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Abstract Recent investigations have pointed to physical entanglements that greatly outnumber chemical crosslinks as key sources of energy dissipation and low friction in hydrogel networks. Slide-ring gels are an emerging class of hydrogels described by their mobile crosslinks, which are formed by rings topologically constrained to slide along linear polymer chains within the network. These materials have enjoyed decades of study by polymer chemists but have been underexplored by the tribology community. In this work, we synthesized a pseudo-rotaxane crosslinker from poly(ethylene glycol) diacrylate (PEG-diacrylate) andα-cyclodextrin-acrylate followed by hydrogel networks by connecting the sliding crosslinks with polyacrylamide chains. The mechanical and tribological properties of slide-ring hydrogels were investigated using a custom-built microtribometer. Slide-ring hydrogels exhibit unique behavior compared to conventional covalently crosslinked polyacrylamide hydrogels and offer a vast design space for future investigations. Graphical Abstract
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Ballistic and Blast-Relevant, High-Rate Material Properties of Physically and Chemically Crosslinked Hydrogels
Abstract BackgroundHydrogels are one of the most ubiquitous polymeric materials. Among them gelatin, agarose and polyacrylamide-based formulations have been effectively utilized in a variety of biomedical and defense-related applications including ultrasound-based therapies and soft tissue injury investigations stemming from ballistic and blast exposures. Interestingly, while in most cases accurate prediction of the mechanical response of these surrogate gels requires knowledge of the underlying finite deformation, high-strain rate material properties, it is these properties that have remained scarce in the literature. ObjectiveBuilding on our prior works using Inertial Microcavitation Rheometry (IMR), here we present a comprehensive list of the high-strain rate (> 10$$^3$$ 1/s) mechanical properties of these three popular classes of hydrogel materials characterized via laser-based IMR, further showing that the choice in finite-deformation, rate-dependent constitutive model can be informed directly by the type of crosslinking mechanism and resultant network structure of the hydrogel, thus providing a chemophysical basis of the the choice of phenomenological constitutive model. MethodsWe analyze existing experimental gelatin IMR datasets and compare the results with prior data on polyacrylamide. ResultsWe show that a Neo-Hookean Kelvin-Voigt (NHKV) model can suitably simulate the high-rate material response of dynamic, physically crosslinked hydrogels like gelatin, while the introduction of a strain-stiffening parameter through the use of the quadratic Kelvin-Voigt (qKV) model was necessary to appropriately model chemically crosslinked hydrogels such as polyacrylamide due to the nature of the static,covalent bonds that comprise their structure. ConclusionsIn this brief we show that knowledge of the type of underlying polymer structure, including its bond mobility, can directly inform the appropriate finite deformation, time-dependent viscoelastic material model for commonly employed tissue surrogate hydrogels undergoing high strain rate loading within the ballistic and blast regimes.
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- Award ID(s):
- 2232428
- PAR ID:
- 10509374
- Publisher / Repository:
- Springer
- Date Published:
- Journal Name:
- Experimental Mechanics
- Volume:
- 64
- Issue:
- 4
- ISSN:
- 0014-4851
- Page Range / eLocation ID:
- 587 to 592
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1007/s11340-024-01043-3
