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This presentation covers noteworthy changes from VIII.1beta0/1 to VIII.1beta2. 6 Li has been fixed (also seen in 7 Li sphere). For 9 Be: we would recommend studying what nuclear data led to an increase in C/E right after peak. For Pb isotopes: we are concerned about new structures introduced after peak. Finally discussed for 239 Pu: Is it worth improving right now?
The aim of this project is to develop methodology to identify and analyze U and Pu containing particles using laser ablation MC-ICP-MS. The final methodology will ultimately be described in a detailed procedural document that will be shared with IAEA-NWAL laboratories. In this report, we describe the Task-1 deliverable; the setup and optimization of hardware required to perform U isotopic analyses by laser ablation MC-ICP-MS.
Idaho National Laboratory (INL) has supported the production of Pu-238 for future NASA deep space missions since 2017. Over this time, INL has worked to improve the qualification process of Pu-238 production targets as well as improve processes related to the shipping, storage, irradiation, and storage of Pu-238 production targets. Qualification of Pu-238 production targets began with flux measurements and scoping analysis to provide fundamental data to confirm the impacts on the operation of the Advanced Test Reactor (ATR), Fig1. Later, initial production targets were irradiated in ATR’s I-7 position, and then the South Flux Trap (SFT). A modified target design was then implemented which would use the full length of the ATR core and increase Pu-238 production. While working to improve and streamline the qualification of the Pu-238 production targets, INL worked to improve multiple operational aspects of the Pu-238 production process. These changes include updating procedures to streamline operations, supporting modification of shipping containers to contain five rather than one production target, reviewing target receipt procedures and changing work flow to provide flexibility in target receipt, and designing and fabricating support equipment for the storage and internal transfer of production targets.
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This project will develop methodology to identify and analyze U and Pu containing particles using laser ablation MC-ICP-MS. The proposed work will involve: i) setup and optimization of the LA-MC-ICP-MS system, ii) testing and validation by analysis of QC standards, iii) designing analytical protocols for single particles, and iv) developing a data processing system. Ultimately, this project will output a detailed operating procedure documenting the experimental techniques and data processing routines required to perform particle identification and analysis by laser ablation MC-ICP-MS, that can be shared with IAEANWAL laboratories.
A MS Excel tool was created to help track Pu-238 production, Np-237 feedstock use, estimate production scenarios, and coordinate planning for shipments. As-run estimates were used as a basis for beginning and end of life isotopic concentrations. Multiple target types were created to demonstrate a proof of concept while actual results were not yet available The initial goals of this production tool were: • Track unirradiated, currently irradiated, and irradiated targets at the Advanced Test Reactor (ATR) • Estimate production yields from irradiated targets in various positions for each cycle • Provide past, current, and future year quantities of Np-237 and Pu-238 at ATR, amounts shipped to ATR and amounts shipped from ATR • Estimate production from current and future target designs based on data from numerical modeling (values will be provided by Idaho National Laboratory (INL)) • After proof of principle, additional work is planned that will further enhance the tool with: o Incorporate the High Flux Isotope Reactor (HFIR) reactor at Oak Ridge National Laboratory (ORNL) for irradiation o Incorporate irradiations and target shipments from ORNL to INL and back to track Np-237 transfers across the Department of Energy (DOE) Complex
Uranium interference is a major problem in conventional 238 Pu analysis. In RIMS, a slight detuning of the resonance laser extinguishes the Pu signal so that the 238 U interference can be accurately quantified and subtracted.
Previously, we presented actinide isotopic and elemental data from fallout melt glass that was measured using high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS). Direct comparison between these measurements and ‘gold standard’ data obtained by multi-collector ICP-MS showed broad overlap, indicating that HR-ICP-MS is a potentially valuable technique for producing actinide elemental and isotopic data on a relatively rapid timescale. To test the usefulness of this technique further, we doped varying amounts of uranium certified reference materials (CRMs) into a rhyolitic rock standard to establish the effects of uranium concentration and isotopic composition on the accuracy of uranium isotopic analyses by HR-ICP-MS. This also enabled us to quantify peak tailing effects from 238 U on the measurement of 239 Pu and 237 Np, which in turn allows us to constrain correction factors based on measured 237 Np/ 238 U and 239 Pu/ 238 U ratios. A second doping study involved the addition of a mixed actinide standard into three samples with different matrix compositions (termed soil, city, and seawater) to assess whether sample chemistry affects the accuracy and precision of these analyses. Results suggest that this is not the case. Systematic offsets were not observed in elemental or isotopic data derived from the three matrix samples. Results indicate that useful actinide isotopic data can be obtained from whole rock solutions by HR-ICP-MS. Our findings also have implications for solid sampling techniques such as laser ablation ICP-MS, which do not require sample dissolution.
