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JAERI-Data/Code 99-001 JAERI-Data/Code 99-001 Consideration on Thermodynamic Data for Predicting Solubility and Chemical Species of Elements in Groundwater Part 1: Tc, U, Am Tetsuji YAMAGUCHI and Seiji TAKEDA Department of Environmental Safety Research Nuclear safety Research Center Tokai Research Establishment Japan Atomic Energy Research Institute Tokai-mura, Naka-gun, Ibaraki-ken (Received January 5, 1999) The solubility determines the release of radionuclides from waste form and is used as a source term in radionuclide migration analysis in performance assessment of radioactive waste repository. Complexations of radionuclides by ligands in groundwater affect the interaction between radionuclides and geologic media, thus affect their migration behavior. Thermodynamic data for Tc, Am and U were reviewed and compiled to be used for predicting the solubility and chemical species in groundwater. Thermodynamic data were reviewed with emphasis on the hydrolysis and carbonate complexation that can dominate the speciation in typical groundwater. Thermodynamic data for other species were selected based on existing databases. Thermodynamic data for other important elements are under investigation, thus shown in an appendix for temporary use. Keywords: Technetium, Uranium, Americium, Thermodynamic Data, Solubility, Aqueous Species, Solid Species, Equilibrium Constant JAERI-Data/Code 99-001 Table A-l. Carbon thermodynamic data. Equilibrium constants at 298.15 K and I = 0 are taken from HATCHES DATABASE, NEA RELEASE 9, 13th March 1996 (available with a floppy disk from Bond, K. A. and Tweed, C. J., Direct line 01235 433867, Direct facsimile 01235 436579) . 0 species reaction logK 2 COs " + 2H* + H20 = CH,° + 2O2 (g) -128.04 H2CO30 CO32" + 2H* = H2CO30 16.68 HCO3" CO32" + H* = HCO3" 10.33 CO32" master species NaHCO3° Na* + CO32" + H* = NaHC03° 10.08 NaCC>3~ Na* + CO32" = NaCOs" 1.27 2 2 MgHCO-T Mg * + CO3 ' + H* = MgHCO3* 11.4 Mg'" + CO32" = . 2.98 MnHCOs* Mn2* CO3 + H* = MnHCOs* 11.6 0 2 2 0 CUCO3 Cu * CO3 = CuCOs 6.73 2 : 2 Cu * 2 CO " = Cu(CO3)2 " 9.83 3 2 CeCO3* Ce * CO3 = CeCOs* 7.94 3 Ce(CO3)2" Ce * + 2CO3~" = Ce(CO3)2" 13.3 3 3 2 3 Ce(CO3)3 ce ; + 3COs " = Ce(CO3>3 " 14.2 S 2 5 Ce(CO3>4 + 4CO3 " = Ce(CO3)4 " 13.7 NdCOs* Nd3* + CO32" = NdCO3* 7.5 2 + 2CO3 " = Nd(CO3)2" 12.53 CH4(g) CO3 + 2H* + H2O = CH4(g) CMg) -125.16 2 2 MgCCb (s) Mg * + CO3 " = MgCO3(s) 7.9 Nesquehonite Mg2* + HCO3" + 3H2O =MgCO3'3H2O(s) + H* -5.14 2 Lansfordite Mg * + HCOs" + 5H2O = MgCOs- 5H20 (s) + H* -4.93 2 Artinite 2Mg * + HCOs" + 5H2O = Mg2CO3(OH)2-3H2O(s) + 3H* -19.95 2 Hydromagnesite 5Mg * + 4HCO3" + 6H2O =Mg5(CO3),(OH)2'4H2O(s) 4 6H* -31.57 2 2 Witherite Ba * + CO3 " = BaCO3 (s) 8.58 Nahcolite Na* + HCOJ" = NaHCOs (s) 0.1 Na2CO3(s) 2Na* + HCOs" = Na2CO3 (s) + H* -11.00 Thermonatrite 2Na* + HCO3" + H2O = Na2CO3 • H2O (s) + H* -10.99 Natron 2Na* + HCO3" + IOH2O = Na2CO3- 10H2O(s) + H* -9.57 Kalicinite K* + HCO3" = KHCO3(s) -0.33 K2CO3-1.5H2O(s) 2K* + HCO3" + 1.5HaO = K2CO3-1.5H2O(s) + H* -13.47 8K* + 6HCO3" + 3H2O = K»H4 (CO3)6-3H2O(s) + 2H* -28.09 KNaCO3'6H2O (s) K* + Na* + HCO3" + 6H2O = KNaCOs- 6H2O(s) + H* -10.32 2 Ag2CO3(s) 2Ag* CO3 " = Ag2COs(s) 11.09 