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Generic repository design concepts and thermal analysis (FY11).

Reference concepts for geologic disposal of used nuclear fuel and high-level radioactive waste in the U.S. are developed, including geologic settings and engineered barriers. Repository thermal analysis is demonstrated for a range of waste types from projected future, advanced nuclear fuel cycles. The results show significant differences among geologic media considered (clay/shale, crystalline rock, salt), and also that waste package size and waste loading must be limited to meet targeted maximum temperature values. In this study, the UFD R&D Campaign has developed a set of reference geologic disposal concepts for a range of waste types that could potentially be generated in advanced nuclear FCs. A disposal concept consists of three components: waste inventory, geologic setting, and concept of operations. Mature repository concepts have been developed in other countries for disposal of spent LWR fuel and HLW from reprocessing UNF, and these serve as starting points for developing this set. Additional design details and EBS concepts will be considered as the reference disposal concepts evolve. The waste inventory considered in this study includes: (1) direct disposal of SNF from the LWR fleet, including Gen III+ advanced LWRs being developed through the Nuclear Power 2010 Program, operating in a once-through cycle; (2) waste generated from reprocessing of LWR UOX UNF to recover U and Pu, and subsequent direct disposal of used Pu-MOX fuel (also used in LWRs) in a modified-open cycle; and (3) waste generated by continuous recycling of metal fuel from fast reactors operating in a TRU burner configuration, with additional TRU material input supplied from reprocessing of LWR UOX fuel. The geologic setting provides the natural barriers, and establishes the boundary conditions for performance of engineered barriers. The composition and physical properties of the host medium dictate design and construction approaches, and determine hydrologic and thermal responses of the disposal system. Clay/shale, salt, and crystalline rock media are selected as the basis for reference mined geologic disposal concepts in this study, consistent with advanced international repository programs, and previous investigations in the U.S. The U.S. pursued deep geologic disposal programs in crystalline rock, shale, salt, and volcanic rock in the years leading up to the Nuclear Waste Policy Act, or NWPA (Rechard et al. 2011). The 1987 NWPA amendment act focused the U.S. program on unsaturated, volcanic rock at the Yucca Mountain site, culminating in the 2008 license application. Additional work on unsaturated, crystalline rock settings (e.g., volcanic tuff) is not required to support this generic study. Reference disposal concepts are selected for the media listed above and for deep borehole disposal, drawing from recent work in the U.S. and internationally. The main features of the repository concepts are discussed in Section 4.5 and summarized in Table ES-1. Temperature histories at the waste package surface and a specified distance into the host rock are calculated for combinations of waste types and reference disposal concepts, specifying waste package emplacement modes. Target maximum waste package surface temperatures are identified, enabling a sensitivity study to inform the tradeoff between the quantity of waste per disposal package, and decay storage duration, with respect to peak temperature at the waste package surface. For surface storage duration on the order of 100 years or less, waste package sizes for direct disposal of SNF are effectively limited to 4-PWR configurations (or equivalent size and output). Thermal results are summarized, along with recommendations for follow-on work including adding additional reference concepts, verification and uncertainty analysis for thermal calculations, developing descriptions of surface facilities and other system details, and cost estimation to support system-level evaluations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Initial Evaluation of Processing Methods for an Epsilon Metal Waste Form

