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At least 217 records · Page 12

Activation Mechanism and Surface Intermediates during Olefin Metathesis by Supported MoO x /Al 2 O 3 Catalysts

The activation of supported MoO x /Al 2 O 3 catalysts and the resulting surface intermediates were examined with in situ DRIFTS during olefin metathesis reaction conditions, aided by C 3 D 6 -C 3 H 6 isotopically labeled switching, C 2 H 4 -C 4 H 8 titration, and temperature programmed reaction experiments. The studies shows that activation by propylene of the surface MoO x sites on Al 2 O 3 initiates by forming surface isopropoxide species that subsequently dehydrogenate to acetone and surface Mo-OH. Desorption of acetone from the catalyst surface reduces the Mo +6 sites to Mo +4 sites, creating a vacancy for coordination of the next CH 2 =CHCH 3 molecule. Oxidative addition from subsequent adsorption of propylene on the surface Mo +4 sites results in formation of surface Mo=CH 2 and Mo=CHCH3 reactive intermediates, oxidizing the reduced surface molybdena sites back to Mo +6 . This study demonstrates the activation mechanism and surface intermediates during olefin metathesis by supported MoO x /Al 2 O 3 catalysts under reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The DarkSide project

DarkSide is a graded experimental project based on radiopure argon, and is now, and will be, used in direct dark matter searches. The present DarkSide-50 detector, operating at the Gran Sasso National Laboratory, is a dual-phase, 50 kg, liquid argon time-projection-chamber surrounded by an active liquid scintillator veto. It is designed to be background free in 3 years of operation. DS-50 performances, when filled with atmospheric argon, are reported. However DS-50 filled with underground argon, shows impressive reduction of the 39Ar isotope. The application of this powerful technology in a future generation of the DarkSide program is discussed.

Agnes, P.↗

Fission Induced Electromagnetic Response

The FIER (Fission Induced Electromagnetic Response) code is a C++ program designed to predict delayed gamma-ray spectra following fission. Given a fissioning isotope and irradiation scheme, FIER will determine the decay chains for each fission fragment and their daughters. Each product’s time-dependent population is calculated using an analytical solution to the Bateman equations that guide decay transmutation. These populations are then used to calculate the number of gamma-ray emissions for a given counting scheme. A Monte Carlo method is also available to determine the uncertainty of the fission product populations and delayed gamma-ray intensities based on the uncertainties on the input nuclear data.

Matthews, EricFrancis [University of California - ↗

Recommendations for the generation, quantification, storage and handling of peptides used for mass spectrometry-based assays

The Clinical Proteomic Tumor Analysis Consortium (1) (CPTAC) of the National Cancer Institute (NCI) is a comprehensive and coordinated effort to accelerate the understanding of the molecular basis of cancer through the application of robust technologies and workflows for the quantitative measurements of proteins. The Assay Development Working Group of the CPTAC Program aims to foster broad uptake of targeted mass spectrometry-based assays employing isotopically labeled peptides for confident assignment and quantification, including multiple reaction monitoring (MRM; also referred to as Selected Reaction Monitoring), parallel reaction monitoring (PRM), and other targeted methods.

Environmental Molecular Sciences Laboratory↗

Performance Evaluation of the CHKED Multi-Elemental Analysis and Software

The Hybrid K-edge Densitometer (HKED) is a high precision safeguards assay system developed by Ottmar and Eberle [1] for quantification of the U and Pu concentrations of dissolver solutions in spent nuclear fuel reprocessing. The HKED measurement supplements traditional destructive assay methods such as Isotope Dilution Mass Spectrometry (IDMS) and is an essential component of the international safeguards program implementation at these facilities. The Canberra Hybrid K-Edge Densitometry (CHKED) software was recently developed by Canberra Industries to better address the changing composition of the nuclear fuel cycle by addition of a multi-elemental analysis capability to the K-Edge transmission measurement. Our evaluation of the CHKED software was performed at the request of the International Atomic Energy Agency (IAEA) to examine the functionality and performance of the CHKED software and algorithms and identify potential areas for improvement of the software. The reader is assumed to be familiar with the HKED technique and its current implementation in safeguards assay of U and Pu in the nuclear fuel cycle. The Canberra Hybrid K-Edge Densitometry CHKED software replicates functionality of the older VMSbased Hybrid K-Edge Densitometer (HKED) software and incorporates additional analysis algorithms and tools. When the traditional HKED analyses are selected, the CHKED software appears to faithfully reproduce the measurement results as reported by the older software. The CHKED software includes a Multi-elemental K-Edge (MEKED) analysis based in part on algorithms devised at Los Alamos National Laboratory. In principle, the MEKED analysis represents a significant advancement over the traditional HKED analysis, providing a capability to analyze the actinide concentrations from complex solutions, such as low U:Pu ratios (e.g., U:Pu = 1:1) including additional minor actinide components such as Np and Am. However, this MEKED analysis is somewhat limited by reliance on a region of interest (ROI) analysis of the spectrum, the need for extensive calibration measurements and a simplistic interpretation of the KED transmission spectrum. Finally, the MEKED algorithm set associated with the CHKED software (V1.0) acquired by Oak Ridge National Laboratory (ORNL) from Canberra Industries does not seem to be “finished” (e.g., the MEKED analysis seems to only determine measurement results for two actinides with while results for the minor actinides appear to be highly dependent on declaration values).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Geochemical Changes in Response to CO 2 Injection in a CO 2 -EOR Complex in Northern Michigan

