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Revitalizing poly(urea)s via disulfide reconfiguration.

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Supramolecular Engineering

Background:

  • Weak bonds typically form soft materials.
  • Supramolecular engineering can create strong materials but often lack robustness at high temperatures due to entropy penalties.

Purpose of the Study:

  • To develop high-performance poly(urea)s with enhanced structural reconfigurability and robustness.
  • To investigate the impact of disulfide bonds on poly(urea) properties.

Main Methods:

  • Replacing carbon atoms with disulfide bonds in poly(urea)s.
  • Analyzing the effects on hydrogen bond assembly, crystallization, and mechanical properties.
  • Investigating thermal stability, hardness, solvent resistance, and recyclability.

Main Results:

  • Disulfide bonds maintained ordered H-bond assembly while suppressing secondary crystallization.
  • Introduced S─S·H─N interactions, enabling chain mobility and reconfiguration below melting temperatures.
  • Achieved thermoplastic-like reprocessability with thermoset-like robustness (e.g., >2 GPa storage modulus, 150°C creep resistance, ceramic-like hardness).
  • Demonstrated acid-catalyzed depolymerization for closed-loop recyclability.

Conclusions:

  • A two-atom structural modification with disulfide bonds revitalizes semicrystalline poly(urea)s.
  • These materials exhibit a unique combination of processability and robustness.
  • The developed poly(urea)s offer a sustainable solution with closed-loop recyclability.