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Codisposal Waste Package Loading Options for DOE SNF and HLW

The U.S. Department of Energy (DOE) is responsible for managing spent nuclear fuel (SNF) that is currently in, or will in the future come into, its possession. DOE must continue to safely store that SNF, transport it to an interim storage site or a repository, and dispose of it. These fuels come from a wide range of reactor types, such as light- and heavy-water-moderated reactors, graphite-moderated reactors, and breeder reactors, with various cladding materials and enrichments. Many of these reactors, now decommissioned, had unique design features, such as core configuration, fuel element and assembly geometry, moderator and coolant materials, operational characteristics, and neutron spatial and spectral properties resulting in a large diversity of reactor and fuel designs. Because of the wide variety and condition of SNF, a robust canister termed the DOE Standardized SNF Canister was proposed that would confine radionuclides and preclude moderator. The DOE Standard SNF Canister had four variations consisting of a 10- or 15-foot length and an 18- or 24-inch diameter. For ultimate disposal in the Yucca Mountain Repository these canisters were to be grouped with 24-inch diameter HLW canisters in a codisposal waste package. The 18-inch DOE Standardized SNF Canister could be placed in the middle of five HLW canisters. The 24-inch DOE Standardized SNF Canister would take the place of one the five HLW canister on the outer ring in the codisposal waste package. No DOE Standardized SNF Canisters have been loaded, and many fuel types can be loaded in multiple canisters. Depending on the selected diameter of the DOE Standardized SNF Canister for a particular fuel, the number of potential codisposal waste packages could vary. In addition, different types of DOE SNF may be able to be combined in a single canister. This could significantly change the number of DOE SNF canisters that are loaded and result in a decrease of the number of total potential codisposal waste packages. Ultimately, if too many HLW canisters need disposition, then a reduction in the number of DOE Standardized SNF Canisters will change the final total of codisposal waste packages very little. Likewise, if the ratio of DOE Standardized SNF Canisters to HLW canister produced is too high, then DOE Standardized SNF Canisters will not have enough HLW canisters to surround them in the codisposal waste package. This paper examines the results of differing loading strategies for a few DOE SNFs. It also compares the ranges of DOE Standardized SNF Canisters that may be produced to the ranges of HLW canisters that may be produced in order to determine potential scenarios.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Microstructural characterization of the oxidation of nuclear graphite under chronic and accident conditions via XCT and synchrotron XCT

Graphite is a candidate material to moderate fast neutrons and for structural components in the US next-generation graphite-moderated reactors. A graphite core is conceived as a large formation of interconnected bricks that primarily serves as the moderator of fast neutrons, holds instrumentation, fuel elements, control rods, and is a receptacle for molten salts for Molten Salt Reactors (MSRs) designs. During the operation of a graphite-moderated power plant, graphite components might be subjected to chronic oxidation during normal operating conditions or aggressive oxidation as a result of accidental ingress of air that reacts vigorously with the graphite core. Using synchrotron, x-ray computed tomography (XCT), this research systematically characterized microstructural changes that accompanied these two oxidation scenarios. Chronic oxidation was studied by characterizing IG-110, PCEA, and NBG-18 specimens that were gradually oxidized in air at a low temperature (520°C). The accidental ingress of air into the graphite reactor was simulated by subjecting the grades mentioned above to high-temperature oxidation at approximately 750°C. This research is the first, in situ, systematic characterization of nuclear graphite microstructural evolution that can be associated with the two possible oxidation scenarios and provide insight into related repercussions. The results show that the microstructure and pore connectivity influence the rate of oxidation and evolution of the microstructure under the two oxidation regimes. These results are crucial to understanding which grades are more resilient to each type of oxidation and documenting the damage created in the graphite.

