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Volume34,Issue2
March/April2015
Pages485491
Remediation/Treatment
Experimentalinvestigationofglasscontentofblastfurnaceslagbydrygranulation
JunxiangLiu, QingboYu
Firstpublished:
13September2014
DOI:
10.1002/ep.12024
Citedby:
0articles
, WenjunDuan, QinQin
Fullpublicationhistory
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Abstract
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ExperimentalinvestigationofglasscontentofblastfurnaceslagbydrygranulationLiu2014EnvironmentalProgress&SustainableEnergyWileyOnlineLibrary
Drygranulation,asanewprocessofmoltenblastfurnaceslag(BFS)treatment,isanattractivealternativetowaterquenching.The
performanceofBFSobtainedfromdrygranulationmustbeassessed.Theglasscontent,whichisasignificantfactortoevaluatethe
performanceofBFSasareplacementmaterialforPortlandcement,wasinvestigatedusingtheXraydiffractionmethod.Theresults
indicatedthattheglasscontentofBFSdecreasedastheslagdropletvelocitywasincreasedanddecreasedwithanincreaseinthe
diameteroftheslagparticles.Fora2.04m/svelocityand0.80mmdiameterofslagparticles,thevalueoftheglasscontentis94%,
whichishigherthanthe91%contentobtainedfromwaterquenching.Toobtainmuchhigherglasscontent,itisbettertocoolthe
moltenBFSfromahigherinitialtemperature.2014AmericanInstituteofChemicalEngineersEnvironProg,34:485491,2015
Providefeedbackorgethelp
INTRODUCTION
Blastfurnaceslag(BFS)isoneofthemostabundantsolidwastesdischargedfrommetallurgicalprocessing.BFS,whichiscomposed
mainlyofCaO,SiO 2 ,Al 2 O 3 ,andMgO,isanexcellentrawmaterialforglassceramics,cement,andaggregate.BFScanhavean
amorphousorglassystructure,whichisformedbyrapidlycoolingtheslag,usuallybywaterquenching.Theglassyslaghaspropertiesof
hydrationandcanbeusedasapartialsubstituteforPortlandcement[ 13 ].Glassyslagisavaluableproductandcanindirectlysave
energyinthecementindustry[ 4 ].Currently,BFS,whichisproducedattemperaturesrangingfrom1450to1650C,istreatedbywater
quenching.InChina,approximately189milliontonsofBFSwereproducedin2011.MostoftheBFSwereusedascementadmixtureor
gravelinroadpavement.Intheprocessofwaterquenching,theheatoftheslagisnotrecovered,despitethelargeheatcontentofmolten
slag.Moreover,largeamountsofenergyareconsumedduringwaterquenching,andharmfulwasteisdischargedintotheenvironment.
Drygranulationformoltenslaghasrecentlyreceivedaconsiderableamountofattentionduetoenvironmentalandenergyconsiderations[
57 ].Thegranulationisperformedusingarotarycuporairblastatomizer.Theparticlesarecooledastheytravelthroughtheairand
thenarecooledfurtherinacoolingbed[ 8 ].ItisnecessarytodemonstratethatBFSobtainedfromdrygranulationcanbeusedasa
replacementmaterialforPortlandcement.
Thereactivityoftheslagisconsideredtobeanimportantparameterforassessingitssuitabilityasacementreplacingmaterial,anditis
influencedbyslagpropertiessuchaschemicalcomposition,glasscontent,fineness,andparticlesizedistribution[ 914 ].Thefineness
andparticlesizedistributioncanbecontrolledbytheoperatingparametersofmilling.Thus,theutilizationofdrygranulationslagis
determinedbytheglasscontent.Douglasetal.studiedtheinfluenceofthechemicalcomposition,glasscontent,andparticlesize
distributiononthecompressivestrengthforthreeBFSs[ 15 ].Theyfoundthatincreasingtheglasscontenthadlittleeffectonthe
compressivestrengthwhenthevalueofglasscontentisover88%.Escalanteetal.foundthattheslagwithahigherglassyfraction(97%)
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exhibitedhigherreactivitythantheslagwithalowerglassyfraction(53.5%)[ 16 ].Thus,glasscontentisasignificantparameterforthe
reactivityofBFS.
