Publications

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Before this LDRD research, no single tool could simulate a very high temperature reactor (VHTR) that is coupled to a secondary system and the sulfur iodine (SI) thermochemistry. Furthermore, the SI chemistry could only be modeled in steady state, typically via flow sheets. Additionally, the MELCOR nuclear reactor analysis code was suitable only for the modeling of light water reactors, not gas-cooled reactors. We extended MELCOR in order to address the above deficiencies. In particular, we developed three VHTR input models, added generalized, modular secondary system components, developed reactor point kinetics, included transient thermochemistry for the most important cycles [SI and the Westinghouse hybrid sulfur], and developed an interactive graphical user interface for full plant visualization. The new tool is called MELCOR-H2, and it allows users to maximize hydrogen and electrical production, as well as enhance overall plant safety. We conducted validation and verification studies on the key models, and showed that the MELCOR-H2 results typically compared to within less than 5% from experimental data, code-to-code comparisons, and/or analytical solutions.

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A series of pressurized sulfuric acid decomposition tests are being performed to (1) obtain data on the fraction of sulfuric acid catalytically converted to sulfur dioxide, oxygen, and water as a function of temperature and pressure, (2) demonstrate real-time measurements of acid conversion for use as process control in the Sulfur-Iodine (SI) thermochemical cycle, and (3) obtain multiple measurements of conversion as a function of temperature within a single experiment. Acid conversion data are presented at pressures of 6 and 11 bars in the temperature range of 750 - 875 °C. The design for an acid decomposer section with heat and mass recovery of undecomposed acid using a direct contact heat exchanger are presented.

A series of pressurized sulfuric acid decomposition tests are being performed to (1) obtain data on the fraction of sulfuric acid catalytically converted to sulfur dioxide, oxygen, and water as a function of temperature and pressure, (2) demonstrate real-time measurements of acid conversion for use as process control in the Sulfur-Iodine (SI) thermochemical cycle, and (3) obtain multiple measurements of conversion as a function of temperature within a single experiment. Acid conversion data are presented at pressures of 6 and 11 bars in the temperature range of 750 - 875 °C. The design for an acid decomposer section with heat and mass recovery of undecomposed acid using a direct contact heat exchanger are presented.

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In an effort to produce hydrogen without the unwanted greenhouse gas byproducts, high-temperature thermochemical cycles driven by heat from solar energy or next-generation nuclear power plants are being explored. The process being developed is the thermochemical production of Hydrogen. The Sulfur-Iodide (SI) cycle was deemed to be one of the most promising cycles to explore. The first step of the SI cycle involves the decomposition of H{sub 2}SO{sub 4} into O{sub 2}, SO{sub 2}, and H{sub 2}O at temperatures around 850 C. In-situ removal of O{sub 2} from this reaction pushes the equilibrium towards dissociation, thus increasing the overall efficiency of the decomposition reaction. A membrane is required for this oxygen separation step that is capable of withstanding the high temperatures and corrosive conditions inherent in this process. Mixed ionic-electronic perovskites and perovskite-related structures are potential materials for oxygen separation membranes owing to their robustness, ability to form dense ceramics, capacity to stabilize oxygen nonstoichiometry, and mixed ionic/electronic conductivity. Two oxide families with promising results were studied: the double-substituted perovskite A{sub x}Sr{sub 1-x}Co{sub 1-y}B{sub y}O{sub 3-{delta}} (A=La, Y; B=Cr-Ni), in particular the family La{sub x}Sr{sub 1-x}Co{sub 1-y}Mn{sub y}O{sub 3-{delta}} (LSCM), and doped La{sub 2}Ni{sub 1-x}M{sub x}O{sub 4} (M = Cu, Zn). Materials and membranes were synthesized by solid state methods and characterized by X-ray and neutron diffraction, SEM, thermal analyses, calorimetry and conductivity. Furthermore, we were able to leverage our program with a DOE/NE sponsored H{sub 2}SO{sub 4} decomposition reactor study (at Sandia), in which our membranes were tested in the actual H{sub 2}SO{sub 4} decomposition step.

