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The objective of this presentation is to identify where nuclear materials are present and what types of measurement techniques might be applicable for a given material.
Nuclear energy is a key component of a global, low-carbon energy future. One of the challenges facing large-scale deployment of nuclear power is the long-term disposition of used nuclear fuel. Due to the political and technical challenges of siting deep geologic storage facilities, reprocessing of used nuclear fuel is desirable to reduce the total volume and decay heat of waste requiring long-term storage, enabling efficient usage of geologic storage repositories. However nuclear fuel reprocessing is complicated by intense multi-component radiation fields that degrade solvent systems that are used for this purpose. Resulting radiolytic degradation can result in reduced performance over time, and generation of additional waste. Thus, an understanding of the radiation-induced chemistry of these reprocessing solvent systems is crucial to for the development of new, radiation-resistant processes for efficiently treating used nuclear fuel. Controlled irradiation experiments combined with high-performance chromatography and mass spectrometry have provided comprehensive knowledge of radiolytic degradation pathways and kinetics, which is needed to predict the effect of radiation-induced chemistry on the performance of the nuclear fuel reprocessing technology. This talk will give an overview of recent progress in research on the radiation chemistry of fuel reprocessing molecules conducted by the Idaho National Laboratory Center for Radiation Chemistry Research (CR2) in conjunction with the Molecular Mass Spectrometry and Chromatography group.
The nuclear fuel cycle presents formidable 10 30+ multiscale challenges for high-efficiency spectroscopic sensing of alpha-neutron-fission radiation signatures amidst extreme gamma-beta radiation backgrounds at various stages of the cycle; it involves diverse arenas ranging from continuous/pulsed power production, security/safeguards, spent fuel, environmental remediation, and personnel health-dosimetry. This paper discusses the novel tensioned metastable fluid detector (TMFD) sensor technology. It discusses the results of studies demonstrating extreme (10 4 Sv/h) gamma-beta field blind high intrinsic efficiencies (80–100%) for neutron-alpha-fission radiation spectrometric detection. Example studies discussed in this paper include Neutron detection with spectroscopy; H*10 neutron radiation dosimetry upwards from ultra-low10 −2 µSv/h levels; Air and/or liquid-borne trace (10 –3 Bq/mL) quantity, 1 keV energy resolved alpha/fission spectroscopy for Rn/Po/U/Pu/Am environmental isotope assays at 106:1 (β:α) ratios; Directional-position enabled extended standoff tracking of neutron emitting (shielded/unshielded) special nuclear materials while stationary or moving at highway speeds; and, U.S. Department of Energy nuclear complex wide nuclear waste reprocessing, criticality safety, health physics, and environmental applications.
Spent nuclear fuel contains heavy element fission products that must be separated for effective reprocessing for a safe and sustainable nuclear fuel cycle. 93 Zr and 99 Tc are high-yield fission products that co-transport in liquid-liquid extraction processes. Here we seek atomic-level information of this co-extraction process, as well as fundamental knowledge about Zr IV (and Hf IV ) aqueous speciation in the presence of topology-directing ligands such as pertechnetate (TcO 4 – ) and non-radioactive surrogate perrhenate (ReO 4 – ). In this context, we show that the flat tetrameric oxyhydroxyl-cluster [M IV 4 (OH) 8 (H 2 O) 16 ] 8+ (and related polymers) is dissociated by perrhenate/pertechnetate to yield isostructural dimers, M 2 (OH) 2 (XO 4 – ) 6 (H 2 O) 6 • 3H 2 O (M=Zr/Hf IV ; X=Re/Tc VII ), elucidated by single-crystal X-ray diffraction. We used these model compounds to understand the pervasive 93 Zr- 99 Tc coextraction with further speciation studies in water, nitric acid, and tetrabutylphosphate (TBP) -kerosene; where the latter two media are relevant to nuclear fuel reprocessing. SAXS (small angle X-ray scattering), compositional evaluation, and where experimentally feasible, ESI-MS (electrospray ionization mass spectrometry) showed that perrhenate/pertechnetate influence Zr/Hf IV -speciation in water. Here, in Zr-XO 4 solvent extraction studies to simulate fuel reprocessing, we provide evidence that TcO 4 – enhances extraction of Zr IV , and compositional analysis of the extracted metal-complexes (Zr-ReO 4 study) is consistent with the crystallized Zr IV 2 (OH) 2 (Re VII O 4 – ) 6 (H 2 O) 6 •dimer.