The overall purpose of the geochemical monitoring program under Midwestern Regional Carbon Sequestration Partnership (MRCSP) is to use stable and radiogenic isotope geochemistry in concert with analysis of general geochemical parameters of fluids and gases and analysis of core samples to determine geochemical processes occurring in the reef structure because of CO 2 injection..

54 ENVIRONMENTAL SCIENCES↗

ORNL Contributions to the ENDF/B-VIII.1 Library [Slides]

For uranium and plutonium isotopes, evaluation work is converging to a stable configuration with an overall satisfactory benchmark performance (more information on the validation tests after CSEWG). Strontium evaluation was included in the repository library and successfully tested by processing codes relative to an alternative quantification of the external function. Cerium covariance matrices were updated to address review comments on the magnitude of the uncertainty. For future uncertainty quantification, theoretical observables should be properly decoupled from current measured guidelines. Tests to correctly include LP (from resonance parameters) fitted to measured energy-averaged data are in progress. Current ENDF files contains experimental LP data.

07 ISOTOPE AND RADIATION SOURCES↗

Sister Rod Destructive Examinations (FY23) Appendix D: Fission Gas, Fuel Burnup, and Fuel Isotopic Measurements

As a part of DOE NE High Burnup Spent Fuel Data Project, Oak Ridge National Laboratory (ORNL) is performing destructive examinations (DEs) of high burnup (HBU) (>45 GWd/MTU) spent nuclear fuel (SNF) rods from the North Anna Nuclear Power Station operated by Dominion Energy. The SNF rods, called sister rods or sibling rods, are all HBU and include four different kinds of fuel rod cladding: standard Zircaloy-4 (Zirc-4), low-tin (LT) Zirc-4, ZIRLO, and M5. The DEs are being conducted to obtain a baseline of the HBU rod’s condition before dry storage and are focused on understanding overall SNF rod strength and durability. Composite fuel and defueled cladding will be tested to derive material properties. Although the data generated can be used for multiple purposes, one primary goal for obtaining the post-irradiation examination data and the associated measured mechanical properties is to support SNF dry storage licensing and relicensing activities by (1) addressing identified knowledge gaps and (2) enhancing the technical basis for post-storage transportation, handling, and subsequent disposition. This appendix documents the status of the ORNL Phase 1 DE activities related to fission gas sample analysis, fuel burnup analysis, and fuel isotopic analysis of selected sister specimens in Phase 1 of the sister rod test program.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Gas Reactor (AGR)-5/6/7 Fuel Irradiation Experiments in the Advanced Test Reactor

The United States Department of Energy’s Very High Temperature Reactor (VHTR) Advanced Gas Reactor (AGR) Fuel Development and Qualification Program will be irradiating up to seven separate low enriched uranium (LEU) tri-isotopic (TRISO) particle fuel (in compact form) experiments in the Advanced Test Reactor (ATR) located at the Idaho National Laboratory (INL). These irradiations and fuel development are being accomplished to support development of the next generation reactors in the United States. The goals of the irradiation experiments are to provide irradiation performance data to support fuel process development, to qualify fuel for normal operating conditions, to support development and validation of fuel performance and fission product transport models and codes, and to provide irradiated fuel and materials for post irradiation examination (PIE) and safety testing. The experiments, which each consist of at least five separate capsules, are being irradiated in an inert sweep gas atmosphere with individual on-line temperature monitoring and control of each capsule. The sweep gases also have on-line fission product monitoring the effluent from each capsule to track performance of the fuel during irradiation. The first two experiments (designated AGR-1 and AGR-2), have been completed. The third and fourth experiments have been combined into a single experiment designated AGR-3/4, which started its irradiation in December 2011 and is currently scheduled to be completed in April 2014. The design of the fuel qualification experiment, designated AGR-5/6/7, is well underway and incorporates lessons learned from the three previous experiments. Various design issues will be discussed with particular details related to selection of thermometry.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

