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DOE OSTI2021

Markov Chain Monte Carlo Predictions of Neutron-rich Lanthanide Properties as a Probe of r -process Dynamics

Lanthanide element signatures are key to understanding many astrophysical observables, from merger kilonova light curves to stellar and solar abundances. To learn about the lanthanide element synthesis that enriched our solar system, we apply the statistical method of Markov Chain Monte Carlo to examine the nuclear masses capable of forming the r-process rare-earth abundance peak. We describe the physical constraints we implement with this statistical approach and demonstrate the use of the parallel chains method to explore the multidimensional parameter space. We apply our procedure to three moderately neutron-rich astrophysical outflows with distinct types of r-process dynamics. We show that the mass solutions found are dependent on outflow conditions and are related to the r-process path. We describe in detail the mechanism behind peak formation in each case. We then compare our mass predictions for neutron-rich neodymium and samarium isotopes to the latest experimental data from the CPT at CARIBU. Here, we find our mass predictions given outflows that undergo an extended (n,γ)⇌(γ,n) equilibrium to be those most compatible with both observational solar abundances and neutron-rich mass measurements.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1991

Powder towpreg process development

The process for dry powder impregnation of carbon fiber tows being developed at LaRC overcomes many of the difficulties associated with melt, solution, and slurry prepregging. In the process, fluidized powder is deposited on spread tow bundles and fused to the fibers by radiant heating. Impregnated tows have been produced for preform, weaving, and composite materials applications. Design and operating data correlations were developed for scale up of the process to commercial operation. Bench scale single tow experiments at tow speeds up to 50 cm/sec have demonstrated that the process can be controlled to produce weavable towpreg. Samples were woven and molded into preform material of good quality.

Baucom, Robert M.↗

NASA NTRS1983

Low cost solar array project. Cell and module formation research area. Process research of non-CZ silicon material

Liquid diffusion masks and liquid dopants to replace the more expensive CVD SiO2 mask and gaseous diffusion processes were investigated. Silicon pellets were prepared in the silicon shot tower; and solar cells were fabricated using web grown where the pellets were used as a replenishment material. Verification runs were made using the boron dopant and liquid diffusion mask materials. The average of cells produced in these runs was 13%. The relationship of sheet resistivity, temperature, gas flows, and gas composition for the diffusion of the P-8 liquid phosphorus solution was investigated. Solar cells processed from web grown from Si shot material were evaluated, and results qualified the use of the material produced in the shot tower for web furnace feed stock.

Source record↗

DOE OSTI2021

High-salinity brine desalination with amine-based temperature swing solvent extraction: A molecular dynamics study

Solvent extraction desalination (SED) is a promising technique for efficiently treating high salinity brines. However, only a few studies in the literature have investigated the influence of the molecular characteristics of the organic solvents on the emergent performance of the separation process. Thus, in this work we investigate the influence of the molecular structure of four different secondary amines on the desalination process of a concentrated aqueous solution of NaCl. Molecular dynamics simulations and free energy calculations are used to obtain the thermodynamic and structural properties of the pure solvent bulk phase, as well as a homogeneous solvent-water bulk mixture. Furthermore, solvent-water and solvent-brine interfacial systems are used to explicitly analyze the water partitioning behavior in the relevant temperature range for SED. The water solubilization in these secondary amines is found to be an exothermic process. Additionally, although the hydrogen-bonding interaction between the water and solvent molecules are beneficial, this interaction is not necessarily the dominant factor for ranking the water solubility performance of the different solvents. Finally, the excess volume of mixing of the bulk solvent-water mixture, as well as the electrostatic surface features of the solvents are also found to provide important clues for screening solvent behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Plasma Wall Interaction with 3-D Plasma Boundaries

