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<p>Reversible and recyclable vitrimers have garnered significant attention in materials science due to their unique smart functionalities and sustainability. However, challenges remain in balancing comprehensive properties with dynamic characteristics. This study proposes an innovative catalyst-free copolymerization strategy, utilizing cyanuric chloride as a scaffold to synthesize a highly symmetrical trialdehyde compound (TFPT). This compound is copolymerized with a rigid building block, 3,3′-dimethyl-4,4′-diaminodicyclohexylmethane (DMDC), and a flexible unit, polyetheramine D230 (PEA), yielding a series of polyimines (TDP-x). It is demonstrated that TDP-x polyimines exhibit a high glass transition temperature (up to 183&#xa0;°C), outstanding mechanical properties (tensile strength: 41.1–66.9&#xa0;MPa, elongation at break: 12.4–16.0%), excellent thermal stability, and remarkable reprocessability (&gt; 90% mechanical property retention after three recycling cycles). Additionally, TDP-x displays shape-memory behavior, solvent resistance, and acid degradability. By tailoring molecular architecture and modulating dynamic networks, this work overcomes limitations of conventional rigid systems, synergistically enhancing flexibility, processability, and multi-cycle recyclability. This approach pioneers new pathways for developing high-performance recyclable vitrimers.</p> Graphical Abstract <p></p>

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Catalyst-free design of high-performance polyimine vitrimers: symmetrical monomer architecture enabling balanced rigidity, recyclability and shape-memory properties

  • 期刊论文

  • 发表日期：

    2025年11月18日

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  • Dapeng Zhang,
  • Yan Song,
  • Xiurong Zhao,
  • Hongbing Hu,
  • Caixia Tang,
  • Hui Liu,
  • Linglan Li,
  • Junfeng Miao

摘要

Reversible and recyclable vitrimers have garnered significant attention in materials science due to their unique smart functionalities and sustainability. However, challenges remain in balancing comprehensive properties with dynamic characteristics. This study proposes an innovative catalyst-free copolymerization strategy, utilizing cyanuric chloride as a scaffold to synthesize a highly symmetrical trialdehyde compound (TFPT). This compound is copolymerized with a rigid building block, 3,3′-dimethyl-4,4′-diaminodicyclohexylmethane (DMDC), and a flexible unit, polyetheramine D230 (PEA), yielding a series of polyimines (TDP-x). It is demonstrated that TDP-x polyimines exhibit a high glass transition temperature (up to 183 °C), outstanding mechanical properties (tensile strength: 41.1–66.9 MPa, elongation at break: 12.4–16.0%), excellent thermal stability, and remarkable reprocessability (> 90% mechanical property retention after three recycling cycles). Additionally, TDP-x displays shape-memory behavior, solvent resistance, and acid degradability. By tailoring molecular architecture and modulating dynamic networks, this work overcomes limitations of conventional rigid systems, synergistically enhancing flexibility, processability, and multi-cycle recyclability. This approach pioneers new pathways for developing high-performance recyclable vitrimers.

Graphical Abstract