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Tuning the Hydrophilic/Hydrophobic Balance to Control the Structure of Chitosan Films and Their Protein Release Behavior

  • Research Article
  • Theme: Recent Trends in the Development of Chitosan-Based Drug Delivery Systems
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Abstract

The control over the crystallinity of chitosan and chitosan/ovalbumin films can be achieved via an appropriate balance of the hydrophilic/hydrophobic interactions during the film formation process, which then controls the release kinetics of ovalbumin. Chitosan films were prepared by solvent casting. The presence of the anhydrous allomorph can be viewed as a probe of the hydrophobic conditions at the neutralization step. The semicrystalline structure, the swelling behavior of the films, the protein/chitosan interactions, and the release behavior of the films were impacted by the DA and the film processing parameters. At low DAs, the chitosan films neutralized in the solid state corresponded to the most hydrophobic environment, inducing the crystallization of the anhydrous allomorph with and without protein. The most hydrophilic conditions, leading to the hydrated allomorph, corresponded to non-neutralized films for the highest DAs. For the non-neutralized chitosan acetate (amorphous) films, the swelling increased when the DA decreased, whereas for the neutralized chitosan films, the swelling decreased. The in vitro release of ovalbumin (model protein) from chitosan films was controlled by their swelling behavior. For fast swelling films (DA = 45%), a burst effect was observed. On the contrary, a lag time was evidenced for DA = 2.5% with a limited release of the protein. Furthermore, by blending chitosans (DA = 2.5% and 45%), the release behavior was improved by reducing the burst effect and the lag time. The secondary structure of ovalbumin was partially maintained in the solid state, and the ovalbumin was released under its native form.

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Acknowledgements

We are grateful to Dominique Gillet (Mahtani Chitosan, India) for complimentarily providing the chitosan samples. We also thank all the BM2-D2AM staff in the CRG group for the help and expertise during the SAXS/WAXS experiments at the ESRF (Figs. 3, 4, and 6) and Ruben Vera for technical assistance at the Centre de Diffraction Henry Longchambon at Université Claude Bernard Lyon 1 (Fig. 5).

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Authors and Affiliations

  1. Ingénierie des Matériaux Polymères, CNRS UMR 5223, Univ Lyon, Université Claude Bernard Lyon 1, 15 bd Latarjet, 69622, Villeurbanne Cedex, France

    Jose Becerra, Guillaume Sudre, Isabelle Royaud, Thierry Delair & Laurent David

  2. Institut Jean Lamour, CNRS UMR 7198, Université de Lorraine, Parc de Saurupt CS 50840, 54011, Nancy Cedex, France

    Isabelle Royaud

  3. Institut de Biologie et Chimie des Protéines (IBCP), Bases Moléculaire et Structurales des Systèmes Infectieux, UMR 5086, 7 passage du Vercors, 69367, Lyon cedex 07, France

    Roland Montserret & Bernard Verrier

  4. CERMAV, Univ. Grenoble Alpes, 38000, Grenoble, France

    Cyrille Rochas

  5. CERMAV, CNRS, 38000, Grenoble, France

    Cyrille Rochas

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  1. Jose Becerra
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  2. Guillaume Sudre
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Correspondence to Laurent David.

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Becerra, J., Sudre, G., Royaud, I. et al. Tuning the Hydrophilic/Hydrophobic Balance to Control the Structure of Chitosan Films and Their Protein Release Behavior. AAPS PharmSciTech 18, 1070–1083 (2017). https://doi.org/10.1208/s12249-016-0678-9

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