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DOE OSTI2014

A Multi-Contact, Low Capacitance HPGe Detector for High Rate Gamma Spectroscopy

The detection, identification and non-destructive assay of special nuclear materials and nuclear fission by-products are critically important activities in support of nuclear non-proliferation programs. Both national and international nuclear safeguard agencies recognize that current accounting methods for spent nuclear fuel are inadequate from a safeguards perspective. Radiation detection and analysis by gamma-ray spectroscopy is a key tool in this field, but no instrument exists that can deliver the required performance (energy resolution and detection sensitivity) in the presence of very high background count rates encountered in the nuclear safeguards arena. The work of this project addresses this critical need by developing a unique gamma-ray detector based on high purity germanium that has the previously unachievable property of operating in the 1 million counts-per-second range while achieving state-of-the-art energy resolution necessary to identify and analyze the isotopes of interest. The technical approach was to design and fabricate a germanium detector with multiple segmented electrodes coupled to multi-channel high rate spectroscopy electronics. Dividing the germanium detector’s signal electrode into smaller sections offers two advantages; firstly, the energy resolution of the detector is potentially improved, and secondly, the detector is able to operate at higher count rates. The design challenges included the following; determining the optimum electrode configuration to meet the stringent energy resolution and count rate requirements; determining the electronic noise (and therefore energy resolution) of the completed system after multiple signals are recombined; designing the germanium crystal housing and vacuum cryostat; and customizing electronics to perform the signal recombination function in real time. In this phase I work, commercial off-the-shelf electrostatic modeling software was used to develop the segmented germanium crystal geometry, which underwent several iterations before an optimal electrode configuration was found. The model was tested and validated against real-world measurements with existing germanium detectors. Extensive modeling of electronic noise was conducted using established formulae, and real-world measurements were performed on candidate front-end electronic components. This initial work proved the feasibility of the design with respect to expected high count rate and energy resolution performance. Phase I also delivered the mechanical design of the detector housing and vacuum cryostat to be built in Phase II. Finally, a Monte Carlo simulation was created to show the response of the complete design to a Cs-137 source. This development presents a significant advance for nuclear safeguards instrumentation with increased speed and accuracy of detection and identification of special nuclear materials. Other significant applications are foreseen for a gamma-ray detector that delivers high energy resolution (1keV FWHM noise) at high count rate (1 Mcps), especially in the areas of physics research and materials analysis.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

Delayed Gamma-Ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

High-energy, beta-delayed gamma-ray spectroscopy is a potential, non-destructive assay techniques for the independent verification of declared quantities of special nuclear materials at key stages of the fuel cycle and for directly assaying nuclear material inventories for spent fuel handling, interim storage, reprocessing facilities, repository sites, and final disposal. Other potential applications include determination of MOX fuel composition, characterization of nuclear waste packages, and challenges in homeland security and arms control verification. Experimental measurements were performed to evaluate fission fragment yields, to test methods for determining isotopic fractions, and to benchmark the modeling code package. Experimental measurement campaigns were carried out at the IAC using a photo-neutron source and at OSU using a thermal neutron beam from the TRIGA reactor to characterize the emission of high-energy delayed gamma rays from 235 U, 239 Pu, and 241 Pu targets following neutron induced fission. Data were collected for pure and combined targets for several irradiation/spectroscopy cycle times ranging from 10/10 seconds to 15/30 minutes.The delayed gamma-ray signature of 241 Pu, a significant fissile constituent in spent fuel, was measured and compared to 239 Pu. The 241 Pu/ 239 Pu ratios varied between 0.5 and 1.2 for ten prominent lines in the 2700-3600 keV energy range. Such significant differences in relative peak intensities make it possible to determine relative fractions of these isotopes in a mixed sample. A method for determining fission product yields by fitting the energy and time dependence of the delayed gamma-ray emission was developed and demonstrated on a limited 235 U data set. De-convolution methods for determining fissile fractions were developed and tested on the experimental data. The use of high count-rate LaBr 3 detectors was investigated as a potential alternative to HPGe detectors. Modeling capabilities were added to an existing framework and codes were adapted as needed for analyzing experiments and assessing application-specific assay concepts. A de-convolution analysis of the delayed gamma-ray response spectra modeled for spent fuel assemblies was performed using the same method that was applied to the experimental spectra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Post Irradiation Examination Plan for High-Burnup Demonstration Project Sister Rods

