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SubmittedManuscript:Confidential
1Title:Reversiblefusionandfissionofgrapheneoxidebasedfibers
2Authors:DanChang1,JingranLiu2,BoFang1,ZhenXu1,ZhengLi1*,YilunLiu2*,Laurence
3Brassart3,FanGuo1,WeiweiGao1&ChaoGao1*
4Affiliations:
51MOEKeyLaboratoryofMacromolecularSynthesisandFunctionalization,Departmentof
6PolymerScienceandEngineering,KeyLaboratoryofAdsorptionandSeparationMaterials&
7TechnologiesofZhejiangProvince,ZhejiangUniversity,38ZhedaRoad,Hangzhou310027,
8China.
92StateKeyLaboratoryforStrengthandVibrationofMechanicalStructures,Schoolof
10Aerospace,Xi’anJiaotongUniversity,Xi’an710049,China.
113DepartmentofMaterialsScienceandEngineering,MonashUniversity,ClaytonVictoria3800,
,UniversityofOxford,OxfordOX13PJ,
13UnitedKingdom.
14*:lizheng_******@(.);******@
15(.);******@(.)
16
17Abstract:
18Stimuli-responsivefusionandfissionarewidelyobservedinbothbio-organizationsand
,thedesignofasystemwithstructureandproperty
21andfissionofwet-spungrapheneoxide(GO)fibers,wherenumbersofmacroscopicfiberscan
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1fuseintoathickerone,andcanalsoseparateintooriginalindividualfibersunderstimulationof
,causedbysolvent
3evaporationandinfiltration,isthekeytothereversiblefusion-
4extendedtoimplementflexibletransitionsbetweencomplexfiberassembliesandtheinclusion
5orexpulsionofguestcompounds.
6OneSentenceSummary:
7Largegeometricaldeformationofmacroscopicfibersenablesreversiblefusionandfission
8undersolventstimuli.
9
10MainText:
11Fusionandfissionbehaviorshavebeenextensivelystudiedinbiology,chemicalengineering
12andtheoreticalphysicstounderstandcellularprocesses,developmorphologicaleventsof
14lipid/surfactant/smallorganicmolecules/polymermicellesandvesiclesareusuallytriggeredby
15eitherintroducingsalts,surfactants,ions,andoxidant/reductantorapplyingUVandvisiblelight
16tochangetheinteractionsinsidebilayermembranes,aswellasbydissolvingadditivessuchas
17saccharidestoaltertheosmoticpressurebetweentheaqueousinteriorofvesiclesandthebulk
18solution(1-6).Similarbehaviorsofmetalparticles/clustersarealsoinducedbyheatorcluster
19deposition(7-9).Althoughprogresshasbeenmadeonfusion-fissionofartificialvesiclesand
20nanoparticles,reversiblefusionandfissionarestilldifficulttorealize,mainlybecauseofthe
22explorationofreversibleandcontrollablefusionandfissionwouldinspirethedevelopmentof
23stimuli-responsivematerials,whichshowpromiseinderivingdynamictransformablesystems
2
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2assembledstructuresisalsoabeneficialattribute.
3Weproposeasolvent-triggeredtopography-regulationstrategytoimplementreversiblefusion
5topology,abundantchemicalmoieties,super-flexibilityandself-adhesioncapability(10-13).
6Afterswelling(14),thewet-spunGOfiberfeaturesashell(anoutermostskin)thatconfinesthe
7movementofinternalGOsheetsandshowsasolvent-triggeredlargevolumechangeandelastic
,thetopographyoffiber
9shellsreversiblyswitchesbetweenawrinkled,tubularstateandaspreadcylindricalstatevia
10swellinganddeswellingthuscausingatransientfiberinterfaceandleadingtocyclicself-fusion
11andself-fissionofanarbitrarynumberofGOfibers().Ineachcycle,thenumber,size,
12composition,structureandpropertyofGOfibersarerecoveredafterfission,exhibitingthe
13precisereversibilityoffusionandfission.
