High-temperature Thermo-oxidative Aging of Vulcanized Natural Rubber Nanocomposites: Evolution of Microstructure and Mechanical Properties

Zhou-Xian Li; Yi-Ran Kong; Xiang-Fei Chen; Ya-Jiang Huang; Ya-Dong Lv; Guang-Xian Li

doi:10.1007/s10118-023-2948-9

Your Location：

Home >

Browse articles >

High-temperature Thermo-oxidative Aging of Vulcanized Natural Rubber Nanocomposites: Evolution of Microstructure and Mechanical Properties

RESEARCH ARTICLE | Updated：2023-07-18

- High-temperature Thermo-oxidative Aging of Vulcanized Natural Rubber Nanocomposites: Evolution of Microstructure and Mechanical Properties
- Chinese Journal of Polymer Science Vol. 41, Issue 8, Pages: 1287-1297(2023)
- Affiliations：
  
  College of polymer science and engineering, State key laboratory of polymer materials engineering of China, Sichuan University, Chengdu 610065, China
- Author bio：
  
  hyj@scu.edu.cn (Y.J.H.)
  guangxianli@scu.edu.cn (G.X.L.)
- Funds：
- DOI：10.1007/s10118-023-2948-9
  CLC：
- Received：10 November 2022，
  
  Revised：2022-12-20，
  
  Accepted：05 January 2023，
  
  Online First：10 March 2023，
  
  Published：01 August 2023
- Accepted：
Scan QR Code
Li, Z. X.; Kong, Y. R.; Chen, X. F.; Huang, Y. J.; Lv, Y. D.; Li, G. X. High-temperature thermo-oxidative aging of vulcanized natural rubber nanocomposites: evolution of microstructure and mechanical properties. Chinese J. Polym. Sci. 2023, 41, 1287–1297

Zhou-Xian Li, Yi-Ran Kong, Xiang-Fei Chen, et al. High-temperature Thermo-oxidative Aging of Vulcanized Natural Rubber Nanocomposites: Evolution of Microstructure and Mechanical Properties[J]. Chinese Journal of Polymer Science, 2023, 41(8): 1287-1297.
Li, Z. X.; Kong, Y. R.; Chen, X. F.; Huang, Y. J.; Lv, Y. D.; Li, G. X. High-temperature thermo-oxidative aging of vulcanized natural rubber nanocomposites: evolution of microstructure and mechanical properties. Chinese J. Polym. Sci. 2023, 41, 1287–1297 DOI： 10.1007/s10118-023-2948-9.

Zhou-Xian Li, Yi-Ran Kong, Xiang-Fei Chen, et al. High-temperature Thermo-oxidative Aging of Vulcanized Natural Rubber Nanocomposites: Evolution of Microstructure and Mechanical Properties[J]. Chinese Journal of Polymer Science, 2023, 41(8): 1287-1297. DOI： 10.1007/s10118-023-2948-9.

摘要

Abstract

The aging of natural rubber (NR) at high temperatures will seriously affect its service lifetime in many key applications. In the present work

the changes in microstructure and mechanical properties of semi-efficient vulcanized NR/carbon black (CB) vulcanizates during thermo-oxidative aging at high temperatures (150−200 °C) and a moderate temperature (95 °C) were compared. At high temperatures

a two-stage aging behavior

which was characteristic of a first rapid decline and then a continuous rise in the crosslinking density (

)

was identified and was found to be closely related to the depletion behavior of antioxidants. The surface cracking behavior observed in the second stage of high-temperature aging was discussed in terms of the grafting reaction of macromolecular radicals on CB particles and thermal expansion. In contrast

the aging of NR at moderate temperatures was much mild

which featured a continuous increase in

and an oxidation mechanism dominated by peroxy radicals attacking double bonds. In general

the mechanical properties of NR vulcanizates during high-temperature aging depended on the competition effects of structural evolution in the crosslinked network and oxidation-induced chain scission.

关键词

Keywords

references

Tabsan,N.;Wirasate,S.;Suchiva,K.Abrasionbehavioroflayeredsilicatereinforcednaturalrubber. Wear 2010 , 269 ,394−404..

