Studies of (Cs,Ba)-hollandite dissolution under gamma irradiation at 95 °c and at pH 2.5, 4.4 and 8.6

T. Suzuki-Muresan, J. Vandenborre, A. Abdelouas, B. Grambow, Satoshi Utsunomiya

Research output: Contribution to journalArticle

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Abstract

In the frame of the former French 1991-law on waste management, which was extended in 2006-law, hollandite ceramic was studied as a potential specific conditioning matrix for caesium isotopes (long-life radionuclide 135Cs and the strong heat generating radionuclide 137Cs). In this general study of Cs-containment in a ceramic matrix, the chemical durability was pointed out as a key property. Leaching experiments in static mode were conducted during 240 days at various pH-values from acidic to alkaline range. The initial leaching rates between 0 and 45 days are faster for Cs than for Ba and the average for the caesium are (1.4 ± 0.1) × 10 -4 g/m2/d (pH 2.5), (6.4 ± 0.9) × 10 -5 g/m2/d (pH 4.4) and (3.1 ± 0.6) × 10 -5 g/m2/d (pH 8.6), and for the barium (6 ± 1) × 10-5 g/m2/d (pH 2.5), (2.8 ± 0.3) × 10-5 g/m2/d (pH 4.4), and (2 ± 2) × 10 -6 g/m2/d (pH 8.6). At the equilibrium between 45 and 240 days, the normalised mass losses average for caesium are (8.2 ± 0.3) × 10-3 g/m2 (pH 2.5), (5.2 ± 0.4) × 10-3 g/m2 (pH 4.4) and (4.1 ± 0.2) × 10 -3 g/m2 (pH 8.6), and for barium (3.7 ± 0.4) × 10-3 g/m2 (pH 2.5), (2.0 ± 0.1) × 10-3 g/m2 (pH 4.4) and (4 ± 2) × 10 -4 g/m2 (pH 8.6). Caesium and barium are incongruently released in solution with a correlation slope close to 0.5 at pH 2.5 and pH 4.4 and very low (near 0.02) in alkaline solution. Sorption experiments with radioactive isotopes (137Cs and 133Ba) were conducted on hollandite pre-leached in aqueous solutions. Caesium and barium release is controlled by the surface reactions. Leaching experiments and isotopic addition experiments (137Cs- and 133Ba-radiotracer) indicate that caesium behaviour is independent on pH-values, whereas barium behaviour is strongly dependent. Additional experiments in the presence of gamma irradiation (60Co source) did not show any significant effect on hollandite leaching process.

Original languageEnglish
Pages (from-to)281-290
Number of pages10
JournalJournal of Nuclear Materials
Volume419
Issue number1-3
DOIs
Publication statusPublished - Dec 1 2011

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Cesium
Barium
dissolving
Dissolution
Leaching
Irradiation
irradiation
Radioisotopes
Experiments
Cesium Isotopes
cesium
barium
leaching
Surface reactions
Waste management
radioactive isotopes
Sorption
Durability
Isotopes
cesium isotopes

All Science Journal Classification (ASJC) codes

  • Nuclear and High Energy Physics
  • Nuclear Energy and Engineering
  • Materials Science(all)

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Studies of (Cs,Ba)-hollandite dissolution under gamma irradiation at 95 °c and at pH 2.5, 4.4 and 8.6. / Suzuki-Muresan, T.; Vandenborre, J.; Abdelouas, A.; Grambow, B.; Utsunomiya, Satoshi.

In: Journal of Nuclear Materials, Vol. 419, No. 1-3, 01.12.2011, p. 281-290.

