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

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A. Discussion of selected references 797NpO 2 (am) + 4CO 2−3+ 2H 2 O Å Np(CO 3 ) 4−4+ 4OH − (A.85)From this last value and the very rough approximation ε(12.25) = (0.38 ±0.18) kg·mol −1 (assuming the same value for ε(12.25) in aqueous Na + and K + media),ε(A.85)= −(0.83 ± 0.31) kg·mol −1 was calculated. From log 10 Ks,4 ◦ (A.85)=−(17.79±0.22) and log 10 K5 ◦(12.25) =−(1.07±0.30) the value log 10 K◦ s,5 (A.84) =−(18.86 ± 0.37) is calculated. From these values, log 10 K s,0 =−(54.48 ± 1.00), essentiallythe same value as was used in Section 8.2.5.2, and also used in [99RAI/HES],ε (CO2−3 ,K+ ) = (0.02 ± 0.01) kg·mol−1 and ε (OH − ,K + ) = (0.09 ± 0.02)kg·mol −1 ,thevalues log 10 β5 ◦(12.23) = (35.62 ± 1.07), log 10 β◦ 4(12.27) = (36.69 ± 1.03), andε (Np(CO3 ) 6−5 ,K+ ) =−(0.73 ± 0.68) kg·mol−1 are also calculated. These recalculatedvalues of β5 ◦ and K s,5 ◦ are more than two orders of magnitude greater than the valuesfrom the analysis in [99RAI/HES]; the differences probably result, at least in part, fromthe different assumptions used for extrapolation to I = 0.The authors concluded from X-ray absorption spectroscopic data that Np(CO 3 ) 6−5is the major solution species when NpO 2 (am) is equilibrated with 0.93 m KHCO 3 or5.4 m K 2 CO 3 aqueous solutions. This is consistent with the stoichiometry for the limitingcomplex assumed in the present review. However, according to the thermodynamicdata used by the authors, less than 1 % of the limiting complex was dissociated in the0.93 m KHCO 3 sample, while (45 ± 26)% dissociation is calculated using the spectrophotometricdata accepted in the present review. The reason for this discrepancy is notknown.
798 A. Discussion of selected referencesFigure A.8: Comparison of experimental data from [99RAI/HES] with values calculatedfrom the model used in the present review to interpret their data ([Np(IV)],[OH − ], [CO 2−3] are molalities).-3-4KOH + 1.78 m K 2 CO 3K 2 CO 3 +0.01MKOHKHCO 3-5log 10[Np(IV)] t-6log 10K° s,5=-18.86∆ε s,5=-0.47log 10 K° s,4=-17.79∆ε s,4=-0.85-7-8-9-2 -1 0 1 2 30.8 log 10[OH - ]+log 10[CO 3 2- ]
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4VOLUMECHEMICALTHERMODYNAMICSCHEMIC
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CHEMICAL THERMODYNAMICSVol. 1. Chem
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Published under the imprint NORTH-H
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viPREFACEviewed several of the othe
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viiiACKNOWLEDGEMENTSand Whiteshell
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xFOREWORDsending comments on the TD
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xiiCONTENTSIII Discussion of neptun
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xivCONTENTS11.1.4.2 Solid neptunium
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CONTENTSxvii20.5.1 PuSb(cr) . . . .
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List of Tables2.1 Symbols and termi
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LIST OF TABLESxxi20.2 Experimental
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List of Figures2.1 Standard order o
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Part IIntroductory material1
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4 1. IntroductionInorganic Complexe
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6 1. Introductionlected, but form a
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Chapter 2Standards, Conventions, an
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2.1 Symbols, terminology and nomenc
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2.2 Units and conversion factors 23
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2.2 Units and conversion factors 25
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2.3 Standard and reference conditio
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2.3 Standard and reference conditio
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2.5 Uncertainty estimates 31Table 2
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2.7 Presentation of the selected da
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2.7 Presentation of the selected da
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Chapter 3Selected neptunium dataThi
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41Table 3.1: Selected thermodynamic
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43Table 3.1: (continued)Compound f
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49Table 3.2: (continued)SpeciesReac
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Chapter 4Selected plutonium dataThi
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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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Page 772 and 773: A. Discussion of selected reference
Page 778 and 779: 5 −10.63±0.11 (g) −12.48±0.23
Page 788 and 789: dataarein1MNa + media, except as no
Page 824 and 825: Appendix BIonic strength correction
Page 826 and 827: B.1 The specific ion interaction eq
Page 836 and 837: B.2 Ion interaction coefficients ve
Page 838 and 839: B.3 Tables of ion interaction coeff
Page 848 and 849: Appendix CAssigned uncertainties
Page 850 and 851: C.2 Two or more independent source
Page 852 and 853: C.2 Two or more independent source
Page 854 and 855: C.3 Several data at different ionic
Page 856 and 857: C.3 Several data at different ionic
Page 858 and 859: C.4 Procedures for data handling 83
Page 860 and 861: C.4 Procedures for data handling 83
Page 862 and 863: Index837
Page 864 and 865: INDEX - GENERAL 839standard state p
Page 866 and 867: INDEX - NEPTUNIUM 841elemental nept
Page 868 and 869: INDEX - PLUTONIUM 843Index - pluton
Page 870: INDEX - PLUTONIUM 845monobismuthide
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