During irradiation of nuclear fuel in a reactor, the five metals, Mo, Pd, Rh, Ru, and Tc, migrate to the fuel grain boundaries and form small metal particles of an alloy known as epsilon metal (ε-metal). When the fuel is dissolved in a reprocessing plant, these metal particles remain behind with a residue - the undissolved solids (UDS). Some of these same metals that comprise this alloy that have not formed the alloy are dissolved into the aqueous stream. These metals limit the waste loading for a borosilicate glass that is being developed for the reprocessing wastes. Epsilon metal is being developed as a waste form for the noble metals from a number of waste streams in the aqueous reprocessing of used nuclear fuel (UNF) - (1) the ε-metal from the UDS, (2) soluble Tc (ion-exchanged), and (3) soluble noble metals (TRUEX raffinate). Separate immobilization of these metals has benefits other than allowing an increase in the glass waste loading. These materials are quite resistant to dissolution (corrosion) as evidenced by the fact that they survive the chemically aggressive conditions in the fuel dissolver. Remnants of ε-metal particles have survived in the geologically natural reactors found in Gabon, Africa, indicating that they have sufficient durability to survive for ≈ 2.5 billion years in a reducing geologic environment. Additionally, the ε-metal can be made without additives and incorporate sufficient foreign material (oxides) that are also present in the UDS. Although ε-metal is found in fuel and Gabon as small particles (≈10 µm in diameter) and has survived intact, an ideal waste form is one in which the surface area is minimized. Therefore, the main effort in developing ε-metal as a waste form is to develop a process to consolidate the particles into a monolith. Individually, these metals have high melting points (2617°C for Mo to 1552°C for Pd) and the alloy is expected to have a high melting point as well, perhaps exceeding 1500°C. The purpose of the work reported here is to find a potential commercial process with which ε-metal plus other components of UDS can be consolidated into a solid with minimum surface area and high strength Here, we report the results from the preliminary evaluation of spark-plasma sintering (SPS), hot-isostatic pressing (HIP), and microwave sintering (MS). Since bulk ε-metal is not available and companies could not handle radioactive materials, we prepared mixtures of the five individual metal powders (Mo, Ru, Rh, Pd, and Re) and baddeleyite (ZrO 2 ) to send the vendors of SPS, HIP, and MS. The processed samples were then evaluated at the Pacific Northwest National Laboratory (PNNL) for bulk density and phase assemblage with X-ray diffraction (XRD) and phase composition with scanning electron microscopy (SEM). Physical strength was evaluated qualitatively. Results of these scoping tests showed that fully dense cermet (ceramic-metal composite) materials with up to 35 mass% of ZrO 2 were produced with SPS and HIP. Bulk density of the SPS samples ranged from 87 to 98% of theoretical density, while HIP samples ranged from 96 to 100% of theoretical density. Microwave sintered samples containing ZrO 2 had low densities of 55 to 60% of theoretical density. Structurally, the cermet samples showed that the individual metals alloyed in to ε-phase - hexagonal-close-packed (HCP) alloy (4-95 mass %), the α-phase - face-centered-cubic (FCC) alloy structure (3-86 mass %), while ZrO 2 remained in the monoclinic structure of baddeleyite. Elementally, the samples appeared to have nearly uniform composition, but with some areas rich in Mo and Re, the two components with the highest melting points. The homogeneity in distribution of the elements in the alloy is significantly improved in the presence of ZrO 2 . However, ZrO 2 does not appear to react with the alloy, nor was Zr found in the alloy.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Iodine Sorption on AgZ-PAN

The Department of Energy (DOE) Nuclear Fuel Cycle and Supply Chain Program Material Recovery and Waste Form Development (MRWFD) Campaign Off-gas Sigma Team has performed research and development on iodine control and iodine waste forms for the past several years. This research and development has included iodine adsorption tests using a laboratory-scale test system containing multiple-segmented fixed beds of iodine adsorbents. Iodine capture performance has been tested using (a) non-radioactive synthetic gas mixtures blended from air, nitrogen, NO, NO 2 , water, to simulate dissolver off-gas (DOG) and vessel off-gas (VOG) streams from used nuclear fuel aqueous reprocessing, (b) inorganic and organic iodine species, and (c) different sorbents. An initial test of silver-functionalized mordenite in polyacrylonitrile matrix (AgZ-PAN) was conducted to assess if this sorbent, initially designed for selective sorption of Xe that evolves into used fuel reprocessing off-gas streams, could also be a candidate for iodine sorption. This test was conducted using the same deep-bed test system and methodologies used in many prior iodine sorption tests using other sorbents. Diatomic iodine (I2) was used as the target iodide in a gas stream containing air, NO, NO 2 , and moisture designed to simulate an aqueous reprocessing dissolver off-gas (DOG) stream.