Arregui Mena, Jose'↗

Treatment of Irradiated Graphite to meet Acceptance Criteria for Waste Disposal: A New IAEA Collaborative Research Program - 12443

World-wide, more than 250,000 tonnes of irradiated graphite have arisen through commercial nuclear-power operations and from military production reactors. Whilst most nations responsible for the generation of this material have in mind repository disposal alongside other radwaste, the lack of progress in this regard has led in some cases to difficulties where, for example, the site of an existing graphite-moderated reactor is required for re-utilisation. In any case, graphite as a radwaste stream has unique chemical and physical properties which may lend itself to more radical and innovative treatment and disposal options, including the recovery of useful isotopes and also recycling within the nuclear industry. Such aspects are important in making the case for future graphite-moderated reactor options (for example, High-Temperature Reactors planned for simultaneous power production and high-grade heat sources for such applications as hydrogen production for road fuel). A number of initiatives have taken place since the mid 1990s aimed at exploring such alternative strategies and, more recently, improving technology offers new options at all stages of the dismantling and disposal process. A new IAEA Collaborative Research Program aims to build upon the work already done and the knowledge achieved, in order to identify the risks and uncertainties associated with alternative options for graphite disposal, along with cost comparisons, thus enabling individual Member States to have the best-available information at their disposal to configure their own programs. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radiation Effects in Graphite

The requirements for a solid moderator are reviewed and the reasons that graphite has become the solid moderator of choice discussed. The manufacture and properties of some currently available near-isotropic and isotropic grades are described. The major features of a graphite moderated reactors are briefly outlined. Displacement damage and the induced structural and dimensional changes in graphite are described. Recent characterization work on nano-carbons and oriented pyrolytic graphites that have shed new light on graphite defect structures are reviewed, and the effect of irradiation temperature on the defect structures is highlighted. Changes in the physical properties of nuclear graphite caused by neutron irradiation are reported. Finally, the importance of irradiation induced creep is presented, along with current models and their deficiencies.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Uranium Oxide Aerosol Transport in Porous Graphite

The objective of this paper is to investigate the transport of uranium oxide particles that may be present in carbon dioxide (CO 2 ) gas coolant, into the graphite blocks of gas-cooled, graphite moderated reactors. The transport of uranium oxide in the coolant system, and subsequent deposition of this material in the graphite, of such reactors is of interest because it has the potential to influence the application of the Graphite Isotope Ratio Method (GIRM). The GIRM is a technology that has been developed to validate the declared operation of graphite moderated reactors. GIRM exploits isotopic ratio changes that occur in the impurity elements present in the graphite to infer cumulative exposure and hence the reactor’s lifetime cumulative plutonium production. Reference Gesh, et. al., for a more complete discussion on the GIRM technology.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Preliminary Benchmark Uncertainties for Deimos, a HALEU-Fueled and Graphite-Moderated Advanced Reactor Testbed

Many advanced reactor concepts will make use of various uranium fuels with levels of enrichment higher than previously seen in current light water reactors. In particular, High-Assay Low Enriched Uranium (HALEU), that is uranium enriched to 235 U ≈ 20 w/o%, is planned to be used in over ten new reactor concepts. HALEU is attractive for advanced reactors as it enables longer intervals between refueling. Unfortunately, little to no experience with HALEU is available in experimental literature raising concerns for not only licensing advanced re actors but also fabrication and transportation of HALEU fuels. This is where Deimos, a Los Alamos National Laboratory internal project, comes in. Deimos is a new critical experiment scheduled for FY24 at the National Criticality Experiments Research Center (NCERC). Deimos is a graphite moderated, graphite and beryllium reflected critical experiment making use of HALEU TRi-structural ISOtropic (TRISO) fuel from the Compact Nuclear Power System (CNPS). This transaction entails a brief description of efforts to benchmark Deimos for inclusion into the International Criticality Safety

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

XRD and SANS evaluation of HOPG and Polycrystalline Graphite

As the primary construction material used in gas-cooled reactor cores, either of high-temperature (HTR) or very high-temperature (VHTR) design, nuclear graphite must be well characterized and variations in its properties upon high-energy neutron irradiation must be known, understood, and predict ed as accurately as possible before a reactor is built and operational. However, even after more than 70 years of operation of graphite-moderated reactors and intense research on graphite’s behavior in an extreme environment created by high temperatures, irradiation, mechanical stress, and chemically reactive (oxidizing) gaseous environment, questions still remain.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Commercial-scale, fluoride-salt-cooled, high-temperature reactors with novel refueling and decay heat removal capabilities

