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At least 55 records · Page 3

Purification and Concentration of 99 Mo from a UREX raffinate

The medical isotope 99m Tc ( t ½ = 6.0 h) accounts for over 80% of isotopes used in diagnostic nuclear medicine today and is normally derived from its transient equilibrium parent 99 Mo ( t ½ = 66 h). To reduce U.S. dependence on 99 Mo derived from HEU by foreign suppliers, the NNSA/M3 program—under the American Medical Isotope Production Act—has been tasked with facilitating the work of domestic 99 Mo suppliers that do not utilize HEU. Superconducting electron linear accelerators with high-Z converter targets can generate bremsstrahlung photons and neutron fluxes that can induce photonuclear reactions and LEU fission. After sufficient production intervals, targets can be rotated out and processed while another batch is irradiated. The process flow chemistry is shown in Figure 1. The irradiated U 3 O 8 targets are retrieved and dissolved in HNO 3 ; the volatile fission products are expelled and captured during this step. The HNO 3 liquor bearing the uranyl, fission and activation products is injected into the UREX suite of liquid-liquid extraction banks. The uranyl is partitioned in typical fashion using tri-$\textit{n}$-butyl phosphate (TBP) in a hydrocarbon diluent. The raffinate—comprising mainly 99 Mo and fission products—is then injected into the MoLLE (Molybdenum Liquid-Liquid Extraction) flowsheet, where the Mo is selectively extracted by an organophosphorous acid extractant such as di-(2-ethylhexyl phosphoric acid) (HDEHP). Trace amounts of Nb, Zr, Np, I, and Te are co-extracted. The Mo is stripped using acetohydroxamic acid (AHA) and fed onto an anion exchange column. Following a series of hydroxide, HCl, and oxalic acid wash steps, the Mo can be recovered in NaOH/NaCl. A manuscript describing this process chemistry in more detail was recently published.

07 ISOTOPE AND RADIATION SOURCES↗

Ion-optical and Associated Magnet Feasibility Study of a High Rigidity Spectrometer

Ion-optical and magnet-feasibility studies were performed for the High Rigidity Spectrometer (HRS) at the Facility for Rare Isotope Beam (FRIB). The High Rigidity Spectrometer (HRS) will be the centerpiece experimental tool of the Facility for Rare-Isotope Beams (FRIB) fast-beam program The high magnetic rigidity of the HRS (8 Tm) will match the rigidities at which rare-isotope production yields at the FRIB fragment separator are maximum across the entire chart of nuclei and enable experiments with the most neutron-rich nuclei available at FRIB. Gain factors in luminosity of up to two orders of magnitude are achievable compared to running with existing spectrometers, which have a maximum rigidity of 4 Tm. The ion-optical studies were performed to ensure that the layout and properties meet the requirements for the scientific program envisioned for and articulated by the FRIB user community. Based on the ion-optical studies, magnet-feasibility studies were carried out to ensure that the magnets required for the HRS meet these requirements and can be constructed. The results of the ion-optical and magnet-feasibility studies form the basis of the pre-conceptual design for the HRS.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Disposition of Newly Generated Transuranic Waste at ORNL - 20107

ORNL operates the High Flux Isotope Reactor, which provides a high neutron source for production of isotopes for medical, industrial, and nuclear research programs and is the US DoE's center for production, storage, and distribution for TRU isotopes (plutonium through californium). Operation of these facilities results in the generation of CH-TRU and RH-TRU waste for disposal at the WIPP. This paper describes the program ORNL is implementing in collaboration with the Carlsbad Field Office National TRU Program Difficult Waste Team to disposition newly generated TRU waste. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Measurement of ( n, γ ) cross section of 90 Zr [Abstract]

