Spin-Coated Polysaccharide-Based Multilayered Freestanding Films with Adhesive and Bioactive Moieties

Abstract

Freestanding films based on catechol functionalized chitosan (CHI), hyaluronic acid (HA), and bioglass nanoparticles (BGNPs) were developed by spin-coating layer-by-layer assembly (SA-LbL). The catechol groups of 3,4-dihydroxy-l-phenylalanine (DOPA) present in the marine mussels adhesive proteins (MAPs) are the main factors responsible for their characteristic strong wet adhesion. Then, the produced films were cross-linked with genipin to improve their stability in wet state. Overall, the incorporation of BGNPs resulted in thicker and bioactive films, hydrophilic and rougher surfaces, reduced swelling, higher weight loss, and lower stiffness. The incorporation of catechol groups onto the films showed a significant increase in the films’ adhesion and stiffness, lower swelling, and weight loss. Interestingly, a synergetic effect on the stiffness increase was observed upon the combined incorporation of BGNPs with catechol-modified polymers, given that such films were the stiffest. Regarding the biological assays, the films exhibited no negative effects on cellular viability, adhesion, and proliferation, and the BGNPs seemed to promote higher cellular metabolic activity. These bioactive LbL freestanding films combine enhanced adhesion with improved mechanical properties and could find applications in the biomedical field, such as guided hard tissue regeneration membranes.

LbL Nano-Assemblies: A Versatile Tool for Biomedical and Healthcare Applications

“…Recently, free-standing films based on catechol functionalized chitosan, hyaluronic acid, and bio-glass nanoparticles were developed by spin-coating LbL [ 79 ]. The incorporation of nanoparticles led to thicker and more hydrophilic films, with rougher surfaces, lower swelling, higher weight loss, and better stiffness.…”

Green approaches for extraction, chemical modification and processing of marine polysaccharides for biomedical applications

“…The effects of either hydration or ionic cross-linking have also been demonstrated as contributing to the development of smart self-sustained membranes denoting adhesive properties and shape memory capability ( Figure 4A ) to be used as implantable biomaterials via minimally invasive surgery ( Borges et al, 2015 ; Silva et al, 2016 ). In addition, bioinspired free-standing membranes functionalized with catechol moieties have shown enhanced mechanical strength, cellular adhesion and proliferation, and adhesive properties for being used as bio-adhesive patches for wound healing and general surgery applications ( Scognamiglio et al, 2016 ; Sousa et al, 2018 ; Moreira et al, 2020 ).…”

A platform for functionalization of cellulose, chitin/chitosan, alginate with polydopamine: A review on fundamentals and technical applications

“…Depending on the deposition method, the morphology and wettability of dopa-chitosan films could be adapted [141]: the interdiffusion of different polyelectrolyte layers was lower and the structure was more homogeneous after spin-coating compared to dip-coating, while the spin-coated films present higher thermal stability, stiffness and lower swelling. Although the adhesive properties somewhat decreased after incorporation of the silver nanoparticles, there was a synergistic effect of silver and catechol on the film stiffness [142]. Alternatively, the silver nanoparticles could be separately coated with catecholconjugated chitosan in order to enhance antibacterial properties [143].…”