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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

An approach to separating Pu, U, and Ti from high-purity graphite for isotopic analysis by MC-ICP-MS

Information about elemental and isotopic systematics of ultra-trace level actinides (e.g. U and Pu) and main group elements (e.g. Ti) present within nuclear grade graphite is vital to the nuclear community for improved reactor operation and security. In support of this, extensive effort has been placed on improving analysis methods (i.e., inductively coupled plasma-mass spectrometry). However, significantly less effort has been devoted to the optimization of chemical separation methods. Within the separation community, commercially available Eichrom™ resins are often employed, as their elution characteristics for various elements have been well studied, but the direct optimization of actinides and trace metal separations from a single sample have not been widely investigated. Here, methods using various Eichrom pre-packed cartridges were explored to achieve separation of ultra-trace levels of U, Pu, and Ti from a variety of graphite samples. Once the validity of the combined separation scheme was established using certified reference materials, the method was applied to historic, unirradiated and irradiated, graphite samples. For all samples investigated, precise isotope ratio measurements for the titanium isotope systems were made.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Investigation of the 244 Pu ⁢( 48 Ca,𝑥⁢𝑛) 292−𝑥 Fl reaction with the LBNL SHREC detector: Investigation of decay chains of isotopes of flerovium (𝑍=114)

The 244 Pu ⁢( 48 Ca,𝑥⁢𝑛)⁢ 292−𝑥 Fl reaction was investigated at Lawrence Berkeley National Laboratory’s 88 Inch Cyclotron using the Berkeley Gas-filled Separator (BGS), the newly installed Superheavy Recoil detector, along with an upgraded digital electronics and data acquisition system. Seven decay chains were observed starting with an evaporation residue, followed by a single 𝛼 decay and a spontaneous fission. The decay characteristics of these seven decay chains led to an assignment to 288 Fl , the product of the 4⁢𝑛 reaction channel. Two additional chains were (tentatively) assigned to the decay of the 3⁢𝑛 exit channel, 289 Fl . Cross sections for the 4⁢𝑛 and 3⁢𝑛 exit channels were 𝜎 prod =6.7⁢($^{36}_{25}$) pb and 𝜎 prod =1.6⁢($^{22}_{11}$) pb, respectively. Another decay chain, tentatively assigned to the 5⁢𝑛 exit channel through the 48 Ca + 244 Pu reaction or the 3⁢𝑛 exit channel of the 48 Ca + 242 Pu reaction, was also detected. Detailed information regarding the observed decay chains and their nuclear structure aspects is discussed, along with the performance of the BGS and the new detection system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Evaluation of uncertainty in antineutrino spectra normalization calculations for advanced nuclear reactor monitoring

Antineutrino detection systems have been envisioned as an important aspect of safeguarding the next generation of nuclear reactors, especially considering designs utilizing exotic fuel cycles. Deployment of antineutrino detection systems for safeguarding applications is hindered by the uncertainties associated with the calculations required for antineutrino spectra measurements and predictions. The focus of this work is to assess the impact of system components on antineutrino spectra normalization uncertainties and their significance in reactor power monitoring sensitivity. The dominant limitation in antineutrino detection calculations is typically the uncertainty associated with a cosmogenic background. This limitation becomes more pronounced when signals are weak, although the issue is mitigated in larger reactors due to their stronger source strength. Additionally, antineutrino emission uncertainties vary with the isotopic composition of the reactor fuel. Unconventional fuel cycles, featuring less common fissioning isotopes, such as Pu-240, introduce larger antineutrino yield uncertainties. The findings from this study suggest that future research on safeguard-targeted antineutrino detection should prioritize background mitigation, particularly when background simulation is necessary. Advanced nuclear reactor designs have a major influence on background understanding and successful system implementation.

Physics↗
DOE OSTI2020

Proven Technologies for the Solidification of Complex Liquid Radioactive Waste (LRW): Global Case Studies of Applications and Disposal Options - 20424

Legacy radioactive waste streams from the Cold War still exist and newly generated waste streams from nuclear power plants and research institutes go untreated and expose environmental hazards at many nuclear sites. The nature of the waste is diverse, depending upon the source or the process from which it originated. The most problematic waste streams include complex liquids such as organic (tri-butyl-phosphate TBP) solutions contaminated with Pu and U isotopes, mixed sludge types, high acid radioactive waste, H-3 contaminated organic and aqueous streams, etc. Technological, environmental and economic challenges exist for the treatment and disposal of such waste streams. A proven technology that has been applied to LRW on a global basis provides one option as a low-cost solution to legacy streams and small volume, highly complex LRW frequently found during decommissioning at nuclear power plants and weapons sites. The engineered polymer technology from Nochar, USA, is capable of solidifying standard and highly complex LLW and ILW waste streams for interim or final storage, or for incineration. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

