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At least 127 records · Page 7

AN X-RAY SPECTRAL MODEL OF REPROCESSING BY SMOOTH AND CLUMPY MOLECULAR TORI IN ACTIVE GALACTIC NUCLEI WITH THE MONACO FRAMEWORK

We construct an X-ray spectral model of reprocessing by a torus in an active galactic nucleus (AGN) with the Monte Carlo simulation framework MONACO. Two torus geometries of smooth and clumpy cases are considered and compared. In order to reproduce a Compton shoulder accurately, MONACO includes not only free electron scattering but also bound electron scattering. Raman and Rayleigh scattering are also treated, and scattering cross sections dependent on chemical states of hydrogen and helium are included. Doppler broadening by turbulence velocity can be implemented. Our model gives results consistent with other available models, such as MYTorus, except for differences due to different physical parameters and assumptions. We studied the dependence on torus parameters for a Compton shoulder, and found that a intensity ratio of a Compton shoulder to the line core mainly depends on column density, inclination angle, and metal abundance. For instance, an increase of metal abundance makes a Compton shoulder relatively weak. Also, the shape of a Compton shoulder depends on the column density. Furthermore, these dependences become different between smooth and clumpy cases. Then, we discuss the possibility of ASTRO-H/SXS spectroscopy of Compton shoulders in AGN reflection spectra.

79 ASTRONOMY AND ASTROPHYSICS↗

Spectroscopic Online Monitoring for Process Control and Safeguarding of Radiochemical Fuel Reprocessing Streams - 13553

There is a renewed interest worldwide to promote the use of nuclear power and close the nuclear fuel cycle. The long term successful use of nuclear power is critically dependent upon adequate and safe processing and disposition of the used nuclear fuel. Liquid-liquid extraction is a separation technique commonly employed for the processing of the dissolved spent nuclear fuel. The instrumentation used to monitor these processes must be robust, require little or no maintenance, and be able to withstand harsh environments such as high radiation fields and aggressive chemical matrices. This paper discusses application of absorption and vibrational spectroscopic techniques supplemented by physicochemical measurements for radiochemical process monitoring. In this context, our team experimentally assessed the potential of Raman and spectrophotometric techniques for on-line real-time monitoring of the U(VI)/nitrate ion/nitric acid and Pu(IV)/Np(V)/Nd(III), respectively, in solutions relevant to spent fuel reprocessing. Both techniques demonstrated robust performance in the repetitive batch measurements of each analyte in a wide concentration range using simulant and commercial dissolved spent fuel solutions. Static spectroscopic measurements served as training sets for the multivariate data analysis to obtain partial least squares predictive models, which were validated using on-line centrifugal contactor extraction tests. Satisfactory prediction of the analytes concentrations in these preliminary experiments warrants further development of the spectroscopy-based methods for radiochemical safeguards and process control. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

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.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Peculiarities of highly burned-up NPP SNF reprocessing and new approach to simulation of solvent extraction processes

Substantiation, general description and performance characteristics of a reprocessing flowsheet for WWER-1000 spent fuel with burn-up >60 GW*day/t U is given. Pu and U losses were <0.1%, separation factor > 10{sup 4}; their decontamination factor from γ-emitting fission products was 4*10{sup 4} and 3*10{sup 7}, respectively. Zr, Tc, Np removal was >98% at U and Pu losses <0.05%. A new approach to simulation of extraction equilibrium has been developed. It is based on a set of simultaneous chemical reactions characterized by apparent concentration constants. A software package was created for simulation of spent fuel component distribution in multistage countercurrent extraction processes in the presence of salting out agents. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Corrosion property of 9Cr-ODS steel in nitric acid solution for spent nuclear fuel reprocessing

Corrosion tests of oxide dispersion strengthened with 9% Cr (9Cr-ODS) steel, which is one of the desirable materials for cladding tube of sodium-cooled fast reactors, in pure nitric acid solution, spent FBR fuel solution, and its simulated solution were performed to understand the corrosion behavior in a spent nuclear fuel reprocessing. In this study, the 9Cr-ODS steel with lower effective chromium content was evaluated to understand the corrosion behavior conservatively. As results, the tube-type specimens of the 9Cr-ODS steels suffered severe weight loss owing to active dissolution at the beginning of the immersion test in pure nitric acid solution in the range from 1 to 3.5 M. In contrast, the weight loss was decreased and they showed a stable corrosion in the higher nitric acid concentration, the dissolved FBR fuel solution, and its simulated solution by passivation. The corrosion rates of the 9Cr-ODS steel in the dissolved FBR fuel solution and its simulated solution were 1-2 mm/y and showed good agreement with each other. The passivation was caused by the shift of corrosion potential to noble side owing to increase in nitric acid concentration or oxidative ions in the dissolved FBR fuel solution and the simulated spent fuel solution. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Vitrification of IFR and MSBR halide salt reprocessing wastes

