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<p>Thermoset plastics underpin structural materials, electronics and transportation, yet the permanent covalent networks that prevent flow and provide dimensional stability also make them difficult to recycle without sacrificing performance. Here we show that high-performance thermosets can be built around dense chain entanglements, the physical interlacing of long polymer strands, rather than dense permanent crosslinks, with only a small number of selectively cleavable junctions preserving connectivity. Long, rigid, entangled polyolefin backbones generated by frontal polymerization form glassy polymers with high stiffness, high toughness and excellent creep suppression yet can be fully deconstructed into soluble, linear oligomers. Varying oligomer length and end-group chemistry enables their reuse as re-entangling building blocks that regenerate thermosets with thermal and mechanical properties that remain unchanged across generations. The strategy further extends to high-temperature fibre-reinforced composite matrices and additively manufactured structures, establishing chain entanglement as a design principle for durable, regenerable thermosets.</p>

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Chain entanglements enable regeneration of high-performance thermosets

  • 期刊论文

  • 发表日期：

    2026年6月15日

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  • Zhenchuang Xu,
  • Edgar B. Mejia,
  • Tyler C. Price,
  • Ignacio Arretche,
  • Shuyi Zhang,
  • Ruishi Lei,
  • Valerie Chen,
  • Hannah Liu,
  • Shaofeng Huang,
  • Boran Chen,
  • Sameh H. Tawfick,
  • Jeremiah A. Johnson,
  • Nancy R. Sottos,
  • Jeffrey S. Moore

摘要

Thermoset plastics underpin structural materials, electronics and transportation, yet the permanent covalent networks that prevent flow and provide dimensional stability also make them difficult to recycle without sacrificing performance. Here we show that high-performance thermosets can be built around dense chain entanglements, the physical interlacing of long polymer strands, rather than dense permanent crosslinks, with only a small number of selectively cleavable junctions preserving connectivity. Long, rigid, entangled polyolefin backbones generated by frontal polymerization form glassy polymers with high stiffness, high toughness and excellent creep suppression yet can be fully deconstructed into soluble, linear oligomers. Varying oligomer length and end-group chemistry enables their reuse as re-entangling building blocks that regenerate thermosets with thermal and mechanical properties that remain unchanged across generations. The strategy further extends to high-temperature fibre-reinforced composite matrices and additively manufactured structures, establishing chain entanglement as a design principle for durable, regenerable thermosets.