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Enhancing Cellulose Nanofibril Compatibility with Epoxy Resins through a Water-Based Surface Hydrophobization

Kevin Oesef1, Emily D Cranston2,3, Yasmine Abdin1

  • 1Department of Materials Engineering, The University of British Columbia, 6350 Stores Road, Vancouver, British Columbia V6T 1Z4, Canada.

ACS Applied Materials & Interfaces
|May 2, 2025
PubMed
Summary

Hydrophobizing cellulose nanofibrils (CNFs) with tannic acid and hexylamine improves their compatibility in polymer composites. This green strategy enhances mechanical properties like tensile modulus and strength in epoxy resins.

Keywords:
alkylaminecellulose nanofibrilscompositeepoxyhydrophobizationsurface modificationtannic acid

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Nanotechnology

Background:

  • Cellulose nanofibrils (CNFs) offer high specific strength and modulus for composite reinforcement.
  • CNFs' inherent hydrophilicity limits their compatibility with polymer matrices, causing aggregation and reduced composite performance.
  • Addressing CNF hydrophilicity is crucial for unlocking their full potential in advanced composites.

Purpose of the Study:

  • To develop a water-based strategy for hydrophobizing CNFs to improve interfacial compatibility in polymer composites.
  • To investigate the reaction mechanism of tannic acid (TA) and hexylamine (HA) modification on CNFs.
  • To evaluate the impact of modified CNFs on the mechanical properties of epoxy resins.

Main Methods:

  • A one-pot, water-based strategy was employed to hydrophobize CNFs using tannic acid (TA) as a primer and hexylamine (HA) as a hydrophobe, creating CNF-TA-HA.
  • Contact angle measurements were used to confirm the hydrophobicity of the modified CNFs.
  • Colorimetric assays were utilized to study the reaction kinetics of the surface modification process.

Main Results:

  • Modified CNFs (CNF-TA-HA) exhibited a stable water contact angle of 100°, indicating successful hydrophobization.
  • The modification reaction followed a unique two-stage process involving rapid surface reaction and slow diffusion into CNF bundles.
  • Incorporating 1% w/w CNF-TA-HA into epoxy significantly improved tensile modulus (36%) and tensile strength (48%) compared to unmodified CNFs.

Conclusions:

  • The TA-HA hydrophobization strategy effectively enhances the interfacial compatibility of CNFs in epoxy composites.
  • This green and scalable method improves composite mechanical properties without degrading intrinsic CNF characteristics.
  • The approach is adaptable to various cellulose nanomaterials, offering a pathway for advanced composite development.