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At least 91 records · Page 5

Status of the nuclear measurement stations for the process control of spent fuel reprocessing at AREVA NC/La Hague

Nuclear measurements are used at AREVA NC/La Hague for the monitoring of spent fuel reprocessing. The process control is based on gamma-ray spectroscopy, passive neutron counting and active neutron interrogation, and gamma transmission measurements. The main objectives are criticality and safety, online process monitoring, and the determination of the residual fissile mass and activities in the metallic waste remained after fuel shearing and dissolution (empty hulls, grids, end pieces), which are put in radioactive waste drums before compaction. The whole monitoring system is composed of eight measurement stations which will be described in this paper. The main measurement stations no. 1, 3 and 7 are needed for criticality control. Before fuel element shearing for dissolution, station no. 1 allows determining the burn-up of the irradiated fuel by gamma-ray spectroscopy with HP Ge (high purity germanium) detectors. The burn-up is correlated to the {sup 137}Cs and {sup 134}Cs gamma emission rates. The fuel maximal mass which can be loaded in one bucket of the dissolver is estimated from the lowest burn-up fraction of the fuel element. Station no. 3 is dedicated to the control of the correct fuel dissolution, which is performed with a {sup 137}Cs gamma ray measurement with a HP Ge detector. Station no. 7 allows estimating the residual fissile mass in the drums filled with the metallic residues, especially in the hulls, from passive neutron counting (spontaneous fission and alpha-n reactions) and active interrogation (fission prompt neutrons induced by a pulsed neutron generator) with proportional {sup 3}He detectors. The measurement stations have been validated for the reprocessing of Uranium Oxide (UOX) fuels with a burn-up rate up to 60 GWd/t. This paper presents a brief overview of the current status of the nuclear measurement stations. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High Temperature Gas-cooled Reactor (HTGR) Graphite Pebble Fuel: Review of Technologies for Reprocessing

This report reviews literature on reprocessing high temperature gas-cooled reactor graphite fuel components. A basic review of the various fuel components used in the pebble bed type reactors is provided along with a survey of synthesis methods for the fabrication of the fuel components. Several disposal options are considered for the graphite pebble fuel elements including the storage of intact pebbles, volume reduction by separating the graphite from fuel kernels, and complete processing of the pebbles for waste storage. Existing methods for graphite removal are presented and generally consist of mechanical separation techniques such as crushing and grinding chemical techniques through the use of acid digestion and oxidation. Potential methods for reprocessing the graphite pebbles include improvements to existing methods and novel technologies that have not previously been investigated for nuclear graphite waste applications. The best overall method will be dependent on the desired final waste form and needs to factor in the technical efficiency, political concerns, cost, and implementation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High Temperature Gas-cooled Reactor (HTGR) Graphite Pebble Fuel: Review of Technologies for Reprocessing

This report reviews literature on reprocessing high temperature gas-cooled reactor graphite fuel components. A basic review of the various fuel components used in the pebble bed type reactors is provided along with a survey of synthesis methods for the fabrication of the fuel components. Several disposal options are considered for the graphite pebble fuel elements including the storage of intact pebbles, volume reduction by separating the graphite from fuel kernels, and complete processing of the pebbles for waste storage. Existing methods for graphite removal are presented and generally consist of mechanical separation techniques such as crushing and grinding and chemical techniques through the use of acid digestion and oxidation. Potential methods for reprocessing the graphite pebbles include improvements to existing methods and novel technologies that have not previously been investigated for nuclear graphite waste applications. The best overall method will be dependent on the desired final waste form and needs to factor in the technical efficiency, political concerns, cost, and implementation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Collocation and integration of reprocessing and repositories: implications for aqueous flowsheets and waste management

It is an accident of history that the current model of the fuel cycle is a separate set of facilities connected by transportation. The question is whether collocation and integration of reprocessing and fuel fabrication with the repository significantly reduce the costs of a closed fuel cycle while improving system performance in terms of safety and long-term repository performance. This paper examines the question in terms of higher-level functional requirements of reprocessing systems and geological repositories.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Spent nuclear fuel reprocessing modeling

