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A Review on the mullins effect in Tough Elastomers and Gels

Acta Mechanica Solida Sinica 2024年第2期37卷 181-214页

作者： Lin Zhan Shaoxing Qu Rui Xiao MOE Key Lab of Disaster Forecast and Control in Engineering College of Mechanics and Construction EngineeringJinan UniversityGuangzhou510632China State Key Laboratory of Fluid Power and Mechatronic System Key Laboratory of Soft Machines and Smart Devices of Zhejiang ProvinceDepartment of Engineering MechanicsZhejiang UniversityHangzhou310027China

Tough elastomers and gels have garnered broad research interest due to their wide-ranging potential applications.However,during the loading and unloading cycles,a clear stress softening behavior can be observed in many material systems,which is also named as the mullins effect.In this work,we aim to provide a complete review of the mullins effect in soft yet tough materials,specifically focusing on nanocomposite gels,double-network hydrogels,and multi-network elastomers.We first revisit the experimental observations for these soft materials.We then discuss the recent developments of constitutive models,emphasizing novel developments in the damage mechanisms or network representations.Some phenomenological models will also be briefly introduced.Particular attention is then placed on the anisotropic and multiaxial modeling aspects.It is demonstrated that most of the existing models fail to accurately predict the multiaxial data,posing a significant challenge for developing future anisotropic models tailored for tough gels and elastomers.

关键词： mullins effect Double-network hydrogels Nanocomposite gels Multi-network elastomers Anisotropic damage model Multiaxial model

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A Microstructural Damage Model toward Simulating the mullins effect in Double-Network Hydrogels

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Acta Mechanica Solida Sinica 2022年第4期35卷 682-693页

作者： Lin Zhan Rui Xiao State Key Laboratory of Fluid Power and Mechatronic System Key Laboratory of Soft Machines and Smart Devices of Zhejiang ProvinceDepartment of Engineering MechanicsZhejiang UniversityHangzhou310027China

The damage models based on the eight-chain model and the affine full-chain network model are not adequate to describe the damage behaviors in double-network(DN)hydrogels.To overcome this limitation,we propose a combined chain stretch model with new damage flow rules.It is demonstrated that the new proposed micro-chain stretch is a reduced form of the complete representation for the transversely isotropic tensor function.As a result,the damage models based on the eight-chain model and the affine model are incorporated as special cases.The effects of chain affineness and network entangling are simultaneously involved in the new model,while only one of these two effects can be characterized in either the eight-chain model or the affine model.It is further shown that the new model can effectively capture the mullins features of the DN hydrogels and achieve better agreement with the experimental data than the affine model and the eight-chain model.

关键词： mullins effect Double-network hydrogel Full-network model Microstructural model

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Microstructure Evolution and Strain Softening of Carbon Black Filled Natural Rubber Vulcanizates

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Chinese Journal of Polymer Science 2023年第12期41卷 1947-1957,I0010页

作者： Xuan-Yu Shi Shi-Hao Sun Li Yang Jun Zhong Xiao-Feng Yu Zheng Xu Min Zuo Yi-Hu Song Qiang Zheng Ministry of Education Key Laboratory of Macromolecular Synthesis and FunctionalizationDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan 030001China

Incorporation of carbon black(CB)in natural rubber(NR)enhances the mullins effect and Payne effect of their vulcanizates,but the strain softening mechanisms and the microstructure evolution in the vulcanizates have not been clearly concluded so far.We investigate the mullins effect and Payne effect of CB filled NR vulcanizates by using cyclic tensile tests at different temperatures and dynamic rheological measurements combined with simultaneous electric conduction.During cyclic stretching,the normalized recovery hysteresis energy and accumulative softening energy for NR/CB vulcanizates with different loadings can be both superimposed on a master curve,indicating that the mullins effect is mainly dominated by the rubber matrix.The irreversible simultaneous resistance evolution also reveals that the structural evolution of nanoparticles(NPs)network is not directly related to the mullins effect.Moreover,the extension of linear viscoelastic region and the hysteresis of Payne effect for filled vulcanizates subjected to cyclic stretching indicate the destruction of CB aggregated structure and the interfacial layers between CB and rubber chains during cyclic stretching.This investigation would be illuminating for the microstructure evolution and strain softening of rubber nanocomposites under harsh service conditions.

