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However, achieving sequence\u2010controlled copolymerization in a one\u2010step and one\u2010pot process remains challenging. This study introduces a solvent\u2010dependent sequence\u2010controlled copolymerization strategy to produce block and statistical copolyesters from 4\u2010phenyl\u20102\u2010oxabicyclo[2.1.1]hexan\u20103\u2010one (4\n                    <jats:sup>Ph<\/jats:sup>\n                    \u2010BL) and\n                    <jats:italic>\u03f5<\/jats:italic>\n                    \u2010caprolactone (\n                    <jats:italic>\u03f5<\/jats:italic>\n                    \u2010CL). The distinct kinetics of the two monomers enable the facile synthesis of diblock and triblock copolyesters, PCL\u2010\n                    <jats:italic>b<\/jats:italic>\n                    \u2010P(4\n                    <jats:sup>Ph<\/jats:sup>\n                    \u2010BL) and P(4\n                    <jats:sup>Ph<\/jats:sup>\n                    \u2010BL)\u2010\n                    <jats:italic>b<\/jats:italic>\n                    \u2010PCL\u2010\n                    <jats:italic>b<\/jats:italic>\n                    \u2010P(4\n                    <jats:sup>Ph<\/jats:sup>\n                    \u2010BL), in non\u2010coordinating solvents, such as dichloromethane and toluene. Conversely, coordinating solvents like tetrahydrofuran, 2\u2010methyltetrahydrofuran, 2,5\u2010dimethyltetrahydrofuran, 1,4\u2010dioxane, and 1,2\u2010dimethoxyethane facilitate frequent transesterifications, yielding statistical copolyesters P[CL\u2010\n                    <jats:italic>stat<\/jats:italic>\n                    \u2010(4\n                    <jats:sup>Ph<\/jats:sup>\n                    \u2010BL)] with varying ratios of heterosequences. Density functional theory (DFT) calculations confirmed that coordinating solvents stabilize the transition state for transesterification, thereby validating their role in triggering this process. By varying the microstructures and compositions, the resultant copolyesters display tunable thermal and mechanical properties, evolving from robust plastics with an ultimate tensile strength of up to 46.3\u00b13.1\u2005MPa to tough elastomers with &gt;99.3\u2009% elastic recovery. All the copolyesters exhibit remarkable thermal stability (\n                    <jats:italic>T<\/jats:italic>\n                    <jats:sub>d,5%<\/jats:sub>\n                    =376\u2009\u00b0C) and maintain desirable chemical circularity (&gt;92\u2009%), supporting a closed\u2010loop life cycle for sustainable material economy.\n                  <\/jats:p>","DOI":"10.1002\/anie.202415388","type":"journal-article","created":{"date-parts":[[2024,11,11]],"date-time":"2024-11-11T23:05:11Z","timestamp":1731366311000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Solvent\u2010Dependent Sequence\u2010Controlled Copolymerization of Lactones: Tailoring Material Properties from Robust Plastics to Tough Elastomers"],"prefix":"10.1002","volume":"64","author":[{"given":"Chaoqun","family":"Weng","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University  Beijing 100871 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2616-9333","authenticated-orcid":false,"given":"Xiao","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University  Beijing 100871 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0050-6699","authenticated-orcid":false,"given":"Xiaoyan","family":"Tang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University  Beijing 100871 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,11,20]]},"reference":[{"key":"e_1_2_8_1_1","unstructured":"\u00a0"},{"key":"e_1_2_8_2_2","doi-asserted-by":"publisher","DOI":"10.1039\/C7GC01496A"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/chem.201704461"},{"key":"e_1_2_8_4_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2018.10.011"},{"key":"e_1_2_8_5_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-020-0190-4"},{"key":"e_1_2_8_6_2","doi-asserted-by":"publisher","DOI":"10.1021\/acsmacrolett.0c00582"},{"key":"e_1_2_8_7_2","doi-asserted-by":"publisher","DOI":"10.1021\/acsmacrolett.0c00789"},{"key":"e_1_2_8_8_2","doi-asserted-by":"publisher","DOI":"10.1039\/D1GC03901F"},{"key":"e_1_2_8_9_2","doi-asserted-by":"publisher","DOI":"10.1007\/s11426-023-1639-2"},{"key":"e_1_2_8_10_2","doi-asserted-by":"publisher","DOI":"10.1002\/asia.202201167"},{"key":"e_1_2_8_11_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202301850"},{"key":"e_1_2_8_12_2","unstructured":"2019 https:\/\/science.osti.gov\/-\/media\/bes\/pdf\/reports\/2020\/Chemical_Upcycling_Polymers.pdf;"},{"key":"e_1_2_8_13_2","unstructured":"Ellen MacArthur Foundation 2021 https:\/\/www.ellenmacarthurfoundation.org\/universal-policy-goals\/overview;"},{"key":"e_1_2_8_14_2","unstructured":"Ellen MacArthur Foundation 2022 https:\/\/www.ellenmacarthurfoundation.org\/towards-a-circular-economy-for-plastics-in-china;"},{"key":"e_1_2_8_15_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.macromol.2c01694"},{"key":"e_1_2_8_16_2","first-page":"1426","volume":"54","author":"Liao X.","year":"2023","journal-title":"Acta Polym. 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