Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Forensics”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 271 records · Page 15

Stable Element Doping of Sol-gel Toward Simulating Environmental Matrix in Surrogate Explosive Nuclear Debris

Training nuclear forensic analysis personnel in post-detonation scenarios is of critical importance to nuclear threat response capabilities. Thus, realistic nuclear debris simulants which resemble the size, color, elemental composition, and radionuclide content of actual nuclear fallout from a recent detonation would be valuable for training nuclear first responders in realistic scenarios. As nuclear fallout types vary significantly in each of these parameters based on detonation environment (rural, urban, maritime etc.) and collection location, the ability to tailor each of these parameters accurately in simulated debris would be of immense benefit to the post-detonation analysis community for training both in-field collections and triage and the validation of laboratory level nuclear forensic techniques. Sol-gel synthesis techniques can provide the tunability of size, shape and composition required for producing surrogate nuclear debris of a wide variety. The sol-gel process consists of forming a metal oxide material, often silica, through polymerization of a metal-alkoxy precursor. In this work, we characterize the ability to load the sol-gel particles with secondary elemental components such as iron, aluminum, and calcium toward approximating the elemental composition of debris from various detonation environments and demonstrate the ability to produce particles with controllable size, shape, and color. We also demonstrate quantitative radionuclide encapsulation toward reproducing the radionuclide content of actual fallout from a recent detonation. Finally, we then employ these techniques in producing simulated aerodynamic debris samples with realistic elemental matrix composition and radionuclide content simulating a recent uranium-fueled detonation taking place in a rural desert environment and compare it to historic fallout from the Nevada Nuclear Security Site.

36 MATERIALS SCIENCE↗

Nuclear Fuel and Pu Redox Studies from The Glenn T. Seaborg Institute at Idaho National Laboratory

The Glenn T. Seaborg Institute at Idaho National Laboratory (INL-GTSI) focuses on advancing fundamental research in the actinide sciences by providing unique opportunities to early career scientists and engineers to gain experience studying the actinide elements and their associated systems. The INL-GTSI is built from three focus areas that are based on the expertise and supporting infrastructure at INL and include solid state chemistry and physics, solution phase chemistry and physics, and forensic and isotope science. INL is the lead Laboratory for nuclear energy research and development in the U. S. and the research on nuclear fuels performed under the INL-GTSI gives good examples of solid state studies. Uranium-Molybdenum (U-Mo) alloys are leading fuel candidates for conversion of high performance research and test reactors to low-enriched fuels. During irradiation, generated fission gas accumulates into bubbles and self-organizes into a gas bubble superlattice (GBS) that effectively stores fission gases and inhibits fuel swelling. A study on the early self- organizing behavior of the GBS shows that not only grain boundaries but the interfaces between the U-Mo matrix and uranium carbide (UC) impurities are important to GBS formation.[1] In solution, understanding the complex redox behavior of plutonium in aqueous environments is critical for establishing optimized nuclear waste reprocessing solvent systems and storage tank environments. INL-GTSI researchers have produced an experimentally validated multi-scale model of the gamma radiation induced behavior of plutonium ions in concentrated aqueous HNO3 solutions.[2] Here, gamma radiation effected only minimal steady state changes in the redox distribution of the plutonium oxidation states. The redox cycling between Pu(IV) and Pu(III) is demonstrated to be mediated by the •OH/NO3• radical oxidation of Pu(III) and the H2O2/HNO3 driven reduction of Pu(IV). The INL-GTSI offers young researchers the unique chance to work directly with actinide bearing materials in a U. S. National Laboratory environment. Further topical areas of interest to the INL-GTSI include, but are not limited to, fundamental actinide properties, structure/property (electronic, magnetic, thermal) relations, actinide quantum criticality, f- electron interactions, electron correlations, computational studies, new phases, defect effects, interface interactions, isotope production and separation, forensic analytical chemistry, structure and dynamic properties of actinides in non-aqueous media, separations chemistry and kinetics for advanced nuclear fuel cycles, radiation effects, and innovative and advanced ligand design for complexation of the actinides.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Angular Correlations of Gamma Rays from Fission Product Solution

