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At least 505 records · Page 28

Where does the sulphur go? Deactivation of a low temperature CO oxidation catalyst by sulphur poisoning

Sulphate formation, occurring preferentially at the CuO/CeOx-ZrOx interface, is responsible for the deactivation of low temperature CO oxidation catalysts. XRD, FTIR and isotope exchange experiments, as well as DFT calculations, reveal the poisoning mechanism of sulphate formation on the CeOx/ZrOx support material. JS, DM, TV and CHFP gratefully acknowledge the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program for the support of their participation in this work. Their studies were performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research, and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the U.S. DOE by Battelle under contract number DE-AC05-76RL01830.

Szanyi, Janos↗

Nuclear programs in India and Pakistan

India and Pakistan launched their respective nuclear programs in the 1940s and 1950s with considerable foreign technical support, especially from the United States Atoms for Peace Program. The technology and training that was acquired served as the platform for later nuclear weapon development efforts that included nuclear weapon testing in 1974 and in 1998 by India, and also in 1998 by Pakistan - which had illicitly acquired uranium enrichment technology especially from Europe and received assistance from China. As of 2013, both India and Pakistan were continuing to produce fissile material for weapons, in the case of India also for nuclear naval fuel, and were developing a diverse array of ballistic and cruise missiles. International efforts to restrain the South Asian nuclear build-up have been largely set aside over the past decade as Pakistani support became central for the U.S. war in Afghanistan and as U.S. geopolitical and economic interests in supporting the rise of India, in part as a counter to China, led to India being exempted both from U.S non-proliferation laws and international nuclear trade guidelines. In the absence of determined international action and with Pakistan blocking the start of talks on a fissile material cutoff treaty, nuclear weapon programs in South Asia are likely to keep growing for the foreseeable future.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

The high pressure gas capabilities at Oak Ridge National Laboratory’s neutron facilities

The study of samples subjected to high pressure gas is an important asset in materials research and has consequently been a priority of the sample environment development at the Oak Ridge National Laboratory’s (ORNL) neutron program. Such effort has resulted in the availability of an extensive combination of pressure cells and gas intensifiers (both commercially available and custom made). These resources are available across both neutron facilities at ORNL: the Spallation Neutron Source and the High Flux Isotope Reactor. Current capabilities include, for example, in situ measurements up to 6 kbar and a 3 kbar hydrogen-capable intensifier with a gas recovery feature. In this communication, we will review the existing suite of high pressure gas capabilities, with special emphasis on recent in-house developments. Finally, a number of examples will be presented to illustrate how such capabilities are being deployed on neutron beamlines to enable frontier science.

47 OTHER INSTRUMENTATION↗

New Cross Section Measurements and Evaluations of Zirconium Isotopes [Slides]

This presentation gives a look to new cross section measurements and evaluations of Zirconium (Zr) isotopes. This lecture includes highlights of accomplishments made in 2022. Additionally, it explains the motivation for investigation, new measurements, and re-evaluation of the Zr isotopes. This presentation concludes with a preliminary evaluation result from RPI 90 Zr evaluation and preliminary results from Eigenvalue sensitivity study on Zr sensitive critical benchmark experiments.

07 ISOTOPE AND RADIATION SOURCES↗

ESTIMATING IMPURITIES IN SURPLUS PLUTONIUM FOR DISPOSITION

The United States holds at least 61.5 metric tons (MT) of plutonium that is permanently excess to use in nuclear weapons programs, including 47.2 MT of weapons-grade plutonium. Surplus inventories will be stored safely by the Department of Energy (DOE) and then transferred to facilities that will prepare the plutonium for permanent disposition. The Savannah River National Laboratory (SRNL) operates a Feed Characterization program for the Office of Fissile Materials Disposition of the National Nuclear Security Administration and the DOE Office of Environmental Management. Many of the items that require disposition are only partially characterized, and SRNL uses a variety of techniques to predict the isotopic and chemical properties that are important for processing through the Mixed Oxide Fuel Fabrication Facility and alternative disposition paths. Recent advances in laboratory tools, including Prompt Gamma Analysis and Peroxide Fusion treatment, provide data on the existing inventories that will enable disposition without additional, costly sampling and destructive analysis.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Post-Irradiation Fracture Toughness Characterization of Generation II FeCrAl Alloys

