Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative Aging

A micromechanical concept of filler-induced stress-softening and hysteresis is established that describes the complex quasi-static deformation behavior of filler reinforced rubbers upon repeated stretching with increasing amplitude. It is based on a non-affine tube model of rubber elasticity and a d...

Full description

Bibliographic Details
Main Authors: Jan Plagge, Manfred Klüppel
Format: Article
Language:English
Published: MDPI AG 2020-06-01
Series:Polymers
Subjects:
Online Access:https://www.mdpi.com/2073-4360/12/6/1350
_version_ 1797565266700271616
author Jan Plagge
Manfred Klüppel
author_facet Jan Plagge
Manfred Klüppel
author_sort Jan Plagge
collection DOAJ
description A micromechanical concept of filler-induced stress-softening and hysteresis is established that describes the complex quasi-static deformation behavior of filler reinforced rubbers upon repeated stretching with increasing amplitude. It is based on a non-affine tube model of rubber elasticity and a distinct deformation and fracture mechanics of filler clusters in the stress field of the rubber matrix. For the description of the clusters we refer to a three-dimensional generalization of the Kantor–Webman model of flexible chain aggregates with distinct bending–twisting and tension deformation of bonds. The bending–twisting deformation dominates the elasticity of filler clusters in elastomers while the tension deformation is assumed to be mainly responsible for fracture. The cluster mechanics is described in detail in the theoretical section, whereby two different fracture criteria of filler–filler bonds are considered, denoted “monodisperse” and “hierarchical” bond fracture mechanism. Both concepts are compared in the experimental section, where stress–strain cycles of a series of ethylene–propylene–diene rubber (EPDM) composites with various thermo-oxidative aging histories are evaluated. It is found that the “hierarchical” bond fracture mechanism delivers better fits and more stable fitting parameters, though the evolution of fitting parameters with aging time is similar for both models. From the adaptations it is concluded that the crosslinking density remains almost constant, indicating that the sulfur bridges in EPDM networks are mono-sulfidic, and hence, quite stable—even at 130 °C aging temperature. The hardening of the composites with increasing aging time is mainly attributed to the relaxation of filler–filler bonds, which results in an increased stiffness and strength of the bonds. Finally, a frame-independent simplified version of the stress-softening model is proposed that allows for an easy implementation into numerical codes for fast FEM simulations
first_indexed 2024-03-10T19:09:41Z
format Article
id doaj.art-f30eb8dd260b4177935ce3ef5d70b97d
institution Directory Open Access Journal
issn 2073-4360
language English
last_indexed 2024-03-10T19:09:41Z
publishDate 2020-06-01
publisher MDPI AG
record_format Article
series Polymers
spelling doaj.art-f30eb8dd260b4177935ce3ef5d70b97d2023-11-20T03:55:18ZengMDPI AGPolymers2073-43602020-06-01126135010.3390/polym12061350Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative AgingJan Plagge0Manfred Klüppel1Deutsches Institut für Kautschuktechnologie e. V., Eupener Str. 33, D-30519 Hannover, GermanyDeutsches Institut für Kautschuktechnologie e. V., Eupener Str. 33, D-30519 Hannover, GermanyA micromechanical concept of filler-induced stress-softening and hysteresis is established that describes the complex quasi-static deformation behavior of filler reinforced rubbers upon repeated stretching with increasing amplitude. It is based on a non-affine tube model of rubber elasticity and a distinct deformation and fracture mechanics of filler clusters in the stress field of the rubber matrix. For the description of the clusters we refer to a three-dimensional generalization of the Kantor–Webman model of flexible chain aggregates with distinct bending–twisting and tension deformation of bonds. The bending–twisting deformation dominates the elasticity of filler clusters in elastomers while the tension deformation is assumed to be mainly responsible for fracture. The cluster mechanics is described in detail in the theoretical section, whereby two different fracture criteria of filler–filler bonds are considered, denoted “monodisperse” and “hierarchical” bond fracture mechanism. Both concepts are compared in the experimental section, where stress–strain cycles of a series of ethylene–propylene–diene rubber (EPDM) composites with various thermo-oxidative aging histories are evaluated. It is found that the “hierarchical” bond fracture mechanism delivers better fits and more stable fitting parameters, though the evolution of fitting parameters with aging time is similar for both models. From the adaptations it is concluded that the crosslinking density remains almost constant, indicating that the sulfur bridges in EPDM networks are mono-sulfidic, and hence, quite stable—even at 130 °C aging temperature. The hardening of the composites with increasing aging time is mainly attributed to the relaxation of filler–filler bonds, which results in an increased stiffness and strength of the bonds. Finally, a frame-independent simplified version of the stress-softening model is proposed that allows for an easy implementation into numerical codes for fast FEM simulationshttps://www.mdpi.com/2073-4360/12/6/1350filled elastomersstress softeningfiller-induced hysteresiscluster mechanicsFEM simulation
spellingShingle Jan Plagge
Manfred Klüppel
Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative Aging
Polymers
filled elastomers
stress softening
filler-induced hysteresis
cluster mechanics
FEM simulation
title Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative Aging
title_full Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative Aging
title_fullStr Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative Aging
title_full_unstemmed Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative Aging
title_short Micromechanics of Stress-Softening and Hysteresis of Filler Reinforced Elastomers with Applications to Thermo-Oxidative Aging
title_sort micromechanics of stress softening and hysteresis of filler reinforced elastomers with applications to thermo oxidative aging
topic filled elastomers
stress softening
filler-induced hysteresis
cluster mechanics
FEM simulation
url https://www.mdpi.com/2073-4360/12/6/1350
work_keys_str_mv AT janplagge micromechanicsofstresssofteningandhysteresisoffillerreinforcedelastomerswithapplicationstothermooxidativeaging
AT manfredkluppel micromechanicsofstresssofteningandhysteresisoffillerreinforcedelastomerswithapplicationstothermooxidativeaging