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Integrated Off-gas System: A Preconceptual Design of an Integrated Off-Gas Treatment System

The U.S. has a vested interest in the advancement of nuclear energy to achieve aggressive net-zero goals, with reprocessing and recycling of used nuclear fuels (UNF) playing a vital role. It will not be possible to meet U.S. regulatory requirements without robust off-gas treatment, so it is crucial to advance treatment technologies to facilitate the design of future reprocessing facilities. For many years, teams of researchers across the U.S. Department of Energy (DOE) National Laboratory complex have been investigating off-gas treatment technologies for the capture and removal of volatile radionuclides (i.e., 85 Kr, Xe, 14 C, and 129 I) and oxides of nitrogen (NO X ) that are produced from reprocessing. These investigations have been focused on developing individual technologies for the capture of Kr, Xe, iodine, and CO 2 . Capture technologies for each constituent were tested independently from one another by utilizing nonradioactive surrogates to simulate simplified off-gas streams. The tests have been relatively small, laboratory-scale experiments of up to approximately 1 L/minute total gas flow rate. To increase the readiness of these technologies for deployment, an integrated test system with a larger-scale capacity is needed to bridge the gap between promising bench scale and fully scalable UNF reprocessing off-gas treatment. This document contains the goals, design basis, functional requirements, preconceptual design, and cost estimates for an integrated off-gas demonstration system for the capture and removal of NO x , Kr, Xe, CO 2 , and iodine at 10× higher throughput than earlier laboratory studies. The order-of-magnitude cost estimate for this system is approximately $\$$886,000. Next phases include conceptual design, detailed design, fabrication, and commissioning.

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Separation of technetium and rare earth metals for co-decontamination process

Poster. In the US there are several technologies under consideration for the separation of the useful components in used nuclear fuel. One such process is the co-decontamination process to separate U, Np and Pu in a single step and produce a Np/ Pu and a U product stream. Although the behavior of the actinide elements is reasonably well defined in this system, the same is not true for the fission products, mainly Zr, Mo, Ru and Tc. As these elements are cationic and anionic they may interact with each other to extract in a manner not predicted by empirical models such as AMUSE. This poster presentation will discuss the initial results of batch contact testing under flowsheet conditions and as a function of varying acidity and flowsheet conditions to optimize recovery of Tc and minimize extraction of Mo, Zr and Ru with the goal of developing a better understanding of the behavior of these elements in the co-decontamination process.

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LWR spent fuel reduction by the removal of U and the compact storage of Pu with FP for long-term nuclear sustainability

Fast breeder reactors (FBR) nuclear fuel cycle is needed for long-term nuclear sustainability while preventing global warming and maximum utilizing the limited uranium (U) resources. The 'Framework for Nuclear Energy Policy' by the Japanese government on October 2005 stated that commercial FBR deployment will start around 2050 under its suitable conditions by the successive replacement of light water reactors (LWR) to FBR. Even after Fukushima Daiichi Nuclear Power Plant accident which made Japanese tendency slow down the nuclear power generation activities, Japan should have various options for energy resources including nuclear, and also consider the delay of FBR deployment and increase of LWR spent fuel (LWR-SF) storage amounts. As plutonium (Pu) for FBR deployment will be supplied from LWR-SF reprocessing and Japan will not possess surplus Pu, the authors have developed the flexible fuel cycle initiative (FFCI) for the transition from LWR to FBR. The FFCI system is based on the possibility to stored recycled materials (U, Pu)temporarily for a suitable period according to the FBR deployment rate to control the Pu demand/supply balance. This FFCI system is also effective after the Fukushima accident for the reduction of LWR-SF and future LWR-to-FBR transition. (authors)

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Final Technical Report: Imaging a Dry Storage Cask with Cosmic Ray Muons

The goal of this project is to build a scaled prototype system for monitoring used nuclear fuel (UNF) dry storage casks (DSCs) through cosmic ray muon imaging. Such a system will have the capability of verifying the content inside a DSC without opening it. Because of the growth of the nuclear power industry in the U.S. and the policy decision to ban reprocessing of commercial UNF, the used fuel inventory at commercial reactor sites has been increasing. Currently, UNF needs to be moved to independent spent fuel storage installations (ISFSIs), as its inventory approaches the limit on capacity of on-site wet storage. Thereafter, the fuel will be placed in shipping containers to be transferred to a final disposal site. The ISFSIs were initially licensed as temporary facilities for ~20-yr periods. Given the cancellation of the Yucca mountain project and no clear path forward, extended dry-cask storage (~100 yr.) at ISFSIs is very likely. From the point of view of nuclear material protection, accountability and control technologies (MPACT) campaign, it is important to ensure that special nuclear material (SNM) in UNF is not stolen or diverted from civilian facilities for other use during the extended storage.

