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Pu IV borophosphate crystallized from a complex solution in a borosilicate glass vial after one year. The suspected leaching of B from the glass vial could have important implications for the corrosion of vitrified nuclear waste.
CaO-SiO{sub 2}-B{sub 2}O{sub 3}-P{sub 2}O{sub 5} glasses have been studied by varying ratios of Copper oxide and Zinc oxide. Glasses were prepared using Sol-Gel technique. Opitical Basicity and oxide ion Polarizability were calculated and discussed in relation with non bridging Oxygen ions (NBOs). Optical basicity is average electron donating capability of an oxide atom. All glasses had a little difference in optical basicity and polarizability values but CZ8 glass (20CaO-60SiO{sub 2}-5B{sub 2}O{sub 3}-5P{sub 2}O{sub 5}-2CuO-8ZnO) came out to show highest optical basicity and polarizability with value 0.5177 and 0.9798 respectively. This showed the highest electron donating tendency of CZ8 glass and highest number of NBOs. These were minimum for CZ2 glass with 8CuO and 2ZnO. In aspect of optical basicity and polarizability glasses follow the series CZ2 < CZ4 < CZ6 < CZ8. Increasing concentration of ZnO and decreasing concentration of CuO lead to higher optical basicity and oxide ion polarizability.
We report a detailed design, fabrication, and characterization of 6 x 6 cm(2) fast timing photodetectors based on next-generation microchannel plates (MCPs). The whole assembly is made of low-cost borosilicate glass materials and hermetically sealed with a bialkali photocathode in a vacuum. The flexible photodetector design provides the potential of modifying individual components as well as the entire configuration to fit for different applications. A series of prototype MCP-photodetectors were fabricated following a step-by-step process including functionalization of glass capillary array through atomic layer deposition, MCP baking and scrubbing, photocathode deposition, and hermetic thermo-compression sealing. The prototype MCP-photodetectors exhibit electron gains well beyond 107 level with good relative uniformity. An excellent rise time of 439 ps, timing distribution root-mean-square at a single photoelectron mode of 105 ps, a timing resolution of 20 ps, and magnetic field tolerance up to 1.3 T were achieved for a photodetector with 10 mu m pore size MCPs, comparing to that of 536 ps, 205 ps, 63 ps, and 0.7 T for the one with 20 mu m pore size MCPs. Published under license by AIP Publishing.
Desulfovibrio alaskensis G20 biofilms were cultivated on 316 steel, 1018 steel, or borosilicate glass under steady-state conditions in electron-acceptor limiting (EAL) and electron-donor limiting (EDL) conditions with lactate and sulfate in a defined medium. Increased corrosion was observed on 1018 steel under EDL conditions compared to 316 steel, and biofilms on 1018 carbon steel under the EDL condition had at least twofold higher corrosion rates compared to the EAL condition. Furthermore, protecting the 1018 metal coupon from biofilm colonization significantly reduced corrosion, suggesting that the corrosion mechanism was enhanced through attachment between the material and the biofilm. Metabolomic mass spectrometry analyses demonstrated an increase in a flavin-like molecule under the 1018 EDL condition and sulfonates under the 1018 EAL condition. These data indicate the importance of S-cycling under the EAL condition, and that the EDL is associated with increased biocorrosion via indirect extracellular electron transfer mediated by endogenously produced flavin-like molecules.