The interaction of the edge plasma and the material surfaces is one of the most critical challenges on the path to harness fusion power as new, fundamental energy source. This challenge typically combines the thrust to reach high density, low temperature (detached) plasmas in front of the divertor target plates as well as understanding the plasma material interaction (PMI) in particular in this regime. The combination of both research thrusts represents an extraordinarily challenging subject encompassing spatial scales spanning nanometers to meters in all states of matter and across a broad energy range. Modeling capabilities, which help to interpret data from nowadays experiments and enable extrapolation to future devices are urgently required. This is in particular true for toroidal magnetic confinement devices with three-dimensional (3D) plasma boundaries. Such plasma boundary geometries occur in tokamaks, when small amplitude magnetic perturbations are used to stabilize the unruly edge plasma or in stellarators, that are inherently 3D plasma confinement devices. In this project, the impact of 3D plasma boundaries on the plasma material interaction (PMI) was assessed. This work focused on plasma boundary conditions, in which high-density conditions at the material surfaces yield mitigation of the otherwise immense heat and particle loads that these materials would see. These so-called high recycling and eventually detached plasma regimes are of great interest for future reactor operation. In the project, key features that are unique to 3D boundaries were explored in comparison to canonically assumed axisymmetric plasma edge situations in tokamaks. In particular, the relevance of the 3D boundary situation in the extrapolation to the plasma boundary solution at ITER, the next step fusion energy experiment under construction as a multi-national, world-wide large-science experiment in southern France, has been explored. The EMC3-EIRENE plasma edge fluid and kinetic neutral transport code has been advanced to cope with the challenging and unprecedented conditions in the ITER boundary plasma including 3D fields that are planned to be used to suppress harmful edge instabilities, the so-called edge localized modes. This is a vital integration challenge for ITER and the results from this grant have provide a leading capability for this assessment. It was shown that the detachment process in a 3D edge solution for ITER follows the recycling regimes that are known from axisymmetric solutions, but that multiple plasma exhaust channels connected to the material surfaces are established which feature individual recycling characteristics. Because these channels touch the material surfaces in the divertor in a 3D geometry, the compatibility with the plasma material interaction (PMI), including erosion and impurity generation has been found to be an important part of the integration challenge. To address this, the fully 3D plasma material interaction code ERO2 has been adapted to these ITER specific geometries and a homogeneous mixing model was implemented, that allows to consider the mixing of Be and Was used at ITER in the PMI modeling. This model enhancement has been used to study non-local migration of Be in the JET ITER like wall configuration and it has been shown that with this model such complex migration processes in ITER relevant plasma shapes and with ITER relevant plasma boundary conditions can be addressed. The combined modeling approach using EMC3-EIRENE as a plasma boundary transport code and the ERO2 specialized PMI model will be an asset for the continued preparations of ITER operation as well as for Fusion Pilot Plant efforts that have emerged in the U.S. during the evolution of this grant. The predictive capability of this numerical tool has been validated at the DIII-D US national fusion facility. Here, dedicated plasma edge diagnostics were implemented to measure the impurity household around a 3D edge plasma during ELM suppression by 3D fields. Dedicated experiments with local material probes using these diagnostics and the state-of-the-art suite of boundary measurements at DIII-D have shown that the 3D perturbation of the plasma edge that is excreted by such 3D control fields yield a perturbation of the plasma boundary flux structure and hence also of the resulting PMI. The 3D boundary plasma is composed out of helical magnetic flux channels that intersect the divertor targets at an angle relative to the main guiding field, i.e., the toroidal magnetic field component of the tokamak. A similar effect has been measured as well on limiter surfaces during the startup campaign at the new stellarator experiment Wendelstein 7-X. These experiments ad initial analysis with the ERO plasma material interaction model, suggested that the place of erosion for a given particle from the surface and its re-deposition can be different in such 3D field geometries yielding potentially a significant level of net-erosion. This is not the case for axisymmetric solutions, where it was shown in the past that the eroded particles are effectively re-deposited into gaps produced by erosion at the same position and hence the net-erosion levels are small. For ITER, the quest to suppress the ELMs and at the same time maintain the integrity of the divertor is an issue, which these fundamental findings will help to resolve. The coupling of this work to the extrapolation in the ITER program has been addressed by both the PI and the lead numerical scientist being ITER Science Fellows in the duration of the contract and forward. A second focus in the exploration of 3D boundary effects on tokamaks and stellarators has been set on the measurement of helium exhaust features with such 3D fields. This is important because He represents the ash of the fusion process and needs to be exhausted. It was shown that 3D field application compatible with suppression of ELMs yields an increase of the helium exhaust performance. The ratio of the effective helium confinement time over the energy confinement time was reduced by almost 50% which demonstrated that the impact of helium accumulation in the plasma core with respect to the confinement of energy to sustain the fusion reaction is significantly improved with such 3D control fields. It was shown that this is the case for tokamaks as well as stellarators. At the Large helical Device in Japan, a similar enhancement of the helium exhaust features when small amplitude additional 3D fields were applied was measured. This is an important additional function of 3D field application and its impact on ITER is presently being studied in combination with investigations of helium exhaust in 3D field geometries of stellarator devices.

