JAEA-Research 2006-038緩衝材間隙水中溶解度計算への適用における放射性元素の熱力学データベースの比較調査Comparison of the Thermodynamic Databases for Radioactive Elements in Application to the Calculation of the Solubilities in the Porewater土井玲祐柴田雅博Reisuke DOI and Masahiro SHIBATA地層処分研究開発部門核種移行研究グループRadionuclide Migration Research Group Geological Isolation Research and Development Directorate July 2006 Japan Atomic Energy Agency日本原子力研究開発機構本レポートは日本原子力研究開発機構が不定期に発行する成果報告書です。本レポートの入手並びに著作権利用に関するお問い合わせは、下記あてにお問い合わせ下さい。なお、本レポートの全文は日本原子力研究開発機構ホームページ（http://www. jaea. go. jp/index. shtml)より発信されています。このほか財団法人原子力弘済会資料センター＊では実費による複写頒布を行っております。 〒319–1195　茨城県那珂郡東海村白方白根2番地4日本原子力研究開発機構　研究技術情報部　研究技術情報課電話029-282-6387, Fax 029-282-5920 * 〒319-1195　茨城県那珂郡東海村白方白根2番地4　日本原子力研究開発機構内This report is issued irregularly by Japan Atomic Energy Agency Inquiries about availability and/or copyright of this report should be addressed to Intellectual Resources Section, Intellectual Resources Department, Japan Atomic Energy Agency 2-4 Shirakata Shirane, Tokai-mura, Naka-gun, Ibaraki-ken 319-1195 Japan Tel +81-29-282-6387,  Fax +81-29-282-5901 ○ Japan Atomic Energy Agency, 2006. JAEA　Reseach 2006　038 5  23 2006 2 JNC   OECD/NEA   Nagra/PSI 319-1194 Comparison of the Thermodynamic Databases for Radioactive Elements in Application to the Calculation of the Solubilities in the Porewater Reisuke DOI and Masahiro SHIBATA Geological Isolation Base Research and Development Unit Geological Isolation Research and Development Directorate Japan Atomic Energy Agency Tokai-mura, Naka-gun, Ibaraki-ken Received May 23, 2006 To calculate the solubility of radioactive elements which is the important parameter for performance assessment of geologinal disposal system, the thermodynamic database must be reliable and based on the latest information. In this research, it has been compared in the caluculation of the solubilities of the representative radioactive elements in the porewater compositions of the compacted bentonite which were set up in the second progress report (H12) that the thermodynamic database of JNC, OECD/NEA, Nagra/PSI. And the causes of the differences among the results from application of different databases were investigated and discussed. Keywords: Solubility, Thermodynamic Database
