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), . https://doi.org/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: firstname.lastname@example.org 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: email@example.com 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: firstname.lastname@example.org 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: email@example.com 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: firstname.lastname@example.org 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: email@example.com –––––––––
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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.
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
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