Here, nuclear fuel cycle and nuclear waste disposal decisions are technologically coupled. However, current nuclear fuel cycle simulators lack dynamic repository performance analysis due to the computational burden of high-fidelity hydrolgic contaminant transport models. The Cyder disposal environment and repository module was developed to fill this gap. It implements medium-fidelity hydrologic radionuclide transport models to support assessment appropriate for fuel cycle simulation in the Cyclus fuel cycle simulator. Rapid modeling of hundreds of discrete waste packages in a geologic environment is enabled within this module by a suite of four closed form models for advective, dispersive, coupled, and idealized con- taminant transport: a Degradation Rate model, a Mixed Cell model, a Lumped Parameter model, and a 1-D Permeable Porous Medium model. A summary of the Cyder module, its timestepping algorithm, and the mathematical models implemented within it are presented. Additionally, parametric demonstrations simulations performed with Cyder are presented and shown to demonstrate functional agreement with parametric simulations conducted in a standalone hydrologic transport model, the Clay Generic Disposal System Model developed by the Used Fuel Disposition Campaign Department of Energy Office of Nuclear Energy.
The nuclear fuel cycle in the United States, specifically the back end portion, remains an unresolved and persistent issue. In comparison with the technical aspects of many different fuel cycles, less attention has been given to public perceptions and attitudes toward certain alternatives. Understanding what the general public values in terms of a nuclear fuel cycle will assist in selecting a nuclear fuel cycle that optimizes the balance between technical feasibility and public acceptance. A multi-criteria decision analysis (MCDA) model was created to incorporate the general public's perceptions on qualified individuals and on important technical and non-technical aspects of any general fuel cycle. Analyzing the pair-wise comparisons for each criterion through the Analytic Hierarchy Process (AHP) yielded the relative importance of each aspect. A major finding is that the general public tend to view environmental scientists as qualified as nuclear engineers and scientists in selecting a method of used nuclear fuel disposal for the United States. (authors)
This article is a review of several accelerator–reactor interface issues and nuclear fuel cycle applications of acceleratordriven subcritical systems. The systems considered here have the primary goal of energy production, but that goal is accomplished via a specific application in various proposed nuclear fuel cycles, such as breed-and-burn of fertile material or burning of transuranic material. Several basic principles are reviewed, starting from the proton beam window including the target, blanket, reactor core, and up to the fuel cycle. We focus on issues of interest, such as the impact of the energy required to run the accelerator and associated systems on the potential electricity delivered to the grid. Accelerator-driven systems feature many of the constraints and issues associated with critical reactors, with the added challenges of subcritical operation and coupling to an accelerator. Reliable accelerator operation and avoidance of beam trips are critically important. One interesting challenge is measurement of blanket subcriticality level during operation. We also review the potential benefits of accelerator-driven systems in various nuclear fuel cycle applications. Ultimately, accelerator-driven subcritical systems with the goal of transmutation of transuranic material have lower 100,000-year radioactivity than a critical fast reactor with recycling of uranium and plutonium.
