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Kinetic analysis suggests that parallel monomolecular (S\n                    <jats:sub>N<\/jats:sub>\n                    1) and bimolecular (S\n                    <jats:sub>N<\/jats:sub>\n                    2) substitution mechanisms contribute to observed rates of C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>5<\/jats:sub>\n                    ClO reactions with methanol (CH\n                    <jats:sub>3<\/jats:sub>\n                    OH) over both Lewis (Sn\u2010BEA) and Br\u00f8nsted acid (Al\u2010BEA) zeolites in liquid solvents. In situ solid\u2010state\n                    <jats:sup>13<\/jats:sup>\n                    C\u2010nuclear magnetic resonance spectroscopy (SS\u2010NMR) measurements give direct evidence for the proposed ring\u2010opened carbocations and activated CH\n                    <jats:sub>3<\/jats:sub>\n                    OH intermediates over these catalysts. Interpretation of time\u2010resolved\n                    <jats:italic>operando<\/jats:italic>\n                    <jats:sup>13<\/jats:sup>\n                    C\u2010SS\u2010NMR spectra shows that C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>5<\/jats:sub>\n                    ClO\u2010derived carbocations and CH\n                    <jats:sub>3<\/jats:sub>\n                    OH\u2010derived surface species convert to ring\u2010opening products through S\n                    <jats:sub>N<\/jats:sub>\n                    1 and S\n                    <jats:sub>N<\/jats:sub>\n                    2 reaction mechanisms and subsequently form distinct product regioisomers. These NMR spectra also reveal a concomitant shift from S\n                    <jats:sub>N<\/jats:sub>\n                    1 to S\n                    <jats:sub>N<\/jats:sub>\n                    2 reactions with increases in the coverage of CH\n                    <jats:sub>3<\/jats:sub>\n                    OH\u2010derived reactive intermediates achieved by control of the local concentrations of CH\n                    <jats:sub>3<\/jats:sub>\n                    OH, C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>5<\/jats:sub>\n                    ClO, and diluting CH\n                    <jats:sub>3<\/jats:sub>\n                    CN. This knowledge provides new insight into the role of coverage on regioselectivity and rates of catalytic reactions of organic species at solid\u2013liquid interfaces.\n                  <\/jats:p>","DOI":"10.1002\/anie.202511944","type":"journal-article","created":{"date-parts":[[2025,10,28]],"date-time":"2025-10-28T04:07:42Z","timestamp":1761624462000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["In Situ NMR and Kinetics Reveal Origins of Regioselectivity Differences for Epichlorohydrin Ring\u2010Opening in Lewis and Br\u00f8nsted Acid Zeolites"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8303-7359","authenticated-orcid":false,"given":"David S.","family":"Potts","sequence":"first","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Illinois Urbana\u2010Champaign  Urbana Illinois 61801 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Huston","family":"Locht","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Illinois Urbana\u2010Champaign  Urbana Illinois 61801 USA"},{"name":"School of Chemical and Biomolecular Engineering Georgia Institute of Technology  Atlanta Georgia 30332 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Sungmin","family":"Kim","sequence":"additional","affiliation":[{"name":"Institute for Integrated Catalysis Pacific Northwest National Laboratory  Richland Washington 99352 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Johannes A.","family":"Lercher","sequence":"additional","affiliation":[{"name":"Institute for Integrated Catalysis Pacific Northwest National Laboratory  Richland Washington 99352 USA"},{"name":"Department of Chemistry and Catalysis Research Center TU M\u00fcnchen  Lichtenbergstrasse 4 85748 Garching Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Jian Zhi","family":"Hu","sequence":"additional","affiliation":[{"name":"Institute for Integrated Catalysis Pacific Northwest National Laboratory  Richland Washington 99352 USA"},{"name":"The Gene &amp; Linda Voiland School of Chemical Engineering and Bioengineering Washington State University  Pullman WA 99164 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0567-8481","authenticated-orcid":false,"given":"David W.","family":"Flaherty","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Illinois Urbana\u2010Champaign  Urbana Illinois 61801 USA"},{"name":"School of Chemical and Biomolecular Engineering Georgia Institute of Technology  Atlanta Georgia 30332 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2025,10,27]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1016\/B978-0-444-53188-9.00001-8"},{"key":"e_1_2_8_2_1","unstructured":"Vol. WO 2020\/176277 A1 2020;"},{"key":"e_1_2_8_3_1","unstructured":"Vol. US 2020\/0231738 A1 2020."},{"key":"e_1_2_8_4_1","unstructured":"Vol. US9 822 087 B2 Dow Global Technologies LLC2017."},{"key":"e_1_2_8_5_1","unstructured":"X.Li L. 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