1977Unpublished venueOpen access

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

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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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What this paper is about

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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Available 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.

Key concepts: Nitric acid, Dissolution, Cerium, Ruthenium, Chemistry, Ozone, Permanganate, Inorganic chemistry

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