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New Physical Insights about Tidal Disruption Events from a Comprehensive Observational Inventory at X-Ray Wavelengths

We perform a comprehensive study of the X-ray emission from 70 transient sources that have been classified as tidal disruption events (TDEs) in the literature. We explore the properties of these candidates, using nearly three decades of X-ray observations to quantify their properties and characteristics. We find that the emission from X-ray TDEs increase by two to three orders of magnitude, compared to pre-flare constraints. These emissions evolve significantly with time, and decay with power-law indices that are typically shallower than the canonical t {sup −5/3} decay law, implying that X-ray TDEs are viscously delayed. These events exhibit enhanced (relative to galactic) column densities and are quite soft in nature, with no strong correlation between the amount of detected soft and hard emission. At their peak, jetted events have an X-ray to optical ratio ≫1, whereas non-jetted events have a ratio ∼1, which suggests that these events undergo reprocessing at different rates. X-ray TDEs have long T {sub 90} values, consistent with what would be expected from a viscously driven accretion disk formed by the disruption of a main-sequence star by a black hole with a mass <10{sup 7} M {sub ⊙}. The isotropic luminosities of X-ray TDEs are bimodal, such that jetted and non-jetted events are separated by a “reprocessing valley” that we suggest is naturally populated by optical/UV TDEs that most likely produce X-rays, but this emission is “veiled” from observations due to reprocessing. Our results suggest that non-jetted X-ray TDEs likely originate from partial disruptions and/or disruptions of low-mass stars.

79 ASTRONOMY AND ASTROPHYSICS↗

Acid Dissolution Behavior of Ferritic FeCrAl Tubes Candidates for Nuclear Fuel Cladding

The international materials community is engaged in finding safer alternatives to zirconium alloys for the cladding of fuel in light water reactors. One solution is to replace the zirconium cladding using ferritic iron-chromium-aluminum (FeCrAl) alloys, which offer extraordinary resistance to high-temperature reaction with air or steam due to the formation of a protective alumina layer on the external surface. It is important to characterize the behavior of FeCrAl not only during accident conditions but in the entire fuel cycle, which may include reprocessing of the used fuel after it is removed from the power reactors. The reprocessing may involve the dissolution of the fuel rods in mineral acids. Little or nothing is known on the dissolution of FeCrAl alloys in common mineral acids, therefore the objective of this research was to study the dissolution of typical cladding tubing having two compositions of FeCrAl (APMT and C26M) in three acids (H 2 SO 4 , HNO 3 , and HCl) as a function of the temperature using both standard ASTM immersion tests as well as electrochemical tests. The dissolution behavior of the FeCrAl alloys is compared to the dissolution capability of other traditional nuclear materials such as austenitic stainless steels (304SS and 316SS) and austenitic nickel alloys (Alloy 600 and Hastelloy C-276). Results show that both C26M and APMT have a higher dissolution capability in the studied mineral acids, which will be beneficial for reprocessing procedures.

36 MATERIALS SCIENCE↗

Waste Estimates for a Future Recycling Plant in the US Based Upon AREVA Operating Experience - 13206

Estimates of process and secondary wastes produced by a recycling plant built in the U.S., which is composed of a used nuclear fuel (UNF) reprocessing facility and a mixed oxide (MOX) fuel fabrication facility, are performed as part of a U.S. Department of Energy (DOE) sponsored study [1]. In this study, a set of common inputs, assumptions, and constraints were identified to allow for comparison of these wastes between different industrial teams. AREVA produced a model of a reprocessing facility, an associated fuel fabrication facility, and waste treatment facilities to develop the results for this study. These facilities were divided into a number of discrete functional areas for which inlet and outlet flow streams were clearly identified to allow for an accurate determination of the radionuclide balance throughout the facility and the waste streams. AREVA relied primarily on its decades of experience and feedback from its La Hague (reprocessing) and MELOX (MOX fuel fabrication) commercial operating facilities in France to support this assessment. However, to perform these estimates for a U.S. facility with different regulatory requirements and to take advantage of some technological advancements, such as in the potential treatment of off-gases, some deviations from this experience were necessary. A summary of AREVA's approach and results for the recycling of 800 metric tonnes of initial heavy metal (MTIHM) of LWR UNF per year into MOX fuel under the assumptions and constraints identified for this DOE study are presented. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Promises and Challenges of Thorium Implementation for Transuranic Transmutation - 13550

