Abstract
Accumulation of plastic waste in the environment is not only a pressing environmental problem but also a waste of resources. Developing chemically recyclable plastics is deemed a viable approach to address the ever-growing plastic crisis, but the synthesis of circular polyolefins remains challenging. Here we demonstrate a ring-strain matched concept for the tailored synthesis of circular polyolefins. By designing a well-defined 16-membered unsaturated lactone (Ester-16), a family of chemically recyclable, high-molecular-weight, high-density polyethylene (HDPE)-like materials is produced by the copolymerization of cyclooctene (COE) with Ester-16, followed by exhaustive hydrogenation. These HDPE-like materials have the desirable bulk properties of HDPE. They can be degraded into a well-defined and easily separable macromonomer, specifically AB-like telechelic PE. The molecular weight of the macromonomer can be precisely tailored as required and depends solely on the feed ratio of [COE]/[Ester-16]. The recycled macromonomer can be easily repolymerized into a high-molecular-weight HDPE-like material. This macromonomer–polymer–macromonomer lifecycle rather than monomer–polymer–monomer lifecycle can be repeated with quantitative yields using a facile isolation process. Overall, this work opens opportunities to improve the sustainability of plastics.
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Fig. 1: Circular HDPE synthesis for sustainable use.
Fig. 2: Unsaturated lactones applied in ROMP.
Fig. 3: Comprehensive properties of degradable polyethylenes.
Fig. 4: Tailored synthesis of circular polyethylenes.
Fig. 5: ‘Macromonomer–polymer–macromonomer’ circular polyethylenes.
Data availability
All data supporting the findings of this study are available in the text, Source data and the Supplementary materials: (1) Supplementary Information: Supplementary Tables 1–6; general synthesis and polymerization, depolymerization, repolymerization and hydrogenation procedures, characterization, and analysis data; Supplementary Figs. 1–79: NMR, NOESY and ESI–MS for monomer; NMR, IR, DSC, DMA, WXRD, GPC, TGA, WCA and tensile testing for polymers; DFT calculation details. (2) Supplementary XYZ file (Supplementary Data 2) from DFT calculation for monomers. (3) The X-ray crystallographic coordinates for structures reported in this study have been deposited at the Cambridge Crystallographic Data Centre (CCDC), under deposition number 2376771. These data can be obtained free of charge from The Cambridge Crystallographic Data Centre via www.ccdc.cam.ac.uk/data_request/cif, and Supplementary cif file can also be found in Supplementary Data 1. Source data are provided with this paper.
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Acknowledgements
We acknowledge financial support from the National Natural Science Foundation of China (nos. 22122110 for Z.J. and 22171038 for X.K.), and the Jilin Provincial Science and Technology Department Program (no. 20230101347JC for Z.J.).
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State Key Laboratory of Polymer Science and Technology, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, China
Peng-An Chen, Kangkang Li & Zhongbao Jian
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei, China
Peng-An Chen & Zhongbao Jian
College of Pharmacy, Dalian Medical University, Dalian, China
Xiaohui Kang
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Z.J. and P.-A.C. conceived this project. P.-A.C. performed all experiments, X.K. conducted DFT calculation and K.L. discussed data. Z.J. wrote the paper.
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Correspondence to Zhongbao Jian.
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Chen, PA., Kang, X., Li, K. et al. Tailored synthesis of circular polyolefins. Nat Sustain (2025). https://doi.org/10.1038/s41893-025-01524-w
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Received:21 September 2024
Accepted:11 February 2025
Published:11 March 2025
DOI:https://doi.org/10.1038/s41893-025-01524-w
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