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DOE OSTI2024

Surveying Phase Modifier Functional Groups for Applications to Ln(III) Separations

The application of N,N,N',N'-tetraoctyl diglycolamide (TODGA) in solvent extraction systems for lanthanide (Ln) separations is well understood. In these systems, the formation of a third phase has motivated the use of phase modifiers to enable higher concentrations of H + and Ln common to industrial processes. Several different phase modifiers with applications to diglycolamide (DGA) systems have previously been reported, with a focus on tri-n-butyl phosphate (TBP), N,N'-dihexylactanamide (DHOA), N,N-dioctyl-2-hydroxyacetamide (DOHyA), N,N'-dimethyl-N,N'-dioctylhexylethoxy malonamide (DMDOHEMA), and octanol. While the primary utility of phase modifiers is the increased metal loading, they can have significant effects on the metal distribution ratios, which are well described by the energetics of the extraction process itself. However, the mechanisms by which phase modifiers impact distribution ratios are not generally understood. This work considers the ability of phase modifiers to affect Ln distribution ratios by using phase modifiers with two different functional groups (–Cl and –C≡N) and an octyl alkyl chain in a TODGA and n-dodecane system. Determining the effect of chlorooctane and octane nitrile is important for understanding how phase modifier functional groups and their hydrogen bonding interactions affect Ln extraction. Through combining distribution ratio measurements with organic phase spectroscopic investigations, the impact of chlorooctane and octane nitrile on Ln extraction and their inner-sphere complexes is reported. The addition of either chlorooctane or octane nitrile to TODGA in n-dodecane decreases Ln extraction while maintaining the same inner-sphere Ln complex. The lack of change in inner-sphere Ln-TODGA coordination upon incorporation of phase modifiers and the significant impact of these phase modifiers on distribution ratios suggest the importance of a supramolecular structure. Understanding the role of chlorooctane and octane nitrile on the organic phase structure at longer length scales has been identified as an avenue for future investigations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Enhancing f -Element Separations with ADAAM-EH: The Impact of Phase Modifiers and a DGA Aqueous Complexant

Recent investigations have used a 2-ethylhexyl diamide amine (ADAAM-EH) for Am/Cm separations in combination with N,N,N ',N '-tetraethyldiglycolamide as an aqueous complexant to achieve an unprecedented separation factor of 41. The aim of this research effort is to understand the speciation of trivalent lanthanide (Ln) and actinide (An) ions in the organic phase of an ADAAM-EH extraction system, both with and without phase modifiers (PM) (1-octanol and tri-n-butyl phosphate (TBP)). Leveraging spectroscopic techniques in combination with distribution ratio measurements provides an understanding of organic phase f-element ligand complexation. In the absence of PM, Ln is extracted in a stoichiometric 1:1 [M(ADAAM-EH) 1 (NO 3 ) x (H 2 O) 1 ](NO 3 ) 3-x complex. The addition of 1-octanol at 20 vol % results in multiple species present. One of the species is the same as the no PM case, and the other species results in an increased -OH coordination to the inner sphere, potentially displacing some NO 3 . In the case of TBP, increasing concentration results in additional red-shifted bands in the UV-visible spectra, suggesting the complexation of additional ligands of either ADAAM-EH or TBP. Finally, the new system knowledge obtained by and spectroscopic experiments will provide benchmarking information for computational studies of the inner- and outer-sphere coordination environments of f-element cations and insights into ADAAM-EH adduct formation with PM, like 1-octanol and TBP.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Improved Thermal Stability of Oxysulfide Glassy Solid-State Electrolytes

In this study, the crystallization kinetics of (oxy)sulfide 70Li 2 S·(30-x)P 2 S 5 ·xP 2 O 5 (x = 0, 2, 5) solid-state electrolytes are reported. It was found that 5 mol% P 2 O 5 glass co-former slowed the crystallization rate of the Li 7 P 3 S 11−x/4 O x/4 ceramic phase by a factor of 10. After 10 min at 230 °C, a 70Li 2 S·30P 2 S 5 sulfide glass was 92% devitrified whereas a 70Li 2 S·25P 2 S 5 ·5P 2 O 5 oxysulfide glass was only 8% devitrified. The improved thermal stability of oxysulfide glasses was then utilized to demonstrate the fabrication of a standalone, reinforced SSE separator by hot pressing. More importantly, it was recognized that the microstructure of 70Li 2 S·25P 2 S 5 ·5P 2 O 5 oxysulfide SSE separators could be modified by hot pressing without changing ionic conductivity. This result was achieved because the precipitation of a superionically conductive Li 7 P 3 S 11−x/4 O x/4 ceramic phase was limited. A study was then conducted to determine what effect microstructure has on the susceptibility of SSE separators to shorting by lithium metal penetration. Hot-pressed separators were found to be more susceptible to shorting than cold-pressed separators. X-ray Computer Tomography (XCT) of post-mortem samples showed that hot-pressed samples failed by transverse microcrack pathways, which underscores the importance of low defect density in dense SSE separators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2004

