The influence of ions on the lubricative abilities of mucin and the role of sialic acids.

Mucus reduces friction between epithelial surfaces by providing lubrication in the boundary and mixed regime. Mucins, the main macromolecule, are heavily glycosylated proteins that polymerise and retain water molecules, resulting in a hydrated biogel. It is assumed that positively charged ions can influence mucin film structure by screening the electrostatic repulsions between the negatively charged glycans on mucin moieties and draw in water molecules via hydration shells. The ionic concentration can vary significantly in different mucus systems and here we show that increasing the ionic concentration in mucin films leads to an increase in lubrication between two polydimethylsiloxane surfaces at sliding contact in a compliant oral mimic. Mucins were found to bind sodium ions in a concentration-dependent manner and increased ionic concentration appears to cause mucin films to swell when assessed by Quartz Crystal hiMicrobalance with Dissipation (QCM-D) analysis. Furthermore, we determined that the removal of negatively charged sialic acid moieties by sialidase digestion resulted in reduced adsorption to hydrophilic surfaces but did not affect the swelling of mucin films with increasing ionic concentrations. Moreover, the coefficient of friction was increased with sialic acid removal, but lubrication was still increased with increasing ionic concentrations. Taken together this suggests that sialic acids are important for lubrication and may exert this through the sacrificial layer mechanism. Ionic concentration appears to influence mucin films and their lubrication, and sialic acids, at least partly, may be important for ion binding.

Exploiting the Synergy between Concentrated Polymer Brushes and Laser Surface Texturing to Achieve Durable Superlubricity.

Friction continues to account for the bulk of energy losses in mechanical systems, with an estimated 23% of the world's total energy consumption used to overcome friction. Concentrated polymer brushes (CPBs) have recently attracted significant scientific and industrial attention, given their ability to achieve superlubricity (i.e., coefficients of friction below 0.01); however, understanding the mechanistic interactions underlying their wear performance has been largely overlooked. Herein, we employ a custom-built optical test apparatus to investigate the inter-dependencies between CPBs and laser-produced surface texture (LST), assessing for the first time the friction, film thickness, and wear behavior in situ and simultaneously. Recent developments in picosecond laser etching allowed us to graft CPBs atop the finest laser-etched matrix of micron-sized dimples reported in literature to date. At low sliding speeds, combined CPB-LST reduces the coefficient of friction to 0.0006, while increasing the CPB durability by up to 34% through a lateral support mechanism offered by the textured micro-features. Furthermore, the imaging results shed light on CPB failure mechanisms. Both these mechanisms of lateral support and failure propagation impact the wear resistance of CPBs and are important in the development of CPBs for future applications (e.g., in low-speed bearings functioning under controlled abrasive wear conditions).

Theoretical demonstration of a capacitive rotor for generation of alternating current from mechanical motion.

Innovative concepts and materials are enabling energy harvesters for slower motion, particularly for personal wearables or portable small-scale applications, hence contributing to a future sustainable economy. Here we propose a principle for a capacitive rotor device and analyze its operation. This device is based on a rotor containing many capacitors in parallel. The rotation of the rotor causes periodic capacitance changes and, when connected to a reservoir-of-charge capacitor, induces alternating current. The properties of this device depend on the lubricating liquid situated between the capacitor's electrodes, be it a highly polar liquid, organic electrolyte, or ionic liquid - we consider all these scenarios. An advantage of the capacitive rotor is its scalability. Such a lightweight device, weighing tens of grams, can be implemented in a shoe sole, generating a significant power output of the order of Watts. Scaled up, such systems can be used in portable wind or water turbines.

Biomimetic Water-Repelling Surfaces with Robustly Flexible Structures.

Biomimetic liquid-repelling surfaces have been the subject of considerable scientific research and technological application. To design such surfaces, a flexibility-based oscillation strategy has been shown to resolve the problem of liquid-surface positioning encountered by the previous, rigidity-based asymmetry strategy; however, its usage is limited by weak mechanical robustness and confined repellency enhancement. Here, we design a flexible surface comprising mesoscale heads and microscale spring sets, in analogy to the mushroomlike geometry discovered on springtail cuticles, and then realize this through three-dimensional projection microstereolithography. Such a surface exhibits strong mechanical robustness against ubiquitous normal and shear compression and even endures tribological friction. Simultaneously, the surface elevates water repellency for impacting droplets by enhancing impalement resistance and reducing contact time, partially reaching an improvement of ∼80% via structural tilting movements. This is the first demonstration of flexible interfacial structures to robustly endure tribological friction as well as to promote water repellency, approaching real-world applications of water repelling. Also, a flexibility gradient is created on the surface to directionally manipulate droplets, paving the way for droplet transport.

