Linear Viscoelasticity Research Articles

Linear viscoelasticity of anisotropic carbon fibers reinforced thermoplastics: From micromechanics to dynamic torsion experiments

Linear viscoelasticity of anisotropic carbon fibers reinforced thermoplastics: From micromechanics to dynamic torsion experiments

A Comparative View of Becker, Lomnitz, and Lambert Linear Viscoelastic Models

We compare the classical viscoelastic models due to Becker and Lomnitz with respect to a recent viscoelastic model based on the Lambert W function. We take advantage of this comparison to derive new analytical expressions for the relaxation spectrum in the Becker and Lomnitz models, as well as novel integral representations for the retardation and relaxation spectra in the Lambert model. In order to derive these analytical expressions, we have used the analytical properties of the exponential integral and the Lambert W function, as well as the Titchmarsh’s inversion formula of the Stieltjes transform. In addition, we prove some interesting inequalities by comparing the different models considered, as well as the non-negativity of the retardation and relaxation spectral functions. This means that the complete monotonicity of the rate of creep and the relaxation functions is satisfied, as required by the classical theory of linear viscoelasticity.

Nonuniversal Dynamics of Hyperbranched Metallo-Supramolecular Polymer Networks by the Spontaneous Formation of Nanoparticles.

Various transient and permanent bonds are commonly combined in increasingly complex hierarchical structures to achieve biomimetic functions, along with high mechanical properties. However, there is a traditional trade-off between mechanical strength and biological functions like self-healing. To fill this gap, we develop a metallo-supramolecular polymer hydrogel based on the hyperbranched poly(ethylene imine) (PEI) backbone and phenanthroline ligands, which have unexpectedly high plateau modulus at low concentrations. Rheological measurements demonstrate nonuniversal metal-ion-specific dynamics, with significantly larger plateau moduli, longer relaxation times, and stronger temperature dependencies, compared to equivalent networks based on model-type telechelic precursors, which cannot be explained by the theory of linear viscoelasticity. TEM images reveal the in situ mineralization of metal ions, which nucleate by the ligand complexation and grow thanks to the spontaneous reducing effect of the PEI backbone. Evidently, the complex lifetime works against Ostwald ripening, resulting in the formation of thermodynamically stable smaller particles. This trend is followed by time-dependent network buildup measurements and is confirmed by a kinetic model for particle formation and aggregation. The spontaneous formation of particles with complex lifetime-dependent sizes can explain the nonuniversal dynamics through the interaction of polymer segments and particles at the nanoscale. This work describes how the polymer backbone can affect the strength and stability of supramolecular bonds, promising for combining high mechanical properties and self-healing comparable to natural tissues.

On the Relation between the Viscoelastic Properties of Granular Hydrogels and Their Performance as Support Materials in Embedded Bioprinting.

Granular hydrogels, formed by jamming microgels suspension, are promising materials for three-dimensional bioprinting applications. Despite their extensive use as support materials for embedded bioprinting, the influence of the particle's physical properties on the macroscale viscoelasticity on one hand and on the printing performance on the other hand remains unclear. Herein, we investigate the linear and nonlinear rheology of κ-carrageenan granular hydrogel through small- and large-amplitude oscillatory shear measurements. We tuned the granular hydrogel's properties by changing the stiffness (soft, medium, stiff) and the packing density of the individual microgels. Characterizations in the linear viscoelasticity regime revealed that the storage modulus of granular hydrogels is not a simple function of microgel stiffness and depends on the microgel packing density. At larger strains, increasing the microgel stiffness reduced the energy dissipation of the granular beds and increased the solid-fluid transition point. To understand how the different rheological properties of granular support materials influence embedded bioprinting, we examined the printing fidelity and cellular filament shrinkage within the granular beds. We found that microgels with low packing density diminished the printing quality, while stiff microgels promoted filament roughness. In addition, we found that highly packed stiff microgels significantly reduced the postprinting contraction of cellular filaments. Overall, this work provides a comprehensive knowledge of the rheology of granular hydrogels that can be used to rationally design support beds for bioprinting applications with specific characteristics.

