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DOE OSTI2015

Plant-Scale Concentration Column Designs for SHINE Target Solution Utilizing AG 1 Anion Exchange Resin

Argonne is assisting SHINE Medical Technologies (SHINE) in their efforts to develop SHINE, an accelerator-driven process that will utilize a uranyl-sulfate solution for the production of fission product Mo-99. An integral part of the process is the development of a column for the separation and recovery of Mo-99, followed by a concentration column to reduce the product volume from 15-25 L to <1 L. Argonne has collected data from batch studies and breakthrough column experiments to utilize the VERSE (Versatile Reaction Separation) simulation program (Purdue University) to design plant-scale product recovery and concentration processes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2022

Development of Laser-Induced Breakdown Spectroscopy for the Californium-252 Supply Program

Calibration-free–laser-induced breakdown spectroscopy (CF-LIBS) is suggested as an alternative to traditional LIBS because it does not rely on calibration curves and instead relies on previously reported parameters called transition probabilities. Transition probabilities are fundamental parameters that describe the probability a specific transition from an upper energy to a lower energy will occur. These values act as internal calibrations and allow concentrations to be calculated based on the plasma temperature and electron density, which can be determined from Saha-Boltzmann methods. CF-LIBS provides the ability to perform elemental concentration estimations on samples without the need for chemical dilutions and only nanograms of material are ablated into the plasma. These benefits can be applied remotely inside hot cells, glove boxes, and radiation hoods through optical fibers. This report summarizes recent efforts to develop CF-LIBS methods for future applications within Oak Ridge National Laboratory’s radioisotope production portfolio, such as the Cf-252 Supply Program. Summaries are provided for the developed Python scripts for data analysis and two studies employing these programs to determine unreported transition probabilities of relevant lanthanides. Additionally, a review of fiber-delivered LIBS and a discussion of a LIBS fiber probe design are provided.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2016

Kinetic Monte Carlo Simulation of Hydrogen Diffusion in Tungsten

Nuclear fusion is considered as the most promising sustainable energy source. If achieved, it could provide electricity to the mankind for millions of years. During the reaction, the fusion ash is continuously removed from the magnetic gap, the divertor region, and the divertor facing component is subjected to intense plasma bombardment. It is proposed to use tungsten as the divertor facing material, because it has low physical sputtering yield and superior thermomechanical properties. However, the high mobility of hydrogen in tungsten and the high bombardment flux bring the hydrogen isotopes deep into the tungsten tile. The presence of hydrogen in tungsten tends to weaken the gram boundaries and produce surface blistering. The ejection of tungsten particulates into the plasma core will cool the reaction and cease the fusion reactions. Therefore, it is important to have a detailed understanding of the hydrogen diffusion in tungsten bulk. The KMC method is a stochastic computer simulation to predict the time evolution of a certain system. Typically, at a given time, the system will evolve through a few possible paths with known probabilities. In each step, the KMC method analyzes the entire system and randomly determines the system evolving events based on all transition rates of all possible events and advance the physical time. This process is repeated till the simulation of the entire physical time is completed. In previous work, the authors developed a kinetic Monte Carlo (KMC) algorithm and program to simulate hydrogen diffusion process on tungsten reconstructed surface. In this article, this KMC method is extended to model the hydrogen diffusion in tungsten bulk. The diffusion coefficients are calculated and fitted to the Arrhenius equation. The result matches the experiment measurement very well. KMC diffusion simulation needs the locations of the hydrogen trapping sites, diffusion paths and the corresponding diffusion energy barriers. The hydrogen interstitial sites in tungsten crystal have been thoroughly studied by density function theory (DFT) and molecular dynamics (MD). Johnson and Carter used DFT to determine the preferred location of the hydrogen interstitial sites m tungsten crystal, which are the tetrahedral sites (T-sites) in body-centered-cubic (bcc) lattice surfaces. All T-sites are located on the surfaces of a lattice cell. There are four T-sites per surface and twelve T-sites per lattice cell. The hydrogen atoms diffuse by traveling from one T-site to one of its nearest four T-site neighbors. Thus, each T-site is surrounded by two neighbors on the same surface, and one neighbor on each of the two adjacent surfaces perpendicular to the surface holding the center T-site. The diffusion barrier between two neighboring T-sites was calculated to be 0.38 eV. Knowing the diffusion path, energy barrier, and the crystal structure, the KMC simulation is readily to be performed. Based on other researchers' DFT calculations, the hydrogen stable interstitial site in tungsten bulk is determined as the tetrahedral site on the surface of the bee lattice. Each T-site has 4 neighbors and the energy barrier between two adjacent T-sites are estimated to be 0.38 eV. Based on those facts and the KMC theory, a MATLAB program is developed to model the hydrogen diffusion in tungsten bulk. In the MATLAB program, substrate temperature, hydrogen concentration, physical time to be simulated, and the number of cycles are all customizable. To compare the KMC determined diffusion coefficients with experiment results in the literature, the simulations are performed for temperature 300 K - 2500 K and low hydrogen concentration (0.1%), mimicking the experiment condition. The calculated diffusion coefficients match the reference values measured by the experiment under low hydrogen concentration condition. The results are also fitted to the Arrhenius equation. The pre-exponential factor and the average activation energy in Arrhenius equation are obtained. The good agreement between simulation and experiment proves that the developed KMC algorithm truly reflect the well-established theory of interstitial hydrogens in tungsten. The developed program could easily be used to model the diffusion process and predict the diffusion coefficients under other concentrations and temperatures. This work is part of the ongoing development of hydrogen diffusion in tungsten integrating surface diffusion (previous work), bulk diffusion (this work), and adsorption/desorption on surface (future work)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Why Lady Godiva Should be Replaced as the Default Validation Experiment for U-235 Nuclear Data

