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Takeshi Fujiyabu

Publications and source records attributed to Takeshi Fujiyabu.

4 recordsLinked to original sources

Polymer Network Diffusion in Charged Gels

The swelling kinetics of charged polymer gels reflect the complex competition among elastic, mixing, and ionic contributions. Here, we used dynamic light scattering to investigate the collective diffusion coefficient of model gels, whose polymer network structure was controlled so that the three contributions were comparable. We demonstrate that the collective diffusion coefficient stems from the sum of elastic, mixing, and ionic contributions, without evident cross-correlations. The significant ionic contribution conforms to the Donnan equilibrium, which explains equilibrium electrical potential gradients in biological systems.

cond-mat.soft

Tri-branched gels: Rubbery materials with the lowest branching factor approach the ideal elastic limit

Unlike hard materials such as metals and ceramics, rubbery materials can endure large deformations due to the large conformational degree of freedom of the crosslinked three-dimensional polymer network. However, the effect of the branching factor of the network on the ultimate mechanical properties of rubbery materials has not yet been clarified. This study shows that tri-branching, which entails the lowest branching factor, results in a large elastic deformation near the theoretical upper bound. This ideal elastic limit is realized by reversible strain-induced crystallization, providing on-demand reinforcement. The findings indicate that the polymer chain is highly orientated along the stretching axis, whereat enhanced reversible strain-induced crystallization is observed in the tri-branched and not in the tetra-branched network. A mathematical theory of structural rigidity is used to explain the difference in the chain orientation. Although tetra-branched polymers have been preferred since the development of vulcanization, these findings highlighting the merits of tri-branching will prompt a paradigm shift in the development of rubbery materials.

cond-mat.mtrl-sci

Temperature Dependence of Polymer Network Diffusion

The swelling dynamics of polymer gels are characterized by the (collective) diffusion coefficient $D$ of the polymer network. Here, we measure the temperature dependence of $D$ of polymer gels with controlled homogeneous network structures using dynamic light scattering. An evaluation of the diffusion coefficient at the gelation point $D_{\mathrm{gel}}$ and the increase therein as the gelation proceeds $ΔD\equiv D-D_{\mathrm{gel}}$ indicates that $ΔD$ is a linear function of the absolute temperature with a significantly large negative constant term. This feature is formally identical to the recently discovered "negative energy elasticity" [Y. Yoshikawa et al., Phys. Rev. X 11, 011045 (2021) (arXiv:1912.13191)], demonstrating a nontrivial similarity between the statics and dynamics of polymer networks.

cond-mat.soft

Damageless Tough Hydrogels with On-demand Self-reinforcement

Most tough hydrogels are reinforced by introducing sacrificial structures that can dissipate input energy. However, since the sacrificial damages cannot recover instantly, the toughness of these gels drops substantially during consecutive cyclic loadings. Here, we propose a new damageless reinforcement strategy for hydrogels utilizing strain-induced crystallization (SIC). In Slide-Ring (SR) gels with freely movable cross-links, crystalline repetitively forms and destructs with elongation and relaxation, resulting in both excellent toughness of 5.5 - 25.2 MJ/m$^3$ and 87% - 95% instant recovery of extension energy between two consecutive 11-fold loading-unloading cycles. Moreover, SIC occurs "on-demandly" at the crack-tip area where strain amplification and stress concentration take place and forces the crack to turn sideways. The instantly reversible tough hydrogels are promising candidates for applications in artificial connective tissues such as tendon and ligament.

cond-mat.mtrl-sci