Advances in Electrokinetic Remediation For The Removal of Organic Contaminants in Soils - InTechOpen

11/20/2015
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EnvironmentalSciences"OrganicPollutantsMonitoring,RiskandTreatment",bookeditedbyM.
NageebRashed,ISBN9789535109488,Published:January30,2013underCCBY3.0license.
TheAuthor(s).
Chapter9
AdvancesinElectrokineticRemediationfortheRemovalofOrganicContaminantsinSoils
ByClaudioCameselle,SusanaGouveia,DjamalEddineAkretcheandBoualemBelhadj
DOI:10.5772/54334
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1.Introduction
MailtoaFriend
2.Electrokineticremediation:Basisandapplications
Figure1.Applicationoftheelectrokineticremediationinacontaminatedsite.
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Figure2.Transportmechanismsinelectrokineticremediation
3.Removaloforganiccontaminantsbyelectrokinetics:Limitationsandenhancements
3.1.Electrokineticremovalofsolubleorganics
Figure3.Chemicalstructureofreactiveblack5
Figure4.RemovalofReactiveBlack5fromakaolinspecimenbyelectrokineticremediation
3.2.Cosolvents
3.3.Surfactants
3.4.Cyclodextrins
4.Combinedtechnologies
4.1.Electrokineticsandchemicaloxidation/reduction
4.2.Electrokineticsandpermeablereactivebarriers
4.3.Bioelectroremediation
4.4.Electroheating
5.Largescaleapplications
6.Futureperspectives
AdvancesinElectrokineticRemediation
fortheRemovalofOrganicContaminants
inSoils
ClaudioCameselle1,SusanaGouveia1,DjamalEddineAkretche2andBoualemBelhadj2
[1]DepartmentofChemicalEngineering,UniversityofVigo,BuildingFundicion,Vigo,
Spain
[2]LaboratoryofHydrometallurgyandInorganicMolecularChemistry,Facultyof
Chemistry,USTHB,BP32,ElAlia,BabEzzouar,Algiers,Algeria
1.Introduction
Soilcontaminationisassociatedtoindustrialactivities,miningexploitationsandwaste
dumping.Itisconsideredaseriousproblemsinceitaffectsnotonlytheenvironment,living
organismsandhumanhealth,butalsotheeconomicactivitiesassociatedwiththeuseofsoil
[1].Therisksassociatedwithsoilcontaminationandsoilremediationareimportantpointsin
theagendaofpoliticians,techniciansandscientificcommunity.Thepresentlegislation
establishesalegalframetoprotectthesoilfrompotentiallycontaminantactivitieshowever,
thepresentsituationofsoilcontaminationistheresultofbadpracticesinthepast,especially
relatedtobadwastemanagement[23].
Soilcontaminationaffectslivingorganismsinthesubsurfacebutalsoaffectstheplantsthat
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accumulatecontaminantsastheygrow.Thus,contaminantsenterthefoodchainwitha
potentialimpactinpublichealth[4].Ontheotherhand,contaminantscanbewashedoutthe
soilbyrainandgroundwater,resultinginthedisseminationofthecontamination.This
processisnotdesirablebecausetheareaaffectedbythecontaminantsisbiggerandbigger
andthepossibleremediationismoredifficultandcostlyastheaffectedareagrows[5].
Therefore,soilcontaminationisaseriousproblemthatrequiresarapidsolutioninorderto
preventmoreenvironmentaldamages.Preventionisthebesttechnologytosaveoursoils
fromthecontamination.Astrictmanagementofthewastesandgoodenvironmental
practicesassociatedtoindustrialactivities,mining,transportationanddumpingmanagement
arerequiredtopreventthecontaminationoftheenvironment.However,manysiteshave
beenidentifiedascontaminatedsites.TheEuropeanUnion,USA,Canada,JapanandSouth
Koreamadealotofeffortsinrecentyearstoidentifythecontaminatedsitesineachcountry.
Thenewlegislation,especiallyintheEuropeanUnion,forcestheadministrationtoidentify
thecontaminatedsitesandevaluatetherisksassociatedtotheenvironmentandpublic
health.Then,theremediationofthosesitesmustbecarriedout,startingwiththeriskiersites
forhumansandlivingorganisms[6].ThisistheaimofthepresentlegislationinSpainabout
themanagementofwastesandsoilcontamination[7,8]whichisthetranspositionofthe
EuropeanDirective2008/98/CE[9].
Soilremediationimpliestheapplicationofatechnologyabletoremoveoreliminatethe
contaminantsfollowingbytherestorationofthesitetotheoriginalstate.Sofar,itsounds
easytodo.However,thereisnotatechnologyabletoremoveanykindofcontaminantsin
anykindofsoil.Moreover,therestorationofthesitetotheoriginalstateisnotalways
possibleduetothecharacteristicsofthesoiland/ortheremediationtechnology.Thus,the
commonobjectiveinsoilremediationistoremovethecontaminantstoasafelevelfor
humansandtheenvironment,andrestorethepropertiesofthesoiltoastateappropriatefor
thecommonsoiluses[1012].So,thefinaltargetconcentrationtoconsiderthesoilnon
contaminatedwillbedifferentdependingonthefutureuseofthesoil:urban,agricultureor
industrial.
Duringthelast20years,scientistandtechniciansspentalotofeffortsinthedevelopingof
innovativetechnologiesforsoilremediation[13].Thosetechnologiesusethephysical,
chemicalandbiologicalprinciplestoremoveand/oreliminatethecontaminantsfromsoil.
Thus,forinstance,bioremediationusesthecapacityofsoilmicroorganismstodegrade
organiccontaminantsintothesoil[14].Thermaldesorptionwasdesignedtoremovevolatile
andsemivolatileorganics.Gasoline,BETX,chlorinatedorganicscanberemovedby
thermaldesorption,butalsoPAHsorPCBs[15].Soilwashingusesasolutioninwaterto
dissolvethecontaminantsfromsoil.Oncethesoilisclean,itcanbestoredinthesameplace
andthecontaminantswillundergoastabilizationprocess[16].Soilremediation
technologiescanbeappliedinsitu,i.e.inthecontaminatedsitewithoutexcavation,orex
situ:thesoilisexcavatedanditistreatedinafacilityspecificallydesignedforthe
remediationprocess.Insitutechnologiesarepreferredbecausetheyresultsinlowercosts,
lessexpositiontothecontaminantsandlessdisruptionoftheenvironment.However,the
controloftheoperationismoredifficultanddependingonthepermeabilityofthesoiland
soilstratification,theoperationmayresultsinverypoorresults.Ontheotherhand,exsitu
technologiespermitabettercontroloftheoperation,andtheremediationresultsarenotvery
affectedbysomesoilcharacteristicsaspermeabilityandstratification[1719].
