Cerium-promoted dissolution of PuO/sub 2/ and PuO/sub 2/--UO/sub 2/ in nitric acid
David A. Horner, D.J. Crouse, J.C. Mailen
Abstract
David A. Horner, D.J. Crouse, J.C. Mailen
Abstract
Several experiments were run to determine the feasibility of using cerium as an alternative to fluoride in promoting rapid dissolution of difficultly soluble PuO/sub 2/ in nitric acid. Results show that Ce/sup 4 +/, but not Ce/sup 3 +/, promotes dissolution with a maximum rate in boiling 4M HNO/sub 3/. Other strong oxidants, including ozone, permanganate, and persulfate, were tested but were shown to be ineffective. During dissolution, the Ce/sup 4 +/ is reduced to Ce/sup 3 +/, which must be reoxidized electrolytically or with ozone. Ruthenium also reduces the Ce/sup 4 +/ catalytically, being oxidized to the volatile RuO/sub 4/. Thus successful application to dissolution of irradiated fuel residues would require modification of the equipment or procedures in such a way as to encourage complete volatilization of ruthenium from the dissolver system. However, application of this method to the treatment of plutonium appears promising.
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Several experiments were run to determine the feasibility of using cerium as an alternative to fluoride in promoting rapid dissolution of difficultly soluble PuO/sub 2/ in nitric acid. Results show that Ce/sup 4 +/, but not Ce/sup 3 +/, promotes dissolution with a maximum rate in boiling 4M HNO/sub 3/. Other strong oxidants, including ozone, permanganate, and persulfate, were tested but were shown to be ineffective. During dissolution, the Ce/sup 4 +/ is reduced to Ce/sup 3 +/, which must be reoxidized electrolytically or with ozone. Ruthenium also reduces the Ce/sup 4 +/ catalytically, being oxidized to the volatile RuO/sub 4/. Thus successful application to dissolution of irradiated fuel residues would require modification of the equipment or procedures in such a way as to encourage complete volatilization of ruthenium from the dissolver system. However, application of this method to the treatment of plutonium appears promising.
Key concepts: Nitric acid, Dissolution, Cerium, Ruthenium, Chemistry, Ozone, Permanganate, Inorganic chemistry