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Crystallizable Aliphatic Chains Enhanced Covalent Adaptable Networks: Fast Reprocessing and Improved Performance.

Yanlin Liu1, Zhen Yu1, Xiwei Xu1,2

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Summary

This study introduces flexible side chains into epoxy covalent adaptable networks (CANs) to enhance reprocessing speed without compromising performance. The findings show improved network dynamics and material properties through innovative molecular design.

Keywords:
covalent adaptable networkscrystallizationepoxy thermosetssegmental motiontransesterification

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Sustainable Materials

Background:

  • Covalent adaptable networks (CANs) offer recyclability but face challenges balancing reprocessing speed and material performance.
  • Existing epoxy-based CANs often require trade-offs between rapid reprocessing and maintaining robust thermal and mechanical properties.

Purpose of the Study:

  • To develop epoxy CANs with accelerated reprocessing capabilities.
  • To investigate the impact of pendent aliphatic chains on transesterification dynamics and network properties.
  • To achieve enhanced reprocessability without sacrificing essential material performance characteristics.

Main Methods:

  • Introduction of pendent aliphatic chain anhydride monoesters into epoxy CANs.
  • Utilizing transesterification as the dynamic mechanism for network adaptation.
  • Employing molecular dynamics simulations to understand segmental mobility.
  • Characterizing thermal and mechanical properties of the modified CANs.

Main Results:

  • Pendent aliphatic chains significantly accelerate transesterification rates by promoting segmental movement and auto-catalysis.
  • Epoxy CANs with a pendent chain carbon number of 12 demonstrated the fastest stress relaxation and reprocessing.
  • Molecular dynamics simulations confirmed that increased segmental mobility enhances reprocessability.
  • Crystallization of the pendent aliphatic chains helped maintain or improve thermal and mechanical properties.

Conclusions:

  • Introducing flexible and crystallizable aliphatic side chains is an effective strategy to accelerate dynamic reactions in CANs.
  • This approach enables faster network rearrangement and reprocessing.
  • The developed epoxy CANs exhibit a superior balance of reprocessability and performance, offering a promising route for sustainable polymers.