FeCrAl alloys are promising candidate materials for the accident tolerant fuel (ATF) cladding application due to their exceptional resistance to oxidation in elevated temperature steam environments. Currently, limited fracture toughness data are available for the FeCrAl alloys, including the FeCrAl alloys newly developed at Oak Ridge National Laboratory (ORNL) under the U.S. Department of Energy’s Advanced Fuels Campaign (AFC) program. In this study, two Generation II candidate FeCrAl alloys, i.e., C06M (81.8Fe-10Cr-6Al-0.03Y-2Mo-0.2Si) and C36M (78.8Fe-13Cr-6Al-0.03Y-2Mo-0.2Si), were irradiated in the High Flux Isotope Reactor (HFIR) at ORNL to assess the fracture characteristics of these alloys after neutron irradiation. A total of six rabbit capsules were irradiated in HFIR at target temperatures of 200°C, 330°C, and 500°C up to target damage doses of 8 displacements per atom (dpa) and 16 dpa. Post-irradiation fracture toughness testing was performed following the Master Curve method in the ASTM E1921 standard. The main findings of this study are:1) Both the C06M and C36M alloys exhibited a similar response to irradiation concerning irradiation hardening and embrittlement.2) The irradiation temperature played different roles in terms of irradiation hardening and embrittlement for both C06M and C36M: after irradiation between 166°C and 204°C, both materials exhibited significant irradiation hardening and embrittlement; after irradiation between 315°C and 343°C, both materials showed small irradiation hardening without irradiation embrittlement. After irradiation between 501°C and 507°C, however, the irradiation softening without irradiation embrittlement was observed in both materials.3) Comparing the microhardness and Master Curve reference temperature T0q before and after neutron irradiation, we did not observe a linear correlation between the two parameters for both C06M and C36M steels. This should be mainly due to a flat response of the Master Curve reference temperature T0q to the irradiations at 166–204°C and 315–343°C ranges4) C06M showed a lower T0q, meaning better toughness, than C36M at the unirradiated condition, and such trend was kept even after neutron irradiation except for the 166–204°C irradiation after which both materials had similar T0q.5) In terms of hardening and embrittlement, the irradiation effect on both C06M and C36M appeared to saturate after an irradiation dose of 7 dpa.

Chen, Xiang↗

Design Optimization for EUROPA Critical Experiment

The Experiment for Unresolved Region Of Plutonium Actinides (EUROPA) is an integral critical experiment currently being designed to target the intermediate energy region of plutonium. Intermediate energies, those between 0.625 eV - 100 keV, contain the end of resolved and beginning of the unresolved resonance region, making experiments in this energy range prudent for validating the representation of cross sections in this transition region. Below is the preliminary design of the experiment to be performed at the National Criticality Experiments Research Center (NCERC). Experiment optimization required an exhaustive down selection of several moderating, absorbing, and reflecting materials using Particle Swarm Optimization (PSO) in order to achieve maximum sensitivity to the intermediate energy region.

07 ISOTOPE AND RADIATION SOURCES↗

Deactivation of the K-27 building at the east Tennessee Technology Park - 15554

In 1942, nearly 24,280 hectares (60,000 acres) of east Tennessee landscape became part of the most significant defense strategy in the history of the United States - the Manhattan Project. Three methods of uranium separation were pursued at the site in the effort to end World War II. What became the K-25 site, now known as the East Tennessee Technology Park, focused on the gaseous diffusion method of uranium enrichment. This paper focuses on the deactivation of the second of five gaseous diffusion plants built on the site. The four-level, rectangular-shaped K-27 came online in 1945 and was tied to the site's original gaseous diffusion plant, K-25. K-27 extended K-25's enriching stages to increase production. The plant supported weapons production and other security strategies until 1964. K-27 spans 35,582 square meters (383,000 square feet) and contains approximately 92,903 square meters (one million square feet) of floor space. During deactivation, workers will use an assembly line process to tackle the 540 process stages housed in 90 cells. While often the less publicized, less visible aspect of building decontamination and decommissioning, deactivation takes more than three times longer than demolition. Crews work in high-risk, high-hazard environments - exposed to extreme temperatures, radiological and chemical contaminants, and deteriorating infrastructure. Therefore, worker safety becomes the most rigorous task performed. K-27 is the fifth and final gaseous diffusion building in the Department of Energy's Oak Ridge Environmental Management program to be demolished. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Progress towards the Facility for Rare Isotope Beams

Muon-based facilities offer a unique potential to provide capabilities at both the Intensity Frontier with Neutrino Factories and the Energy Frontier with Muon Colliders ranging from the Higgs energy to the multi-TeV energy range. They rely on novel technology with challenging parameters, for which the feasibility is currently being assessed by the U.S. Muon Accelerator Program (MAP) [1]. A realistic scenario for a complementary series of staged facilities with increasing complexity and significant physics potential at each stage has been developed. It takes advantage of and leverages the capabilities already planned at Fermilab, especially Project X and LBNE. Each stage is defined in such a way as to provide an R&D platform to validate the technologies required for subsequent stages. The rationale and sequence of a realistic staging process are presented.

