Addressing astringency of grape seed extract by covalent conjugation with lupin protein.

Astringency of phenolic-rich foods is a key tactile perception responsible for acceptability/rejection of plant extracts as ingredients in formulations. Covalent conjugation of phenolic extracts with plant proteins might be a promising strategy to control astringency, but suffers from a lack of mechanistic understanding from the lubrication point of view. To shed light on this, this ex vivo study evaluated the effect of conjugation of a phenolic grape seed extract (GSE) with legume protein (lupin, LP) on tribological and surface adsorption performance of GSE in the absence and presence of human saliva (ex vivo). Tribological results confirmed GSE had an inferior lubrication capacity as compared to LP. The lubrication performance of LP-GSE dispersions was comparable to their corresponding LP dispersion (p > 0.05) when covalently conjugated with LP (LP-GSE) with increasing LP:GSE ratio up to 1:0.04 w/w and at a specific degree of conjugation (DC: 2%). Tribological and surface adsorption measurements confirmed the tendency of GSE to interact with human saliva (ex vivo, n = 17 subjects), impairing the lubricity of salivary films. The covalent bonding of LP to GSE hindered GSE's interaction with human saliva, implying the potential influence of covalent conjugation on attenuating astringency. LP appeared to compete with human saliva for surface adsorption and governed the lubrication behaviour in LP-GSE dispersions. Findings from this study provide valuable knowledge to guide the rational design of sustainable, functional foods using conjugation of phenolics with plant proteins to incorporate larger proportions of health-promoting phenolics while controlling astringency, which needs validation by sensory trials.

Insights into the Multiscale Lubrication Mechanism of Edible Phase Change Materials.

Investigation of a lubrication behavior of phase change materials (PCM) can be challenging in applications involving relative motion, e.g., sport (ice skating), food (chocolates), energy (thermal storage), apparel (textiles with PCM), etc. In oral tribology, a phase change often occurs in a sequence of dynamic interactions between the ingested PCM and oral surfaces from a licking stage to a saliva-mixed stage at contact scales spanning micro- (cellular), meso- (papillae), and macroscales. Often the lubrication performance and correlations across length scales and different stages remain poorly understood due to the lack of testing setups mimicking real human tissues. Herein, we bring new insights into lubrication mechanisms of PCM using dark chocolate as an exemplar at a single-papilla (meso)-scale and a full-tongue (macro) scale covering the solid, molten, and saliva-mixed states, uniting highly sophisticated biomimetic oral surfaces with in situ tribomicroscopy for the first time. Unprecedented results from this study supported by transcending lubrication theories reveal how the tribological mechanism in licking shifted from solid fat-dominated lubrication (saliva-poor regime) to aqueous lubrication (saliva-dominant regime), the latter resulted in increasing the coefficient of friction by at least threefold. At the mesoscale, the governing mechanisms were bridging of cocoa butter in between confined cocoa particles and fat coalescence of emulsion droplets for the molten and saliva-mixed states, respectively. At the macroscale, a distinctive hydrodynamic viscous film formed at the interface governing the speed-dependent lubrication behavior indicates the striking importance of multiscale analyses. New tribological insights across different stages and scales of phase transition from this study will inspire rational design of the next generation of PCM and solid particle-containing materials.

Synergistic Microgel-Reinforced Hydrogels as High-Performance Lubricants.

The ability to create a superlubricious aqueous lubricant is important for various biological and technological applications. Here, a nonlipid biolubricant with strikingly low friction coefficients is fabricated (patented) by reinforcing a fluid-like hydrogel composed of biopolymeric nanofibrils with proteinaceous microgels, which synergistically provide superlubricity on elastomeric surfaces in comparison to any of the sole components. This two-component lubricant composed of positively charged lactoferrin microgels and negatively charged κ-carrageenan hydrogels is capable of exceeding the high lubricating performance of real human saliva in tribo tests using both smooth and textured surfaces, latter mimicking the human tongue's wettability, topography, and compliance. The favorable electrostatic attraction between mutually oppositely charged microgels and the hydrogel reinforces the mechanical properties of the hydrogel, allowing friction reduction by combining the benefits of both viscous and hydration lubrication. The superlubricity of these microgel-reinforced hydrogels offers a unique prospect for the fabrication of biocompatible aqueous lubricants for dry-mouth therapy and/or designing of nonobesogenic nutritional technologies.

Surface Fatigue Behavior of a WC/aC:H Thin-Film and the Tribochemical Impact of Zinc Dialkyldithiophosphate.

In wind turbine gearboxes, (near-)surface initiated fatigue is attributed to be the primary failure mechanism. In this work, the surface fatigue of a hydrogenated tungsten carbide/amorphous carbon (WC/aC:H) thin-film was tested under severe cyclic tribo-contact using polyalphaolefin (PAO) and PAO + zinc dialkyldithiophosphate (ZDDP) lubricants. The film was characterized in terms of its structure and chemistry using X-ray diffraction, analytical transmission electron microscopy, including electron energy loss spectroscopy (EELS), as well as X-ray photoelectron spectroscopy (XPS). The multilayer carbon thin-film exhibited promising surface fatigue performance showing a slight change in the hybridization state of the aC:H matrix. Dehydrogenation of the thin-film and subsequent transformation of cleaved C-H bonds to nonplanar sp2 carbon rings were inferred from EELS and XPS results. While tribo-induced changes to the aC:H matrix were not influenced by a nanometer-thick ZDDP reaction-film, the rate of oxidation of WC and its oxidation state were affected. While accelerating surface fatigue on a steel surface, the ZDDP-tribofilm protected the WC/aC:H film from surface fatigue. In contrast to the formation of polyphosphates from ZDDP molecules on steel surfaces, it appeared that on the WC/aC:H thin film surface, ZDDP molecules decompose to ZnO, suppressing the oxidative degradation of WC.