Contents
1. K
1) 2 OECD/NEA TDB 21 1998 U,Am Tc JNC JNC-TDB Yui et al.1999    ²) Np(   ) Sm,Cm,
Am OECD/NEA 1980 Phase
8 U, Am, Tc, Np, Pu, Se, Ni, Zr OECD/NEA （ ） （ ） Nagra PSI (Hummel et al.2002 31 ) OECD/NEA TDB OECD/NEA 2001 OECD/NEA 2 NEA PSI 2 JAEA-TDB 99 2.1 2. JNC-TDB (http://migrationdb.jnc.go.jp) 011213c2 2 2 991231c2 21 Pu,Am 011213c2 991231c2 011213c2 JNC-TDB NEA NEA-TDB (Guillaumout  2003 4) up-date 3) PSI Nagra/PSI 01/01 PSI-TDB 2005' NEA-TDB 03000c0 PSI-TDB PSI Waste management laboratory web (http://les.web.psi.ch/TDBbook) auxiliary data NAPSI 290502(260802) 2.2 2.1 PHREEQC 6 ) 2.3 2 NEA PSI Se, U, Np, Pu, Th, Am Th NEA-TDB  (03000c0) Se PSI-TDB NEA Se JNC-TDB Th Olin et al.20057 03000c0 NEA-TDB PSI-TDB Se Se FeSe2 2 Se(cr) 81 FRHP pH SRHP pH 2.4 3 8 2.1
2.5 JNC NEA PSI 2.3 3. 2 6 3 JNC-TDB PHREEQC 1% 2 3) 2
2.1 2 PHREEQE 0.3mol/kg 0.3 mol/kg Davies 3.1 (Se) SRHP
FeSe 2 (cr) 2 al.2005 6 Olin et FRHP 3.1.1 Se 3.1.2 PSI-TDB JNC-TDB PSI-TDB 1.877× 10 7 mol/l HSe  = Se (cr)+ H + +2e K 3.1.1 Se(cr) FeSe 2 (cr) 2 3.1.2 3.1.1 JNC-TDB 1.869×  10 7 mol/L, NEA-TDB (3-1-1) logK = 7.720(JNC-TDB), 7.770(NEA-TDB(Olin et al.2005 6)),7.700(PSI-TDB) JNC-TDB (3-1-1) JNC-TDB (3-1-2) (3-1-3) Se = SeO 4 2 -4H 2 O +6e +8H + (3-1-2) logK = -88.920(JNC-TDB) SeO 4 2 -4H 2 O +8e +9H + = HSe + (3-1-3) logK = 81.200(JNC-TDB),81.548(NEA-TDB(Olin et al.2005 6 )) PSI-TDB (3-1-4) (3-1-5)        (3-1-6) (3-1-1) (3-1-4) Se(cr) = SeO 3 2 -3H 2 O +4e +6H + logK =-61.286(NEA-TDB(Olin et al.2005 6 )) ,-61.2900(PSI-TDB) SeO 3 2 * -3H 2 O +6e +8H + = H 2 Se (3-1-5) logK = 57.3900(PSI-TDB) H 2 Se -H + = HSe + (3-1-6) logK = -3.8000(PSI-TDB) NEA-TDB(Olin et al.2005 )      (3-1-3)      (3-1-4)     (3-1-7) 3-1-1 SeO 4 2 -H 2 O +2e +2H + = SeO 3 2 - logK = 27.578(JNC-TDB),28.032(NEA-TDB(Olin et al.2005 6 ))
3-1-1
3.1.2 Se SRHP 10°mol/l
3.1.3 2
Se(cr) FRHP 3-1-1 K FRHP
