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Pool, Karl N.

Publications and source records attributed to Pool, Karl N..

Thermal properties of U-Mo alloys irradiated under high fission power density

A variety of physical and thermal property measurements made on irradiated U-Mo alloy monolithic fuel samples with a Zr diffusion barrier and clad in Al alloy 6061 are reported. These properties form the basis for additional investigations in thermal behavior of U-Mo fuel under high performance research reactor irradiation conditions. Measurements were performed on samples harvested from fuel plates irradiated under high fission power density and surface heat flux and complement previous measurements on samples subjected to moderate fission power density and surface heat flux. Specific heat capacity of irradiated monolithic U-Mo increases with increasing temperature and fission density, but carries large uncertainties associated with thickness measurements used to determine the mass fraction of the layer constituents for extraction of the U-Mo specific heat capacity, specifically the very thin and nonuniform Zr diffusion barrier. Density of irradiated monolithic U-Mo decreases with increasing fission density resulting from fission gas swelling and porosity formation. Thermal diffusivity of irradiated monolithic U-Mo increased with increasing temperature and decreased with increasing fission density. Thermal conductivity of irradiated monolithic U-Mo increased with increasing temperature, and in general, appeared to decrease and become less sensitive to temperature with increasing fission density. Thermal conductivity measurements compared to a semi-empirical model agreed within ±30%. It is suspected that the main driver in deviation between model calculations and measurements is the fission gas swelling determination, which does not account for fission power density or irradiation temperature.

uranium (U), molybdenum, nuclear fuel, thermal con↗

Compilation of PRF Canyon Floor Pan Sample Analysis Results

On September 28, 2015, debris collected from the PRF (236-Z) canyon floor, Pan J, was observed to exhibit chemical reaction. The material had been transferred from the floor pan to a collection tray inside the canyon the previous Friday. Work in the canyon was stopped to allow Industrial Hygiene to perform monitoring of the material reaction. Canyon floor debris that had been sealed out was sequestered at the facility, a recovery plan was developed, and drum inspections were initiated to verify no additional reactions had occurred. On October 13, in-process drums containing other Pan J material were inspected and showed some indication of chemical reaction, limited to discoloration and degradation of inner plastic bags. All Pan J material was sealed back into the canyon and returned to collection trays. Based on the high airborne levels in the canyon during physical debris removal, ETGS (Encapsulation Technology Glycerin Solution) was used as a fogging/lock-down agent. On October 15, subject matter experts confirmed a reaction had occurred between nitrates (both Plutonium Nitrate and Aluminum Nitrate Nonahydrate (ANN) are present) in the Pan J material and the ETGS fixative used to lower airborne radioactivity levels during debris removal. Management stopped the use of fogging/lock-down agents containing glycerin on bulk materials, declared a Management Concern, and initiated the Potential Inadequacy in the Safety Analysis determination process. Additional drum inspections and laboratory analysis of both reacted and unreacted material are planned. This report compiles the results of many different sample analyses conducted by the Pacific Northwest National Laboratory on samples collected from the Plutonium Reclamation Facility (PRF) floor pans by the CH2MHill’s Plateau Remediation Company (CHPRC). Revision 1 added Appendix G that reports the results of the Gas Generation Rate and methodology. The scope of analyses requested by CHPRC includes the determination of common anions, gamma spectrometry, metals, corrosivity, organics and alpha spectrometry (note: alpha spectrometry was cancelled during the performance of this work with concurrence from CHPRC). Results may help elucidate the components that led to the unexpected reaction in the canyon as well as inform the radiological and hazardous characteristics. The specific anions, gamma emitters, organics and metals requested by CHPRC are provided in the analytical reports sections. The individual analyses were conducted under the Plutonium Finishing Plant (PFP) Floor Pan Evaluation Project Quality Assurance Project Plan (PFP Floor Pan Evaluation QAPP, Revision 0.) developed by PNNL specifically for this project. The final reports for each analysis set are included in this compilation of the results. Each package was reviewed under the PFP Floor Pan Evaluation Project Quality Assurance Project Plan so no additional reviews were conducted in this compilation task. The Gas Generation Rates in Appendix G were conducted under the PNNL “How Do I…” quality assurance program and were NOT conducted under the Plutonium Finishing Plant (PFP) Floor Pan Evaluation Project Quality Assurance Project Plan (PFP Floor Pan Evaluation QAPP, Revision 0.).