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Time cycle analysis and simulation of material flow in MOX process layout

The (U,Pu)O{sub 2} MOX fuel is the driver fuel for the upcoming PFBR (Prototype Fast Breeder Reactor). The fuel has around 30% PuO{sub 2}. The presence of high percentages of reprocessed PuO{sub 2} necessitates the design of optimized fuel fabrication process line which will address both production need as well as meet regulatory norms regarding radiological safety criteria. The powder pellet route has highly unbalanced time cycle. This difficulty can be overcome by optimizing process layout in terms of equipment redundancy and scheduling of input powder batches. Different schemes are tested before implementing in the process line with the help of a software. This software simulates the material movement through the optimized process layout. The different material processing schemes have been devised and validity of the schemes are tested with the software. Schemes in which production batches are meeting at any glove box location are considered invalid. A valid scheme ensures adequate spacing between the production batches and at the same time it meets the production target. This software can be further improved by accurately calculating material movement time through glove box train. One important factor is considering material handling time with automation systems in place.

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A burnup credit approach irradiated fast-neutron reactor fuels/ nuclides of interest and fuel storage application - 14248

The concept of taking into account the reduction of the reactivity of nuclear used fuel due to their burnup is referred to as 'Burnup Credit' (BUC). Economic incentives offered by the implementation of a BUC methodology in criticality analyses of Light Water Reactor (LWR) used fuel facilities are nowadays well-demonstrated. The current prospect of reprocessing the fissile and fertile subassemblies of the PHENIX reactor in France, and the development of the 4.-Generation Fast-neutron Reactors (FR) enable research projects in relevant fuel cycle operations. Under these circumstances, the CEA and AREVA-NC have decided to study a burnup credit approach for irradiated fuels of the PHENIX reactor. This paper focuses on a preliminary investigation on the use of burnup credit for used FR fuel operations. The first step consists in analyzing and selecting the nuclides of interest for burnup calculation, on the basis of the 27 BUC nuclides (12 actinides and 15 fissions products) chosen for LWR-MOx fuels [1]. These nuclides are then involved in a criticality calculation (a used fuel pool) to highlight the interest of a BUC approach. This study highlights the interest of a burnup credit approach for FR fuels and shows that the highest contribution to reactivity loss is due to only one fission product: the {sup 149}Sm. The opportunity to take account of only one fission product is highly promising and will considerably simplify the way to determine a penalizing fuel inventory. Moreover, it is to notice that results for different configurations may differ from those obtained for a fuel storage application. Thus, specific analyses have to be carried out in order to study the applicability of the conclusions of this paper. (authors)

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Strategies for thorium fuel cycle transition in the SD-TMSR

Liquid-fueled Molten Salt Reactor (MSR) systems represent advances in safety, economics, and sustainability. The MSR has been designed to operate with a Th/ 233 U fuel cycle with 233 U used as startup fissile material. Since 233 U does not exist in nature, we must examine other available fissile materials to start up these reactor concepts. This work investigates the fuel cycle and neutronics performance of the Single-fluid Double-zone Thorium-based Molten Salt Reactor (SD-TMSR) with different fissile material loadings at startup: High Assay Low Enriched Uranium (HALEU) (19.79%), Pu mixed with HALEU (19.79%), reactor-grade Pu (a mixture of Pu isotopes chemically extracted from Pressurized Water Reactor (PWR) spent nuclear fuel (SNF) with 33 GW d/tHM burnup), transuranic elements (TRU) from Light Water Reactor (LWR) SNF, and 233 U. The MSR burnup routine provided by SERPENT-2 is used to simulate the online reprocessing and refueling in the SD-TMSR. The effective multiplication factor, fuel salt composition evolution, and net production of 233 U are studied in the present work. Additionally, the neutron spectrum shift during the reactor operation is calculated. The results show that the continuous flow of reactorgrade Pu helps transition to the thorium fuel cycle within a relatively short time (≈ 4.5 years) compared to 26 years for 233 U startup fuel. Finally, using TRU as the initial fuel materials offers the possibility of operating the SD-TMSR for an extended period of time (≈ 40 years) without any external feed of 233 U.

