11 february 2019 - Materials, Mechanical, Civil Engineering, Electrochemistry Ph.D. title
Functionalization of cellulose nanofibrils for the development of biobased medical devices.
Julien BRAS, Associate Professor HDR, Grenoble INP-Pagora / LGP2 ♦♦ Naceur BELGACEM, Professor, Grenoble INP-Pagora / LGP2 ♦♦ Elisa ZENO, Research Engineer (CTP)
In line with the ever-increasing academic and industrial interest for wood derived nanocellulose, the present work investigates the chemical surface modification of cellulose nanofibrils (CNFs) for biomedical application.
Drugs and prodrugs of active principle ingredients (APIs) were covalently immobilized or adsorbed onto CNFs films or suspensions. For covalent immobilization, the first strategy selected calls for water-based and single step esterification of CNF films. The resulting materials demonstrated antibacterial activity against both gram-positive and gram-negative bacterial strains, with a prolonged contact-active effect.
In the second strategy, CNFs suspensions were modified through a multistep reaction, involving amidation and click chemistry, still water-based. Highly innovative characterization tools, such as dynamic nuclear polarization (DNP) enhanced nuclear magnetic resonance (NMR), complemented well-established techniques to confirm the success of grafting.
In parallel to covalent immobilization, an adsorption strategy was also adopted, on both CNFs films and suspensions. Then, the CNF films with grafted or adsorbed APIs were used for preparing 100% CNF membrane for potential topical applications. Another component of this work used CNF suspensions with grafted or adsorbed APIs that were embedded in collagen matrices to prepare composites for designing soft tissue repair implants. Antibacterial activity against both aerobic and anaerobic bacteria, together with controlled release properties were assessed confirming that such composites present the expected active properties, and can be used for the design of innovative medical devices.
The CERISE project, conducted under the auspices of the Tec21 Laboratory of Excellence and the Carnot PolyNat Institute, aims to develop a new process for manufacturing cellulose nanofibrils (CNF) with a high dry matter content and low energy consumption. Twin screw extrusion (TSE) – industrially well-known energy-efficient and highly adaptable technique – was optimized to produce CNF at 20 % dry content. By decreasing considerably their water content, this new strategy improves their transport cost, their storage and extends their field of application.
The objectives were to
• Develop new pretreatments of cellulose fibers to facilitate the nanofibrillation and produce high quality functionalized CNF.
• Optimize TSE screw profile and conditions to produce CNF.
• Prepare new materials made of this new type of CNF.
Four chemical pretreatments, identified as easily industrializable, have been optimized. Extrusion nanofibrillation was simulated by software to obtain optimal extrusion conditions. This cost-effective approach was validated at semi-industrial scale. Various applications are considered for these new NFC with a high dry matter content.