3D plasma edge transport↗

DOE OSTI2025

Advanced Brine Processing to Enable U.S. Lithium Independence (CRADA Report)

Current production of LiOH, which is needed to make Li-ion battery cathode active materials, utilizes a multistep process including solar evaporation, precipitation with Na 2 CO 3 and then conversion to LiOH using Ca(OH) 2 . This process requires a large amount of land area for solar evaporation, the right weather conditions, and chemicals for the conversion process that result in NaCl and CaCO 3 waste products. The production of Ca(OH) 2 is very energy intensive and evolves significant quantities of CO 2 . An alternative process flow utilizing direct lithium extraction techniques, followed by a chemical free conversion process can have benefits in reducing the needed land requirements and chemicals for traditional brine processing. There are many potential direct lithium extraction technologies that are currently being developed. The direct lithium extraction process from typical brine sources will produce a LiCl solution with some impurities including typically high concentrations of Na. This brine then needs to be converted to LiOH for use in battery cathode production. Ideally this conversion could occur without the use of additional chemicals. Electrochemistry can do this conversion either via electrolysis or bipolar membrane electrodialysis (BPED) to produce LiOH and HCl in solution. BPED utilized bipolar membranes to split water, which has a reduced potential as compared to splitting water at electrodes into hydrogen and oxygen gas. This reduced potential required results in a significant energy savings for BPED over electrolysis methods. This CRADA project aimed to develop such an integrated process using direct lithium extraction followed by BPED to produce a LiOH solution. That solution can then be crystallized into battery grade LiOH. In particular, Albemarle utilized a direct lithium extraction process to produce a concentrated LiCl solution that could be used for the BPED process. The BPED process was first tested using various LiCl solutions with impurity ions added at bench scale to understand the effects of impurities and determine processing parameters. Then testing was performed using the direct lithium extracted brine at the bench scale before scaling the process up. After the process was scaled up a long duration test was carried out to estimate the lifetime of the membranes, which is key to the economics of the BPED process.

25 ENERGY STORAGE↗

DOE OSTI2026

Designing a Robust MEA-Based Post-Combustion Carbon Capture Process with Capture Rate Guarantees

This work presents an application of the nonlinear two-stage robust optimization solver PyROS to the model-based design and operation of a monoethanolamine scrubbing process for CO2 capture under epistemic uncertainty. Through this application, risk-averse process designs are successfully obtained for CO2 capture targets ranging from 90% to over 99%. In particular, the risk-averse solutions for CO2 capture targets of up to 98% are shown to be only marginally more expensive than their nominally optimal counterparts. Thus, the results demonstrate the utility of recently developed nonlinear robust optimization approaches for the solution of large-scale chemical process models under uncertainty.