Both of the genuinely sustainable (breeder) nuclear fuel cycles (IFR - Integral Fast Reactor - and MSBR - Molten Salt Breeder Reactor -) studied by the USA's national laboratories would generate high level reprocessing waste (HLRW) streams consisting of a relatively small amount ( about 4 mole %) of fission product halide (chloride or fluoride) salts in a matrix comprised primarily (about 95 mole %) of non radioactive alkali metal halide salts. Because leach resistant glasses cannot accommodate much of any of the halides, most of the treatment scenarios previously envisioned for such HLRW have assumed a monolithic waste form comprised of a synthetic analog of an insoluble crystalline halide mineral. In practice, this translates to making a 'substituted' sodalite ('Ceramic Waste Form') of the IFR's chloride salt-based wastes and fluoroapatite of the MSBR's fluoride salt-based wastes. This paper discusses my experimental studies of an alternative waste management scenario for both fuel cycles that would separate/recycle the waste's halide and immobilize everything else in iron phosphate (Fe-P) glass. It will describe both how the work was done and what its results indicate about how a treatment process for both of those wastes should be implemented (fluoride and chloride behave differently). In either case, this scenario's primary advantages include much higher waste loadings, much lower overall cost, and the generation of a product (glass) that is more consistent with current waste management practices. (author)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Multiple recycle of REMIX fuel based on reprocessed uranium and plutonium mixture in thermal reactors

REMIX fuel consumption in WWER-1000 is considered. REMIX fuel is fabricated from non-separated mixture of uranium and plutonium obtained during NPP spent fuel reprocessing with further makeup by enriched natural uranium. It makes possible to recycle several times the total amount of uranium and plutonium obtained from spent fuel with 100% loading of the WWER-1000 core. The stored SNF could be also involved in REMIX fuel cycle by enrichment of regenerated uranium. The same approach could be applied to closing the fuel cycle of CANDU reactors. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The used nuclear fuel problem - can reprocessing and consolidated storage be complementary?

This paper describes our CISF (Consolidated Interim Storage Facilities) and Reprocessing Facility concepts and show how they can be combined with a geologic repository to provide a comprehensive system for dealing with spent fuels in the USA. The performance of the CISF was logistically analyzed under six operational scenarios. A 3-stage plan has been developed to establish the CISF. Stage 1: the construction at the CISF site of only a rail receipt interface and storage pad large enough for the number of casks that will be received. The construction of the CISF Canister Handling Facility, the Storage Cask Fabrication Facility, the Cask Maintenance Facility and supporting infrastructure are performed during stage 2. The construction and placement into operation of a water-filled pool repackaging facility is completed for Stage 3. By using this staged approach, the capital cost of the CISF is spread over a number of years. It also allows more time for a final decision on the geologic repository to be made. A recycling facility will be built, this facility will used the NUEX recycling process that is based on the aqueous-based PUREX solvent extraction process, using a solvent of tri-N-butyl phosphate in a kerosene diluent. It is capable of processing spent fuels at a rate of 5 MT per day, at burn-ups up to 50 GWD per ton of spent fuels and a minimum of 5 years out-of-reactor cooling.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Study on release and transport of aerial radioactive materials in reprocessing plants

The release and transport characteristics of radioactive materials at a boiling accident of the high active liquid waste (HALW) in a reprocessing plant have been studied for improving experimental data of source terms of the boiling accident. In the study, a heating test and a thermogravimetry and differential thermal analysis (TG-DTA) test were conducted. In the heating test using a simulated HALW, it was found that ruthenium was mainly released into the air in the form of gas and that non-volatile elements were released into the air in the form of mist. In the TG-DTA test, the rate constants and reaction heat of thermal decomposition of ruthenium nitrosyl nitrate were obtained from TG and DTA curves. (authors)

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

New method of uranium and plutonium extraction in reprocessing of the spent nuclear fuel

