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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\u2010induced physicochemical changes in zeolite, their ultimate impact on the organic reaction mechanism governed by the hydrocarbon pool dual\u2010cycle 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\u2010to\u2010hydrocarbons 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 \u201cmobility\u2010dependent\u201d solid\u2010state NMR spectroscopy. This multimodal characterization approach was instrumental in elucidating elusive mechanistic information in the dual\u2010cycle mechanism, shedding light on phenomena such as the unchanged ethylene selectivity despite decreasing aromatics selectivity, while ethylene could solely be derived from arene\u2010based reaction intermediates. This study could improve the process efficiency in zeolite catalysis by connecting steaming\u2010induced changes in the organic reaction mechanisms with inorganic material aspects.<\/jats:p>","DOI":"10.1002\/anie.202414724","type":"journal-article","created":{"date-parts":[[2024,10,22]],"date-time":"2024-10-22T22:25:51Z","timestamp":1729635951000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["The Paradoxical Influence of Hydrothermally Treated Zeolites on the Hydrocarbon Pool Mechanism"],"prefix":"10.1002","volume":"64","author":[{"given":"Xuan","family":"Gong","sequence":"first","affiliation":[{"name":"College of Chemistry and Molecular Sciences Wuhan University  Wuhan 430072 Hubei P.\u2005R. 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