For the past seven decades the Lady Godiva benchmark (HEU-MET-FAST-001) has been the primary experiment used for 235 U nuclear data validation. The papers associated with large nuclear data library releases such as ENDF/B-VII.1 and ENDF/B-VIII.0 refer to it frequently. The reasons why HEU-MET-FAST-001 has been used as the primary validation experiment for 235 U nuclear data validation will be discussed in the following section. However, as discussed among the benchmark community, the standards associated with International Criticality Safety Benchmark Evaluation Project (ICSBEP) evaluations have changed throughout time; this is subject of the OECD/NEA WPEC (Working Party on Nuclear Criticality Safety) Subgroup 8. HEU-MET-FAST-001 is an older benchmark (issued during the inaugural year of ICSBEP in 1996 with only minor revisions occurring since then) and (along with many of the other benchmarks from this era) does not meet the standards for a modern benchmark. This work explores why HEU-MET-FAST-001 is useful for 235 U nuclear data validation and discusses other alternative validation experiments.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2024

Qualifying the Instrument Thimble 11 Test Position in the Advanced Test Reactor Critical

The Advanced Test Reactor (ATR) is a versatile nuclear research reactor located at the Idaho National Laboratory (INL) in Eastern Idaho, United States of America. It is one of the most powerful and flexible research reactors in the world and is primarily used for materials testing, isotope production and basic nuclear science research. The ATR is a light-water-cooled, beryllium-moderated reactor with a nominal thermal power capacity of 250 MW utilizing specially designed fuel, arranged in a serpentine pattern to create 9 flux traps. The special design of ATR allows for the neutron flux within each of the flux traps providing flexibility for experiments, programs and allowing experiments with different dose requirements to be irradiated simultaneously. The Advance Test Reactor Critical (ATRC) is a full-scale replica of the ATR core but is housed in a pool instead of a pressure vessel. ATRC is usually operated at less than 600 watts [1]. There are 12 dry instrument thimbles located around the outside of the core tank where a variety of measurement equipment is housed to facilitate reactor operations. Currently Instrument Thimble 11 (IT-11) is not utilized in ATR or ATRC. A range of measurements is ongoing to qualify IT-11 as a test platform for nuclear instrumentation research, development and further experimentation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Initial Findings in Qualifying the Instrument Thimble 11 Position in the Advanced Test Reactor Critical

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

DOE OSTI2018

The 2017 Nonlinear Mechanics and Dynamics Research Institute.

