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However, undesirable changes in Br\u00f6nsted acid site (BAS) densities always offset this advantage in acid\u2010catalyzed reactions. In this context, the crucial roles of spatial aluminum (Al) distribution were unraveled during alkali\u2010treatment of MFI zeolite and the desirable BAS density was achieved in obtained hierarchical samples for the target reactions. Various characterization methods, particularly the multiple one\u2010 and two\u2010dimensional magic\u2010angle spinning (MAS) NMR techniques, were performed to track the alkali\u2010treatment processes. For the sample with a more uniform spatial Al distribution, more tetrahedral Al sites would fall off and migrate around the Si\u2010OH in zeolite as Al(OH)\n                    <jats:sub>4<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    . Those re\u2010deposited Al(OH)\n                    <jats:sub>4<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    sites were easily transformed into NMR\u2010invisible Al sites during the calcination process, which contributed negligibly to both Br\u00f6nsted and Lewis acidities, thus being referred to \u201cacid\u2010free\u201d Al species. While most tetrahedral Al sites were preserved after the alkali\u2010treatment of sample with non\u2010uniform Al distribution and the BAS density gradually increased with treatment time. According to the requirements of typical acid\u2010catalyzed reactions, such as catalytic cracking of 1,3,5\u2010triisopropylbenzene and methanol\u2010to\u2010olefins, the desired hierarchical zeolite catalysts were developed by matching the amounts of extracted Si and generated \u201cacid\u2010free\u201d Al during the precise alkali\u2010treatment.\n                  <\/jats:p>","DOI":"10.1002\/anie.202416564","type":"journal-article","created":{"date-parts":[[2024,10,14]],"date-time":"2024-10-14T10:05:04Z","timestamp":1728900304000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":26,"title":["Unravelling the Crucial of Spatial Al Distribution to Realize Precise Alkali\u2010Treatment for Target Acid\u2010Catalyzed Reactions"],"prefix":"10.1002","volume":"64","author":[{"given":"Junjie","family":"Li","sequence":"first","affiliation":[{"name":"The State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian 116023 P. 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