Study of Dynamic Modulus of Asphalt Mix after Reinforcement of Sandstone

Sandstone has poor mechanical properties. To facilitate the application of sandstone into asphalt mixtures, sandstone was treated by immersion in sodium silicate solution, and the dynamic modulus after reinforcement was used as a criterion. The results showed that the mechanical properties of the sandstone aggregate treated with sodium silicate were improved, and the dynamic modulus was increased by 18.2%, which will help to reduce rutting. The dynamic modulus and phase angle can be effectively predicted over a wide frequency range using the sigma function and the Kramers–Kronig relationship. Sandstone asphalt mixtures basically conform to linear viscoelasticity, but the phase angle changes are more complicated at high temperatures and do not vary monotonically with frequency. By calculating the rutting coefficient, fatigue coefficient, and DSRFn parameters for performance prediction, it was found that an increase in dynamic modulus resulted in a significant increase in the rutting coefficient but a decrease in the cracking resistance.

A Note on Some Novel Laplace and Stieltjes Transforms Associated with the Relaxation Modulus of the Andrade Model

In the framework of linear viscoelasticity, the authors have previously calculated a novel inverse Laplace transform involving the Mittag–Leffler function in order to calculate the relaxation modulus in the Andrade model. Here, we generalize this result, calculating the inverse Laplace transform of a given function Fα,βs by using two different approaches: the Bromwich integral and the decomposition of Fα,βs in simple fractions. From both calculations, we obtain a set of novel Laplace and Stieltjes transforms.

Nonlinear viscoelastic effect on the fatigue performance of wood tar-based rejuvenated asphalt

The nonlinear viscoelasticity (NLVE) effects of rejuvenated asphalt are often neglected during fatigue degradation, potentially leading to misjudgment of its true fatigue performance. To more accurately quantify the fatigue life of rejuvenated asphalt under NLVE effects, frequency sweep (FS), incremental stress sweep (ISS), and linear amplitude sweep (LAS) tests were used to study two types of rejuvenated asphalt. FS and ISS tests respectively obtained the dynamic modulus |G*|LVE and |G*|NLVE representing the linear viscoelasticity (LVE) and NLVE of rejuvenated asphalt, and incorporated them into the simplified viscoelastic continuum damage (S-VECD) model to establish the fatigue failure criterion and predict the fatigue life of rejuvenated asphalt under high strain levels in LAS tests. The findings indicate that the NLVE-based-S-VECD model quantifies fatigue damage in rejuvenated asphalt lower than the LVE model, and the fatigue life of rejuvenated asphalt increases significantly after considering the NLVE effect. Besides, the failure difference (∆GR) and failure area difference (∆A) defined during the modeling process explain the impact of NLVE on the fatigue failure criterion average pseudo strain energy release rate (GR) of rejuvenated asphalt, validating the necessity of incorporating NLVE into the fatigue performance analysis of rejuvenated asphalt. Therefore, it's necessary to account for the impact of NLVE effect on the fatigue performance of rejuvenated asphalt in engineering practice, which will contribute to the development and application of rejuvenator.

A finite strain viscoelastic model with damage and tension–compression asymmetry considerations for solid propellants

A short survey on the experimental testing of solid propellants has highlighted finite strain responses that are temperature-dependent, viscoelastic with damage, and exhibit tension/compression asymmetry. Consequently, a finite strain viscoelastic model that satisfies the principles of thermodynamics has been developed. This model is based on the common multiplicative decomposition of the deformation gradient into elastic and viscous components, with considerations for damage and asymmetry. The model has been tested against three sets of data from the literature, carefully selected to represent the various characteristics of solid propellants. The model accurately reproduces uniaxial tension responses at different strain rates and temperatures, with the capability to account for superimposed hydrostatic pressure. Notably, these satisfactory representations require only five fitting parameters, in addition to the typical identification of polymer linear viscoelasticity and time–temperature superposition. Finally, an attempt to reproduce both tension and compression tests conducted independently on the same material underscores the need to account for tension–compression asymmetry, as defined in the proposed constitutive equations. This finding advocates for new tests, such as compression following tension and vice versa.

Melt blending of commercial linear polyethylene with low-entangled ultra-high molecular weight polyethylene: From dispersion compatibility to viscoelastic scaling laws

