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DOI: 10.4018/IJANR.2019010103 International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 Copyright©2019,IGIGlobal.CopyingordistributinginprintorelectronicformswithoutwrittenpermissionofIGIGlobalisprohibited. 26 3D-Printed Conductive Filaments Based on Carbon Nanostructures Embedded in a Polymer Matrix: A Review Diogo José Horst, Department of Mechanical Engineering and Sciences, Federal University of Santa Catarina - UFSC, Joinville, Brazil https://orcid.org/0000-0003-4971-4912 Pedro Paulo Andrade Junior, Department of Mechanical Engineering and Sciences, Federal University of Santa Catarina - UFSC, Joinville, Brazil ABSTRACT Conductiveandmagneticfilamentsarerevolutionizingthree-dimensionalprinting(3DP)toanew level.Thisreviewstudypresentsthecurrentstateoftheartonthesubject,summarizingrecenthigh impactstudiesaboutmainadvancesregardingtheapplicationof3DPfilamentsbasedoncarbon nanostructuressuchasgraphene,carbonfibers,nanotubes,andconductivecarbonblackembeddedin apolymermatrix,byreviewingitsmaincharacteristicsandshowingthemainproducersandalsothe productsavailableonthemarket.Theavailabilityofinexpensive,reliable,andelectricallyconductive materialwillbeindispensableforthefabricationofcircuitsandsensorsbeforethefullpotentialof 3DPforcustomizedproductsincorporatingelectricalelementscanbefullyexplored. KEywoRDS Additive Manufacturing, Carbon Nanostructures, Conductive Filaments, Magnetic Filaments, Polymer Nanocomposites INTRoDUCTIoN 3DPisrevolutionizingtheworld,computerdesignedobjectsfabricatedusing3D-printerscanbemore complexthanconventionallymachinedparts,suchemergentmanufacturingtechnologypromisesto boostthefabricationofhighlysophisticatedpartsdirectlyfromcomputer-aideddesigns.Nowitis possibleto3DPlightweightstructureswithhighdimensionalaccuracyatlowercostforcustomized geometries(Chua&Leong2016).Overthepastfewyears,theintrinsiclimitationsofneatpolymers, metals, and ceramics have propelled toward better alternative composite materials to enhance mechanicalandotheressentialproperties;nowadays3DPresearchfollowsasimilardirectionfrom neattocompositematerial(Veluetal.,2019). 3DPfilamentsinfusedwithcarbonnanotubessuchasgraphenearenowcommerciallyavailable,with thepromisetoproduceconductiveandmagneticcomposites(Al-Haririetal.,2016;Kwoketal.,2017). https://orcid.org/0000-0003-4971-4912 International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 27 3DPutilizesdifferenttechniquesforthemanufacturingofprototypes,themaintechniquesinclude: inkjetprinting(IJP);fuseddepositionmodeling(FDM);fabricationwithfusedfilament(FFF);powder- bed fusion (PBD);micro-stereolithography (MSL);dynamicopticalprojection stereolithography (DOPsL);direct-writeassembly(DW);selectivelasersintering(SLS);solvent-cast3DP(SC-3DP); conformal3DP(C-3DP);two-photonpolymerization(TPP);UV-3DP;andstereolithography(SLA); amongothers(Farahanietal.,2016;Tianetal.,2016). 3DPofpolymernanocomposites(PNCs)witharelativelylowamountoflayeredsilicatefillers orconductivenanofillers,suchascarbonnanotubes,grapheneandmetalparticlesareusedtobuild objectswithmultifunctionalpropertieshavinggoodelectricalandthermalconductivity,mechanical strength,andstiffnessatrelativelowcost(Postiglioneetal.,2015;Francis&Jain2016). InconductivePNCs,theelectricalconductivityisgovernedbyelectricalpercolation,which requires a minimum filler content (volume fraction) to convert an insulating polymer matrix intoaconductivecomposite (Aligetal.,2007).Thisminimumvolumefractionofnanofillers, referredaspercolationthreshold,stronglydependsonfactorslike,shapeandsizedistributionof thenanofillers(Otten&VanDerSchoot2009;Gnanasekaranetal.,2014),attractiveinteractions (Vigologetal.,2005),andprocessingmethodssuchasdispersionandagglomerationofnanofillers (Gnanasekaranetal.,2016). Severalstudieshavebeenreportedon3DPofconductivePNCs,basedonconventionallyused3D printingpolymerslikepolylacticacid(PLA)andacrylonitrilebutadienestyrene(ABS)(Tianetal., 2016;Guoetal.,2015;Rymansaibetal.,2016;Weietal.,2015).However,thedevelopmentofnew conductivePNCmaterialsforadesktop3Dprinterishighlydesirabletoachievebetterprintability, mechanicalpropertiesandelectricalconductivity(Gnanasekaranetal.,2017). Insidethiscontext,thisreviewstudypresentrecentadvancestowardstheapplicationof3DP technologyusingconductiveandmagneticfilamentsbasedoncarbonnanostructuresembeddedin