This test plan describes the experimental work to be implemented by the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE) to characterize high burnup (HBU) spent nuclear fuel (SNF) in conjunction with the High Burnup Dry Storage Cask Research and Development Project and serves to coordinate and integrate the multi-year experimental program to collect and develop data regarding the continued storage and eventual transport of HBU (i.e., >45 GWd/MTU) SNF. The work scope involves the development, performance, technical integration, and oversight of measurements and collection of relevant data, guided by analyses and demonstration of need.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

Destructive examination of shipping package 9975-02101

Destructive and non-destructive examinations have been performed on the components of shipping package 9975-02101 as part of the comprehensive Model 9975 package surveillance program. This package is one of ten high-wattage packages that were selected for field surveillance in FY15, and was identified to contain several non-conforming conditions. Most of these conditions (mold, stains, drum corrosion, calculated fiberboard dimensions and fiberboard damage) relate to the accumulation of water in the outer and lower portions of the cane fiberboard assembly. In the short term, this causes local but reversible changes in the fiberboard properties. Long-term effects can include the permanent loss of fiberboard properties (thus far observed only in the bottom fiberboard layers) and reduced drum integrity due to corrosion. The observed conditions must be fully evaluated by KAC to ensure the safety function of the package is being maintained. Three of the other nine FY15 high-wattage packages examined in the K-Area Complex showed similar behavior. Corrosion of the overpack drum has been seen primarily in those packages with relatively severe fiberboard degradation. Visual examination of the drums in storage for external corrosion should be considered as a screening tool to identify additional packages with potential fiberboard degradation. Where overpack drum corrosion has been observed, it is typically heaviest adjacent to the stitch welds along the bottom edge. It is possible that changes to the stitch weld design would reduce the degree of corrosion in this area, but would not eliminate it. Several factors can contribute to the concentration of moisture in the fiberboard, including higher than average initial moisture content, higher internal temperature (due to internal heat load and placement with the array of packages), and the creation of additional moisture as the fiberboard begins to degrade.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Destructive Examination of Shipping Package 9975-02019

Destructive and non-destructive examinations have been performed on the components of shipping package 9975-02019 as part of a comprehensive SRS surveillance program for plutonium material stored in the K-Area Complex (KAC). During the field surveillance inspection of this package in KAC, two non-conforming conditions were noted: the axial gap of 1.577 inch exceeded the 1 inch maximum criterion, and two areas of dried glue residue were noted on the upper fiberboard subassembly. This package was subsequently transferred to SRNL for more detailed inspection and destructive examination. In addition to the conditions noted in KAC, the following conditions were noted: - Numerous small spots of corrosion were observed along the bottom edge of the drum. - In addition to the smeared glue residue on the upper fiberboard subassembly, there was also a small dark stain. - Mold was present on the side and bottom of the lower fiberboard subassembly. Dark stains from elevated moisture content were also present in these areas. - A dark spot with possible light corrosion was observed on the primary containment vessel flange, and corresponding rub marks were observed on the secondary containment vessel ID. - The fiberboard thermal conductivity in the radial orientation was above the specified range. When the test was repeated with slightly lower moisture content, the result was acceptable. The moisture content for both tests was within a range typical of other packages in storage. The observed conditions must be fully evaluated by KAC to ensure the safety function of the package is being maintained. Several factors can contribute to the concentration of moisture in the fiberboard, including higher than average initial moisture content, higher internal temperature (due to internal heat load and placement within the array of packages), and the creation of additional moisture as the fiberboard begins to degrade.

42 ENGINEERING↗

DOE OSTI2016

Non-destructive Preirradiation Assessment of UN / U-Si “LANL1” ATF formulation

The goal of the Advanced Non-destructive Fuel Examination (ANDE) work package is the development and application of non-destructive neutron imaging and scattering techniques to ceramic and metallic nuclear fuels, ultimately also to irradiated fuels. The results of these characterizations provide complete pre- and post-irradiation on length scales ranging from mm to nm, guide destructive examination, and inform modelling efforts. Besides technique development and application to samples to be irradiated, the ANDE work package also examines possible technologies to provide these characterization techniques pool-side, e.g. at the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) using laser-driven intense pulsed neutron and gamma sources. Neutron tomography and neutron diffraction characterizations were performed on nine pellets; four UN/ U-Si composite formulations (two enrichment levels), three pure U 3 Si 5 reference formulations (two enrichment levels), and two reject pellets with visible flaws (to qualify the technique). The 235 U enrichments ranged from 0.2 to 8.8 wt. %. The nitride/silicide composites are candidate compositions for use as Accident Tolerant Fuel (ATF). The monophase U 3 Si 5 material was included as a reference. Pellets from the same fabrication batches will be inserted in the Advanced Test Reactor at Idaho during 2016. We have also proposed a data format to build a database for characterization results of individual pellets. Neutron data reported in this report were collected in the LANSCE run cycle that started in September 2015 and ended in March 2016. This report provides the results for the characterized samples and discussion in the context of ANDE and APIE. We quantified the gamma spectra of several samples in their received state as well as after neutron irradiation to ensure that the neutron irradiation does not add significant activation that would complicate shipment and handling. We demonstrated synchrotron-based 3D X-ray microscopy on the composite fuel materials, providing unparalleled level of detail on the 3D microstructure. Furthermore, we initiated development of shielding containers allowing the characterizations presented herein while allowing handling of irradiated samples.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