36 MATERIALS SCIENCE↗

K West Basin Sand Filter Backwash Sample Analysis

A sand filter is used to help maintain water clarity at the K West Basin where highly radioactive sludge is stored. Eventually that sand filter will require disposal. The radionuclide content of the solids trapped in the sand filter will affect the selection of the sand filter disposal pathway. The Pacific Northwest National Laboratory (PNNL) was contracted by the K Basin Operations & Plateau Remediation Project (operations contractor CH2M Hill) to analyze the radionuclide content of the solids collected from the backwash of the K West Basin sand filter. The radionuclide composition in the sand filter backwash solids will be used by CH2M Hill to determine if the sand filter media and retained sludge solids will be designated as transuranic waste for disposal purposes or can be processed through less expensive means. On October 19, 2015, K Basin Operations & Plateau Remediation Project staff backwashed the sand filter into the North Load-Out Pit (NLOP) and immediately collected sample slurry from a sampling tube positioned 24 in. above the NLOP floor. The 764 g sand filter backwash slurry sample, KW-105 SFBW-001, was submitted to PNNL for analysis on October 20, 2015. Solids from the slurry sample were consolidated into two samples (i.e., a primary and a duplicate sample) by centrifuging and measured for mass (0.82 g combined – wet centrifuged solids basis) and volume (0.80 mL combined). The solids were a dark brown/orange color, consistent with iron oxide/hydroxide. The solids were dried; the combined dry solids mass was 0.1113 g, corresponding to 0.0146 weight percent (wt%) solids in the original submitted sample slurry. The solids were acid-digested using nitric and hydrochloric acids. Insoluble solids developed upon dilution with 0.5 M HNO 3 , corresponding to an average 6.5 wt% of the initial dry solids content. The acid digestate and insoluble solids were analyzed separately by gamma spectrometry. Nominally, 7.7% of the 60 Co was present in the insoluble solids; less than 1% of other gamma-emitters (i.e., 137 Cs, 154/155 Eu, and 241 Am) were present in the insoluble solids. Aliquots of the acid digestate were analyzed directly using gamma energy analysis (GEA) and after separations for 238 Pu, 239+240 Pu, 237 Np, and 241 Am radioisotopes using alpha energy analysis (AEA). The 90 Sr was measured by liquid scintillation counting (LSC) on the Sr-separated fraction. The plutonium isotopic distribution of the acid digestate was analyzed following Pu separations by thermal ionization mass spectrometry (TIMS). A table summarizes the results for the primary and duplicate samples. The 239+240 Pu concentration (µCi/g dry) relative to 90 Sr and to 137 Cs concentrations (µCi/g dry) was examined. The K West Basin sludge has a 239+240 Pu/ 90 Sr ranging from 0.1 to 1.2 and the 239+240 Pu/ 137 Cs ratio ranging from 0.10 to 0.47. In contrast, the sand filter backwash solids 239+240 Pu/ 90 Sr ratio was 10.6 and the 239+240 Pu/ 137 Cs ratio was 2.0. The ratio differences indicate a relative enhancement of the Pu concentration in the sand filter solids relative to the 137 Cs and 90 Sr sludge concentrations currently in the K West Basin. A dose-to-curie radioisotope evaluation of the sand filter waste form may need to consider this dissimilarity.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Fuel Thermo-physical Characterization Project. Fiscal Year 2014 Final Report

The Office of Material Management and Minimization (M3) Reactor Conversion Fuel Thermo-Physical Characterization Project at Pacific Northwest National Laboratory (PNNL) was tasked with using PNNL facilities and processes to receive irradiated low enriched uranium–molybdenum (LEU-Mo) fuel plate samples and perform analysis in support of the M3 Reactor Conversion Program. This work is in support of the M3 Reactor Conversion Fuel Development Pillar that is managed by Idaho National Laboratory. The primary research scope was to determine the thermo-physical properties as a function of temperature and burnup. Work conducted in Fiscal Year (FY) 2014 complemented measurements performed in FY 2013 on four additional irradiated LEU-Mo fuel plate samples. Specifically, the work in FY 2014 investigated the influence of different processing methods on thermal property behavior, the absence of aluminum alloy cladding on thermal property behavior for additional model validation, and the influence of higher operating surface heat flux / more aggressive irradiation conditions on thermal property behavior. The model developed in FY 2013 and refined in FY 2014 to extract thermal properties of the U-Mo alloy from the measurements conducted on an integral fuel plate sample (i.e., U-Mo alloy with a thin Zr coating and clad in AA6061) continues to perform very well. Measurements conducted in FY 2014 on samples irradiated under similar conditions compare well to measurements performed in FY 2013. In general, there is no gross influence of fabrication method on thermal property behavior, although the difference in LEU-Mo foil microstructure does have a noticeable influence on recrystallization of grains during irradiation. Samples irradiated under more aggressive irradiation conditions, e.g., higher surface heat flux, revealed lower thermal conductivity when compared to samples irradiated at moderate surface heat fluxes, with the exception of one sample. This report documents thermal property measurements conducted in FY 2014 and compares results to values obtained from literature and measurements performed in FY 2013, where applicable, along with appropriate discussion.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