Purpose: Recent research has shown that KCl:Eu2+ has great potential for use in megavoltage radiation therapy dosimetry because this material exhibits excellent storage performance and is reusable due to strong radiation hardness. This work reports our attempts to fabricate 2D KCl:Eu2+ storage phosphor films (SPFs) using both a physical vapor deposition (PVD) method and a tape casting method. Methods: A thin layer of KCl:Eu2+ was deposited on a substrate of borosilicate glass (e.g., laboratory slides) with a PVD system. For tape casting, a homogenous suspension containing storage phosphor particles, liquid vehicle and polymer binder was formed and subsequently cast by doctor-blade onto a polyethylene terephthalate substrate to form a 150 μm thick SPF. Results: X ray diffraction analysis showed that a 10 μm thick PVD sample was composed of highly crystalline KCl. No additional phases were observed, suggesting that the europium activator had completed been incorporated into the KCl matrix. Photostimulated luminescence and photoluminescence spectra suggested that F (Cl−) centers were the electron storage centers post x ray irradiation and that Eu2+ cations acted as luminescence centers in the photostimulation process. The 150 μm thick casted KCl:Eu2+ SPF showed sub-millimeter spatial resolution. Monte Carlo simulations further demonstrated that the admixture of 20% KCl:Eu2+ and 80% low Z polymer binder exhibited almost no energy dependence in a 6 MV beam. KCl:Eu2+ pellet samples showed a large dynamic range from 0.01 cGy to 60 Gy dose-to-water, and saturated at approximately 500 Gy as a Result of its intrinsic high radiation hardness. Conclusions: This discovery research provides strong evidence that KCl:Eu2+ based SPF with associated readout apparatus could Result in a novel electronic film system that has all the desirable features associated with classic radiographic film and, importantly, water equivalence and the capability of permanent identification of each detector. This work was supported in part by NIH Grant No. R01CA148853. The authors would like to thank Paul Leblans (AGFA Healthcare, Belgium) for many helpful discussions on this topic.
The response of model contamination particles located on the surface of a multilayer dielectric mirror when exposed to 1053 nm laser pulses of 10 ps or 0.6 ps duration is investigated. Four different particle types were studied: stainless steel, borosilicate glass, polyethylene, and polytetrafluoroethylene, all having an average diameter of about 40 μm. Irradiation with one laser pulse caused particles to eject from the surface with an onset fluence in the range 5× to 100×, depending on the particle type, below the particle-free, laser-induced damage threshold of the mirror. Morphological analysis showed, however, that the ejection process always generated ablation craters and/or secondary contamination, both of which can degrade the performance of the optic during subsequent pulses. Here, ejection and damage mechanisms are discussed for each particle type.
Measurement of two-dimensional angle-resolved optical scattering (TAOS) patterns is an attractive technique for detecting and characterizing micron-sized high-speed flying particles. The elastic-scattering intensity pattern from a single particle as a function of spherical coordinate angles θ and ϕ provides detailed information on the particle’s morphology. By use of an ellipsoidal reflector and a high-speed CCD camera, scattering from a CW-laser was detected and resolved over a large angular range (θ from 12° to 168° and ϕ from 0° to 360°) from spherically shaped particles (e.g., amorphous silica and borosilicate glass) flowing through the reflector’s focal plane at speeds of 20 to 30 m/s. The scattering pattern from individual particles flying through the focal plane of the ellipsoid mirror provides insights about a particle’s size, clustering, roughness, and velocity.
Young’s modulus is an important parameter for characterizing the strength of, and wave propagation through, a given material. This study improves the estimation of Young’s modulus using the impulse excitation technique based on an experimental analysis of 19 borosilicate glass bars. Analysis of the frequency equations relating Young’s modulus to the out-of-plane and in-plane flexural resonant frequencies of rectangular prisms has been conducted for both the fundamental frequency and its overtones at higher orders of vibration. Furthermore, the Young’s moduli of three novaculite rocks with various porosities were then measured up to the seventh order of vibration to validate the optimum shear constant equation for estimating Young’s modulus. Young’s modulus was found to be nearly frequency independent for these rock samples.
ABSTRACT Nuclear energy is one option to meet rising electricity demands, although one concern of this technology is the proper capture and storage of radioisotopes produced during fission processes. One of the more difficult radioisotopes is 129 I due to its volatility and poor solubility in traditional waste forms such as borosilicate glass. Iodosodalite has been previously proposed as a viable candidate to immobilize iodine due to high iodine loading and good chemical durability. Iodosodalite was traditionally synthesized using solid state and hydrothermal techniques, but this paper discusses an aqueous synthesis approach to optimize and maximize the iodosodalite yield. Products were pressed into pellets and fired with glass binders. Chemical durability and iodine retention results are included.
