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Nonlinear rheology of concentrated spherical silica suspensions: 3. Concentration dependence

by: Hiroshi Watanabe, Ming-Long Yao, Kunihiro Osaki, Toshiyuki Shikata, Hirokazu Niwa, Yotaro Morishima
Rheologica Acta, Vol. 38, No. 1. (12 May 1999), pp. 2-13.


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Nonlinear rheology was examined for concentrated suspensions of spherical silica particles (with radius of 40 nm) in viscous media, 2.27/1 (wt/wt) ethylene glycol/glycerol mixture and pure ethylene glycol. The particles were randomly and isotropically dispersed in the media in the quiescent state, and their effective volume fraction &#123eff ranged from 0.36 to 0.59. For small strains, the particles exhibited linear relaxation of the Brownian stress &#134B due to their diffusion. For large step strains &#110, the nonlinear relaxation modulus G(t,&#110) exhibited strong damping and obeyed the time-strain separability. This damping was related to &#110-insensitivity of strain-induced anisotropy in the particle distribution that resulted in decreases of &#134B/&#110. The damping became stronger for larger &#123eff. This &#123eff dependence was related to a hard-core volume effect, i.e., strain-induced collision of the particles that is enhanced for larger &#123eff. Under steady/transient shear flow, the particles exhibited thinning and thickening at low and high &#110&#163, respectively. The thinning behavior was well described by a BKZ constitutive equation using the G(t,&#110) data and attributable to decreases of a Brownian contribution, &#134B/&#110&#163. The thickening behavior, not described by this equation, was related to dynamic clustering of the particles and corresponding enhancement of the hydrodynamic stress at high &#110&#163. In this thickening regime, the viscosity growth &#109+ after start-up of flow was scaled with a strain &#110&#163t. Specifically, critical strains &#110d and &#110s for the onset of thickening and achievement of the steadily thickened state were independent of &#110&#163 but decreased with increasing &#123eff. This &#123eff dependence was again related to the hard-core volume effect, flow-induced collision of the particles enhanced for larger &#123eff.


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