Surface modification of the cellulose nanocrystals through vinyl silane grafting

Incompatibility of nanocellulose with non-polar polymer matrices disrupts the interfacial interaction and results in aggregation and phase separation. In this study a facile and environmentally friendly method was used to partially substitute the surface hydroxyl groups by attaching polysiloxane to impart hydrophobic properties. The silanization reaction proceeded with hydrolysis of triethoxyvinylsilane (TEVS) into reactive silanols followed by condensation to form the branched polymer. These polysiloxane oligomers were chemically grafted to form alkoxy silane bonds on the surface of CNCs. A suitable degree of hydrophilic-hydrophobic balance of the modified CNCs was achieved which improved their dispersion in hydrophobic matrix poly(butylene adipate-co-terephthalate) (PBAT). FTIR, NMR (¹³C and ²⁹Si) and XPS demonstrated successful surface chemical modification and confirmed extent of silanization as a function of silane concentration. XRD showed successful grafting of the vinyl silane agent and confirmed polymorph structure of the nanocellulose was retained. The results from TEM and AFM demonstrated successful coating of nano whiskers at 5 wt% silane loading. The successful grafting of the silane agent with pendant vinyl groups improved surface hydrophobicity. These results show that this facile method produces adequately surface modified CNC which can be used as filler in hydrophobic matrices of bioplastics.