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Therefore, strategically weakening zeolite acidity is essential for balancing reactivity with stability. The local coordination environment of framework aluminum usually governs its acidity. Hydroxylation of framework aluminum is often inevitable under high\u2010temperature and humid \u201cworking\u201d conditions; however, the impact of hydroxyl coordination on the relevant acidity and catalytic behavior remains unclear. Here, we demonstrate how hydroxylation of framework aluminum strategically moderates acidity and enhances catalytic stability. Density functional theory (DFT) calculations predict that an increase in the hydroxyl groups coordinated to framework aluminum leads to a progressive weakening of Br\u00f8nsted acidity. We experimentally validate this prediction by precisely manipulating hydroxylation in ZSM\u20105 zeolite via steaming treatment and analyzing the effects using 2D NMR spectroscopy with 2\u2013\n                    <jats:sup>13<\/jats:sup>\n                    C\u2010acetone as a probe molecule. The hydroxylated aluminum sites exhibit reduced adsorption and activation of methanol in the dehydration reaction, consistent with their weaker acidity. Catalytic tests reveal that the hydroxylated samples significantly enhance catalyst lifespan in the MTO process, while preserving stable reactivity. These findings provide key insights into how coordination perturbations influence zeolite acidity and catalytic performance, offering valuable guidance for designing zeolites with targeted catalytic functions.\n                  <\/jats:p>","DOI":"10.1002\/anie.202518228","type":"journal-article","created":{"date-parts":[[2026,1,27]],"date-time":"2026-01-27T13:18:07Z","timestamp":1769519887000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Steering Zeolite Br\u00f8nsted Acidity and Catalytic Consequence Through Manipulating the Coordination Environment of Framework Aluminum"],"prefix":"10.1002","volume":"65","author":[{"given":"Youdong","family":"Xing","sequence":"first","affiliation":[{"name":"Interdisciplinary Institute of NMR and Molecular Sciences Hubei Province for Coal Conversion and New Carbon Materials School of Chemistry and Chemical Engineering Wuhan University of Science and Technology  Wuhan P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xianfeng","family":"Yi","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance Spectroscopy and Imaging National Center for Magnetic Resonance in Wuhan Wuhan Institute of Physics and Mathematics Innovation Academy for Precision Measurement Science and Technology Chinese Academy of Sciences  Wuhan P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fengqing","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance Spectroscopy and Imaging National Center for Magnetic Resonance in Wuhan Wuhan Institute of Physics and Mathematics Innovation Academy for Precision Measurement Science and Technology Chinese Academy of Sciences  Wuhan P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yao","family":"Xiao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance Spectroscopy and Imaging National Center for Magnetic Resonance in Wuhan Wuhan Institute of Physics and Mathematics Innovation Academy for Precision Measurement Science and Technology Chinese Academy of Sciences  Wuhan P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wanyi","family":"Gan","sequence":"additional","affiliation":[{"name":"Interdisciplinary Institute of NMR and Molecular Sciences Hubei Province for Coal Conversion and New Carbon Materials School of Chemistry and Chemical Engineering Wuhan University of Science and Technology  Wuhan P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Molly Meng\u2010Jung","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Applied Physics The Hong Kong Polytechnic University  Hong Kong P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7115-6510","authenticated-orcid":false,"given":"Anmin","family":"Zheng","sequence":"additional","affiliation":[{"name":"Interdisciplinary Institute of NMR and Molecular Sciences Hubei Province for Coal Conversion and New Carbon Materials School of Chemistry and Chemical Engineering Wuhan University of Science and Technology  Wuhan P.R. 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