Abstract
The palladium-black-catalyzed electrogenerative hydrogenation of ethylene was investigated over partially wettable, porous, commercial electrodes between +0.6 and 0 V. In perchloric acid electrolyte, hydrogen ion transport in the catalyst pores was rapid, but ethylene pore diffusion became rate limiting below 0.3 atm partial pressure. A simple pore model treatment allows the incorporation of an electrochemical Thiele modulus. With this treatment, the evaluation of intrinsic electrode kinetic parameters from apparent ones is demonstrated. A mechanistic model is proposed involving the surface insertion of ethylene to adsorbed hydrogen atoms followed by slow hydrogen addition to the resulting surface ethyl radicals. This model is used to explain differences in reaction rate, overpotential, and selectivity for double bond reduction on palladium and platinum.
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