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The built of hierarchy in zeolites, especially with low aluminum stability or high Si\/Al ratio, often suffers from uncontrolled destruction of zeolitic framework, accompanied by a significant loss of microporous domains and intrinsic acidity after desilication. Here, we report a novel and simple methodology for preparation of hierarchical zeolites with highly complete framework and minimum sacrifice of microporosity and acidity. The pre\u2010impregnated amines in zeolite micropores act as inner pore\u2010directing agents (iPDAs), largely protecting the zeolitic framework and moderating the silicon extraction during the alkaline treatment. The resulting hierarchical zeolites exhibit high crystallinity, tunable hierarchy, stable framework, and well\u2010preserved acidity, endowing them with significantly improved mass transport properties and enhanced activities in catalytic conversion of methanol or furfural.<\/jats:p>","DOI":"10.1002\/anie.202411446","type":"journal-article","created":{"date-parts":[[2024,8,23]],"date-time":"2024-08-23T00:54:21Z","timestamp":1724374461000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":35,"title":["Constructing Hierarchical Zeolites with Highly Complete Framework via Controlled Desilication"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4102-2938","authenticated-orcid":false,"given":"Xiaochun","family":"Zhu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and Environment China University of Petroleum (Beijing) Beijing 102249 (P. 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