ETHYLENE OXIDATION OVER AG AND AG-AU ALLOY CATALYSTS
Abstract
THE MECHANISM OF ETHYLENE EPOXIDATION OVER AG AND AG-AU ALLOY CATALYSTS WAS STUDIED IN ORDER TO EXAMINE THE GEOMETRIC AND ELECTRONIC TYPE EFFECTS INDUCED BY THE PRESENCE OF AU TO THE CHEMISORBING AND CATALYTIC PROPERTIES OF AG. CATALYSTS WERE CHARACTERIZED USING XRD, SEM, XPS AND SELECTIVE CHEMISORPTION MEASUREMENTS. OXYGEN ADSORPTION WAS STUDIED USING SERS, TPD, TPR AND GRAVIMETRIC METHODS. THE THREE ADSORBED OXYGEN SPECIES OBSERVED (ATOMIC, MOLECULAR AND SUBSURFACE) WERE FOUND TO BE STRONGLY AFFECTED BY THE PRESENCE OF AU. KINETIC EXPERIMENTS CONDUCTED IN A WIDE RANGE OF TEMPERATURES AND PARTIAL PRESSURE SHOWED THAT, UPON ALLOYING WITH AU, CATALYTIC ACTIVITY REACHES A MAXIMUM FOR CATALYSTS CONTAINING 5-10% AU AND DROPS TO ZERO FOR SURFACES WITH MORE THAN 40% AU. A MECHANISTIC MODEL FOR ETHYLENE EPOXIDATION OVER AG SURFACES IS PROPOSED AND SUCCESSFULLY TESTED.
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