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It has been demonstrated that organic electron\u2010deficient pnictogen atoms can act as prospective Lewis acids. Here, we present a catalytic approach for the asymmetric synthesis of chiral P<jats:sup>III<\/jats:sup> compounds by combining intramolecular PnB interactions and carbene catalysis. Our design features a pre\u2010chiral phosphorus molecule bearing two electron\u2010withdrawing benzoyl groups, resulting in the formation of a \u03c3\u2010hole at the P atom. X\u2010ray and non\u2010covalent interaction (NCI) analysis indicate that the model substrates exhibit intrinsic PnB interaction between the oxygen atom of the formyl group and the phosphorus atom. This induces a conformational locking effect, leading to the crystallization of the phosphorus substrate in a preferred conformation (<jats:italic>P<\/jats:italic>2<jats:sub>1<\/jats:sub>2<jats:sub>1<\/jats:sub>2<jats:sub>1<\/jats:sub> chiral group). Under the catalysis of <jats:italic>N<\/jats:italic>\u2013heterocyclic carbene, the aldehyde moiety activated by the pnictogen bond selectively reacts with an alcohol to yield the corresponding chiral monoester\/phosphorus product with excellent enantioselectivity. This Lewis acidic phosphorus center, aroused by the non\u2010polarized intramolecular pnictogen bond interaction, assists in conformational and selective regulations, providing unique opportunities for catalysis and beyond.<\/jats:p>","DOI":"10.1002\/anie.202404477","type":"journal-article","created":{"date-parts":[[2024,4,26]],"date-time":"2024-04-26T18:00:29Z","timestamp":1714154429000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":31,"title":["Carbene\u2010Catalyzed and Pnictogen Bond\u2010Assisted Access to P<sup>III<\/sup>\u2010Stereogenic Compounds"],"prefix":"10.1002","volume":"63","author":[{"given":"Jianjian","family":"Liu","sequence":"first","affiliation":[{"name":"National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education Guizhou University  550025 Guiyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Deng","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education Guizhou University  550025 Guiyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuyang","family":"Liang","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education Guizhou University  550025 Guiyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mali","family":"Zhou","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education Guizhou University  550025 Guiyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengcheng","family":"Zheng","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education Guizhou University  550025 Guiyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0573-257X","authenticated-orcid":false,"given":"Yonggui Robin","family":"Chi","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education Guizhou University  550025 Guiyang China"},{"name":"School of chemistry, chemical engineering, and biotechnology Nanyang Technological University  637371 Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,6,11]]},"reference":[{"key":"e_1_2_2_1_1","unstructured":"\u00a0"},{"key":"e_1_2_2_2_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.chemosphere.2014.01.030"},{"key":"e_1_2_2_3_2","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.ade6923"},{"key":"e_1_2_2_4_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.2434996"},{"key":"e_1_2_2_5_1","unstructured":"\u00a0"},{"key":"e_1_2_2_6_2","doi-asserted-by":"publisher","DOI":"10.1002\/cmdc.201800693"},{"key":"e_1_2_2_7_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.medidd.2020.100063"},{"key":"e_1_2_2_8_2","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202003033"},{"key":"e_1_2_2_9_1","unstructured":"\u00a0"},{"key":"e_1_2_2_10_2","first-page":"387","volume-title":"Organophosphorus Pesticides: Organic and BiologicalChemistry","author":"Eto M.","year":"1974"},{"key":"e_1_2_2_11_2","doi-asserted-by":"publisher","DOI":"10.1007\/978-3-642-68441-8"},{"key":"e_1_2_2_12_1","unstructured":"\u00a0"},{"key":"e_1_2_2_13_2","first-page":"44","volume":"48","author":"Vasant S. 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