The increasing demand for low-viscosity engine oil has underscored the role of zinc dialkyldithiophosphates (ZDDP) as a conventional anti-wear and antioxidant additive. It is essential to investigate the influence of modern additives such as cyclopropanecarboxylic acid (CPCa) and Ni nanoparticles on the tribological performance of ZDDP for practical commercial oil application. According to the experimental results, Ni nanoparticles formed a protective film that exhibited a synergistic effect with ZDDP. A significantly higher concentration of sulphur in the tribofilm was detected compared to ZDDP by itself, which was responsible for a 27.6% lower wear loss. Meanwhile, a competitive effect between CPCa and ZDDP resulted in a dramatic increase in friction and unstable anti-wear performance. This was demonstrated by a localized formation of the ZDDP tribofilm on the wear surfaces after the friction test. These results have highlighted the synergistic and competitive effects of emerging additives (CPCa and Ni nanoparticles) in the ZDDP tribofilm formation between the sliding steel contacts. This further suggests a new approach to increase the efficiency of ZDDP’s tribological performance at cold start-up processes.

To comply with the high demand for efficient and sustainable lubrications, carbon-based tribofilms and/or nanomaterials have emerged as a potential solution that can resolve the current major shortcomings of phosphorus- and sulphur-rich tribofilms and protective coatings. Although their employment is still in the early stages of realization and research, these tribofilms receive significant interest due to their capability to continuously and in situ repair/replenish themselves during sliding, which has been an ultimate goal of all moving mechanical systems. Structurally, these tribofilms are complex and predominantly amorphous or disordered with/without graphitic domains (e.g., graphene/graphite, onion-like carbon, etc.). Chemically, the compositions of these tribofilms vary significantly with environments, conditions, and material precursors. Yet, the structural properties of carbon-based tribofilms remain largely ambiguous, which precludes a full understanding of the mechanisms underlying the formation and lubrication performance. This review will summarize the current state-of-art research about the in situ carbon-based tribofilms that have been published since the pioneering works. Particularly, this work will highlight the recent approaches to generate these tribofilms, their associated lubrication performance, current understanding of the formation mechanics, common analytical approaches for these tribofilms, and the compatibility of these tribofilms with other additives. Together, the overall outlooks will be drawn, demonstrating the knowledge gaps and proposing further investigation tactics to tackle these emerging issues.

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