JHR Project: a future Material Testing Reactor working as an International user Facility: The key-role of instrumentation in support to the development of modern experimental capacity

Research and development on fuel and material behaviour under irradiation is a key issue for sustainable nuclear energy in order to meet specific needs by keeping the best level of safety. These needs mainly deal with a constant improvement of performances and safety in order to optimize the fuel cycle and hence to reach nuclear energy sustainable objectives. A sustainable nuclear energy requires a high level of performances in order to meet specific needs such as: - Pursuing improvement of the performances and safety of present and coming water cooled reactor technologies. This will require a continuous R and D support following a long-term trend driven by the plant life management, safety demonstration, flexibility and economics improvement. Experimental irradiations of structure materials are necessary to anticipate these material behaviours and will contribute to their optimisation. - Upgrading continuously nuclear fuel technology in present and future nuclear power plants to achieve better performances and to optimise the fuel cycle keeping the best level of safety. Fuel evolution for generation II, III and III+ is a key stake requiring developments, qualification tests and safety experiments to ensure the competitiveness and safety: experimental tests exploring the full range of fuel behaviour determine fuel stability limits and safety margins, as a major input for the fuel reliability analysis. To perform such accurate and innovative progress and developments, specific and ad hoc instrumentation, irradiation devices, measurement methods are necessary to be set up inside or beside the material testing reactor (MTR) core. These experiments require beforehand in situ and on line sophisticated measurements to accurately determine different key parameters such as thermal and fast neutron fluxes and nuclear heating in order to precisely monitor and control the conducted assays. The new Material Testing Reactor JHR (Jules Horowitz Reactor) currently under construction at CEA Cadarache research centre in the south of France will represent a major Research Infrastructure for scientific studies regarding material and fuel behavior under irradiation. It will also be devoted to medical isotopes production. Hence JHR will offer a real opportunity to perform R and D programs regarding needs above and hence will crucially contribute to the selection, optimization and qualification of these innovative materials and fuels. The JHR reactor objectives, principles and main characteristics associated to specific experimental devices associated to measurement techniques and methodology, their performances, their limitations and field of applications will be presented and discussed. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Investigating Similarity Differences for Light-Water-Moderated and Polyethylene-Moderated Systems

Oak Ridge National Laboratory has performed validation studies in support of Pacific Northwest Laboratory’s analysis of the Sum-of-Fractions method. Work in a companion paper examines the validation methods and results for various mixtures of fissile isotopes in various concentrations moderated and reflected by light-water and polyethylene. Those results indicate a greater coverage of critical experiments for validating light water moderated and reflected systems vs. those with polyethylene. The work presented here details the analysis of differences between light-water and polyethylene systems developed from the different concentration mixtures utilized in the Sum-of-Fractions validation study. Differences in actinide contributions are detailed, explaining the differences in ck for the various systems. The available tools and analysis techniques in TSUNAMI are described to illustrate how these types of differences can be understood by practitioners.

07 ISOTOPE AND RADIATION SOURCES↗

Toward Predictive Theories of Nuclear Reactions Across the Isotopic Chart: Web Report

Recent years have seen exciting new developments and progress in nuclear structure theory, reaction theory, and experimental techniques, that allow us to move towards a description of exotic systems and environments, setting the stage for new discoveries. The purpose of the 5-week program was to bring together physicists from the low-energy nuclear structure and reaction communities to identify avenues for achieving reliable and predictive descriptions of reactions involving nuclei across the isotopic chart. The 4-day embedded workshop focused on connecting theory developments to experimental advances and data needs for astrophysics and other applications. Nuclear theory must address phenomena from laboratory experiments to stellar environments, from stable nuclei to weakly-bound and exotic isotopes. Expanding the reach of theory to these regimes requires a comprehensive understanding of the reaction mechanisms involved as well as detailed knowledge of nuclear structure. A recurring theme throughout the program was the desire to produce reliable predictions rooted in either ab initio or microscopic approaches. At the same time it was recognized that some applications involving heavy nuclei away from stability, e.g. those involving fi ssion fragments, may need to rely on simple parameterizations of incomplete data for the foreseeable future. The goal here, however, is to subsequently improve and refine the descriptions, moving to phenomenological, then microscopic approaches. There was overarching consensus that future work should also focus on reliable estimates of errors in theoretical descriptions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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

