Ultra-responsive soft matter from strain-stiffening hydrogels

Jaspers, Maarten; Dennison, Matthew; Mabesoone, Mathijs F. J.; MacKintosh, F. C.; Rowan, Alan E.; Kouwer, Paul H. J.

doi:10.1038/ncomms6808

Cited by 204 publications

(284 citation statements)

References 26 publications

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“…• C), highly cross-linked gels are formed with a linear shear moduli G 0 ≃ 100 Pa [19,20]. For 19.5 < ∼ T < ∼ 21…”

Section: Methodsmentioning

confidence: 99%

“…K and σ are in units of the spring constant k. Squares show ℓp/ℓ0 = ∞ (athermal), circles ℓp/ℓ0 = 10 and triangles ℓp/ℓ0 = 1 where ℓp is the persistence length. We estimate that our experimental systems are in the range ℓp/ℓ0 = 1 − 10 [19,20]. Dashed line shows K ∼ σ α dependence, and indicates the region over which we fit to find α.…”

Section: Simulationsmentioning

confidence: 99%

“…In this paper, we study hydrogels based on synthetic semi-flexible polymers, (ethylene glycol)-substituted polyisocyanides [19,20]. Dissolved in water and heated above the gelation temperature (Tgel 19 C), the polymers bundle together to form an intertwined network that makes up the gel.…”

Section: Introductionmentioning

confidence: 99%

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Critical behaviour in the nonlinear elastic response of hydrogels

et al. 2016

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In this paper we study the elastic response of synthetic hydrogels to an applied shear stress. The hydrogels studied here have previously been shown to mimic the behaviour of biopolymer networks when they are sufficiently far above the gel point. We show that near the gel point they exhibit an elastic response that is consistent with the predicted critical behaviour of networks near or below the isostatic point of marginal stability. This point separates rigid and floppy states, distinguished by the presence or absence of finite linear elastic moduli. Recent theoretical work has also focused on the response of such networks to finite or large deformations, both near and below the isostatic point. Despite this interest, experimental evidence for the existence of criticality in such networks has been lacking. Using computer simulations, we identify critical signatures in the mechanical response of sub-isostatic networks as a function of applied shear stress. We also present experimental evidence consistent with these predictions. Furthermore, our results show the existence of two distinct critical regimes, one of which arises from the nonlinear stretch response of semi-flexible polymers.

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“…• C), highly cross-linked gels are formed with a linear shear moduli G 0 ≃ 100 Pa [19,20]. For 19.5 < ∼ T < ∼ 21…”

Section: Methodsmentioning

confidence: 99%

Section: Simulationsmentioning

confidence: 99%

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Critical behaviour in the nonlinear elastic response of hydrogels

et al. 2016

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“…[39] Due to the high water content and tunable mechanical properties, [40] they represent ideal scaffolds to encapsulate, stabilize, culture, and deliver living cells, [41,42] proteins, [43] and oligonucleotides. [44] In order to study the potential of these materials as drug carrier hydrogels with sustained release properties, different bioactive cargo were loaded into the gels and the release kinetics was monitored by HPLC and optical methods.…”

Section: Introductionmentioning

confidence: 99%

Self‐Assembly of Amphiphilic Janus Dendrimers into Mechanically Robust Supramolecular Hydrogels for Sustained Drug Release

Nummelin

Liljeström

Saarikoski

et al. 2015

Chemistry A European J

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Abstract:Compounds that can gelate aqueous solutions offer an intriguing toolbox to create functional hydrogel materials for biomedical applications. Here we show that amphiphilic Janus dendrimers with low molecular weights can readily form selfassembled fibers at very low mass proportion (0.2 per cent by mass) creating supramolecular hydrogels (G'>>G'') with outstanding mechanical properties, where the storage modulus G'>1000 Pa. The G' and gel melting temperature can be tuned by modulating the position or number of hydrophobic alkyl chains in the dendrimer structure, thus enabling an exquisite control over the mesoscale material properties in these molecular assemblies. The gels are formed within seconds by simple injection of ethanol-solvated dendrimers into an aqueous solution. Cryogenic transmission electron microcopy, small-angle x-ray scattering and scanning electron microscopy were used to confirm the fibrous structure morphology of the gels. Furthermore, we show that the gels can be efficiently loaded with different bioactive cargo, such as active enzymes, peptides or small molecule drugs to be used for sustained release in drug delivery.

