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9.2 Aqueous neptunium group 17 (halogen) complexes 157[69KRY/KOM3] are corrected for the formation of NpNO 3+3(see Appendix A) andused in the evaluation procedure of log ∗ 10 β1 ◦ . The values reported for log 10 ∗ β 1 at20 ◦ C[66AHR/BRA] and 23 ◦ C[90SAW/CHA2] are corrected to 25 ◦ Cbyusingtheenthalpy value selected below.The values for log ∗ 10 β 1 are in good agreement with the exception of the mostrecent determination of this constant by Sawant, Chaudhuri and Patil [90SAW/CHA2],who used a fluoride ion selective electrode. The constants reported in that study forU(IV) and Pu(IV) are also inconsistent with those of other determinations. Furtherirregularities, cf. Appendix A, have led us to exclude the constants reported in[90SAW/CHA2] from the selection procedure. Having done this, a simultaneousdetermination of log ∗ 10 β1 ◦ and ε by weighted linear regression appears feasible, cf.Figure 9.1, wherethe25 ◦ C data from [66AHR/BRA, 69KRY/KOM, 69KRY/KOM3,75PAT/RAM, 76BAG/RAM, 76CHO/UNR] are used. The resulting value islog ∗ 10 β1 ◦ (9.4, q = 1, 298.15 K) = (5.78 ± 0.14). The slope of the straight line inFigure 9.1 corresponds to ε(9.4, q = 1) = −(0.12 ± 0.04)kg·mol −1 , whichcompares well with ε =−0.14kg·mol −1 estimated for the corresponding U(IV)-HFreaction [92GRE/FUG]. We convert this constant to conform to Equation (9.5) usingour selected protonation constant of fluoride [92GRE/FUG]. The resulting selectedvalue islog 10 β1 ◦ (9.5, q = 1, 298.15 K) = 8.96 ± 0.14.It should be noted that Krupka et al. [85KRU/RAI] observed no measurable increaseof Np(IV) solubility in the presence of up to 100 ppm fluoride. However, thisobservation is not necessarily in contradiction with our selected value, cf. Appendix A.For the formation of the 1:2 complex, NpF 2+2, Ahrland and Brandt [66AHR/BRA]published two values measured independently with a cation exchange method andwith a redox electrode, respectively. The values are in very good agreement, as isthe value published by Patil and Ramakrishna [75PAT/RAM] who used a solventextraction technique. Again, the value published by Sawant, Chaudhuri and Patil[90SAW/CHA2] differs considerably from the other values and is omitted in the selectionprocedure. The values of log ∗ 10 β2 ◦ listed in Table 9.3 are obtained by extrapolatingthe reported constants to I = 0byusingε(9.4, q = 2) =−(0.18 ± 0.15)kg·mol −1from the corresponding U(IV) fluoride system [92GRE/FUG], where the uncertaintyhas been increased by 0.05. The weighted average of the three valuesis log ∗ 10 β2 ◦ (9.4, q = 2) = (9.34 ± 0.29). We convert this value to conform toEquation (9.5) using our selected protonation constant of fluoride [92GRE/FUG]. Theresulting selected value islog 10 β2 ◦ (9.5, q = 2, 298.15 K) = 15.7 ± 0.3Data for the 1:3 and 1:4 complexes were published by Ahrland and Brandt[66AHR/BRA], and by Sawant, Chaudhuri and Patil [90SAW/CHA2]. The valuesdiffer considerably, even after correction to I = 0 using the ε values fromthe corresponding U(IV) fluoride system [92GRE/FUG], cf. Table 9.3. If weuse ε (NpF+3 ,ClO − 4 ) ≈ ε (M + ,ClO − 4 ) ≈ 0.3kg·mol −1 (cf. Appendix B) instead of
158 9. Neptunium group 17 (halogen) compounds and complexesTable 9.3: Experimental equilibrium data for the neptunium(IV) fluoride system.Method Ionic t log ∗ 10 β q(a)medium ( ◦ C)Np 4+ + HF(aq) Å NpF 3+ + H +log 10 ∗ β ◦ (a)qReferencecix 4 M HClO 4 20 (4.82 ± 0.02) [66AHR/BRA]4MHClO 4 25 (4.79 ± 0.10) (b,c)cix 2 M HClO 4 25 (4.70 ± 0.30) (b) [69KRY/KOM]1MHClO 4 25 (4.56 ± 0.30) (b)cix 2 M HNO 3 25 (4.75±0.30) (b,d) [69KRY/KOM3]1 M HNO 3 25 (4.74±0.30) (b,d)dis-HD 2 M HClO 4 25 (4.62 ± 0.20) (b) [75PAT/RAM]dis-HTTA 2 M HClO 4 25 (4.60 ± 0.20) (b)dis-HTTA 2 M HClO 4 25 (4.70 ± 0.15) (b) [76BAG/RAM]dis 1 M HClO 4 10 4.71 [76CHO/UNR]1MHClO 4 25 (4.60 ± 0.20) (b)1MHClO 4 40 4.52ise-F − 1M 23 5.21 (c,e) [90SAW/CHA2](H,Na)ClO 4Np 4+ + 2HF(aq) Å NpF 2+2+ 2H +cix 4 M HClO 4 20 (7.57 ± 0.15) (b) (9.30±0.75) [66AHR/BRA]red 4 M HClO 4 20 (7.51 ± 0.15) (b,f) (9.24±0.75)dis-HTTA 2 M HClO 4 25 (7.49 ± 0.40) (b) (9.44±0.52) [75PAT/RAM]dis-HTTA 2 M HClO 4 25 (7.38 ± 0.30) (b) (9.32±0.45) [76BAG/RAM]ise-F − 1M 23 8.62 (e) 10.49 [90SAW/CHA2](H,Na)ClO 4Np 4+ + 3HF(aq) Å NpF + 3 + 3H+red 4 M HClO 4 20 9.85 (f) 11.8 [66AHR/BRA]ise-F − 1MHClO 4 23 11.20 (e) 13.4 [90SAW/CHA2]Np 4+ + 4HF(aq) Å NpF 4 (aq) + 4H +red 4 M HClO 4 20 ∼ 11.15 (f) 13.3 [66AHR/BRA]ise-F − 1MHClO 4 23 14.15 (e) 16.4 [90SAW/CHA2](a) Refers to the reactions indicated, the ionic strength and temperature given in the table. log ∗ 10 βq◦is in molal units, at I = 0 and 298.15 K.(b) Uncertainty estimated in this review (cf. Appendix A).(c) Corrected to 25 ◦ C using the reaction enthalpy selected in this review.(d) Corrected for the formation of NpNO 3+3(cf. Appendix A).(e) The published values refer to Reactions (9.5) and have been converted to conform to the reactionsof this table (cf. Appendix A).(f) Reported as stepwise constants:log 10 ∗ K 2 = (2.69 ± 0.10), log 10 ∗ K 3 = (2.34 ± 0.15), andlog 10 ∗ K 4 ≈ 1.3. They are converted to overall formation constants by using log 10 ∗ K 1 = 4.82from the ion exchange experiments [66AHR/BRA] (see Appendix A).
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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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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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12.1 Neptunium carbon compounds and
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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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