The long-term wide development of nuclear power requires new approaches towards the realization of nuclear fuel cycle, namely, closed nuclear fuel cycle (CNFC) with respect to fission materials. Plant nuclear fuel cycle (PNFC), which is in fact the reprocessing of spent nuclear fuel unloaded from the reactor and the production of new nuclear fuel (NF) at the same place together with reactor plant, can be one variant of CNFC. Developing and projecting of PNFC is a complicated high-technology innovative process that requires modern information support. One of the components of this information support is developed by the authors. This component is the programme conducting calculations for various variants of process flow sheets for reprocessing SNF and production of NF. Central in this programme is the blocks library, where the blocks contain mathematical description of separate processes and operations. The calculating programme itself has such a structure that one can configure the complex of blocks and correlations between blocks, appropriate for any given flow sheet. For the ready sequence of operations balance calculations are made of all flows, i.e. expenses, element and substance makeup, heat emission and radiation rate are determined. The programme is open and the block library can be updated. This means that more complicated and detailed models of technological processes will be added to the library basing on the results of testing processes using real equipment, in test operating mode. The development of the model for the realization of technical-economic analysis of various variants of technologic PNFC schemes and the organization of 'operator's advisor' is expected. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Novel sorbent development and evaluation for the capture of krypton and xenon from nuclear fuel reprocessing off-gas stream

The release of volatile radionuclides generated during Used Nuclear Fuel reprocessing in the US will most certainly need to be controlled to meet US regulatory emission limits. A US DOE sponsored Off-Gas Sigma Team has been tasked with a multi-lab collaborative research and development effort to investigate and evaluate emissions and immobilization control technologies for the volatile radioactive species generated from commercial Used Nuclear Fuel (UNF) Reprocessing. Physical Adsorption technology is a simpler and potential economical alternative to cryogenic distillation processes that can be used for the capture of krypton and xenon and has resulted in a novel composite sorbent development procedure using synthesized mordenite as the active material. Utilizing the sorbent development procedure, Idaho National Laboratory sigma team members have developed two composite sorbents that have been evaluated for krypton and xenon capacities at ambient and 191 K temperature using numerous test gas compositions. Adsorption isotherms have been generated to predict equilibration and maximum capacities enabling modeling to support process equipment scale-up. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Management of HL deposits for the D and D of UP1 reprocessing plant - retrieval and treatment scenarios - 15295

Built in 1958 on the Marcoule CEA site, the UP1 facility, was the 1. French industrial (500 t U / year) reprocessing plant based on the PUREX process. The plant, which has stopped operation in 1997, constitutes with its auxiliary workshop (vitrification workshop, glass canister storage), one of the largest and most challenging decommissioning project in France. In about 40 years of operation, various type of fuels elements such as metallic uranium, U-Al fuel rods, Phenix breeder elements or PWR fuel have been reprocessed, thereby requiring several plant and process adaptations. Resulting from these complex process chemistry and operation history, significant fouling of the chemical plant circuits and components has occurred. The fission product (FP) concentration process is particularly concerned. Preliminary investigation performed in 2010 in the evaporator's feeding tanks revealed the presence of significant amounts of sludge and dose rates as high as 250 Gy/h. Therefore a thorough investigation campaign, including visual inspection, volume quantification, deposits sampling, and radiological characterization of the components of this workshop has been initiated in 2013. Chemical analysis performed so far show that the solids are mainly composed of zirconium phosphates, 'MoZr' compounds and nitrate salt precipitates. But the presence of insoluble fines arising from the dissolution workshop and organic residues resulting from the TBP decomposition has also been evidenced in some of the tanks. The numerous constraints associated with the management of such highly active sludge, with Cs-137 specific activity ranging from 1 to 10 GBq/g, and a complex physico-chemical composition, lead CEA to investigate the implementation of an in situ conditioning treatment able to produce a waste package complying with existing evacuation routes and/or on-site storage facilities. The full paper presents an overview of the UP1 D and D project and then focuses on the possible dismantling scenarios for the FP concentration workshop, including the evaluation of different strategies for the highly active deposits management. The investigations and deposits characterization program will be developed so as the sampling methodologies that has been specifically tuned. In the light of the best actual knowledge of the deposits properties, the recovery and conditioning treatment scenarios will be exposed, considering, as a case study, the development of a specific vitrification tool to be implemented In Situ and specifically designed to match the requirements and constraints of the D and D project: adequately dimensioned, compact, flexible with respect to the feed composition, for a limited duration of use and designed to be dismantled. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Magnox Reprocessing TDN Reactors: Utilising 3D Printing and X-Ray Imaging to Re-Design and Test Fluidising Air Nozzles - 16402

