Revisiting the Origins of the Fracture Energy of Tough Double-Network Hydrogels with Quantitative Mechanochemical Characterization of the Damage Zone

Matsuda, Takahiro; Kawakami, Runa; Nakajima, Tasuku; Hane, Yukiko; Gong, Jian Ping

doi:10.1021/acs.macromol.1c01214

Cited by 38 publications

(30 citation statements)

References 64 publications

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“…In the present work, the high toughness of our BSA/PAAm OHG may originate from the high viscosity of the mixture solvent (glycerol/H 2 O) and the plastic deformation of BSA biomacromolecules. Matsuda single-edge notch test and the controlled swelling PAAm hydrogel (ϕ PAAm = 28 wt %) estimated by a pure shear test were 343 J/m 2 and 500 J/m 2 , 40,41 respectively, which are lower than that of PAAm OHG in this work with a similar polymer content (T = 640 J/m 2 , ϕ PAAm = 30 wt %). The higher toughness of PAAm OHG may be caused by the glycerol.…”

Section: Mechanical Properties Of Bsa/paam Ohgsmentioning

confidence: 51%

Tough Adhesive, Antifreezing, and Antidrying Natural Globulin-Based Organohydrogels for Strain Sensors

Yang

Liu

et al. 2022

ACS Appl. Mater. Interfaces

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Hydrogels are often used to fabricate strain sensors; however, they also suffer from freezing at low temperatures and become dry during long-time storage. Encapsulation of hydrogels with elastomers is one of the methods to solve these problems although the adhesion between hydrogels and elastomers is usually low. In this work, using bovine serum protein (BSA) as the natural globulin model and glycerol/H 2 O as the mixture solvent, BSA/polyacrylamide organohydrogels (BSA/PAAm OHGs) were prepared by a facile photopolymerization approach. At the optimal condition, BSA/PAAm OHG demonstrated not only high toughness but also tough adhesion properties, which could strongly adhere to various substrates, such as glass, metals, rigid polymeric materials (even poly(tetrafluoroethylene), i.e., PTFE), and soft elastomers. Moreover, BSA/PAAm OHG was flexible and showed tough adhesion at −20 °C. The toughening mechanism and the adhesive mechanism were proposed. On being encapsulated by poly(dimethylsiloxane) (PDMS), it illustrated good antidrying performance. After introducing a conductive filler, the encapsulated BSA/PAAm OHG could be used as a strain sensor to detect human motions. This work provides a better understanding of the adhesive mechanism of natural proteinbased organohydrogels.

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Section: Mechanical Properties Of Bsa/paam Ohgsmentioning

confidence: 51%

Tough Adhesive, Antifreezing, and Antidrying Natural Globulin-Based Organohydrogels for Strain Sensors

Yang

Liu

et al. 2022

ACS Appl. Mater. Interfaces

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“…The high modulus ratio (hard to soft) increases the energy dissipation zone size, which is beneficial for improving the toughness. Besides, when such IR-WR samples are elongated, DND is preferentially destroyed, leading to a large energy dissipation, similar to the energy dissipation of a double network. − Consequently, the toughness of IR-WR samples dramatically increases.…”

Section: Results and Discussionmentioning

confidence: 99%

Generic Recycling Strategy to Improve Robustness of Recycled Rubbers through Bioinspired Multiphase Network

Zhou

Huang

Liu

et al. 2022

ACS Sustainable Chem. Eng.

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Recycling of rubbers is extraordinarily important for the sustainable development of the rubber industry. However, the traditional rubber recycling processes do not only deteriorate the properties of recycled rubbers but also bring environmental pollution. Inspired by the structure of mussel byssus, our group designs bioinspired multiphase network to improve the robustness of recycled rubbers. Through increasing the content of dynamic S− S cross-links, we improve the interface interaction between isoprene rubber (IR) and waste rubber (WR). Further, the combination of IR with WR forms a dense network domain (DND) and a sparse network domain (SND), constructing the bioinspired multiphase cross-linking network. Such a multiphase network contributes to stress transfer. Upon stretching, the preferential rupture of DND improves the toughness through energy dissipation. Compared with the previous works, our designed recycled rubbers exhibit superior properties. This work presents a simple generic method to increase the robustness of recycled rubbers through bioinspired multiphase network.

