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Here, we harness this challenging property as a stereocontrol element through the integration of dynamic ligand exchange with designed hydrogen\u2010bonding interactions between a chiral phosphine ligand and the quinoline substrate. This creates a confined microenvironment that stabilizes the chiral palladium complex and directs a highly enantioselective allylic amination\/alkynylation cascade. This approach enables the first asymmetric allylic dearomatization of quinolines with terminal alkynes, affording a broad range of N\u2010heterocycles bearing two stereocenters in good yields (up to 85%) with excellent enantioselectivities (up to 99% e.e.) and diastereoselectivities (&gt;20:1 d.r.). Mechanistic studies, including in situ\n                    <jats:sup>31<\/jats:sup>\n                    P NMR and DFT calculations, reveal that the hydrogen\u2010bond interactions\u00a0are essential for dynamic ligand exchange, and their\u00a0disruption leads to loss of enantiocontrol. This work demonstrates that dynamic regulation of the ligand\u2010exchange equilibrium can be an effective strategy for harnessing strong substrate coordination in asymmetric catalysis.\n                  <\/jats:p>","DOI":"10.1002\/anie.9070689","type":"journal-article","created":{"date-parts":[[2026,8,13]],"date-time":"2026-08-13T15:40:00Z","timestamp":1786635600000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Asymmetric Allylic Dearomatization of Quinolines via Dynamic Ligand Exchange"],"prefix":"10.1002","volume":"65","author":[{"given":"Jian\u2010Feng","family":"Xu","sequence":"first","affiliation":[{"name":"College of Chemical Engineering Zhejiang University of Technology  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li","family":"Zhou","sequence":"additional","affiliation":[{"name":"College of Chemical Engineering Zhejiang University of Technology  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xue\u2010Pei","family":"Bai","sequence":"additional","affiliation":[{"name":"College of Chemical Engineering Zhejiang University of Technology  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4609-0350","authenticated-orcid":false,"given":"Bing","family":"Xu","sequence":"additional","affiliation":[{"name":"School of Pharmacy Naval Medical University Shanghai China"},{"name":"Department of Chemistry Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi\u2010Xia","family":"Jia","sequence":"additional","affiliation":[{"name":"College of Chemical Engineering Zhejiang University of Technology  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-3948-3773","authenticated-orcid":false,"given":"Wen\u2010Yu","family":"Huang","sequence":"additional","affiliation":[{"name":"College of Chemical Engineering Zhejiang University of Technology  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,13]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/ar500167f"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscentsci.0c01651"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja0608139"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/ol102190s"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201404286"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.8b00136"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5b10440"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557-020-0489-1"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja0734849"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200904981"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja111540g"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201303994"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201502708"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201507848"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201511663"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.6b01962"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.6b01693"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c09974"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202012861"},{"key":"e_1_2_8_21_1","first-page":"5102","article-title":"N,N\u2010c\u2010Binding Catalysis","volume":"60","author":"G\u00f3mez\u2010Mart\u00ednez M.","year":"2021","journal-title":"Angewandte Chemie International Edition"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c03048"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201064590\u2010w"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.3c00625"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1002\/9781118839621"},{"key":"e_1_2_8_26_1","doi-asserted-by":"crossref","unstructured":"E. 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