Inthisstudy,thequantitativeXraydiffractionmethodwasappliedtoevaluatetheglasscontentofslagparticlesobtainedfroma
laboratoryscaletestofdrygranulation.Themechanismofglassphaseformationwasinvestigatedaccordingtothetheoryof
crystallization.TheXraydiffractionpatternsofslagparticleswereanalyzedtoassesstheperformanceofBFSslag.Theeffectsof
velocity,thediameteroftheslagparticles,andtheinitialtemperatureofmoltenslagontheglasscontentofBFSweredetermined.
MATERIALSANDMETHODS
ParticlesfromDryGranulation
Thesphericalslagparticlesusedinthisstudywereobtainedfromdrygranulation.Theexperimentalapparatusfordrygranulation
consistedofthreeparts,includingatundish,rotarydevice,andslagcollector,asshowninFigure1a.Thehightemperaturemoltenslag
waspouredintorotarycupthroughthetundish.Thedistancebetweenthetundishandrotarycupwaskeptconstantat500mm.Theslag
collector,2.2mindiameter,whichwasusedtocollectslagparticles,wasmadeofstainlesssteelplatesbywelding.Therotarycupwas
connectedtoanelectricmotorbyflange,andtheangularspeedoftheelectricmotorwascontrolledbyaspeedcontroller.Intheprocess
ofdrygranulation,themoltenslag,whichwasheatedbyelectricfurnace,waspouredintotherotarycupwithahighrotatingspeed.Under
theactionofcentrifugalforce,theliquidslagreleasedfromtheedgeofrotarycupwasgranulatedintosmallsphericalparticles.Theglass
phaseformedinaparticularcoolingratewhentheparticletraveledthroughtheair.Figure1bshowsthegranulationofmoltenslagviathe
rotarycup.Inthisstudy,thesampleparticleswereselectedonebyone.Thevalueofparticlediameterismeasuredbymicrometer,and
thevalueoferroris0.003mm.Thus,theparticleswithdiameterof0.80mm,1.22mm,1.72mm,2.25mm,and2.85mmwereobtained,
respectively.Thechemicalcompositionoftheslagparticleswasanalyzedbyinductivelycoupledplasmaatomicemissionspectrometry
(ICPAES,IRISAdvantage,US),andthemainchemicalcomponents(masspercent,%)oftheslagwereCaO41.21,SiO 2 34.38,Al 2 O 3
11.05,MgO8.22,andTiO 2 0.35.
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Figure1.
Openinfigureviewer
(a)Schematicdiagramofexperimentalapparatus.(b)Photographofgranulationofmoltenslag.[Colorfigurecanbeviewedin
theonlineissue,whichisavailableatwileyonlinelibrary.com.]
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SamplePreparationforXRayDiffraction
Tocompareglasscontentofparticlesobtainedfromdrygranulationwiththatofparticlesobtainedfromwaterquenching,therewastwo
kindsofsamplepreparation.Thefirstissamplepreparationofparticlesobtainedfromwaterquenching,andthesecondissample
preparationofparticlesobtainedfromdrygranulation.TheparticlesbywaterquenchingwereobtainedfromAnsteel.Inthefirstsample
preparation,theslagparticlesweredriedat1055Candpouredintothemillcontainerwithanappropriateamountofcyclohexane.To
reducethemaximumdiameterofalloftheparticlestolessthan20m,themixtureshouldbegroundforsometime.Finally,themixture
wasdriedagainatroomtemperatureinafumecupboardtoremovethecyclohexane.Inthesecondsamplepreparation,theparticles
werepouredintothemillcontainerwithanappropriateamountofcyclohexanedirectly.Then,theprocedureofsamplepreparationwas
thesameasthatofthefirstsamplepreparation.
CalculationoftheGlassContent
AccordingtoBSEN151671:2006,thesampleswereanalyzedusinganXraydiffractometersystem(X'PertPro)[ 17 ].Thetest
conditionswereaCuKsourcedriven,40kVand40mAandascanningspeedof1/min.TheXraydiffractionpatternofslagwithglass
andcrystallinematerialcomponentisshowninFigure2.Drawastraightlineacrossthediffractionpatternsuchthatitpassesthroughthe
pointsoftheinterplanarspacingvaluesbetween0.404nmand0.237nmwhencopperKradiationwasused,i.e.,at22and38,
respectively.Thislinerepresentsthelinearbackgroundassociatedwiththediffractionpattern.Consideronlythoseareasinthecalculation
thatarecontainedwithintheregionsbetween22and38andthatareabovethelinearbackground.Definetheamorphousregion
between22and38bydrawingalinethroughthemidpointofthevariationofdiffractedintensityrepresentingthehump,interpolatingits
pathbelowthosediffractionsthatareduetocrystallinematerial.
