chemical thermodynamics of neptunium and plutonium - U.S. ...

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LIST OF TABLESxxi20.2 Experimental equilibrium data for the plutonium(IV) nitrate system . . . . . . . . . . . . 40720.3 Experimental equilibrium data for the dioxoplutonium(VI) nitrate system . . . . . . . . . 41420.4 Experimental equilibrium data for the Pu(IV) phosphate system . . . . . . . . . . . . . . . 41720.5 Literature equilibrium constants for the Pu(VI) phosphate system . . . . . . . . . . . . . . 41921.1 Summary of experimental results concerning PuO 2+2 -CO2− 3complexes. . . . . . . . . . . 43221.2 Recommended values in the Pu(VI) carbonate system . . . . . . . . . . . . . . . . . . . . 43321.3 Experimental equilibrium data for the plutonium(III) thiocyanate system . . . . . . . . . . 44323.1 Authors list . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 543A.1 Calculated and observed values for the first hydrolysis constants of several tripositive ions(from [54HIN]). . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 583A.2 Equilibrium constants referring to Reaction (A.33) as reported in [69KRY/KOM,69KRY/KOM3] . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 620A.3 Equilibrium constants referring to Reaction (A.34) as reported in [69KRY/KOM2,69KRY/KOM4] . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 621A.4 Values of the formation constant of NpSO 2−4 from the reaction of Np 4+ with HSO − 4 basedon a recalculation of the results of Patil and Ramakrishna [73PAT/RAM]. . . . . . . . . . 645A.5 Thermodynamic constants of M(IV) hydrolysis at ≈ 25 ◦ Casgivenby[74SOL]. . . . . . . 651A.6 Standard potentials (I = 0) from measurements of the Np(VI)/Np(V) redox couple inaqueous carbonate media. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 671A.7 Formation constants of thiocyanate complexes reported in [78RAO/BAG2] at different temperatures. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 674A.8 Stability constants of Np(V) and Pu(V) complexes with various ligands as given in[78MOS/POZ] and[79MOS/POZ]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 680A.9 Formation constants for neutral plutonium(IV) complexes as given by [80SOL/ZAK]. . . . 685A.10 Hydrolysis constants for trivalent Pu, Am, Sm and Eu as given by [82NAI/CHA]. . . . . . 689A.11 Results from refitting Maya’s solubility data for Np(V) in carbonate solutions. . . . . . . . 692A.12 Values of the formation constant of Pu(SO 4 ) − 2 from the reaction of Pu3+ with HSO − 4 basedon a recalculation of the results of Nash and Cleveland [83NAS/CLE2]. . . . . . . . . . . 694A.13 Values of temperature coefficients for standard potentials from Blanc and Madic[84BLA/MAD]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 696A.14 Table of values and limiting values of formation constants based on reassessment of Maya’spotentiometric titration data [84MAY] . . . . . . . . . . . . . . . . . . . . . . . . . . . . 704A.15 Calculation of the maximum value of the formation constant of some complexes of Np(IV) 715A.16 Results of recalculations of the data of Brand and Cobble [70BRA/COB] . . . . . . . . . . 726A.17 Values of the formation constant for NpO 2 CO − 3 in 0.1 M NaClO 4 from various analysesof the spectrophotometric measurements of Nitsche, Standifer and Silva [90NIT/STA]. . . 737A.18 Experimental conditions of the [90RIG] publication spectrophotometric measurements. . . 740A.19 Np(V) carbonate complexation constants deduced from the spectrophotometric measurementsreported in [90RIG]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 741A.20 Curve fitting results of solubility measurements of Np(V) in 2 M NaClO 4 carbonate/bicarbonate/carbonicacid aqueous solutions [84VIT, 85CÔM, 85KIM, 86GRE/ROB,90RIG] . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 743A.21 Determination of the stoichiometry of a hydrated Na (2x−1) NpO 2 (CO 3 ) x (s) solid phasefrom solubility data [84VIT, 85CÔM, 85KIM, 86GRE/ROB, 90RIG] . . . . . . . . . . . . 744A.22 Formation constants of fluoride complexes of tetravalent actinides as reported by Sawant,Chaudhuri and Patil [90SAW/CHA2] . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 748A.23 Formation constants of fluoride complexes of tetravalent actinides [90SAW/CHA2] aftercorrection for the protonation constant offluoride . . . . . . . . . . . . . . . . . . . . . . 749A.24 Comparison of the formation constants of the U(IV) fluoride complexes of[90SAW/CHA2] with those selected in the TDB uranium review [92GRE/FUG] . . . . . . 749A.25 Curve fitting results for solubility measurements of Np(V) in carbonate/bicarbonate/carbonicacid aqueous solutions [91KIM/KLE, 94NEC/KIM, 95FAN/NEC, 95NEC/FAN,95NEC/RUN] . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 752
