Tuning the Viscoelasticity of Hydrogen-Bonded Polymeric Materials through Solvent Composition

Mathis, Lele; Chen, Yaoyao; Shull, Kenneth R.

doi:10.1021/acs.macromol.8b00344

Cited by 10 publications

(16 citation statements)

References 52 publications

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“…As f d increased from 10 to 100 vol %, the swelling ratio in length of the gel, S , increased from 1 to 2.5 (Figure b). Different S of gel in the mixture solution was due to the different solvent quality for the solubility of polymer chains and different dissociation degree of the hydrogen bonds . Then, the swollen gel was transferred into a large amount of water, in which the gel contacted its volume to some extent and reached the equilibrium state.…”

Section: Results and Discussionmentioning

confidence: 99%

“…Different S of gel in the mixture solution was due to the different solvent quality for the solubility of polymer chains and different dissociation degree of the hydrogen bonds. 54 Then, the swollen gel was transferred into a large amount of water, in which the gel contacted its volume to some extent and reached the equilibrium state. The volume contraction of gel was related to the re-formation of hydrogen bonds.…”

Section: Tunable Properties Of the Hydrogelmentioning

confidence: 99%

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A Tough and Stiff Hydrogel with Tunable Water Content and Mechanical Properties Based on the Synergistic Effect of Hydrogen Bonding and Hydrophobic Interaction

et al. 2018

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Hydrogels are usually recognized as soft and weak materials, the poor mechanical properties of which greatly limit their applications as structural elements. Designing of hydrogels with high strength and high modulus has both fundamental and practical significances. Herein we report a series of tough, stiff, and transparent hydrogels facilely prepared by copolymerization of 1-vinylimidazole and methacrylic acid in dimethyl sulfoxide followed by solvent exchange to water. The equilibrated hydrogels with water content of 50–60 wt % possessed excellent mechanical properties, with tensile breaking stress, breaking strain, Young’s modulus, and tearing fracture energy of 1.3–5.4 MPa, 40–330%, 20–170 MPa, and 600–4500 J/m2, respectively. These tough hydrogels were also stable over a wide pH range (2 ≤ pH ≤ 10), resulting from the formation of dense and robust hydrogen bonds between imidazole and carboxylic acid groups. Moreover, the water content and mechanical properties of one gel can be adjusted over a wide range by controlling the dissociation and re-formation of hydrogen bonds during the solvent exchange and heating process; the treated hydrogel with specific characters was stable in water at room temperature. This is because the density of hydrogen bonds can be modulated at high temperature yet immediately fixed at room temperature due to the high stiffness and glassy state of the hydrogel. This strategy to prepare tough and stiff hydrogels should be applicable to other systems as structural materials with promising applications in diverse fields.

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Section: Results and Discussionmentioning

confidence: 99%

Section: Tunable Properties Of the Hydrogelmentioning

confidence: 99%

A Tough and Stiff Hydrogel with Tunable Water Content and Mechanical Properties Based on the Synergistic Effect of Hydrogen Bonding and Hydrophobic Interaction

et al. 2018

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“…Quite similarly, it has been recently reported that the solvent composition tunes in a controlled fashion the strength of the hydrogen bond-based cross-links between two polyelectrolytes, leading to frequency shifts of the frequency-dependent complex moduli of polymer complexes. 17 In these examples, the solvent composition influences uniquely the strength and/or amount of crosslinks between polymer chains, presumably not the chain conformation itself. In this framework, studies on the cosolvency or co-nonsolvency effect on polymer gels are rather scarce.…”

Section: ■ Introductionmentioning

confidence: 99%

“…In ref the chemical cross-linking of gelatin is induced by an external additive, whose solubility depends on the water/ethanol content, thus leading to gels whose viscoelasticity depends on the solvent composition. Quite similarly, it has been recently reported that the solvent composition tunes in a controlled fashion the strength of the hydrogen bond-based cross-links between two polyelectrolytes, leading to frequency shifts of the frequency-dependent complex moduli of polymer complexes . In these examples, the solvent composition influences uniquely the strength and/or amount of cross-links between polymer chains, presumably not the chain conformation itself.…”

Section: Introductionmentioning

confidence: 99%

Tailoring the Viscoelasticity of Polymer Gels of Gluten Proteins through Solvent Quality

et al. 2020

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We investigate the linear viscoelasticity of polymer gels produced by the dispersion of gluten proteins in water/ethanol binary mixtures with various ethanol contents, from pure water to 60% v/v ethanol. We show that the complex viscoelasticity of the gels exhibits a time/solvent composition superposition principle, demonstrating the self-similarity of the gels produced in different binary solvents. All gels can be regarded as near critical gels with characteristic rheological parameters, elastic plateau, and characteristic relaxation time, which are related to one another, as a consequence of self-similarity, and span several orders of magnitude when changing the solvent composition. Thanks to calorimetry and neutron scattering experiments, we evidence a cosolvency effect with better solvation of the complex polymer-like chains of the gluten proteins as the amount of ethanol increases. Overall, the gel viscoelasticity can be accounted for by a unique characteristic length characterizing the cross-link density of the supramolecular network, which is solvent composition-dependent. On a molecular level, these findings could be interpreted as a transition of the supramolecular interactions, mainly H-bonds, from intra- to interchains, which would be facilitated by the disruption of hydrophobic interactions by ethanol molecules. This work provides a new insight for tailoring the gelation process of complex polymer gels.

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“…Quite similarly, it has been recently reported that the solvent composition tunes in a controlled fashion the strength of the hydrogen bonds-based crosslinks between two polyelectrolytes, leading to frequency shifts of the frequency dependent complex moduli of polymer complexes. 17 In these examples, the solvent composition influences uniquely the strength and/or amount of crosslinks between polymer chains, presumably not the chain conformation itself. In this framework, studies on co-solvency or co-nonsolvency effect on polymer gels are rather scarce.…”

Section: Introductionmentioning

confidence: 99%

Tailoring the viscoelasticity of polymer gels of gluten proteins through solvent quality

Costanzo,

Banc,

Louhichi

et al. 2020

Preprint

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We investigate the linear viscoelasticity of polymer gels produced by the dispersion of gluten proteins in water:ethanol binary mixtures with various ethanol contents, from pure water to 60 % v:v ethanol. We show that the complex viscoelasticity of the gels exhibits a time/solvent composition superposition principle, demonstrating the self-similarity of the gels produced in different binary solvents. All gels can be regarded as near critical gels with characteristic rheological parameters, elastic plateau and characteristic relaxation time, which are related one to another, as a consequence of self-similarity, and span several orders of magnitude when changing the solvent composition. Thanks to calorimetry and neutron scattering experiments, we evidence a co-solvency effect with a better solvation of the complex polymer-like chains of the 1

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Tuning the Viscoelasticity of Hydrogen-Bonded Polymeric Materials through Solvent Composition

Cited by 10 publications

References 52 publications

A Tough and Stiff Hydrogel with Tunable Water Content and Mechanical Properties Based on the Synergistic Effect of Hydrogen Bonding and Hydrophobic Interaction

A Tough and Stiff Hydrogel with Tunable Water Content and Mechanical Properties Based on the Synergistic Effect of Hydrogen Bonding and Hydrophobic Interaction

Tailoring the Viscoelasticity of Polymer Gels of Gluten Proteins through Solvent Quality

Tailoring the viscoelasticity of polymer gels of gluten proteins through solvent quality

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