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At least 91 records · Page 5

A protected annealing strategy to enhanced light emission and photostability of YAG:Ce nanoparticle-based films

A significant obstacle in the development of YAG:Ce nanoparticles as light converters in white LEDs and as biological labels is associated with the difficulty of finding preparative conditions that allow simultaneous control of structure, particle size and size distribution, while maintaining the optical properties of bulk samples. Preparation conditions frequently involve high-temperature treatments of precursors (up to 1400 C), which result in increased particle size and aggregation, and lead to oxidation of Ce(III) to Ce(IV). We report here a process that we term protected annealing, that allows the thermal treatment of preformed precursor particles at temperatures up to 1000 C while preserving their small size and state of dispersion. In a first step, pristine nanoparticles are prepared by a glycothermal reaction, leading to a mixture of YAG and boehmite crystalline phases. The preformed nanoparticles are then dispersed in a porous silica. Annealing of the composite material at 1000 C is followed by dissolution of the amorphous silica by hydrofluoric acid to recover the annealed particles as a colloidal dispersion. This simple process allows completion of YAG crystallization while preserving their small size. The redox state of Ce ions can be controlled through the annealing atmosphere. The obtained particles of YAG:Ce (60 {+-} 10 nm in size) can be dispersed as nearly transparent aqueous suspensions, with a luminescence quantum yield of 60%. Transparent YAG:Ce nanoparticle-based films of micron thickness can be deposited on glass substrates using aerosol spraying. Films formed from particles prepared by the protected annealing strategy display significantly improved photostability over particles that have not been subject to such annealing.

36 MATERIALS SCIENCE↗

Large-Batch Reduction of Molybdenum Trioxide

Unconverted, isotopically-enriched molybdenum metal must be recovered from the spent radiopharmaceutical solution used in NorthStar’s Technetium-99m generator and reused. The recycle process begins by recovering the metal from the aqueous potassium molybdate (K 2 MoO 4 ) solutions as molybdenum trioxide (MoO 3 ) employing a process developed at Argonne National Laboratory. The MoO 3 powder is subsequently reduced to molybdenum metal powder which can be blended with new powder and further processed into a flowable form to be used to produce target disks for irradiation. The molybdenum oxide reduction process has been examined and scaled to produce kilogram quantities of metal powder suitable for processing into a useable form employing spray drying or similar technique and ultimately used for target fabrication.

36 MATERIALS SCIENCE↗

Assessment of Benefits of Solid-State Advanced Manufacturing Processes for Nuclear Energy Products

The Advanced Materials and Manufacturing Technology (AMMT) program develops cross cutting technologies in support of a broad range of nuclear reactor technologies and maintains U.S. leadership in materials and manufacturing technologies for nuclear energy applications. This overall project provides the U.S. Department of Energy a critical feasibility study comparison of three solid-state processes to other AM processes, thereby providing the feasibility of the solid-state processes examined to manufacture 316H SS and ODS steel components: • Fused-filament fabrication (FFF): This work provides an initial evaluation of the impact of powder morphology and sizes on the FFF process, and the feasibility and adaptability for different material systems, to use FFF for ODS steels and 316 SS. • Shear-assisted processing and extrusion (ShAPE): Specifically for this portion of the project on ShAPE tube forming, the objectives will be to determine the feasibility to direct tube forming of high tensile strength steel tubing, specifically for ODS steel to determine the effect of the patented extrusion process on the dispersoids of the ODS material. Additionally, as often ODS powders are mechanically alloyed and therefore more platelike or angular, this feasibility was to explore the impact on the optimization process and initial feasibility of direct tube forming. • Cold spray and friction stir additive manufacturing as a stretch goal: Bulk and near net shape manufacturing processes for high-temperature, high-strength alloys are needed. Additionally, cold spray techniques can be applied in-situ at the operational level for repair and can provide multiple benefits to the nuclear industry. These tasks aim to provide information to show benefits of cold spray during the full life cycle, namely research and development, product manufacturing, and repair to mention a few key points.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

