Ammonium polyuranate precipitation from fluoride solutions : an experimental study of the UO{sub 3}-HF-NH{sub 3}-H{sub 2}O system as applied in UF{sub 6} processing.
In the ammonium diuranate (ADU) process, UF{sub 6} is reacted with water, and the acidic solution of uranyl fluoride is treated with aqueous ammonia to precipitate ammonium polyuranate for subsequent reduction to UO{sub 2} and production of fuel pellets for commercial nuclear reactors. Our experiments simulated adding aqueous ammonia to the reaction products of UF{sub 6} and water in typical ADU processes. Chemical and X-ray diffraction analysis of products from the experiments are consistent with postulated chemical equilibria in which solids with structures close to that of ammonium polyuranate are formed from co-precipitation of the NH{sub 4}{sup +}(aq) cation with (previously unreported) anions of the form UO{sub 2}F{sub 3-x}(OH){sub x}{sup -}(aq). More efficient separations of solid products were obtained at NH{sub 4}OH:UF{sub 6} ratios of 19 or greater, with x closer to the value of 3 for the hypothetical formation of pure ammonium polyuranate. Supplementary experiments in the current study and a previous study in our laboratory indicated that nominal uranium concentrations of 90 mg/l in the filtrate resulting from such separations could be reduced to microgram per liter levels by batch mixing a 1-to-2.5 aqueous diluate of the filtrate with the Diphonix{reg_sign} ion exchange resin. Our study further demonstrated that reaction of the purified NH{sub 4}OH-NH{sub 4}F diluate with aqueous Ca(OH){sub 2} at 80 to 90 C could produce essentially uranium-free CaF{sub 2} and an ammonia distillate, as useful waste-conversion end products from a modified ADU process.
- Research Organization:
- Argonne National Laboratory (ANL)
- Sponsoring Organization:
- SC
- DOE Contract Number:
- AC02-06CH11357
- OSTI ID:
- 964635
- Report Number(s):
- ANL/CSE/JA-62887
- Journal Information:
- Nucl. Technol., Journal Name: Nucl. Technol. Journal Issue: 3 ; Sep. 2009 Vol. 167; ISSN 0029-5450; ISSN NUTYBB
- Country of Publication:
- United States
- Language:
- ENGLISH
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