Nuclear proliferomics: A new field of study to identify signatures of nuclear materials as demonstrated on alpha-UO3

Schwerdt, Ian J.; Brenkmann, Alexandria; Martinson, Sean; Albrecht, Brent D.; Heffernan, Sean; Klosterman, Michael R.; Kirkham, Trenton; Taşdizen, Tolga; McDonald, Luther W.

doi:10.1016/j.talanta.2018.04.092

Cited by 34 publications

(19 citation statements)

References 50 publications

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“…Thermal expansion during heating, and contraction from cooling, would also give rise to the deformations seen in these particles. The observed reduction in particle size corresponds with previous studies, which have demonstrated that uranium oxide particle size decreases with increasing temperature [7]. However, particle size may again increase above a threshold temperature, as sintering effects occur.…”

Section: Sem Analysissupporting

confidence: 88%

“…This is a significant finding in the context of nuclear forensic application, as these particles of U 3 O 8 may be traced back to their uranyl oxalate precursor. These particles of U 3 O 8 can be differentiated, therefore, from those obtained by the thermal decomposition of other precursors (such as studtite), so that the provenance of an intercepted U 3 O 8 material may be more accurately determined in the field [2,7,34].…”

Section: Sem Analysismentioning

confidence: 99%

“…Other intermediates exist, such as uranyl peroxide ([(UO 2 )(O 2 )(H 2 O) 2 ]•2H 2 O), which is produced following a similar processing route and has been extensively studied for its material properties [2][3][4][5][6]. Furthermore, some recent characterisations have been focused on the nuclear forensic implications of uranyl peroxides and its oxides [7]. Neither the material characteristics nor the nuclear forensic signatures of the oxalate intermediate have been reported extensively.…”

Section: Introductionmentioning

confidence: 99%

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Nuclear forensic signatures and structural analysis of uranyl oxalate, its products of thermal decomposition and Fe impurity dopant

Thompson

Stennett

Gilbert

et al. 2021

J Radioanal Nucl Chem

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Uranyl oxalate (UO2C2O4·xH2O) may exist at the back-end of the nuclear fuel cycle (NFC) as an intermediate in spent fuel reprocessing. The conditions used in aqueous reprocessing and thermal treatment can affect the physical and chemical properties of the material. Furthermore, trace impurities, such as Fe, may incorporate into the structure of these materials. In nuclear forensics, understanding relationships between processing variables aids in determination of provenance and processing history. In this study, the thermal decomposition of UO2C2O4·3H2O and phase analysis of its thermal products are examined. Their morphologies are discussed with respect to a matrix of solution processing conditions.

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Section: Sem Analysissupporting

confidence: 88%

Section: Sem Analysismentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Nuclear forensic signatures and structural analysis of uranyl oxalate, its products of thermal decomposition and Fe impurity dopant

Thompson

Stennett

Gilbert

et al. 2021

J Radioanal Nucl Chem

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“…References [1][2][3][4][5][6][7] describe pre-detonation nuclear forensics goals. Pre-detonation nuclear forensics focuses on determining the source and route of nuclear materials and devices prior to their use in an improvised nuclear device or radiological dispersal device.…”

Section: Introductionmentioning

confidence: 99%

“…Baseline morphology and discussion of the technical production details for four precipitation conditions (ADU, AUC, SDU, and MDU) are provided in [1,2]. Subsequent studies have investigated the quantitative morphological variations for a selection of these materials due to processing, aging, and/or storage conditions [3,4,7]. One related inference goal is to determine factors that impact particle morphology, such as calcination temperature, production pathway involving UO3, U3O8, or UO2, at 400 • C, 800 • C, and 510 • C (in H2), respectively, and impurities for a given precipitation condition.…”

Section: Introductionmentioning

confidence: 99%

Overview of Algorithms for Using Particle Morphology in Pre-Detonation Nuclear Forensics

et al. 2021

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A major goal in pre-detonation nuclear forensics is to infer the processing conditions and/or facility type that produced radiological material. This review paper focuses on analyses of particle size, shape, texture (“morphology”) signatures that could provide information on the provenance of interdicted materials. For example, uranium ore concentrates (UOC or yellowcake) include ammonium diuranate (ADU), ammonium uranyl carbonate (AUC), sodium diuranate (SDU), magnesium diuranate (MDU), and others, each prepared using different salts to precipitate U from solution. Once precipitated, UOCs are often dried and calcined to remove adsorbed water. The products can be allowed to react further, forming uranium oxides UO3, U3O8, or UO2 powders, whose surface morphology can be indicative of precipitation and/or calcination conditions used in their production. This review paper describes statistical issues and approaches in using quantitative analyses of measurements such as particle size and shape to infer production conditions. Statistical topics include multivariate t tests (Hotelling’s T2), design of experiments, and several machine learning (ML) options including decision trees, learning vector quantization neural networks, mixture discriminant analysis, and approximate Bayesian computation (ABC). ABC is emphasized as an attractive option to include the effects of model uncertainty in the selected and fitted forward model used for inferring processing conditions.

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The thermal decomposition of studtite: analysis of the amorphous phase

Thompson

Frankland

Bright

et al. 2021

J Radioanal Nucl Chem

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Studtite is known to exist at the back-end of the nuclear fuel cycle as an intermediate phase formed in the reprocessing of spent nuclear fuel. In the thermal decomposition of studtite, an amorphous phase is obtained at calcination temperatures between 200 and 500 °C. This amorphous compound, referred to elsewhere in the literature as U2O7, has been characterised by analytical spectroscopic methods. The local structure of the amorphous compound has been found to contain uranyl bonding by X-ray absorption near edge (XANES), Fourier transform infrared and Raman spectroscopy. Changes in bond distances in the uranyl group are discussed with respect to studtite calcination temperature. The reaction of the amorphous compound with water to form metaschoepite is also discussed and compared with the structure of schoepite and metaschoepite by X-ray diffraction. A novel schematic reaction mechanism for the thermal decomposition of studtite is proposed.

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Nuclear proliferomics: A new field of study to identify signatures of nuclear materials as demonstrated on alpha-UO3

Cited by 34 publications

References 50 publications

Nuclear forensic signatures and structural analysis of uranyl oxalate, its products of thermal decomposition and Fe impurity dopant

Nuclear forensic signatures and structural analysis of uranyl oxalate, its products of thermal decomposition and Fe impurity dopant

Overview of Algorithms for Using Particle Morphology in Pre-Detonation Nuclear Forensics

The thermal decomposition of studtite: analysis of the amorphous phase

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