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A series of three pressurized sulfuric acid decomposition tests were performed to (1) obtain data on the fraction of sulfuric acid catalytically converted to sulfur dioxide, oxygen, and water as a function of temperature and pressure, (2) demonstrate real-time measurements of acid conversion for use as process control, (3) obtain multiple measurements of conversion as a function of temperature within a single experiment, and (4) assess rapid quenching to minimize corrosion of metallic components by undecomposed acid. All four of these objectives were successfully accomplished. This report documents the completion of the NHI milestone on high pressure H{sub 2}SO{sub 4} decomposition tests for the Sulfur-Iodine (SI) thermochemical cycle project. All heated sections of the apparatus, (i.e. the boiler, decomposer, and condenser) were fabricated from Hastelloy C276. A ceramic acid injection tube and a ceramic-sheathed thermocouple were used to minimize corrosion of hot liquid acid on the boiler surfaces. Negligible fracturing of the platinum on zirconia catalyst was observed in the high temperature decomposer. Temperature measurements at the exit of the decomposer and at the entry of the condenser indicated that the hot acid vapors were rapidly quenched from about 400 C to less than 20 C within a 14 cm length of the flow path. Real-time gas flow rate measurements of the decomposition products provided a direct measurement of acid conversion. Pressure in the apparatus was preset by a pressure-relief valve that worked well at controlling the system pressure. However, these valves sometimes underwent abrupt transitions that resulted in rapidly varying gas flow rates with concomitant variations in the acid conversion fraction.

This work describes the design, computational prototyping, fabrication, and characterization of a microfabricated thermal conductivity detector ({mu}TCD) to analyze the effluent from a micro-gas chromatograph column ({mu}GC) and to complement the detection efficacy of a surface acoustic wave detector in the micro-ChemLab{trademark} system. To maximize the detection sensitivity, we designed a four-filament Wheatstone bridge circuit where the resistors are suspended by a thin silicon nitride membrane in pyramidal or trapezoidal shaped flow cells. The geometry optimization was carried out by simulation of the heat transfer in the devices, utilizing a boundary element algorithm. Within microfabrication constraints, we determined and fabricated nine sensitivity-optimized geometries of the {mu}TCD. The nine optimal geometries were tested with two different flow patterns. We demonstrated that the perpendicular flow, where the gas directly impinged upon the membrane, yielded a sensitivity that is three times greater than the parallel flow, where the gas passed over the membrane. The functionality of the {mu}TCD was validated with the theoretical prediction and showed a consistent linear response to effluent concentrations, with a detection sensitivity of 1 ppm, utilizing less than 1 W of power.

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Experimental data are compiled and reviewed for aerosol particle releases due to combustion in air of Plutonium (Pu). The aerosol release fraction (ARF), which is the mass of Pu aerosolized, divided by the mass of Pu oxidized, is dependent on whether the oxidizing Pu sample is static (i.e. stationary) or dynamic (i.e. falling in air). ARF data are compiled for sample masses ranging from 30 mg to 1770 g, oxidizing temperatures varying from 113 C to {approx}1000 C, and air flow rates varying from 0.05 m/s to 5.25 m/s. The measured ARFs range over five orders of magnitude. The maximum observed static ARF is 2.4 x 10{sup -3}, and this is the recommended ARF for safety studies of static Pu combustion.

