Material Nuclear fuel

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:

Ce

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

Zr

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

U

Lines [nm]:

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

O

Lines [nm]:

O I 777.19 nm

Si

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

Analysis of simulated high burnup nuclear fuel by laser induced breakdown spectroscopy

Author: Singh, M. ; et. al.

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

Applications

DOI: 10.1016/j.sab.2017.03.012

Authors
Banerjee, J. ; Bhagat, R. K. ; Sarkar, A.

Keywords

LIBS; SIMFUEL; AHWR; Argon; Nuclear;INDUCED PLASMAS; URANIUM; THORIUM; LIBS; SPECTROMETRY; EMISSION; GLASS

Abstract

Advanced Heavy Water Reactor (AHWR) grade (Th-U)O-2 fuel sample and Simulated High Burn-Up Nuclear Fuels (SIMFUEL) samples mimicking the 28 and 43 GWd/Fe irradiated burn-up fuel were studied using laser-induced breakdown spectroscopy (LIBS) setup in a simulated hot-cell environment from a distance of >1.5 m. Resolution of <38 pm has been used to record the complex spectra of the SIMFUEL samples. By using spectrum comparison and database matching >60 emission lines of fission products was identified. Among them only a few emission lines were found to generate calibration curves. The study demonstrates the possibility to investigate impurities at concentrations around hundreds of ppm, rapidly at atmospheric pressure without any sample preparation. The results of Ba and Mo showed the advantage of LIBS analysis over traditional methods involving sample dissolution, which introduces possible elemental loss. Limits of detections (LOD) under Ar atmosphere shows significant improvement, which is shown to be due to the formation of stable plasma. (C) 2017 Elsevier B.V. All rights reserved.

Area:

Industry

Material:

Nuclear fuel

Elements:

Mo

Lines [nm]:

Mo II 253.85 nm Mo I 255.09 nm Mo II 259.37 nm Mo II 265.34 nm Mo II 266.06 nm Mo II 267.28 nm Mo II 267.33 nm Mo I 267.99 nm Mo II 268.32 nm Mo II 268.80 nm Mo II 270.14 nm Mo II 271.74 nm Mo II 274.63 nm Mo II 276.98 nm Mo II 277.54 nm Mo II 278.00 nm Mo II 281.62 nm Mo II 284.82 nm Mo II 285.32 nm Mo II 286.38 nm Mo II 287.15 nm Mo II 308.76 nm Mo II 312.20 nm Mo I 313.26 nm Mo I 320.88 nm Mo I 383.38 nm Mo I 390.30 nm Mo I 418.83 nm Mo I 470.72 nm

Zr

Lines [nm]:

Zr II 256.89 nm Zr II 257.14 nm Zr II 267.86 nm Zr II 270.01 nm Zr II 274.26 nm Zr II 274.59 nm Zr II 284.46 nm Zr II 327.31 nm Zr II 327.93 nm Zr II 328.47 nm Zr II 343.82 nm Zr I 386.39 nm Zr I 389.03 nm Zr I 468.78 nm Zr I 468.85 nm Zr I 471.01 nm Zr I 477.23 nm

Th

Lines [nm]:

Th II 254.81 nm Th II 406.92 nm Th II 420.89 nm Th I 459.54 nm Th II 486.32 nm Th II 491.98 nm Th II 513.11 nm

Ce

Lines [nm]:

Ce II 276.14 nm Ce II 322.71 nm Ce I 513.78 nm Ce I 560.13 nm Ce I 569.70 nm

Sr

Lines [nm]:

Sr II 407.77 nm Sr II 421.55 nm Sr I 460.73 nm Sr I 496.23 nm

...

Emmision lines:
Mo II 253.85 nm
Th II 254.81 nm
Mo I 255.09 nm
Zr II 256.89 nm
Zr II 257.14 nm
Mo II 259.37 nm
Ba I 264.65 nm
Mo II 265.34 nm
Mo II 266.06 nm
Mo II 267.28 nm
Mo II 267.33 nm
Zr II 267.86 nm
Mo I 267.99 nm
Mo II 268.32 nm
Mo II 268.80 nm
Zr II 270.01 nm
Mo II 270.14 nm
Mo II 271.74 nm
Zr II 274.26 nm
Zr II 274.59 nm
Mo II 274.63 nm
Ce II 276.14 nm
Mo II 276.98 nm
Mo II 277.54 nm
Mo II 278.00 nm
Mo II 281.62 nm
Zr II 284.46 nm
Mo II 284.82 nm
Mo II 285.32 nm
Mo II 286.38 nm
Mo II 287.15 nm
Ru I 290.89 nm
Mo II 308.76 nm
Mo II 312.20 nm
Mo I 313.26 nm
Mo I 320.88 nm
Ce II 322.71 nm
Zr II 327.31 nm
Zr II 327.93 nm
Zr II 328.47 nm
Zr II 343.82 nm
Mo I 383.38 nm
Zr I 386.39 nm
Zr I 389.03 nm
Mo I 390.30 nm
Th II 406.92 nm
Sr II 407.77 nm
Mo I 418.83 nm
Th II 420.89 nm
Sr II 421.55 nm
Nd II 423.24 nm
Ba II 455.40 nm
Th I 459.54 nm
Sr I 460.73 nm
Y I 467.49 nm
Zr I 468.78 nm
Zr I 468.85 nm
Mo I 470.72 nm
Zr I 471.01 nm
Sm I 476.03 nm
Zr I 477.23 nm
Th II 486.32 nm
Nd I 488.38 nm
Y II 490.01 nm
Th II 491.98 nm
Ba II 493.41 nm
Nd I 494.48 nm
Sr I 496.23 nm
Th II 513.11 nm
Ce I 513.78 nm
Ce I 560.13 nm
Ce I 569.70 nm