One of the key final steps in reprocessing spent nuclear fuel is the conversion of highly concentrated uranyl nitrate hexahydrate liquor [> 1000 gU/litre] into uranium trioxide (UO{sub 3}) powder by thermal decomposition using Thermal Denitration (TDN) reactors. The TDN reactors in the Magnesium non-oxidising (Magnox) fuel reprocessing plant are high aspect ratio fluidising beds, which suffer from poor fluidization and UO{sub 3} powder blockages. It is widely understood that these issues arise from the inadequate design of the fluidising air distributors (nozzles), which are located around the base of the TDN reactors. A non-active test rig was constructed at the National Nuclear Laboratory (NNL) experimental facility in Workington, Cumbria (UK) which used compressed air at ambient temperature to assess the performance of the current fluidising air nozzle designs (datum) against a range of new nozzle designs. Full-scale nozzle designs were manufactured using a 3-Dimensional (3D) printer and tested to obtain data of both quantitative and qualitative nature. NNL then collaborated with the Chemical Engineering Department at University College London (UCL) to further assess the fluidising potential of the new nozzle designs. Images of inside the fluidized bed were taken utilising a unique X-Ray facility. The results from this study will allow new nozzle designs to be recommended, manufactured and installed, which will ensure improved fluidization of the TDN reactor bed and prevent blockages with UO{sub 3} powder. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Development of On-Line Spectroscopic pH Monitoring for Nuclear Fuel Reprocessing Plants: Weak Acid Schemes

Knowledge of real-time solution properties and composition is a necessity for any spent nuclear fuel reprocessing method. Metal-ligand speciation in aqueous solutions derived from the dissolved commercial spent fuel is highly dependent upon the acid concentration/pH, which influences extraction efficiency and the resulting speciation in the organic phase. Spectroscopic process monitoring capabilities, incorporated in a counter current centrifugal contactor bank, provide a pathway for on-line real-time measurement of solution pH. The spectroscopic techniques are process-friendly and can be easily configured for on-line applications, while classic potentiometric pH measurements require frequent calibration/maintenance and have poor long-term stability in aggressive chemical and radiation environments. Our research is focused on developing a general method for on-line determination of pH of aqueous solutions through chemometric analysis of Raman spectra. Interpretive quantitative models have been developed and validated under the range of chemical composition and pH using a lactic acid/lactate buffer system. The developed model was applied to spectra obtained on-line during solvent extractions performed in a centrifugal contactor bank. The model predicted the pH within 11% for pH > 2, thus demonstrating that this technique could provide the capability of monitoring pH on-line in applications such as nuclear fuel reprocessing.

pH, spectroscopic monitoring, on-line monitoring, ↗

Covalent Adaptable Networks: Reprocessable Cross-Linked Polymers

Thermoset polymers have desirable properties, such as excellent thermal and mechanical stability, but their covalent cross-links typically prevent repair or recycling. By enabling and controlling dynamic exchange reactions within polymer networks, their covalent bonds rearrange and allow the polymer to be reshaped. These viscoelastic polymer networks, now known as covalent adaptable networks (CANs), are an important frontier for improving plastic circularity, as well as for designing valuable stimuli-responsive materials. This Review describes the history of CANs, dating back to the early days of polymer science, and the evolution of their classification and nomenclature. A comprehensive survey of dynamic reactions and linkage chemistries is provided, as well as methods to characterize and reprocess CANs. Beyond straightforward reprocessing, many advanced applications of CANs and their composites are now emerging. Lastly, we provide perspective on how the development of new chemistries, strategies to control stimuli-responsive bond exchange and mechanical properties, and a deep understanding of exchange reactions will advance this field toward scalable, sustainable, and high-value materials.

