Closed‐Loop Recyclable Vitrimer Plastics from PET Waste: A Design for Circularity

Plastics are essential to modern society, but their low recycling rates and inefficient end‐of‐life management pose a significant environmental challenge. Here, we present an efficient strategy for upcycling post‐consumer poly(ethylene terephthalate) (PET) waste into robust, closed‐loop recyclable vitrimer plastics and composites to address this issue. Our catalyst‐free aminolysis utilizes readily available amines to deconstruct diverse PET wastes into macromonomers which are upcycled into vitrimer plastics, exhibiting superior mechanical properties and exceeding the ultimate tensile stress and Young’s Modulus of virgin PET by 80% and 150% respectively. These vitrimers exhibit excellent healability, shape memory, thermal reprocessability, and closed‐loop chemical recyclability, enabling quantitative macromonomer recovery even from mixed plastic waste streams and glass/carbon fiber reinforced vitrimer composites. Furthermore, the vitrimer resin yields robust GFRV and CFRV composites with tensile strengths exceeding those of traditional epoxy composites by 100% and 80%, respectively, while maintaining complete chemical recyclability of both constituent materials. A preliminary techno‐economic analysis confirms the cost‐effectiveness and competitiveness of our facile PET deconstruction approach, which is potentially adaptable to other condensation polymers. This study presents a facile approach to upcycling plastic waste into versatile, circular plastics, offering a sustainable solution to global plastic waste management and fostering a circular plastic economy.