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This method adopts allylic alcohol\u2010containing diynes and provides efficient access to multi\u2010functional pyrrolidines and tetrahydrofurans in high to excellent stereoselectivities. Mechanistic studies highlighted an innovative catalytic pathway that differs from the classical enyne cycloisomerization and involves initiation at the allylic alcohol moiety. Diverse derivatizations of the heterocyclic products including intriguing skeletal rearrangements have also been demonstrated.<\/jats:p>","DOI":"10.1002\/anie.202421153","type":"journal-article","created":{"date-parts":[[2025,2,5]],"date-time":"2025-02-05T13:39:46Z","timestamp":1738762786000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Desymmetrization of 1,4\u2010Diynes by Allylic Alcohol\u2010Triggered Redox Enyne Cycloisomerization"],"prefix":"10.1002","volume":"64","author":[{"given":"Fangyuan","family":"Wang","sequence":"first","affiliation":[{"name":"Department of Chemistry National University of Singapore  3 Science Drive 3, Republic of Singapore Singapore 117543"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenxuan","family":"Lin","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering and Chongqing Key Laboratory of Theoretical and Computational Chemistry Chongqing University  Chongqing 400030 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chia","family":"Hui Yeh","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  3 Science Drive 3, Republic of Singapore Singapore 117543"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Lan","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering and Chongqing Key Laboratory of Theoretical and Computational Chemistry Chongqing University  Chongqing 400030 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2944-1315","authenticated-orcid":false,"given":"Yu","family":"Zhao","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  3 Science Drive 3, Republic of Singapore Singapore 117543"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,2,14]]},"reference":[{"key":"e_1_2_3_1_1","unstructured":"For selected reviews see:"},{"key":"e_1_2_3_2_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.6b00094"},{"key":"e_1_2_3_3_2","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00666A"},{"key":"e_1_2_3_4_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.trechm.2021.12.010"},{"key":"e_1_2_3_5_2","first-page":"106","author":"N\u00e1jera C.","year":"2022","journal-title":"Tetrahedron"},{"key":"e_1_2_3_6_2","doi-asserted-by":"publisher","DOI":"10.31635\/ccschem.024.202403839"},{"key":"e_1_2_3_7_1","unstructured":"For selected reviews see:"},{"key":"e_1_2_3_8_2","doi-asserted-by":"publisher","DOI":"10.1039\/C6CS00023A"},{"key":"e_1_2_3_9_2","doi-asserted-by":"publisher","DOI":"10.1002\/ijch.201700060"},{"key":"e_1_2_3_10_2","doi-asserted-by":"publisher","DOI":"10.1002\/ajoc.202300554"},{"key":"e_1_2_3_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/tcr.202300066"},{"key":"e_1_2_3_12_1","unstructured":"\u00a0"},{"key":"e_1_2_3_13_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201205416"},{"key":"e_1_2_3_14_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.orglett.8b02982"},{"key":"e_1_2_3_15_1","author":"Kohnke P.","year":"2024","journal-title":"Angew. 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