{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T15:26:06Z","timestamp":1787153166372,"version":"build-2736575974"},"reference-count":56,"publisher":"American Chemical Society (ACS)","issue":"32","license":[{"start":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T00:00:00Z","timestamp":1786320000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T00:00:00Z","timestamp":1786320000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T00:00:00Z","timestamp":1786320000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100012166","name":"National Key Research and Development Program of China","doi-asserted-by":"publisher","award":["2023YFA1507602"],"award-info":[{"award-number":["2023YFA1507602"]}],"id":[{"id":"10.13039\/501100012166","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100003399","name":"Science and Technology Commission of Shanghai Municipality","doi-asserted-by":"publisher","award":["2024ZDSYS02"],"award-info":[{"award-number":["2024ZDSYS02"]}],"id":[{"id":"10.13039\/501100003399","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22472037"],"award-info":[{"award-number":["22472037"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,19]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Strongly alkaline synthesis of zeolites is efficient, yet often induces silanol defects and Al zoning with elevated external acidity, while acid- or near-neutral routes commonly depend on fluoride mineralization or preformed seeds to sustain crystallization. Here, we report a fluoride-free, seed-free, one-pot sequential alkaline-acid strategy that affords high-yield ZSM-5 nanosheets under near-neutral acidic conditions. In this route, the initial alkaline stage promotes the formation of abundant precursor nuclei, while the subsequent near-neutral stage enables near-complete crystallization, thereby overcoming sluggish spontaneous nucleation in nonalkaline media. The obtained nanosheets possess reduced silanol-related defects, enhanced framework Al incorporation, and weakened outer-region Al enrichment, accompanied by lower external\/near-surface Br\u00f8nsted acidity and a low fraction of proximate Al sites. Systematic variation of acidification pH and timing shows that lower synthesis alkalinity promotes sheet-like morphology, reduces silanol-related defects, and decreases external\/near-surface Br\u00f8nsted acidity, whereas delayed acidification after the growth inflection point leads to stronger Al expulsion and more pronounced outer-region Al enrichment. Crystallization tracking, together with NaOH etching, reveals preferential c-axis elongation and a weakened Al expulsion process under near-neutral acidic conditions, accounting for reduced outer-region Al enrichment and lower Al-pair fraction in the final nanosheets. Catalytic probing using 1,3,5-triisopropylbenzene cracking confirms reduced external\/near-surface acidity, while lactic acid-to-lactide conversion tests show improved shape-selective performance with reduced coke formation. This work provides a practical strategy for simultaneously regulating silanol-related defects, framework Al distribution, and acid-site accessibility in ZSM-5 nanosheets.<\/jats:p>","DOI":"10.1021\/jacs.6c12379","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T09:01:51Z","timestamp":1786352511000},"page":"35077-35089","source":"Crossref","is-referenced-by-count":0,"title":["One-Pot Sequential\nAlkaline-Acid Route to ZSM-5\nNanosheets with Low Framework Defects and Suppressed Aluminum Zoning"],"prefix":"10.1021","volume":"148","author":[{"given":"Wei","family":"Chen","sequence":"first","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"He","family":"Li","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiayu","family":"Yu","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yujing","family":"Chen","sequence":"additional","affiliation":[{"name":"SINOPEC Dalian Research Institute of Petroleum and Petrochemicals Co., Ltd. , ,","place":["Dalian, China, 116045"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling","family":"Ding","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ke","family":"Du","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Di","family":"Pan","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1463-9927","authenticated-orcid":true,"given":"Yi","family":"Tang","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1148-949X","authenticated-orcid":true,"given":"Yahong","family":"Zhang","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,10]]},"reference":[{"issue":"20","key":"2026081910214780700_cit1","doi-asserted-by":"publisher","first-page":"11194","DOI":"10.1021\/acs.chemrev.0c00016","article-title":"Hierarchically\nstructured zeolites: from design to application","volume":"120","author":"Chen","year":"2020","journal-title":"Chem. 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Technol."},{"issue":"52","key":"2026081910214780700_cit5","doi-asserted-by":"publisher","first-page":"48235","DOI":"10.1021\/jacs.5c17648","article-title":"A funnel-structured\n12 \u00d7 10-ring\nzeolite customized for biomass catalytic pyrolysis","volume":"147","author":"Wu","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"0","key":"2026081910214780700_cit6","doi-asserted-by":"publisher","first-page":"127","DOI":"10.1039\/jr9480000127","article-title":"33. Synthesis\nof a zeolitic mineral with chabazite-like sorptive properties","author":"Barrer","year":"1948","journal-title":"J. Chem. Soc."},{"issue":"3","key":"2026081910214780700_cit7","doi-asserted-by":"publisher","first-page":"663","DOI":"10.1021\/cr020060i","article-title":"The hydrothermal synthesis of zeolites: history and\ndevelopment from the earliest days to the present time","volume":"103","author":"Cundy","year":"2003","journal-title":"Chem. 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Solid State Chem."},{"issue":"22","key":"2026081910214780700_cit32","doi-asserted-by":"publisher","first-page":"10792","DOI":"10.1021\/acs.jpcc.3c01533","article-title":"Chemical shift\nanisotropy: a promising parameter to\ndistinguish the 29Si NMR peaks in zeolites","volume":"127","author":"Dib","year":"2023","journal-title":"J. Phys. Chem. C"},{"issue":"10","key":"2026081910214780700_cit33","doi-asserted-by":"publisher","first-page":"1010","DOI":"10.1038\/nmat4941","article-title":"One-pot\nsynthesis of silanol-free nanosized MFI zeolite","volume":"16","author":"Grand","year":"2017","journal-title":"Nat. Mater."},{"issue":"1","key":"2026081910214780700_cit34","doi-asserted-by":"publisher","first-page":"137","DOI":"10.1016\/0021-9517(84)90059-9","article-title":"A Fourier-transform infrared spectral\nstudy of H-ZSM-5 surface sites and reactivity sequences in methanol\nconversion","volume":"88","author":"Sayed","year":"1984","journal-title":"J. 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Mater."},{"issue":"10","key":"2026081910214780700_cit48","doi-asserted-by":"publisher","first-page":"12196","DOI":"10.1007\/s12274-023-5749-0","article-title":"Urea-assisted\nmorphological\nengineering of MFI nanosheets with tunable b-thickness","volume":"16","author":"Yue","year":"2023","journal-title":"Nano Res."},{"issue":"24","key":"2026081910214780700_cit49","doi-asserted-by":"publisher","first-page":"13444","DOI":"10.1002\/anie.202102621","article-title":"Observing a zeolite\nnucleus (subcrystal) with a uniform framework\nstructure and its oriented attachment without single-molecule addition","volume":"60","author":"Sheng","year":"2021","journal-title":"Angew. Chem., Int. 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