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<p>The environmental impact of non-recyclable thermoset waste demands sustainable polymer solutions. Existing dynamic covalent boronic ester chemistries operate at relatively low temperatures (&lt;150 °C), resulting in insufficient stability to meet thermoset performance requirements. Here, we overcome these limitations through a <i>N</i>-iminodiacetic acid (<i>N</i>-IDA) boronate system featuring a strengthened internal B–N coordination bond. This enhanced B–N bond (~1.65 Å) endows the dynamic covalent bonds with both exceptional thermal stability and controllable exchange above 150 °C. We leverage this chemistry to develop radical crosslinkers compatible with commercial monomers and thermoplastics. The resulting recyclable thermosets demonstrate exceptional thermal stability, chemical durability under harsh environments (85 °C/85% RH, 7 days), and excellent dimensional stability. This stability–exchange dichotomy is exemplified in heat-shrinkable crosslinked polyethylene (XLPE), where the enhanced B–N coordination maintains network integrity at service temperatures (&lt;150 °C) while enabling thermal reprocessability above 150 °C. By extending the operational range of boronic ester-based dynamic chemistry to high temperature domains, this work provides a scalable pathway toward recyclable thermosets without stability compromises.</p>

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Enhanced B–N coordinated dynamic boronate chemistry for recyclable thermosets with elevated stability

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月18日

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  • Chaoran Xu,
  • Congze He,
  • Jin Dong,
  • Jie Yun,
  • Shicheng Yang,
  • Yuxuan Du,
  • Zhikang Xie,
  • Xiaoru Dong,
  • Zhuo Li,
  • Krzysztof Matyjaszewski,
  • Xiangcheng Pan

摘要

The environmental impact of non-recyclable thermoset waste demands sustainable polymer solutions. Existing dynamic covalent boronic ester chemistries operate at relatively low temperatures (<150 °C), resulting in insufficient stability to meet thermoset performance requirements. Here, we overcome these limitations through a N-iminodiacetic acid (N-IDA) boronate system featuring a strengthened internal B–N coordination bond. This enhanced B–N bond (~1.65 Å) endows the dynamic covalent bonds with both exceptional thermal stability and controllable exchange above 150 °C. We leverage this chemistry to develop radical crosslinkers compatible with commercial monomers and thermoplastics. The resulting recyclable thermosets demonstrate exceptional thermal stability, chemical durability under harsh environments (85 °C/85% RH, 7 days), and excellent dimensional stability. This stability–exchange dichotomy is exemplified in heat-shrinkable crosslinked polyethylene (XLPE), where the enhanced B–N coordination maintains network integrity at service temperatures (<150 °C) while enabling thermal reprocessability above 150 °C. By extending the operational range of boronic ester-based dynamic chemistry to high temperature domains, this work provides a scalable pathway toward recyclable thermosets without stability compromises.