<p>We report thiourea-based polymer networks (TPNs) synthesized <i>via</i> a simple, by-product-free polyaddition using aromatic diisothiocyanates, short-chain alkylenediamines, and a triamine crosslinker. The TPNs exhibit excellent mechanical performance (tensile strength up to ≈74&#xa0;MPa, elastic modulus of ≈2.4 GPa) along with thermadapt shape memory behaviors. Thiourea moieties act as dual-functional motifs, forming dense hydrogen-bonding interactions while enabling dynamic covalent bond exchange at elevated temperatures. This duality allows for catalyst-free thermal reprocessing and chemical recycling without compromising mechanical integrity. These findings highlight the potential of TPNs as robust, thermally adaptive, and recyclable materials for sustainable and intelligent structural applications.</p> Graphical Abstract <p></p>

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Strong and stiff thiourea-based polymer networks with thermadapt shape memory and on-demand recycling capabilities

  • Jiseok Han,
  • Juntae Joo,
  • Sangmin Park,
  • Wonmoo Byun,
  • Guk-Yun Noh,
  • Jae Hyuk Hwang,
  • Woohwa Lee,
  • Chang-Geun Chae,
  • Sungmin Park,
  • Hyun Kim,
  • Yong Seok Kim,
  • Jae-Hak Choi,
  • Yong-Seok Choi,
  • Dong-Gyun Kim

摘要

We report thiourea-based polymer networks (TPNs) synthesized via a simple, by-product-free polyaddition using aromatic diisothiocyanates, short-chain alkylenediamines, and a triamine crosslinker. The TPNs exhibit excellent mechanical performance (tensile strength up to ≈74 MPa, elastic modulus of ≈2.4 GPa) along with thermadapt shape memory behaviors. Thiourea moieties act as dual-functional motifs, forming dense hydrogen-bonding interactions while enabling dynamic covalent bond exchange at elevated temperatures. This duality allows for catalyst-free thermal reprocessing and chemical recycling without compromising mechanical integrity. These findings highlight the potential of TPNs as robust, thermally adaptive, and recyclable materials for sustainable and intelligent structural applications.

Graphical Abstract