A Machine Learning Method for the Forensics Attribution of Separated Plutonium

Plutonium (Pu) source attribution would be a powerful tool to support nuclear nonproliferation efforts. This capability to find the source of a Pu sample would act as a deterrent to smuggling efforts, and also help regulatory agencies verify declared nuclear activities. Work at Texas A&M University yielded a nuclear forensics methodology, which is capable of determining separated Pu’s reactor of origin, fuel burnup, and the time since irradiation (TSI)—three parameters of interest. The methodology used a set of ten intra-element isotopic ratios found in separated Pu, which was compared to a library of isotopic ratio values produced using neutronics simulations for reactors of interest. By calculating the probability that unknown Pu sample’s isotopic ratio set matched a set in the library, the methodology could predict the three parameters of interest of the sample. One shortcoming of this methodology was an inability to correctly attribute spoofed Pu, where Pu sourced from two different reactors or two different fuel burnup levels are mixed. A new methodology to rectify this vulnerability using machine learning (ML) technique is developed, instead of the maximum likelihood calculation previously used and the results are satisfactory. The ML approach leverages the existing simulated data for training the algorithm, but use them efficiently by only using intra-element isotope ratios that contribute to the attribution one of the three parameters at a time. Previously, all isotope ratios were used to attribute all three parameters together. The new methodology attributes the Pu parameters in three steps, one for each parameter, rather than resolving all of the three parameters simultaneously like the previous maximum likelihood approach. First, a support vector machine classifier with a set of seven isotopic ratios finds the reactor of origin and a set of regression models trained using gaussian process predicts the burnup with a different set of seven isotopes. Finally, TSI is calculated analytically using decay equations. Thus far, the new methodology is capable of attributing pure Pu samples and has been validated using experimental data. The next step will to be augment the classifier training data set with spoofed Pu data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Galactic chemical evolution with the short-lived isotopes 53 Mn, 60 Fe, 182 Hf, and 244 Pu

We run a three-dimensional Galactic chemical evolution (GCE) model to follow the propagation of 53 Mn from supernovae of type Ia (SNIa), 60 Fe from core-collapse supernovae (CCSNe), 182 Hf from intermediate mass stars (IMSs), and 244 Pu from neutron star mergers (NSMs) in the Galaxy. We compare the GCE of these short-lived radioactive isotopes (SLRs) to recent detections on the deep-sea floor. We find that although these SLRs originate from different sites, they often arrive conjointly on Earth.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Dose reconstruction for plutonium-239 intakes at the Rocky Flats Plant

Purpose: The Rocky Flats (RF) Plant was a weapons manufacturing facility that operated from the early 1950s to 1989. Its primary missions were the production of plutonium (Pu) pits for thermonuclear weapons and the processing of retired weapons for Pu recovery. The purpose of this study was to estimate radiation doses to a cohort of 4499 RF workers from an intake of 239 Pu, the primary plutonium isotope handled at the site. Materials and methods: The latest biokinetic models of the International Commission on Radiological Protection, or site-specific variations of those models, were used to estimate 239 Pu intakes for each worker based on model fits to bioassay data often coupled with lung measurements. Results: Urinary excretion and lung retention data for most 239 Pu intakes could be fit reasonably well by a mixture of Pu dioxide and moderately soluble material. For some workers, better fits were obtained by application of other absorption types including Type S, 239 Pu nitrate, or pure 239 Pu dioxide, or by assuming intake via a wound. The lungs typically received the highest tissue doses, with fifty-year committed equivalent doses in the range of 0.5–1 Sv for 275 workers, 1–5 Sv for 115 workers, and greater than 5 Sv for 12 workers. Conclusions: RF was a unique site regarding a large number of lung measurements available for determining the appropriate absorption types for inhaled material. Further, this provided higher confidence in reconstructed 239 Pu doses than is generally gained from urinary data alone.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2022

Measurement of the Effective Capture Cross Section of 238 Np in the High Flux Isotope Reactor

