In this work, we present an innovative strategy for the grafting of an antibacterial agent onto nanocellulose materials in supercritical carbon dioxide (scCO2). Dense cellulose nanofibril (CNF) nanopapers were prepared and subsequently functionalized in supercritical carbon dioxide with an aminosilane, N-(6-aminohexyl)aminopropyltrimethoxysilane (AHA-P-TMS). Surface characterization (X-ray photoelectron spectroscopy, contact angle, ζ-potential analysis) evidenced the presence of the aminosilane. The results show that the silane conformation depends on the curing process: a nonpolycondensed conformation of grafted silane with the amino groups facing outwards was favored by curing in an oven, while the curing step performed in scCO2 yielded CNF structures with the alkyl chain facing outwards. The grafted nanopapers exhibited antibacterial activity, and no antibacterial agent was released into the media. Furthermore, these materials proved to benefit from low cytotoxicity. This study offers a proof of concept for the covalent grafting of active species on nanocellulose structures and the control of aminosilane orientation using a green and controlled approach. These newly designed materials could be used for their antibacterial activity in the biomedical field. Thus, perspectives for topical administration and design of wound dressing could be envisaged.
Keywords: aminosilane; antibacterial; cellulose nanofibrils; functionalization; supercritical carbon dioxide.