One Step Creation of Multifunctional 3D Architectured Hydrogels Inducing Bone Regeneration

Neffe, Axel T.; Pierce, Benjamin F.; Tronci, Giuseppe; Ma, Nan; Pittermann, Erik; Gebauer, Tim; Frank, Oliver; Schossig, Michael; Xu, Xun; Willie, Bettina M.; Forner, Michèle; Ellinghaus, Agnes; Lienau, Jasmin; Duda, Georg N.; Lendlein, Andreas

doi:10.1002/adma.201404787

Cited by 101 publications

(80 citation statements)

References 40 publications

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“…37,38 Gelatin solutions exhibit a thermo-reversible Sol-Gel transition and form gels upon cooling below 30°C. The SolGel phase transition of gelatin solutions is attributed to the supramolecular assembly and disassembly of the tri-helix structure as a result of the formation and breakage of intermolecular hydrogen bonds at low and high temperatures, respectively.…”

Section: Resultsmentioning

confidence: 99%

One-pot solvent exchange preparation of non-swellable, thermoplastic, stretchable and adhesive supramolecular hydrogels based on dual synergistic physical crosslinking

et al. 2018

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With their unique properties of self-healing and viscoelasticity, physically crosslinked supramolecular hydrogels are promising materials for soft robotics, wearable electronics and biomedical applications. However, the weak mechanical properties of supramolecular hydrogels, especially those prepared with natural polymers, limit their wide-spread application, and swelling is one of the key factors that contributes to the weakening of hydrogels. Herein, we utilize a simple one-pot solvent exchange method to prepare non-swellable, thermoplastic and tough supramolecular gelatin hydrogels based on two synergistic physical crosslinkings, namely, the self-assembled tri-helix structure of gelatin and the hydrophobic aggregation of gelatin-grafted and free hydrophobic motifs. The obtained hydrogels possess a stable water content above 70% with extended incubation in water. These hydrogels are highly malleable upon heating but are extremely stretchable and tough after cooling to room temperature. Furthermore, the supramolecular gelatin hydrogels exhibit robust adhesion to various material surfaces and minimal cytotoxicity. NPG Asia Materials (2018) 10, e455; doi:10.1038/am.2017.208; published online 5 January 2018 INTRODUCTION Hydrogels, due to their high water content and tunable physical and biological properties, are extensively used in soft robotics, wearable electronics and biomedical applications. 1-6 Supramolecular hydrogels, which are solely stabilized by physical crosslinkings, such as host-guest interactions, electrostatic attraction and hydrophobic aggregation, have recently received increasing attention due to their unique properties, including self-healing, energy dissipation and viscoelasticity. 7-13 However, the poor mechanical performance of supramolecular hydrogels, especially hydrogels prepared with natural polymers, which possess superior biocompatibility and bioactivity, remain a major hurdle to the wide-spread application of these hydrogels. To improve the mechanical properties of chemically crosslinked hydrogels, researchers have developed ingenious strategies, including nanocomposite hydrogels, double-network hydrogels, hybrid crosslinking hydrogels and tetra-polyethylene glycol hydrogels. [14][15][16][17][18][19][20][21][22] Recently, increasing research attention has been dedicated to enhancing the mechanical performance of physically crosslinked supramolecular hydrogels. One recent study demonstrated very tough physical hydrogels composed of polyampholytes. 23 Another study showed that pre-assembled host

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Section: Resultsmentioning

confidence: 99%

One-pot solvent exchange preparation of non-swellable, thermoplastic, stretchable and adhesive supramolecular hydrogels based on dual synergistic physical crosslinking

et al. 2018

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“…In regeneration, human mesenchymal stem cells (hMSCs) from the bone marrow stroma are believed to play an important role due to their ability for self‐renewal and differentiation into different mature cells like osteoblasts, adipocytes and chondrocytes 5. Numerous studies have shown that the mechanical properties of the cell's microenvironment, such as the substrate stiffness, have a fundamental effect on hMSC cell fate and function and impact tissue regeneration 6, 7, 8, 9. Recently, evidence is rising that the geometrical properties of the cell's environment also play an important role as regulators of cell behavior 10, 11, 12, 13, 14, 15, 16, 17, 18, 19.…”

