techniques (nitrogen adsorption–desorption isotherms, scanning electron microscopy, X-ray diffraction, temperature-programmed reduction, Raman spectroscopy and X-ray photoelectron spectroscopy) and applied in the direct conversion of methane to C1 oxygenates. The addition of a small amount of nitric oxide to the reaction mixture reduced the energy barrier for H-abstraction, increasing the methane conversion and formaldehyde yield. Correlations between the characterization and activity results indicate that the reaction occurs on tetrahedrally coordinated vanadium sites, as the maximum formaldehyde yield was found for the catalyst with a vanadium content of 1.5 wt%, which has a high surface density of well-dispersed tetrahedrally coordinated monomeric or slightly oligomerized VO species. On the other hand, a high space velocity and CH:O ratio decrease the subsequent oxidation to carbon oxides, increasing oxygenate formation.