Masked Proportional Routing

Masked proportional routing is an improved procedure for choosing links between adjacent nodes of a network for the purpose of transporting an entity from a source node ("A") to a destination node ("B"). The entity could be, for example, a physical object to be shipped, in which case the nodes would represent waypoints and the links would represent roads or other paths between waypoints. For another example, the entity could be a message or packet of data to be transmitted from A to B, in which case the nodes could be computer-controlled switching stations and the links could be communication channels between the stations. In yet another example, an entity could represent a workpiece while links and nodes could represent, respectively, manufacturing processes and stages in the progress of the workpiece towards a finished product. More generally, the nodes could represent states of an entity and the links could represent allowed transitions of the entity. The purpose of masked proportional routing and of related prior routing procedures is to schedule transitions of entities from their initial states ("A") to their final states ("B") in such a manner as to minimize a cost or to attain some other measure of optimality or efficiency. Masked proportional routing follows a distributed (in the sense of decentralized) approach to probabilistically or deterministically choosing the links. It was developed to satisfy a need for a routing procedure that 1. Does not always choose the same link(s), even for two instances characterized by identical estimated values of associated cost functions; 2. Enables a graceful transition from one set of links to another set of links as the circumstances of operation of the network change over time; 3. Is preferably amenable to separate optimization of different portions of the network; 4. Is preferably usable in a network in which some of the routing decisions are made by one or more other procedure(s); 5. Preferably does not cause an entity to visit the same node twice; and 6. Preferably can be modified so that separate entities moving from A to B do not arrive out of order.

Wolpert, David↗

NASA NTRS2004

Unsteady Aerodynamic Response of a Linear Cascade of Airfoils in Separated Flow

The overall objective of this research program was to investigate methods to modify the leading edge separation region, which could lead to an improvement in aeroelastic stability of advanced airfoil designs. The airfoil section used is representative of current low aspect ratio fan blade tip sections. The experimental potion of this study investigated separated zone boundary layer from removal through suction slots. Suction applied to a cavity in the vicinity of the separation onset point was found to be the most effective location. The computational study looked into the influence of front camber on flutter stability. To assess the influence of the change in airfoil shape on stability the work-per-cycle was evaluated for torsion mode oscillations. It was shown that the front camberline shape can be an important factor for stabilizing the predicted work-per-cycle and reducing the predicted extent of the separation zone. In addition, data analysis procedures are discussed for reducing data acquired in experiments that involve periodic unsteady data. This work was conducted in support of experiments being conducted in the NASA Glenn Research Center Transonic Flutter Cascade. The spectral block averaging method is presented. This method is shown to be able to account for variations in airfoil oscillation frequency that can occur in experiments that force oscillate the airfoils to simulate flutter.

Capece, Vincent R.↗

DOE OSTI2022

Tuning moiré excitons and correlated electronic states through layer degree of freedom

Moiré coupling in transition metal dichalcogenides (TMDCs) superlattices introduces flat minibands that enable strong electronic correlation and fascinating correlated states, and it also modifies the strong Coulomb-interaction-driven excitons and gives rise to moiré excitons. Here, we introduce the layer degree of freedom to the WSe 2 /WS 2 moiré superlattice by changing WSe 2 from monolayer to bilayer and trilayer. We observe systematic changes of optical spectra of the moiré excitons, which directly confirm the highly interfacial nature of moiré coupling at the WSe 2 /WS 2 interface. In addition, the energy resonances of moiré excitons are strongly modified, with their separation significantly increased in multilayer WSe 2 /monolayer WS 2 moiré superlattice. The additional WSe 2 layers also modulate the strong electronic correlation strength, evidenced by the reduced Mott transition temperature with added WSe 2 layer(s). The layer dependence of both moiré excitons and correlated electronic states can be well described by our theoretical model. Our study presents a new method to tune the strong electronic correlation and moiré exciton bands in the TMDCs moiré superlattices, ushering in an exciting platform to engineer quantum phenomena stemming from strong correlation and Coulomb interaction.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Heterogeneous Morphologies and Hardness of Co-Sputtered Thin Films of Concentrated Cu-Mo-W Alloys

Heterogeneous microstructures in Cu-Mo-W alloy thin films formed by magnetron co-sputtering immiscible elements with concentrated compositions are characterized using scanning transmission electron microscopy (STEM) and nanoindentation. In this work, we modified the phase separated structure of a Cu-Mo immiscible system by adding W, which impedes surface diffusion during film growth. The heterogeneous microstructures in the Cu-Mo-W ternary system exhibited bicontinuous matrices and agglomerates composed of Mo(W)-rich phase. This is unique, as these are the slower-diffusing species, contrasting past reports of binary Cu-Mo thin films that exhibited Cu-rich agglomerates. The bicontinuous matrices comprised of Cu-rich and Mo(W)-rich phases exhibited bilayer thicknesses of less than 5 nm. The hardness of these thin films measured using nanoindentation is reported and compared to similar multilayers and nanocomposites in binary systems.