2.Electrokineticremediation:Basisandapplications
Electrokineticremediationisanenvironmentaltechniqueespeciallydevelopedforthe
removalofcontaminantsinsoil,sedimentsandsludge,althoughitcanbeappliedtoany
solidporousmaterial[20].Electrokineticremediationisbasedintheapplicationofadirect
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electriccurrentoflowintensitytotheporousmatrixtobedecontaminated[21].Theeffect
oftheelectricfieldinducesthemobilizationandtransportationofcontaminantsthroughthe
porousmatrixtowardstheelectrodes,wheretheyarecollected,pumpedoutandtreated.
Mainelectrodes,anodeandcathode,areinsertedintothesoilmatrix,normallyinsidea
chamberwhichisfillwithwaterortheappropriatesolutiontoenhancetheremovalof
contaminants(Figure1).Typically,avoltagedropof1VDC/cmisappliedtothemain
electrodes.
Figure1.
Applicationoftheelectrokineticremediationinacontaminatedsite.
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Contaminantsaretransportedoutofthesoildueseveraltransportationmechanismsinduced
bytheelectricfield[22,23]:
Electromigrationisdefinedasthetransportationofionsinsolutionintheinterstitial
fluidinthesoilmatrixtowardstheelectrodeoftheoppositecharge(Figure2).Cations
movetowardthecathode(negativeelectrode),andanionsmovetowardtheanode
(positiveelectrode).Theionicmigrationorelectromigrationdependsonthesizeand
chargeoftheionandthestrengthoftheelectricfield.
Electroosmosisisthenetfluxofwaterorinterstitialfluidinducedbytheelectricfield
(Figure2).Electroosmosisisacomplextransportmechanismthatdependsonthe
electriccharacteristicsofthesolidsurface,thepropertiesoftheinterstitialfluidand
theinteractionbetweenthesolidsurfaceandthecomponentsinsolution.Theelectro
osmoticflowtransportsoutoftheporousmatrixanychemicalspeciesinsolution.
Soilsandsedimentsareusuallyelectronegative(solidparticlesarenegatively
charged),sotheelectroosmoticflowmovestowardthecathode.Inthecaseof
electropositivesolidmatrixes,theelectroosmoticflowmovestowardtheanode.
Detailedinformationaboutelectroosmosiscanbefoundinliterature[24].
Electrophoresisisthetransportofchargedparticlesofcolloidalsizeandbound
contaminantsduetotheapplicationofalowdirectcurrentorvoltagegradientrelative
tothestationaryporefluid.Comparedtoionicmigrationandelectroosmosis,mass
transportbyelectrophoresisisnegligibleinlowpermeabilitysoilsystems.However,
masstransportbyelectrophoresismaybecomesignificantinsoilsuspensionsystems
anditisthemechanismforthetransportationofcolloids(includingbacteria)and
micelles.
Diffusionreferstothemasstransportduetoaconcentrationgradient,nottoavoltage
gradientastheprevioustransportmechanisms.Duringtheelectrokinetictreatmentof
contaminatedsoils,diffusionwillappearasaresultoftheconcentrationgradients
generatedbytheelectromigrationandelectroosmosisofcontaminants.Diffusive
transportisoftenneglectedconsideringitslowervelocitycomparedto
electromigrationandelectroosmosis.
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Figure2.
Transportmechanismsinelectrokineticremediation
Thetwomaintransportmechanismsinelectrokineticremediationareelectromigrationand
electroosmosis[25].Theextentofelectromigrationofagiveniondependsonthe
conductivityofthesoil,soilporosity,pHgradient,appliedelectricpotential,initial
concentrationofthespecificionandthepresenceofcompetitiveions.Electromigrationis
themajortransportprocessesforionicmetals,polarorganicmolecules,ionicmicellesand
colloidalelectrolytes.
Theelectroosmoticflowdependsonthedielectricconstantandviscosityofporefluidas
wellasthesurfacechargeofthesolidmatrixrepresentedbyzetapotential.Thezeta
potentialisafunctionofmanyparametersincludingthetypesofclaymineralsandionic
speciesthatarepresentaswellasthepH,ionicstrength,andtemperature.Electroosmosisis
consideredthedominanttransportprocessforbothorganicandinorganiccontaminantsthat
areindissolved,suspended,emulsifiedorsuchsimilarforms.Besides,electroosmoticflow
thoughlowpermeabilityregionsissignificantlygreaterthantheflowachievedbyan
ordinaryhydraulicgradient,sotheelectroosmoticflowismuchmoreefficientinlow
permeabilitysoils[26].
Theapplicationofanelectricfieldtoamoistenporousmatrixalsoinduceschemical
reactionsintothesoilandupontheelectrodesthatdecisivelyinfluencesthechemical
transportationandspeciationofthecontaminantsandotherconstituentsofthesoil.
Chemicalreactionsincludeacidalkalinereactions,redoxreaction,adsorptiondesorption
anddissolutionprecipitationreactions.Suchreactionsdramaticallyaffectthespeciationof
thecontaminantsandthereforeaffectthetransportationandcontaminantremovalefficiency
[27].Themainreactionintheelectrochemical/electrokineticsystemsisthedecomposition
ofwaterthatoccursattheelectrodes.Theelectrolyticdecompositionofwaterreactions
generatesoxygengasandhydrogenions(H+ )duetooxidationattheanodeandhydrogen
gasandhydroxyl(OH )ionsduetoreductionatthecathodeasshowninequations1and2.
