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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 ↗

NASA NTRSDate not supplied

Am-241 Powered Dynamic Radioisotope Power System (DRPS) for Long Duration Lunar Rovers

For more than half a century most deep space and planetary missions have utilised Pu-238 as the isotope of choice for fuelling radioisotope thermoelectric generators and radioisotope heater units. In Europe, Am-241 based fuel has been selected and developed as part of the European Space Agency funded radioisotope power system program to provide technology solutions in the form of radioisotope thermoelectric generators and radioisotope heater units. A concurrent design study, in collaboration with NASA Glenn Research Centre, has been undertaken to design and develop a dynamic radioisotope power conversion concept that uses the European Large Heat Source. This is a 200 Wth Am-241 based heat source being developed for ESA and is an essential building block for the University of Leicester led radioisotope thermoelectric generator programme. This study aims to expand on the applications of the Am-241 based heat source within and outside Europe. The advancement in Am-241 power technologies could give rise to a suitable and sustainable addition to current Pu-238 based technologies, making the solar system and beyond more accessible for science and exploration mission.

Dynamic Radioisotope Power System↗

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↗

NASA NTRS1977

Isotopic and chemical investigations on Angra dos Reis

Isotope ratios and chemical abundance measurements for a variety of elements are reported for total meteorite and mineral separates of the Angra dos Reis achondrite. U-Pb, Th-Pb, and Pb-Pb ages are concordant at 4.54 eons for the total meteorite and for high-purity whitlockite, which indicates that Angra dos Reis is an early planetary differentiate that has not been disturbed for these systems since 4.54 eons ago. The implications of different ratios of Sr-87 and Sr-86 found in different components are discussed. Xe isotopic measurements show that Pu-244 was enriched in the whitlockite relative to the pyroxene by a factor of about 18. Chemical enrichment factors between the whitlockite and the fassaitic pyroxene in Angra dos Reis are presented

Wasserburg, G. J.↗

NASA NTRS1992

Search for Cm-248 in the early solar system

Possible evidence for the presence of Cm-248 in the early solar system was reported from fission gas studies (Rao and Gopalan, 1973) and recently from studies of very high nuclear track densities (not less than 5 x 10 exp 8/sq cm) in the merrillite of the H4 chondrite Forest Vale (F.V.) (Pellas et al., 1987). We report here an analysis of the isotopic abundances of xenon in F.V. phosphates and results of track studies in phosphate/pyroxene contacts. The fission xenon isotopic signature clearly identifies Pu-244 as the extinct progenitor. We calculate an upper limit Cm-248/Pu-244 to be less than 0.0015 at the beginning of Xe retention in F.V. phosphates. This corresponds to an upper limit of the ratio Cm-248/U-235 of not greater than 5 x 10 exp -5 further constraining the evidence for any late addition of freshly synthesized actinide elements just prior to solar system formation. The fission track density observed after annealing the phosphates at 290C (1 hr, which essentially erases spallation recoil tracks) is also in agreement with the Pu-244 abundance inferred from fission Xe. The spallation recoil tracks produced during the 76 Ma cosmic-ray exposure account for the very high track density in merrillites.

Lavielle, B.↗

NASA NTRS1987

Al-26, Pu-244, Ti-50, REE, and trace element abundances in hibonite grains from CM and CV meteorites

Hibonites from the CM meteorites Murchison, Murray, and Cold Bokkeveld, and hibonites and Ti-rich pyroxene from the CV chondrite Allende are studied. Electron microprobe measurements of major element concentrations and track and ion probe measurements of Mg and Ti isotopic ratios, rare earth elements (REEs), and trace element abundances are analyzed. Correlations between isotopic anomalies in Ti, Al-26, Pu-244, and Mg-26(asterisk) are examined. Ti isotopic anomalies are compared with REE and trace element abundance patterns. Reasons for the lack of Al-26 in the hibonites are investigated and discussed. It is observed that there is no correlation between the Ti isotopic compositions, and the presence of Mg-26(asterisk), Pu-244, and REE and trace element patterns in individual hibonite samples. The data reveal that hibonites are not interstellar dust grains but formed on a short time scale and in localized regions of the early solar system.

