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Herein, we report a sustainable approach using cycloketones as secondary nitrogen\u2010free organic structure\u2010directing agents (NF\u2010OSDAs) to fabricate two\u2010dimensional (2D) MWW zeolites. Cyclobutanone (Cy4) directs the formation of ultrathin nanosheets featuring expanded interlayer spacing and tunable aluminum distribution. We demonstrate that Na\n                    <jats:sup>+<\/jats:sup>\n                    \u2010cycloketone complexes selectively occupy specific pore environments, effectively reducing the population of T\n                    <jats:sub>6<\/jats:sub>\n                    \u2013T\n                    <jats:sub>7<\/jats:sub>\n                    framework aluminum (Al\n                    <jats:sub>F<\/jats:sub>\n                    ) sites and migrating to T\n                    <jats:sub>2<\/jats:sub>\n                    Al\n                    <jats:sub>F<\/jats:sub>\n                    sites, promoting external Br\u00f8nsted acidity. The resulting Cy4\u2010MWW catalyst exhibits outstanding performance in bulky\u2010molecule transformations. Mechanistic studies reveal that cycloketones undergo in situ self\u2010condensation to generate dimeric species that function as pivotal structural directors. Their steric presence affects layer thickness and nanosheet packing, whereas their Na\n                    <jats:sup>+<\/jats:sup>\n                    \u2010coordinated forms strongly interact with T\n                    <jats:sub>2<\/jats:sub>\n                    Al\n                    <jats:sub>F<\/jats:sub>\n                    sites, thereby driving aluminum migration from the confined T\n                    <jats:sub>6<\/jats:sub>\n                    \u2013T\n                    <jats:sub>7<\/jats:sub>\n                    Al\n                    <jats:sub>F<\/jats:sub>\n                    positions to accessible T\n                    <jats:sub>2<\/jats:sub>\n                    Al\n                    <jats:sub>F<\/jats:sub>\n                    sites. This strategy exhibits broad versatility across a range of cycloketones (Cy4\u2013Cy10), enabling the concurrent tuning of both the MWW architecture and its aluminum distribution.\n                  <\/jats:p>","DOI":"10.1002\/anie.5569126","type":"journal-article","created":{"date-parts":[[2026,7,3]],"date-time":"2026-07-03T17:36:55Z","timestamp":1783100215000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Green Synthesis of Ultrathin MWW Zeolites With Tunable Al\u2010T Sites Using Nitrogen\u2010Free Secondary OSDAs for Catalytic Cracking"],"prefix":"10.1002","volume":"65","author":[{"given":"Haocheng","family":"Zhang","sequence":"first","affiliation":[{"name":"Department of Chemistry College of Smart Materials and Future Energy State Key Laboratory of Porous Materials for Separation and Conversion Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Laboratory of Advanced Materials Fudan University  Shanghai People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianyu","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Synergistic Chem\u2010Bio Synthesis School of Chemistry and Chemical Engineering Shanghai Jiao Tong University  Shanghai People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuang","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Green Chemical Engineering and Industrial Catalysis SINOPEC Shanghai Research Institute of Petrochemical Technology Co., Ltd.  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