Heavy atoms present challenges to atomic theory calculations due to the large number of electrons and their complicated interactions. Conventional approaches such as calculations based on Cowan’s code are limited and require a large number of parameters for energy agreement. One promising approach is relativistic configuration-interaction and many-body perturbation theory (CI-MBPT) methods. We present CI-MBPT results for various atomic systems where this approach can lead to reasonable agreement: La I, La II, Th I, Th II, U I, Pu II. Among atomic properties, energies, g-factors, electric dipole moments, lifetimes, hyperfine structure constants, and isotopic shifts are discussed. While in La I and La II accuracy for transitions is better than that obtained with other methods, more work is needed for actinides.
As part of the nuclear data evaluation and validation cycle, the ENDF/B-VIII.0 cross-section library released in 2018 requires testing to determine areas of improvement and deterioration. Previous work by the authors investigated the performance of 16 O, 56 Fe, and 63,65 Cu cross sections, with this study acting as an extension of the prior work. In addition to the isotopes and nuclear criticality safety benchmarks of interest to the prior work, benchmarks from the International Criticality Safety Benchmark Evaluation Project Handbook were selected for their k eff sensitivity to 1 H, C, 58,60 Ni, 182,183,184,186 W, 235,238U, or 239 Pu cross sections and were modeled in the SCALE code system maintained by Oak Ridge National Laboratory. In total, 253 benchmark configurations were selected for their sensitivities and modeled using SCALE 6.2.4 Criticality Safety Analysis Sequences (CSAS) continuous-energy Monte Carlo k eff calculations. This collection includes and expands upon the 99 benchmarks in the prior work. The AMPX-processed ENDF/B-VIII.0 library was decomposed into individual ENDF/B-VIII.0 datum libraries for each isotope of interest. Doing so allowed for the individual substitution of an ENDF/B-VIII.0 cross section in the place of ENDF/B-VII.1, determining isotope-specific effects of ENDF/B-VIII.0 relative to ENDF/B-VII.1. Full library calculations with entirely ENDF/B-VII.1 data or entirely ENDF/B-VIII.0 data were also executed. As a measure of performance, the average relative deviation was determined as the ratio of the deviation between calculated and experimental keff to the propagated calculational and experimental uncertainty. With calculated full library and isotope-specific ENDF/B-VIII.0 k eff ’s, an optimized combination of data libraries was estimated and confirmed with SCALE calculations. This showed that reverting 239 Pu, 58 Ni, 16 O, and 65 Cu cross sections to ENDF/B-VII.1 resulted in improved performance relative to the full ENDF/B-VIII.0 library. Across all 253 benchmarks, the average relative deviation was 1.29σ for the full ENDF/B-VII.1 library, 1.17σ for the full ENDF/B-VIII.0 library, and 0.97σ for the optimized combination. The reversion of 239 Pu, 58 Ni, 16 O, and 65 Cu cross sections to ENDF/B-VII.1 in the 99 benchmarks of the prior work resulted in further improved experimental agreement compared to the previously reported improvement from 16 O and 65 Cu alone. Therefore, it is suggested that applications with significant sensitivities to 239 Pu, 58 Ni, 16 O, and 65 Cu consider their choice of nuclear data library.
Idaho National Laboratory (INL) has an ongoing effort to produce Pu-238 for NASA deep space missions. Recent work at INL has consisted of irradiation of Pu 238 production targets in the Advanced Test Reactor (ATR), generating more than an estimated 400 grams of Pu-238 heat source material between March and October 2023. Additionally, INL began qualifying Pu-238 production targets with a higher loading of Np-237 to further increase the production of Pu-238 production in later years. INL has also updated the analysis as a result of operational changes at ATR. One instance was updating the analysis to enable a single Pu-238 production target to be run in ATR’s South Flux Trap (SFT), rather than the previous seven production targets, to make use of a spare target from a discontinued design. Higher lobe powers in ATR were also analyzed due to potential changes in planned lobe powers.
A highly-enriched 233 U reference material (>0.99987 n( 233 U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233 U to further reduce trace amounts of contaminant Pu in the material. The purified 233 U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Furthermore, modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233 U certified reference materials.