The civilian nuclear fuel cycle is an industrial process that produces electrical power from the nuclear fission of uranium. Using a measurement system to accurately account for nuclear material, such as uranium, in a fuel cycle is important because of the possible loss or diversion of this potentially dangerous material. A measurement system is defined by a set of measurement methods, or “devices,” used to account for material flows and inventory values at specific locations in the fuel cycle. Here, we develop a simulation-optimization algorithm and an integer-programming model to find the best, or near-best, resource-limited measurement system with a high degree of confidence. The simulation-optimization algorithm minimizes a weighted sum of false positive and false negative diversion-detection probabilities while accounting for material quantities and measurement errors across a finite, discrete time horizon in hypothetical non-diversion and diversion contexts. In each time period, the estimated cumulative material unaccounted for is compared to a fixed or an optimized threshold value to assess if a “significant amount of material” is lost from a measurement system. The integer-programming model minimizes the population variance of the estimated material loss, i.e., material unaccounted for, in a measurement system. We analyze three potential problems in nuclear fuel cycle measurement systems: (i) given location-dependent device precisions, find the configuration of n devices at n locations ( n = 3) that gives the lowest corresponding objective values using the simulation-optimization algorithm and integer-programming model, (ii) find the location at which improving device precision reduces objective values the most using the simulation-optimization algorithm, and determine the effect of measurement frequency on measurement system configurations and objective values using the simulation-optimization algorithm. We obtain comparable results for each problem at least an order of magnitude faster than existing methods do. Using an optimized, rather than fixed, detection threshold in the simulation-optimization algorithm reduces the weighted sum of false positive and false negative probabilities.
The inverse sensitivity/uncertainty quantification (IS/UQ) method has recently been implemented in the Inverse Sensitivity/UnceRtainty Estimator (INSURE) module of the AMPX cross section processing system [M.E. Dunn and N.M. Greene, “AMPX-2000: A Cross-Section Processing System for Generating Nuclear Data for Criticality Safety Applications,” Trans. Am. Nucl. Soc. 86, 118–119 (2002)]. The IS/UQ method aims to quantify and prioritize the cross section measurements along with uncertainties needed to yield a given nuclear application(s) target response uncertainty, and doing this at a minimum cost. Since in some cases the extant uncertainties of the differential cross section data are already near the limits of the present-day state-of-the-art measurements, requiring significantly smaller uncertainties may be unrealistic. Therefore, we have incorporated integral benchmark experiments (IBEs) data into the IS/UQ method using the generalized linear least-squares method, and have implemented it in the INSURE module. We show how the IS/UQ method could be applied to systematic and statistical uncertainties in a self-consistent way and how it could be used to optimize uncertainties of IBEs and differential cross section data simultaneously. We itemize contributions to the cost of differential data measurements needed to define a realistic cost function.
We report simulation of the nuclear fuel cycle can be performed using a wide range of techniques and methodologies. Past efforts have focused on specific fuel cycles or reactor technologies. The CYCLUS fuel cycle simulator seeks to separate the design of the simulation from the fuel cycle or technologies of interest. In order to support this separation, a robust supply–demand communication and solution framework is required. Accordingly an agent-based supply-chain framework, the Dynamic Resource Exchange (DRE), has been designed implemented in CYCLUS. It supports the communication of complex resources, namely isotopic compositions of nuclear fuel, between fuel cycle facilities and their managers (e.g., institutions and regions). Instances of supply and demand are defined as an optimization problem and solved for each timestep. Importantly, the DRE allows each agent in the simulation to independently indicate preference for specific trading options in order to meet both physics requirements and satisfy constraints imposed by potential socio-political models. To display the variety of possible simulations that the DRE enables, example scenarios are formulated and described. Important features include key fuel-cycle facility outages, introduction of external recycled fuel sources (similar to the current mixed oxide (MOX) fuel fabrication facility in the United States), and nontrivial interactions between fuel cycles existing in different regions.
