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Neptunium redox speciation and determination of its total concentration in dissolved fuel simulant solutions by spectrophotometry

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Abstract

Two new approaches to measure Np concentration in dissolved used nuclear fuel simulant (aqueous feed for PUREX process) by spectrophotometry are developed. The first approach is based on chemical reduction of Np in the feed to its tetravalent state using ascorbic acid with simultaneous conversion of Pu(IV) to Pu(III). Interfering effects from light absorbing fission and corrosion products are accounted for by measuring optical absorbance spectrum of aqueous raffinate after extraction of U, Np, and Pu by tributyl phosphate in dodecane. The second approach uses no chemical treatment at all and relies on spontaneous valency adjustment of Np to Np(V) by dilution of the feed with water to reduce its acidity to low decimolar range of nitric acid concentration. Results of Np determination in the feed by spectrophotometry are in good agreement with its concentration measured by ICP-MS.

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Acknowledgements

This work was funded by the U.S. Department of Energy’s Office of Nuclear Energy, through the Nuclear Technologies Research and Development Program. Pacific Northwest National Laboratory is operated by Battelle Memorial Institute for the U.S. Department of Energy under contract DE-AC05-76RL01830.

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Correspondence to Sergey I. Sinkov.

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Sinkov, S.I., Hall, G.B., Heller, F.D. et al. Neptunium redox speciation and determination of its total concentration in dissolved fuel simulant solutions by spectrophotometry. J Radioanal Nucl Chem 331, 5579–5595 (2022). https://doi.org/10.1007/s10967-022-08665-8

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