The cross sections of 237 Np and 238 Np are important for accurate modeling and simulation of 238 Pu in the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL). Uncertainties in these cross sections can impact the ability to predict and optimize the target design and loading for 238 Pu production targets. The effective capture cross section of 237 Np in the location of pneumatic tube 1 in HFIR was measured as a first step in the measurement of the 238 Np capture and fission cross sections. Here, we describe the flux measurements, 237 Np experiments, and data analysis of the 237 Np capture cross section in HFIR.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Particulate plutonium released from the Fukushima Daiichi meltdowns

Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O 2 nanoparticles, <~10 nm, one of which is enriched in Pu adjacent to fragments of Zr-cladding. The isotope ratios, 235 U/ 238 U, 240 Pu/ 239 Pu, and 242 Pu/ 239 Pu, of the CsMPs were determined to be ~0.0193, ~0.347, and ~0.065, respectively, which are consistent with the calculated isotopic ratios of irradiated-fuel fragments. Thus, considering the regional distribution of CsMPs, the long-distance dispersion of Pu from FNDPP is attributed to the transport by CsMPs that have incorporated nanoscale fuel fragments prior to their dispersion up to 230 km away from the Fukushima Daiichi reactor site.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2021

Direct analysis of cotton swipes for plutonium isotope determination by microextraction-ICP-MS

This study demonstrates a method for determining the isotopic composition of low-level (sub-pg) plutonium (Pu) directly from a cotton swipe. Environmental sample (ES) swipes are routinely employed as a tool for monitoring activities in nuclear facilities. Traditional ES swipe analysis, as employed in nuclear safeguards, utilizes laborious ashing, digestion, and chemical separation procedures prior to mass spectrometric (MS) analysis. Here, an innovative sample introduction technique employing a microextraction probe to extract Pu directly from the swipe surface is described. The microextraction probe lowers onto the swipe surface, seals on a small area (8 mm 2 ), and delivers solvent (2% HNO 3 ) to extract actinide material that may be present. The extracted analyte is subsequently directed into a sector field inductively coupled plasma (ICP)-MS for isotope ratio determination. This microextraction-ICP-MS method successfully determined the isotopic composition ( 240 Pu/ 239 Pu and 242 Pu/ 239 Pu) of three Pu certified reference materials (CRM 136, 137, and 138) that were deposited (1 pg) onto ES swipes. The percent relative difference from the certified value, uncorrected for instrumental fractionation, was <2% for the 240 Pu/ 239 Pu ratio on all three CRMs and <10% for the 242 Pu/ 239 Pu ratio on CRM 136 and 138. Here, the percent relative standard deviation, an estimate of the sample-to-sample isotopic precision, was <4% for the 240 Pu/ 239 Pu and <15% for the 242 Pu/ 239 Pu. Method limits of detection were determined, based on measurements of an enriched 244 Pu material, to be ~7 fg. Additionally, a mixed uranium (U) and Pu deposition was made to determine the method's ability to simultaneously extract U and Pu and determine the isotopic composition of both analytes.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Progress on Pu-238 Production at INL From February 2022 to December 2022

Idaho National Laboratory (INL) has continued to qualify irradiation positions in the Advanced Test Reactor (ATR) for Pu-238 production to support NASA deep space missions. Over the past year, INL qualified Np-237 targets for ATR’s North East Flux Trap (NEFT), inner A, and H positions. Work has begun to requalify the South Flux Trap (SFT) and qualify the East Flux Trap (EFT) for the ATR GEN I target and is midway through the qualification process. This paper gives an overview of operational and technical activities from February 2022 to December 2022.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2020

A Rapid Sequential Separation Method for Determination of Actinides and TENORM in Fracking Wastes - 20223