Quarterly highlights are: (1) The integration of Denovo and AMP was demonstrated in an AMP simulation of the thermo-mechanics of a complete fuel assembly; (2) Bison was enhanced with a mechanistic fuel cracking model; (3) Mechanistic algorithms were incorporated into various lower-length-scale models to represent fission gases and dislocations in UO2 fuels; (4) Marmot was improved to allow faster testing of mesoscale models using larger problem domains; (5) Component models of reactor piping were developed for use in Relap-7; (6) The mesh generator of Proteus was updated to accept a mesh specification from Moose and equations were formulated for the intermediate-fidelity Proteus-2D1D module; (7) A new pressure solver was implemented in Nek5000 and demonstrated to work 2.5 times faster than the previous solver; (8) Work continued on volume-holdup models for two fuel reprocessing operations: voloxidation and dissolution; (9) Progress was made on a pyroprocessing model and the characterization of pyroprocessing emission signatures; (10) A new 1D groundwater waste transport code was delivered to the used fuel disposition (UFD) campaign; (11) Efforts on waste form modeling included empirical simulation of sodium-borosilicate glass compositions; (12) The Waste team developed three prototypes for modeling hydride reorientation in fuel cladding during very long-term fuel storage; (13) A benchmark demonstration problem (fission gas bubble growth) was modeled to evaluate the capabilities of different meso-scale numerical methods; (14) Work continued on a hierarchical up-scaling framework to model structural materials by directly coupling dislocation dynamics and crystal plasticity; (15) New 'importance sampling' methods were developed and demonstrated to reduce the computational cost of rare-event inference; (16) The survey and evaluation of existing data and knowledge bases was updated for NE-KAMS; (17) The NEAMS Early User Program was launched; (18) The Nuclear Regulatory Commission (NRC) Office of Regulatory Research was introduced to the NEAMS program; (19) The NEAMS overall software quality assurance plan (SQAP) was revised to version 1.5; and (20) Work continued on NiCE and its plug-ins and other utilities, such as Cubit and VisIt.
Current mesoscale models lack the necessary physical parameters to accurately describe the interactions that occur between particles during compaction. This work presents a methodology by which the mechanical and fracture properties of single particles can be determined. Preliminary results for a system of borosilicate glass spheres are presented, illustrating the effect of particle size and strain-rate on the compression response of individual micron-sized particles.
Plans for the treatment of high level waste (HL W) at the Hanford Tank Waste Treatment and Immobilization Plant (WTP) are based upon the inventory of the tank wastes, the anticipated performance of the pretreatment processes, and current understanding of the capability of the borosilicate glass waste form. The WTP HLW melter design, unlike earlier DOE melter designs, incorporates an active glass bubbler system. The bubblers create active glass pool convection and thereby improve heat and mass transfer and increase glass melting rates. The WTP HLW melter has a glass surface area of 3.75 m 2 and depth of ~ 1.1 m. The two melters in the HLW facility together are designed to produce up to 7.5 MT of glass per day at 100% availability. Further increases in HL W waste processing rates can potentially be achieved by increasing the melter operating temperature above 1150°C and by increasing the waste loading in the glass product. Increasing the waste loading also has the added benefit of decreasing the number of canisters for storage.
