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EmergingContaminantsinSoiland GroundwaterSystems
Occurrence,Impact,FateandTransport
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Emerging ContaminantsinSoil andGroundwater Systems
Occurrence,Impact,FateandTransport
Editedby BinGao
DepartmentofAgriculturalandBiologicalEngineering, UniversityofFlorida,Gainesville,FL,UnitedStates
Elsevier
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2.Occurrencesandimpactsofpharmaceuticalsand
2.4.1Overview15
2.5.2TranslocationofPPCPsfromsoilsandgroundwater intothefoodchain20
2.5.3Risksandimpactsofpharmaceuticals21
2.5.4RisksandimpactsofPCPs22
2.5.5Antibioticresistance23
2.6.1Sulfonamides24 2.6.2DEET28
3.Fateandtransportofpharmaceuticalsand personalcareproductsinsoilsandgroundwater
HaoChenandLintaAkhtar
3.1Overview
3.2Interactionwithsoilcomponents
3.2.1Hydrophobicity,polarity,andionizationof pharmaceuticalandpersonalcareproducts51
3.2.2Sorptionofpharmaceuticalandpersonalcareproducts tosoilmatrix51
3.2.3Pharmaceuticalandpersonalcareproductinteraction withplantroots60
3.3Pharmaceuticalandpersonalcareproductsfieldtransport studiesandmodeling 62
3.4Typicalsystemsofpharmaceuticalandpersonalcare productfateandtransportresearch 63
3.4.1Landfills63
3.4.2Septicsystem65
3.4.3Agriculturearea66
4.Occurrencesandimpactsofperfluorinatedcompounds insoilsandgroundwater 83
JianZhang,ShengsenWang,XianniYangandXiaozhiWang
4.1Overview 83
4.1.1Overviewofperfluorinatedcompounds83
4.1.2CategoriesofPFCs84
4.1.3Chemicalstructureandproperties86
4.2Applicationsandsources 88
4.2.1Mainapplications88 4.2.2Sources88
4.3Occurrences 90
4.3.1Occurrencesinsoils90
4.3.2Occurrencesingroundwater91
4.4Analyticaltechniques 95
4.4.1Sampling95
4.4.2Samplepretreatment96
4.4.3Instrumentalanalysis99
4.4.4Qualityassuranceandqualitycontrol99
4.5Risksandimpacts 100 4.5.1RisksofPFCs100
4.6Casestudies 107
4.7Conclusionandperspectives 109 References 110
5.Fateandtransportofperfluorinatedcompoundsin soilsandgroundwater 119
ChengliangLiandLongfeiLiu
5.1Overviewofper-andpolyfluoroalkylsubstances 119
5.2Interactionswithsoils 124
5.2.1Sorptionofper-andpolyfluoroalkylsubstances124 5.2.2Importantfactors131
5.3Retention,transport,andrelease 142
5.3.1Fateandtransportofper-andpolyfluoroalkyl substancesinsoilsandgroundwater142
5.3.2Impactfactors144
5.4Conceptualmodelsofper-andpolyfluoroalkylsubstance retention 152
5.4.1Solid-phaseadsorption152
5.4.2Partitioningtoair154
5.4.3Adsorptiontoair waterinterface155
5.4.4Nonaqueous-phaseliquids-waterpartitioning155
5.4.5Adsorptionatthenonaqueous-phaseliquids water interface156
5.5Conclusionandperspectives 156 References 157
6.Occurrencesandimpactsofengineerednanoparticles insoilsandgroundwater 165
YulinZheng,XianChen,NedgineD.Joseph,YueZhang,HaoChen andBinGao
6.1Overview 165
6.2Classificationofnanoparticles 166
6.2.1Definition166
6.2.2Naturalnanoparticles166
6.2.3Engineerednanoparticles167
6.3Sources,occurrences,andpathwaysofENPs 174
6.3.1Pathways174
6.3.2EnvironmentalconcentrationsofENPs175
6.3.3ENPsinsoilsandgroundwater176
6.4Analyticaltechniques 183
6.4.1Separationandsamplepreparation183
6.4.2Detectionandcharacterization185
6.5Risksandimpacts 187
6.5.1Transformations187
6.5.2Risksandimpacts193
6.6CasestudyofAgENPs 194
6.7Conclusionsandperspectives 197 References 197
7.Fateandtransportofengineerednanoparticlesin soilsandgroundwater 205
HuiminSun,ShiZhou,YanjiJiang,XianglongXi,YuehuiTan, GuangcaiZhang,NanJiang,TingZhou,XianqiangYin,MeiWang andBinGao
7.1Overview 206
7.1.1Classificationandapplicationsofmanufactured nanomaterials206
7.1.2ENPsinsoilsandgroundwater207
7.1.3RisksofENPsinsoilsandgroundwater209
7.2TransformationandstabilityofsubsurfaceENPs 210
7.2.1TransformationofENPsinthesubsurfaceenvironment210
7.2.2StabilityofENPsinthesubsurfaceenvironment210
7.3Retention,transport,andrelease 212
7.3.1EffectsofphysicochemicalpropertiesofENPs212
7.3.2Effectsofphysicochemicalpropertiesofporousmedia219
7.3.3Effectsofflowhydraulicpropertiesand solutionchemistry225
7.3.4Soilcolloids230
