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However, under practical zeolite catalytic systems, water coexists with organic guest molecules within the confined microporous environment, giving rise to dynamical and multicomponent host\u2013guest interactions. Combining in situ spectroscopic characterization with theoretical calculations, this study unveils, at the molecular level, the dynamic ternary interplay among zeolite, confined aromatics, and water during SAPO\u201034\u2010catalyzed methanol\u2010to\u2010olefins (MTO) reaction. The confined aromatics generated in situ spatially and electronically modify the zeolite framework, forming a molecular shield that protects the zeolite framework from hydrolytic attack. More importantly, water acts as a molecular scissor, continuously trimming the alkyl side\u2010chains of confined aromatics, thereby retarding their polycyclic growth while promoting the efficient and sustained formation of light olefins. Across a series of eight\u2010membered\u2010ring (8\u2010MR) zeolites (SAPO\u201034, SAPO\u201018, and SSZ\u201013), co\u2010feeding water results in an orders\u2010of\u2010magnitude enhancement of catalyst lifetime while maintaining stable olefin production. The dynamic cooperative interplay among zeolite, confined aromatics, and water governs the framework stability and catalytic longevity during MTO conversion. This mechanistic insight extends the conceptual boundaries of zeolite host\u2013guest chemistry and opens new avenues for harnessing the beneficial role of water in zeolite catalysis.<\/jats:p>","DOI":"10.1002\/anie.2757170","type":"journal-article","created":{"date-parts":[[2026,3,12]],"date-time":"2026-03-12T08:06:31Z","timestamp":1773302791000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Unveiling Zeolite\u2010Confined Aromatic\u2010Water Dynamic Interplay in Methanol\u2010to\u2010Olefins Catalysis"],"prefix":"10.1002","volume":"65","author":[{"given":"Chengwei","family":"Zhang","sequence":"first","affiliation":[{"name":"National Engineering Research Center of Lower\u2010Carbon Catalysis Technology Dalian National Laboratory For Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian 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