Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels

Grad, Emilia M.; Tunn, Isabell; Voerman, Dion; León, Alberto Sanz de; Hammink, Roel; Blank, Kerstin

doi:10.3389/fchem.2020.00536

Cited by 16 publications

(8 citation statements)

References 61 publications

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“…Interchain crosslinks are more likely to create elastically active bonds compared to intrachain bonds. 45 We postulated that by changing the structure of the crosslinker, the proportion of interchain and intrachain crosslinks can be altered. 45 Further, different crosslinkers may possess different interchain bond strengths due to their structural differences.…”

Section: Introductionmentioning

confidence: 99%

“…45 We postulated that by changing the structure of the crosslinker, the proportion of interchain and intrachain crosslinks can be altered. 45 Further, different crosslinkers may possess different interchain bond strengths due to their structural differences. 46,47 Therefore, HGs with different stiffness would be achievable by merely changing the crosslinker.…”

Section: Introductionmentioning

confidence: 99%

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Repurposing pinacol esters of boronic acids for tuning viscoelastic properties of glucose-responsive polymer hydrogels: effects on insulin release kinetics

et al. 2022

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Repurposing pinacol esters of boronic acids for tuning viscoelastic properties of glucose-responsive polymer hydrogels: effects on insulin release kinetics

et al. 2022

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“…Unlike randomly crosslinked networks, sPEG hydrogels evenly distribute applied mechanical loads on all bonds and dissipate mechanical energy by controlled uncoiling 30 of the network segments. [31][32][33][34][35] This renders any detection of force-in-duced events using optical force probes 36 based on covalent bond scission difficult and hence serves as an ideal proof-ofconcept application for our mechanochromic macrocrosslinkers. We show that PyMC endows the sPEG hydrogels with reversible mechanochromic behavior in the elastic deformation regime.…”

Section: Introductionmentioning

confidence: 99%

Pyrene-Based Macrocrosslinkers with Supramolecular Mechanochromism for Elastic Deformation Sensing in Hydrogel Networks

Rasch

Göstl

2022

Organic Materials

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Excimer-containing polymers with supramolecular mechanochromism are an attractive and well-investigated class of mechanoresponsive materials. However, only recently steps toward mechanophore-like mechanochromic systems that are anchored within the parent polymer structure and that show defined optical transitions on the molecular scale have been reported. However, the multi-step syntheses of these constructs are tedious. Here we report the development of a series of pyrene-based macrocrosslinkers that display supramolecular mechanochromism and are readily synthesized from mostly commercial reagents. We incorporate the water-soluble macrocrosslinkers in hydrogel networks and demonstrate their reversible mechanochromic behavior in the elastic deformation regime.

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“…[21,22] However, research in polymer mechanochemistry until now mainly focused on understanding the force-induced chemical transformations and their impact on material properties. Although force was shown to impact naturally occurring macromolecules both on the single molecule level [23][24][25] as well as in cells, [26,27] tissues, [28] and biohybrid materials, [29] the USinduced activation of biomacromolecules to achieve biological function remained unexplored. We herein display the unprecedented activation of genetically engineered proteins [30] by US firstly on a GFP model system and eventually with the release of an inhibitor of the enzyme trypsin turning "on" its catalytic activity.…”

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confidence: 99%

Controlling Optical and Catalytic Activity of Genetically Engineered Proteins by Ultrasound

et al. 2020

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Ultrasound (US) produces cavitation-induced mechanical forces stretching and breaking polymer chains in solution. This type of polymer mechanochemistry is widely used for synthetic polymers, but not biomacromolecules, even though US is biocompatible and commonly used for medical therapy as well as in vivo imaging. The ability to control protein activity by US would thus be a major stepping-stone for these disciplines. Here, we provide the first examples of selective protein activation and deactivation by means of US. Using GFP as a model system, we engineer US sensitivity into proteins by design. The incorporation of long and highly charged domains enables the efficient transfer of force to the protein structure. We then use this principle to activate the catalytic activity of trypsin by inducing the release of its inhibitor. We expect that this concept to switch "on" and "off" protein activity by US will serve as a blueprint to remotely control other bioactive molecules.

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Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels

Cited by 16 publications

References 61 publications

Repurposing pinacol esters of boronic acids for tuning viscoelastic properties of glucose-responsive polymer hydrogels: effects on insulin release kinetics

Repurposing pinacol esters of boronic acids for tuning viscoelastic properties of glucose-responsive polymer hydrogels: effects on insulin release kinetics

Pyrene-Based Macrocrosslinkers with Supramolecular Mechanochromism for Elastic Deformation Sensing in Hydrogel Networks

Controlling Optical and Catalytic Activity of Genetically Engineered Proteins by Ultrasound

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