关键词： mullins effect Payne effect Conductive connected network Nanocomposites

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Energy dissipation in the mullins effect of NBR vulcanizate

Energy dissipation in the Mullins effect of NBR vulcanizate

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中国化学会第12届复杂流体流变学学术研讨会

作者： Zhiyun Li YH Song Qiang Zheng Department of Polymer Science and Engineering University of Zhejiang

The mullins effect of filled vulcanizates has attracted wide attention for its use to reflect the mechanical property during cyclic deformations.However,the mechanisms of this effect are still ambiguous.In this work,we divide the dissipation energy generated during constant-velocity cyclic deformations of filled NBR vulcanizates into a reversible and an irreversible loss part and quantitatively analyze the change of dissipation energy and its recovery with respect to crosslinking degree of the rubber phase and content of carbon black.The results show that（1） the reversible energy loss can be superposed well onto a master curve determined by the microscopic strain of the rubber phase,suggesting a cause involving in the friction of free chains dangling from the rubber network;（2） the irreversible part is related to both the microscopic strain of the rubber phase and the content of carbon black,revealing a secondary origination from the filler and interface;（3） the energy dissipation in the first stretch can basically recover after a long time conditioning of the stretched vulcanizates,revealing that the energy dissipation is essentially related to the viscoelastic deformation of the rubber phase in the vulcanizates.

关键词： mullins effect Energy dissipation

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Tough and tunable adhesion of hydrogels:experiments and models

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Acta Mechanica Sinica 2017年第3期33卷 543-554页

作者： Teng Zhang Hyunwoo Yuk Shaoting Lin German A.Parada Xuanhe Zhao Department of Mechanical and Aerospace Engineering Syracuse University Soft Active Materials Laboratory Department of Mechanical Engineering Massachusetts Institute of Technology Department of Civil and Environmental Engineering Massachusetts Institute of Technology

As polymer networks infiltrated with water, hydrogels are major constituents of animal and plant bodies and have diverse engineering applications. While natural hydrogels can robustly adhere to other biological materials, such as bonding of tendons and cartilage on bones and adhesive plaques of mussels, it is challenging to achieve such tough adhesions between synthetic hydrogels and engineering materials. Recent experiments show that chemically anchoring long-chain polymer networks of tough synthetic hydrogels on solid surfaces create adhesions tougher than their natural counterparts, but the underlying mechanism has not been well understood. It is also challenging to tune systematically the adhesion of hydrogels on solids. Here, we provide a quantitative understanding of the mechanism for tough adhesions of hydrogels on solid materials via a combination of experiments, theory, and numerical simulations. Using a coupled cohesive-zone and mullins-effect model validated by experiments, we reveal the interplays of intrinsic work of adhesion, interfacial strength, and energy dissipation in bulk hydrogels in order to achieve tough adhesions. We further show that hydrogel adhesion can be systematically tuned by tailoring the hydrogel geometry and silanization time of solid substrates, corresponding to the control of energy dissipation zone and intrinsic work of adhesion, respectively. The current work further provides a theoretical foundation for rational design of future biocompatible and underwater adhesives.

关键词： Adhesion Hydrogels Soft materials mullins effect

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Modeling the Damage and Self-healing Behaviors of Plasticized PVC Gels

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Acta Mechanica Solida Sinica 2021年第4期34卷 466-476页

作者： Ninghan Tang Dong Lei Ji Lin Yanjie Wang Rui Xiao College of Mechanics and Materials Hohai UniversityNanjing211100China Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province Department of Engineering MechanicsZhejiang UniversityHangzhou310027China School of Mechanical and Electrical Engineering Hohai UniversityChangzhou CampusChangzhou213022China

Plasticized polyvinyl chloride(PVC)gel is a type of electroactive polymers,which has potentials to be applied as soft actuators.However,few studies have been performed to investigate the mechanical responses of PVC gels in cyclic loading conditions.In this work,we combined experiments and theory to characterize the mechanical responses of two plasticized PVC gels.The gels were subjected to different types of loading-unloading-reloading cycles.The experimental results showed that the plasticized PVC gels exhibited stress softening response(the mullins effect)in the cyclic tests.Meanwhile,the gels regained some strength after annealing at room temperature for several hours,indicating the self-healing ability of gels.We further extended the eight-chain model with incorporation of the chain dissociation and reassociation mechanism.The developed constitutive model is able to reproduce the mullins effect and the recovery of the mullins effect observed in the experiments.Our results clearly show that understanding the complex mechanical response is crucial for the applications of plasticized PVC gels.

关键词： PVC gels mullins effect Electroactive polymers Self-healing Modeling

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