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DOE OSTI2024

Gamma-ray imaging of Np-237 metal using an organic glass imager

Neutron and gamma-ray imaging systems are deployed within the field of nuclear safeguards for the detection and localization of special nuclear materials and other materials of interest. 237 Np is one of these materials of interest due its presence in spent nuclear fuel and potential for use in nuclear weapons when purified. Here, for the first time, a 6 kg neptunium sphere (98.8 wt% 237 Np) was measured using a dual-particle imager, from the University of Michigan, consisting of organic glass and inorganic scintillators. The novel composition of organic glass scintillator was recently developed at Sandia National Labs and has been used in particle imaging systems due to its time resolution and particle discrimination capabilities. Gamma-ray energy spectra from single and coincident events were extracted and the sequencing of Compton scatter and photoelectric absorption gamma-ray events was used to generate images using simple backprojection. The emissions of interest in this work are the 312 keV and 416 keV gamma rays from 233 Pa, a daughter isotope from the neptunium decay series. The results of this work show that there is close agreement between the true source location in angular space and the converged location from the gamma ray images created using the system. The gamma spectroscopy from single and coincident events also identified the characteristic emission from the daughter isotope and could be used to assist with the identification of 237 Np. Furthermore, successful localization of the source with 5 s of data demonstrates the practical application of the imaging system for imaging and detection of material in weapons-useable quantities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Comparative uptake, translocation, and plant mediated transport of Tc-99, Cs-133, Np-237, and U-238 in Savannah River Site soil columns for the grass species Andropogon virginicus

Here, this study examines the ability of the grass species Andropogon virginicus to alter the subsurface transport and redistribution of a suite of radionuclides ( 99 Tc, 133 Cs (stable analog for 135 Cs and 137 Cs), 237 Np, 238 U) with varying chemical behaviors in a Savannah River Site soil via the use of vegetated and unvegetated soil columns. After an acclimation period, a small volume of solution containing all radionuclides was introduced into the columns via Rhizon© pore water sampling tubes. Plants were grown for an additional 4 weeks before shoots were harvested, and columns were prepared for sampling. Plant presence led to decreased radionuclide release from the columns, mainly due to radionuclide specific combinations of system hydrology differences resulting from plant transpiration as well as plant uptake. For the most mobile radionuclides, 99 Tc followed by 237 Np, plant presence resulted in significantly different soil concentration profiles between vegetated and unvegetated columns, including notable upward migration for 237 Np in columns with plants. Additionally, plant uptake of 99 Tc was the greatest of all the radionuclides, with plant tissues containing an average of 44 % of the 99 Tc, while plant uptake only accounted for <2 % of 237 Np and <0.5 % of 133 Cs and 238 U in the system. Although overall plant uptake of 133 Cs and 238 U were similar, the majority of 133 Cs taken up by plants was associated with 133 Cs already available in the aqueous phase while 238 U uptake was mainly associated with the solid phase, meaning that plant activity resulted in a fraction of the native 238 U being mobilized and thus, made available for plant uptake. Overall, this study quantified the influence of several plant-mediated physical and biogeochemical factors that have significant influence on radionuclide mobility and transport in this complex system which can be further utilized in future system or site-specific environmental transport and risk assessment models.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Np-237 LoD Measurement by TIMS-Multi-Ion Counting Total Evaporation [Poster]

Requests for ultra-low-level 237 Np analyses highlight the importance of a robust chemical purification and measurement technique for Np. In FY2022, LANL is quantifying the instrumental 237 Np LoD. Need to incorporate a chemical purification procedure for TIMS-MICTE sample preparation. What is the recovery of the chemical purification procedure? What is the ultimate detection limit that can be achieved while incorporating a chemical purification procedure? We have adapted and refined the Pu TIMS-MICTE method for Np analyses. We have determined expected uncertainties for 237 Np TIMS-MICTE measurements. We have increased sensitivity through technique improvements. We have improved method reliability for Np analyses and increased throughput. Apply knowledge gained from progress made in FY2022 to further develop Np sample purification and analyses by TIMSMICTE.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Pu-238 Production Calculator and Estimation Tool

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

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2022

Progress on Pu-238 Production at INL From March 2021 to February 2022

Idaho National Laboratory has completed irradiation of Np-237 targets in the Advanced Test Reactor’s (ATR) South Flux Trap (SFT) and I-7 positions. INL also progressed qualification of new ATR Gen 1 Np-237 targets for the North East Flux Trap (NEFT), inner A, and H positions. This slide show is based upon artifact INL/CON-22-65729-Rev000 and gives an overview of operational and technical activities from March 2021 to February 2022.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2022

Progress on Pu-238 Production at Idaho National Laboratory From March 2021 to February 2022

Idaho National Laboratory has completed irradiation of Np-237 targets in the Advanced Test Reactor’s (ATR) South Flux Trap (SFT) and I-7 positions. INL also progressed qualification of new ATR Gen 1 Np-237 targets for the North East Flux Trap (NEFT), inner A, and H positions. This paper gives an overview of operational and technical activities from March 2021 to February 2022.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2023

