Polyethylene Materials with Tunable Degradability by Incorporating In-Chain Mechanophores.

Autor: Zhang X; Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs, School of Chemistry and Chemical Engineering, Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai 200240, China., Zhao Y; Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs, School of Chemistry and Chemical Engineering, Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai 200240, China., Chen M; Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs, School of Chemistry and Chemical Engineering, Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai 200240, China., Ji M; Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs, School of Chemistry and Chemical Engineering, Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai 200240, China., Sha Y; Department of Chemistry and Material Science, College of Science, Nanjing Forestry University, Nanjing 210037, China., Nozaki K; Department of Chemistry and Biotechnology, School of Engineering, The University of Tokyo, Tokyo 113-8656, Japan., Tang S; Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs, School of Chemistry and Chemical Engineering, Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University, Shanghai 200240, China.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2024 Aug 28; Vol. 146 (34), pp. 24024-24032. Date of Electronic Publication: 2024 Aug 17.
DOI: 10.1021/jacs.4c07445
Abstrakt: Polyolefins are recognized as fundamental plastic materials that are manufactured in the largest quantities among all synthetic polymers. The chemical inertness of the saturated hydrocarbon chains is crucial for storing and using polyolefin plastics, but poses significant environmental challenges related to plastic pollution. Here, we report a versatile approach to creating polyethylene materials with tunable degradability by incorporating in-chain mechanophores. Through palladium-catalyzed coordination/insertion copolymerization of ethylene with cyclobutene-fused comonomers, several cyclobutane-fused mechanophores were successfully incorporated with varied insertion ratios (0.35-26 mol %). The resulting polyethylene materials with in-chain mechanophores exhibit both high thermal stability and remarkable acid resistance. Upon mechanochemical activation by ultrasonication or ball-milling, degradable functional units (imide and ester groups) are introduced into the main polymer chain. The synergy of mechanochemical activation and acid hydrolysis facilitates the efficient degradation of high molecular weight polyethylene materials into telechelic oligomers.
Databáze: MEDLINE