The lubrication behavior of the hydrated biopolymers that constitute tissues in organisms differs from that outlined by the classical Stribeck curve, and studying hydrogel lubrication is a key pathway to understand the complexity of biolubrication. Here, we have investigated the frictional characteristics of polyacrylamide (PAAm) hydrogels with various acrylamide concentrations, exhibiting Young's moduli (E) that range from 1 to 40 kPa, as a function of applied normal load and sliding velocities by colloid probe lateral force microscopy. The speed-dependence of the friction force shows an initial decrease in friction with increasing velocity, while, above a transition velocity V*, friction increases with speed. This study reveals two different boundary lubrication mechanisms characterized by distinct scaling laws. An unprecedented and comprehensive study of the lateral force loops reveals intermittent friction or stick-slip above and below V*, with characteristics that depend on the hydrogel network, applied load, and sliding velocity. Our work thus provides insight into the closely tied parameters governing hydrogel lubrication mechanisms, and stick-slip friction.

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Since their inception, hydrogels have gained popularity among multiple fields, most significantly in biomedical research and industry. Due to their resemblance to biological tribosystems, a significant amount of research has been conducted on hydrogels to elucidate biolubrication mechanisms and their possible applications as replacement materials. This review is focused on lubrication mechanisms and covers friction models that have attempted to quantify the complex frictional characteristics of hydrogels. From models developed on the basis of polymer physics to the concept of hydration lubrication, assumptions and conditions for their applicability are discussed. Based on previous models and our own experimental findings, we propose the viscous-adhesive model for hydrogel friction. This model accounts for the effects of confinement of the polymer network provided by a solid surface and poroelastic relaxation as well as the (non) Newtonian shear of a complex fluid on the frictional force and quantifies the frictional response of hydrogels-solid interfaces. Finally, the review delineates potential areas of future research based on the current knowledge.

Recognizing the limitations of solid-supported lipid bilayers to reproduce the behavior of cell membranes, including bendability, transmembrane protein inclusion, and virus entry, this study describes a novel biomimetic system for cell membranes with the potential to overcome these and other limitations. The developed strategy utilizes a hydrogel with tunable mechanical behavior that resembles those of living cells as the soft support for the phospholipid bilayer, while a polyelectrolyte multilayer film serves as an intermediate layer to facilitate the self-assembly of the lipid bilayer on the soft cushion. Quartz crystal microbalance studies show that, upon coming into contact with the polyelectrolyte film, vesicles fuse and rupture to yield a robust lipid bilayer. Fluorescence recovery after photobleaching confirms the formation of a membrane, while atomic force microscopy shows a low adhesion between the indenting probe and the bilayer. More importantly, in comparison to the solid-supported lipid bilayer, the response of this biomimetic system to nanoindentation demonstrates its increased mechanical stability and bendability when assembled on a soft cushion. Hence, the developed hydrogel-supported lipid bilayers can mimic biomechanical properties of cell membranes, which will enable scientists to study and to understand biophysicochemical interactions between cell membranes and extracellular entities.

Biological tribosystems enable diverse functions of the human body by maintaining extremely low coefficients of friction via hydrogel-like surface layers and a water-based lubricant. Although stiction has been proposed as a precursor to damage, there is still a lack of knowledge about its origin and its relation to the hydrogel’s microstructure, which impairs the design of soft matter as replacement biomaterials. In this work, the static friction of poly­(acrylamide) hydrogels with modulated composition was investigated by colloidal probe lateral force microscopy as a function of load, temperature, and loading time. Temperature-dependent studies enable to build a phase diagram for hydrogel’s static friction, which explains stiction via (polymer) viscoelastic and poroelastic relaxation, and a subtle transition from solid- to liquid-like interfacial behavior. At room temperature, the static friction increases with loading time, a phenomenon called contact aging, which stems from the adhesion of the polymer to the colloid and from the drainage-induced increase in contact area. Contact aging is shown to gradually vanish with increase in temperature, but this behavior strongly depends on the hydrogel’s composition. This work scrutinizes the relation between the microstructure of hydrogel-like soft matter and interfacial behavior, with implications for diverse areas of inquiry, not only in biolubrication and biomedical applications but also in soft robotics and microelectromechanical devices, where the processes occurring at the migrating hydrogel interface are of relevance. The results support that modulating both the hydrogel’s mesh size and the structure of the near-surface region is a means to control static friction and adhesion. This conceptual framework for static friction will foster further understanding of the wear of hydrogel-like materials.