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An Industrial Perspective of Research Within the DISTINCTIVE Program - 18045

UK Engineering and Physical Sciences Research Council (EPSRC) and three industrial partners, the Nuclear Decommissioning Authority (NDA), the National Nuclear Laboratory (NNL) and Sellafield Ltd (SL) are supporting the DISTINCTIVE (Decommissioning, Immobilisation and Storage Solutions for Nuclear Waste Inventories) consortium of eleven universities to carry out research in four theme areas of importance to the UK nuclear industry: Advanced Gas-cooled Reactor (AGR), Magnox and exotic spent fuels; PuO{sub 2} and fuel residues; legacy ponds and silo wastes; and structural integrity. This paper describes the main industry challenges in each of these theme areas and some of industry led activities to address these challenges, and provides examples of where the DISTINCTIVE research output is assisting the nuclear industry in meeting these challenges. (authors)

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The INFODEM Information Centre at CEA Marcoule: A Unique Information Tool in Europe About Nuclear Decommissioning - 16217

In September 2014, the French Alternative Energies and Atomic Energy Commission (CEA) inaugurated a unique information center focused on decommissioning of its nuclear facilities. This facility, named INFODEM information center, is inside the main building of the G1 nuclear reactor at Marcoule, a nuclear site in the south of France with world-recognized expertise in decommissioning. Constructed in the 1950's, the G1 reactor was the first industrial-scale reactor for plutonium production in France; it was also used to produce electricity. Operations ceased in 1968, and it was progressively dismantled (through removal of fuel and main components) and placed in monitoring status. In the 1980s, mockups of fuel cycle process equipment were built under a temporary mission to support development activities for the La Hague reprocessing plant. When that ended, further dismantling occurred, and during 1996 through 2010, the site established itself as a reference example for worldwide nuclear dismantling activities. In 2012, the project to establish an information center at the reactor began, targeting three main audiences: the public, agency personnel and politicians, and technical professionals. Considerable thought went into the facility design, to address the interests and information needs of these three audiences. The INFODEM concept extended over 800 square meters (about 960 square yards), to host an informative tour addressing several major themes: CEA's D and D strategy, programs, skills, tools and methodologies and 'everyday life' on decommissioning projects. Illustrating its unique value and considerable success, INFODEM received the Public Information Prize from the French Nuclear Energy Society (SFEN) in June 2015. (authors)

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Application of Modular Design in Abatement of Fuel Element Debris (FED) Liquid Waste Stream - 16635

This paper provides a description of the processes applied within the Aqueous Discharge Abatement Plant (ADAP) at Bradwell nuclear power plant in the UK. This incorporates the Fuel Element Debris (FED) abatement plant and the Modular Active Effluent Treatment Plant (MAETP). These plants are housed in adjacent, but separate, structures and are inter-linked and share common services and control systems. The FED abatement plant, which has a shorter mission than MAETP, can be removed for decommissioning or redeployment without any impact to MAETP operation. ADAP treats aqueous waste streams generated during the ongoing decontamination and decommissioning (D and D) operations for release from the Bradwell Power Station. The plant is designed to receive and treat two major classes of liquids: 1. Slightly contaminated water from various D and D sources and collected rainwater from the power station, referred to as Aqueous Effluent (AE). 2. Dissolved fuel element debris solution. This comprises of contaminated magnesium alloy (generated during the stripping of external structures from spent Magnox fuel elements prior to shipment for reprocessing) which has been dissolved in nitric acid. All received wastes are treated to remove heavy metals and radioactive constituents prior to isolation, sampling, verification, and ultimately release to the Blackwater Estuary. The treatment consists of multiple processes including precipitation, filtration, adsorption and ion exchange carefully designed to remove targeted radionuclides and heavy metals. (authors)

