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Compositional Tuning Reveals a Pathway to Achieve a Strong and Lubricious Double Network in Agarose-Polyacrylamide Hydrogels

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Abstract

Hydrogels, bearing microstructural semblance to biological tissues, are prime candidates for translation replacement materials. Among them, double network (DN) hydrogels are at the forefront with their superior mechanical properties compared to conventional single network hydrogels. However, the functional design of the microstructure to control mechanical and tribological performance still poses a challenge. Here, hydrogels composed of physically crosslinked agarose and chemically crosslinked poly(acrylamide) were studied by spectroscopy, dynamic light scattering, atomic force microscopy and rheology. A viable hydrogel formed with the lowest acrylamide concentration, but the loose PAAm network did not reinforce the agarose network. Increasing the monomer and crosslinker concentration led to fast gelation of the second network, yielding poorly interconnected acrylamide-rich domains within the agarose network, and a weak and heterogenous hydrogel. Reducing the crosslinking degree to the half slowed down gelation, which favored the formation of an interpenetrating PAAm network, affording a two-fold increase in strength. While the adhesion of the investigated hydrogels is remarkably dictated and reduced by agarose, their frictional characteristics are highly sensitive to the composition. Importantly, friction can be modulated by varying the imbibed fluid.

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Acknowledgements

We acknowledge the Materials Research Laboratory (MRL) at UIUC for providing the DLS facility.

Funding

This material is based upon work supported by the National Science Foundation under Grant No. CMMI-1761696.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, IL, 61801, USA

    Tooba Shoaib, Paige Prendergast & Rosa M. Espinosa-Marzal

  2. Department of Civil and Environmental Engineering, University of Illinois at Urbana Champaign, Urbana, IL, 61801, USA

    Rosa M. Espinosa-Marzal

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  1. Tooba Shoaib
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  2. Paige Prendergast
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All authors contributed to the study conception and design. Material preparation and data collection were performed by Tooba Shoaib and Paige Prendergast, and analysis was carried out by all authors. The first draft of the manuscript was written by Tooba Shoaib and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to Rosa M. Espinosa-Marzal.

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Shoaib, T., Prendergast, P. & Espinosa-Marzal, R.M. Compositional Tuning Reveals a Pathway to Achieve a Strong and Lubricious Double Network in Agarose-Polyacrylamide Hydrogels. Tribol Lett 70, 71 (2022). https://doi.org/10.1007/s11249-022-01604-4

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