polymermatrix,byshowingitsmaincharacteristicsandalsosummarizestheproducercompanies andproductsavailableinthemarket. STATE-oF-THE-ART Carbon Nanotubes (CNT) CNTareknownfortheiroptimalmechanical,electricalandthermalproperties,whichmakesthema suitablecandidatetointegrate3DPpolymers.MultiwallCarbonNanotubes(MWCNTs)havestructural defectswhichprovidesuitablenucleationsitesallowingstronginteractionswithpolymers(McCarthy etal.,2000)andforcross-linkingandfunctionalization(Gaoetal.,2013;Venturaetal.,2010). AhomogeneousdispersionCNT´sinpolymericsolutionsisessentialforenhancedCNTbased filaments.ThefamiliarproblemofCNTsaggregationcanbedetrimentaltoFDM,possiblycausing blockagesatthenozzleandfluxinstabilitywhileprinting,soresearchhasfocusedondeterminingthe concentrationofCNTsthatwouldsurpassthepercolationthresholdwhilemaintainingtheparameters for3Dprinting(Al-Haririetal.,2016). ContinuousCNTyarnfilamentscanbeemployedasaninherentlymultifunctionalfeedstockfor 3DP,sinceitbecomespossibletouseasinglematerialtoimpartmultiplefunctionalitiesincomponents andtakeadvantageofthetailor-abilityofferedbyFFFoverotherconventionalfabricationtechniques (Gardneretal.,2016). ThereisthepossibilitytotapintotheelectricalpropertiesofCNTsinordertofabricateconductive composites using a standard commercial 3D-printer (Gonzalez et al., 2017). Lee et al. (2018) investigatedthe3DPofnano-conductiveMWCNTsscaffoldsfornerveregeneration,byincorporating MWCNTswithPEGDAtherebyenhancingelectricalpropertiesaswellasnanofeaturesonthesurface ofthescaffold.AnSLA3DPwasemployedtofabricateawell-dispersedMWCNT-hydrogelcomposite neuralscaffoldwithatunableporousstructure.3DPallowedtheeasyfabricationofcomplex3D scaffoldswithextremelyintricatemicro-architecturesandcontrolledporosity. International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 28 Eshkalaketal.(2017)presentareviewonIJPofCNTcompositesforsmartapplications.IJPis emergingasanattractivetechnologyforwidevarietyofindustrialandscientificapplicationsdueto itsmildness,simplicity,low-costandscalabilityofproduction.Itcanperformasacarriermedium fornumberoffillermaterialsandrecentlyCNTinkhasbeenutilizedininkjetprinting.Outstanding characteristicsofCNT´sandtheirreasonableprice,hasmadethistechnologyagoodchoiceforvarious electronicapplicationssuchassensors,transparentelectrodes,flexibleandprintableelectronics.One wayofobtaininghighlyconductivepatternssuchaselectriccircuitsisthroughtheincorporationof conductiveorganicandmetallicparticlesandalsopolymersintocarbonnanotubes. Graphene (Gr) Sinceglobalizationhastakenplace,carbon(indifferentforms)hasbeenconsideredafundamental material inmostofthe three-dimensional(3D) / four-dimensional(4D)printingapplications (Singhetal.,2018;Horstetal.,2018).Grapheneisahighlyexpensiveengineeringmaterialwith remarkablemechanical/metallurgical/thermal/andelectricalproperties.Somestudiesreported the production of low-cost Gr-reinforced polymer matrix-based feedstock filament for FDM applications(Singh&Kumar,2018). Graphenehasriseninpopularityasamaterialthatwouldrevolutionizeelectronics;fortunately, Gr has safely passed the peak of overestimated expectations and is now settling on some novel applications,due its interestingpropertiessuchas lowresistivity,excellent thermalconductivity, opticaltransparency,andhighelectronmobility.Grexhibitsarangeofexceptionalqualitiesincluding flexibilityandconductivity.3DPfilamentsaugmentedwithGrhavethepotential toenhancethe manufacturingprocessofstrongconductivecomposites.Therearemanyapplicationsofthesecarbon nanostructuredadditives in3DPfilaments includingsensors, trackpads,electromagnetic,andRF shielding(Al-Haririetal.,2016). 3D-Gr-basedarchitecturessuchasGr-basedhydrogels,aerogels,foams,andspongeshaveattracted hugeattentionowingto thecombinationof thestructural interconnectivitiesandtheoutstanding propertiesofGrofferinginterestingstructureswithlowdensity,highporosity,largesurfacearea, stablemechanicalproperties,fastmassandoptimalelectrontransport.Beingextensivelystudiedfor awiderangeofapplicationsincludingcapacitors,batteries,sensors,catalysts,etc.(Yangetal.,2015). Overthelastdecade,agreatdealofresearchhasbeendevotedtothedesignanddevelopment ofGr-basedpolymernanocompositescharacterizedbyaprescribedarrangementofthegraphene- basednanosheets intospatiallysegregated3Darchitectures.Theformationofacontinuousfiller networkobtainedbyconfiningthenanosheetsintoaconstrainedvolumeofthepolymericmatrix isparticularlyattractivefromatechnologicalpointofview.Indeed,therealizationofsegregated 3D-Gr-basedarchitecturesallowstoproperlytailortheoverallperformancesoftheresultingpolymer nanocomposites,providingsignificantimprovementsintermsofstructuralandfunctionalfeatures (Salzanoetal.,2018). Cardosoetal.