LEU-Mo Fuel Out-of-Pile Characterization for TUM (Final Report)

The Technische Universität München (TUM) located in Germany requested that Pacific Northwest National Laboratory (PNNL) perform thermal-physical property measurement services for determining the thermal conductivities of irradiated U-Mo dispersion fuel samples. Two dispersion fuel segments containing U-7Mo dispersion fuel in an Al-2wt% Si matrix harvested from the AFIP-1 irradiation experiment were provided to PNNL for this effort. The segments were sectioned into samples for pycnometry (density) and laser flash analysis (thermal diffusivity), differential scanning calorimetry (specific heat capacity), and optical metallography (thickness, image analysis). This report summarizes the findings of the analysis performed at TUM’s request.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development and validation of capabilities to measure thermal properties of layered monolithic U-Mo alloy plate-type fuel

The uranium-molybdenum (U-Mo) alloy in a monolithic form has been proposed as one fuel design capable of converting some of the world’s highest power research reactors from the use of high enriched uranium (HEU) to low enriched uranium (LEU). One aspect of the fuel development and qualification process is to demonstrate appropriate understanding of thermal conductivity behavior of the fuel system as a function of temperature and expected irradiation conditions. The purpose of this paper is to verify and validate the functionality of equipment methods installed in hot cells for eventual measurements on irradiated uranium-molybdenum (U-Mo) monolithic fuel specimens, procedures to operate the equipment, and models to extract the desired thermal properties. The results presented here demonstrate the adequacy of the equipment, procedures and models that have been developed for this purpose based on measurements conducted on surrogate depleted uranium-molybdenum (DU-Mo) alloy samples containing a zirconium diffusion barrier and clad in aluminum alloy 6061 (AA6061). The results are in excellent agreement with thermal property data reported in the literature for similar U-Mo alloys as a function of temperature.

multi-layer↗

Determination of Uranium Metal Concentration in Irradiated Fuel Storage Basin Sludge Using Selective Dissolution

Uranium metal corroding in water-saturated sludges now held in the US Department of Energy Hanford Site K West irradiated fuel storage basin can create hazardous hydrogen atmospheres during handling, immobilization, or subsequent transport and storage. Knowledge of uranium metal concentration in sludge thus is essential to safe sludge management and process design, requiring an expeditious routine analytical method to detect uranium metal concentrations as low as 0.03 wt% in sludge even in the presence of 30 wt% or higher total uranium concentrations.

Nuclear fuel storage basin sludge↗

Characterization Data Package for Containerized Sludge Samples Collected from Engineered Container SCS-CON-210

This data package contains the K Basin sludge characterization results obtained by Pacific Northwest National Laboratory during processing and analysis of four sludge core samples collected from Engineered Container SCS-CON-210 in 2010 as requested by CH2M Hill Plateau Remediation Company. Sample processing requirements, analytes of interest, detection limits, and quality control sample requirements are defined in the KBC-33786, Rev. 2. The core processing scope included reconstitution of a sludge core sample distributed among four to six 4-L polypropylene bottles into a single container. The reconstituted core sample was then mixed and subsampled to support a variety of characterization activities. Additional core sludge subsamples were combined to prepare a container composite. The container composite was fractionated by wet sieving through a 2,000 micron mesh and a 500-micron mesh sieve. Each sieve fraction was sampled to support a suite of analyses. The core composite analysis scope included density determination, radioisotope analysis, and metals analysis, including the Waste Isolation Pilot Plant Hazardous Waste Facility Permit metals (with the exception of mercury). The container composite analysis included most of the core composite analysis scope plus particle size distribution, particle density, rheology, and crystalline phase identification. A summary of the received samples, core sample reconstitution and subsampling activities, container composite preparation and subsampling activities, physical properties, and analytical results are presented. Supporting data and documentation are provided in the appendices. There were no cases of sample or data loss and all of the available samples and data are reported as required by the Quality Assurance Project Plan/Sampling and Analysis Plan.

core sampling↗