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“…Mechanophore motifs that alter their optical properties with respect to applied loadmechanochromophores and/or mechanofluorophores (hereafter referred to as luminescent mechanophores)have emerged as the preferred tool to visualize such force-sensitive chain level behavior (Chen et al, 2021a;Göstl et al, 2017). Embedded luminescent mechanophores in elastomer networks have confirmed that chains located far from the crack surface (compared to the chain length) become ruptured during crack advance (Boots et al, 2022;Ducrot et al, 2014;Matsuda et al, 2020Matsuda et al, , 2021Slootman et al, 2020), supporting the postulated mechanism of dissipation and toughness enhancement. Unsurprisingly, viscoelastic effects and microscopic dynamics have been found to influence and interplay with the extent of delocalized chain scission measured via luminescent mechanophores (Slootman et al, 2020(Slootman et al, , 2022.…”

Section: Introductionmentioning

confidence: 90%

A statistical mechanics framework for polymer chain scission, based on the concepts of distorted bond potential and asymptotic matching

Mulderrig¹,

Talamini²,

Bouklas³

2022

Preprint

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To design increasingly tough, resilient, and fatigue-resistant elastomers and hydrogels, the relationship between controllable network parameters at the molecular level (bond type, non-uniform chain length, entanglement density, etc.) to macroscopic quantities that govern damage and failure must be established. Many of the most successful constitutive models for elastomers have been rooted in statistical mechanical treatments of polymer chains. Typically, such constitutive models have used variants of the freely jointed chain model with rigid links. However, since the free energy state of a polymer chain is dominated by enthalpic bond distortion effects as the chain approaches its rupture point, bond extensibility ought to be accounted for if the model is intended to capture chain rupture. To that end, a new bond potential is supplemented to the freely jointed chain model (as derived in the uFJC framework of Buche and Silberstein (2021) and Buche et al. ( 2022)), which we have extended to yield a tractable, closed-form model that is amenable to constitutive model development. Inspired by the asymptotically matched uFJC model response in both the low/intermediate chain force and high chain force regimes, a simple, quasi-polynomial bond potential energy function is derived. This bond potential exhibits harmonic behavior near the equilibrium state and anharmonic behavior for large bond stretches tending to a characteristic energy plateau (akin to the Lennard-Jones and Morse bond potentials). Using this bond potential, approximate yet highlyaccurate analytical functions for bond stretch and chain force dependent upon chain stretch are established. Then, using this polymer chain model, a stochastic thermal fluctuation-driven chain rupture framework is developed. This framework is based upon a force-modified tilted bond potential that accounts for distortional bond potential energy, allowing for the derivation and subsequent calculation of the dissipated chain scission energy. The cases of rate-dependent and rate-independent scission are accounted for throughout the rupture framework. The impact of Kuhn segment number on chain rupture behavior is also investigated. The model is fit to single-chain mechanical response data collected from atomic force microscopy tensile tests for validation and to glean deeper insight into the molecular physics taking place. Due to their analytical nature, this polymer chain model and the associated rupture framework can be straightforwardly implemented in finite element models accounting for fracture and fatigue in polydisperse elastomer networks.

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Revisiting the Origins of the Fracture Energy of Tough Double-Network Hydrogels with Quantitative Mechanochemical Characterization of the Damage Zone

Cited by 38 publications

References 64 publications

Tough Adhesive, Antifreezing, and Antidrying Natural Globulin-Based Organohydrogels for Strain Sensors

Tough Adhesive, Antifreezing, and Antidrying Natural Globulin-Based Organohydrogels for Strain Sensors

Generic Recycling Strategy to Improve Robustness of Recycled Rubbers through Bioinspired Multiphase Network

A statistical mechanics framework for polymer chain scission, based on the concepts of distorted bond potential and asymptotic matching

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