Spatial distribution of uranium isotopes in solid nuclear materials using laser ablation multi-collector ICP-MS

Krachler, Michael; Varga, Zsolt; Nicholl, Adrian; Wallenius, Maria; Mayer, Klaus

doi:10.1016/j.microc.2018.03.038

Cited by 39 publications

(38 citation statements)

References 20 publications

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“…Traditional isotopic measurements are conducted using acid digestion followed by ion exchange chromatography, which can take weeks to complete [17]. Recent advances in MC-ICP-MS instrumentation combined with laser ablation technology have provided the ability to obtain accurate chemical (e.g., [51]) and isotopic results within days (e.g., [66]).…”

Section: Discussionmentioning

confidence: 99%

The Role of Continental Crust in the Formation of Uraninite-Based Ore Deposits

et al. 2020

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This study reports trace element abundances and Pb, Sr, and U isotopic signatures of uraninite from a variety of ore deposits in order to establish baseline forensic information for source attribution of raw, natural U-rich samples. Trace element concentrations, reported here, provide insights into uraninite crystal substitution mechanisms and possible crustal sources of U, including mobility of trace elements between pristine versus altered fractions. Spatially resolved laser ablation (LA) multicollector (MC) inductively coupled plasma mass spectrometry (ICP-MS) analyses were used to determine secondary 207Pb-206Pb isochron ages, and these were validated by corroborative results obtained by solution mode (SM) MC-ICP-MS for the same sample. Secondary Pb-Pb isochron ages obtained, in this study, indicate that uraninite alteration occurs shortly after ore mineralization. Initial 87Sr/86Sr values correlate in general with host craton age, and therefore suggest that uraninite ore formation is closely linked to the nature of the bedrock geology. The δ238U values are explained by invoking multiple physicochemical conditions and parameters such as temperature, nuclear field shift, oxidation, and source rock composition. The δ234U values indicate that the uraninites, investigated here, have undergone recent alteration, but the latter has not perturbed the Pb-Pb secondary isochron ages.

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Section: Discussionmentioning

confidence: 99%

The Role of Continental Crust in the Formation of Uraninite-Based Ore Deposits

et al. 2020

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“…However, Spano et al () recently demonstrated that the REE mass fractions within U ore and UOCs measured by laser ablation (LA‐) ICP‐MS are identical to those obtained via SM‐ICP‐MS. Although the former are associated with higher relative uncertainties compared to corresponding SM analyses, determination of the REE contents by LA‐ICP‐MS is a potentially powerful nuclear forensic tool (e.g., Krachler et al ). This is primarily because in situ analyses can be conducted much more quickly than SM analyses due to the ease of sample preparation.…”

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confidence: 99%

Happy Jack Uraninite: A New Reference Material for High Spatial Resolution Analysis of U‐Rich Matrices

Dorais

Simonetti

Corcoran

et al. 2019

Geostandard Geoanalytic Res

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There is currently a lack of well‐characterised matrix‐matched reference materials (RMs) for forensic analysis of U‐rich materials at high spatial resolution. This study reports a detailed characterisation of uraninite (nominally UO2+x) from the Happy Jack Mine (UT, USA). The Happy Jack uraninite can be used as a RM for the determination of rare earth element (REE) mass fractions in nuclear materials, which provide critical information for source attribution purposes. This investigation includes powder X‐ray diffraction (pXRD) data, as well as major, minor and trace element abundances determined using a variety of micro‐analytical techniques. The chemical signature of the uraninite was investigated at the macro (cm)‐scale with micro‐X‐ray fluorescence (µXRF) mapping and at high spatial resolution (tens of micrometre scale) using electron probe microanalysis (EPMA) and laser ablation‐inductively coupled plasma‐mass spectrometry (LA‐ICP‐MS) analyses. Based on EPMA results, the uraninite is characterised by homogeneous UO2 and CaO contents of 91.57 ± 1.49% m/m (2s uncertainty) and 2.70 ± 0.38% m/m (2s), respectively. Therefore, CaO abundances were used as the internal standard when conducting LA‐ICP‐MS analyses. Overall, the major element and REE compositions are homogeneous at both the centimetre and micrometre scales, allowing this material to be used as a RM for high spatial resolution analysis of U‐rich samples.

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“…Further experimental details were reported earlier. [10][11][12] The Faraday detectors of a double-focusing multi-collector inductively coupled plasma mass spectrometer (MC-ICP-MS, Nu Plasma™, NU Instruments, Wrexham, Wales, U.K.) measured the abundance of 235 U and 238 U in the ablated particle cloud. Before switching to LA, the MC-ICP-MS was tuned for sensitivity and stability of U signals in solution mode employing an aqueous 30 ng L À1 U calibration solution having natural U isotopic composition.…”

Section: Instrumentationmentioning

confidence: 99%

“…1 Nowadays, the accurate and precise determination of the elemental and/or isotopic composition of advanced crystalline materials is of utmost importance to guarantee their properties and to identify potential contaminants. [2][3][4][5][6][7][8][9][10][11][12] Classical analytical approaches employing dissolution of a fragment of such materials followed by subsequent chemical analysis are not effective because their features are captured either in thin (nm to mm thick) layers or within local hot spots. Therefore, solid sampling techniques such as Electro-Thermal Vaporisation (ETV) or Laser Ablation (LA) are employed frequently for this purpose.…”

Section: Introductionmentioning

confidence: 99%

“…7 The lateral resolution of a few mm enables identifying potential inhomogeneity within a sample, with extended line scan analysis providing results reecting bulk analysis. 11,12 In addition, depth proling capabilities of LA provide sub-mm depth resolution. 4,[6][7][8] Despite all of its advantages, LA-ICP-MS suffers from some important limitations such as non-uniform ablation processes and matrix-dependent melting events.…”

Section: Introductionmentioning

confidence: 99%

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Single shot laser ablation MC-ICP-MS for depth profile analysis of U isotopes in UO₂ single crystals

Krachler

Bulgheroni

Ferri

et al. 2019

J. Anal. At. Spectrom.

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Spatial distribution of uranium isotopes in solid nuclear materials using laser ablation multi-collector ICP-MS

Cited by 39 publications

References 20 publications

The Role of Continental Crust in the Formation of Uraninite-Based Ore Deposits

The Role of Continental Crust in the Formation of Uraninite-Based Ore Deposits

Happy Jack Uraninite: A New Reference Material for High Spatial Resolution Analysis of U‐Rich Matrices

Single shot laser ablation MC-ICP-MS for depth profile analysis of U isotopes in UO₂ single crystals

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Spatial distribution of uranium isotopes in solid nuclear materials using laser ablation multi-collector ICP-MS

Cited by 39 publications

References 20 publications

The Role of Continental Crust in the Formation of Uraninite-Based Ore Deposits

The Role of Continental Crust in the Formation of Uraninite-Based Ore Deposits

Happy Jack Uraninite: A New Reference Material for High Spatial Resolution Analysis of U‐Rich Matrices

Single shot laser ablation MC-ICP-MS for depth profile analysis of U isotopes in UO2 single crystals

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Single shot laser ablation MC-ICP-MS for depth profile analysis of U isotopes in UO₂ single crystals