Closing the nuclear fuel cycle could be simplified by recovering the actinides U through Am as a group. This could be achieved by converting U, Np, Pu and Am to the hexavalent state. Uranium, Np and Pu are readily oxidized to the hexavalent state. Generation of hexavalent Am in acidic solutions is more difficult, as the standard reduction potential of the Am(VI) /Am(III) couple (+1.68 V in 1 M HClO4) is well outside of the electrochemical stability window of water. While the oxidation and separation of Am has been demonstrated under laboratory conditions, several issues could plague scale up and implementation of this separation with used fuel. Two primary concerns are considered. The first issue concerns the stability of the oxidized Am. The second involves the undesirable co-extraction of tetravalent f-elements with the hexavalent actinides. To address the first concern regarding Am redox instability, Am reduction will be monitored under a variety of different conditions to establish the means of improving the stability of Am(VI) in the organic phase. Identifying the components contributing most significantly to its reduction will allow thoughtful modification of the process. To address the second concern, we propose to apply branched chain extractants to separate hexavalent actinides from tetravalent f-elements. Both branched monoamide and organophosphorus extractants have demonstrated significant selectivity for UO22+ versus Th4+, with separation factors generally on the order of 100. The efforts of this two-pronged research program should represent a significant step forward in the development of aqueous separations approaches designed to recover the U-Am actinides based on the availability of the hexavalent oxidation state. For the purposes of this proposal, separations based on this approach will be called SAn(VI) separations, indicating the Separation of An(VI).
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Management of spent nuclear fuel and high-level radioactive waste consists of three main phases – storage, transportation, and disposal – commonly referred to as the back end of the nuclear fuel cycle. Current practice for commercial spent nuclear fuel management in the United States (US) includes temporary storage of spent fuel in both pools and dry storage systems at operating or shutdown nuclear power plants. Storage pools are filling to their operational capacity, and management of the approximately 2,200 metric tons of spent fuel newly discharged each year requires transferring older and cooler spent fuel from pools into dry storage. Unless a repository becomes available that can accept spent fuel for permanent disposal, projections indicate that the US will have approximately 136,000 metric tons of spent fuel in dry storage systems by mid-century, when the last plants in the current reactor fleet are decommissioned. Current designs for dry storage systems rely on large multi-assembly canisters, the most common of which are so-called “dual-purpose canisters” (DPCs). DPCs are certified for both storage and transportation, but are not designed or licensed for permanent disposal. The large capacity (greater number of spent fuel assemblies) of these canisters can lead to higher canister temperatures, which can delay transportation and/or complicate disposal. This current management practice, in which the utilities continue loading an ever-increasing inventory of larger DPCs, does not emphasize integration among storage, transportation, and disposal. This lack of integration does not cause safety issues, but it does lead to a suboptimal system that increases costs, complicates storage and transportation operations, and limits options for permanent disposal. This paper describes strategies for improving integration of management practices in the US across the entire back end of the nuclear fuel cycle. The complex interactions between storage, transportation, and disposal make a single optimal solution unlikely. However, efforts to integrate various phases of nuclear waste management can have the greatest impact if they begin promptly and continue to evolve throughout the remaining life of the current fuel cycle. A key factor that influences the path forward for integration of nuclear waste management practices is the identification of the timing and location for a repository. The most cost-effective path forward would be to open a repository by mid-century with the capability to directly dispose of DPCs without repackaging the spent fuel into disposalready canisters. Options that involve repackaging of spent fuel from DPCs into disposalready canisters or that delay the repository opening significantly beyond mid-century could add 10s of billions of dollars to the total system life cycle cost.
The aim for storage of spent nuclear fuel (SNF) either in wet or in dry storage systems is to ensure general safety objective s are met throughout a desired storage period. Staff at the Savannah River National Laboratory (SRNL), in collaborations with partners at other national laboratories, industry research organizations, and the University of South Carolina (UofSC), have performed materials aging testing and analyses, and have established nuclear materials aging management programs to support extended periods of safe storage of research reactor (RR) SNF and of commercial power reactor (PR) SNF pending ultimate disposal. Several example challenges include susceptibility of aluminum SNF from research reactors to corrosion in poor quality water (wet storage). In dry storage, aluminum SNF can release hydrogen via radiolysis of the hydrated oxides on the aluminum cladding. Austenitic stainless steel canisters used for dry storage are susceptible to chloride-induced stress corrosion cracking (outside-in attack) that threaten the confinement boundary provided by the canister. This paper further describes these challenges, among others, and the formulated solutions to support extended safe storage of SNF.