This paper focuses on the challenges of implementing a thorium fuel cycle for recycle and transmutation of long-lived actinide components from used nuclear fuel. A multi-stage reactor system is proposed; the first stage consists of current UO{sub 2} once-through LWRs supplying transuranic isotopes that are continuously recycled and burned in second stage reactors in either a uranium (U) or thorium (Th) carrier. The second stage reactors considered for the analysis are Reduced Moderation Pressurized Water Reactors (RMPWRs), reconfigured from current PWR core designs, and Fast Reactors (FRs) with a burner core design. While both RMPWRs and FRs can in principle be employed, each reactor and associated technology has pros and cons. FRs have unmatched flexibility and transmutation efficiency. RMPWRs have higher fuel manufacturing and reprocessing requirements, but may represent a cheaper solution and the opportunity for a shorter time to licensing and deployment. All options require substantial developments in manufacturing, due to the high radiation field, and reprocessing, due to the very high actinide recovery ratio to elicit the claimed radiotoxicity reduction. Th reduces the number of transmutation reactors, and is required to enable a viable RMPWR design, but presents additional challenges on manufacturing and reprocessing. The tradeoff between the various options does not make the choice obvious. Moreover, without an overarching supporting policy in place, the costly and challenging technologies required inherently discourage industrialization of any transmutation scheme, regardless of the adoption of U or Th. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Generic Repository Concepts and Thermal Analysis for Advanced Fuel Cycles - 12477

A geologic disposal concept for spent nuclear fuel (SNF) or high-level waste (HLW) consists of three components: waste inventory, geologic setting, and concept of operations. A set of reference geologic disposal concepts has been developed by the U.S. Department of Energy (DOE), Used Fuel Disposition campaign. Reference concepts are identified for crystalline rock, clay/shale, bedded salt, and deep borehole (crystalline basement) geologic settings. These were analyzed for waste inventory cases representing a range of waste types that could be produced by advanced nuclear fuel cycles. Concepts of operation consisting of emplacement mode, repository layout, and engineered barrier descriptions, were selected based on international progress. All of these disposal concepts are enclosed emplacement modes, whereby waste packages are in direct contact with encapsulating engineered or natural materials. Enclosed modes have less capacity to dissipate heat than open modes such as that proposed for a repository at Yucca Mountain. Thermal analysis has identified important relationships between waste package size and capacity, and the duration of surface decay storage needed to meet temperature limits for different disposal concepts. For the crystalline rock and clay/shale repository concepts, a waste package surface temperature limit of 100 deg. C was assumed to prevent changes in clay-based buffer material or clay-rich host rock. Surface decay storage of 50 to 100 years is needed for disposal of high-burnup LWR SNF in 4-PWR packages, or disposal of HLW glass from reprocessing LWR uranium oxide (UOX) fuel. High-level waste (HLW) from reprocessing of metal fuel used in a fast reactor could be disposed after decay storage of 50 years or less. For disposal in salt the rock thermal conductivity is significantly greater, and higher temperatures (200 deg. C) can be tolerated at the waste package surface. Decay storage of 10 years or less is needed for high-burnup LWR SNF in 4-PWR packages, while 12-PWR packages could be emplaced after 40 years or less. HLW from reprocessing LWR UOX fuel or metal fuel from fast reactors, could be disposed of in salt after 10 to 50 years of decay storage depending on the specific composition and other factors. For the deep borehole disposal concept no near-field temperature limits are recognized because no performance credit is taken for waste form or waste package integrity, or containment by the near-field host rock. These results show the key differences in thermal management strategies available to the U.S. repository program, given the range of disposal concepts. A host medium such as salt with greater thermal conductivity and peak temperature tolerance could shorten decay storage by 50 years, or facilitate the use of larger waste packages. The LWR UOX SNF evaluated in this study represents that which could be produced in the coming decades. The existing, lower burnup used fuel that is presently in storage at many LWR locations across the U.S. is significantly cooler, and analyses of this type could be used to show that disposal is possible with less decay storage or larger waste packages. We note that while the temperature limits and waste package capacities used in this study are similar to those used internationally and in past U.S. studies, they might be increased as the result of ongoing research and development activities. This study selected enclosed emplacement modes to conform with disposal concepts developed internationally and previously in the U.S. Open modes (such as that proposed for a repository at Yucca Mountain) afford additional flexibility in waste management and the necessary investment, because the same facility serves both storage and disposal functions. Use of open modes, and combined analysis of storage, transportation, and disposal functions, are appropriate to consider in future studies of this type. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Reactor Graphite Handling. Problems and Solutions - 17208

