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Spent Nuclear Fuel and High-Level Radioactive Waste Inventory Report

This report provides information on the inventory of commercial spent fuel (SNF) and high-level radioactive waste (HLW) in the United States, as well as non-commercial SNF and HLW in the U.S. Department of Energy (DOE) complex. Actual or estimated quantitative values for current inventories are provided along with inventory forecasts derived from examining different future commercial nuclear power generation scenarios. The report also includes select information on the characteristics associated with the wastes examined (e.g., type, packaging, heat generation rate, decay curves). This report was produced for the U.S. Department of Energy (DOE) to support various analyses on options for storage and transport of SNF and HLW and sponsored by DOE’s Office of Spent Fuel and Waste Disposition (SFWD). The report draws from and complements a previously issued report, Fuel Cycle Potential Waste Inventory for Disposition, developed for DOE’s Used Nuclear Fuel Research & Development Campaign. The current report is not intended as a revision to either Fuel Cycle Potential Waste Inventory for Disposition or Evaluation of Options for Permanent Geologic Disposal of Spent Nuclear Fuel and High-Level Radioactive Waste in Support of a Comprehensive National Nuclear Fuel Cycle Strategy from which some underlying data is used as referenced in the current report. Rather, this report is intended as a stand-alone report providing estimates of current and projected SNF and HLW inventory and has been generated for SFWD planning purposes. This is a technical report that does not take into account contractual limitations or obligations under the Standard Contract for Disposal of Spent Nuclear Fuel and/or High-Level Radioactive Waste (Standard Contract) (10 CFR Part 961). For example, under the provisions of the Standard Contract, spent nuclear fuel in multi-assembly canisters is not an acceptable waste form, absent a mutually agreed to contract amendment. To the extent discussions or recommendations in this report conflict with the provisions of the Standard Contract, the Standard Contract governs the obligations of the parties, and this report in no manner supersedes, overrides, or amends the Standard Contract. This report reflects technical work which could support future decision making by DOE. No inferences should be drawn from this report regarding future actions by DOE, which are limited both by the terms of the Standard Contract and a lack of Congressional appropriations for the Department to fulfill its obligations under the Nuclear Waste Policy Act including licensing and construction of a spent nuclear fuel repository.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis with the ORIGEN Module of PNAR Spent Fuel Measurements for Nuclear Safeguards Applications

This report documents the analysis of the Passive Neutron Albedo Reactivity (PNAR) measurements for 23 boiling water reactor spent fuel assemblies that were performed in Finland under Action Sheet 65, which is an international collaboration on spent fuel safeguards verification methods in the context of the Finnish spent fuel encapsulation/repository system. PNAR measures the passive neutron and gamma emission rates from each of the spent fuel assemblies like a Fork detector, and it also measures the PNAR ratio, which is expected to correlate with the net neutron multiplication of the measured fuel assembly. The analysis was performed with the Oak Ridge Isotope Generation and Depletion (ORIGEN) Data Analysis Module, which was originally developed for predicting Fork detector spent fuel measurement signals in real time and has been integrated into the Integrated Review and Analysis Package developed by Euratom and the International Atomic Energy Agency. The module includes the ORIGEN burnup analysis code and integrates detector response functions pregenerated using the MCNP Monte Carlo transport code to predict the detector signals in several seconds per assembly. In this study, new response functions specific to the analyzed PNAR measurements were generated for the ORIGEN Module. The study also analyzes the impact of using detailed fuel design and operation information vs. standard safeguards information on the results calculated with the ORIGEN Module. Using detailed information reduced the standard deviation of the relative differences between calculated and measured neutron count rates among the 23 assemblies from ~10% to ~4%. The results obtained using standard safeguards information for these PNAR measurements were similar to those obtained for the Fork detector. A clear trend was found between the calculated net neutron multiplications and the measured PNAR ratios of the 23 assemblies. An uncertainty assessment of the calculations was also performed to estimate the potential impact of the accuracy and the completeness of declaration information on the calculated results for the count rates and net neutron multiplications. The ORIGEN Module predictions for PNAR signals and net neutron multiplication are expected to directly support the safeguards inspectors’ efforts to verify operator declarations of a spent fuel assembly in real time in safeguards practices.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fork Experiments in the Hot Cell Using Spent Fuel Rods for International Nuclear Safeguards

