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At least 55 records · Page 3

Safeguards Lessons Learned from the Rokkasho Reprocessing Plant - 19502

Once operational, the Rokkasho Reprocessing Plant (RRP) will have an operating throughput of 800 MT of uranium in irradiated LWR fuel per year. In order to establish effective and efficient safeguards at RRP, the safeguards discussion with the IAEA was initiated in 1988. However, at that time there were no available models or guidelines that could be used as a reference and multiple difficulties were recognized for the implementation of safeguards into a large scale reprocessing plant. Therefore, from 1988 to 1992, a multinational forum, referred to as LASCAR (Large Scale Reprocessing Plant Safeguards) [1], provided the recommendations on how an effective safeguards approach could be implemented into a large scale reprocessing plant while efficiently using existing resources. During the course of safeguards discussions between the IAEA, the State, and JNFL, the use of operator's equipment and measurement systems (by signal splitting with authentication) for inspections was studied. JNFL also examined incorporating inspection requirements into the process design: to reduce the costs associated with system installation and future system maintenance and to ensure effective, efficient, and credible safeguards implementation into the RRP (this approach has essentially become the 'Safeguards by Design (SBD)' process). From these studies and JNFL's experience of implementing safeguards into a new plant [2], JNFL established and applied signal splitting from operator's equipment as a means for providing inspectors required safeguards information. In addition, the LASCAR findings were utilized to establish the safeguards implemented into the RRP. Safeguards implementation into RRP commenced March 31, 2006. On June 4, 2008, the IAEA approved the 'integrated safeguards approach' for RRP. This paper provides a high level overview of the major safeguards implemented at RRP and the lessons learned from this implementation that can be applied to existing or future similar facilities. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Dioctyl ether radiolysis under used nuclear fuel reprocessing conditions: Foundational knowledge for the development of sacrificial ligand grafts

Radiation-induced ligand destruction and concomitant degradation product formation is unavoidable under envisioned used nuclear fuel reprocessing conditions, and ultimately limits the recyclability of a given solvent system formulation. With this in mind, a novel approach to ligand innovation for advanced separations processes is in the design of tailored “protomolecules,” which when exposed to ionizing radiation undergo desired chemical transformations, thereby allowing for a reprocessing solvent system to advantageously evolve with absorbed radiation dose. Here we provide foundational knowledge for the time-resolved (electron pulse) and steady-state (cobalt-60 gamma) radiolytic behavior of dioctyl ether, a protomolecule grafting surrogate. Gamma irradiation of single-phase solutions of dioctyl ether (5–100 vol.%) in n-dodecane resulted in the loss of dioctyl ether (G = -0.72 µmol J –1 ) and the formation of octane (G = 0.11 µmol J –1 ) and octanol (G = 0.15 µmol J –1 ) degradation products, the latter of which is a known reprocessing phase modifier and radioprotectant. Further, these radiation-induced changes were attributed to direct radiation effects, for more concentrated dioctyl ether solutions, and indirect radiation effects, predominantly driven by the reaction of dioctyl ether with the dodecane radical cation, for which we report a second-order rate coefficient of k = (1.53 ± 0.05) × 10 10 L mol –1 s –1 . Under typical biphasic extraction (4.0 mol L –1 HNO 3 ) and strip (0.1 mol L –1 HNO 3 ) reprocessing conditions, gamma irradiation of 5 vol.% dioctyl ether solvent systems afforded negligible change in the rate of parent molecule destruction but promoted significant differences in the radiolytic behavior of its degradation products. These differences are attributed to their respective interactions with [dioctyl ether/HNO 3 /H 2 O] and [octanol/HNO 3 /H 2 O] adducts extracted into the organic phase. Overall, these results support the grafting of ether linkages to advanced separations ligands (e.g., modified diglycolamides).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

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).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Reprocessable polyhydroxyurethane networks reinforced with reactive polyhedral oligomeric silsesquioxanes (POSS) and exhibiting excellent elevated temperature creep resistance

