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RAMM-TM for detection of gas leakage from canisters containing spent nuclear fuel

Remote Area Modular Monitoring (RAMM) for canister surface temperature measurement (TM), or RAMM-TM, is a novel remote monitoring device for detection of gas leakage based on surface temperature measurements of canisters containing spent nuclear fuel. Here we describe the development of RAMM-TM, as is the demonstration of its performance in detecting canister gas leakage from a small, simulated chloride-induced stress corrosion crack in experiments using a 1/4.5-scale model cask. Both helium and air gas leakage from a canister were detected within hours after the start of the leakage. The change in surface temperatures at the top and bottom of the canister (ΔTBT) during gas leakage (depressurization) triggered automatic alarms, providing a sound basis for early detection of gas leakage from the canister. This methodology would allow consequence management through the implementation of mitigatory actions to continue effective aging management and to reduce risks to public safety, health, and the environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A risk-informed assessment tool to support review of license amendment requests for spent nuclear fuel dry cask storage systems

We report that while risk-informed safety evaluations are common methodologies used by the U.S. Nuclear Regulatory Commission (NRC), their application in the field of commercial spent nuclear fuel (SNF) dry storage has received limited attention. For instance, license amendment requests (LARs) for SNF dry cask storage systems (DCSSs) are evaluated according to U.S. NRC standard review plans (SRPs). However, risk-informed LAR review strategies could improve the understanding of critical system modifications, and lead to more predictable, efficient, and consistent LAR review processes. A methodology to develop a risk-informed LAR review tool is presented. Although focused on DCSSs, this methodology can be used to develop similar tools for a broad spectrum of safety-relevant systems. The end product (i.e., the tool) includes a tree diagram to help visualize the review risk significances assigned to a predefined set of system modifications and supporting rationale documentation. Instructions support correct tool application and provide the user with a path to incorporate currently unevaluated modifications in the tool structure. The demonstration of the methodology leads to the conclusion that risk-informed reviews of DCSS LARs are possible, although the tool precision could benefit from additional risk information. Further, the results indicate that many typical LARs involve low-risk or medium-risk modifications.

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Using temperature and flow fields to detect gas leakage from canisters containing spent nuclear fuel: Applications to RAMM-TM

The multi-physics STAR-CCM+ code has been used to simulate the temperature and flow fields in canister gas leakage experiments conducted by using a 1/4.5-scale model storage cask. The simulations were conducted at Argonne National Laboratory’s Laboratory Computing Resource Center, utilizing high-performance computing resources. Development of STAR-CCM+ simulation models for the 1/4.5-scale model cask is described herein, followed by validation of the simulation results against experimental data. Canister depressurization and thermal response during gas leakage are discussed, along with analyses of the leakage path and allowable leakage rate. The insights gained from the STAR-CCM+ simulations and leakage analyses will help guide future experiments and actual industry applications of Argonne’s Remote Area Modular Monitoring system for canister surface temperature measurement (RAMM-TM) to enable effective aging management of spent fuel during extended dry storage, as well as help reduce risks to public safety and health and protect the environment.

Canister gas leakage↗

History and status of spent fuel treatment at the INL Fuel Conditioning Facility

Experimental Breeder Reactor II (EBR-II) had an illustrious operational history from 1964 to 1994 as one of the first sodium-cooled fast reactors to use sodium-bonded metallic driver fuels and blankets. EBR-II was a testbed for fuel development and reactor design principles. Following shutdown, it was decided to use electrometallurgical methods to treat the spent fuel and blanket materials for final disposition. Here, this paper provides a brief history of U.S. liquid metal cooled reactor development with emphasis on EBR-II, and a technical description of the electrometallurgical methods.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Non-destructive evaluation and machine learning methods for inspection of spent nuclear fuel canisters: A state-of-the-art review

