Effect of Base Oil and Thickener on Texture and Flow of Lubricating Greases: Insights from Bulk Rheometry, Optical Microrheology and Electron Microscopy

The structure and flow behavior of lubricating greases depend on the base oil and the type and concentration of the dissolved thickener. In this study, the linear viscoelastic properties of greases were characterized by combining oscillatory shear and squeeze flow covering a broad frequency range (0.1-10(5) rad s(-1)). Multiple-particle tracking (MPT) microrheology and scanning electron microscopy (SEM) provided further insight into local viscoelastic properties and sample structure on a submicron-length scale. The type and viscosity of the base oil did not affect the absolute value of the complex viscosity and the filament shape formed by a given thickener. High-frequency shear modulus data, however, indicated that the thickener lithium 12-hydroxystearate formed stiffer networks/filaments in poly-alpha-olefins than in mineral oils. As expected, the viscosity increased with increased thickener concentrations, but microscopy and high-frequency rheometry revealed that the thickness, length, and stiffness of the individual filaments did not change. In mineral oil, the 12-hydroxystearate thickeners yielded higher viscosity than the corresponding stearates with the same metal ion. The filamentous lithium thickeners created stronger networks than the roundish aggregates formed by magnesium and zinc stearate. Network mesh sizes varying between approximately 100 nm and 300 nm were consistently determined from SEM image analysis and MPT experiments. The MPT experiments further disclosed the existence of gel-like precursors of approximately 130 mu m at thickener concentrations far below the critical value at which a sample-spanning network resulting in a characteristic grease texture is formed.