The problem of industrial uranium-graphite reactors and NPP units decommissioning is one of the urgent tasks that require efficient and cost-effective solutions. To date, only Russia has already shut down and subject to decommissioning more than 120 objects. World-wide, more than 260,000 ton of irradiated graphite have arisen from the commercial nuclear power operations, research reactors, and defense production reactors. Under the circumstances the problem to develop cost-effective methods of the irradiated graphite management has appeared. Alternative disposal options for the irradiated graphite were discussed for at least 25-30 years. To date, various methods of irradiated graphite reprocessing have been proposed. They are based on the application of different physical and chemical processes, most of which involve incineration of the entire mass of graphite. However, they all have disadvantages, and do not solve the whole complex of problems. The primary goal of the research presented here was to carry out a study aimed at the development of a more simple technology (as compared to the incineration of the entire mass of graphite) that would provide for the graphite purification and allow the possibility of its transfer to the less hazardous waste category followed by the disposal of it in a near-surface repository. To achieve it is proposed to consider two directions, each of them reducing the cost of graphite reprocessing and the waste volume disposed of in the repository. The first alternative is based on the principle of partitioning radionuclides of different nature from the graphite, thus allowing to transfer it into the LLW category and minimize the volume of secondary waste products. The second option to change the reprocessing technology is the idea to use reactor graphite as the starting material to produce stable final waste form compositions intended for the long-term storage of radioactive waste including transuranic elements. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

EDF's used fuel management french policy - 15199

Regarding back-end fuel cycle, EDF's strategy, implemented from the very beginning of French nuclear production, consists in reprocessing of used fuel; decision to recycle plutonium in French PWR was taken from 1984. This reprocessing and recycling strategy, relying on existing industrial facilities (AREVA La Hague and Melox plants), has proven to be reliable and efficient. Treatment leads to a stabilization of used fuel total inventory in interim storage. Vitrification process ensures a safe packaging for high level and long-lived waste under a reduced volume. Recycling of fissile materials saves natural uranium requirements. Concentration of Pu in MOX used fuel leaves open the option to reuse it for starting next Generation IV systems beyond 2040. In 2008, EDF and AREVA, supported by French Government, agreed on commercial terms covering long term fuel reprocessing and recycling (up to 2040). Currently, EDF fuel management strategy relies on flow equilibrium in order to respect fuel cycle consistency and sustainability. The underlying principle is to strictly adjust separated plutonium production to recycling possibilities (i.e. licensed reactors and MOX fuel fabrication facilities). Given that fuel cycle policy, any trend in NPP core management that may impact the fuel cycle should be anticipated within times in order to avoid technical or administrative incompatibilities, and guarantee a high level of safety and robustness. In collaboration with industrial operators, EDF have to perform periodic 'Cycle Impact' analyses and report to the French Nuclear Safety Authority (ASN); next exercise is scheduled by the end of 2016. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Life Extension of Nuclear Plant Facilities through Monitoring and Detailed Analysis - 16175