First Examination of Irradiated Fuel with Pulsed Neutrons at LANSCE (Preliminary Results)

We present preliminary results on the characterization of an irradiated U-lOZr-lPd fuel sample that was prepared from the irradiated AFC-3A-R5A sample. U-lOZr metallic fuels are researched as host materials for potential transmutation fuels and the addition of palladium strives to bind lanthanides, thus preventing fuel-cladding chemical interactions (FCCI). These interactions limit the lifetime of metallic fuels and are caused by migration of lanthanide fission products to the periphery of the fuel slug, where they start to interact with the D9 or HT9 steel cladding, ultimately leading to failure of the mechanical integrity of the cladding. Neutrons offer bulk characterization of irradiated materials for which X-ray tomography methods are not suitable due to the immense gamma background emitted from the samples. In particular pulsed neutrons provide information from the ability to resolve the neutron energy using their time-of-flight and thus the potential to utilize neutron absorption resonance to characterize the spatial distribution of isotopes. This, in turn, may allow to characterize the distribution of fission and neutron capture products non-destructively and may ultimately be applied to the bulk of an irradiation capsule prior to destructive post-irradiation examination to identify regions of interest. To allow the characterization of entire irradiation capsules, a cask is under development in the advanced post-irradiation work package at LANL and progress on this development was reported elsewhere. In parallel, an irradiated U-lOZr-lPd sample cut from the AFC-3AR5A irradiation was shipped to LANL and will be fully characterized with an NSUF funded rapid turnaround experiment (RTE) in the 2020 LANSCE run cycle. The sample emits at a dose rate of ~3R/hr on contact and is therefore manageable with remote handling, without requiring a cask. The disk-shaped material is larger than samples prepared for analysis using electron or X-ray methods and is therefore an intermediate step towards characterization of bulk samples at LANSCE. However, since it covers the full diameter of the irradiated fuel slug, some insight on redistribution of elements, spatially resolved information on microstructure, e.g. phase composition and texture, will be possible using the pulsed neutron-based methods developed for fuel characterization at LANSCE. This report describes the development of procedures to handle the sample at LANSCE as well as preliminary data and results from tests conducted in December 2019 on the energy-resolved neutron imaging (ERNI) beam line at flight path 5 and the high pressure-preferred orientation diffractometer (HIPPO) at LANSCE. This effort is a collaboration between LANL, INL, and ORNL. To compare our capabilities with prior work, we present an overview of previously reported bulk characterization of irradiated or spent fuels. The overview addresses neutron diffraction and neutron absorption resonance spectroscopy, both of which have only few reported applications on irradiated or spent nuclear fuel, as well as neutron radiography. This literature review was already described in a previous report but is repeated here to put our current efforts in context of previous work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Cold Testing for Characterization of Oxide Feed Impurities in Support of the ARIES Program

The Advanced Recovery and Integrated Extraction System (ARIES) Program converts surplus plutonium metal components into an oxide powder form and packages the material for final disposition. In support of the ARIES program, over a metric ton (MT) of plutonium has been removed from surplus nuclear weapons since 1998 and packaged for long-term storage in 3013 cans. The oxide production rate is anticipated to increase substantially over the next decade in support of dilute and dispose goals. Analytical chemistry data from destructive analysis of the resulting 70+ blend lots to date has been reported for contaminants in the product oxide. Changes in the Pu product specification for Pu oxide product, induced by a different pit mix, the LANL swap program and processing Alternate (non-Pit Pu) Feed Stock (AFS) metals, will affect the level and the mix of these contaminants in the upcoming years. With these changes in feed material, it will be important to provide fast and efficient measurement of elemental impurities in the oxide to be certain that the process is under control and to monitor the anticipated changes from the historical blend lot data. Non-destructive methods need to be evaluated for the characterization of the plutonium oxide product and the quantification of the impurities at the current and anticipated levels. A feasibility study has begun to investigate the applicability of new spectroscopic methods for oxide impurity characterization. To this end, here we describe the preparation of surrogate materials to support these investigations, and the results of a feasibility study investigating the use of LIBS (Laser Induced Breakdown Spectroscopy) to characterize the surrogate materials as calibration standards.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Performance of Pulsed Thermal Tomography Imaging with Machine Learning-Based Classification of Defects in Additively Manufactured Structures

