Abstract
Plastics are critical in facilitating the comfort and quality of everyday life. Most plastics are discarded after a single use, wasting the energy and carbon consumed for their production and incurring environmental costs. Thus, closed-loop production and recycling processes are needed to mitigate energy and carbon loss toward a net-zero carbon economy. Here, we show that poly(ethylene terephthalate) (PET) can be efficiently deconstructed into small-molecule α,ω-dialkenenyl terephthalates using organocatalyzed transesterification. The resulting compounds can be polymerized by acyclic diene metathesis (ADMET) polymerization, affording unsaturated semi-aromatic polyesters with thermomechanical properties dependent on the monomer structure and the catalyst used for their synthesis. High-molecular-weight ADMET polymers form free-standing films that are ductile and tough with mechanical properties similar to widely used commodity plastics. Crucially, the ADMET polymers can be deconstructed to monomers using Retro-ADMET and re-polymerized by ADMET polymerization, establishing closed-loop circularity for a unique class of materials.
| Original language | English |
|---|---|
| Article number | 101734 |
| Journal | Cell Reports Physical Science |
| Volume | 4 |
| Issue number | 12 |
| DOIs | |
| State | Published - Dec 20 2023 |
Funding
This research was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. 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. The 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). The authors thank Yue Yuan for their review of the manuscript. Conceptualization, J.C.F. and T.S.; methodology, J.C.F. and T.S.; investigation, J.C.F. J.Z. M.A. M.A.R. J.T.D. C.G. N.G. and Z.D.; writing – original draft, J.C.F.; writing – review & editing, J.C.F. J.T.D. I.P. and T.S.; supervision, J.C.F. and T.S.; funding acquisition, T.S. and I.P. The authors declare no competing financial interests. We support inclusive, diverse, and equitable conduct of research. This research was supported by the US Department of Energy , Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division . 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. The 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 ). The authors thank Yue Yuan for their review of the manuscript.
| Funders | Funder number |
|---|---|
| DOE Public Access Plan | |
| US government retains | |
| U.S. Department of Energy | |
| Office of Science | |
| Basic Energy Sciences | |
| Division of Materials Sciences and Engineering | |
| UT-Battelle | DE-AC05-00OR22725 |
Keywords
- closed-loop manufacturing
- green chemistry
- olefin metathesis
- plastics upcycling
- polymer chemistry
- polymer deconstruction
- polymer structure-property relationships
