Abstract

Chitosan (Chi) and 77KS, a lysine-derived surfactant, form polyelectrolyte complexes that reverse their charge from positive to negative at higher 77KS concentrations, forming aggregates that have been embedded with amoxicillin (AMOX). Dispersion of this complex was used to coat polydimethylsiloxane (PDMS) films, with an additional layer of anionic and hydrophilic hyaluronic acid (HA) as an outer adsorbate layer to enhance protein repulsion in addition to antimicrobial activity by forming a highly hydrated layer in combination with steric hindrance. The formed polysaccharide-based bilayer on PDMS was analyzed by water contact angle measurements, X-ray photoelectron spectroscopy (XPS), and surface zeta (ζ)-potential. All measurements show the existence and adhesion of the two layers on the PDMS surface. Part of this study was devoted to understanding the underlying protein adsorption phenomena and identifying the mechanisms associated with biofouling. Thus, the adsorption of a mixed-protein solution (bovine serum albumin, fibrinogen, γ-globulin) on PDMS surfaces was studied to test the antifouling properties. The adsorption experiments were performed using a quartz crystal microbalance with dissipation monitoring (QCM-D) and showed improved antifouling properties by these polysaccharide-based bilayer coatings compared to a reference or for only one layer, i.e., the complex. This proves the benefit of a second hyaluronic acid layer. Microbiological and biocompatibility tests were also performed on real samples, i.e., silicone discs, showing the perspective of the prepared bilayer coating for medical devices such as prostheses, catheters (balloon angioplasty, intravascular), delivery systems (sheaths, implants), and stents.

Highlights

  • An additional coating of hyaluronic acid (HA) has been shown to improve the properties of protein-repellent and anti-biofilm surfaces, based on a highly hydrated negatively charged hydrophilic layer resulting from a combination of steric repulsive interactions and surface hydration

  • Due to the unique properties of HA, a layer of HA was applied to the Au-PDMS/Chi-77KS/HA and Au-PDMS/Chi-77KS/AMOX/HA samples, to further improve the protein-repelling behavior

  • The additional HA layer was confirmed by X-ray photoelectron spectroscopy (XPS) and surface zeta (ζ)-potential measurements

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Summary

Introduction

An effective implant material should have a functional surface that is antimicrobial, biocompatible with the human organism and disinfects the surrounding tissue after insertion without affecting the human body’s immune response to microorganisms. Current research focuses on advanced surface treatments that prevent microorganism adhesion, inhibit their growth, and interrupt biofilm formation [1,2]. Surface treatment with polyelectrolytes is one of the promising means to combat implant-associated biofilm infections [3]. Polyelectrolytes are charged polymers consisting of ionizable groups attached to polymer chains and show a strong tendency to adsorb on solid surfaces. They are valued as surface coatings and can be used in many processes, including

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