In this work, the effect of humidity and water intercalation on the friction and wear behavior of few-layers of graphene and graphene oxide (GO) was studied using friction force microscopy. Thickness measurements demonstrated significant water intercalation within GO affecting its surface topography (roughness and protrusions), whereas negligible water intercalation of graphene was observed. It was found that water intercalation in GO contributed to wearing of layers at a relative humidity as low as ∼30%. The influence of surface wettability and water adsorption was also studied by comparing the sliding behavior of SiO/GO, SiO/Graphene, and SiO/SiO interfaces. Friction for the SiO/GO interface increased with relative humidity due to water intercalation and condensation of water. In contrast, it was observed that adsorption of water molecules lubricated the SiOSiO interface due to easy shearing of water on the hydrophobic surface, particularly once the adsorbed water layers had transitioned from "ice-like water" to "liquid-like water" structures. Lastly, an opposite friction trend was observed for the graphene/SiO interface with water molecules failing to lubricate the interface as compared to the dry graphene/SiO contact.
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In this work, the tribological behavior of ultrathin-MoS2 was investigated to understand the independent roles of water and oxidation. Water adsorption was identified as the primary interfacial mechanism for both SiO2/pristine-MoS2 and SiO2/graphene interfaces, however, tribological behavior of pristine-MoS2 was observed to be more sensitive to presence of water due to stronger MoS2-water interaction.Comparison of pristine-MoS2 and oxidized-MoS2 revealed that the oxidation of MoS2 significantly increased its friction and sensitivity to water by play a more detrimental role. The specific effect of oxygen on friction via chemical interactions was studied in isolation through density functional theory (DFT) simulations of a tip sliding on MoS2 basal planes and over edges before and after oxidation. The maximum change in energy, or energy barrier correlating with friction, as the tip moved across the surface, increased after oxidation by up to 66% for the basal plane and by 25% at the edge. Charge density analysis suggests that the more localized and non-uniform interfacial charge distribution on oxygen rich surfaces, as compared to pristine surfaces, leads to higher resistance to sliding. This confirms that oxygen presence alone increases friction and when coupled with the presence of water, both effects are additive in increasing friction.
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