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Here, we introduce hydrothermal annealing as a facile and highly effective method to improve the activity and lifetime of zeolite catalysts. This post\u2010synthesis treatment uses a siliceous growth solution at approximate solubility of zeolite crystals with high temperature to alter the physicochemical properties of as\u2010synthesized materials. We employ the methanol\u2010to\u2010hydrocarbons (MTH) process as a benchmark reaction, along with a wide range of characterization techniques, to assess the impact of annealing on four nanosized and hierarchical ZSM\u20105 materials compared to a commercial sample. Our findings reveal that annealing significantly increased cumulative MTH turnover without appreciably altering product selectivity, despite non\u2010obvious changes to zeolite structure as a result of the annealing process. Comparisons of catalyst performance are made under identical reaction conditions using a descriptor that correlates cumulative turnovers to compositional, mass transport, and textural properties of each material \u2013 in line with growing efforts to increase rigor and reproducibility in the field of catalysis. The collective approach used in this study serves as a guideline for establishing structure\u2010composition\u2010performance relationships for zeolite\u2010based catalysts across wide\u2010ranging applications.<\/jats:p>","DOI":"10.1002\/anie.202515008","type":"journal-article","created":{"date-parts":[[2026,1,16]],"date-time":"2026-01-16T05:23:21Z","timestamp":1768541001000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Hydrothermal Annealing of Hierarchical ZSM\u20105 Zeolites Improves Catalytic Performance"],"prefix":"10.1002","volume":"65","author":[{"given":"Kumari","family":"Shilpa","sequence":"first","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Houston  Houston Texas TX 77204 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Heng","family":"Dai","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Houston  Houston Texas TX 77204 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"Lu","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Johns Hopkins University  Baltimore Maryland 21287 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinwei","family":"Ye","sequence":"additional","affiliation":[{"name":"Inorganic Chemistry and Catalysis Group, Institute for Circular and Sustainable Chemistry Faculty of Science Utrecht University Universiteitsweg 99 Utrecht 3584 CG The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Carolin","family":"Rieg","sequence":"additional","affiliation":[{"name":"Inorganic Chemistry and Catalysis Group, Institute for Circular and Sustainable Chemistry Faculty of Science Utrecht University Universiteitsweg 99 Utrecht 3584 CG The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Song","family":"Luo","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering University of Massachusetts  Amherst Massachusetts 01003 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Han","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering University of Massachusetts  Amherst Massachusetts 01003 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Omar","family":"Abdelrahman","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Houston  Houston Texas TX 77204 USA"},{"name":"Department of Chemical Engineering University of Massachusetts  Amherst Massachusetts 01003 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Fan","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering University of Massachusetts  Amherst Massachusetts 01003 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bert M.","family":"Weckhuysen","sequence":"additional","affiliation":[{"name":"Inorganic Chemistry and Catalysis Group, Institute for Circular and Sustainable Chemistry Faculty of Science Utrecht University Universiteitsweg 99 Utrecht 3584 CG The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Michael","family":"Tsapatsis","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Johns Hopkins University  Baltimore Maryland 21287 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2296-3428","authenticated-orcid":false,"given":"Jeffrey D.","family":"Rimer","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Houston  Houston Texas TX 77204 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,1,15]]},"reference":[{"key":"e_1_2_7_1_1","first-page":"86","volume":"6","author":"Meisel S.","year":"1976","journal-title":"Chem. 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