Abstract

Microcalorimetric and infrared spectroscopic (FTIR) measurements for the adsorption of ethylene on Pd/SiO2 and Pd/Sn/SiO2 catalysts (4 wt % Pd, Pd/Sn = 3) have been performed at temperatures of 300, 263, and 233 K. In addition, microcalorimetric measurements were made for H2 and CO adsorption and FTIR studies were conducted of CO adsorption at 300 K on these catalysts. Quantum chemical calculations employing density functional theory (DFT) were performed using Pd10 and Pd6Sn4 clusters. Ethylene adsorption on the catalysts results in the formation of ethylidyne species, di-σ-bonded ethylene, and π-bonded ethylene species at 300 K, with initial heats of adsorption of 160 and 110 kJ/mol for the Pd and Pd/Sn catalysts, respectively. Only di-σ-bonded ethylene and π-bonded ethylene species form at 263 and 233 K, with the π-bonded ethylene species dominating. The initial heats of ethylene adsorption are equal to 110 and 102 kJ/mol on Pd/SiO2 at 263 and 233 K, respectively; and these values are equal to 90 and 85...

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