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Evidence of Radiolytic Oxidation of 241Am in Na+ / Cl / HCO3/ CO2−3 Media.

Published online by Cambridge University Press:  01 January 1992

Eric Giffaut
Affiliation:
CEA, Department of Waste Management and Storage, Section of Geochemistry, BP 6, 92265, Fontenay aux Roses cedex, France
Pierre Vitorge
Affiliation:
CEA, Department of Waste Management and Storage, Section of Geochemistry, BP 6, 92265, Fontenay aux Roses cedex, France
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Abstract

This paper examines Americium behaviour in CI media at room temperature in connection with environmental and waste disposal programs. Most published values on U, Np, Pu and Am complexation in chloride media have been determined using extraction methods. Spectrophotometric techniques are not sensitive enough to prove actinide complexation by chloride, which is confirmed in this paper for Am(III).

Am(OH)3(s), AmOHCO3(s), Am2(CO3)3(s) or NaAm(CO3)2(s) solid phases can control the Am solubility, depending on the chemical conditions of the aqueous phase (usually PCO2). 241Am solubility is here found to be higher in NaCl 4M media than in NaCl 0.1 M (up to 3 orders of magnitude). Addition of a reducing agent (metallic iron) lowers the solubility. After a week, solubilities in NaCl 0.1 M and 4 M are similar. These results are consistent with Am(III) radiolytic oxidation to Am(V), due to cc radiations. Little evidence of Cl or mixed Cl-CO2−3 complexes is found in these conditions. In Na+-OH-Cl media, 241Am(III) oxidation had also been proposed. Slow kinetics of precipitation could induce experimental uncertainities.

Type
Research Article
Copyright
Copyright © Materials Research Society 1993

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