As a renewable nanomaterial, cellulose nanocrystal (CNC) isolated from wood grants excellent mechanical properties in developing high performance nanocomposites. This study was undertaken to compare the reinforcing efficiency of two different CNCs, i.e., cellulose nanowhiskers (CNWs) and cellulose nanofibrils (CNFs) from hardwood bleached kraft pulp (HW-BKP) as reinforcing agent in polyvinyl alcohol (PVA)-based nanocomposite. The CNWs were isolated by sulfuric acid hydrolysis while the CNFs were isolated by 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-mediated oxidation. Based on measurements using transmission electron microscopy, the individual CNWs were about 6.96±0.87 nm wide and 178±55 nm long, while CNFs were 7.07±0.99 nm wide. The incorporation of CNWs and CNFs into the PVA matrix at 5% and 1% levels, respectively, resulted in the maximum tensile strength, indicating different efficiencies of these CNCs in the nanocomposites. Therefore, these results suggest a relationship between the reinforcing potential of CNCs and their physical characteristics, such as their morphology, dimensions, and aspect ratio.

This work attempted to fabricate organic/inorganic nanocomposite by combining organic cellulose nanofibrils (CNFs), isolated by 2,2,6,6-tetramethylpiperidine-1-oxy radical (TEMPO)-mediated oxidation of native cellulose with inorganic nanoclay. The morphology and dimension of CNFs, and tensile properties and thermal stability of CNF/clay nanocomposites were characterized by transmission electron microscope (TEM), tensile test, and thermogravimetry (TG), respectively. TEM observation showed that CNFs were fibrillated structure with a diameter of about 4.86±1.341 nm. Tensile strength and modulus of the hybrid nanocomposite decreased as the clay content of the nanocomposite increased, indicating a poor dispersion of CNFs or inefficient stress transfer between the CNFs and clay. The elongation at break increased at 1% clay level and then continuously decreased as the clay content increased, suggesting increased brittleness. Analysis of TG and derivative thermogravimetry (DTG) curves of the nanocomposites identified two thermal degradation peak temperatures (Tp1 and Tp2), which suggested thermal decomposition of the nanocomposites to be a two steps-process. We think that Tp1 values from 219.6℃ to 235℃ resulted from the sodium carboxylate groups in the CNFs, and that Tp2 values from 267℃ to 273.5℃ were mainly responsible for the thermal decomposition of crystalline cellulose in the nanocomposite. An increase in the clay level of the CNF/clay nanocomposite predominately affected Tp2 values, which continuously increased as the clay content increased. These results indicate that the addition of clay improved thermal stability of the CNF/clay nanocomposite but at the expense of nanocomposite’s tensile properties.