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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 703 records · Page 39
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Microchannel reactive distillation for the conversion of aqueous ethanol to ethylene

Here we demonstrate the proof-of-concept for microchannel reactive distillation for alcohol-to-jet application: combining ethanol/water separation and ethanol dehydration in one unit operation. Ethanol is first distilled into the vapor phase, converted to ethylene and water, and then the water co-product is condensed to shift the reaction equilibrium. Process intensification is achieved through rapid mass transfer—ethanol stripping from thin wicks using novel microchannel architectures—leading to lower residence time and improved separation efficiency. Energy savings are realized with integration of unit operations. For example, heat of condensing water can offset vaporizing ethanol. Furthermore, the dehydration reaction equilibrium shifts towards completion by immediate removal of the water byproduct upon formation while maintaining aqueous feedstock in the condensed phase. For aqueous ethanol feedstock (40% w ), 71% ethanol conversion with 91% selectivity to ethylene was demonstrated at 220 °C, 600 psig, and 0.28 h -1 wt hour space velocity. 2.7 stages of separation were also demonstrated, under these conditions, using a device length of 8.3 cm. This provides a height equivalent of a theoretical plate (HETP), a measure of separation efficiency, of ~3.3 cm. By comparison, conventional distillation packing provides an HETP of ~30 cm. Thus, 9.1× reduction in HETP was demonstrated over conventional technology, providing a means for significant energy savings and an example of process intensification. Finally, preliminary process economic analysis indicates that by using microchannel reactive distillation technology, the operating and capital costs for the ethanol separation and dehydration portion of an envisioned alcohol-to-jet process could be reduced by at least 35% and 55%, respectively, relative to the incumbent technology, provided future improvements to microchannel reactive distillation design and operability are made.

10 SYNTHETIC FUELS↗
DOE OSTI2023

Separation of volatile organic contaminants from water using a direct-contact dehumidifier: An experimental study and modeling

A packed-bed, direct-contact dehumidifier (PB-DCD) has been developed to selectively condense water from a gaseous mixture of organic contaminants. In this process, hot air is humidified by mixing with wastewater vapor in a static mixer and is dehumidified by subcooled fresh water passing through the PB-DCD in a counter-current configuration. The goal of this study is to understand the relationship between various operating parameters and how they affect separation of isopropyl alcohol (IPA) from the gaseous mixture with the purpose of expanding the investigation to other contaminants in the future. The process has been successfully used to separate IPA from wastewater. Different parameters including the concentration of IPA in water, feed temperature, air-to-vapor ratio, and cooling-water-to-vapor mass ratio, as well as residence time were examined to determine their influence on contaminant separation and clean water recovery rate. The Buckingham Pi theorem was applied to reduce the number of studying variables by generating non-dimensional groups. Experiments were performed to determine the relationship between the non-dimensional parameters and model mass transfer in the system. Mass transfer coefficients for multicomponent gaseous mixture condensation in a packed-bed direct contact condenser column are calculated and a modified correlation of mass transfer is developed. The parameters of the mass transfer model are obtained from operating conditions of the PB-DCD, stream conditions and thermodynamic properties. A modified Sherwood correlation is developed to predict IPA separation from a gaseous mixture consisting of air, water, and IPA. The modified Sherwood correlation is applied to successfully predict the Sherwood number with a mean absolute error equal to 6.6 %. According to the experimental results, the maximum IPA separation achieved was 76.3 %, which corresponds to a water recovery rate of 58.7 %.

42 ENGINEERING↗
DOE OSTI2026

Validation of electron backscattering in the MCNP6.3 code

A new electron backscattering validation suite has been developed for the MCNP® code. The calculations in this suite cover both condensed history and single-event transport methods, seven different elemental materials ranging from beryllium to uranium, and incident electron energies from 200 eV to 14.1 MeV. In general, the accuracy of the MCNP code for electron backscattering calculations is energy-dependent. For incident electron energies below 2 keV, the condensed history method is not applied while the single-event method shows poor agreement with experimental measurements due to poor accuracy of the underlying atomic data. For incident energies between 2 keV and 256 keV, the single-event method typically shows better agreement with experiments, while for incident energies above 256 keV the condensed history method gives better accuracy. Additionally, agreement with experimental data is generally worse for low- Z materials such as beryllium and carbon, which may reflect deficiencies in the data or physics underlying electron transport through light elements in the MCNP code. The new electron backscattering validation suite, along with the previously introduced electron stopping power and Lockwood energy deposition validation suites, provide MCNP users with a quantified understanding of the uncertainties in electron transport calculations. Future improvements to electron transport in the MCNP code are necessary for low energies (≤ 2 keV) and for low- Z materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Intense formation of secondary ultrafine particles from Amazonian vegetation fires and their invigoration of deep clouds and precipitation