This work leveraged the rare availability of 25 full-length pressurized water reactor spent fuel rods and 1 irradiated mixed-oxide rod at an Oak Ridge National Laboratory hot cell. This was done to collect measurement data with two Fork detectors to assess the detectors’ capability of verifying operator declaration data and detecting partial defects in spent fuel, which are the two primary goals of international safeguards on spent nuclear fuel. The data can also be used to benchmark the ORIGEN module, which has been adopted in the International Atomic Energy Agency’s (IAEA’s)/European Atomic Energy Community’s (Euratom’s) Integrated Review and Analysis Program to predict the Fork detector count rates in real time. In this project, the authors first calibrated two Fork detectors—a standard one and a modified one—by using known strong neutron and gamma sources. Then, the authors measured all 26 fuel rods at multiple locations along the length. The fuel rods were then assembled into three arrays—2 × 2, 3 × 3, and 5 × 5—by using specially designed support grids to mimic fuel assemblies and measure the arrays with both detectors. For the 5 × 5 array, 4 and 8 fuel rods of the array were replaced in two separate cases with short stainless-steel rods to mimic two partial defect scenarios, and the arrays were measured before and after the replacements. Polyethylene blocks were used in this experiment to mimic water. The results show that the Fork detectors were able to verify operator declarations and detect partial defects in spent fuel, and the authors were the first to demonstrate this through experiments. A discovery was also made that determined the root cause of the nonlinear response to gamma dose in the ion chambers used in IAEA and Euratom’s Fork detectors. After the experiments, both detectors were retrieved from the hot cell for future use. The data collected in this project will be used in a parallel International Nuclear Safeguards Engagement Program (INSEP) project to enhance the safeguards in the Finnish spent fuel encapsulation plant, and the data will be useful to other projects in the future given the increased safeguards needs due to spent fuel transfer and disposal activities worldwide.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

ADDITIVE MANUFACTURING AND REGULATORY TESTING OF CANISTERS FOR SPENT NUCLEAR FUEL MANAGEMENT

The back end of the fuel cycle focuses on the interim storage, transportation, and final disposition of the spent nuclear fuel from nuclear reactors. Commercial light water nuclear power stations across the United States operate with fuel assemblies being irradiated for up to 6 years (planned) in the reactor pressure vessel. After their planned irradiation, the fuel assemblies are moved to a spent fuel pool within the facility complex. After the spent nuclear fuel is removed from the fuel pool, it is typically inserted into a welded metal canister that can be transferred between overpacks for storage, transportation and possibly disposal. Most dry storage systems being used by industry today use dual purpose canisters (DPCs), designed for use in storage and transportation overpacks, but not specifically designed for disposal. Triple purpose-canisters, designed for disposal in addition to storage and transportation, have also been researched. Traditional manufacturing methods for spent fuel canisters involve fusion welding along the length or circumference of the canister which results in high tensile residual stresses in the joint weld zone (WZ) and heat affected zone (HAZ). In this paper, spent fuel canister designs were printed by wire arc additive manufacturing (AM) using the 316L SS welding wire to demonstrate: 1. Feasibility of spent nuclear fuel canister fabrication using this advanced manufacturing method, 2. Dynamic response of the additive manufacture canister design when subjected to the federally mandated Normal Conditions of Transport (NCT) and Hypothetical Accident Conditions (HAC) physical tests for Type B packages. This paper will focus on the canister printing design and structural tests. The AM 3D printed design, regulatory testing, and post-test evaluation of the canister tested to the 10 CFR 71.71 and 10 CFR 71.73 requirements will be presented. One AM canister design was subjected to the penetration, free drop, and puncture test. Before and after the dynamic structural tests, the AM canister design was scanned with a handheld scanner to capture a 3D CAD geometry to compare to the 3D printed canister design in the deformed shape. The scanned geometry was sectioned in areas with deformation and the cross-section profile was measured to determine accurate and repeated results of the deformed shape of the AM canister design.