Section: Introductionmentioning

confidence: 99%

Surface Curvature Differentially Regulates Stem Cell Migration and Differentiation via Altered Attachment Morphology and Nuclear Deformation

et al. 2016

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Signals from the microenvironment around a cell are known to influence cell behavior. Material properties, such as biochemical composition and substrate stiffness, are today accepted as significant regulators of stem cell fate. The knowledge of how cell behavior is influenced by 3D geometric cues is, however, strongly limited despite its potential relevance for the understanding of tissue regenerative processes and the design of biomaterials. Here, the role of surface curvature on the migratory and differentiation behavior of human mesenchymal stem cells (hMSCs) has been investigated on 3D surfaces with well‐defined geometric features produced by stereolithography. Time lapse microscopy reveals a significant increase of cell migration speed on concave spherical compared to convex spherical structures and flat surfaces resulting from an upward‐lift of the cell body due to cytoskeletal forces. On convex surfaces, cytoskeletal forces lead to substantial nuclear deformation, increase lamin‐A levels and promote osteogenic differentiation. The findings of this study demonstrate a so far missing link between 3D surface curvature and hMSC behavior. This will not only help to better understand the role of extracellular matrix architecture in health and disease but also give new insights in how 3D geometries can be used as a cell‐instructive material parameter in the field of biomaterial‐guided tissue regeneration.

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“…53,54 We found that this material was able to accelerate bone healing and osseointegration. This type of biomaterial 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 (cell-and factor-free) is of great interest in bone regeneration because it allows more realistic translation to clinical application 31,55 Computerized micro-tomography (µ-CT) scans were performed on bone samples that were retrieved at different time points 3, 7 and 14 days after surgery for NMP treated and nontreated defects. At day 3, there was no visible difference on the µ-CT scans between the control and NMP group.…”

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confidence: 99%

Two-Dimensional Magnesium Phosphate Nanosheets Form Highly Thixotropic Gels That Up-Regulate Bone Formation

Laurenti¹,

Subaie

Abdallah³

et al. 2016

Nano Lett.

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Hydrogels composed of two-dimensional (2D) nanomaterials have become an important alternative to replace traditional inorganic scaffolds for tissue engineering. Here, we describe a novel nanocrystalline material with 2D morphology that was synthesized by tuning the crystallization of the sodium-magnesium-phosphate system. We discovered that the sodium ion can regulate the precipitation of magnesium phosphate by interacting with the crystal's surface causing a preferential crystal growth that results in 2D morphology. The 2D nanomaterial gave rise to a physical hydrogel that presented extreme thixotropy, injectability, biocompatibility, bioresorption, and long-term stability. The nanocrystalline material was characterized in vitro and in vivo and we discovered that it presented unique biological properties. Magnesium phosphate nanosheets accelerated bone healing and osseointegration by enhancing collagen formation, osteoblasts differentiation, and osteoclasts proliferation through up-regulation of COL1A1, RunX2, ALP, OCN, and OPN. In summary, the 2D magnesium phosphate nanosheets could bring a paradigm shift in the field of minimally invasive orthopedic and craniofacial interventions because it is the only material available that can be injected through high gauge needles into bone defects in order to accelerate bone healing and osseointegration.

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One Step Creation of Multifunctional 3D Architectured Hydrogels Inducing Bone Regeneration

Cited by 101 publications

References 40 publications

One-pot solvent exchange preparation of non-swellable, thermoplastic, stretchable and adhesive supramolecular hydrogels based on dual synergistic physical crosslinking

One-pot solvent exchange preparation of non-swellable, thermoplastic, stretchable and adhesive supramolecular hydrogels based on dual synergistic physical crosslinking

Surface Curvature Differentially Regulates Stem Cell Migration and Differentiation via Altered Attachment Morphology and Nuclear Deformation

Two-Dimensional Magnesium Phosphate Nanosheets Form Highly Thixotropic Gels That Up-Regulate Bone Formation

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