This report is a presentation, with slides noting, Over 40 experiments were completed during this run using X-ray imaging on the IMPULSE system at Sector 32 IDB; Summary of new experiments: Idealized sphere compaction – Capture progression of dynamic densification through an idealized system on 0.500 mm borosilicate glass spheres (Slide 1); Detonator and EBW Imaging Experiments on IMPULSE – First time HE was intentionally detonated at APS (Slide 2); Spall and high strain rate crack nucleation/propagation in PMMA – PCI data is providing new and unique insights for model validation (Slide 3); Fiber composite for armor applications was studied under ballistic impact of Dyneema (Collaboration with Army Research Laboratory) (Slide 4). Summary of on-going experiments; Crack propagation in vitreous carbon – observed crack motion and caustic; Jet formation experiments on large grain cerium to examine phase dependent strength; Ballistic impact of Comp-B and TNT to examine thermo-mechanical response in-situ with various penetrator geometries to vary shear concentration. Other efforts: IMPULSE system moved and installed in Sector 35 (DCS). This includes the 4-frame X-ray detection system, 4- channel PDV, and other gun diagnostics; New remotely operated mobile IMPULSE structure in fabrication – to be delivered to APS in April; 4 Mini-VISAR Systems and 4-channel PDV installed in DCS instrumentation room with all associated diagnostics.
The isotope 99 Tc is an important fission product generated from nuclear power production. Because of its long half-life (t 1/2 = 2.13 ∙ 10 5 years) and beta-radiotoxicity (β⁻ = 292 keV), it is a major concern in the long-term management of spent nuclear fuel. In the spent nuclear fuel, Tc is present as an alloy with Mo, Ru, Rh, and Pd called the epsilon-phase, the relative amount of which increases with fuel burn-up. In some separation schemes for spent nuclear fuel, Tc would be separated from the spent fuel and disposed of in a durable waste form. Technetium waste forms under consideration include metallic alloys, oxide ceramics and borosilicate glass. In the development of a metallic waste form, after separation from the spent fuel, Tc would be converted to the metal, incorporated into an alloy and the resulting waste form stored in a repository. Metallic alloys under consideration include Tc–Zr alloys, Tc–stainless steel alloys and Tc–Inconel alloys (Inconel is an alloy of Ni, Cr and iron which is resistant to corrosion). To predict the long-term behavior of the metallic Tc waste form, understanding the corrosion properties of Tc metal and Tc alloys in various chemical environments is needed, but efforts to model the behavior of Tc metallic alloys are limited. One parameter that should also be considered in predicting the long-term behavior of the Tc waste form is the ingrowth of stable Ru that occurs from the radioactive decay of 99 Tc ( 99 Tc → 99 Ru + β⁻). After a geological period of time, significant amounts of Ru will be present in the Tc and may affect its corrosion properties. Studying the effect of Ru on the corrosion behavior of Tc is also of importance. In this context, we studied the electrochemical behavior of Tc metal, Tc-Ni alloys (to model Tc-Inconel alloy) and Tc-Ru alloys in acidic media. The study of Tc-U alloys has also been performed in order to better understand the nature of Tc in metallic spent fuel. Computational modeling and simulations were performed to shed light on experimental results and explain structural and kinetics trends.
This final report (M5NU-12-NY-AU # 0202-0410) summarizes the results of the project titled “Alternative High-Performance Ceramic Waste Forms,” funded in FY12 by the Nuclear Energy University Program (NEUP Project # 12-3809) being led by Alfred University in collaboration with Savannah River National Laboratory (SRNL). The overall focus of the project is to advance fundamental understanding of crystalline ceramic waste forms and to demonstrate their viability as alternative waste forms to borosilicate glasses. We processed single- and multiphase hollandite waste forms based on simulated waste streams compositions provided by SRNL based on the advanced fuel cycle initiative (AFCI) aqueous separation process developed in the Fuel Cycle Research and Development (FCR&D). For multiphase simulated waste forms, oxide and carbonate precursors were mixed together via ball milling with deionized water using zirconia media in a polyethylene jar for 2 h. The slurry was dried overnight and then separated from the media. The blended powders were then subjected to melting or spark plasma sintering (SPS) processes. Microstructural evolution and phase assemblages of these samples were studied using x-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersion analysis of x-rays (EDAX), wavelength dispersive spectrometry (WDS), transmission electron spectroscopy (TEM), selective area x-ray diffraction (SAXD), and electron backscatter diffraction (EBSD). These results showed that the processing methods have significant effect on the microstructure