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Synthesising Fe-Mo catalysts supported on silica for the selective oxidation of methane to formaldehyde
Síntesis de catalizadores de Fe-Mo soportados sobre sílice para la oxidación selectiva de metano hasta formaldehído
DOI:
https://doi.org/10.15446/ing.investig.v29n1.15143Keywords:
Fe-Mo/SiO2 catalysts, formaldehyde, selective oxidation, sol-gel (en)catalizadores Fe-Mo/SiO2, formaldehido, oxidación selectiva, sol-gel (es)
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The selective oxidation of methane to formaldehyde was analysed using iron-molybdenum catalysts supported on silica prepared by the sol-gel method which leads to obtaining a greater surface area and high iron and molybdenum metal dispersion on the silica’s amorphous surface. Seven catalysts were prepared, one of them as silica support, another as 0.5% wt iron load without molybdenum and the remaining five having 0.1%-1.0% weight molybdenum and 0.5% wt iron loads. The highest BET areas were 830 and 879 m2.g-1 for catalysts 2 (0.5% Fe - 0% Mo) and 4 (0.5% Fe - 0.3% Mo) respectively, having 28% average microporosity and 47% average mesoporosity. X-ray diffraction confirmed the catalysts’ amorphous structure. The TPR spectrum showed low hydrogen consumption attributed to the absence of isolated Fe and Mo species. ESCA analysis revealed the same Fe/Mo atomic ratio on the catalyst surface as in the bulk preparation. Catalytic activity was carried out at atmospheric pressure, CH4/ O2/N2 = 7.5/1/4 reaction mixture, 400-800°C temperature interval. Catalysts 4 (0.5% Fe - 0.3% Mo), 5 (0.5% Fe - 0.5% Mo) and 7 (0.5% Fe - 1.0% Mo) displayed greater methane conversion, whereas catalysts 5 (0.5% Fe - 0.5% Mo), 4 (0.5% Fe - 0.3% Mo), 2 (0.5% Fe - 0% Mo) and 7 (0.5% Fe - 1.0% Mo) gave better formaldehyde product results. The highest conversion per-centage (4.07% mol) was presented at 700°C for catalyst 4 (0.5% Fe-0.3% Mo). Formaldehyde yield was 202,0 gHCHO.kg-1cata.h-1 at this temperature.
Materiales de hierro-molibdeno soportados sobre sílice fueron obtenidos por el método sol-gel para evaluar su actividad catalítica en la reacción de oxidación selectiva de metano hasta formaldehído. Este método permite obtener un área superficial extensa y una alta dispersión de los metales sobre la superficie amorfa de la sílice. Se prepararon siete (7) catalizadores, uno del soporte de sílice, otro con carga de Fe 0,5% sin molibdeno, y los otros cinco (5) con la misma carga de Fe 0,5% pero con cargas variables de molibdeno entre 0,1-1,0% en peso. Las mayores áreas BET fueron del orden de 830 y 879 m2.g-1 para los catalizadores 2 (Fe0,5%-Mo0%) y 4 (Fe0,5%-Mo0,3%), con porcentajes promedio de 28% de microporosidad y 47% de mesoporosidad. La difracción de rayos X confirma la estructura amorfa de los catalizadores. El espectro TPR mostró bajo consumo de hidrógeno, atribuido a la ausencia de especies aisladas de Fe y Mo. El análisis ESCA registró la misma relación atómica Fe/Mo en la superficie del catalizador como en el bulk. La actividad catalítica es determinada a presión atmosférica, con mezcla de reacción CH4/O2/N2 =7.5/1/4, intervalo de temperatura 400-800 °C. Los catalizadores 4 (Fe0,5%-Mo0,3%), 5 (Fe0,5%-Mo0,5%) y 7 (Fe0,5%-Mo1,0%) presentan la mayor conversión de metano, mientras los catalizadores 5 (Fe0,5%-Mo0,5%), 4 (Fe0,5%-Mo0,3%), 2 (Fe0,5%-Mo0%) y 7 (Fe0,5%-Mo1,0%) dan los mejores resultados de producción de formaldehído. Para el catalizador 4 (Fe0,5%-Mo0,3%), la mayor conversión (4,07 mol%) se presenta a 700 °C. A esta temperatura la producción de formaldehído es de 202,0 gHCHO.kg-1cata.h-1.
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Copyright (c) 2009 Carlos Alberto Guerrero Fajardo, Francisco José Sánchez Castellanos
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