Nuclear energy is among the cleanest and most efficient energy sources currently available. The operation of nuclear power plants (NPPs) produces large amounts of high-level radioactive waste known as spent nuclear fuel (SNF). Currently, large amounts of SNF is stored in dry cask storage systems (DCSSs) for extended interim storage until a permanent disposal solution becomes available. During the extended interim storage, the DCSS, particularly the SNF canisters, may degrade and abnormal conditions may occur. Therefore, non-destructive evaluation (NDE) and machine learning (ML) approaches are necessary for inspection of SNF canisters. This paper presents a state-of-the-art review of literature by summarizing recent progress made on the applications of NDE and ML for inspection of SNF canisters. Sixteen NDE methods are examined and compared: visual inspection, ultrasonic guided waves (UGWs), laser-based approaches, acoustic emission (AE), eddy current testing (ECT), non-invasive acoustic sensing, dynamic modal testing, cosmic ray muons tomography, neutron imaging, gamma rays detection, fiber optical sensors, through-wall communications, X-ray computed tomography (CT), vibrothermography, monoenergetic photon sources, and surface acoustic wave (SAW) sensors. The technology readiness level (TRL) for each method is assessed and compared. Recent publications on ML-enhanced visual inspection, AE, non-invasive acoustic sensing, dynamic modal testing, and neutron imaging for SNF canisters are summarized and future research needs are identified. In conclusion, this review article provides a convenient reference on the state-of-the-art applications of NDE and ML methods for inspection of SNF canisters.

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Design and Optimization of the Direct Recycling of Spent Li-Ion Battery Cathode Materials

Direct regeneration of spent Li-ion batteries based on the hydrothermal relithiation of cathode materials is a promising next-generation recycling technology. In order to demonstrate the feasibility of this approach at a large scale, we systematically design and optimize the process parameters to minimize both energy and raw material costs. Specifically, the effects of regenerative processing parameters on the composition, structure, and electrochemical performance of the regenerated cathode materials are investigated via systematic characterization and testing. From this analysis, it was found that the raw material costs can be substantially reduced by either replacing the typically employed 4 M LiOH solution by a cost-effective mixture of 0.1 M LiOH and 3.9 M KOH or recycling of the concentrated 4 M LiOH for continuous relithiation processes. Finally, life cycle analysis suggests that this strategy results in reduced energy consumption and greenhouse gas emissions, leading to an increased potential revenue, particularly when compared with hydro- and pyrometallurgical recycling methods.

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Momentum informed muon scattering tomography for monitoring spent nuclear fuels in dry storage cask

Development of an effective monitoring method for spent nuclear fuel (SNF) in a dry storage cask (DSC) is important to meet the increasing demand for dry storage investigations. The DSC investigation should provide information about the quantity of stored SNF, and quality assurance of materials should be possible without opening the cask. However, traditional nondestructive examination (NDE) methods such as x-rays are difficult to deploy for DSC investigation because a typical DSC is intentionally designed to shield against radiation. To address this challenge, cosmic ray muons (CRMs) are used as an alternative NDE radiation probe because they can easily penetrate an entire DSC system; however, a wide application of muons is often hindered due to the naturally low CRM flux (~10 4 muons/m 2 /min). This paper introduces a newly proposed imaging algorithm, momentum-informed muon scattering tomography (MMST) , and presents how a limitation of the current muon scattering tomography technique has been addressed by measuring muon momentum. To demonstrate its functionality, a commercial DSC with 24 pressurized light water reactor fuel assemblies (FAs) and the MMST system were designed in GEANT4. Three noticeable improvements were observed for MMST system as a DSC investigation tool: (1) a signal stabilization, (2) an enhanced capability to differentiate various materials, and (3) statistically increased precision to identify and locate missing FAs. The results show that MMST improves the investigation accuracy from 79 to 98% when one FA is missing and 51% to 88% when one-half FA is missing. The advancement of the NDE technique using CRM for DSC verification is expected to resolve long-standing problems in increasing demand for DSC inspections and nuclear security.

