Abstract

The interaction of methane with the surfaces of silica-, alumina- and titania-supported Pd catalysts has been studied by means of adsorption microcalorimetry and temperature-programmed surface reaction (TPSR) with hydrogen in a flow system at atmospheric pressure. For adsorption temperatures ranging between 300 and 700 K, a complete dissociation of CH 4 occurred which resulted in the formation of C(ads) clusters of different sizes as well as graphitic carbon. The subsequent temperature-programmed hydrogenation of C(ads) mainly produced CH 4 together with trace amounts of C 2H 6 and C 2H 4. With an increasing number of Pd surface atoms, more C(ads) was formed upon contact with CH 4; the reactivity towards hydrogenation was, however, not markedly affected. Compared to Pd/SiO 2, the reactivity of deposited carbon to hydrogenation, the C 2 yield and the C 2H 4/C 2H 6 ratio were higher for Pd/TiO 2 and Pd/Al 2O 3 catalysts, while the tendency for the formation of graphitic carbon was lower.

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