Fission products from photon-induced fission are routinely used at Idaho National Laboratory as part of nuclear forensics activities. Typically, the focus is on fission products with relatively large fission yields (Ba-140, Mo-99, etc.). The nuclear data associated with the well-known isotopes have small uncertainties, and many have well-known angular correlations between emitted gamma-rays, if applicable. However, for isotopes with smaller fission yields or less intense gamma-ray emission intensities, the nuclear decay schemes and gamma-ray emission intensities may be less well-known. The Germanium Rotational Measurements for Angular Correlation (GeRMAC) system was designed to use two high-purity germanium (HPGe) detectors in a coincidence counting set-up but allows one of the HPGe detectors to rotate at a constant distance from a radioactive source, changing the relative angle between the two HPGe detectors. Angular correlations can then be determined from the relative photopeak areas between two gamma-rays emitted as part of the same nuclear decay. By recording the HPGe spectra in list mode, the angular correlations of gamma-rays emitted from complex sources, consisting of multiple isotopes, can be measured simultaneously and the individual isotope emissions can be isolated. Using the GeRMAC system, a multi-isotope fission product source, produced with photon-induced fission of U-238, was measured using a single rotational arc (180 degrees) to obtain the angular correlation between gamma-rays emitted by the large number of fission products contained in the solution with an angular accuracy of 1 degree. In particular, La-140 (38 gamma rays) and Nd-147 (26 gamma rays) are of interest to the nuclear forensics community.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Investigation of UO 2 doped with Fe 2 O 3 sintered under a reducing atmosphere

Nuclear fuel produced with trace amounts of transition metal additives is of potential interest for introducing intentional signatures for accelerating nuclear forensics. In this work, we investigate the effects on microstructure, grain size, crystal structure, and stoichiometry when trace amounts of Fe in the form of Fe 2 O 3 are added to UO 2 . Sintering of compacts with different concentrations, from 250 to 3000 ppmw, was performed under a reducing atmosphere at 1773 K. The persistence of the taggant during the fuel fabrication process as well as its impact on grain size, crystal lattice, and first-neighbor chemistry was evaluated using inductively coupled plasma–optical emission spectroscopy, powder X-ray diffraction (pXRD), Raman spectroscopy, scanning electron microscopy–backscatter electron spectroscopy, energy dispersive spectroscopy, and thermogravimetric analysis. We observed that a negligible amount of Fe was lost during sintering. Our results indicate that the feedstock, Fe 2 O 3 transforms into Fe and FeO under the test sintering conditions. For all compositions, metallic Fe precipitate was found in grain boundaries as a secondary phase. In conclusion, the potential incorporation of ionic Fe into the UO 2 unit cell was determined by pXRD and Raman spectra.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Natural isotopic compositions of titanium, iron, and nickel observed in commercial fuel pellets – Promising candidate elements for stable isotope tagging

Stable isotope taggants would constitute unique identifiers for nuclear fuel cycle materials, resulting in expedited timelines and high confidence provenance assessments for nuclear forensics investigations. However, reliably identifying and interpreting stable isotope taggants in nuclear materials recovered from outside of regulatory control will largely be predicated on the assumption that the taggant element intrinsic to the untagged nuclear material exhibits natural isotopic ratios. Here, we present high-precision Ti, Fe, and Ni isotope compositions in 13 commercial low-enriched uranium (LEU) fuel pellets to assess the suitability of these transition metals as stable isotope taggants. Our investigations reveal limited isotope variations among the fuel pellets in all three elements, which are consistent with small mass-dependent isotope fractionations, comparable to variations previously reported for natural samples. In practice, isotopically tagged nuclear materials are expected to fall along isotopic mixing lines, since intrinsic background levels of taggant elements dilute the taggant towards natural isotope compositions. Furthermore, the observation that Ti, Fe, and Ni isotope compositions in a suite of LEU fuel pellets are close to or indistinguishable from estimates for the Bulk Silicate Earth demonstrates that a two end-member mixing assumption would be valid for these transition metals, indicating that all three are promising candidate elements for stable isotope tagging. Finally, we present mass balance calculations to quantify isotopic perturbations expected from admixing isotopically anomalous Ti, Fe, and Ni taggants to assess the interplay between elemental and taggant concentrations and find favorable compromises for facilitating successful taggant identification with current analytical methods.

