给水工程英文文献翻译.docx

给水工程英文文献翻译.docx

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给水工程英文文献翻译

附录C：

外文文献及其译文

外文文献：

RemovalofPharmaceuticalsduringDrinkingWaterTreatment

Theeliminationofselectedpharmaceuticals（bezafibrate,clofibricacid,carbamazepine,diclofenac）duringdrinkingwatertreatmentprocesseswasinvestigatedatlabandpilotscaleandinrealwaterworks.Nosignificantremovalofpharmaceuticalswasobservedinbatchexperimentswithsandundernaturalaerobicandanoxicconditions,thusindicatinglowsorptionpropertiesandhighpersistencewithnonadaptedmicroorganisms.Theseresultswereunderscoredbythepresenceofcarbamazepineinbankfiltratedwaterwithanaerobicconditionsinawaterworksarea.Flocculationusingiron（III）chlorideinlab-scaleexperiments（Jartest）andinvestigationsinwaterworksexhibitednosignificanteliminationoftheselectedtargetpharmaceuticals.However,ozonationwasinsomecasesveryeffectiveineliminatingthesepolarcompounds.Inlabscaleexperiments,0.5mg/Lozonewasshowntoreducetheconcentrationsofdiclofenacandcarbamazepinebymorethan90%,whilebezafibratewaseliminatedby50%witha1.5mg/Lozonedose.Clofibricacidwasstableevenat3mg/Lozone.Underwaterworksconditions,similarremovalefficiencieswereobserved.Inadditiontoozonation,filtrationwithgranularactivatedcarbon（GAC）wasveryeffectiveinremovingpharmaceuticals.Exceptforclofibricacid,GACinpilot-scaleexperimentsandwaterworksprovidedamajoreliminationofthepharmaceuticalsunderinvestigation.

Introduction

InGermany,somepharmaceuticalsareusedinquantitiesofmorethan100t/yr

（1）.Pharmacokineticstudiesexhibitthatanappreciableproportionoftheadministeredpharmaceuticalsareexcretedviafecesandurine

（2）andthusarepresentinthedomesticwastewater.Afurthersourceforthecontaminationofwastewaterisassumedtobethedisposalof（expired）medicineviatoilets.However,thisportionisverydifficulttoestimatebecausereliabledataarenotavailable.Afterpassingthroughsewagetreatmentplants（STPs）,pharmaceuticalresiduesenterreceivingwaters.Pointdischargesfrompharmaceuticalmanufacturerscanalsocontributetocontaminationofriversandcreeks（3）.Firstresultsconcerningenvironmentaloccurrenceofpharma-ceuticalsarereportedbyGarrisonetal.（4）andHigniteandAzarnoff（5）,whodetectedclofibricacidinthelowermicrogramsperliterrangeintreatedsewageintheUnitedStates.Furtherstudiesin1981inGreatBritainrevealedthatpharmaceuticalsarepresentinriversupto1íg/L（6）.OnIonaIsland（Vancouver,Canada）Rogersetal.（7）identifiedthetwoantiphlogisticsibuprofenandnaproxeninwaste-water.Recentinvestigationsshowedtheexposureofawiderangeofpharmaceuticalsfrommanymedicinalclasses（e.g,betablockers,sympathomimetics,antiphlogistics,lipidregu-lators,antiepileptics,antibiotics,vasodilators）toriversandcreeks.ReviewsfromHalling-Sørensenetal.（8）,DaughtonandTernes（9）,andJørgensenetal.（10）summarizemostoftheliteratureinthisnewemergingfieldabouttheenviron-mentalrelevanceofpharmaceuticals.Furthermore,Mohleetal.（11）,Alderetal.（12）,Ternesetal.（3）,andZuccatoetal.（13）havereportedtheidentificationofpharmaceuticalsintheaquaticenvironment.

Contaminationisinfluencedbytherelativeportionsofrawandtreatedwastewater（14）suchthatevensmallriversandcreekscanbehighlycontaminated.Groundwateriscontaminatedwithpharmaceuticalsprimarilybyinfiltrationofsurfacewatercontainingpharmaceuticalresiduesaswellasbyleaksinlandfillsitesandsewerdrains.Becauseofthewidespreadoccurrenceofpharmaceuticalsintheaquaticenvironmentandsometimesalsointherawwaterofwaterworks,afewcasessurfacedwherepharmaceuticalsweredetectedindrinkingwaterinthelowernanogramsperliterrange（15,16）.Althoughuptonownoadversehealtheffectscanbeattributedtotheconsumptionofpharmaceuticalsattheselowconcentrationlevels,basedonprecautionaryprinciples,drinkingwatershouldbefreeofsuchanthro-pogeniccontaminants.

Currently,fewpapershavebeenpublisheddealingwiththeremovalofpharmaceuticalsindrinkingwatertreatment.Ozonationandespeciallyadvancedoxidationprocessesseemtobeveryeffectiveinremovalofdiclofenac,whileclofibricacidandibuprofenwereoxidizedinlab-scaleexperimentsmainlybyozone/H2O2asshownbyZwienerandFrimmel（17）.Hebereretal.（18）exhibitedthatreverseosmosisisappropriatetoremoveavarietyofdifferentpharmaceuticalsfromhighlycontaminatedsurfacewaters.