The rapid development of covalent adaptable networks or vitrimers shows promise for addressing the long-standing recycling issues associated with conventional, permanently cross-linked thermosets. At the same time, it is important to demonstrate that properties of reprocessable polymer networks can be optimized to meet the ongoing demand for high-performance materials. We have fabricated reprocessable polyhydroxyurethane (PHU) network composites reinforced with reactive polyhedral oligomeric silsesquioxanes (POSS). With functionalized POSS serving as a fraction of the cross-linkers, the PHU–POSS network nanocomposites exhibit significantly enhanced storage modulus at the rubbery plateau region relative to the neat PHU network. With up to 10 wt% POSS loading, these network composites can undergo melt-state reprocessing at 140 °C with 100% property recovery associated with cross-link density. We also show that hydroxyurethane dynamic chemistry leads to excellent creep resistance at elevated temperature up to 90 °C and is unaffected by reactive incorporation of POSS. In conclusion, this study demonstrates the effectiveness of POSS as nanofillers for designing high-performance, organic-inorganic dynamic PHU networks with excellent reprocessability.

42 ENGINEERING↗

Reprocessable and Recyclable Polymer Network Electrolytes via Incorporation of Dynamic Covalent Bonds

Mechanically durable polymer network electrolytes are desirable for batteries; however, covalent cross-linking adversely affects their large-scale manufacturing, and they are difficult to recycle post-lifespan. In this work, we address the electrolyte reprocessability and recyclability challenges through the use of dynamic covalent bonds for polymer network solid electrolytes. Specifically, the associative dynamic vinylogous urethane motif is incorporated into a poly(ethylene oxide) network electrolyte containing lithium bis(fluorosulfonyl)imide (LiFSI) salt. The resulting dynamic covalent network electrolyte possesses a modest ion conductivity (~10–5 S/cm at room temperature) and good reprocessability. Stress–relaxation studies indicate that the LiFSI salt can catalyze the bond exchange and enhance the network dynamics. Furthermore, the reprocessability associated with bond exchange can be tuned by simply adjusting the formulation of reagent compositions, in which increasing the amount of excess amine or using a shorter chain of PEO prepolymer can further enhance the network dynamics and corresponding reprocessability.

25 ENERGY STORAGE↗

Spiroborate-Linked Ionic Covalent Adaptable Networks with Rapid Reprocessability and Closed-Loop Recyclability

Covalent adaptable networks (CANs) represent a novel class of polymeric materials crosslinked by dynamic covalent bonds. Since their first discovery, CANs have attracted great attention due to their high mechanical strength and stability like conventional thermosets under service conditions and easy reprocessability like thermoplastics under certain external stimuli. Here, we report the first example of ionic covalent adaptable networks (ICANs), a type of crosslinked ionomers, consisting of negatively charged backbone structures. More specifically, two ICANs with different backbone compositions were prepared through spiroborate chemistry. Given the dynamic nature of the spiroborate linkages, the resulting ionomer thermosets display rapid reprocessability and closed-loop recyclability under mild conditions. The materials mechanically broken into smaller pieces can be reprocessed into coherent solids at 120 °C within only 1 min with nearly 100% recovery of the mechanical properties. Upon treating the ICANs with dilute hydrochloric acid at room temperature, the valuable monomers can be easily chemically recycled in almost quantitative yield. Furthermore, this work demonstrates the great potential of spiroborate bonds as a novel dynamic ionic linkage for development of new reprocessable and recyclable ionomer thermosets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluation of Tritium Management Approaches on Tritium Waste Volumes in Reprocessing Plants