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Development of U and Pu Co-Recovery Process (Co-Processing) for Future Reprocessing

Co-processing process, which is the modified Purex process focused on co-recovery of Pu and U, has been studied at Operation Testing Laboratory, Tokai Reprocessing Plant in JAEA. The set up of the process was performed with flow-sheets study by process calculation to avoid Pu isolation in the whole process and to co-recover Pu/U product solution with a suitable Pu/U ratio (0.5< Pu/U <2). The initial Pu/U ratios of the feed solutions were taken as 1%, 3% and 20% considering the composition of the future spent fuels. The verification of the flow-sheets for each feed solutions were carried out with mixer-setters and active Pu/U feed solutions, focusing on the partitioning unit, and favorable back extraction performances of Pu accompanied by U were observed at all cases of the given feed solutions. According to these results, the co-processing process showed a good prospect to treat all kinds of future fuels from LWR, LWR-MOX and FBR, and a good prospect to be simplified by omitting the Pu/U purification cycle.

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The TRANSCEND Consortium - In-situ Identification of Surface Corrosion Products on Spent Nuclear Fuels - 20276

The management of spent nuclear fuel is a major ongoing concern for the UK owing to the cessation of reprocessing operations at Sellafield and the large, complex inventory arising from Magnox, AGR, PWR and prototype reactors. Retrieval and relocation operations for legacy fuels are imminent and therefore, any models that enhance our understanding of fuel evolution will help mitigate the risks associated with fuel storage and disposal. The TRANSCEND Consortium on nuclear waste management comprises four work packages, within this current paper we provide a summary overview of progress to date and illustrative results from Theme 3: Spent Nuclear Fuels. (authors)

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Submersible ROVs pioneer decommissioning of a legacy nuclear fuel storage pond - 15368

Submersible Remote Handling Vehicles (ROVs) are being used in innovative ways at the Sellafield decommissioning, reprocessing and nuclear waste management facility in the UK in a legacy fuel storage pond in support of pond decommissioning. A wide range of sensors and tooling attached to submersible ROVs are being used to characterise the contents of the pond and perform a wide range of maintenance and material retrieval tasks. Visual surveys, sludge and liquor sampling and radiological surveys are just some of the characterisation projects undertaken with the help of the ROVs. The ROVs have also been deployed with tooling including manipulators which can retrieve debris from the pond floor. A variety of mini and work class ROVs are used in the ponds and these can access areas of the pond that the traditional technologies such as long reach tooling and manipulators from overhead cranes cannot reach safely, efficiently and cost effectively. The ROVs are controlled at a distance from the pond to minimise operator exposure to radiation and avoid potential radiological contamination. (authors)

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Estimation of carbon 14 inventory in hull and end-piece wastes from Japanese commercial reprocessing operation

Hull and end-piece wastes generated from reprocessing plant operations are expected to be disposed of in a deep underground repository as Group 2 TRU wastes under the Japanese classification system. The activated metals that compose the spent fuel assemblies such as Zircaloy claddings and stainless steel nozzles are mixed and compressed after fuel dissolution, and then stuffed into stainless steel canisters. Carbon 14 is a typical activated product in the hulls and end-pieces and is mainly generated by the {sup 14}N(n,p){sup 14}C reaction. In the previous safety assessment of the TRU waste in Japan, the radionuclides inventory was calculated by ORIGEN-2 code. Some conservative assumptions and preliminary estimates were used in this calculation. For example, total radionuclides generated from a single type of fuel assembly (45 GWd/tU for a PWR unit), and the thickness of the Zircaloy oxide film on the hulls (80 μm) were both overestimated. The second assumption in particular has a large effect on exposure dose evaluation. Therefore, it is essential to have a realistic source term evaluation regarding such items as the C-14 inventory and its distribution to waste parts. In the present study, a C-14 inventory of the hull and end-piece wastes from the operation of a commercial reprocessing plant in Japan corresponding to 32,000 tU (16,000 tU in each BWR and PWR) was calculated. Analysis using individual irradiation conditions and fuel characteristics was conducted on 6 types of fuel assemblies for BWRs and 12 types for PWRs (4 pile types x 3 burnup limits). The oxide film thickness data for each fuel type cladding were obtained from the published literature. Activation calculations were performed by using ORIGEN-2 code. For the amount of spent assembly and other waste characteristics, representative values were assumed based on the published literature. As a preliminary experiment, C-14 in irradiated BWR claddings was measured and found to be consistent with the calculated activation. The total C-14 inventory was estimated as 4.46x10{sup 14} Bq, consisting of 2.58x10{sup 14} Bq for BWRs and 1.87x10{sup 14} Bq for PWRs, and is consistent with the safety assessment of 4.4x10{sup 14} Bq. However, the distribution of the C-14 inventory to hull oxide, which was estimated under the assumption of instantaneous radionuclide release in the safety assessment, decreased from 5.72x10{sup 13} Bq (13% of the total) in the previous assessment to 1.30x10{sup 13} Bq (2.9% of the total; consisting of 1.48x10{sup 12} for BWRs and 1.15x10{sup 13} for PWRs). In other words, the exposure dose peak is reduced to approximate 25% of its previous value due to the use of detailed oxide film data that the BWR cladding has a thin oxide film. Other instantaneous release components for C-14 such as the fuel residual were negligible. (authors)

