Startseite Naturwissenschaften Modeling the sorption of Np(V) on Na-montmorillonite – effects of pH, ionic strength and CO2
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Modeling the sorption of Np(V) on Na-montmorillonite – effects of pH, ionic strength and CO2

  • Raphael Scholze , Samer Amayri und Tobias Reich EMAIL logo
Veröffentlicht/Copyright: 27. Mai 2019
Radiochimica Acta
Aus der Zeitschrift Radiochimica Acta Band 107 Heft 7

Abstract

Results from batch type experiments were modeled using the 2 SPNE SC/CE model developed by Bradbury and Baeyens. This work focused on the applicability of this model to the sorption of Np(V) on Na-montmorillonite under high saline conditions (0.1–3.0 M NaCl) in the pH range of 2–10 and in the presence of dissolved CO2 (p(CO2) = 10−3.3 atm). Under ambient air conditions two additional surface complexation species had to be taken into account, which are ternary species involving one carbonate ligand (≡SONpO2(CO3)2−, ≡SONpO2(CO3)Na−). The gained set of complexation parameters was successfully tested over a wide range of Np(V) concentrations (10−4 to 10−12 M) under Ar atmosphere and ambient air condition.

Keywords: Neptunium; Np(V); montmorillonite; sorption; modeling; 2 SPNE SC/CE

Dedicated to: The memory of Prof. Dr. Günter Herrmann.

Acknowledgement

This work was financially supported by the Federal Ministry for Economic Affairs and Energy under contract No. 02E10981 and 02E11415A. We thank T. Billington, A. Damm and Ch. Fuhr for the experimental assistance. Furthermore, we thank B. Baeyens and M. Marques Fernandes at Paul Scherrer Institute (PSI/LES) for their valuable comments and suggestions.

Appendix

Table A1:

Buffer solutions used in the batch sorption experiments [13].

BufferpKapH range
AA (acetic acid)4.764.3–5.3
MES (2-(N-morpholino)ethanesulfonic acid)6.155.7–6.7
MOPS (3-(N-morpholino)propanesulfonic acid)7.206.8–7.7
TRIS (Tris(hydroxymethyl)aminomethane)8.067.5–8.5
CHES (2-(cyclohexylamino)ethanesulfonic acid)9.559.0–10.0
Table A2:

Experimental conditions of the batch sorption experiments.

[Np(V)] mol/LAtmospherepHS/L ratio g/LLiquid phaseFigure
8×10−6Ar6–104–100.1 M NaCl1
8×10−6Ar6–104–101.0 M NaCl1
3.5×10−12Ambient air2.5–9170.1 M NaCl2, 3
3.5×10−12Ambient air5–9171.0 M NaCl2, 3
1×10−8Ambient air6–933.0 M NaCl2, 3
10−6–10−12Ambient air8100.1 M NaCl4
10−4–10−11Ar8.540.1 M NaCl5
10−4–10−11Ar8.541.0 M NaCl5
10−4–1011Ar8.543.0 M NaCl5
Table A3:

Used complexation constants for the aquatic speciation.

Reactionlog K0Reference
Na++CO32−→Na(CO3)−1.27a[39]
H++CO32−→H(CO3)−10.329±0.020[39]
NpO2++H2O→NpO2(OH)+H+−11.3±0.7[33]
NpO2++2 H2O→NpO2(OH)2−+2 H+−23.6±0.5[33]
NpO2++CO32−→NpO2(CO3)−4.96±0.06[33]
NpO2++2 CO32−→NpO2(CO3)23−6.53±0.10[33]
NpO2++3 CO32−→NpO2(CO3)35−5.50±0.15[33]
NpO2++2 CO32−+H2O→NpO2(CO3)2(OH)4−+H+−5.30±1.17[33]

  1. aCalculated from ΔfG0 values.

Table A4:

Used SIT parameters [39].

Species 1Species 2ε
CO32−Na+−0.08±0.03
HCO3−Na+0.00±0.02
OH−Na+0.04±0.01
NpO2(CO3)−Na+−0.18±0.15
NpO2(CO3)23−Na+−0.33±0.17
NpO2(CO3)35−Na+−0.53±0.19
NpO2(CO3)2OH4−Na+−0.40±0.19
NpO2(OH)2−Na+−0.01±0.07
H+Cl−0.12±0.01
NpO2+Cl−0.09±0.05
Na+Cl−0.03±0.01

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Received: 2019-01-22
Accepted: 2019-04-24
Published Online: 2019-05-27
Published in Print: 2019-07-26

©2019 Walter de Gruyter GmbH, Berlin/Boston

Artikel in diesem Heft

  1. Frontmatter
  2. Preface
  3. Günter Herrmann (1925–2017): A tribute to his research and organizational achievements
  4. The research reactor TRIGA Mainz – a strong and versatile neutron source for science and education
  5. Copper-catalyzed click reactions: quantification of retained copper using 64Cu-spiked Cu(I), exemplified for CuAAC reactions on liposomes
  6. Reactions of fission products from a 252Cf source with NO and mixtures of NO and CO in an inert gas
  7. From SRAFAP to ARCA and AIDA – developments and implementation of automated aqueous-phase rapid chemistry apparatuses for heavy actinides and transactinides
  8. Production and study of chemical properties of superheavy elements
  9. Precise ground state properties of the heaviest elements for studies of their atomic and nuclear structure
  10. Modeling the sorption of Np(V) on Na-montmorillonite – effects of pH, ionic strength and CO2
  11. Determination of complex formation constants of neptunium(V) with propionate and lactate in 0.5–2.6 m NaCl solutions at 22–60°C using a solvent extraction technique
  12. Nuclear forensics on uranium fuel pellets
  13. Recent developments in resonance ionization mass spectrometry for ultra-trace analysis of actinide elements
  14. Measurement of the laser resonance ionization efficiency for lutetium
https://doi.org/10.1515/ract-2019-3109
Schlagwörter für diesen Artikel
Neptunium; Np(V); montmorillonite; sorption; modeling; 2 SPNE SC/CE

Artikel in diesem Heft

  1. Frontmatter
  2. Preface
  3. Günter Herrmann (1925–2017): A tribute to his research and organizational achievements
  4. The research reactor TRIGA Mainz – a strong and versatile neutron source for science and education
  5. Copper-catalyzed click reactions: quantification of retained copper using 64Cu-spiked Cu(I), exemplified for CuAAC reactions on liposomes
  6. Reactions of fission products from a 252Cf source with NO and mixtures of NO and CO in an inert gas
  7. From SRAFAP to ARCA and AIDA – developments and implementation of automated aqueous-phase rapid chemistry apparatuses for heavy actinides and transactinides
  8. Production and study of chemical properties of superheavy elements
  9. Precise ground state properties of the heaviest elements for studies of their atomic and nuclear structure
  10. Modeling the sorption of Np(V) on Na-montmorillonite – effects of pH, ionic strength and CO2
  11. Determination of complex formation constants of neptunium(V) with propionate and lactate in 0.5–2.6 m NaCl solutions at 22–60°C using a solvent extraction technique
  12. Nuclear forensics on uranium fuel pellets
  13. Recent developments in resonance ionization mass spectrometry for ultra-trace analysis of actinide elements
  14. Measurement of the laser resonance ionization efficiency for lutetium
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