20 FOSSIL-FUELED POWER PLANTS↗

NASA NTRS2016

Low Temperature Regolith Bricks for In-Situ Structural Material

Current technology for producing in-situ structural materials on future missions to Mars or the moon relies heavily on energy-intensive sintering processes to produce solid bricks from regolith. This process requires heating the material up to temperatures in excess of 1000 C and results in solid regolith pieces with compressive strengths in the range of 14000 to 28000 psi, but are heavily dependent on the porosity of the final material and are brittle. This method is currently preferred over a low temperature cementation process to prevent consumption of precious water and other non-renewable materials. A high strength structural material with low energy requirements is still needed for future colonization of other planets. To fulfill these requirements, a nano-functionalization process has been developed to produce structural bricks from regolith simulant and shows promising mechanical strength results. Functionalization of granular silicate particles into alkoxides using a simple low temperature chemical process produces a high surface area zeolite particles that are held together via inter-particle oxygen bonding. Addition of water in the resulting zeolite particles produces a sol-gel reaction called "inorganic polymerization" which gives a strong solid material after a curing process at 60 C. The aqueous solution by-product of the reaction is currently being investigated for its reusability; an essential component of any ISRU technology. For this study, two batches of regolith bricks are synthesized from JSC-1A; the first batch from fresh solvents and chemicals, the second batch made from the water solution by-product of the first batch. This is done to determine the feasibility of recycling necessary components of the synthesis process, mainly water. Characterization including BET surface area, SEM, and EDS has been done on the regolith bricks as well as the constituent particles,. The specific surface area of 17.53 sq m/g (average) of the granular regolith material was obtained from nitrogen adsorption isotherm measurement. The size, shape and textures of regolith from SEM shows that the particles are 25-50 micrometers in size and mostly irregular in shape (Figure 1a). The elemental composition of regolith was identified from EDS analysis showed the presence of Si, Al, Fe, Na, Mg, Ca, Ti, O and C (see figure 1b). Each set of cylindrical brick samples were prepared by low energy process, and cured for 21 and 28 days, respectively to compare their compressive strength. Figure 1c, and d shows the JSC-1A brick and the compressive strength measurements. The results from the 21 day cured bricks (2 bricks) have been done and yielded an aver-age strength of 3050 psi, considerably higher than Portland cement mortars (Type IV and V). This promising technology provides the benefits of construction material similar to concrete, with a low complexity, low energy synthesis process and the likelihood of complete reusability of precious resources. Compressive strength using this method can be improved by increasing the surface area of the particles, using bi-modal particle size distribution, and adding certain additives to increase inter-particle forces.

ISRU↗

DOE OSTI2021

Modification of Wool Fibers via Base/Cationic Detergent Pretreatment and Transglutaminase-mediated Reaction of Keratin

The surface modification of wool fibers is an important part of the textile industry to add functionality and stability to wool products. In this study, we developed a process utilizing a base/cationic surfactant solution pretreatment followed by an enzyme-mediated keratin crosslinking reaction to modify the wool fibers. Changes in water contact angle demonstrated the successful transformation of the hydrophobic wool surface to a more hydrophilic one after soaking in sodium carbonate solution containing hexadecyltrimethylammonium bromide (CTAB). The treated fabrics were further characterized by colorimetry and fluorescent spectrometry. Results showed that the pretreatment increased the yellowness of fabrics and caused some structural changes among certain amino acids, such as tryptophan and cystine. Keratin extracted from coarse wool fibers was further applied on pretreated fabrics through a microbial transglutaminase (mTGase) mediated reaction under mild conditions. Morphological characterization via SEM demonstrated the effective coverage of keratin on the scales of wool. The current method may provide an alternative processing protocol to modify wool fibers and improve the quality and performance of wool products.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Acid–Base Properties of Azo Dyes in Solution Studied Using Spectrophotometry and Colorimetry

Colorimetry and spectrophotometry with chemometric data processing were used to study the acid–base properties of azo dyes in aqueous solution. The capabilities of both methods were compared. Ionization constants of all the functional groups of the azo compounds studied could be determined relative to the change in the specific color difference depending on the acidity of the medium. The colorimetric functions of ion-molecular forms of azo compounds used as an analytical signal allow us to obtain complete information on the acid–base equilibrium in a wide acidity range.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1991

LaRC dry powder towpreg process

The dry powder towpreg process overcomes many of the difficulties associated with melt, solution and slurry prepregging of advanced composite materials. In the process, fluidized powder is deposited on spread tow bundles and melted on the fibers by radiant heating to adhere the polymer to the fiber. Bench scale design and operating data have been correlated for use in process scale up to commercial operation. Powdered towpreg has been woven and molded into preform material of good quality. Cost estimates suggest that processing costs are comparable to those of conventional hot melt prepreg. In the future, from a part fabrication point of view, powder coated prepreg tape, woven broad goods and woven and braided preforms may be considered as options to similar materials made by other methods.

