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Adsorption and Microcalorimetric Measurements on the Interaction of CO and H2 with Polycrystalline Ru and Ru/TiO2 Catalyst
A microcalorimeter equipped with gas circulation cells and coupled at outlet to a gas chromatograph was used for the simultaneous measurements of the uptake and the differential heat (qd) evolved during the adsorption of CO and H2 pulses over polycrystalline ruthenium metal and a RuTiO2 catalyst in the temperature range 300-475 K and as a function of surface coverage. The initial differential heat for the adsorption of CO and H2 over polycrystalline ruthenium at 300 K was 120 and 65 kJ mol-1, respectively, the corresponding values in the case of RuTiO2 being around 130 and 57 kJ mol-1. With the rise in sample temperature, the qd for CO adsorption over Ru metal remained almost constant, while in the case of Ru/TiO2 it decreased substantially. The fraction of CO or H2 adsorbed, conversion of COad to CO2, and the corresponding values of heat evolved showed different trends, when these samples were exposed to the successive CO or H2 pulses at different temperatures. The H2 adsorption is found to be suppressed on Ru/TiO2, particularly at the low sample temperatures. Also, the CO adsorption over Ru/TiO2 at temperatures above 400 K resulted in the partial reduction of the support, and this is facilitated by the heat evolved at the metal/support interfaces during CO chemisorption. On the other hand, the CO dissociation followed by CO(ad) + O(ad) reaction was a predominant step giving rise to CO2 formation in the case of Ru metal. This study also confirms that, for both the samples, while the CO adsorption remains uninhibited by the preadsorbed H2, the catalyst surface covered with the CO was completely inaccessible to subsequent H2 adsorption.
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Reference£º
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI