Author: Campbell, K. R.

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2 articles found

Phase discrimination of uranium oxides using laser-induced breakdown spectroscopy

Author: Campbell, K. R. ; et. al.

Journal: Spectrochimica Acta Part B: Atomic Spectroscopy (2017)

DOI: 10.1016/j.sab.2017.05.007

Authors
Barefield, J. E. ; Clegg, S. M. ; Colgan, J. P. ; Czerwinski, K. R. L. ; Judge, E. J. ; Kilcrease, D. P. ; Wilkerson, M. P. ; Wozniak, N. R.

Keywords

Laser-induced breakdown spectroscopy; Uranium; Phase identification;EMISSION; FEMTOSECOND; STRENGTHS; SPECTRA; PLASMA; LIBS

Abstract

Nuclear forensics goals for characterizing samples of interest include qualitative and quantitative analysis of major and trace elements, isotopic analysis, phase identification, and physical analysis. These samples may include uranium oxides UO2, U3O8, and UO3, which play an important role in the front end of the nuclear fuel cycle, from mining to fuel fabrication. The focus of this study is to compare the ratios of the intensities of uranium and oxygen emission lines which can be used to distinguish between different uranium oxide materials using Laser-Induced Breakdown Spectroscopy (LIBS). Measurements at varying laser powers were made under an argon atmosphere at 585 Torr to ensure the oxygen emission intensity was originating from the sample, and not from the atmosphere. Fifteen uranium emission lines were used to compare experimental results with theoretical calculations in order to determine the plasma conditions. Using a laser energy of 26 mJ, the uranium lines 591.539 and 682.692 nm provide the highest degree of discrimination between the uranium oxides. The study presented here suggests that LIBS is useful for discriminating uranium oxide phases, UO2, U3O8, and UO3. (C) 2017 Elsevier B.V. All rights reserved.

Area:

Nuclear industry

Material:

Uranium oxide

Elements:

Lines [nm]:

U II 409.01 nm U II 417.16 nm U II 424.17 nm U II 424.44 nm U I 424.63 nm U II 434.17 nm U I 435.57 nm U II 454.36 nm U I 455.20 nm U I 462.02 nm U II 462.71 nm U I 463.16 nm U I 591.54 nm U I 639.54 nm U I 682.69 nm

Lines [nm]:

O I 777.19 nm O I 777.42 nm O I 777.54 nm

Emmision lines:
U II 409.01 nm
U II 417.16 nm
U II 424.17 nm
U II 424.44 nm
U I 424.63 nm
U II 434.17 nm
U I 435.57 nm
U II 454.36 nm
U I 455.20 nm
U I 462.02 nm
U II 462.71 nm
U I 463.16 nm
U I 591.54 nm
U I 639.54 nm
U I 682.69 nm
O I 777.19 nm
O I 777.42 nm
O I 777.54 nm

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

Author: Campbell, K. R. ; et. al.

Journal: Spectrochimica Acta Part B: Atomic Spectroscopy (2017)

Applications

DOI: 10.1016/j.sab.2017.04.006

Authors
Barefield, J. E. ; Clegg, S. M. ; Colgan, J. P. ; Czerwinski, K. R. L. ; Judge, E. J. ; Kilcrease, D. P.

Keywords

Matrix effects; Laser-induced breakdown spectroscopy; Uranium; Limit of detection;URANIA; WASTE; UO2; ZR

Abstract

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 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 (R-2) >0.97 for both the binary and ternary oxides. The cerium LOD in the (U,Ce)O-2 matrix ranged from 034 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. The effect of multiple elements in the plasma and the impact on the LOD is discussed. (C) 2017 Elsevier B.V. All rights reserved.

