Density Functional Theory Study of Ethylene Protonation over HZSM-5 Zeolite with Neighboring Brönsted Acid Sites

doi:10.3724/SP.J.1088.2011.10110

Abstract

Abstract: By the density functional theory method, the effect of different acid sites and neighboring acid sites on ethylene protonation over HZSM-5 zeolite was investigated. The calculations were based on the 20T cluster model and carried out at the B3LYP/6-31G(d,p) theoretical level. The structure, atomic charges, and the energy of the ethylene adsorption species, transition state, and the surface alkoxide products were examined. The results indicated that the next-nearest-neighboring acid sites led to obvious decrease in acid strength and adsorption energy but slight decrease in activation energy, while the next-next-nearest-neighboring acid sites had a very slender effect on acid strength and the affection on ethylene protonation could be neglected. The activation energy and reaction energy had no inevitable correlation with the acid strength but virtually depended on the location and chemical environment of the acid sites in HZSM-5 zeolite. If the transition-state structure is much resembling to the carbenium ion, the activation energy would be higher.

Key words: HZSM-5 zeolite, ethylene protonation, Brönsted acid site, neighboring acid sites, density functional theory

REN Jue, ZHOU Dan-Hong, LI Jing-Hong, CAO Liang, XING Shuang-Ying. Density Functional Theory Study of Ethylene Protonation over HZSM-5 Zeolite with Neighboring Brönsted Acid Sites[J]. Chinese Journal of Catalysis, 2011, 32(6): 1056-1062.

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