The need for speed – Burnup determination of spent nuclear fuel

Roach, Benjamin D.; Rogers, Kayron T.; Zirakparvar, N. Alex; Delashmitt, Jeffrey S.; Metzger, Shalina C.; Manard, Benjamin T.; Keever, Tamara J.; Giaquinto, J.M.; Hexel, Cole R.

doi:10.1016/j.talo.2022.100152

Cited by 4 publications

(15 citation statements)

References 33 publications

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“…The composition of the fuel post irradiation depends on the fuel properties, positioning within a reactor, power levels, irradiation duration, and many other conditions. Multicollector inductively coupled plasma–mass spectrometry or thermal ionization mass spectrometry are often used to monitor burnup (e.g., 148 Nd) compared with residual uranium and plutonium concentrations . These methods typically require high-pressure ion chromatographic separations to measure the concentrations and isotopic compositions of neodymium, plutonium, and uranium.…”

Section: Resultsmentioning

confidence: 99%

Comparing Sensor Fusion and Multimodal Chemometric Models for Monitoring U(VI) in Complex Environments Representative of Irradiated Nuclear Fuel

Sadergaski,

Andrews,

Wilson

2024

Anal. Chem.

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Optical sensors and chemometric models were leveraged for the quantification of uranium(VI) (0–100 μg mL–1), europium (0–150 μg mL–1), samarium (0–250 μg mL–1), praseodymium (0–350 μg mL–1), neodymium (0–1000 μg mL–1), and HNO3 (2–4 M) with varying corrosion product (iron, nickel, and chromium) levels using laser fluorescence, Raman scattering, and ultraviolet–visible–near-infrared absorption spectra. In this paper, an efficient approach to developing and evaluating tens of thousands of partial least-squares regression (PLSR) models, built from fused optical spectra or multimodal acquisitions, is discussed. Each PLSR model was optimized with unique preprocessing combinations, and features were selected using genetic algorithm filters. The 7-factor D-optimal design training set contained just 55 samples to minimize the number of samples. The performance of PLSR models was evaluated by using an automated latent variable selection script. PLS1 regression models tailored to each species outperformed a global PLS2 model. PLS1 models built using fused spectra data and a multimodal (i.e., analyzed separately) approach yielded similar information, resulting in percent root-mean-square error of prediction values of 0.9–5.7% for the seven factors. The optical techniques and data processing strategies established in this study allow for the direct analysis of numerous species without measuring luminescence lifetimes or relying on a standard addition approach, making it optimal for near-real-time, in situ measurements. Nuclear reactor modeling helped bound training set conditions and identified elemental ratios of lanthanide fission products to characterize the burnup of irradiated nuclear fuel. Leveraging fluorescence, spectrophotometry, experimental design, and chemometrics can enable the remote quantification and characterization of complex systems with numerous species, monitor system performance, help identify the source of materials, and enable rapid high-throughput experiments in a variety of industrial processes and fundamental studies.

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Section: Resultsmentioning

confidence: 99%

Comparing Sensor Fusion and Multimodal Chemometric Models for Monitoring U(VI) in Complex Environments Representative of Irradiated Nuclear Fuel

Sadergaski,

Andrews,

Wilson

2024

Anal. Chem.

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“…103,104 A wide range of U-series geochemistry applications to the Earth sciences was thoroughly summarized in "Uranium-series Disequilibrium, Applications to Earth, Marine and Environmental Sciences". 105 The uranium and thorium decay-series contain radioactive isotopes of many elements (in particular, 234,235,238 U, 230,232 Th, 231 Pa, 226 Ra and 227 Ac) with varied physicochemical properties leading to a fractionation (mainly elemental fractionation) within the chain in different geological environments during geochemical processes. The accurate measurement of these radionuclides and more specically their elemental ratios (i.e., 230 Th/ 238 U, 238 U/ 232 Th, 231 Pa/ 235 U, 226 Ra/ 230 Th) allows the investigation of processes occurring on time scales from a hundred years to ∼600 000 years.…”

