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At least 451 records · Page 25

New Resolved Resonance Region Evaluation for 63Cu and 65Cu for Nuclear Criticality Safety Program

A new resolved resonance region evaluation of 63Cu and 65Cu was done in the energy region from 10-5 eV to 99.5 keV. The R-Matrix SAMMY method using the Reich-Moore approximation was used to create a new set of consistent resonance parameters. The new evaluation was based on three experimental transmission data sets; two measured at ORELA and one from MITR, and two radiative capture experimental data sets from GELINA. A total of 141 new resonances were identied for 63Cu and 117 for 65Cu. The corresponding set of external resonances for each isotope was based on the identied resonances above 99.5 keV from the ORELA transmission data. The negative external levels (bound levels) were determined to match the dierential thermal cross section measured at the MITR. Double dierential elastic scattering cross sections were calculated from the new set of resonance parameters. Benchmarking calculations were carried out on a set of ICSBEP benchmarks. This work is in support of the DOE Nuclear Criticality Safety Program.

Sobes, Vladimir↗

Can a radiological event impact a criticality safety program: Lessons learned at WIPP - 14350

Any accident at a nuclear facility impacts all departments involved in the operation of the facility. The radiological release that occurred on February 14, 2014 has halted all waste disposal operations at the Waste Isolation Pilot Plant (WIPP) and has resulted in detailed reviews of all safety management programs. This paper describes the initial reactions to the event, criticality issues with recovery operations, corrective actions for the criticality safety program from independent reviews, and the importance of configuration management to criticality safety. The nature, location, and timing of the event resulted in significant delays in determining the cause of the event. During this time multiple theories on the initiator of the event were postulated including and inadvertent criticality event. However, the timing of the event, average fissile gram equivalent (FGE) loading of waste containers compared to analyzed FGE loads, and isotopic analysis of fixed air samples taken during the event proved it was not an inadvertent criticality event. Recovery activities such as replacing contaminated high efficiency particulate (HEPA), filters and disposing of site generated waste have also been reviewed to prevent criticality safety issues. Post event corrective actions in all departments have impacted how future operations at WIPP will be conducted, including corrective actions for the criticality safety program. The event has also proven the importance of configuration management and the effect a change can have on a process. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Studies of exotic nuclei with few-nucleon transfer reactions (Final Report)

This document serves as the final report on work done on the research supported by U. S. DOE Grant DE-FG02-ER-41320, A. H. Wuosmaa Principal Investigator, supporting institution Western Michigan University. The grant was first funded in 2004, and continued until the PI officially terminated his employ at Western Michigan University and moved to the University of Connecticut in August of 2014. Throughout its course, the goals of this project have been to determine the properties of exotic nuclei using few nucleon transfer reactions, and to develop new technical approaches to study such transfer reactions in inverse kinematics, in particular with rare-isotope beams. The work focused primarily on light-exotic nuclei studied using beams of rare-isotope beams produced at the ATLAS facility at Argonne National Laboratory. Additional research was conducted at the Michigan State University National Superconducting Cyclotron Laboratory, and the Western Michigan University Tandem Van de Graaff accelerator laboratory. A major goal and significant accomplishment of the program was the conceptual design, development, construction, commissioning and utilization of the HELIOS (HELIcal Orbit Spectrometer) device at Argonne National Laboratory. The concept of the solenoid spectrometer was presented in the first proposal submitted for this grant program, and with the close of this grant project the device is operating routinely and has been used in more than 20 experiments since its initial commissioning in 2008. The main physics goals of this project included producing new data for p and light-sd shell nuclei to test the predictions of ab-initio theoretical methods, as well as shell-model calculations for sd nuclei. Over its course, the project has generated data for (d,p), (d, 3 He) and (d, 4 He) reactions on many nuclei far from stability, and the data have informed both ab-initio and shell-model approaches.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Assembly and Delivery of Rabbit Capsules for Irradiation of Silicon Carbide Cladding Tube Specimens in the High Flux Isotope Reactor

