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Predicting self-diffusion coefficients in semi-crystalline and amorphous solid dispersions using free volume theory.

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A new model predicts active ingredient self-diffusivity in polymers, simplifying formulation design. Kinetic fragility significantly impacts molecular migration, with fragile polymers facilitating faster diffusion.

Keywords:
Amorphous polymersDiffusionDrug diffusion coefficientFragilityFree volume theoryMolecular mobilitySemi-crystalline polymersSolid dispersions

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Area of Science:

  • Materials Science
  • Chemical Engineering
  • Pharmaceutical Sciences

Background:

  • Self-diffusion of active ingredients (AI) in polymeric solid dispersions is crucial for formulation design but difficult to measure.
  • Existing methods for measuring AI self-diffusivity are time-consuming due to slow diffusion kinetics.

Purpose of the Study:

  • To present a time-saving platform for predicting AI self-diffusivity in amorphous and semi-crystalline polymers.
  • To utilize a modified free volume theory (FVT) for accurate diffusivity predictions.

Main Methods:

  • A modified Vrentas and Duda free volume theory (FVT) was employed.
  • The model requires pure-component properties as input.
  • Predictions were made for AI self-diffusion in various polymers across different temperatures, compositions, and crystallinity ranges.

Main Results:

  • The study successfully predicted AI self-diffusion coefficients for imidacloprid, indomethacin, and deltamethrin in several polymers.
  • Kinetic fragility of the solid dispersion was identified as a key factor influencing molecular migration.
  • Fragile polymers showed higher self-diffusion coefficients due to increased mobile regions.

Conclusions:

  • The modified FVT provides a simple and time-saving method for predicting AI self-diffusivity.
  • Kinetic fragility and heterogeneous dynamics significantly influence AI mobility in solid dispersions.
  • The model accounts for structural and thermophysical properties, and diffusion path tortuosity in semi-crystalline polymers.