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Development of Streamlined Nuclear Safety Analysis Tool for Spent Nuclear Fuel Applications

To understand the changing nuclear and mechanical characteristics of spent nuclear fuel (SNF) or used nuclear fuel (UNF) and the different storage, transportation, and disposal systems at various stages within the waste management system, different types of analyses are required. These analyses require the use of assorted tools and numerous types of data. Using the appropriate modeling and simulation (M&S) parameters and selecting from the diversity of analytic tools to conduct SNF analyses can be a tedious, error-prone, and time-consuming undertaking for analysts and reviewers alike. A new, integrated data and analysis system was designed to simplify and automate performance of accurate, efficient evaluations for characterizing the input to the overall U.S. nuclear waste management system—the UNF-Storage, Transportation & Disposal Analysis Resource and Data System (UNF-ST&DARDS). A relational database has been assembled to provide a standard means by which UNF-ST&DARDS can succinctly store and retrieve M&S parameters for specific SNF analysis. A library of various analysis model templates is used to communicate M&S parameters for the most appropriate M&S application. A process manager facilitates performance of actual as-loaded, assembly-specific, and cask-specific evaluations. Interactive visualization capabilities facilitate data analysis and results interpretation. To date, UNF-ST&DARDS has completed (1) explicit depletion and decay analysis of every fuel assembly (~245 000) discharged from commercial U.S. reactors through June 2013, with 13 cooling time steps (results include isotopic compositions for 142 isotopes, and radiation and thermal source terms); (2) SNF radiation dose rate evaluations at 1 m for all the fuel assemblies discharged through June 2013; and (3) criticality, shielding, thermal, and containment analyses of hundreds of loaded casks. In conclusion, UNF-ST&DARDS also provides various automated report generation capabilities with dynamic figure and table update capabilities based on changes to the Unified Database.

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Drying of Spent Nuclear Fuel: Considerations and Examples

A recently revised American Society for Testing and Materials consensus standard guide for drying of spent nuclear fuel (SNF) provides considerations and guidance for preparing SNF for its safe storage in a sealed dry storage system. The standard discusses (1) needs for drying, (2) techniques to dry, and (3) demonstration of adequate dryness. No specific approach is prescribed since the effective techniques and needs for drying depend on the specifics of the fuel and dry storage system. Here, this paper discusses these topics using examples for both Zr-alloy-clad commercial SNF and for aluminum-alloy-clad research reactor SNF. Residual water can include free water (liquid and/or vapor), physisorbed water bound to internal surfaces, and chemisorbed water incorporated into surface films, such as (oxy)hydroxides. The potential impacts of these residual waters are corrosion/oxidation, radiolytic breakdown into gaseous and/or reactive species, and canister pressurization. For commercial SNF, inadvertent free water, even up to large amounts (e.g., 10+ mol), is not predicted to cause adverse corrosion degradation, except possible fuel oxidation for breached SNF. For aluminum-clad SNF, the production of radiolytic hydrogen with contribution from the chemisorbed water in its hydrated oxides is a primary consideration. For both SNF systems, canister pressurization is predicted to be well within the canister design, and flammability would not pose a safety concern using an oxygen limit of 5 vol % criterion. (Flammability control can be achieved by limiting either hydrogen or oxygen, and an oxygen limit is expected to be easier to meet in the presence of radiolytic H 2 generation.) The two primary technologies for SNF drying, vacuum drying and forced-gas dehydration, are described herein, and drying tests and campaigns using these methods are cited. Dryness criteria and the methods used to detect and measure residual (free) water are also discussed.