xxiiLIST OF TABLESA.26 Temperature dependence of redox couples [92CAP]. . . . . . . . . . . . . . . . . . . . . 757A.27 Values of the potentials for the irreversible plutonium couples as calculated by Capdevila[92CAP]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 758A.28 Estimation of formation constants Np(V) carbonate complexes from solubility measurementsof [93LEM/BOY] . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 763A.29 Values of ε (NpO+2,ClO − 4 ) recalculated in this review from the measurements of[91KIM/KLE, 94NEC/KIM, 95NEC/FAN, 95NEC/RUN] . . . . . . . . . . . . . . . . . . 776A.30 Formal potentials for the Np(V)/Np(IV) couple in Na 2 CO 3 (aq) solutions as calculatedfrom values in [96DEL/VIT]. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 787B.1 Debye-Hückel constants at several temperatures . . . . . . . . . . . . . . . . . . . . . . . 805B.2 Preparation of experimental data for the extrapolation to I = 0 . . . . . . . . . . . . . . . 807B.3 Ion interaction coefficients ε for cations . . . . . . . . . . . . . . . . . . . . . . . . . . . 813B.4 Ion interaction coefficients ε for anions . . . . . . . . . . . . . . . . . . . . . . . . . . . . 819B.5 Ion interaction coefficients ε 1 and ε 2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 822
Page 1 and 2: 4VOLUMECHEMICALTHERMODYNAMICSCHEMIC
Page 3 and 4: CHEMICAL THERMODYNAMICSVol. 1. Chem
Page 5 and 6: Published under the imprint NORTH-H
Page 7 and 8: viPREFACEviewed several of the othe
Page 9 and 10: viiiACKNOWLEDGEMENTSand Whiteshell
Page 11 and 12: xFOREWORDsending comments on the TD
Page 13 and 14: xiiCONTENTSIII Discussion of neptun
Page 15: xivCONTENTS11.1.4.2 Solid neptunium
Page 18 and 19: CONTENTSxvii20.5.1 PuSb(cr) . . . .
Page 20 and 21: List of Tables2.1 Symbols and termi
Page 24 and 25: List of Figures2.1 Standard order o
Page 26: Part IIntroductory material1
Page 29 and 30: 4 1. IntroductionInorganic Complexe
Page 31 and 32: 6 1. Introductionlected, but form a
Page 34 and 35: Chapter 2Standards, Conventions, an
Page 36 and 37: 2.1 Symbols, terminology and nomenc
Page 48 and 49: 2.2 Units and conversion factors 23
Page 50 and 51: 2.2 Units and conversion factors 25
Page 52 and 53: 2.3 Standard and reference conditio
Page 54 and 55: 2.3 Standard and reference conditio
Page 56 and 57: 2.5 Uncertainty estimates 31Table 2
Page 58 and 59: 2.7 Presentation of the selected da
Page 60: 2.7 Presentation of the selected da
Page 64 and 65: Chapter 3Selected neptunium dataThi
Page 66 and 67: 41Table 3.1: Selected thermodynamic
Page 68 and 69: 43Table 3.1: (continued)Compound f
Page 70 and 71: 45Table 3.1: (continued)Compound f
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47Table 3.2: Selected thermodynamic
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49Table 3.2: (continued)SpeciesReac
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Chapter 4Selected plutonium dataThi
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55Table 4.1: Selected thermodynamic
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57Table 4.1: (continued)Compound f
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61SpeciesPu(OH) 3 (cr)ReactionTable
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Chapter 5Selected auxiliary dataThi
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(footnotes continued)(p) Data from
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79Table 5.2: (continued)Species Rea
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81Table 5.2: (continued)Species Rea
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Chapter 6Elemental neptunium6.1 Nep
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6.1 Neptunium crystal and liquid 87
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6.2 Neptunium ideal monatomic gas 8
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92 7. Neptunium aqua ionsE ◦′ (
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94 7. Neptunium aqua ionsto the sta
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96 7. Neptunium aqua ions(∂ E ◦
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98 7. Neptunium aqua ionsnon-system
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100 7. Neptunium aqua ionsto the re
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102 7. Neptunium aqua ionsTable 7.4
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Chapter 8Neptunium oxygen andhydrog
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8.1 Aqueous neptunium hydroxide com
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8.2 Crystalline and amorphous neptu
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132 9. Neptunium group 17 (halogen)
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178 10. Neptunium group 16 compound
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Chapter 11Neptunium group 15compoun
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11.1 Neptunium nitrogen compounds a
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11.2 Neptunium phosphorus compounds
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11.2 Neptunium phosphorus compounds
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Chapter 12Neptunium group 14compoun