Flexibility-Patterned Liquid-Repelling Surfaces.

Droplets impacting solid surfaces is ubiquitous in nature and of practical importance in numerous industrial applications. For liquid-repelling applications, rigidity-based asymmetric redistribution and flexibility-based structural oscillation strategies have been proven on artificial surfaces; however, these are limited by strict impacting positioning. Here, we show that the gap between these two strategies can be bridged by a flexibility-patterned design similar to a trampoline park. Such a flexibility-patterned design is realized by three-dimensional projection micro-stereolithography and is shown to enhance liquid repellency in terms of droplet impalement resistance and contact time reduction. This is the first demonstration of the synergistic effect obtained by a hybrid solution that exploits asymmetric redistribution and structural oscillation in liquid-repelling applications, paving the rigidity-flexibility cooperative way of wettability tuning. Also, the flexibility-patterned surface is applied to accelerate liquid evaporation.

Macroscale Superlubricity and Polymorphism of Long-Chain n-Alcohols.

Simple n-alcohols, such as 1-dodecanol, show anomalous film-forming and friction behaviors under elastohydrodynamic lubrication (EHL) conditions, as found inside bearings and gears. Using tribometer, diamond anvil cell (DAC), and differential scanning calorimetry (DSC) experiments, we show that liquid 1-dodecanol undergoes a pressure-induced solidification when entrained into EHL contacts. Different solid polymorphs are formed inside the contact depending on the temperature and pressure conditions. Surprisingly, at a moderate temperature and pressure, 1-dodecanol forms a polymorph that exhibits robust macroscale superlubricity. The DAC and DSC experiments show that superlubricity is facilitated by the formation of lamellar, hydrogen-bonded structures of hexagonally close-packed molecules, which promote interlayer sliding. This novel superlubricity mechanism is similar to that proposed for the two-dimensional materials commonly employed as solid lubricants, but it also enables the practical advantages of liquid lubricants to be maintained. When the pressure is increased, 1-dodecanol undergoes a polymorphic transformation into a phase that gives a higher friction. The DAC and DSC experiments indicate that the high-friction polymorph is an orthorhombic crystal. The polymorphic transformation pressure coincides with the onset of a dimple formation in the EHL films, revealing that the anomalous film shapes are caused by the formation of rigid orthorhombic crystals inside the contact. This is the first demonstration of a macroscale superlubricity in an EHL contact lubricated by a nonaqueous liquid that arises from bulk effects rather than tribochemical transformations at the surfaces. Since the superlubricity observed here results from phase transformations, it is continuously self-replenishing and is insensitive to surface chemistry and topology. This discovery creates the possibility of implementing superlubricity in a wide range of machine components, which would result in enormous improvements in efficiency and durability.

Effects of beverage carbonation on lubrication mechanisms and mouthfeel.

The perception of carbonation is an important factor in beverage consumption which must be understood in order to develop healthier products. Herein, we study the effects of carbonated water on oral lubrication mechanisms involved in beverage mouthfeel and hence taste perception. Friction was measured in a compliant PDMS-glass contact simulating the tongue-palate interface (under representative speeds and loads), while fluorescence microscopy was used to visualise both the flow of liquid and oral mucosal pellicle coverage. When carbonated water is entrained into the contact, CO2 cavities form at the inlet, which limit flow and thus reduce the hydrodynamic pressure. Under mixed lubrication conditions, when the fluid film thickness is comparable to the surface roughness, this pressure reduction results in significant increases in friction (>300% greater than under non-carbonated water conditions). Carbonated water is also shown to be more effective than non-carbonated water at debonding the highly lubricious, oral mucosal pellicle, which again results in a significant increase in friction. Both these transient mechanisms of starvation and salivary pellicle removal will modulate the flow of tastants to taste buds and are suggested to be important in the experience of taste and refreshment. For example this may be one reason why flat colas taste sweeter.

Liquid repellency enhancement through flexible microstructures.

