We have investigated the tribological properties of surfaces with adsorbed poly(L-lysine)-graft-poly(ethylene glycol) (PLL-g-PEG) sliding in aqueous glycerol solutions under different lubrication regimes. Glycerol is a polar, biocompatible liquid with a significantly higher viscosity than that of water. Macrotribological performance was investigated by means of pin-on-disk and mini-traction-machine measurements in glycerol-PLL-g-PEG-aqueous buffer mixtures of varying compositions. Adsorption studies of PLL-g-PEG from these mixtures were conducted with the quartz-crystal-microbalance technique. The enhanced viscosity of the glycerol-containing lubricant reduces the coefficient of friction due to increased hydrodynamic forces, leading to a more effective separation of the sliding partners, while the presence of hydrated polymer brushes at the interface leads to an entropically driven repulsion, which also helps mitigate direct asperity–asperity contact between the solid surfaces under boundary-lubrication conditions. The combination of polymer layers on surfaces with aqueous phases of enhanced viscosity thus enables the friction to be reduced by several orders of magnitude, compared to the behavior of pure water, over a large range of sliding speeds. The individual contributions of the polymer and the aqueous glycerol solutions in reducing the friction have been studied across different lubrication regimes.
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