Section: Isotope Dilution Uncertaintymentioning

confidence: 99%

“…105 The uranium and thorium decay-series contain radioactive isotopes of many elements (in particular, 234,235,238 U, 230,232 Th, 231 Pa, 226 Ra and 227 Ac) with varied physicochemical properties leading to a fractionation (mainly elemental fractionation) within the chain in different geological environments during geochemical processes. The accurate measurement of these radionuclides and more specically their elemental ratios (i.e., 230 Th/ 238 U, 238 U/ 232 Th, 231 Pa/ 235 U, 226 Ra/ 230 Th) allows the investigation of processes occurring on time scales from a hundred years to ∼600 000 years. To this end, radionuclide concentrations are accurately determined in environmental samples by ID-MS.…”

Section: Isotope Dilution Uncertaintymentioning

confidence: 99%

“…The 233 Pa spike is calibrated using commercially available 156 or "in-house" 231 Pa standard solutions calibrated against the HU-1. Recent developments allow the measurement of quantities as low as 0.1 fg of 231 Pa by MC-ICP-MS. 102,157 TIMS protocols for 231 Pa analysis allow the determination of as little as a few tens of fg to a few ag. 153,158 Moreover, high resolution ICP-MS (HR-ICP-MS) reported LOD values were close to 0.02 fg kg −1 .…”

Section: Application For Radionuclide Measurementmentioning

confidence: 99%

“…To this end, ID-MS is the method that can achieve the best results, provided there is rigor in the choice of the isotopic spikes, in the chemical purication of the material and in the mass spectrometric measurements. The uncertainties of the half-lives of the parent nuclides and of the daughter products (mainly 234 U- 230 Th, 235 U- 231 Pa, 234 U- 238 Pu, 235 U- 239 Pu, 236 U- 240 Pu, 238 U- 242 Pu and 241 Pu-241 Am) are very low (between less than 0.01% and 0.4% (for 231 Pa)) and their contribution to the global uncertainty is generally negligible.…”

Section: Nuclear Forensicsmentioning

confidence: 99%

See 2 more Smart Citations

An isotope dilution mass spectrometry overview: tips and applications for the measurement of radionuclides

Quemet,

Hubert,

Gourgiotis

et al. 2024

J. Anal. At. Spectrom.

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Complete resolution across the neodymium/samarium isotopic envelope with a liquid sampling‐atmospheric pressure glow discharge — Orbitrap mass spectrometer

Goodwin,

Shrestha,

Manard

et al. 2024

Rapid Comm Mass Spectrometry

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RationaleNd and Sm isotope ratios play an important role in geological dating and as nuclear forensic signatures; however, the overlap of the respective 144, 148, 150 Nd/Sm isobars requires prior separations to be performed before analysis on typical MS platforms. The work presented here overcomes these isobaric interferences using ultrahigh‐mass resolution to alleviate interference without prior chemical separations.MethodsA liquid sampling‐atmospheric pressure glow discharge ion source was coupled to a standard, QExactive Focus Orbitrap mass spectrometer, providing a mass resolution of ~80 k. A Spectroswiss FTMS booster X2 data acquisition package was used to collect extended transients, providing much higher mass resolution; ~230 k and ~600 k are employed here for Nd and Sm isotopes.ResultsWhile the standard Orbitrap resolution is far greater than typical “atomic” MS platforms, it was insufficient to alleviate all isobars. The use of a resolution of ~230 k resulted in baseline separation across the entire isotopic envelope for both Nd and Sm. Isotope ratios obtained from Nd:Sm mixtures using high‐resolution were equivalent to those found for individual‐element solutions, while isotope ratios obtained at a resolution of ~80 k (standard for the OEM data system) showed large deviations.ConclusionsUse of ultrahigh‐resolution is an attractive alternative to extensive chemical separations to alleviate severe isobaric interferences. Sufficient mass resolution greatly reduces/eliminates the need for sample manipulations (separations) before analysis while reducing costs and total analysis times.

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The need for speed – Burnup determination of spent nuclear fuel

Cited by 4 publications

References 33 publications

Comparing Sensor Fusion and Multimodal Chemometric Models for Monitoring U(VI) in Complex Environments Representative of Irradiated Nuclear Fuel

Comparing Sensor Fusion and Multimodal Chemometric Models for Monitoring U(VI) in Complex Environments Representative of Irradiated Nuclear Fuel

An isotope dilution mass spectrometry overview: tips and applications for the measurement of radionuclides

Complete resolution across the neodymium/samarium isotopic envelope with a liquid sampling‐atmospheric pressure glow discharge — Orbitrap mass spectrometer

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