(2018)investigatedpotentialapplicationsoflow-costfuseddepositionmodeling 3D-printerstofabricatemultiuse3D-printedelectrochemicalcellsforfloworbatchmeasurementsas wellasthe3DPofelectrochemicalsensingplatforms.Theauthorssuccessfully3DPelectrochemical cells and sensors using acrylonitrile butadiene styrene (ABS) and conductive graphene-doped polylacticacid(G-PLA)filaments. Huang et al. (2019) studied a graphene-based elastomer for sensors with tunable and high sensitivitywasfabricatedbyusingthree-dimensionalprinting,inwhichaprintableinkwasdeveloped by homogenizing graphene and polydimethylsiloxane (PDMS). To make the elastomer tunable andhighlysensitive,differentmicrostructuresGr-PDMScanbeformed.Thecontrollabledesign and scalable fabricationof the advanced functionalmaterial suggests that tunable strain sensors andwearabledeviceshavegreatpotentialfordifferentapplications,whichisafindingthatcanbe referencedbyfuturestudieson3D-Grbasedsensors. International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 29 Themanufacturing3D-Grmonolithwithhighmechanicalandelectricalperformancehasbecome anurgentissueinviewoftheirpotentialapplicationsinenergyandelectronicsfields.Duetothe structurerigidityandpoorliquid-phaseprocessingcapabilityofgraphenesheets,itischallenging tofabricate3D-Grmonolithwithhighmechanicalperformance,includingstrength,toughnessand resiliency.Maetal.(2019)demonstrateastrategytofabricatehigh-performance;shape-designable 3D-Grmonoliththrougha3DPmethodbasedonlarge-sizedgrapheneoxide(LGO)fluidink.The resultingmonolithexhibitslowdensity(12.8mg/cm3),highelectricalconductivity(41.1S/m),high specificstrength(10.7×103N·m/Kg)andcompressibility(upto80%compressivestrain).Sucha 3DP techniqueenables to achieve complicatedmonolith structures andbroadens the application rangeofgraphene. Mohan et al. (2018) demonstrate the development of novel highly conductive 3D-printable hybridpolymer-graphenecomposites.Thekeyfactorsidentifiedhaveincludedthepolarityofthe primarypolymer,thelevelofhomogeneityofthedispersionoftheconductivefillermaterialsand thecrystallinityoftheresultingcompositewhichinthiscaseisincreasedbytheadditionofsucrose. Optimizing for these factors the production method has been able to manufacture samples with anelectricalconductivityofupto14.2S.cm−1atfillerloadingof10wt.%grapheneand10wt.% conductivepolymerinthebasepolymethylmethacrylatematrix.Thesehavebeeninvestigatedfor applicationin3DPasanalternativetowiringorexpensiveprintableconductiveinks,andsuccessful sampleshavebeenproducedwithanelectricalconductivityof11.3S.cm−1. Huangetal.(2018)demonstratedanovelstrategytoprepareprintablegrapheneinkisreported first,andthree-dimensionalscaffoldswithhighcontent(50wt%)andalignedgrapheneareachieved bythree-dimensionalprinting.Fromresultsadequateshearthinningandrheologybehaviorarerequired forprintablegrapheneinktoflowthroughthenozzlesmoothlyandself-supportduringtheprinting process.Thescaffoldswithdifferentcontentsandprintingparametersexhibitgoodresolutionand goodbondingbetweenlayers.Thealignmentofgraphenesheetsalongthedirectionofflowingcan beobservedduetotheshearstressinthenozzle.Whenthetemperaturerisesupto450°C,electrical conductivitiesalong transversand longitudinaldirectionsof50wt%areenhanced to479.2and 425.6S/m, which are 6.7 and 8.4 times higher than that at room temperature, respectively. The alignmentcancontributetotheelectricalanisotropyofthree-dimensionalgraphenescaffolds.The electricalresistancevariationsundercompressionandelectricalanisotropydemonstratethepotential applicationofthegraphenescaffoldsinelectricaldevice,sensor,especiallycombinedwith3DP. Azharietal.(2017)introduceapowder-bedtechniqueforthefabricationofcrack-free,mm-thick graphene-basedelectrodes,withhighsurfaceareathatcanbeprintedincomplexshapes.Whilethis technologyhasthepotentialtobeusedinmanyapplicationsincludingenergystorage,conversion, andsensing. Inhiswork, theydemonstrate theiruseashighperformancesupercapacitors.From results,devicesfabricatedusingthermallyexfoliatedgrapheneoxidepowderhadgravimetricandareal capacitanceof~260Fg−1and~700mFcm−2,respectivelyat5mVs−1in1MH2SO4electrolyte.The supercapacitorsretained80%oftheircapacityover1000cycles.Thistechniqueprovidesapromising routeforthefabricationandcommercializationofthick,porousgraphene-baseddevices. Carbon Black (CB) Dawoudetal.