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Engineering Free Volume within Frontal Ring-Opening Metathesis Polymerization via Pendant Plasticization.

Kevin A Stewart1, Francesca J Lombardi1, Sky D Cao1

  • 1Department of Chemistry, University of Utah, Salt Lake City, Utah, USA.

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Summary
This summary is machine-generated.

This study introduces side-chain plasticization for frontal ring-opening metathesis polymerization (FROMP), enabling tunable elastomeric materials. By incorporating alkyl groups, researchers achieved significant property modifications, expanding FROMP applications.

Keywords:
entanglementfrontal polymerizationfrontal ring‐opening metathesis polymerizationmaterial manufacturingreactive manufacturing

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Organic Synthesis

Background:

  • Frontal ring-opening metathesis polymerization (FROMP) offers efficient synthesis of polymers but is limited by rigid backbones.
  • Existing FROMP materials lack tunable properties, restricting their application range.

Purpose of the Study:

  • To develop a side-chain plasticization strategy for FROMP to expand accessible material properties.
  • To investigate the effect of varying alkyl chain lengths on polymer network characteristics and performance.

Main Methods:

  • Copolymerization of norbornene esters with varying n-alkyl side chains (n=8, 12, 16) using dicyclopentadiene (DCPD) or hydrogenated DCPD (DCPD-H2).
  • Characterization of material properties including glass transition temperature (Tg), moduli, and elongation at break.
  • Free-volume analysis using dynamic mechanical analysis (DMA) and solvent swelling ratios.

Main Results:

  • Incorporation of n-alkyl side chains predictably reduced Tg and moduli, transitioning materials from rigid thermosets to elastomers with >800% elongation.
  • Pendant length and distribution were identified as key factors controlling network porosity and mobility.
  • High-alkyl content formulations exhibited nonlinear front propagation (spin modes) and strain-induced whitening.

Conclusions:

  • Side-chain engineering is a versatile strategy to expand FROMP into elastomeric regimes.
  • This approach provides a scalable pathway to soft, tunable, and structurally programmable materials.
  • The findings open opportunities for spatial patterning and molecular alignment in advanced polymer systems.