Neutron irradiation of silicon carbide (SiC)-based fuel cladding under a high radial heat flux presents a critical challenge for SiC cladding concepts in light water reactors (LWRs). Fission heating in the fuel provides a high heat flux through the cladding, which, combined with the degraded thermal conductivity of SiC under irradiation, results in a large temperature gradient through the thickness of the cladding. The strong temperature dependence of swelling in SiC creates a complex stress profile in SiCbased cladding tubes as a result of differential swelling. The Nuclear Science User Facilities (NSUF) Program within the US Department of Energy Office of Nuclear Energy is supporting research efforts to improve the scientific understanding of the effects of irradiation on SiC cladding tubes. Ultimately, the results of this project will provide experimental validation of multi-physics models for SiC-based fuel cladding during LWR operation. The first objective of this project is to irradiate tube specimens using a previously developed design that allows for irradiation testing of miniature SiC tube specimens subjected to a high radial heat flux. The previous “rabbit” capsule design uses the gamma heating in the core of the High Flux Isotope Reactor (HFIR) to drive a high heat flux through the cladding tube specimens. A compressible aluminum foil allows for a constant thermal contact conductance between the cladding tubes and the rabbit housing despite swelling of the SiC tubes. To allow separation of the effects of irradiation from those due to differential swelling under a high heat flux, a new design was developed under the NSUF program. This design allows for irradiation of similar SiC cladding tube specimens without a high radial heat flux. This report briefly describes the irradiation experiment design concepts, summarizes the irradiation test matrix, and reports on the successful delivery of six rabbit capsules to the HFIR. Rabbits of both low and high heat flux configurations have been assembled, welded, evaluated, and delivered to the HFIR along with a complete quality assurance fabrication package. These rabbits contain a wide variety of specimens including monolith tubes, SiC fiber SiC matrix (SiC/SiC) composites, duplex specimens (inner composite, outer monolith), and specimens with a variety of metallic or ceramic coatings on the outer surface. The rabbits are targeted for insertion during HFIR cycle 475, which is scheduled for September 2017.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effect of high fluence neutron irradiation on transport properties of thermoelectrics

Thermoelectric materials were subjected to high fluence neutron irradiation in order to understand the effect of radiation damage on transport properties. This paper is relevant to the NASA Radioisotope Thermoelectric Generator (RTG) program in which thermoelectric elements are exposed to radiation over a long period of time in space missions. Selected n-type and p-type bismuth telluride materials were irradiated at the High Flux Isotope Reactor with a neutron fluence of 1.3 × 10 18 n/cm 2 (E > 0.1 MeV). The increase in the Seebeck coefficient in the n-type material was partially off-set by an increase in electrical resistivity, making the power factor higher at lower temperatures. For the p-type materials, although the Seebeck coefficient was not affected by irradiation, electrical resistivity decreased slightly. The figure of merit, zT, showed a clear drop in the 300–400 K range for the p-type material and an increase for the n-type material. Considering that the p-type and n-type materials are connected in series in a module, the overall irradiation damages at the device level were limited. Finally, these results, at neutron fluences exceeding a typical space mission, are significant to ensure that the radiation damage to thermoelectrics does not affect the performance of RTGs.

36 MATERIALS SCIENCE↗

Blind QC trend presentation

Blind testing is used to evaluate performance of the radiobioassay laboratory. DOE-STD-1112-2019 requires a radiobioassay program to perform blind testing at a documented frequency including accuracy, false positive, false negative, and sensitivity evaluations. INL trends accuracy determinations over time for bias, agreement, and precision. Trends have been identified for certain isotopes in urine and feces that have not been fully explained. This presentation will review those identified trends and discuss possible causes and solutions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Nucleosynthesis for Science and Security: Preparing for a Nuclear and Chemical Sciences Program at FRIB