New particle formation (NPF) in fire smoke is thought to be unlikely due to large condensation and coagulation sinks that scavenge molecular clusters. We analyze aircraft measurements over the Amazon and find that fires significantly enhance NPF and ultrafine particle (UFP < 50 nm diameter) numbers compared to background conditions, contrary to previous understanding. We identify that the nucleation of dimethylamine with sulfuric acid, which is aided by the formation of extremely low volatility organics in biomass-burning smoke, can overcome the large condensation and coagulation sinks and explain aircraft observations. We show that freshly formed clusters rapidly grow to UFP sizes through biomass-burning secondary organic aerosol formation, leading to a 10-fold increase in UFP number concentrations. Here, we find a contrasting effect of UFPs on deep convective clouds compared to the larger particles from primary emissions for the case investigated here. UFPs intensify the deep convective clouds and precipitation due to increased condensational heating, while larger particles delay and reduce precipitation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Hydrodynamic behavior of wrapped coil water heater tank

In this work, a numerical investigation using computational fluid dynamics (CFD) has been carried out to analyze the thermal behavior of a water tank integrated to a heat pump water heating system (HPWH). The heat pump condenser is a long coil wrapped around the water tank and insulated from outside from which heat is transferred from the heat pump cycle into the water stored inside the tank. The simulated water tank has a capacity of about 170 L with the charging inlet located at the bottom segment of the tank and the discharging outlet located at the top segment of the tank like commercially available water heaters. The tank was simulated during charging/discharging process with isothermal boundary condition at the tank wall to represent the majority of the process for refrigerant condensation inside the heat pump condenser (excluding superheated and sub-cooled section). Three flow rates were selected to represent low, medium and high flow pattern. Both mean and turbulent flow properties were calculated and analyzed. Heat transfer mechanisms inside the tank are quantified by calculating Richardson and Péclet numbers to show the relative contribution of driving forces. The calculations show that advection is dominant over diffusion. Mixing factor is calculated and presented. It is found that the rate of increase of mixing is nonlinear with the increase in flow rate. Mixing increased by a factor of four when the flow rate increased by a factor of two.

stratification↗
DOE OSTI2020

Metabolic engineering of β-oxidation to leverage thioesterases for production of 2-heptanone, 2-nonanone and 2-undecanone

Medium-chain length methyl ketones are potential blending fuels due to their cetane numbers and low melting temperatures. Biomanufacturing offers the potential to produce these molecules from renewable resources such as lignocellulosic biomass. Here, we designed and tested metabolic pathways in Escherichia coli to specifically produce 2-heptanone, 2-nonanone and 2-undecanone. We achieved substantial production of each ketone by introducing chain-length specific acyl-ACP thioesterases, blocking the β-oxidation cycle at an advantageous reaction, and introducing active β-ketoacyl-CoA thioesterases. Using a bioprospecting approach, we identified fifteen homologs of E. coli β-ketoacyl-CoA thioesterase (FadM) and evaluated the in vivo activity of each against various chain length substrates. The FadM variant from Providencia sneebia produced the most 2-heptanone, 2-nonanone, and 2-undecanone, suggesting it has the highest activity on the corresponding β-ketoacyl-CoA substrates. We further tested enzyme variants, including acyl-CoA oxidases, thiolases, and bi-functional 3-hydroxyacyl-CoA dehydratases to maximize conversion of fatty acids to β-keto acyl-CoAs for 2-heptanone, 2-nonanone, and 2-undecanone production. In order to address the issue of product loss during fermentation, we applied a 20% (v/v) dodecane layer in the bioreactor and built an external water cooling condenser connecting to the bioreactor heat-transferring condenser coupling to the condenser. Finally, using these modifications, we were able to generate up to 4.4 g/L total medium-chain length methyl ketones.

