Strategies to Enable Selective and Stable Conversion of Methanol over Zeolites to Target Hydrocarbons

• Main Author: Shi, Zhichen
• Format: Dissertation
• Language: English
• Published: ProQuest Dissertations & Theses 01-01-2022
• Subjects: Chemical engineering
• ISBN: 9798351430201

Methanol-to-hydrocarbons (MTH) conversion over solid acid catalysts is one of the largest-scale catalytic processes for the commercial valorization of low-value carbon sources to fuels and chemical production. The complex reaction network, intrapore diffusion limitations, and continuous on-stream deactivation, however, prevail during MTH to prevent the accurate measurement of reaction rates, mechanistic interpretation of product selectivity, and elucidation of species and pathways relevant to catalyst deactivation. In this dissertation, we combine rigorous assessment of catalyst performance, chemical kinetics, kinetic modeling, and density functional theory calculations to probe molecular events describing light olefins production and catalyst deactivation in this chemistry. These mechanistic understandings, taken together with recent development in syngas-to-hydrocarbons catalysis, further allowed us to develop and understand strategies that involve optimizing materials properties and co-processing gas-phase molecules for stable and selective production of hydrocarbons from methanol and syngas.