AtAnode(Oxidation):
0
2H 2 O 4e-+4H+(aq) +O2(gas) E =-1.229V
(1)
Options
ViewEquation
Bookmark
AtCathode(Reduction):
4H 2 O+4e- 2H 2(gas) +4OH
(aq)
E =-0.828V
(2)
Options
ViewEquation
Bookmark
Essentially,acidisproducedattheanodeandalkalinesolutionisproducedatthecathode,
therefore,pHinthecathodeisincreased,whilepHattheanodeisdecreased.Themigration
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ofH+ ionsfromtheanodeandOH fromthecathodeintothesoilleadstodynamicchanges

insoilpH.H+ isabouttwiceasmobileasOH ,sotheprotonsdominatethesystemandan
acidfrontmovesacrossthesoiluntilitmeetsthehydroxylfrontinazonenearthecathode
wheretheionsmayrecombinetogeneratewater.Thus,thesoilisdividedintowzoneswith
asharppHjumpinbetween:ahighpHzoneclosetothecathode,andalowpHzoneonthe
anodeside.TheactualsoilpHvalueswilldependontheextentoftransportofH+ andOH
ionsandthegeochemicalcharacteristicsofthesoil.Theimplicationsoftheseelectrolysis
reactionsareenormousintheelectrokinetictreatmentsincetheyimpactthe
absorption/desorptionofthecontaminants,thedissolution/precipitationreactions,chemical
speciationandthedegradationofthecontaminants.Moreover,pHchangesintothesoil
affectsthecontaminantmigration,andtheevolutionoftheelectroosmoticflowwhichis
decisiveintheremovalofnonchargedorganiccontaminants[20].Inelectrokinetic
remediation,itisalsocommontheuseofchemicaltoenhancethedissolutionandthe
transportationofthecontaminants.Theenhancingchemicalaregoingtointeractwiththe
soilandthecontaminants,thereforeitisnecessarytoevaluatethegeochemistryofthesoil
andthepossiblereactionswiththeenhancingchemicals,consideringatthesametimethe
effectofthepH,inordertodesignasatisfactorytechniquethatremovesoreliminatesthe
contaminantskeepingthenaturalpropertiesofthesoilforitsuseaftertheremediation
process.
3.Removaloforganiccontaminantsbyelectrokinetics:
Limitationsandenhancements
Electrokineticremediationwasfirstproposedandtestedfortheremovalofheavymetalsand
otherchargedinorganiccontaminantsinsoils,sedimentsandsludges.However,the
electrokineticremediationisalsousefulfortheremovaloreliminationoforganic
contaminants[28].Consideringthedifferentphysicochemicalpropertiesoftheorganic
contaminantscomparedtothepropertiesofheavymetals,theoperatingconditionsofthe
electrokinetictreatmentandtheenhancingchemicalswillberatherdifferentthanthoseused
forheavymetalpollutedsoils.Themaintransportationmechanismsinelectrokinetic
remediationare:electromigrationandelectroosmosis.Ingeneral,themoredangerousand
persistentorganiccontaminantsarenotsolubleinwater(whichistheinterstitialfluidin
naturalsoils)andareneitherionicnorionizablemolecules.Therefore,electromigration
cannotbeconsideredasthetransportmechanismsfororganiccontaminants.Electroosmosis
isthenetfluxofwaterinthesoilmatrixthatflowsthroughthesoilfromoneelectrodetothe
otherduetotheeffectoftheelectricfield.Electroosmoticflowmovestowardsthecathode
inelectronegativelychargedsoils,whichisthemostcommoncase.Again,organic
contaminantsarenotsolubleinwaterandthereforetheireliminationfromsoilscannotbe
achievedinanunenhancedelectrokinetictreatment.Inordertoachieveaneffectiveremoval
oreliminationoforganiccontaminantsfromsoils,theirsolubilityinhastobeenhancedwith
theuseofcosolvents,surfactantsoranyotherchemicalagent.Alternatively,theremovalor
eliminationoforganiccontaminantscanbeachievedbythecombinationofelectrokinetics
andotherremediationtechniquessuchaschemicaloxidation/reduction,permeablereactive
barriers,electrolyticreactivebarriersorthermaltreatment.Fortheremovaloforganic
contaminants,bothsolubilizationofthecontaminantsandadequateelectroosmoticfloware
required,whichappeartobequitechallengingtoaccomplishsimultaneously.Theelectro
osmoticflowisfoundtobedependentonthemagnitudeandmodeofelectricpotential
application.Theelectroosmoticflowishigherinitiallyunderhigherelectricpotential,butit
reducesrapidlyinashortperiodoftime.Interestingly,theuseofeffectivesolubilizingagent
(surfactant)andperiodicvoltageapplicationwasfoundtoachievethedualobjectivesof
generatinghighandsustainedelectroosmoticflowandatthesametimeinduceadequate
masstransferintoaqueousphaseandsubsequentremoval.Periodicvoltageapplication
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consistsofacycleofcontinuousvoltageapplicationfollowedbyaperiodofdowntime
wherethevoltagewasnotappliedwasfoundtoallowtimeforthemasstransfer,orthe
diffusionofthecontaminantfromthesoilmatrix,tooccurandalsopolarizethesoil
particles.Severallaboratorystudieshavedemonstratedsuchdesirableelectroosmoticflow
behaviorinaconsistentmanner,butfielddemonstrationprojectsareneededtovalidate
theseresultsunderscaleupfieldconditions[29,30].
