The Paradoxical Influence of Hydrothermally Treated Zeolites on the Hydrocarbon Pool Mechanism.

Autor: Gong X; College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China.; KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Jiang S; College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China., Dikhtiarenko A; KAUST Core Labs, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Nastase SAF; KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Abou-Hamad E; KAUST Core Labs, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Ye Y; College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China., Zhou H; College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China., You X; College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China., Khairova R; KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Patarroyo J; KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Cavallo L; KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Gascon J; KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia., Chowdhury AD; College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Oct 22, pp. e202414724. Date of Electronic Publication: 2024 Oct 22.
DOI: 10.1002/anie.202414724
Abstrakt: Understanding the mechanistic intricacies of hydrothermally treated zeolite is crucial for valorizing any oxygen-containing renewable feedstocks (e. g., methanol, carbon dioxide, biomass). Additionally, the regeneration of deactivated zeolite catalysts under oxidative conditions, akin to hydrothermal treatment, is essential in industrial processes. While research in this area has predominantly focused on characterizing steaming-induced physicochemical changes in zeolite, their ultimate impact on the organic reaction mechanism governed by the hydrocarbon pool dual-cycle mechanism remains unclear. To bridge this knowledge gap, this study investigates the effect of steamed zeolite on the organic reaction mechanism during the industrially significant methanol-to-hydrocarbons process. We achieved this objective by strategically integrating catalytic and control experiments over the pristine and steamed zeolites and their advanced characterization, including under operando conditions, XRD structural refinement, and using "mobility-dependent" solid-state NMR spectroscopy. This multimodal characterization approach was instrumental in elucidating elusive mechanistic information in the dual-cycle mechanism, shedding light on phenomena such as the unchanged ethylene selectivity despite decreasing aromatics selectivity, while ethylene could solely be derived from arene-based reaction intermediates. This study could improve the process efficiency in zeolite catalysis by connecting steaming-induced changes in the organic reaction mechanisms with inorganic material aspects.
(© 2024 Wiley-VCH GmbH.)
Databáze: MEDLINE