The natural cartilage layer exhibits excellent interface low friction and good load-bearing properties based on the mechanically controlled adaptive lubrication mechanism. Understanding and imitating such a mechanism is important for developing high-load-bearing water-lubrication materials. Here, we report the successful preparation of thermoresponsive layered materials by grafting a poly(3-sulfopropyl methacrylate potassium salt) (PSPMA) polyelectrolyte brush onto the subsurface of an initiator-embedded high strength hydrogel [poly(N-isopropylacrylamide-co-acrylic acid-co-initiator/Fe3+)] [P(NIPAAm-AA-iBr/Fe3+)]. The top soft hydrogel/brush composite layer provides aqueous lubrication, while the bottom thermoresponsive hydrogel layer exhibits adaptive load-bearing capacity that shows tunable stiff or modulus in response to the temperature above and below the lower critical solution temperature (LCST, 32.5 °C). An obvious friction-reduction feature is realized above the LCST, resulting from the dynamic increase of the bottom layer mechanical modulus. Furthermore, in situ lubrication-improvement behavior is achieved upon applying a near-infrared (NIR) laser onto the surface of Fe3O4 nanoparticle (NP)-integrated layered materials. Such a typical lubrication-regulated behavior can be attributed to the synergy effect of the improved load-bearing capacity of the bottom layer and the enhanced lubrication behavior of the top layer with an increase in the polyelectrolyte brush chain density, which is similar to the mechanically controlled adaptive lubrication mechanism of the natural cartilage layer. Current research results provide an inspiration for developing novel biomimetic lubrication materials with considerable load-bearing capacity and also propose a strategy for designing intelligent/stable friction-actuation devices.
Keywords: biomimetic layered material; friction control; hydrogels; polymer brush; thermoresponsive.