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Mechanical responses after the uniaxial deformation of graded styrene–butadiene rubber (SBR) with a gradient in the crosslink points in the thickness direction were investigated as compared with those of homogenously vulcanized SBR samples. The elongational residual strain of a graded sample was found to depend on the part with a high crosslink density. Therefore, it showed good rubber elasticity. After stress removal, moreover, the graded sample showed a marked warpage. This suggested that shrinking stress acted on the surface with a high crosslink density, which would avoid a crack growth on the surface. The sample shape was then recovered to be flat very slowly, indicating that the shrinking stress worked for a long time. This unique rubber elasticity, i.e., slow strain recovery with an excellent strain recovery, makes graded rubber highly significant.

We survey, in a partial way, multi-scale approaches for the modelling of rubber-like and soft tissues and compare them with classical macroscopic phenomenological models. Our aim is to show how it is possible to obtain practical mathematical models for the mechanical behaviour of these materials incorporating mesoscopic (network scale) information. Multi-scale approaches are crucial for the theoretical comprehension and prediction of the complex mechanical response of these materials. Moreover, such models are fundamental in the perspective of the design, through manipulation at the micro- and nano-scales, of new polymeric and bioinspired materials with exceptional macroscopic properties.

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. This study explores the interplay between non‐uniform strain and crystallization near crack‐tips in natural rubber, employing micro‐scale DIC and micro‐beam scanning X‐ray scattering. Local maximum tensile strain predominantly dictates local crystallinity, while shear strain governs crystal orientation. These findings shed light on how crystallization contributes to the crack growth resistance of natural rubber.

This study investigated the properties of the natural rubber (NR) foam filled with azodicarbonamide (ADC) blowing agents by combination to various ratios of epoxidized NR (ENR) for flexible foam applications. Compound operation was prepared with an open two-roll mill and the production was fabricated by compression molding. The study elucidated properties related to crosslinking behaviors, mechanical and dynamic properties, elasticity, abrasion, weathering resistance, and sound absorption efficiency. The ENR and ADC concentrations affected the tensile testing and also the durability properties of the NR/ENR. The NR and ENR foam of 60/40 filled with 10 phr of ADC demonstrated good properties across various parameters, showing acceptable tensile properties, abrasion resistance, and QVA light resistance. Additionally, the presence of a closed-cell structure in the blends reduced crack propagation in the NR matrix during aging, improving weathering resistance. The absorption coefficient increased with higher ADC content, being optimal at 15 phr, due to the lower density and higher porosity of the opened-cell material, which enhances its ability to interact more effectively with incoming energy at 1600 and 6400 Hz. The findings encourage the use of ENR for blending in NR for improved ENR and ADC concentrations since dipole-dipole interaction from ENR-ADC caused ADC dispersability, providing complexed foam structures for force expansion and aslo sound wave absorption.

Being able to predict the lifetime of elastomers is fundamental for many industrial applications. The evolution of both tensile and compression behavior of unfilled and filled neoprene rubbers was studied over time for different ageing conditions (70 °C, 80 °C and 90 °C). While Young’s modulus increased with ageing, the bulk modulus remained almost constant, leading to a slight decrease in the Poisson’s ratio with ageing, especially for the filled rubbers. This evolution of Poisson’s ratio with ageing is often neglected in the literature where a constant value of 0.5 is almost always assumed. Moreover, the elongation at break decreased, all these phenomena having a similar activation energy (~80 kJ/mol) assuming an Arrhenius or pseudo-Arrhenius behavior. Using simple scaling arguments from rubber elasticity theory, it is possible to relate quantitatively Young’s modulus and elongation at break for all ageing conditions, while an empirical relation can correlate Young’s modulus and hardness shore A. This suggests the crosslink density evolution during ageing is the main factor that drives the mechanical properties. It is then possible to predict the lifetime of elastomers usually based on an elongation at break criterion with a simple hardness shore measurement.

Network structures of various polymers have significant effects on their mechanical properties; therefore, numerous studies have investigated the constitutive relationship between symmetrical network structures and their rubber elasticity in polymers. However, few studies have focused on asymmetrical network structures in polymers that undergo bond exchange reactions, self-assembly, or mechanochemical coupling—all of which are induced by transition probabilities of chemical bonding processes. In this study, an extended constraint junction and phantom network model is formulated using the tree-growing theory to establish a constitutive relationship between asymmetrical network structures and their rubber elasticity in polymers. A free-energy equation is further developed to explore working principles of configurational transitions on the dynamic rubber elasticity of symmetrical and asymmetrical network structures. The constitutive relationship between dynamic rubber elasticity and symmetrical and asymmetrical network structures has also been proposed for the gels undergoing mechanochemical and hydromechanical coupling. Finally, the effectiveness of this newly proposed tree-growing model has been verified by comparing with the classical affine network model, finite element analysis, and the experimental results of gels reported in literature.

