Cellulosic nanofibers filled poly(β-hydroxybutyrate): Relations between viscoelasticity of composites and aspect ratios of nanofibers.

Dispersion states are vital for fibrous nanocelluloses to be used as reinforcements for polymers, which is highly dependent on geometry of nanocelluloses. Three types of nanocelluloses with various fiber aspect ratios were used to prepare target composite samples with poly(β-hydroxybutyrate) in this work. Viscoelasticity/elastoplasticity were used as probes to detect the flexibility-morphology relations of nanocelluloses in polymer. Cellulose nanocrystals (aspect ratio = 8) were rigid in polymer, retaining their rod-like shape, whereas bacterial celluloses (aspect ratio = 600) fully flexible, forming closely networked structure, and cellulose nanofibers (aspect ratio = 70) semi-flexible, dispersing as loosely flocculated clusters. Owing to these differences, the viscoelastic flow and elastoplastic deformation of three kinds of composites differed from one another. The strain-scaling and hysteresis work-scaling behaviors were then used to establish relaxation scale-structure correlations of target samples. This work provides interesting information around regulating the dispersion of nanocelluloses in polymer composites by tailoring aspect ratios of nanocelluloses.