Theobjectiveoftheworkpresentedherewastostudytheefficiencyofdifferenttreatmentstepstoremovetheanti-phlogisticdiclofenac,theantiepilepticcarbamazepine,andthelipidregulatorsclofibricacidandbezafibrateduringdrinkingwatertreatment.Therefore,theprimaryeliminationoftheselectedpharmaceuticalswasinvestigatedunderlaboratory,pilot,andrealwaterworksconditions.Inadditiontoprocessessuchasbankfiltrationandartificialgroundwaterrecharge,widelyusedtechniquesforsurfacewatertreatmentsuchasactivatedcarbonfiltration,ozonation,andfloccula-tionwereinvestigated.ThemonitoringresultsoftwoGermanwaterworksareextendedbylab-andpilot-scaleexperimentstoobtainmoregeneralizedresults.

ExperimentalSection

SelectedPharmaceuticals.Foralllab-andpilot-scalespikingexperiments,fourrelevantpharmaceuticals（theantiphlo-gisticdiclofenac,theantiepilepticcarbamazepine,thelipidregulatorsclofibricacidandbezafibrate）havebeenselectedastargetcompounds.TheirmolecularstructuresareshowninTable1.ThesecompoundshavebeenchosenbecauseoftheirpredominantoccurrenceinGermanfeedingwatersforwaterworkssuchasrivers,bankfiltrates,andground-water（14,19）.Additionally,theantiepilepticprimidonewasincludedinoxidationexperimentsandawaterworkssurvey.

TABLE1.SelectedTargetPharmaceuticals

AnalyticalMethods.Thedeterminationofthepharma-ceuticalswasperformedusingdifferentanalyticalmethods（seeTable2）.Allmethodswerebasedonasolid-phaseextractionoftheanalytesontoRP-C18orLichroluteENmaterial.Aftersolid-phaseextraction（SPE）andanelutionstepwithmethanoloracetone,thecompoundswerederivatizedusingdifferentagents.Eitheramethylationwithdiazomethane（20）orasilylationwithamixtureofN,O-bis（trimethylsilyl）acetamide（BSA）and5%trimethylchlo-rosilane（TMCS）（Fa.Fluka,Buchs,Schweiz）wereused（60minat120°C）（21）.CarbamazepinewasdeterminedaftersilylationeitherbyamixtureofMSTFA/TMSI/DTE（N-methyl-N-（trimethylsilyl）

trifluoroacetamide/trimethylsilylim-idazol/dithioerytrit;1000íL/2íL/2íg）（22）orbyamixtureofBSA/TMCS.Forprimidone,anacetylationbyacetanhy-drideandethanolaminewasused（22）.Inallcases,GC-MSwasusedforthedetectionoftheanalytes.Furtherdetailsofthemethodsarereportedinrefs19-22.

Allmethodsenabletheprecisedeterminationofthetargetpharmaceuticalsinriverwateranddrinkingwater.Aninterlaboratorycomparisonexercise（ICE）betweenthethreeparticipatinglaboratoriesatthebeginningandtheendofthestudyconfirmedthequalityoftheanalyticalmethods.Groundwaterandsurfacewatersampleswerespikedwiththeselectedpharmaceuticalsandanalyzedbyallthreelaboratoriestoconfirmtherecoveriesoftheanalytesintherespectivematrixes.Themeanrecoveryofthespikedconcentrationsalwaysexceeded70%throughdifferentspikinglevels:

0.40-0.90íg/Linsurfacewaterand0.030-0.20íg/Lindrinkingwater.Therelativestandarddeviationsbetweenthethreeparticipatinglaboratorieswereingeneralbelow25%.Thus,itcouldbeshownthat（i）thedifferenceoffoundconcentrationswasminorbetweenthethreelaboratoriesand（ii）thespikedconcentrationcouldbedetectedinthegroundwaterandsurfacewateraccuratel.

LimitsofQuantification（LOQ）andCalibration.TheLOQwascalculatedaccordingtotheGermanDIN32645（23）withaconfidenceintervalof99%usingthestandarddeviationofalinearregressioncurve.Calibrationrangesfrom0.005to0.050íg/Landfrom0.05to1íg/Lwereusedwithatleastsevenconcentrationlevelsbyspikinggroundwater.LOQisanothertermforlimitofdetermination（LOD）mentionedinDIN32645.SincethecalculatedLOQvalueswerealwaysbetweenthefirstandthesecondcalibrationpoints,theLOQusedwassetasthesecondlowestcalibrationpointofthelinearcorrelationtoensureaprecisequantification.Hence,theLOQwereatleast20ng/Lfordiclofenac,carbamazepine,primidone,andclofibricacidanddownto50ng/Lforbezafibrate.However,withafinalvolumeof100íLinsteadof1mL,LOQdownto2ng/Lwereachievedforclofibricacid,primidone,diclofenac,andcarbamazepineanddownto10ng/Lforbezafibrate.Thecalibrationwasperformedoverthewholeprocedureafterspikinggroundwaterwiththestandardmixtureoftheselectedpharmaceuticals.Thecalculationoftheconcentrationsinnativesampleswascarriedoutusingsurrogatestandards（seeTable2）andalinear7-10pointcalibrationcurve.

ReferenceStandards.Thereferencestandardsclofibricacid,bezafibrate,carbamazepine,diclofenac,andprimidoneaswellasthesurrogatestandardsmeclofenamicacidand2,3-dichlorophenoxyaceticacid（2,3-D）werepurchasedfromSigma,Germany;dihydrocarbamazepinewaspurchasedfromAlltech,Germany.Allstandardsweredissolvedinmethanol（1mg/mL）anddilutedwithmethanoltothefinalstocksolutionof10íg/mL.

TreatmentProcessesUsedinWaterworks.（a）StudyofBiodegradationinBatchExperimentswithNativeSurfaceWater,Groundwater,andDifferentFilterMaterials.Bio-degradationisoneofthecrucialfactorsthatdeterminetheeli