以太西无烟煤为碳源制备单壁碳纳米管

614Vol161No1420104CIESCJournalApril20101,1,1,1,2(1,,116012;2,116023):,,,,,Y2O3Ni,0105MPa,,;40%();115214nm,199m2g-1,01388cm3g-1,60%,C2CN:;;;:TQ536;TB383:A:0438-1157(2010)04-1040-07Preparationandcharacterizationofsingle2walledcarbonnanotubesfromTaixianthraciteLIZhentao1,DONGQiang1,LIUHong1,QIUJieshan1,2(1CarbonResearchLaboratory,CenterforNanoMaterialsandScience,StateKeyLaboratoryofFineChemicals,SchoolofChemicalEngineering,DalianUniversityofTechnology,Dalian116012,Liaoning,China;2KeyLaboratoryforMicro/NanoTechnologyandSystemofLiaoningProvince,DalianUniversityofTechnology,Dalian116023,Liaoning,China)Abstract:Single2walledcarbonnanotubes(SWCNTs)arepreparedinlargescalefromTaixianthracitecoalusingarcdischargetechnique1Thepropertiesofthearcplasmaduringthearcingprocessareanalyzedinsituusingopticalemissionspectroscopy(OES)andarecorrelatedtotheyieldofSWCNTstounderstandthegrowthmechanismofSWCNTs1TheSWCNTsarecharacterizedbyTEM,TGA,RamanspectroscopyandN2adsorptiontechnique1TheresultsshowthatTaixianthraciteisasuitablecarbonsourceformassproductionofSWCNTswithY2O3andNiascatalystsataheliumpressureof0105MPa1TheyieldofSWCNTsincreasesasthecarbonizationtemperatureofcoal2basedanodeincreases1IntheSWCNTs,therearemetalsandmineralsthataccountforabout40%(mass).Thecoal2basedSWCNTshaveadiameterof115214nmandasurfaceareaof199m2g-11TheOESanalysisrevealsthatactivespeciessuchasC22009-10-27,2009-12-23::(1981),,:(20725619,20836002)Receiveddate:2009-10-27.Correspondingauthor:Prof.QIUJieshan,jqiu@dlut1edu1cnFoundationitem:supportedbytheNationalNaturalScienceFoundationofChina(20725619,20836002).dimersandCNspeciesarepresentinthearcingplasmaandtheactiveintermediatesinvolvedintheformationandgrowthofSWCNTs.Keywords:single2walledcarbonnanotubes;coal;arcdischarge;opticalemissionspectroscopy(SWCNTs)[122],SWCNTsSWCNTs,[3210][11][12],,SWCNTsSWCNTsMansour[13]SWCNTs,SWCNTs,SWCNTs,SWC2NTs,,,,,SWC2NTs[14215],SWCNTs,,,,,(),,,(OES),,SWCNTs,SWCNTs,,,1111SWCNTs1SWCNTs,[14215],:150m200m,10MPa10mm,N2,,,,,,,23mm,,1Table1AnalysisdataofTaixicoalProximateanalysis/%(mass)MadAdVdafUltimateanalysis/%(daf,mass)CHNSO111031259126921193105111811072151bydifference.112SWCNTsSWCNTs:(TEM,PhilipsTecnaiG220,200kV);(TGA/SDTA851e,50mlmin-1,10min-1,25,900);(Raman,JYLabRamHR800,He2Ne,14014:63218nm);(ASAP22020,77K,3005h)1131,Andor(EMCCD,1600400),,,EMCCD,1Fig11OESanalysissystem2211900,SWCNTs2,2,SWCNTs,0103MPa,SWCNTs,2SWCNTsFig12VariationofSWCNTsyieldwithHepressure0105MPa;0105MPa,SWCNTsSWCNTs,0105MPa212900,0105MPa,SWCNTs,22,YNi,