Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Near-infrared spectra and molar absorption coefficients of trivalent lanthanides dissolved in molten LiCl–KCl eutectic

Journal Article · · Progress in Nuclear Energy
 [1];  [2]
  1. Univ. of Nevada, Reno, NV (United States); OSTI
  2. Univ. of Nevada, Reno, NV (United States)
Determining the concentration of the dissolved lanthanide species in LiCl–KCl eutectic salt is important to the development of pyrochemical reprocessing of used nuclear fuel. In this process, lanthanide fission products are found dissolved in the electrorefiner electrolyte in their trivalent oxidation state. The presence of dissolved trivalent lanthanides increases the liquidus temperature of the electrolyte mixture and can lead to the formation of insoluble oxide or oxychloride phases and must therefore be continuously monitored and controlled during the operation. Absorbance spectroscopy is a promising method for continuous measurement of the concentration of lanthanides and other elements dissolved in the electrolyte. The absorption of light by elements is linearly proportional to the concentration of the element for relatively dilute solutions according to the Beer-Lambert law. Although measurement of the absorption of ultraviolet and visible range light by lanthanides in LiCl–KCl eutectic molten salt have been explored previously, near infrared (NIR) absorption spectroscopy has received far less attention. It may, however, provide a better analytical signal when insoluble phases are present due to less Raleigh scattering compared to shorter wavelength radiation. Additionally, it may allow for concentration determination for certain elements using NIR absorption features where UV and visible range features are overlapping with features from other species. In this study, we report the UV–Vis–NIR spectra of the trivalent lanthanide chlorides of neodymium, samarium, and dysprosium in LiCl–KCl eutectic. Molar absorption coefficients are reported for analytically useful absorption maxima, with a focus on the molar absorption coefficients for NIR absorption maxima which have not been reported previously. Additionally, we observe a NIR-range absorption band of Nd3+ which was previously predicted but never experimentally observed. Here, we compare the calculated crystal field levels to the newly observed absorbance band and find them to be in good agreement with previous predictions.
Research Organization:
Univ. of Nevada, Reno, NV (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Nuclear Energy (NE); USNRC
Grant/Contract Number:
NE0008889
OSTI ID:
2418345
Alternate ID(s):
OSTI ID: 1884356
Journal Information:
Progress in Nuclear Energy, Journal Name: Progress in Nuclear Energy Journal Issue: C Vol. 152; ISSN 0149-1970
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (26)

The Bouguer‐Beer‐Lambert Law: Shining Light on the Obscure journal August 2020
A MATLAB™ code to perform weighted linear regression with (correlated or uncorrelated) errors in bivariate data journal April 2011
Development of pyroprocessing technology journal January 1997
Application of the pyrochemical process to recycle of actinides from LWR spent fuel journal January 1997
The optical absorption and emission spectra of Cs2NaSmCl6 journal June 1981
Hypersensitivity in the electronic transitions of lanthanide and actinide complexes journal February 1976
Electronic absorption spectra of lanthanides in a molten chloride journal March 2003
Electronic absorption spectra of lanthanides in a molten chloride journal August 2007
Optical absorption and fluorescence properties of trivalent lanthanide chlorides in high temperature molten LiCl–KCl eutectic journal October 2016
Optical and NIR luminescence spectral studies: Nd3+-doped borosilicate glasses journal September 2019
Thermal analysis of projected molten salt compositions during FFTF and EBR-II used nuclear fuel processing journal July 2019
Temperature dependence of the f←f hypersensitive transitions of Ho3+ and Nd3+ in molten salt solvents and the structure of the LaCl3–KCl melts journal January 2006
A review of separation processes proposed for advanced fuel cycles based on technology readiness level assessments journal November 2019
Optical absorption and near infrared emissions of Nd3+ doped fluorophosphate glass journal December 2012
Absorption Spectra of the Lanthanides in Fused Lithium Chloride-Potassium Chloride Eutectic journal August 1961
Absorption spectroscopy for the quantitative prediction of lanthanide concentrations in the 3LiCl–2CsCl eutectic at 723 K journal January 2016
Luminescence and excitation spectra of Nd3+ in Cs2NaGdCl6 : NdCl 3? 6 journal January 1991
Charge-transfer spectra and some related phenomena journal January 1954
Spectral Intensities of the Trivalent Lanthanides and Actinides in Solution. II. Pm 3+ , Sm 3+ , Eu 3+ , Gd 3+ , Tb 3+ , Dy 3+ , and Ho 3+ journal November 1968
Electronic Energy Levels in the Trivalent Lanthanide Aquo Ions. I. Pr 3+ , Nd 3+ , Pm 3+ , Sm 3+ , Dy 3+ , Ho 3+ , Er 3+ , and Tm 3+ journal November 1968
Optical spectra and crystal field analysis of Dy3+ in Cs2NaDyCl6 and Cs2NaYCl6: Dy3+(5 mol %) journal February 1985
Optical spectra and crystal field analysis of Nd3+ in the cubic Cs2NaYCl6 host journal January 1985
Design and performance of high-temperature furnace and cell holder for in situ spectroscopic, electrochemical, and radiolytic investigations of molten salts journal August 2020
Unified equations for the slope, intercept, and standard errors of the best straight line journal March 2004
Development of Pyroprocessing and its Future Direction journal April 2008
Pyroprocessing Flowsheets for Recycling used Nuclear fuel journal August 2011