2-Heptanone↗
DOE OSTI2025

Thermal Oxo-degradation and Catalytic Upgrading of Plastic Waste to Light Olefins for a Circular Economy

The commercialization of conventional pyrolysis of plastic in an inert atmosphere has been hindered by large thermal requirements stemming from long reaction rates. The rate of thermal depolymerization of waste plastics can be accelerated by the addition of oxygen in a process known as thermal oxo-degradation (TOD). This study offers the prospect of TOD to upcycle postconsumer waste rapidly and efficiently. Using moderate temperatures and small amounts of air in a fluidized bed reactor, we demonstrated that waste high-density polyethylene and polypropylene are rapidly deconstructed to condensable products. These condensable products were catalytically upgraded in a micropyrolysis reactor using commercially available zeolite (HZSM-5) to monomeric olefins. The olefin yields proved to be greater than those achieved through the catalytic upgrading of condensable products from (nonoxidative) the pyrolysis of the same plastic wastes. The coupling of TOD with catalytic upgrading proves to be an energy-efficient pathway in a plastics circular economy for the production of light olefins from wastes.

Enthalpy↗
DOE OSTI2022

Deciphering Photochemical Reaction Pathways of Aqueous Tetrachloroauric Acid by X-ray Transient Absorption Spectroscopy

Photolysis reaction pathways of [Au(III)Cl 4 ] - in aqueous solution have been investigated by time-resolved X-ray absorption spectroscopy. Ultraviolet excitation directly breaks the Au-Cl bond in [Au(III)Cl 4 ] - to form [Au(II)Cl 3 ] - that becomes highly reactive within 79 ps. Disproportionation of [Au(II)Cl 3 ] - generates [Au(I)Cl 2 ] - , which is stable for ≤ 10 mu s. In contrast, intense near-infrared lasers photolyze water to generate hydrated electrons, which then reduce [Au(III)Cl 4 ] - to [Au(II)Cl 3 ] - at 5 ns. Hydrated electrons further induce a chain reaction from [Au(II)Cl 3 ] - to [Au(0)Cl] - by successively removing one Cl - . The zero-valency Au anions quickly polymerize and condense to form Au nanoparticles, which become the dominating product after 400 s. Here our results reveal that the condensation of zero-valency Au starts with dimerization of gold clusters coordinated with chloride ions rather than direct condensation of pristine Au atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Single-Step Conversion of Ethanol to n-Butene over Ag-ZrO2/SiO2 Catalysts

Ethanol is a promising platform molecule for production of a variety of fuels and chemicals. Of particular interest is producing middle distillate fuels (i.e., jet and diesel blendstock) from renewable ethanol feedstock. State-of-the-art alcohol-to-jet technology requires multiple process steps based on catalytic dehydration of ethanol to form ethylene, followed by sometimes a multi-step oligomerization, and then hydrotreatment and distillation. Here we report on a new catalytic route in which ethanol is directly converted to n-butene (1- and 2-butene mixtures) over Ag-ZrO2/SBA-16, thus offering the potential for a reduction in the number of required processing steps versus conventional alcohol-to-jet technology. This catalyst system provides the balanced metal and Lewis acid sites required to selectively facilitate a cascading sequence of reactions that includes dehydrogenation, aldol condensation, Meerwein–Ponndorf–Verley reduction, dehydration, and hydrogenation. High conversion and selectivity toward either n-butene or 1,3-butadiene is achieved by tuning the hydrogen feed partial pressure and other process/catalyst parameters. With sufficient hydrogen partial pressure 1,3-butadiene is completely and selectively hydrogenated to form n-butene. The reaction mechanism was elucidated through operando-nuclear magnetic resonance investigations coupled with reactivity measurements. Combined experimental-computational investigation reveals how changes in silver and zirconium composition and the silver oxidation state affects reactivity under controlled hydrogen partial pressures and after prolonged run times. Finally, catalyst effectiveness also was demonstrated when using wet ethanol feed, thus highlighting process flexibility in terms of feedstock purity requirements. This work was financially supported by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office, and was performed at the Pacific Northwest National Laboratory (PNNL) under Contract No. DE-AC05-76RL01830 and the National Renewable Energy Laboratory under Contract No. DE-AC36- 08GO28308. Part of the work conducted by S. A. Akhade was performed under the auspices of the U.S. DOE at Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344. This work was partly supported through the PNNL-WSU Distinguished Graduate Research Program for ADW. NMR and XPS experiments were performed using EMSL (grid.436923.9), a DOE Office of Science User Facility sponsored by the Office of Biological and Environmental Research