(2018)studiedthestrainsensingbehaviorof3D-printedofCBfilledwithABS(CB- ABS).Experimentalworkrevealedthatinternalstressescanbedetectedbasedonmonitoringthe changeinresistanceasaresponsetostrain.Thefunctionalizedcompositecanbeusedasastrain sensorasforhealthmonitoringpurposes,togiveanexample. Jayanth & Senthil (2019) also studied CB-ABS filaments for the 3DP of low-cost concave capacitivesensorusedtomeasurethevoidfractionoftwo-phaseflow.Thevariationincapacitance valuesof3DPsensorwasfoundtobelesswhencomparedtoacoppersensor,butstillmeasurable, thecapacitancevalueincreaseswithanincreaseinwidthandthicknessofthe3DPCB-ABSsensor. International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 30 Flowersetal.(2017)describedtheuseofdual-materialfusedfilamentfabricationfor3DPof electroniccomponentsandcircuitswithconductivethermoplasticfilaments.Theresistivityoftraces printedfromconductivethermoplasticfilamentsmadewithcarbon-black,graphene,andcopperas conductivefillerswasfoundtobe12,0.78,and0.014Ωcm,respectively,enablingthecreationof resistorswithvaluesspanning3ordersofmagnitude.Thecarbonblackandgraphenefilamentswere brittleandfracturedeasily,butthecopper-basedfilamentcouldbebentatleast500timeswithlittle changeinitsresistance.Impedancemeasurementsmadeonthethermoplasticfilamentsdemonstrate thatthecopper-basedfilamenthadanimpedancesimilartoacopperPCBtraceatfrequenciesgreater than1MHz.Dual3DPmaterialwasusedtofabricateavarietyofinductorsandcapacitorswith properties thatcouldbepredictably tunedbymodifyingeither thegeometryof thecomponents, orthematerialsusedtofabricatethecomponents.Theseresistors,capacitors,andinductorswere combinedtocreateafully3D-printedhigh-passfilterwithpropertiescomparabletoitsconventional counterparts.Therelativelylowimpedanceofthecopper-basedfilamentenableditsusefor3DP ofareceivercoilforwirelesspowertransfer.ThepotentialofusingFFFtocreatecomplexcircuits composedofeitherembeddedorfully-printedelectroniccomponentsisshowed. Carbon Fibers (CF) Lietal.(2016)investigatedthecontinuousCF´sreinforcedwithPLA(CF-PLA).Theexperimental resultsdemonstratedthatthetensilestrengthandflexuralstrengthsofmodifiedcarbonfiberreinforced compositeswere13.8%and164%higherthanoriginalcarbonfiberreinforcedsamples. Zhuetal.(2018)developedanovelmethodtofabricatecarbonfiberreinforcedSiC(CF/SiC) compositesbycombining3DPandliquidsiliconinfiltrationprocess.Greenpartsarefirstlyfabricated through3DPfromastartingphenolicresincoatedcarbonfibercompositepowder;thenthegreen partsaresubjectedtovacuumresininfiltrationandpyrolysissuccessivelytogeneratecarbonfiber/ carbon(CF/C)preforms;finally,theCf/CpreformsareinfiltratedwithliquidsilicontoobtainCF/ SiCcomposites.Fromresults,the3DPprocessingparametersshowsignificanteffectsonthephysical propertiesofthegreenpartsandalsotheresultantCF/Cpreforms,consequentlygreatlyaffecting themicrostructuresandmechanicalperformancesofthefinalCF/SiCcomposites.Theoveralllinear shrinkageoftheCF/SiCcompositesislessthan3%,andthemaximumdensity,flexuralstrengthand fracturetoughnessare2.83±0.03g/cm3,249±17.0MPaand3.48±0.24MPam1/2,respectively.It demonstratesthecapabilityofmakingnearnet-shapeCf/SiCcompositepartswithcomplexstructures. Conductivesiliconrubbers(CSRs)arepotentialcandidatesforstrainsensorapplicationowing totheirspecificelectricalresponseandsuperiormechanicalflexibility.Huangetal.(2018)studied carbonfiber-filledCSRsprintedbyanextrusiondevice.Thixotropicagentwasadded tomodify mobilityandviscosityoftheliquidCSR.ItwasfoundthattheCSRwith5wt%thixotropicagent additionexhibitedbettershape-retention.Fibersinmatrixwereobservedtobeorientedintheprinting directionresultinginananisotropicelectricalandmechanicalbehavior.TheprintedCSRsshowed betterelectricalandmechanicalpropertiesalongtheorientationdirectionoffibers.Inparticular,the volumeresistivityattheorientationdirectionwas6.8timeslowerthanthatatperpendiculardirection. Highertensilestrength,largerelongationatbreak,andhigherYoung’smoduluswerefoundalong theorientationdirectionwhentheprintedCSRswerestretched,wherealargenumberoffiberswere pulledoutandvisibleholesremainedatthefracturedsurface.ElectricalresponsesoftheCSRsunder variousloadings,includingstretching,compressing,bending,twistingandcyclicfolding,wereclosely relatedwithdeformationsoftheCSRs.Sandwichstrainsensorswerefinallyfabricatedtoverifya practicalapplicationasmotionsensoroftheprintedCSRs. Haoetal.