Abstract

To enhance the cytocompatibility of polycaprolactone (PCL), cell-adhesive gelatin is covalently immobilized onto the PCL film surface via two surface-modified approaches: a conventional chemical immobilization process and a surface-initiated atom transfer radical polymerization (ATRP) process. Kinetics studies reveal that the polymer chain growth from the PCL film using the ATRP process is formed in a controlled manner, and that the amount of immobilized gelatin increases with an increasing concentration of epoxide groups on the grafted P(GMA) brushes. In vitro cell adhesion and proliferation studies demonstrate that cell affinity and growth are significantly improved by the immobilization of gelatin on PCL film surfaces, and that this improvement is positively correlated to the amount of covalently immobilized gelatin. With the versatility of the ATRP process and tunable grafting efficacy of gelatin, this study offers a suitable methodology for the functionalization of biodegradable polyesters scaffolds to improve cell-material interactions.

Highlights

  • Due to its slow degradation rate in vivo, good processability, and appropriate mechanical properties, polycaprolactone (PCL) is currently being extensively investigated as a scaffold material for tissue engineering applications [1,2,3,4,5,6,7,8]

  • With the versatility of the atom transfer radical polymerization (ATRP) process and tunable grafting efficacy of gelatin, this study offers a suitable methodology for the functionalization of biodegradable polyesters scaffolds to improve cell–material interactions

  • PCL substrates were successfully modified via the conventional chemical immobilization process and surfaceinitiated ATRP of glycidyl methacrylate (GMA)

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Summary

Introduction

Due to its slow degradation rate in vivo, good processability, and appropriate mechanical properties, polycaprolactone (PCL) is currently being extensively investigated as a scaffold material for tissue engineering applications [1,2,3,4,5,6,7,8]. One such alternative is the use of surface-initiated atom transfer radical polymerization (ATRP) method to covalently attach polymer brushes in a tunable and controllable manner [33,34,35] This approach allows the preparation of polymer brushes bearing reactive pendant groups, such as hydroxyl, carboxylic acid, or epoxide groups, which provide highly reactive binding sites for bioactive macromolecules at the brush interfaces [36]. Gelatin was used as the model protein, as its cell-binding properties have been previously demonstrated [38] Using both a conventional chemical immobilization process and surface-initiated ATRP, gelatin was covalently immobilized onto the PCL substrates with different surface-grafting densities. In vitro cell adhesion, spreading and proliferation studies were carried out to evaluate the cytocompatibility of the modified PCL surface

Materials
Preparation of Polycaprolactone Film and Aminolysis Process
Immobilization of Gelatin onto the Aminolyzed PCL Film Surface
Surface-initiated ATRP of GMA and Conjugation of Gelatin
Determination of Grafting Density of Polymer Brushes and Conjugated Gelatin
Characterization of Surface-Functionalized PCL films
Cell Adhesion and Proliferation
Cell Imaging
2.10 Statistical Analysis
Aminolysis of PCL Film Surface
Surface-Initiated ATRP of GMA and Immobilization of Gelatin
Surface Wettability and Topography
Cell Adhesion
Cell Proliferation
Stability of Gelatin-Immobilized Surface
Conclusion
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