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Figure2.
Openinfigureviewer
SchematicrepresentationofaportionofXraydiffractionpattern.
Themasscontentofglass( G )canbecalculatedbythefollowingequation.
(1)
where W 1 isthemassofglassintheslagand W 2 isthemassofcrystallinematerialintheslag.
ChungproposedamatrixflushingmethodforquantitativemulticomponentanalysisbyXraydiffraction[ 18 ].Hefoundthattheratioof
crystallinematerialtoglasscanbeexpressedasfollow:
(2)
where I c istheintensityofcrystallinematerial, I g istheintensityofglass,and K istheslagglassquotient.IntheXraydiffractionpattern,
theratio, I c / I g ,canbeexpressedasfollows[ 19,20 ]:
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(3)
Table1.RatioofpurelyglassyBFStopurelycrystallineBFS.
PurelyglassyBFS, W 1 (g)
PurelycrystallineBFS, W 2 (g)
W 2/ W
18.2600.001
1.7400.001
0.09530.0001
0.1070.006
18.2600.001
2.1400.001
0.11720.0001
0.1320.003
18.2600.001
2.5400.001
0.13910.0001
0.1520.004
18.2600.001
2.9400.001
0.16100.0001
0.1820.006
18.2600.001
3.3400.001
0.18290.0001
0.2030.005
18.2600.001
7.7400.001
0.42390.0001
0.4720.004
18.2600.001
11.7400.001
0.64290.0001
0.7140.002
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I c/ I
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Figure3.
Openinfigureviewer
Relationshipbetween W 2 / W 1 and I c / I g .
Themechanismofmatrixflushingmethodisthesameasthatofdegreeofcrystallinity(DOC)method,inwhichtheweightfractionof
glassymaterialcanbeexpressedasfollows.
(4)
Madsen etal .[ 21 ]foundthattheDOCmethodprovideshighaccuracywhentheglasscontentishigh.Therelativebiaswaslowerthan
3%whentheglassycontentwashigherthan50%.
RESULTSANDDISCUSSION
XRayDiffraction
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Figure4.
Openinfigureviewer
XraydiffractionpatternsofBFSwithdifferentdegreesofcrystallization.
Figure5showstheXraydiffractiontracesforsamplesA,B,andC.Figure5ashowsthattheonlycrystallinephaseinBFSwith100%
crystallinematterwasakermanite(2CaOMgO2SiO 2 ),whichisconsistentwiththeresultsofPurwanto etal .,Williamson etal .,and
RogersandWilliamson[ 2224 ].Figures5band5cshowthatthemaincrystallinephaseinBFSwasmerwinite(3CaOMgO2SiO 2 ),
whichisconsistentwiththeresultsofFredericcia etal .[ 25 ].Fredericcia etal .foundthattheprimarycrystallinephasewasmerwinite,
with10%Al 2 O 3 intheCaOSiO 2 Al 2 O 3 MgOsystem.InsampleB,asmallamountofgehlenite[ 23,24 ](2CaOAl 2 O 3 SiO 2 )canbe
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observed.InpreparationofsampleA,BFSwasheatedto1500Cinanelectricfurnace,for12h,andwasthencooledinairuntiltheinner
temperatureofelectricfurnacedroppedto25C.TheonlycrystallinephaseinBFSwasakermaniteundertheconditionofslowcooling.In
theprocessofwaterquenchingordrygranulation,BFSwascooledrapidly,from1500Cto100Cinafewseconds.Therewasalmostno
akermaniteformedinBFS,butasmallamountofmerwiniteformedinit.
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Figure5.
Openinfigureviewer
(a)XraydiffractionpatternofBFSwith100%crystalline.(b)XraydiffractionpatternofBFSwith91%glass.(c)Xraydiffraction
patternofBFSwith94%glass.
EffectofSlagDropletVelocity
ThemoltenBFS,whichwassuppliedtothecenteroftherotarycup,accumulatedalongtheedgeoftherotarycupasathinliquidtorus.