Sun, Molly [Northwestern University, Evanston, IL ↗

Numerical simulations of turbulent molecular clouds regulated by reprocessed radiation feedback from nascent super star clusters

Radiation feedback from young star clusters embedded in giant molecular clouds (GMCs) is believed to be important to the control of star formation. For the most massive and dense clouds, including those in which super star clusters (SSCs) are born, pressure from reprocessed radiation exerted on dust grains may disperse a significant portion of the cloud mass back into the interstellar medium. Using our radiation hydrodynamics code, Hyperion, we conduct a series of numerical simulations to test this idea. Our models follow the evolution of self-gravitating, strongly turbulent clouds in which collapsing regions are replaced by radiating sink particles representing stellar clusters. We evaluate the dependence of the star formation efficiency (SFE) on the size and mass of the cloud and κ, the opacity of the gas to infrared (IR) radiation. We find that the single most important parameter determining the evolutionary outcome is κ, with κ≳15 cm{sup 2} g{sup −1} needed to disrupt clouds. For κ=20−40 cm{sup 2} g{sup −1}, the resulting SFE = 50%−70% is similar to empirical estimates for some SSC-forming clouds. The opacities required for GMC disruption likely apply only in dust-enriched environments. We find that the subgrid model approach of boosting the direct radiation force L/c by a “trapping factor” equal to a cloud’s mean IR optical depth can overestimate the true radiation force by factors of ∼4−5. We conclude that feedback from reprocessed IR radiation alone is unlikely to significantly reduce star formation within GMCs unless their dust abundances or cluster light-to-mass ratios are enhanced.

79 ASTRONOMY AND ASTROPHYSICS↗

The Future of Nuclear Energy: Electrochemical Reprocessing of Fuel Takes Center Stage

Nuclear power plants use energy-dense fuel and provide dependable baseload energy without generating greenhouse gas emissions. Despite these advantages, the long-term management of used nuclear fuel (UNF) remains a key challenge due to its lifetime (hundreds of thousands of years) and radiotoxicity. The components of UNF that contribute the most to this challenge are the actinide elements. A potential solution to this issue is to separate these radioisotopes from the bulk of the UNF and recycle them as fuel in advanced nuclear reactors. These separations can be achieved using electrochemical reprocessing, which employs electrochemical conversion and electrodeposition in a high-temperature molten salt electrolyte medium to separate the actinides from UNF. In this work, we review the current status, fundamental challenges, and future prospects of electrochemical reprocessing as they relate to UNF recycling.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Insight into “Changing-look” AGN Mrk 1018 from the Fe Kα Line: The Reprocessing Gas Has Yet to Fully Respond to the Fading of the AGN

Mrk 1018 is a “changing-look” active galactic nucleus (AGN) whose optical spectrum transitioned from a Type 1.9 to a Type 1 between 1979 and 1984, and then back to a Type 1.9 in 2015. This latest transition was accompanied by a decrease in X-ray flux. We analyze the Chandra spectra from 2010 and 2016 and NuSTAR spectra from 2016, with a careful treatment of pileup in the Chandra spectrum from 2010, and self-consistently model absorption, reflection, and Fe Kα line emission in the X-ray spectra from 2016. We demonstrate that while the 2–10 keV X-ray flux decreased by an order of magnitude (1.46{sub −0.13}{sup +0.10}×10{sup −11}–1.31{sub −0.04}{sup +0.09}×10{sup −12} erg s{sup −1} cm{sup −2}), the Fe Kα equivalent width (EW) increased from 0.18{sub −0.12}{sup +0.17} to 0.61{sub −0.25}{sup +0.27} keV due to a depressed AGN continuum. We jointly fit the Chandra and NuSTAR spectra from 2016 using the physically motivated MYTorus model, and find that the torus orientation is consistent with a face-on geometry and that lines of sight intersecting the torus are ruled out. While we measure no line-of-sight absorption, we do measure a column density of N{sub H}=5.38{sub −4.0}{sup +14}×10{sup 22} cm{sup −2} for gas out of the line of sight that reprocesses the X-ray emission. We find a high relative normalization between the Compton-scattered emission and transmitted continuum, which is indicative of time lags between the primary X-ray source and reprocessing gas. We predict that the Fe Kα line will respond to the decrease in AGN flux, which would manifest as a decrease in the Fe Kα EW.

79 ASTRONOMY AND ASTROPHYSICS↗

Reprocessed MPL data sets

This dataset contains reprocessed micropulse lidar (MPL) data (equivalent to the ARM cloud mask VAP's lidar fields) which were carefully corrected for each site. These reprocessed data were used in Silber et al. (JGR, 2018). The data extend up to a height of 15 km and have vertical and temporal resolutions of 15 m and 30 s, respectively.