It is shown that a two-stage process of uranium and plutonium extraction during the reprocessing of spent nuclear fuel solves the problem of obtaining a high-concentrated extract without increasing the loss risk with raffinate and avoids the accumulation of plutonium in the unit. A possible further optimization of the process would be the creation of steps inside the stages.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An advanced hybrid reprocessing system based on UF{sub 6} volatilization and chromatographic separation

To recover U, Pu, MA (Np, Am, Cm) and some specific fission products FPs (Cs, Sr, Tc, etc.) from various spent nuclear fuels (LWR/FBR: Oxide, Metal Fuels), we are studying an advanced hybrid reprocessing system based on UF6 volatilization (Pyro) and chromatographic separation (Aqueous). Spent fuels are de-cladded by means of thermal and mechanical methods and then applied to the fluorination/volatilization process, which selectively recovers the most amount of U. Then, the remained fuel components are converted to oxides and dissolved by HNO{sub 3} solution. Compared to U, since Pu, MA and FPs are significantly less abundant in spent fuels, the scale of the aqueous separation process could become reasonably small and result in less waste. For the chromatographic separation processes, we have prepared different types of porous silica-based organic/inorganic adsorbents with fast diffusion kinetics, improved chemical stability and low pressure drop in a packed column. So they are advantageously applicable to efficient separation of the actinides and FP elements from the fuel dissolved solution. In this work, adsorption and separation behavior of representative actinides and FP elements was studied. Small scale separation tests using simulated and genuine fuel dissolved solutions were carried out to verify the feasibility of the proposed process. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Improvements to neutron detection of Pu in solvent for an aqueous buffer tank, magnox reprocessing plant, Sellafield - 14216

The PP Active Feed Tank (PPAFT) is a buffer tank that is not safe by geometry and which is located between the Medium Active (MA) and Plutonium Purification (PP) cycles of the chemical separation process in the Magnox Reprocessing Plant. The PPAFT receives Pu nitrate in acid which has been conditioned ready for the extraction of Pu with TBP/OK (tri-butyl phosphate in kerosene) solvent in the PP Cycle. The criticality safety case for the PPAFT recognises that during both normal operations and potential maloperations solvent which is dissolved (TBP which is present in solution but can be released upon a change in acidity) and entrained (TBP/OK physically carried over but not in solution) will accumulate in the PPAFT. The only practicable route out for Pu in solvent in the PPAFT is the normal process route out from the base of the PPAFT to the PP cycle through intermediate vacuum lift and feed vessels. However, the dished end base of the PPAFT and the intermediate vacuum lift and feed vessels are of particularly challenging geometry. There are five neutron monitors placed around the PPAFT for the detection of Pu in solvent. The original design intent of the neutron detection system was that any single monitor should be able to reveal an accumulation of Pu in solvent before it would potentially be unsafe if fed downstream. However, over time there have been changes to the fuel feed and chemical process of the plant which have had the potential to affect the performance of the neutron monitoring system. The ability of the neutron monitoring system to function to its original intent was questioned. Work has recently been carried out to investigate the capabilities of the PPAFT neutron monitoring system for current plant conditions and to identify potential improvements while making best use of the existing neutron monitors. It was found that moving a neutron monitor from the side to the top of the PPAFT and adding alarms based on the ratio of signals from multiple neutron detectors would be effective in improving detection of Pu in solvent. This paper describes the challenges involved in detecting thin layers of Pu in solvent using neutron monitors, discusses the improvements made to the PPAFT neutron monitors and details the combination of real plant data and modelling with the shielding code MCBEND used to provide confidence in the enhanced neutron monitoring system. (author)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Silver Sulfide and Silver Sulfate as Aging Byproducts and Adsorbents for Gaseous Iodine Capture in Spent Nuclear Fuel Reprocessing