Additive manufacturing (AM) is an emerging method for cost-efficient fabrication of complex topology nuclear reactor parts from high-strength corrosion resistance alloys, such as stainless steel and Inconel. AM of metallic structures for nuclear energy applications is currently based on laser powder bed fusion (LPBF) process. Some of the challenges with using LPBF method for nuclear manufacturing include the possibility of introducing pores into metallic structures. Integrity of AM structures needs to be evaluated nondestructively because material flaws could lead to premature failures in high temperature nuclear reactor environment. Currently, there exist limited capabilities to evaluate actual AM structures non-destructively. Pulsed Thermal Tomography Imaging (PTT) provides a capability for non-destructive evaluation (NDE) of subsurface defects in arbitrary size structures. The PTT method is based on recording material surface temperature transients with infrared (IR) camera following thermal pulse delivered on material surface with flash light. The PTT method has advantages for NDE of actual AM structures because the method involves one-sided non-contact measurements and fast processing of large sample areas captured in one image. Following initial qualification of an AM component for deployment in a nuclear reactor, a PTT system can also be used for in-service nondestructive evaluation (NDE) applications. In this report, we describe recent progress in enhancing PTT capabilities in detecting and visualizing microscopic defects in metallic specimens. The thermal tomography (TT) algorithm obtains depth reconstructions of spatial effusivity from the data cube of sequentially recorded surface temperatures. However, interpretation of TT images is non-trivial because of blurring of images with increasing depth. To address this challenge, we have developed a deep learning convolutional neural network (CNN) to classify size and orientation subsurface defects in simulated TT images. CNN is trained on a database of TT images created for a set of simulated metallic structures with elliptical subsurface voids. Test of CNN performance demonstrate the ability to classify radii and angular orientation of subsurface defects in TT images. In addition, we have shown that CNN trained on elliptical defects is capable of classifying irregular-shaped defects obtained from scanning electron microscopy (SEM) of stainless steel sections printed with LPBF.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Destructive Examination of Shipping Package 9975-02731

Destructive and non-destructive examinations were performed on the components of the package 9975-02731 as part of a comprehensive Savannah River Site surveillance program for plutonium materials stored in the K-Area Complex (KAC). The package stored nuclear materials in KAC for 13.8 years. Inspection of the package during opening in KAC noted one non-conforming condition: a large discolored area on the upper fiberboard subassembly. The package was subsequently transferred to Savannah River National Laboratory for more detailed examination. In addition to the observation noted in KAC, the following conditions were observed: (1) Axial gap of 1.021 inch slightly exceeded the 1 inch maximum criterion, and (2) Lead shield height exceeded drawing tolerance of 24.7 inch by 0.019 inch. Visual examination of the upper fiberboard assembly and analysis of the discolored fiberboard indicate the discoloration was due to wood glue residue. The physical, thermal, and mechanical properties of the fiberboard met the acceptance criteria and/or were within the range of previously tested fiberboard and baseline samples. The visual, microscopic and tensile testing results were consistent with previous O-ring and baseline Viton results. The lead shield surface was covered with corrosion product as observed on other shields but there was no evidence of excessive blistering, flaking, or spalling. Besides minor and expected corrosion, no evidence of a degraded condition was found in this package. Examination of the 9975-02731 corroborates existing evidence that the 9975 package is robust and the components can perform their expected functions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

