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

Xuan-Yu Shi; Shi-Hao Sun; Li Yang; Jun Zhong; Xiao-Feng Yu; Zheng Xu; Min Zuo; Yi-Hu Song; Qiang Zheng

doi:10.1007/s10118-023-3025-0

Your Location：

Home >

Browse articles >

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

RESEARCH ARTICLE | Updated：2023-11-27

- Microstructure Evolution and Strain Softening of Carbon Black Filled Natural Rubber Vulcanizates
- Microstructure Evolution and Strain Softening of Carbon Black Filled Natural Rubber Vulcanizates
- 高分子科学（英文版） 2023年41卷第12期页码：1947-1957
- Affiliations：
  
  a.Ministry of Education, Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering, Zhejiang University, Hangzhou 310027, China
  b.Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030001, China
- Author bio：
  
  kezuomin@zju.edu.cn (M.Z.)
  zhengqiang@zju.edu.cn (Q.Z.)
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (Nos. 51790503, 52273084 and 51873181).;Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-023-3025-0.
- DOI：10.1007/s10118-023-3025-0
  中图分类号：
- 收稿：2023-04-28，
  
  修回：2023-6-19，
  
  录用：2023-7-3，
  
  网络首发：2023-08-22，
  
  纸质出版：2023-12-01
- Accepted：
Scan QR Code
Shi, X. Y.; Sun, S. H.; Yang, L.; Zhong, J.; Yu, X. F.; Xu, Z.; Zuo, M.; Song, Y. H.; Zheng, Q. Microstructure evolution and strain softening of carbon black filled natural rubber vulcanizates. Chinese J. Polym. Sci. 2023, 41, 1947–1957

Xuan-Yu Shi, Shi-Hao Sun, Li Yang, et al. Microstructure Evolution and Strain Softening of Carbon Black Filled Natural Rubber Vulcanizates[J]. Chinese Journal of Polymer Science, 2023, 41(12): 1947-1957.
Shi, X. Y.; Sun, S. H.; Yang, L.; Zhong, J.; Yu, X. F.; Xu, Z.; Zuo, M.; Song, Y. H.; Zheng, Q. Microstructure evolution and strain softening of carbon black filled natural rubber vulcanizates. Chinese J. Polym. Sci. 2023, 41, 1947–1957 DOI： 10.1007/s10118-023-3025-0.

Xuan-Yu Shi, Shi-Hao Sun, Li Yang, et al. Microstructure Evolution and Strain Softening of Carbon Black Filled Natural Rubber Vulcanizates[J]. Chinese Journal of Polymer Science, 2023, 41(12): 1947-1957. DOI： 10.1007/s10118-023-3025-0.

摘要

The Mullins effect is mainly dominated by the natural rubber (NR) matrix and the effect of carbon black (CB) phase is the strain amplification of NR viscoelasticity. Cyclic stretching may lead to the destruction of CB aggregates and the interface between CB and NR segments.

Abstract

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

Keywords

references

Murphy,W.N.Therationaluseofvulcanizablerubber. Am. J. Dent. Sci. 1891 , 25 ,124−128..

Yamashita,S.;Takahashi,S.Molecularmechanismsofnaturalrubberbiosynthesis. Annu. Rev. Biochem. 2020 , 89 ,821−851..

Song,Y.;Zheng,Q.Conceptsandconflictsinnanoparticlesreinforcementtopolymersbeyondhydrodynamics. Prog. Mater. Sci. 2016 , 84 ,1−58..

Song,Y.;Zheng,Q.A.Linearviscoelasticityofpolymermeltsfilledwithnano-sizedfillers. Polymer 2010 , 51 ,3262−3268..

Tan,Y.;Wang,L.;Xiao,J.;Zhang,X.;Wang,Y.;Liu,C.;Zhang,H.;Liu,C.;Xia,Y.;Sui,K.Synchronousenhancementandstabilizationofgrapheneoxideliquidcrystals:inductiveeffectofsodiumalginatesindifferentconcentrationzones. Polymer 2019 , 160 ,107−114..

vanBeilen,J.B.;Poirier,Y.Establishmentofnewcropsfortheproductionofnaturalrubber. Trends Biotechnol. 2007 , 25 ,522−529..

Liu,J.;Wu,S.;Tang,Z.;Lin,T.;Guo,B.;Huang,G.Newevidencedisclosedfornetworkinginnaturalrubberbydielectricrelaxationspectroscopy. Soft Matter 2015 , 11 ,2290−2299..