Powder-free natural rubber gloves for chemical migration resistance of food-contact grade are prepared using a variety of fillers, including ground calcium carbonate (GCC), precipitated calcium carbonate (PCC), aluminum silicate (AS), and barium sulfate (BS)-filled natural rubber (NR), respectively. The properties of NR gloves, including mechanical, dynamic mechanical, and thermal properties, were investigated. Furthermore, the overall migration test of NR gloves was conducted according to the regulations for food contact gloves (EU Regulation No. 10/2011), using 3% acetic acid as the simulant. Among the fillers studied, the plate-like particles of AS facilitated the most effective filler-rubber interactions and reinforce-mentin AS-filled natural rubber (NR/AS). Consequently, the highest crosslink density, force at break, and damping properties of NR gloves were achieved by applying AS in the NR matrix. Moreover, the lowest overall migration level was observed for NR/AS with a value of 5.35 mg/dm2, which complies with EU Regulation (overall migration of food simulants shall not exceed 10 mg/dm2). Therefore, NR gloves filled with AS are suitable for food-contacting NR gloves.

Epoxidized natural rubber (ENR) with varying levels of epoxide groups ranging from 10 to 50 mol% was prepared and dynamically phenolic vulcanized by blending it with poly(ether-block-amide) copolymer (PEBA). The results indicate that the thermoplastic vulcanizates (TPVs) of ENR/PEBA blends display a sea-island morphology and enhance a number of properties. Specifically, increasing the epoxide content and PEBA proportion enhances strength properties, including higher Young’s modulus (stiffness), toughness, tensile properties, and hardness, along with smaller vulcanized ENR domains dispersed in the PEBA matrix. Moreover, the decrease in tension set values indicates an improvement in the elastic properties. The attributed cause of this is the interaction between the polar groups present in the phenolic-cured ENR domains and the PEBA molecules. As a result, interfacial adhesion between the ENR domains and PEBA interfaces improved, contributing to the observed enhancements in the strength and elastic properties of the TPVs with smaller ENR domains. Furthermore, an increase in the epoxide content was found to be correlated with a decrease in tanδ and tension set, which further supported the observed improvements in strength and elasticity. Additionally, the ENR/PEBA blends showed a single glass transition temperature (Tg), while pure PEBA exhibited two Tgs. The presence of a single Tg in the ENR/PEBA blend is attributed to the overlapping of the Tg of the ENR and PEBA immiscible blend components.

One of the most important challenges in polymer science is a rigorous understanding of the molecular mechanisms of rubber elasticity by relating macroscopic deformation to molecular changes and deriving the constitutive stress–strain equation for the elastomeric network. The models developed from the last century to today describe many aspects of the physics of rubber elasticity; although these theories are successful, they are not complete. In this review we analyze the main theoretical and phenomenological models of rubber elasticity, including their assumptions, main characteristics, and stress–strain equations. Then, we compare the predictions of the theories to our experimental data of polydimethylsiloxane (PDMS) rubber, in order to highlight the goodness of the reviewed models. The nonaffine and phenomenological deformation models verify the experimental curves in tension and compression in the whole investigated deformation range λ≤2. On the contrary, the affine deformation hypothesis is rigorously verified only in the deformation range λ≤1.

The rubber elasticity theory has been lengthily applied to several polymeric hydrogel substances and upgraded from idealistic models to consider imperfections in the polymer network. The theory relies solely on hyperelastic material models in order to provide a description of the elastic polymer network. While this is also applicable to polymer gels, such hydrogels are rather characterized by their water content and visco-elastic mechanical properties. In this work, we applied rubber elasticity constitutive models through hyperelastic parameter identification of hydrogels based on their stress–strain response to compression. We further performed swelling experiments and determined the intrinsic properties, i.e., density, of the specimens and their components. Additionally, we estimated their equilibrium swelling and employed it in the swelling-equilibrium theory in order to determine the polymer–solvent interaction parameter of each hydrogel with regard to cross-linking. Our results show that the average mesh size obtained from the rubber elasticity theory can be regarded as a concentration-dependent characteristic length of the hydrogel’s network and couples the non-linear elastic response to the specimens’ inherent visco-elasticity through hysteresis as a quantifier of energy dissipation under large deformation.