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Polyhydroxyalkanoate (PHA) is a biodegradable plastic with great potential for tackling plastic waste and marine pollution issues, but its commercial applications have been limited due to its poor processability. In this study, surface-modified cellulose nanocrystals were used to improve the mechanical properties of PHA composites produced via a melt-extrusion process. Double silanization was conducted to obtain hydrophobically treated CNC-based fillers, using tetraethyl orthosilicate (TEOS) and methyltrimethoxysilane (MTMS). The morphology, particle size distributions, and surface characteristics of the silanized CNCs and their compatibility with a PHA polymer matrix differed by the organosiloxane treatment and drying method. It was confirmed that the double silanized CNCs had hydrophobic surface characteristics and narrow particle size distributions, and thereby showed excellent dispersibility in a PHA matrix. Adding hydrophobically treated CNCs to form a PHA composite, the elongation at break of the PHA composites was improved up to 301%, with little reduction of Young's modulus, compared to pure PHA. Seemingly, the double silanized CNCs added played a similar role to a nucleation agent in the PHA composite. It is expected that such high ductility can improve the mechanical properties of PHA composites, making them more suitable for commercial applications.

Changes in Mechanical Properties of Polyhydroxyalkanoate with Double Silanized Cellulose Nanocrystals Using Different Organosiloxanes