David C. Gerlach

Trawsfynydd Plutonium Estimate

Report serves to document an estimate of the cumulative plutonium production of the Trawsfynydd Unit II reactor (Traws II) over its operating life made using the Graphite Isotope Ratio Method (GIRM). The estimate of the plutonium production in Traws II provided in this report has been generated under blind conditions. In other words, the estimate ofthe Traws II plutonium production has been generated without the knowledge of the plutonium production declared by the reactor operator (Nuclear Electric). The objective of this report is to demonstrate that the GIRM can be employed to serve as an accurate tool to verify weapons materials production declarations.

Determination of Light Water Reactor Fuel Burnup with the Isotope Ratio Method

For the current project to demonstrate that isotope ratio measurements can be extended to zirconium alloys used in LWR fuel assemblies we report new analyses on irradiated samples obtained from a reactor. Zirconium alloys are used for structural elements of fuel assemblies and for the fuel element cladding. This report covers new measurements done on irradiated and unirradiated zirconium alloys, Unirradiated zircaloy samples serve as reference samples and indicate starting values or natural values for the Ti isotope ratio measured. New measurements of irradiated samples include results for 3 samples provided by AREVA. New results indicate: 1. Titanium isotope ratios were measured again in unirradiated samples to obtain reference or starting values at the same time irradiated samples were analyzed. In particular, 49Ti/48Ti ratios were indistinguishably close to values determined several months earlier and to expected natural values. 2. 49Ti/48Ti ratios were measured in 3 irradiated samples thus far, and demonstrate marked departures from natural or initial ratios, well beyond analytical uncertainty, and the ratios vary with reported fluence values. The irradiated samples appear to have significant surface contamination or radiation damage which required more time for SIMS analyses. 3. Other activated impurity elements still limit the sample size for SIMS analysis of irradiated samples. The sub-samples chosen for SIMS analysis, although smaller than optimal, were still analyzed successfully without violating the conditions of the applicable Radiological Work Permit

Radiochemistry of the 3M SBMF-40VF filter media used by the DOE CTBT Radionuclide Aerosol Sampler/Analyzer (RASA)

The Comprehensive Test Ban Treaty calls for the monitoring of aerosol radionuclides throughout the globe. Pacific Northwest National Laboratory has developed the Radionuclide Aerosol Sampler/Analyzer (RASA) for the Department of Energy to automatically collect and measure radioactive aerosols from the atmosphere. The RASA passes high volumes of air through a 3MTM Substrate Blown Microfiber Media (SBMF) specifically designated as SBMF-40VF. It then automatically moves the filter media in front of a high-purity germanium detector and collects a gamma spectrum. If further analysis on the filter is desired, the filter is sent to a laboratory and radiochemical analysis is performed. This paper discusses the method of dissolution of the SBMF-40VF filter media and the separation of the radioisotopes of interest.

Uranium Oxide Aerosol Transport in Porous Graphite

The objective of this paper is to investigate the transport of uranium oxide particles that may be present in carbon dioxide (CO2) gas coolant, into the graphite blocks of gas-cooled, graphite moderated reactors. The transport of uranium oxide in the coolant system, and subsequent deposition of this material in the graphite, of such reactors is of interest because it has the potential to influence the application of the Graphite Isotope Ratio Method (GIRM). The GIRM is a technology that has been developed to validate the declared operation of graphite moderated reactors. GIRM exploits isotopic ratio changes that occur in the impurity elements present in the graphite to infer cumulative exposure and hence the reactor’s lifetime cumulative plutonium production. Reference Gesh, et. al., for a more complete discussion on the GIRM technology.

GUM Analysis for SIMS Isotopic Ratios in BEP0 Graphite Qualification Samples, Round 2

This report describes GUM calculations for TIMS and SIMS isotopic ratio measurements of reactor graphite samples. These isotopic ratios are used to estimate reactor burn-up, and currently consist of various ratios of U, Pu, and Boron impurities in the graphite samples. The GUM calculation is a propagation of error methodology that assigns uncertainties (in the form of standard error and confidence bound) to the final estimates.

Final Report on Isotope Ratio Techniques for Light Water Reactors

The Isotope Ratio Method (IRM) is a technique for estimating the energy or plutonium production in a fission reactor by measuring isotope ratios in non-fuel reactor components. The isotope ratios in these components can then be directly related to the cumulative energy production with standard reactor modeling methods.

Measurement Protocols for Optimized Fuel Assembly Tags

This report describes the measurement protocols for optimized tags that can be applied to standard fuel assemblies used in light water reactors. This report describes work performed by the authors at Pacific Northwest National Laboratory for NA-22 as part of research to identify specific signatures that can be developed to support counter-proliferation technologies.

Selected Isotopes for Optimized Fuel Assembly Tags

In support of our ongoing signatures project we present information on 3 isotopes selected for possible application in optimized tags that could be applied to fuel assemblies to provide an objective measure of burnup. 1. Important factors for an optimized tag are compatibility with the reactor environment (corrosion resistance), low radioactive activation, at least 2 stable isotopes, moderate neutron absorption cross-section, which gives significant changes in isotope ratios over typical fuel assembly irradiation levels, and ease of measurement in the SIMS machine 2. From the candidate isotopes presented in the 3rd FY 08 Quarterly Report, the most promising appear to be Titanium, Hafnium, and Platinum. The other candidate isotopes (Iron, Tungsten, exhibited inadequate corrosion resistance and/or had neutron capture cross-sections either too high or too low for the burnup range of interest.

GUM Analysis for TIMS and SIMS Isotopic Ratios in Graphite

This report describes GUM calculations for TIMS and SIMS isotopic ratio measurements of reactor graphite samples. These isotopic ratios are used to estimate reactor burn-up, and currently consist of various ratios of U, Pu, and Boron impurities in the graphite samples. The GUM calculation is a propagation of error methodology that assigns uncertainties (in the form of standard error and confidence bound) to the final estimates.