Injectable poly(oligoethylene glycol methacrylate)-based hydrogels with tunable phase transition behaviours: Physicochemical and biological responses

Smeets, Niels M. B.; Bakaic, Emilia; Patenaude, Mathew; Hoare, Todd

doi:10.1016/j.actbio.2014.05.035

Cited by 67 publications

(161 citation statements)

References 66 publications

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“…The swelling rate constant k also generally increases with increasing CNC loading except at extremely high CNC contents (Table 2), again suggesting that faster swelling kinetics are generally achieved in the presence of CNCs. In contrast, PO 10 -based hydrogels which exhibit volume phase transition temperatures of ~ 33 °C) 24 gradually de-swell to reach an equilibrium swelling value lower than the initial normalized hydrogel weight, consistent with a thermoresponsive hydrogel ( Figure 3B). …”

Section: Hydrogel Swelling and Degradationmentioning

confidence: 95%

“…For PO 100 -0 gels, complete network degradation was achieved after only 50 minutes; in contrast, 300 minutes is required for full dissolution of the PO 100 -4.95 gels. PO 10 series hydrogels degrade much slower than their PO 100 series counterparts, attributable to both the higher crosslink density (due to shorter ethylene oxide side chains which impart less steric hindrance to cross-linking 24 ) and lower water content of these gels. Still, PO 10 -1.65 gels resist dissolution longer than PO 10 -0 gels, again suggesting that CNCs play a role in enhancing the network structure.…”

Section: Hydrogel Swelling and Degradationmentioning

confidence: 99%

“…Previously, both CNCs 32,35 and POEGMA hydrogels 8,24 have been shown in various studies to be non-cytotoxic. Here, we show that POEGMA-CNC nanocomposite hydrogels are also non-cytotoxic, with CNC loading having no significant impact on cell viability.…”

Section: Cell Interactions With Hydrogelsmentioning

confidence: 99%

“…We have previously reported extensively on modular POEGMA hydrogels cross-linked via hydrazone bonds, formed by reactive extrusion of aldehyde and hydrazide-functionalized precursor polymers. 8,[22][23][24][25][26] Hydrogel properties including the lower critical solution temperature (LCST), cross-link density, swelling ratio, and cell adhesion can be modified by varying the ethylene oxide side chain length, 24 combining multiple precursor polymers, 22 or introducing hydrophobic domains into the precursor polymers. 26 However, the mechanical strength of these materials remains limited; more specifically, in the context of the highly protein and cell-repellent POEGMA hydrogels based on long oligo(ethylene glycol) side chains, even highly functionalized precursor polymers (30 mol % hydrazide or aldehyde-bearing repeat units) lead to hydrogels with only moderate mechanical strength (~1 kPa shear storage modulus).…”

Section: Introductionmentioning

confidence: 99%

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Enhanced Mechanical Properties in Cellulose Nanocrystal–Poly(oligoethylene glycol methacrylate) Injectable Nanocomposite Hydrogels through Control of Physical and Chemical Cross-Linking

2016

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While injectable hydrogels have several advantages in the context of biomedical use, their generally weak mechanical properties often limit their applications. Herein we describe in situgelling nanocomposite hydrogels based on poly(oligoethylene glycol methacrylate) (POEGMA) and rigid rod-like cellulose nanocrystals (CNCs) that can overcome this challenge. By physically incorporating CNCs into hydrazone cross-linked POEGMA hydrogels, macroscopic properties including gelation rate, swelling kinetics, mechanical properties, and hydrogel stability can be readily tailored. Strong adsorption of aldehyde and hydrazide modified POEGMA precursor polymers onto the surface of CNCs promotes uniform dispersion of CNCs within the hydrogel, imparts physical cross-links throughout the network, and significantly improves mechanical strength overall, as demonstrated by quartz crystal microbalance gravimetry and rheometry.When POEGMA hydrogels containing mixtures of long and short ethylene oxide side chain precursor polymers were prepared, transmission electron microscopy reveals that phase segregation occurs with CNCs hypothesized to preferentially locate within the stronger adsorbing short side chain polymer domains. Incorporating as little as 5 wt % CNCs results in dramatic enhancements in mechanical properties (up to 35-fold increases in storage modulus) coupled with faster gelation rates, decreased swelling ratios, and increased stability versus hydrolysis. Furthermore, cell viability can be maintained within 3D culture using these hydrogels independent of the CNC content. These properties collectively make POEGMA-CNC

