Key points are not available for this paper at this time.
Abstract Cellulose nanocrystals (CNCs) are bio-based building blocks for sustainable advanced materials with prospective applications in polymer composites, emulsions, electronics, sensors, and biomedical devices. However, their high surface area-to-volume ratio promotes agglomeration, which restrains their performance in size-driven applications, thereby hindering commercial CNC utilization. In this regard, ultrasonication is commonly applied to disperse CNCs in colloidal suspensions; however, ultrasonication methodology is not yet standardized and knowledge of the effects of ultrasound treatments on CNC size distribution is scarce. The major goals of this study were attributed to targeted breakage of CNC agglomerates and clusters by ultrasound. The evolution of particle size distribution and potential de-sulfation by ultrasonication as well as the long-term stability of ultrasonicated CNC suspensions were investigated. Colloidal suspensions of sulfated CNCs were isolated from cotton α-cellulose. Effects of ultrasonication on particle size distribution were determined by asymmetrical flow field-flow fractionation (AF4) coupled with on-line multi-angle light scattering and ultraviolet spectroscopy. These results were complemented with off-line dynamic light scattering. High ultrasound energy densities facilitated cumulative dispersion of CNC clusters. Consequently, the mean rod length decreased logarithmically from 178.1 nm at an ultrasound energy input of 2 kJ g −1 CNC to 141.7 nm (− 20%) at 40 kJ g −1 CNC. Likewise, the hydrodynamic diameter of the particle collective decreased logarithmically from 94.5 to 73.5 nm (− 22%) in the same processing window. While the rod length, below which 95 wt% of the CNCs were found, decreased from 306.5 to 231.8 nm (− 24%) from 2 to 40 kJ g −1 CNC, the shape factor of the main particle fraction ranged from 1.0 to 1.1, which indicated a decreasing number of dimers and clusters in the particle collective. In summary, progressing ultrasonication caused a shift of the particle length distribution to shorter particle lengths and simultaneously induced narrowing of the distribution. The suspension’s electrical conductivity concurrently increased, which has been attributed to faster diffusion of smaller particles and exposure of previously obscured surface charges. Colloidal stability, investigated through electrical AF4 and electrophoretic light scattering, was not affected by ultrasonication and, therefore, indicates no de-sulfation by the applied ultrasound treatment. Occurrence of minor CNC agglomeration at low ultrasound energy densities over the course of 6 months suggest the effect was not unmitigatedly permanent.
Metzger et al. (Wed,) studied this question.