Decoupling between Translational Diffusion and Viscoelasticity in Transient Networks with Controlled Network Connectivity

Katashima, Takuya; Kobayashi, Ryunosuke; Ishikawa, Shohei; Naito, Mitsuru; Miyata, Kanjiro; Chung, Ung‐il; Sakai, Takamasa

doi:10.3390/gels8120830

Cited by 4 publications

(3 citation statements)

References 40 publications

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“…In this section, I discuss a study that contrasts diffusivity with viscoelasticity using a model system 16) . By mixing two unique prepolymers off-stoichiometrically, I ensured a uniform concentration and network strand length, concentrating on the effects of network connectivity.…”

Section: Relationship Between Lve and Diffusivitymentioning

confidence: 99%

Precise Rheological Analysis of Permanently and Transiently Crosslinked Polymer Networks with Well-Controlled Structures

Katashima

2023

J. Soc. Rheol., Jpn

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Polymer networks, distinguished by their crosslinking structures-which can be either stable or transient-display prominent rheological properties. Nevertheless, the inability to control these network structures obstructs a fundamental understanding of the molecular mechanisms and their subsequent applications. Recently, I have conceptualized model transient networks formed of star-shaped polymers, utilizing reversible interactions. In this review, I will elucidate our most recent studies, emphasizing the relationships between the viscoelasticity and the microscopic molecular dynamics, encompassing diffusivity and binding/dissociation kinetics. Moreover, I will highlight a medical application of this knowledge: a carrier material meticulously designed for the adeno-associated virus vector.

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Section: Relationship Between Lve and Diffusivitymentioning

confidence: 99%

Precise Rheological Analysis of Permanently and Transiently Crosslinked Polymer Networks with Well-Controlled Structures

Katashima

2023

J. Soc. Rheol., Jpn

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“…Based on the prior section, there is a clear necessity for model materials with precisely controlled network structures to elucidate molecular mechanisms. Recently, we developed model transient networks utilizing tetrafunctional precursors (Tetra-PEG slimes) by employing dynamic covalent bonds between 4-carboxy-3-fluorophenylboronic acid (FPBA) and glucono-δ-lactone (GDL) as reversible crosslinks [30,[68][69][70]. Due to the temporal characteristics of the crosslinkers, the Tetra-PEG slime exhibits the flow behavior in a long time limit, classified into transient networks.…”

Section: Relationships Between Translational Diffusion and Viscoelast...mentioning

confidence: 99%

“…p is defined as the ratio of the connected end groups of prepolymers against the total end groups at the equilibrium state. p is estimated as [68,70]:…”

Section: Relationships Between Translational Diffusion and Viscoelast...mentioning

confidence: 99%

Probing the Molecular Mechanism of Viscoelastic Relaxation in Transient Networks

Michida,

Chung,

Katashima

2023

Gels

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Hydrogels, which have polymer networks through supramolecular and reversible interactions, exhibit various mechanical responsibilities to its surroundings. The influence of the reversible bonds on a hydrogel’s macroscopic properties, such as viscoelasticity and dynamics, is not fully understood, preventing further innovative material development. To understand the relationships between the mechanical properties and molecular structures, it is required to clarify the molecular understanding of the networks solely crosslinked by reversible interactions, termed “transient networks”. This review introduces our recent progress on the studies on the molecular mechanism of viscoelasticity in transient networks using multiple methods and model materials. Based on the combination of the viscoelasticity and diffusion measurements, the viscoelastic relaxation of transient networks does not undergo the diffusion of polymers, which is not explained by the framework of conventional molecular models for the viscoelasticity of polymers. Then, we show the results of the comparison between the viscoelastic relaxation and binding dynamics of reversible bonds. Viscoelastic relaxation is primarily affected by “dissociation dynamics of the bonds” and “network structures”. These results are explained in the framework that the backbone, which is composed of essential chains supporting the stress, is broken by multiple dissociation events. This understanding of molecular dynamics in viscoelasticity will provide the foundation for designing transient networks.

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Elucidating Nonlinear Stress Relaxation in Transient Networks through Two-Dimensional Rheo-Optics

Yamamoto,

Yamagata,

Sato

et al. 2024

ACS Macro Lett.

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This study aims to elucidate the origin of nonlinear stress relaxation behaviors in transient networks using a systematically controlled model system consisting of the tetra-armed polyethylene glycols (Tetra-PEG slime) in conjunction with twodimensional rheo-optics observations. Transient networks, characterized by their temporary cross-links, are extensively utilized in selfhealing and robust materials. However, the molecular mechanisms governing their viscoelastic responses to large deformations have remained elusive. This is primarily due to the heterogeneous structures inherent in conventional transient networks and a scarcity of detailed experimental evaluations. By employing Tetra-PEG slime, which is distinguished by its regular structure with uniform strand lengths and functionalities, and the polarization imaging method, we overcome these obstacles. Our results reveal that the damping phenomena observed under large step strains arise from spatially heterogeneous relaxation, predominantly driven by network strand pullout. These insights lay a solid foundation for understanding the intricate rheological properties of transient networks.

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Decoupling between Translational Diffusion and Viscoelasticity in Transient Networks with Controlled Network Connectivity

Cited by 4 publications

References 40 publications

Precise Rheological Analysis of Permanently and Transiently Crosslinked Polymer Networks with Well-Controlled Structures

Precise Rheological Analysis of Permanently and Transiently Crosslinked Polymer Networks with Well-Controlled Structures

Probing the Molecular Mechanism of Viscoelastic Relaxation in Transient Networks

Elucidating Nonlinear Stress Relaxation in Transient Networks through Two-Dimensional Rheo-Optics

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