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At least 325 records · Page 18

Development of spectroscopy apparatus for molten salt reactor safeguards and material characterization

A molten salt reactor (MSR) produces nuclear fission energy using mixture of fissile and non-fissile salts. Salt in the reactor functions as the nuclear material and the coolant allowing for a safer design. International nuclear safeguards is the monitoring of nuclear reactors, nuclear fuel, and irradiated material to prevent the proliferation of nuclear weapon grade material in hostile foreign nations. The mixture of salt creates a proliferation risk as it generates a conglomeration of fuel, daughter nuclei, and corrosive material. A method to monitor and measure the materials present in the reactor is essential to the scalable deployment of MSRs. The objective of this project was to design a spectroscopy apparatus for aqueous salt so it can be measured and collected consistently in the aerosol phase.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Implementation of Microcalorimeter Array Technology for Safeguards of Nuclear Material

Safeguards of nuclear materials depends on both destructive and nondestructive assay (DA and NDA respectively). Ultra-high resolution microcalorimeter gamma spectroscopy has the potential to substantially reduce the performance gap between NDA and DA methods in determination of plutonium isotopic composition. This paper details the setup of a cryostat and microwave readout system for microcalorimeter gamma spectroscopy, the functionality of which has been successfully demonstrated.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Polyatomic interferences on high precision uranium isotope ratio measurements by MC-ICP-MS: Applications to environmental sampling for nuclear safeguards

Modern mass spectrometry and separation techniques have made measurement of major uranium isotope ratios a routine task; however accurate and precise measurement of the minor uranium isotopes remains a challenge as sample size decreases. One particular challenge is the presence of isobaric interferences and their impact on the accuracy of minor isotope 234 U and 236 U measurements. Furthermore, we present techniques used for routine U isotopic analysis of environmental nuclear safeguards samples and evaluate polyatomic interferences that negatively impact accuracy as well as methods to mitigate their impacts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Conceptual design study of neutron detectors for safeguards measurement of an irradiated pebble

Nuclear material control and accounting (MC&A) of pebble-bed reactors (PBRs) is challenging because a PBR utilizes hundreds of thousands of identical, unmarked pebbles that are continuously recirculated through the core. To develop tools that enable the implementation of international safeguards, especially in the context of MC&A of spent pebbles, we designed and simulated three neutron detection concepts to determine fissile content in individual pebbles: a differential die-away (DDA) detector, a californium interrogation prompt neutron (CIPN) detector, and a passive neutron albedo reactivity (PNAR) detector using Monte Carlo calculations. Burnup calculations were performed on the spent pebbles from the PBMR-400 classic PBR. The varying neutron and gamma source terms, and isotopic compositions in the spent pebbles calculated at various burnup levels were used in the neutron detector models. DDA was found to be sensitive to the number of passes a pebble has had through the core and to the fissile content contained in a spent pebble. Optimization in the DDA design further increased the neutron count rates and thus reduced counting uncertainty. Meanwhile, passive neutron counting using the same detector body could distinguish pebbles with different numbers of passes, but its response was dominated by neutron-emitting actinides and was not sensitive to fissile content. On the other hand, the PNAR technique was not viable for a single pebble but performed reasonably for a 27-pebble array, which suggested potential use for verification measurements of containers filled with 27 or more spent pebbles.

CIPN↗

Improved evaluation of safeguards parameters from spent fuel measurements with the Differential Die-Away (DDA) instrument

The Differential Die-Away (DDA) technique is a highly sensitive non-destructive assay method for characterizing and detecting the presence of fissile material within an item of interest. DDA utilizes a series of pulses from a neutron generator (NG) to actively interrogate an item of interest. The die-away time of the neutron population induced by this active interrogation and the integral of the total differential die-away signal can be used to characterize items such as nuclear waste drums and spent nuclear fuel assemblies. In this work, Los Alamos National Laboratory (LANL) conceptualized, designed, and fabricated a DDA instrument that was deployed for field test measurements at the Central Interim Storage Facility for Spent Nuclear Fuel (Clab) in Oskarshamn, Sweden. The instrument performed multiple static measurements at fixed locations and dynamic axial scans of 15 pressurized water reactor (PWR) and 10 boiling water reactor (BWR) spent fuel assemblies, collecting both passive and active measurement data. The static assays of the assemblies measured the differential die-away signal, die-away time, and total passive neutron emission rate to create calibration curves for the evaluation of assembly multiplication, burnup, initial enrichment, effective fissile mass, and total elemental plutonium mass. Each calibration curve was optimized by minimizing the relative root mean square error (RRMSE) of assembly assay results compared to declared assembly parameters. The same quantities were also measured with the axial scans, and the resulting data were applied in two ways: (1) in the creation of calibration curves to improve evaluation of the same safeguards parameters as static assays, and (2) for comparison to simulation. In most cases, across both PWR and BWR assemblies, axial scan data improved the estimation of the above parameters, quantified by decreasing the calibration curve RRMSE. These axial scan results demonstrate the ability of the DDA instrument and analysis method to characterize spent PWR and BWR fuel as well as, or better than, a static assay of the same assembly. Furthermore, the DDA instrument’s unique ability to obtain both active and passive data in a single, axial scan of an entire spent fuel assembly represents a more efficient and accurate way of assaying spent fuel for verification purposes. These results represent a significant advancement for characterizing spent nuclear fuel compared to current technologies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Neutron resonance transmission analysis prototype system for thorium fuel cycle safeguards