Dagle, Vanessa↗
DOE OSTI2024

Mechanism and Kinetics of Ethanol–Acetaldehyde Conversion to 1,3-Butadiene over Isolated Lewis Acid La Sites in Silanol Nests in Dealuminated Beta Zeolite

Biomass-derived ethanol (EtOH) and acetaldehyde (AcH) conversion to 1,3-butadiene (1,3-BD) is an alternative process for 1,3-BD production. The present investigation reports the preparation and characterization of isolated La sites introduced into the silanol nests in DeAlBEA as well as detailed studies of the mechanism and kinetics for the conversion of an EtOH-AcH mixture to 1,3-BD. La sites supported on DeAlBEA are found to be present as (≡SiO) 2 La-OH groups that are H-bonded with adjacent Si-OH groups, possessing high C-C coupling activity and stability, superior to state-of-the-art Y-DeAlBEA. La sites supported on silica (La-SiO 2 ) with a similar chemical structure but no H-bonding interaction with Si-OH groups were prepared for comparison. Lewis acid La sites promote AcH aldol condensation, and the activity of such sites is nearly identical for both La-DeAlBEA and La-SiO 2 . Further, the rate of C 4 product formation increases by a factor of 4.8 upon addition of EtOH to the feed of AcH over La-DeAlBEA, whereas that over La/SiO 2 remains unchanged. Investigation of the mechanism and kinetics of AcH aldol condensation and EtOH-AcH conversion to 1,3-BD revealed two C-C bond forming pathways-AcH aldol condensation by Lewis acid La sites and direct coupling of EtOH-AcH over H-bonded (≡SiO) 2 La-OH···HO-Si≡ sites. This study provides important information about the role of the local environment of isolated Lewis acid sites and their effects on the direct coupling of EtOH and AcH to form 1,3-BD.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

A Pair of 2D Quantum Liquids: Investigating the Phase Behavior of Indirect Excitons

Long-lived indirect excitons (IXs) exhibit a rich phase diagram, including a Bose–Einstein condensate (BEC), a Wigner crystal, and other exotic phases. Recent experiments have hinted at a “classical” liquid of IXs above the BEC transition. To uncover the nature of this phase, we use a broad range of theoretical tools and find no evidence of a driving force toward classical condensation. Instead, we attribute the condensed phase to a quantum electron–hole liquid (EHL), first proposed by Keldysh for direct excitons. Taking into account the association of free carriers into bound excitons, we study the phase equilibrium between a gas of excitons, a gas of free carriers, and an EHL for a wide range of electron–hole separations, temperatures, densities, and mass ratios. Our results agree reasonably well with recent measurements of GaAs/AlGaAs coupled quantum wells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Aerosol Impacts on Mesoscale Convective Systems Forming Under Different Vertical Wind Shear Conditions

