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Masterbatch composites made from starch/glycerol mixtures having 50 parts per hundred resin (phr) of three cellulose nanofibrils (CNFs) with different chemical compositions were prepared by pre-gelatinizing starch to create better dispersion of CNFs. The CNF contents were adjusted to 1, 5, 10, and 30 phr by adding ungelatinized starch and glycerol to the obtained masterbatch composite. The composite was then extruded at 150 oC using a twin-screw extruder. The average diameters of the lignocellulose nanofibrils (LCNF), holocellulose nanofibrils (HCNF), and pure cellulose nanofibrils (PCNF) were 53.1, 24.4, and 22.4 nm, respectively. By increasing the CNF content in all nanocomposites, the tensile strength and elastic modulus were improved, whereas the elongation at break was diminished. Tensile properties were higher in the order of thermoplastic starch (TPS)/HCNF > TPS/PCNF > TPS/LCNF nanocomposites when the same CNF content was used. The addition of LCNF and PCNF also improved the thermal and moisture stability, whereas a negative effect was found in the TPS/HCNF nanocomposite. The effect of the LCNF on the thermal and water stability was greater than that of the HCNF and PCNF composites. The water uptake of the TPS/HCNF nanocomposite was higher than that of the TPS without CNFs.

Property comparison of thermoplastic starch reinforced by cellulose nanofibrils with different chemical compositions