3.1.Electrokineticremovalofsolubleorganics
Althoughmostdangerousorganiccontaminantsinsoils,sedimentsandsludgesare
persistenthydrophobicorganics,severalworksinliteraturefocusedonthetreatmentofsoils
withsolubleorganics.Thus,reactiveblack5isacommondyeusedintheindustry.Reactive
black5isacomplexorganicmoleculedifficulttobiodegradeintheenvironmentandshows
asignificanttoxicityforlivingorganismsinsoilsandwater.Reactiveblack5issolublein
water,butitcanberetainedinsoilsandsedimentsadsorbeduponthesurfaceofmineral
particlesandorganicmatter.Consideringthechemicalstructureofthereactiveblack5
(figure3),themoleculecanbeionizedatalkalinepHwhenthesulfonicgroupsare
neutralizedformingananionwith4negativecharges.Inthisconditions,reactiveblack5
canbetransportedbyelectrokineticstowardtheanode,butonlyifthemoleculeisin
solution.Thedesorptionofthemoleculecanbeachievedusingpotassiumsulfateasflushing
solutionintheanodeandcathodechambers.Figure4showstheadvanceoftheReactive
Black5towardtheanodebyelectromigration.Theadvanceofthedayisevidentinthe4th
dayoftreatment,anditiscompletelyremovedfromthesoilin5days.Theremovalof
Reactiveblack5isonlypossiblewhenthemoleculeisdesorbedfromthesoilparticlesbut
theelectromigrationwasonlypossiblewhenthepHintothesoilwasalkaline[31].ThepH
wascontrolledintheanode(thelefthandsideinfigure4)atavaluebelow7andthe
alkalinefrontelectrogeneratedatthecathode(therighthandsideinfigure4)advanced
throughthesoilfavoringthedissolutionandelectromigrationofreactiveblack5.Negligible
ReactiveBlack5wasobservedifthepHintothesoilwasnotalkaline.
Figure3.
Chemicalstructureofreactiveblack5
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http://www.intechopen.com/books/organicpollutantsmonitoringriskandtreatment/advancesinelectrokineticremediationfortheremovaloforganic
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Figure4.
RemovalofReactiveBlack5fromakaolinspecimenbyelectrokineticremediation
3.2.Cosolvents
Mostoforganiccontaminantsofenvironmentalconcernarepracticallyinsolubleinwater
buttheycanbedissolvedinotherorganicsolvents.Thus,theuseofotherprocessingfluid
thanwatermayhelpinthedesorptionanddissolutionoftheorganiccontaminantsinsoils,
sedimentsandsludges.Electrokineticremediationisaninsitutechnique,andwateris
alwayspresentinsoils.So,theorganicsolventwillnotbeusedalonebutincombination
withwaterasacosolvent.Thus,thepossibleorganicsolventstobeusedarenowreducedto
thosemisciblewithwater.Butthisisnottheuniqueconditionacosolventhastomeet.
Organiccosolventshavetobesafefortheenvironmentorwithaminorenvironmental
impact,andithastobeeasytorecoverfromsoilafterthetreatment.Apartfromthe
environmentallimitationsintheselectionofthecosolvents,therearealsosometechnical
aspectstotakeintoaccount.Theuseofcosolventsmixedwithwaterdecreasesthe
conductivityoftheprocessingfluidduetothedecreaseofsaltssolubilityintheorganicco
solvent.Itdecreasesthecurrentintensitythroughthesoil.Thepresenceofanorganicco
solventwillalsoaffectstheviscosityoftheprocessingfluidandchangetheinteraction
betweentheprocessingfluidandthesoilparticles.Thosealterationswillimpactdirectlythe
evolutionoftheelectroosmoticflowwhichisthemaintransportationmechanismforthe
removaloforganiccontaminants.Anyrate,theincreaseinthecontaminantsolubilitydueto
theuseofthecosolventmaylargelycompensatethedecreaseintheelectroosmoticflow,
beingtheresultpositivefortheremovaloftheorganiccontaminants.Someoftheco
solventsusedinliteratureare:ethanol,nbutanol,nbutylamine,tetrahydrofuran,oracetone
[26,3234].Phenanthrenewasthetargetcontaminantinthestudieswithcosolvents.The
removalofphenanthenewasnegligiblewhenwaterwasusedasflushingsolutionbutthe
removedfractionofphenanthreneclearlyincreasedwiththeuseofcosolvents,especiallyn
butylaminewhichresultedinaremovalof43%in127daysinalabtestwithasoilspecimen
of20cmlong.TheremovalcanbeenhancedcontrollingothervariablessuchasthepHinto
thesoilandimprovingtheelectroosmoticflowoperatingathighervoltagegradientorwith
periodicvoltageapplication[34].
3.3.Surfactants
Thenamesurfactantistheshortversionofsurfaceactiveagent.Itmeansthattheso
calledsurfactantsareagroupofsubstancesthathasincommonaspecialcapacitytochange
thesurfacepropertiesofthesolutionwhentheyarepresent.Inenvironmentalapplications,
theinterestofsurfactantsistheirabilitytolowerthesurfaceandinterfacialtensionofwater
improvingthesolubilityofhydrophobicorganics.Thereisawidevarietyofchemical
structuresandfamiliesthatfitsinthedefinitionofsurfactant.Basicallyasurfactantisa
chemicalcompoundwhosemoleculeincludesahydrophilicgroupinonesideofthe
moleculeandintheoppositesideahydrophobicgrouporchain.Theinteractionofthe
hydrophilicgroupwithwaterassuresitssolubilitywhereastheinteractionofthe
hydrophobicgroupwiththeorganiccontaminantsassuresthesolubilizationofhydrophobic
organics.Thehydrophobicgrouporchaininthesurfactantmoleculeisrepelledbywater,so
thesurfactantmoleculestendtoformsphericalstructureswiththehydrophilicgroupoutside
andthehydrophobicchainsinside.Thesesphericalstructuresarecalledmicelles.Thus,the
surfactantcreatesahydrophobicenvironmentveryappropriateforthesolubilizationof
organiccompounds.Theformationofmicellesdependsonthesurfactantconcentrationand
themicelleformationreachamaximumforasurfactantconcentrationcalledCMCcritical
micelleconcentration[26].
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Thereisawidevarietyofchemicalstructuresinthesurfactants,butusuallytheyare
classifiedbytheelectricchargeinthemoleculein4groups:cationic,anionic,neutraland
zwitterionic(includespositiveandnegativechargesinthesamemolecule).Inenvironmental
applications,neutraloranionicsurfactantsarepreferredbecausecationicsurfactantstendto
interactwiththesoilparticles,retardingtheiradvanceandreducingtheireffectiveness[26].
Thetoxicityofsurfactantstothesoilmicroorganismsitisalsoveryimportantforthe
remediationandrestorationofsoils.Thatiswhyinrecentyearstheresearchwasredirected
totheuseofnaturalsurfactantsorbiosurfactants[35].
