Examination of the Theories of Rubber Elasticity Using an Ideal Polymer Network

Akagi, Yuki; Katashima, Takuya; Katsumoto, Yukiteru; Fujii, Kenta; Matsunaga, Takuro; Chung, Ung‐il; Shibayama, Mitsuhiro; Sakai, Takamasa

doi:10.1021/ma201088r

Cited by 131 publications

(127 citation statements)

References 30 publications

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“…25 Using FT-IR, p was estimated as the peak intensity ratio of amide to sum of amide and carboxyl groups. 21 Fig . 1 shows the reaction conversion as a function of t deg .…”

Section: B Reaction Conversion Was Tuned By the Pre-dissociation Of mentioning

confidence: 99%

“…[18][19][20] Although the connectivity and spatial heterogeneities were observed, the degree of heterogeneity was much smaller than that of conventional gels. [21][22][23] In previous studies, we have revealed the requirement conditions for the models predicting G of Tetra-PEG gel, and estimated the credible values of ν and N. [14][15][16][17] Thus, we can calculate and use the values of ν and N from feed condition with no ambiguity.…”

Section: Introductionmentioning

confidence: 99%

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Fracture energy of polymer gels with controlled network structures

Akagi

Sakurai

Gong

et al. 2013

The Journal of Chemical Physics

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111

112

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We have investigated the fracture behaviors of tetra-arm polyethylene glycol (Tetra-PEG) gels with controlled network structures. Tetra-PEG gels were prepared by AB-type crosslink-coupling of mutually reactive tetra-arm prepolymers with different concentrations and molecular weights. This series of controlled network structures, for the first time, enabled us to quantitatively examine the LakeThomas model, which is the most popular model predicting fracture energies of elastomers. The experimental data showed good agreement with the Lake-Thomas model, and indicated a new molecular interpretation for the displacement length (L), the area around a crack tip within which the network strands are fully stretched. L corresponded to the three times of end-to-end distance of network strands, regardless of all parameters examined. We conclude that the Lake-Thomas model can quantitatively predict the fracture energy of polymer network without trapped entanglements, with the enhancement factor being near 3.

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“…25 Using FT-IR, p was estimated as the peak intensity ratio of amide to sum of amide and carboxyl groups. 21 Fig . 1 shows the reaction conversion as a function of t deg .…”

Section: B Reaction Conversion Was Tuned By the Pre-dissociation Of mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Fracture energy of polymer gels with controlled network structures

Akagi

Sakurai

Gong

et al. 2013

The Journal of Chemical Physics

Self Cite

111

112

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“…[12][13][14][15][16][17][18][19][20][21] Tetra-PEG gels are formed from mutually reactive tetra-armed PEG prepolymers in an aqueous solution (AB-type crosslink coupling, Figure 1e). The prepolymers have amine and activated ester end groups, resulting in linking through amide bonds.…”

Section: Introductionmentioning

confidence: 99%

Experimental verification of homogeneity in polymer gels

Sakai

2014

Polym J

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The realization of an ideal polymer network that is free from heterogeneity is one of the ultimate goals in polymer science. Heterogeneity is known to be an inherent property of polymer networks. To realize an ideal polymer network, we need to develop methods to achieve a homogeneous network structure and to confirm the network homogeneity. This is a dilemma, as the former method needs to be verified by the latter method, while the latter method needs to be examined by the former method. To resolve this situation, a series of studies on polymer networks with well-defined properties is needed. We recently designed and fabricated novel Tetra-polyethyleneglycol (PEG) hydrogels. Characterization by small angle neutron scattering, infrared spectroscopy, nuclear magnetic resonance and tearing experiments indicates that Tetra-PEG gels have highly suppressed heterogeneity. In this review, we show a series of experimental results from Tetra-PEG gels and discuss the results in terms of network homogeneity. Finally, using Tetra-PEG gels as a model system, we examine models for predicting the elastic modulus of polymer gels and show that Tetra-PEG gels are useful as a model system for evaluating models that predict the physical properties of polymer networks.

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“…According to our previous studies, Tetra-PEG gels at preparation state can be treated as to such ideal networks. [36,37,39] As shown in Figure 3b, when we increased f m from the fully swollen state to the fully deswollen state, the slopes at …”

Section: à2mentioning

confidence: 80%

“…[36] Investigations of infrared spectroscopy and 1 H multiple-quantum nuclear magnetic resonance revealed that the connectivity heterogeneities (unreacted ends and intramolecular links) are highly suppressed compared with conventional rubbery materials. [37,38] The investigation of the small deformation and the fracture test showed that the elasticity of the Tetra-PEG gels simply originates from the chemical crosslinks, and that the contribution of entanglement couplings between network strands is negligible. [39] Based on these results, Tetra-PEG gel is a promising model system as ideal polymer networks.…”

Section: Introductionmentioning

confidence: 99%

Effect of Swelling and Deswelling on Mechanical Properties of Polymer Gels

Katashima

Chung

Sakai

2015

Macromolecular Symposia

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Summary: Polymer gels exhibit some unique features that are not seen in the uncrosslinked polymer system, rubber elasticity and swelling. In this paper, we review our recent studies towards the molecular understanding of the relationship between the elasticity and the swelling ratio using the Tetra-PEG gels. The dependence of the polymer volume fraction of interest state (f m ) on the elasticity exhibits the power-law behaviors and the crossovers at f Ã and f c due to the presence of the excluded volume effect and the supercoiling. The Obukhov model successfully describes the power-law behaviors. The fractal dimension of network strands (D f ) based on the stress-elongation relationships using the Pincus blob revealed that the gyration radius of the network strands decreases with deswelling in affine manner. As for the equilibrium swelling, the definite f 0 -dependences of f m and E s are observed due to the effect of the excluded volume effect at preparation state. The Obukhov model can predict this result, while the C Ã theorem cannot predict it. Using the polymer gels with precisely controlled network structures, we successfully verify the molecular models to describe the relationships between the elasticity and the swelling degree of polymer gels.

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Examination of the Theories of Rubber Elasticity Using an Ideal Polymer Network

Abstract: Constant amounts of TAPEG and TNPEG (80 mg/mL) were dissolved in phosphate buffer (25 mM, pH 7.4) and phosphate-citric acid buffer (25 mM, pH5.8), respectively.

Cited by 131 publications

References 30 publications

Fracture energy of polymer gels with controlled network structures

Fracture energy of polymer gels with controlled network structures

Experimental verification of homogeneity in polymer gels

Effect of Swelling and Deswelling on Mechanical Properties of Polymer Gels

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