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<p>Photoinitiated free radical polymerization (PFRP) is favoured for its simplicity and rapid processing, but typically yields heterogeneous networks with densely crosslinked nanoclusters embedded in a loosely connected matrix, leading to structural weaknesses and mechanical deterioration. Here we incorporate a photocoupling reaction into PFRP systems to convert weakly interconnected nanoclusters into a robust, interlinked network, facilitating effective load transfer between soft and hard phases and enhancing the mechanical properties. This is achieved by partially substituting vinyl moieties with <i>o</i>-nitrobenzyl groups, which generate nitroxides upon photoirradiation with a temporal delay. This allows nanoclusters to form initially, and then enables propagating radicals to couple efficiently within them. Hydrogels synthesized via this approach demonstrate boosted tensile strength up to 20-fold and toughness up to 70-fold compared with PFRP methods, and still gelate within seconds. This strategy demonstrates versatility across various systems and offers a scalable approach for producing high-performance hydrogels and polymer networks.</p><p></p>

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Photocoupling of propagating radicals during polymerization realizes universal network strengthening

  • 期刊论文

  • 发表日期：

    2025年9月2日

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  • Bingkun Bao,
  • Chutong Shi,
  • Qingmei Zeng,
  • Ting Chen,
  • Chaonan Xiao,
  • Li Jiang,
  • Tuan Liu,
  • Jing Lyu,
  • Wenxin Wang,
  • Linyong Zhu,
  • Qiuning Lin

摘要

Photoinitiated free radical polymerization (PFRP) is favoured for its simplicity and rapid processing, but typically yields heterogeneous networks with densely crosslinked nanoclusters embedded in a loosely connected matrix, leading to structural weaknesses and mechanical deterioration. Here we incorporate a photocoupling reaction into PFRP systems to convert weakly interconnected nanoclusters into a robust, interlinked network, facilitating effective load transfer between soft and hard phases and enhancing the mechanical properties. This is achieved by partially substituting vinyl moieties with o-nitrobenzyl groups, which generate nitroxides upon photoirradiation with a temporal delay. This allows nanoclusters to form initially, and then enables propagating radicals to couple efficiently within them. Hydrogels synthesized via this approach demonstrate boosted tensile strength up to 20-fold and toughness up to 70-fold compared with PFRP methods, and still gelate within seconds. This strategy demonstrates versatility across various systems and offers a scalable approach for producing high-performance hydrogels and polymer networks.