The 2017 Nonlinear Mechanics and Dynamics (NOMAD) Research Institute was successfully held from June 19 to July 28, 2017. NOMAD seeks to bring together participants with diverse technical backgrounds to work in small teams to utilize an interactive approach to cultivate new ideas and approaches in engineering . NOMAD provides an opportunity for researchers - especially early career researchers - to develop lasting collaborations that go beyond what can be established from the limited interactions at their institutions or at annual conferences. A total of 17 students from around the world came to Albuquerque, New Mexico to participate in the six - week long program held at the University of New Mexico campus. The students collaborated on one of six research projects that were developed by various mentors from Sandia National Laboratories, academia, and other government laboratories. In addition to the research activities, the students attended weekly technical seminars, toured the National Museum of Nuclear Science & History, and socialized at various off - hour events including an Albuquerque Isotopes baseball game. At the end of the summer, the students gave a final technical presentation o n their research findings that was broadcast via Skype. Many of the research discoveries made at NOMAD are published as proceedings at technical conference s and have direct alignment with the critical mission work performed at Sandia.

42 ENGINEERING↗

DOE OSTI2018

FY18Q2 Quarterly Report: Radiation Enhanced Diffusion of Ag, Ag-Pd, Eu, and Sr in Neutron Irradiated PyC/SiC Diffusion Couples

Obtaining accurate diffusion kinetics in materials representative of those found in tristructural-isotopic (TRISO) coated particle fuel is needed to predict the diffusive release of fission products in reactor. Planar diffusion couples with representative pyrocarbon (PyC) and silicon carbide (SiC) layers are being produced using the same fluidized-bed chemical vapor deposition (FBCVD) technology used to produce TRISO particles from the first irradiation experiment of the Advanced Gas Reactor (AGR) Fuel Qualification and Development Program. The layer properties of the planar diffusion couples are tailored to meet the specified PyC density and microstructure of the SiC layer as defined by the AGR program. The influence of these variables on diffusion is also being explored by producing PyC and SiC variants.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2018

FY18Q3 Quarterly Report: Radiation Enhanced Diffusion of Ag, Ag-Pd, Eu, and Sr in Neutron Irradiated PyC/SiC Diffusion Couples

36 MATERIALS SCIENCE↗

DOE OSTI2018

Design and Synthesis of Materials with High Capacities for Hydrogen Physisorption

Slit pore or planar geometries are the optimal morphology for adsorbents. Our initial effort was to explore single layer graphene as the ideal platform for adsorbents. As literature processes for graphene synthesis proved unreliable in generating structures of relevance, we concentrated our efforts on metal functionalization in order to enhance the normally modest 4-6 kJ/mole typical of carbons. The results of interest through this effort are the 32-36 g/l volume densities projected for 100 bar pressure for Cu modified material at 77K. Modest material compression would improve these values to densities comparable to 700 bar compressed gas tanks. Thermal Program Desorption (TPD) results from the same metal modified material showed hydrogen release over two temperature ranges. The initial range is 100 to 190 K from normally physisorbed gas while chemisorbed hydrogen from the Cu surface showed desorption starting at 300 K. This work suggests a pathway toward higher temperature utility based on both physisorption and chemisorption phenomena. Chemisorption was validated by observing isotope exchange with deuterium.

08 HYDROGEN↗

DOE OSTI2021

Mechanical Properties of Additively Manufactured 316L Stainless Steel Before and After Neutron Irradiation (FY21)

This report presents the materials property data of additively manufactured (AM) 316L stainless steel (SS) accumulated for the assessment of core materials in the Transformational Challenge Reactor (TCR) program. The TCR manufacturing approach includes using the laser powder bed fusion (LPBF) method for metallic (316L and Inconel 718) components. To assess the mechanical performance of printed components in reactor-relevant conditions and build a property database for the AM materials, mechanical tests and evaluations were performed before and after neutron irradiation. Miniature tensile specimens were irradiated in the High Flux Isotope Reactor to 0.2, 2, 8, and 10 dpa at target temperatures of 300 and 600°C. Postirradiation evaluation for the 0.2 and 2 dpa specimens was performed during FY20 and FY21, and the results are presented and discussed in this document.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