Wei, J.↗

Improvement of analytical capabilities of neutron activation analysis laboratory at the Colombian Geological Survey

The Neutron Activation Analysis (NAA) laboratory at the Colombian Geological Survey has developed a technique for multi-elemental analysis of soil and plant matrices, based on Instrumental Neutron Activation Analysis (INAA) using the comparator method. In order to evaluate the analytical capabilities of the technique, the laboratory has been participating in inter-comparison tests organized by Wepal (Wageningen Evaluating Programs for Analytical Laboratories). In this work, the experimental procedure and results for the multi-elemental analysis of four soil and four plant samples during participation in the first round on 2015 of Wepal proficiency test are presented. Only elements with radioactive isotopes with medium and long half-lives have been evaluated, 15 elements for soils (As, Ce, Co, Cr, Cs, Fe, K, La, Na, Rb, Sb, Sc, Th, U and Zn) and 7 elements for plants (Br, Co, Cr, Fe, K, Na and Zn). The performance assessment by Wepal based on Z-score distributions showed that most results obtained |Z-scores| ≤ 3.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DICER: A new instrument at LANSCE to constrain neutron capture rates on radionuclides

. With very few exceptions, direct measurements of neutron capture rates on radionuclides have not been possible. A number of indirect methods have been pursued such as the surrogate method, the γ-ray strength function method, the Oslo method and the β-Oslo method. Substantial effort has been devoted to quantify the usually large systematic errors that accompany the results from these techniques. A new instrument has been developed at the Los Alamos Neutron Science Center (LANSCE) to provide more accu rate data on several radionuclides relevant to nuclear criticality safety, radiochemical diagnostics, astrophysics, nuclear forensics and nuclear security, by measuring the transmission of neutrons through radioactive samples and studying resonance properties. The Device for Indirect Capture on Radionuclides (DICER) and as sociated radionuclide production at the Isotope Production Facility (IPF), both at LANSCE, as well radioactive sample fabrication, have been under development the last few years. A description of the new apparatus, data on a few mid-weight stable isotopes and efforts on radionuclide measurements will be presented.

Nuclear Criticality Safety Program (NCSP)↗

Operation of the “Small” BioAMS spectrometers at CAMS: Past and future prospects

A summary of results from the solid samples run on our compact 1 MV AMS system over its 13.5 years of operation is presented. On average 7065 samples per year were measured with that average dropping to 3278 samples per year following the deployment of our liquid sample capability. Although the dynamic range of our spectrometer is 4.5 orders in magnitude, most of the measured graphitic samples had 14 C/C concentrations between 0.1 and 1 modern. Furthermore, the measurements of our ANU sucrose standard followed a Gaussian distribution with an average of 1.5082 ± 0.0134 modern. The LLNL biomedical AMS program supported many different types of experiments, however, the large majority of samples measured were derived from animal model systems. We have transitioned all of our biomedical AMS measurements to the recently installed 250 kV SSAMS instrument with good agreement compared in measured 14C/C isotopic ratios between sample splits. We then present results from replacement of argon stripping gas with helium in the SSAMS with a 22% improvement in ion transmission through the accelerator and high-energy analyzing magnet.

14C↗

Effect of Pt promotion on Ni/Al{sub 2}O{sub 3} for the selective catalytic reduction of NO with hydrogen

Ni/Al{sub 2}O{sub 3} (10 wt.% Ni) and Ni-Pt/Al{sub 2}O{sub 3} (10 wt.% Ni, 0.5 wt.% Pt) were comparatively tested in the hydrogen selective catalytic reduction process (H{sub 2}-SCR), at reaction temperatures below 350°C. Catalytic activity tests consisted in temperature programmed reactions (TPRea) under plug flow conditions from 50 to 350°C, with a temperature rate of 5°C/min, using a feed stream with a reactant ratio NO:H{sub 2} = 1:1.3 and a GHSV of 4500 h{sup −1}. Promotion with Pt increases the catalytic performances of the Ni based catalyst, in respect to NO conversion, N{sub 2} selectivity and N{sub 2} yield. The reaction temperatures for NO conversion above 95% decrease significantly due to Pt addition, from 250°C for Ni/Al{sub 2}O{sub 3} to 125°C for Ni-Pt/Al{sub 2}O{sub 3}. Characterization of catalysts was performed by: X ray powder diffraction (XRD) for the estimation of Ni crystallite size, temperature programmed reduction (TPR) for the catalyst reducibility, temperature programmed desorption of hydrogen (H{sub 2}-TPD) for the investigation of active sites and metal dispersion on the support, N{sub 2} adsorption-desorption isotherms at −196°C for the determination of total specific surface area and pore size distribution, and H/D isotopic exchange on the catalyst surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

