Ionic Liquids Grafted Cellulose Nanocrystals for High-Strength and Toughness PVA Nanocomposite

The surface functionalization of cellulose nanocrystals (CNCs) is of significant importance for promoting its diverse applications. However, the efficient strategy reported so far for cation functionalization of CNCs remains limited owing to the electrostatic attraction between cationic modifiers and electronegative CNCs. Herein, a cationized CNC (CNC-LA-IL) has been successfully prepared in aqueous media by grafting the [VBIm] [BF4], a kind of ionic liquid (IL), on the surface of a sulfated CNC using lactic acid (LA) as a linker molecule. This surface functionalization not only converts the negative charge of CNC suspensions to a positive charge (zeta potential reversed from -35 to +40 mV) but also leads to enhanced thermal stability and redispersibility of the dried CNC. To examine the reinforcing effect of IL-modified CNCs, poly(vinyl alcohol) (PVA)/CNC-LA-IL nanocomposite films were further prepared by the solution casting method. To one's surprise, the as-prepared PVA/CNC-LA-IL films exhibit extraordinary improvement in both the tensile strength (92%) and the toughness (166%) with only a 0.3 wt % CNC loading. This study provides a green and facile method to achieve ionic liquids grafted CNCs for high-performance nanocomposites.