Martinez, Oscar↗

An Alternative to the Continued Accumulation of Separated Plutonium in Japan: Dry Cask Storage of Spent Fuel

As of the end of 2017, Japan had a stockpile of 48 tons of separated plutonium. It will take more than a decade for Japan to convert most of that plutonium into “mixed-oxide” (MOX) fuel and load it into power reactors licensed to use such fuel. This is a very costly program. Including the cost of reprocessing, MOX fuel costs about ten times more than the low-enriched-uranium fuel that otherwise would be used by these reactors. Yet Japan has a policy to start separating more plutonium from spent reactor fuel as soon as the Rokkasho Reprocessing Plant can be put into operation – currently projected for 2021 after 24 years of delay due to a variety of technical problems and upgrades in safety requirements. Japan’s government remains committed to this costly and troubled program primarily because, pending the availability of additional spent-fuel storage space on or off site, reprocessing is seen as the only way to get spent fuel out of reactor pools that are getting full. Because of concerns about the safety of dense-packed spent-fuel pools, however, the prefectures and towns hosting Japan’s power reactors are beginning to accept on-site storage of spent fuel in dry casks. This is the option the United States and many other countries chose after they cancelled their reprocessing programs and their powerplant pools filled up. Its increasing availability in Japan, if backed by a determined policy to accelerate its introduction, should make it possible to cancel reprocessing in Japan as well.

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Further Evaluation of the Neutron Resonance Transmission Analysis (NRTA) Technique for Assaying Plutonium in Spent Fuel

This is an end-of-year report (Fiscal Year (FY) 2011) for the second year of effort on a project funded by the National Nuclear Security Administration's Office of Nuclear Safeguards (NA-241). The goal of this project is to investigate the feasibility of using Neutron Resonance Transmission Analysis (NRTA) to assay plutonium in commercial light-water-reactor spent fuel. This project is part of a larger research effort within the Next-Generation Safeguards Initiative (NGSI) to evaluate methods for assaying plutonium in spent fuel, the Plutonium Assay Challenge. The second-year goals for this project included: (1) assessing the neutron source strength needed for the NRTA technique, (2) estimating count times, (3) assessing the effect of temperature on the transmitted signal, (4) estimating plutonium content in a spent fuel assembly, (5) providing a preliminary assessment of the neutron detectors, and (6) documenting this work in an end of the year report (this report). Research teams at Los Alamos National Laboratory (LANL), Lawrence Berkeley National Laboratory (LBNL), Pacific Northwest National Laboratory (PNNL), and at several universities are also working to investigate plutonium assay methods for spent-fuel safeguards. While the NRTA technique is well proven in the scientific literature for assaying individual spent fuel pins, it is a newcomer to the current NGSI efforts studying Pu assay method techniques having just started in March 2010; several analytical techniques have been under investigation within this program for two to three years or more. This report summarizes work performed over a nine month period from January-September 2011 and is to be considered a follow-on or add-on report to our previous published summary report from December 2010 (INL/EXT-10-20620).

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A novel application of cosmic rays for spent nuclear fuel monitoring - 15738

