Marine-origin polysaccharides-based free-standing multilayered membranes as sustainable nanoreservoirs for controlled drug delivery

resumo

The layer-by-layer (LbL) assembly technology has been widely used to functionalise surfaces and precisely engineer robust multilayered bioarchitectures with tunable structures, compositions, properties, and functions at the nanoscale by resorting to a myriad of building blocks exhibiting complementary interactions. Among them, marine-origin polysaccharides are a sustainable renewable resource for the fabrication of nanostructured biomaterials for biomedical applications owing to their wide bioavailability, biocompatibility, biodegradability, non-cytotoxicity, and non-immunogenic properties. Chitosan (CHT) and alginate (ALG) have been widely employed as LbL ingredients to shape a wide repertoire of size- and shape-tunable electrostatic-driven multilayered assemblies by exploring their opposite charge nature. However, the insolubility of CHT in physiological conditions intrinsically limits the range of bioapplications of the as-developed CHT-based LbL structures. Herein, we report the preparation of free-standing (FS) multilayered membranes made of water-soluble quaternised CHT and ALG biopolymers for controlled release of model drug molecules. The influence of the film structure in the drug release rate is studied by assembling two distinct set-ups of FS membranes, having the model hydrophilic drug fluorescein isothiocyanate-labelled bovine serum albumin (FITC-BSA) either as an intrinsic building block or added as an outer layer after the LbL assembly process. Both FS membranes are characterised for their thickness, morphology, in vitro cytocompatibility, and release profile, with those having FITC-BSA as an intrinsic LbL ingredient denoting a more sustained release rate. This work opens up new avenues for the design and development of a wide array of CHT-based devices for biomedical applications, overcoming the limitations associated with the insolubility of native CHT under physiological conditions.

palavras-chave

CONTROLLED-RELEASE; CHITOSAN-ALGINATE; POLYMER-FILMS; LAYER; CAPSULES; NANOPARTICLES; STABILITY; COATINGS; BUILDUP; LINKING

categoria

Materials Science

autores

Sousa, CFV; Monteiro, LPG; Rodrigues, JMM; Borges, J; Mano, JF

Grupos

G5 - Materiais Biomiméticos, Biológicos e Vivos

Projectos

Unlocking the scientific excellence and innovation capacity of the University of Aveiro in supramolecular multicomponent biomaterials for enabling advanced biomaterials for healthcare (SUPRALIFE)

Collaboratory for Emerging Technologies, CoLab (EMERGING TECHNOLOGIES)

CICECO - Aveiro Institute of Materials (UIDB/50011/2020)

CICECO - Aveiro Institute of Materials (UIDP/50011/2020)

Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)

Rede Nacional de Ressonância Magnética Nuclear (PTNMR)

agradecimentos

This work was funded by the European Union's Horizon Europe research and innovation programme under the grant agreement No. 101079482 ("SUPRALIFE"). The financial support by the Portuguese Foundation for Science and Technology (FCT) through the individual PhD grants (2020.04408.BD, C. F. V. S.; 2020.06767.BD, L. P. G. M.), and individual Junior Researcher (CEECIND/01363/2018, J. M. M. R.) and Assistant Researcher (2020.00758.CEECIND, J. B.) contracts under the Scientific Employment Stimulus - Individual Call is gratefully acknowledged. This work was developed within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020, UIDP/50011/2020 & LA/P/0006/2020, financed by national funds through the FCT/MCTES (PIDDAC). The NMR spectrometers are part of the National NMR Network (PTNMR) and are partially supported by Infrastructure Project No. 022161 (co-financed by FEDER through COMPETE 2020, POCI and PORL and FCT through PIDDAC). The authors gratefully acknowledge Dr Helene L. Lauzon from Primex ehf (Siglufjordur, Iceland) for kindly providing the chitosan batch used in this work, and Prof. Rute Ferreira and Dr Sandra Correia from CICECO-Aveiro Institute of Materials, Department of Physics, University of Aveiro (Aveiro, Portugal) for the kind assistance with the WCA measurements.