(2018)studiedacontinuouscarbon-fiberreinforcedthermosettingcompositesprepared using3DPfollowedbycharacterizationoftheirmechanicalproperties.First,a3DPplatformwas fabricatedtopreparethecompositesbasedonFDM.Then,thecompositeslaminaandgridswere manufacturedusinganFDM-basedplatform,andthenthemechanicalpropertiesofthecomposite laminawerecharacterized.Theresultsshowedthatthemechanicalperformanceofthe3D-printed International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 31 thermosettingcompositeswassuperiortothatofsimilar3D-printedthermoplasticcompositesand 3D-printedshortcarbonfiberreinforcedcomposites. Yaoetal.(2017)presentedatechniqueforbothstructuralreinforcementandself-monitoringof thermoplasticpartsmanufacturedbyFDM.ContinuouscarbonfibertowswereembeddedintoFDM printedstructuresduringtheprintingprocess,andthestrengthandpiezoresistivebehaviorofthe printedstructureswereevaluated.ThespecimensreinforcedwithCfshowedastrengthincreaseof70% andflexuralstrengthincreaseof18.7%comparedtonon-reinforcedspecimens.Inaddition,theslope offractionalchangeinelectricresistancewithstrainbecameagoodindicatorofstrainmeasurement withintheelasticregionanddamagedetectionintheyieldregion.Furthermore,lightweightandprint durationreductionswereachievedbydecreasingthefilldensitywhilemaintainingthestructural strength,whereup to26.01%weight reductionand11.41%print time reductionswereachieved withoutdecreasingthetensilestrength. Caminero et al. (2018) investigated the impact damage resistance of 3D-printed continuous fiberreinforcedthermoplasticcompositesusingfuseddepositionmodeling.Itwasobservedthatthe effectoflayerthicknessofnylonsamplesontheimpactperformancewasdifferentforflatandon- edgesamples.Impactstrengthincreasesaslayerthicknessincreasesinflatsamplesbut,conversely, itdecreasesinon-edgesamples,depictingamorebrittlefracture.Inaddition,theresultsshowthat impactstrengthincreasesasfibervolumecontent increasesinmostcases.Glassfiberreinforced samplesexhibitsthehighestimpactstrengthandcarbonfiberreinforcedsamplesthelowestoneand similar tonylonperformance.Furthermore,on-edge reinforced samples exhibithighervaluesof impactstrengththanflatreinforcedsamples.Theimpactstrengthexhibitedby3D-printedcomposites issignificantlyhigherthantheusual3D-printedthermoplasticsand,insomecases,evenbetterthan commonpre-preg.materials. Theincreasingneedforprototypingandcustomizationoffiberreinforcedpolymercomposite partsispromptinginnovationsinnewmanufacturingprocessestorealizeshortmanufacturingcycle timeandlowproductioncost,whichischallengingtoaccomplishusingconventionalmoldingprocess. Gohetal.(2018)madeacomparisonoffracturebehaviorsbetween3D-printedcarbonandglassfiber reinforcedcompositesisperformed.TheFFFtechniquewasemployedtofabricatecontinuouscarbon andglassFRTPcompositesanditsmicrostructuralcharacteristicsandtheresultingtensile,flexural, andquasi-staticindentationcharacteristicsoftheprintedcompositeswereexamined. Bloketal.(2018)investigatedthe3DPoffiberreinforcedthermoplasticcomposites.Carbon fiberswereembeddedintoathermoplasticmatrixtoincreasestrengthandstiffness.Fromresults, theprintingofcontinuouscarbonfibersusingtheMarkOneprintergivessignificantincreasesin performance over unreinforced thermoplastics, with mechanical properties in the same order of magnitudeoftypicalunidirectionalepoxymatrixcomposites.Themethod,however,islimitedin design freedomas thebrittle continuouscarbon fibers cannotbedeposited freely through small steeringradiiandsharpangles.Filamentswithembeddedshortcarbonmicrofibers(~100μm)show betterprintcapabilitiesandaresuitableforusewithstandardprintingmethods,butonlyoffera slightincreaseinmechanicalpropertiesoverthepurethermoplasticproperties.Itishypothesized thatincreasingthefiberlengthinshortfiberfilamentisexpectedtoleadtoincreasedmechanical properties,potentiallyapproachingthoseofcontinuousfibercomposites,whilstkeepingthehigh degreeofdesignfreedomoftheFFFprocess. Tian et al. (2016) investigated a novel 3DP based fabrication process of Continuous Fiber ReinforcedThermoplasticComposites(CFRTPCs).ContinuousCF-PLAfilamentwereutilizedas reinforcingphaseandmatrix,respectively,andsimultaneouslyfedintotheFDMprocessrealizingthe integratedpreparationandformingofCFRTPCs.Interfacesandperformanceofprintedcomposites