Marchello, Joseph M.↗

NASA NTRS1971

Bayesian recursive image estimation.

A procedure for recursively estimating images that are characterized statistically by the mean and correlation functions associated with the random process representing the brightness level is proposed for the case where the images are corrupted by additive noise. First, a dynamic model is developed with a response characteristic which matches that of the scanner output (the input of the estimator is the output of a horizontal line scanner) in a statistical sense. Such models have the form of an ordinary differential or difference equation with white noise input. An insignificant approximation is introduced by using a constant-coefficient model. The appropriate model is a vector valued difference equation with the solution representing a vector Markov process. The next step is to obtain the minimum mean square estimate of the image by using a Kalman filter. Since the image estimation is an interpolation problem, two successive runs over the observation are performed in opposite directions and the resultant estimates are averaged. Examples are included for illustration.

Nahi, N. E.↗

NASA NTRS1982

Exact triple integrals of beam functions

Definite triple integrals encountered in applying the Galerkin method to the problem of heat and mass transfer across rectangular enclosures are discussed. Rather than evaluating them numerically, the technique described by Reid and Harris (1958) was extended to obtain the exact solution of the integrals. In the process, four linear simultaneous equations with triple integrals as unknowns were obtained. These equations were then solved exactly to obtain the closed form solution. Since closed form representations of this type have been shown to be useful in solving nonlinear hydrodynamic problems by series expansion, the integrals are presented here in general form.

Jhaveri, B. S.↗

NASA NTRS1997

Microgravity Processing and Photonic Applications of Organic and Polymeric Materials

Some of the primary purposes of this work are to study important technologies, particularly involving thin films, relevant to organic and polymeric materials for improving applicability to optical circuitry and devices and to assess the contribution of convection on film quality in unit and microgravity environments. Among the most important materials processing techniques of interest in this work are solution-based and by physical vapor transport, both having proven gravitational and acceleration dependence. In particular, PolyDiAcetylenes (PDA's) and PhthaloCyanines (Pc's) are excellent NonLinear Optical (NLO) materials with the promise of significantly improved NLO properties through order and film quality enhancements possible through microgravity processing. Our approach is to focus research on integrated optical circuits and optoelectronic devices relevant to solution-based and vapor processes of interest in the Space Sciences Laboratory at the Marshall Space Flight Center (MSFC). Modification of organic materials is an important aspect of achieving more highly ordered structures in conjunction with microgravity processing. Parallel activities include characterization of materials for particular NLO properties and determination of appropriation device designs consistent with selected applications. One result of this work is the determination, theoretically, that buoyancy-driven convection occurs at low pressures in an ideal gas in a thermalgradient from source to sink. Subsequent experiment supports the theory. We have also determined theoretically that buoyancy-driven convection occurs during photodeposition of PDA, an MSFC-patented process for fabricating complex circuits, which is also supported by experiment. Finally, the discovery of intrinsic optical bistability in metal-free Pc films enables the possibility of the development of logic gate technology on the basis of these materials.