7.3.5Heavymetalsandorganicpollutants232
7.4Modeling 232
7.4.1Derjaguin Landau Verwey Overbeektheory232
7.4.2FiltrationofENPsinthesubsurfaceenvironment235
7.4.3One-dimensionalconvectivedispersionmodelfor saturatedporousmedia237
7.4.4One-dimensionalconvectivedispersionmodelfor unsaturatedporousmedia237
7.5Conclusionsandperspectives 238 References 239 Furtherreading 250
8.Occurrencesandimpactsofmicroplasticsin soilsandgroundwater 253 JinshengHuang,PanfengWu,ShunanDongandBinGao
8.1Overview 253
8.2Occurrencesandsources 256
8.2.1OccurrencesofMPsinsoilsandgroundwater256
8.2.2SourcesofMPsinsoils263
8.2.3SourcesofMPsingroundwater268
8.3Analyticaltechniques 269
8.3.1Generalprocedures269
8.3.2Samplecollection269
8.3.3Samplepreparation271
8.3.4Extraction272
8.3.5Identificationandquantification276
8.4Risksandimpacts 281
8.4.1Soilpropertiesandmicrobiota282
8.4.2Plantsandanimals283
8.4.3Humanexposure284
8.5Casestudies 285
8.5.1MPsingroundwaterwellsinIndia285
8.5.2MPsinpublicdrinkingwaterfountainsinMexico287
8.6Conclusionandperspectives 288 References 289
9.Fateandtransportofmicroplasticsinsoilsand groundwater 301 ShunanDong,ZebinYu,JunHuangandBinGao
9.1Overview 301
9.1.1Importanceofmicroplastictransportinsoilsand groundwater301
9.1.2Chaptergoals303
9.2Stabilityandaggregationofmicroplasticsinporewater 303
9.2.1Aggregationkinetic303
9.2.2Criticalcoagulationconcentration304
9.2.3Keyfactorsofmicroplasticaggregation304
9.3Retentionandtransportofmicroplasticsinsoiland groundwatersystems 307
9.3.1Chemicalfactors307
9.3.2Physicalfactors313
9.3.3Biologicalfactors317
9.4Cotransportwithothercontaminants 321
9.4.1Solublecontaminants321
9.4.2Micro/nanoparticles321
9.4.3Releasedcontaminantsbymicroplastics322
9.5Futureprospects 322 Acknowledgment 323 References 323 Index331
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Listofcontributors
LintaAkhtar DepartmentofAgriculture,UniversityofArkansasatPineBluff,Pine Bluff,AR,UnitedStates
HaoChen DepartmentofAgriculture,UniversityofArkansasatPineBluff,Pine Bluff,AR,UnitedStates
XianChen SchoolofChemistryandEnvironmentalEngineering,JiangsuUniversity ofTechnology,Changzhou,P.R.China
ShunanDong CollegeofAgriculturalScienceandEngineering,HohaiUniversity, Nanjing,P.R.China
BinGao DepartmentofAgriculturalandBiologicalEngineering,Universityof Florida,Gainesville,FL,UnitedStates
JinshengHuang DepartmentofAgriculturalandBiologicalEngineering,University ofFlorida,Gainesville,FL,UnitedStates
JunHuang HualanDesign&ConsultingGroupCo.Ltd.,Nanning,P.R.China; CollegeofCivilEngineeringandArchitecture,GuangxiUniversity,Nanning, P.R.China
NanJiang CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
YanjiJiang CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
NedgineD.Joseph DepartmentofChemicalEngineering,UniversityofFlorida, Gainesville,FL,UnitedStates
ChengliangLi CollegeofResourcesandEnvironment,ShandongAgricultural University,Tai’An,P.R.China
LongfeiLiu CollegeofResourcesandEnvironment,ShandongAgricultural University,Tai’An,P.R.China
HuiminSun CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
YuehuiTan CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
MeiWang SchoolofWaterConservancyandEnvironment,ZhengzhouUniversity, Zhengzhou,P.R.China
ShengsenWang CollegeofEnvironmentalScienceandEngineering,Yangzhou University,Yangzhou,P.R.China
XiaozhiWang CollegeofEnvironmentalScienceandEngineering,Yangzhou University,Yangzhou,P.R.China
PanfengWu JiangsuNantongEnvironmentalMonitoringCenter,Nantong,P.R. China
XianglongXi CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
XianniYang CollegeofEnvironmentalScienceandEngineering,Yangzhou University,Yangzhou,P.R.China
YichengYang DepartmentofAgriculturalandBiologicalEngineering,Universityof Florida,Gainesville,FL,UnitedStates
XianqiangYin CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
ZebinYu SchoolofResources,EnvironmentandMaterials,GuangxiUniversity, Nanning,P.R.China
GuangcaiZhang CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
