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Developing green manufacturing solutions is the long\u2010sought aspiration to reduce the carbon footprint of polyolefins and alleviate dependence on petroleum resources. Herein, electron\u2010rich phosphinephenolato nickel(II) complexes render bio\u2010based dimethyl carbonate (DMC) the desirable medium for the practically efficient production of high\u2010density polyethylene (HDPE) with comparable activity to metallocene catalysts. Mechanistic investigation identified that DMC could facilitate pyridine dissociation yet avoid overly strong coordination to nickel, enabling smooth ethylene substitution and consequently polymerization. Incorporation of carbonate\u2010containing comonomer afforded polar polyethylene with robust activity, which could be further tailored through microstructural refinement to customized functionalities. This work illustrated the harmonious interaction of carbonate with a polymerization catalyst that contributes a bio\u2010based solution toward sustainable manufacturing and functionalization of polyolefins.<\/jats:p>","DOI":"10.1002\/anie.3998761","type":"journal-article","created":{"date-parts":[[2026,10,4]],"date-time":"2026-10-04T10:02:44Z","timestamp":1791108164000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Bio\u2010Based Solution for Polyolefin Synthesis Enabled by Carbonate Solvent and Comonomer"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-4627-3366","authenticated-orcid":false,"given":"Xin","family":"Xu","sequence":"first","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials (Ministry of Education) Frontier Science Center for New Organic Matter, Institute of Polymer Chemistry, College of Chemistry Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Luqiang","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Chemical Power Sources Frontier Science Center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinrong","family":"Niu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials (Ministry of Education) Frontier Science Center for New Organic Matter, Institute of Polymer Chemistry, College of Chemistry Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinzhu","family":"Niu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials (Ministry of Education) Frontier Science Center for New Organic Matter, Institute of Polymer Chemistry, College of Chemistry Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0028-2717","authenticated-orcid":false,"given":"Ke R.","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Chemical Power Sources Frontier Science Center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7714-6206","authenticated-orcid":false,"given":"Fei","family":"Lin","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials (Ministry of Education) Frontier Science Center for New Organic Matter, Institute of Polymer Chemistry, College of Chemistry Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,4]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"crossref","unstructured":"N.Karali N.Khanna andN.Shah Climate Impact of Primary Plastic Production(Lawrence Berkeley National Laboratory Sustainable Energy and Environmental Systems 2024).","DOI":"10.2172\/2336721"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.5b00310"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.3c00587"},{"key":"e_1_2_8_5_1","first-page":"1","volume-title":"Ullmann's Encyclopedia of Industrial Chemistry","author":"Jeremic D.","year":"2014"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aao6711"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adh3353"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abi8183"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abh4308"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.add1088"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abc5441"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aah5744"},{"key":"e_1_2_8_13_1","unstructured":"A. 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