Reactions of light hydrocarbons in acid zeolites using electronic structure calculations
Date
2024
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Publisher
University of Delaware
Abstract
The so-called “shale gas boom” of the past decade has resulted in a steadily increasing supply of natural gas and light alkanes. The abundance of these feedstocks has presented an opportunity to revisit and replace existing petroleum-based processes for many commodity and fine chemicals. Commercial processes for various platform chemicals, such as olefins and aromatic hydrocarbons, already exist for light alkane and natural-gas-derived methanol. Many utilize zeolite-based catalysts; zeolites are microporous aluminosilicates. This class of catalyst is among the oldest and most robust because of their high stability. But despite their ubiquity and age in the chemical industry, there are still a lot of unknowns with regards to their catalytic mechanism. The aims of this dissertation are to address the knowledge gaps in the fundamental reaction mechanisms by which zeolites convert light alkanes, and tangentially methanol, into aromatics and light olefins. To overcome current limitations in experimental work, electronic structure calculations, particularly density functional theory (DFT), is utilized to identify possible reaction mechanisms and calculate relevant thermodynamics and kinetics, and predict structures for intermediates and transition states.
Description
Keywords
Aromatization, Carbocation rearrangements, Dehydrogenation, Hexatriene, Spin crossing, Zeolites