and thus the performance of these waste forms. The Ce substitution into zirconolite and pyrochlore materials was investigated using a combination of experimental (in situ XRD and x-ray absorption near edge structure (XANES)) and modeling techniques to study these single phases independently. In zirconolite materials, a transition from the 2M to the 4M polymorph was observed with increasing Ce content. The resulting powders were consolidated via SPS. Ce was reduced to the trivalent oxidation state and the zirconolite was converted into undesirable perovskite. The zirconolite polymorphs found in the synthesized powders were recovered after a post-SPS heat treatment in air. These results demonstrated the potential of processing in controlling the phase assemblage in these waste forms. Hollandites with Cr 3+ trivalent cations were identified as potential hosts for Cs immobilization and are being investigated for Cs retention properties. Series of compositions Ba 1.15-x Cs 2x Cr 2.3 Ti 5.7 O 16 , with increasing Cs loadings, were prepared by sol-gel process and characterized for structural parameters. Structural characterization was performed by a combination of powder XRD and neutron powder diffraction. Phase pure hollandite adapting monoclinic symmetry (I2/m) was observed for 0 ≤ x ≤ 0.55. These results were used to develop a new structural model to interpret Cs immobilization in these hollandites. Performance of these waste forms were evaluated for chemical durability and radiation resistance. Product consistency testing (PCT) and vapor hydration testing (VHT) were used for testing of chemical durability. Radiation resistance was tested using He + ions to simulate $\alpha$ particles and heavy ions such as Au 3+ to simulate a recoil. These results showed that these waste forms were chemically durable. The waste forms also amorphized to various degrees on exposure to simulated radiation.
This report is a summary of the international collaboration and laboratory work funded by the US Department of Energy Office of Nuclear Energy Spent Fuel and Waste Science & Technology (SFWST) as part of the Sandia National Laboratories Salt R&D work package. This report satisfies milestone levelfour milestone M4SF-17SN010303014. Several stand-alone sections make up this summary report, each completed by the participants. The first two sections discuss international collaborations on geomechanical benchmarking exercises (WEIMOS) and bedded salt investigations (KOSINA), while the last three sections discuss laboratory work conducted on brucite solubility in brine, dissolution of borosilicate glass into brine, and partitioning of fission products into salt phases.
Safety issues in nuclear power plants are of extreme importance. Numerous sensors are used within nuclear power plants for sensing and monitoring of its critical operation parameters. As currently implemented, during massive losses of power across the plant in accidents, the backup batteries for the monitoring sensors will ultimately be drained and can cease to operate. The overall objective of this NEUP project is to develop a novel self-powered wireless hybrid sensor which can accurately monitor both pressure and temperature using a single device, even in the extreme harsh environments of severe nuclear accidents, without the requirement of external electricity. At Virginia Tech side, a heat pipe assisted thermoelectric generator (TEG) energy harvester and associated power management and data transmission circuits were developed. The energy harvester can produce electrical power continuously, even in loss of plant and external power situations, providing power for important data transmission for accident diagnosis. The self-powered sensing system could be integrated directly onto key nuclear components including pipes, pump housings, heat exchangers, reactor vessels, and shielding structures inside and outside of the reactor core. Two TEG based energy harvesters which can work in relatively low (50-250 ºC) and high temperature ranges (250-350 ºC) were established and tested. In the prototypes, heat pipes were introduced to reduce the heat resistances of the device at the hot and cold ends. The power output of the heat pipe assisted TEG module is 2.22 W, which is 6 times more than one using an aluminum rod. In-lab tests showed that these devices canmeet the requirement to power the sensors and circuit during normal and off-normal conditions.Amodel was then built to analyze the thermal network in the energy harvester, and was used to optimize its performance and reduce its geometry size. The design and testing of the vibrational energy harvester were completed. The harvester, has shown to effectively increase the vibrational potential of the main coolant pump, though it has been shown that thermal energy has a much higher potential for the powering of sensors. In this project, a self-start charger circuit for the energy harvester was designed to regulate and manage the power. An energy storage element was incorporated into the energy harvesting module