A short primer on benzene, toluene, ethylbenzene and xylenes (BTEX) in the environment and in hydraulic fracturing fluids

DrFredericLeuschandDrMichaelBartkow,GriffithUniversitySmartWaterResearchCentre 17Nov2010 1. Somenotesaboutconcentrations Concentrationsinwaterinthisdocumentaregenerallygivenaspartperbillion(ppb),equivalenttoonemicrogram perlitre(g/L).Amicrogramisamillionthofagram.Oneppbisroughlyequivalenttoateaspoonofmaterialinan Olympicsizeswimmingpool.Notethatppbairconcentrationscannotsimplybeconvertedtog/m3(andviceversa) butrequireaconversionfactor. 2. WhatisBTEX? BTEXisanabbreviationusedforfourrelatedcompoundsfoundincoaltar,crudepetroleumandawiderangeof petroleumproducts.ThecompoundsareBenzene,Toluene,EthylbenzeneandXylenes. Table1.Name,chemicalabstractserviceregistrynumber(CASRN,auniqueidentifier)andchemicalstructureof benzene,toluene,ethylbenzeneandxylenes(BTEX). Compound Benzene CASRN 71432 Chemicalstructure

Toluene Ethylbenzene 108883 100414 Xylenes 1330207 Oncereleasedintheenvironment,BTEXcompoundsusuallyevaporatequicklyintotheair.BTEXcanalsodissolvein water,anditmaybefoundinsurfaceandgroundwateratcontaminatedsitesorinclosevicinitytonaturaloil,coal andgasdeposits.

BTEXintheenvironment 3. SourcesofBTEX BTEXarenaturallyoccurringcompoundsincrudeoil.Benzeneforexampleisfoundatlevelsupto4g/Lincrude petroleum,andcanbefoundinseawater(0.8ppb)inthevicinityofnaturalgasandpetroleumdeposits(IPCS1993). OthernaturalsourcesofBTEXcompoundsincludegasemissionsfromvolcanoesandforestfires(IPCS1985,1993, 1996,1997;ATSDR2007a). TheprimarymanmadesourcesofBTEXintotheenvironmentareviaemissionsfrommotorvehiclesandaircraft exhaust,lossesduringpetrolmarketing,spillsandcigarettesmoke.BTEXarecreatedandusedduringtheprocessing ofrefinedpetroleumproductsandcoalandduringtheproductionofchemicalintermediatesandconsumerproducts suchaspaintsandlacquers,thinners,rubberproducts,adhesives,inks,cosmeticsandpharmaceuticalproducts(IPCS 1985,1993,1996,1997;NTP2005).BTEXcompoundsareamongthemostabundantlyproducedchemicals,with worldwideannualproductionof810milliontonsofbenzene(NTP2005),510milliontonsoftoluene(ATSDR2000), 510milliontonsofethylbenzene(IPCS1996)and1015milliontonsofxylenes(IPCS1997). ThemajorityofBTEXreleasedintotheenvironmententertheatmospheredirectly.BTEXmaybeintroducedinto waterbyindustrialeffluentsandatmosphericpollution,butreleasesofBTEXtowateraremainlyrelatedtospillsof petrolandpetroleumproductsorproximitytonaturaldepositsofpetroleumandnaturalgas(IPCS1985,1993,1996, 1997).Ifpresentindrinkingwatersources,BTEXcompoundscanbeefficientlyremovedbyactivatedcarbon filtration(NHMRC2004). 3.1. BTEXinhydraulicfracturingfluids BTEXcontainingpetroleumproducts(suchasdiesel)havebeenusedasadditivesinstimulationfluids,particularlyin hydraulicfracturing(fraccing).Wellstimulationisusedtoincreaseproductioninoilandgaswellsbyimprovingthe flowofhydrocarbonsintotheoilwell.Fraccingistheprocessofpumpinghighpressurefluidsintoacoalseamto fracturetheseamandallowgastoflowintothegaswell,thusmaximizingextraction.Fraccingfluidconsistsmostly ofwaterandsandbutsmallamountsofadditivesareusedtothickenthefluidandimprovetheefficiencyofthe process,thusreducingtheneedforexcesswateruse.TheuseofBTEXasanadditiveinfraccingfluidshasinthepast beenpermittedincoalseamgasextraction;howeversince2003theUSindustryhasvoluntarilyagreedto discontinueusingBTEXinfraccingfluidsduetotheavailabilityofsaferalternatives(USEPA2004).InQueensland, BTEXisstrictlyregulatedandmustnotbeusedinstimulationfluidsinamountsgreaterthanthatprovidedbythe legislation(SoQ2010). 4. ExposuretoBTEX ThepresenceofBTEXinpetrolandasawidelyusedindustrialsolventcanresultinsignificantandwidespread emissionstotheenvironment(Table2).ThemostimportantsourceofhumanexposuretoBTEXisfrombreathingof contaminatedair,particularlyinareasofheavymotorvehicletraffic,petrolstationsandthroughcigarettesmoke (IPCS1985,1993,1996,1997;WHO,2008).Cigarettesmokeinparticularcancontributehalfofthedailyexposureto BTEXcompounds(ATSDR2007a).ExposuretoBTEXfromwatercontributesonlyasmallpercentageofthetotaldaily intake,comparedwithinhaledairanddietarysources(Table3).