The UK has accumulated a substantial legacy of radioactive waste from various civil nuclear and defence programmes. Presently, however most of the UK radioactive waste is generated from nine power stations which generate approximately one sixth of the of the country's electricity. Irradiated fuel is removed from these reactors and safe management of the radioactive solid and liquid effluents is required. The safe management of these effluents is essential. Sellafield, in West Cumbria UK, contains two reprocessing plants, one designed to process nuclear fuel from Magnox reactors (CO{sub 2} cooled with Uranium bar fuel) and the other to process nuclear fuel from Advanced Gas cooled Reactors and Pressurized Water Reactors. The reprocessing stage enables extraction of fissile material for recycling. This leaves a volume of dilute but high-level waste. The high-level radioactive liquid waste is concentrated to reduce its volume and then incorporated into borosilicate glass, using a process called vitrification. The glass is then poured into stainless steel containers and placed in long term storage. This required concentration of HLW liquor is achieved using a suite of aging evaporators. All evaporators are of similar design constructed from corrosion resistant stainless steel having dimensions height ∼11 m, internal diameter 3.05 m and capable of holding 13.7 m{sup 3} of liquor. The basic principle of operation is to heat the dilute liquor under partial vacuum, at constant volume, until the target concentration is achieved. Heating of the liquor is achieved using steam heated coils within the evaporator, and steam in the jacket which surrounds the lower half of the evaporator vessel. The evaporator is then brought to atmospheric pressure and the concentrated liquor is ejected whilst hot. The evaporator is then cooled with water cooled coils and a water filled jacket. New dilute liquor is then added for a new batch. The process is then repeated. As the evaporators reach the end of their original design life accurate prediction of the current condition of nuclear plant facilities is essential to safely justify continued plant operation by ensuring structural integrity. This poses a significant challenge as many aging UK nuclear facilities were not inherently built with inspection in mind. The potential life limiting components of the HA evaporators at Sellafield are the surfaces that contact the product liquor at elevated temperatures i.e. the steam heated surfaces of the coils within the evaporator vessel and the vessel base and wall surrounded by the steam jacket. Each heating component is critical to the operational life of the evaporator - the removal from service of a coil heating component significantly reduces the operational flexibility and remnant life of this plant. Over the last decade a variety of cutting-edge expertise and methodologies have been utilised to accurately measure and then predict the current condition of the plant and also to predict its remnant life. This paper provides an overview of the development of several techniques deployed, namely non-destructive testing/inspection, in-house software development and finite element modelling. These methods have been validated by lab-scale or full-scale experiments along with historical plant data. These techniques have been evolved and refined for over a decade, providing vital insights into the physical behaviour of this complex reprocessing system. This enables not only accurate assessment of the current condition of the plant equipment but also allows scientifically underpinned predictions to be made of how it will behave into the future. This is critical for Sellafield as this knowledge feeds into their safety case to the Office of Nuclear Regulation to justify continued operation. It is concluded that this integrated approach provides a robust analysis tool which has driven change and optimisation of plant procedures ensuring continued safe operation whilst extending the life of the facility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Plans for the Removal of Inventory from HLW Storage Tanks and Impact on Vitrification Feeds - 18175

Over the next 4 years Sellafield will cease reprocessing nuclear fuel. This represents a significant change in the mission of Sellafield Ltd, shifting the site focus from reprocessing operations to preparations for decommissioning. The storage tanks which have stored the acidic high level waste produced during reprocessing will require washing out. These tanks have been used since the 1950's and over time the nature of this waste has changed. It poses unique challenges for both removal and vitrification. A large collaborative programme of work is underway at Sellafield to characterise this inventory and prepare a strategy for its removal and vitrification. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Going from Closed to Open and Then Back Again: How to Keep a Level Head

Nuclear Energy is a mature, reliable low carbon technology with a secure and abundant fuel source and is an essential contributor to the energy mix. The UK has a long history of using nuclear energy and has a long standing world class expertise in the recycling of used nuclear fuel with three generations of industrial scale reprocessing plant operating on the Sellafield site, as well as the Thorp Miniature Pilot Plant in the 1980's, and a vibrant, internationally recognised R and D capability at the National Nuclear Laboratory (NNL). However, the reprocessing plants at Sellafield are both scheduled to finish around 2020 with Thorp and Magnox plants moving to post operational clean out (POCO). This will move the UK from a closed fuel cycle to an open one. Within the UK a decision has been made to refresh the current nuclear energy plants to at least replacement of the existing nuclear fleet. This will mean the building of new nuclear power plant to ensure energy production of 16 GWe per annum. With the closure of the UK's reprocessing plants, these new nuclear power plants will operate on an open fuel cycle with long term storage of used fuel followed by disposal. However it is also recognised that this may not be enough and as such expansion scenarios ranging from 16 to 75 GWe nuclear energy production are being considered through the development of a UK Road map. Within these energy scenarios, a variety of options are being evaluated including electricity generation only, electricity generation plus heat, open versus closed fuel cycles, Generation III versus Generation IV systems and combinations of the above. What is clear is that the deciding factor on the type and mix of any energy programme will not be on technology choice alone. Instead a complex mix of Government policy, relative cost of nuclear power, market decisions and public opinion will influence the rate and direction of growth of any future energy programme. At the ANS Winter Meeting 2013 a number of these techniques were presented. What was clear from the fuel cycle scenario modelling was the requirement for the utilisation of a closed fuel cycle to enable the expansion beyond 16 GWe. It is therefore a necessity for the UK to keep options open for a potential return to a closed fuel cycle in the future. The requirement to maintain the skills and capabilities to do so will be an essential part of any future nuclear strategy. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An Investigation on the Sustainability of a Sodium-cooled Breed-and-Burn Fast Reactor (B and BR)

