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Assessment of the Use of Nitrogen Trifluoride for Purifying Coolant and Heat Transfer Salts in the Fluoride Salt-Cooled High-Temperature Reactor

Description: This report provides an assessment of the use of nitrogen trifluoride for removing oxide and water-caused contaminants in the fluoride salts that will be used as coolants in a molten salt cooled reactor.
Date: September 28, 2010
Creator: Scheele, Randall D. & Casella, Andrew M.
Partner: UNT Libraries Government Documents Department

Radiation Detection Computational Benchmark Scenarios

Description: Modeling forms an important component of radiation detection development, allowing for testing of new detector designs, evaluation of existing equipment against a wide variety of potential threat sources, and assessing operation performance of radiation detection systems. This can, however, result in large and complex scenarios which are time consuming to model. A variety of approaches to radiation transport modeling exist with complementary strengths and weaknesses for different problems. This variety of approaches, and the development of promising new tools (such as ORNL’s ADVANTG) which combine benefits of multiple approaches, illustrates the need for a means of evaluating or comparing different techniques for radiation detection problems. This report presents a set of 9 benchmark problems for comparing different types of radiation transport calculations, identifying appropriate tools for classes of problems, and testing and guiding the development of new methods. The benchmarks were drawn primarily from existing or previous calculations with a preference for scenarios which include experimental data, or otherwise have results with a high level of confidence, are non-sensitive, and represent problem sets of interest to NA-22. From a technical perspective, the benchmarks were chosen to span a range of difficulty and to include gamma transport, neutron transport, or both and represent different important physical processes and a range of sensitivity to angular or energy fidelity. Following benchmark identification, existing information about geometry, measurements, and previous calculations were assembled. Monte Carlo results (MCNP decks) were reviewed or created and re-run in order to attain accurate computational times and to verify agreement with experimental data, when present. Benchmark information was then conveyed to ORNL in order to guide testing and development of hybrid calculations. The results of those ADVANTG calculations were then sent to PNNL for compilation. This is a report describing the details of the selected Benchmarks and results from ...
Date: September 24, 2013
Creator: Shaver, Mark W.; Casella, Andrew M.; Wittman, Richard S. & McDonald, Ben S.
Partner: UNT Libraries Government Documents Department

Evaluation and Testing of the ADVANTG Code on SNM Detection

Description: Pacific Northwest National Laboratory (PNNL) has been tasked with evaluating the effectiveness of ORNL’s new hybrid transport code, ADVANTG, on scenarios of interest to our NA-22 sponsor, specifically of detection of diversion of special nuclear material (SNM). PNNL staff have determined that acquisition and installation of ADVANTG was relatively straightforward for a code in its phase of development, but probably not yet sufficient for mass distribution to the general user. PNNL staff also determined that with little effort, ADVANTG generated weight windows that typically worked for the problems and generated results consistent with MCNP. With slightly greater effort of choosing a finer mesh around detectors or sample reaction tally regions, the figure of merit (FOM) could be further improved in most cases. This does take some limited knowledge of deterministic transport methods. The FOM could also be increased by limiting the energy range for a tally to the energy region of greatest interest. It was then found that an MCNP run with the full energy range for the tally showed improved statistics in the region used for the ADVANTG run. The specific case of interest chosen by the sponsor is the CIPN project from Las Alamos National Laboratory (LANL), which is an active interrogation, non-destructive assay (NDA) technique to quantify the fissile content in a spent fuel assembly and is also sensitive to cases of material diversion. Unfortunately, weight windows for the CIPN problem cannot currently be properly generated with ADVANTG due to inadequate accommodations for source definition. ADVANTG requires that a fixed neutron source be defined within the problem and cannot account for neutron multiplication. As such, it is rendered useless in active interrogation scenarios. It is also interesting to note that this is a difficult problem to solve and that the automated weight windows generator in MCNP actually ...
Date: September 24, 2013
Creator: Shaver, Mark W.; Casella, Andrew M.; Wittman, Richard S. & Hayes, John W.
Partner: UNT Libraries Government Documents Department

Nitrogen Trifluoride-Based Fluoride- Volatility Separations Process: Initial Studies

Description: This document describes the results of our investigations on the potential use of nitrogen trifluoride as the fluorinating and oxidizing agent in fluoride volatility-based used nuclear fuel reprocessing. The conceptual process uses differences in reaction temperatures between nitrogen trifluoride and fuel constituents that produce volatile fluorides to achieve separations and recover valuable constituents. We provide results from our thermodynamic evaluations, thermo-analytical experiments, kinetic models, and provide a preliminary process flowsheet. The evaluations found that nitrogen trifluoride can effectively produce volatile fluorides at different temperatures dependent on the fuel constituent.
Date: September 28, 2011
Creator: McNamara, Bruce K.; Scheele, Randall D.; Casella, Andrew M. & Kozelisky, Anne E.
Partner: UNT Libraries Government Documents Department

Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY12 Status Report

Description: Executive Summary Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today’s confirmatory methods. This document is a progress report for FY2012 PNNL analysis and algorithm development. Progress made by PNNL in FY2012 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel assemblies. PNNL further refined the semi-empirical model developed in FY2011 based on singular value decomposition (SVD) to numerically account for the effects of self-shielding. The average uncertainty in the Pu mass across the NGSI-64 fuel assemblies was shown to be less than 3% using only six calibration assemblies with a 2% uncertainty in the isotopic masses. When calibrated against the six NGSI-64 fuel assemblies, the algorithm was able to determine the total Pu mass within <2% uncertainty for the 27 diversion cases also developed under NGSI. Two purely empirical algorithms were developed that do not require the use of Pu isotopic fission chambers. The semi-empirical and purely empirical algorithms were successfully tested using MCNPX simulations as well applied to experimental data measured by RPI using their LSDS. The algorithms were able to describe the 235U masses of the RPI measurements with an average uncertainty of 2.3%. Analyses were conducted that provided valuable insight with ...
Date: September 28, 2012
Creator: Kulisek, Jonathan A.; Anderson, Kevin K.; Casella, Andrew M.; Siciliano, Edward R. & Warren, Glen A.
Partner: UNT Libraries Government Documents Department

Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

Description: Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&amp;D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today's confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of ...
Date: September 30, 2011
Creator: Kulisek, Jonathan A.; Anderson, Kevin K.; Bowyer, Sonya M.; Casella, Andrew M.; Gesh, Christopher J. & Warren, Glen A.
Partner: UNT Libraries Government Documents Department

Experimental Results for SimFuels

Description: Assessing the performance of Spent (or Used) Nuclear Fuel (UNF) in geological repository requires quantification of time-dependent phenomena that may influence its behavior on a time-scale up to millions of years. A high-level waste repository environment will be a dynamic redox system because of the time-dependent generation of radiolytic oxidants and reductants and the corrosion of Fe-bearing canister materials. One major difference between used fuel and natural analogues, including unirradiated UO2, is the intense radiolytic field. The radiation emitted by used fuel can produce radiolysis products in the presence of water vapor or a thin-film of water that may increase the waste form degradation rate and change radionuclide behavior. To study UNF, we have been working on producing synthetic UO2 ceramics, or SimFuels that can be used in testing and which will contain specific radionuclides or non-radioactive analogs so that we can test the impact of radiolysis on fuel corrosion without using actual spent fuel. Although, testing actual UNF would be ideal for understanding the long term behavior of UNF, it requires the use of hot cells and is extremely expensive. In this report, we discuss, factors influencing the preparation of SimFuels and the requirements for dopants to mimic the behavior of UNF. We have developed a reliable procedure for producing large grain UO2 at moderate temperatures. This process will be applied to a series of different formulations.
Date: August 22, 2012
Creator: Buck, Edgar C.; Casella, Andrew M.; Skomurski, Frances N.; MacFarlan, Paul J.; Soderquist, Chuck Z.; Wittman, Richard S. et al.
Partner: UNT Libraries Government Documents Department

Deposition Velocities of Newtonian and Non-Newtonian Slurries in Pipelines

Description: The WTP pipe plugging issue, as stated by the External Flowsheet Review Team (EFRT) Executive Summary, is as follows: “Piping that transports slurries will plug unless it is properly designed to minimize this risk. This design approach has not been followed consistently, which will lead to frequent shutdowns due to line plugging.” A strategy was employed to perform critical-velocity tests on several physical simulants. Critical velocity is defined as the point where a stationary bed of particles deposits on the bottom of a straight horizontal pipe during slurry transport operations. Results from the critical velocity testing provide an indication of slurry stability as a function of fluid rheological properties and transport conditions. The experimental results are compared to the WTP design guide on slurry transport velocity in an effort to confirm minimum waste velocity and flushing velocity requirements as established by calculations and critical line velocity correlations in the design guide. The major findings of this testing is discussed below. Experimental results indicate that the use of the Oroskar and Turian (1980) correlation in the design guide is conservative—Slurry viscosity has a greater affect on particles with a large surface area to mass ratio. The increased viscous forces on these particles result in a decrease in predicted critical velocities from this traditional industry derived equations that focus on particles large than 100 m in size. Since the Hanford slurry particles generally have large surface area to mass ratios, the reliance on such equations in the Hall (2006) design guide is conservative. Additionally, the use of the 95% percentile particle size as an input to this equation is conservative. However, test results indicate that the use of an average particle density as an input to the equation is not conservative. Particle density has a large influence on the overall result returned ...
Date: March 25, 2009
Creator: Poloski, Adam P.; Adkins, Harold E.; Abrefah, John; Casella, Andrew M.; Hohimer, Ryan E.; Nigl, Franz et al.
Partner: UNT Libraries Government Documents Department