Deep space exploration requires specialized sources for both thermal and power applications. Radioactive decay heat of plutonium-238 (238Pu) provides these sources in the form of radioisotope thermoelectric generators (RTGs). The 238 Pu is produced via neutron capture reaction involving neptunium-237 ( 237 Np) target material. Continual optimization of 237 Np target materials and evaluation of potential alternative targets for production of 238 Pu RTGs are advantageous for meeting ongoing space power system resource requirements. Current production of 238 Pu for RTGs for the United States space program utilizes neptunium dioxide ( 237 NpO 2 ) targets; however, the use of neptunium mononitride ( 237 NpN) presents an opportunity to increase the mass of 237 Np per target compared to the dioxide form, as well as increase the thermal conductivity of the target. To assess the viability of a 237 NpN target material, the material chemistry must be thoroughly evaluated, including synthesis methods and dissolution and reprocessing schemes. This review presents a summary of synthesis pathways for 237 NpN based on published literature on actinide mononitrides. Specific literature on 237 NpN is limited, necessitating evaluation of other actinide systems to gather parallels. This suggests a need for additional experimental studies on 237 NpN. A particular limitation in the existing literature is a lack of information on the differences in material characteristics, such as morphology, particle size, and trace chemical impurities, as a function of synthesis method. These parameters may affect subsequent reactor performance or dissolution of irradiated targets. The evaluation of existing literature is presented with a focus on the efficacy of 237 NpN targets for 238 Pu production.
Idaho National Laboratory (INL) has continued in the effort to produce Pu-238 to support NASA deep space missions. In support of the production goal of contributing 700 g to the 1.5 kg per year constant rate production of Pu-238 heat source material in the United States by 2026. All available inner core positions of the Advanced Test Reactor (ATR) have been qualified for production for a 20% Np target, with efforts nearing completion for a 30% Np target further increasing production amounts. This includes the North East Flux Trap (NEFT), South Flux Trap (SFT), Inner A, H positions. With the completion of qualifying the inner core of ATR, work has started on the qualifying the outer core. The portion of the outer core that will produce Pu-238 includes the Large and Medium I positions. With the continued qualification work, INL is on track to contribute to the production goal by 2026.
This analysis was completed to support the irradiation of plutonium fuel services (PFS) targets in the NEFT in the Advanced Test Reactor (ATR) as a part of the campaign to restart domestic production of plutonium-238 used in radioisotope power systems (RPS) by the National Aeronautical and Space Administration (NASA) and Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Nuclear Infrastructure Program (NE-3). Referred to as the PFS-ATR-GEN1-NEFT experiment, the assembly was designed to hold 46 PFS targets in the NEFT. The scope of this paper is to outline the MOPY method used to calculate the heat generation rates (HGRs), flux, fission density, and quantify the viability of the target design for Pu-238 production in ATR.
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 to 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 July 2023.
Technologies that enable near real-time isotopic analysis of advanced molten salt reactor (MSR) fuels are critically needed to safeguard these reactors, increase their operational efficiency, and enable their widespread deployment with confidence. We present a systematic approach to developing near real-time dissolution and chemical isolation of U, Pu, and major fission products from highly radioactive chloride molten salt samples. Chemical yields greater than 95% were observed for both uranium and the lanthanides. Interference reduction enabled the detection and quantification of key diagnostic isotopes (including 112Ag, 147Nd, and 153Sm) that were previously undetectable in the original sample. The results from this initial scoping study lay the foundation for the development of future automated systems that can enable cost-efficient, near-real time chemical separation and analysis of extremely highly radioactive molten salt samples.
Classifiers for dissolution events at a radiochemical processing facility are studied using gamma spectra measurements of effluents collected by a high purity germanium detector located at its off-gas stack. Data sets collected at the Oak Ridge National Laboratory’s Radiochemical Engineering Development Center under a Pu dissolution campaign spanning a three months period are utilized. Features corresponding to the activity levels of 15 radionuclides, including isotopes of iodine, krypton, and xenon, that are indicated by the target decay chains, are computed from the spectra at 1 hour intervals. A conceptualization diagram is developed to reflect the steps from the source to measurement to feature computation that depend on fission products indicated by decay chains, chemical processing, and effluents transport to the off-gas stack. A diverse set of eight classifiers based on different design principles are trained using the ground truth data for this campaign, and the outputs of top three classifiers, namely, classification trees, Ensemble of Trees (EOT), and k-nearest neighbor, are combined using EOT classifier-fuser. Our results show that for 5-fold cross validation, features associated with isotopes of xenon provide the lowest classification error among the different elements across the classifiers; the classification error is furthered improved when all 15 isotope features are used by each classifier, and it is again improved by the fusion of three classifiers. Further reduction in classification error is achieved by using a measurement window of 1-2 days which is identified based on half-life time estimates of the isotopes; it is long enough for the stabilization of feature estimates while being short enough not to be affected by the follow on dissolution events. As a net result of feature and classifier fusion, combined with the incorporation of decay chain and isotope half-life information, this approach achieves 98% detection rate while maintaining a false alarm rate under 2% for this data set.