weresystematicallystudiedbyanalyzingtheinfluencingofprocessparametersonthetemperatureand pressureintheprocess.Formingmechanismofmultipleinterfaceswasproposedandutilizedtoexplain thecorrelationsbetweenprocessandperformance.Thefibercontentoftheprintedspecimenscanbe easilycontrolledbychangingtheprocessparameters.Whenthefibercontentreached27%,flexural International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 32 strengthof335MPaandmodulusof30GPawereobtainedfortheprintedcompositespecimens. Compositecomponentsfabricateddemonstratedtheprocessfeasibility,potentialapplicationscould befoundinthefieldofaviationandaerospace. other Polymer Nanocomposites (PNCs) Dickson et al. (2017) evaluated the performance of continuous carbon, Kevlar and glass fiber reinforcedcompositesmanufacturedusingFDMtechnique.Itwasdemonstratedthatamongthefibers investigated,thosefabricatedusingcarbonfiberyieldedthelargestincreaseinmechanicalstrength perfibervolume.Itstensilestrengthvalueswereupto6.3timeshigherthanthoseobtainedwiththe non-reinforcednylonpolymer.Asthecarbonandglassfibervolumefractionincreasedsotoodid thelevelofairinclusioninthecompositematrix,whichimpactedonmechanicalperformance.As aresult,amaximumefficiencyintensilestrengthwasobservedinglassspecimenasfibercontent approached22.5%,withhigherfibercontents(upto33%),yieldingonlyminorincreasesinstrength. Kwoketal.(2017)describedthefabrication,characterization,stresstesting,andapplicationof alow-costthermoplasticconductivecompositethathasbeenprocessedintofilamentformfor3DP. Sanatgaretal.(2017)investigatedanovelprintingprocessfordepositionofpolymersonsynthetic fabrics to introduce more flexible, resource-efficient and cost-effective textile functionalization processes thanconventionalprintingprocess like screenand inkjetprinting.Thepolymerswere printedindifferentseriesofexperimentaldesign:nylononpolyamide66(PA66)fabrics,polylactic acid(PLA)onPA66fabric,PLAonPLAfabric,andfinallynanosizecarbonblack/PLA(CB/PLA) andmulti-wallcarbonnanotubes/PLA(CNT/PLA)nanocompositesonPLAfabrics.Tekinalpetal. (2014)researchedshortfiber(0.2–0.4mm)reinforcedacrylonitrile–butadiene–styrenecompositesasa feedstockfor3D-printingintermsoftheirprocessability,microstructureandmechanicalperformance. Theadditivecomponentswerecomparedwithtraditionalcompressionmoldedcomposites. Sweeneyetal.(2017)studiedtheweldingof3D-printedcarbonnanotube–polymercomposites bylocallyinducedmicrowaveheating.Akeyobstaclefacing3D-printedplasticpartsinengineering applicationsistheweakweldbetweensuccessivefilamenttraces,whichoftenleadstodelamination andmechanicalfailure.Theresultsshowedafterprinting,microwaveirradiationisshowntoimprove theweldfracturestrengthby275%. Huetal.(2018)analyzedthe3DPofgraphene-aluminumnanocomposites.Fromresults,the Vickershardnessandnano-indentationtestsshowedthatthehardnessofthecompositeswasgreatly enhanced.Comparedwithpurealuminumcounterpart,theVickershardnessofthebestcomposite sample achieves a 75.3% increase. The experimental results suggest the efficacy of laser 3DP technologytofabricateGr-Alcomposites. Kim et al. (2017) evaluated the 3DP of multiaxial force sensors using carbon nanotube (CNT)/thermoplasticpolyurethane(TPU)nanocompositefilaments.Dueitscustomizability,rapid manufacturing,andeconomicfeasibility,thismanufacturingapproachallowsdirectfabricationof multiaxialsensorswithoutadditionalassemblyorintegrationprocesses. Kimetal.(2018)studiedtheeffectofFDM3DPonthreephasedielectricnanocompositesusing poly(vinylidene)fluoride(PVDF),BaTiO3(BT),andmultiwallcarbonnanotubes(CNTs).PVDF polymerandBTceramicsarepiezo-,pyro-anddi-electricmaterialsextensivelyused for sensor andenergystorage/harvestingapplicationsduetotheiruniquecharacteristicofdipolepolarization. To increase dielectric property, CNTs have been recently utilized for uniform dispersion of BT nanoparticles,ultrahighpolarizationdensity,andlocalmicro-capacitoramongmatrix.Itwasproved that3DPprocessprovideshomogeneousdispersionofnanoparticles,alleviatingagglomerationof nanoparticlesandreducingmicro-crack/voidsinmatrixwhichcanpotentiallyenhancetheirdielectric propertythantraditionalmethods. Muetal.