纳米孔对铀ⅵ在水—矿物界面吸附和解吸影响-effect of nanopores on adsorption and desorption of uranium ⅵ at water-mineral interface.docx

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2018-07-27 发布于上海
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纳米孔对铀ⅵ在水—矿物界面吸附和解吸影响-effect of nanopores on adsorption and desorption of uranium ⅵ at water-mineral interface.docx

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纳米孔对铀ⅵ在水—矿物界面吸附和解吸影响-effect of nanopores on adsorption and desorption of uranium ⅵ at water-mineral interface

sorptionbehaviorsaredependentofpH,carbonateconcentrationandionicstrength.Themaximalsorptionofnanoporousandnon-nanoporousmaterialsoccurredatcircumneutralpH,thesorptioncapacityofnon-nanoporousmaterialsdecreasewithcarbonateandionicstrength,butnanoporousmaterialsareinsentivetoionicstrengtheffect,whichestablishthatthepredominatesorptionmechanismfornanoporousmaterialsareinner-spheresorptionwhileouter-spheresorptionfornon-nanoporousmaterials.TheU(Ⅵ)sorptionbehaviorofhydrotalcitearesimilartonanoporousaluminabecausethedistanceofinterlayerofhydrotalciteisonly0.78nm,whichisregardtotheverysmallnanopore.Sequentialdesorptionandfixeddesorptionaredependentofdesorptiontimeandextractant(NaHCO3)concentration.Fixeddesorptionresultsindicatethatonly5%ofU(Ⅵ)wasdesorbedfromnanoporousaluminaatlowNaHCO3(0.01M)solution,and60%U(Ⅵ)wasdesorbedevenat3highconcentration(0.1MNaHCO3),interestedenough,theamountofdesorbedU(Ⅵ)decreasewiththehigherNaHCO3(from0.5Mto1.0M),becausedesorbedU(Ⅵ)complexedwithCO2-anionandformUO2(CO3)34-enterintointerlayerathigherconcentration.Thesequentialdesorptionresultsalsodeterminethatthereareverystrongchemicalaffinityofnanoporousmaterials.Accordingtosurfacecomplexationmodeling(SCM),wesimulatedtheisothermalsorptionandsorptionbehaviorsatdifferentpHbyusingPHREEQCsoftware,themodelresultsareconsistentwithexperimentaldataatlowconcentration.ThemechanismofU(Ⅵ)sorptionontonaturalsediment(suchasFRC-FieldResearchCenter,OakRidge,TN)isstillambiguousnowadays.Therefore,thesurfacepropertiesofFRCsedimentwerecharacterizedbyXRDpatterns,SSAanalysis,TEMimagesandacid-basetitration.AccordingtoXRDpattern,therearemassiveamountofquartzandclayminerals,theoccurrenceoflowintensitypeaksofgoethiteinclayeymineralsindicatethattherearenanoporousgoethitecoexistwithcalyminerals.Theremarkablechangeofsurfaceaciditycoeffient(△pK=pK1-pK2)estimatethattherearemassivebulkparticles(suchasquartz)inthesediments.Theoccurrenceandamount(1%)ofnanoporousgoethiteinclayeysampleswereclarifiedintermsofTEMimagesandBCDanalysisres