This study investigates the dispersion and compatibility of low-entangled “dis-entangled” UHMWPE (dis-UH) in a high-density polyethylene (HDPE) matrix using solvent-free melt-blending conditions and compares it with entangled UHMWPE (eUH) in the same matrix. The findings reveal that dis-UH/HDPE exhibits a significantly lower viscosity ratio than eUH/HDPE (1 and 4, respectively), indicating a lower critical capillary number (Cacritical), thus enhanced dispersion and compatibility. Blends with varying dis-UH content up to 20 wt% show homogeneity, evidenced by DSC and SEM analysis, and demonstrate improved mechanical properties by 36 % in the maximum stress (σmax) and 39 % in Young's modulus (E). Linear viscoelasticity assessments reveal that higher dis-UH content slow the dynamics and increase the apparent weight average molecular weight (Mw), consistent with previous reports for linear entangled PE. The zero-shear viscosity (η0) scaling with Mw (η0∝Mn) is adjusted for high polydispersity, yielding a transitional point in the scaling exponent (n) from 3.6 to 3 at a reptation number of entanglement segments (Mr/Me) of ∼287, in line with theoretical predictions. To rationalize the success of the homogenization process, we propose a qualitative molecular picture inspired from the constraint release Rouse mechanism involved in the disorientation process of bi-disperse linear polymers. In the case of dis-UH/HDPE blends, with initially lower density of long-long entanglements within dis-UH, and the highest density of short-short entanglements within HDPE matrix, the formation of long-short entanglements between dis-UH and HDPE is facilitated, which results in successful homogenization process. In the contrary, the establishment of long-short entanglements in eUH/HDPE blends will require unwinding of the long-long entanglements, which holds a higher kinetic barrier compared to dis-UH/HDPE blends, leading to unsuccessful homogenization.

Stress-controlled medium-amplitude oscillatory shear (MAOStress) of PVA–Borax

We report the first-ever complete measurement of MAOStress material functions, which reveal that stress can be more fundamental than strain or strain rate for understanding linearity limits as a function of Deborah number. The material used is a canonical viscoelastic liquid with a single dominant relaxation time: polyvinyl alcohol (PVA) polymer solution cross-linked with tetrahydroborate (Borax) solution. We outline experimental limit lines and their dependence on geometry and test conditions. These MAOStress measurements enable us to observe the frequency dependence of the weakly nonlinear deviation as a function of stress amplitude. The observed features of MAOStress material functions are distinctly simpler than MAOStrain, where the frequency dependence is much more dramatic. The strain-stiffening transient network model was used to derive a model-informed normalization of the nonlinear material functions that accounts for their scaling with linear material properties. Moreover, we compare the frequency dependence of the critical stress, strain, and strain-rate for the linearity limit, which are rigorously computed from the MAOStress and MAOStrain material functions. While critical strain and strain-rate change by orders of magnitude throughout the Deborah number range, critical stress changes by a factor of about 2, showing that stress is a more fundamental measure of nonlinearity strength. This work extends the experimental accessibility of the weakly nonlinear regime to stress-controlled instruments and deformations, which reveal material physics beyond linear viscoelasticity but at conditions that are accessible to theory and detailed simulation.

Janus nanoparticles as efficient interface compatibilizer in blends of polylactide and elastomers: Importance of interfacial relaxation on toughening

For blending immiscible polymers, such as in the toughening modification of polylactide (PLA) via blending with rubbery materials, interfacial compatibilization is of great significance while the mechanism, especially the role of interfacial rheology, remains elusive. In this study, styrene-butadiene block copolymer elastomer (SBC) was employed to toughen PLA and a dumbbell-shaped Janus nanoparticle (JNP) consisting of polymethyl methacrylate and polystyrene spheres with equal size (∼80 nm) was used as the compatibilizer. Located at the interface, JNPs exhibited a great compatibilization efficiency in PLA/SBC blends, as demonstrated by the good morphology stabilization against droplet coalescence under static annealing and low shear flow conditions, as well as by the resistance against droplet breakup under high shear flow conditions. Moreover, as revealed from the linear viscoelasticity of JNP compatibilized blends, when JNP loading is more than 2 phr, aside from shape relaxation, an interfacial relaxation dominated by Marangoni stress was observed, indicating the possibility of particle redistribution on droplet surfaces. However, when loading is more than 4 phr, relaxations in the terminal zone no longer exist, implying the possible formation of a particle network on the droplet surface. This is consistent with the mechanical properties. The blend shows the greatest toughness at JNP loading around 3 phr, while the toughness is very poor when JNP loading is either too low or too high. This suggests interfacial relaxation to be crucial to guarantee a good toughening effect of SBC in PLA.

Sequence-encoded Spatiotemporal Dependence of Viscoelasticity of Protein Condensates Using Computational Microrheology.