Short Communication on ""Direct compositional quantification of (U-Th)O-2 - MOX nuclear fuel using ns-UV-LIBS and chemometric regression models""

Author: Singh, M. ; et. al.

Journal: Journal of Nuclear Materials (2017)

Applications Chemometrics

DOI: 10.1016/j.jnucmat.2016.11.025

Authors
Mao, X. L. ; Russo, R. E. ; Sarkar, A.

Keywords

LIBS; Chemometrics; PLSR; Nuclear fuel; AHWR;INDUCED BREAKDOWN SPECTROSCOPY; NANOSECOND 266 NM; WAVELENGTH DEPENDENCE; GLASS; THORIUM; URANIUM; SPECTROMETRY

Abstract

The determination of uranium with composition varying from 0% to 35 wt% in (Th-U)O-2 mixed oxide fuel using laser induced breakdown spectroscopy (LIBS) utilizing partial least square regression (PLSR) has been demonstrated. Good agreement between expected and experiment results using 266 nm, 532 nm and 1064 nm was shown. The analytical results at 266 nm of 2-3% precision and similar to 1% accuracy (bias) satisfy the acceptance criteria range for chemical analysis in the nuclear industry. (C) 2016 ElseVier B.V. All rights reserved.

Area:

Nuclear industry

Material:

Nuclear fuel ; Uranium oxide

Elements:

U

Lines [nm]:

U II 367.01 nm U II 447.23 nm

Emmision lines:
U II 367.01 nm
U II 447.23 nm

The effect of ambient gas on measurements with microwave-assisted laser-induced plasmas in MA-LIBS with relevance for the analysis of nuclear fuel

Author: Khumaeni, A. ; et. al.

Journal: Journal of Radioanalytical and Nuclear Chemistry (2017)

Applications

DOI: 10.1007/s10967-016-5020-1

Authors
Akaoka, K. ; Miyabe, M. ; Wakaida, I.

Keywords

Laser-induced breakdown spectroscopy (LIBS); Microwave-assisted laser-induced breakdown spectroscopy (MA-LIBS); Effect of ambient gas; Analysis of Ca impurity in Gd2O3;INDUCED BREAKDOWN SPECTROSCOPY; ATOMIC EMISSION-SPECTROMETRY; URANIUM; ENHANCEMENT; IMPURITIES; EXTRACTION; ABLATION

Abstract

The effect of ambient gas on measurements with microwave-assisted laser-induced plasma in microwave-assisted laser-induced breakdown spectroscopy(MA-LIBS) was studied with relevance for the analysis of nuclear fuel. A pelletized gadolinium oxide (Gd2O3) sample, which was used as a simulated nuclear fuel, was irradiated by a pulsed Nd:YAG laser (532 nm, 5 mJ) coupled with microwaves (2.45 GHz, 400 W) under various gases of air, Ar, and He. Microwaves can be effectively used to enhance laser-induced plasma emissions. The emission spectrums of Gd obtained by MA-LIBS in Ar and He gases are much better than those of the air case. Namely, the spectral lines can be clearly identified and are far from molecular bands. Furthermore, the emission intensity is highest with low background emissions. Linear calibration curves of Ca in the concentration range between 0 and 500 mg/kg as an impurity in Gd2O3 have been successfully obtained in all gases. The detection limits of Ca impurity in air, Ar and He gases were 2, 0.8 and 0.6 mg/kg, respectively, which are much lower than the required limits of Ca impurity in nuclear fuels.

Area:

Nuclear industry

Material:

Gadolinium oxide ; Nuclear fuel

Elements:

Gd

Lines [nm]:

Gd I 422.59 nm Gd II 342.25 nm Gd II 391.65 nm

Ca

Lines [nm]:

Ca II 393.37 nm

Emmision lines:
Gd II 342.25 nm
Gd II 391.65 nm
Ca II 393.37 nm
Gd I 422.59 nm

Material: Nuclear fuel

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