3.1.3 Se SRHP (3-1-1) (3-1-1) (3-1-1) Cross et al.1987 91 PSI-TDB JNC-TDB K (3-1-6) Perrin 1982 101 (3-1-6) PSI Séby et al.,20011) Se Perrin 1982 101 Se NEA et al.2005 6 al.,1923 13) (3-1-6) Hlasko et Bruner et al.,1913 12 K Olin Olin et al.2005 6 Olin et al.2005 9 Hagisawa,1941 14) Perrin 1982 100 Perrin 1982 10) JAEA-TDB 3.2 (Th) Th Rai et al.,1995 15) NEA-TDB Th PHREEQC ThO 2 (am) JNC-TDB PSI-TDB 3.2.1 Th FRHP FRHP 3.2.1 PSI-TDB ThO 2 (s,am) = Th 4+ +2H 2 O -4H + (3-2-1) logK = 10.500(JNC-TDB), 9.9000(PSI-TDB) PSI-TDB JNC-TDB Th 4+ + CO 3 2  +3H 2 O -3H + = Th(OH) 3 CO 3 logK = -3.720(JNC-TDB), -3.1000(PSI-TDB) CO 3 2  + H + = HCO 3 logK = 10.327(JNC-TDB), 10.329(PSI-TDB) Th(OH) 3 CO 3         ThO 2 +H 2 O + HCO 3 logK = 3.547(JNC-TDB), 3.5290(PSI-TDB) (3-2-4)        (3-2-1)   ,  (3-2-2) (3-2-3) K PSI-TDB (3-2-4)
3.2.2 Th  SRHP JNC-TDB  PSI-TDB K        JNC-TDB (3-2-4) (3-2-4) JNC-TDB   2.264× 10 4 (mo/l), PSI-TDB     1.574× 10 2 (mo/l) PSI-TDB HCO 3 CH 4 JNC:PHREEQE Original 16), CO 3 2 + 10H + 8e -3H 2 O = CH 4 (3-2-5) logK = 41.071(JNC-TDB), 37.1782(PSI-TDB) C logK pH, Eh C PSI:NIST(= PSI-TDB Th(CO 3 ) 5 6 3% JNC-TDB        3.9× 10 -21 (mol/l) (3-2-6) (3-2-6) Th 4+ + 5CO 32 * = Th(CO 3 ) 56 * logK = 27.100(JNC-TDB), 29.800(PSI-TDB) CO 3 ² K (3-2-5) K 1.5× 10 7 (mol/l)
3.2.3 Th Th(OH) 3 CO 3 . (3-2-4) K JNC-TDB   PSI-TDB SRHP HCO 3 Th(CO 3 ) 56 JNC-TDB PSI-TDB 3.3 (Np) Rai and Ryan(1985) 18) NpO 2 (am) ( NpO 2 (am) NpO² xH²O) NpO₂(am) 3.3.1 Np  FRHP JNC-TDB JNC-TDB JNC-TDB Np(OH)²(CO 3 )²² (3-3-1), logK = 4.408 Np(OH) 2 (CO 3 ) 2 ²  = NpO 2 + 2HCO 3  NEA-TDB Np(OH) 2 (CO 3 ) 2 2 Np(CO 3 ) 4 JNC-TDB (3-3-2), Np(CO 3 ) 4 * logK=5.318(NEA-TDB) , 3.126(PSI-TDB) NEA-TDB Np(CO 3 ) 4 Np(CO 3 ) 4 0.16 3.3.1 K (3-3-2) (3-3-3) (3-3-3) NpO₂(am) = Np₄+ + 2H₂O -4H+ logK=1.510(JNC-TDB), -0.695(NEA-TDB), 1.5000(PSI-TDB) K  NEA-TDB (3-3-2) Np(OH)4 JNC-TDB     3.2× 10 9 (mol/l )  NEA-TDB       9.9× 10 -10 (mol/l )  PSI-TDB NEA-TDB 5.0×  10°(mol/l ) Np(OH) 4 = NpO 2 (am) + 2H 2 O logK = 8.49(JNC-TDB), 9.000(NEA-TDB), 8.3000(PSI-TDB) (3-3-4)
K (3-3-4) NEA-TDB Np 4+ + 4H 2 O -4H + = Np(OH) 4 logK = -10.00(JNC-TDB), -8.305(NEA-TDB), -9.800(PSI-TDB)
3.3.2 SRHP FRHP Np(OH)4 2.7× 10 ° (mol/l) JNC-TDB NEA-TDB 3.3.1 (3-3-5)         K NEA-TDB Np(OH)4 8.3× 10 -10 (mol/l)  PSI-TDB      4.2× 10 -9 (mol/l) (3-3-3) (3-3-4) Np(CO 3 )4 K 3.3.1 3-3-3