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Cost-Benefit Assessment of Krypton and Xenon Recovery from Aqueous Reprocessing

The purpose of this paper is to provide an understanding of the cost-benefit of capturing Kr and Xe from the existing process of aqueous reprocessing of UNF. The study accomplishes this with a market assessment of Xe prices and volumes today, coupled with a cost estimate of Kr and Xe capture out of cryogenic distillation within aqueous reprocessing. The market assessment shows that the average price of Xe is about $\$ $60/L while the average price of Kr is about $\$ $1/L. The assessment also shows that the market structure for Xe is one of oligopoly, in other words, very few suppliers to the Xe market. The assessment shows growing demand for Xe, particularly in medical applications like anesthesia. The cost assessment finds the unit cost of Xe to range from $\$ $71.50/L to $\$ $131.13/L. This range is only slightly above the current range of market prices today, and with growing demand for Xe, prices could reach the range it would take to support extraction of Xe from aqueous reprocessing. On the other hand, the estimated cost range for Kr is $\$ $830.15/L up to $\$ $1,522.52/L, which far exceeds the range of market prices for Kr. However, as the text notes, Kr capture is already part of aqueous reprocessing so these costs are sunk costs (already incurred) whereas the cost estimates for Xe are marginal cost (if Xe is desired, then the cost estimate would result from the Xe capture).

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Finding ways to reduce nuclear waste: searching for the unknown one step at a time