Monitoring nuclear waste and controlling spent nuclear fuel at its source is one of the main strategies to minimize the risks of nuclear proliferation and reduce potential homeland threats. Storage of high level waste from a fission reactor typically involves placing spent fuel in sealed dry casks. After the spent nuclear fuel has been placed inside the dry cask, the cask is welded, not allowing for visual inspection. Conventional methods for examining the interior of materials e.g., X-rays, are limited by the fact that they cannot penetrate very dense well-shielded objects. Instead, cosmic ray muons have the potential to allow for assessment of spent nuclear fuel stored within sealed dense dry casks. Objectives: 1.Exploit the ability of cosmic ray muons to penetrate high density materials allowing the distribution of materials within the object to be inferred from the muon tracks. 2. Develop a monitoring system that tracks the path of cosmic ray muons, including their deflection and attenuation, to identify the contents of a closed dry cask. Methods: - Monte-Carlo simulations using Geant4; - Bayesian decision theory for signal classification; - Wavelet analysis for noise cancellation; - Chaotic Neural Networks for signal encryption. Results: 1. Preliminary statistical analysis proved that the method is feasible and has the ability to identify the presence of spent nuclear fuel in a dry cask. 2. Using monoenergetic muons, a dry cask with one fuel assembly missing can be correctly identified with error rate <1%. Broader merit: Once completed, the proposed project for cosmic ray muon transport will enable a new and potentially transformative approach towards efficient, inexpensive and remote cosmic ray muon applications in archaeology, medicine and safeguarding of nuclear materials.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A New Safeguards Technique for Spent Fuel Verification in Dry Storage by Using He-4 Detectors - 18262

It is demanded to find key issues and critical paths for verifying and monitoring a spent nuclear fuel cask or storage with a purpose of non-proliferation of nuclear weapon. However, unfortunately there are no reliable methods to verify the containment in a spent nuclear fuel cask or storage. Therefore, research and development (R and D) has been continuously required to develop new and alternative technologies for searching and verifying undeclared nuclear materials, activities, and facilities. Therefore, the present authors have developed a new safeguards technique of passively scanning a spent fuel cask or storage using pressurized He-4 scintillation neutron detectors. A new approach is to quickly verify content in a spent nuclear fuel cask or presence of all special nuclear materials in unknown packages by comparing experimental and computational results. For that, the present authors have developed a new algorithm and user-interface coupled ORIGEN-ARP and MCNP codes, and the prototype safeguards apparatus employing the array of He-4 fast neutron detectors has been designed, built, and tested. The feasibility test of this new apparatus has been performed with Cf-252 neutron sources and the laboratory scale model cask, minimized by a factor of ten compared to the actual dimension of a KN-21 cask. This technique has several advantages over current methods based on neutron and gamma detection; (1) incident neutron energy information is preserved, (2) disturbance of gamma-ray is excellently rejected (discriminated), and (3) much higher neutron counts and operational cost and space-effectiveness are expected since no moderator is required for fast neutrons. The final goal of this study will (1) conduct a prototype instrument and employ it to monitor a nuclear spent fuel cask or storage at a commercial nuclear power reactor facilities, (2) use spectral-specific measurement data to show proof of concept for measurable data successfully converted to quantifiable signatures, such as diversion/removal of fuel, and maintenance of fuel and cask integrity of fuel, and (3) develop a cask imaging capability. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Regulatory Basis for Dry Spent Nuclear Fuel Storage Canister Inspections

Nuclear power plants in the United States began moving Spent Nuclear Fuel (SNF) from wet storage to dry storage in Independent Spent Fuel Storage Installations (ISFSIs) in 1986 at Surry station in Virginia. Dry storage represented an innovative solution to the problem created by the U.S. government's failure to fulfill its obligation to begin removing SNF from power plant sites. Today, about 70 ISFSIs have been placed into operation on the sites of current, or former nuclear power plants. There are currently over 2,200 SNF dry storage systems (DSSs) in service at these locations. Thirteen of these ISFSIs are located at sites with no operating reactor, and this number is due to increase in the coming years. Operating nuclear power stations use ISFSI storage to maintain wet storage capacity for recently discharged SNF. Permanently shutdown nuclear power plants use ISFSI storage to allow decommissioning and dismantlement of the power plant structures, systems, and components. The U.S. Nuclear Regulatory Commission (NRC) regulates the licensing, construction, and operation of ISFSIs under Title 10 of the U.S. Code of Federal Regulations, Energy, Part 72, Licensing Requirements for the Independent Storage of Spent Nuclear Fuel, High-Level Radioactive Waste, and Reactor-Related Greater than Class-C Waste (10 CFR 72). When the regulations in 10 CFR 72 were created around 1980, 20 years was chosen by the NRC as the license term for a specific ISFSI license and later, for a DSS Certificate of Compliance (CoC). Twenty years was, at the time, believed to be a sufficient time period for on-site interim dry storage of spent nuclear fuel before the U.S. government began moving the spent fuel away from the plant site for final disposal. Little, if any consideration was given to providing a regulatory framework for extending ISFSI licenses and DSS CoCs beyond 20 years at that time. However, shortly after the turn of the century, with still no federal program for removing SNF from reactor sites on the near-term horizon it became apparent that most DSSs would be required to remain in service at the ISFSIs beyond the initial 20-year license term. Operation beyond the original license term requires the specific license or the DSS CoC (used at a general license ISFSI) to be renewed. The requirements for renewal of a specific ISFSI license or a DSS CoC include addressing age-related degradation of structures, systems, and components that perform or support safety functions. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Regulatory perspective of boiling water reactor peak reactivity credit in spent fuel storage and transportation - 14592

