Among friction modifier lubricant additives, molybdenum dialkyldithiocarbamate (MoDTC) provides excellent friction behavior in boundary lubricated tribocontacts. It is well established that the low friction obtained with MoDTC is as a result of the formation of lattice structure MoS 2 nanosheets. However, the relationship between the molybdenum species quantity, its distribution on the contact surface, and the friction behavior is not yet fully understood. In this work, Raman microscopy and atomic force microscopy (AFM) have been used with the aim of understanding the link between the friction behavior and the MoDTC/ZDDP tribofilm formation and removal. Tribotests were coupled with a collection of ex-situ Raman intensity maps to analyze the MoS 2 tribofilm buildup. Post-test AFM analyses were implemented on the ball wear scar to acquire the average MoDTC/ZDDP tribofilm thickness. In-situ Raman spectra analyses were carried out to detect the MoS 2 tribofilm removal. A good correlation was achieved between the friction coefficient measurements and Raman maps when using a linear relationship between the microscopic friction and the local amount of MoS 2 tribofilm. After a rapid increase, the average MoDTC/ ZDDP tribofilm thickness levels out to a steady state as the friction drop ceases. The removal rate of MoS 2 from tribofilms, obtained at different temperatures, suggests that the MoS 2 tribofilms are much easier to remove from tribocontacts compared to antiwear ZDDP tribofilms. This is the first study that sets out a framework to link MoS 2 amount and coverage to the friction behavior, providing the basis for developing numerical models capable of predicting friction by taking into account tribochemistry processes.

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