Abstract
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. 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.
| Original language | English |
|---|---|
| Article number | e202500898 |
| Journal | ChemSusChem |
| Volume | 18 |
| Issue number | 18 |
| DOIs | |
| State | Published - Sep 23 2025 |
Funding
This research was supported by the US Department of Energy, office of science, basic energy sciences, materials sciences and engineering division. The fabrication and characterization of glass/carbon fiber composites were supported by the United States Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies office (VTO). The matrix‐assisted laser desorption ionization time‐of‐flight experiment was conducted at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, office of science user facility at Oak Ridge National Laboratory. This manuscript has been authored by UT‐Battelle, LLC, under contract DE‐AC05‐00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid‐up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe‐public‐access‐plan).
Keywords
- PET upcycling
- closed-loop recycling
- recyclable composites
- shape memory
- vitrimers