CLOSEOUT REPORT FOR HYBRID SULFUR PRESSURIZED BUTTON CELL TEST FACILITY

This document is the Close-Out Report for design and partial fabrication of the Pressurized Button Cell Test Facility at Savannah River National Laboratory (SRNL). This facility was planned to help develop the sulfur dioxide depolarized electrolyzer (SDE) that is a key component of the Hybrid Sulfur Cycle for generating hydrogen. The purpose of this report is to provide as much information as possible in case the decision is made to resume research. This report satisfies DOE Milestone M3GSR10VH030107.0. The HyS Cycle is a hybrid thermochemical cycle that may be used in conjunction with advanced nuclear reactors or centralized solar receivers to produce hydrogen by watersplitting. The HyS Cycle utilizes the high temperature (>800 C) thermal decomposition of sulfuric acid to produce oxygen and regenerate sulfur dioxide. The unique aspect of HyS is the generation of hydrogen in a water electrolyzer that is operated under conditions where dissolved sulfur dioxide depolarizes the anodic reaction, resulting in substantial voltage reduction. Low cell voltage is essential for both high thermodynamic efficiency and low hydrogen cost. Sulfur dioxide is oxidized at the anode, producing sulfuric acid that is sent to the high temperature acid decomposition portion of the cycle. Sulfur dioxide from the decomposer is cycled back to electrolyzers. The electrolyzer cell uses the membrane electrode assembly (MEA) concept. Anode and cathode are formed by spraying a catalyst, typically platinized carbon, on both sides of a Proton Exchange Membrane (PEM). SRNL has been testing SDEs for several years including an atmospheric pressure Button Cell electrolyzer (2 cm{sup 2} active area) and an elevated temperature/pressure Single Cell electrolyzer (54.8 cm{sup 2} active area). SRNL tested 37 MEAs in the Single Cell electrolyzer facility from June 2005 until June 2009, when funding was discontinued. An important result of the final months of testing was the development of a method that prevents the formation of a sulfur layer previously observed in MEAs used in the Hybrid Sulfur Cycle electrolyzer. This result is very important because the sulfur layer increased cell voltage and eventually destroyed the MEA that is the heart of the cell. Steimke and Steeper [2005, 2006, 2007, 2008] reported on testing in the Single Cell Electrolyzer test facility in several periodic reports. Steimke et. al [2010] issued a final facility close-out report summarizing all the testing in the Single Cell Electrolyzer test facility. During early tests, significant deterioration of the membrane occurred in 10 hours or less; the latest tests ran for at least 200 hours with no sign of deterioration. Ironically, the success with the Single Cell electrolyzer meant that it became dedicated to long runs and not available for quick membrane evaluations. Early in this research period, the ambient pressure Button Cell Electrolyzer test facility was constructed to quickly evaluate membrane materials. Its small size allowed testing of newly developed membranes that typically were not available in sizes large enough to test in the Single Cell electrolyzer. The most promising membranes were tested in the Single Cell Electrolyzer as soon as sufficient large membranes could be obtained. However, since the concentration of SO{sub 2} gas in sulfuric acid decreases rapidly with increasing temperature, the ambient pressure Button Cell was no longer able to achieve the operating conditions needed to evaluate the newer improved high temperature membranes. Significantly higher pressure operation was required to force SO{sub 2} into the sulfuric acid to obtain meaningful concentrations at increased temperatures. A high pressure (200 psig), high temperature (120 C) Button Cell was designed and partially fabricated just before funding was discontinued in June 2009. SRNL completed the majority of the design of the test facility, including preparation of a process and instrument drawing (P&ID) and preliminary designs for the major components. SRNL intended to complete the designs and procure or fabricate the specialized equipment, including all wetted-parts for handling the SO{sub 2}/sulfuric acid reactants. The portion of the P&ID that included commercial equipment, standard tubing, controls, and structural systems was procured from a commercial partner (Giner Electrochemical Systems LLC). This report summarizes the objectives, preliminary design, and status of the test facility. At the time of this report, SRNL was continuing discussions with potential partners for transfer of the technology for use under other programs.

08 HYDROGEN↗

Integration and software for thermal test of heat rate sensors

A minicomputer controlled radiant test facility is described which was developed and calibrated in an effort to verify analytical thermal models of instrumentation islands installed aboard the space shuttle external tank to measure thermal flight parameters during ascent. Software was provided for the facility as well as for development tests on the SRB actuator tail stock. Additional testing was conducted with the test facility to determine the temperature and heat flux rate and loads required to effect a change of color in the ET tank external paint. This requirement resulted from the review of photographs taken of the ET at separation from the orbiter which showed that 75% of the external tank paint coating had not changed color from its original white color. The paint on the remaining 25% of the tank was either brown or black, indicating that it had degraded due to heating or that the spray on form insulation had receded in these areas. The operational capability of the facility as well as the various tests which were conducted and their results are discussed.

