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

Danielson, Mary K.; Gainaru, Catalin; Demchuk, Zoriana; Pan, Chuyi; Choi, Jihye; Zhang, Hong‐Hai; Foster, Jeffrey C.; Saito, Tomonori; Rahman, Md Anisur

doi:10.1002/cssc.202500898

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

Journal Article · Tue Jun 17 00:00:00 EDT 2025 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.202500898· OSTI ID:2573085

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Plastics are essential to modern society, but their low recycling rates and inefficient end-of-life management pose a significant environmental challenge. Herein, the efficient strategy for upcycling postconsumer poly(ethylene terephthalate) (PET) waste into robust, closed-loop recyclable vitrimer plastics and composites is presented to address this issue. The catalyst-free aminolysis utilizes readily available amines to deconstruct diverse PET wastes into macromonomers, which are upcycled into vitrimers, 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 (G/CFRV) 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 technoeconomic analysis confirms the costeffectiveness and competitiveness of the facile PET deconstruction approach, which is potentially adaptable to other condensation polymers. Further, this study presents a facile approach to upcycling plastic waste into circular plastics and composites, offering a sustainable solution to global plastic waste management and fostering a circular economy.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2573085

Journal Information:: ChemSusChem, Journal Name: ChemSusChem; ISSN 1864-5631; ISSN 1864-564X

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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