14ContinuousGOfiberswerepreparedfollowingawet-spinningprotocol()(15,16).In
,wedemonstratethereversiblefusionandfissioninvolvingupto100GOfibers(movie
16S1).Forsimplicity,thefusedGOfiberassembledbynindividualfibersisdenotedasFuF-n,and
17thecorrespondingfissuredindividualdriedGOfiberisdenotedasFiF-
18processrequiresthreesteps,includingsolvent-swellingoffibersinabundle,drawingthefiber
19bundleoutofthesolvent,andair-
20inasolvent,splittingofswelledfiberbundles,anddryingofthefissuredfibersseparately(see
21supplementarymaterials).
22Insituopticalmicroscopyandexsituscanningelectronmicroscopy(SEM)showthewater-
23inducedfusionandfissionprocesses(,CtoF,,andmoviesS2andS3).
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1Swellingratio,definedastheratioofswelledfiberdiametertorawfiberdiameter,isemployed
2toquantifytheextentofswellingwhichisinfluencedbysolventtype,chemicalnatureofGO
3fibersaswellasthesoakingtime()(17).Theequilibrium-swelledGOfibersrandomly
4immersedinwaterexhibitaswellingratioof541%withacore-shellstructure,wherethecore
5(poresizeof2-5µmafterfreeze-drying,innerwallthicknessof28±8nm)isenclosedbyaskin-
6likeshell(about80±18nm-thick)ofdenselypackedGOsheetsthatorientalongthe
7circumference(,).ThisdifferentarrangementofGOsheets
8withintheouterlayerandinnerfiberisafeaturedstructureofwet-spunfibers,whichoriginates
9fromthealigningeffectduringfiberextrusion,andisenhancedbydoublediffusiveconvection
10inthecoagulationbath(18).Thethicknessofbothshellandinnerwalldependsontheswelling
,
12theseswelledfiberscollecttogetheranddeformintoacylindricalgroupspontaneouslyasthey
-drying(0-40min),theswelledfibersbondtogether
14accompaniedwithadaptivecrumplingoffibershellsexhibitingavolumeshrinkageof98%(Fig.
151,C1toC4andD1toD4).Meanwhile,
-situX-raydiffraction(XRD)characterizations().Consequently
17(40min),theresultedFuF-100featurescompactpackingofGOplatelets(interlayerspacingof
,-3)withatensilestrengthof281MPa(,GtoI).GOfibers
19alsofusewhiledryingnotundertension,despitethedecreaseindensityandtensilestrength
20comparedwiththosedryingundertension().
21FissionofFuF-100startswithahomogeneousswellingwhenitisre-soakedinwater,and
22smallgapsemergeattheinter-(150s),a
23rapidgappropagation,alongwithvolumeexpansionofthewholefiberassemblyleadstothe
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1completefissioninto100individualquasi-
2foralongtimeratherthandissolvingintopiecesdespiteaswellingratioof538%,alsoowingto
,solventinfiltrationcauses
4expansionbetweenGOsheets,
5().Afterdryingseparately,theinterlayerspacingbetweenGOsheets(),density
6(-3)andtensilestrength(259MPa)ofFiFs-100areclosetothoseofFuF-100().
7In-situopticalmicroscopy/polarizedopticalmicroscopyobservationsonthecross-sectionoftwo
8GOfibersduringtheirfusionandfissionfurtherverifytheabovedescription(movieS3).
9AGOfiberwaslabelledwithfluorescent1,1,2-triphenyl-2-(4-bromomethylphenyl)ethylene
10(TPE-Br)andsilicon(Si)
11andapristineoneunderfluorescencemicroscoperevealsnosubstanceexchangeacrossthefiber
12interface(,AtoD,).Energydispersivespectroscopy(EDS)analysis
13performedonaneatGOfiberandanothercompositeSi/GOfiber(,EtoL,
14andS11)showsthatfusionwasfinallyaccomplishedbyinterlockingofthesynergistically
15crumpledshells,andfissionwasinducedbytopographicalrecoveryofshellswithopposite
16normalvectorsingeometryonbothsidesofthebondinginterface(,L).