Wojciechowski, C. J.↗

Disintegration of liquid sheets

The development, stability, and disintegration of liquid sheets issuing from a two-dimensional air-assisted nozzle is studied. Detailed measurements of mean drop size and velocity are made using a phase Doppler particle analyzer. Without air flow the liquid sheet converges toward the axis as a result of surface tension forces. With airflow a quasi-two-dimensional expanding spray is formed. The air flow causes small variations in sheet thickness to develop into major disturbances with the result that disruption starts before the formation of the main break-up region. In the two-dimensional variable geometry air-blast atomizer, it is shown that the air flow is responsible for the formation of large, ordered, and small chaotic 'cell' structures.

Mansour, Adel↗

Controlling Flows Of Two Ingredients For Spraying

Closed-loop servo control subsystem incorporated, as modification, into system controlling flows of two ingredients mixed and sprayed to form thermally insulating foams on large tanks. Provides steady flows at specified rates. Foams produced smoother and of higher quality. Continued use of system results in substantial reduction in cost stemming from close control of application of foam and consequent reduced use of material.

Chandler, Huel H.↗

The Effects of Sooting and Radiation on Droplet Combustion

The burning of liquid hydrocarbon fuels accounts for a significant portion of global energy production. With predicted future increases in demand and limited reserves of hydrocarbon fuel, it is important to maximize the efficiency of all processes that involve conversion of fuel. With the exception of unwanted fires, most applications involve introduction of liquid fuels into an oxidizing environment in the form of sprays which are comprised of groups of individual droplets. Therefore, tremendous benefits can result from a better understanding of spray combustion processes. Yet, theoretical developments and experimental measurements of spray combustion remains a daunting task due to the complex coupling of a turbulent, two-phase flow with phase change and chemical reactions. However, it is recognized that individual droplet behavior (including ignition, evaporation and combustion) is a necessary component for laying the foundation for a better understanding of spray processes. Droplet combustion is also an ideal problem for gaining a better understanding of non-premixed flames. Under the idealized situation producing spherically-symmetric flames (produced under conditions of reduced natural and forced convection), it represents the simplest geometry in which to formulate and solve the governing equations of mass, species and heat transfer for a chemically reacting two phase flow with phase change. The importance of this topic has promoted extensive theoretical investigations for more than 40 years.

Lee, Kyeong-Ook↗

Vacuum Plasma Spray of Cu-8Cr-4Nb for Advanced Liquid-Fuel Combustion Chambers

Vacuum plasma spray (VPS) formed Cu-8Cr-4Nb alloy, with low oxygen, exhibits higher strength at room and elevated temperature than material formed by extrusion. The VPS formed material exhibits slightly lower ductility than the extruded material. VPS forming of Cu-8Cr-4Nb can be used to produce near net structures with mechanical properties comparable to current extruded material.

Zimmerman, F.↗

MODELING THE INFLUENCE OF NOZZLE-GENERATED TURBULENCE ON DIESEL SPRAYS

Predictive engine simulations are key for rapidly exploring and optimizing the design of cleaner burning and more fuel efficient engines. Injection strategies in advanced engine concepts are resulting in the injection and atomization of fuel under a wide range of operating conditions in order to meet stringent emission regulations. However, the physics governing the breakup of an injected liquid fuel jet into droplets under these conditions have not been well studied or experimentally characterized to date. In the sprays literature, three agents have been proposed as the likely mechanisms contributing to primary atomization in diesel sprays, namely the aerodynamic growth of waves on the fuel jet surface, turbulence generated in the injector nozzle, and cavitation. If computational design tools are to be used to guide the use of direct injection strategies for cleaner and more fuel efficient engines, the physics underpinning the role of these primary atomization mechanisms must be better understood to ensure the development of predictive simulations of fuel-air mixing and vaporization within the engine. Thus, the central aim of this thesis is to improve the physical representation of spray breakup physics within today’s engine simulation packages. The work presented in this thesis investigates the role of the proposed physical mechanisms on the primary atomization process in diesel sprays. In order to advance current understanding of spray breakup, the dynamic and geometric factors contributing to cavitation were suppressed so that primary atomization due to aerodynamics and nozzle-generated turbulence could be studied in isolation. In the absence of sufficiently resolved images to visualize the primary atomization process under dieselrelevant conditions, droplet sizing spray measurements are needed to characterize the outcomes of the spray breakup process. Therefore, a new experimental methodology was developed and applied in a high-pressure spray chamber to characterize the average size of droplets formed from the spray breakup process. This experimental data, in conjunction with x-ray measurements from the Advanced Photon Source at Argonne National Laboratory, have been used to assess predictions from existing spray breakup models. Comparison between predicted and measured drop size distributions revealed that a spray atomization model, premised on droplet formation from the growth of aerodynamically induced instabilities, could capture experimentally observed sensitivities and features in the measured droplet size distributions under conventional diesel engine conditions. However, for injection into relatively lower ambient density environments, aerodynamic breakup models could not accurately predict the initial rate of droplet size decrease in the near-nozzle region, suggesting that other mechanisms, such as turbulence generated inside the nozzle, likely augment and enhance the primary breakup process. Evaluation of newly available droplet sizing measurements under low ambient density conditions allowed for the turbulence-induced breakup process to be studied, while minimizing the influence of aerodynamic inertial forces on the spray. Although several turbulence-induced breakup models have been proposed in the literature, the scaling of droplet sizes with the integral length scale, assumed in the majority of turbulent breakup models, was found to be inconsistent with the experimentally observed trends in droplet size along the spray centerline. However, empirical correlations describing droplets formed from eddies within the inertial sub-range of the turbulence spectrum were better able to capture the measured sensitivities in droplet size to changes in ambient and injection conditions. These findings informed recommendations for an improved hybrid spray breakup model, capable of representing both aerodynamic and turbulent breakup mechanisms in the atomization of non-cavitating diesel sprays.