for sensors and wireless transceivers in an off-normal situation. The signal conditioning and wireless communication electronic circuits were developed and tested in the lab. An important consideration for an energy harvester within a nuclear power plant is the level of radiation it will encounter during operation. The two main sources of radiation in a nuclear power plant are gamma and neutron radiation. Aradiation experiment was conducted in the Westinghouse Electric Company during which the prototypes were placed in a 106 rad radiation environment to test their ability to operate in the extreme environment. The results showed that this level of radiation had little effect on the performance of the TEGmaterial and heat pipe heat exchanging system. Its influence on the circuit was still under research, however the need for more development on radiation hardened electronics is needed. Pressure measurement based on piezoelectric crystal resonators has advantages over the commercially available methods like capacitive, electromagnetic, optical, potentiometric, and piezo resistive strain gauges. Since the output of piezoelectric based sensors are digital in format, it has a very high resolution, high accuracy, and long-term stability. Quartz is one of the commonly used piezoelectric material in digital pressure sensors design. This material is elastic in nature, providing high stability, high repeatability, high elasticity, repeatable mechanical behavior for many cycles of operation, and is free of hysteresis. The quartz resonator has a high Q, which means that very high vibration can be driven with the very low electric power. Langasite (LGS) is a new promising piezoelectric material that combines the advantageous properties of quartz with a better performance at high temperatures. LGS will not undergo any phase transitions up to its melting temperature of 1473 C, and hence, the application of Langasite in measuring pressure at high temperatures is promising. In this project, the design and fabrication of the piezo oscillator crystal for temperature and pressure measurement has been completed. The entire sensor has been fabricated and tested to see its sensitivity to temperature and pressure changes. The design and optimization of the radiation shielding systems that can effective protect the duel-mode Langasite sensor inside reactor core were demonstrated. To maximize the radiation shielding effectiveness, different types of materials are investigated based upon recent developments of radiation shielding systems including aluminum + Boron carbide and bismuth borosilicate glass B2O3 in addition to tungsten/B4C. New materials based upon metatheses is included as potential shielding to mitigate neutron fluencies. The radiation shielding effectiveness of selected composites are evaluated within a broader neutron spectrum from thermal, epithermal, fast (1 MeV) and 15 MeV neutrons. Performance analysis was also conducted to evaluate the effects of selected composite systems.Aconceptual design was also proposed for the packaging and integration of the radiation shielding system with the sensor, and its applicability within the reactor core was discussed. At end of the project, all components necessary for a complete sensing and monitoring system, including a langasite sensor, electrodes, the TEG harvester, an energy storage device, and power management and transmission electronics were integrated to demonstrate feasibility in powering the sensor. Finally, integration of each component into a full package, and a full demonstration were done.
The Savannah River Site (SRS) Liquid Waste System (LWS) contains approximately 66 tons of mercury within the liquids, salts, and sludges that are currently being processed into final wasteforms for disposal. Mercury concentrations within the system exceed those typically experienced in environmental or industrial systems; thus, management of mercury compounds continues to be a priority for SRS. In the LWS, waste is vitrified into a borosilicate glass wasteform that contains most of the radioactivity, while the lower activity solutions are dispositioned in a low-level grout wasteform, or “saltstone”. The alkaline, high ionic strength caustic wastes are pumped, evaporated, and otherwise managed throughout the LWS and Defense Waste Processing Facility (DWPF) as they are stored and prepared for conversion to the final wasteforms. Because of the complexity of this system, a key component of effective mercury management in the LWS requires analysis of mercury in various physical phases. The high concentration of mercury within the SRS LWS has the potential to generate vapor-phase contamination. Elemental mercury (Hg 0 ), dimethylmercury ((CH 3 ) 2 Hg), and methylmercury (CH 3 Hg + ) are among species known or suspected to contribute to the flux of mercury from liquid to vapor phase (Iverfeldt and Lindquist, 1982). Chemical speciation affects not only mercury behavior in LWS operations but may also affect the performance of mercury treatment and removal technologies in the LWS.