Many biomolecular condensates act as viscoelastic complex fluids with distinct cellular functions. Deciphering the viscoelastic behavior of biomolecular condensates can provide insights into their spatiotemporal organization and physiological roles within cells. Though there is significant interest in defining the role of condensate dynamics and rheology in physiological functions, the quantification of their time-dependent viscoelastic properties is limited and mostly done through experimental rheological methods. Here, we demonstrate that a computational passive probe microrheology technique, coupled with continuum mechanics, can accurately characterize the linear viscoelasticity of condensates formed by intrinsically disordered proteins (IDPs). Using a transferable coarse-grained protein model, we first provide a physical basis for choosing optimal values that define the attributes of the probe particle, namely its size and interaction strength with the residues in an IDP chain. We show that the technique captures the sequence-dependent viscoelasticity of heteropolymeric IDPs that differ either in sequence charge patterning or sequence hydrophobicity. We also illustrate the technique's potential in quantifying the spatial dependence of viscoelasticity in heterogeneous IDP condensates. The computational microrheology technique has important implications for investigating the time-dependent rheology of complex biomolecular architectures, resulting in the sequence-rheology-function relationship for condensates.

RHEOLOGICAL PROPERTIES OF LOW-TEMPERATURE GEL-FORMING COMPOSITIONS

In this work, the rheological properties of low-temperature versions of gel-forming compositions developed at the IPC SB RAS are studied. A composition on an inorganic basis and a composition comprising a polymer and inorganic components are intended to increase oil recovery from low temperature reservoirs. The measurements were carried using a Haake Viscotester iQ rheometer with a CC25 coaxial cylinder measuring system in oscillatory mode with controlled strain at a frequency of 1 Hz. During the oscillation test, the dependences of the elastic modulus G' and the viscosity modulus G'' on the strain amplitude were recorded, the ranges of linear viscoelasticity of the samples under study were established, and the strain value for kinetic experiments was chosen. At a given strain value (0.01), the kinetic dependences of G' were obtained and the dynamics of the rheological properties and the strength of the formed structure were evaluated. The time of gelation onset has been found. It was 2300 s at 38 °C, 3900 s at 30 °C, and 21000 s at 20 °C for the inorganic composition and 200 s at 70 °C, 570 s at 60 °C, and 1920 s at 50 °C for the polymer-inorganic composition. The time required to form a gel of maximum strength also was found to be increased with increasing temperature. It has been established that for all systems under study the time of gel formation was reduced with increasing temperature, while the strength of the formed structure also increased. A slight increase in the maximum value of the modulus G' (33490 and 32805 Pa) was observed for the composition on an inorganic basis at 38 and 30 °C respectively as compared with the maximum of the dependence obtained at 20 °C (24660 Pa). The major increase in the value of the modulus G' has been recorded for the composition on a polymer-inorganic basis with increase in temperature. In this case the value of the modulus G' increased from 8970 Pa at 50 °C to 11680 Pa at 60 °C and 14590 Pa at 70 °C, while the general form of the rheokinetic dependence for different compositions and temperatures remained the same. For citation: Kozhevnikov I.S., Bogoslovskii А.V. Rheological properties of low-temperature gel-forming compositions. ChemChemTech [Izv. Vyssh. Uchebn. Zaved. Khim. Khim. Tekhnol.]. 2024. V. 67. N 8. P. 22-28. DOI: 10.6060/ivkkt.20246708.1t.

Effect of molecular structure on the dynamics and viscoelasticity of vitrimers

Vitrimers are a class of dynamic polymer networks that perform bond-exchange reactions (BERs) under environmental stimuli while preserving network connectivity. The viscoelastic properties of vitrimers are not only dependent on the kinetics of BERs, but also the architectures of polymer matrix. Here, we investigate the influence of polymer architectures on the dynamics and linear viscoelasticity of vitrimers through varying the sticker (reactive bead) distribution in the precursor chain and the BERs energy barrier (Ub) by performing hybrid molecular dynamics-Monte Carlo simulations. Increasing Ub, vitrimers with block and gradient distributions exhibit considerably faster relaxations of chain ends, Rouse mode, and stress and lower zero-shear viscosity than the analogs with random and uniform distributions, in qualitative agreement with the predictions of the sticky Rouse model. In contrast, the distribution of stickers has a small influence on the relaxation of dynamic bonds regardless of the Ub value. By comparing the molecular structures of vitrimers with different distributions of stickers, we find that the molecular defects, especially the relatively longer dangling end in block and gradient distributions, impair the effect of dynamic bonds on the dynamics and viscoelasticity of vitrimers. This suggests that the dangling defects can be leveraged for further development of recyclable and healable materials with fast stress relaxation and improved flowability.

Microstructures and Rheological Properties of Short-Side-Chain Perfluorosulfonic Acid in Water/2-Propanol.

