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γ-Radiolysis of NaCl Brine in the Presence of UO2(s): Effects of Hydrogen and Bromide

Published online by Cambridge University Press:  19 October 2011

Volker Metz
Affiliation:
volker@ine.fzk.de, Forschungszentrum Karlsruhe / Research Center Karlsruhe, Institute for Radioactive Waste Disposal (FZK-INE), Helmholtz-Platz, Eggenstein-Leopoldshafen, D-76344, Germany, ++49-7247-82-8078, ++49-7247-82-4308
Elke Bohnert
Affiliation:
bohnert@ine.fzk.de, Forschungszentrum Karlsruhe / Research Center Karlsruhe, Institute for Radioactive Waste Disposal (FZK-INE), Helmholtz-Platz, Eggenstein-Leopoldshafen, D-76344, Germany
Manfred Kelm
Affiliation:
kelm@ine.fzk.de, Forschungszentrum Karlsruhe / Research Center Karlsruhe, Institute for Radioactive Waste Disposal (FZK-INE), Helmholtz-Platz, Eggenstein-Leopoldshafen, D-76344, Germany
Dieter Schild
Affiliation:
schild@ine.fzk.de, Forschungszentrum Karlsruhe / Research Center Karlsruhe, Institute for Radioactive Waste Disposal (FZK-INE), Helmholtz-Platz, Eggenstein-Leopoldshafen, D-76344, Germany
Jörgen Reinhardt
Affiliation:
reinj@server1.rz.uni-leipzig.de, IOM, Leibniz-Institut für Oberflächenmodifizierung, Permoserstr. 15, Leipzig, D-04318, Germany
Bernhard Kienzler
Affiliation:
kienzler@ine.fzk.de, Forschungszentrum Karlsruhe / Research Center Karlsruhe, Institute for Radioactive Waste Disposal (FZK-INE), Helmholtz-Platz, Eggenstein-Leopoldshafen, D-76344, Germany
Michael R. Buchmeiser
Affiliation:
michael.buchmeiser@iom-leipzig.de, IOM, Leibniz-Institut für Oberflächenmodifizierung, Permoserstr. 15, Leipzig, D-04318, Germany
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Abstract

Concentrated NaCl solution was γ-irradiated in autoclaves under a pressure of 25 MPa. A set of experiments were conducted in 6 mol (kg H2O)-1 NaCl solution in presence of UO2(s) pellets; in a second set of experiments γ-radiolysis of the NaCl brine was studied without UO2(s). Hydrogen, oxygen and chlorate were formed as lonγ-lived radiolysis products. Due to the high external pressure, all radiolysis products remained dissolved. H2 and O2 reached steady state concentrations in the range of 5·10-3 to 6·10-2 mol (kg H2O)-1 corresponding to gas partial pres-sure of ∼2 to ∼20 MPa. Radiolytic formation of hydrogen and oxygen increases with the concentration of bromide added to solution. Both, in the presence of bromide, resulting in a relatively high radiolytic yield, and in the absence of bromide surfaces of the UO2(s) samples were oxi-dized, and concentration of dissolved uranium reached the solubility limit of schoepite / NaUO2O(OH)(cr) transition. At the end of the experiments the pellets were covered by a surface layer of a secondary solid phase having a composition close to Na2U2O7. The experimental results demonstrate that bromide counteracts an H2 inhibition effect on radiolysis gas production, even at a concentration ratio of [H2] / [Br-] > 100. The present observations are related to the competitive reactions of OH radicals with H2, Br- and Cl-. A similar competition of hydrogen and bromide, controlling the yield of γ-radiolysis products, is expected for solutions of lower Cl- concentration

Type
Research Article
Copyright
Copyright © Materials Research Society 2007

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References

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