JianZhang CollegeofEnvironmentalScienceandEngineering,Yangzhou University,Yangzhou,P.R.China
YueZhang DepartmentofAgriculturalandBiologicalEngineering,Universityof Florida,Gainesville,FL,UnitedStates
YulinZheng DepartmentofAgriculturalandBiologicalEngineering,Universityof Florida,Gainesville,FL,UnitedStates
ShiZhou CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
TingZhou CollegeofNaturalResourcesandEnvironment,NorthwestA&F University,Yangling,P.R.China
Chapter1 Introduction
BinGao
DepartmentofAgriculturalandBiologicalEngineering,UniversityofFlorida,Gainesville,FL, UnitedStates
ChapterOutline
1.1Overviewofsoilsandgroundwater1 1.2Typicalsoilandgroundwater contaminants2
1.3Emergingcontaminants3 1.4Organizationofthisbook4
1.1Overviewofsoilsandgroundwater
Sincethisbookmainlyfocusesonsoilandgroundwatercontamination,itis necessarytofirsttalkaboutsomebasicsofsoilsandgroundwater.Aswe know,thenaturalearthenvironmentcanberoughlyclassifiedintothreeinteractivezoneslayeredfromthetoptothebottomasatmosphere,surface,and subsurface(Fig.1.1).Soilsandgroundwaterarethetwomaincomponentsof thesubsurfaceenvironmentandcanbefurtherdividedintotwozones,the vadosezoneandgroundwater(Fig.1.1).Inthesoilandgroundwatersystems, soilservesasthematrixandwaterflowswithinthesoilpores.Infact,soils
arethemostcommonnaturalporousmediathatcanholdandstorewater insidetheirporesthroughthecapillaryforce.Asaresult,waterexistsinboth thevadosezoneandgroundwater.Duetothecombinedeffectofgravityand capillaryforces,thevadosezoneisonlypartiallysaturatedwithwater,while groundwateristhesaturatedzone(aquifer)belowthewatertable.
1.2Typicalsoilandgroundwatercontaminants
Typicalsoilandgroundwatercontaminantscanbecategorizedintothree types:metals/metalloids,organics,andnutrients(Fig.1.2).Typicalmetal andmetalloidcontaminantsthatarefrequentlydetectedinsoilsandgroundwaterincludinglead(Pb),chromium(Cr),arsenic(As),Zinc(Zn),cadmium (Cd),copper(Cu),mercury(Hg),andnickel(Ni),whichareoftencalled heavymetals.Theseheavymetalsmaybereleasedfromnaturalprocesses (e.g.,weathering)intothesoilsandgroundwater.However,industrialactivitiesthatinvolvetheacquisition,production,utilization,anddischargeofheavymetal containingmaterialsorwastesarethemaincontributorofthis typeofcontaminantsinthesubsurface.Inaddition,agriculturalpractices suchaslandapplicationoffertilizers,pesticides,manure,andbiosolidsthat oftencontaintraceamountsofheavymetalsmayalsocausetheiraccumulationsinsoilsandeventualreleaseintogroundwater.Themostcommonand toxicorganiccontaminantsinsoilsandgroundwaterarepersistentorganic compoundsincludingchlorinatedcompoundssuchastetrachloroethylene
(PCE),trichloroethylene,andpolychlorinatedbiphenyls;aromatichydrocarbonssuchasbenzene,toluene,xylenes,andpolycyclicaromatichydrocarbons;andpesticidessuchasinsecticidesandherbicides.Theyaregenerally releasedintothesoilandgroundwaterenvironmentduetoirresponsible industrialactivitiessuchaspinelineandstoragetankleaking,hazardous wasteandwastewaterdisposable,andabandonedanduncontrolledhazardous wastesites.Whenpesticidesaresprayedonagriculturalland,someofthem maybecarriedbywaterflowintothesubsurfacetodegradesoilandgroundwaterquality.Excessnutrientssuchasnitrogen(mainlynitrate)insoilsand groundwatermayalsopresentseriouscontaminationrisks.
Intheliteratureofsoilandgroundwatercontamination,thereareplenty ofresearchpapersandbooksonthefateandimpactsoftheabovementionedtypicalcontaminants,whicharenotcoveredinthisbook.Instead, thisworkfocusesonemergingcontaminantsinthesoilandgroundwater system.
1.3Emergingcontaminants
Emergingcontaminants,alsocalledcontaminantsofemergingconcern,refer agroupofnewlysurfacedenvironmentalpollutantsthatoftenhavenotbeen regulatedundercurrentenvironmentalregulationsorlaws.Emergingcontaminantsusuallyarerecalcitrant,toxic,bioaccumulable,andthusmayhave strongadverseimpactsontheecosystemsandpublichealth.Theyare increasinglybeingdetectedatlowlevelsinsoilsandgroundwater.With increasingpublicawarenessandadvancinganalyticaltechnologies,moreand moreemergingcontaminantshavebeenidentifiedandaddedtothelist.