Four radionuclides have been identified as likely to be volatilized during the reprocessing of nuclear fuel in amounts such that their gaseous release needs to be controlled to meet US regulatory requirements. These radionuclides are 3 H, 14 C, 85 Kr, and 129 I. While iodine has been the focus of a number of studies due to the high decontamination factor (DF) requirements on multiple off-gas pathways, it is also clear that the control of tritium could also be a significant issue for future reprocessing plants, especially if processing relatively short-cooled fuels (e.g., <10-yr post reactor discharge). Like iodine, tritium contained in a used nuclear fuel (UNF) matrix will be released into the liquid and off-gas streams during fuel reprocessing. The amount released into the process streams is a function of the type and burnup of the fuel processed, and the chemical processes and processing conditions employed within the reprocessing plant. The required DF for 3 H could be as high as 200, depending on the age of the fuel processed. This study examines three main cases with a number of subcases for comparative purposes.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Pressure Induced Densification and Compression in a Reprocessed Borosilicate Glass

Pressure induced densification and compression of a reprocessed sample of borosilicate glass has been studied by X-ray radiography and energy dispersive X-ray diffraction using a Paris-Edinburgh (PE) press at a synchrotron X-ray source. The reprocessing of a commercial borosilicate glass was carried out by cyclical melting and cooling. Gold foil pressure markers were used to obtain the sample pressure by X-ray diffraction using its known equation of state, while X-ray radiography provided a direct measure of the sample volume at high pressure. The X-ray radiography method for volume measurements at high pressures was validated for a known sample of pure α-Iron to 6.3 GPa. A sample of reprocessed borosilicate glass was compressed to 11.4 GPa using the PE cell, and the flotation density of pressure recovered sample was measured to be 2.755 gm/cc, showing an increase in density of 24%, as compared to the starting sample. The initial compression of the reprocessed borosilicate glass measured by X-ray radiography resulted in a bulk modulus of 30.3 GPa in good agreement with the 32.9 GPa value derived from the known elastic constants. This method can be applied to variety of amorphous materials under high pressures.

36 MATERIALS SCIENCE↗

Joint Modeling of Quasar Variability and Accretion Disk Reprocessing Using Latent Stochastic Differential Equations

Quasars are bright active galactic nuclei powered by the accretion of matter around supermassive black holes at the center of galaxies. Their stochastic brightness variability depends on the physical properties of the accretion disk and black hole. The upcoming Rubin Observatory Legacy Survey of Space and Time (LSST) is expected to observe tens of millions of quasars, so there is a need for efficient techniques like machine learning that can handle the large volume of data. Quasar variability is believed to be driven by an X-ray corona, which is reprocessed by the accretion disk and emitted as UV/optical variability. We are the first to introduce an auto-differentiable simulation of the accretion disk and reprocessing. We use the simulation as a direct component of our neural network to jointly model the driving variability and reprocessing, trained with supervised learning on simulated LSST-like 10 yr quasar light curves. We encode the light curves using a transformer encoder, and the driving variability is reconstructed using latent stochastic differential equations, a physically motivated generative deep learning method that can model continuous-time stochastic dynamics. By embedding the physical processes of the driving signal and reprocessing into our network, we achieve a model that is more robust and interpretable. We demonstrate that our model outperforms a Gaussian process regression baseline and can infer accretion disk parameters and time delays between wave bands, even for out-of-distribution driving signals. Our approach provides a powerful framework that can be adapted to solve other inverse problems in multivariate time series.

Fagin, Joshua [City Univ. of New York (CUNY), NY (↗

Optical reprocessing of gamma-ray bursts

One model for the optical flashes associated with three cosmic gamma-ray burst sources invokes the reprocessing of some of the gamma-radiation emitted by a hypothesized collapsed object in the surface layers of a nearby companion star. This model was investigated by carrying out detail, fully hydrodynamical calculations of such reprocessing in the surface layers of very low mass stars. It is found that, at most, 7 percent of the gamma-ray fluence incident on the companion star is reprocessed into the blue band; the time scale for this reprocessing is typically 100 s, which is long compared to the duration of the gamma-ray burst itself. Using this result, it is shown that there is marginal agreement between the observed and calculated ratios of gamma-ray fluence to optical fluence at earth.