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12.1 Neptunium carbon compounds and
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cal 0.3-1.6 M Na 2 SO 4 25 r H m =
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vlt 0 25 (0.340±0.002) (k) [95OFF/
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sol K + ,CO 2−3 , 20 −(2.31±0.
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sp 0.1 M NaCl 23 (4.68±0.03) [96RU
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dis 0.2 M NaClO 25 2.93 (3.42±1.0)
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sol 1 M NaCl 23 (2.06±0.13) [96RUN
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sol 0.15 M Na 2 CO 3 −(2.58±0.64
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sol 1 M NaClO 30 −(4.0±0.2) [93L
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sol 3 M NaClO 25 −(2.14±0.18)
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(f) Values selected in this review
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(V vs. SHE) (V vs. SHE) (V · K −
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(h) 1MK 2 CO 3 is written in Table
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2 3 r H m (5.0±2.0)log 10 β 2 MO
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290 13. Neptunium group 2 (alkaline
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292 14. Neptunium group 1 (alkali)
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Part IVDiscussion of plutonium data
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298 15. Elemental plutoniumTable 15
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300 15. Elemental plutoniumfrom 298
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302 16. Plutonium aqua ionsthe prop
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304 16. Plutonium aqua ions298.15 K
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306 16. Plutonium aqua ionsE ◦ =
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308 16. Plutonium aqua ionsSm ◦ (
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310 16. Plutonium aqua ionsstandard
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312 16. Plutonium aqua ions r H ◦
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314 16. Plutonium aqua ionsE ◦′
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316 16. Plutonium aqua ionsFigure 1
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318 17. Plutonium oxygen and hydrog
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1:1 pot RT 1 M NaClO 4 −5.71 [49K
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Chapter 18Plutonium group 17 (halog
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18.1 Plutonium halide compounds 347
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18.2 Aqueous plutonium group 17 (ha
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PuO 2+2+ 3F − Å PuO 2 F − (b)3
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390 19. Plutonium group 16 compound
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Chapter 20Plutonium group 15 compou
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20.1 Plutonium nitrogen compounds a
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Pu + NO 3Å PuNO 3sp 2 M HClO 4 20
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3 3 3dis, TTA 6 M (? HCl or HClO 4
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20.2 Plutonium phosphorus compounds
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20.2 Plutonium phosphorus compounds
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20.3 Solid plutonium phosphorus com
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20.4 Plutonium arsenic compounds 42
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20.6 The plutonium-bismuth system 4
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20.6 The plutonium-bismuth system 4
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446 22. Plutonium group 2 (alkaline
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Chapter 23Plutonium group 1 (alkali
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452 BIBLIOGRAPHY[47GIN/COR][48KRA/N
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454 BIBLIOGRAPHY[49MAG/LAC][49ROB][
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456 BIBLIOGRAPHY[51WES/EYR][51WES/W
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458 BIBLIOGRAPHY[55COH/SUL]Cohen, D
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460 BIBLIOGRAPHYmetals in connectio
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462 BIBLIOGRAPHY[59SHE/TIM][59STU][
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464 BIBLIOGRAPHY[61SCH][61STO/FRY][
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466 BIBLIOGRAPHY[63ROB/WAL] Roberts
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468 BIBLIOGRAPHY[64SIL/MAR][65CHO/K
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470 BIBLIOGRAPHY[66DAN/ORL][66FRO/K
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472 BIBLIOGRAPHY[67ERM/STA][67FRL/C
