화학공학소재연구정보센터
Journal of Catalysis, Vol.383, 24-32, 2020
Kinetics of aromatics hydrogenation on HBEA
Zeolite HBEA catalyzes hydrogenation of aromatic hydrocarbons-methyl-substituted benzenes (benzene and toluene), alkenyl-substituted benzenes (styrene), and polycyclics (naphthalene)-in presence of excess H-2 at high-temperatures (573-748 K) with rates that depend linearly on aromatic and H-2 pressures. The observed kinetic behavior can be rationalized based on a sequence of elementary steps where the first hydrogenation step of the adsorbed benzenic intermediate is rate-determining while subsequent hydrogenation and desorption steps are quasi-equilibrated and H+ is the most abundant surface species. Styrene hydrogenation exhibits the highest rates among the aromatics considered and results exclusively in ethylbenzene synthesis; in contrast, benzene/toluene and naphthalene hydrogenation results in formation of their triply-hydrogenated five-membered ring and doubly-hydrogenated ring open analogs, respectively. Based on independent studies involving co-reaction of cyclohexene and 1-methyl-1-cyclopentene with H-2, we infer their facile interconversion and hydrogenation to methylcyclopentane implying that conversion of benzene to methylcyclopentane likely occurs via intervening formation of both five- and six-membered ring intermediates. Taken together, these studies demonstrate feasibility of aromatics hydrogenation and propensity of benzenic rings in these hydrocarbons to undergo ring reduction or ring opening during their activation with H-2 on Bronsted acid zeolites. (C) 2020 Elsevier Inc. All rights reserved.