Spontaneous shrinkage drives macromolecule encapsulation into layer-by-layer assembled biopolymer microgels
Jack Campbell1, Aaron Taghavi2, Alexander Preis3
1Department of Chemistry and Forensics, School of Science and Technology, Nottingham Trent University, Clifton Lane, Nottingham NG11 8NS, United Kingdom; Bavarian Polymer Institute, Friedrich-Alexander-Universität Erlangen-Nürnberg, Dr.-Mack-Straße 77, 90762 Fürth, Germany.
Journal of Colloid and Interface Science
|December 28, 2022
Summary
Surface-supported hyaluronate/poly-l-lysine microgels exhibit anomalous shrinkage. This shrinkage is driven by macromolecule encapsulation, offering a novel method for one-step surface biofunctionalization of biomaterials.
Area of Science:
- Biomaterials Science
- Polymer Chemistry
- Surface Science
Background:
- Hyaluronate/poly-l-lysine (HA/PLL) microgels show unique, anomalous shrinkage exceeding other multilayer systems.
- Understanding macromolecule encapsulation and retention within these microgels is crucial for their application.
Purpose of the Study:
- Investigate the capability of HA/PLL microgels for macromolecule encapsulation and retention.
- Propose shrinkage-driven assembly of biopolymer microgels as a novel tool for one-step surface biofunctionalization.
Main Methods:
- Utilized dextrans (DEX) and charged derivatives (CM-DEX, DEAE-DEX) to assess effects of mass and net charge on microgel shrinkage and entrapment.
- Formed microgels on silicone catheter surfaces to demonstrate biointerface tailoring potential.
Main Results:
- Microgel shrinkage is highly dependent on the net charge and mass of encapsulated macromolecules.
- Neutral DEX inclusion significantly reduces shrinkage; charged DEXs interact with polyelectrolytes, leading to comparable shrinkage.
- Carboxymethyl-dextran (CM-DEX) shows significantly higher retention than diethylaminoethyl-dextran (DEAE-DEX).
Conclusions:
- Insights into macromolecular entrapment mechanisms enhance understanding of molecular dynamics in multilayer assemblies.
- Biodegradable microgel organization on biomaterial surfaces offers potential for diverse bioapplications.
- Shrinkage-driven assembly provides a novel approach for surface biofunctionalization.