Frazier, Donald O.↗

DOE OSTI2019

Real time monitoring of the chemistry of hydroxylamine nitrate and iron as surrogates for nuclear materials processing

The separation of actinides in aqueous solution often involves changes in redox chemistry achieved by reagents such as hydroxylamine nitrate (HAN). As a result, in situ monitoring of the chemistry of HAN in contact with plutonium and neptunium in concentrated nitric acid at 35°C is important for the efficacy of Pu-238 extraction. A spectroscopic method of following the chemistry of HAN in contact with iron (as a simulant for plutonium) was developed, using a quantum cascade laser-attenuated total reflectance (QCL-ATR) system. The mid-infrared (3.67–12.5 μm) was chosen for its ability to distinguish the molecular vibrations of analytes and exclude the background absorption of the concentrated HNO 3 matrix. The concentrations of chemical species found in the reaction were drawn from the collected QCL power data using Beer’s law after a baseline correction. These data were qualitatively compared to a kinetic rate model based on a simplified reaction mechanism. The QCL-ATR method can help assess the areas of stability of HAN, nitrate/nitrite interactions, and assist process control of actinide separations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Novel Lattice Solutions for the LHeC

Unprecedently high luminosity of 10 34 cm -2 s -1 , promised by the LHeC accelerator complex poses several beam dynamics and lattice design challenges. As part of accelerator design process, exploration of innovative beam dynamics solutions and their lattice implementations is the key to mitigating performance limitations due to fundamental beam phenomena, such as: synchrotron radiation and collective instabilities. This article will present beam dynamics driven approach to accelerator design, which in particular, addresses emittance dilution due to quantum excitations and beam breakup instability in a large scale, multi-pass Energy Recovery Linac (ERL). The use of ERL accelerator technology to provide improved beam quality and higher brightness continues to be the subject of active community interest and active accelerator development of future Electron Ion Colliders (EIC). Here, we employ current state of though for ERLs aiming at the energy frontier EIC. We will follow conceptual design options recently identified for the LHeC. The main thrust of these studies was to enhance the collider performance, while limiting overall power consumption through exploring interplay between emittance preservation and efficiencies promised by the ERL technology. Here, this combined with a unique design of the Interaction Region (IR) optics gives the impression that luminosity of 10 34 cm -2 s -1 is indeed feasible.

43 PARTICLE ACCELERATORS↗

NASA NTRS1989

Image processing software for providing radiometric inputs to land surface climatology models

During the First International Land Surface Climatology Project (ISLSCP) Field Experiment (FIFE), 80 gigabytes of image data were generated from a variety of satellite and airborne sensors in a multidisciplinary attempt to study energy and mass exchange between the land surface and the atmosphere. To make these data readily available to researchers with a range of image data handling experience and capabilities, unique image-processing software was designed to perform a variety of nonstandard image-processing manipulations and to derive a set of standard-format image products. The nonconventional features of the software include: (1) adding new layers of geographic coordinates, and solar and viewing conditions to existing data; (2) providing image polygon extraction and calibration of data to at-sensor radiances; and, (3) generating standard-format derived image products that can be easily incorporated into radiometric or climatology models. The derived image products consist of easily handled ASCII descriptor files, byte image data files, and additional per-pixel integer data files (e.g., geographic coordinates, and sun and viewing conditions). Details of the solutions to the image-processing problems, the conventions adopted for handling a variety of satellite and aircraft image data, and the applicability of the output products to quantitative modeling are presented. They should be of general interest to future experiment and data-handling design considerations.

Newcomer, Jeffrey A.↗

DOE OSTI2017

Ketonization of levulinic acid and γ-valerolactone to hydrocarbon fuel precursors

We studied a new process for direct conversion of either levulinic acid (LA) or γ-valerolactone (GVL) to hydrocarbon fuel precursors. The process involves passing an aqueous solution of LA or GVL containing a reducing agent, such as ethylene glycol or formic acid, over a ketonization catalyst at 380–400 °C and atmospheric pressure to form a biphasic liquid product. The organic phase is significantly oligomerized and deoxygenated and comprises a complex mixture of open-chain alkanes and olefins, aromatics, and low concentrations of ketones, alcohols, ethers, and carboxylates or lactones. Carbon content in the aqueous phase decreases with decreasing feed rate; the aqueous phase can be reprocessed through the same catalyst to form additional organic oils to improve carbon yield. Catalysts are readily regenerated to restore initial activity. Furthermore, the process might be valuable in converting cellulosics to biorenewable gasoline, jet, and diesel fuels as a means to decrease petroleum use and decrease greenhouse gas emissions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