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In this study, we present the synthesis and characterization of the first isolable free plumbylyne radical <jats:bold>2<\/jats:bold> bearing a one\u2010coordinate Pb(I) atom. It reacts with an <jats:italic>N<\/jats:italic>\u2010heterocyclic carbene (NHC) to afford a two\u2010coordinate NHC\u2010ligated Pb(I) radical <jats:bold>3<\/jats:bold>. <jats:bold>2<\/jats:bold> and <jats:bold>3<\/jats:bold> represent the first isolable Pb(I)\u2010based radicals. Theoretical calculations and electron paramagnetic resonance analysis revealed that the unpaired electron mainly resides at the Pb 6p orbital in both radicals. Owing to the unique one\u2010coordinate nature of the Pb atom in <jats:bold>2<\/jats:bold>, it possesses two\u2010fold orbital pseudo\u2010degeneracy and substantial unquenched orbital angular momentum, and exhibits hitherto strongest <jats:italic>g<\/jats:italic>\u2010factor anisotropy (<jats:italic>g<\/jats:italic><jats:sub>x,y,z<\/jats:sub>=1.496, 1.166, 0.683) amongst main group radicals. Preliminary investigations into the reactivity of <jats:bold>2<\/jats:bold> unveiled its Pb\u2010centered radical nature, and plumbylenes were isolated as products.<\/jats:p>","DOI":"10.1002\/anie.202402093","type":"journal-article","created":{"date-parts":[[2024,3,5]],"date-time":"2024-03-05T03:04:09Z","timestamp":1709607849000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":33,"title":["An Isolable One\u2010Coordinate Lead(I) Radical with Strong <i>g<\/i>\u2010Factor Anisotropy"],"prefix":"10.1002","volume":"63","author":[{"given":"Haonan","family":"Chen","sequence":"first","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Guangdong Basic Research Center of Excellence for Functional Molecular Engineering School of Chemistry IGCME Sun Yat-sen University  Guangzhou 510275 China"},{"name":"Innovation Center for Chemical Sciences Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials Science Soochow University  Suzhou 215123 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wang","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences  457 Zhongshan Road Dalian 116023 China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongmin","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Guangdong Basic Research Center of Excellence for Functional Molecular Engineering School of Chemistry IGCME Sun Yat-sen University  Guangzhou 510275 China"},{"name":"Innovation Center for Chemical Sciences Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials Science Soochow University  Suzhou 215123 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yizhen","family":"Chen","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Guangdong Basic Research Center of Excellence for Functional Molecular Engineering School of Chemistry IGCME Sun Yat-sen University  Guangzhou 510275 China"},{"name":"Innovation Center for Chemical Sciences Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials Science Soochow University  Suzhou 215123 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zheng","family":"Liu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Guangdong Basic Research Center of Excellence for Functional Molecular Engineering School of Chemistry IGCME Sun Yat-sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9747-1412","authenticated-orcid":false,"given":"Shengfa","family":"Ye","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences  457 Zhongshan Road Dalian 116023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6972-2197","authenticated-orcid":false,"given":"Gengwen","family":"Tan","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Guangdong Basic Research Center of Excellence for Functional Molecular Engineering School of Chemistry IGCME Sun Yat-sen University  Guangzhou 510275 China"},{"name":"Innovation Center for Chemical Sciences Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials Science Soochow University  Suzhou 215123 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Song","family":"Gao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Guangdong Basic Research Center of Excellence for Functional Molecular Engineering School of Chemistry IGCME Sun Yat-sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,4,10]]},"reference":[{"key":"e_1_2_3_1_1","unstructured":"\u00a0"},{"key":"e_1_2_3_2_2","doi-asserted-by":"publisher","DOI":"10.1039\/b908048a"},{"key":"e_1_2_3_3_2","doi-asserted-by":"publisher","DOI":"10.1021\/cr100133q"},{"key":"e_1_2_3_4_2","doi-asserted-by":"publisher","DOI":"10.1038\/nature08634"},{"key":"e_1_2_3_5_2","first-page":"289","volume-title":"Multiply Bonded Compounds of Group 14 Elements","author":"Lee V. 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