The isotopes of Zr with A = [90, 91, 92, 94] make up more than 97% of naturally occurring Zr and are important to many nuclear applications such as nuclear reactors. One of the attractive qualities of naturally occurring Zr isotopes is that they have a low σγ/σt ratio at most neutron energies, such that they improve the neutron economy in reactors by preferentially scattering neutrons rather than absorbing them. This same quality also presents a challenge to measuring the capture cross section, σγ, of Zr isotopes. The ENDF/B-VIII.0 library has a relative uncertainty of approximately 10-20% for incident neutron energies < 0.1 MeV, and uncertainty greater than 20% for energies > 0.1 MeV for the majority of natural Zr isotopes. This motivated the Nuclear Criticality Safety Program (NCSP) to embark on a campaign to accurately measure and evaluate these isotopes of Zr. Here we will show energy-dependent neutron capture cross section measurements for the first enriched sample to be measured: 90 Zr. The measurements of isotopically enriched samples are being carried out at the Geel Electron Linear Accelerator (GELINA) facility of the Joint Research Center - Geel (JRC-Geel) of the European Union. As isotopic enrichment is a costly process we are careful not to activate any of the samples, as this may hinder future radiation-sensitive measurements. The activation analysis is presented in a report by Brown et al.. Once we were satisfied that the Zr samples would not be activated by the measurements, the 90 Zr sample was fabricated at Oak Ridge National Laboratory (ORNL) and shipped to GELINA. The dimensions of the cylindrical sample are approximately 0.12 cm thick and a radius of 2.5 cm. Since 90 Zr is not chemically reactive to air, bare metallic samples were employed. The sample was measured at a flight path (FP) length of 60 m, using four C 6 D 6 detectors on FP14. The final paper will include experimental details and measured cross section data for 90 Zr compared to current evaluated nuclear data libraries.

07 ISOTOPE AND RADIATION SOURCES↗

Optimizing the 8 Li yield for the IsoDAR Neutrino Experiment

The focus of this paper is on optimizing the electron-antineutrino source for the IsoDAR (Isotope Decay at Rest) experimental program. IsoDAR will perform sensitive short-baseline neutrino oscillation and electroweak measurements, among other Beyond Standard Model searches, in combination with KamLAND and/or other suitable detectors. IsoDAR will rely on the high-Q β– decay of the 8 Li isotope for producing electron-antineutrinos, created mainly via neutron capture in an isotopically enriched 7 Li sleeve surrounding the Be target. In particular, this paper examines the performance, defined in terms of absolute 8 Li (or, equivalently, electron-antineutrino) production rate, of various candidate sleeve materials, including a lithium-fluoride, beryllium-fluoride mixture (“FLiBe”) sleeve and a homogeneous mixture of lithium and beryllium (“Li-Be”). Furthermore, these studies show that the 8 Li yield can be increased substantially by employing a Li-Be sleeve and therefore motivate significant changes to the nominal IsoDAR design.

47 OTHER INSTRUMENTATION↗

An Unbalanced Battle in Excellence: Revealing Effect of Ni/Co Occupancy on Water Splitting and Oxygen Reduction Reactions in Triple–Conducting Oxides for Protonic Ceramic Electrochemical Cells

Porous electrodes that conduct electrons, protons, and oxygen ions with dramatically expanded catalytic active sites can replace conventional electrodes with sluggish kinetics in protonic ceramic electrochemical cells. In this work, a strategy is utilized to promote triple conduction by facilitating proton conduction in praseodymium cobaltite perovskite through engineering non-equivalent B-site Ni/Co occupancy. Surface infrared spectroscopy is used to study the dehydration behavior, which proves the existence of protons in the perovskite lattice. The proton mobility and proton stability are investigated by hydrogen/deuterium (H/D) isotope exchange and temperature-programmed desorption. It is observed that the increased nickel replacement on the B-site has a positive impact on proton defect stability, catalytic activity, and electrochemical performance. This doping strategy is demonstrated to be a promising pathway to increase catalytic activity toward the oxygen reduction and water splitting reactions. The chosen PrNi 0.7 Co 0.3 O 3–δ oxygen electrode demonstrates excellent full-cell performance with high electrolysis current density of –1.48 A cm –2 at 1.3 V and a peak fuel-cell power density of 0.95 W cm –2 at 600 °C and also enables lower-temperature operations down to 350 °C, and superior long-term durability.

08 HYDROGEN↗

Production of NBL PO plutonium isotopic standards CRM 136A, CRM 137A, and CRM 138A

Lawrence Livermore National Laboratory (LLNL) produced approximately 1 mg units of purified Pu from the parent New Brunswick Laboratory (NBL) certified reference materials (CRM) 137, 136 and 138 isotopic standards for the NBL Program Office (NBL PO) as detailed in the revised project plan. As stated in the plan, three representative units of each material were dispensed at the same time to be characterized at LLNL and provide informational values for the quantity of Pu and progeny nuclides in each unit. NBL PO intends to collect and evaluate isotopic measurement data from multiple laboratories and certify these materials as new isotopic standards C137A, C136A, and C138A, respectively. Soon after production eleven units of each analytical standard were shipped to other analytical laboratories for the certification effort, and 121, 119, and 119 units of C137A, C136A and C138A, respectively were shipped to Mickey Finch at Y12 NBL distribution center in November 2024 (30-gallon drum, TID 003777 PRL 7000005043). Residual purified Pu from the effort is being stored indefinitely in B332 at LLNL. Detailed methods can be found in the production plan, and this report describes and documents aspects of the production effort that are not in or were modified from the original production plan.