Emerging thorium-based reactor designs and fuel cycles present challenges to traditional non-destructive assay techniques used in international safeguards. Specifically, assaying the masses of 233 U and 235 U when they are present together in samples with high gamma ray backgrounds is difficult because of similar passive neutron signatures and relatively weak gamma-ray emissions of 233 U. The Pacific Northwest National Laboratory (PNNL) and the Massachusetts Institute of Technology (MIT) are developing a compact neutron resonance transmission analysis (NRTA) system as one potential solution to these challenges. The NRTA technique provides isotopic information for a sample via neutron time-of-flight (TOF) measurements that exploit a sample’s epithermal neutron resonance cross-sections. A recently developed portable NRTA system uses a commercially available, pulsed deuterium-tritium neutron generator with a ~2 m flight path and a GS20 lithium glass scintillator detector. Finally, this paper describes the prototype NRTA system design, a refined radiation transport model of the system, preliminary measurements with thorium and uranium sources, and demonstration of a quantitative isotopic estimation algorithm.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Employing antineutrino detectors to safeguard future nuclear reactors from diversions

The Non-Proliferation Treaty and other non-proliferation agreements are in place worldwide to ensure that nuclear material and facilities are used only for peaceful purposes. Antineutrino detectors, sensitive to reactor power and fuel changes, can complement the tools already at the disposal of international agencies to safeguard nuclear facilities and to verify the States' compliance with the agreements. Recent advancement in these detectors has made it possible to leverage them to reduce the likelihood of an undetected diversion of irradiated nuclear material. We study the sensitivity of antineutrino monitors to fuel divergence from two reactor types: a traditional light-water reactor and an advanced sodium-cooled reactor design, a likely candidate for future deployment. The analysis demonstrates that a variety of potential diversion scenarios can be detected by such a system. We outline recent developments in monitoring capabilities and discuss their potential security implications to the international community.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Probabilistic risk analysis toward cost-effective 3S (safety, safeguards, security) implementation

Probabilistic Risk Analysis (PRA) has been introduced for several decades in safety and nuclear advanced countries have already used this methodology in their own regulatory systems. However, PRA has not been developed in safeguards and security so far because of inherent difficulties in intentional and malicious acts. In this paper, probabilistic proliferation and risk analysis based on random process is applied to hypothetical reprocessing process and physical protection system in nuclear reactor with the Markov model that was originally developed by the Proliferation Resistance and Physical Protection Working Group (PRPPWG) in Generation IV International Framework (GIF). Through the challenge to quantify the security risk with a frequency in this model, integrated risk notion among 3S to pursue the cost-effective installation of those countermeasures is discussed in a heroic manner.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Rapid Analytical Methodology for Chloride Molten Salt Reactor Safeguards and Process Monitoring

Technologies that enable near real-time isotopic analysis of advanced molten salt reactor (MSR) fuels are critically needed to safeguard these reactors, increase their operational efficiency, and enable their widespread deployment with confidence. We present a systematic approach to developing near real-time dissolution and chemical isolation of U, Pu, and major fission products from highly radioactive chloride molten salt samples. Chemical yields greater than 95% were observed for both uranium and the lanthanides. Interference reduction enabled the detection and quantification of key diagnostic isotopes (including 112Ag, 147Nd, and 153Sm) that were previously undetectable in the original sample. The results from this initial scoping study lay the foundation for the development of future automated systems that can enable cost-efficient, near-real time chemical separation and analysis of extremely highly radioactive molten salt samples.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗

