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Experiments and Modeling of Flow-Enhanced Nucleation in LLDPE.

David A Nicholson1, Marat Andreev1, Kenneth L Kearns2

  • 1Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.

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|August 23, 2022
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Summary

This study introduces a new framework to measure flow-enhanced nucleation (FEN) in polymers. The method accurately predicts how shear flow accelerates polymer crystallization, aiding in processing optimization.

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Area of Science:

  • Polymer Science
  • Materials Science
  • Rheology

Background:

  • Flow-enhanced nucleation (FEN) significantly impacts polymer crystallization kinetics.
  • Quantifying FEN is crucial for optimizing polymer processing and material properties.
  • Existing models often lack a direct link between molecular dynamics and macroscopic crystallization behavior.

Purpose of the Study:

  • To develop and validate a computational and experimental framework for quantifying flow-enhanced nucleation (FEN) in polymers.
  • To establish a predictive model linking polymer melt shear history to crystallization kinetics.
  • To demonstrate the framework's efficacy using industrial-grade linear low-density polyethylene (LLDPE).

Main Methods:

  • Experimental kinetic measurements of isothermal crystallization using fast-scanning calorimetry (FSC) on presheared LLDPE melts.
  • Computational modeling of shear effects on melt conformation tensor using the discrete slip-link model (DSM).
  • Relating the conformation tensor to nucleation kinetics acceleration via a validated expression based on nematic order.

Main Results:

  • The developed framework accurately quantifies FEN in LLDPE.
  • The model successfully relates shear-induced changes in molecular conformation to accelerated nucleation kinetics.
  • A single adjustable parameter was determined by fitting to experimental FSC data, validating the model's predictive capability.

Conclusions:

  • The presented framework provides a robust method for quantifying FEN in polymers.
  • This work represents a significant advancement towards integrated processing models for crystallizable polymers.
  • The findings enable better control over polymer crystallization during manufacturing processes.