Radiochemical methodologies applied to determination of zirconium isotopes in low-level waste samples from nuclear power plants

Oliveira, Thiago C.; Monteiro, Roberto Pellacani Guedes; Kastner, Geraldo Frederico; Bessueille-Barbier, Frédérique; Oliveira, Arno Heeren de

doi:10.1007/s10967-014-3283-y

Cited by 8 publications

(6 citation statements)

References 6 publications

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“…Determination of zirconium concentration and isotope abundance is important for different applications such as life science [1], geology [2][3][4][5][6], environment [7], forensics [8] or nuclear field [9][10][11][12][13]. In nuclear applications, zirconium is used as a construction material in nuclear reactors [14] and is a fission product: the radioactive 93 Zr isotope is produced mainly by nuclear fission of uranium-235 in nuclear fuel.…”

Section: Introductionmentioning

confidence: 99%

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Quemet

Maillard

Ruas

2015

International Journal of Mass Spectrometry

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A new Thermal Ionization Mass Spectrometer (TIMS) analytical procedure was developed to measure with high accuracy the zirconium isotope abundance and concentration without molybdenum correction in nuclear samples. A zirconium selective separation using UTEVA column was used before the TIMS measurement in order to remove all possible isobaric interferences (Mo, Y, Nb and Ru) in the solution. The separated solution was then deposited onto a filament previously outgassed for 4 hours to reduce the molybdenum traces in the filament. Then, the filament was introduced into the TIMS source and was maintained for 4 hours at a current of 5 A (ionization filament) and 1.2 A (evaporation filament) in order to eliminate all molybdenum trace present in the filament and in the sample. This methodology allowed the zirconium isotope abundance determination without using the molybdenum interference correction equation. The analytical results obtained with a natural solution after separation is in good accordance with the reference values: bias lower than 0.16 % for the 90 Zr, 91 Zr, 92 Zr and 94 Zr isotope abundance, and a bias of ~0.8 % for the minor isotope (96 Zr) were observed. This zirconium abundance determination methodology was used on three nuclear samples. Then, the calibration of a 91 Zr spike solution was performed by reverse isotope dilution using a SPEX standard zirconium solution. The zirconium concentration determination was then performed on the three nuclear samples by isotope dilution using the SPEX standard zirconium solution and the 91 Zr spike solution. The final uncertainties were estimated to be lower than 1 %.

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Section: Introductionmentioning

confidence: 99%

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Quemet

Maillard

Ruas

2015

International Journal of Mass Spectrometry

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“…Oliveira et al [13,14] tested a procedure combining ion exchange chromatography on Dowex resin, liquid-liquid extraction using TTA and extraction chromatography on TRU resin (which contains octylphenyl N,N'-di-isobutyl carbamoyl phosphine oxide, CMPO and TBP, manufactured by TrisKem International). Sample was loaded onto Dowex ion exchange column in 9 M HNO3 and column was washed with 9 M HNO3, then the liquid-liquid extraction developed by Espartero at al.…”

Section: Separation Methods Of 93 Zrmentioning

confidence: 99%

“…When using LSC, standard solution of 63 Ni is typically used for calibration, i. e. for optimization of the energy window and for determination of detection efficiency, as 63 Ni is a β --emitter with Eβ,max (66 keV) similar to that of 93 Zr [7,9,14,20]. When using ICP-MS, standard solution of natural Zr (containing 92 Zr and 94 Zr) is typically used for calibration and calculation of the detection limits.…”

Section: Measurement Techniques Of 93 Zrmentioning

confidence: 99%

“…When using ICP-MS, standard solution of natural Zr (containing 92 Zr and 94 Zr) is typically used for calibration and calculation of the detection limits. Natural Nb ( 93 Nb) can be used as well, as ionization energies of Zr (6.63 eV) and 93 Nb (6.76 eV) are similar [14].…”

Section: Measurement Techniques Of 93 Zrmentioning

confidence: 99%

“…When measuring it by LSC, complete separation from β-emitting and X-ray emitting radionuclides (e.g. 3 H, 14 C, 54 Mn, 55 Fe, 60 Co, 63 Ni, 65 Zn, 90 Sr, 90 Y, 93m Nb, 94 Nb, 93 Mo, 133 Ba, 137 Cs, 152 Eu, 239 Np, 241 Pu) is necessary [4]. When measuring it by ICP-MS, isobaric ( 93 Nb, 93m Nb and 93 Mo) and polyatomic (e.g., 92 Zr 1 H) interferences as well as abundance sensitivity affect the results [5,6].…”

Section: Introductionmentioning

confidence: 99%

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Determination of 93Zr in nuclear power plant wastes

Osváth

Vajda²,

Molnár³

et al. 2017

J Radioanal Nucl Chem

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Interference-free determination of sub ng kg−1 levels of long-lived 93Zr in the presence of high concentrations (μg kg−1) of 93Mo and 93Nb using ICP-MS/MS

Petrov¹,

Russell

Douglas³

et al. 2017

Anal Bioanal Chem

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Long-lived high abundance radionuclides are of increasing interest with regard to decommissioning of nuclear sites and longer term nuclear waste storage and disposal. In many cases, no routine technique is available for their measurement in nuclear waste and low-level (ng kg) environmental samples. Recent advances in ICP-MS technology offer attractive features for the selective and sensitive determination of a wide range of long-lived radionuclides. In this work, inductively coupled plasma-tandem mass spectrometry (ICP-MS/MS)-based methodology, suitable for accurate routine determinations of Zr at very low (ng kg) levels in the presence of high levels (μg kg) of the isobaric interferents Nb andMo (often present in nuclear waste samples), is reported for the first time. Additionally, a novel and systematic strategy for method development based on the use of non-radioactive isotopes is proposed. It relies on gas-phase chemical reactions for different molecular ion formation to achieve isobaric interference removal. Using cell gas mixtures of NH/He/H or H/O, and suitable mass shifts, the signal from the Nb andMo isobaric interferences on Zr were suppressed by up to 5 orders of magnitude. The achieved limit of detection forZr was 1.3 × 10 Bq g (equivalent to 0.14 ng kg). The sample analysis time is 2 min, which represents a significant improvement in terms of sample throughput, compared to liquid scintillation counting methods. The method described here can be used for routine measurements of Zr at environmentally relevant levels. It can also be combined with radiometric techniques for use towards the standardisation ofZr measurements. Graphical abstract Interference-free determination of Zr in the presence of high concentrations of isobaricMo and Nb by ICP-MS/MS.

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Radiochemical methodologies applied to determination of zirconium isotopes in low-level waste samples from nuclear power plants

Cited by 8 publications

References 6 publications

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Determination of 93Zr in nuclear power plant wastes

Interference-free determination of sub ng kg−1 levels of long-lived 93Zr in the presence of high concentrations (μg kg−1) of 93Mo and 93Nb using ICP-MS/MS

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