33 ADVANCED PROPULSION SYSTEMS↗

A model for eruption behavior of a volcanic vent in eastern Mare Serenitatis

The origin is considered of droplets of ultramafic composition which are present in all soils collected from the mare surface at the Apollo 17 landing site. The droplets consist of homogeneous orange glass or their partially crystallized equivalent, the black droplets. These clastic deposits have a mean grain size of 40 micrometers. The droplet formation ages range from 3.5 to 3.83 b.y. It has been proposed that the droplets formed as a spray of low viscosity melt during lava fountaining. Based upon the thermal history as determined by studying olivine and particle shapes, two models for the formation of the sequence of droplets represented by samples 74001 and 74220 are presented. Both models assume, as proposed by Heiken et al. (1974), that the droplets were formed as a spray from a lava fountain and the compound forms were evidence for 'recycling' of solid, cooler droplets back into the fountain, encountering molten droplets before being deposited.

Heiken, G.↗

A study of the current group evaporation/combustion theories

Liquid fuel combustion can be greatly enhanced by disintegrating the liquid fuel into droplets, an effect achieved by various configurations. A number of experiments carried out in the seventies showed that combustion of droplet arrays and sprays do not form individual flames. Moreover, the rate of burning in spray combustion greatly deviates from that of the single combustion rate. Such observations naturally challenge its applicability to spray combustion. A number of mathematical models were developed to evaluate 'group combustion' and the related 'group evaporation' phenomena. This study investigates the similarity and difference of these models and their applicability to spray combustion. Future work that should be carried out in this area is indicated.

Shen, Hayley H.↗

Five kHz thermometry in turbulent spray flames using chirped-probe-pulse femtosecond CARS, part II: Structure of reaction zones

Temperature was measured in turbulent spray flames of ethanol and acetone stabilized on the piloted Sydney Needle Spray Burner (SYNSBURN TM ) using single-laser-shot, chirped-probe-pulse femtosecond coherent anti-Stokes Raman spectroscopy (CPP-fs-CARS) with a repetition rate of 5 kHz. The burner features air-blast atomization of liquid injected from a needle that can be translated by a length Lr within a co-flowing air stream so that piloted spray flames ranging from dilute to dense can be studied. Part I of these investigations has reported on the CPP-fs-CARS technique and extensive details of data processing methodology. Part II is concerned with the structure of the reaction zones at different spray loadings and for different departures from blow-off. While not performed simultaneously, measurements of the size distribution of liquid fragments are also reported and discussed in conjunction with the measured temperature. Measured probability density functions of temperature show that for flames with the same liquid loading but different recess lengths, Lr, the near-field spray structure that forms upstream of x/D = 10 affects flame structure and stability further downstream. As the spray exiting the burner becomes denser, with a higher proportion of ligaments and ‘irregular’ shaped objects, the entrainment of hot pilot gases into the spray envelope is affected, hence changing the rates of vaporization and subsequent combustion. The reported results will also form a useful platform for validating sub-models of atomization and combustion in turbulent, dilute to dense spray flames.