Duetotheactionofthecentrifugalforce,theliquidtorusbecameunstablereleasingfromtheedgeofrotarycup,andchangedintoseveral
ligamentarystreams.Next,theligamentarystreamsbrokedownintodropsduetothegrowthofdisturbancealongthem,asshownin
Figure2.Thefrictionbetweenmoltenslagandtheinnerwalloftherotarycupenabledmoltenslagtoattainthesamerotationalvelocityas
thatoftherotarycup.Theradialvelocitycomponentofmoltenslagcanbenegligibleincomparisonwiththetangentialvelocityofthe
rotarycup.Therefore,themoltendropspersistedintheirinitialvelocityandwerecooledbythesurroundingair.
Inordertoobtainglassyslag,theliquiddropletmustbecooled,withoutcrystallizationintervening,toasufficientlylowtemperature.The
increaseofviscositywithdecreaseoftemperaturecausesittoreachastateofsuchhighviscositythatitactseffectivelylikeasolid[ 26 ].
Thus,theglasscontentinslagparticlesisdeterminedbythecoolingrateofliquidslagdroplets.
Figure6showstheXraydiffractionpatternsofBFSatdifferentslagdropletvelocitiesfora2.25mmdiameterslagdroplet.Thepatterns
indicatethattheheightofpeakMincreasedandthattheareaofhumpbecamesmallerwithanincreaseintheslagdropletvelocity.Figure
7showstherelationshipbetweentheslagdropletvelocityandtheglasscontent.Therangeofglasscontentis893%to76.03%.Itis
clearthattheglasscontentofBFSdecreasedastheslagdropletvelocitywasincreased.Theminimumvalueoftheglasscontentwas76
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3%,andBFStreatedbydrygranulationcanbeusedasacementreplacingmaterial.AccordingtoBSEN151671:2006,theglass
contentofBFS,whichwillbeusedascementreplacingmaterial,shallnotbelessthan67%.Foragivendiameterslagdropletorparticle,
thecoolingspeed,whichisdeterminedbyitsvelocity,determinedtheglasscontentoftheBFS.Inheattransferenhancementterms,there
willbeahighercoolingrateasthevelocityofslagdropletisincreased[ 27 ].
Figure6.
Openinfigureviewer
XraydiffractionpatternsofBFSatdifferentslagdropletvelocity.
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Figure7.
Openinfigureviewer
Relationshipbetweenslagdropletvelocityandglasscontent.
Intheexperiment,theflightdistancewasonly1.1m,andtherewaslittletimeforcoolingatthevelocityofslagdroplet,1.33.5m/s.
Subsequently,thehigheristhevelocity,theearlierthedropletsarriveattheslagcollectorandthelongertimetheyspendonthisslag
collector,wherethecoolingratesarerelativelylow.Therefore,theextentofcrystallizationoftheparticlesislargerwhenthevelocity
increases,whichisconsistentwiththeresultsofQin etal .[ 28 ].Duetothelowcoolingrate,itwasbeneficialtotheformationof
crystallization.Toobtainahighglasscontent,theremustbealargediameterslagcollectorforthecoolingtobesufficientlyrapid.
EffectoftheSlagParticleDiameter
Figure8showstheXraydiffractionpatternsofBFSatdifferentdiametersfora2.04m/svelocityofslagparticle.Itisclearthattheheight
ofpeakMincreasedastheslagparticlediameterwasincreased.Atthesametime,theareaofhumpbecamesmallerduetothelower
glasscontent.Figure9showstherelationshipbetweendiameteroftheslagparticlesandtheglasscontent.Therangeoftheglass
contentis943%to70.03%.ThisresultindicatesthattheglasscontentoftheBFSdecreasedwithanincreaseindiameteroftheslag
particles.Themaximumvalueoftheglasscontentwas943%,whichwashigherthan913%obtainedfromwaterquenching.The
minimumvalueofglasscontentwithadiameterof2.85mmwas703%,morethan67%,andtheparticlescanbeusedasacement
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replacementmaterial.Therefore,insomeparticularoperatingparameters,drygranulation,whichisanewtechniquetocoolmoltenBFS,
isbeneficialfortheresourceutilizationofBFS.
Figure8.
Openinfigureviewer
XraydiffractionpatternsofBFSatdifferentdiameter.
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Figure9.
Openinfigureviewer
Relationshipbetweendiameterandglasscontent.
