Rapid Solvent-Free Microcrystalline Cellulose Melt Functionalization withl-Lactide for the Fabrication of Green Poly(lactic acid) Biocomposites

Abstract

A green approach is proposed to achieve a rapid surface functionalization of microcrystalline cellulose (MCC) in 30 min by a solvent-free "grafting from" reaction of l-lactide through compression molding without the need for an inert atmosphere. A sufficient hydrophobization of the MCC surface is achieved with an amount of grafted poly(l-lactic acid) (PLLA) oligomers of 7 wt % with respect to MCC. The obtained MCC-g-PLLA is subsequently melt-compounded with poly(lactic acid) (PLA) through extrusion and injection molding. As a result of higher compatibility and interfacial adhesion of the functionalized filler with PLA, PLA/MCC-g-PLLA biocomposites with a cellulose content ranging from 4 to 20 wt % exhibit an enhancement in important physicochemical properties (i.e., water vapor barrier, crystallinity, stiffness) compared to both pure PLA and formulations containing an equal or higher amount of nonfunctionalized MCC. At the same time, the materials retain the mechanical strength and resistance to thermal degradation of PLA. The physicochemical characteristics, excellent biocompatibility, and biodegradability of PLA and cellulose and the simplicity, rapidity, and cost-effectiveness of the grafting process render these biocomposites suitable for several applications within the plastics domain including packaging, agriculture, automotive, consumer goods, and household appliances.