Spectroscopic monitoring of spent nuclear fuel reprocessing streams: An evaluation of spent fuel solutions via Raman, visible, and near-infrared spectroscopy

S. A. Bryan, T. G. Levitskaia, A. M. Johnsen, C. R. Orton, J. M. Peterson

Research output: Contribution to journalArticlepeer-review

48 Scopus citations

Abstract

The potential of using optical spectroscopic techniques, such as Raman and visible/near infrared (Vis/NIR), for on-line process control and special nuclear materials accountability applications at a spent nuclear fuel reprocessing facility was evaluated. The availability of on-line, real-time techniques that directly measure process concentrations of nuclear materials will enhance the performance and proliferation resistance of the solvent extraction processes. Further, on-line monitoring of radiochemical streams will also improve reprocessing plant operation and safety. This paper reviews the current state of development of the spectroscopic on-line monitoring techniques for such solutions. To further examine the applicability of optical spectroscopy for this application, segments of a spent nuclear fuel, with approximate burn-up values of 70MWd/kg M, were dissolved in concentrated nitric acid and adjusted to varying final concentrations of HNO3- The resulting spent fuel solutions were batch-contacted with tributyl phosphate/n-dodecane organic solvent. The feed and equilibrium aqueous and loaded organic solutions were subjected to optical measurements. The obtained spectra showed the presence of quantifiable Raman bands due to NO3- and UO 22+ and Vis/NIR bands due to multiple species of Pu(IV), Pu(VI), Np(V), the Np(V)-U(VI) cation-cation complex, and Nd(III) in fuel solutions. This result justifies spectroscopic techniques as a promising methodology for monitoring spent fuel processing solutions in real-time. The fuel solution was quantitatively evaluated based on spectroscopic measurements and was compared to inductively coupled plasma-mass spectroscopy analysis and Oak Ridge Isotope Generator (ORIGEN)-based estimates.

Original languageEnglish (US)
Pages (from-to)563-571
Number of pages9
JournalRadiochimica Acta
Volume99
Issue number9
DOIs
StatePublished - Sep 2011

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry

Fingerprint Dive into the research topics of 'Spectroscopic monitoring of spent nuclear fuel reprocessing streams: An evaluation of spent fuel solutions via Raman, visible, and near-infrared spectroscopy'. Together they form a unique fingerprint.

Cite this