Intentional forensics↗

Chemical speciation correlated with microstructural heterogeneity of interdicted uranium materials

Two uranium powders seized by law enforcement in Victoria, Australia, have been characterized by established nuclear forensic methods in a previously published study. Here, in this work, the results of further characterization by a scanning transmission x-ray microscope (STXM) operating in the soft x-ray regime are reported. STXM images are used to estimate the elemental distribution in micrometer-scale particles of each powder, and oxygen K-edge absorption spectra are used to determine the chemical state of uranium. The results of the current study are consistent with the previous analysis; the first powder is found to be a potassium-uranium hydrate, while the second powder is determined to be a mixture of uranium oxides primarily consisting of UO 3 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

New measurements of gamma-ray energies and their absolute intensities from the decay of 231 Pa

Accurate nuclear data for the decay of 231 Pa is highly important for non-destructive analysis in the areas of radiochronometry and nuclear forensics. However, the evaluated nuclear data for this isotope is lacking; many previous measurements have large uncertainties and only two measurements are used to determine the absolute intensities. In this work, we present modern measurements of the major gamma-ray emissions from the decay of 231 Pa to 227 Ac including the energies and absolute intensities. For many of these measurements, the error envelopes have been significantly decreased compared to previous measurements, while remaining in good agreement. The absolute intensity of the 283 keV reference line was measured as 0.0163(2).

231Pa↗

International interlaboratory compilation of trace element concentrations in the CUP-2 uranium ore concentrate standard

Herein, a nuclear forensics investigation involving a uranium ore concentrate relies on accurate and precise analysis of impurities. Analytical data defensibility requires the use of reference materials as part of quality control. This study presents a compilation of trace element concentration results of the CUP-2 Uranium Ore Concentrate Standard measured by 11 different laboratories. The laboratories employed various dissolution methods, analytical preparation methods, and instrumental platforms. The data presented here contain concentrations of 66 impurities with up to 138 individual data points for each impurity. Consensus values have been assigned to each impurity following a statistical analysis of the data set.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Radiochronometric analysis of an historic Cs-137 activity standard

In this work, a 137 Cs activity standard discovered during routine inventory was analyzed to determine its model age using radiochronometry. The aqueous activity standard was separated using an established separation method that employs commercially available Sr resin. The method was also tested against a nuclear forensics reference material developed specifically for benchmarking 137 Cs radiochronometry methods. Results of the analyses showed good agreement between the results and the certified values of the reference material. Analysis of the discovered activity standard were also in good agreement with the activity certification date, though uncertainty was higher due to natural Ba contaminating the sample and the stable 133 Cs used as a carrier during the standard’s production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Radioxenon signatures of molten salt reactors

Developments of molten salt reactor (MSR) technologies are making rapid progress across the globe. These reactor designs involve properly controlling radionuclides through off-gas systems. This work examines radioxenon emissions and assesses treaty detection technology to be used for monitoring. This work also includes a sensitivity study with ORIGEN on the nuclear forensic signals possible from a MSR. Multiple Isotope Ratio Comparison (MIRC) plots are used to compare the ratios of radioxenon isotopes in an MSR to a highly enriched uranium (HEU) reactor. Finally, the results show that MSR emissions may significantly overlap with signals produced in a HEU reactor and that changing reactor operations or retaining emissions in an off-gas system can significantly shift the radioxenon signature away from the HEU pulse.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Retention of radionuclides in sol–gel surrogate nuclear explosive debris

Sol–gel vitrification can be used to rapidly produce solid, vitreous materials to support nuclear forensics research. Here, this work investigates three sol–gel synthetic approaches’ ability to retain fission products within the glass as a function of drying temperature. Eight of the ten fission products studied were quantitatively retained (less than 5% losses) at temperatures up to 600 °C for glasses prepared using an acidic catalyst and at temperatures up to 300 °C for glasses prepared using a basic catalyst. Both systems show partial loss of ruthenium and complete loss of iodine at temperatures above 300 and 100 °C, respectively.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