42 ENGINEERING↗

A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte

In this work we introduce an approach to fabricate a solid composite electrolyte film that is thin, ionically conductive, and mechanically robust with good potential for manufacturability, in the application of lithium metal batteries. First a doped-lithium aluminum titanium phosphate ceramic thin film with thickness of ~25 μm is formed by aqueous spray coating, a scalable process. The film is partially sintered to form a three-dimensionally interconnected structure with a dense backbone. It is then backfilled with a crosslinkable poly(ethylene oxide) (PEO)-based polymer electrolyte. We report the composite has very high ceramic loading of 77 wt% (61 vol%) and an ionic conductivity of 3.5 × 10 -5 S/cm at 20 °C with an activation energy of 0.43 eV. The main ion transport pathway is through the ceramic network, predicted by modelling and verified by experiments. Owing to the interconnected structure of the ceramic, the composite electrolyte exhibits much improved mechanical strength.

25 ENERGY STORAGE↗

Hydrogen rich gas generator

A process and apparatus is described for producing a hydrogen rich gas by introducing a liquid hydrocarbon fuel in the form of a spray into a partial oxidation region and mixing with a mixture of steam and air that is preheated by indirect heat exchange with the formed hydrogen rich gas, igniting the hydrocarbon fuel spray mixed with the preheated mixture of steam and air within the partial oxidation region to form a hydrogen rich gas.

Houseman, J.↗

Effect of Properties/Injection Schedule on Fuel Spray Mixing

The DOE project for Co-Optimization of Fuels and Engines seeks to define both fuel properties and engine hardware to create cleaner and more fuel-efficient engines. Fuel spray technologies are central to this goal as the spray injection determines the combustible mixtures formed within the engine. Sprays are known to affect bum rate and efficiency, particulate formation and emissions, as well as temperature and engine knock sites. Computational fluid dynamic models must predict complicated interaction between plumes and vaporization to be useful as a design tool for industry. Changes in fuel properties are expected to affect fuel delivery. While Co-Optima fuels may be selected for chemical criteria, such as high octane number rating, an understanding of how the physical properties affect spray performance is necessary to optimize fuel delivery. Many of the selected Co-Optima fuels have properties that are different than standard gasoline, requiring investigations for their performance. A new continuous-flow spray chamber facility has been completed, offering capability to control the pressure and temperature of the gases at engine-relevant conditions at the time of injection as well as a massive increase in data throughput. Direct-injection multi-hole gasoline sprays for different Co-Optima fuels are investigated in this chamber.

02 PETROLEUM↗

A detailed numerical investigation of Burke-Schumann gaseous and spray flames

The classical Burke-Schumann gaseous diffusion flame, and the effect of introducing fuel in the form of liquid sprays are investigated numerically. The time-dependent two-dimensional, axisymmetric conservation equations are solved for the gas phase. A Lagrangian approach is used for the dispersed phase. The chemical reactions are modeled through the one-step global reaction scheme. The numerical results show that the computed flame structure is significantly different from that given by the analytical solution. The computed flame is about 15 percent longer and 5 percent narrower than the classical Burke-Schumann flame. The predicted flame shape is, however, in better agreement with experimental observations than the Burke-Schumann flame. The effects of introducing liquid sprays is found to produce thinner and longer flames than its counterpart gaseous flame. A detailed comparison of the structures of gaseous and spray flames is made, and the differences are discussed.

Mawid, M. A.↗

Effect of an oxide layer on high velocity impact of tantalum particles characterized using molecular dynamics

Micro-cold spray, also commonly referred to as the aerosol deposition method or vacuum kinetic spraying, is a process for depositing nanostructured films of metals and ceramics by impacting solid nanoparticles at high velocity onto a substrate at room temperature and at low pressures. Tantalum films deposited by micro-cold spray are desirable because tantalum is non-reactive to certain molten metals and can therefore serve as a non-reactive barrier coating. However, unlike most other metals deposited by micro-cold spray, tantalum quickly forms an oxide layer when exposed to air. In the deposition of films using traditional cold spray with much larger particles, native oxides must fracture for particle–substrate bonding to occur. Furthermore, the fraction of the particle that is oxidized in micro-cold spray and the strain rates experienced by the particles upon impact are both much larger than in cold spray, suggesting that the role of the oxide on film deposition may be distinct. The effect of this oxide layer on particle deformation and adherence to a substrate under high strain rates is studied using molecular dynamics simulations. The effect of oxide layer thickness, particle diameter, and impact velocity are examined.

42 ENGINEERING↗