ON-LINE MONITORING FOR PROCESS CONTROL AND SAFEGUARDING OF RADIOCHEMICAL STREAMS AT SPENT FUEL REPROCESSING PLANTS

The International Atomic Energy Agency (IAEA) has established international safeguards standards for fissionable material at spent nuclear fuel reprocessing plants to ensure that significant quantities of weapons-grade nuclear material are not diverted from these facilities. Currently, methods to verify material control and accountancy (MC&A) at these facilities require time-consuming and resource-intensive destructive assay (DA). Leveraging new on-line non-destructive assay (NDA) techniques in conjunction with the traditional and highly precise DA methods may provide a more timely, cost-effective and resource-efficient means for MC&A verification at such facilities. Pacific Northwest National Laboratory (PNNL) is developing on-line NDA process monitoring technologies, including a spectroscopy-based monitoring system, to potentially reduce the time and resource burden associated with current techniques. The spectroscopic monitor continuously measures chemical compositions of the process streams including actinide metal ions (U, Pu, Np), selected fission products, and major non-radioactive flowsheet chemicals using UV-vis-near infrared and Raman spectroscopy. This paper provides an overview of the methods and reports our on-going efforts to develop and demonstrate the technologies. Our ability to identify material intentionally diverted from a liquid-liquid extraction contactor system was successfully tested using on-line process monitoring as a means to detect the amount of material diverted. A chemical diversion and detection of that diversion, from a solvent extraction scheme was demonstrated using a centrifugal contactor system operating a tributyl phosphate based extraction. A portion of the feed from a counter-current extraction system was diverted while a continuous extraction experiment was underway; the spectroscopic on-line process monitoring system was simultaneously measuring the feed, raffinate and organic products streams. The amount observed to be diverted by on-line spectroscopic process monitoring was in excellent agreement with values based from the known mass of sample directly diverted from system feed solution.

Np↗

DOE OSTI2019

Materials Characterization and Interrogation using Terahertz Radiation

Terahertz (THz) radiation is a powerful tool for characterizing materials and interrogating complex systems. The low-energy, non-ionizing nature of THz photons make it ideal for use as a non-destructive, non-contacting probe. Identification of materials by their unique THz response is possible through various absorption mechanisms, including vibrational (phonon) and rotational spectra. The Drude-like response of materials allows for non-contact electrical conductivity measurements as well. In the additive and advanced manufacturing realm, high sampling rates (kHz) and ability to extract electrical conductivity and composition makes in-situ THz imaging and spectroscopy a prime candidate for monitoring melt-pool dynamics in metal 3D printers. The fiberization of pulsed lasers systems enables the use of THz radiation to monitor oxide layer growth and characterize microstructure in challenging environments, whether ex-situ (e.g. post irradiation hot-cells) or in-situ (e.g. Transient Test Reactor, TREAT), through time of flight measurements and unique vibrational spectra of materials, providing crucial data on previously out of reach processes. While security imaging using THz radiation is already employed in airport body scanners, further miniaturization and ruggedization of THz systems enables materials characterization during field operations, adding a necessary and complementary tool to the arsenal of spectroscopic technologies available to the military and first responders. Cybersecurity is also a major focus for the coming decades; the use of THz interrogation methods to monitor integrated circuit operations provides a non-contacting, undetectable probe for system verification.

36 MATERIALS SCIENCE↗

DOE OSTI2020

MESOSCALE THERMAL TRANSPORT MEASUREMENTS OF MULTI-PHASE AND POROUS NUCLEAR FUELS USING A SQUARE-WAVE PULSE THERMOREFLECTANCE TECHNIQUE

The safe and efficient operation of nuclear reactors require accurate knowledge of peak temperatures in the fuel assemblies. The temperature profiles are governed by the thermal transport properties of the fuel, namely the thermal conductivities (k) and thermal diffusivities (D). These values can be very difficult to measure as they are known to vary considerably from the measured bulk values of the fresh fuel, and quickly degrade with increasing burnup [1 -3] . Laser-based techniques have been effectively used for non-destructive and non-contact thermal transport measurements of a wide variety of materials, including nuclear materials [4-6] that would otherwise prove too hazardous or difficult to measure otherwise. In this study, a new thermoreflectance technique known as square-pulse transient thermoreflectance (SPTR) is described and used to determine the mesoscale thermal diffusivity of both uranium sesquisilicide (U3Si2) and uranium nitride (UN) phases in a composite fuel with micron level spatial resolution [7]. This technique employs a rapid train of square-wave pulses from an excitation laser to create a periodic heat flux on a gold coated sample surface. Surface adsorption results in transient film temperatures and hence rapid fluctuations in thermoreflectance that can be measured via a detection laser coupled with a digital oscilloscope. The lasers are coaxially focused on the sample surface, allowing for a sample measurement area of a single convolved laser spot size (~2 µm). A sensitivity analysis was conducted to identify key measurement parameters of this technique using reference materials with a range of thermal conductivities comparable to those of both ceramic, composite, and metal nuclear fuel types (1.4 – 27.2 W/m-K). The reference materials were measured using the new technique as well as a spatial-domain thermoreflectance technique (SDTR) previously reported for a comparison [8]. Additionally, measurements of several U3Si2 and UN phase regions of a polished UN/U3Si2 (70/30 vol.%) sample were taken, and the resulting calculated D values are reported, with both techniques showing excellent agreement between samples. This technique was used to scan a multiphase region at 5 micron increments to generate a local diffusivity map, demonstrating the utility of the techniques for measuring thermal transport properties in specimens with precipitates and secondary phases. Furthermore, the technique is currently being applied to measure thermal properties of Fast Flux Test Reactor (FFTR) irradiated metal fuel specimens whose porous microstructure make it very difficult to measure using other techniques. Comparison of the local scale measurements are compared with the pre-irradiated fuel samples to show the degradation of thermal transport in fuels due to pores from fission gas bubbles and other irradiation induced defects.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Production of Particle Reference and Quality Control Materials

