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Herein, we disclose a palladium\u2010catalyzed enantioselective hydrosilylation that enables the construction of a C(sp\n                    <jats:sup>2<\/jats:sup>\n                    )\u2500Si bond, affording a regioselective route to\n                    <jats:italic>gem<\/jats:italic>\n                    \u2010phosphorylsilylalkenes bearing contiguous Si\u2010 and P\u2010stereocenters. This transformation operates through a synergistic combination of desymmetrization of dihydrosilanes and diastereomeric resolution (DR) of unsymmetrical and racemic alkynylphosphoryl substrates, in which a diverse array of silicon\u2010stereogenic\n                    <jats:italic>gem<\/jats:italic>\n                    \u2010phosphorylsilylalkenes and their structural analogues bearing additional P\u2010stereogenic centers in good yields and high enantioselectivities (up to 98:2 er). Furthermore, the synthetic utility of this methodology is underscored by the concise preparation of structurally diverse organosilicon frameworks. Mechanistic investigations, supported by density functional theory (DFT) calculations, have been performed to delineate the reaction pathway and rationalize the observed regio\u2010 and enantioselectivity.\n                  <\/jats:p>","DOI":"10.1002\/anie.3747908","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T03:54:52Z","timestamp":1792036492000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Synthesis of\n                    <i>gem<\/i>\n                    \u2010Phosphorylsilylalkenes Bearing Si\/Si,P\u2010Stereogenic Centers by Regio\u2010 and Enantio\u2010Selective Pd\u2010Catalyzed Hydrosilylation"],"prefix":"10.1002","author":[{"given":"Meng\u2010Ling","family":"Pu","sequence":"first","affiliation":[{"name":"Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical Engineering Hangzhou Normal University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Heng","family":"Xu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical Engineering Hangzhou Normal University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"An\u2010Jiu","family":"Wen","sequence":"additional","affiliation":[{"name":"Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical Engineering Hangzhou Normal University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu\u2010Ting","family":"Yang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical Engineering Hangzhou Normal 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zheng","family":"Xu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical Engineering Hangzhou Normal University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9105-1740","authenticated-orcid":false,"given":"Fuk Yee","family":"Kwong","sequence":"additional","affiliation":[{"name":"Department of Chemistry and State Key Laboratory of Synthetic Chemistry The Chinese University of Hong Kong  Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5705-0015","authenticated-orcid":false,"given":"Li\u2010Wen","family":"Xu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education College of Material Chemistry and Chemical Engineering Hangzhou Normal University  Hangzhou China"},{"name":"Department of Chemistry and State Key Laboratory of Synthetic Chemistry The Chinese University of Hong Kong  Hong Kong China"},{"name":"Institute of Drug Discovery and Technology, and Qian Xuesen Collaborative Research Center of Astrochemistry and Space Life Sciences Ningbo University  Ningbo China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,14]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.31635\/ccschem.024.202303678"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201059364\u20103"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.1c00212"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3QO01725G"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.orglett.3c01702"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.201203803"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201610121"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202001799"},{"key":"e_1_2_8_10_1","doi-asserted-by":"crossref","first-page":"881","DOI":"10.1016\/j.chempr.2019.02.001","article-title":"Cobalt\u2010Catalyzed 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