The neutron induced total, elastic, and capture cross sections of 63,65 Cu isotopes were selected for evaluation in the resolved and unresolved resonance energy ranges by the National Criticality Safety Program to resolve discrepancies related to benchmark performance. This is especially evident for the series of ZEUS benchmarks in which copper is used as a reflector. Because copper is also used as structural material in both fission and fusion reactors, the need to address benchmark discrepancies linked to nuclear data deficiencies is a task of primary importance. The aim of this work is to describe the steps of evaluation work towards a consistent improvement of the benchmark performance. The R-matrix analysis with the SAMMY code focused on the 63 Cu(n,γ) reaction channel between 100-300 keV coupled to unresolved resonance region parameters up to 650 keV to fit average cross section data from a recent experiment. Due to the high sensitivity of many benchmarks to elastic scattering angular distribution data, especially for the 65 Cu isotope, the impact of these data was tested by generating Legendre coefficients from both resonance parameters and the Hauser-Feshbach model. Guided by the findings of Shaw et al., the performance of the current evaluation for 65 Cu was compared to that of ENDF/B-VII.1 and ENDF/B-VIII.0 by testing the reactivity coefficients corresponding to the validation suite of experimental criticality benchmarks for thermal, intermediate, and fast systems taken from the International Criticality Safety Benchmark Experiments Project Handbook. The benchmark performance is especially sensitive to 63 Cu(n,γ) and 65 Cu elastic scattering for neutron energies in the 100–500 keV region, whereas 100 keV is the upper limit of the resolved resonance region in the ENDF/B-VIII.0 evaluations for 63,65 Cu. The results highlight the need to handle the transition from the resolved resonance region to the high energy region carefully.

07 ISOTOPE AND RADIATION SOURCES↗

Waste Management Strategies for Production of Mo-99

Production of Mo-99 for medical isotope use is being investigated using dissolved low enriched uranium (LEU) fissioned using an accelerator driven process. With the production and separation of Mo-99, a low level waste stream will be generated. Since the production facility is a commercial endeavor, waste disposition paths normally available for federally generated radioactive waste may not be available. Disposal sites for commercially generated low level waste are available, and consideration to the waste acceptance criteria (WAC) of the disposal site should be integral in flowsheet development for the Mo-99 production. Pending implementation of the “Uranium Lease and Take-Back Program for Irradiation for Production of Molybdenum-99 for Medical Use” as directed by the American Medical Isotopes Production Act of 2012, there are limited options for disposing of the waste generated by the production of Mo-99 using an accelerator. The commission of a trade study to assist in the determination of the most favorable balance of production throughput and waste management should be undertaken. The use of a waste broker during initial operations of a facility has several benefits that can offset the cost associated with using a subcontractor. As the facility matures, the development of in-house capabilities can be expanded to incrementally reduce the dependence on a subcontractor.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Equilibrium Isotope Fractionation with LANL Thermochemical Code Magpie

This report demonstrates calculations of equilibrium isotope fractionation with thermochemical code magpie developed and maintained under the ASC-PEM-HE program at LANL. All the necessary background is provided, and the results of our calculations are compared with literature data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

R “SHINY” GUI DEVELOPMENT FOR URANIUM ISOTOPIC ANALYSIS WITH MATRIX-ASSISTED IONIZATION MASS SPECTROMETRY

The international nuclear safeguards community continues to seek rapid, accurate, and precise characterization capabilities for the in-field measurement of uranium isotopic compositions in nuclear facilities. Mass spectrometry (MS) is considered the “gold standard” for analysis of relatively long-lived actinides such as uranium (U) and plutonium; however, conventional MS analysis often requires time consuming sample preparation and complex analytical methodologies that are difficult to perform in-field or in-facility. Matrix assisted ionization (MAI) is a novel ambient ionization MS technique (i.e., MAI-MS) that potentially addresses these challenges due to the relative simplicity of the ionization phenomenon and ruggedness of ambient MS instrumentation. Savannah River National Laboratory (SRNL, USA) has demonstrated this technique for nanogram-level 235U/238U isotope ratio measurements within seconds, with percent-level analytical uncertainties capable of discriminating depleted, natural, and low-enriched uranium. Current experimental work on developing MAI methods for uranium isotopic analysis has been enabled by parallel development of a comprehensive MAI-MS data analysis suite at SRNL. Development of this bespoke data analysis software was necessary because commercially available ambient MS software is poorly suited for uranium isotope ratio measurement. The effort leverages the power of R, a popular open-source programming language, and Shiny, an R package providing tools for graphical user interface (GUI) and web interface coding. This software allows researchers without any programming experience to harness and utilize R’s considerable data analysis/visualization power.

LaBone, Elizabeth D.↗