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Drying and Analysis of Aluminum (Oxy)hydroxide Films for Dry Storage of Aluminum-Clad Spent Nuclear Fuels

In aluminum-clad spent nuclear fuels, an (oxy)hydroxide layer on the surface of the cladding hosts chemisorbed water formed during reactor and post-discharge exposure to water. Any residual water is susceptible to generating hydrogen via radiolysis, which can be a risk associated with dry fuel storage. Engineering-scale forced helium dehydration (FHD) and vacuum drying tests were conducted on mock-up fuel assemblies that included corroded aluminum surrogate plates to assess the removal of bulk and chemisorbed water. Thermogravimetric analysis was performed on samples of the surrogate plates, both undried control samples used to determine onset temperatures associated with a phase change occurring in the oxide layer and samples from drying tests used to determine the effectiveness of each drying method. Both vacuum drying and FHD processes were capable of removing bulk water. However, FHD was determined to provide additional drying capabilities, including partial removal of chemisorbed water from bayerite due to the higher temperatures during drying. In conclusion, the temperature threshold for partial dehydroxylation of the oxide layer was determined to be around 220°C, meaning any drying methods attempting to remove chemisorbed water must exceed 220°C.

chemisorbed water↗

Digital Twin Technology for Safety, Security, and Training in Spent Nuclear Fuel Handling

The increasing complexity of spent nuclear fuel handling requires significant resources to ensure safety, security, and personnel training. As nuclear facilities have continued to advance in scale and technology, the integration of digital tools has become indispensable. Among these tools, digital twins, which are virtual models of physical systems, are emerging as invaluable tools for enhancing safety protocols, security measures, and training in the nuclear sector. These models were conceptualized in the Industry 4.0 revolution. Digital twins can process data from physical systems in real time (by using sensors), include multiple code packages to enable simulations of different physics applications, and even implement artificial intelligence or machine learning techniques for advanced data processing. Despite the advantages that digital twins provide, challenges still exist regarding their widespread implementation. For instance, data used by a digital twin must be accurate to ensure that the digital twin is accurately tuned. Furthermore, if insecure digital twins are targeted by hackers, then they can pose serious risks to the security and safety of nuclear facilities.

Digital twins↗

Expected total counts for the Self-Interrogation Neutron Resonance Densitometry measurements of spent nuclear fuel

The Self-Interrogation Neutron Resonance Densitometry (SINRD) is a passive neutron technique that aims at a direct quantification of {sup 239}Pu in spent fuel assemblies by measuring the attenuation of the neutron flux in the energy region close to the 0.3 eV resonance of {sup 239}Pu. The {sup 239}Pu mass is estimated by calculating the SINRD signature, that is the ratio between the neutron counts in the fast energy region and around the 0.3 eV resonance region. The SINRD measurement approach in this study consisted in introducing a small neutron detector in the central guide tube of a PWR 17x17 fuel assembly. In order to measure the neutron flux in the energy regions defined in the SINRD signature, different detector types were used. The response of a bare {sup 238}U fission chamber is considered for the determination of the fast neutron flux, while other thermal-epithermal detectors wrapped in neutron absorbers are envisaged to measure the neutron flux around the resonance region. This paper provides an estimation of the total neutron counts that can be achieved with the detector types proposed for the SINRD measurement. In the first section a set of detectors are evaluated in terms of total neutron counts and sensitivity to the {sup 239}Pu content, in order to identify the optimal measurement configuration for each detector type. Then a study is performed to increase the total neutron counts by increasing the detector size. The study shows that the highest total neutron counts are achieved by using either {sup 3}He or {sup 10}B proportional counters because of the high neutron efficiency of these detectors. However, the calculations indicate that the biggest contribution to the measurement uncertainty is due to the measurement of the fast neutron flux. Finally, similar sensitivity to the {sup 239}Pu content is obtained by using the different detector types for the measurement of the neutron flux close to the resonance region. Therefore, the total neutron counts associated to each detector type will play a major role in the selection of the detector types used for the SINRD measurement. (authors)

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Status of the nuclear measurement stations for the process control of spent fuel reprocessing at AREVA NC/La Hague