The Impact of Increased Requirements for Verification Measurements of Category III and IV Receipts

As part of the regular nuclear material accounting and control process, sites that have accountable nuclear material regularly perform measurements of the material in their possession. The expectation for the type of measurements and their frequency is set out in Department of Energy (DOE) Order 474.2, and further detailed in each site’s respective material control and accountability (MC&A) plan and associated controlling documents. The measurements of interest in this report are those performed on external (between DOE sites) transfer receipts of Category III or IV accountable materials. In 2020, a revision of DOE Order 474.2 was proposed that would significantly increase the requirement that measurements be performed upon receipt of material, and further, that those measurements be quantitative verification (rather than qualitative confirmatory) measurements. A survey was performed of DOE sites to discuss the impact on their MC&A measurements program if more rigorous verification measurements requirements for Category III and IV receipts were implemented. An assessment of nondestructive assay (NDA) measurement instruments to meet those needs was also performed. Across the board, sites indicated that personnel and budget would cause the largest impact. Sites which are qualified as Category I/II indicated a reduced impact as these sites already have the measurement capabilities and some personnel but would require the acquisition of additional measurement systems. Category III/IV sites indicated a much larger impact as these sites generally have smaller MC&A programs. A few smaller sites stated a measurement program would need to be created to handle the demand. Calorimetry, quantitative gamma spectroscopy and neutron coincidence counting systems were identified as common systems that could meet the verification measurement requirements. The other, and perhaps larger issue is the need for calibration standards for the calorimetry and neutron coincidence counting systems. It is proposed that a comparative study be performed for ISOCS and ISOTOPICS, qualification of a COTS calorimetry system be performed, and development of an AWCC system that uses a neutron generator.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2026

Laser Spectroscopy of Exotic Atoms and Molecules Containing Octupole-Deformed Nuclei

This project investigated the nuclear, atomic, and molecular structure of exotic atoms and molecules containing actinide isotopes. These short-lived radioactive systems are challenging to produce and study in the laboratory, yet they offer unique opportunities for fundamental science. These nuclei are predicted to exhibit pear-shaped (octupole) deformation, a rare collective nuclear behavior that dramatically enhances their sensitivity to fundamental physics phenomena such as time-reversal- and parity-violating effects. Such enhancements make them ideal probes for exploring open questions in our understanding of the universe such as the origin of the matter–antimatter asymmetry of the universe. To realize these measurements, the project led the development of a new laser spectroscopy experiment at MIT, and later commissioned at the Facility for Rare Isotope Beams (FRIB) at Michigan State University: the Resonance Ionization Spectroscopy Experiment (RISE). RISE combines the spectroscopic precision of collinear laser spectroscopy with the sensitivity of particle-detection techniques, enabling measurements of rare isotopes produced at rates as low as a few ions per second. The beamline was designed, built, and installed, and was successfully commissioned at FRIB during the grant period. RISE is now a permanent capability of the FRIB facility, and has produced several results on the study of rare atoms and molecules for nuclear structure and fundamental symmetries. In parallel with the FRIB program, the project contributed to the first precision laser-spectroscopy measurements of short-lived radioactive molecules. Working with international collaborators at CERN's ISOLDE facility, the team conducted pioneering experiments on radium monofluoride (RaF) and actinium monofluoride (AcF). The results from this work have been published in major journals of science, including Nature, Science, Nature Physics, Nature Communications, and Physical Review Letters. These findings have guided future experiments on the laser cooling of radioactive molecules, opening a new platform for precision tests of fundamental symmetries.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2022

Deployment of the HFIRCON transport and depletion tool for plutonium-238 production studies

