Understanding Brønsted-Acid Catalyzed Monomolecular Reactions of Alkanes in Zeolite Pores by Combining Insights from Experiment and Theory

摘要: Acidic zeolites are effective catalysts for the cracking of large hydrocarbon molecules into lower molecular weight products required transportation fuels. However, ways in which zeolite structure affects catalytic activity at Bronsted protons not fully understood. One way to characterize influence on catalysis is study alkane and dehydrogenation very low conversion, conditions kinetics well defined. To understand effects measured rate coefficient (kapp ), it necessary identify equilibrium constant adsorption reactant state (Kads-H+ ) intrinsic reaction (kint temperatures, since kapp proportional product Kads-H+ kint . We show that cannot be calculated from experimental data collected near ambient temperature, but can, however, estimated accurately configurational-bias Monte Carlo (CBMC) simulations. Using monomolecular C3 -C6 alkanes as an example, we review recent efforts aimed elucidating acid site location framework observed values its components,