The U.S. Nuclear Regulatory Commission (NRC) performs reviews of applications for spent nuclear fuel transportation packages and storage casks to ensure pertinent safety regulations are met. Among other acceptance criteria, these regulations require that the package be subcritical under a variety of normal, off-normal and accident conditions. Currently, all spent nuclear fuel transportation packages and storage casks assume fresh fuel (i.e., the fuel is unirradiated) in their criticality safety analyses for boiling water reactor (BWR) fuels. Reviews using this conservative assumption are less complex. The fresh fuel assumption for BWR fuel does not allow the presence of gadolinium (often called the 'fresh fuel no-Gad' assumption), an integral burnable absorber present in nearly all BWR fuel assemblies. More recently, applicants began requesting credit for the reactivity reduction due to depletion. This credit is commonly referred to as 'burnup credit' (BUC). As of today, NRC recommends that only analyses for Pressurized Water Reactor (PWR) spent fuel implement BUC. This is due to the fact there is limited directly applicable data available to benchmark codes for depletion and reactivity calculations for BWR BUC analyses, and determining the most reactive irradiation conditions is much less straightforward than for PWR BUC analyses. Similar to what was done for PWR BUC, the NRC staff and its contractors have begun identifying and prioritizing significant technical issues so that a technical basis for the allowance of BWR BUC can be developed. BWR fuel exhibits a peak in reactivity where initial gadolinium is depleted. Crediting burnup at this point is generally referred to as using a 'peak reactivity method'. This is a conservative approach and a method routinely used in BWR spent fuel pool criticality analyses. NRC is implementing a two-phased approach in investigating BWR BUC. Phase 1 investigates peak reactivity credit and Phase 2 evaluates BUC at a typical discharge exposure. This paper discusses peak reactivity credit and its history in regulatory analyses, challenges the NRC expects in reviewing an application requesting peak BWR reactivity credit for a spent fuel transportation package or storage cask, the work that is being performed by NRC contractors to address these challenges, and future work on peak reactivity credit and full BWR BUC. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Safeguards-by-Design: Guidance for Independent Spent Fuel Dry Storage Installations (ISFSI)

This document summarizes the requirements and best practices for implementing international nuclear safeguards at independent spent fuel storage installations (ISFSIs), also known as Away-from- Reactor (AFR) storage facilities. These installations may provide wet or dry storage of spent fuel, although the safeguards guidance herein focuses on dry storage facilities. In principle, the safeguards guidance applies to both wet and dry storage. The reason for focusing on dry independent spent fuel storage installations is that this is one of the fastest growing nuclear installations worldwide. Independent spent fuel storage installations are typically outside of the safeguards nuclear material balance area (MBA) of the reactor. They may be located on the reactor site, but are generally considered by the International Atomic Energy Agency (IAEA) and the State Regulator/SSAC to be a separate facility.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Evaluation of PBR Spent Fuel Criticality and Dose Rate Compliance for Storage and Transportation