Nuclear measurements are used at AREVA NC/La Hague for the monitoring of spent fuel reprocessing. The process control is based on gamma-ray spectroscopy, passive neutron counting and active neutron interrogation, and gamma transmission measurements. The main objectives are criticality and safety, online process monitoring, and the determination of the residual fissile mass and activities in the metallic waste remained after fuel shearing and dissolution (empty hulls, grids, end pieces), which are put in radioactive waste drums before compaction. The whole monitoring system is composed of eight measurement stations which will be described in this paper. The main measurement stations no. 1, 3 and 7 are needed for criticality control. Before fuel element shearing for dissolution, station no. 1 allows determining the burn-up of the irradiated fuel by gamma-ray spectroscopy with HP Ge (high purity germanium) detectors. The burn-up is correlated to the {sup 137}Cs and {sup 134}Cs gamma emission rates. The fuel maximal mass which can be loaded in one bucket of the dissolver is estimated from the lowest burn-up fraction of the fuel element. Station no. 3 is dedicated to the control of the correct fuel dissolution, which is performed with a {sup 137}Cs gamma ray measurement with a HP Ge detector. Station no. 7 allows estimating the residual fissile mass in the drums filled with the metallic residues, especially in the hulls, from passive neutron counting (spontaneous fission and alpha-n reactions) and active interrogation (fission prompt neutrons induced by a pulsed neutron generator) with proportional {sup 3}He detectors. The measurement stations have been validated for the reprocessing of Uranium Oxide (UOX) fuels with a burn-up rate up to 60 GWd/t. This paper presents a brief overview of the current status of the nuclear measurement stations. (authors)

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Risk Assessment of Salmonellosis from Consumption of Alfalfa Sprouts and Evaluation of the Public Health Impact of Sprout Seed Treatment and Spent Irrigation Water Testing

Abstract We developed a risk assessment of human salmonellosis associated with consumption of alfalfa sprouts in the United States to evaluate the public health impact of applying treatments to seeds (0–5‐log 10 reduction in Salmonella ) and testing spent irrigation water (SIW) during production. The risk model considered variability and uncertainty in Salmonella contamination in seeds, Salmonella growth and spread during sprout production, sprout consumption, and Salmonella dose response. Based on an estimated prevalence of 2.35% for 6.8 kg seed batches and without interventions, the model predicted 76,600 (95% confidence interval (CI) 15,400 – 248,000) cases/year. Risk reduction (by 5 ‐ to 7‐fold) predicted from a 1‐log 10 seed treatment alone was comparable to SIW testing alone, and each additional 1‐log 10 seed treatment was predicted to provide a greater risk reduction than SIW testing. A 3‐log 10 or a 5‐log 10 seed treatment reduced the predicted cases/year to 139 (95% CI 33 – 448) or 1.4 (95% CI <1 – 4.5), respectively. Combined with SIW testing, a 3‐log 10 or 5‐log 10 seed treatment reduced the cases/year to 45 (95% CI 10–146) or <1 (95% CI <1 – 1.5), respectively. If the SIW coverage was less complete (i.e., less representative), a smaller risk reduction was predicted, e.g., a combined 3‐log 10 seed treatment and SIW testing with 20% coverage resulted in an estimated 92 (95% CI 22 – 298) cases/year. Analysis of alternative scenarios using different assumptions for key model inputs showed that the predicted relative risk reductions are robust. This risk assessment provides a comprehensive approach for evaluating the public health impact of various interventions in a sprout production system.

60 APPLIED LIFE SCIENCES↗

Analytical Sensitivity Analysis of a Spent Nuclear Fuel Cask

Here, we report nuclear science and engineering is a field increasingly dominated by computational studies resulting from increasingly powerful computational tools. As a result, analytical studies, which previously pioneered nuclear engineering, are increasingly viewed as secondary or unnecessary. However, analytical solutions to reduced-fidelity models can provide important information concerning the underlying physics of a problem and aid in guiding computational studies. Similarly, there is increased interest in sensitivity analysis studies. These studies commonly use computational tools. However, providing a complementary sensitivity study of relevant analytical models can lead to a deeper analysis of a problem. This work provides the analytical sensitivity analysis of the one-dimensional (1D) cylindrical mono-energetic neutron diffusion equation using the forward sensitivity analysis procedure (FSAP) developed by Cacuci. Further, these results are applied to a reduced-fidelity model of a spent nuclear fuel cask, demonstrating how computational analysis might be improved with a complementary analytic sensitivity analysis.