Fast reactor can effectively handle the used nuclear fuel (UNF) by transmuting long-living transuranic (TRUs) into relatively short-living fission products. It can also be used to produce fissile from fertile nuclides as fuels for another reactor. The breed-and-burn fast reactor (B and BR) is a unique concept of fast reactor, which can breed the fissile fuels and use the bred fuels in situ. Thanks to this characteristic, the fuel utilization in a B and BR can be extremely high and even the recycled fuel of a B and BR can be used as a fuel to spawn the next generation B and BR. The UNF from the first B and BR should be reprocessed or reconditioned so that it can be reused in the second B and BR. A fuel reprocessing technology named melt refining was used in EBR-II from 1964 to 1969 and it was also applied in our previous study which showed that second B and BR can be started using the recycled UNF of first B and BR. However, about 95% of rare earths are removed during the melt refining and the associated processes are not very simple. Moreover, the actinide loss can also be significant. To enhance the proliferation-resistance and economy of the reprocessing, a super-simplified melt and treatment (SSMT) process without removing rare earth nuclides is suggested and the feasibility study to start the second B and BR using SSMT is carried out in this paper. The neutronics simulations were done using the Monte Carlo code McCARD in conjunction with ENDF/B-VII cross-section library. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Used Nuclear Fuel Management in Asia

Used fuel discharged from nuclear reactors are presently stored in wet pools or in dry cask at-reactor and/or away-from- reactor sites. Only a few countries reprocess their civilian used fuel, notably France, Russia, and UK. No country has yet operated a geologic repository to dispose of civilian used fuel or high-level radioactive wastes (HLW). As a result, the management and disposal of used fuel and HLW are viewed as the Achilles' heel of nuclear power. Figure 1 shows the used fuel inventory in the United States (US) and East Asian nuclear power programs. The inventory is estimated based on that in 2010 and the projected growth of nuclear power in these programs to 2020 and 2030. Figure 1 indicates that in 2010, the US had about 63,900 tons of used fuel from light-water reactors (LWR), more than the statutory limit of what was supposed to go into the now-abandoned Yucca Mountain Repository, and accounting for more than 33% of global used LWR fuel total. Currently, about 2,000 tons of used fuel are generated in the existing US LWRs annually. Russia had 25,100 tons of used fuel in 2010. Based on a modest growth of nuclear power, its used fuel inventory is expected to increase to about 31,800 and 38,000 tons by 2020 and 2030, respectively. The nuclear energy programs in East Asia (China, Japan, ROK, and Taiwan) account for 19% of global used LWR fuel inventory in 2010. China's used fuel inventory in 2010 was relatively small at 1,900 tons, but is expected to grow rapidly to {approx}12,400 and {approx}31,000 tons in 2020 and 2030, respectively, based on its expanding nuclear power program (from the current installed capacity of 21.8 GW to {approx}60 and {approx}200 GW in 2020 and 2030, respectively). Besides PWRs, China also operates 2 Candu reactors which each produces roughly 8 times more used fuel in tons than a PWR of the same power. The used Candu fuel inventory would increase from 950 tons in 2010 to 2,850 and 4,750 tons in 2020 and 2030, respectively. Used fuel in Japan, ROK, and Taiwan are US-obligated. Japan's future trends of used fuel inventory are uncertain due to the unknown numbers and timing of the currently-shutdown nuclear power plants that would be allowed for restart, and the uncertain future of Japan's reprocessing at Rokkasho. Under two scenario cases (a no-nuke/no-reprocessing and a 80%-nuke with reprocessing), the Japanese used fuel inventory could be capped from 2020 to 2030 to {approx}21,500 tons for the first case, and to {approx}22,500 tons for the second. The ROK's used PWR fuel inventory would increase from 4,900 tons in 2010 to about 8,800 and 14,000 tons in 2020 and 2030, respectively. Its used Candu fuel inventory would also increase from 5,900 tons in 2010 to about 9,700 and 13,500 tons in 2020 and 2030, respectively. The Taiwan used fuel inventory should be kept at current level as nuclear power is being phase out. Its growth should be modest from 3,000 tons in 2010 to about 4,300 and 5,000 tons in 2020 and 2030, respectively even if the 4. nuclear power station would start and the operation of existing LWRs is extended. Used fuel inventory in other East Asian countries (DPRK, Vietnam, etc.) should be small, if any before 2030.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Dynamic Diketoenamine Crosslinking Unlocks Vinyl Polymer Vitrimers From β ‐Triketone Chemistry