Research output: Contribution to journalArticle

Suzuki-Muresan, T. ; Vandenborre, J. ; Abdelouas, A. ; Grambow, B. ; Utsunomiya, Satoshi. / Studies of (Cs,Ba)-hollandite dissolution under gamma irradiation at 95 °c and at pH 2.5, 4.4 and 8.6. In: Journal of Nuclear Materials. 2011 ; Vol. 419, No. 1-3. pp. 281-290.
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abstract = "In the frame of the former French 1991-law on waste management, which was extended in 2006-law, hollandite ceramic was studied as a potential specific conditioning matrix for caesium isotopes (long-life radionuclide 135Cs and the strong heat generating radionuclide 137Cs). In this general study of Cs-containment in a ceramic matrix, the chemical durability was pointed out as a key property. Leaching experiments in static mode were conducted during 240 days at various pH-values from acidic to alkaline range. The initial leaching rates between 0 and 45 days are faster for Cs than for Ba and the average for the caesium are (1.4 ± 0.1) × 10 -4 g/m2/d (pH 2.5), (6.4 ± 0.9) × 10 -5 g/m2/d (pH 4.4) and (3.1 ± 0.6) × 10 -5 g/m2/d (pH 8.6), and for the barium (6 ± 1) × 10-5 g/m2/d (pH 2.5), (2.8 ± 0.3) × 10-5 g/m2/d (pH 4.4), and (2 ± 2) × 10 -6 g/m2/d (pH 8.6). At the equilibrium between 45 and 240 days, the normalised mass losses average for caesium are (8.2 ± 0.3) × 10-3 g/m2 (pH 2.5), (5.2 ± 0.4) × 10-3 g/m2 (pH 4.4) and (4.1 ± 0.2) × 10 -3 g/m2 (pH 8.6), and for barium (3.7 ± 0.4) × 10-3 g/m2 (pH 2.5), (2.0 ± 0.1) × 10-3 g/m2 (pH 4.4) and (4 ± 2) × 10 -4 g/m2 (pH 8.6). Caesium and barium are incongruently released in solution with a correlation slope close to 0.5 at pH 2.5 and pH 4.4 and very low (near 0.02) in alkaline solution. Sorption experiments with radioactive isotopes (137Cs and 133Ba) were conducted on hollandite pre-leached in aqueous solutions. Caesium and barium release is controlled by the surface reactions. Leaching experiments and isotopic addition experiments (137Cs- and 133Ba-radiotracer) indicate that caesium behaviour is independent on pH-values, whereas barium behaviour is strongly dependent. Additional experiments in the presence of gamma irradiation (60Co source) did not show any significant effect on hollandite leaching process.",
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N2 - In the frame of the former French 1991-law on waste management, which was extended in 2006-law, hollandite ceramic was studied as a potential specific conditioning matrix for caesium isotopes (long-life radionuclide 135Cs and the strong heat generating radionuclide 137Cs). In this general study of Cs-containment in a ceramic matrix, the chemical durability was pointed out as a key property. Leaching experiments in static mode were conducted during 240 days at various pH-values from acidic to alkaline range. The initial leaching rates between 0 and 45 days are faster for Cs than for Ba and the average for the caesium are (1.4 ± 0.1) × 10 -4 g/m2/d (pH 2.5), (6.4 ± 0.9) × 10 -5 g/m2/d (pH 4.4) and (3.1 ± 0.6) × 10 -5 g/m2/d (pH 8.6), and for the barium (6 ± 1) × 10-5 g/m2/d (pH 2.5), (2.8 ± 0.3) × 10-5 g/m2/d (pH 4.4), and (2 ± 2) × 10 -6 g/m2/d (pH 8.6). At the equilibrium between 45 and 240 days, the normalised mass losses average for caesium are (8.2 ± 0.3) × 10-3 g/m2 (pH 2.5), (5.2 ± 0.4) × 10-3 g/m2 (pH 4.4) and (4.1 ± 0.2) × 10 -3 g/m2 (pH 8.6), and for barium (3.7 ± 0.4) × 10-3 g/m2 (pH 2.5), (2.0 ± 0.1) × 10-3 g/m2 (pH 4.4) and (4 ± 2) × 10 -4 g/m2 (pH 8.6). Caesium and barium are incongruently released in solution with a correlation slope close to 0.5 at pH 2.5 and pH 4.4 and very low (near 0.02) in alkaline solution. Sorption experiments with radioactive isotopes (137Cs and 133Ba) were conducted on hollandite pre-leached in aqueous solutions. Caesium and barium release is controlled by the surface reactions. Leaching experiments and isotopic addition experiments (137Cs- and 133Ba-radiotracer) indicate that caesium behaviour is independent on pH-values, whereas barium behaviour is strongly dependent. Additional experiments in the presence of gamma irradiation (60Co source) did not show any significant effect on hollandite leaching process.

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