Maintaining the superior performance of new analytical instrumentation and pushing the boundaries of ever-smaller particle analysis by methods such as secondary ion mass spectrometry (SIMS) has become limited by the availability of certified particle standards for calibration, quality control, and validation. To meet this growing demand for a reliable and universal approach to the generation of uranium particle reference material, the Pacific Northwest National Laboratory (PNNL) and Savannah River National Laboratory (SRNL) are collaborating on a joint venture that establishes a number of chemical pathways to the fabrication, purification, and stabilization of uranium particle material to within a fixed particle size range, and well-characterized isotopics. PNNL particle standards are designed and tailored to meet the criteria essential to the calibration and benchmarking of instruments used in both the non-destructive and destructive assay of particulate material, typically collected from environmental swipe sampling. Previous testing and optimization of this colloidal approach to particulate material has centred on tight size distributions, singular composition and density, uniform morphology, and tailored isotopic abundances. Extensive validation of this material has since been performed, both at the National Institute of Standards and Technology (NIST) and the International Atomic Energy Agency (IAEA), demonstrating its suitability for quality control needs of large geometry (LG)-SIMS analysis. Building on this momentum, the production of low-enriched uranium particle reference material, with specially tailored isotopics, has moved from development to full operation. Herein, various aspects of the production cycle will be discussed, including detailed accounts of the technical methodologies being employed, as well as insights into the sample characterization and acceptance testing requirements.

Nuclear Safeguards, Particle Standards, IAEA↗

DOE OSTI2015

Impact of lump characteristics on self-shielding corrections of active neutron interrogation on fissile material in waste - 15405

Non-destructive active neutron assay techniques such as active neutron coincidence counting, differential die away analysis or the californium shuffler method rely on the interrogation of fissile nuclear materials by an external neutron source. Whether it is a spontaneous fission or (α,n) neutron source, like {sup 252}Cf or AmLi; or a fusion neutron generator, all of these techniques rely on induced secondary fission events to provide prompt or delayed neutron signals that serve as the basis for the fissile material quantification. The accuracy of these fissile mass measurements is therefore dependent on the neutron interrogation efficiencies determined for calibration reference standards and whether the measured items are comparable to the calibration condition. In such favorable conditions, it is possible to establish a reliable empirical non-linear relationship between apparent (uncorrected) and real or true fissile mass. However, in waste measurements, this is unlikely to be the case; thus a calibration approach that takes account of the neutron self-shielding effect is required. By incorporating the Self-Shielding Factor (SSF) of the calibration reference standards, a linear mass calibration factor [s{sup -1}. {sup 239}Pu{sub eq} g{sup -1}] can be found; this calibration is accurate for waste in which the fissile material is 'infinitely dilute' i.e. the waste exhibits no self-shielding; this is assumed to be representative of dispersed material. The self-shielding correction and its systematic uncertainty are then left to be treated as part of the Total Measurement Uncertainty (TMU) evaluation associated with the assay result. The derivation of the TMU contribution associated with the self-shielding effect in nuclear waste is a complex problem for which a reliable evaluation has to be performed. This is usually based on assuming 'worst case scenarios' for the distribution of material that can arise in a particular waste stream. Such an approach is conservative, but often very penalizing, especially if one considers larger lumps (those containing grams of fissile material); for such lumps, the self-shielding correction becomes very significant, potentially altering the mass of {sup 239}Pu{sub eq} by over an order of magnitude. A worst case 'nuclear safety value' may not be the most appropriate choice for building a consignment best estimate or repository sentencing value for an item. In the present work the authors describe a numerical approach to study the variability of neutron self-shielding factors associated with distributions of a wide range of lump characteristics in terms of size, shape, chemical composition, density and isotopic composition. The described novel calculation tool is capable of accurately predicting the real impact of random distribution of lumps in a waste material, and allowed to show that given reasonable, defensible, assumptions on the composition of the lumps in waste stream, the systematic error component of the DDA TMU can be significantly reduced. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Life Extension of Nuclear Plant Facilities through Monitoring and Detailed Analysis - 16175