In my home country, Venezuela, research has been stagnant. Due to the political turmoil and the crisis, many educated people have left the country in search for a better life. This has caused a deficit in any technological and scientific advances, making Venezuela one of the first South American countries to have its rate of publications decline by 29% in 2013. Currently, Venezuela lacks the infrastructure and the means to keep up with the research progress as compared to other countries in South America, such as Brazil. Since coming to the United States (US), and currently working for a national laboratory, the active research environment endorses a wide range of careers and engineering programs that allow researchers to thrive at any given field. Researchers have access to funds and tools to succeed in developing materials for the future. There are 17 national laboratories in the US, and all of these have a different research focus/objective. As examples, Los Alamos National Laboratory and Sandia National Laboratory focus is on national homeland security, weapon science, radiation effects, among others. Argonne National Laboratory focuses on nuclear energy, energy storage, high performance computing, etc. At Idaho National Laboratory (INL) the research focuses on innovating nuclear energy and clean energy resources, critical infrastructure materials, along with fuel cycle solutions to manage, dispose and find ways to recycle current and future radiological waste. Compared to other national laboratories, INL focuses slightly more on applied processes and how nuclear energy can be innovated to next reactor design and technologies. The research being conducted at INL made me apply for a Seaborg distinguished postdoctoral position. For the position itself, the researcher must submit a proposal related to actinide chemistry on a research field area. In this position, 50% of my time will be focused on my own proposal. The proposal that I am working on is focused on the innovation of nuclear energy and fuel cycle recycling, which is why I was mainly interested on working at this national laboratory. To give a bit more context of what my proposal is about, a little bit of background is necessary: After the nuclear fuel (UO2) is used in a reactor, the fuel matrix is then characterized by various fission products (FP). Among these FP (including rare earth elements, alkali/alkaline earths, and actinides), many can potentially be recovered through nuclear reprocessing technologies. In pyroprocessing, the used nuclear fuel undergoes electrochemical dissolution into a molten chloride salt mixture in an electrorefiner. Initially, uranium is reduced onto an inert cathode by applied potentials. However, numerous remaining FPs accumulate in the melt and pose challenges for recovery by an inert electrode, particularly the rare earth elements (e.g., Nd, Gd, Pr, Sm) due to their multivalent oxidation states and tendencies toward side reactions, leading to their dissolution in the electrolyte. These recovery challenges result in inefficiencies and necessitate the continual discarding of the molten chloride salt, thereby generating additional waste. Furthermore, the presence of rare earth elements and other fission products in the molten salt electrolyte alters its physical and chemical properties, affecting both uranium recovery efficiency and the longevity of the molten chloride salt. To improve the recovery efficiency of the FP, specifically rare earth elements, I am investigating the fundamental interactions between rare earth elements in the molten chloride salt and their metallic form. The kinetic pathways and the chemical reactions of these elements will give insights on how the recovery efficiency can be improved. The interactions and speciation of these elements are being studied by spectro-electrochemistry at high temperature environments in quartz and other ceramic materials (e.g., alumina crucibles). Some of the challenges I am facing specifically relates the reactivity of some of these elements with different glass and crucible materials. Although my research focuses on fundamental science, it will benefit the applied process by generating new scientific knowledge and closing the gap for an efficient recycling of the waste: one step at a time.

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A Rinsing Effluent Evaporator for Dismantling Operations - 13271

Between 1958 and 1997, the UP1 plant at Marcoule - located in the south of France - reprocessed and recycled nearly 20,000 MT of used fuel from special defense applications reactors, as well as fuel from the first generation of electricity generating reactors in France (natural uranium fuel, CO{sub 2}-cooled, graphite-moderated). Decommissioning and Dismantling of the UP1 plant and its associated units started in 1998. Since 2005, the UP1 facility has been operated by AREVA as the Marcoule Management and Operation contractor for French Atomic Energy Commission (CEA). An important part of this decommissioning program deals with the vitrification facility of Marcoule. This facility includes 20 tanks devoted to interim storage of highly active solutions, prior to vitrification. In 2006, a rinsing program was defined as part of the tank cleanup strategy. The main objective of the rinsing phases was to decrease activity in order to limit the volume of 'long-life active' waste produced during the decommissioning operations, so the tanks can be dismantled without the need of remote operations. To enable this rinsing program, and anticipating large volumes of generated effluent, the construction of an evaporation unit proved to be essential. The main objective of this unit was to concentrate the effluent produced during tank rinsing operations by a factor of approximately 10, prior to it being treated by vitrification. The evaporator design phase was launched in September 2006. The main challenge for the Project team was the installation of this new unit within a nuclear facility still in operation and in existing compartments not initially designed for this purpose. Cold operating tests were completed in 2008, and in May 2009, the final connections to the process were activated to start the hot test phase. During the first hot test operations performed on the first batches of clean-up effluent, the evaporator had a major operating problem. Extremely large quantities of foam were produced, affecting the evaporator operation, and creating the risk of a reduction in its capacity and throughput performance. A task force of AREVA process, operations, and safety experts from Marcoule and the La Hague reprocessing complex was assembled. New operating parameters were defined and tested to improve the process. Since then, the evaporator has performed very satisfactorily. The foam buildup phenomenon has been brought under complete control. All the different types of effluents produced during cleanup operations have been concentrated, and the results obtained in terms of quality and throughput, have ensured a consistent supply to the vitrification unit. The evaporator was operated until the end of April 2012, and enabled the production of 500 cubic meters of very high activity effluent, concentrating the fission products rinsed from the storage tanks. The evaporator will now be deactivated and decommissioned, with the first rinsing and cleanup operations scheduled to begin in 2014. (authors)

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