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S/O and vinyl isomerization enables ultrafast cationic ring-opening polymerization toward CO2-derived polythioester with migrated in-chain C=C substituents

Author

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  • Zong-Bin Lu

    (University of Science and Technology of China)

  • Shun-Ran Peng

    (University of Science and Technology of China)

  • Zhe Wang

    (University of Science and Technology of China)

  • Yu Xiong

    (University of Science and Technology of China)

  • Lei Xia

    (Hefei University of Technology)

  • Guang Chen

    (University of Science and Technology of China)

  • Xuan Nie

    (University of Science and Technology of China)

  • Chun-Yan Hong

    (University of Science and Technology of China)

  • Ze Zhang

    (University of Science and Technology of China)

  • Ye-Zi You

    (University of Science and Technology of China)

Abstract

Developing high-performance CO2-based polymers is promising to address the challenges of CO2 sequestration and the environmental impact of petroleum-based plastics. The δ-lactone 3-ethylidene-6-vinyltetrahydro-2H-pyran-2-one and its derivatives, synthesized from CO2 with 1,3-butadiene, have emerged as very promising CO2-derived monomers. However, their general ring-opening polymerizations face challenges with thermodynamics and kinetics, generally resulting in long reaction times, low conversions, and low-molecular-weight polyesters with poor mechanical properties. Herein, we report a dual isomerization-driven cationic ring-opening polymerization (DI-CROP) of a CO2-derived thionolactone, 3-ethyl-6-vinyltetrahydro-2H-pyran-2-thione, in which the relayed S/O and vinyl isomerizations significantly enhance polymerization activity, enabling the rapid synthesis of high-molecular-weight CO2-based polythioesters, achieving near-quantitative conversion within just a few minutes. Also, the relayed S/O and vinyl isomerizations in DI-CROP can easily migrate C=C substituents on the ring of thionolactone into its backbone. These features further enable the production of sustainable CO2-based materials through efficient copolymerization and post-polymerization functionalization. This study enriches the realm of isomerization-driven polymerizations, and provides a new synthetic approach to CO2-derived polymeric materials.

Suggested Citation

  • Zong-Bin Lu & Shun-Ran Peng & Zhe Wang & Yu Xiong & Lei Xia & Guang Chen & Xuan Nie & Chun-Yan Hong & Ze Zhang & Ye-Zi You, 2025. "S/O and vinyl isomerization enables ultrafast cationic ring-opening polymerization toward CO2-derived polythioester with migrated in-chain C=C substituents," Nature Communications, Nature, vol. 16(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-64559-9
    DOI: 10.1038/s41467-025-64559-9
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    References listed on IDEAS

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    1. Cameron Hepburn & Ella Adlen & John Beddington & Emily A. Carter & Sabine Fuss & Niall Mac Dowell & Jan C. Minx & Pete Smith & Charlotte K. Williams, 2019. "The technological and economic prospects for CO2 utilization and removal," Nature, Nature, vol. 575(7781), pages 87-97, November.
    2. Coralie Jehanno & Jill W. Alty & Martijn Roosen & Steven Meester & Andrew P. Dove & Eugene Y.-X. Chen & Frank A. Leibfarth & Haritz Sardon, 2022. "Critical advances and future opportunities in upcycling commodity polymers," Nature, Nature, vol. 603(7903), pages 803-814, March.
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