The viscosity and viscoelasticity of polyelectrolyte solutions with a single electrostatic interaction have been carefully studied experimentally and theoretically. Despite some theoretical models describe experimental results well, the influence of multiple interactions (electrostatic and hydrophobic) on rheological scaling is not yet fully resolved. Herein, we systematically study the microstructures and rheological properties of short-side-chain perfluorosulfonic acid (S-PFSA), the most promising candidate of a proton exchange membrane composed of a hydrophobic backbone with hydrophilic side-chains, in water/2-propanol. Small-angle X-ray scattering confirms that semiflexible S-PFSA colloidal particles with a length of ~38 nm and a diameter of 1-1.3 nm are formed, and the concentration dependence of the correlation length (ξ) obeys the power law ξ~c-0.5 consistent with the prediction of Dobrynin et al. By combining macrorheology with diffusing wave spectroscopy microrheology, the semidilute unentangled, semidilute entangled, and concentrated regimes corresponding to the scaling relationships ηsp~c0.5, ηsp~c1.5, and ηsp~c4.1 are determined. The linear viscoelasticity indicates that the entanglement concentration (ce) obtained from the dependence of ηsp on the polymer concentration is underestimated owing to hydrophobic interaction. The true entanglement concentration (cte) is obtained by extrapolating the plateau modulus (Ge) to the terminal modulus (Gt). Furthermore, Ge and the plateau width, τr/τe (τr and τe denote reptation time and Rouse time), scale as Ge~c2.4 and τr/τe~c4.2, suggesting that S-PFSA dispersions behave like neutral polymer solutions in the concentrated regime. This work provides mechanistic insight into the rheological behavior of an S-PFSA dispersion, enabling quantitative control over the flow properties in the process of solution coating.

Complex viscosity and cohesive energy density of mixtures of sodium hyaluronate and hypromellose for medical devices

In the present study binary formulations of sodium hyaluronate (▪) and hypromellose (▪) were proposed as medical devices in the field of eye surgeries. Viscoelasticity is tested directly on binary solutions while the rheological behavior in the human eye is mimicked by monitoring the viscoelasticity of ternary mixtures ▪/▪/▪. Both binary and ternary formulations were rheologically characterized at 25∘C and 37∘C by means of measurements in the oscillatory regime. Amplitude sweep tests revealed that the range of linear viscoelasticity is strongly dependent on the concentration of ▪. For the proposed formulations, it was ascertained that the cohesive energy density at 37∘C decreases as ▪ concentration surges; in contrast, at 25∘C we detected an increase of cohesive energy were detected. At ▪ mass fraction of α1, the two obtained values were comparable. Frequency sweep tests revealed the pseudoplastic character of the binary formulations. In order to fit the complex viscosity modules, the Carreau-Yasuda model was modified. Numerical analysis of the results indicates that the best-fit to the model is obtained when the characteristic parameters take constant values, i.e. n=0 and m=1, regardless of the composition of the formulation. This implies that the modulus of complex viscosity decays hyperbolically. Frequency sweep tests on the ternary formulations were analyzed in terms of both the modulus of complex viscosity to confirm the previous scientific evidence together with an investigation of the phase shift angle between the viscous and elastic components. The results indicate that the addition of water has a different impact on the structure and the cohesion of the mixture at different temperatures. These results suggest that the ternary mixture structure can be sensitively modulated by temperature and the content of water.

Linking Chemical Structure to the Linear and Nonlinear Properties of Asphalt Binders

The study described in this paper aims to establish the relationship between the chemical composition and rheological properties of asphalt binders in both the linear viscoelastic (LVE) and nonlinear viscoelastic (NLVE) domains. Two asphalt binders with different penetration grades were subjected to four distinct aging treatments of varying severity, resulting in changes in their chemical fingerprints. Chemical characteristics of the asphalt binders were analyzed using thin-layer chromatography (TLC), Fourier Transform infrared spectroscopy (FTIR), and gel permeation chromatography (GPC). Frequency sweep tests were conducted to evaluate the LVE behavior of the asphalt binders, while multiple stress creep recovery (MSCR) tests were employed to assess their NLVE properties. With regard to the LVE properties, rheological index ( R) and zero shear viscosity (ZSV) derived from the Christensen-Anderson-Marasteanu (CAM) model exhibited high correlations with FTIR and molecular weight distribution (MWD) parameters. Additionally, the polydispersity index (PDI) displayed a stronger correlation with LVE-based parameters. Findings from the MSCR tests revealed that the sensitivity of the percentage recovery ( %R) to chemical composition, as opposed to nonrecoverable creep compliance ( Jnr), can be largely attributed to the degree of nonlinearity. Furthermore, it was observed that lower molecular weight molecules exert a greater influence on %R in the nonlinear domain. Finally, it was found that Jnrslope is a more reliable parameter than Jnrdiff for assessing the effects of chemical makeup on stress and temperature sensitivity.