BTEXintheenvironment 4.1. Benzene(IPCS1993,ATSDR2007a,NTP2005) Outdoorenvironmentallevelsofbenzenerangefrom0.2g/m3(0.06ppb)inremoteruralareasto349g/m3(107 ppb)inindustrialcentreswithahighdensityofmotorvehicletraffic.Thepercentageofbenzeneinunleadedpetrol isapproximately12%.Drivingamotorvehicleonehourperdayisestimatedtoadd40gofbenzenetoapersons dailyintake.Levelsupto10,000g/m3(3,000ppb)havebeenmeasuredinairatpetrolstations.Spendingalittle under2min/weektorefuelacaratthepetrolstationleadstoanadditionalestimateddailyintakeof10g.Benzene hasbeendetectedatlevelsashighas500g/m3(154ppb)inindoorresidentialair.Cigarettesmokecontributes significantamountsofbenzenetothelevelsreportedinindoorair,withsmokersinhalingapproximately1,800g benzene/dcomparedto50g/dbynonsmokers.Benzenecanalsooccurinfoodsanddrinksasaproductofa reactionbetweenbenzoateandascorbicacid,andhasbeenfoundinsoftdrinksintheUKatconcentrationsashigh as28ppb(g/L)(FSA,2006).Incomparison,benzeneconcentrationsinwateraregenerallylow(Table2). 4.2. Toluene(IPCS1985,ATSDR2000) Thelargestsourceoftoluenereleaseisduringtheproduction,transport,anduseofpetrol,whichcontainsabout5 8%toluene.Theconcentrationsoftolueneinairhavebeenfoundtobequitelowinremoteareas,butlevelsof525 g/m3(1.36.6ppb)arecommoninsuburbanandurbanareas,withlevelsashighas1,310g/m3(350ppb)inareas ofhightrafficdensity.Concentrationatpetrolstationcanbeashighas9,000g/m3(2,400ppb),andrefillingacar canaddsignificantlytodailytolueneintake.Tolueneisalsoacommonindoorcontaminant,beingusedincommon householdproductssuchaspaints,adhesivesandnailpolish,aswellasfromcigarettesmoke.Tolueneis occasionallydetectedindrinkingwatersupplies,butoccurrenceisnotwidespreadandlevelsaregenerallybelow3 ppb(butcangoashighas3,500ppbingroundwaterfromindustriallypollutedsites)(Table2). 4.3. Ethylbenzene(IPCS1996,ATSDR2007b) Ethylbenzeneisubiquitousinambientair,primarilyasaresultofindustrialreleasesandvehicleemissions.Petrol containsabout12%ethylbenzene.Ethylbenzeneconcentrationsrangingfrom0.74to360g/m3(0.183ppb)have beenmeasuredaturbansites.Levelsfoundatruralsitesaregenerally<2g/m3(<0.46ppb).Ethylbenzenereleases totheairespeciallyinindoorenvironmentscanoccurwiththeuseofconsumerproductssuchaspesticides,liquid processphotocopiersandplotters,solvents,carpetglue,paints,varnishes,automotiveproducts,adhesives,and fabricandleathertreatmentsthatcontainethylbenzene.Ethylbenzeneisdetectedinfrequentlyindrinkingwater (Table2).Ethylbenzenelevelsinuncontaminatedgroundwateraregenerally<0.1ppb.However,muchhigherlevels havebeenreportedforgroundwatercontaminatedviawastedisposal,fuelspillageandindustrialfacilities.Ata solventrecoveryfacility,ethylbenzeneconcentrationsofupto28,000ppbweremeasuredincontaminated groundwater. 4.4. Xylenes(IPCS1997,ATSDR2007c) Xyleneisprimarilyreleasedfromindustrialsources,inmotorvehicleexhaust(petrolcontains710%xylenes),and duringitsuseasasolvent.Typically,backgroundlevelsofxyleneinambientairarearound1g/m3(0.23ppb),butin suburbanareasitisaround3g/m3(0.69ppb).Higherlevelshavebeenmeasuredinurbanandindustrializedareas, upto775g/m3(178ppb).Insomecases,indoorlevelsofxylenecanbehigherthanoutdoorlevels,especiallyin buildingswithpoorventilation.Typically,backgroundlevelsofxylenesinsurfaceandgroundwatersarelow(<0.1 ppb)(Table2).Muchhigherlevelshavebeenmeasuredinsomeindustrialareasandareasassociatedwiththeoil industry.