Spent tri-structural isotropic (TRISO)–based fuels have a strong track record in storage and transportation without documented incidents. This work seeks to reduce uncertainty to aid in more informed spent fuel management of TRISO-based fuels by modeling both fresh and spent pebble bed reactor (PBR) fuel and comparing the results to the regulatory standards from 10 CFR 71. SCALE was used for all modeling due to it having fast and accurate methods for handling PBR fuel modeling, as well as having an efficient method for shielding calculations in monaco with automated variance reduction using importance calculations (MAVRIC), which utilizes the consistent adjoint-driven importance sampling (CADIS) and the forward-weighted consistent adjoint-driven importance sampling (FW-CADIS) methods. KENO-VI was used for all criticality calculations, TSUNAMI was used for uncertainty quantification on k-effective, TRITON and the Oak Ridge isotope generation code (ORIGEN) were both used for depletion of the fuel, and MAVRIC was used for shielding calculations. For criticality assessments, this study focused on the requirement that the value of the neutron multiplication factor, k-effective (k-eff), would not exceed a peak value of 0.95, including uncertainty, with 95% confidence. Criticality was initially examined by modeling fresh fuel from three different designs—HTR-10 fuel, PBMR-400 fuel, and demonstration fuel representative of a TRISO-fueled modern high-temperature gas reactor (HTGR) design, henceforth referred to as Demo HTGR—and placing them into various sized containers with conditions described in 10 CFR 71 to quantify the peak k-eff state. When the peak value of 0.95 k-eff was exceeded, mitigation methods were examined in those scenarios. Burnup credit, pebble displacement in areas of strong neutron multiplication, and random pebble replacement using pebbles of various compositions and replacement fractions were examined. In summary, the criticality of PBR fuels can be well accounted for by restricting container size, taking credit for burnup, or by displacing/replacing pebbles. Uncertainty of the k-eff due to nuclear data uncertainties was recorded at ~0.6644%Δk/k, or roughly 664% mil (pcm). The nuclear data–induced uncertainty was relatively small and should not require significant modification in the design to be accounted for. Revisions to the evaluated nuclear data file values have been shown to have a larger impact than nuclear data–induced uncertainty. For dose rate aspects, U.S. Nuclear Regulatory Commission regulations require a maximum dose rate of 10 millirem per hour (mrem/h) at 2 meters. In examining the dose rate behavior of spent PBR fuel, the representative Demo HTGR fuel was modeled exclusively due to it possessing the highest target burnup of the examined fuels. Equilibrium cycle modeling methods were used to produce a higher-fidelity discharge isotopic composition than simple assumptions, such as reflected pebbles. The discharge composition was used as a source term in the fixed-source transport shielding calculations, and dose rates were calculated at 2 m for the shortest possible cooling time. The low concentration of fuel material led to dose rates that were in line with regulatory limits, despite the high burnup when compared to traditional light water reactor fuels. In conclusion, the methods employed in this study would require more work to further verify and validate and are limited to the criticality and dose rate analyses performed.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Integral nuclear data validation using experimental spent nuclear fuel compositions

Measurements of the isotopic contents of spent nuclear fuel provide experimental data that are a prerequisite for validating computer codes and nuclear data for many spent fuel applications. Under the auspices of the Organisation for Economic Co-operation and Development (OECD) Nuclear Energy Agency (NEA) and guidance of the Expert Group on Assay Data of Spent Nuclear Fuel of the NEA Working Party on Nuclear Criticality Safety, a new database of expanded spent fuel isotopic compositions has been compiled. The database, Spent Fuel Compositions (SFCOMPO) 2.0, includes measured data for more than 750 fuel samples acquired from 44 different reactors and representing eight different reactor technologies. Measurements for more than 90 isotopes are included. This new database provides data essential for establishing the reliability of code systems for inventory predictions, but it also has broader potential application to nuclear data evaluation. Furthermore, the database, together with adjoint based sensitivity and uncertainty tools for transmutation systems developed to quantify the importance of nuclear data on nuclide concentrations, are described.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Preliminary study on direct recycling of spent PWR fuel in PWR system

