In the present article, the rheological behavior and phase stability of concentrated silica suspensions were investigated experimentally by examining the effects of particle size and temperature. The silica particles were stabilized by adsorption of a silane coupling agent, ␥-methacryloxypropyl triethoxy silane ͑MPTES͒. The MPTES-coated silica particles behaved like hard spheres and exhibited the dispersion stability in tetrahydrofurfuryl alcohol which was used as a refractive-index matching solvent. For a monodisperse suspension, the limiting viscosities at high shear rates were correlated satisfactorily with the Krieger-Dougherty equation until the particle volume fraction reached 0.45 above which the limiting high-shear-rate viscosities did not exist. The highly concentrated monodisperse suspensions above ϭ 0.50 displayed the rapidly shear thinning viscosity at low shear rates and underwent the shear thickening at high shear rates. Specifically, the onset of shear thickening shifted to a higher shear rate either as temperature rose or as the suspension became stable. The dichroism from light passed in the flow-gradient direction probed the most effectively the order-disorder transition such as disappearance of hexagonally ordered layered structure and formation of particle clustering, which caused shear thickening at high shear rates. The abrupt change in dichroism caused by the breakdown of hexagonally layered structure occurred almost 1 decade before the onset of shear thickening. Finally, the bimodal suspensions prepared here possessed the reduced shear viscosity and stress in comparison with the monodisperse suspensions of identical volume fraction. The degree of the viscosity reduction became conspicuous for concentrated suspensions usually above ϭ 0.40.
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