BTEXintheenvironment Table2.Reportedconcentrationsofbenzene,toluene,ethylbenzeneandxylene(BTEX)inairandwater. Air(g/m3) Remoteruralarea Industrialcentrewithhightraffic density Water(ppborg/L) Surfacewater Contaminatedsurfacewater Groundwater Contaminatedgroundwater Drinkingwater Benzene 0.216 Upto349 <0.12.1 Upto100 <0.11.8 Upto330 <0.15 Toluene 0.5260 Upto1,310 <115 NA <1100 Upto3,500 <127 Ethylbenzene 0.21.6 Upto360 <0.11.8 Upto15 <0.11.1 Upto2,000 <110 Xylenes <0.13 Upto775 <0.11.2 Upto32 <0.10.5 Upto1,340 <0.112

Notes:AlldatainthistablefromATSDR2000,2007a,2007band2007c;IPCS1985,1993,1996and1997;NTP2005;WHO2008;andNHMRC 2004.

Table3.Estimateddailyintakesofbenzene,toluene,ethylbenzeneandxylenes(BTEX).Allvaluesareinalling/d. Airbreathing Cigarettesmoking Food Drinkingwater Benzene 901,300 1,800 Upto250 Upto10b Toluene 212,000 2,000 Upto64 Upto43 Ethylbenzene 23,600 40a NA Upto20b Xylenes 702,000 Upto190a NA Upto24b

Notes:Unlessotherwiseindicated,alldatainthistablefromATSDR2000,2007a,2007band2007c;IPCS1985,1993,1996and1997;NTP a b 2005;WHO2008;andNHMRC2004. Assuming5cigarettes/d; Assuming2L/d.NA:Notapplicable.

4.5. ExposuretoBTEXfromhydraulicfracturing TherearetwopotentialexposuresourcestoBTEXfromhydraulicfracturing:1)useofBTEXinfraccingfluids,and2) fracturingthroughhydrologicconfininglayerandcreatingofahydrauliccommunicationbetweenthecoalseamand undergroundaquifersusedforgroundwater. AreportbytheUSEnvironmentalProtectionAgency(USEPA)showedthatifBTEXwasusedasanadditivetofraccing fluids,theconcentrationofBTEXatthepointofinjectionwouldbe454,400ppbforbenzene,12031,000ppbfor toluene,1208,700ppbforethylbenzeneand33026,000ppbforxylenes(USEPA2004).Thereportconcludedthat whiletheseconcentrationswerehigh,theriskofcontaminatinggroundwatersourcesofdrinkingwaterwasminimal duetorecoveryofinjectedfluids(6882%)combinedwiththemitigatingeffectsofdilutionanddispersion, adsorptionandbiodegradation(USEPA2004). BTEXarenaturalcompoundsfoundincrudeoil,coalandgasdeposits.Assuch,theymaybenaturallypresentatlow concentrationsingroundwaterabstractedfromaquifersinthevicinityofthesedeposits,whetherBTEXhasbeen usedinfraccingfluidsornot.HydraulicfracturingmaycausealinkbetweenBTEXrichcoalseamandnearby groundwater.Theextentandnatureofthesefracturesdependonthedepthofthefracturingprocessandthelocal geomorphology.Aftercarefulmodellingandevaluation,theUSEPAreportconcludesthatthepossiblehydraulic connectionsareunlikelytorepresentasignificantpotentialthreattodrinkingwatersourcedfromgroundwater (USEPA2004).