With recent advances in unconventional drilling technology in the US and around the world, the risks of environmental contamination and exposure due to technologically enhanced naturally occurring radioactive materials (TENORM) from fracking wastes have also surfaced. Although the Permian Basin (southeastern New Mexico, western Texas) has long been a modest producer of oil, the advent of fracking technology a decade ago turned it into hot property for producers. A 2018 assessment of undiscovered, technically recoverable continuous oil and gas resources by the U.S. Geological Survey estimates an average 46.3 billion barrels of oil and 281 trillion cubic feet of gas. This is likely to increase the use of unconventional drilling and TENORM generation. TENORM concentrations in oil and gas exploration and production waste can be several hundred to several thousand times higher than background TENORM concentrations. Both the thorium and uranium decay chains contribute to airborne radionuclides arising from the radon gas escaping the ground and subsequently decaying as airborne particulates. Additionally, radon decay products {sup 210}Pb and {sup 210}Po can build up in scale on the internal surfaces of oil and gas handling pipes and in sludge in refineries, becoming potential inhalation and ingestion hazards for workers. Furthermore, southeastern NM is also home to world's only licensed and operating transuranic nuclear waste repository, the DoE's Waste Isolation Pilot Plant (WIPP). Plutonium isotopes ({sup 239+240}Pu) and {sup 241}Am, are expected to account for more than 99% of the total radioactivity scheduled for disposal in the WIPP repository. Thus, an improved understanding of the environmental fate and transport of TENORM, liberated by unconventional drilling, is essential to assess how best to protect individuals and the environment. In this context, accurate measurement of TENORM and actinides in environmental and biological samples is essential. In this presentation, a new sequential method for the separation and pre-concentration of actinides (Pu, Am, Np) and TENORM (Po, U and Th) derived from oil and gas exploration is proposed. The TEVA method involves a rapid co-precipitation step to remove matrix interferences from the samples, followed by plutonium oxidation state adjustment to Pu (IV) and an incubation period of ∼ 1 hour at 50-60 deg. C to allow the resultant Po (II) to oxidize into Po(IV). The polonium, neptunium, thorium and plutonium are then separated on a TEVA column, while americium and uranium are separated on a TRU column. After separation, the alpha counting source was prepared by micro-precipitation with copper sulfide (CuS) for polonium and neodymium fluoride (NdF{sub 3}) for actinides. The efficiency and reliability of the procedures were tested by analyzing filter, drinking water and frack sand samples. The method is simple, robust and can be performed quickly with excellent removal of interferences, high chemical recovery and very good alpha peak resolution. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2026

An Updated Picture of Presolar History from Short-lived Radioactive Isotopes and Inferences on the Birth of the Sun

We examine the origin of the short-lived radionuclides (SLRs; defined as having half-lives between 0.1 and 100 Ma) present in the early solar system (ESS) by investigating how predictions of their abundances in the interstellar medium (ISM) from steady-state equilibrium relate to their ESS values. For this, we take into account the non-negligible time t iso elapsed between the isolation of the presolar molecular cloud and the formation of the ESS, during which the SLRs decayed freely. We also consider the alternative scenario in which the presolar molecular cloud remained partially mixed with the ISM, with a mixing timescale t mix . We find that the ESS abundances of 107 Pd and 182 Hf produced by slow neutron captures (s-process) and of 53 Mn and 60 Fe produced by explosive nucleosynthesis can be consistently explained within these scenarios. Their required tiso is 9–12 Ma and their required tmix is 11–14 Ma (with one potential exception of t mix = 38 Ma), depending on galactic uncertainties, such as the galactic star formation history and efficiency and the star-to-gas mass ratio. Another s -process SLR, 205 Pb, has a more uncertain ESS value and falls within only some of these time values. The same applies to the SLRs produced by the p -process ( 92 Nb and 146 Sm), depending on the latter’s half-life. In agreement with previous studies, we find that the ESS abundances of the rapid neutron-capture isotopes ( 129 I, 244 Pu, and 247 Cm) and of the most short-lived radionuclides ( 26 Al, 36 Cl, and 41 Ca) cannot be explained by assuming steady-state equilibrium in the ISM.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Gamma ray analysis of the K2 containers

The K2 containers contain PuO2 with 238 Pu being the most abundant isotope of all plutonium isotopes. The purpose of this analysis is to determine the light element impurities in the PuO2. These light elements can interact with the alpha particles from plutonium decay to release gamma rays, protons, and neutrons through the reactions (α,α’), (α,p), and (α,n) respectively. The gamma rays released by the interactions can be measured and compared with the gamma rays released by the plutonium. The ratios of the gamma rays from the interactions and the plutonium gamma rays allow for the determination of the impurities in the items. The elements that can be detected are Lithium (Z=3), Beryllium (Z=4), Boron (Z=5), Fluorine (Z=9), Sodium (Z=11), Magnesium (Z=12), Aluminum (Z=13), Silicon (Z=14), Phosphorous (Z=15), Chlorine (Z=17), and Potassium (Z=19).