36 MATERIALS SCIENCE↗

NASA NTRS1972

An economical net solar flux radiometer.

The theory and design of an economical solar flux radiometer readily adaptable to the conventional radiosonde system are presented in response to the need cited by the Atmospheric Radiation Working Group (1971) for the development of an inexpensive light-weight short-wave radiometer sonde. Prototype instrument tests and current modifications are discussed. It is shown that the basic instrument can be easily modified to measure separately the upward and downward directed flux components, in addition to the net flux.

Darkow, G. L.↗

NASA NTRS1978

Upgraded viscous flow analysis of multielement airfoils

A description of an improved version of the NASA/Lockheed multielement airfoil analysis computer program is presented. The improvements include several major modifications of the aerodynamic model as well as substantial changes of the computer code. The modifications of the aerodynamic model comprise the representation of the boundary layer and wake displacement effects with an equivalent source distribution, the prediction of wake parameters with Green's lag-entrainment method, the calculation of turbulent boundary layer separation with the method of Nash and Hicks, the estimation of the onset of confluent boundary layer separation with a modified form of Goradia's method, and the prediction of profile drag with the formula of Squire and Young. The paper further describes the modifications of the computer program for which the structured approach to computer software development was employed. Important aspects of the structured program development such as the functional decomposition of the aerodynamic theory and its numerical implementation, the analysis of the data flow within the code, and the application of a pseudo code are discussed.

Brune, G. W.↗

NASA NTRS1979

Upgraded viscous flow analysis of multi-element airfoils

A description of an improved version of the NASA/Lockheed multi-element airfoil analysis computer program is presented. The improvements include several major modifications of the aerodynamic model as well as substantial changes of the computer code. The modifications of the aerodynamic model comprise the representation of the boundary layer and wake displacement effects with an equivalent source distribution, the prediction of wake parameters with Green's lag-entrainment method, the calculation of turbulent boundary layer separation with the method of Nash and Hicks, the estimation of the onset of confluent boundary layer separation with a modified form of Goradia's method, and the prediction of profile drag with the formula of Squire and Young. The modifications of the computer program for which the structured approach to computer software development was employed are also described. Important aspects of the structured program development such as the functional decomposition of the aerodynamic theory and its numerical implementation, the analysis of the data flow within the code, and the application of a pseudo code are discussed.

Brune, G. W.↗

NASA NTRS1979

Length and bursting of separation bubbles: A physical interpretation

A physical interpretation of the observed form of the pressure distribution beneath a two-dimensional separation bubble which modified the external inviscid pressure distribution only locally is given in terms of boundary layer concepts. A simple method for estimating along a mean streamline entrained into the underside of a growing shear layer through the transition region is discussed, and predictions of bubble bursting conditions and a lower bound on the bubble length are compared with experiment.

Russell, J. M.↗

NASA NTRS1988

Algebraic turbulence models for the computation of two-dimensional high speed flows using unstructured grids

The incorporation of algebraic turbulence models in a solver for the 2-D compressible Navier-Stokes equations using triangular grids is described. A practical way to use the Cebeci Smith model, and to modify it in separated regions is proposed. The ability of the model to predict high speed, perfect gas boundary layers is investigated from a numerical point of view.

Rostand, Philippe↗

NASA NTRS1989

Algebraic turbulence models for the computation of two-dimensional high-speed flows using unstructured grids

The incorporation of algebraic turbulence models in a solver for the 2-D compressible Navier-Stokes equations using triangular grids is described. A practial way to use the Cebeci Smith model, and to modify it in separated regions is proposed. The ability of the model to predict high speed, perfect gas boundary layers is investigated from a numerical point of view.

Rostand, Philippe↗

NASA NTRS2002

Report on Project to Characterize Multi-Junction Solar Cells in the Stratosphere using Low-Cost Balloon and Communication Technologies

Balloon, control and communication technologies are under development in our laboratory for testing multi-junction solar cells in the stratosphere to achieve near AM0 conditions. One flight, Suntracker I, has been carried out reported earlier. We report on our efforts in preparation for a second flight, Suntracker II, that was aborted due to hardware problems. The package for Suntracker I system has been modified to include separate electronics and battery packs for the 70 centimeter and 2 meter systems. The collimator control system and motor gearboxes have been redesigned to address problems with the virtual stops and backlash. Surface mount technology on a printed circuit board was used in place of the through-hole prototype circuit in efforts to reduce weight and size, and improve reliability. A mobile base station has been constructed that includes a 35' tower with a two axis rotator and multi-element yagi antennas. Modifications in Suntracker I and the factors that lead to aborting Suntracker II are discussed.

