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Fe/SiO2 catalysts for the selective oxidation of methane to formaldehyde
Catalizadores Fe/SiO2 para la oxidación selectiva de metano hasta formaldehído
DOI:
https://doi.org/10.15446/ing.investig.v26n2.14735Keywords:
Fe/Si0 catalyst, formaldehyde, selective oxidation, sol-gel (en)catalizadores Fe/Si0, formaldehído, oxidación selectiva, sol-gel (es)
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Selective oxidation of methane to formaldehyde was analysed with iron catalysts supported on silica prepared by the sol-gel method, leading to obtaining a large support surface area facilitating high dispersion of iron on silica’s amorphous surface. Seven catalysts were prepared; one of them corresponded to the silica support and another five having an iron load 0.1-0.5% in weight. Catalyst 7 (0.5% Fe in weight) was prepared with neutral pH control and had the most homogeneous characteristics since it did not present isolated iron species, corroborated by SEM and TEM analysis. The highest BET areas were 1,757 and 993 m2.g-1 for 0.5% Fe catalysts, having an average 36% microporosity and 43% mesoporosity. X-ray diffraction confirmed the catalyst’s amorphous structure. Catalytic activity was carried out with catalyser 7 at atmospheric pressure in a quartz reactor using a CH4/O2/N2=7.5/1/4 reaction mixture at 400-750°C temperature range. Reaction products were analysed by gas chromatography with TCD. The heterogeneous catalysts displayed greater methane conversion (but with methanol selectivity) whereas homogenous catalyst 7 gave better results regarding formaldehyde. The highest conversion percentage (8.60% mol) for catalyser 7 was presented at 650°C. Formaldehyde selectivity was 50% mol in the 600-650°C range and maximum yield (0.31g HCHO/Kg catalyst) was found in this range; it was thus considered that 650°C for the reaction was thereby the best operating temperature.
La oxidación selectiva de metano a formaldehido fue analizada con catalizadores de hierro soportados sobre sílice preparados por el método sol-gel, el cual permite obtener gran área superficial del soporte facilitando una alta dispersión del hierro sobre la matriz amorfa de la sílice. Se prepararon siete (7) catalizadores, uno de ellos correspondiente al soporte de sílice, otros cinco (5) con cargas de hierro entre 0,1-0,5 % en peso. El catalizador No.7 (0,5% Fe en peso) se prepara con control de pH neutro y resultó de características más homogéneas ya que no se presentaron especies aisladas de hierro, corroborado por análisis SEM y TEM. Las áreas BET mayores son del orden de 1 757 y 993 m2.g-1 para los catalizadores de 0,5% Fe, con porcentajes promedio del 36% de microporosidad y 43% de mesoporosidad. La difracción de rayos X confirma la estructura amorfa del catalizador. La actividad catalítica es realizada con el catalizador No. 7 a presión atmosférica en reactor de cuarzo, mezcla de reacción CH4/O2/N2 =7.5/1/4, intervalo de temperatura 400-750°C. Los productos de reacción son analizados por cromatografía de gases con TCD. Los catalizadores heterogéneos presentan mayor conversión de metano pero con selectividad al metanol, mientras que el catalizador homogéneo No. 7 da mejores resultados en formaldehido. Para el catalizador 7, el porcentaje más alto de conversión (8,60 mol%) se presenta a 650°C. La selectividad al formaldehido está en 50 mol% entre 600-650°C y en este intervalo se encuentra el máximo rendimiento (0,31 g HCHO/kg catalizador), considerando así que la temperatura de operación es de 650°C.
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1. William Giovanni Cortés-Ortiz, Alexander Baena-Novoa, Carlos Alberto Guerrero-Fajardo. (2019). Structuring-agent role in physical and chemical properties of Mo/SiO2 catalysts by sol-gel method. Journal of Sol-Gel Science and Technology, 89(2), p.416. https://doi.org/10.1007/s10971-018-4892-7.
2. Carlos Alberto Guerrero Fajardo, Francisco José Sánchez Castellanos. (2009). Synthesising Fe-Mo catalysts supported on silica for the selective oxidation of methane to formaldehyde. Ingeniería e Investigación, 29(1), p.53. https://doi.org/10.15446/ing.investig.v29n1.15143.
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Copyright (c) 2006 Carlos Alberto Guerrero Fajardo, Yvonne N’Guyen, Claire Courson, Anne Cécile Roger
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