Abstract
Rates of C3-C5 ketone hydrogenation are measured in the vapor phase over Ru/SiO2. Reaction kinetics are considered through a range of ketone partial pressures (0.3–30Torr), hydrogen partial pressures (90–900Torr), and reaction temperatures (322–456K). Ketone hydrogenation is observed to be facile, with site time yields ranging from 0.14s−1 for 2-pentanone to 0.37s−1 for acetone at 322K and 1.2 bar H2. At low temperatures, apparent reaction orders and kinetic barriers are similar for all ketones. During acetone hydrogenation at higher temperatures, (422K), the ketone order increases from 0 to 0.4, while the hydrogen order increases from 0.5 to 0.9. Furthermore, the apparent barrier decreases from ≈50kJmol−1 at 322K to ≈18kJmol−1. Apparent trends in hydrogenation rates are interpreted at an elementary level using a microkinetic analysis that is based on a Horiuti-Polanyi mechanism involving two distinct surface sites.
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