3.3.3  Np (3-3-3) JNC-TDB (3-3-5) PSI-TDB         Lemire et al.,2001 21) PSI-TDB         Lemire Rai and Ryan,1985 18) et al.,2001 21) Lemire et al.,2001 21 ) PSI     up-data NEA NEA      Guillaumont,2003 4 ) Np Neck JAEA-TDB Neck and and Kim,2001 20 ) Kim,2001 201 3.4 (Pu) 2 Pu 991231c2 PuO 2 (am) PuO 2 (am) 3.4.1  Pu  FRHP JNC-TDB NEA-TDB PSI-TDB JNC-TDB Pu(   ) Pu(   ) Pu(OH)²(CO³)²²²²  NEA-TDB PSI-TDB PSI-TDB NEA-TDB Pu(   )    Pu(CO 3 ) 4 *,  Pu(CO 3 ) 5 * [Pu(CO 3 ) 4 7.94 ×   10 -14 (mol/l)(NEA-TDB),   1.28 × Pu(CO 3 ) 5 10  ¹ 4 (mol/l)(PSI-TDB) 1.05 ×  10 -17 (mol/l)(NEA-TDB),  1.02 × 10־18 (mol/l)(PSI-TDB)] PSI-TDB NEA-TDB Pu(OH)4 Pu(OH) 4 = PuO 2 (am)+ 2H 2 O logK = 10.000(JNC-TDB), 10.825(NEA-TDB), 10.400(PSI-TDB) Pu(OH)4 9.93× 10 -11 (mo/l)(JNC-TDB),1.49× 10 -11 (mo/l)(NEA-TDB), 3.95× (3-4-1) 10  ¹¹ (mo/l)(PSI-TDB) (3-4-1) K K (3-4-2)         (3-4-3) K PuO 2 (am) = Pu 4+ + 2H 2 O -4H + (3-4-2) logK = -0.850(JNC-TDB), -2.325(NEA-TDB), -2.0000(PSI-TDB) Pu 4+ + 4H 2 O -4H + = Pu(OH) 4 (3-4-3) logK = -9.150(JNC-TDB), -8.500(NEA-TDB), -8.400(PSI-TDB)
3.4.2 Pu  SRHP PuOH²† (3-4-4) PuOH²+ + 2H²O = PuO² + 3H + e logK = -9.650(JNC-TDB), -8.469(NEA-TDB), -7.7900(PSI-TDB) K        JNC-TDB, NEA-TDB, PSI-TDB NEA-TDB PuOH²† (3-4-4) PuO₂(am) = Pu 4+ + 2H₂O -4H† logK = -0.850(JNC-TDB), -2.325(NEA-TDB), -2.0000(PSI-TDB) Pu 3+ + H 2 O -H + = PuOH 2+ logK = -6.400(JNC-TDB), -6.900{NEA-TDB    (3-4-6)-(3-4-7)       }, -6.9000 (PSI-TDB) Pu 4+ + H 2 O -H + +e = PuOH 2+ Pu 4+ + e = Pu 3+ logK = 16.900(JNC-TDB), 17.694(NEA-TDB), 16.6900(PSI-TDB) NEA-TDB (3-4-4) (3-4-2)       (3-4-5) K JNC-TDB Pu(OH)² † NEA-TDB NEA-TDB PSI-TDB Pu³+ 1 Pu³+ (3-4-9) Pu³+ + 2H₂O = PuO₂ + 4H† +e logK = -16.050(JNC-TDB), -15.369(NEA-TDB), -14.6900(PSI-TDB) K PSI-TDB JNC-TDB NEA-TDB PSI-TDB NEA-TDB Pu³÷ (3-4-8) JNC-TDB (3-4-4) K (3-4-7)
3.4.3 Pu PSI-TDB NEA-TDB Pu(   ) (3-4-3) JNC-TDB           Yamaguchi et al.,1994 22) Lierse & Kim,1986 ²³³ (I=1M, HClO 4 /NaClO 4 ) PSI-TDB Neck and Kim,2001 209 0.1M, KOH) Neck and Kim,2001 20 ) pH 7 NEA-TDB PuO₂(hyd,aged) Pu(   ) Pu(   ) Knopp et al.,199925) , Neck & Kim,199926) , Neck and Kim,2001 201 NEA K NEA JAEA-TDB Neck and Kim,2001 201    NEA Knopp et al.,199925) , Neck & Kim,199926) , PSI Neck and Kim,2001 20 ) JNC-TDB Pu(   ) Am(   ) NEA-TDB PSI-TDB Hummel et al.2002 31 Am(   ) Am JNC-TDB Pu(   ) NEA PSI-TDB 3.5 (Am) 2 991231c2 AmOHCO 3 (cr) NEA-TDB AmOHCO3 AmOHCO 3 (cr) 0.5H 2 O(cr) AmOHCO 3 (am,hyd) AmOHCO 3 (am,hyd) (3-5-1)   (3-5-3) K AmOHCO3(cr) 2 1) NEA-TDB AmOHCO 3 0.5H 2 O(cr) 3.5.1 FRHP Am Am(CO 3 )²², Am(CO 3 )² AmSiO(OH) ²+