Awidevarietyofsurfactantshavebeenusedinelectrokineticremediationfortheremoval
oforganiccontaminants:Sodiumdodecylsulfate(SDS),Brij35,Tween80,IgepalCA720,
Tergitolandother.Targetcontaminantinthesestudiesincludeshydrophobicandpersistent
organicssuchas:phenanthrene,DDT,diesel,dinitrotoluene,hexachlorobenzeneandothers.
Ingeneral,itcanbeconcludethatthereportedresultsinliteraturearequitegoodreaching
removalefficienciesover80%inmanystudies,atleastinbenchscalelaboratorytestwith
bothmodelandrealcontaminatedsoils[36,37].Reddyetal.demonstratedtheremovalof
phenanthrenebyelectrokineticsusingsurfactantsasanenhancedflushingsolutioninthe
electrodechambers.Differenttypesofsoils,commonlykaolinandglacialtill,wereusedin
thisstudy.Ingeneral,thereisnoeliminationofphenanthrenewhenwaterwasusedas
flushingsolutiondespitethelargeelectroosmoticflowregisteredintheseexperiments.The
useofsurfactantssuchasIgepalCA720,Tween80orWitconoltendtodecreasethe
electroosmoticflowduetothechangesintheinteractionoftheflushingsolutionwiththe
soilparticlesurface,thedecreasingintheelectricconductivityofthesystem,andthe
increaseoftheviscosityoftheflushingsolution.Despitethedecreasingoftheelectro
osmoticflow,theincreaseofphenanthrenesolubilityinthesurfactantflushingsolution
resultedinaveryimportanttransportationandremovalofphenanthreneinthefluid
collectedonthecathodeside.Thespecificremovalresultsdidnotonlydependonthetype
andconcentrationofsurfactantbutalsointhepHevolutionintothesoil,thetypeofsoiland
theionicstrengthintheprocessingfluid.Thosevariablesaffectthesolubilizationofthe
organiccontaminantsbythesurfactant,butthemaininfluenceisinthedevelonmentand
evolutionoftheelectroosmoticflow.Thus,thelimitationofveryacidicenvironmentsinto
thesoilavoidsasharpreductionoftheelectroosmoticflow.Thiscanbeachieved
controllingthepHontheanodeorusingabufferingsolutionwiththeflushingsurfactant
solution.Thebufferingcapacityofthesoilalsocontributestoavoidtheacidificationofthe
interstitialfluid[26,33,38,39].However,theonlyuseofsurfactantsseemstobenot
enoughtogetacompleteremovalofphenanthrenefrompollutedsoils,anditisnecessaryto
enhancetheelectroosmoticflowusinghighvoltagegradients(2V/cmorhigher)andeven
theuseofperiodicvoltageapplicationsoperatingwithaconstantvoltagedrop
intermittently.Theperiodicvoltageapplicationresultedinabout90%ofthephenanthrene
removedonthecathodesolution[40].
3.4.Cyclodextrins
Glucosemayformcyclicstructureswith6,7or8moleculescalledcyclodextrins.The
resultingmoleculehasthestructureofatruncatedcone.Theinternalcavityhasdifferent
sizedependingonthenumberofglucoseunits.Theinnerdiameterofthemoleculeranged
from0.450.53nmforcyclodextrin(ringof6glucosemolecules)0.600.65nmfor
cyclodextrin(ringof7glucosemolecules)and0.750.85nmforcyclodextrin(ringof8
glucosemolecules).CyclodextrinshowsanamphiphilicbehaviorduetotheringsofOH
groupspresentatthebothendsofthemolecule.Thehydroxylgroupsarepolarandconferto
thecyclodextrinthesolubilityinwater.However,theinnersurfaceofthemoleculeis
hydrophobicandcyclodextrinscanaccommodatedifferentnonpolar,hydrophobic
moleculessuchasaliphatic,aromaticorlipophiliccompounds.Moreover,thedifferentsize
oftheinnercavityoftheciclodextrinmoleculescanbeusedasaselectthemoleculestobe
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trappedinside,andtherefore,transportedandremoved.
Cyclodextrinshavebeenusedtoenhancetheremovalofhydrophobicorganicssuchas
phenanthrene[41],dinitrotoluene[42],theherbicideatrazine[43],andothercontaminants
[44]inrealandmodelsoils.Ingeneral,cyclodextrinsarefacilitatingagentsthatimprovethe
removaloforganiccontaminantsfromsoilcomparedtootherexperimentswithunenhanced
electrokinetics,butresultsfromcyclodextrintestsareusuallylesseffectivethantestwith
surfactants,ironnanoparticlesorwithchemicaloxidants.Theefficiencyoftheremovalcan
beenhancedcombiningmorethanonefacilitatingagent.Thus,Phametal.[45]and
Oonnittanetal.[46]usedtheelectrokinetictreatmentwithacyclodrextringflushing
solution,combinedwithultrasoundsorchemicaloxidationwithhydrogenperoxide.
Anyway,theuseofcyclodextrinsmayenhancetheremovalofthehydrophobic
contaminantsbuttheresultsareusuallylowerthanthatfoundwithsurfactants.
4.Combinedtechnologies
4.1.Electrokineticsandchemicaloxidation/reduction
Electrokineticremediationisatechniquethatremovesthecontaminantsfromthe
contaminatedsoilbytransportation(electroosmosisandelectromigration).However,
organiccontaminantsaredifficulttoremovefromsoils,mainlyduetothelowsolubilityin
water,andtheirstrongadsorptiontoorganicmatterandsoilparticles.Therearesomeother
waystolookattheproblemoforganiccontaminantsinsoil.Onepossibilityistodegradethe
contaminantsinsitu.Toachievesuchdegradation,itisnecessarytocreatetheadequate
conditionsintothesoilsupplyingstrongoxidizingchemicalstothesoilporestoperformthe
degradationinsitu.Oxidantssuchasozone,hydrogenperoxideorpersulfatecanbe
transportedintodesoilbyelectromigrationand/orelectroosmosis.Astheoxidantsadvance
throughthesoil,theyreactwiththeorganiccontaminantsresultinginsmallermolecules
usuallylesstoxicthattheoriginalones.Theobjectiveistobeabletocompletelyoxidizethe
organiccontaminantstocarbondioxideandwater.Ifsuchcompletedegradationisnot
possibleundertheoperatingconditionsintothesoil,theformationofsimplermoleculesare
consideredenough,becausesmallandsimplermoleculescanbedegradedeasilybythe
microorganismsintothesoil.Thus,thistechnologycanbeaveryattractivesolutionforthe
degradationofcomplexorganiccontaminantsintosoil.Thistechnologydoesnotgenerate
wasteeffluentswithharmfulcompoundsbecausetheyaredestroyedintothesoil.Moreover,
thecontactoftheworkerswiththecontaminantsandcontaminatedsoilparticlesarereduced
toaminimum,whichisaveryimportantpointinthefieldoperation.
