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In this study, we demonstrate a solvent\u2010switching strategy to upcycle waste polyethylene terephthalate (PET) into monomer terephthalic acid (TPA) and key bulk feedstocks for biodegradable polymers, such as lactic acid (LA) or glycolic acid (GA). PET undergoes rapid and mild depolymerization into its monomers TPA and ethylene glycol (EG) under the catalysis of a manganese complex. When methanol (MeOH) is used as the solvent, it undergoes selective dehydrogenative coupling with in situ generated EG, efficiently yielding TPA and LA with yields exceeding 98%. By replacing MeOH with\n                    <jats:italic>tert<\/jats:italic>\n                    \u2010amyl alcohol (\n                    <jats:italic>t<\/jats:italic>\n                    \u2010AmOH), PET is quantitatively converted into TPA and GA. The PET conversion mechanism was elucidated through deuterium\u2010labeling experiments and molecular model studies. This work presents a sustainable and innovative approach for upcycling waste PET into high\u2010value products while opening a new route to synthesize biopolymer monomers, which are essential for developing chemically recyclable and biodegradable polymers, thereby advancing the production of sustainable single\u2010use polymer products.\n                  <\/jats:p>","DOI":"10.1002\/anie.202505490","type":"journal-article","created":{"date-parts":[[2025,6,7]],"date-time":"2025-06-07T06:14:03Z","timestamp":1749276843000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["Adjustable Upcycling of Polyethylene Terephthalate to Biodegradable Polymer Monomers by Mn\u2010Catalyzed Solvent Switching Strategy"],"prefix":"10.1002","volume":"64","author":[{"given":"Shun","family":"Zhang","sequence":"first","affiliation":[{"name":"Collaborative Innovation Center for Eco\u2010Friendly and Fire\u2010Safety Polymeric Materials 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