The fluoride-salt-cooled high-temperature reactor (FHR) is a new solid-fuel, graphite-moderated reactor concept. Recent work has developed test and demonstration-scale FHR designs. From this work, a new 'fuel-inside-radial-moderator' (FIRM) assembly concept has emerged that offers several important advantages, from neutron economy to refueling. In this work we discuss the potential benefits and challenges associated with designing a commercial-scale, FIRM-based FHR. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Chemical Characterization and Removal of Carbon-14 from Irradiated Graphite II - 13023

Approximately 250,000 tonnes of irradiated graphite waste exists worldwide and that quantity is expected to increase with decommissioning of Generation II reactors and deployment of Generation IV gas-cooled, graphite moderated reactors. This situation indicates the need for a graphite waste management strategy. Of greatest concern for long-term disposal of irradiated graphite is carbon-14 (C-14), with a half-life of 5730 years. Study of irradiated graphite from some nuclear reactors indicates C-14 is concentrated on the outer 5 mm of the graphite structure. The aim of the research presented last year and updated here is to identify the chemical form of C-14 in irradiated graphite and develop a practical method by which C-14 can be removed. A nuclear-grade graphite, NBG-18, and a high-surface-area graphite foam, POCOFoam{sup R}, were exposed to liquid nitrogen (to increase the quantity of C-14 precursor) and neutron-irradiated (10{sup 13} neutrons/cm{sup 2}/s). Finer grained NBG-25 was not exposed to liquid nitrogen prior to irradiation at a neutron flux on the order of 10{sup 14} /cm{sup 2}/s. Characterization of pre- and post-irradiation graphite was conducted to determine the chemical environment and quantity of C-14 and its precursors via the use of surface sensitive characterization techniques. Scanning Electron Microscopy (SEM) was used to evaluate the morphological features of graphite samples. The concentration, chemical composition, and bonding characteristics of C-14 and its precursors were determined through X-ray Photoelectron Spectroscopy (XPS), Time-of-Flight Secondary Ion Mass Spectrometry (SIMS), and Energy Dispersive X-ray Analysis Spectroscopy (EDX). Results of post-irradiation characterization of these materials indicate a variety of surface functional groups containing carbon, oxygen, nitrogen and hydrogen. During thermal treatment, irradiated graphite samples are heated in the presence of an inert carrier gas (with or without oxidant gas), which carries off gaseous products released during treatment. Graphite gasification occurs via interaction with adsorbed oxygen complexes. Experiments in argon were performed at 900 deg. C and 1400 deg. C to evaluate the selective removal of C-14. Thermal treatment also was performed with the addition of 3 and 5 volume % oxygen at temperatures 700 deg. C and 1400 deg. C. Thermal treatment experiments were evaluated for the effective selective removal of C-14. Lower temperatures and oxygen levels correlated to more efficient C-14 removal. (authors)

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Plutonium Production Reactor Progression Problems: Magnox Neutronics Benchmarks

The goal of this document is to provide a set of comprehensive benchmarking neutronics problems for gas-cooled, graphite-moderated reactors. The problems are designed to be representative problems that increase in complexity to test performance of various codes. For the simulation of the benchmarking problems, the Shift Monte Carlo code and MPACT deterministic code are chosen because of their state-of-the-art capabilities, which are optimized for various reactor designs. Because these codes have been developed primarily for light water reactor applications, their application to graphite-moderated, gas-cooled reactors has not been extensively explored. This report attempts to evaluate benchmarks for a Magnox-style reactor, one that is graphite-moderated and gas-cooled. Parameters that are calculated and presented in this benchmark include the eigenvalue, peaking factors, and isotope concentrations. Results show good agreement between Shift and MPACT, and demonstrate the capability of MPACT to model graphite-moderated systems well.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Removal of 14 C from Irradiated Graphite for Graphite Recycle and Waste Volume Reduction