Preliminary study on direct recycling of PWR spent fuel to support SUPEL (Straight Utilization of sPEnt LWR fuel in LWR system) scenario has been conducted. Several spent PWR fuel compositions in loaded PWR fuel has been evaluated to obtain the criticality of reactor. The reactor can achieve it criticality for U-235 enrichment in the loaded fresh fuel is at least 4.0 a% with the minimum fraction of the spent fuel in the core is 15.0 %. The neutron spectra become harder with the escalating of U-235 enrichment in the loaded fresh fuel as well as the amount of the spent fuel in the core.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An Evaluation of a Neutron Time Correlated Interrogation Method for Measurement of Fissile Content in Research Reactor Spent Fuel Assemblies

There are many research reactors worldwide that have been, or are being converted from the use of high enrichment uranium (HEU) to low enrichment uranium (LEU, < 20% enriched). The verification of fissile content and initial enrichment of the spent fuel is needed for the effective safeguards of the fuel. The advanced experimental fuel counter (AEFC) was developed for the measurement of spent fuel rods and assemblies from research reactors for safeguards verification. This measurement system contains components for active neutron interrogation, passive neutron totals counting, neutron coincidence counting, and gross gamma-ray counting. This report presents the first application of the time correlated interrogation technique for the measurement of the 235 U content in research reactor spent fuel assemblies. The technique, called time correlated induced fission (TCIF), uses a 252 Cf neutron source to irradiate the fuel assembly, and the subsequent induced fission events in the fissile material are measured by coincidence counting. The doubles rates are enhanced by having the neutron trigger events from both the 252 Cf source and the induced fission neutrons in the same time gate in the coincidence analysis. The average neutrons per fission of the 252 Cf source is 3.76 and the induced fission neutrons for 235 U is 2.44, so the number of neutrons that are produced is higher than for random neutron interrogation. This high effective neutron number increases the multiplicity counting rates and reduces the statistical error. The background coincidence counts from the 252 Cf are reduced by the water in the sample cavity and the polyethylene surrounding the 3 He detector tubes. This method of active neutron interrogation has been applied to the measurement of spent research reactor (IRT) fuel assemblies. The advanced experimental fuel counter (AEFC) was used to compare the TCIF method with the typically used AmLi neutron interrogation source that emits neutrons that are random in time. The statistical uncertainty for the use of the random neutron source (AmLi) and the time correlated source ( 252 Cf) for spent fuel interrogations was evaluated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An Alternative Conceptual Model for the Spent Nuclear Fuel–Water Interaction in Deep Geologic Disposal Conditions

For the long-term safety assessment of direct disposal of spent nuclear fuel in deep geologic repositories, knowledge on the radionuclide release rate from the UO 2 matrix is essential. This work provides a conceptual model to explain the results of leaching experiments involving used nuclear fuel or simulant materials in confirmed reducing conditions. Key elements of this model are: direct effect of radiation from radiolytic species (including defects and excited states) in the solid and in the first water layers in contact with its surface; and excess H 2 may be produced due to processes occurring at the surface of the spent fuel and in confined water volumes, which may also play a role in keeping the spent fuel surface in a reduced state. The implication is that the fractional radionuclide release rate used in most long-term safety assessments (10 -7 year -1 ) is over estimated because it assumes that there is net UO 2 oxidation caused by radiolysis, in contrast with the alternative conceptual model presented here. Furthermore, conventional water radiolysis models and radiation chemical yields published in the literature are not directly applicable to a heterogeneous system such as the spent fuel–water interface. Suggestions are provided for future work to develop more reliable models for the long-term safety assessment of spent nuclear fuel disposal.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DEVELOPMENT OF METHODOLOGY AND FIELD DEPLOYABLE SAMPLING TOOLS FOR SPENT NUCLEAR FUEL INTERROGATION IN LIQUID STORAGE