Rhodochrosite Mn2* + CO32" = MnCOs(s) 10.41 2 2 Siderite Fe * + CO3 ' = FeCO3(s) 10.90 2 Smithsonite Zn * + HCOs" = ZnCO3(s) + H* -0.45 2 Azurite 3Cu * + 2HCO3" + 2H2O = Cu3(CO3)2(OH)2(s) + 4H -9.21 Malachite 2Cu2* + HCO3" + 2H2O = CU2CO3 (OH) 2 (s) + 3H* -5.97 La2(CCb)3(s) 2La" = La2(CO3)3(s) 33.4 3 2 Ce2(CO3)3(s) 2Ce * + 3CO3 ' = Ce2(CO3)3(s) 35.11 3 2 NdOHCO3(s) Nd * + CO3 " + H2OO = NdOHCONdOHCO3 3(s(s) + H* 7.89 Burkeite 6Na* + HCOa" + 2SO42" = NaeCOs (SO.) 2 (s) + H* -9.65 Dawsonite Na* + Al3* + HCO3" + 2H2O = NaAlCOs (OH) 2 (s) + 3H* -4.68 see calcium thermodynamic data CaCO3° see calcium thermodynamic data C0HCO3* see cobalt thermodynamic data C0CO30 see cobalt thermodynamic data NiHCO3* see nickel thermodynamic data NiCOs0 see nickel thermodynamic data 2 Ni (CO3)2 " see nickel thermodynamic data SrCOs0 see strontium thermodynamic data 3 Tc(OH)2(CO3)2 see technetium thermodynamic data Tc(OH)2CO3° see technetium thermodynamic data see technetium thermodynamic data TcOH(CO3)2" see technetium thermodynamic data Cs2CO3° see cesium thermodynamic data SmCOs* see samarium thermodynamic data Sm (CO3) 2" see samarium thermodynamic data EUCOJ* see europium thermodynamic data Eu(CO3)2" see europium thermodynamic data PbCO,0 see lead thermodynamic data -27- JAERI-Data/Code 99-001 Pb(CO3)2 see lead thermodynamic data RaHCCb* see radium thermodynamic data RaC03° see radium thermodynamic data ThCCb2* see thorium thermodynamic data see uranium thermodynamic data 6 U(CO3)5 see uranium thermodynamic data USCN3* see uranium thermodynamic data U(SCN)2 see uranium thermodynamic data see uranium thermodynamic data see uranium thermodynamic data UO (CO ) see uranium thermodynamic data 2 3 see uranium thermodynamic data see uranium thermodynamic data see uranium thermodynamic data (UO2)3(OH)3CO3* (UO2) (OH)3CO3" see uranium thermodynamic data 2 see uranium thermodynamic data see uranium thermodynamic data UO2SCN* see uranium thermodynamic data UO2(SCN) see uranium thermodynamic data UO2(SCN) see uranium thermodynamic data see uranium thermodynamic data see neptunium thermodynamic data see neptunium thermodynamic data see neptunium thermodynamic data see neptunium thermodynamic data Np(CO3) see neptunium thermodynamic data see neptunium thermodynamic data see neptunium thermodynamic data see neptunium thermodynamic data NpOiCOs" 2 see neptunium thermodynamic data NpO2(CO3)2 " see neptunium thermodynamic data NpO2 (003)3*" 6 see neptunium thermodynamic data (NpO2)3(CO3)6 " 2 see neptunium thermodynamic data NpO2(OH)2CO3 " see plutonium thermodynamic data see plutonium thermodynamic data Pu see plutonium thermodynamic data 3 Pu(CO3)3 see plutonium thermodynamic data PUCO32* see plutonium thermodynamic data Pu(CO3)2° see plutonium thermodynamic data see plutonium thermodynamic data see plutonium thermodynamic data 6 Pu(CO3)5 " see plutonium thermodynamic data Pu(OH)2(CO3) see plutonium thermodynamic data see plutonium thermodynamic data PuOaCOj see plutonium thermodynamic data PUO2CO3 see plutonium thermodynamic data see plutonium thermodynamic data see americium thermodynamic data see americium thermodynamic data Am (CO3) see americium thermodynamic data see americium thermodynamic data Am0HC03° see americium