The nuclear fuel cycle is a complex entity, with many stages and possibilities, encompassing natural resources, energy, science, commerce, and security, involving a host of nations around the world. This overview describes the process for generating nuclear power using fissionable nuclei.
Electricity generated using nuclear power accounted for 18.9% of all electricity consumed in the United States in 2021, putting it in third place behind natural gas (38%) and coal (22%) power plants. Nuclear power plants boast a significantly higher uptime or capacity factor—90% and above—compared to 49.1% for coal fired power plants and 56.6% for natural gas power plants. Renewable energy sources, such as solar photovoltaic (PV) and wind electricity, have lower capacity factors: 24.9% and 36.3%, respectively. In addition, nuclear power is cleaner than both coal and natural gas fired power plants. With the passing of the 2022 Inflation Reduction Act, significant tax credits will be claimed by producers of hydrogen with well-to-gate greenhouse gas (GHG) emissions below 0.45 kg CO 2e /kg H 2 . This has sparked interest in using clean sources of electricity, including nuclear power, to generate H 2 via water electrolysis. As uranium is a primary fuel for modern nuclear power plants, the upstream emissions from nuclear fuel production greatly impact the GHG emissions related to all nuclear power end use. Therefore, it is important to accurately determine the upstream emissions associated with the nuclear fuel cycle of nuclear power production in the United States. In this analysis, the nuclear fuel cycle was separated into distinct steps to allow better understanding of the chemical and energy inputs at each step of the fuel cycle. This also provides details of the GHG emissions at each step in the nuclear fuel cycle. The transportation distance for each step of the fuel cycle was updated to account for the locations of uranium processing facilities along the supply chain of the current U.S. nuclear power plants. Finally, all the updated values were incorporated into Argonne National Laboratory’s Greenhouse Gases, Regulated Emissions, and Energy Use in Technologies (GREET) model.
Future nuclear fuel cycle options may present advantages over today’s once-through fuel cycle. Nuclear fuel cycle simulation tools assess the performance of those fuel cycles as well as the dynamics of long-term technology transitions. In many nuclear fuel cycle simulation tools, it has historically been the responsibility of the user to manually define facility deployment schemes and all facility parameters. While this is straightforward in simple fuel cycles, transitions from one fuel cycle to another can be more complex. In particular, deployment schemes for supportive fuel cycle facilities beyond the reactor become complex if the analyst desires to avoid gaps in the nuclear fuel and power supply chain during those transition scenarios. As nuclear fuel cycle analysis approaches questions regarding the feasibility and performance of the deployment schemes and technology choices during technology transition, automation of this historically manual process is necessary. The main objective of this work was to develop and demonstrate Cyclus automation capabilities toward key nuclear fuel cycle transition scenarios. While deploying reactors to meet power demand is trivial, and existed in the earliest versions of CYCLUS, automated, predictive deployment and decommissioning of other facilities is more complex. These include mining, milling, enrichment, fuel fabrication, reprocessing, and others. For example, a balanced closed fuel cycle may require ensuring that there is enough fast reactor fuel for their operation and may drive deployment of a fleet of light water reactors. This concern comprises the main challenge that drove the project effort. The Demand-Driven Cycamore Archetype project (NEUP-FY16-10512) aimed to develop CYCAMORE demand-driven deployment capabilities and thereby automate transition scenario definition. The developed software package, d3ploy, in the form of a CYCLUS Institution agent, deploys Facilities to meet the front-end and back-end demands of the fuel cycle. The University of South Carolina and the University of Illinois applied multiple algorithmic approaches to this challenge. This project developed an in situ demand-driven development schedule calculation through non-optimizing, deterministic-optimizing, and stochastic-optimizing algorithms as CYCLUS archetypes and demonstrated these new archetypes in program-supporting fuel cycle transition scenarios. Both objectives were achieved. This report documents the results and deliverables obtained toward these achievements in detail.