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Guest-host supramolecular assembly of injectable hydrogel fibers for cell encapsulation

Beverly Miller, Audrey Hansrisuk, Christopher B. Highley, View ORCID ProfileSteven R. Caliari
doi: https://doi.org/10.1101/2021.02.26.430926
Beverly Miller
1Department of Chemical Engineering, University of Virginia, Charlottesville, Virginia 22904
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Audrey Hansrisuk
2Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904
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Christopher B. Highley
1Department of Chemical Engineering, University of Virginia, Charlottesville, Virginia 22904
3Department of Biomedical Engineering, University of Virginia, Charlottesville, Virginia 22904
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Steven R. Caliari
1Department of Chemical Engineering, University of Virginia, Charlottesville, Virginia 22904
3Department of Biomedical Engineering, University of Virginia, Charlottesville, Virginia 22904
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  • ORCID record for Steven R. Caliari
  • For correspondence: caliari@virginia.edu
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Abstract

The fibrous architecture of the extracellular matrix (ECM) is recognized as an integral regulator of cell function. However, there is an unmet need to develop mechanically robust biomaterials mimicking nanofibrous tissue topography that are also injectable to enable minimally invasive delivery. In this study we have developed a fibrous hydrogel composed of supramolecularly-assembled hyaluronic acid (HA) nanofibers that exhibits mechanical integrity, shear-thinning, rapid self-healing, and cytocompatibility. HA was modified with methacrylates to permit fiber photocrosslinking following electrospinning and either ‘guest’ adamantane or ‘host’ β-cyclodextrin groups to guide supramolecular fibrous hydrogel assembly. Analysis of fibrous hydrogel rheological properties showed that the mixed guest-host fibrous hydrogel was more mechanically robust (6.6 ± 2.0 kPa, storage modulus (G′)) than unmixed guest hydrogel fibers (1.0 ± 0.1 kPa, G′) or host hydrogel fibers (1.1 ± 0.1 kPa, G′) separately. The reversible nature of the guest-host supramolecular interactions also allowed for shear-thinning and self-healing behavior as demonstrated by cyclic deformation testing. Human mesenchymal stromal cells (hMSCs) encapsulated in fibrous hydrogels demonstrated satisfactory viability following injection and after seven days of culture (> 85%). Encapsulated hMSCs were more spread and elongated when cultured in viscoelastic guest-host hydrogels compared to non-fibrous elastic controls, with hMSCs also showing significantly decreased circularity in fibrous guest-host hydrogels compared to non-fibrous guest-host hydrogels. Together, these data highlight the potential of this injectable fibrous hydrogel platform for cell and tissue engineering applications requiring minimally invasive delivery.

Competing Interest Statement

The authors have declared no competing interest.

Copyright 
The copyright holder for this preprint is the author/funder, who has granted bioRxiv a license to display the preprint in perpetuity. It is made available under a CC-BY 4.0 International license.
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Posted February 26, 2021.
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Guest-host supramolecular assembly of injectable hydrogel fibers for cell encapsulation
Beverly Miller, Audrey Hansrisuk, Christopher B. Highley, Steven R. Caliari
bioRxiv 2021.02.26.430926; doi: https://doi.org/10.1101/2021.02.26.430926
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Guest-host supramolecular assembly of injectable hydrogel fibers for cell encapsulation
Beverly Miller, Audrey Hansrisuk, Christopher B. Highley, Steven R. Caliari
bioRxiv 2021.02.26.430926; doi: https://doi.org/10.1101/2021.02.26.430926

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