Ontheotherhand,thechemicaldestructionoforganiccontaminantscanbecarriedoutby
chemicalreduction,whenareductivechemicalprocessresultsinlesstoxiccompounds.
Thus,organochlorinepesticidescanbedegradedbyreductivedechlorination.Theresultis
theorganicmoleculewithoutchlorineatomsinitsstructure.Thus,theresultedorganic
compoundsaremuchlesstoxicthantheoriginalcompoundandtheycanbeeasilydegraded
bythemicroorganismsintothesoil.
Thereareseveralapplicationsofchemicaloxidationcombinedwithelectrokineticsin
literature.YukselenAksoyandReddy[47]havetestedthedegradationofPCBin
contaminatedsoilsbypersulfate.Sodiumpersulfateisastrongoxidizingagentwitha
standardreductionpotentialof2.7Vwhichassurestheeffectiveoxidationofmostofthe
organiccontaminants.Persulfateisfirstlytransportedintothesoilbyelectromigration
and/orelectroosmosis,andthenitisactivatedbypHortemperature.Toactivethe
persulfate,itisnecessarytoachieveover45Coracidifythesoilbelow4.Bothconditions
canbereachedwiththeelectricfield.Highvoltagegradientresultsintheheatingofsoil
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andtheacidfrontelectrogeneratedattheanodecanacidifythesoil.So,inthiscasethe
applicationoftheelectricfieldnotonlywasusedasatransportationmechanismbutasa
tooltocontrolthekeyvariablesoftheprocess.Inthiswork[47],thehighestdegradationof
PCBswasachievedinakaolinspecimenwitha77.9%ofremovalwhentemperaturewas
usedasactivatorofthepersulfate.
Thecombinationofelectrokineticsandchemicaloxidationwastestedinacontaminatedsoil
withhexachlorobenzene[46,48].Hydrogenperoxidewassuppliedtothesoilfromthe
anodeinaFentonlikeprocesswheretheironcontentinthesoilwassufficienttoactivate
thedescompositionofH2O2forthegenerationofhydroxylradicals(OH).60%ofHCB
waseliminatedfromthesoilin10daysoftreatmentavoidingthedeactivationoftheFenton
reagentathighpHvalues.Higherremovalcanbeachievedatlongertreatmenttime,
controllingthepHintheoptimumrangeforFentonreagentwhichisslightlyacid
environments.AtalkalinepH,H2O2decomposesinwaterandoxygenanddonotformOH
radicals.
TheuseofFe0fortheremediationofsoilshasbeenusedrecentlyfortheabilityofthe
nativeirontocatalyzethereductivedechlorinationoforganiccompoundssuchas
pentachlorophenol,trichloroethylene,hexachlorobenzeneandothers.Inthistechnology,the
electricfieldcanbeusedasadrivingforcetotransportthenanoparticlesintothesoil.Reddy
andKarri[49]foundthatthecombinationofelectrokineticremediationandFe0
nanoparticlescanbeappliedfortheremovalofpentachlorophenolfromsoil.The
transportationofFe0nanoparticleswasdeterminedbytheironconcentrationintothesoilat
theendoftheexperiments.Ironconcentrationattheendoftheexperimentsincreasedwith
theinitialFe0concentrationusedintheanodeandwiththevoltagegradient.However,the
transportofnanoparticleswaslimitedbytheiraggregation,settlementandpartialoxidation
withintheanode.Pentachlorophenolwaspartiallyreduced(4050%)intothesoil,buta
completePCPeliminationwasfoundnearthecathodeduetothecombinationofFe0andthe
reductivedechlorinationwithinthecathode.Inordertofavorthetransportationof
nanoparticlesintothesoil,newstrategiesareneededtopreventaggregation,settlementand
oxidationofironnanoparticlesforenhancedremediationofsoils.Cameselleetal.[50]
studiedthesurfacecharacteristicsoftheironnanoparticlesandproposedseveraldispersant
tofavorthetransportationandavoidaggregationandsettlement.Amongthedispersants
proposedaluminumlactatepresentsgoodcharacteristicstobeusedinlargescale
application.OthermetalliccatalystssuchasCu/FeorPd/Febimetalmicroscaleparticles
weresatisfactorilyusedfortheremediationofsoilswithorganochlorines..Dechlorinationof
hexachlorobenzeneupto98%wasachievedwithCu/Fe[51]andonly60%withPd/Fe[52].
4.2.Electrokineticsandpermeablereactivebarriers
Permeablereactivebarriers(PRB)arepassiveremediationsystemsespeciallydesignedfor
theremediationofcontaminatedgroundwater.PRBsconsistofdiggingatrenchinthepath
offlowinggroundwaterandthenfillingitwithaselectedpermeablereactivematerial.As
thecontaminatedgroundwaterpassesthroughthePRB,contaminantsreactwiththeactive
materialinthePRBbeingabsorbed,precipitatedordegraded.Cleangroundwaterexitsthe
PRB.InthedesignofaPRBseveralfactorshavetobetakingintoaccount.First,thenature
andthechemicalpropertiesofthecontaminantshavetobeconsideredfortheselectionof
thereactivematerial.Fororganiccontaminants,materialssuchasactivecarbonorFe0were
used.Organiccontaminantscanberetainedinintheporousstructureoftheactivecarbon.
