Spectroscopic Monitoring of Spent Nuclear Fuel Reprocessing Streams: An Evaluation of Spent Fuel Solutions via Raman, Visible, and Near-Infrared Spectroscopy

Journal Article · Thu Sep 01 04:00:00 EDT 2011 · Radiochimica Acta, 99(9):563-571

DOI:https://doi.org/10.1524/ract.2011.1865· OSTI ID:1023722

Bryan, Samuel A; Levitskaia, Tatiana G; Johnsen, Amanda M; Orton, Christopher R; Peterson, James M

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. Availability of on-line real-time techniques that directly measure process concentrations of nuclear materials will enhance 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 report reviews current state of development of the spectroscopic on-line monitoring techniques for such solutions. To further examine applicability of optical spectroscopy for monitoring reprocessing solutions, segments of a spent nuclear fuel, with approximate burn-up values of 70 MWd/kgM, 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/dodecane organic solvent. The feed and equilibrium aqueous and loaded organic solutions were subjected to optical measurements. The obtained spectra showed the presence of the quantifiable Raman bands due to NO3- and UO22+ 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, justifying spectroscopic techniques as a promising methodology for monitoring spent fuel processing solutions in real-time. Quantitative evaluation of the fuel solution was performed based on spectroscopic measurements and compared to ICP-MS analysis.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1023722
• Report Number(s): PNNL-SA-75142; AF5805000
• Journal Information: Radiochimica Acta, 99(9):563-571, Journal Name: Radiochimica Acta, 99(9):563-571 Journal Issue: 9 Vol. 99; ISSN RAACAP; ISSN 0033-8230
• Country of Publication: United States
• Language: English

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
AQUEOUS SOLUTIONS
COMPARATIVE EVALUATIONS
EQUILIBRIUM
EVALUATION
FUEL REPROCESSING PLANTS
FUEL SOLUTIONS
INFRARED SPECTRA
MONITORING
NEODYMIUM COMPLEXES
NEPTUNIUM COMPLEXES
NITRIC ACID
NUCLEAR FUELS
NUCLEAR MATERIALS MANAGEMENT
ON-LINE SYSTEMS
ORGANIC SOLVENTS
PERFORMANCE
PLUTONIUM COMPLEXES
PROCESS CONTROL
PROCESSING
PROLIFERATION
RAMAN SPECTROSCOPY
REPROCESSING
REVIEWS
SAFETY
SOLUTIONS
SOLVENT EXTRACTION
SPECTRA
SPECTROSCOPY
SPENT FUELS
VISIBLE SPECTRA
commercial nuclear fuel, process monitoring, Raman, visible, and near-infrared spectroscopy
quantitative measurement of uranium, neptunium, and plutonium.