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Nanocellulose-based materials functionalized in supercritical CO2 for antimicrobial wound dressing applications

Abstract : In a context where the need for innovative medical devices is increasing and the environmental issue is becoming a major concern, the objective of the project the aim of the project was to prepare antimicrobial wound dressings using the greenest possible way. For this purpose, nanocelluloses have been chosen as bio-based and biocompatible building blocks for the design of porous architectures and their functionalization with antimicrobial agents was then undertaken in supercritical CO2 medium (CO2sc) used as an alternative to organic solvents and by taking advantage of its specificities such as high diffusivity, easy removal of solvent and residual reagents and compatibility with fragile materials. Thus, 2D and 3D structures, nanopapers, cryogels and aerogels, were prepared from cellulose nanofibrils (CNFs) and nanocrystals (CNCs), and exhibited various properties in terms of morphology, porosity and specific surface area. In order to introduce antibacterial functionality, cryogels prepared from nanocellulose with varied surface chemistries were impregnated in scCO2 with a synthetic antibiotic, ciprofloxacin. Impregnated cryogels exhibited antibacterial activity against both gram-negative and gram-positive bacterial strains. Then, four materials of increasing specific surface area, all prepared from CNFs, were impregnated with an essential oil molecule, thymol. Results show a direct relationship between of the amount of impregnated molecules and the specific surface that leads in the case of cryo- and aerogels to good antimicrobial properties against two types of bacteria and yeast. In a second strategy, covalent grafting of CNFs structures in supercritical CO2 was investigated with a novel antibacterial aminosilane. Surface analysis characterizations methods (X-ray photoelectron spectroscopy, contact angle and surface zeta potential analysis) confirmed the successful grafting on nanopapers. The contact active properties of grafted nanopapers and cryogels were assessed. These results are very promising for the design of antimicrobial bio-based and biocompatible medical devices using supercritical conditions.
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Clémentine Darpentigny. Nanocellulose-based materials functionalized in supercritical CO2 for antimicrobial wound dressing applications. Polymers. Université Grenoble Alpes, 2019. English. ⟨NNT : 2019GREAV052⟩. ⟨tel-02953391⟩

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