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“…To this end, 2.5 wt %aqueous solutions of PDA containing 5mol % DA-N 3 and DA-Ac were recorded before,a nd 24 ha fter, the addition of Na-ascorbate (Figure 2b). Gelation through bundle formation is ac ommon feature of PIC gels [11,23,24] as well as certain biopolymers,such as fibrin. [6] In contrast, PDA gels follow ar ather different gelation mechanism:t here,t he formation of covalent links occurs at random positions along the fiber contour (Scheme 1a).…”

mentioning

confidence: 99%

Strain Stiffening Hydrogels through Self‐Assembly and Covalent Fixation of Semi‐Flexible Fibers

et al. 2017

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Biomimetic,strain-stiffening materials are reported, made through self-assembly and covalent fixation of small building blocks to form fibrous hydrogels that are able to stiffen by an order of magnitude in response to applied stress. The gels consist of semi-flexible rodlike micelles of bisurea bolaamphiphiles with oligo(ethylene oxide) (EO) outer blocks and ap olydiacetylene (PDA) backbone.T he micelles are fibers,composed of 9-10 ribbons.Agelation method based on Cu-catalyzed azide-alkyne cycloaddition (CuAAC), was developed and shown to lead to strain-stiffening hydrogels with unusual, yet universal, linear and nonlinear stress-strain response.U pon gelation, the X-ray scattering profile is unchanged, suggesting that crosslinks are formed at random positions along the fiber contour without fiber bundling. The work expands current knowledge about the design principles and chemistries needed to achieve fully synthetic,b iomimetic soft matter with on-demand, targeted mechanicalp roperties.Many natural soft tissues respond to small strains with al arge change in mechanical properties.Aparticularly advantageous response of natural materials is to stiffen when exposed to small strains.T his behavior can counteract large deformations,which otherwise might compromise their integrity.S uch complex, non-linear mechanical behavior is shared by an umber of proteins arranged into network architectures,including actin, [1,2] collagen, [3,4] fibrin, [5,6] and all types of intermediate filaments.[7] However,t his type of adaptivity is unmatched in the vast majority of synthetic materials,including many artificial extracellular matrices. Considerable effort has gone into the creation of synthetic materials that are mechanically indistinguishable from natural systems,f or potential application in tissue engineering or regenerative medicine.Inthis context, avariety of theoretical models has been proposed to establish the fundamental design principles of synthetic biogels. [8][9][10] Early theoretical work [8] suggests that strain-stiffening is inherent to any connected mesh of semi-flexible filaments.I nl ater work, [10] it was shown that even for stiff polymers,s tiffening is universally expected for generic,g eometric reasons.F or all its ubiquity in natural materials,the general absence of strong strain-stiffening in synthetic gels is perhaps all the more remarkable.T he reason for this,l argely,h as been the difficulty to obtain semi-flexible or even stiff polymers (synthetic polymers are generally very flexible) with strong crosslinks or long-lived entanglements which can, moreover, remain intact at sufficiently large stresses to permit the polymers to enter their nonlinear extensional regimes.Recent work of Kouwer et al. [11] on entangled networks of bundled polyisocyanopeptides (PICs), presented the first synthetic system mimicking the strain-stiffening mechanisms of biopolymer networks and showed considerable potential to further exploit the high degree of control over design parameters in synthetic molecules....

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Ultra-responsive soft matter from strain-stiffening hydrogels

Cited by 204 publications

References 26 publications

Critical behaviour in the nonlinear elastic response of hydrogels

Critical behaviour in the nonlinear elastic response of hydrogels

Self‐Assembly of Amphiphilic Janus Dendrimers into Mechanically Robust Supramolecular Hydrogels for Sustained Drug Release

Strain Stiffening Hydrogels through Self‐Assembly and Covalent Fixation of Semi‐Flexible Fibers

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