Fahey, A. J.↗

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↗

NASA NTRS1985

Noble gas component organization in Apollo 14 breccia 14318 I-129 and Pu-244 regolith chronology

Drozd et al. (1972) have first detected the presence of Xe-129 in lunar material. Bernatowicz et al. (1979, 1980) established that this xenon component resides exclusively on grain surfaces and confirmed previous observations that it is less tightly bound than other surface components. The present investigation extends many of the observations made on the basis of a study of the 14301 to 14318, which is the only other lunar regolith breccia for which the isotopic structure of 'parentless xenon' has been accurately resolved. Actually this isotope has two parents, including Pu-244 and I-129, which are both now extinct. Attention is given to the analyzed samples, the employed analytical methods, the petrology and chemistry of the grain size separates, and stepwise heating experiments. On the basis of the obtained results, it is concluded that the I-Pu-Xe system can be used as a chronometer.

Swindle, T. D.↗

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↗

NASA NTRS2008

Radioisotope Power: A Key Technology for Deep Space Exploration

A Radioisotope Power System (RPS) generates power by converting the heat released from the nuclear decay of radioactive isotopes, such as Plutonium-238 (Pu-238), into electricity. First used in space by the U.S. in 1961, these devices have enabled some of the most challenging and exciting space missions in history, including the Pioneer and Voyager probes to the outer solar system; the Apollo lunar surface experiments; the Viking landers; the Ulysses polar orbital mission about the Sun; the Galileo mission to Jupiter; the Cassini mission orbiting Saturn; and the recently launched New Horizons mission to Pluto. Radioisotopes have also served as a versatile heat source for moderating equipment thermal environments on these and many other missions, including the Mars exploration rovers, Spirit and Opportunity. The key advantage of RPS is its ability to operate continuously, independent of orientation and distance relative to the Sun. Radioisotope systems are long-lived, rugged, compact, highly reliable, and relatively insensitive to radiation and other environmental effects. As such, they are ideally suited for missions involving long-lived, autonomous operations in the extreme conditions of space and other planetary bodies. This paper reviews the history of RPS for the U.S. space program. It also describes current development of a new Stirling cycle-based generator that will greatly expand the application of nuclear-powered missions in the future.

Schmidt, George↗

NASA NTRS2009

Radioisotope Power: A Key Technology for Deep Space Explorations

Schmidt, George R.↗

DOE OSTI2024

Conceptual Spacer Design for the ATR GEN I Target for Pu-238 Production in the Advanced Test Reactor at Idaho National Laboratory

The initial target design used for Pu-238 production at Idaho National Laboratory was designed by Oak Ridge National Laboratory to optimize the production of Pu-238 in the High Flux Isotope Reactor (HFIR) and are referred to as HFIR GEN II targets. To take advantage of the Advanced Test Reactor’s (ATR) taller active core region a redesign of the HFIR GEN II targets was needed. It was proposed to stack two HFIR GEN II targets nose to nose about the core center line; however, this resulted in excessive neutron and photon heating in the pellets located in the center. This peak heating was not desirable so three alternative designs were investigated for the ATR GEN I targets. The python-based code, MCNP to ORIGEN2 in Python (MOPY), was used to calculate the heating rates after 40 days of irradiation to capture the effects of each configuration. The purpose of this paper is to document the details of these conceptual design calculations and comparisons for the ATR GEN I targets.

07 ISOTOPE AND RADIATION SOURCES↗

NASA NTRS1994

Primitive Xe in the atmospheres of Earth and mars

Published data on Xe isotope compositions in primitive carbonaceous meteorites are examined using multidimensional correlation analysis. Distribution of the Xe data in multidimensional data space, except for (129)Xe, can be characterized by a single component, whose isotope composition is identical to 'H plus L minus Xe'. Additional small contributions to the data variations, less than 1 percent of total variations, can be attributed to 'S minus Xe' as well as atmospheric contamination. Isotopic composition of primitive Xe common to the Earth's atmosphere and carbonaceous meteorites are determined with the same assumption as adopted by Pepin and Phinney: primitive Xe is precisely related to fission-free Xe in the Earth's atmosphere by mass fractionation. The determined isotopic composition of primitive Xe is closer to Solar-type Xe, rather than U-Xe (and the primitive Xe estimated from chondrite-achondrite correlation. Hence, the present published data on Xe isotope compositions in meteorites do not seem to require any special component for the primitive Xe common to the Earth's atmosphere and carbonaceous meteorites. Thus Earth's accreting planetesimals would have trapped Xe from the surrounding nebula gases where Xe isotope composition is identical to Solar-type Xe. The trapped Xe was subsequently subject to isotopic fractionation due to gravitational separation as planetesimals grew. Finally fissiogenic Xe from (244)Pu was added to form the present Xe isotope composition of the Earth's atmosphere. The amount of fissiogenic (136)Xe is estimated to be 2.6 percent of the total amount of (136)Xe in the atmosphere, which is about a half of that estimated by Pepin and Phinney (4.65 percent).

Igarashi, G.↗