Artificial liquid-repellent surfaces have attracted substantial scientific and industrial attention with a focus on creating functional topological features; however, the role of the underlying structures has been overlooked. Recent developments in micro-nanofabrication allow us now to construct a skin-muscle type system combining interfacial liquid repellence atop a mechanically functional structure. Specifically, we design surfaces comprising bioinspired, mushroom-like repelling heads and spring-like flexible supports, which are realized by three-dimensional direct laser lithography. The flexible supports elevate liquid repellency by resisting droplet impalement and reducing contact time. This, previously unknown, use of spring-like flexible supports to enhance liquid repellency provides an excellent level of control over droplet manipulation. Moreover, this extends repellent microstructure research from statics to dynamics and is envisioned to yield functionalities and possibilities by linking functional surfaces and mechanical metamaterials.

Self-Compensating Liquid-Repellent Surfaces with Stratified Morphology.

Artificial liquid-repellent surfaces have recently attracted vast scientific attention; however, achieving mechanical robustness remains a formidable challenge before industrialization can be realized. To this end, inspired by plateaus in geological landscapes, a self-compensating strategy is developed to pave the way for the synthesis of durable repellent surfaces. This self-compensating surface comprises tall hydrophobic structural elements, which can repel liquid droplets. When these elements are damaged, they expose shorter structural elements that also suspend the droplets and thus preserve interfacial repellency. An example of this plateau-inspired stratified surface was created by three-dimensional (3D) direct laser lithography micro-nano fabrication. Even after being subjected to serious frictional damage, it maintained static repellency to water with a contact angle above 147° and was simultaneously able to endure high pressures arising from droplet impacts. Extending the scope of nature-inspired functional surfaces from conventional biomimetics to geological landscapes, this work demonstrates that the plateau-inspired self-compensating strategy can provide an unprecedented level of robustness in terms of sustained liquid repellency.

Three-Dimensional Printed Surfaces Inspired by Bi-Gaussian Stratified Plateaus.

Wettability of artificial surfaces is attracting increasing attention for its relevant technological applications. Functional performance is often achieved by mimicking the topographical structures found in natural flora and fauna; however, surface attributes inspired by geological landscapes have so far escaped attention. We reproduced a stratified morphology of plateaus with a bi-Gaussian height distribution using a three-dimensional direct laser lithography. The plateau-inspired artificial surface exhibits a hydrophobic behavior even if fabricated from a hydrophilic material, giving rise to a new wetting mechanism that divides the well-known macroscopic Wenzel and Cassie states into four substates. We have also successfully applied the plateau-inspired structure to droplet manipulation.

Bi-Gaussian Stratified Wetting Model on Rough Surfaces.

Wetting mechanisms on rough surfaces were understood from either a monolayer or a multiscale perspective. However, it has recently been shown that the bi-Gaussian stratified nature of real surfaces should be accounted for when modeling mechanisms of lubrication, sealing, contact, friction, acoustic emission, and manufacture. In this work, a model combining Wenzel and Cassie theories was put forward to predict the static contact angle of a droplet on a bi-Gaussian stratified surface. The model was initially applied to numerically simulated surfaces and subsequently demonstrated on hydrophilic steel and hydrophobic self-assembled monolayer specimens with preset bi-Gaussian stratified topographies. In the Wenzel state, both the upper and the lower surface components are fully wetted. In the Cassie state, the upper component is still completely wetted, while the lower component serves as gas traps and reservoirs. By this model, wetting evolution was assessed, and the existence of different wetting states and potential state transitions was predicted.

3D Measurements of Lubricant and Surface Temperatures Within an Elastohydrodynamic Contact.

We present an infrared microscopy technique, capable of measuring the temperature of both the bounding surfaces and the oil film in an elastohydrodynamic contact. This technique can, for the first time, spatially resolve the oil film temperature in three dimensions. The contact is produced by loading a steel ball against a sapphire disc, and the film is viewed using an infrared microscope focussing through the disc. Two band pass filters are used to isolate the radiation from the oil film, and Planck's law is applied to data obtained at a known temperature as part of the calibration procedure. The proposed technique requires the emissivity of the oil film to be measured, which is acquired in situ and is shown to vary strongly as a function of thickness and temperature. The technique is validated under pure rolling conditions, when the temperature of the oil film is equal to the controlled lubricant reservoir temperature, and also compared to an equation commonly used to predict average film temperatures, confirming the value of the unknown constant. The technique is then used to gain insights into the thermal/rheological behaviour within a contact. This is important since the temperature of elastohydrodynamic contacts is critical in determining friction and hence the efficiency of machine components and this technique enables much needed validation and provides input data for CFD and numerical simulations.