Chen,Q.;Zhang,Z.;Huang,Y.;Zhao,H.;Chen,Z.;Gao,K.;Yue,T.;Zhang,L.;Liu,J.Structure-mechanicsrelationofnaturalrubber:insightsfrommoleculardynamicssimulations. ACS Appl. Polym. Mater. 2022 , 4 ,3575−3586..

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

Grasland,F.;Chazeau,L.;Chenal,J.M.Aboutthermo-oxidativeageingatmoderatetemperatureofconventionallyvulcanizednaturalrubber. Polym. Degrad. Stabil. 2019 , 161 ,74−84..

Lee,Y.H.;Cho,M.;Nam,J.D.;Lee,Y.EffectofZnOparticlesizesonthermalagingbehaviorofnaturalrubbervulcanizates. Polym. Degrad. Stabil. 2018 , 148 ,50−55..

Zhang,Z.;Sun,J.;Lai,Y.;Wang,Y.;Liu,X.;Shi,S.;Chen,X.Effectsofthermalagingonuniaxialratchetingbehaviorofvulcanisednaturalrubber. Polym. Test. 2018 , 70 ,102−110..

Datta,R.;Huntink,N.;Datta,S.;Talma,A.Rubbervulcanizatesdegradationandstabilization. Rubber. Chem. Technol. 2007 , 80 ,436−480..

Howse,S.;Porter,C.;Mengistu,T.;Petrov,I.;Pazur,R.J.Experimentaldeterminationofthequantityanddistributionofchemicalcrosslinksinunagedandagednaturalrubber.II:Asulfurdonorsystem. Rubber. Chem. Technol. 2019 , 92 ,513−530..

Zheng,W.;Liu,L.;Zhao,X.;He,J.;Wang,A.;Chan,T.W.;Wu,S.Effectsoflanthanumcomplexonthethermo-oxidativeagingofnaturalrubber. Polym. Degrad. Stabil. 2015 , 120 ,377−383..

Choi,S.S.;Kim,E.Anovelsystemformeasurementoftypesanddensitiesofsulfurcrosslinksofafilledrubbervulcanizate. Polym. Test. 2015 , 42 ,62−68..

Sun,Y.;Huang,J.;He,J.;Tang,Z.;Zhu,L.;Liu,F.Effectsofanovelhinderedphenolsamariumcomplexonthethermo-oxidativeagingofstyrene-butadienerubber/silicacomposites. Polym. Degrad. Stabil. 2021 , 185 ,109482..

Colin,X.;Audouin,L.;Verdu,J.Kineticmodellingofthethermaloxidationofpolyisopreneelastomers.Part3:Oxidationinducedchangesofelasticproperties. Polym. Degrad. Stabil. 2007 , 92 ,906−914..

Li,G.Y.;Koenig,J.L.Areviewofrubberoxidation. Rubber. Chem. Technol. 2005 , 78 ,355−390..

Alroqi,A.A.;Wang,W.;Zhao,Y.Aircrafttiretemperatureattouchdownwithwheelprerotation. J. Aircraft. 2016 , 54 ,926−938..

Chen,X.;Kong,Y.;Wang,M.;Huang,X.;Huang,Y.;Lv,Y.;Li,G.Wearandagingbehaviorofvulcanizednaturalrubbernanocompositesunderhigh-speedandhigh-loadslidingwearconditions. Wear 2022 , 498 ,204341..

Valentín,J.L.;Mora-Barrantes,I.;Carretero-González,J.;López-Manchado,M.A.;Sotta,P.;Long,D.R.;Saalwächter,K.Novelexperimentalapproachtoevaluatefiller-elastomerinteractions. Macromolecules 2010 , 43 ,334−346..

Wang,M.;Wang,R.;Chen,X.;Kong,Y.;Huang,Y.;Lv,Y.;Li,G.Effectofnon-rubbercomponentsonthecrosslinkingstructureandthermo-oxidativedegradationofnaturalrubber. Polym. Degrad. Stabil. 2022 , 196 ,109845..