Basedontheirsizesandstructures,emergingcontaminantscanbeput intotwomaincategories,chemicalsofemergingconcern(CECs)andparticlesofemergingconcern(PECs)(Fig.1.2).CECsconsistofmanychemical compoundsincludingpharmaceuticalsandpersonalcareproducts(PPCPs) andperfluorinatedcompounds(PFCs);whilePECsmainlycomprisetwo typesofparticulatepollutants,engineerednanoparticles(ENPs)andmicroplastics(MPs).TheconcentrationsofCECsinsoilsandgroundwaterare oftenatthelower μg/Llevel,whicharehardtobedetectedwithoutsophisticatedanalyticalinstrumentsuchasliquidchromatography-massspectrometry (LC-Ms)andLC-Ms/MS.AmongdifferenttypesofCECs,PPCPsandPFCs arethemostnotoriousonesthathavebeenfrequentlydetectedinsoilsand groundwater.ThereforethisbookonlycoversPPCPsandPFCsastherepresentativeCECsinsoilsandgroundwater.ForPCEs,theavailabilityand capacityoftheanalyticaltechniquesfordetectingENPsandMPsinenvironmentalsamplesstillneedimprovement.Nevertheless,goodprogresshas beenmadetowardtheexpandingofknowledgeontheoccurrences,fate,and impactsofENPsandMPsinsoilsandgroundwater,whichistheotherfocus ofthisbook.
4 EmergingContaminantsinSoilandGroundwaterSystems
1.4Organizationofthisbook
Theaimofthisbookistosummarizethecurrentstateofknowledgeandthe mostrecentresearchadvancementinemergingcontaminantsinsoilsand groundwater.Thebookhasninechapterscenteronfourtypesofmostwellknownemergingcontaminants,PPCPs,PFCs,ENPs,andMPs.Afterthe introductionchapter(Chapter1:Introduction),theoccurrencesandimpacts ofPPCPsinsoilsandgroundwaterarepresentedin Chapter2,Occurrences andImpactsofPharmaceuticalsandPersonalCareProductsinSoilsand Groundwater,whichnotonlyprovidesanoverviewofthepropertiesofdifferenttypesPPCPs,butalsooutlinesthedetailsontheirsources,detection methods,andpotentialrisksinsoilsandgroundwater. Chapter3,Fateand TransportofPharmaceuticalsandPersonalCareProductsinSoilsand Groundwater,mainlyfocusesonthefateandtransportofPPCPsinthesubsurface.Itsummarizesfindingsfromthemostrecentexperimentaland modelingstudiesontheretention,transport,andreleaseofPPCPsinthe vadosezoneandgroundwater.Thenextsixchaptersusethesamearrangementas Chapter2-3 with Chapter4-5 onPFCs, Chapter6-7 onENPs,and Chapter8-9 onMPs.Thisbookprojectwasinitiated,developed,andfinishedduringthecovid-19pandemic.Itistheresultofexcellentteamwork withtremendousindividualcommitmentsandeffortsfromeachofthecontributorsofallthechapters.
Chapter2
Occurrencesandimpactsof pharmaceuticalsandpersonal careproductsinsoilsand groundwater
YichengYang,YulinZheng,JinshengHuang,YueZhangandBinGao DepartmentofAgriculturalandBiologicalEngineering,UniversityofFlorida,Gainesville,FL, UnitedStates
ChapterOutline
2.1Overview5
2.2ClassificationsofPPCPs7
2.2.1Definition7
2.2.2Pharmaceuticals9
2.2.3Personalcareproducts10
2.3Pathwaysandmainsourcesof PPCPsinsoilsandgroundwater11
2.3.1Pathways11
2.3.2Domesticsewage12
2.3.3Landfill14
2.4Analyticaltechniques15
2.4.1Overview15
2.4.2Samplecollectionand preservation15
2.4.3Samplepreparation17
2.4.4Instrumentanalysisand detection18
2.1Overview
2.4.5Dataanalysis19
2.4.6Qualitycontrol19
2.5Risksandimpacts19
2.5.1Overview19
2.5.2TranslocationofPPCPsfrom soilsandgroundwaterintothe foodchain20
2.5.3Risksandimpactsof pharmaceuticals21
2.5.4RisksandimpactsofPCPs22
2.5.5Antibioticresistance23
2.6CasestudiesofPPCPsinsoilsand groundwater24
2.6.1Sulfonamides24
2.6.2DEET28
2.7Conclusionandperspectives32 References33
Pharmaceuticalandpersonalcareproducts(PPCPs)arerapidlygrowingemergingenvironmentalcontaminantsthathavebeendetectedinalmostallenvironmentalmatrices,includingsoilsandgroundwater(Barcelo ´ &Petrovic,2007).