Irradiation of {sup 237}Np-bearing targets in Oak Ridge National Laboratory's (ORNL) High Flux Isotope Reactor (HFIR) results in the efficient production of {sup 238}Pu, which, in the form of heat source PuO{sub 2}, is used as a reliable power source for deep-space and planetary NASA missions. A technology demonstration subproject was initiated at ORNL in 2011 to develop and implement the technology required to establish a {sup 238}Pu supply chain. A systematic progression of NpO{sub 2}/Al cermet (20 vol.% NpO{sub 2}) activities to date has successfully demonstrated target fabrication, irradiation, and chemical recovery processes. Recent program tasks have included the development of the HFIRCON transport and depletion tool for efficient reactor physics analyses and the evaluation of increased NpO{sub 2} loadings (i.e., beyond 20 vol.%) and NpN-based targets. This paper documents the deployment of the HFIRCON code to assess various Np concentrations in NpO{sub 2}- and NpN-based targets in HFIR's inner small vertical experiment facilities. Results indicate that {sup 238}Pu production and quality can be enhanced with increased Np loadings; however, target conversion rates are reduced. The results recorded in this paper, thermal and material balance evaluations, and testing requirement planning will be used to determine whether increased NpO{sub 2} loadings or NpN-based targets will be further considered. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2017

Post-Closure Environmental Sampling and Inspection at the Amchitka Island, Alaska, Site - 17251

In the 1960's and early 1970's, three underground nuclear tests were conducted on Amchitka Island, Alaska. In 1965, the US Department of Defense-in conjunction with the US Atomic Energy Commission (AEC)-conducted the first of these nuclear tests, Long Shot, to provide data that would improve US capabilities for detecting underground nuclear explosions. In 1969, AEC conducted the second test, Milrow, to explore the feasibility of detonating a much larger device. In 1971, AEC conducted the third test, Cannikin, which was the largest underground test ever conducted by the US. The Long-Term Surveillance Plan (LTSP) for the Amchitka, Alaska, Site details how the US Department of Energy Office of Legacy Management (LM) intends to fulfill its mission to protect human health and the environment at and around the Amchitka Island site. The LTSP calls for monitoring to be performed every 5 years, at least during the initial phase of the project. The purpose of the monitoring is to develop a baseline of activity concentrations for selected radionuclides in biota, water, and soil, both on Amchitka Island and at the reference location on Adak Island, approximately 322 kilometers (200 miles) northeast of Amchitka. In addition to the environmental monitoring activities, seven mud pit caps that contain diesel-contaminated soils are inspected. The plan for biological and water sampling (both seawater and freshwater) during the May 2016 sampling event was developed through close coordination with the primary stakeholders, including the Alaska Department of Environmental Conservation, the Aleutian Pribilof Islands Association, and the US Fish and Wildlife Service. The environmental sampling in 2016 is a continuation of LM's evaluation of Amchitka Island's environment. Previous results from similar monitoring programs in 2004 and 2011 indicate that the environment is not being impacted by radionuclide migration and uptake from the underground nuclear testing conducted beneath Amchitka Island; consequently, subsistence and commercial-catch seafood is safe for human consumption. The collection of biota samples (rockfish, Irish lords, greenling, and rockweed) for cesium-134 ({sup 134}Cs), cesium-137 ({sup 137}Cs), plutonium-239 ({sup 239}Pu), plutonium-240 ({sup 240}Pu), and freshwater and seawater samples for {sup 134}Cs, {sup 137}Cs, and tritium ({sup 3}H) was the primary objective of the 2016 sampling effort. Rockfish, Irish lords, and greenling are resident, nonmigratory fish species that spend their entire life cycle in the marine environment, and rockweed is an inter-tidal species that may concentrate cesium. The seawater samples were collected primarily to determine if leakage from the Long Shot detonation could be detected and, secondarily, to compare with the background seawater samples collected from Adak Island. Cesium isotopes are also being analyzed to better understand the potential impact that the Fukushima-Daiichi release might have on the Amchitka and Adak environments. The target detection limits used for the 2016 sampling are lower than those used in previous studies. The lower detection limits make it possible for LM to delineate background activity levels for the radionuclides of interest. Data from the 2016 sampling event go beyond assessing food safety and focus on detecting leakage from the underground nuclear explosions. Additionally, the baseline activity concentrations obtained for the reference area (Adak Island) will enable identification of quantitative statistical trends in the results of future sampling programs. Sampling programs conducted in 2021 and beyond will have an objective to assess the statistical trends of radioactivity levels in the Amchitka Island environment. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

