Abstract Two series of sulfated zirconia-ceria based catalysts have been prepared by coprecipitation of the Zr 4+ and Ce 3+ salts, which were then sulfated by impregnation using H 2… Click to show full abstract
Abstract Two series of sulfated zirconia-ceria based catalysts have been prepared by coprecipitation of the Zr 4+ and Ce 3+ salts, which were then sulfated by impregnation using H 2 SO 4 and [(NH 4 ) 2 S 2 O 8 ] and calcined at 650 °C for 4 h. The sulfated and persulfated Zr-Ce-O samples were synthesized with Zr/Ce ratios ranging from 1 to 15. The textural, structural and surface characteristics of the resulting modified catalysts were determined by N 2 adsorption-desorption, XRD, XPS spectroscopy and TPD of NH 3 , and results were related to their catalytic behaviour. The catalysts were tested in the direct conversion of methane at high temperature (650 °C) under fuel-rich conditions to obtain C 1 oxygenates (CH 3 OH and HCHO). Experiments were conducted using low O 2 /CH 4 ratio mixtures and high space velocity. It was shown that O 2 /CH 4 feeds resulted in practically total combustion of CH 4 when sulfated/persulfated ceria-zirconia catalysts are used, while the nature of the different phases modifies the surface acidity, which plays a crucial role on the extent of deep oxidation reactions.
               
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