Ghosh,P.;Katare,S.;Patkar,P.;Caruthers,J.M.;Venkatasubramanian,V.;Walker,K.A.Sulfurvulcanizationofnaturalrubberforbenzothiazoleacceleratedformulations:fromreactionmechanismstoarationalkineticmodel. Rubber. Chem. Technol. 2003 , 76 ,592−693..

Fu,D.H.;Zhan,Y.H.;Yan,N.;Xia,H.S.Acomparativeinvestigationonstraininducedcrystallizationforgrapheneandcarbonnanotubesfillednaturalrubbercomposites. Express Polym. Lett. 2015 , 9 ,597−607..

Li,Y.;Liu,X.;Hu,X.;Luo,W.Changesintensileandtearingfracturepropertiesofcarbon-blackfilledrubbervulcanizatesbythermalaging. Polym. Adv. Technol. 2015 , 26 ,1331−1335..

Huang,M.;Lu,J.;Han,B.;Qiu,M.;Zhang,L.Covalentgraftingapproachforimprovingthedispersionofcarbonblackinstyrene-butadienerubbercompositesbycopolymerizing p -(2,2’-diphenylethyl)styrenewithathermallydecomposedtriphenylethanependant. Ind. Eng. Chem. Res. 2016 , 55 ,9459−9467..

Jamroż,M.;Kozłowski,K.;Sieniakowski,M.;Jachym,B.UseofESRtoinvestigateformationoffreeradicalsoncompoundingrubberswithcarbonblacks. J. Polym. Sci., Part A: Polym. Chem. 1977 , 15 ,1359−1367..

Luo,K.;You,G.;Zhao,X.;Lu,L.;Wang,W.;Wu,S.Synergisticeffectsofantioxidantandsilicaonenhancingthermo-oxidativeresistanceofnaturalrubber:Insightsfromexperimentsandmolecularsimulations. Mater. Design. 2019 , 181 ,107944..

Yurekli,K.;Krishnamoorti,R.;Tse,M.;McElrath,K.;Tsou,A.;Wang,H.C.Structureanddynamicsofcarbonblack-filledelastomers. J. Polym. Sci., Part B: Polym. Phys. 2001 , 39 ,256−275..

Schwartz,G.A.;Cerveny,S.;Marzocca,Á.J.;Gerspacher,M.;Nikiel,L.Thermalagingofcarbonblackfilledrubbercompounds.I.Experimentalevidenceforbridgingflocculation. Polymer 2003 , 44 ,7229−7240..

Xu,Z.;Song,Y.;Zheng,Q.Payneeffectofcarbonblackfillednaturalrubbercompoundsandtheircarbonblackgels. Polymer 2019 , 185 ,121953..

Thajudin,N.L.N.;Zainol,M.H.;Shuib,R.K.Intrinsicroomtemperatureself-healingnaturalrubberbasedonmetalthiolateionicnetwork. Polym. Test. 2021 , 93 ,106975..

Naskar,K.;Kokot,D.;Noordermeer,J.Influenceofvariousstabilizersonageingofdicumylperoxide-curedpolypropylene/ethylene-propylene-dienethermoplasticvulcanizates. Polym. Degrad. Stabil. 2004 , 85 (2),831−839..

Edge,M.;Allen,N.S.;Gonzalez-Sanchez,R.;Liauw,C.M.;Read,S.J.;Whitehouse,R.B.TheinfluenceofcureandcarbonblackonthehightemperatureoxidationofnaturalrubberI.Correlationofphysico-chemicalchanges. Polym. Degrad. Stabil. 1999 , 64 ,197−205..

Chaikumpollert,O.;Sae-Heng,K.;Wakisaka,O.;Mase,A.;Yamamoto,Y.;Kawahara,S.Lowtemperaturedegradationandcharacterizationofnaturalrubber. Polym. Degrad. Stabil. 2011 , 96 ,1989−1995..

Zhuo,W.Y.;Wang,Q.L.;Li,G.;Yang,G.;Zhang,H.;Xu,W.;Niu,Y.H.;Li,G.X.Detectionofthedestructionmechanismofperfluorinatedelastomer(FFKM)networkunderthermo-oxidativeagingconditions. Chinese J. Polym. Sci. 2022 , 40 ,504−514..

