4.8 Article

Which Biopolymers Are Better for the Fabrication of Multilayer Capsules? A Comparative Study Using Vaterite CaCO3 as Templates

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 2, Pages 3259-3269

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c21194

Keywords

multilayer; polyelectrolyte; calcium carbonate; vaterite; hard templating; sacrificial

Funding

  1. Nottingham Trent University
  2. Europeans Union [LIGHTOPLEX-747245]
  3. NTU Bursary

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Polymer layer-by-layer assembly is a promising method for advanced drug delivery platforms and biomimetic materials, but the design of biopolymer capsules poses challenges. This study examines the formation mechanism of multilayer biocapsules templated upon CaCO3 crystals and evaluates the structure-property relationship of capsules made of different biopolymers.
The polymer layer-by-layer assembly is accounted among the most attractive approaches for the design of advanced drug delivery platforms and biomimetic materials in 2D and 3D. The multilayer capsules can be made of synthetic or biologically relevant (e.g., natural) polymers. The biopolymers are advantageous for bioapplications; however, the design of such biocapsules is more challengeable due to intrinsic complexity and lability of biopolymers. Until now, there are no systematic studies that report the formation mechanism for multilayer biocapsules templated upon CaCO3 crystals. This work evaluates the structure-property relationship for 16 types of capsules made of different biopolymers and proposes the capsule formation mechanism. The capsules have been fabricated upon mesoporous cores of vaterite CaCO3, which served as a sacrificial template. Stable capsules of polycations poly-L-lysine or protamine and four different polyanions were successfully formed. However, capsules made using the polycation collagen and dextran amine underwent dissolution. Formation of the capsules has been correlated with the stability of the respective polyelectrolyte complexes at increased ionic strength. All formed capsules shrink upon core dissolution and the degree of shrinkage increased in the series of polyanions: heparin sulfate < dextran sulfate < chondroitin sulfate < hyaluronic acid. The same trend is observed for capsule adhesiveness to the glass surface, which correlates with the decrease in polymer charge density. The biopolymer length and charge density govern the capsule stability and internal structure; all formed biocapsules are of a matrix-type, other words are microgels. These findings can be translated to other biopolymers to predict biocapsule properties.

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