This project developed methodology and field deployable tools (test kits) to analyze the chemical and microbiological condition of the fuel storage medium and determine the oxide thickness on the spent fuel basin materials. The overall objective of this project was to determine the amount of time fuel has spent in a storage basin to determine if the operation of the reactor and storage basin is consistent with safeguard declarations or expectations. This project developed and validated forensic tools that can be used to predict the age and condition of spent nuclear fuels stored in liquid basins based on key physical, chemical and microbiological basin characteristics. Key parameters were identified based on a literature review, the parameters were used to design test cells for corrosion analyses, tools were purchased to analyze the key parameters, and these were used to characterize an active spent fuel basin, the Savannah River Site (SRS) L-Area basin. The key parameters identified in the literature review included chloride concentration, conductivity, and total organic carbon level. Focus was also placed on aluminum based cladding because of their application to weapons production. The literature review was helpful in identifying important parameters, but relationships between these parameters and corrosion rates were not available. Bench scale test systems were designed, operated, harvested, and analyzed to determine corrosion relationships between water parameters and water conditions, chemistry and microbiological conditions. The data from the bench scale system indicated that corrosion rates were dependent on total organic carbon levels and chloride concentrations. The highest corrosion rates were observed in test cells amended with sediment, a large microbial inoculum and an organic carbon source. A complete characterization test kit was field tested to characterize the SRS L-Area spent fuel basin. The sampling kit consisted of a TOC analyzer, a YSI multiprobe, and a thickness probe. The tools were field tested to determine their ease of use, reliability, and determine the quality of data that each tool could provide. Characterization was done over a two day period in June 2011, and confirmed that the L Area basin is a well operated facility with low corrosion potential.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Assessing the Feasibility of Using Neutron Resonance Transmission Analysis (NRTA) for Assaying Plutonium in Spent Fuel Assemblies

Neutron resonance transmission analysis (NRTA) is an active-interrogation nondestructive assay (NDA) technique capable of assaying spent nuclear fuel to determine plutonium content. Prior experimental work has definitively shown the technique capable of assaying plutonium isotope composition in spent-fuel pins to a precision of approximately 3%, with a spatial resolution of a few millimeters. As a Grand Challenge to investigate NDA options for assaying spent fuel assemblies (SFAs) in the commercial fuel cycle, Idaho National Laboratory has explored the feasibility of using NRTA to assay plutonium in a whole SFA. The goal is to achieve a Pu assay precision of 1%. The NRTA technique uses low-energy neutrons from 0.1-40 eV, at the bottom end of the actinide-resonance range, in a time-of-flight arrangement. Isotopic composition is determined by relating absorption of the incident neutrons to the macroscopic cross-section of the actinides of interest in the material, and then using this information to determine the areal density of the isotopes in the SFA. The neutrons used for NRTA are produced using a pulsed, accelerator-based neutron source. Distinguishable resonances exist for both the plutonium (239,240,241,242Pu) and uranium (235,236,238U) isotopes of interest in spent fuel. Additionally, in this energy range resonances exists for six important fission products (99Tc, 103Rh, 131Xe, 133Cs, 145Nd, and 152Sm) which provide additional information to support spent fuel plutonium assay determinations. Based on extensive modeling of the problem using Monte Carlo-based simulation codes, our preliminary results suggest that by rotating an SFA to acquire four symmetric views, sufficient neutron transmission can be achieved to assay a SFA. In this approach multiple scan information for the same pins may also be unfolded to potentially allow the determination of plutonium for sub-regions of the assembly. For a 17 ? 17 pressurized water reactor SFA, a simplistic preliminary analysis indicates the mass of 239Pu may be determined with a precision on the order of 5%, without the need for operator-supplied fuel information or operational histories. This paper will present our work to date on this topic, indicate our preliminary findings for a conceptual assay approach, discuss resilience against spoofing, and outline our future plans for evaluating the NRTA technique for SFA plutonium determination.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