Wu,J.;Qu,W.;Huang,G.;Wang,S.;Huang,C.;Liu,H.Super-resolutionfluorescenceimagingofspatialorganizationofproteinsandlipidsinnaturalrubber. Biomacromolecules 2017 , 18 ,1705−1712..

Harwood,J.A.C.;Mullins,L.;Payne,A.R.Strssssofteninginnaturalrubbervulcanizates.2.stresssofteningeffectsinpuregumandfillerloadedrubbers. J. Appl. Polym. Sci. 1965 , 9 ,3011−3021..

Diani,J.;Fayolle,B.;Gilormini,P.AreviewontheMullinseffect. Eur. Polym. J. 2009 , 45 ,601−612..

Kakavas,P.A.Mechanicalpropertiesofbondedelastomerdiscssubjectedtotriaxialstress. J. Appl. Polym. Sci. 1996 , 59 ,251−261..

Merckel,Y.;Diani,J.;Brieu,M.;Caillard,J.ConstitutivemodelingoftheanisotropicbehaviorofMullinssoftenedfilledrubbers. Mech. Mater. 2013 , 57 ,30−41..

Payne,A.R.;Whittake.ReEffectofvulcanizationonlow-straindynamicpropertiesoffilledrubbers. J. Appl. Polym. Sci. 1972 , 16 ,1191−1212..

Song,Y.;Du,M.;Yang,H.;Zheng,Q.Structureandviscoelasticityofrubbermaterials. Acta Polymerica Sinica (inChinese) 2013 ,1115−1130..

Chazeau,L.;Brown,J.D.;Yanyo,L.C.;Sternstein,S.S.ModulusrecoverykineticsendotherinsightsintothePayneeffectforfilledelastomers. Polym. Compos. 2000 , 21 ,202−222..

Payne,A.R.Elasticityofcarbonblacknetworks. J. Colloid Sci. 1964 , 19 ,744−754..

Nagaraja,S.M.;Mujtaba,A.;Beiner,M.Quantificationofdifferentcontributionstodissipationinelastomernanoparticlecomposites. Polymer 2017 , 111 ,48−52..

Leblanc,J.L.Simplifiedmodelingcalculationstoenlightenthemechanicalproperties(modulus)ofcarbonblackfilleddienerubbercompounds. J. Appl. Polym. Sci. 2011 , 122 ,599−607..

Meier,J.G.;Klueppel,M.Carbonblacknetworkinginelastomersmonitoredbydynamicmechanicalanddielectricspectroscopy. Macromol. Mater. Eng. 2008 , 293 ,12−38..

Papon,A.;Merabia,S.;Guy,L.;Lequeux,F.;Montes,H.;Sotta,P.;Long,D.R.Uniquenonlinearbehaviorofnano-filledelastomers:fromtheonsetofstrainsofteningtolargeamplitudesheardeformations. Macromolecules 2012 , 45 ,2891−2904..

Majeste,J.;Vincent,F.Akineticmodelforsilica-filledrubberreinforcement. J. Rheol. 2015 , 59 ,405−427..

Clough,J.M.;Creton,C.;Craig,S.L.;Sijbesma,R.P.CovalentbondscissionintheMullinseffectofafilledelastomer:real-timevisualizationwithmechanoluminescence. Adv. Funct. Mater. 2016 , 26 ,9063−9074..

Stoeckelhuber,K.W.;Svistkov,A.S.;Pelevin,A.G.;Heinrich,G.Impactoffillersurfacemodificationonlargescalemechanicsofstyrenebutadiene/silicarubbercomposites. Macromolecules 2011 , 44 ,4366−4381..

Coquelle,E.;Bossis,G.Mullinseffectinelastomersfilledwithparticlesalignedbyamagneticfield. Int. J. Solids Struct. 2006 , 43 ,7659−7672..

Song,Y.;Zeng,L.;Zheng,Q.Reconsiderationoftherheologyofsilicafillednaturalrubbercompounds. J. Phys. Chem. B 2017 , 121 ,5867−5875..

Qian,D.;Meng,F.ModellingMullinseffectinducedbychaindelaminationandreattachment. Polymer 2021 , 222 ,123608..

Li,X.;Tian,C.;Li,H.;Liu,X.;Zhang,L.;Hong,S.;Ning,N.;Tian,M.Combinedeffectofvolumefractionsofnanofillersandfiller-polymerinteractionson3DmultiscaledispersionofnanofillerandPayneeffect. Compos. Part A-Appl. Sci. Manuf. 2022 , 152 ,106722..