and nuclear chemistry↗

The new Batch Mode Ion Source for stand-alone operation at the Facility for Rare Isotope Beams (FRIB)

Gas stoppers have been used for a long-standing successful science program at Michigan State University with stopped and rare-isotope beams produced by projectile fragmentation. The National Superconducting Cyclotron Laboratory’s Coupled Cyclotron Facility has recently transitioned into the Facility for Rare Isotope Beams (FRIB) laboratory to provide rare isotopes using a high-power superconducting linear accelerator and new production facilities. To allow the science program with stopped and reaccelerated beams to continue during the transition period, a stand-alone capability was added. The Batch Mode Ion Source (BMIS) was built and has been providing beams of long-lived and stable isotopes of a variety of elements for successful user experiments. Finally, the BMIS system is described and results from the production of various beams are presented.

47 OTHER INSTRUMENTATION↗

A Tool Kit for Generating Simulated Radiation Measurements for Advanced Reactor Safeguards and Security

A tool kit was developed to simulate and analyze passive radiation measurements of molten salt reactor (MSR) operations to support development of nuclear safeguards approaches for this emerging reactor technology. A Transient Simulation Framework of Reconfigurable Modules (TRANSFORM) multiphysics simulation of an MSR produces time-dependent isotopic inventories at user-selected locations within the model. The tool kit implements the Gamma Detector Response and Analysis Software (GADRAS) application programming interface to inject the TRANSFORM isotopic inventories extracted/processed by a Python pipeline into GADRAS models of user-defined geometries. The TRANSFORM inventories are the source terms used to obtain synthetic measurements from GADRAS-defined detectors. The speed of TRANSFORM and GADRAS simulations enables surveying the large design space of MSRs (e.g., fuel type, fuel salt composition, number of loops) and the plethora of measurements (e.g., location, detector type, and collimation) within the reactor. This has enabled timely assessment of the various measurement locations and detectors to identify the most effective and efficient safeguards approach for a specific MSR design. Lastly, the tool kit also simulates extracted samples that can be aged to a desired dose, enabling stakeholders to optimize a measurement plan to use sample analysis as an element within a broader material accountancy plan.

Westphal, Greg↗

Management of Legacy Enriched Uranium and Transuranic Materials at ORNL - 19062

The DOE manages an inventory of materials that contains a range of long-lived radioactive isotopes that were produced from the 1960's through the 1980's. These materials were made by irradiating targets in production reactors to produce special heavy isotopes for DOE programmatic use, scientific research, and industrial and medical applications. ORNL uses these materials in DoE's center for production, storage, and distribution of transuranium isotopes (plutonium through californium) for the heavy-element research program and has used them as feedstock in the Calutron Electromagnetic Isotope Enrichment Facility, one of only two facilities in the world with capabilities to enrich radioisotopes in multigram quantities. Both the production reactors and enrichment facilities have been shut down, and many of these unique materials will not be produced again in the foreseeable future [1, 2]. As a result, ORNL has an inventory of radioisotopes that are being held for reuse because their potential intrinsic value to DOE, but many of these materials have no currently defined use. ORNL is undertaking an initiative to more actively manage these materials by reviewing the existing inventory to determine if the contents have programmatic use. Steps are being taken to process, repackage, and stage the materials for distribution to programmatic users or for waste disposal, primarily at WIPP. This paper describes the approach that ORNL has taken to determine whether the inventory of materials should be kept or disposed and the processes that are being used to manage or disposition the materials. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Consistent $\overline{ν}$ evaluation for minor U isotopes with $\tt{CGMF}$

Following several successful prompt $\overline{ν}$ evaluations using $\tt{CGMF}$, including consistent evaluations for minor Pu isotopes, we detail in this report our efforts to perform a consistent $\overline{ν}$ evaluation for minor U isotopes during FY25. Although we have not yet produced a finalized evaluation, we present the progress that we have made towards such an evaluation for 232,233,234,236,237,239 U prompt $\overline{ν}$. Our milestone explicitly calls out evaluations for 233 U, 234 U, and 236 U, however, to better constrain the model with reliable experimental $\overline{ν}$ data, we also include 235 U and 238 U in the evaluation procedure. Then, we additionally produce evaluations for 232 U, 237 U and 239 U $\overline{ν}$ as a byproduct. Elsewhere, we will report our efforts on a stand-alone 233 U $\overline{ν}$ evaluation. This report is organized in the following manner. In Sec. 2, we briefly outline the updates to CGMF that were needed to be able to calculate all of these minor U fission reactions. The experimental data overview is given in Sec. 3. The evaluation methodology and results are presented in Secs. 4 and 5, respectively. Finally, we conclude and outline work for FY26 in Sec. 6.