PPCPsconsistoftwomajorcategoriesbasedontheiruses.Oneispharmaceuticals,whicharemainlyusedtodiagnose,prevent,ortreatthediseaseofhumans andanimalsforrestoringandimprovingfunctions(Pateletal.,2019).Theother ispersonalcareproducts(PCPs)includingagroupofchemicalstoprotect humansfrompotentialharmforimprovinglifequality(Brausch&Rand,2011). ExamplesofsometypicalPPCPsincludebroad-spectrumantibiotics,analgesics [e.g.,acetaminophen(Tylenol),ibuprofen(Advil),andaspirin],hormones,nonsteroidalanti-inflammatorydrugs(NSAIDs), β-blockers,lipidregulators,mood regulators,preservatives,disinfectants,insectrepellents,cosmetics,fragrances, andotherchemicalsubstancesusedwidelyindailylifefordifferentpurposes. DetailsoftheclassificationsofPPCPsaresummarizedin Section2.2.
ThelargeconsumptionofPPCPscausesthemtoentertheaqueousenvironmentdirectlyorindirectlythroughvarioushumanactivitiesincludinglivestock breeding,aquaculture,sewagedischarge,compostfertilizing,andlandfill.The concentrationlevelofPPCPsinsurfacewaterandgroundwaterisfromng/Lto μg/L.ManyPPCPsarepolar,highlybioactive,andopticallyactive.Theirconcentrationsintheenvironmentareusuallyhigherthanthetraceconcentrations. IthasbeenrecognizedthatcontinuousexposuretoPPCPsevenatlowconcentrationscanresultinunexpectedconsequences,whichmaybecomeathreatto thehumanandecologicalenvironment(Suietal.,2015).SincePPCPscan causeseriousenvironmentalandhealthrisks,theyhaveraisedcontinuedconcerninpastyears.TherearevarioustypesofPPCPswithdistinctproperties,so theirenvironmentalimpactsandriskscouldbeverydifferent.However,the potentialrisksofPPCPstotheenvironmentandtheecosystemcanneverbe underestimatedasmostofthemsharethesamenotoriouscharacteristics.(1) PPCPsarepseudo-persistentbecausetheirtransformationandremovalratesare relativelyhighinthenaturalenvironment.Nevertheless,PPCPs’introduction viasewagetreatmentplants(STPs)andsepticsystemsiscontinuousandincessant.(2)EachofthePPCPsisdevelopedforcertainbiologicalpurposes.Asa result,theycanmakebiologicaleffects,includingboththeexpectedandthe unexpectedones(sideeffects).(3)SomePPCPsmayhaveharmful xenobiotics-likephysicochemicalbehaviors,becausetheycanpersistforalong timebeforemakingacuringeffect.ThesePPCPsareoftenencapsulatedby certaincoatingmaterialsforavoidingthesubstancesfrombecominginactiveor degraded.SomePPCPsmayhavehighlipophilicityforpassingthroughmembranes.(4)Theheavyuseofpharmaceuticals,especiallyantibiotics,iscommon notonlyinhumandiseasetreatmentsbutalsoinveterinarymedicine.Inaddition,awiderangeofPCPshavebeendevelopedandusedindailylifeinrecent years.Morethan3000PPCPsarecurrentlyavailabletothepublicandnew substancesenterthemarketcontinuously(Arpin-Pontetal.,2016;Barcelo ´ & Petrovic,2007).Itisthusveryimportanttounderstandthefateandimpactsof PPCPsintheenvironment.Thebookisonemergingcontaminantsinsoilsand groundwater,sothischaptermainlyfocusesontheoccurrencesandimpactsof PPCPsinthesubsurface.
AnunavoidableconsequenceoftheincreaseduseofPPCPsistheir detectionintheenvironment,es peciallyintheaqueoussystems. OccurrencesofPPCPsinsurfacewater,STPeffluent,andwastewater treatmentplant(WWTP)effluenthavebeenwelldocumentedintheliterature( Esplugasetal.,2007;Kimetal.,2009;Yangetal.,2017 ). Becausethenaturalearthenvironmentismadeofinteractivezones(see Fig.1.1 ),PPCPsintheaquaticenvironmentcanbeanimportantsource ofPPCPsinsoilsandgroundwater( Christouetal.,2017 ).Infact,many studieshavealsobeenconductedtoexplorethesources,occurrences, andpathwaysofPPCPsinsoilsandgroundwater,whichisoneofthe focusesofthischapter( Section2.3 ).Ingeneral,theconcentrationsof PPCPsreportedinmostaquaticenvironmentsarelowandintheng/Lto lowmg/Lrange.PPCPconcentrationsinsoilsandgroundwatercanbe evenlowerthanthoseinsurfacewaterandwastewater( Lyuetal., 2020 ).ThereforeappropriateanalyticaltechniquesfordetectingPPCPs insoilsandgroundwaterareessentialandthusareanotherfocusofthis chapter( Section2.4 ). Section2.5 mainlycoverstherisksandimpactsof PPCPsinsoilsandgroundwater.TwocasestudiesoftwotypesoftypicalPPCPsinsoilsandgroundwaterarealsopresentedin Section2.6 .At theend( Section2.7 ),theperspectivesandpotentialfutureresearch directionsaresummarizedanddiscussed.