IDB Loader

SAND2024-08428O The IDB Loader is a database designed to hold gamma spectra. IDB is a web-accessible database of reference gamma spectra for measuring uranium (U) and plutonium (Pu) isotopic composition. The database, developed by the International Atomic Energy Agency (IAEA), provides access to well-characterized groups of gamma spectra curated by international experts in gamma spectroscopy. It was created to promote sustainability and maintenance of software used to determine the isotopic abundances of U and Pu. The IDB Loader works by uploading one set of spectral data into an existing IDB. The Data Loader package includes documentation describing the IDB's table, the format of the spectral data, and a description of the loader program. The IDB is currently hosted by the IAEA at: https://nds.iaea.org/idb Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Schwartz, Steven↗

Corrosion Evaluation of RERTR Uranium Molybdenum Fuel

As part of the National Nuclear Security Agency (NNSA) mandate to replace the use of highly enriched uranium (HEU) fuel for low enriched uranium (LEU) fuel, research into the development of LEU fuel for research reactors has been active since the late 1970’s. Originally referred to as the Reduced Enrichment for Research and Test Reactor (RERTR) program the new effort named Global Threat Reduction Initiative (GTRI) is nearing the goal of replacing the standard aluminum clad dispersion highly enriched uranium aluminide fuel with a new LEU fuel. The five domestic high performance research reactors undergoing this conversion are High Flux Isotope reactor (HFIR), Advanced Test Reactor (ATR), National Institute of Standards and Technology (NIST) Reactor, Missouri University Research Reactor (MURR) and the Massachusetts Institute of Technology Reactor II (MITR-II). The design of these reactors requires a higher neutron flux than other international research reactors, which to this point has posed unique challenges in the design and development of the new mandated LEU fuel. The new design utilizes a monolithic fuel configuration in order to obtain sufficient 235U within the LEU stoichoimetry to maintain the fission reaction within the domestic test reactors. The change from uranium aluminide dispersion fuel type to uranium molybdenum (UMo) monolithic configuration requires examination of possible corrosion issues associated with the new fuel meat. A focused analysis of the UMo fuel under potential corrosion conditions, within the ATR and under aqueous storage indicates a slow and predictable corrosion rate. Additional corrosion testing is recommended for the highest burn-up fuels to confirm observed corrosion rate trends. This corrosion analysis will focus only on the UMo fuel and will address corrosion of ancillary components such as cladding only in terms of how it affects the fuel. The calculations and corrosion scenarios are weighted with a conservative bias to provide additional confidence with the results. The actual corrosion rates of UMo fuel is very likely to be lower than assumed within this report which can be confirmed with additional testing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Updates and Validation for the n+ 63,65 Cu Cross Sections [Slides]

The RRR and URR parameters for 63,65 Cu have been optimized to transmission and capture data. Several data sets have been newly incorporated in this evaluation. The angular distribution parameters have been adopted from differential measurements, as was done in ENDF/B-V. The performance of this evaluation in the integral benchmark calculations is favorable, and the validation is ongoing.

07 ISOTOPE AND RADIATION SOURCES↗

Improving the probability tables of the cross section of near closed-shell nuclei [Slides]

The level density distribution of near closed-shell nuclei is much lower than the typical nucleus, therefore, the cross sections show significant fluctuations, and these fluctuations are not predictable. The current methodology used to describe such behavior and construct the probability table of the cross section is based on the extrapolation of the average resonance widths and average resonance spacings from the resonance region and use these parameters to construct the probability table. Although this is a standard and widely used technique, it does not take into account the existing experimental data, such for total and the elastic cross section. Our goal is to extend the current theory and provide a more general approach to compute the probability distribution function of the cross section combining the existing probability tables and the available experimental data. Results will be presented for 90 Zr.

07 ISOTOPE AND RADIATION SOURCES↗