On the linear viscoelastic behavior of semidilute polydisperse bubble suspensions in Newtonian media

In this work, we investigated the linear viscoelasticity of semidilute polydisperse bubble suspensions via small amplitude oscillatory shear (SAOS) tests performed in a rheo-optical setup. For all tested suspensions, the measured viscoelastic moduli (G′, G″) aligned with the theoretical predictions of the Jeffreys model for average dynamic capillary numbers (⟨Cd⟩) greater than unity. But at lower ⟨Cd⟩ values, experimental G′ values exceeded theoretical predictions. To investigate this, we considered the effects of suspension polydispersity and various SAOS measurement artifacts, including bubble rise, coalescence, and changes in suspension microstructure over time. Polydispersity could not cause the observed deviation, because the viscoelastic trends deviate from those of classic single-mode relaxation only for bimodal bubble size distributions with equal volume fractions of very small and very large bubbles; in any other case, the polydisperse suspension behaves as monodisperse with a bubble radius equal to the volume-weighted mean radius. Furthermore, bubble rise proved to play a minor role, while SAOS rheo-optical experiments revealed that bubble size and organization varied negligibly during our measurements. The G′ deviation at low ⟨Cd⟩ values was linked to bubble fluid dynamic interactions induced by the bubble spatial distribution. Image analysis showed that at low bubble volume fractions, stronger and prolonged preshearing reduces these interactions by increasing the average interbubble distance. But this effect is negligible in denser suspensions, which show similar G′ trends for any applied preshearing. Finally, a multimode Jeffreys model fitted to the experimental data showed that bubble interactions complicate the relaxation process, introducing multiple relaxation modes.

Scaling of the linear viscoelasticity of entangled poly(ethylene oxide) aqueous solutions

The dynamic modulus of polymer solutions and melts can be expressed as a universal function of reduced frequency when the modulus is scaled by a characteristic value according to the scaling theory of polymer physics. Although the plot of the scaled modulus as a function of the scaled frequency supports the theory, it suffers from considerable scattered distribution of data points around the hypothetical master curve. Compared with the master curve of the time–temperature superposition (TTS) of polymer melts, the master curve of polymer solutions has poor quality. Furthermore, the scale factors of polymer solutions may not show a clear dependency on molecular weight and concentrations. Experimental errors and molecular weight distribution appear to enhance the inaccuracy of the master curve. Therefore, we apply a global optimization for the superposition of the viscoelastic data of polymer solutions with various molecular weights and concentrations. The global optimization resulted in the superposition of data as accurate as that of TTS. Furthermore, the numerically determined shift factors, which were relative scale factors, showed clear dependences on molecular weight and concentrations. We compared our global optimization with previous scaling methodologies.

Impact of Sacrificial Hydrogen Bonds on the Structure and Properties of Rubber Materials: Insights from All-Atom Molecular Dynamics Simulations.

The inclusion of sacrificial hydrogen bonds is crucial for advancing high-performance rubber materials. However, the molecular mechanisms governing the impact of these bonds on material properties remain unclear, hindering progress in advanced rubber material research. This study employed all-atom molecular dynamics simulations to thoroughly investigate how hydrogen bonds affect the structure, dynamics, mechanics, and linear viscoelasticity of rubber materials. As the modified repeating unit ratio (β) increased, both interchain and intrachain hydrogen bond content rose, with interchain bonds playing a predominant role. This physical cross-linking network formed through interchain hydrogen bonds restricts molecular chain movement and relaxation and raises the glass transition temperature of rubber. Within a certain content of hydrogen bonds, the mechanical strength increases with increasing β. However, further increasing β leads to a subsequent decrease in the mechanical performance. Optimal mechanical properties were observed at β = 6%. On the other hand, a higher β value yields an elevated stress relaxation modulus and an extended stress relaxation plateau, signifying a more complex hydrogen-bond cross-linking network. Additionally, higher β increases the storage modulus, loss modulus, and complex viscosity while reducing the loss factor. In summary, this study successfully established the relationship between the structure and properties of natural rubber containing hydrogen bonds, providing a scientific foundation for the design of high-performance rubber materials.