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Monica Bulacu1, Erik van der Giessen

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Summary

Molecular dynamics simulations reveal connector chains enhance polymer-polymer adhesion. The debonding energy scales with chain length, offering insights for industrial applications in polymer reinforcement.

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Area of Science:

  • Polymer Physics
  • Materials Science
  • Computational Chemistry

Background:

  • Enhancing polymer-polymer adhesion is crucial for material performance.
  • Connector chains at interfaces can improve interfacial strength.
  • Understanding disentanglement mechanics is key to designing effective polymer composites.

Purpose of the Study:

  • To investigate the tensile disentanglement of connector chains between polymer bulks using molecular dynamics simulations.
  • To determine the factors controlling the debonding energy (G) between polymer layers.
  • To explore the role of chain length, density, and connectivity on interfacial adhesion.

Main Methods:

  • Extensive molecular dynamics simulations employing a coarse-grained Kremer-Grest model.
  • Modeling polymer chains as sequences of beads connected by springs, including chain stiffness.
  • Analysis of entropic and energetic responses via conformation tensor and internal parameter modifications.

Main Results:

  • Observed forced reptation of connector chains during disentanglement, following an effective 'tube'.
  • Debonding energy (G) scales with connector chain length (n) with an exponent of approximately 2 (G ∝ n^2), consistent with reptation theory.
  • Areal density and chain length are primary determinants of interfacial adhesion; minor variations observed with stitch number and length distribution.

Conclusions:

  • Connector chain length is the dominant factor in polymer-polymer adhesion, with a power-law relationship observed.
  • The number of stitches and random length distribution effects are coupled and require careful consideration, especially for experimental comparisons.
  • Findings provide valuable constitutive laws for simulating polymer adhesion at larger scales, aiding industrial applications like polymer reinforcement.