Lubrication is critical in order to achieve high efficiency and reliability of machine elements such as gears, bearings, and other moving mechanical assemblies (MMA). In space applications, tribological properties of lubricants are quickly growing more important. Traditional space systems such as satellites imply MMA such as gyroscopes, antenna pointing mechanisms, and solar array drives. These MMA operate in high vacuum (<10-5 Pa) under lightly loaded conditions. Modern space missions on the other hand, such as remotely operated vehicles used for in-situ Mars exploration relies on different types of MMA. In these robotic systems, electromechanical actuators are being used extensively to provide controlled motion. Gears and bearings in these actuators operate in an atmosphere mainly consisting of CO2 at ~10+3 Pa under heavily loaded contact conditions. In these conditions, the tribosystem is likely to operate in the boundary lubricated regime, with consequent risk of high friction and wear. High molecular weight fluids have significant heritage in space because of their low vapor pressure. They are currently employed as lubricants in a wide range of space applications, as they meet high demands on resistance to vacuum outgassing. Unfortunately, the large molecules are susceptible to degradation under heavy load. Ionic liquids (ILs) on the other hand, are synthetic fluids that consist entirely of ion pairs with opposing charge. The resulting ion bonds enable inherently low vapor pressure of the fluid without the need for a high molecular weight. For this reason ILs have been advocated as potential lubricants for space applications, but so far compatibility issues have hampered their use as lubricants. Countless IL variations are possible, and solutions are thus likely to exist. Constituent ions can be designed individually and combined in various configurations. However, the fundamental understanding of the lubricating mechanism of ionic liquids is still incomplete, and consequently the optimum molecular structure for IL lubricants remain unknown. In this thesis, a stepwise approach to molecular design of IL lubricants is described, and the resulting hydrocarbon-mimicking ionic liquids are evaluated in tribological experiments. In this thesis, the experiments focus on tribological performance, using steel-steel tribopairs in air environment under boundary lubrication (Paper I). Boundary film formation under a range of contact pressures and temperatures, is analyzed after tribotesting by optical profilometry, scanning electron microscopy (SEM), and energy dispersive X- iii ray spectroscopy (EDS) in Paper II. The analysis reveal formation of a highly effective boundary film based on silicate, that can be further enhanced by amine additives. This thesis demonstrates the feasibility of improving tribological performance of ionic liquids by molecular design. / Projekt: Rymdforskarskolan 2015