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Restoring Carboxylates on Highly Modified Alginates Improves Gelation, Tissue Retention and Systemic Capture.

C T Moody1, A E Brown2, N P Massaro3

  • 1Joint Department of Biomedical Engineering, University of North Carolina at Chapel Hill and North Carolina State University at Raleigh, NC United States of America; Comparative Medicine Institute, North Carolina State University, Raleigh, NC United States of America.

Acta Biomaterialia
|November 3, 2021
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Restoring carboxyl groups in alginate hydrogels during modification improves their mechanical properties and tissue retention. This advancement enhances alginate

Keywords:
AlginateBioconjugationClick chemistryDrug captureIonic cross-linking

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Area of Science:

  • Biomaterials Science
  • Hydrogel Engineering
  • Tissue Engineering

Background:

  • Alginate hydrogels are versatile biomaterials for drug delivery and tissue engineering.
  • Traditional alginate modification depletes carboxyl groups, compromising gel integrity and calcium cross-linking.
  • High-substitution alginate modifications often lead to significant mechanical property loss.

Purpose of the Study:

  • To investigate alginate modifications that replenish carboxyl groups to overcome mechanical property loss.
  • To assess the impact of restored carboxyl groups on hydrogel mechanics, including calcium cross-linking, shear-thinning, and self-healing.
  • To evaluate the in vivo performance of modified alginate hydrogels for tissue retention and drug delivery applications.

Main Methods:

  • Synthesized alginate hydrogels with azide modifications designed to restore carboxyl groups.
  • Characterized hydrogel properties: calcium cross-linking, shear-thinning, and self-healing.
  • Assessed tissue retention at intramuscular injection sites and cyclooctyne capture in vivo.

Main Results:

  • Alginate modifications restoring carboxyl groups maintained calcium cross-linking and hydrogel self-healing properties.
  • High-degree carboxyl-restoring modifications improved tissue retention at injection sites.
  • These modified hydrogels demonstrated enhanced capture of blood-circulating cyclooctynes compared to controls.

Conclusions:

  • Alginate modifications that replenish carboxyl groups significantly improve hydrogel mechanics and in vivo performance.
  • This approach overcomes limitations of traditional high-substitution modifications.
  • Restoring carboxyl groups offers a promising strategy for advanced clinical applications of alginate hydrogels.