Spontaneous shrinkage drives macromolecule encapsulation into layer-by-layer assembled biopolymer microgels

Campbell, J, Taghavi, A, Preis, A, Martin, S, Skirtach, AG, Franke, J, Volodkin, D ORCID: https://orcid.org/0000-0001-7474-5329 and Vikulina, A ORCID: https://orcid.org/0000-0001-9427-2055, 2023. Spontaneous shrinkage drives macromolecule encapsulation into layer-by-layer assembled biopolymer microgels. Journal of Colloid and Interface Science, 635, pp. 12-22. ISSN 0021-9797

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Abstract

Hypothesis: Recently, the anomalous shrinkage of surface-supported hyaluronate/poly-l-lysine (HA/PLL) microgels (µ-gels), which exceeds that reported for any other multilayer-based systems, has been reported [1]. The current study investigates the capability of these unique µ-gels for the encapsulation and retention of macromolecules, and proposes the shrinkage-driven assembly of biopolymer-based µ-gels as a novel tool for one-step surface biofunctionalization.

Experiments: A set of dextrans (DEX) and their charged derivatives - carboxymethyl (CM)-DEX and diethylaminoethyl (DEAE)-DEX - has been utilized to evaluate the effects of macromolecular mass and net charge on µ-gel shrinkage and macromolecule entrapment. µ-gels formation on the surface of silicone catheters exemplifies their potential to tailor biointerfaces.

Findings: Shrinkage-driven µ-gel formation strongly depends on the net charge and mass content of encapsulated macromolecules. Inclusion of neutral DEX decreases the degree of shrinkage several times, whilst charged DEXs adopt to the backbone of oppositely charged polyelectrolytes, resulting in shrinkage comparable to that of non-loaded µ-gels. Retention of CM-DEX in µ-gels is significantly higher compared to DEAE-DEX. These insights into the mechanisms of macromolecular entrapment into biopolymer-based µ-gels promotes fundamental understanding of molecular dynamics within the multilayer assemblies. Organization of biodegradable µ-gels at biomaterial surfaces opens avenues for their further exploitation in a diverse array of bioapplications.

Item Type:	Journal article
Publication Title:	Journal of Colloid and Interface Science
Creators:	Campbell, J., Taghavi, A., Preis, A., Martin, S., Skirtach, A.G., Franke, J., Volodkin, D. and Vikulina, A.
Publisher:	Elsevier BV
Date:	April 2023
Volume:	635
ISSN:	0021-9797
Identifiers:	Number Type 10.1016/j.jcis.2022.12.115 DOI S0021979722022639 Publisher Item Identifier 1759142 Other
Rights:	Copyright: © 2022 The Author(s). Published by Elsevier Inc. This is an open access article distributed under the terms of the Creative Commons CC-BY Attribution 4.0 International license, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Divisions:	Schools > School of Science and Technology
Record created by:	Linda Sullivan
Date Added:	10 May 2023 10:11
Last Modified:	10 May 2023 10:11
URI:	https://irep.ntu.ac.uk/id/eprint/48916

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