Do,T.-T.;Celina,M.;Fredericks,P.M.Attenuatedtotalreflectanceinfraredmicrospectroscopyofagedcarbon-filledrubbers. Polym. Degrad. Stabil. 2002 , 77 ,417−422..

Song,P.;Wan,C.;Xie,Y.;Zhang,Z.;Wang,S.Stepwiseexfoliationofboundrubberfromcarbonblacknanoparticlesandthestructurecharacterization. Polym. Test. 2018 , 71 ,115−124..

Colin,X.;Audouin,L.;Verdu,J.Kineticmodellingofthethermaloxidationofpolyisopreneelastomers.Part1:Unvulcanizedunstabilizedpolyisoprene. Polym. Degrad. Stabil. 2007 , 92 ,886−897..

Jordan,M.Interfacesincomposites.reinforcementofelastomersbycarbonblack. J. Macromol. Sci. A 1974 , 8 ,579−592..

Dong,R.;Zhao,M.;Xia,W.;Yi,X.;Dai,P.;Tang,N.Chemicalandmicroscopicinvestigationofco-pyrolysisofcrumbtirerubberwithwastecookingoilatmildtemperature. Waste. Manage. 2018 , 79 ,516−525..

Kilbane,J.J.Desulfurizationofcoal:themicrobialsolution. Trends. Biotechnol. 1989 , 7 ,97−101..

Candau,N.;Laghmach,R.;Chazeau,L.;Chenal,J.M.;Gauthier,C.;Biben,T.;Munch,E.Strain-inducedcrystallizationofnaturalrubberandcross-linkdensitiesheterogeneities. Macromolecules 2014 , 47 ,5815−5824..

Tomer,N.S.;Delor-Jestin,F.;Singh,R.P.;Lacoste,J.Cross-linkingassessmentafteracceleratedageingofethylenepropylenedienemonomerrubber. Polym. Degrad. Stabil. 2007 , 92 ,457−463..

Candau,N.;Oguz,O.;Peuvrel-Disdier,E.;Bouvard,J.L.;Pradille,C.;Billon,N.Strain-inducednetworkchainsdamageincarbonblackfilledEPDM. Polymer 2019 , 175 ,329−338..

Baba,M.;Nedelec,J.;Lacoste,J.;Gardette,J.;Morel,M.Crosslinkingofelastomersresultingfromageing:useofthermoporosimetrytocharacterisethepolymericnetworkwithn-heptaneascondensate. Polym. Degrad. Stabil. 2003 , 80 ,305−313..

Baba,M.;Gardette,J.L.;Lacoste,J.CrosslinkingonageingofelastomersII.Comparisonofsolventfreezingpointdepressionandconventionalcrosslinkingevaluation. Polym. Degrad. Stabil. 1999 , 65 ,415−420..

Views

611

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Bismaleimide Dielectric Films with Superior High-temperature Breakdown Strength via a Rationally Designed Crosslinked Network for Embedded Film Capacitors

Achieving High Energy Density at 200 °C in All-organic Polyimide Dielectrics Enabled by an Ultra-low Loading Multifunctional Porphyrin Crosslinker

Dipolar Glass Polymers for Capacitive Energy Storage at Room Temperatures and Elevated Temperatures

Silk Sericin-inspired Poly-β-homoserine for Protein Protection

Alternating Poly(ether-alt-ester)s with High Glass Transition Temperature Enabled by Rotationally Constrained Biaryl Units

Related Author

Qi-Yan Zhang

Li-Na Huang

Li Tan

Shuang-Wu Huang

Gu-Qiao Ding

Jun Zhang

Nan Hai

Peng Wu

Related Institution

State Key Laboratory of Radio Frequency Heterogeneous Integration, College of Electronics and Information Engineering, Institute of Microelectronics (IME), Shenzhen University

State Key Laboratory of Materials for Integrated Circuits, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences

School of Chemistry and Chemical Engineering, Ningxia University

National and Local Joint Engineering Laboratory for Synthetic Technology of High-Performance Polymer, Jilin University

Aerospace Research Institute of Materials & Processing Technology

⁰