A new paradigm for the molecular basis of rubber elasticity

Hanson, Darlene; Barber, Jeffrey

doi:10.1080/00107514.2015.1006810

Cited by 13 publications

(5 citation statements)

References 58 publications

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“…[6e] It is important to note that achieving both elasticity and self‐healing properties simultaneously is difficult, because most elastomers, such as polyisoprene or poly(dimethylsiloxane) (PDMS), depend on strong covalently bonded crosslinks . In traditional elastomers, the entropy of hindered or aligned polymer chain decreases at higher strain and allows the material to recover to its original state driven by entropic gain . On the other hand, most self‐healing systems rely on the weak dynamic noncovalent interactions to recover the material's properties.…”

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confidence: 99%

An Elastic Autonomous Self‐Healing Capacitive Sensor Based on a Dynamic Dual Crosslinked Chemical System

et al. 2018

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Adopting self-healing, robust, and stretchable materials is a promising method to enable next-generation wearable electronic devices, touch screens, and soft robotics. Both elasticity and self-healing are important qualities for substrate materials as they comprise the majority of device components. However, most autonomous self-healing materials reported to date have poor elastic properties, i.e., they possess only modest mechanical strength and recoverability. Here, a substrate material designed is reported based on a combination of dynamic metal-coordinated bonds (β-diketone-europium interaction) and hydrogen bonds together in a multiphase separated network. Importantly, this material is able to undergo self-healing and exhibits excellent elasticity. The polymer network forms a microphase-separated structure and exhibits a high stress at break (≈1.8 MPa) and high fracture strain (≈900%). Additionally, it is observed that the substrate can achieve up to 98% self-healing efficiency after 48 h at 25 °C, without the need of any external stimuli. A stretchable and self-healable dielectric layer is fabricated with a dual-dynamic bonding polymer system and self-healable conductive layers are created using polymer as a matrix for a silver composite. These materials are employed to prepare capacitive sensors to demonstrate a stretchable and self-healable touch pad.

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confidence: 99%

An Elastic Autonomous Self‐Healing Capacitive Sensor Based on a Dynamic Dual Crosslinked Chemical System

et al. 2018

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“…According to the new paradigm for the molecular basis of rubber elasticity, 25 three extension regimes should be identified: low, medium, and high. In the low extension, the rubber elasticity is associated with the distribution of end-toend distances of molecular kinks.…”

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confidence: 99%

Elastocaloric effect dependence on pre-elongation in natural rubber

Xie

Sebald

Guyomar

2015

Applied Physics Letters

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In the context of solid-state-cooling, the elastocaloric effect offers a very large controlled entropy change based in low-cost polymers, especially natural rubber which is environmentally friendly. However, large elastocaloric activity requires large elongation (>5), which makes this material impractical for cooling systems due to the large change in sample's area. By performing a pre-elongation, area change is limited, and β=−∂γ/∂λ (where γ is the specific entropy and λ is the elongation) is larger. The highest β value is obtained when pre-elongation is right before (at the “eve”) the onset of the strain-induced crystallization, which is also interpreted in the view of molecular conformation. Experimental results obtained on a natural rubber sample showed an adiabatic temperature change of 4.3 °C for pre-elongation of 4 with further elongation of 4 (true strain change of 69%). Furthermore, the entropy exhibits a quasi-linear dependence on elongation, and the β value is found to be 6400 J K−1 m−3.

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“…In this situation, the number of accessible chain configurations decreases, which in turn creates an entropic force that limits further chain elongation, since every system tends towards higher entropy. Analogous to mechanical springs, entropic forces exhibit a linear relationship with the chain's end-to-end distance for minor extensions [34]. However, it is important to note that any restriction on chain configurations results in an entropic force, so compressing a molecular chain also gives rise to forces driven by entropy [35,36].…”

Section: Discussionmentioning

confidence: 99%

Intact Transition Epitope Mapping—Force Interferences by Variable Extensions (ITEM-FIVE)

Koy,

Röwer,

Thiesen

et al. 2024

Biomolecules

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Investigations on binding strength differences of non-covalent protein complex components were performed by mass spectrometry. T4 fibritin foldon (T4Ff) is a well-studied miniprotein, which together with its biotinylated version served as model system to represent a compactly folded protein to which an Intrinsically Disordered Region (IDR) was attached. The apparent enthalpies of the gas phase dissociation reactions of the homo-trimeric foldon F-F-F and of the homo-trimeric triply biotinylated foldon bF-bF-bF have been determined to be rather similar (3.32 kJ/mol and 3.85 kJ/mol) but quite distinct from those of the singly and doubly biotinylated hetero-trimers F-F-bF and F-bF-bF (1.86 kJ/mol and 1.08 kJ/mol). Molecular dynamics simulations suggest that the ground states of the (biotinylated) T4Ff trimers are highly symmetric and well comparable to each other, indicating that the energy levels of all four (biotinylated) T4Ff trimer ground states are nearly indistinguishable. The experimentally determined differences and/or similarities in enthalpies of the complex dissociation reactions are explained by entropic spring effects, which are noticeable in the T4Ff hetero-trimers but not in the T4Ff homo-trimers. A lowering of the transition state energy levels of the T4Ff hetero-trimers seems likely because the biotin moieties, mimicking intrinsically disordered regions (IDRs), induced asymmetries in the transition states of the biotinylated T4Ff hetero-trimers. This transition state energy level lowering effect is absent in the T4Ff homo-trimer, as well as in the triply biotinylated T4Ff homo-trimer. In the latter, the IDR-associated entropic spring effects on complex stability cancel each other out. ITEM-FIVE enabled semi-quantitative determination of energy differences of complex dissociation reactions, whose differences were modulated by IDRs attached to compactly folded proteins.

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A new paradigm for the molecular basis of rubber elasticity

Cited by 13 publications

References 58 publications

An Elastic Autonomous Self‐Healing Capacitive Sensor Based on a Dynamic Dual Crosslinked Chemical System

An Elastic Autonomous Self‐Healing Capacitive Sensor Based on a Dynamic Dual Crosslinked Chemical System

Elastocaloric effect dependence on pre-elongation in natural rubber

Intact Transition Epitope Mapping—Force Interferences by Variable Extensions (ITEM-FIVE)

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