07 ISOTOPE AND RADIATION SOURCES↗

Iodine Effects on Medical Isotope Producer Delay & Guard Bed Temperature and Performance in Support of NA-23 Program

In support of NA-23’s objective to accelerate the establishment of a reliable commercial United States (U.S.) domestic supply of 99Mo produced without the use of highly enriched uranium (HEU), the Pacific Northwest National Laboratory (PNNL) was tasked with modeling the performance of activated carbon delay and guard beds that may be typical for non-HEU 99Mo production processes. The specific tasks accomplished by PNNL included calculations of long-term effects of iodine on delay bed performance and development of a finite element simulation to better understand delay bed performance under various scenarios specifically with radioxenon and radioiodine decay heating of the delay beds. The main issue of interest in this study is understanding the effect of iodine on the abatement performance of the beds if iodine is not sufficiently removed from gases prior to reaching the delay beds. Finite element simulations of delay bed performance were developed using COMSOL Multiphysics® Software. These simulations are based on partial differential equations that describe xenon and iodine adsorption, heat transfer and decay of radioxenon and radioiodine isotopes. Heat transfer in the activated carbon beds is simulated with a heat source tied to the decay of radioactive xenon and iodine species. These simulations were used to investigate delay bed temperature and hold up time using radioxenon and radioiodine activities and flowrates expected from a non-HEU production process. A bounding case scenario was simulated, where all the iodine was released into the delay beds due to insufficient guarding of the delay beds. In addition, preliminary investigations of the guard beds were conducted.

07 ISOTOPE AND RADIATION SOURCES↗

Reaction Pathways and Kinetics for Selective Catalytic Reduction (SCR) of Acidic NO x Emissions from Power Plants with NH 3

We report that selective catalytic reduction (SCR) of NO x with NH 3 by supported vanadium oxide catalysts is an important technology for reducing acidic NO x emissions from stationary sources and mobile diesel vehicles. However, rational design of improved catalysts is still hampered by a lack of consensus about reaction pathways and kinetics of this critical technology. The SCR fundamentals were resolved by applying multiple time-resolved in situ spectroscopies (ultraviolet–visible light (UV-vis), Raman and temperature-programmed surface reaction (TPSR)) and isotopically labeled molecules ( 18 O 2 , H 2 18 O, 15 N 18 O, ND 3 ). Finally, this series of experiments directly revealed that the SCR reaction occurs at surface V 5+ O 4 sites that are maintained in the oxidized state by O 2 and the rate-determining step involves the reduction of V 5+ O 4 sites by NO and NH 3 , specifically the breaking of N–H bonds during the course of formation or decomposition of the NO–NH 3 intermediate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Status of Post Irradiation Examination of FCAB and FCAT Irradiation Capsules

A series of irradiation programs are ongoing to address the need for determining the radiation tolerance of FeCrAl alloys. These irradiation programs, deemed the FCAT and FCAB irradiation programs, use the High Flux Isotope Reactor (HFIR) to irradiate second generation wrought FeCrAl alloys and early-generation powder-metallurgy (PM) oxide dispersion-strengthened (ODS) FeCrAl alloys. Irradiations have been or are being performed at temperatures of 200°C, 330°C, and 550°C from doses of 1.8 dpa up to 16 dpa. Preliminary post-irradiation examination (PIE) on low dose (<2 dpa) irradiation capsules of tensile specimens has been performed. Analysis of co-irradiated SiC thermometry have shown reasonable matching between the nominal irradiation temperatures and the target irradiation temperatures. Room temperature tensile tests have shown typical radiation-induced hardening and embrittlement at irradiations of 200°C and 330°C, but a propensity for softening when irradiated to 550°C for the wrought alloys. The PM-ODS FeCrAl specimens showed less hardening compared to the wrought alloys. Future PIE includes high temperature tensile tests on the low dose irradiation capsules as well as the determination of reference fracture toughness transition temperature, T o , in alloys irradiated to 7 dpa and higher.