thermodynamic data AmOH(CO3)2 see americium thermodynamic data Am(OH)2CO3 see americium thermodynamic data AmSCN2* see americium thermodynamic data see curium thermodynamic data CmC03* see calcium thermodynamic data Alstonite see calcium thermodynamic data Aragonite see calcium thermodynamic data Barytocalcite see calcium thermodynamic data Calcite see calcium thermodynamic data Monohydrocalcite see calcium thermodynamic data Vaterite see calcium thermodynamic data Dolomite-dis see calcium thermodynamic data Dolomite see calcium thermodynamic data Dolomite-ord see calcium thermodynamic data Gaylussite see calcium thermodynamic data Huntite see calcium thermodynamic data Pirssonite -28- JAERI-Data/Code 99-001 CoCCMs) see cobalt thermodynamic data NiCOj(s) see nickel thermodynamic data SrCCMs) see strontium thermodynamic data Strontianite see strontium thermodynamic data NbC(cr) see niobium thermodynamic data Nb2C(cr) see niobium thermodynamic data CSHCOJ(S) see cesium thermodynamic data Cs CCMs) see cesium thermodynamic data 2 see samarium thermodynamic data SmOHCCMs) see samarium thermodynamic data Eu (CO )3(s) see europium thermodynamic data 2 3 see europium thermodynamic data Eu2(CO3)3-3H2O(s) PbCO (s) see lead thermodynamic data 3 see radium thermodynamic data RaCCMs) see uranium thermodynamic data U02CCMs) see uranium thermodynamic data see uranium thermodynamic data UC(cr) see uranium thermodynamic data a -UCI.M (cr) see uranium thermodynamic data see neptunium thermodynamic data NaNpO2CO3-3.5H2O(s) see neptunium thermodynamic data NpO2CO3(s) see plutonium thermodynamic data PUOHCO3 (s) see plutonium thermodynamic data Pu(OH)2CO3(s) see plutonium thermodynamic data PuOzCCMs) see americium thermodynamic data Am2(CO3)3(s) see americium thermodynamic data AmOHCCb (s) see americium thermodynamic data Am2C3 (cr) see curium thermodynamic data CmOHCO3(s) -29- JAERI-Data/Code 99-001 Table A-2. Calcium thermodynamic data. Equilibrium constants at 298.15 K and I = 0 are taken from HATCHES DATABASE, NEA RELEASE 9, 13th March 1996 (available with a floppy disk from Bond, K. A. and Tweed, C. J., Direct line 01235 433867, Direct facsimile 01235 436579) . species reaction log K° Ca(II) Ca2* master species CaOH* Ca2* + H2O = CaOH* + H* -12.6 CaHCCb Ca2* + H* + CO32" = CaHCCb* 11.35 2 2 0 CaCO3° Ca * + CO3 " = CaCCb 3.15 2 2 CaSO4° Ca * + SO4 " = CaSO4° 2.31 2 CaNCh* Ca * + NO3" = CaNO3* 0.6 2 Ca(N Ca * + 2NO3" = Ca(NO3)2° 0.5 2 Ca * + F" = CaF* 0.94 CaF* 2 3 Ca * + 2H* + PO4 " = CaH2PO4* 20.96 2 3 Ca * + 2PO4 " + 4H* = Ca (H2PO4> 2° 39.45 Ca2* + H* + PO43" = CaHPCu" CaHPO« 2 2 15.09 3Ca * + 2PO4 " = Ca3(PO<)2° 0.35 Ca2* + PO43" = CaP(V 2 0 6.46 Ca * + B (OH) 3 = CaH2BO3* + H* -7.44 CaHA* Ca2* + HA" = CaHA* 4.7 Ca(EN)2* Ca2* + EN° = Ca(EN) 0.4 Ca(ETHA)2* Ca2* + ETHA0 = Ca (ETHA)" 3.67 Ca(ACET)* Ca2* + ACET° = Ca(ACET)' +. Hw -3.58 Ca(ACET)2° Ca2* + 2ACET0 = Ca (ACET) 20° + 2H* -5.52 2 0 Ca(ACET)3" Ca * + 3ACET = Ca (ACET) 3" + 3H* -9.83 Ca(ACET)42" Ca2* + 4ACET0 = Ca (ACET) ,2~ + 4H* -15.44 Ca(GLYCE)* Ca2* + GLYCE0 = Ca (GLYCE) * + H* -13.1 Ca(BENZ)* Ca2* + BENZ" = Ca (BENZ) * 0.74 Ca(DBP)* Ca2* + DBP" = Ca(DBP)* -0.2 Ca(EDMA)* Ca2* + EDMA"
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