The addition of surface-modified cellulose nanocrystals (CNCs) to polymeric matrices can lead to an enhancement of the mechanical and optical properties of host polymers. The use of surfactants can provide an easy and effective way to change the CNC functionality and to evaluate the effects of surface chemistry in the reinforcement mechanisms. In this work, CNCs were solution blended with polylactic acid (PLA) and melt extruded into films. The PLA toughness increased from 1.70 MJ/m3to 2.74 MJ/m3, a 61% increase, with the addition of 1% of decylamine-modified CNCs without a decrease of the tensile strength or modulus. In this work, we investigated the use of two surfactants, decylamine and cetyltrimethylammonium bromide, to enhance CNC compatibility with the hydrophobic PLA matrix. Decylamine at 1.0 wt.% with respect to CNC loading was found to significantly enhance CNC compatibility and property enhancement. The low concentration of surfactant is notable, as other works typically use significantly higher loadings for CNC incorporation and property enhancement. At high CNC concentrations, mechanical properties decreased but the aligned assembly of the CNCs provided intricate colors to the films when observed between crossed polars. The alignment and nanoscale structure of CNCs within the films play an important role in the properties obtained.
Synthetic Strategies for the Fabrication of Cationic Surface-Modified Cellulose Nanocrystals