2.2ClassificationsofPPCPs
2.2.1Definition
Asindicatedintheprevioussectio n,PPCPscanbeclassifiedintotwo majorgroupsandmultiplesubgroup saccordingtotheirpropertiesand applications.Pharmaceu ticalsgenerallyconsistofantibioticdrugs,endocrinehormones,antipyreticsandanal gesics,anti-inflammatorydrugs, β-blockers,andbloodlipidregulato rs.PCPsarechemicalsusedincosmetics(e.g.,makeups,perfumes,mois turizers,etc.),hygieneproducts (shampoos,toothpaste,deodorants,e tc.),andprotectives[insectrepellents,sunscreenultravio let(UV)filters,etc.]. Table2.1 listssomeofthe commonlyusedPPCPsthathavebeendetectedintheenvironment.To date,morethan3000PPCPshavebeenusedforbothhumansandanimals toimprovetheirlivingstandards( Muthanna&Plosz,2008 ).Afterbeing releasedintothesoilandgroundwaterenvironment,mostofthePPCPs canbedegradedchemicallyorbiologically( Reddersenetal.,2002 ).Itis commonthatthedegradedPPCPconcentrationsinsoilsandgroundwater aresignificantlylowerthanthatofthecorrespondingoriginalcompounds, consideringthatmostofthePPCPsarenotpersistent.Someofthe PPCPs,however,areverystableinsoilsandgroundwaterandthusrequire specialattention( Hirschetal.,1999 ).
8 EmergingContaminantsinSoilandGroundwaterSystems
TABLE2.1 ClassificationsofPPCPs.
TypicalclassesRepresentativecompounds
A.Pharmaceuticals
A1.Broad-spectrumantibiotics
1aLevofloxacin
1bPenicillin
A2.Hormones
2a17-β-Estradiol(E2)
2bEstriol(E3)
2cEstrone(E1)
A3.Nonsteroidalanti-inflammatorydrugs (NSAIDs)
3aDiclofenac
3bIbuprofen
3cNaproxen
A4. β-Blockers
4aMetoprolol
4bPropranolol
A5.Bloodlipidregulators
5aClofibricacid
5bGemfibrozil
B.Personalcareproducts
B1.Preservatives
6aParabens
B2.Bactericides/disinfectants
7aMethyltriclosan
7bTriclocarban(TCC)
7cTriclosan(TCS)
B3.Insectrepellents
8a N,N-diethyl-meta-toluamide(DEET)
B4.Fragrances
9aGalaxolidefragrance(HHCB)
9bToxalidefragrance(AHTN) (Continued )
TABLE2.1 (Continued)
TypicalclassesRepresentativecompounds
B5.SunscreenUVfilters
10a2-Ethyl-hexyl-4-trimethoxycinnamate (EHMC)
10b4-Methyl-benzylidene-camphor(4MBC)
10cOctyl-methoxycinnamate(OMC)
10dOctyl-triazone(OC)
Source:FromYang,Y.,Ok,Y.S.,Kim,K.H.,Kwon,E.E.,&Tsang,Y.F.(2017).Occurrencesand removalofpharmaceuticalsandpersonalcareproducts(PPCPs)indrinkingwaterandwater/ sewagetreatmentplants:Areview. ScienceoftheTotalEnvironment, 596 597,303 320. https:// doi.org/10.1016/j.scitotenv.2017.04.102
2.2.2Pharmaceuticals
Pharmaceuticalcompoundsaremainl ydevelopedforcuringdiseases; thereforethemostcommonlyusedpharmaceuticalsareoftenassociated withcommonhumanandanimaldiseases.Manycompoundshavebeen developedasdrugsforhumanandveterinarymedicine.Forhumanpharmaceuticalsalone,thereareabout12,000approvedcompoundsand manyofthemhavereceivedconsiderableconcern. Fig.2.1 provides someexamplesofthemostcommonlydetectedpharmaceuticalsinthe environment,whichcanbeclassifiedintosevencategoriesincluding antibiotics,NSAIDs,antihypertensive s,lipidregulators,antidepressants, anticonvulsants,andhormones( Cizmasetal.,2015 ).Amongthem,antibioticshavereceivedspecialattentionbecausetheyarethemostwidely usedforbothhumansandanimalsandthusarethemostfrequently detectedintheenvironmentincludingsoilandgroundwatersystems ( Chaturvedietal.,2021;Kovalakovaetal.,2020 ).Basedontheiroccurrencesinsoilsandgroundwater,sever alsubgroupsofantibioticssuchas sulfonamides,fluoroquinolone s,tetracyclines,macrolides,and β-lactam haveattractedmuchresearchinterestintheliterature( Daietal.,2020; Riazetal.,2018;Wegst-Uhrichetal.,2014 ).Manyofthemareamphotericandionizablecompounds,grantingthemgoodsolubilityinwater andthusrelativelyhighmobilityin soilsandgroundwater.Inadditionto antibiotics,synthetichormoneshavealsobeenfrequentlydetectedin soilsandgroundwaterandthusreceivedmuchattention( Gottschall etal.,2013 ).Amongthem,17-estradiolisa representativethataffects theovariesandplacenta( Panetal.,2009;Xuetal.,2020 ).