A Qualitative Investigation of Deposition Velocities of a Non-Newtonian Slurry in Complex Pipeline Geometries

Description: The External Flowsheet Review Team (EFRT) has identified the issues relating to the Waste Treatment and Immobilization Plant (WTP) pipe plugging. Per the review’s executive summary, “Piping that transports slurries will plug unless it is properly designed to minimize this risk. This design approach has not been followed consistently, which will lead to frequent shutdowns due to line plugging.” To evaluate the potential for plugging, testing was performed to determine critical velocities for the complex WTP piping layout. Critical velocity is defined as the point at which a moving bed of particles begins to form on the pipe bottom during slurry-transport operations. Pressure drops across the fittings of the test pipeline were measured with differential pressure transducers, from which the critical velocities were determined. A WTP prototype flush system was installed and tested upon the completion of the pressure-drop measurements. We also provide the data for the overflow relief system represented by a WTP complex piping geometry with a non-Newtonian slurry. A waste simulant composed of alumina (nominally 50 μm in diameter) suspended in a kaolin clay slurry was used for this testing. The target composition of the simulant was 10 vol% alumina in a suspending medium with a yield stress of 3 Pa. No publications or reports are available to confirm the critical velocities for the complex geometry evaluated in this testing; therefore, for this assessment, the results were compared to those reported by Poloski et al. (2008) for which testing was performed for a straight horizontal pipe. The results of the flush test are compared to the WTP design guide 24590-WTP-GPG-M-0058, Rev. 0 (Hall 2006) in an effort to confirm flushing-velocity requirements.
Date: May 11, 2009
Creator: Yokuda, Satoru T.; Poloski, Adam P.; Adkins, Harold E.; Casella, Andrew M.; Hohimer, Ryan E.; Karri, Naveen K. et al.
Partner: UNT Libraries Government Documents Department

Lead Slowing Down Spectrometer Status Report

Description: This report documents the progress that has been completed in the first half of FY2012 in the MPACT-funded Lead Slowing Down Spectrometer project. Significant progress has been made on the algorithm development. We have an improve understanding of the experimental responses in LSDS for fuel-related material. The calibration of the ultra-depleted uranium foils was completed, but the results are inconsistent from measurement to measurement. Future work includes developing a conceptual model of an LSDS system to assay plutonium in used fuel, improving agreement between simulations and measurement, design of a thorium fission chamber, and evaluation of additional detector techniques.
Date: June 7, 2012
Creator: Warren, Glen A.; Anderson, Kevin K.; Bonebrake, Eric; Casella, Andrew M.; Danon, Yaron; Devlin, M. et al.
Partner: UNT Libraries Government Documents Department

Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY12 Status Report

Description: Executive Summary The Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign is supporting a multi-institutional collaboration to study the feasibility of using Lead Slowing Down Spectroscopy (LSDS) to conduct direct, independent and accurate assay of fissile isotopes in used fuel assemblies. The collaboration consists of Pacific Northwest National Laboratory (PNNL), Los Alamos National Laboratory (LANL), Rensselaer Polytechnic Institute (RPI), Idaho State University (ISU). There are three main challenges to implementing LSDS to assay used fuel assemblies. These challenges are the development of an algorithm for interpreting the data with an acceptable accuracy for the fissile masses, the development of suitable detectors for the technique, and the experimental benchmarking of the approach. This report is a summary of the progress in these areas made by the collaboration during FY2012. Significant progress was made on the project in FY2012. Extensive characterization of a “semi-empirical” algorithm was conducted. For example, we studied the impact on the accuracy of this algorithm by the minimization of the calibration set, uncertainties in the calibration masses, and by the choice of time window. Issues such a lead size, number of required neutrons, placement of the neutron source and the impact of cadmium around the detectors were also studied. In addition, new algorithms were developed that do not require the use of plutonium fission chambers. These algorithms were applied to measurement data taken by RPI and shown to determine the 235U mass within 4%. For detectors, a new concept for a fast neutron detector involving 4He recoil from neutron scattering was investigated. The detector has the potential to provide a couple of orders of magnitude more sensitivity than 238U fission chambers. Progress was also made on the more conventional approach of using 232Th fission chambers as fast neutron detectors. For benchmarking measurements, ...
Date: October 1, 2012
Creator: Warren, Glen A.; Anderson, Kevin K.; Casella, Andrew M.; Danon, Yaron; Devlin, M.; Gavron, A. et al.
Partner: UNT Libraries Government Documents Department

