Superlubricity of tetrahedral amorphous carbon (ta-C) coatings under boundary lubrication with organic friction modifiers is important for industrial applications, but the underlying mechanisms remain elusive. Here, combined experiments and simulations unveil a universal tribochemical mechanism leading to superlubricity of ta-C/ta-C tribopairs. Pin-on-disc sliding experiments show that ultra- and superlow friction with negligible wear can be achieved by lubrication with unsaturated fatty acids or glycerol, but not with saturated fatty acids and hydrocarbons. Atomistic simulations reveal that, due to the simultaneous presence of two reactive centers (carboxylic group and C=C double bond), unsaturated fatty acids can concurrently chemisorb on both ta-C surfaces and bridge the tribogap. Sliding-induced mechanical strain triggers a cascade of molecular fragmentation reactions releasing passivating hydroxyl, keto, epoxy, hydrogen and olefinic groups. Similarly, glycerol’s three hydroxyl groups react simultaneously with both ta-C surfaces, causing the molecule’s complete mechano-chemical fragmentation and formation of aromatic passivation layers with superlow friction.

In this study, both the plasma process of filtered laser-arc evaporation and the resulting properties of tetrahedral amorphous carbon coatings are investigated. The energy distribution of the plasma species and the arc spot dynamics during the arc evaporation are described. Different ta-C coatings are synthesized by varying the bias pulse time and temperature during deposition. An increase in hardness was observed with the increased overlapping of the bias and arc pulse times. External heating resulted in a significant loss of hardness. A strong discrepancy between the in-plane properties and the properties in the film normal direction was detected specifically for a medium temperature of 120 °C during deposition. Investigations using electron microscopy revealed that this strong anisotropy can be explained by the formation of nanocrystalline graphite areas and their orientation toward the film’s normal direction. This novel coating type differs from standard amorphous a-C and ta-C coatings and offers new possibilities for superior mechanical behavior due to its combination of a high hardness and low in-plane Young’s Modulus.

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To meet the surging needs in energy efficiency and eco-friendly lubricants, a novel superlubricious technology using a vegetable oil and ceramic materials is proposed. By coupling different hydrogen-free amorphous carbon coatings with varying fraction of sp2 and sp3 hybridized carbon in presence of a commercially available silicon nitride bulk ceramic, castor oil provides superlubricity although the liquid vegetable oil film in the contact is only a few nanometres thick at most. Besides a partial liquid film possibly separating surfaces in contact, local tribochemical reactions between asperities are essential to maintain superlubricity at low speeds. High local pressure activates chemical degradation of castor oil generating graphitic/graphenic-like species on top of asperities, thus helping both the chemical polishing of surface and its chemical passivation by H and OH species. Particularly, the formation of the formation of −(CH2−CH2)n− noligomers have been evidenced to have a major role in the friction reduction. Computer simulation unveils that formation of chemical degradation products of castor oil on friction surfaces are favoured by the quantity of sp2-hybridized carbon atoms in the amorphous carbon structure. Hence, tuning sp2-carbon content in hydrogen-free amorphous carbon, in particular, on the top layers of the coating, provides an alternative way to control superlubricity achieved with castor oil and other selected green lubricants.