Wang,S.;Chester,S.A.ModelingthermalrecoveryoftheMullinseffect. Mech. Mater. 2018 , 126 ,88−98..

Ma,C.;Ji,T.;Robertson,C.G.;Rajeshbabu,R.;Zhu,J.;Dong,Y.MolecularinsightintotheMullinseffect:irreversibledisentanglementofpolymerchainsrevealedbymoleculardynamicssimulations. Phys. Chem. Chem. Phys. 2017 , 19 ,19468−19477..

Song,Y.;Zheng,Q.Applicationoftwophasemodeltolineardynamicrheologyoffilledpolymermelts. Polymer 2011 , 52 ,6173−6179..

Li,Z.;Song,Y.;Zheng,Q.Payneeffectandweakovershootinrubbernanocomposites. Chinese J. Polym. Sci. 2022 , 40 ,85−92..

Shi,X.;Sun,S.;Zhao,A.;Zhang,H.;Zuo,M.;Song,Y.;Zheng,Q.InfluenceofcarbonblackonthePayneeffectoffillednaturalrubbercompounds. Compos. Sci. Technol. 2021 , 203 ,108586..

Song,Y.;Xu,Z.;Wang,W.;Zheng,Q.Payneeffectofcarbonblackfillednaturalrubbernanocomposites:Influencesofextraction,crosslinking,andswelling. J. Rheol. 2021 , 65 ,807−820..

Zhong,X.;Song,Y.;Zheng,Q.;Wang,W.InfluenceofcoagentsonPayneeffectofbutadienerubbervulcanizates. Polymer 2021 , 212 ,123298..

Xu,H.;Xia,X.;Hussain,M.;Song,Y.;Zheng,Q.Linearandnonlinearrheologicalbehaviorsofsilicafillednitrilebutadienerubber. Polymer 2018 , 156 ,222−227..

Yang,R.;Song,Y.;Zheng,Q.Payneeffectofsilica-filledstyrene-butadienerubber. Polymer 2017 , 116 ,304−313..

Hussain,M.;Yasin,S.;Akram,M.A.;Xu,H.;Song,Y.;Zheng,Q.Influenceofionicliquidsonstructureandrheologicalbehaviorsofsilica-filledbutadienerubber. Ind. Eng. Chem. Res. 2019 , 58 ,18205−18212..

Xu,Y.;Xu,H.;Zheng,Q.;Song,Y.Influenceofionicliquidsonrheologicalbehaviorsofpolyisoprenerubber/silicacompounds. Polymer 2019 , 183 ,121898..

Le,H.H.;Pham,T.;Henning,S.;Klehm,J.;Wiessner,S.;Stoeckelhuber,K.W.;Das,A.;Hoang,X.T.;Do,Q.K.;Wu,M.;Vennemann,N.;Heinrich,G.;Radusch,H.J.Formationandstabilityofcarbonnanotubenetworkinnaturalrubber:effectofnon-rubbercomponents. Polymer 2015 , 73 ,111−121..

Huang,M.;Tunnicliffe,L.B.;Zhuang,J.;Ren,W.;Yan,H.;Busfield,J.J.C.Strain-dependentdielectricbehaviorofcarbonblackreinforcednaturalrubber. Macromolecules 2016 , 49 ,2339−2347..

Steinhauser,D.;Moewes,M.;Klueppel,M.Carbonblacknetworkinginelastomersmonitoredbysimultaneousrheologicalanddielectricinvestigations. J. Phys. Condens. Matter 2016 , 28 ,495103..

Beutier,C.;David,L.;Sudre,G.;Cassagnau,P.;Heuillet,P.;Cantaloube,B.;Serghei,A.In-situcoupledmechanical/electricalinvestigationsofEPDM/CBcompositematerials:theelectricalsignatureofthemechanicalMullinseffect. Compos. Sci. Technol. 2022 , 218 ,109144..

Taniguchi,Y.;Mai,T.;Yamaguchi,M.;Tsunoda,K.;Urayama,K.InvestigatingmultiaxialMullinseffectofcarbon-black-reinforcedelastomersusingelectricalresistivitymeasurements. ACS Appl. Polym. Mater. 2022 , 4 ,1139−1149..