SWCNTs,Y2O3Ni1120100()SWCNTs,SWCNTs,,SWCNTs[16]213SWCNTs,2SWCNTsTable2EffectofcatalystsontheyieldofSWCNTsCatalystRatioofcatalysts(mass)Erosionrateofanode/mgs-1ArHeProductionrateofSWCNTs/%ArHeYFe72071401070120YNi7206901706181YNi3151071001144156YNiS72026901151123YFeS720261001360128Y2O3Ni112068017510189CoNi3371201210115FeSNi715561201210114FeS196901281100240161Themassofcoalis100g.,,,,,HNO,,SWCNTs3SWCNTs,3,SWCNTs,:,,,,SWCNTs;,,,C23SWCNTsFig13VariationofSWCNTsyieldwithcarbonizationtemperatureofcoal2basedcarbonrods4XRD4,,(002),214SWCNTsY2O3Ni,900,0105MPa,SWCNTs10%,SWCNTsSWCNTs5SWCNTs,,SWCNTs,1020nm,,,SWCNTs,;DG,6SWCNTs,61584cm-1G1320cm-1D,IG/ID16D34014:[17],,SWCNTs(RBM),3,107149165cm-1,SWCNTs,r=238/d0193[18],SWCNTs213611651148nm6SWCNTsFig16RamanspectrumofSWCNTsderivedfromTaixicoalSWCNTs7SWCNTs,,380,SWCNTs,,720,,,SWCNTs40%()7SWCNTsFig17TGcurveofSWCNTsderivedfromTaixicoal8SWCNTs,P/P00101,,;P/P00101018,,,;P/P0018,,,,BET199m2g-1,01388cm3g-1,60%BJH,23nm,SWCNTsSWCNTsSWCNTs,SWCNTs,SWCNTs,8SWCNTsFig18N2adsorptionisothermandporesizedistributionofSWCNTs215SWCNTs,9,437474515563612nmC2(Swand3g-a3u)v=210-1-2C2,,,,C2,4401619Fig19OESspectrumofarcplasmaduringarcingcoal2basedcarbon400nmC3[19221],[22223],C2,385132386110386197388115nmCN(violetsystem),10,N,Makita[24]N10CNFig110OESspectrumofCN3,SWCNTs,SWCNTs,Y2O3Ni,,0105MPa,SWCNTsSWC2NTs,SWCNTs115214nm,199m2g-1,01388cm3g-1,SWCNTsC2CNReferences[1]IijimaS,IchihashiT1Single2shellcarbonnanotubesof12nmdiameter1Nature,1993,363:6032605[2]BethuneDS,KiangCH,DeVriesMS,etal1Cobalt2catalysedgrowthofcarbonnanotubeswithsingle2atomic2layerwalls1Nature,1993,363:6052607[3]JournetC,MaserWK,BernierP,etal1Largescaleproductionofsinglewalledcarbonnanotubesbytheelectricarctechnique1Nature,1997,388:7562758[4]LiuChang(),CongHongtao(),ChengHuiming(),etal1Synthesisofsinglewalledcarbonnanotubesbyasemicontinuoushydrogenarcmethod1NewCarbonMaterials(),2000,15(2):125[5]LiuChang(),ChengHuiming().Synthesisofcarbonnanotubesbyelectricarcmethod1NewCarbonMaterials(),2001,16(1):67271[6]KeidarM1Factorsaffectingsynthesisofsinglewallcarbonnanotubes1Science,1996,273:4832487[7]LX,DuF,MaYF,etal1Synthesisofhighqualitysingle2walledcarbonnanotubesatlargescalebyelectricarcusingmetalcompounds1Carbon,2005,43:202022022[8]MakitaY,SuzukiS,KatauraH,etal1Synthesisofsinglewallcarbonnanotubesbyusingarcdischargetechniqueinnitrogenatmosphere1TheEuropeanPhysicalJournalD,2005,34:2872289[9]YaoMG,LiuBB,ZouYG,etal1Synthesisofsingle2wallcarbonnanotubesandlongnanotuberibbonswithHo/Niascatalystbyarcdischarge1