FIGURE2.1 Mostcommonlydetectedpharmaceuticalsintheenvironment. FromCizmas, LeslieSharma,VirenderKGray,ColeMMcDonald,ThomasJ.Pharmaceuticalsandpersonal careproductsinwaters:occurrence,toxicity,andrisk. Environmentalchemistryletters, 13(4), 381 394.
2.2.3Personalcareproducts
PCPsoftencontainavarietyofcompoundsincludingoneswithsevere, unknown,minor,orevennoenvironmentalrisks,whichmaketheclassificationofPCPsintheenvironmentverydifficult.Ingeneral,PCPsinthemarket aredividedintodifferentcategoriesbasedontheirusessuchasoralcare,skin care,haircare,bodycare,decorativecosmetics,etc.Afterthedisposal,much attentionhasbeenpaidtothetoxiccompoundsinthePCPs.ForPCPsinsoils andgroundwater,bisphenolAisoneofthemostcommonlydetectedtoxic compounds(Careghinietal.,2015).BisphenolAisproducedinlargequantitiesforusewidelyinmanyconsumerproductsindailylife.Itbelongsto endocrinecompoundsandcandisrupthumanhormonesecretionandalso affectsoilecosystemfunctions(Novoetal.,2018).Pesticides,fungicides,and herbicidesarealsocommonlyusedinPPCstoimprovelifequality.Forexample,insectrepellent(bugspray)oftencontainssyntheticchemicalcompounds astheactiveingredienttokillbugs.Someofthecommonlyusedcompounds include N,N-diethyl-meta-toluamide(DEET),Icaridin, p-menthane-3,8-diol, ethylbutylacetylaminopropionate,and2-undecanone,whichmaybeindirectly releasedintothesoilandgroundwatersystemsaftertheuse.Inadditiontothe indirectrelease,someoftheseactiveingredientsinpesticides,herbicides,and
fungicidesusedinagriculturalproductioncanbedirectlyreleasedintosoilsto affectthequalityandhealthofsubsurfacesystems(Tianetal.,2016;Zhang etal.,2013).Onceenteringthesoilandgroundwatersystems,itisalmost impossibletodeterminewhetherthesecompoundsarefromthePCPsoragriculturalpractices.
2.3PathwaysandmainsourcesofPPCPsinsoilsand groundwater
2.3.1Pathways
Asshownin Fig.2.2,PPCPscanenterthesoilandgroundwatersystems throughseveralpathways(Boxalletal.,2012;Lambropoulou&Nollet, 2014;Priceetal.,2010).ThemostcommonPPCPpollutionhotspots includeWWTPs/STPs,septictanks,hospitals,animalfarms,aquaticfarms, andagriculturalland(especiallytheoneswithmanuresandbiosolidapplications).Furthermore,untreatedhouseholdeffluentandtreatedeffluentsfrom industriesandmedicalservicesmaycontainsomepartiallydegradedand refractoryPPCPs.ThisPPCPs-contaminatedwatermaydirectlydischarge intovariousreceivingwaterbodieswithoutpropertreatment. Luoetal. (2014) reviewedtheoccurrencesofPPCPsinaquaticenvironments,
FIGURE2.2 SummaryofthepathwaysofPPCPsintosoilsandgroundwater.
includingsewage,surfacewater,andgroundwater.Becausesoilsandwater areinteractive,PPCPresiduesincanalsoenterthesubsurfaceenvironment throughthenaturalhydrologiccycle(Mompelatetal.,2009;Petrovi ´ cetal., 2003).
Althoughdifferenttechnologieshavebeenappliedtotreatmunicipal wastewater,domesticsewageisstilloneofthemajorsourcesofPPCPs releasedintothesoilandgroundwatersystems.Thereareseveralother PPCPexposurepathwaysincludingtheunusedmedicinedisposalinlandfills, veterinarymedicinesrunofffromfarmyards,disposaloftheanimalcarcasses,andreclaimedwaterirrigation(Awadetal.,2014;Ficketal.,2009). ThemanagementandusepracticesofPPCPsvaryindifferentregionsofthe world.Hence,thesignificanceofdifferentPPCPsexposurepathwaysinsoils andgroundwatercanvarygeographically.Forexample,incertainregions aroundtheworld,theconnectivitytoSTPsislimited.Thereforeexposure modelsbasedonaspecificregionmaynothavewideapplicability.