Nuclear reactions are vital to nuclear science and its many applications: they are the mechanism for forging elements in the cosmos, the source of energy for both stars and nuclear weapons, the principal probes used to study nuclear properties, and the primary diagnostic signatures for stockpile stewardship and nuclear forensics. Yet, most reaction experiments have been confined to the small fraction of all nuclei that are stable, and a theoretical foundation for reactions with a true predictive capability is lacking. The Facility for Rare Isotope Beams (FRIB), the flagship U.S. facility in low-energy nuclear science, will offer the opportunity to rectify the long-standing gap in understanding reactions on radioactive nuclei. The work performed in this LDRD project brought together the experimental nuclear physics, radiochemistry, nuclear theory, and high-performance computing expertise of the Nuclear and Chemical Sciences Division to develop new techniques that will be needed to exploit FRIB beams to better understand nuclear reactions. Novel isotope-harvesting techniques were developed to demonstrate that samples could be collected at the National Superconducting Cyclotron Laboratory (NSCL) at Michigan State University (the facility which FRIB builds upon) for direct measurements of long-lived radioisotopes. For isotopes too short lived for direct measurements, indirect approaches were developed that would ultimately be used with high-intensity FRIB radioactive beams. Finally, to better interpret experimental results and reliably extend predictions beyond the available data, a foundation was established for a fully microscopic and unified description of the structure, interactions, and dynamics of two reacting nuclei that moves beyond empirical models. This work has positioned the team for a leadership role at FRIB, enabling LLNL to maintain a world-class nuclear science program and to compete for future talent and funding, both of which are vital for continuing support of the laboratory’s stockpile stewardship mission.

42 ENGINEERING↗

Nature of Reactive Hydrogen for Ammonia Synthesis over a Ru/C12A7 Electride Catalyst

Recently, there have been renewed interests in exploring new catalysts for ammonia synthesis under mild conditions. Electride-based catalysts are among the emerging ones. Ruthenium particles supported on an electride composed of a mixture of calcium and aluminum oxides (C12A7) have attracted great attention for ammonia synthesis due to their facile ability in activating N2 under ambient pressure. However, the exact nature of the reactive hydrogen species and the role of electride support still remain elusive for this catalytic system. Here, we report for the first time that the surface-adsorbed hydrogen, rather than the hydride encaged in the C12A7 electride, plays a major role in ammonia synthesis over the Ru/C12A7 electride catalyst with the aid of in situ neutron scattering techniques. Combining in situ neutron diffraction, inelastic neutron spectroscopy, density functional theory (DFT) calculation, and temperature-programmed reactions, the results provide direct evidence for not only the presence of encaged hydrides during ammonia synthesis but also the strong thermal and chemical stability of the hydride species in the Ru/C12A7 electride. Steady state isotopic transient kinetic analysis (SSITKA) of ammonia synthesis showed that the coverage of reactive intermediates increased significantly when the Ru particles were promoted by the electride form (coverage up to 84%) of the C12A7 support rather than the oxide form (coverage up to 15%). Such a drastic change in the intermediate coverage on the Ru surface is attributed to the positive role of electride support where the H2 poisoning effect is absent during ammonia synthesis over Ru. The finding of this work has significant implications for understanding catalysis by electride-based materials for ammonia synthesis and hydrogenation reactions in general.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fuel Cycle Research & Development Technical Monthly – May 2012

