We report a procedure to obtain the search distance used to determine particle contact in dense suspensions of smooth and rough colloids. This method works by summing physically relevant length scales in an uncertainty analysis and does not require detailed quantification of the surface roughness. We suspend sterically stabilized, fluorescent poly(methyl methacrylate) colloids in a refractive index-matched solvent, squalene, in order to ensure hard sphere-like behavior. High speed centrifugation is used to pack smooth and rough colloids to their respective jamming points, ϕ J . The jammed suspensions are subsequently diluted with known volumes of solvent to ϕ < ϕ J . Structural parameters obtained from confocal laser scanning micrographs of the diluted colloidal suspensions are extrapolated to ϕ J to determine the mean contact number at jamming, 〈 z 〉 J . Contact below jamming refers to nearest neighbors at a length scale below which the effects of hydrodynamic or geometric friction come into play. Sensitivity analyses show that a deviation of the search distance by 1% of the particle diameter results in 〈 z 〉 changing by up to 10%, with the error in contact number distribution being magnified in dense suspensions ( ϕ > 0.50) due to an increased number of nearest neighbors in the first coordination shell.
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Hydrodynamic origin for the suspension viscoelasticity of rough colloids
We report the linear rheology for dense suspensions of sterically stabilized smooth and mesoscopically rough colloids interacting as hard particles. Small amplitude oscillatory measurements reveal that rough colloids at high volume fractions exhibit storage and loss moduli that are orders of magnitude greater than smooth colloids. Frequency-concentration superposition is used to collapse the viscoelasticity data onto a master curve, where shift factors suggest a more elastic microstructure and reduced cage volume for rough particles. A combination of the mode-coupling theory, hydrodynamic modeling, and the activated hopping theory shows that these rough particles with significantly reduced localization lengths tend to become trapped in their glassy cages for extended periods of time. High-frequency data show that rough colloids, but not smooth colloids, display a transition from a free-draining to a fully lubricated state above the crossover volume fraction and, furthermore, exhibit solidlike behavior. Scaling analyses support the idea that lubrication forces between interlocking asperities are enhanced, leading to rotational constraints and stress-bearing structures that significantly elevate the viscoelasticity of dense suspensions. The results provide a framework for how particle surface topology affects the linear rheology in applications such as coatings, cement, consumer products, and shock-absorbing materials.
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- NSF-PAR ID:
- 10403198
- Date Published:
- Journal Name:
- Journal of Rheology
- Volume:
- 66
- Issue:
- 5
- ISSN:
- 0148-6055
- Page Range / eLocation ID:
- 895 to 906
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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We report a combined rheology, x-ray photon correlation spectroscopy, and modeling study of gel formation and aging in suspensions of nanocolloidal spheres with volume fractions of 0.20 and 0.43 and with a short-range attraction whose strength is tuned by changing temperature. Following a quench from high temperature, where the colloids are essentially hard spheres, to a temperature below the gel point, the suspensions form gels that undergo aging characterized by a steadily increasing elastic shear modulus and slowing, increasingly constrained microscopic dynamics. The aging proceeds at a faster rate for stronger attraction strength. When the attraction strength is suddenly lowered during aging, the gel properties evolve non-monotonically in a manner resembling the Kovacs effect in glasses, in which the modulus decreases and the microscopic dynamics become less constrained for a period before more conventional aging resumes. Eventually, the properties of the gel following the decrease in attraction strength converge to those of a gel that has undergone aging at the lower attraction strength throughout. The time scale of this convergence increases as a power law with the age at which the attraction strength is decreased and decreases exponentially with the magnitude of the change in attraction. A model for gel aging in which particles attach and detach from the gel at rates that depend on their contact number reproduces these trends and reveals that the non-monotonic behavior results from the dispersion in the rates that the populations of particles with different contact number adjust to the new attraction strength.
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We present a numerical study of non-colloidal spherical and rigid particles suspended in Newtonian, shear thinning and shear thickening fluids employing an immersed boundary method. We consider a linear Couette configuration to explore a wide range of solid volume fractions ( $0.1\leqslant \unicode[STIX]{x1D6F7}\leqslant 0.4$ ) and particle Reynolds numbers ( $0.1\leqslant Re_{p}\leqslant 10$ ). We report the distribution of solid and fluid phase velocity and solid volume fraction and show that close to the boundaries inertial effects result in a significant slip velocity between the solid and fluid phase. The local solid volume fraction profiles indicate particle layering close to the walls, which increases with the nominal $\unicode[STIX]{x1D6F7}$ . This feature is associated with the confinement effects. We calculate the probability density function of local strain rates and compare the latter’s mean value with the values estimated from the homogenisation theory of Chateau et al. ( J. Rheol. , vol. 52, 2008, pp. 489–506), indicating a reasonable agreement in the Stokesian regime. Both the mean value and standard deviation of the local strain rates increase primarily with the solid volume fraction and secondarily with the $Re_{p}$ . The wide spectrum of the local shear rate and its dependency on $\unicode[STIX]{x1D6F7}$ and $Re_{p}$ point to the deficiencies of the mean value of the local shear rates in estimating the rheology of these non-colloidal complex suspensions. Finally, we show that in the presence of inertia, the effective viscosity of these non-colloidal suspensions deviates from that of Stokesian suspensions. We discuss how inertia affects the microstructure and provide a scaling argument to give a closure for the suspension shear stress for both Newtonian and power-law suspending fluids. The stress closure is valid for moderate particle Reynolds numbers, $O(Re_{p})\sim 10$ .more » « less
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$N_1$ $N_2$ $15\,\% \leq \phi \leq 50\,\%$ $Mn$ $Mn < 1$ $N_1$ $N_2$ $\phi < 30\,\%$ $\phi \ge 30\,\%$ $Mn \ge 1$ $\phi \ge 30\,\%$ $\phi = 50\,\%$ $N_1$ $N_2$ $Mn \gg 1$ $Mn = 1$
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1122/8.0000424
