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Minerals
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Nuclear Forensic Applications in Geoscience and Radiochemistry
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Nuclear Forensic Applications in Geoscience and Radiochemistry

A special issue of Minerals (ISSN 2075-163X). This special issue belongs to the section "Mineral Geochemistry and Geochronology".

Deadline for manuscript submissions: closed (31 December 2019) | Viewed by 21444

Special Issue Editor

Dr. Antonio Simonetti

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Guest Editor
Department of Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, IN 46556, USA
Interests: isotope geochemistry; geochronology; laser ablation-ICP-MS; nuclear forensics; geochemistry; igneous petrology; carbonatites
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

A vital component of global nuclear security is the prevention of the theft and trafficking of nuclear materials. Hence, the primary objectives of forensic analysis of (pre-detonation) nuclear materials are to determine the provenance of interdicted materials so as to deter actions that would utilize illicit nuclear material, and to monitor compliance with the United Nations Nuclear Nonproliferation Treaty. Nuclear forensic analysis exploits the fact that certain signatures are unique to the geologic origin for a sample of interest. The different types of critical evidence sought for forensic purposes typically include morphological attributes, isotopic measurements, age data, and trace element compositions (in particular, rare earth element concentrations) of nuclear materials at both bulk and high spatial resolution scales.

This Special Issue invites contributions that focus on reporting forensic investigations of nuclear materials covering the early part of the nuclear fuel cycle, from natural uranium-rich ores/minerals (e.g., uraninite) to uranium oxide concentrates (UOCs) and nuclear fuel pellets using a wide variety of established and novel analytical methods and approaches. This includes the examination of morphological features of nuclear materials that develop due to changing environmental conditions and/or aging, identifying chemical and/or isotopic signatures related to U metal processing, multi-component statistical analysis of existing or new chemical/isotopic databases, establishing reference materials for micro-analyses conducted at high-spatial resolution, and corroborating and/or developing new baseline forensic signatures in raw ores from varying uranium deposit types.

Dr. Antonio Simonetti
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Minerals is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2400 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Uranium
  • Uraninite
  • Uranium ore concentrate
  • Nuclear fuel cycle
  • Source attribution
  • Nuclear nonproliferation
  • Nuclear forensics

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Published Papers (5 papers)