Nativeironhasbeenusedforthereductivedechlorinationofpesticidesandother
organochlorines.Theflowrateofgroundwaterandthereactionrateofthecontaminants
withtheactivematerialinthePRBareusedtodefinethewidthofthebarrier.Theresident
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timeofthegroundwaterinthebarrierhastobeenoughtoreachacompleteremovalor
degradationofthecontaminants.Finally,theporousstructureofthebarrierhastoconferthe
barrieritselfapermeabilityvaluehigherthanthesurroundingsoil,toassurethatallthe
groundwaterpassthroughthebarrierandtherewillnotbebypass.Themainadvantagesof
thePRBarethestableoperationforlongtreatmenttime,evenseveralyears,withverylow
investmentandmaintenancecosts.Anyway,thelimitedresultsfoundinseveralapplication
impulsetheresearchinseveraldirectionsinordertoimprovetheremovalofthe
contaminants[53].OnepossibilityisthecombinationofthePRBwithelectrokinetic
remediation.
ThecombinationofelectrokineticremediationwithPRBhasbeensatisfactoryusedto
remediatesoilspollutedwithheavymetalssuchaschromium.Theelectricfieldtransports
thechromiumtowardsthemainelectrodes,butintheirway,thechromiumionspassthrough
aPRBmadeofelementaliron.Thechemicalreductionofchromiumtakesplacesreacting
withtheelementaliron.Theelectricfieldalsoplaysaroleinthereductionofthechromium
[54].Inthecaseoforganiccontaminants,ChangandCheng[55]appliedthecombinationof
PRBwithelectrokineticstoremediateasoilspecimencontaminatedwithperchloroethilene.
Theexperimentswerecarriedoutataconstantvoltagedropof1v/cmandsodiumcarbonate
0.01Mwasusedasprocessingfluidtoavoidtheformationofanacidfrontintheanode.It
eliminatestheacidificationofthesoilandthepossiblenegativeeffectsontheelectro
osmoticflow.ThePRBweremadeofnanoparticlesofelementalironandzinc.The
perchloroethyleneisdechlorinateduponthenanoparticlesofironandzinc.However,the
formationofferricoxideandferrichydroxideslimitstheactivityofthePRBandits
operationallife.Theprotonselectrogeneratedatthecathodecancontributeinthe
solubilizationandremovaloftheferrichydroxidesincreasingtheactivityanddurationof
thePRB.Moreover,theprotonalsofavorsthedechlorinationreaction.Inconclusion,the
formationofH+ionsintheanodefavorstheeliminationofperchloroethylene.Asthe
voltagedropappliedtothesystemincreases,theformationofH+upontheanodealso
increasesresultinginmoreandfasterperchloroethyleneremoval.Thus,theoperationat2
V/cmresultedintheremovalofalmos99%oftheinitialperchloroethyleneinonly10days
ofoperation.
ChungandLee[56]appliedacombinationofelectrokineticswithPBfortheremediationof
thetetrachloroethylenecontaminatedsoilsandgroundwater.Theinterestofthisworkisthe
mediausedinthePRB.Theauthorsusedamixtureofsandwithamaterialtheycalled
atomizingslag(materialpatented)whichisbasicallyamixtureofoxidesofSi,Fe,Caand
Al.Theatomizingslagismainlyusedasaconstructionmaterialbutitwasselectedforthe
PRBbecauseismuchcheaperthanothermaterialsreportedinliteraturesuchasiron
nanoparticles.Theoperationofsuchsysteminsituresultedintheremovalof90%ofthe
tetrachloroethyleneconsideringtheconcentrationsmeasuredbeforeandafterthesystem
electrokineticPRBconfirmeingthesuitabilityofthistechnologyforitsapplicationinsituto
contaminatedsoils.
4.3.Bioelectroremediation
Thecombinationofelectrokineticremediationwithbioremediationhasshownsome
interestingresultsthatpromisethistechnologyagooddevelopmentinthenearfuture.
Basically,theapplicationofanelectricfieldtoapollutedsitemayhelpinthemobilization
ofthecontaminants.Thatmobilizationmakesthecontaminantsavailableforthe
microorganisms.Atthesametime,soilbacteriaarelikeacolloidwithasurfacecharge.So,
theycanbemovedundertheeffectoftheelectricfield.Thetransportofbacteria,evenin
smalldistances,mayhelpintheinteractionbetweenthebacteriaandthecontaminants.
Finally,theelectricfieldcanbeusedasatransportationmechanismtointroduceintothesoil
thenutrientsandotherchemicalsthatmayfacilitatethebacterialgrowthanddevelopment,
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aswellasthesupplyofotherchemicalsthatcancontributetothedegradationofthe
contaminants[57,58].
Lageman[59]developedatechnologycalledElectrokineticBiofence(EBF).Theaimofthe
EBFistoenhancebiodegradationoftheVOCsinthegroundwateratthezoneofthefence
byelectrokineticdispersionofthedissolvednutrientsinthegroundwater.EBFwhich
consistsofarowofalternatingcathodesandanodeswithamutualdistanceof5m.
Upstreamofthelineofelectrodes,aseriesofinfiltrationwellswereinstalled,whichhave
beenperiodicallyfilledwithnutrients.AfterrunningtheEBFfornearly2years,clearresults
havebeenobserved.Theconcentrationofnutrientsinthezonehasincreased,thechloride
indexisdecreasing,andVOCsarebeingdechlorinatedbybioactivity.Theelectricalenergy
fortheEBFisbeingsuppliedbysolarpanels.
4.4.Electroheating
Theremovalofvolatileandsemivolatileorganicsfromsoilcanbecarriedoutheatingthe
soil,evaporatingthevolatileorganicsandaspiratingthevapors,whichinturnaretrappedin
theappropriateabsorbentsuchasactivecarbontobefinallyeliminatedbyincineration.The
heatingofsoilcanbedoneinseveralways.Onepossibilityistheuseofanelectriccurrent.
Soilisnotagoodelectricconductor,sothepassingofanelectriccurrentgeneratesheat.In
electrokienticremediation,itisusedacontinuouselectriccurrentbecausetheobjectiveisto
transporttheionicandnonioniccontaminantsoutofthesoil.Inthecaseofelectroheating,a
transportationofthecontaminantsusingtheelectricfieldasadrivenforceisnotnecessary.
