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.

This study was aimed at the development of a better understanding of the agglomeration behavior of sulfated cellulose nanocrystals (CNCs) in the presence of sulfates with monovalent (NH₄⁺, K⁺, Na⁺) and divalent (Ca²⁺) cations, and to demonstrate their potential in simple and efficient product separation. Protonated CNCs were counterion-exchanged and their ionic strength was increased by adding sulfates of the respective cation to trigger agglomeration. The critical concentrations of agglomeration (CAC) and peptization (CPC) were determined. We found that the agglomeration behavior of CNCs could be attributed to matching affinities between the cations and the sulfate half-ester groups on the CNC surfaces. Based on these findings, a facile and efficient downstream process was designed to separate CNCs from neutralized reactant solutions using CAC and CPC. This method provides colloidally stable CNCs at high yield provided by centrifugation. When salt concentrations in the product are maintained below the CAC, as prepared CNCs from neutralized reactant solutions might be used in hydrogels and emulsions.

Cellulose nanocrystals (CNC) and starch nanoparticles (SNP) have remarkable physical and mechanical characteristics. These properties particularly facilitate their application as high-performance components of bio-based packaging films as alternatives to fossil-based counterparts. This study demonstrates a time-efficient and resource-saving extraction process of CNC and SNP by sulfuric acid hydrolysis and neutralization. The yields of the hydrolyzed products were 41.4% (CNC) and 32.2% (SNP) after hydrolysis times of 3 h and 120 h, respectively. The nanoparticle dispersions were wet-coated onto poly(lactic acid) (PLA) and paper substrates and were incorporated into starch films. No purification or functionalization of the nanoparticles was performed prior to their application. Techno-functional properties such as the permeability of oxygen and water vapor were determined. The oxygen permeability of 5–9 cm³ (STP) 100 µm m⁻² d⁻¹ bar⁻¹ at 50% relative humidity and 23 °C on PLA makes the coatings suitable as oxygen barriers. The method used for the extraction of CNC and SNP contributes to the economic production of these nanomaterials. Further improvements, e.g., lower ion concentration and narrower particle size distribution, to achieve reproducible techno-functional properties are tangible.

Efficient chemical modification of cellulose nanocrystals (CNCs) by grafting commonly involves aprotic solvents, toxic reactants, harsh reaction conditions, or catalysts, which have negative effects on the particle character, reduced dispersibility and requires further purification, if products are intended for biomedical applications. This work, in contrast, presents a robust, facile, and green synthesis protocol for the grafting of an amino-reactive fluorophore like fluorescein isothiocyanate (FITC) on aqueous CNCs, combining and modifying existent approaches in a two-step procedure. Comparably high grafting yields were achieved, which were confirmed by thermogravimetry, FTIR, and photometry. The dispersive properties were confirmed by DLS, AF4-MALS, and TEM studies. The presented route is highly suitable for the introduction of silane-bound organic groups and offers a versatile platform for further modification routes of cellulose-based substrates.

Sulfuric acid‐catalyzed hydrolysis of cellulose commonly isolates cellulose nanocrystals (CNCs). Neutralizing the reactant solution with sodium hydroxide facilitates efficient downstream processing, but residual salt remains in the product. This study examines the reinforcing effects of CNCs from suspensions that contain residual salt on the mechanical properties of thermoplastic starch nanocomposites. By reinforcing starch films with up to 5 wt% CNCs, stiffness and strength are improved by 118% and 79%, respectively, indicating a good dispersion of CNCs in the starch matrix. Compared to nanocomposites incorporating salt‐free CNCs, the remaining salt has no significant impact on the material's mechanical performance. The results indicate great potential of CNCs containing residual salt as biobased, low‐cost nanofiller in hydrophilic polymer matrices.