JNC-TDB AmSiO(OH) 32+ (3-5-1) AmCO 3 + H 2 O = AmOHCO 3 + H + logK=0.900(JNC-TDB), 0.399(NEA-TDB AmOHCO 3 0.5H 2 O(cr) ), -1.801(NEA-TDB AmOHCO 3 (am,hyd) ), -0.600(PSI-TDB) (3-5-2) Am(CO 3 )²  + H 2 O = AmOHCO 3 + HCO 3   T logK=6.527(JNC-TDB 011213c2), 5.826(NEA-TDB AmOHCO 3   0.5H 2 O(cr) ), 3.626(NEA-TDB AmOHCO 3 (am,hyd) ), 5.229(PSI-TDB) Am(CO 3 ) 3 · + H 2 O + H + = AmOHCO 3 + 2HCO 3 · (3-5-3) logK=13.954(JNC-TDB), 14.053(NEA-TDB AmOHCO 3 0.5H 2 O(cr) ), 11.853(NEA-TDB AmOHCO 3 (am,hyd) ） 12.658(PSI-TDB) JNC-TDB K (3-5-2) Am(CO 3 )² K JNC-TDB AmOHCO 3 (3-5-4) logK=-8.500(JNC-TDB), -8.399(NEA-TDB AmOHCO 3    0.5H 2 O(cr)                  ), -6.199(NEA-TDB AmOHCO 3 (am,hyd) -7.200(PSI-TDB) Am(CO 3 ) 2 logK=-12.300(JNC-TDB),-12.300(NEA-TDB), -12.300(PSI-TDB) (3-5-2) (3-5-4) JNC-TDB K 3-5-1 K 3-5-6 AmCO 3 logK=-7.600(JNC-TDB), -8.000(NEA-TDB), -7.800(PSI-TDB) K K 3-5-3 (3-5-7) AmCO 3 logK=-15.200(JNC-TDB), -15.000(NEA-TDB), -15.200(PSI-TDB)
3.5.2  Am  SRHP NEA-TDB(AmOHCO 3 [Am(CO 3 )² JNC-TDB 10 8 (mol/l)(NEA-TDB AmOHCO 3  0.5H 2 O(cr) Am(CO 3 ) 2 HCO 3 HCO3 10 -4 (mol/l)(JNC-TDB)  2.134× 10 -2 (mol/l)(NEA-TDB)  1.622× 10 -2 (mol/l)(PSI-TDB) AmCO 3 + (3-5-1) PSI-TDB AmOH²+  Am(OH)²+ 1% 8.31× 10°(mol/l)(JNC-TDB), AmOH²+ AmOH²+ 1.759× 10 -11 (mol/l)(NEA-TDB), 5.956× 10 -10 (mol/l)(PSI-TDB) PSI-TDB (3-5-8) AmOH²† + HCO 3  = AmOHCO 3 + H† logK = 4.573(JNC-TDB), 5.272(NEA-TDB), 4.171(PSI-TDB) (3-5-8) (3-5-9) Am³+ + H 2 O −H + = AmOH²+ logK = -6.400(JNC-TDB), -7.200(NEA-TDB), -7.3000(PSI-TDB) Am(OH)² + Am(OH) 2 †        HCO 3 † = AmOHCO 3 + H 2 O logK = 12.273(JNC-TDB), 13.172(NEA-TDB), 12.071(PSI-TDB) (3-5-10) K Am³+ + 2H₂O −2H† = Am(OH)₂ † logK = -14.100(JNC-TDB), -15.100(NEA-TDB), -15.200(PSI-TDB)