Zhao,A.;Shi,X.;Sun,S.;Zhang,H.;Zuo,M.;Song,Y.;Zheng,Q.InsightsintothePayneeffectofcarbonblackfilledstyrene-butadienerubbercompounds. Chinese J. Polym. Sci. 2021 , 39 ,81−90..

Holt,A.P.;Sangoro,J.R.;Wang,Y.Y.;Agapov,A.L.;Sokolov,A.P.Chainandsegmentaldynamicsofpoly(2-vinylpyridine)nanocomposites. Macromolecules 2013 , 46 ,4168−4173..

Flory,P.J.;Rehner,J.Statisticalmechanicsofcross-linkedpolymernetworks.II.Swelling. J. Chem. Phys. 1943 , 11 ,521−526..

Huneau,B.Strain-inducedcrystallizationofnaturalrubber:areviewofX-raydiffractioninvestigations. Rubber Chem. Technol. 2011 , 84 ,425−452..

Li,Z.;Xu,H.;Xia,X.;Song,Y.;Zheng,Q.EnergydissipationaccompanyingMullinseffectofnitrilebutadienerubber/carbonblacknanocomposites. Polymer 2019 , 171 ,106−114..

Li,Z.;Wen,F.;Hussain,M.;Song,Y.;Zheng,Q.ScalinglawsofMullinseffectinnitrilebutadienerubbernanocomposites. Polymer 2020 , 193 ,122350..

Hou,F.;Song,Y.;Zheng,Q.Influenceofliquidisoprenerubberonstrainsofteningofcarbonblackfilledisoprenerubbernanocomposites. Chinese J. Polym. Sci. 2021 , 39 ,887−895..

Song,Y.;Zheng,Q.Aguideforhydrodynamicreinforcementeffectinnanoparticle-filledpolymers. Crit. Rev. Solid State Mat. Sci. 2016 , 41 ,318−346..

Hu,Z.;Zhou,J.;Song,Y.;Zheng,Q.;Wang,W.Strainsofteningofnaturalrubbercompositesfilledwithcarbonblackandaramidfiber. J. Rheol. 2023 , 67 ,157−168..

Perez-Aparicio,R.;Vieyres,A.;Albouy,P.;Sanseau,O.;Vanel,L.;Long,D.R.;Sotta,P.Reinforcementinnaturalrubberelastomernanocomposites:breakdownofentropicelasticity. Macromolecules 2013 , 46 ,8964−8972..

Aranguren,M.I.;Mora,E.;Degroot,J.V.;Macosko,C.W.Effectofreinforcingfillersontherheologyofpolymermelts. J. Rheol. 1992 , 36 ,1165−1182..

Nasr,G.M.Vulcanizationconditions:HowtheyaffecttheelectricalconductivityofSBRloadedwiththepercolationconcentrationofFEF-black. Polym. Test. 1996 , 15 ,585−591..

Li,B.;You,W.;Peng,L.;Huang,X.;Yu,W.Revealingthesheareffectontheinterfaciallayerinpolymernanocompositesthroughnanofiberreorientation. Macromolecules 2023 , 56 ,3050−3063..

Kluppel,M.;Schramm,J.Ageneralizedtubemodelofrubberelasticityandstresssofteningoffillerreinforcedelastomersystems. Macromol. Theor. Simul. 2000 , 9 ,742−754..

Suzuki,N.;Ito,M.;Yatsuyanagi,F.Effectsofrubber/fillerinteractionsondeformationbehaviorofsilicafilledSBRsystems. Polymer 2005 , 46 ,193−201..

Wolff,S.;Wang,M.J.;Tan,E.H.Fillerelastomerinteractions.7.studyonboundrubber. Rubber Chem. Technol. 1993 , 66 ,163−177..

浏览量

223

Downloads

CSCD

文章被引用时，请邮件提醒。

Submit

工具集

关联资源

Influence of Antioxidants and Deep Eutectic Solvent on Vulcanization Kinetics and Mechanical Behaviors of Natural Rubber/Styrene-Butadiene Rubber Blend and Composites

Structural Optimization of Polyimide Foam via Composition with Hyperbranched Polymer Modified Fluorinated Carbon Nanotubes

Sliding Dynamics of Ring Chain on a Rod-Coil Block Copolymer in Rotaxane

Porous Organic Polymers for Photocatalytic Hydrogen Peroxide Production: Recent Advances and Future Perspectives

Upgrading Commercially Available Polyethylene to High-value Materials with Strong Mechanical Performance and Hydrophilicity by Blending with Ethylene/meta-Methoxystyrene Copolymers