36 MATERIALS SCIENCE↗

Documentation Package Supporting Fabrication of Doped UO 2 Samples for MiniFuel Irradiation and Fission Gas Release Benchmarking

The Oak Ridge National Laboratory (ORNL) is looking into the fabrication of high performance UO 2 fuel candidates via the addition of dopants to the UO 2 . The addition of dopants is proposed to cause enlarged grains that will slow down fission gas release from the irradiated fuel pellet candidates. The Cr-doped UO 2 pellets were fabricated from a microspherical feedstock, and enlarged grains were observed during the microstructural characterization. Irradiation under the Miniature Fuel program in the High Flux Isotope Reactor at ORNL will enable the study of irradiation response of such potential fuel candidates and will allow fission gas release benchmarking for these fuel candidates.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mixed-phase orographic cloud microphysics during StormVEx and IFRACS

Wintertime mixed-phase orographic cloud (MPC) measurements were conducted at the Storm Peak Laboratory (SPL) during the Storm Peak Lab Cloud Property Validation Experiment (StormVEx) and Isotopic Fractionation in Snow (IFRACS) programs in 2011 and 2014, respectively. The data include 92 h of simultaneous measurements of supercooled liquid cloud droplet and ice particle size distributions (PSDs). Average cloud droplet number concentration (CDNC), droplet size (NMD), and liquid water content (LWC) were similar in both years, while ice particle concentration (Ni) and ice water content (IWC) were higher during IFRACS. The consistency of the liquid cloud suggests that SPL is essentially a cloud chamber that produces a consistent cloud under moist, westerly flow during the winter. A variable cloud condensation nuclei (CCN)-related inverse relationship between CDNC and NMD strengthened when the data were stratified by LWC. Some of this variation is due to changes in cloud base height below SPL. While there was a weak inverse correlation between LWC and IWC in the data as a whole, a stronger relationship was demonstrated for a case study on 9 February 2014 during IFRACS. A minimum LWC of 0.05 g m–3 showed that the cloud was not completely glaciated on this day. Erosion of the droplet distribution at high IWC was attributed to the Wegener–Bergeron–Findeisen process as the high IWC was accompanied by a 10-fold increase in Ni. A relationship between large cloud droplet concentration (25–35 µm) and small ice particles (75–200 µm) under cold (<–8 °C) but not warm (>–8 °C) conditions during IFRACS suggests primary ice particle production by contact or immersion freezing. The effect of blowing snow was evaluated from the relationship between wind speed and Ni and by comparing the relative (percent) ice particle PSDs at high and low wind speeds. These were similar, contrary to expectation for blowing snow. However, the correlation between wind speed and ice crystal concentration may support this explanation for high crystal concentrations at the surface. Secondary processes could have contributed to high crystal concentrations but there was no direct evidence to support this. Further experimental work is needed to resolve these issues.

54 ENVIRONMENTAL SCIENCES↗

Additively Manufactured Pressure Limiting Irradiation Capsule for the High Flux Isotope Reactor

The Advanced Materials and Manufacturing Technologies (AMMT) program previously demonstrated an additively manufactured (AM) irradiation capsule (commonly referred to as a “rabbit”) from 316H stainless steel (SS) for insertion into the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL)1. This report details efforts to design and fabricate an AM pressure limiting structure (PLS) into one of the end caps of a rabbit capsule and qualify it for insertion into HFIR. The PLS includes a thin cylindrical rupture wall, a shield, and internal supports to facilitate printing and ensure mechanical integrity. Its overall dimensions are 9-mm tall and 10-mm in diameter— equivalent to about one-fourth of the size of a AAA battery. The PLS maintains safe internal operating pressures for a rabbit capsule while in the reactor. Although this application is specific to HFIR, the approach lends itself to further applications in industrial, aeronautical, advanced space and power generation environments. Several PLS rabbits capsules have been successfully designed, fabricated, pressure tested, and qualified for future insertion into the HFIR for irradiation and post-irradiation evaluation.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Electrochemical Kinetics of Stable Isotopes (Final Report)

Stable isotopes are sensitive indicators to the mass transport and chemical reactions that occur during potentiostat-controlled electroplating of metals from aqueous (and some non-aqueous) metal-salt solutions. The goal of this research program is to measure the stable isotope fractionation during electrochemical processes, how the isotope-dependent rates are sensitive to chemistry, temperature, and electrochemical kinetics, and to use these measurements to develop a theoretical framework for a kinetic isotope effect that is able to predict kinetic isotope fractionation factors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