Role of Surface Hydroxyls and Lattice Oxygen in Governing Selectivity and Restructuring During Acetic Acid Conversion on Fe 3 O 4 (001)

Understanding the reactivity of carboxylic acids on metal oxide surfaces is critical for elucidating ketonization mechanisms relevant to biomass upgrading. Here, we investigate the adsorption and thermal decomposition of acetic acid (CH 3 COOH) on Fe 3 O 4 (001) using scanning tunneling microscopy (STM), temperature-programmed reaction spectroscopy (TPRS), and X-ray photoelectron spectroscopy (XPS). At room temperature, acetic acid adsorbs dissociatively to form ordered bidentate acetate (CH 3 COO) overlayer that lifts the (√2 × √2)R 45° surface reconstruction. TPRS reveals ketene (CH 2 CO) as the dominant product, along with CO, CO 2 , and H 2 O, the latter evolving via a Mars–van Krevelen (MvK) mechanism. Isotopic labeling shows preferential CO 2 formation from the carboxyl carbon and a more balanced CO/CO 2 ratio from the methyl carbon, suggesting distinct oxidation pathways. STM imaging reveals embedded acetate intermediates filling surface oxygen vacancies created in MvK steps. Upon product formation completion (~700 K), extensive surface etching is observed, with pits elongated along the octahedral Fe rows. Approximately 20% of the surface oxygen is removed, consistent with vacancy formation stoichiometry inferred from product distributions. These findings demonstrate that carboxylate-induced restructuring of Fe 3 O 4 (001) involves both surface healing and reduction processes, offering mechanistic insights relevant to ketonization and broader carboxylic acid chemistry on metal oxides.

acetic acid↗

DOE OSTI2020

Theory Manual for the Fuel Cycle Analysis Code REBUS

REBUS is a system of programs designed for the fuel cycle analysis of fast reactors and accelerator-driven systems. The first version of REBUS was developed in 1970 for calculating the equilibrium operating conditions of liquid metal fast breeder reactors. During the past five decades, various extensions and refinements have been made in the simulation of material motions in fuel cycle facilities and the solution of the neutronics and isotopic transmutation equations that govern the reactor behavior. The latest version complies with the standard code practices and interface dataset specifications of the committee on computer code coordination (CCCC). This report provides a detailed description of the physical processes and their mathematical models and solution methods of the current production version of REBUS. The models of the facilities and physical processes involved in fast reactor fuel cycle are first discussed. Then the mathematical formulation of these physical models is presented, followed by detailed discussions of solution methods of the resulting set of equations. Finally the output edit quantities are discussed along with their definitions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

The 2018 Nonlinear Mechanics and Dynamics Research Institute

The 2018 Nonlinear Mechanics and Dynamics (NOMAD) Research Institute was successfully held from June 18 to August 2, 2018. NOMAD brings together participants with diverse technical backgrounds to work in small teams to cultivate new ideas and approaches in engineering mechanics and dynamics research. NOMAD provides an opportunity for researchers -- especially early career researchers - to develop lasting collaborations that go beyond what can be established from the limited interactions at their institutions or at annual conferences. A total of 17 students came to Albuquerque, New Mexico to participate in the seven-week long program held at the Mechanical Engineering building on the University of New Mexico campus. The students collaborated on one of six research projects that were developed by various mentors from Sandia National Laboratories, University of New Mexico, and academic institutions. In addition to the research activities, the students attended weekly technical seminars, various tours, and socialized at various off-hour events including an Albuquerque Isotopes baseball game. At the end of the summer, the students gave a final technical presentation on their research findings. Many of the research discoveries made at NOMAD are published as proceedings at technical conferences and have direct alignment with the critical mission work performed at Sandia.

42 ENGINEERING↗