3.5.3     Am Am 3-5-4 K JNC-TDB PSI-TDB NEA  Am Silva et al.(1995) 281 Silva et al.1984 291     Meril,L. & Fuger,L.,1996 301 NEA-TDB JNC-TDB Am(   ) Neck et al.(1998) 31) NEA-TDB Stadler & Kim,1988 32) , Runde & Kim,1994 33) , Edelstein et al.,1983 34) , Caceci & Choppin,198335) , Wimmer et al.,1992369,Fanghänel et al.,199437) SIT model JAEA-TDB K Neck et al.(1998) 31) NEA (U) 3.6 Rai et al.(1995) 15) Na 2 SO 3 UO 2 (am) 10 -75 atm O 2 U(    )O2(am) 0.01mol/l NaOH UO 2 (am) FRHP 3.6.1 U U(  )  U(  ) U(   ) UO 2 (CO 3 ) 3 ~   (3-6-1) K PSI-TDB (3-6-1) PSI-TDB K (3-6-1) K (3-6-1) (3-6-5) (3-6-6) (3-6-7) PSI-TDB UO 2 (s) UO 2 (am) K (3-6-2) UO 2 (CO 3 ) 2 ² K UO2(CO3)2 10 7 (mol/l)(JNC-TDB)  7.3× 10 9 (mol/l) (NEA-TDB)  1.3× 10 9 (mol/l)(PSI-TDB)]  (3-5-2) K (3-6-6) (3-6-2) (3-6-5) K [1.5 × (3-6-7) U Rai et al.(1995) 15) U(   ) 8 U(   ) 3.6.2 JNC-TDB JNC-TDB U(OH)²(CO 3 )²² (3-6-4) NEA-TDB      PSI-TDB         U(OH) 2 (CO 3 ) 2 2 U(OH)4 K (3-6-3) (3-6-3) UO₂(CO₃)₃ 4  + 3H† + 2e = UO₂ + 3HCO₃ . (3-6-1) logK = 15.859(JNC-TDB), 16.674(NEA-TDB), 18.419(PSI-TDB) (3-6-2) UO2 (CO3)2 2 + 2H + + 2e + 2HCO3 . logK = 10.192(JNC-TDB), 11.577(NEA-TDB), 12.752(PSI-TDB) 2 U(OH) 4 = UO 2 + 2H 2 O (3-6-3) logK = 8.690(JNC-TDB), 8.500(NEA-TDB), 9.0000(PSI-TDB) (3-6-4) U(OH)²(CO 3 )²² = UO 2 + 2HCO 3 . logK = 4.764(JNC-TDB) (3-6-5) UO 2 (am) = -4H + +2H 2 O + U 4+ logK = 2.560(JNC-TDB) (3-6-6) UO₂(am,hyd) = -4H† +2H₂O + U 4÷ logK = 1.505(NEA-TDB) (3-6-7) UO 2 (s) = -4H + +2H 2 O + U 4+ logK =-0.000(PSI-TDB)
3.6.2  U  SRHP PSI-TDB NEA-TDB UO2(CO3)34 JNC-TDB 0.04% 2.477× HCO 3 10 -4(mol/l)(JNC-TDB)   2.134× 10 -2(mol/l) (NEA-TDB)   1.622× 10 -2(mol/l) (PSI-TDB) 3.2.2 CH 4 JNC-TDB UO 2 (CO 3 ) 3 4 K JNC-TDB (3-6-1) HCO 3 U(OH) 4     (3-6-3) UO 2 (CO 3 ) 3 - UO 2 (CO 3 ) 3 - 3.6.4 U(   ) U(OH) 4 U(   ) U(OH)4 [U(OH) 4 9.59 × 2.63 ×  10°(mol/l)(NEA-TDB) (3-6-5)   (3-6-7) (3-6-8) 10 -10 (mol/l)(PSI-TDB)]     U(OH)4 (3-6-5)    (3-6-7) K U(OH) 4 U 4+ -4H + +4H 2 O = U(OH) 4 (3-6-8) logK = -11.250(JNC-TDB), -10.005(NEA-TDB), -9.0000(PSI-TDB)
3.6.3  U K (3-6-5)   (3-6-7) K JNC-TDB        Rai et al.,1997 38) K UO 2 (am)     UO 2 (cr) PSI-TDB NEA-TDB Neck & Kim,2001 39) K Neck & Kim,200139) PSI-TDB NEA-TDB U(OH)²(CO3)²² FRHP JAEA-TDB U(   ) K 4. Se, U, Np, Pu, Th, Am JNC-TDB   NEA-TDB 4.1
PHREEQC K CO 3 ² /CH 4 HCO 3 1. PSI-TDB
JNC-TDB NEA-TDB PSI-TDB SIT model JAEA-TDB
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