Crystallization and Stress Relaxation in Highly Stretched Samples of Natural Rubber and Its Synthetic Analogue

Tosaka, Masatoshi; Kawakami, Daisuke; Senoo, Kazunobu; Kohjiya, Shinzo; Ikeda, Yuko; Toki, Shigeyuki; Hsiao, Benjamin S.

doi:10.1021/ma060407+

Cited by 97 publications

(110 citation statements)

References 22 publications

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“…The crystallinity was followed by WAXD and the results showed a small shifting towards higher values for λ A . These measurements confirmed that the results obtained by Miyamoto et al 51 for IR are also valid for NR. However, the faster SIC kinetics for NR compared to IR reduces this strain rate effect.…”

Section: Strain Ratesupporting

confidence: 91%

“…The work of Choi and Roland 50 on NR crosslinked with peroxide confirms this kind of evolution for stress relaxation. Similar results have been established by WAXD on NR and IR by Tosaka et al, 51 who showed that SIC kinetics and consecutively stress relaxation are much slower in the case of IR. The short-term crystallization for a static stretch is much more difficult to analyze than long-term crystallization because λ max is never reached instantaneously; moreover, conventional x-ray diffraction requires slow data acquisition (typically few minutes) that is not compatible with the study of short-time effects.…”

Section: Strain-induced Crystallization and Mechanical Behavior supporting

confidence: 89%

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Strain-Induced Crystallization of Natural Rubber: A Review of X-Ray Diffraction Investigations

Huneau

2011

Rubber Chemistry and Technology

205

157

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Strain-induced crystallization of natural rubber was discovered in 1925 by the means of x-ray diffraction and has been widely investigated by this technique until today. The studies devoted to the structure of the crystalline phase of natural rubber are first reviewed. This structure is strongly anisotropic and can be related to the exceptionally good strength and fatigue properties of this material. The relationships between strain-induced crystallization of natural rubber and its mechanical response, during static or tension-retraction tests, are also reviewed and discussed; in particular, the hysteresis of the stress-strain curve is mainly explained by strain-induced crystallization. The kinetics of crystallization under both static and cyclic deformation is also discussed, as well as the influence of different factors, depending either on material composition (crosslink density, carbon black fillers) or on external parameters (temperature, strain rate. . . )

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Section: Strain Ratesupporting

confidence: 91%

Section: Strain-induced Crystallization and Mechanical Behavior supporting

confidence: 89%

Strain-Induced Crystallization of Natural Rubber: A Review of X-Ray Diffraction Investigations

Huneau

2011

Rubber Chemistry and Technology

205

157

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“…Such a big difference in i would have been detectable. 50,51 presented that the initial rate of SIC is faster for the samples with the higher . Then the predicted dependence of i on would appear more strongly, if the kinetics has really affected.…”

Section: Incipient Strain Of Crystallizationmentioning

confidence: 99%

“…These results are consistent with the classic experimental studies. 9,11 Tosaka et al 50,51 studied SIC and corresponding stress relaxation during the shorter time ranging ca. 8 s to 30 min for NR and IR samples with various .…”

Section: Crystallization Under Constant Strainmentioning

confidence: 99%

“…In the latter stage of SIC, the necessity to exclude Strain-induced Crystallization of NR the crosslinking from crystallizing molecular chains would retard the crystallization rate, and at the same time, would diminish the attainable crystallinity. 9,11,42 According to the new results, 50,51 we may have to reconsider the material design when we expect the reinforcing effect of SIC for quickly deformed products.…”

Section: Crystallization Under Constant Strainmentioning

confidence: 99%

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Strain-Induced Crystallization of Crosslinked Natural Rubber As Revealed by X-ray Diffraction Using Synchrotron Radiation

Tosaka

2007

Polym J

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ABSTRACT:Strain-induced crystallization (SIC) of natural rubber (NR) has been extensively studied even before the advent of macromolecular physics. However, there are still some unsolved basic issues in this field. In this review article, classic studies on SIC of NR are briefly introduced, and then recent results by synchrotron X-ray diffraction studies in separate papers by different authors are categorized and interpreted on the basis of molecular models. Cyclic deformation experiments provided information on partial orientation of the network-chains, on nucleation and morphological changes of crystals and on stress field around the strain-induced crystals. On the other hand, experiments under constant strain provided information on kinetics of SIC, on stress relaxation due to SIC, and so on. The experimental results could be explained under the assumption that the SIC is dominated by strain, and that the crystals are of foldedchain type. However, in order to consistently explain the various experimental results, we have to establish a unified molecular model of the network structure. [doi:10.1295/polymj.PJ2007059] KEY WORDS Network-chain Density / Crosslinking / Supercooling / Entropy / Rubber Elasticity / Crystallite Size / Entanglement / Natural rubber (NR) from Hevea latex is an indispensable material for many industrial and household applications, 1 which is constituted of cis-1,4-polyisoprene (ca. 94%) and non-rubber components such as proteins (ca. 2%) and lipid (ca. 3%).2 The versatility of the plant-derived NR is mainly due to its outstanding tensile properties and the good crack growth resistance. We still cannot reproduce the good performance of the NR products using synthetic cis-1,4-polyisoprene rubber (IR). The superiority of NR has been thought to originate from its ability to crystallize immediately by expansion; by contrast, crystallinity of IR is not as high as NR because of the lower regularity of the main-chain structure. 2,3 In this context, straininduced crystallization (SIC) of NR has been extensively studied even before the advent of macromolecular physics.

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Unraveling Non‐Uniform Strain‐Induced Crystallization Near a Crack Tip in Natural Rubber

Mai,

Yasui,

Tanaka

et al. 2024

Advanced Science

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Strain‐induced crystallization (SIC) in natural rubber (NR) near crack tips significantly enhances crack growth resistance, but understanding the interplay between local strain field and crystallization remains challenging due to confined and heterogeneous characteristics. Using micro‐scale digital image correlation (DIC) and scanning wide‐angle X‐ray diffraction (WAXD, with a narrow 10 µm square beam), this study maps local strain tensor properties and SIC in the vicinity of the crack tip and its peripheral zone (≈3 mm × 1 mm area). The analysis reveals a significant correlation between these properties. In the peripheral zone, there is a noticeable deviation of both the principal strain axis and the crystal orientation from the crack opening direction. These deviations are linearly correlated, which indicates that shear strain plays a significant role in determining the crystal orientation. Crucially, the maximum tensile component in the tensor of local principal strains predominantly dictates local crystallinity. This simplicity is attributed to the limited variation in types of deformation within the SIC region, with corresponding to deformations falling between planar and uniaxial stretching. These findings pave the way for predicting crystallinity distribution using solely strain field data, offering valuable insights into the role of SIC in enhancing the crack growth resistance of NR.

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Crystallization and Stress Relaxation in Highly Stretched Samples of Natural Rubber and Its Synthetic Analogue

Cited by 97 publications

References 22 publications

Strain-Induced Crystallization of Natural Rubber: A Review of X-Ray Diffraction Investigations

Strain-Induced Crystallization of Natural Rubber: A Review of X-Ray Diffraction Investigations

Strain-Induced Crystallization of Crosslinked Natural Rubber As Revealed by X-ray Diffraction Using Synchrotron Radiation

Unraveling Non‐Uniform Strain‐Induced Crystallization Near a Crack Tip in Natural Rubber

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