Melia, F.↗

Gamma-ray burst reprocessing in an accretion disk

The observational consequences of the reprocessing of gamma-ray burst (GRB) photons by an accretion disk surrounding a neutron star are explored. Reprocessing of gamma rays by cold disks driven by dynamical viscosity of nonrelativistic, degenerate electrons results in an optical/UV fluence relative to the gamma-ray fluence at earth of greater than 0.001, for GRB energies of (1-10) x 10 to the 37th ergs, and distances of 15-250 pc. The spectrum peaks in the optical/UV with a soft X-ray cutoff due to the inner edge of the disk, which lies very near the surface of the neutron star for magnetic fields less than 1 TG. The optical/UV peak is partially due to reprocessing in the outer part of the cold disk, which remains optically thick to gamma rays. At these distances, a positive identification of a quiescent counterpart is expected at an IR (K) sensitivity less than 2 microJy. On the other hand, compact binary systems with standard alpha disks and accretion rates resulting from Roche-lobe overflow must be located at least several hundred pc away in order to have escaped detection down to the current IR sensitivity. The optical/UV fluence resulting from reprocessing in these systems is deficient by at least an order of magnitude compared to the observed values.

Melia, Fulvio↗

On the Reprocessing and Reanalysis of Observations for Climate

The long observational record is critical to our understanding of the Earths climate, but most observing systems were not developed with a climate objective in mind. As a result, tremendous efforts have gone into assessing and reprocessing the data records to improve their usefulness in climate studies. The purpose of this paper is to both review recent progress in reprocessing and reanalyzing observations, and to summarize the challenges that must be overcome in order to improve our understanding of climate and variability. Reprocessing improves data quality through more scrutiny and improved retrieval techniques for individual observing systems, while reanalysis merges many disparate observations with models through data assimilation, yet both aim to provide an climatology of Earth processes. Many challenges remain, such as tracking the improvement of processing algorithms and limited spatial coverage. Reanalyses have fostered significant research, yet reliable global trends in many physical fields are not yet attainable, despite significant advances in data assimilation and numerical modeling. Oceanic reanalyses have made significant advances in recent years, but will only be discussed here in terms of progress toward integrated Earth system analyses. Climate data sets are generally adequate for process studies and large-scale climate variability. Communication of the strengths, limitations and uncertainties of reprocessed observations and reanalysis data, not only among the community of developers, but also with the extended research community, including the new generations of researchers and the decision makers is crucial for further advancement of the observational data records. It must be emphasized that careful investigation of the data and processing methods are required to use the observations appropriately.

Uncertainty↗

Impact of Reprocessed Uranium Management on the Homogeneous Recycling of Transuranics in PWRs

This article presents the results of a neutronics analysis related to the homogeneous recycling of transuranics (TRU) in PWRs with a MOX fuel using enriched uranium instead of depleted uranium. It also addresses an often, if not always, overlooked aspect related to the recycling of TRU in PWRs, namely the use of reprocessed uranium. From a neutronics point of view, it is possible to multi-recycle the entirety of the plutonium with or without neptunium and americium in a PWR fleet using MOX-EU fuel in between one third and two thirds of the fleet. Recycling neptunium and americium with plutonium significantly decreases the decay heat of the waste stream between 100 to 1,000 years compared to those of an open fuel cycle or when only plutonium is recycled. The uranium present in MOX-EU used fuel still contains a significant amount of 235 uranium and recycling it makes a major difference on the natural uranium needs. For example, a PWR fleet recycling its plutonium, neptunium and americium in MOXEU needs 28 percent more natural uranium than a reference UO 2 open cycle fleet generating the same energy if the reprocessed uranium is not recycled and 19 percent less if the reprocessed uranium is recycled back in the reactors, i.e. a 47 percent difference.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Aqueous Reprocessing of Used Nuclear Fuel

Aqueous reprocessing of used nuclear fuel has a long history of successful operation worldwide. The history of aqueous reprocessing and a description of current and past operating aqueous reprocessing facilities are provided and the main types of solvent extraction equipment utilized in the nuclear industry are described. While the PUREX process is well established for separating U and Pu from used nuclear fuel, numerous variants to the PUREX process are being developed and are described. Finally, advanced separation processes in which minor actinides are separated from the used nuclear fuel are a key research focus worldwide. These processes and the current state of development are discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Commercial Nuclear Reprocessing in the United States

