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Title: Laser-induced breakdown spectroscopy of light water reactor simulated used nuclear fuel: Main oxide phase

We show the analysis of light water reactor simulated used nuclear fuel using laser-induced breakdown spectroscopy (LIBS) is explored using a simplified version of the main oxide phase. The main oxide phase consists of the actinides, lanthanides, and zirconium. The purpose of this study is to develop a rapid, quantitative technique for measuring zirconium in a uranium dioxide matrix without the need to dissolve the material. A second set of materials including cerium oxide is also analyzed to determine precision and limit of detection (LOD) using LIBS in a complex matrix. Two types of samples are used in this study: binary and ternary oxide pellets. The ternary oxide, (U,Zr,Ce)O 2 pellets used in this study are a simplified version the main oxide phase of used nuclear fuel. The binary oxides, (U,Ce)O 2 and (U,Zr)O 2 are also examined to determine spectral emission lines for Ce and Zr, potential spectral interferences with uranium and baseline LOD values for Ce and Zr in a UO 2 matrix. In the spectral range of 200 to 800 nm, 33 cerium lines and 25 zirconium lines were identified and shown to have linear correlation values (R 2) > 0.97 for both the binary and ternarymore » oxides. The cerium LOD in the (U,Ce)O 2 matrix ranged from 0.34 to 1.08 wt% and 0.94 to 1.22 wt% in (U,Ce,Zr)O 2 for 33 of Ce emission lines. The zirconium limit of detection in the (U,Zr)O 2 matrix ranged from 0.84 to 1.15 wt% and 0.99 to 1.10 wt% in (U,Ce,Zr)O 2 for 25 Zr lines. Finally, the effect of multiple elements in the plasma and the impact on the LOD is discussed.« less
Authors:
 [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [2] ; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Nevada, Las Vegas, NV (United States)
Publication Date:
Report Number(s):
LA-UR-16-29410
Journal ID: ISSN 0584-8547
Grant/Contract Number:
AC52-06NA25396; NA0000979
Type:
Accepted Manuscript
Journal Name:
Spectrochimica Acta. Part B, Atomic Spectroscopy
Additional Journal Information:
Journal Volume: 133; Journal Issue: C; Journal ID: ISSN 0584-8547
Publisher:
Elsevier
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 36 MATERIALS SCIENCE; Matrix effects; Laser-induced breakdown spectroscopy; Uranium; Limit of detection
OSTI Identifier:
1356143

Campbell, Keri R., Judge, Elizabeth J., Barefield, James E., Colgan, James Patrick, Kilcrease, David Parker, Czerwinski, Ken R., and Clegg, Samuel M.. Laser-induced breakdown spectroscopy of light water reactor simulated used nuclear fuel: Main oxide phase. United States: N. p., Web. doi:10.1016/j.sab.2017.04.006.
Campbell, Keri R., Judge, Elizabeth J., Barefield, James E., Colgan, James Patrick, Kilcrease, David Parker, Czerwinski, Ken R., & Clegg, Samuel M.. Laser-induced breakdown spectroscopy of light water reactor simulated used nuclear fuel: Main oxide phase. United States. doi:10.1016/j.sab.2017.04.006.
Campbell, Keri R., Judge, Elizabeth J., Barefield, James E., Colgan, James Patrick, Kilcrease, David Parker, Czerwinski, Ken R., and Clegg, Samuel M.. 2017. "Laser-induced breakdown spectroscopy of light water reactor simulated used nuclear fuel: Main oxide phase". United States. doi:10.1016/j.sab.2017.04.006. https://www.osti.gov/servlets/purl/1356143.
@article{osti_1356143,
title = {Laser-induced breakdown spectroscopy of light water reactor simulated used nuclear fuel: Main oxide phase},
author = {Campbell, Keri R. and Judge, Elizabeth J. and Barefield, James E. and Colgan, James Patrick and Kilcrease, David Parker and Czerwinski, Ken R. and Clegg, Samuel M.},
abstractNote = {We show the analysis of light water reactor simulated used nuclear fuel using laser-induced breakdown spectroscopy (LIBS) is explored using a simplified version of the main oxide phase. The main oxide phase consists of the actinides, lanthanides, and zirconium. The purpose of this study is to develop a rapid, quantitative technique for measuring zirconium in a uranium dioxide matrix without the need to dissolve the material. A second set of materials including cerium oxide is also analyzed to determine precision and limit of detection (LOD) using LIBS in a complex matrix. Two types of samples are used in this study: binary and ternary oxide pellets. The ternary oxide, (U,Zr,Ce)O2 pellets used in this study are a simplified version the main oxide phase of used nuclear fuel. The binary oxides, (U,Ce)O2 and (U,Zr)O2 are also examined to determine spectral emission lines for Ce and Zr, potential spectral interferences with uranium and baseline LOD values for Ce and Zr in a UO2 matrix. In the spectral range of 200 to 800 nm, 33 cerium lines and 25 zirconium lines were identified and shown to have linear correlation values (R2) > 0.97 for both the binary and ternary oxides. The cerium LOD in the (U,Ce)O2 matrix ranged from 0.34 to 1.08 wt% and 0.94 to 1.22 wt% in (U,Ce,Zr)O2 for 33 of Ce emission lines. The zirconium limit of detection in the (U,Zr)O2 matrix ranged from 0.84 to 1.15 wt% and 0.99 to 1.10 wt% in (U,Ce,Zr)O2 for 25 Zr lines. Finally, the effect of multiple elements in the plasma and the impact on the LOD is discussed.},
doi = {10.1016/j.sab.2017.04.006},
journal = {Spectrochimica Acta. Part B, Atomic Spectroscopy},
number = C,
volume = 133,
place = {United States},
year = {2017},
month = {4}
}