A chromatography chemistry for purifying $\mathrm{Pa}$ from $\mathrm{U-Nb}$ metal alloys

Here we present a chromatography chemistry for purifying protactinium from uranium metal alloys containing weight-percent concentrations of niobium. Niobium is precipitated in 9 M HCl without the co-precipitation of Pa as demonstrated by gamma-ray spectrometry. Protactinium is further purified using Bio-Rad™ anion resin AG® 1-X8 and 9 M HCl + 0.0128 M HF. A Pa/Nb separation factor of 85,000 and a 90% Pa recovery is demonstrated, which is amenable to 231 Pa concentration determination by isotope dilution and 231 Pa/ 235 U model age calculation for nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Removal of fission product tellurium and iodine from recently irradiated HEU using copper metal

Gamma detection of select fission products or activation products such as 153 Sm and 239 Np in a fission sample is difficult due to gamma interferences from radiotellurium and radioiodine. To aid in the detection of these difficult-to-detect nuclides, the radiotellurium and radioiodine were removed using Cu metal turnings. This method is highly effective at the removal of the interfering radionuclides removing > 98% of the radiotellurium and radioiodine. A mechanistic study was conducted. Determining the deposition mechanism, using a number of techniques including XANES and electrochemistry providing an understanding of the electrochemical path for the Te deposition. Initial work focused on the use of stable Te, further expanding into activated TeO 2 , and a fresh fission sample. Importantly, this method presents a rapid method for the direct detection of select fission products that could have a significant impact on nuclear related fields including nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Model ages of three uranium metal CRMs and implications for radiochronometry data interpretation

In this study, we report 230 Th/ 234 U and 231 Pa/ 235 U model ages in three uranium metal certified reference materials with distinct production histories and isotopic compositions ranging from depleted to highly enriched (CRMs 112-A, 115, and 116-A). Here, our results provide the first model age values for these materials using multiple radiochronometers, which can be used as reference values for quality control of radiochronometry measurements performed during nuclear forensic investigations. Furthermore, we evaluate the model ages in the context of available production records for the materials, which provides insight into the processes that may impact radiochronometry systems during uranium metal production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Single particle trace element analysis of uranium oxide standards with laser-induced breakdown spectroscopy

Femtosecond Laser-Induced Breakdown Spectroscopy (LIBS) was used to analyze over 1000 individual particles of uranium oxide trace element standard CRM124. Intra-granular analysis showed elemental concentrations were consistent across different surface locations on each uranium grain. However, inter-granular comparison revealed large heterogeneity between different grains of the same sample. By comparing the distribution of elemental concentrations across the particle populations, we were able to correctly identify a manufacturing process involving wet chemistry, rather than a dry mixing of two powders to give an overall chemical average. In conclusion, this demonstrates the utility of LIBS as a large-scale single particle analysis tool for nuclear forensics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Neutron capture signatures determined from gadolinium isotope compositions of uranium ore concentrates using MC-ICPMS

We present Gd isotope compositions on 25 well-characterized uranium ore concentrates (UOCs). About half the UOCs have isotope depletions in 157 Gd coupled with anticorrelated excesses in 158 Gd due to neutron capture effects. UOCs from older ore bodies and with higher U contents show larger neutron capture effects than UOCs from younger ore bodies with lower U contents. These Gd data are correlated with their previously measured Sm isotope compositions, and we use the Sm data to estimate the neutron fluence of these samples. In conclusion, this work demonstrates how Gd isotope signatures can be employed as a new tool for nuclear forensics.

Earth Sciences↗

Recovery of stable isotope taggants along a wet production pathway of uranium dioxide

Stable isotope taggants added to nuclear materials could be utilized as diagnostic nuclear forensics signatures; however, intentionally adding taggants is a relatively new and untested concept with respect to the nuclear fuel cycle. Here, in this study, we added trace amounts of stable Mo and W isotope taggants to starting materials used to synthesize UO 2 along a wet synthesis pathway. Successful incorporation and recovery of the Mo and W taggants was achieved in the UO 2 product and all its precursors. This study demonstrates the efficacy of stable isotope tagging along a wet UO 2 production pathway.

Nuclear forensics↗