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

Zong-Bin Lu, Shun-Ran Peng, Zhe Wang, Yu Xiong, Lei Xia (), Guang Chen, Xuan Nie, Chun-Yan Hong (), Ze Zhang () and Ye-Zi You ()
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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

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-64559-9

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