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Review of passive corrosion studies of carbon steel in concrete in the context of disposal of HLW and spent fuel in Belgium

The Supercontainer (SC) design is the preferred option for the final disposal of high level nuclear waste and spent fuel in Belgium. The SC consists of a carbon steel overpack surrounded by a very thick concrete buffer, contained within a stainless steel envelope. In this highly alkaline environment of the annulus and under normal conditions (without the ingress of aggressive species), the carbon steel overpack will be protected by a passive oxide film, which is believed to result in very low and almost negligible uniform corrosion rates. This paper discusses the modeling efforts simulating the evolution of various parameters that can potentially influence the corrosion processes (temperature, pH, saturation degree and concentration of aggressive species). The outcome of the Belgian experimental program to study the passive uniform corrosion of carbon steel in concrete is also addressed. Long-term uniform corrosion rates are determined using different independent techniques (hydrogen gas measurements by means of manometric gas cells or pressure transducers, long-term passive current density measurements). (authors)

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Radionuclide inventory of vitrified waste after spent nuclear fuel reprocessing at La Hague

The primary aim of the present work was to determine the inventories of the radionuclides and stable elements in vitrified high-level waste produced at La Hague and delivered to Germany, which are of importance for long-term safety assessment of final repositories for radioactive wastes. For a subset of these radionuclides and stable elements, the inventories were determined - either by direct measurements or by involving established correlations - and reported by AREVA. This allowed verification of the validity of application of a model approach utilizing the data of burnup and activation calculations and auxiliary information on the reprocessing and vitrification process operated at La Hague. Having proved that such a model approach can be applied for prediction of inventories of actinides, fission and activation products in vitrified waste, the present work estimated the minimum, average and maximum inventories of the radionuclides, which are of importance for long-term safety assessment of final repositories for radioactive waste but were not reported by AREVA for delivered CSD-V canisters. The average and maximum inventories in individual CSD-V canisters predicted in the present approach were compared to the inventories predicted by Nagra for canisters with vitrified waste delivered from La Hague to Switzerland [1]. This comparison revealed a number of differences between these inventories despite the fact that the canisters delivered to Switzerland were produced in essentially the same way and from the common reprocessing waste stock as CSD-V canisters delivered to Germany. Therefore, a further work is required in order to identify the reason for the discrepancy in the present estimation versus the Nagra estimation [1]. Such a work should also address the recommendation by the international peer review of the Safety Report of the Project Opalinus Clay to obtain estimates of the inventories of long-lived mobile radionuclides (such as {sup 14}C, {sup 36}Cl, {sup 79}Se, and {sup 129}I), which contribute most to the dose estimates in the radiological safety assessments, if possible, in agreement with other countries with similar waste streams in order for a coordinated set of data to be generated [2]. Since vitrified waste from reprocessing of spent nuclear fuel at La Hague was delivered to several countries - Belgium, France, Germany, Japan, Netherlands, and Switzerland - an international effort can be recommended. (authors)

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End-to-end calculation of the radiation characteristics of VVER-1000 spent fuel assemblies

The results of end-to-end calculation of the radiation characteristics of VVER-1000 spent nuclear fuel are presented. Details of formation of neutron and gamma-radiation sources are analyzed. Distributed sources of different types of radiation are considered. A comparative analysis of calculated radiation characteristics is performed with the use of nuclear data from different ENDF/B and EAF files and ANSI/ANS and ICRP standards.

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