The aim of the research presented here was to identify the chemical form of 14 C in irradiated graphite. A greater understanding of the chemical form of this longest-lived isotope in irradiated graphite will inform not only management of legacy waste, but also development of next generation gas-cooled reactors. Approximately 250,000 metric tons of irradiated graphite waste exists worldwide, with the largest single quantity originating in the Magnox and AGR reactors of UK. The waste quantity is expected to increase with decommissioning of Generation II reactors and deployment of Generation I gas-cooled, graphite moderated reactors. Of greatest concern for long-term disposal of irradiated graphite is carbon-14 14 C, with a half-life of 5730 years.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Sampling and Analysis Plan for Investigation of Undeclared Nuclear Activities - 20104

The nuclear-centered energy policy in South Korea is moving towards a nuclear-free era. It also facilitates an action or progress on the denuclearization of the Korean peninsula. The Nuclear Safety and Security Commission (NSSC) launched a new R and D project which attempts to verify nuclear activities via analyzing environmental samples. Environmental samples possibly contain significant radiological information relevant to past undeclared activities. In order to precisely verify them, it is essential to provide 1) the concrete information of target facilities, 2) appropriate methodologies and procedures, and 3) well-suited instrumentation and equipment corresponding to sample signatures. It is also important to provide scientific reliability or validity in any process such as sample collection, handling, transportation and laboratory analysis. Therefore, the information of nuclear facilities (fuel fabrication plant, graphite moderated reactor, reprocessing plant) in North Korea are reviewed in order to determine parameters for appropriate sampling methods representing a facility's characteristics. Secondly, a sampling procedure for radioactive elements is being developed based on international and domestic standards such as ASTM (American Society for Testing and Materials), KS (Korean industrial Standards), and International Atomic Energy Agency (IAEA) manuals. The procedure contains some specific information including sampling process, sampling tools, amount of sample, sample identification, and other related information. Developing the qualified national guidelines is most important since sampling and analyzing results can be used as evidences of nuclear activities. The guideline developed through this work will clearly define various methodologies such as document verification, sampling procedures, collection methods, sample storage criteria, chain of custody, and transportation conditions. The final objective of this work is to establish the infrastructure and regulatory framework for assessment of nuclear activities, and provide a national guideline for sampling and analysis. This will bring confidence in the results and play a critical role in complete denuclearization progress in South Korea. (authors)

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Historic and modern nuclear graphite impurities: Pathways to improved waste strategies

Graphite has been used in large volumes as a structural material and neutron moderator since the earliest days of nuclear fission. However, no international consensus exists on the disposal of irradiated graphite, leaving much of the historic radioactive graphite inventory in interim vault or silo storage. With several new graphite-moderated reactors planned or under construction, the issue of graphite waste management is becoming increasingly urgent. This paper reviews and quantifies impurities in both historic and modern nuclear graphite, with emphasis on nitrogen—responsible for much of the 14 C inventory—and chlorine, which plays a critical role in repository performance and design. Modern graphites, benefitting from stringent quality-control measures developed for non-nuclear industries, meet or exceed the ASTM Ultra-High Purity nuclear standards, even without halide purification. Both chlorine and nitrogen concentrations have declined over time. For chlorine, identified as a key impurity influencing U.S. waste repository design, we propose a target of 0.1 appm in as-fabricated billets as a reasonable benchmark. Nitrogen sources are traced throughout the graphite production process, with surface and bulk concentrations characterized for all materials studied. Modern graphites commonly exhibit nitrogen levels below 5 appm, with values approaching 1 appm achievable. Using such reduced-nitrogen grades is critical to keeping graphite-induced radioactivity below the greater-than-Class-C waste threshold, thereby avoiding disposal cost penalties of nearly an order of magnitude.

