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Rational Design of Ionomer Microstructures for Thermally Reprocessable Materials with Creep Resistance and

Chia-Chi Tsai1, Hanwen Fan2, Yuxiao Zhou2

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New diblock copolymers (ionomers) offer high creep resistance and recoverability, combined with excellent thermal processability. This breakthrough in sustainable polymer design enables reprocessable elastomers with enhanced mechanical integrity.

Keywords:
block copolymercreep resistanceionomerrecoverabilityreprocessable elastomerself-assemblystructure−property relationshipsustainability

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Nanotechnology

Background:

  • Designing sustainable polymers requires balancing mechanical properties like creep resistance with reprocessability.
  • Conventional ionomers often sacrifice thermal processability due to ion dissociation at elevated temperatures.

Purpose of the Study:

  • To develop novel charge-neutral diblock copolymers (ionomers) with improved creep resistance and recoverability.
  • To achieve thermal processability in ionomers by controlling ion distribution and self-assembly.

Main Methods:

  • Synthesis of diblock copolymers with 18 mol % ammonium chloride.
  • Characterization of mechanical properties including creep resistance and recoverability.
  • Analysis of self-assembled morphology using techniques like transmission electron microscopy.
  • Evaluation of thermal processability via compression molding.

Main Results:

  • Diblock ionomers exhibited >90% recovery after five creep cycles and were compression moldable at 80 °C.
  • These ionomers self-assembled into an inverse hexagonal (iHEX) morphology with a continuous glassy ionic matrix and rubbery neutral cylinders.
  • The nanostructure, featuring large interdomain spacing (>30 nm), enhanced elasticity and prevented softening at high temperatures, unlike statistical ionomers.
  • The unentangled flexible blocks within the cylinders facilitated processability.

Conclusions:

  • Precise control over ion distribution in diblock ionomers enables the creation of reprocessable elastomers with superior mechanical properties.
  • This work establishes a general design principle for nanostructured dynamic polymers with enhanced integrity, recoverability, and sustainability.
  • The developed ionomers outperform conventional statistical ionomers in terms of both mechanical performance and processability.