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Here, we demonstrate their non\u2010negligible catalytic role in methanol conversion using pure silica MFI zeolite (Silicalite\u20101). Two silicalite\u20101 samples with different crystal sizes, micron\u2010sized (Sil1_micro) and nano\u2010sized (Sil1_nano), were synthesized and investigated by in situ and operando FTIR spectroscopy using probe molecules (carbon monoxide, pyridine, and methanol). multivariate\u2010curve regression by alternating least squares was applied to elucidate the influence of the silanol hydrogen\u2010bonding network on catalytic reactivity. Distinct acid\u2013base behaviors were identified: isolated and weakly hydrogen\u2010bonded silanols are active at low temperatures, whereas strongly hydrogen\u2010bonded silanols become catalytically relevant at higher temperatures. Methanol adsorption studies reveal a unique bidentate coordination mode in Sil1_nano, associated with weakly hydrogen\u2010bonded geminal silanols, which promotes the formation of reactive intermediates and dual coke species. In contrast, Sil1_micro, characterized by a higher fraction of strongly hydrogen\u2010bonded silanols, exhibits a different methanol reactivity pattern. These results demonstrate that silanol groups are active functional entities rather than passive defects, capable of driving methanol reforming\u2010like transformations and steering coke formation pathways.<\/jats:p>","DOI":"10.1002\/smll.73802","type":"journal-article","created":{"date-parts":[[2026,5,26]],"date-time":"2026-05-26T12:32:08Z","timestamp":1779798728000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Silanol Networks Control Methanol Reactivity in Nano\u2010 and Micron\u2010sized Silicalite\u20101"],"prefix":"10.1002","volume":"22","author":[{"given":"Francesco","family":"Dalena","sequence":"first","affiliation":[{"name":"Normandie Univ, ENSICAEN, UNICAEN, CNRS Laboratoire Catalyse et Spectrochimie  Caen 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