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Catalytic Control of Crystallization in Dynamic Networks.

Alexa S Kuenstler1, Christopher N Bowman1,2

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Catalyst nucleophilicity controls polymer bond exchange rates, impacting crystallization. Faster bond exchange initially slows crystallization but promotes long-term crystal rearrangement and growth.

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Chemical Engineering

Background:

  • Semicrystalline polymer networks rely on dynamic covalent bonds for self-healing and recyclability.
  • Understanding the interplay between bond exchange dynamics and crystallization is crucial for designing advanced polymer materials.

Purpose of the Study:

  • To investigate how catalyst nucleophilicity influences thiol-thioester bond exchange dynamics.
  • To determine the effect of varying bond exchange rates on the crystallization behavior of polymer networks.

Main Methods:

  • Utilized a model semicrystalline polymer network with catalysts of varying nucleophilic strength.
  • Employed differential scanning calorimetry (DSC) for isothermal crystallization measurements.
  • Performed Lauritzen-Hoffman analysis to study nucleation barriers.

Main Results:

  • Catalyst nucleophilicity tuned covalent bond exchange time scales (τ) over 10^1–10^3 s.
  • Increased bond exchange rates led to decreased melting temperatures and slowed crystallization kinetics.
  • A significant increase in the secondary nucleation barrier was observed in dynamic networks.

Conclusions:

  • Catalyst-controlled bond exchange dynamics directly influence polymer crystallization.
  • While faster bond exchange initially hinders crystallization, it facilitates long-term crystal rearrangement and growth.
  • These findings offer insights into designing dynamic polymer networks with tunable properties.