Siloxane-based polymers (polysiloxanes) exhibit a range of volume, viscosity, and pressure-viscosity behaviors that are strongly influenced by the macromolecular structure. In this report, a combination of extant rheological models is applied to develop a molecular-rheological modeling formalism that predicts polysiloxane rheological properties, such as specific volume, which means density, viscosity, and pressure-viscosity index variations with macromolecular structure, pressure, and temperature. Polysiloxane molecular features are described in terms of alkyl branch length L, pendant type J, density of branch functional monomers Q, and degree of polymerization DP. Both new and published data are used for model parameter determination and validation. Several siloxane-based polymers with alkyl, aryl, alkyl-aryl, cycloalkyl, and halogenated branches were synthesized to examine the modeled relationship between their molecular structures and rheological behaviors.
Siloxane-based polymers (polysiloxanes) are susceptible to temporary shear-thinning that manifests as a reduction of elastohydrodynamic film thickness with increasing entrainment speed or effective shear rate. The departure from Newtonian film thickness can be predicted with the power-law exponent ns, an indicator of the severity of shear-thinning in a polymeric fluid that is influenced by the macromolecular structure. In this paper, a combination of extant rheological and tribological models is applied to determine the power-law exponent of several polysiloxanes using film thickness measurements. Film thickness data at several temperatures and slide-to-roll ratios are used to validate the methodology for several siloxane-based polymers with alkyl and aryl branches.
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