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-degradationisoneofthecrucialfactorsthatdeterminetheeliminationoforganiccompoundsduringarti