Mirza, Ali↗

NASA NTRS2004

Preparation of Proton Exchange Membranes and Lithium Batteries from Melamine-containing Ormosils

Our laboratory has recently reported a series of rodcoil polymers for lithium batteries that display dimensionally stable films with good ionic conductivity. The rod segments consist of rigid linear and branched polyimides and the coil segments are polyethylene oxides (PEO). It has been proposed that good mechanical and transport properties are due to phase separation between the rod and coil segments. It was also observed that increased branching and molecular weight lead to increased conductivity. The following study was undertaken to assess the effects of phase separation in polyalkylene oxides connected by melamine linkages. Melamine was chosen as the linking unit because it provides a branching site, cation binding sites to help ionic transport between polymer chains, and the opportunity for self assembly through hydrogen bonding. Polymers were made by the reaction of cyanuric chloride with a series of amine-terminated alkylene oxides. A linear polymer was first made, followed by reaction of the third site on cyanuric chloride with varying ratios of monofunctional Jeffamine and (3-aminopropyl)triethoxysilane. The lithium trifluoromethane sulfonamide-doped polymers are then crosslinked through a sol-gel process to form free-standing films. Initial results have shown mechanically strong films with lithium conductivities on the order of 2 x 10(exp -5) S/cm at ambient temperature. In a separate study, organically modified silanes (Ormosils) that contain sulfonic acid derivatized melamines have been incorporated into proton exchange membranes. The membranes are made by reaction of the primary amine groups of various ratios of melamine derivative and difunctional Jeffamine (MW = 2000) with the epoxide group of (3-Glycidyloxypropyl)trimethoxysilane. The films were then cross-linked through a sol-gel process. Resulting sulfuric acid doped films are strong, flexible, and have proton conductivities on the order of 2 x l0(exp -2) S/cm (120 C, 25% relative humidity). Our best results have been observed when films contain 60% PEO and 40% sulfonated melamine.

Tigelaar, Dean M.↗

NASA NTRS2023

Computational Study of Vortex-Induced Separation for a 5-Bladed Rotor

This work computationally investigated the rotor blade vortex-induced separation recently observed during an aerodynamic rotor test campaign in the NASA Langley Research Center 14- by 22-Foot Subsonic Tunnel. Two separate approaches (i.e., airfoil modification and blade tip modification) were studied to mitigate the vortex-induced separation. Low-fidelity tools based on blade element momentum theory were shown to mispredict the rotor inflow and were also shown to not capture the vortex-induced separation caused by perpendicular blade-vortex interaction. This misprediction was exploited to isolate the aerodynamic thrust deficit caused by the vortex-induced separation (i.e., 20%) from the thrust deficit due to inflow variation (i.e., 31%). High-fidelity tools were shown to reasonably predict aerodynamic forces within 13% and flow separation when compared to experimental results. The modified airfoil variant of the baseline rotor effectively mitigated the vortex-induced separation while the blade tip modified variant still showed separation, though the size and strength of the vortex was reduced. Acoustic predictions were underpredicted by 10 dB from preliminary measurements taken in the untreated wind tunnel. Broadband noise contributions from different rotor blade sections showed that self-noise due to flow separation and other turbulent boundary layer mechanisms was the dominant noise source for all three rotor cases, followed by blade-wake interaction noise caused by perpendicular blade-vortex interactions.

aerodynamics↗

NASA NTRS1985

High cycle life secondary lithium battery

A secondary battery (10) of high energy density and long cycle is achieved by coating the separator (18) with a film (21) of cationic polymer such as polyvinyl-imidazoline. The binder of the positive electrode (14) such as an ethylene-propylene elastomer binder (26) containing particles (28) of TiS.sub.2 chalcogenide can also be modified to contain sulfone functional groups by incorporating liquid or solid sulfone materials such as 0.1 to 5 percent by weight of sulfolane into the binder. The negative lithium electrode (14), separator (18) and positive electrode (16) are preferably spirally wound and disposed within a sealed casing (17) containing terminals (32, 34). The modified separator and positive electrode are more wettable by the electrolytes in which a salt is dissolved in a polar solvent such as sulfolane.

Yen, Shiao-Ping S.↗

NASA NTRS1974

Extension of a vortex-lattice method to include the effects of leading-edge separation

Vortex-lattice methods have been used successfully to obtain the aerodynamic coefficients of lifting surfaces without leading-edge separation. It is shown how an existing vortex-lattice method can be modified to include the effects of leading-edge separation. The modified version is then used to calculate the aerodynamic loads on a highly swept delta wing. The results are compared with Peckham's (1958) experimental data.

Mook, D. T.↗