Area:

Nuclear industry

Material:

Nuclear fuel

Elements:

Lines [nm]:

Ce II 380.81 nm Ce II 407.35 nm Ce II 447.12 nm Ce II 457.23 nm Ce II 535.35 nm Ce I 571.90 nm Ce II 395.25 nm Ce II 395.63 nm Ce II 428.94 nm Ce II 444.44 nm Ce II 448.39 nm Ce II 404.08 nm Ce II 438.22 nm Ce II 507.97 nm Ce I 581.29 nm Ce II 401.24 nm Ce II 438.68 nm Ce II 439.17 nm Ce II 452.31 nm Ce II 452.85 nm Ce II 460.64 nm Ce II 488.25 nm Ce I 512.96 nm Ce II 394.28 nm Ce II 399.38 nm Ce II 416.99 nm Ce II 435.27 nm Ce II 441.88 nm Ce II 452.74 nm Ce I 522.35 nm Ce II 540.92 nm Ce II 547.23 nm Ce I 594.09 nm

Lines [nm]:

Zr II 244.99 nm Zr II 272.26 nm Zr II 273.49 nm Zr II 274.26 nm Zr II 275.22 nm Zr II 281.87 nm Zr II 282.56 nm Zr II 284.46 nm Zr II 305.48 nm Zr II 310.66 nm Zr II 316.60 nm Zr II 327.31 nm Zr II 332.68 nm Zr II 335.61 nm Zr II 335.73 nm Zr II 338.83 nm Zr II 339.20 nm Zr II 339.31 nm Zr II 340.48 nm Zr II 341.03 nm Zr II 348.12 nm Zr II 355.66 nm Zr II 357.25 nm Zr II 357.69 nm Zr I 360.12 nm Zr II 361.31 nm Zr II 383.68 nm Zr II 444.30 nm

Lines [nm]:

U I 339.04 nm U II 339.48 nm U II 424.44 nm

Lines [nm]:

O I 777.19 nm

Lines [nm]:

Si I 288.16 nm

Emmision lines:
Zr II 244.99 nm
Zr II 272.26 nm
Zr II 273.49 nm
Zr II 274.26 nm
Zr II 275.22 nm
Zr II 281.87 nm
Zr II 282.56 nm
Zr II 284.46 nm
Si I 288.16 nm
Zr II 305.48 nm
Zr II 310.66 nm
Zr II 316.60 nm
Zr II 327.31 nm
Zr II 332.68 nm
Zr II 335.61 nm
Zr II 335.73 nm
Zr II 338.83 nm
U I 339.04 nm
Zr II 339.20 nm
Zr II 339.31 nm
U II 339.48 nm
Zr II 340.48 nm
Zr II 341.03 nm
Zr II 348.12 nm
Zr II 355.66 nm
Zr II 357.25 nm
Zr II 357.69 nm
Zr I 360.12 nm
Zr II 361.31 nm
Ce II 380.81 nm
Zr II 383.68 nm
Ce II 394.28 nm
Ce II 395.25 nm
Ce II 395.63 nm
Ce II 399.38 nm
Ce II 401.24 nm
Ce II 404.08 nm
Ce II 407.35 nm
Ce II 416.99 nm
U II 424.44 nm
Ce II 428.94 nm
Ce II 435.27 nm
Ce II 438.22 nm
Ce II 438.68 nm
Ce II 439.17 nm
Ce II 441.88 nm
Zr II 444.30 nm
Ce II 444.44 nm
Ce II 447.12 nm
Ce II 448.39 nm
Ce II 452.31 nm
Ce II 452.74 nm
Ce II 452.85 nm
Ce II 457.23 nm
Ce II 460.64 nm
Ce II 488.25 nm
Ce II 507.97 nm
Ce I 512.96 nm
Ce I 522.35 nm
Ce II 535.35 nm
Ce II 540.92 nm
Ce II 547.23 nm
Ce I 571.90 nm
Ce I 581.29 nm
Ce I 594.09 nm
O I 777.19 nm

Co-author: Campbell, K. R.

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Author: Campbell, K. R.

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Co-author: Campbell, K. R.

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