(2017)DLPofconductivecomplexstructures.ADLPbased3DPtechniquewasexplored tomanufactureelectricallyconductiveobjectsofpolymernanocomposites.Theconcentrationsof MWCNTaswellastheprintingparameterswereinvestigatedtoyieldoptimalconductivityandprinting International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 33 quality.Resultsshowedthat0.3wt%loadingofMWCNTintheresinmatrixcanprovidethemaximum electricalconductivityof0.027S/mundertheresinviscositylimitthatallowshighprintingquality. Withelectricconductivity,theprintedMWCNTnanocompositescanbeusedassmartmaterialsand structureswithstrainsensitivityandshapememoryeffect.Theprintedconductivecomplexstructures ashollowcapacitivesensor,electricallyactivatedshapememorycomposites,stretchablecircuits, showstheversatilityofDLP3DPforconductivecomplexstructures.Inaddition,mechanicaltests showedthattheadditionofMWCNTcouldslightlyincreasethemodulusandultimatetensilestress whiledecreasingslightlytheultimatestretch,indicatingthatthenewfunctionalityisnotobtainedat thepriceofsacrificingmechanicalproperties. He et al. (2016) demonstrated that printing a conductive ink formulated by blending 3D porousGr-CNTassemblywith ionic liquid(IL)ontwo-dimensional2Dgraphenepaper, leading toa freestandingGPsupportedgraphene–CNT–ILnanocomposite (graphene–CNT–IL/GP).The incorporationofhighlyconductiveCNTsintographeneassemblyeffectivelyincreasesitssurfacearea andimprovesitselectricalandmechanicalproperties.Thegraphene–CNT–IL/GP,asfreestandingand flexiblesubstrates,allowsforefficientloadingofPtAualloynanoparticlesbymeansofultrasonic-electrochemicaldeposition.OwingtothesynergisticeffectofPtAualloynanoparticles,3Dporous graphene–CNTscaffold,ILbinderand2DflexibleGPsubstrate,theresultantlightweightnanohybrid paperelectrodeexhibitsexcellentsensingperformancesinnonenzymaticelectrochemicaldetection ofglucoseintermsofsensitivity,selectivity,reproducibilityandmechanicalproperties. Zhongetal.(2017)studiedtheextrusionbasedon3DPofgrapheneoxide(GO)/geopolymer (GOGP)nanocomposite.TheadditionofGOingeopolymericaqueousmixture(alumiosilicateand alkaline-sourceparticles)dramaticallychangesitsrheologyproperties,andenablethe3DPthatcannot berealizedsolelybygeopolymer.The3DPGOGPstructuresexhibitedhighmechanicalproperties withcompressivestrengthhigherthan30MPa,andelectricalconductivityof102S/mwasachieved afterannealing,whichisamongthehighestconductiveceramicnanocomposites. Commercial Filaments Available for 3DP Table 1 presents a list of the main commercial producers of 3DP filaments based on carbon nanostructuresembeddedinpolymermatrix: 3DP is a layer-by-layer process having the ability to fabricate sensors and circuits by depositing conductive and magnetic filaments to build electronic components via digital control.3DPisrevolutionizingtheworld;mainlybecausecomputerdesignedobjectsfabricated using 3D printers can be more complex than conventional machined parts. This niche of technologyseemstobeatransformativetoolwithmoreflexibilityfor3DP,sinceconductive andmagneticfilamentspresentanewchapterin3DPhavinggainedcurrentvastinterestasit offerssignificantadvantagesoverthetraditionalmaterials.Advancesintechnologiesrelated tocarbonnanostructuresembeddedinpolymermatrixwillleadtodesignnovel3DPmaterials withspecificadvantages.3DPpotentiallyoffersahighdegreeoffreedomforthecustomization ofpracticalproductsthatincorporateelectricalcomponents.Theavailabilityofinexpensive, reliable,electricallyconductivematerialwillbeindispensableinthefabricationofcircuits andsensorsbeforethefullpotentialof3DPforcustomizedproductsincorporatingelectrical elementscanbefullyexplored. CoNCLUSIoN Thisreviewstudysummarizesthecurrentstateoftheartconcerningthe3DPofconductiveand magneticfilamentsbasedoncarbonnanostructuresaimingthepotentialapplicationofthesematerials. Currentlythereisawiderangeofcommerciallyavailablefilamentsandthisnumberwillincreaseby International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 34 continued on following page Table 1. 3DP filaments based on polymer nanocomposites Company Product Material Extruder Temp (C°) Platform Temp (C°) 3DXTech CarbonX PEEK,Ultem,PC, Nylon,PETG,ABS, PLA 380°-410°C 360-390°C 280-310°C 240-270°C 230-260°C 220-240°C 190-220°C. 130-150°C 140-160°C 110-120°C 80-100°C 70a90°C 100-110°C 23-60°C Functionalize F-Electric PLA 215-230°C X<70°C Filabot MWCNT1 GraphiteInfused Filament NanotubePellets ABSBased 160-180°C 225-235°C 80-100°C 100-110°C BlackMagic3D Conductive Thermoplastic Graphene G6-Impact PlAPELLETS HIPS-Carbon 210-230°C 210-230°C 60-80°C 60-80°C AngstronMaterials GrapheneEnhancedNanocomposites PP,PC,ABS notavailable notavailable CheapTubesInc Carbonnanotube Masterbatches Conductive nanotubesComposite IndustrialGrade MultiWalled