Chlorine↗

NRC Licensing Status Summary Report for NGNP

The Next Generation Nuclear Plant (NGNP) Project, initiated at Idaho National Laboratory (INL) by the U.S. Department of Energy (DOE) pursuant to provisions of the Energy Policy Act of 2005, is based on research and development activities supported by the Department of Energy Generation IV Nuclear Energy Systems Initiative. The principal objective of the NGNP Project is to support commercialization of high temperature gas-cooled reactor (HTGR) technology. The HTGR is a helium-cooled and graphite moderated reactor that can operate at temperatures much higher than those of conventional light water reactor (LWR) technologies. The NGNP will be licensed for construction and operation by the Nuclear Regulatory Commission (NRC). However, not all elements of current regulations (and their related implementation guidance) can be applied to HTGR technology at this time. Certain policies established during past LWR licensing actions must be realigned to properly accommodate advanced HTGR technology. A strategy for licensing HTGR technology was developed and executed through the cooperative effort of DOE and the NRC through the NGNP Project. The purpose of this report is to provide a snapshot of the current status of the still evolving pre-license application regulatory framework relative to commercial HTGR technology deployment in the U.S. The following discussion focuses on (1) describing what has been accomplished by the NGNP Project up to the time of this report, and (2) providing observations and recommendations concerning actions that remain to be accomplished to enable the safe and timely licensing of a commercial HTGR facility in the U.S.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Validation of the U.S. NRC NGNP evaluation model with the HTTR

The High Temperature Test Reactor (HTTR) was modeled with TRITON/PARCS. Traditional light water reactor (LWR) homogenization methods rely on the short mean free paths of neutrons in LWR. In gas-cooled, graphite-moderated reactors like the HTTR neutrons have much longer mean free paths and penetrate further into neighboring assemblies than in LWRs. Because of this, conventional lattice calculations with a single assembly may not be valid. In addition to difficulties caused by the longer mean free paths, the HTTR presents unique axial and radial heterogeneities that require additional modifications to the single assembly homogenization method. To handle these challenges, the homogenization domain is decreased while the computational domain is increased. Instead of homogenizing a single hexagonal fuel assembly, the assembly is split into six triangles on the radial plane and five blocks axially in order to account for the placement of burnable poisons. Furthermore, the radial domain is increased beyond a single fuel assembly to account for spectrum effects from neighboring fuel, reflector, and control rod assemblies. A series of five two-dimensional cases, each closer to the full core, were calculated to evaluate the effectiveness of the homogenization method and cross-sections. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Radiation Effects in Graphite

Graphite has been a core structural material and neutron moderator since the first man-made chain reaction experiment in Chicago. This article will discuss the requirements of what makes graphite a good solid moderator. The manufacture and properties of some currently available near-isotropic and isotropic grades are described. The major features of a graphite moderated reactors are briefly outlined. Displacement damage and the induced structural and dimensional changes in graphite are described. Recent characterization work on nano-carbons and oriented pyrolytic graphites that have shed new light on graphite defect structures are reviewed, and the effect of irradiation temperature on the defect structures is highlighted. Changes in the physical properties of nuclear graphite caused by neutron irradiation are reported. Finally, the importance of irradiation induced creep is presented, along with current models and their deficiencies.

Campbell, Anne↗

Graphite Moderation in Fast Reactors

With the renewed interest in designing and building a fast test reactor in the U.S., several new reactor concepts have been emerging. Although the main mission of a fast test reactor would be to enable high fast flux irradiation capability, there could be added value for such a fast test reactor to also offer thermal neutron irradiation capabilities. As such, several of these concepts considered the use of a moderator material in a Sodium-cooled Fast Reactor (SFR), which is claimed to also offer benefits with respect of mass of fuel required. The work discussed in this paper focuses on exploring and assessing the benefits and challenges resulting from making use of thermalized neutrons to reduce the critical fuel mass. The analyses are performed for a graphite moderating material, using a simple core model to easily identify the phenomena observed. It is found that it is necessary to reduce the fuel enrichment near the moderated regions in order to avoid unacceptable power peaking. In the end, use of moderating materials outside a SFR core does not provide significant benefit in term of fuel volume reduction, but allows for a noticeable reduction of the mass of fissile material needed. However, it also implies a number of additional challenges which are highlighted in this paper.

core optimization↗