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Use of bone meal amendments to immobilise Pb, Zn and Cd in soil, A leaching column study.pdf

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Use of bone meal amendments to immobilise Pb, Zn and Cd in soil, A leaching column study.pdf

,MUSEUMRECEIVED25AUGUST2005;RECEIVEDINREVISEDFORM7FEBRUARY2006;ACCEPTED10FEBRUARY2006ANEXTENDED18MONTHSLEACHINGCOLUMNSTUDYOFMETALPB,ZN,CDIMMOBILISATIONUSINGBONEMEALASASOURCEOFPHOSPHATE,DEMONSTRATINGPOSITIVERESULTSABSTRACTTHEAIMOFTHISSTUDYISTOTESTTHESTABILISATIONOFMETALSINCONTAMINATEDSOILSVIATHEFORMATIONOFLOWSOLUBILITYMETALPHOSPHATESBONEAPATITE,INTHEFORMOFCOMMERCIALLYAVAILABLEBONEMEAL,WASTESTEDASAPHOSPHATESOURCEONAMINEWASTECONTAMINATEDMADEGROUNDWITHHIGHLEVELSOFPB,ZNANDCDTRIPLICATELEACHINGCOLUMNSWERESETUPATBONEMEALTOSOILRATIOSOF125AND110,INADDITIONTOUNAMENDEDCONTROLS,ANDWERERUNFOR18MONTHSTHECOLUMNSWEREIRRIGATEDDAILYWITHASYNTHETICRAINSOLUTIONATPHOF2,3,AND44AFTER100DAYS,THELEACHATEPB,ZNANDCDCONCENTRATIONSOFALLAMENDEDCOLUMNSWERESIGNIFICANTLYREDUCEDFOR110TREATMENTS,RELEASEOFTHESEMETALSWASSUPPRESSEDTHROUGHOUTTHETRIALFOR125TREATMENTS,ZNANDCDCONCENTRATIONSINTHELEACHATESBEGANTOINCREASEAFTER300DAYSDTPAANDWATEREXTRACTIONSSHOWEDTHATPBANDCDWEREMORESTRONGLYHELDINTHEAMENDEDSOILSTHISSTUDYCONCLUDESTHATTHECOMPLEXITYOFSOILPROCESSESANDTHESMALLQUANTITIESOFMETALSSEQUESTEREDPRECLUDEDDETERMINATIONOFAMETALIMMOBILISATIONMECHANISMC2112006ELSEVIERLTDALLRIGHTSRESERVEDKEYWORDSMETALIMMOBILISATION;PHOSPHATE;BONEMEAL;APATITE;LEAD;ZINC;CADMIUM;SOILCOLUMN1INTRODUCTIONMETALSMAYBEPRESENTINSOILSFROMAVARIETYOFSOURCESANDCANREPRESENTAPOTENTIALHAZARDTOHUMANSANDTHEENVIRONMENTIFTHEYAREREADILYRELEASEDINTOSOILSOLUTIONORAREOTHERWISEAVAILABLETOBIOLOGICALPROCESSESHOWEVER,IFSUCHMETALSAREBOUNDUPINRELATIVELYINERTANDINSOLUBLECOMPOUNDS,THEDANGERTHEYREPRESENTISREDUCEDSUBSTANTIALLYTHEPHOSPHATESOFMANYMETALSINCLUDINGPB,ZN,CD,CUANDARESTABLEACROSSAVERYWIDERANGEOFENVIRONMENTALEHANDPHCONDITIONSTHERENOWEXISTSASIGNIFICANTBODYOFRESEARCHSHOWINGSUCHCOMPOUNDSMAYREADILYFORM,GIVENTHEPRESENCEOFASOURCEWHICHRELEASESSUFFICIENTPHOSPHATETOSOLUTIONEGVALSAMIJONESETAL,1998;CAOETAL,2003;HETTIARACHCHIANDPIERZYNSKI,2004THEAMENDMENTOFSOILSWITHPHOSPHATEMAYHAVETHEPOTENTIALTOREDUCESIGNIFICANTLYMETALBIOAVAILABILITYANDRELEASETOGROUNDANDSURFACEWATERSMUCHOFTHISRESEARCHHASLARGELYBEENCONCERNEDWITHPBUSEOFBONEMEALAMENDMENTSINSOILALEACHINGIRSNEDDONA,1,MORUEETXEBARRIAAEVALSAMIJONESADEPARTMENTOFMINERALOGY,THENATURALHISTORYBENVIRONMENTALSCIENCE,SCHOOLOFBIOSCIENCE,THEUNIVERSITYCDEPARTMENTOFSOILSCIENCE,SCHOOLOFHUMANANDENVIRONMENTALSCIENCES,ENVIRONMENTALPOLLUTION144ANDNICANHAVEEXCEPTIONALLYLOWSOLUBILITIESNRIAGU,1984CORRESPONDINGAUTHORTEL4421079425334;FAX4421079425537EMAILADDRESSEVALSAMIJONESNHMACUKEVALSAMIJONES1PRESENTADDRESSCAWTHRONINSTITUTE,98HALIFAXSTREETEAST,PRIVATEBAG2,NELSON,NEWZEALAND02697491/SEEFRONTMATTERC2112006ELSEVIERLTDALLRIGHTSRESERVEDDOI101016/JENVPOL200602008TOIMMOBILISEPB,ZNANDCDCOLUMNSTUDYB,MEHODSONA,C,PFSCHOFIELDA,A,,CROMWELLROAD,LONDONSW75BD,UKOFNOTTINGHAM,UNIVERSITYPARK,NOTTINGHAMNG72RD,UKTHEUNIVERSITYOFREADING,WHITEKNIGHTS,READINGRG66DW,UK2006816E825WWWELSEVIERCOM/LOCATE/ENVPOLIMMOBILISATIONVIATHEPRECIPITATIONOFTHEPBAPATITEGROUPMINERALPYROMORPHITEPB5PO43OHINTHEPRESENCEOFSOLUBLEPHOSPHATEINSYNTHETICSOLUTIONS,PYROMORPHITEHASBEENSHOWNTOFORMRAPIDLYINCONDITIONSCONSISTENTWITHTHOSEFOUNDINMANYSOILENVIRONMENTSXUANDSCHWARTZ,1994INSEVERALEXPERIMENTSUSINGMETALCONTAMINATEDSOILS,EVIDENCEFORPBPHOSPHATEFORMATIONHASBEENOBTAINEDEGCOTTERHOWELLSETAL,1994EXPERIMENTSWHEREPBUPTAKEBYPLANTSWASMEASUREDHAVEINDICATEDTHATITSAVAILABILITYISREDUCEDINPHOSPHATETREATEDCONTAMINATEDSOILSLAPERCHEETAL,1997;BROWNETAL,1999THEFORMATIONOFOTHERMETALPHOSPHATES,INCLUDINGTHOSEOFZN,CU,CDANDU,HASALSOBEENIMPLICATEDMAETAL,1994;CHENETAL,1997;VALSAMIJONESETAL,1998ANDINSOILS,THEBIOAVAILABILITYOFMETALSHASBEENREDUCEDSIGNIFICANTLYAFTERPHOSPHATEADDITIONHETTIARACHCHIANDPIERZYNSKI,1999GIVENTHATPHOSPHATEITSELFCANLEADTOENVIRONMENTALPROBLEMSSUCHASEUTROPHICATIONOFSURFACEWATERS,DUETOITSROLEASANUTRIENT,THECHOICEOFPHOSPHATESOURCEFORSOILREMEDIATIONISANIMPORTANTONEFURTHERMORETHEPRESENCEOFARSENICINMANYMETALCONTAMINATEDSOILSSHOULDBETAKENINTOCONSIDERATION,ASAQUEOUSPHOSPHATEMAYCOMPETEWITHARSENATEFORADSORPTIONSITESANDMAYCAUSEASMOBILIZATIONEGBOISSONETAL,1999THECALCIUMPHOSPHATEMINERALHYDROXYLAPATITECA5PO43OHHASARELATIVELYLOWSOLUBILITYWHENPRESENTINITSROCKCRYSTALFORMTHOUGHWORKBYSOMERESEARCHERSSUPPORTSITSPOTENTIALFORREMEDIATIONOFTOXICMETALCONTAMINATIONINSOILSHETTIARACHCHIANDPIERZYNSKI,2002;CAOETAL,2003HYDROXYLAPATITEISALSOTHEPRINCIPALMINERALCONSTITUENTOFBONE,ANDBONEMEALHASBEENIDENTIFIEDASAPOTENTIALLYAPPROPRIATESOURCEOFPHOSPHATEDUETOTHEMODERATESOLUBILITYASSOCIATEDWITHITSCARBONATECONTENTTUNG,1998;VALSAMIJONESETAL,1998ANDPOORLYCRYSTALLINESTRUCTURECHEUNGETAL,2002EARLIERWORKWITHBONEMEALAMENDMENTSHASBEENENCOURAGINGLABORATORYEXPERIMENTSUSINGAVARIETYOFSOILSHAVESHOWNRELEASEOFMETALSTOPOREWATERSTOBEREDUCEDSIGNIFICANTLY,WITHACORRESPONDINGREDUCTIONINMETALSAVAILABILITYTOPLANTSANDSOILORGANISMSHODSONANDVALSAMIJONES,2000A;DAVIESETAL,2003ITHASALSOBEENSHOWNRECENTLYTHATINCINERATEDBONEMEALISAVERYEFFECTIVESORBINGAGENTFORASVSNEDDONETAL,2005THEPREVIOUSWORKONMETALIMMOBILIZATIONBYBONEMEALWASCARRIEDOUTMOSTLYONACIDICSOILSANDFORSHORTPERIODSOFTIMEUPTO4MONTHSTHEREFORE,THEPERMANENCEOFSUCHREDUCTIONSNEEDSTOBEDEMONSTRATEDFURTHER,ESPECIALLYINSOILSWITHHIGHMETALLOADINGSACROSSARANGEOFSOILCOMPONENTFRACTIONSTHISPAPERREPORTSONTHERESULTSOFANEXTENDED18MONTHSLEACHINGSTUDYCARRIEDOUTTOINVESTIGATETHEEFFECTIVENESSOFBONEMEALAMENDMENTSINREDUCINGTHEMOBILITYOFTHEMETALSPB,ZNANDCDINACONTAMINATEDMINEWASTEMADEGROUNDOFABOVENEUTRALPH2MATERIALSANDMETHODS21SOILTHECHOSENSOILACTUALLYMADEGROUNDWASFROMANAREAOFEXTENSIVEGRAVELTAILINGSASSOCIATEDWITHHISTORICALPBMININGATNENTHEADINCUMBRIA,UKTHISWASAHETEROGENEOUSMADEGROUND,DERIVEDFROMACARBONATEHOSTEDIRSNEDDONETAL/ENVIRONMENTALOREMETALSLEACHINTOSURFACEWATERSFROMTHESPOILHEAPSANDTAILINGSDAMSANDALSOFROMDISUSEDMINEADITSDUETOINTERACTIONWITHCALCAREOUSCARBONIFEROUSROCKS,CATCHMENTWATERSHAVEHIGHHARDNESSGENERALLYGREATERTHAN200MG/LASCACO3,HIGHALKALINITYGENERALLYGREATERTHAN100MG/LASHCO3C255ANDPHINTHERANGE74E80NUTTALLANDYOUNGER,2000DUETOELEVATEDLEVELSOFZN,THERIVERNENTHASAVERYLIMITEDAQUATICFAUNAOTHERECOTOXICMETALSSUCHASPB,CDANDASAREALSOPRESENTNUTTALLANDYOUNGER,1999ATTHENENTHEADSITE,MADEGROUNDUSEDINTHETRIALWASREMOVEDTOADEPTHOF20CMANDTOENSUREHOMOGENEITY,WASDRYSIEVEDTO2MMANDWELLMIXEDUSINGTHE2MMSIZEFRACTIONALSOSERVEDTOBOTHMAXIMISEREACTIVESURFACEAREAANDMINIMISETHEPOTENTIALFORCHANNELLINGFLOWREGIMESINTHECOLUMNSPRIORTOSIEVING,THETEXTUREOFTHESOILWASTHATOFASANDYGRAVEL,WITH72OFTHEMATERIALINTHE2MMSIZEFRACTIONANDAFURTHER26BETWEEN2MMAND75MM22LEACHINGCOLUMNSSETUPINORDERTOFACILITATECOMPARISONTOEARLIERWORKWITHOTHERSOILS,THELEACHINGCOLUMNEXPERIMENTSWERESETUPFOLLOWINGAMETHODOLOGYUSEDPREVIOUSLYANDDESCRIBEDINDETAILINHODSONANDVALSAMIJONES2000BSEEALSOHODSONETAL,2001,ANDASCHEMATICINHODSONANDLANGAN,1999THECOLUMNSWEREMADEFROMINVERTED250MLPOLYPROPYLENEBOTTLESWITHTHEIRBASESREMOVEDANDASMALLHOLEDRILLEDINTHEIRCAPSTHESOILWASUNDERLAINBYALAYEROFQUARTZWOOLANDANOTHEROFPOLYPROPYLENEBEADSTOFILTERTHELEACHATEANDENSUREFREEDRAINAGETHESELAYERSWEREREPEATEDATTHETOPOFTHESOILCOLUMNTOAIDINEVENIRRIGANTDISTRIBUTIONANDLIMITEVAPORATIVELOSSESTHECOLUMNSWEREPROTECTEDFROMLIGHTTOINHIBITALGALGROWTHBONEMEALANDSOILWEREMIXEDTOGETHERTHOROUGHLYTOENSUREHOMOGENEITY;200GOFAIRDRIEDSOILOR200GSOILINSOIL/BONEMEALMIXWASADDEDTOEACHCOLUMNTHEDIAMETEROFTHE250MLPOLYPROPYLENEBOTTLESWAS57MMANDTHEDEPTHOFTHESOILCOLUMNWASAPPROXIMATELY65MMTHEVARIABLESEXAMINEDWEREBONEMEALTOSOILRATIONOAMENDMENT,125AND110ANDIRRIGANTPH2,3AND44;PHWASADJUSTEDBYSMALLADDITIONSOFNITRICACID,FROMASTARTINGVALUEOF48ALLOFTHEEXPERIMENTSWERECARRIEDOUTINTRIPLICATEIRRIGATIONWASCARRIEDOUTMANUALLYBYPIPETTEFIVEDAYSPERWEEK,10MLOFASYNTHETIC‘‘RAIN’’SOLUTIONWASDISTRIBUTEDEVENLYTOTHETOPOFTHECOLUMNSTHEIRRIGANTWASFORMULATEDSOASTOAPPROXIMATETHECOMPOSITIONOFNATURALRAINTABLE1ANDAPPLIESTOIRRIGANTPHOF44THETWOLOWERPHVALUESWEREUSEDTOTESTTHEPOTENTIALEFFECTSOFACIDIFICATIONEGVIAACIDRAINTOTHETREATMENTTHEIRRIGATIONRATEWASCHOSENDBASEDONSURFACEAREAFORINFILTRATIONDEQUIVALENTTOANNUALPRECIPITATIONOF1300MMRAINFALLFORTHENENTHEADAREAFORTHEYEARTOOCTOBER1,2001WAS1247MM;DATAFROMBOLTSHOPEPARKSYNOPTICSTATIONHTTP//WWWMETOFFICECOM/CLIMATE/UK/NETWORKS/INDEXHTMLTHELEACHATECOLLECTEDBENEATHTHECOLUMNS,WASSAMPLEDATINTERVALSOVERTHECOURSEOFTHETRIALANDANALYSEDFORMETALS,CAANDPBYICPOESINDUCTIVELYCOUPLEDPLASMAEOPTICALEMISSIONSPECTROMETRYLEACHATESWERECOLLECTEDIN100MLPOLYPROPYLENESAMPLEBOTTLESTOWHICH1MLCONCENTRATEDARISTARGRADENITRICACIDHADBEENADDEDLEACHATESWERECOLLECTEDWEEKLY,ANDTHEPREACIDIFICATIONWASUNDERTAKENTOSTABILISETHELEACHATEDURINGTHECOLLECTIONPERIODONOCCASIONS,UNACIDIFIEDLEACHATESWERECOLLECTED,FILTEREDANDTHENACIDIFIED,TOASCERTAINTHATPREACIDIFICATIONOFCOLUMNFILTEREDLEACHATESDIDNOTINTRODUCEANYERRORSINTHEMEASUREDCONCENTRATIONSLEACHATESWEREVISUALLYEXAMINEDFORTURBIDITYBUTNONEWASEVEROBSERVED23SAMPLEPREPARATIONANDANALYSISTHEPREACIDIFIEDLEACHATESWEREWEIGHEDTOALLOWFORDILUTION,THENFILTEREDMILLIPORE022MINTOPOLYPROPYLENEVIALSSAMPLESWERESTOREDAT4C14CFORNOMORETHAN5DAYSBEFOREANALYSISPREACIDIFICATIONOFTHELEACHATETABLE1COLUMNIRRIGANTCOMPOSITIONANITRATEAMMONIUMNAMGCACHLORIDESULPHATE247047180036029348106UNITSAREMG/L817POLLUTION1442006816E825ACONCENTRATIONSMEASUREDATPH48ANDPRIORTOPHADJUSTMENTFOREACHINDIVIDUALIRRIGANTPH22ISTRYWEREPERFORMEDUSINGAVARIANVISTAPROAXIALICPOES;12KWRFPOWERANDUSINGAMEINHARDTCONCENTRICNEBULISERMATRIXMATCHEDSTANDARDSANDBLANKSWEREUSED,TOGETHERWITHAMONITORINGSTANDARDOFKNOWNCOMPOSITIONEVERY10SAMPLESFORTHEANALYSESPERFORMEDBYICPOES,ACALIBRATIONSTANDARDWASANALYSEDATREGULARINTERVALSWITHINEACHRUNTOMONITORINSTRUMENTSTABILITYONTHEBASISOFTHISCALIBRATIONSTANDARDANANALYTICALPRECISIONOFBETTERTHAN2ISESTIMATEDFORALLANALYTESINHOUSEDETECTIONSLEVELSWEREESTABLISHEDAS1MG/LFORCD,5MG/LFORPBAND10MG/LFORZN,CU,FE,AL,CA,MG,NAANDPANALYSESFORORGANICCARBONWEREPERFORMEDONASHIMADZUTOC5000ANALYSER,WITHAPRECISIONOF2ANDDETECTIONLEVELOF200MG/LANIONSNITRATE,AMMONIUM,CHLORIDEANDSULPHATEWEREANALYSEDBYIONCHROMATOGRAPHYUSINGADIONEXDX300COLUMNAS4A;PRECISIONISESTIMATEDAT5ANDDETECTIONLEVELSAT100MG/LFORTHESEANALYSES24MATERIALSCHARACTERISATIONLABORATORYANALYSISINDICATEDASOILPHRANGINGFROM76TO80BASEDONA11RATIOOFSOILANDDEIONISEDWATERANDRELATIVELYHIGHMETALCONCENTRATIONSTABLE2XRAYPOWDERDIFFRACTIONDATAWEREC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