Deposition Velocities of Non-Newtonian Slurries in Pipelines: Complex Simulant Testing

Description: One of the concerns expressed by the External Flowsheet Review Team (EFRT) is about the potential for pipe plugging at the Waste Treatment and Immobilization Plant (WTP). Per the review’s executive summary, “Piping that transports slurries will plug unless it is properly designed to minimize this risk. This design approach has not been followed consistently, which will lead to frequent shutdowns due to line plugging.” To evaluate the potential for plugging, deposition-velocity tests were performed on several physical simulants to determine whether the design approach is conservative. Deposition velocity is defined as the velocity below which particles begin to deposit to form a moving bed of particles on the bottom of a straight horizontal pipe during slurry-transport operations. The deposition velocity depends on the system geometry and the physical properties of the particles and fluid. An experimental program was implemented to test the stability-map concepts presented in WTP-RPT-175 Rev. 01. Two types of simulant were tested. The first type of simulant was similar to the glass-bead simulants discussed in WTP-RPT-175 Rev. 0 ; it consists of glass beads with a nominal particle size of 150 µm in a kaolin/water slurry. The initial simulant was prepared at a target yield stress of approximately 30 Pa. The yield stress was then reduced, stepwise, via dilution or rheological modifiers, ultimately to a level of <1 Pa. At each yield-stress step, deposition-velocity testing was performed. Testing over this range of yield-stress bounds the expected rheological operating window of the WTP and allows the results to be compared to stability-map predictions for this system. The second simulant was a precipitated hydroxide that simulates HLW pretreated sludge from Hanford waste tank AZ-101. Testing was performed in a manner similar to that for the first simulant over a wide range of yield stresses; however, an additional test ...
Date: July 1, 2009
Creator: Poloski, Adam P.; Bonebrake, Michael L.; Casella, Andrew M.; Johnson, Michael D.; Toth, James J.; Adkins, Harold E. et al.
Partner: UNT Libraries Government Documents Department

Characterization, Leaching, and Filtration Testing for Tributyl Phosphate (TBP, Group 7) Actual Waste Sample Composites

Description: .A testing program evaluating actual tank waste was developed in response to Task 4 from the M-12 External Flowsheet Review Team (EFRT) issue response plan. The bulk water-insoluble solid wastes that are anticipated to be delivered to the Waste Treatment and Immobilization Plant (WTP) were identified according to type such that the actual waste testing could be targeted to the relevant categories. Eight broad waste groupings were defined. Samples available from the 222S archive were identified and obtained for testing. The actual waste-testing program included homogenizing the samples by group, characterizing the solids and aqueous phases, and performing parametric leaching tests. The tributyl phosphate sludge (TBP, Group 7) is the subject of this report. The Group 7 waste was anticipated to be high in phosphorus as well as aluminum in the form of gibbsite. Both are believed to exist in sufficient quantities in the Group 7 waste to address leaching behavior. Thus, the focus of the Group 7 testing was on the removal of both P and Al. The waste-type definition, archived sample conditions, homogenization activities, characterization (physical, chemical, radioisotope, and crystal habit), and caustic leaching behavior as functions of time, temperature, and hydroxide concentration are discussed in this report. Testing was conducted according to TP-RPP-WTP-467.
Date: March 9, 2009
Creator: Edwards, Matthew K.; Billing, Justin M.; Blanchard, David L.; Buck, Edgar C.; Casella, Amanda J.; Casella, Andrew M. et al.
Partner: UNT Libraries Government Documents Department

Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY11 Status Report

Description: Executive Summary Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today’s confirmatory assay methods. This document is a progress report for FY2011 collaboration activities. Progress made by the collaboration in FY2011 continues to indicate the promise of LSDS techniques applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model demonstrated the potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space. Similar results were obtained using a perturbation approach developed by LANL. Benchmark measurements have been successfully conducted at LANL and at RPI using their respective LSDS instruments. The ISU and UNLV collaborative effort is focused on the fabrication and testing of prototype fission chambers lined with ultra-depleted 238U and 232Th, and uranium deposition on a stainless steel disc using spiked U3O8 from room temperature ionic liquid was successful, with improving thickness obtained. In FY2012, the collaboration plans a broad array of activities. PNNL will focus on optimizing its empirical model and minimizing its reliance on calibration data, as well continuing efforts on developing an analytical model. Additional measurements are planned at LANL ...
Date: August 1, 2011
Creator: Warren, Glen A.; Casella, Andrew M.; Haight, R. C.; Anderson, Kevin K.; Danon, Yaron; Hatchett, D. et al.
Partner: UNT Libraries Government Documents Department