2.3.2Domesticsewage
DomesticsewageisoneofthemajorcontributorstoPPCPpollutantsinsoils andgroundwater.Drugsforhumanoranimaltreatmentcanalwaysfindtheir wayintotheenvironmentincludingsoilsandgroundwater.Inparticular, pharmaceuticalswithhighstabilityandsolubility,suchasmethotrexate,are excretedfromthebodyviaexcretion,dischargedintotheseweragesystems, andfinallyreleasedintosoilsandgroundwater(Kimetal.,2011;Kimura etal.,2007).PCPs,includingmakeups,toothpaste,soaps,handsanitizers, UVfilters,etc.,arewashedofffromhumanbeingswithwastewaterintothe STPs.Inaddition,sloughingduringrecreationalactivities,suchasswimming,cancontributetoPCPdischarge(Brausch&Rand,2011).These PPCPsandtheirderivativesinthesewagesystemscanbeamajorpollution sourcetosoilsandgroundwaterbecausetheconventionalSTPsandWWTPs arenotdesignedtoandthushavelimitedabilitytotreattheseemergingcontaminants(Kostichetal.,2014;Yangetal.,2017).
Typicaltreatmentprocessesforsewage(Fig.2.3),includingscreening, degritting,primarysedimentation,aerationtanks,andfinalsedimentation, cannoteliminatePPCPsefficiently(Carballaetal.,2004).PPCPremovalin STPs/WWTPsiscomplicatedandcloselyrelatedtothebiologicalandphysicochemicalpropertiesofcontaminants,includinghydrophilicity,solubility (Evgenidouetal.,2015),volatility,andbiodegradability(Jonesetal.,2005). SomePPCPssuchastetracyclinecanbeeffectivelyeliminatedfromsewage (Yangetal.,2017).However,inconventionalSTPs/WWTPswithprimary andsecondarytreatmentprocesses,mostPPCPscanbeonlypartiallyeliminated.Thecapabilityofsedimentationastheprimarytreatmentprocess,in removingPPCPs,canbeverylimitedduetothehydrophilicnatureofmost PPCPs(Carballaetal.,2005).ComparedwiththatofPCPs,theremoval
FIGURE2.3 Typicaltreatmentprocessesforsewage:(A)FlowdiagramofconventionalSTPs; (B)FlowdiagramofconventionalWTPs. FromYang,Y.,Ok,Y.,Kim,K.,Kwon,E.,&Tsang, Y.(2017).Occurrencesandremovalofpharmaceuticalsandpersonalcareproducts(PPCPs)in drinkingwaterandwater/sewagetreatmentplants:Areview. ScienceoftheTotalEnvironment, 596 597,303 320. https://doi.org/10.1016/j.scitotenv.2017.04.102.
efficiencyofpharmaceuticalsbytheprimarytreatmentismuchlower.For example,tetracyclineandmethylparabencanberemovedinsedimentation tanksbutthereisnoconsiderablereductioninibuprofenandsulfamethoxazole(Yangetal.,2017).Secondarytreatmentmainlyreferstobiologicalprocesses[e.g.,activatedsludgeprocess(ASP)]andremovesPPCPsthroughthe partition,adsorption,biotransformation,andbiodegradation(McClellan& Halden,2010).TheremovalrateofPPCPsinASPisclosedrelatedtothe natureofPPCPs,hydraulicretentiontime,sludgeage,adsorptioncapacity onsludge,andreactordesign(Evgenidouetal.,2015).Duringthebiological process,evenifinthesameclass,theremovalratesofdifferentPPCPscan vary.Ibuprofen,ketoprofen,anddiclofenacareallNSAIDs.Ibuprofenand ketoprofenbiodegradationratescanbeupto75% 87%,butthediclofenac removalrateisusuallylowerthan25%duringsecondarytreatment(Salgado etal.,2012;Wangetal.,2014).
TertiarytreatmentprocesseshavebeenusedtoremovethePPCPsthat arepoorlyeliminatedbythesecondarytreatmentprocesses.Several advancedtreatmenttechnologiessuchasmembranefiltration,activatedcarbonadsorption,andadvancedoxidationprocesses(AOPs)havebeenapplied inthetertiarytreatmenttoremovePPCPsfromsecondary-treatedwastewater.Membranefiltrationprocesses,includingnanofiltration(NF)andreverse osmosis(RO),arepromisingtreatmentmethodstoremovePPCPsfrom wastewater(Nghiemetal.,2004;Yoonetal.,2006).Ultrafiltration(UF)and microfiltration(MF)mayalsobeusedforremovingPPCPs.However,their removalperformancesarenotideal,consideringthattheirmembranepore sizesareconsiderablylargerthanmostPPCPmolecules.WhileNFandRO
