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Synergistic Microgel-Reinforced Hydrogels as High-Performance Lubricants.

ABSTRACT: 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 ?-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.

SUBMITTER: Hu J

PROVIDER: S-EPMC7745723 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Synergistic Microgel-Reinforced Hydrogels as High-Performance Lubricants.

Hu Jing J Andablo-Reyes Efren E Soltanahmadi Siavash S Sarkar Anwesha A

ACS macro letters 20201116 12

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 ...[more]

PMID: 33344040

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Project description:Starch-based emulsion microgel particles with different starch (15 and 20 wt %) and oil contents (0-15 wt %) were synthesized, and their lubrication performance under physiological conditions was investigated. Emulsion microgels were subjected to skin mimicking or oral cavity mimicking conditions, i.e., smooth hydrophobic polydimethylsiloxane ball-on-disc tribological tests, in the absence or presence of salivary enzyme (?-amylase). In the absence of enzyme, emulsion microgel particles (30-60 vol % particle content) conserved the lubricating properties of emulsion droplets, providing considerably lower friction coefficients (? ? 0.1) in the mixed lubrication regime compared to plain microgel particles (0 wt % oil). Upon addition of enzyme, the lubrication performance of emulsion microgel particles became strongly dependent on the particles' oil content. Microgel particles encapsulating 5-10 wt % oil showed a double plateau mixed lubrication regime having a lowest friction coefficient ? ? 0.03 and highest ? ? 0.1, the latter higher than with plain microgel particles. An oil content of 15 wt % was necessary for the microgel particles to lubricate similarly to the emulsion droplets, where both systems showed a normal mixed lubrication regime with ? ? 0.03. The observed trends in tribology, theoretical considerations, and the combined results of rheology, light scattering, and confocal fluorescence microscopy suggested that the mechanism behind the low friction coefficients was a synergistic enzyme- and shear-triggered release of the emulsion droplets, improving lubrication. The present work thus demonstrates experimentally and theoretically a novel biolubricant additive with stimuli-responsive properties capable of providing efficient boundary lubrication between soft polymeric surfaces. At the same time, the additive should provide an effective delivery vehicle for oil soluble ingredients in aqueous media. These findings demonstrate that emulsion microgel particles can be developed into multifunctional biolubricant additives for future use in numerous soft matter applications where both lubrication and controlled release of bioactives are essential.

Project description:Articular cartilage has limited capacity for regeneration and when damaged cannot be repaired with currently available metallic or synthetic implants. We aim to bioengineer a microfibre-reinforced hydrogel that can capture the zonal depth-dependent mechanical properties of native cartilage, and simultaneously support neo-cartilage formation. With this goal, a sophisticated bi-layered microfibre architecture, combining a densely distributed crossed fibre mat (superficial tangential zone, STZ) and a uniform box structure (middle and deep zone, MDZ), was successfully manufactured via melt electrospinning and combined with a gelatin-methacrylamide hydrogel. The inclusion of a thin STZ layer greatly increased the composite construct's peak modulus under both incongruent (3.2-fold) and congruent (2.1-fold) loading, as compared to hydrogels reinforced with only a uniform MDZ structure. Notably, the stress relaxation response of the bi-layered composite construct was comparable to the tested native cartilage tissue. Furthermore, similar production of sulphated glycosaminoglycans and collagen II was observed for the novel composite constructs cultured under mechanical conditioning w/o TGF-ß1 supplementation and in static conditions w/TGF-ß1 supplementation, which confirmed the capability of the novel composite construct to support neo-cartilage formation upon mechanical stimulation. To conclude, these results are an important step towards the design and manufacture of biomechanically competent implants for cartilage regeneration. STATEMENT OF SIGNIFICANCE: Damage to articular cartilage results in severe pain and joint disfunction that cannot be treated with currently available implants. This study presents a sophisticated bioengineered bi-layered fibre reinforced cell-laden hydrogel that can approximate the functional mechanical properties of native cartilage. For the first time, the importance of incorporating a viable superficial tangential zone (STZ) - like structure to improve the load-bearing properties of bioengineered constructs, particularly when in-congruent surfaces are compressed, is demonstrated. The present work also provides new insights for the development of implants that are able to promote and guide new cartilaginous tissue formation upon physiologically relevant mechanical stimulation.

Dataset Information

Synergistic Microgel-Reinforced Hydrogels as High-Performance Lubricants.

Publications

Synergistic Microgel-Reinforced Hydrogels as High-Performance Lubricants.

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