The UK has accumulated a substantial legacy of radioactive waste from various civil nuclear and defence programmes. Presently, however most of the UK radioactive waste is generated from nine power stations which generate approximately one sixth of the of the country's electricity. Irradiated fuel is removed from these reactors and safe management of the radioactive solid and liquid effluents is required. The safe management of these effluents is essential. Sellafield, in West Cumbria UK, contains two reprocessing plants, one designed to process nuclear fuel from Magnox reactors (CO{sub 2} cooled with Uranium bar fuel) and the other to process nuclear fuel from Advanced Gas cooled Reactors and Pressurized Water Reactors. The reprocessing stage enables extraction of fissile material for recycling. This leaves a volume of dilute but high-level waste. The high-level radioactive liquid waste is concentrated to reduce its volume and then incorporated into borosilicate glass, using a process called vitrification. The glass is then poured into stainless steel containers and placed in long term storage. This required concentration of HLW liquor is achieved using a suite of aging evaporators. All evaporators are of similar design constructed from corrosion resistant stainless steel having dimensions height ∼11 m, internal diameter 3.05 m and capable of holding 13.7 m{sup 3} of liquor. The basic principle of operation is to heat the dilute liquor under partial vacuum, at constant volume, until the target concentration is achieved. Heating of the liquor is achieved using steam heated coils within the evaporator, and steam in the jacket which surrounds the lower half of the evaporator vessel. The evaporator is then brought to atmospheric pressure and the concentrated liquor is ejected whilst hot. The evaporator is then cooled with water cooled coils and a water filled jacket. New dilute liquor is then added for a new batch. The process is then repeated. As the evaporators reach the end of their original design life accurate prediction of the current condition of nuclear plant facilities is essential to safely justify continued plant operation by ensuring structural integrity. This poses a significant challenge as many aging UK nuclear facilities were not inherently built with inspection in mind. The potential life limiting components of the HA evaporators at Sellafield are the surfaces that contact the product liquor at elevated temperatures i.e. the steam heated surfaces of the coils within the evaporator vessel and the vessel base and wall surrounded by the steam jacket. Each heating component is critical to the operational life of the evaporator - the removal from service of a coil heating component significantly reduces the operational flexibility and remnant life of this plant. Over the last decade a variety of cutting-edge expertise and methodologies have been utilised to accurately measure and then predict the current condition of the plant and also to predict its remnant life. This paper provides an overview of the development of several techniques deployed, namely non-destructive testing/inspection, in-house software development and finite element modelling. These methods have been validated by lab-scale or full-scale experiments along with historical plant data. These techniques have been evolved and refined for over a decade, providing vital insights into the physical behaviour of this complex reprocessing system. This enables not only accurate assessment of the current condition of the plant equipment but also allows scientifically underpinned predictions to be made of how it will behave into the future. This is critical for Sellafield as this knowledge feeds into their safety case to the Office of Nuclear Regulation to justify continued operation. It is concluded that this integrated approach provides a robust analysis tool which has driven change and optimisation of plant procedures ensuring continued safe operation whilst extending the life of the facility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2018

Hanford Under-tank Inspection with Ultrasonic Volumetric Non-destructive Examination Technology - 18470

