Two-dimensional covalent organic frameworks (2D COFs) are an emerging class of crystalline porous materials formed through covalent bonds between organic building blocks. COFs uniquely combine a large surface area, an excellent stability, numerous abundant active sites, and tunable functionalities, thus making them highly attractive for numerous applications. Especially, their abundant active sites and weak interlayer interaction make these materials promising candidates for tribological research. Recently, notable attention has been paid to COFs as lubricant additives due to their excellent tribological performance. Our review aims at critically summarizing the state-of-art developments of 2D COFs in tribology. We discuss their structural and functional design principles, as well as synthetic strategies with a special focus on tribology. The generation of COF thin films is also assessed in detail, which can alleviate their most challenging drawbacks for this application. Subsequently, we analyze the existing state-of-the-art regarding the usage of COFs as lubricant additives, self-lubrication composite coatings, and solid lubricants at the nanoscale. Finally, critical challenges and future trends of 2D COFs in tribology are outlined to initiate and boost new research activities in this exciting field.

A reduced graphene oxide coating was deposited on a titanium substrate for potential anti-friction applications in nano- or micro-mechanical systems. A γ-aminopropyltriethoxysilane coating was self-assembled on the substrate as an adhesive interlayer beforehand. The process parameters of self-assembly and hydrothermal reduction of graphene oxide coating were explored via water contact angle and tribological tests. Insufficient self-assembly duration of graphene oxide layer can be detected by water contact angle results, and the corresponding coating displayed a higher coefficient of friction and shorter anti-wear lifetime than the optimized one. Proper hydrothermal temperature and duration were also confirmed by its water contact angle, coefficient of friction and anti-wear lifetime. Noticeably, excessive hydrothermal temperature or duration would reduce the coefficient of friction, but diminish the anti-wear resistance. The optimized process parameters were confirmed as assembly duration of graphene oxide coating for 12 h, hydrothermal reduction duration of 6-8 h at 135 °C. Nano tribological behaviors of the obtained hydrothermal reduced graphene oxide coating by AFM tester were then investigated under various testing circumstances. The results showed that the coating performed reliable and low adhesion and friction forces under all circumstances. The nanowear resistance of the titanium substrate was significantly strengthened by the prepared coating.

Adaptive wear-resistant coatings produced by physical vapor deposition (PVD) are a relatively new generation of coatings which are attracting attention in the development of nanostructured materials for extreme tribological applications. An excellent example of such extreme operating conditions is high performance machining of hard-to-cut materials. The adaptive characteristics of such coatings develop fully during interaction with the severe environment. Modern adaptive coatings could be regarded as hierarchical surface-engineered nanostructural materials. They exhibit dynamic hierarchy on two major structural scales: (a) nanoscale surface layers of protective tribofilms generated during friction and (b) an underlying nano/microscaled layer. The tribofilms are responsible for some critical nanoscale effects that strongly impact the wear resistance of adaptive coatings. A new direction in nanomaterial research is discussed: compositional and microstructural optimization of the dynamically regenerating nanoscaled tribofilms on the surface of the adaptive coatings during friction. In this review we demonstrate the correlation between the microstructure, physical, chemical and micromechanical properties of hard coatings in their dynamic interaction (adaptation) with environment and the involvement of complex natural processes associated with self-organization during friction. Major physical, chemical and mechanical characteristics of the adaptive coating, which play a significant role in its operating properties, such as enhanced mass transfer, and the ability of the layer to provide dissipation and accumulation of frictional energy during operation are presented as well. Strategies for adaptive nanostructural coating design that enhance beneficial natural processes are outlined. The coatings exhibit emergent behavior during operation when their improved features work as a whole. In this way, as higher-ordered systems, they achieve multifunctionality and high wear resistance under extreme tribological conditions.