This work describes the design, simulation, fabrication and characterization of a microfabricated thermal conductivity detector to be used as an extension of the {micro}ChemLab{trademark}. The device geometry was optimized by simulating the heat transfer in the device, utilizing a boundary element algorithm. In particular it is shown that within microfabrication constraints, a micro-TCD optimized for sensitivity can be readily calculated. Two flow patterns were proposed and were subsequently fabricated into nine-promising geometries. The microfabricated detector consists of a slender metal film, supported by a suspended thin dielectric film over a pyramidal or trapezoidal silicon channel. It was demonstrated that the perpendicular flow, where the gas directly impinges on the membrane, creates a device that is 3 times more sensitive than the parallel flow, where the gas passed over the membrane. This resulted in validation of the functionality of a microfabricated TCD as a trace-level detector, utilizing low power. the detector shows a consistent linear response to concentration and they are easily able to detect 100-ppm levels of CO in He. Comparison of noise levels for this analysis indicates that sub part per million (ppm) levels are achievable with the selection of the right set of conditions for the detector to operate under. This detector was originally proposed as part of a high-speed detection system for the petrochemical gas industry. This system was to be utilized as a process monitor to detect reactor ''upset'' conditions before a run away condition could occur (faster than current full-scale monitoring systems were able to achieve). Further outlining of requirements indicated that the detection levels likely achievable with a TCD detector would not be sufficient to meet the process condition needs. Therefore the designed and fabricated detector was integrated into a detection system to showcase some technologies that could further the development of components for the current gas phase {micro}ChemLab as well as future modifications for process monitoring work such as: pressurized connections, gas sampling procedures, and packed columns. Component integration of a microfabricated planar pre-concentrator, gas-chromatograph column and TCD in the separation/detection of hydrocarbons, such as benzene, toluene and xylene (BTX) was also demonstrated with this system.

Three levels of fission product diffusional release models are solved exactly. First, the Booth model for a homogeneous uncoated spherical fuel particle is presented and an improved implementation is suggested. Second, the release from a fuel particle with a single barrier layer is derived as a simple alternative to account for a coating layer. Third, the general case of release from a multicoated fuel particle is derived and applied to a TRISO-coated fuel. Previous approaches required approximate numerical solutions for the case of an arbitrary number of coatings with arbitrary diffusivities and arbitrary coating interface conditions.

An exact two-dimensional solution is derived for determining the fluid flow rates into a borehole and to the surface from which the borehole was drilled. The solution is for a single fluid phase in a disturbed rock zone (DRZ) that surrounds the borehole with a radius specified to be either finite or infinite. The solution is restricted to constant homogeneous rock and fluid properties in the DRZ, and pressures in the borehole and at the surface of the drift that are maintained constant at ambient conditions. A major objective of the work is to provide a benchmark for more detailed numerical calculations that include variable physical properties and an arbitrary DRZ geometry. However in addition, this work extends previous exact solutions for one-dimensional flow by: (1) allowing for a DRZ of finite but arbitrary extent, (2) accounting for depressurization due to mining the drift before drilling the borehole, and (3) accounting for two-dimensional variations of the fluid pressure caused by simultaneous fluid flow to the drift and to the borehole.

The CONTAIN code is a system-level analysis tool developed for the USNRC, and is intended for best-estimate prediction of conditions which might occur in the containment building of a nuclear power plant during a severe accident. A key feature of the code is that it models the containment phenomena in an integrated manner. In particular, the CONTAIN code models some of the complex ways that thermal hydraulics and aerosol phenomena interact with each other. The Light Water Reactor Aerosol Containment Experiment (LACE) progarm is a program to aid researchers in their understanding of thermal hydraulic and aerosol behavior within containments. The purpose of this paper is to report on best-estimate LA-4 post-test calculations that have been completed with the most recent version of the CONTAIN code, version 1.11. An analysis of experimental data and review of the blind post-test CONTAIN calculations is used to justify a re-calculation of the experiment and to establish a best-estimate calculation. The best-estimate calculation shows that reasonably good agreement between thermal hydraulic predictions and data can be obtained with the current CONTAIN models by varying experimental parameters within their uncertainties. Furthermore, with the recently added solubility model for hygroscopic aerosols, the best-estimate calculation gives aerosol behavior that is in good agreement with aerosol data. 10 refs., 16 figs.

An exact solution is derived for one-dimensional radionuclide transport under time-varying fluid-flow conditions including radioactive decay but with the approximation that all radionuclides have identical retardation factors. The solution is used to obtain exact expressions for the cumulative radionuclide mass transported past a fixed point in space over a given time period, and to assess the effects of a periodic perturbation and a step change on the fluid-flow velocity and dispersion coefficient. 14 refs., 3 figs., 3 tabs.