Abstract

Electrospun membranes have been widely used as scaffolds for soft tissue engineering due to their extracellular matrix-like structure. A mussel-inspired coating approach based on 3,4-dihydroxy-DL-phenylalanine (DOPA) polymerization was proposed to graft gelatin (G) onto poly(lactic-co-glycolic) acid (PLGA) electrospun membranes. PolyDOPA coating allowed grafting of gelatin to PLGA fibers without affecting their bulk characteristics, such as molecular weight and thermal properties. PLGA electrospun membranes were dipped in a DOPA solution (2 mg/mL, Tris/HCl 10 mM, pH 8.5) for 7 h and then incubated in G solution (2 mg/mL, Tris/HCl 10 mM, pH 8.5) for 16 h. PLGA fibers had an average diameter of 1.37 ± 0.23 µm. Quartz crystal microbalance with dissipation technique (QCM-D) analysis was performed to monitor DOPA polymerization over time: after 7 h the amount of deposited polyDOPA was 71 ng/cm2. After polyDOPA surface functionalization, which was, also revealed by Raman spectroscopy, PLGA membranes maintained their fibrous morphology, however the fiber size and junction number increased. Successful functionalization with G was demonstrated by FTIR-ATR spectra, which showed the presence of G adsorption bands at 1653 cm−1 (Amide I) and 1544 cm−1 (Amide II) after G grafting, and by the Kaiser Test, which revealed a higher amount of amino groups for G functionalized membranes. Finally, the biocompatibility of the developed substrates and their ability to induce cell growth was assessed using Neonatal Normal Human Dermal Fibroblasts.

Highlights

  • Extracellular matrix (ECM) constitutes the natural environment interacting with cells: it is based on biopolymers arranged in a complex nanoscale topography and supplies haptotactic and chemotactic cues to cells

  • Electrospun poly(lactic-co-glycolic) acid (PLGA) membranes were prepared and surface grafted with G through a polyDOPA intermediate coating, following a mussel inspired approach

  • After gelatin grafting the fiber diameter and the number of fiber junctions increased compared to the samples functionalized with gelatin by simple physical adsorption (Figure 1b,d, respectively). These results suggested that the amount of immobilized gelatin was probably higher on PLGA-DOPA-G membranes as compared to PLGA- G membranes

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Summary

Introduction

Extracellular matrix (ECM) constitutes the natural environment interacting with cells: it is based on biopolymers arranged in a complex nanoscale topography and supplies haptotactic and chemotactic cues to cells. Electrospun matrices, characterized by ultrafine continuous fibers, high surface-to-volume ratio, high porosity, and variable pore-size distribution, can morphologically mimic the structure of the natural ECM and are optimal substrates for Tissue Engineering (TE) [1,2]. Many synthetic and natural polymers have been electrospun to prepare fibrous membranes. Bioartificial materials are combinations of natural and synthetic polymers, aimed at synergistically combining their characteristics, to obtain new multicomponent materials with cell-adhesion ability and tailored mechanical properties and degradation rate [5,6,7,8]. Bioartificial tissue engineered scaffolds were prepared by electrospinning fibrous membranes in which the fiber core was made of a synthetic polymer and the shell consisted of a natural polymer guiding cell response [9]. Bioartificial membranes were prepared by electrospinning blends of natural and synthetic polymers [10] or by grafting natural polymers onto electrospun membranes made of synthetic polymers [11]

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