17Onthebasisoftheabovecharacterizations,fusionandfissionwerefoundtobeconductedby
18reversiblecrumplingandspreadingoffibershellswhiledeswellingandreswelling(,and
).HeretheGOfibershellisdefinedastheoutermostdenselayerofasaturated
20swelledGOfiber,characterizedbymacro-scalecylindricalconfiguration,micro-scaleripples
21andnanoscalecloselyorganizedGOplatelets().Theshellplaysamajorroleinthe
22reversiblefusion-fissionprocessbecauseitistheboundarycontactingwithadjacentfibers,
23whichprovidesinter-fiberbonding/debondingandprotectsinner-fiberGOsheetsfromdiffusion.
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1AswelledGOfiberalmostmaintainsaconstantperimeterduringdeswellingandreswelling
2courses,indicatingonlyelasticdeformationoccursattheshell().Theshellcrumplesand
3spreadsduetowrinklingandunfoldingoftheripplemicrostructures,withthecurvatureradiusof
4theripplesvariesintherangeofabout10nmto83µm(,,A1toB4).Atthe
5sametime,theinner-fiberGOsheetsdeformaccordinglysincetheyareinterconnectedinthe
,thereversiblefusion-fissioncapabilityisonlyfoundinwet-spunGO
-spunGOfiberscanbefused,theyfailedtofissure,mainlyattributedtothe
8insufficiencyofadenseandprotectiveshell()(19).Thetopographicalandvolumetric
9evolutionoffibersduringfusionprocessisdrivenbythesurfacetensionofsolvent(20)andthe
10Laplacepressuredifference(Pc)(21).TheattractivestressPcfacilitatesfurtherbondingoffiber
11shellsvianon-covalentinteractions(π-πinteractionandhydrogenbonding(22)),aswellas
12subsequentwrinklingofGOsheetsanddensifyingofthewholefiberbundle().During
13thefusionprocess,thesolvent-responsivefibershellactsasanelasticbarrier,preventingthe
,thefusiondegree,proposedtoevaluate
15thefusionstatus(seesupplementarymaterialsforcalculation),risesfrom0%(unfused)to100%
16(fused)uponswellingandtraversesahemifusedregion(swellingratiofrom165%to358%)(fig.
17S16).
18Conversely,fissionisattributedtothecylindricalgeometry-drivendetachmentbetweenfiber
19shells().AstheFuFissoakedingoodsolventsforGO,thesolventinfiltrationweakens
20theadhesionstrength(sad*)betweenindividualfibers(23).Thetendencyofcylindrical
21geometryreversionattheinterfacecontributestotheinterfacialdetachabilityandcompelsthe
(denoted
23asfissionstresssfis)ofelastictensilestressse1andswellingpressurepsalongtheinward-
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1pointingnormaldirectionofthecurvedmicroelement(seesupplementarymaterials).This
2hypothesisisfurtherconfirmedbyfiniteelementanalysis,whichshowssfisisgeneratedbythe
3curvedgeometryofshellwhentheswellingratioofindividualfiberssurpassesasufficiently
4highvalue(475%and521%forseparationofpoint1and2,respectively)(,BtoEand
5movieS5).Furtherswellingleadstotherisingsfis,whichconsequentlyreachesapeakvalue
6equaltosad*,thefission
7capabilityofFuF-2wasinitiatedwhentheaverageswellingratioofindividualfiberstraversesa
8criticalrangefrom310%to419%,eitherbyapplyingpolarity-enhancedsolventorreducingthe
9pre-treatingtemperatureontheFuF-2().Additionally,incontrasttoGOfibers,GO
10beltsfeaturingadistinctflattopographyafterswellingareabletobefusedtogetherbutfailto
11fissure,duetotheabsenceofanarcconformationofGOsheetsstoredinwrinklesthuslackinga
12drivingforcesfisforself-fission().
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