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Microfluidic Assembly of Degradable, Stereocomplexed Hydrogel Microparticles.

Gianna G Tutoni1, Samantha M McDonald1, Ruoyu Zhong2

  • 1Department of Chemistry, Duke University, Durham, North Carolina 27708, United States.

Journal of the American Chemical Society
|May 15, 2024
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This study introduces a novel method for creating tunable hydrogel microparticles (HMPs) using stereocomplexation, a physical cross-linking technique. This approach avoids covalent methods, enabling more translationally relevant HMPs for tissue engineering and drug delivery.

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Area of Science:

  • Biomaterials Science
  • Polymer Chemistry
  • Tissue Engineering
  • Drug Delivery

Background:

  • Hydrogel microparticles (HMPs) show promise in tissue engineering and drug delivery.
  • Covalent cross-linking methods limit the translational potential of HMPs.
  • Stereocomplexation offers a robust, degradable alternative for HMP fabrication.

Purpose of the Study:

  • To develop translationally relevant hydrogel microparticles (HMPs) using stereocomplexation.
  • To demonstrate the fabrication of well-defined HMPs with tunable sizes.
  • To confirm stereocomplexation and enable functionalization of HMPs.

Main Methods:

  • Polymerization of 4-arm polyethylene glycol (PEG) stars with poly(l-lactic acid) (PLLA).
  • Synthesis of complementary propargyl-containing ABA cross-linkers with poly(d-lactic acid) (PDLA).
  • Microfluidic fabrication of HMPs via stereocomplexation and stabilization in deionized water.
  • Characterization using wide-angle X-ray scattering (WAXS) and differential scanning calorimetry (DSC).
  • Functionalization via thiol-yne click chemistry.

Main Results:

  • Fabrication of well-defined HMPs with controlled diameters (33.7–105.7 μm) via microfluidics.
  • WAXS confirmed stereocomplexed poly(lactic acid) (PLA) formation.
  • DSC verified stereocomplexation with characteristic crystallization and melting points.
  • Successful pre- or post-assembly functionalization using thiol-yne click chemistry.

Conclusions:

  • Stereocomplexation provides a viable, non-covalent cross-linking strategy for HMP fabrication.
  • The developed microfluidic method allows for precise control over HMP size.
  • The propargyl handle enables versatile functionalization for advanced applications in tissue engineering and drug delivery.