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474 BIBLIOGRAPHY[68KRU/SAV][68KRY/K
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476 BIBLIOGRAPHY[69KEN/LEA][69KRY/K
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478 BIBLIOGRAPHY[70HIN/COB][70KRO/G
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480 BIBLIOGRAPHY[71MOS][71MOS2][71M
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482 BIBLIOGRAPHY[72MET/GUI][72NIK/S
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484 BIBLIOGRAPHY[73PAT/RAM2][73PIT]
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486 BIBLIOGRAPHY[74SAV][74SIM/VOL][
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488 BIBLIOGRAPHY[75OSB/FLO][75PAT/R
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490 BIBLIOGRAPHY298.15 K”, J. Che
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492 BIBLIOGRAPHY[76VOL/VIS][77BAG/R
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494 BIBLIOGRAPHY[78HAL/LEE][78HUR][
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496 BIBLIOGRAPHYof plutonium(IV)”
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498 BIBLIOGRAPHYNa 0.6 NpO 2 (CO 3
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500 BIBLIOGRAPHY[81CHI/AKH][81CIA/F
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502 BIBLIOGRAPHY[81WOO][82ALC/ROB][
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504 BIBLIOGRAPHY[83ALL][83BES/LIN][
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506 BIBLIOGRAPHY[83SCH/GOR]Schmidt,
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508 BIBLIOGRAPHY[84LEM][84LIE/KIM][
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510 BIBLIOGRAPHY[85CÔM][85EIS/KIM]
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512 BIBLIOGRAPHY[85NEW/SUL][85RAI/R
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514 BIBLIOGRAPHY[86FAH][86FRE/KEL]F
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516 BIBLIOGRAPHY[87BEN][87BEN/HOF][
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518 BIBLIOGRAPHY[88HIR/LIE][88ITU][
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520 BIBLIOGRAPHYGeochim. Cosmochim.
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522 BIBLIOGRAPHY[90BEN][90CAP/VIT][
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524 BIBLIOGRAPHY254, 258, 258, 264,
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526 BIBLIOGRAPHY[91MEI][91NIT][91OK
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528 BIBLIOGRAPHYment”, Waste Mana
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530 BIBLIOGRAPHY[93ERI/NDA][93GIF/V
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532 BIBLIOGRAPHY[93TAY/LEM][93WEG/O
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534 BIBLIOGRAPHYpages 222, 223, 226
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536 BIBLIOGRAPHYK, gas-phase infrar
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538 BIBLIOGRAPHY[96ALL/VEI][96CAP/V
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540 BIBLIOGRAPHY[97CAP/VIT][97FEL/R
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542 BIBLIOGRAPHY[99RAI/HES2][99RAR/
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544 LIST OF CITED AUTHORSTable 23.1
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Appendix ADiscussion of selected re
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A. Discussion of selected reference
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5 −10.63±0.11 (g) −12.48±0.23
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dataarein1MNa + media, except as no
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Appendix BIonic strength correction
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B.1 The specific ion interaction eq
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B.2 Ion interaction coefficients ve
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B.3 Tables of ion interaction coeff
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Appendix CAssigned uncertainties
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C.2 Two or more independent source
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C.2 Two or more independent source
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C.3 Several data at different ionic
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C.3 Several data at different ionic
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C.4 Procedures for data handling 83
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C.4 Procedures for data handling 83
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Index837
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INDEX - GENERAL 839standard state p
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INDEX - NEPTUNIUM 841elemental nept
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INDEX - PLUTONIUM 843Index - pluton
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INDEX - PLUTONIUM 845monobismuthide
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