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The interaction of iodine with insoluble residue in the dissolution of simulated spent-fuel pellets

Journal Article · · Nuclear Technology; (United States)
OSTI ID:5649949
; ; ;  [1]
  1. Japan Atomic Energy Research Inst., Physical Chemistry Lab., Tokai-mura, Ibaraki-ken 319-11 (JP)
To properly control radioiodine ({sup 129}I) when reprocessing nuclear fuels, it is important to understand the interaction between iodine and the insoluble residue produced during the dissolution of spent fuels. Simulated spent-fuel pellets ({approximately} 1 g each) equivalent to spent fuel with a burnup of 5% fima were dissolved in 4.1 M HNO{sub 3} or a simulated spent-fuel solution to examine this interaction and the material balance of iodine. In dissolution in 4.1 M HNO{sub 3}, 2 to 5% of the iodine in the pellet is conveyed to the insoluble residue (8 {plus minus} 1 mg), 1 to 5% remains in solution, and the balance volatilizes into the off-gas. The process that incorporates iodine into the residue is the formation of slightly soluble iodides, such as PdI{sub 2} and AgI, on the surface of the residue. The quantity of iodine in the residue averages 1.1 {plus minus} 0.5 Mg I/mg of residue. Pellet dissolution in simulated spent-fuel solutions with a uranium concentration of {ge}170 g U/{ell} and corresponding amounts of fission product elements causes a marked increase in the amount of residue and a significant increase in the amount of iodine involved. This phenomenon is due to the secondary precipitation of some metal molybdates. The PdI{sub 2} and AgI in the residue are in equilibrium with Pd{sup 2+}, Ag{sup +}, and I{sup {minus}} in the solution. The I{sup {minus}} can be oxidized into I{sub 2} in a hot nitric acid solution bubbled with NO{sub 2}. The action of NO{sub 2} causes part of the iodine in the residue to be eluted into the solution and then volatilized into the off-gas during the operation to expel iodine (IO{sup {minus}}{sup 3}) form the solution. A process consisting of (a) heating of the residue in a IO{sup {minus}}{sub 3}-concentrated HNO{sub 3} at 100{degrees} C will transfer 50 to 90% of the iodine in the residue to the gas phase. The remaining iodine is probably inside the residue as it is difficult to remove.
OSTI ID:
5649949
Journal Information:
Nuclear Technology; (United States), Journal Name: Nuclear Technology; (United States) Vol. 94:1; ISSN NUTYB; ISSN 0029-5450
Country of Publication:
United States
Language:
English