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Microextraction–TQ–ICP–MS for the Direct Analysis of U and Pu from Cotton Swipes

Here, the microextraction sampling technique was integrated with triple quadrupole–inductively coupled plasma–mass spectrometry (TQ–ICP–MS) to directly sample and measure the isotopic compositions of uranium (U) and plutonium (Pu) from cotton swipes. Once extracted, the U/Pu were directed into the TQ–ICP–MS instrument for isotopic determination. Carbon dioxide (CO 2 ) and helium (He) gases were delivered to a collision reaction cell within the ICP–MS system for ion separation. The CO 2 reacts with the U + forming UO + which is ultimately separated from the Pu + ions of interest in the third quadrupole. This study demonstrates direct liquid extraction of U/Pu from a solid surface and subsequent measurement by TQ–ICP–MS in <60 s. Flow rates were optimized (0.3 mL min –1 CO 2 and 5 mL min –1 He) in the reaction cell of the ICP–MS system to maximize the Pu signal while minimizing U interferences (i.e., 238 U + tail and 238 UH + ) at m/z 239. Low levels of Pu (~2 pg) were deposited on a cotton swipe along with U at concentrations ranging from 20 to 200 ng. The 240 Pu/ 239 Pu ratio was measured with <7% relative difference from the certified value at all U concentrations. Major and minor U isotope ratios were also measured with <4% relative difference. This highlights that the microextraction–TQ–ICP–MS method can extract a mixed U/Pu sample directly from a cotton swipe and measure both isotopic systems without chemical separation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Measuring Neptunium Concentration using Optical Spectrometry for the Pu-238 Supply Program

Targets containing 237 Np are irradiated at the High Flux Isotope Reactor at Oak Ridge National Laboratory to produce 238 Pu, as plutonium dioxide (PuO 2 ), a heat source material for use in future NASA space missions. Kilogram quantities of Np are processed yearly and developing methods to efficiently characterize and monitor the Np processing streams with optical spectroscopy and real-time monitoring software is a critical aspect of this effort. Here, we evaluate how ultraviolet/visible/near-infrared (UV-Vis-NIR) absorbance and Raman spectroscopic techniques are applicable to characterizing concentrated Np solutions and provide proof-of-principle and proof-of-concept results for each technique. Both techniques were tested in lab-scale studies and should improve the timeliness of production efforts. However, spectrophotometry is the more mature option and has been successfully demonstrated in a hot cell environment. An overview of the initial findings, a brief demonstration, and areas for future work will be highlighted in this report.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Multi-element isotopic analysis of hot particles from Chornobyl

Microscopic fuel fragments, so-called “hot particles”, were released during the 1986 accident at the Chornobyl nuclear powerplant and continue to contaminate the exclusion zone in northern Ukraine. Isotopic analysis can provide vital information about sample origin, history and contamination of the environment, though it has been underutilized due to the destructive nature of most mass spectrometric techniques, and inability to remove isobaric interference. Recent developments have diversified the range of elements that can be investigated through resonance ionization mass spectrometry (RIMS), notably in the fission products. The purpose of this study is to demonstrate the application of multi-element analysis on hot particles as relates to their burnup, particle formation in the accident, and weathering. The particles were analysed with two RIMS instruments: resonant-laser secondary neutral mass spectrometry (rL-SNMS) at the Institute for Radiation Protection and Radioecology (IRS) in Hannover, Germany, and laser ionization of neutrals (LION) at Lawrence Livermore National Laboratory (LLNL) in Livermore, USA. Comparable results across instruments show a range of burnup dependent isotope ratios for U and Pu and Cs, characteristic of RBMK-type reactors. Results for Rb, Ba and Sr show the influence of the environment, retention of Cs in the particles and time passed since fuel discharge.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Cumulative fission yields of short-lived fission products from 235 U and 239 Pu measured by HPGe gamma-ray spectroscopy

In this study, we present a preliminary investigation focused on determining cumulative fission yields for short-lived fission products. Our analysis involves examining gamma spectra from the irradiated samples of 235 U and 239 Pu using the High Flux Isotope Reactor. The motivation stems from the observed discrepancy in the antineutrino energy spectrum within the range of 5 to 7 MeV. While several hypotheses have been proposed, a thorough analysis of fission yields provides an additional way of gaining insight into this unexplained phenomenon. Our study suggests that the measured gamma rays from 100 Nb, 140 Cs and 95 Sr are consistent with the expected values. However, 93 Rb, 96 Y, 97 Y and 142 Cs cannot be quantified due to insufficient statistics, interference from other gamma rays and the Compton scattering background. Additionally, the calculated cumulative fission yields based on the measured 140 Cs and 95 Sr are found to be consistent with the JEFF3.3 fission yield library. In conclusion, the present work shows that the potential of improving gamma-ray spectroscopy in the fission yields as a means to improve our understanding of the antineutrino spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