Speed-Induced Extensibility Elastomers with Good Resilience and High Toughness

Chen, Haiming; Koh, J. Justin; Long, Chuanjiang; Liu, Siqi; Shi, Huihui; Min, Jiakang; Zhou, Lili; He, Chaobin

doi:10.1021/acs.macromol.1c00175

Cited by 20 publications

(14 citation statements)

References 48 publications

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“…The intramolecular cross-linking reaction helps reduce the polymer coils' size, while the intermolecular cross-linking reaction makes these coils more tightly distributed, resulting in the more apparent intermolecular entanglement of HA. 50 The entangled molecular coils have more substantial internal entropy elasticity 51 and show better toughness but the insertion capability becomes worse, which can also be verified from the previous MN mechanical property test, where the mechanical properties of the cHA MN decreased significantly compared to the common HA MN. 48 4.3.…”

Section: Molecular Configuration Of Hasupporting

confidence: 63%

Mesoscopic Simulation for the Effect of Cross-Linking Reactions on the Drug Diffusion Properties in Microneedles

Feng

Zhang

et al. 2021

J. Chem. Inf. Model.

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The drug diffusion issue in microneedles is the focus of its medical application. It will not only affect the distribution of drugs in the needle body but will also have an impact on the drug release performance of the microneedle. The utilization of cross-linked polymer materials to obtain the drug diffusion control has been experimentally verified as a feasible method. However, the mechanism research on the molecular level is still incomplete. In this study, the dissipative particle dynamics (DPD) simulation has been applied to study the effect of the crosslinking reaction on drug diffusion in hyaluronic acid microneedles. We have discovered that when the cross-linking degree reaches 90%, the diffusion coefficient of the drug is 6.45 times lower than that of the uncross-linked system. The main reason for the decline in drug diffusion ability is that the cross-linking reaction varies the conformation of the polymer. The amplification in the cross-linking degree makes the polymer coils more compact and approach each other, finally forming a continuously distributed cross-linked network, which reduces its degradation rate in the body. Simultaneously, these cross-linked networks can also hinder the interaction of soluble drugs with water, thereby preventing the premature release of drugs. The simulation results are consistent with the data collected in the previous microneedle experiment. This work will be an extension of DPD simulation in the application of biological materials. HIGHLIGHT FOR REVIEWERS• Cross-linking reaction model is established in the DPD simulation for microneedle research. • The cross-linking reaction inhibits the diffusion of the drug by hindering the interaction between the drug and the water molecules. • The amplification in the cross-linking degree leads to a continuously distributed cross-linked network. • The simulation results are consistent with the data collected in the previous microneedle experiment.

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Section: Molecular Configuration Of Hasupporting

confidence: 63%

Mesoscopic Simulation for the Effect of Cross-Linking Reactions on the Drug Diffusion Properties in Microneedles

Feng

Zhang

et al. 2021

J. Chem. Inf. Model.

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“…The stretched SAXS pattern perpendicular to the fiber axis of pH 13.97 microfiber signifies the presence of aligned nanostructures, as proven by the AFM results. The extension and reorientation of macromolecule chains in the pH 9.14 microfiber under stretching produce scattering centers perpendicular to the stretching direction 39 , and the continuously increased macromolecule orientation within 800% tensile strain leads to intensified and narrowed scattering in the perpendicular direction (Supplementary Fig. 13b, d–f ).…”

Section: Resultsmentioning

confidence: 99%

Macromolecule conformational shaping for extreme mechanical programming of polymorphic hydrogel fibers

Wang

Chan

et al. 2022

Nat Commun

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Mechanical properties of hydrogels are crucial to emerging devices and machines for wearables, robotics and energy harvesters. Various polymer network architectures and interactions have been explored for achieving specific mechanical characteristics, however, extreme mechanical property tuning of single-composition hydrogel material and deployment in integrated devices remain challenging. Here, we introduce a macromolecule conformational shaping strategy that enables mechanical programming of polymorphic hydrogel fiber based devices. Conformation of the single-composition polyelectrolyte macromolecule is controlled to evolve from coiling to extending states via a pH-dependent antisolvent phase separation process. The resulting structured hydrogel microfibers reveal extreme mechanical integrity, including modulus spanning four orders of magnitude, brittleness to ultrastretchability, and plasticity to anelasticity and elasticity. Our approach yields hydrogel microfibers of varied macromolecule conformations that can be built-in layered formats, enabling the translation of extraordinary, realistic hydrogel electronic applications, i.e., large strain (1000%) and ultrafast responsive (~30 ms) fiber sensors in a robotic bird, large deformations (6000%) and antifreezing helical electronic conductors, and large strain (700%) capable Janus springs energy harvesters in wearables.

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“…It has been well established that based on good mobility among the molecular chains, significant intermolecular slipping would occur in the PDES elastomer when the external force is sufficient to overcome the energy of intermolecular dynamic bonds, which exhibit the high stretchability of the PDES . The formation of dynamic bonds between AA and IM was strong, leading to excellent strain at break and high toughness.…”

Section: Resultsmentioning

confidence: 99%

Cross-Linked, Transient Ionic Conductive Elastomer with Extreme Stretchability, Healability, and Degradability for Detecting Human Motions

Jia-hua

Shi

et al. 2022

ACS Appl. Polym. Mater.

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The fabrication of solvent-free ionic conductive elastomers with high stretchability and degradability is highly desired yet challenging now. Here, solvent-free ionic conductive elastomers were fabricated by the polymerization of acrylic acid (AA)/1-vinylimidazole (IM)-type deep eutectic solvent. An ion pair between AA and IM was formed in the deep eutectic solvent during fabrication. Dynamic bonding including hydrogen bonding and ionic bonding between AA and IM attracted the polymeric chain crosslinking into a liquid-free polymer elastomer without extra cross-linkers. As-prepared conductive elastomers exhibit high transparency (91.4%), ultrahigh stretchability (1464%), fast autonomous self-healing, and degradability. Furthermore, the deep eutectic solvent-based elastomers could be easily attached to human skin and human activities could be detected with high sensitivity. The resulting ionic conductive elastomer with transparency, adhesiveness, self-healing ability, and degradation would meet the Sustainable Development Goals and have potential applications for wearable devices.

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Speed-Induced Extensibility Elastomers with Good Resilience and High Toughness

Cited by 20 publications

References 48 publications

Mesoscopic Simulation for the Effect of Cross-Linking Reactions on the Drug Diffusion Properties in Microneedles

Mesoscopic Simulation for the Effect of Cross-Linking Reactions on the Drug Diffusion Properties in Microneedles

Macromolecule conformational shaping for extreme mechanical programming of polymorphic hydrogel fibers

Cross-Linked, Transient Ionic Conductive Elastomer with Extreme Stretchability, Healability, and Degradability for Detecting Human Motions

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