The U.S. Department of Energy (DOE) and the Hanford Site Tank Operations Contractor Washington River Protection Solutions, LLC (WRPS) are sponsoring a non-destructive evaluation (NDE) technology development program to identify and mature volumetric (non-visual) NDE technology that will enable the examination of Hanford double-shell tank (DST) bottoms. NDE technology for Hanford under-tank examination will be made possible through technology maturation that includes adaptation of NDE sensor technology to overcome access challenges presented by tank risers and refractory pad air-slots, followed by integration with robotic delivery systems, and ultimately qualification and deployment of the inspection systems. The stages of technology maturation and the testing and evaluation required to support the process are organized under three program phases: Phase I - NDE Capability Testing: Identify and down-select NDE technologies based on flaw detection and characterization abilities only; Phase 2 - NDE Delivery System Testing: Mature promising NDE technologies to adapt transducer hardware and robotic delivery system to address access challenges; Phase 3 - Full-scale Demonstration of Integrated NDE System: Demonstrate adapted NDE technologies in a cold test platform to challenge flaw detection and navigation abilities. Phase I of the program, which was initiated and completed in FY2017, focused on completing the following five key activities: 1. Identifying a broad cross section of potentially applicable NDE volumetric inspection technologies for under-tank examination. 2. Down-selecting the broad set of NDE technologies to a set of strong candidates based on initial flaw detection performance and potential to be adapted/matured to overcome primary tank access challenges posed by access risers and/or refractory pad air-slots. 3. Evaluating the flaw detection performance of the candidate sensors through testing. 4. Using the test results to baseline sensor performance against the flaw detection requirements established for high-level waste tanks. 5. Assessing the trade-offs and vulnerabilities of the candidate sensors that would negatively impact sensor performance reliability or complicate tank inspection operations. The completion of the first three key activities satisfied the first two Phase I test objectives, which were to complete Technology Screening and Sensor Effectiveness Testing. Completion of the fourth key activity satisfied the final test objective of Phase I, which was to determine the extent to which the sensors can satisfy high-level waste tank flaw detection requirements. Sensor flaw detection performance testing yielded several suitable sensor technology options, although each has specific risks or challenges that would need to be accepted or overcome. Thus, the fifth key activity was performed to evaluate sensor risks and challenges for consideration with flaw detection performance. The Phase I evaluation outcomes will be used to support the Phase I programmatic objective, which is to identify one or more NDE sensor technologies for adaptation and maturation for the DST environment. Selection of one or more sensors will mark the culmination of Phase I of the NDE Technology Development Program and allow progression to Phase II.

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DOE OSTI2020

Augmented Monitoring and Condition Assessment Program for SNF Wet Storage Life Extension - 20489

Approximately 27 MTHM of spent nuclear fuel (SNF) owned and managed by the U.S. Department of Energy, Office of Environmental Management is stored in the L Basin at the Savannah River Site (SRS). This 'DOE SNF' is comprised of approximately 12,000 aluminum-clad, aluminum-based fuel assemblies (∼7 MTHM), and approximately 2000 non-aluminum fuel assemblies (∼20 MTHM). A program is in progress to perform Non-Destructive Examination (NDE) of the fuel and their storage containers to characterize the materials' condition, and to evaluate the effects of service to enable continued safe wet storage of the SNF. The Augmented Monitoring and Condition Assessment Program (AMCAP), a two-part program to develop and implement remote underwater Non-Destructive Examination of the aluminum SNF, and of the containers of the non-aluminum SNF, respectively, is aimed at the characterization and evaluation of corrosion degradation of aluminum fuel and container materials. The predominant design of the aluminum SNF (ASNF) stored in L Basin is the Materials Test Reactor (MTR) equivalent design, a plate fuel design. These SNF are stored in 5'' diameter tubes or 5'' x 5'' squares (called bundles) that are nominally 12' or up to 14' long. The SNF is de-bundled and inspected using a custom-designed MTR Fuel Inspection Table. The inspection table provides for indexed fuel positioning for a video camera examination with controlled lighting. A total of 10 of the SNF originating from foreign research and test reactors were selected for examination based on burnup, enrichment, and prior damage caused by service/storage history. A special inspection campaign of these 10 assemblies is in progress. The observed corrosion damage included minor to moderate attack from general corrosion, pitting, crevice, end grain and galvanic corrosion. Example results from the completed inspections are shown and discussed. The focus is a comparison of the as-received condition versus the as-found current storage condition that will serve to validate Water Chemistry and Corrosion Monitoring Programs. The non-aluminum SNF (NASNF) stored in L Basin are of diverse design that includes various geometries with claddings of stainless steel, Zircaloy, and Hastelloy. The fuel core materials include uranium alloys, oxides/mixed oxides, and carbides. These SNF materials, originating from early experimental and test reactors, are in various physical forms including single fuel elements and cut pieces. The fuel is stored in L Basin in various configurations including in direct bundled storage in aluminum tubes and in isolation cans that are in the bundles or in a larger over-size storage container (OSC). Concern with inside-out corrosion and the potential loss of configuration control and ability to handle the storage containers prompted the development of remote NDE methods that include visual and UT technologies to assess the condition of the containers. Candidate stored materials were selected for a special inspection campaign; the development of the NDE methods for the inspection for galvanic, crevice and sediment-induced corrosion (inside-out) are discussed. A summary of the SNF storage in L Basin at the SRS, and an overview of the AMCAP to enable continued safe storage of DOE SNF are described. (authors)

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