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<p>Developing low-cost, high-performance, and chemically recyclable alternatives to bulk polyolefin commodities is critical. Aromatic polyesters synthesized via ring-opening copolymerization (ROCOP) of phthalic anhydride (PA) and olefin-derived epoxides are promising candidates. However, achieving high molecular weight (MW) and chemical recyclability to monomers remain key challenges, especially for epoxides with high isomerization tendency including styrene oxide, 2-vinyloxirane, and isobutylene oxide. Here, we report an organic acid-base pair-mediated strategy for the ROCOP of PA and these bulk-olefin-derived epoxides to produce high-MW (<i>M</i><sub>n</sub> = 105.1–163.3 kDa) polyesters. This strategy effectively suppressed acidic impurities-triggered, PA-mediated self-catalytic isomerization of these acid-sensitive epoxides. The produced high-MW polyesters showed superior mechanical and processing properties comparable to commodity polystyrene as well as high tensile strength (53.1–58.9 MPa) and Young’s modulus (2.16–3.02 GPa). Furthermore, these materials can be chemically recycled into PA and aldehyde monomers under mild conditions, enabling the end-of-life recycling options for ROCOP-derived polyesters.</p>

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Acid-base pair-mediated copolymerization of acid-sensitive epoxides and cyclic anhydride for synthesizing recyclable thermoplastics

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月12日

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  • Zhenbiao Xie,
  • Zhenjie Yang,
  • Chenyang Hu,
  • Mingxin Niu,
  • Yulu Zhang,
  • Te Yang,
  • Xuan Pang,
  • Xuesi Chen

摘要

Developing low-cost, high-performance, and chemically recyclable alternatives to bulk polyolefin commodities is critical. Aromatic polyesters synthesized via ring-opening copolymerization (ROCOP) of phthalic anhydride (PA) and olefin-derived epoxides are promising candidates. However, achieving high molecular weight (MW) and chemical recyclability to monomers remain key challenges, especially for epoxides with high isomerization tendency including styrene oxide, 2-vinyloxirane, and isobutylene oxide. Here, we report an organic acid-base pair-mediated strategy for the ROCOP of PA and these bulk-olefin-derived epoxides to produce high-MW (Mn = 105.1–163.3 kDa) polyesters. This strategy effectively suppressed acidic impurities-triggered, PA-mediated self-catalytic isomerization of these acid-sensitive epoxides. The produced high-MW polyesters showed superior mechanical and processing properties comparable to commodity polystyrene as well as high tensile strength (53.1–58.9 MPa) and Young’s modulus (2.16–3.02 GPa). Furthermore, these materials can be chemically recycled into PA and aldehyde monomers under mild conditions, enabling the end-of-life recycling options for ROCOP-derived polyesters.