The short presentation outline: Reprocessing Overview; Events leading up to Carter’s Policy; Results of the decision; Policy since Nuclear Nonproliferation Act. Conclusions reached: Reprocessing ban has become an easy and visible fix to the public concern about proliferation, but has not completely stopped proliferation; and, Reprocessing needs to become detached from political considerations, so technical research can continue, regardless of the policy decisions we decide to take.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Abatement of radioiodine in aqueous reprocessing off-gas

The reprocessing used nuclear fuel (UNF) releases volatile fission and activation products, including 129 I, into the off-gas of a processing plant. Mitigation of the release of vapor phase radionuclides is necessary for meeting regulatory requirements in the United States and other countries. In an aqueous reprocessing plant, volatile radioiodine could be present in several forms, depending on the chemistry of the process used. Inorganic iodine will be the predominate species in any shearing or voloxidation pretreatment off-gas and dissolver off-gas (DOG). Organic iodides such as CH 3 I, C 4 H 9 I, and C 12 H 25 I have been proposed to be generated during solvent extraction; thus, these species must be captured from the vessel off-gas (VOG). The abatement of inorganic and organic iodide species to meet United States regulatory requirements has been demonstrated in laboratory experiments using Ag-based solid sorbents. The data presented in this paper includes the effect of gas composition (e.g., the presence of water vapor and NO x ), iodine speciation (I 2 , CH 3 I, C 4 H 9 I, C 12 H 25 I), and sorbent bed parameters (e.g., temperature, sorbent age) on complete iodine capture on Ag-mordenite in an aqueous reprocessing plant.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Swift Monitoring of NGC 4151: Evidence for a Second X-Ray/UV Reprocessing

Swift monitoring of NGC 4151 with an ∼6 hr sampling over a total of 69 days in early 2016 is used to construct light curves covering five bands in the X-rays (0.3–50 keV) and six in the ultraviolet (UV)/optical (1900–5500 Å). The three hardest X-ray bands (>2.5 keV) are all strongly correlated with no measurable interband lag, while the two softer bands show lower variability and weaker correlations. The UV/optical bands are significantly correlated with the X-rays, lagging ∼3–4 days behind the hard X-rays. The variability within the UV/optical bands is also strongly correlated, with the UV appearing to lead the optical by ∼0.5–1 days. This combination of ≳3 day lags between the X-rays and UV and ≲1 day lags within the UV/optical appears to rule out the “lamp-post” reprocessing model in which a hot, X-ray emitting corona directly illuminates the accretion disk, which then reprocesses the energy in the UV/optical. Instead, these results appear consistent with the Gardner and Done picture in which two separate reprocessings occur: first, emission from the corona illuminates an extreme-UV-emitting toroidal component that shields the disk from the corona; this then heats the extreme-UV component, which illuminates the disk and drives its variability.

79 ASTRONOMY AND ASTROPHYSICS↗

Dismantling of HLLW Process Installations of the German Reprocessing Facility (WAK) - Progress and first Experiences in Hot Application of Remote Techniques - 17083

Decommissioning and dismantling of the former German Pilot Reprocessing Plant Karlsruhe (WAK) including the Vitrification Facility (VEK) is being executed in different Project steps related to the reprocessing, HLLW storage and vitrification complexes. While inside the reprocessing building the total inventory of process equipment has already been dismantled and disposed of, the HLLW storage and vitrification complex has been placed out of operation since vitrification was finalized in year 2010 and is now under deconstruction. This paper describes the progress and experiences made in dismantling of the process cells of the HLLW storage building. The major challenges of the dismantling are the high dose rates up to 70 Sv/h and the locking technology for the removal of the hot cell installations. As well as the adaption and extensive prototype testing of the remote handling equipment which was applied to dismantle the hot cell equipment prior to the start of the dismantling. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