Covalent adaptable networks (CANs) offer a compelling strategy to unite the mechanical robustness of thermosets with the reprocessability of thermoplastics, yet achieving simultaneous durability, processability, and true recyclability remains challenging. We introduce diketoenamine (DKE) vitrimers derived from β-triketone methacrylate monomers and demonstrate how rational monomer design dictates network processability, viscoelasticity, and recyclability. By systematically varying the spacer length between the β-triketone (TK) moiety and the polymer backbone, we identify a key structure–property relationship that dictates vitrimer behavior. Networks bearing TK pendants minimally displaced from the backbone suppress creep but exhibit limited stress relaxation, whereas extended spacers yield lower glass transition temperatures, higher effective crosslink densities, and efficient stress dissipation, enabling optical transparency and reprocessability. Extending this platform to ultra-high molecular-weight prepolymers introduces physical entanglements as secondary crosslinks, further enhancing dimensional stability without compromising processability. Both mechanical and chemical recycling validate the closed-loop circularity of these materials. Furthermore, these results establish TK methacrylates as a versatile platform for designing high-performance vitrimers that integrate durability, reprocessability, and true closed-loop recyclability.

closed-loop recyclability↗

Pertechnetate/perrhenate–capped Zr/Hf–Dihydroxide Dimers: Elucidating Zr–TcO 4 Co–Mobility in the Nuclear Fuel Cycle

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.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Improving the Recyclability of Polymer Composites With Cellulose Nanofibrils

Cellulose nanofibers (CNFs) have been widely studied for their reinforcing potential in high-performance composites. While there are numerous publications on CNF-reinforced composites in a variety of polymer matrices, few have considered the recyclability of such thermoplastic composites and whether the incorporation of CNFs deteriorates or improves their performance upon reprocessing. In this study, two thermoplastic resins, poly(lactic acid) (PLA), and glycol-modified polyethylene terephthalate (PETg), were prepared with CNF reinforcement and thermomechanically recycled to investigate the effect of CNF inclusion on the composite properties after reprocessing as well as their effect on the composites’ number of useful life cycles. Additionally, changes in mechanical, thermal, rheological, molecular, and microstructural properties of the composites and/or base resins were monitored as a function of cycle numbers. As is typical, the polymers’ molecular weight and mechanical performance deteriorated with continued processing. However, the addition of spray dried CNF was found to better maintain the mechanical performance of both polymers throughout multiple recycling steps as compared to neat samples. For example, the tensile strength of PETg with 20 wt% CNF after 6 processing cycles was found to exceed that of virgin neat PETg, and higher loadings of CNF were found to preserve a higher yield strength during multiple rounds of reprocessing compared to PETg composites with lower CNF loadings. Ultimately this study indicates that the addition of CNF to some thermoplastic materials can increase both their sustainability by offsetting the use of high-embodied energy resins and their circularity by enabling performance retention over more use cycles.

42 ENGINEERING↗