Theglassystructureformisgreater,thesmalleristhecrystallizationrateandthelargeristhecoolingrate[ 29 ].Theheattransfer
coefficientdecreasedasthediameterofslagparticlewasincreased.Foragivenslagdropletvelocity,thesmalldiameterslagparticlemay
cooldownquicklyandestablishahighdegreeofundercooling,andthelargediameterslagparticlecooleddownslowlyduetotheirhigh
mass.Asaresult,thereisahighglasscontentofslagparticleswithsmalldiameter.
Intheprocessofdisintegrationbyarotarycup,therewillbelargeamountofparticleswitharangeofparticlesize.Theaveragediameter
oftheparticlesisdeterminedbytherotaryspeedoftherotarycup[ 30 ].Atahighrotaryspeed,therewillbemorelittlediameterparticles
emerge,whichresultinlowvalueoftheaveragediameter.However,thehighrotaryspeedrequiresalargediameterofthedrygranulation
device,whichmayresultinahighcostofslagtreatment.TheoptimaloperatingparametersofdrygranulationtoreuseBFSwithalowcost
mustbedetermined.
EffectoftheInitialTemperature
DefinethetemperatureofmoltenBFStakenfromtheelectricfurnaceastheinitialtemperature.ThemoltenBFSwaspouredintothe
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centerofrotarycupthroughthetundishandbrokenupintosmallsphericalparticles.Duringtheprocess,thetemperatureofslagparticles
wasconsistentwiththeinitialtemperatureofthemoltenBFS.Figure10showstheXraydiffractionpatternsoftheBFSatthreedifferent
initialtemperaturesfor2.25mmdiameterslagparticleanda2.04m/svelocity.TheheightofpeakMdecreasedwithanincreaseinthe
initialtemperatureofthemoltenBFS.Theslagparticlesobtainedat1500Cweretransparentandtheslagparticlesobtainedat1400C
werecloudy.Thisphenomenonindicatedthattheglasscontentoftheformerslagparticleswashigherthanthatofthelatterones.
Figure10.
Openinfigureviewer
XraydiffractionpatternsofBFSatdifferentinitialtemperature.
Figure11showstherelationshipbetweentheinitialtemperatureandtheglasscontent.ItisclearthattheglasscontentoftheBFS
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increasedastheinitialtemperatureofmoltenBFSwasincreased.Asmentionedabove,thereisaglassyphaseinamoltenstate,anda
higherinitialtemperatureresultsinalargeramountofglassyphasebecauseaveryhighinitialtemperatureresultsincompletemelting
andtotaleliminationofallofthenuclei/embryosinthesystem.
Figure11.
Openinfigureviewer
Relationshipbetweeninitialtemperatureandglasscontent.
CONCLUSIONS
Thisstudyfocusedontheeffectofvelocity,diameteroftheslagparticles,andinitialtemperatureofthemoltenslagontheglasscontentof
theBFSobtainedfromthelaboratoryscaledrygranulation.ThemaingoalwastoassesstheperformanceofBFSparticles,obtainedfrom
drygranulationasareplacementmaterialforPortlandcement.
ByanalyzingXraydiffractionpatterns,theonlycrystallinephaseinBFSwith100%crystallinematerialwasfoundtobeakermanite.
Becauseofrapidcooling,themaincrystallinephaseinBFSobtainedfromwaterquenchinganddrygranulation,wasmerwinite.Inthe
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processofdrygranulation,themaximumvalueoftheglasscontentwas943%,whichwashigherthanthe913%obtainedfromwater
quenching.TheglasscontentofBFSdecreasedasthevelocityoftheslagparticlewasincreasedanddecreasedwithanincreaseinthe
diameterofslagparticles.Toobtainamuchhigherglasscontent,itisbettertokeepthemoltenBFSatahigherinitialtemperature.
Therefore,theoptimaloperatingparametersofdrygranulationtotransformBFSintoresourceswithahighvalueaddedmustbe
determined.
ACKNOWLEDGMENTS
ThisresearchwassupportedbytheNationalNaturalScienceFoundationofChina(51274066,51304048),theNationalScience
FoundationforPostdoctoralScientistsofChina(2013M541240),theFundamentalResearchFundsfortheCentralUniversities
(N130402019),andtheNationalKeyTechnologiesR&DProgramofChina(2013BAA03B03).
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