Evaporative evolution of a Na–Cl–NO3–K–Ca–SO4–Mg–Si brine at 95°C Experiments and modeling relevant to Yucca Mountain, Nevada.docVIP

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Evaporative evolution of a Na–Cl–NO3–K–Ca–SO4–Mg–Si brine at 95°C Experiments and modeling relevant to Yucca Mountain, Nevada.doc

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Evaporative evolution of a Na–Cl–NO3–K–Ca–SO4–Mg–Si brine at 95°C Experiments and modeling relevant to Yucca Mountain, Nevada

GEOCHEMICALTRANSACTIONS VOLUME6,NUMBER2 JUNE2005 EvaporativeevolutionofaNa–Cl–NO –K–Ca–SO –Mg–Sibrineat95°C: 3 4 ExperimentsandmodelingrelevanttoYuccaMountain,Nevada MaureenAlai,a?MarkSutton,andSusanCarroll LawrenceLivermoreNationalLaboratory,Livermore,California94550 ?Received5November2004;accepted21April2005;published7June2005? AsyntheticTopopahSpringTuffwaterrepresentativeofonetypeofporewateratYuccaMountain, NVwasevaporatedat95°Cinaseriesofexperimentstodeterminethegeochemicalcontrolsfor brinesthatmayformon,andpossiblyimpactuponthelong-termintegrityofwastecontainersand drip shields at the designated high-level, nuclear-waste repository. Solution chemistry, condensed vaporchemistry,andprecipitatemineralogywereusedtoidentifyimportantchemicaldividesand tovalidategeochemicalcalculationsofevaporatingwaterchemistryusingahightemperaturePitzer thermodynamicdatabase.Thewaterevolvedtowardacomplex“sulfatetype”brinethatcontained about45mol%Na,40mol%Cl,9mol%NO ,5mol%K,andlessthan1mol%eachofSO , 3 4 Ca,Mg,?CO2?aq?,F,andSi.Allmeasuredionsinthecondensedvaporphasewerebelowdetection limits. The mineral precipitates identi?ed were halite, anhydrite, bassanite, niter, and nitratine. Trends in the solution composition and identi?cation of CaSO4 solids suggest that ?uorite, carbonate,sulfate,andmagnesium-silicateprecipitationcontroltheaqueoussolutioncompositionof sulfate type waters by removing ?uoride, calcium, and magnesium during the early stages of evaporation.Inmostcases,thehightemperaturePitzerdatabase,usedby EQ3/6geochemicalcode, suf?ciently predicts water composition and mineral precipitation during evaporation. Predicted solution compositions are generally within a factor of 2 of the experimental values. The model predicts that sepiolite, bassanite, amorphous silica, calcite, halite, and brucite are the solubility controllingmineralphases. ?2005AmericanInstituteofPhysics.?DOI:10.1063/1.1935432? I.INTRODUCTION ally describes the chemical evolution of dil