In-situ engineering catalytically active surfaces for tribocatalysis with layered double hydroxide nanoparticles

Ensuring long-lasting lubrication is vital for sustainable machinery operation, made possible by self-regenerating carbon-based tribofilms via tribocatalysis. Conventional methods use expensive catalytic coatings, posing challenges for replacement and maintenance in practice. Here, we are proposing catalytic layered double hydroxide (LDH) nanoparticles as cost-effective and easily replenished lubricant additives to engineer catalytically active surfaces in situ where binary and ternary LDHs with Ni²⁺, Co²⁺, and/or Cu²⁺ divalent cations alongside Al³⁺ trivalent cations are investigated for lubrication performance. Under 100 °C sliding condition equivalent to the lubricating temperature in an internal combustion engine, NiCoAl–CO₃ LDH exhibits the lowest wear losses alongside the durable low-friction regime. This excellent performance is attributed to Co-containing spinel and oxide phases in the catalytic tribo-oxide layer which help stabilize and maintain the microstructures of the tribo-oxide layer. In contrast, deterioration in lubrication performance at this temperature was observed for copper-containing LDHs, especially NiCuAl–CO₃ LDHs, which is due to the reduction of metallic oxides that drive phase separation in the catalytic oxide tribo-layers. The more stable tribo-oxide layers can result in thick, durable carbon-based tribofilm during sliding along with higher resistance to plastic deformation bulk interlayer. This study offers valuable insight into the synergy of catalytic oxide materials, opening avenues for a rational design of innovative catalytic nano-materials for tribocatalysis processes.