DECONTAMINATION OF ZIRCALOY SPENT FUEL CLADDING HULLS

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The reprocessing of commercial spent nuclear fuel (SNF) generates a Zircaloy cladding hull waste which requires disposal as a high level waste in the geologic repository. The hulls are primarily contaminated with fission products and actinides from the fuel. During fuel irradiation, these contaminants are deposited in a thin layer of zirconium oxide (ZrO{sub 2}) which forms on the cladding surface at the elevated temperatures present in a nuclear reactor. Therefore, if the hulls are treated to remove the ZrO{sub 2} layer, a majority of the contamination will be removed and the hulls could potentially meet acceptance criteria for disposal ... continued below

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Rudisill, T & John Mickalonis, J September 27, 2006.

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The reprocessing of commercial spent nuclear fuel (SNF) generates a Zircaloy cladding hull waste which requires disposal as a high level waste in the geologic repository. The hulls are primarily contaminated with fission products and actinides from the fuel. During fuel irradiation, these contaminants are deposited in a thin layer of zirconium oxide (ZrO{sub 2}) which forms on the cladding surface at the elevated temperatures present in a nuclear reactor. Therefore, if the hulls are treated to remove the ZrO{sub 2} layer, a majority of the contamination will be removed and the hulls could potentially meet acceptance criteria for disposal as a low level waste (LLW). Discard of the hulls as a LLW would result in significant savings due to the high costs associated with geologic disposal. To assess the feasibility of decontaminating spent fuel cladding hulls, two treatment processes developed for dissolving fuels containing zirconium (Zr) metal or alloys were evaluated. Small-scale dissolution experiments were performed using the ZIRFLEX process which employs a boiling ammonium fluoride (NH{sub 4}F)/ammonium nitrate (NH{sub 4}NO{sub 3}) solution to dissolve Zr or Zircaloy cladding and a hydrofluoric acid (HF) process developed for complete dissolution of Zr-containing fuels. The feasibility experiments were performed using Zircaloy-4 metal coupons which were electrochemically oxidized to produce a thin ZrO{sub 2} layer on the surface. Once the oxide layer was in place, the ease of removing the layer using methods based on the two processes was evaluated. The ZIRFLEX and HF dissolution processes were both successful in removing a 0.2 mm (thick) oxide layer from Zircaloy-4 coupons. Although the ZIRFLEX process was effective in removing the oxide layer, two potential shortcomings were identified. The formation of ammonium hexafluorozirconate ((NH{sub 4}){sub 2}ZrF{sub 6}) on the metal surface prior to dissolution in the bulk solution could hinder the decontamination process by obstructing the removal of contamination. The thermal decomposition of this material is also undesirable if the cladding hulls are melted for volume reduction or to produce waste forms. Handling and disposal of the corrosive off-gas stream and ZrO{sub 2}-containing dross must be addressed. The stability of Zr{sup 4+} in the NHF{sub 4}/NH{sub 4}NO{sub 3} solution is also a concern. Precipitation of ammonium zirconium fluorides upon cooling of the dissolving solution was observed in the feasibility experiments. Precipitation of the solids was attributed to the high fluoride to Zr ratios used in the experiments. The solubility of Zr{sup 4+} in NH{sub 4}F solutions decreases as the free fluoride concentration increases. The removal of the ZrO{sub 2} layer from Zircaloy-4 coupons with HF showed a strong dependence on both the concentration and temperature. Very rapid dissolution of the oxide layer and significant amounts of metal was observed in experiments using HF concentrations {ge} 2.5 M. Treatment of the coupons using HF concentrations {le} 1.0 M was very effective in removing the oxide layer. The most effective conditions resulted in dissolution rates which were less than approximately 2 mg/cm{sup 2}-min. With dissolution rates in this range, uniform removal of the oxide layer was obtained and a minimal amount of Zircaloy metal was dissolved. Future HF dissolution studies should focus on the decontamination of actual spent fuel cladding hulls to determine if the treated hulls meet criteria for disposal as a LLW.

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  • Report No.: WSRC-TR-2006-00321
  • Grant Number: DE-AC09-08SR22470
  • DOI: 10.2172/939424 | External Link
  • Office of Scientific & Technical Information Report Number: 939424
  • Archival Resource Key: ark:/67531/metadc898397

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  • September 27, 2006

Added to The UNT Digital Library

  • Sept. 27, 2016, 1:39 a.m.

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  • Dec. 12, 2016, 6:28 p.m.

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Rudisill, T & John Mickalonis, J. DECONTAMINATION OF ZIRCALOY SPENT FUEL CLADDING HULLS, report, September 27, 2006; [Aiken, South Carolina]. (digital.library.unt.edu/ark:/67531/metadc898397/: accessed December 13, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.