BRR Cask Use for Pu-238 Isotope Production

The Department of Energy (DOE), in partnership with its national laboratories and the National Aeronautics and Space Administration (NASA), is responsible to produce Pu-238 isotope in the United States for use in space exploration. Major activities in the DOE complex are focused at Idaho National Laboratory (INL) and Oak Ridge National Laboratory (ORNL). INL is responsible for storing Np-237 feedstock, irradiation qualification in the Advanced Test Reactor (ATR), and irradiating targets containing Np-237 to produce Pu-238. ORNL is responsible for target design, target fabrication, irradiation qualification in HFIR, and processing of targets to extract Pu-238 heat source material. A key part of the program lifecycle is moving irradiated targets from INL to ORNL. The BEA Research Reactor (BRR) cask was identified as a potential shipping cask for the transport of both unirradiated and irradiated targets between the project sites. This paper will discuss the production at INL and shipment of Pu-238 to ORNL using the BRR cask.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2024

Progress on Pu-238 production at Idaho National Laboratory from February 2022 to July 2023

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.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2021

Distribution of U, Pu and Np in a Mo-99 Recovery Process using Sachtopore NP (titania based) Absorbent Material

A laboratory scale mockup of a prototypical Mo-99 recovery process has been operated in a radioactive materials hood at Savannah River National Laboratory. This equipment has been operated with realistic concentrations of uranium (U-238), plutonium (94% Pu-239), neptunium (Np-237), and non-radioisotopes of common fission products (including Mo). The goal of this work was to determine the amounts of U, Pu, and Np in the liquid waste streams created by the wash streams for the production process. The key question was how the initial acid wash volume will be handled, as this solution contains residual raffinate which amounted to ~ 3% ofthe mass ofthe feed solution in this experiment. If the initial 1.9 bed volumes (BV) of acid wash were recycled as in this experiment then the combined wash solutions can be expected to contain 0.4 g U/L, 2.7 pg Pu/L and < 14 pg Np/L. If, on the other extreme, the entire acid wash solution was discarded as waste, then the combined wash solutions can be expected to contain 11 g U/L, 3.8 pg Pu/L and ~ 80 pg Np/L. The Sachtopore NP absorbent (for Mo-99 recovery) retains a minuscule fraction ofthe U (2.3 mg U per g titania or 0.03% ofthe U in the feed). The uncertainties are too large to determine how close the absorbent is to saturation with U. Less mass but a higher fraction ofthe total Np was retained by the absorbent (0.7 pg Np per g titania or ~2% of the Np in the feed). As has been reported elsewhere, a large fraction ofthe Pu fed to the titania bed was retained by the absorbent (92% of Pu in the feed or 20 pg per g titania).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Hanford Site Composite Analysis: LLBG-200-W B Vadose Zone Model

The objectives of the vadose modeling for the updated Hanford Site Composite Analysis (CA) are to simulate the flow and transport of water and radionuclide releases from the surface to the water table and to provide radionuclide transfer rates to the CA saturated zone model (CP-57037, Model Package Report: Plateau to River Groundwater Model, Version 8.3). Water additions include natural recharge and water discharged to the ground as a result of industrial processes associated with Hanford Site operations. Contaminant sources include radionuclides in water discharged to the ground during operations and radionuclides disposed “dry” in solid waste burial grounds or other means. The following 16 radionuclides were selected for this modeling effort: carbon-14 (C-14), chlorine-36 (Cl-36), tritium (H-3), iodine-129 (I-129), neptunium-237 (Np-237), rhenium-187 (Re-187), strontium-90 (Sr-90), technetium-99 (Tc-99), uranium-232 (U-232), uranium-233 (U-233), uranium-234 (U-234), uranium-235 (U-235), uranium-236 (U-236), uranium-238 (U-238), radium-226 (Ra-226), and thorium-230 (Th-230). The simulation time starts in 1943 and ends at 12070, which is 10,000 years after assumed Hanford Site closure in 2070. The parallel version of the Subsurface Transport Over Multiple Phases (STOMP 1 ) simulator, officially named the exascale Subsurface Transport Over Multiple Phases (eSTOMP), is used to simulate flow and transport for the vadose models. The documentation for the STOMP code is comprehensive. The theoretical and numerical approaches applied in the STOMP code are documented in a published theory guide (PNNL-12030, STOMP Subsurface Transport Over Multiple Phases Version 2.0 Theory Guide). The code has undergone a rigorous verification procedure against analytical solutions, laboratory-scale experiments, and field-scale demonstrations. The application guide (PNNL-11216, STOMP Subsurface Transport Over Multiple Phases Application Guide) provides instructive examples in the application of the code to classical groundwater problems. The user’s guide (PNNL-15782, STOMP: Subsurface Transport Over Multiple Phases Version 4.0: User’s Guide) describes the general use, input file formatting, compilation, and execution of the code. The primary output of the vadose zone modeling is radionuclide transfer rates to the groundwater for input into the saturated zone model. The rates will be summed over the 100 by 100 m saturated zone model grid cells that fall within the vadose zone model source domain.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Vadose Zone Model for B-63 Area for Composite Analysis (Rev. 1)