Ultra-secure RF Tags for Safeguards and Security - SBIR Phase II Final Report

This is the Final Report for the DOE Phase II SBIR project “Ultra-secure RF Tags for Safeguards and Security.” The topics covered herein include technical progress made, progress against the planned milestones and deliverables, project outcomes (results, collaborations, intellectual property, etc.), and a discussion on future expectations of deployment and impacts of the results of this work. In brief, all planned work for the project was successfully completed, on or ahead of schedule and on budget. The major accomplishment was the successful development of a very advanced passive ultra-secure RFID tag system with combined security features unmatched by any commercially available ones. These tags have high-level dynamic encrypted authentication, a novel tamper-proofing mechanism, system software including graphical user interfaces and networking, and integration with a fiber-optic seal mechanism. This is all accomplished passively (with no battery) by incorporating sophisticated hardware in the tag which harvests the energy from the RFID readers that are interrogating the tag. Based on initial feedback (and deployments) at DOE’s Lawrence Livermore National Laboratory (LLNL), it is anticipated these tags and their offspring will meet DOE and international community needs for highly secure RFID systems. Beyond the accomplishment of those original objectives for the ultra-secure RF tags, major new spin-off thrusts from the original work were identified and successfully pursued with the cognizance of the DOE sponsor office. In particular, new classes of less sophisticated RFID tags were developed whose lineage derives from the core R&D thrusts of this SBIR. These RF “tag variants” have some, but not necessarily all, of the advanced characteristics described above and can therefore be less expensive and meet far wider markets. With customer pull from the DOE and its national laboratories, new RFID tags and systems (including custom readers and software) for government needs in asset management and tracking were developed. These were tested at a national laboratory and other government facilities, and resulted in immediate procurement actions by the government and deployment of these new systems. Thus, commercialization of the results of this Phase II DOE SBIR was already underway before the end of the SBIR itself. More importantly, operations involving asset management at selected DoE and government sites are already being impacted favorably and could have much broader impacts in the near future.

42 ENGINEERING↗

Uncertainty Quantification for Nuclear Safeguards and Non-Destructive Assay - Fact Sheet

UQ is the scientific art of generating confidence statements. Without defensible UQ physical measurements and calculations have no meaning. The UQ team performed a series of case studies with the following results: minimum detectable activity of a Tomographic Gamma-Ray Scanning system was determined using the Currie formalism. Bootstrapping method was used to generate fluorescence yield parameters and uncertainties. For Hybrid K-Edge Densitometry (HKED) measurements, these parameters can be used to predict the concentration of plutonium and quantify uncertainty in HKED models for nuclear safeguards measurements. Detection efficiency was determined for a coincidence counter using covariance data. The use of covariance information drastically reduced the total uncertainty in the average detection efficiency.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

OR14-V-Uncertainty-PD2La Uncertainty Quantification for Nuclear Safeguards and Nondestructive Assay Final Report

The various methods of nondestructive assay (NDA) of special nuclear material (SNM) have applications in nuclear nonproliferation, including detection and identification of illicit SNM at border crossings and quantifying SNM at nuclear facilities for safeguards. No assay method is complete without “error bars,” which provide one way of expressing confidence in the assay result. Consequently, NDA specialists typically provide error bars and also partition total uncertainty into “random” and “systematic” components so that, for example, an error bar can be developed for the total mass estimate in multiple items. Uncertainty Quantification (UQ) for NDA has always been important, but it is recognized that greater rigor is needed and achievable using modern statistical methods.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

INITIAL Reactor Safeguards Laboratory

The safeguards and core cooling laboratory will consist of sample activation, sample measurement and sample analysis. Two activation samples of natural UO 2 will be irradiated in the reflector region of the McClellan Nuclear Research Center (MNCR). One sample will be cadmium covered and the other will not have cadmium covering (bare). Both samples will be measured with a HPGe detector, where energy and efficiency calibrations are necessary. Analysis is detailed below in the analysis section.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Plutonium particle analysis by LG-SIMS and LA-MC-ICP-MS for environmental safeguards

During nuclear facility inspections, International Atomic Energy Agency (IAEA) inspectors collect dust particles using cotton swipes. Analysis of these swipes is an extremely powerful tool with which to confirm treaty compliance or identify treaty violations. Through particle analysis it is possible to identify individual particles representative of nuclear activities. Uranium particle analysis is a reasonably mature technique used by IAEA and its Network of Analytical Laboratories for treaty verification. However, the IAEA has recently identified the maturation of plutonium and mixed uranium-plutonium particle analysis techniques as a top priority. We propose to address this area directly by developing the new methods necessary to analyze samples containing plutonium and mixed uranium-plutonium particles. The end products of this study will be: (A) more accurate and ultra-precise isotopic characterization of plutonium -bearing particles from environmental swipe samples, and (B) development and validation of laser ablation particle analysis techniques as robust and accurate analysis methodologies for future safeguards missions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