Management and Integration LANL - Initial coordination meetings with NE and NA-20 were held the first week of May. Additional meetings, to include NA-82 and the new Proliferation and Terrorism Risk Assessment task are scheduled for June. Work package planning as part of the NTD transition is ongoing. Microcalorimetry LANL - Some parts to attempt repair of a malfunctioning water chiller that has been holding up work on the current detector array have arrived. We will attempt to begin running the compressor/cryostat next week to resume work on commissioning the detector array. We have also been working on a backup plan to temporarily move our system to a different lab space. Completed data analysis and prepared a paper summarizing Pu measurements for peer-review journal. Two members of our team presented work at the SORMA West 2012 conference. Completed data analysis and prepared a milestone report summarizing the development of Monte Carlo tools to study systematic errors. Electrochemical Sensor INL - The second sensor test was stopped short due to the work stand-down. Some activities related to this work have resumed, but not all. The sensor used during the second test was removed from the furnace and it showed cracks and later crumbled when being rinsed for sample preparation. The sensor material will be submitted to SEM analysis once work is resumed in the facilities where analysis is performed. A third sensor test has started. Tests with different arrangements will continue and will be oriented based on post-test analysis of the first three sensor tests. Materials with different annealing temperatures will also be prepared for analysis. Lead slowing down spectrometer LANL - Continued work on perturbation method for LSDS analysis. We are running simulations to delineate issues and are checking additional data libraries to see whether there are differences in simulation results. Electrochemical sensor INL - The second sensor test was stopped short due to the work stand-down. Some activities related to this work have resumed, but not all. The sensor used during the second test was removed from the furnace and it showed cracks and later crumbled when being rinsed for sample preparation. The sensor material will be submitted to SEM analysis once work is resumed in the facilities where analysis is performed. A third sensor test has started. Tests with different arrangements will continue and will be oriented based on post-test analysis of the first three sensor tests. Materials with different annealing temperatures will also be prepared for analysis. Fast Neutron Multiplicity analysis INL - The University of Michigan team continues its work on the post-experiment analysis of the validation data from JRC ISPRA, as well as scoping studies using the simulation tool MCNPX-PoliMi. At INL, our new staff member working on this project is now working to model performance capabilities for the fast-neutrons scintillator design concepts. At INL our primary analysis approach is focused on the Feynman mean-to-variance approach. At the University of Michigan, the primary analysis approach is multiplicity coincidence analysis. Fast Neutron Imaging to Quantify Nuclear Materials ORNL - Completed additional measurements of the two 'trainer' configurations as well as calibration measurements with sources on an x-y stage. The imager was shipped to Pantex for an NA-22 obligation at the end of May. Lead Slowing Down Spectrometer LANL - Continued to look into He4 detector. A Swiss company was located that makes He4 detectors and associated electronics. Had a teleconference with them to assess the possible help we can get from them. We are also looking in to constructing one locally. Ongoing perturbation calculations are providing information on the fundamental systematic error limits of LSDS. In order to achieve separating the contribution of Pu and 235U to the signal, there will need to be tight controls on systematic errors. Multi-isotope Process Monitor PNNL - Attended a training call in advanced multivariate classification and analysis methods. These methods were applied to the multivariate analysis of fuel characteristics based on simulated gamma. Work continued on a computational framework to quantify the impact of gamma-ray counting statistical precision on principal component regression (PCR) analysis of a multi-component (i.e. multi-isotope) gammaray spectrum. Tests of the simulation framework are anticipated to begin in early June. Development of a proposal to instrument H-Canyon is being prepared in conjunction with SRNL and the NNSA's NGSI program is ongoing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Neutron Capture and Transmission Measurements of 54 Fe at the RPI LINAC [Slides]

Transmission and capture measurements provide a wholistic set of experimental data to start resonance evaluation on 54 Fe. Analysis thus far supports that changes are needed in 54 Fe evaluation. Major accomplishments include the completion of radiative capture measurements of 54 Fe and the completion of total cross section measurements of 54 Fe. Future work includes the completion of data analysis relevant to capture and transmission measurements (May 2022), complete fitting of new resonance parameters to 54 Fe data (early 2023), and completion of all required deliverables for graduation (May 2023).

07 ISOTOPE AND RADIATION SOURCES↗

Energy Dependent Fission Product Yields (2nd year Milestone and Deliverables)

Introduction to the project: One of the Laboratory missions is to provide consistent, high-precision fission product; yield data critical for testing fission models and maintaining the safety and security of the nation’s nuclear weapons stockpile. However, high-quality, energy-differential fission product yield data is missing for certain actinides and neutron energies important to constrain the new U.S. Nuclear Data Program evaluation effort; It has been shown that the reactor antineutrino anomaly may be at least partially caused by roughly 20 fission products. The fission product yield data is missing or incomplete for many of these isotopes, thus it is necessary to accurately determine these values to better constrain the anomaly; Aitor Bracho is measuring very short-lived (seconds to minutes) fission product yields of 235 U and 239 Pu using monoenergetic neutron beams at E n = 60 and 560 keV; Aitor Bracho is using a direct approach utilizing a state-of-the-art rabbit transfer system, superior HPGe detector, and digital acquisition systems for fission decay measurements. The goals of this project: lop experimental capabilities and data analysis techniques to carry out the gamma-ray spectra analysis necessary for fission product yield calculation; Provide high-precision and energy-dependent fission product data supporting fission theory, neutrino physics, and applied physics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Report on New and Upgraded National User Facilities in Basic Energy Sciences

On December 1, 2023, the Director of the of the Office of Science (SC) charged all the Department of Energy Office of Science Federal Advisory Committees to respond to look toward the scientific horizon and identify what new or upgraded facilities will best serve the SC community needs in the next ten years (2024-2034). This report by the Basic Energy Sciences Advisory Committee (BESAC) assess facilities for the Basic Energy Sciences (BES) program.

07 ISOTOPE AND RADIATION SOURCES↗