The objectives of the vadose modeling for the updated Hanford Site composite analysis (CA) are to simulate the flow and transport of water and radionuclide releases from the surface to the water table and to provide radionuclide transfer rates for the plateau to river (P2R) model, version 8.3 (CP-57037, Model Package Report: Plateau to River Groundwater Model, Version 8.3). Water additions include natural recharge and water discharged to the ground as a result of industrial processes associated with Hanford Site operations. Contaminant sources include radionuclides in water discharged to the ground during operations and radionuclides disposed “dry” in solid waste burial grounds or other means. The following 16 radionuclides were selected for this modeling effort; carbon-14 (C-14), chlorine-36 (Cl-36), tritium (H-3), iodine-129 (I-129), neptunium-237 (Np-237), rhenium-187 (Re-187), strontium-90 (Sr-90), technetium-99 (Tc-99), uranium-232 (U-232), uranium-233 (U-233), uranium-234 (U-234), uranium-235 (U-235), uranium-236 (U-236), uranium-238 (U-238), radium-226 (Ra-226), and thorium-230 (Th-230). The simulation time starts in 1943 and ends at 12070, which is 10,000 years after assumed Hanford Site closure in 2070.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Vadose Zone Model for LLBG-200W A for Composite Analysis

The objectives of the vadose modeling for the updated Hanford Site composite analysis (CA) are to simulate the flow and transport of water and radionuclide releases from the surface to the water table and to provide radionuclide transfer rates for the plateau to river (P2R) model, version 8.3 (CP-57037, Model Package Report: Plateau to River Groundwater Model, Version 8.3). Water additions include natural recharge and water discharged to the ground as a result of industrial processes associated with Hanford Site operations. Contaminant sources include radionuclides in water discharged to the ground during operations and radionuclides disposed “dry” in solid waste burial grounds or other means. The following 16 radionuclides were selected for this modeling effort: carbon-14 (C-14), chlorine-36 (Cl-36), tritium (H-3), iodine-129 (I-129), neptunium-237 (Np-237), rhenium-187 (Re-187), strontium-90 (Sr-90), technetium-99 (Tc-99), uranium-232 (U-232), uranium-233 (U-233), uranium-234 (U-234), uranium-235 (U-235), uranium-236 (U-236), uranium-238 (U-238), radium-226 (Ra-226), and thorium-230 (Th-230). The simulation time starts in 1943 and ends at 12070, which is 10,000 years after assumed Hanford Site closure in 2070.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Vadose Zone Model for LLBG-200W A for Composite Analysis

The objectives of the vadose modeling for the updated Hanford Site composite analysis (CA) are to simulate the flow and transport of water and radionuclide releases from the surface to the water table and to provide radionuclide transfer rates for the plateau to river (P2R) model, version 8.3 (CP-57037, Model Package Report: Plateau to River Groundwater Model, Version 8.3). Water additions include natural recharge and water discharged to the ground as a results of industrial processes associated with Hanford Site operations. Contaminant sources include radionuclides in water discharged to the ground during operations and radionuclides disposed "dry" in solid waste burial grounds or other means. The following 16 radionuclides were selected for this modeling effort: carbon-14 (C-14), chlorine-36 (Cl-36), tritium (H-3), iodine-129 (I-129), neptunium-237 (Np-237), rhenium-187 (Re-187), strontium-90 (Sr-90), technetium-99 (tc-99), uranium-232 (U-232), uranium-233 (U-233), uranium-234 (U-234), uranium-235 (U-235), uranium-236 (U-236), uranium-238 (U-238), radium-226 (Ra-226), and thorium-230 (Th-230). The simulation time starts in 1943 and ends at 12070, which is 10,000 years after assumed Hanford Site closure in 2070.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Vadose Zone Model for B-63 Area for Composite Analysis (Rev. 2)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

OVERVIEW OF RECENT PU-238 PRODUCTION ACTIVITIES AT IDAHO NATIONAL LABORATORY

The Plutonium Fuel Services (PFS) program at Idaho National Laboratory (INL) is active in the qualification of irradiation targets containing Np-237 for irradiation in the Advanced Test Reactor (ATR) to produce Pu-238 for future NASA missions. INL qualified and loaded 7 targets in ATR’s South Flux Trap (SFT) for cycle 169A, which occurred in Spring 2021. This program was reinitiated after two baseline production targets in three positions validated significant production of Pu-238 [ref.1]. The validation model was followed by the PFS-1 experimental test in the ATRC (Critical) facility [ref.2]. This paper outlines the progress and status of the PFS program. The qualification effort, safety analysis, hardware status, and future activities for qualification of an updated target design for use in the ATR will be discussed.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Pu-238 Production Calculator and Estimation Tool in the Advanced Test Reactor

A MS Excel tool was created to help track Pu-238 production, Np-237 feedstock use, estimate production scenarios, and coordinate planning for shipments at the Idaho National Laboratory (INL) and Advanced Test Reactor (ATR). 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.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Progress on Pu-238 Production at Idaho National Laboratory 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 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↗