Hybrid Enrichment Assay Methods for a UF6 Cylinder Verification Station: FY10 Progress Report

Pacific Northwest National Laboratory (PNNL) is developing the concept of an automated UF6 cylinder verification station that would be located at key measurement points to positively identify each cylinder, measure its mass and enrichment, store the collected data in a secure database, and maintain continuity of knowledge on measured cylinders until the arrival of International Atomic Energy Agency (IAEA) inspectors. At the center of this unattended system is a hybrid enrichment assay technique that combines the traditional enrichment-meter method (based on the 186 keV peak from 235U) with non-traditional neutron-induced high-energy gamma-ray signatures (spawned primarily by 234U alpha emissions and 19F(alpha, neutron) reactions). Previous work by PNNL provided proof-of-principle for the non-traditional signatures to support accurate, full-volume interrogation of the cylinder enrichment, thereby reducing the systematic uncertainties in enrichment assay due to UF6 heterogeneity and providing greater sensitivity to material substitution scenarios. The work described here builds on that preliminary evaluation of the non-traditional signatures, but focuses on a prototype field system utilizing NaI(Tl) and LaBr3(Ce) spectrometers, and enrichment analysis algorithms that integrate the traditional and non-traditional signatures. Results for the assay of Type-30B cylinders ranging from 0.2 to 4.95 wt% 235U, at an AREVA fuel fabrication plant in Richland, WA, are described for the following enrichment analysis methods: 1) traditional enrichment meter signature (186 keV peak) as calculated using a square-wave convolute (SWC) algorithm; 2) non-traditional high-energy gamma-ray signature that provides neutron detection without neutron detectors and 3) hybrid algorithm that merges the traditional and non-traditional signatures. Uncertainties for each method, relative to the declared enrichment for each cylinder, are calculated and compared to the uncertainties from an attended HPGe verification station at AREVA, and the IAEA’s uncertainty target values for feed, tail and product cylinders. A summary of the major findings from the field measurements and subsequent analysis follows: • Traditional enrichment-meter assay using specially collimated NaI spectrometers and a Square-Wave-Convolute algorithm can achieve uncertainties comparable to HPGe and LaBr for product, natural and depleted cylinders. • Non-traditional signatures measured using NaI spectrometers enable interrogation of the entire cylinder volume and accurate measurement of absolute 235U mass in product, natural and depleted cylinders. • A hybrid enrichment assay method can achieve lower uncertainties than either the traditional or non-traditional methods acting independently because there is a low degree of correlation in the systematic errors of the two individual methods (wall thickness variation and 234U/235U variation, respectively). This work has indicated that the hybrid NDA method has the potential to serve as the foundation for an unattended cylinder verification station. When compared to today’s handheld cylinder-verification approach, such a station would have the following advantages: 1) improved enrichment assay accuracy for product, tail and feed cylinders; 2) full-volume assay of absolute 235U mass; 3) assay of minor isotopes (234U and 232U) important to verification of feedstock origin; single instrumentation design for both Type 30B and Type 48 cylinders; and 4) substantial reduction in the inspector manpower associated with cylinder verification.