Cellulose nanofibrils constitute an attractive raw material for carbon-neutral, biodegradable, nanostructured materials. Aqueous suspensions of these nanofibrils are stabilized by electrostatic repulsion arising from deprotonated carboxyl groups at the fibril surface. In the present work, a new model is developed for predicting colloidal stability by considering deprotonation and electrostatic screening. This model predicts the fibril-fibril interaction potential at a given pH in a given ionic strength environment. Experiments support the model predictions that aggregation is induced by decreasing the pH, thus reducing the surface charge, or by increasing the salt concentration. It is shown that the primary mechanism for aggregation upon the addition of salt is the surface charge reduction through specific interactions of counterions with the deprotonated carboxyl groups, and the screening effect of the salt is of secondary importance.

Networks of aggregated colloidal particles are solidlike and can sustain an applied shear stress while exhibiting little or no creep; however, ultimately they will catastrophically fail. We show that the time delay for this yielding decreases in two distinct exponential regimes with applied stress. This behavior is universal and found for a variety of colloidal gel systems. We present a bond-rupture model that quantitatively describes this behavior and highlights the role of mesoscopic structures. Our result gives new insight into the nature of yielding in these soft solid materials.

This work aims at understanding the excellent ability of nanocelluloses to disperse carbon nanomaterials (CNs) in aqueous media to form long-term stable colloidal dispersions without the need for chemical functionalization of the CNs or the use of surfactant. These dispersions are useful for composites with high CN content when seeking waterbased, efficient, and green pathways for their preparation. To establish a comprehensive understanding of such dispersion mechanism, colloidal characterization of the dispersions has been combined with surface adhesion measurements using colloidal probe atomic force microscopy (AFM) in aqueous media. AFM results based on model surfaces of graphene and nanocellulose further suggest that there is an association between the nanocellulose and the CN. This association is caused by fluctuations of the counterions on the surface of the nanocellulose inducing dipoles in the sp 2 carbon lattice surface of the CNs. Furthermore, the charges on the nanocellulose will induce an electrostatic stabilization of the nanocellulose−CN complexes that prevents aggregation. On the basis of this understanding, nanocelluloses with high surface charge density were used to disperse and stabilize carbon nanotubes (CNTs) and reduced graphene oxide particles in water, so that further increases in the dispersion limit of CNTs could be obtained. The dispersion limit reached the value of 75 wt % CNTs and resulted in high electrical conductivity (515 S/cm) and high modulus (14 GPa) of the CNT composite nanopapers.

We study the geometry of biopolymer networks and effects of the geometry on bulk mechanical properties. It is shown numerically that the physical network geometry can be quantified statistically and regenerated from its statistical description, so that the regenerated network exhibits the same network mechanics as the physical network in the elastic regime. A collagen-I biopolymer network is used for validation. The method enables parametric studies of the network geometry, whose parameters are often difficult to vary independently in experiments.

Sample-spanning networks of aggregated colloidal particles have a finite stiffness and deform elastically when subjected to a small shear stress. After some period of creep, these gels ultimately suffer catastrophic failure. This delayed yielding is governed by the association and dissociation dynamics of interparticle bonds and the strand structure of the gel. We derive a model which connects the kinetics of the colloids to the erosion of the strand structure and ultimately to macroscopic failure. Importantly, this model relates time-to-failure of the gel to an applied static stress. Model predictions are in quantitative agreement with experiments. It is predicted that the strand structure, characterized by its mesh size and strand coarseness, has a significant impact on delay time. Decreasing the mesh size or increasing the strand thickness makes colloidal gels more resilient to delayed yielding. The quench and flow history of gels modify their microstructures. Our experiments show that a slow quenching increases the delay time due to the coarsening of the strands; by contrast, preshear reduces the delay time, which we explain by the increased mesh size as a result of shear-induced fracture of strands.