Theelectricfieldisonlyusedasasourceofenergythatistransformedfromelectricenergy
intoheat.Thatiswhyinelectroheatingthecontinuouselectricfieldissubstitutedbyan
alternatecurrentthatsuppliestheenergybutdoesnotinducetransportation.Soilisnota
goodelectricconductor.Theconductivityofsoilsismuchlowerthanthetypicalelectric
conductorsuchasmetals.Theconductivityofsoillargelyvarieswiththemoisturecontent
andthepresenceofmobileions.Anyway,theconductivityofsoilisusuallylowandthe
heatingiseasytoachievewithanalternatecurrent.Itisrecommendabletoavoidtheuseof
electroheatinginsaturatedsoils.Asoilsaturatedinmoisturefavorsthetransportationof
currentinsteadoftheelectricheating.
Electroheatingshowsseveraladvantagesformothertechnologiesdesignedfortheremoval
ofvolatileorganicsfromsoils.Inelectroheating,theheatingofsoilisdirectlyrelatedtothe
electricfieldintensity.So,theincreaseoftemperatureandthefinaltemperatureinthesoil
canbeeasilycontrolledadjustingtheintensityoftheelectricfield.Furthermore,theheatis
generatedintothesoil,inthewholevolumeatthesametime,achievingamoreuniform
temperatureintheareatobetreated.Theuniformtemperaturepermitsauniformremovalof
thecontaminantsandamoreefficientuseoftheenergy.
ElectricalheatingwasusedintheremediationofacontaminatedsiteinZeist,the
Netherlands[60].Thesitewasseverelypollutedwithchlorinatedsolventssuchas
perchloroethylene(PCE)andtrichloroethylene(TCE)andtheirdegradationproductsarecis
1,2dichloroethene(CDCE)andvinylchloride(VC).Satisfactoryresultswereobtainedin
theapplicationofelectricalheatingsoilandgroundwaterinthesourceareas,combinedwith
soilvaporextractionandlowyieldgroundwaterpumping,andenhancingbiodegradationin
thegroundwaterplumearea.Twoyearsofheatingand2.5yearsofbiodegradationhasbeen
resultedinnearcompleteremovalofthecontaminants.Afullscaleimplementationofsix
phaseelectricalheatingtechnologywasusedinSheffield,UK[61].TerraVacLtd.
demonstratedhowremediationtimescalescanbereducedfrommonths/yearstoweeks,with
anelectricalheatingcapableofremediationofsoilindifficultgeologicalconditionsandin
densepopulatedurbanareas.TCEandVCwereremediatedbyelectricalheatingupto
99.99%.Smith[62]appliedtheelectroheatingtechnologyfortheremediationof
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dicholormethane,ethylenedibromide,triclhoroethaneandtetrachloroethane.Electroheating
wasaneffectivetechnologyfortheremediationofsuchorganiccontaminants,butduring
theremediationprocess,theelevationoftemperatureincreasesthesolubilityofthe
contaminantsinthegroundwater,theactivityofsoilmicroorganismsisenhancedandsome
reactions,suchashydrolysisofthecontaminantsandthedesorptionofgases,takesplace.
Thosefactorsmayaffecttheremovalofthecontaminantsanditinfluencehastobe
considered.
5.Largescaleapplications
Electrokineticremediationhasbeenusedasaremediationtechnologyinseveraltestsatfield
scale.IntheUSA,fieldprojectswerecarriedoutorfundedbyUSEPA,DOE,ITRC,US
ArmyEnvironmentalCentre,aswellascompanieslikeElectropetroleumInc.[63],Terran
Corporation,andMonsanto,Dupont,andGeneralElectricwhichdevelopedtheLasagnaTM
technology[64,65].InEurope,morefieldprojectswithelectrokineticremediationhave
beencarriedout,speciallyassociatedtothecommercialactivityoftheHakMilieutechniek
Company[66,67].Recently,somefieldexperienceswerereportedinJapanandKorea[68].
Someofthesetestsdealabouttheremediationofpollutedsiteswithorganiccontaminants
suchasorganochlorides,PAHsandPCBs.Consideringtheinformationavailablein
literature,thecostoffieldapplicationofelectrokineticremediationisaboutanaverage
valueof200$/m3forbothorganicandinorganiccontaminants,howeveritmustbekeptin
mindthatelectrokineticremediation,likeanyotherremediationtechnology,issitespecific
andthecostscanbevaryfromlessthan100tomorethan400$/m3[69].
6.Futureperspectives
Thescientificknowledgeaccumulatedinthelast20yearsconductedtoseverallessons
learnedthatmustbekeepinmindinthedesignofprojectsfortheremediationof
contaminatedsites.Thus,theremediationofcontaminatedsoilswithorganiccontaminants
issitespecific.Theresultsobtainedintheremediationofasitecannotbeassumedforother
contaminatedsites.Thisisduetothelargeinfluenceofthephysicochemicalpropertiesof
thesoilanditspossibleinteractionswiththeorganiccontaminantsintheresultsofthe
electrokineticremediationtreatment.Besides,thechemicalsusedforenhancingthe
electrokinetictreatmentmaycomplicatethebehaviorofthesystemandtheremovalresults
maylargelyvaryfromonesitetoanother.Recently,ithasbeenconsideredthatthe
combinationofseveralremediationtechniquesmayimprovetheremediationresults,
especiallyinsiteswithcomplexcontamination,includingrecalcitrantorganicscompounds
andinorganiccontaminants.Thecombinationofelectrokineticswithbioremediation,
phytoremediation,chemicaloxidationorelectricalheating,presentsveryinteresting
perspectivesfortheremediationofdifficultsites.Itisexpectedthecombinationof
remediationtechnologiestoimprovetheremediationresults,savingenergyandtime.
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Advances in Electrokinetic Remediation For The Removal of Organic Contaminants in Soils - InTechOpen

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2H 2 O 4e-+4H+(aq) +O2(gas) E =-1.229V

4H 2 O+4e- 2H 2(gas) +4OH

ofH+ ionsfromtheanodeandOH fromthecathodeintothesoilleadstodynamicchanges

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