While it is considered a promising adsorbent for radioiodine capture in spent nuclear fuel reprocessing off-gas, silver functionalized silica aerogel (Ag 0 -aerogel) experiences a capacity loss when exposed to other off-gas components (O 2 , H 2 O, NO, and NO 2 ) through a process known as aging. Ag 2 S and Ag 2 SO 4 were identified as major byproducts of aging, but their impact on iodine adsorption remains unclear. Thus, to further investigate aging, we loaded Ag 2 S and Ag 2 SO 4 powders with molecular iodine (I 2 ) at 150 °C and characterized their properties. The I 2 adsorption capacity of Ag 2 SO 4 was 0.12 wt % after 72 h, suggesting its formation directly reduces the capacity of the Ag 0 -aerogel. Conversely, Ag 2 S had an iodine capacity of 86.8 wt % and near total Ag utilization after 240 h. Given its high capacity and availability, we evaluated the feasibility of Ag 2 S as an I 2 adsorbent in future applications. Finally, several drawbacks need to be overcome, including the relatively slow uptake rate, potential emission of another hazardous byproduct (SO 2 ), and potential aging effects (e.g., Ag 2 S conversion to Ag 2 SO 4 ) before Ag 2 S can be applied for the radioiodine capture process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers

Linear–bottlebrush–linear (LBBL) triblock copolymers represent an emerging system for creating multifunctional nanostructures. Their self-assembly depends on molecular architecture but remains poorly explored. We synthesize polystyrene- block -bottlebrush polydimethylsiloxane- block -polystyrene triblock copolymers with controlled molecular architecture and use them as a model system to study the self-assembly of LBBL polymers. Unlike classical stiff rod-flexible linear block copolymers that are prone to form highly ordered nanostructures such as lamellae, at small weight fractions of the linear blocks, LBBL polymers self-assemble to a disordered sphere phase, regardless of the bottlebrush stiffness. Microscopically, characteristic lengths increase with the bottlebrush stiffness by a power of 2/3, which is captured by a scaling analysis. Macroscopically, the formed nanostructures are ultrasoft, reprocessable elastomers with shear moduli of about 1 kPa, two orders of magnitude lower than that of conventional polydimethylsiloxane elastomers. Our results provide insights on exploiting the self-assembly of LBBL polymers to create soft functional nanostructures.

36 MATERIALS SCIENCE↗

Mechanically robust and reprocessable imine exchange networks from modular polyester pre-polymers

Covalent adaptable networks (CANs) containing reversible cross-links impart recyclability to thermoset materials without sacrificing their desirable properties (e.g. high tensile strength and solvent resistance). In addition to thermal recycling, the sustainability of these materials may be further improved by incorporating bio-sourced monomers or by enabling alternate end-of-life fates, such as biodegradation or recovery of starting materials. The alternating ring-opening copolymerisation of epoxides and cyclic anhydrides permits the modular synthesis of polyester pre-polymers that can then be cross-linked to form dynamic imine-linked networks. In this work, we report the synthesis and characterisation of five imine exchange polyester CANs with varied cross-linking densities and pre-polymer architectures. While the materials exhibit characteristic thermoset properties at service temperatures, differences in pre-polymer architecture produce distinct dynamic mechanical effects at elevated temperatures. The networks may be thermally reprocessed with full recovery of their tensile strengths and cross-linking densities, dissociated to pre-polymer, or hydrolytically degraded.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DEVELOPMENT OF A HYDROGEN MORDENITE SORBENT FOR THE CAPTURE OF KRYPTON FROM USED NUCLEAR FUEL REPROCESSING OFF-GAS STREAMS

A novel new sorbent for the separation of krypton from off-gas streams resulting from the reprocessing of used nuclear fuel has been developed and evaluated. A hydrogen mordenite powder was successfully incorporated into a macroporous polymer binder and formed into spherical beads. The engineered form sorbent retained the characteristic surface area and microporosity indicative of mordenite powder. The sorbent was evaluated for krypton adsorption capacities utilizing thermal swing operations achieving capacities of 100 mmol of krypton per kilogram of sorbent at a temperature of 191 K. A krypton adsorption isotherm was also obtained at 191 K with varying krypton feed gas concentrations. Adsorption/desorption cycling effects were also evaluated with results indicating that the sorbent experienced no decrease in krypton capacity throughout testing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterization and simulation of soft gamma-ray mirrors for their use with spent fuel rods at reprocessing facilities

The use of a grazing incidence optic to selectively reflect K-shell fluorescence emission and isotope-specific lines from special nuclear materials is a highly desirable nondestructive analysis method for use in reprocessing fuel environments. Preliminary measurements have been performed, and a simulation suite has been developed to give insight into the design of the x ray optics system as a function of the source emission, multilayer coating characteristics, and general experimental configurations. As a result, the experimental results are compared to the predictions from our simulation toolkit to illustrate the ray-tracing capability and explore the effect of modified optics in future measurement campaigns.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