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Research

19 pages, 2600 KiB  
Article
Geochronology of Uraninite Revisited
by Loretta Corcoran and Antonio Simonetti
Minerals 2020, 10(3), 205; https://doi.org/10.3390/min10030205 - 25 Feb 2020
Cited by 12 | Viewed by 4343
Abstract
Identification of uraninite provenance for the purpose of nuclear forensics requires a multifaceted approach. Various geochemical signatures, such as chondrite normalized rare earth element patterns, help identify and limit the potential sources of uraninite based on the geological setting of the uranium ore [...] Read more.
Identification of uraninite provenance for the purpose of nuclear forensics requires a multifaceted approach. Various geochemical signatures, such as chondrite normalized rare earth element patterns, help identify and limit the potential sources of uraninite based on the geological setting of the uranium ore mineralization. The inclusion of accurate age determinations to discriminate geochemical signatures for natural uranium ores may help to potentially restrict geographical areas for provenance consideration. Determining a robust age for uraninite formation is somewhat difficult, due to well known, inherent difficulties associated with open system behavior that involve either uranium and/or lead loss or gain. However, open system behavior should not perturb their Pb isotopic compositions to the same degree as Pb isotopes should not fractionate during alteration processes. Here, a suite of pristine and altered samples of uraninite was examined for their Pb isotope compositions, and these yielded geologically meaningful secondary Pb–Pb isochron ages. The degree of alteration within individual uraninite samples, which is extremely variable, does not appear to affect the calculated ages. The approach adopted here yields insightful age information, and hence, is of great value for source attribution in forensic analyses of raw nuclear materials. Full article
(This article belongs to the Special Issue Nuclear Forensic Applications in Geoscience and Radiochemistry)
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27 pages, 3296 KiB  
Article
The Role of Continental Crust in the Formation of Uraninite-Based Ore Deposits
by Stefanie R. Lewis, Antonio Simonetti, Loretta Corcoran, Stefanie S. Simonetti, Corinne Dorais and Peter C. Burns
Minerals 2020, 10(2), 136; https://doi.org/10.3390/min10020136 - 6 Feb 2020
Cited by 5 | Viewed by 3972
Abstract
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 [...] Read more.
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. Full article
(This article belongs to the Special Issue Nuclear Forensic Applications in Geoscience and Radiochemistry)
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11 pages, 1755 KiB  
Article
Rare Earth Element Determination in Uranium Ore Concentrates Using Online and Offline Chromatography Coupled to ICP-MS
by Veronica C. Bradley, Benjamin T. Manard, Benjamin D. Roach, Shalina C. Metzger, Kayron T. Rogers, Brian W. Ticknor, Sarah K. Wysor, John D. Brockman and Cole R. Hexel
Minerals 2020, 10(1), 55; https://doi.org/10.3390/min10010055 - 8 Jan 2020
Cited by 30 | Viewed by 4515
Abstract
The determination of trace elements, particularly rare earth elements, in uranium ore concentrates (UOCs) is important as the pattern can be indictive ore characteristics. Presented here is a methodology for accurately quantifying rare earth elements (REE) in UOCs. To improve the measurement uncertainty, [...] Read more.
The determination of trace elements, particularly rare earth elements, in uranium ore concentrates (UOCs) is important as the pattern can be indictive ore characteristics. Presented here is a methodology for accurately quantifying rare earth elements (REE) in UOCs. To improve the measurement uncertainty, isotope dilution mass spectrometry (IDMS) was utilized over other quantification techniques such as external calibration or standard addition. The isotopic determinations were measured by inductively coupled plasma-mass spectrometry (ICP-MS). To obtain high-fidelity isotopic measurements, separation of the REE from the uranium matrix was achieved by high-performance ion chromatography (HPIC), reducing the isobaric interferences. After separation, the target analytes were analyzed in two different modalities. For high precision analysis, the separated analytes were collected and measured by ICP-MS in an “offline” fashion. For a rapid approach, the separated analytes were sent directly into an ICP-MS for “online” analysis. These methods have been demonstrated to accurately quantify the REE content in a well-characterized UOC sample. Full article
(This article belongs to the Special Issue Nuclear Forensic Applications in Geoscience and Radiochemistry)
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20 pages, 4604 KiB  
Article
Multivariate Analysis Based on Geochemical, Isotopic, and Mineralogical Compositions of Uranium-Rich Samples
by Loretta Corcoran, Antonio Simonetti, Tyler L. Spano, Stefanie R. Lewis, Corinne Dorais, Stefanie Simonetti and Peter C. Burns
Minerals 2019, 9(9), 537; https://doi.org/10.3390/min9090537 - 5 Sep 2019
Cited by 17 | Viewed by 3782
Abstract
The chemical and isotopic (U, Pb, Sr) signatures for a suite (n = 23) of pristine (>80 wt. % UO2) and altered uraninite samples (>70–80 wt. % UO2) from various locations worldwide have been determined for the purpose of [...] Read more.
The chemical and isotopic (U, Pb, Sr) signatures for a suite (n = 23) of pristine (>80 wt. % UO2) and altered uraninite samples (>70–80 wt. % UO2) from various locations worldwide have been determined for the purpose of identifying potential fingerprints for nuclear forensic analysis. The characterization of the uraninite samples included determination of major, minor and trace element contents, Sr, Pb, and U isotopic compositions, and secondary mineral assemblages. Due to the multivariate approach adopted in this study, principal component analysis (PCA) has been employed to allow the direct comparison of multiple variable types. The PCA results indicate that the geological origin (sandstone, metamorphite, intrusive, granite and unconformity) of pristine uraninite can be readily identified utilizing various combinations of major and/or trace element concentrations with isotopic compositions. Full article
(This article belongs to the Special Issue Nuclear Forensic Applications in Geoscience and Radiochemistry)
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22 pages, 2389 KiB  
Article
A NanoSIMS 50 L Investigation into Improving the Precision and Accuracy of the 235U/238U Ratio Determination by Using the Molecular 235U16O and 238U16O Secondary Ions
by N. Alex Zirakparvar, Cole R. Hexel, Andrew J. Miskowiec, Julie B. Smith, Michael W. Ambrogio, Douglas C. Duckworth, Roger Kapsimalis and Brian W. Ticknor
Minerals 2019, 9(5), 307; https://doi.org/10.3390/min9050307 - 18 May 2019
Cited by 7 | Viewed by 3857
Abstract
A NanoSIMS 50 L was used to study the relationship between the 235U/238U atomic and 235U16O/238U16O molecular uranium isotope ratios determined from a variety of uranium compounds (UO2, UO2F [...] Read more.
A NanoSIMS 50 L was used to study the relationship between the 235U/238U atomic and 235U16O/238U16O molecular uranium isotope ratios determined from a variety of uranium compounds (UO2, UO2F2, UO3, UO2(NO3)2·6(H2O), and UF4) and silicates (NIST-610 glass and the Plesovice zircon reference materials, both containing µg/g uranium). Because there is typically a greater abundance of 235U16O+ and 238U16O+ molecular secondary ions than 235U+ and 238U+ atomic ions when uranium-bearing materials are sputtered with an oxygen primary ion beam, the goal was to understand whether use of 235U16O/238U16O has the potential for improved accuracy and precision when compared to the 235U/238U ratio. The UO2 and silicate reference materials showed the greatest potential for improved accuracy and precision through use of the 235U16O/238U16O ratio as compared to the 235U/238U ratio. For the UO2, which was investigated at a variety of primary beam currents, and the silicate reference materials, which were only investigated using a single primary beam current, this improvement was especially pronounced at low 235U+ count rates. In contrast, comparison of the 235U16O/238U16O ratio versus the 235U/238U ratio from the other uranium compounds clearly indicates that the 235U16O/238U16O ratio results in worse precision and accuracy. This behavior is based on the observation that the atomic (235U+ and 238U+) to molecular (235U16O+ and 238U16O+) secondary ion production rates remain internally consistent within the UO2 and silicate reference materials, whereas it is highly variable in the other uranium compounds. Efforts to understand the origin of this behavior suggest that irregular sample surface topography, and/or molecular interferences arising from the manner in which the UO2F2, UO3, UO2(NO3)2·6(H2O), and UF4 were prepared, may be a major contributing factor to the inconsistent relationship between the observed atomic and molecular secondary ion yields. Overall, the results suggest that for certain bulk compositions, use of the 235U16O/238U16O may be a viable approach to improving the precision and accuracy in situations where a relatively low 235U+ count rate is expected. Full article
(This article belongs to the Special Issue Nuclear Forensic Applications in Geoscience and Radiochemistry)
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