Mechanically robust electrospun hydrogel scaffolds crosslinked Mechanically robust electrospun...

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  • Mechanically robust electrospun hydrogel scaffolds crosslinked via supramolecular interactions Citation for published version (APA): Mollet, B. B., Spaans, S., Goodarzy Fard, P., Bax, N. A. M., Bouten, C. V. C., & Dankers, P. Y. W. (2017). Mechanically robust electrospun hydrogel scaffolds crosslinked via supramolecular interactions. Macromolecular Bioscience, 17(9), [1700053]. https://doi.org/10.1002/mabi.201700053

    DOI: 10.1002/mabi.201700053

    Document status and date: Published: 01/09/2017

    Document Version: Accepted manuscript including changes made at the peer-review stage

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    Download date: 08. Feb. 2021

    https://doi.org/10.1002/mabi.201700053 https://doi.org/10.1002/mabi.201700053 https://research.tue.nl/en/publications/mechanically-robust-electrospun-hydrogel-scaffolds-crosslinked-via-supramolecular-interactions(15b1e662-de90-4dcf-8df3-14f90fd70bd5).html

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    DOI: 10.1002/marc.((insert number)) ((or ppap., mabi., macp., mame., mren., mats.)) Full Paper Mechanically robust electrospun hydrogel scaffolds crosslinked via supramolecular interactions Björne B. Mollet, Sergio Spaans, Parinaz Goodarzy Fard, Noortje A.M. Bax, Carlijn V.C. Bouten, Patricia Y.W. Dankers* ––––––––– Dr. B.B. Mollet Institute for Complex Molecular Systems and Laboratory of Chemical Biology Department of Biomedical Engineering Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, Netherlands E-mail: b.b.mollet@tue.nl MSc S. Spaans Institute for Complex Molecular Systems and Laboratory for Cell and Tissue Engineering, Department of Biomedical Engineering Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, Netherlands E-mail: s.spaans@tue.nl BSc P. Goodarzy Fard Institute for Complex Molecular Systems and Laboratory of Chemical Biology Department of Biomedical Engineering Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, Netherlands E-mail: parinazgofa@yahoo.com Dr. N.A.M. Bax Institute for Complex Molecular Systems and Laboratory for Cell and Tissue Engineering, Department of Biomedical Engineering Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, Netherlands E-mail: n.a.m.bax@tue.nl Prof. Dr. C.V.C. Bouten Institute for Complex Molecular Systems and Laboratory for Cell and Tissue Engineering, Department of Biomedical Engineering Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, Netherlands E-mail: c.v.c.bouten@tue.nl Dr. Dr. P.Y.W. Dankers Institute for Complex Molecular Systems, Laboratory of Chemical Biology and Laboratory for Cell and Tissue Engineering Department of Biomedical Engineering Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, Netherlands E-mail: p.y.w.dankers@tue.nl –––––––––

    mailto:b.b.mollet@tue.nl mailto:s.spaans@tue.nl mailto:parinazgofa@yahoo.com javascript:linkTo_UnCryptMailto('pdlowr-q1d1p1edaCwxh1qo'); mailto:c.v.c.bouten@tue.nl mailto:p.y.w.dankers@tue.nl

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    One of the major challenges in the processing of hydrogels based on poly(ethylene glycol)

    (PEG) is to create mechanically robust electrospun hydrogel scaffolds without chemical cross-

    linking post-processing. In this study, this was achieved by the introduction of physical

    crosslinks in the form of supramolecular hydrogen bonding ureido-pyrimidinone (UPy)

    moieties, resulting in chain-extended UPy-PEG polymers (CE-UPy-PEG) that could be

    electrospun from organic solvent. The resultant fibrous meshes were swollen in contact with

    water and formed mechanically stable, elastic hydrogels, while the fibrous morphology

    remained intact. Mixing up to 30 wt% gelatin with these CE-UPy-PEG polymers introduced

    bioactivity into these scaffolds, without affecting the mechanical properties. Manipulating the

    electrospinning parameters resulted in meshes with either small or large fiber diameters, i.e.

    0.63±0.36 µm and 2.14±0.63 µm, respectively. In that order, these meshes provided support

    for renal epithelial monolayer formation or a niche for the culture of cardiac progenitor cells.

    1. Introduction

    For regenerative medicine and tissue engineering purposes a diversity of biomaterial

    hydrogels, ranging from natural to synthetic, have been described and studied,1–6 each with

    their specific advantages and limitations. Hydrogels of natural origin, such as collagen or its

    denatured form gelatin, hyaluronic acid, and matrigel, a widely applied commercial

    extracellular matrix (ECM) mimic, all provide biological environments that promote cellular

    survival and interaction with cells.7 However, the variable composition of these materials, and

    their complex and not-well understood interactions with cells, challenge controlled

    application. In addition, origin-related safety concerns put constraints on their use in the

    medical field.8 On top of that, the possibility to tune the mechanical or topological properties

    of these molecularly pre-defined hydrogels is limited. Inert synthetic hydrogels, on the other

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    hand, allow adjustable composition and hence predictable and tunable properties. However,

    synthetic materials lack bioactive cues for engagement of specific interaction with cells. To

    bridge the gap between natural and synthetic hydrogels, researchers have simply mixed

    hydrogel components of natural and synthetic origin to achieve hybrid hydrogels with

    synergistic effects.9–11

    To enable the formation of structurally defined, freestanding meshes, the hydrogel system

    must allow processing and acquire mechanically robust properties. Electrospinning is an

    attractive processing technique for the formation of fibrous meshes. By controlling fiber

    diameter, the pore size can be tuned. This allows the formation of scaffolds either distinctly

    suitable to function as 2D support, or 3D scaffolds that allow cell infiltration. Electrospinning

    of natural,12,13 synthetic14–17 and hybrid18 hydrogelators has been performed extensively.

    However, all these biomaterials require chemical cross-linking post-electrospinning to prevent

    complete dissolution or fast degradation of the nano-to-micro fibrous structures in aqueous

    environments and/or to improve poor mechanical properties. A hydrogel material that forms

    strong physical cross-links could circumvent the need of chemical cross-linking, while

    retaining the opportunity for processing.

    Here we demonstrate the use of a supramolecular hydrogelator based on poly(ethylene glycol)

    (PEG) with multiple ureido-pyrimidinone (UPy)-moieties in the backbone,19 electrospun into

    mechanically strong, microfibrous meshes (Figure 1A). While this chain-extended UPy-PEG

    (CE-UPy-PEG) has a nearly identical chemical composition compared to its telechelic

    analogues, it exhibits completely different, exceptional mechanical properties.20–23 In the dry

    state, this supramolecular polymer forms a tough material with shape memory properties,

    whereas in the hydrated state a strong and highly elastic hydrogel is formed.19 In the

    equilibrium hydrated state, the bulk hydrogel (with 10 kg · mol-1 PEG-block) contains ~85

    wt% water. This hydrogel material showed nearly perfect strength recovery even at large

    deformation (> 300%).19 Hence, the increased chain length, realized through chain-extension,

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    and the ability to form physical cross-links substantially enhanced the strength, ductility, and

    stability of this material in water. Importantly, no chemical cross-linking is needed to achieve

    these remarkable material properties while at the same time the physical cross-links, formed

    by hydrogen-bo