54 ENVIRONMENTAL SCIENCES↗

Novel Sorbent Development and Evaluation for the Capture of Krypton and Xenon from Nuclear Fuel Reprocessing Off-Gas Streams

The release of volatile radionuclides generated during Used Nuclear Fuel reprocessing in the US will most certainly need to be controlled to meet US regulatory emission limits. A US DOE sponsored Off-Gas Sigma Team has been tasked with a multi-lab collaborative research and development effort to investigate and evaluate emissions and immobilization control technologies for the volatile radioactive species generated from commercial Used Nuclear Fuel (UNF) Reprocessing. Physical Adsorption technology is a simpler and potential economical alternative to cryogenic distillation processes that can be used for the capture of krypton and xenon and has resulted in a novel composite sorbent development procedure using synthesized mordenite as the active material. Utilizing the sorbent development procedure, INL sigma team members have developed two composite sorbents that have been evaluated for krypton and xenon capacities at ambient and 191 K temperature using numerous test gas compositions. Adsorption isotherms have been generated to predict equilibration and maximum capacities enabling modeling to support process equipment scale-up.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Novel Sorbent Development and Evaluation for the Capture of Krypton and Xenon from Nuclear Fuel Reprocessing Off-Gas Streams

The release of volatile radionuclides generated during Used Nuclear Fuel reprocessing in the US will most certainly need to be controlled to meet US regulatory emission limits. A US DOE sponsored Off-Gas Sigma Team has been tasked with a multi-lab collaborative research and development effort to investigate and evaluate emissions and immobilization control technologies for the volatile radioactive species generated from commercial Used Nuclear Fuel (UNF) Reprocessing. Physical Adsorption technology is a simpler and potential economical alternative to cryogenic distillation processes that can be used for the capture of krypton and xenon and has resulted in a novel composite sorbent development procedure using synthesized mordenite as the active material. Utilizing the sorbent development procedure, INL sigma team members have developed two composite sorbents that have been evaluated for krypton and xenon capacities at ambient and 191 K temperature using numerous test gas compositions. Adsorption isotherms have been generated to predict equilibration and maximum capacities enabling modeling to support process equipment scale-up.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Separation of Xenon from Krypton in UNF Reprocessing Off-Gas

Reprocessing of used nuclear fuel (UNF) results emits several volatile radionuclides that must be removed from the bulk off gas prior to release in order to meet U.S. regulatory emission requirements. After other volatile radionuclides have been removed, krypton (Kr) remains, along with associated with xenon (Xe) in the gas stream. The half-life of Xe is short enough that by the time UNF is sufficiently cooled to be reprocessed Xe is no longer a radiological concern and it may be release to atmosphere or collected for other purposes. Kr, however, must be placed in long term storage. In order to ensure the smallest practical volume for long term storage, the Xe, which is nearly ten times the volume of Kr, must be separated from the Kr. Although cryogenic distillation has been used successfully for this purpose, high capital and operational cost, along with safety considerations, made development of gas adsorption processes for separation of Xe and Kr attractive. INL developed an engineered form sorbent consisting of silver mordenite in a polyacrylonitrile matrix (AgZ-PAN) capable of complete separation of Xe from Kr in a single pass, allowing Kr to be captured downstream with no detectable Xe present.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multiscale Evaluation of Acetohydroxamic Acid (AHA) Radiolysis Under Used Nuclear Fuel Reprocessing Solvent System Conditions

Acetohydroxamic acid (AHA) has been proposed as an alternative agent for the selective separation of plutonium and neptunium from co-extracted uranium during the reprocessing of used nuclear fuel. However, the fundamental radiolytic behavior of this molecule under envisioned process conditions – i.e., acidic biphasic solvent systems – is not sufficiently understood to support process applications. Here we present a systematic irradiation study (steady-state gamma and time-resolved pulsed electron) into the radiolytic integrity of AHA and formation of degradation products in aqueous nitric acid (HNO3) solutions (0.2 M) in presence and absence of an organic phase, comprising current (tri-butyl phosphate - TBP) and future (N,N-di-(2-ethylhexyl)butyramide - DEHBA and di-2-ethylhexylisobutyramide - DEHiBA) reprocessing ligands dissolved in n-dodecane diluent. Experimental data are complimented by predictive multiscale model calculations for the elucidation of underpinning mechanisms.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