BTEXintheenvironment 5. ImpactsofexposuretoBTEX 5.1. Inhumans AfterexposuretoBTEX,severalfactorsdeterminewhetherharmfulhealtheffectswilloccur,aswellasthetypeand severityofsuchhealtheffects.ThesefactorsincludetheamountofBTEXtowhichyouareexposedandthelengthof timeoftheexposure,aswellaswhichBTEXcompoundyouwereexposedto.OfthefourBTEXcompounds,benzene isthemosttoxic.MosttoxicitydataisavailableforairborneexposuretoBTEX,asthisisthemostcommonrouteof exposuretothesevolatilecompounds. Benzeneisrapidlyandefficientlyabsorbedandwidelydistributedthroughoutthebody.Exposuretoveryhigh concentrationsinair(10,000,000ppbandabove)cancausedeath(ATSDR2007a).Lowerlevels(700,0003,000,000 ppb)cancausedrowsiness,dizziness,rapidheartrate,headaches,tremors,confusion,andunconsciousness.Long termexposuretobenzenecancausecancerofbloodformingorgans(leukaemia).Eatingfoodsordrinkingliquids containinghighlevelsofbenzenecancausevomiting,irritationofthestomach,dizziness,sleepiness,convulsions, rapidheartrate,coma,anddeath.Thehealtheffectsthatmayresultfromeatingfoodsordrinkingliquidscontaining lowerlevelsofbenzenearenotknown(ATSDR2007a). Tolueneisreadilyabsorbedfromthegastrointestinaltractafteringestion,andisdistributedpreferentiallyinadipose tissue,thenthekidneys,liverandbrain.Themaineffectoftolueneisonthebrainandnervoussystem,withfatigue anddrowsinessbeingthemostobvioussymptoms(ATSDR2000). Ethylbenzeneisreadilyabsorbedfromthehumangastrointestinaltract.Animalstudiesshowenlargementofthe liverandkidneyathighdoses(400mg/kgbodyweightperday).Livereffectswerealsoobservedinanumberof inhalationstudies.Ingeneral,acuteandchronictoxicityislowinhumansalthoughsymptomssuchasirritationof eyesandtherespiratorytracthavebeenreportedathighlevelsofexposureinair(IPCS1996).Exposuretorelatively lowconcentrationsofethylbenzeneforseveraldaystoweeksresultedinpotentiallyirreversibledamagetotheinner earandhearingofanimals(ATSDR2007b). Xylenesarereadilyabsorbedafterinhalation.Bothshortandlongtermexposuretohighconcentrationsofxylene canalsocauseanumberofeffectsonthenervoussystem,suchasheadaches,lackofmusclecoordination,dizziness, confusion,andchangesinone'ssenseofbalanceaswellasirritatetheeyesandrespiratorytract(ATSDR2007c,IPCS 1997). 5.2. Inaquaticorganisms ToxicitytestingforBTEXcompoundshavealsobeenconductedonaquaticorganisms.Typicallywaterconcentrations inexcessof1mg/Larerequiredtoproduceacutetoxiceffectsinorganismssuchasalgae,daphnidsandfish.Dueto lowbackgroundconcentrationsofthesechemicalsinwater,rapidvolatilizationanddegradationprocessesandtheir lowtomoderatetoxicity,theoverallrisktotheaquaticenvironmentisthereforeconsideredlow.Itshouldbe noted,however,thathigherconcentrationsofthesechemicalscanoccurinwateratcontaminatedsites(IPCS1985, 1996,1997,USEPA2010).

BTEXintheenvironment 6. GuidelineBTEXlevels 6.1. Water PublichealthguidelinesforBTEXareavailablefordrinkingwaterintheAustralianDrinkingWaterGuidelines(ADWG; NHMRC2004).Inair,differenttypesofguidelinesareavailableforbothambientandoccupationalsettings(Air ToxicsNEPM;EPHC2004). Benzeneisaknowncarcinogen(cancercausing).TheADWGspecifythatitshouldnotbedetectedindrinkingwater. Forpracticalreasons,thedrinkingwaterguidelineforbenzeneis1ppb(whichistheanalyticaldetectionlimit) (NHMRC2004).Theremainingchemicals(toluene,ethylbenzeneandxylenes)arenotrecognizedascarcinogenic (IARC1989)andtheirdrinkingwaterguidelinesaremuchhigher(Table4). Itisimportanttounderstandthathealthguidelines(suchastheADWG)arebasedonanacceptabledailyintake.This istheamountofachemicalthatcanbeingestedeverydayoveralifetimewithoutadverseeffect.Drinkingwater guidelinesaresetaccordingtoanacceptabledailyintakebasedona70kgpersondrinking2litresofwatereveryday for70years.Theseguidelinesprovideasignificantmarginofsafetyforexamplemostpeopledonotdrink2litres ofwaterperdayandtheyarenotconstantlyexposedtoguidelinelevelsofcontaminantsintheirdrinkingwater supply.Thismeansthatshorttermexceedanceoftheguidelinesdonotnecessarilyrepresentasignificanthealthrisk dependingonhowoftenandhowlongtheseexceedancesoccur(enHealth2002). ThefollowingtablesummarizescurrentAustralianandselectedinternationalguidelinesbothfordrinkingand environmentalwatersforthefourcomponentsofBTEX. Table4.Waterguidelinesforbenzene,toluene,ethylbenzeneandxylene(BTEX).Allvaluesareinppb(g/L). Benzene Toluene CASRN1 71432 108883 QPHR2 1 800 ADWG3 1 800 (25for aesthetics)* 300 (3foraesthetics)* 600 (20for aesthetics)* WHO DWG4 10 700 USNPDWS5 5 1000 ANZECC(99% protection)6 600 180