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Section: Hydrogel Swelling and Degradationmentioning

confidence: 95%

Section: Hydrogel Swelling and Degradationmentioning

confidence: 99%

Section: Cell Interactions With Hydrogelsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Enhanced Mechanical Properties in Cellulose Nanocrystal–Poly(oligoethylene glycol methacrylate) Injectable Nanocomposite Hydrogels through Control of Physical and Chemical Cross-Linking

2016

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“…Hydrazone bonds formed between aldehyde and hydrazide groups are hydrolytically degradable, relatively slowly (over months) at neutral pH but significantly faster at acidic pH values. 55 The microstructure of the aerogels and the resulting hydrogels was controlled by varying the weight ratio of CNC-to-POEGMA, the total concentration of these components in the precursor suspension, and the freezecasting temperature. The well-established cytocompatibility of CNCs 44,[56][57][58] and POEGMA, 59,60 the degradability of the hydrazone cross-linked networks, and the anisotropy of these hydrogels suggests their potential utility in biomedical applications.…”

Section: Introductionmentioning

confidence: 99%

Composite Hydrogels with Tunable Anisotropic Morphologies and Mechanical Properties

et al. 2016

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Fabrication of anisotropic hydrogels exhibiting direction-dependent structure and properties have attracted great interest in biomimicking, tissue engineering and bioseparation. Herein, we report a single-step freeze casting-based fabrication of structurally and mechanically anisotropic aerogels and hydrogels composed of hydrazone cross-linked poly(oligoethylene glycol methacrylate) (POEGMA) and cellulose nanocrystals (CNCs). We show that by controlling the composition of the CNC/POEGMA dispersion and the freeze casting temperature, aerogels with fibrillar, columnar, or lamellar morphologies can be produced. Small-angle X-ray scattering experiments show that the anisotropy of the structure originates from the alignment of the mesostructures, rather than the CNC building blocks. The composite hydrogels show high structural and mechanical integrity and a strong variation in Young's moduli in orthogonal directions. The controllable morphology and hydrogel anisotropy, coupled with hydrazone cross-linking and biocompatibility of CNCs and POEGMA, provide a versatile platform for the preparation of anisotropic hydrogels.

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Injectable and Dynamically Crosslinked Zwitterionic Hydrogels for Anti‐Fouling and Tissue Regeneration Applications

Pan,

Dorogin,

Lofts

et al. 2024

Adv Healthcare Materials

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We report a zwitterionic injectable and degradable hydrogel based on hydrazide and aldehyde‐functionalized [2‐(methacryloyloxy)ethyl] dimethyl‐(3‐sulfopropyl)ammonium hydroxide (DMAPS) precursor polymers that can address practical in vivo needs. Zwitterion fusion interactions between the zwitterionic precursor polymers create a secondary physically crosslinked network to enable much more rapid gelation than previously reported with other synthetic polymers, facilitating rapid gelation at much lower polymer concentrations or degrees of functionalization than previously accessible in addition to promoting zero swelling and long‐term degradation responses and significantly stiffer mechanics than are typically accessed with previously reported low‐viscosity precursor gelation systems. The hydrogels maintain the highly anti‐fouling properties of conventional zwitterionic hydrogels against proteins, mammalian cells, and bacteria while also promoting anti‐fibrotic tissue responses in vivo. Furthermore, the use of the hydrogels for effective delivery and subsequent controlled release of viable cells with tunable profiles both in vitro and in vivo was demonstrated, including the delivery of myoblasts in a mouse skeletal muscle defect model for reducing the time between injury and functional mobility recovery. The combination of the injectability, degradability, and tissue compatibility achieved offers the potential to expand the utility of zwitterionic hydrogels in minimally‐invasive therapeutic applications.This article is protected by copyright. All rights reserved

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Injectable poly(oligoethylene glycol methacrylate)-based hydrogels with tunable phase transition behaviours: Physicochemical and biological responses

Cited by 67 publications

References 66 publications

Enhanced Mechanical Properties in Cellulose Nanocrystal–Poly(oligoethylene glycol methacrylate) Injectable Nanocomposite Hydrogels through Control of Physical and Chemical Cross-Linking

Enhanced Mechanical Properties in Cellulose Nanocrystal–Poly(oligoethylene glycol methacrylate) Injectable Nanocomposite Hydrogels through Control of Physical and Chemical Cross-Linking

Composite Hydrogels with Tunable Anisotropic Morphologies and Mechanical Properties

Injectable and Dynamically Crosslinked Zwitterionic Hydrogels for Anti‐Fouling and Tissue Regeneration Applications

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