CNT-PA6-15, CNT-PC-10, CNT-ABS-10, CNT-PP-20, CNT-PP-15, Carbonnanotubes notavailable notavailable Nanocyl PlasticylMWCNTS PA1501,PA1502, PA1503,HDPE1501, POM1001, TPU1001,PP2001, PC1501,ABS1501, EVA2001, LDPE2001, PEEK1001, HIPS1001, PTB1501, SEBS1001, PETG1001 notavailable notavailable ZyvexTechnologies ZNT(Zyvex nanotube technology) EpovexAdhesive Polymermodified carbonnanotube additive Carbonnanotube- enhancedtwo-part epoxyadhesives notavailable notavailable Vartega VartegaRecycledCarbonFiber ABS,PA6,PA66, PBT,PC,PE,PEI, PEEK,PEK,POM, PP,PPS,PSU,PU notavailable notavailable Advanc3D AdWirePremium PLA notavailable notavailable AvanteTechnology FilaOneGrey FilaOne 205–210°C Stratasys FDMPC Nylon ABS notavailable notavailable International Journal of Applied Nanotechnology Research Volume 4 • Issue 1 • January-June 2019 35 thecomingyearsfollowingtheevolutionofthetheme.Thereisenormousscopefortheapplication ofthispromisingtechnologyindesigningvariouscomponentsandproducts,itsfuturewillrelyon itsprospectivetoprovide3DPsystemscapableofmanufacturingsensorsandelectronics.Conductive andmagneticfilamentsarerevolutionizingthe3DPtechnologytoanewlevel. Funding ThisstudywassupportedbytheCoordenaçãodeAperfeiçoamentodePessoaldeNívelSuperior– CAPES,Brazil[FinancialCode001]. Company Product Material Extruder Temp (C°) Platform Temp (C°) Innofil3D Innoflex40,45,60 Thermoplastic Copolyester Elastomer(TPC) 230-250°C notavailable 0-30°C notavailable Formfutura CarbonFil PETG 230-265°C 0-60°C Ziro CarbonFiber Filament ConductiveFilament PLA ABS 210-240°C 210-250°C donotneed 100-110°C Proto-pasta Electrically Conductive CarbonFiber PLA HTPLA,PLA 210-250°C 210-230°C donotneed donotneed Matterhackers NylonX PROSeriesCarbon ColorFabbXT-CF20 CarbonFiber Reinforced Nylon PETG PLA PLA PLA 250-265°C 240-260°C185- 205°C 240-260°C 190-210°C 60-65°C 60-70°C donotneed 70-90°C donotneed Yasin3D SpoolConductiv CarbonFiber LightWeightCarbon ABS ABS,PLA ABS 200-260 donotneed Hawkvine CarbonFiber PLA,ABS,PETG,Nylon 210-240°C 210-240°C 50°C 50°C Haydale Graphene-enhanced PLA 200-210°C 58°C AtomicFilament CarbonFiber Extreme CarbonFiberUltra PLA, PETG ABS 190-230°C 240-265°C 235-255°C notavailable Sunlu SuperSept Conductive highstrength ABS PLA,ABS PLA 190-220°C 190-220-°C 210-240°C notavailable Icefilaments CARBON PET notavailable notavailable Dezhijian HighRigidity ConductiveABS Carbonfiber ABS ABS PETG 230-270°C 230-260°C 230-250°C donotneed 100-120°C 80-100°C 3DPrinterPro Carbonfiber ABS 220-260°C notavailable Graphene3DLab Graphene PLA,ABS notavailable notavailable Table 1. 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Horst has Post-Doctorate in Mechanical Engineering and Sciences, Federal University of Santa Catarina, UFSC (2018-2019). D.Eng of Production from Federal University of Technology - Paraná, UTFPR (2016). M.Eng of Production from Federal University of Technology - Paraná (2013). Bachelor’s at Biology from Leonardo da Vinci Universitary Center (2009). Bachelor’s at Mechanical Technology from Santa Catarina State University, UDESC (2010). Professional Technician in Electromechanics from National Service of Industrial Apprenticeship, SENAI (2005). Currently is a researcher in the following areas: Bioengineering, Nanotechnology, Graphene and Carbon Nanostructures, Ceramic Materials, Polymerics and Metals, Electro-Mechanics, Renewable Energies, and Innovation, Technology and Sustainability. Pedro Paulo Andrade, Jr., has a PhD in Industrial Engineering, graduated in Economics Engineering from the Federal University of Santa Catarina (UFSC). Currently he is associate professor at the Federal University of Santa Catarina. He has several articles published and has participated in diverse symposiums and conferences. Supervises PhD and master’s degrees projects and thesis, as well as specialization and undergraduate students, always seeking to meet the premise of the Brazilian public university: by teaching, researching and helping in community extension projects. Areas of knowledge from the past five (5) years: economics engineering and cost analysis; management of technological innovation; economy and transport planning Yang,Z.,Chabi,S.,&Zhu,Y.(2015).Preparationof3Dgraphene-basedarchitecturesandtheirapplicationsin supercapacitors.Prog. in Nat.Sci.: Mat. Int.,25(6),554–562. Yao, X., Luan, C., Zhang, D., Lan, L., & Fu, J. (2017). 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