Ethylbenzene Xylene

100414 1330207

300 600

300 500

700 10000 (totalxylenes)

50 200

ChemicalAbstractServicesRegistryNumber;2QueenslandPublicHealthRegulation(QHPR2005);3AustralianDrinkingWaterGuidelines 4 5 (NHMRC2004); WorldHealthOrganisationDrinkingWaterGuidelines(WHO2008); UnitedStatesNationalPrimaryDrinkingWater 6 Standards(USEPA2003); AustralianandNewZealandEnvironmentConservationCouncilEnvironmentalProtectionGuidelines(ANZECC 2000).*Toluene,ethylbenzeneandxyleneshavealoweraestheticsguidelinesthanahealthguideline.Thisisbecausethesecompoundswill benoticeablebysmellortastebeforetheybecomeahealthrisk.

BTEXintheenvironment 6.2. Air TheNationalEnvironmentProtection(AirToxics)Measure(AirToxicsNEPM)providesaframeworkformonitoring, assessingandreportingonambientlevelsoffiveairtoxicsthatincludesbenzene,tolueneandxylenetoassistinthe futuredevelopmentofnationalairqualitystandardsforthesepollutants.TheAirToxicsNEPMusestheterm 'monitoringinvestigationlevels'forairtoxics.Iftheselevelsareexceededthenfurtherinvestigationmaybe appropriate,butexceedancedoesnotindicatethatadversehealtheffectswilloccurandthegoalistogather sufficientdatanationallytofacilitatedevelopmentofstandards.Aswiththedrinkingwaterguidelines,benzenehas thelowestvalueat3ppb(Table5). InQueensland,theEnvironmentalProtection(Air)Policy2008(SoQ2008)specifiesguidelinesforbenzene,toluene andxylenesinairtoensureprotectionofhumanandenvironmentalhealthfromthosepollutantsinair(Table5). TheguidelineslevelsarebasedontheAirToxicsNEPMinvestigationslevels. Table5.Airqualityguidelinesforbenzene,toluene,ethylbenzeneandxylene(BTEX).Allvaluesareinppb. CASRN NEPMAirToxics (AnnualAverage) 3 100 NA 200 Queensland(Air)EPP (AnnualAverage) 3 100a NA 200b

Benzene Toluene Ethylbenzene Xylene

71432 108883 100414 1330207

Notes:awithconcentrationsupto1,000ppbacceptableforupto24h.bwithconcentrationsupto250ppbacceptable
forupto24h.NA:Notapplicable

7. Conclusions TheprimaryexposuretoBTEXisfrombreathingaircontaminatedbymotorvehicleemissions,industrialuseand cigarettesmoke.Thelevelsindrinkingwaterareusuallyverylowandintakefromdrinkingandfoodsourcesis usuallyminorincomparison.However,contaminationfromfuelspillageandindustrialactivitiescanresultin localisedhighconcentrationsinsurfaceandgroundwater.Inthoseinstances,activatedcarbonfiltrationisan effectivetreatmentoptiontoreduceBTEXconcentrationstoacceptablelevels. UseofBTEXinfraccingfluidsiscurrentlyoutoffavourduetotheavailabilityofsaferalternatives.Nevertheless,if BTEXwereusedinfraccingfluids,itisunlikelytosignificantlycontributetocontaminationofdrinkingwaterfrom groundwatersources.Groundwaterinthevicinityofnaturaloil,gasandcoaldepositsmayhowevercontainelevated levelsofnaturallyoccurringBTEXcompounds.Thelocalgeomorphologyandpossibilityofcreatinghydraulic connectionsbetweencoalseamandnearbygroundwatermustbetakenintoaccountpriortousinghydraulic fracturing.

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