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Register a new userPredicting and assessing rupture in protein gels under oscillatory shear
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Soft materials may break irreversibly upon applying sufficiently large shear oscillations, a process which physical mechanism remains largely elusive. In this work, the rupture of protein gels made of sodium caseinate under an oscillatory stress is shown to occur in an abrupt, brittle-like manner. Upon increasing the stress amplitude, the build-up of harmonic modes in the strain response can be rescaled for all gel concentrations. This rescaling yields an empirical criterion to predict the rupture point way before the samples are significantly damaged. Fatigue experiments under stress oscillations of constant amplitude can be mapped onto the former results, which indicates that rupture is independent of the temporal pathway in which strain and damage accumulate. Finally, using ultrasonic imaging, we measure the local mechanical properties of the gels before, during and after breakdown, showing that the strain field remains perfectly homogeneous up to rupture but suddenly gives way to a solid-fluid phase separation upon breakdown.
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We examine microstructural and mechanical changes which occur during oscillatory shear flow and reformation after flow cessation of an intermediate volume fraction colloidal gel using rheometry and Brownian Dynamics (BD) simulations. A model depletion colloid-polymer mixture is used, comprising of a hard sphere colloidal suspension with the addition of non-adsorbing linear polymer chains. Results reveal three distinct regimes depending on the strain amplitude of oscillatory shear. Large shear strain amplitudes fully break the structure which results into a more homogenous and stronger gel after flow cessation. Intermediate strain amplitudes densify the clusters and lead to highly heterogeneous and weak gels. Shearing the gel to even lower strain amplitudes creates a less heterogonous stronger solid. These three regimes of shearing are connected to the microscopic shear-induced structural heterogeneity. A comparison with steady shear flow reveals that the latter does not produce structural heterogeneities as large as oscillatory shear. Therefore oscillatory shear is a much more efficient way of tuning the mechanical properties of colloidal gels. Moreover, colloidal gels presheared at large strain amplitudes exhibit a distinct nonlinear response characterized largely by a single yielding process while in those presheared at lower rates a two step yield process is promoted due to the creation of highly heterogeneous structures.
Cellulose nanocrystals (CNC) are naturally-derived nanostructures of growing importance for the production of composites having attractive mechanical properties, and offer improved sustainability over purely petroleum-based alternatives. Fabrication of CNC composites typically involves extrusion of CNC suspensions and gels in a variety of solvents, in the presence of additives such as polymers and curing agents. However, most studies so far have focused on aqueous CNC gels, yet the behavior of CNC-polymer gels in organic solvents is important to their wider processability. Here, we study the rheological behavior of composite polymer-CNC gels in dimethylformamide, which include additives for both UV and thermal crosslinking. Using rheometry coupled with in-situ infrared spectroscopy, we show that under external shear, CNC-polymer gels display progressive and irreversible failure of the hydrogen bond network that is responsible for their pronounced elastic properties. In the absence of cross-linking additives, the polymer-CNC gels show negligible recovery upon cessation of flow, while the presence of additives allows the gels to recover via van der Waals interactions. By exploring a broad range of shear history and CNC concentrations, we construct master curves for the temporal evolution of the viscoelastic properties of the polymer-CNC gels, illustrating universality of the observed dynamics with respect to gel composition and flow conditions. We therefore find that polymer-CNC composite gels display a number of the distinctive features of colloidal glasses and, strikingly, that their response to the flow conditions encountered during processing can be tuned by chemical additives. These findings have implications for processing of dense CNC-polymer composites in solvent casting, 3D printing, and other manufacturing techniques.
The aggregation of protein-stabilised emulsions leads to the formation of emulsion gels. These soft solids are classically envisioned as droplet-filled matrices. Here however, it is assumed that protein-coated sub-micron droplets contribute to the network formation in a similar way to proteins. Emulsion gels are thus envisioned as composite networks made of proteins and droplets. Emulsion gels with a wide range of composition are prepared and their viscoelasticity and frequency dependence are measured. Their rheological behaviours are then analysed and compared with the properties of pure gels presented in the first part of this study. The rheological behaviour of emulsion gels is shown to depend mostly on the total volume fraction, while the composition of the gel indicates its level of similarity with either pure droplet gels or pure protein gels. These results converge to form an emerging picture of protein-stabilised emulsion gel as intermediate between droplet and protein gels. This justifies a posteriori the hypothesis of composite networks, and opens the road for the formulation of emulsion gels with fine-tuned rheology.
When calcium salts are added to an aqueous solution of polysaccharide pectin, ionic cross-links form between pectin chains, giving rise to a gel network in dilute solution. In this work, dynamic light scattering (DLS) is employed to study the microscopic dynamics of the fractal aggregates (flocs) that constitute the gels, while rheological measurements are performed to study the process of gel rupture. As calcium salt concentration is increased, DLS experiments reveal that the polydispersities of the flocs increase simultaneously with the characteristic relaxation times of the gel network. Above a critical salt concentration, the flocs become interlinked to form a reaction-limited fractal gel network. Rheological studies demonstrate that the limits of the linear rheological response and the critical stresses required to rupture these networks both decrease with increase in salt concentration. These features indicate that the ion-mediated pectin gels studied here lie in a `strong link regime that is characterised by inter-floc links that are stronger than intra-floc links. A scaling analysis of the experimental data presented here demonstrates that the elasticities of the individual fractal flocs exhibit power-law dependences on the added salt concentration. We conclude that when pectin and salt concentrations are both increased, the number of fractal flocs of pectin increases simultaneously with the density of crosslinks, giving rise to very large values of the bulk elastic modulus.
We report on experiments that probe the stability of a two-dimensional jammed granular system formed by imposing a quasistatic simple shear strain $gamma_{rm I}$ on an initially stress free packing. We subject the shear jammed system to quasistatic cyclic shear with strain amplitude $deltagamma$. We observe two distinct outcomes after thousands of shear cycles. For small $gamma_{rm I}$ or large $deltagamma$, the system reaches a stress-free, yielding state exhibiting diffusive strobed particle displacements with a diffusion coefficient proportional to $deltagamma$. For large $gamma_{rm I}$ and small $deltagamma$, the system evolves to a stable state in which both particle positions and contact forces are unchanged after each cycle and the response to small strain reversals is highly elastic. Compared to the original shear jammed state, a stable state reached after many cycles has a smaller stress anisotropy, a much higher shear stiffness, and less tendency to dilate when sheared. Remarkably, we find that stable states show a power-law relation between shear modulus and pressure with an exponent $betaapprox 0.5$, independent of $deltagamma$. Based on our measurements, we construct a phase diagram in the $(gamma_{rm I},deltagamma)$ plane showing where our shear-jammed granular materials either stabilize or yield in the long-time limit.
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