Following our previous study of wind shear effect on mesoscale convective system (MCS) organization under a clean atmospheric condition using the Weather Research and Forecasting model coupled with Spectral-Bin Microphysics, we conduct sensitivity simulations by increasing cloud condensation nuclei (CCN) concentration and investigate aerosol impacts on MCSs forming under different wind shear conditions. We find that, aerosols induce stronger updrafts and downdrafts in all MCSs. The stronger updrafts and enlarged convective core area contribute to larger vertical mass fluxes and enhance precipitation, indicating convective invigoration. Increased updraft speed below 8-km altitude mainly results from enhanced condensational heating, and increased water loading effect is not large enough to overcome the increase in thermal buoyancy. Interestingly, above 8-km altitude we see reduced updraft speed by the increased aerosols due to reduced vertical pressure perturbation gradient force, and weakened depositional growth due to competition of water vapor by enhanced condensation. The accumulated rainfall and mean rain rate are increased, with an increased occurrence frequency of heavy rain. The increase of rain rate is seen in both convective and stratiform regions, with a more significant increase in convective rain rate. In general, we see a higher frequency of deep convective cloud in the polluted condition because of invigorated convection, and more stratiform/anvil clouds, but a lower frequency of shallow warm clouds. The unanimously invigorated MCSs by aerosols under various wind shear conditions revealed by this study has an important implication in weather and climate at warm and humid regions that are influenced by pollution.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Stable Machine‐Learning Parameterization of Subgrid Processes in a Comprehensive Atmospheric Model Learned From Embedded Convection‐Permitting Simulations

Modern climate projections often suffer from inadequate spatial and temporal resolution due to computational limitations, resulting in inaccurate representations of sub-grid processes. A promising technique to address this is the multiscale modeling framework (MMF), which embeds a kilometer-resolution cloud-resolving model (CRM) within each atmospheric column of a host climate model to replace traditional convection and cloud parameterizations. Machine learning offers a unique opportunity to make MMF more accessible by emulating the embedded CRM and reducing its substantial computational cost. Although many studies have demonstrated proof-of-concept success of achieving stable hybrid simulations, it remains a challenge to achieve near operational-level success with real geography and comprehensive variable emulation that includes, for example, explicit cloud condensate coupling. In this study, we present a stable hybrid model capable of integrating for at least 5 years with near operational-level complexity, including coarse-grid geography, seasonality, explicit cloud condensate and wind predictions, and land coupling. Our model demonstrates skillful online performance, achieving a 5-year zonal mean tropospheric temperature bias within 2 K, water vapor bias within 1 g/kg, and a precipitation root mean square error of 0.96 mm/day. Key factors contributing to our online performance include an expressive U-Net architecture and physical thermodynamic constraints for microphysics. With microphysical constraints mitigating unrealistic cloud formation, our work is the first to demonstrate realistic multi-year cloud condensate climatology under the MMF framework. Despite these advances, online diagnostics reveal persistent biases in certain regions, highlighting the need for innovative strategies to further optimize online performance.

Hu, Zeyuan [NVIDIA Corporation, Santa Clara, CA (U↗
DOE OSTI2021

New particle formation in the remote marine boundary layer

Marine low clouds play an important role in the climate system, and their properties are sensitive to cloud condensation nuclei concentrations. While new particle formation represents a major source of cloud condensation nuclei globally, the prevailing view is that new particle formation rarely occurs in remote marine boundary layer over open oceans. Here we present evidence of the regular and frequent occurrence of new particle formation in the upper part of remote marine boundary layer following cold front passages. The new particle formation is facilitated by a combination of efficient removal of existing particles by precipitation, cold air temperatures, vertical transport of reactive gases from the ocean surface, and high actinic fluxes in a broken cloud field. The newly formed particles subsequently grow and contribute substantially to cloud condensation nuclei in the remote marine boundary layer and thereby impact marine low clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Significance of the organic aerosol driven climate feedback in the boreal area

Aerosol particles cool the climate by scattering solar radiation and by acting as cloud condensation nuclei. Higher temperatures resulting from increased greenhouse gas levels have been suggested to lead to increased biogenic secondary organic aerosol and cloud condensation nuclei concentrations creating a negative climate feedback mechanism. Here, we present direct observations on this feedback mechanism utilizing collocated long term aerosol chemical composition measurements and remote sensing observations on aerosol and cloud properties. Summer time organic aerosol loadings showed a clear increase with temperature, with simultaneous increase in cloud condensation nuclei concentration in a boreal forest environment. Remote sensing observations revealed a change in cloud properties with an increase in cloud reflectivity in concert with increasing organic aerosol loadings in the area. The results provide direct observational evidence on the significance of this negative climate feedback mechanism.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Non-equilibrium anti-Stokes Raman spectroscopy for investigating Higgs modes in superconductors

Abstract Even before its role in electroweak symmetry breaking, the Anderson-Higgs mechanism was introduced to explain the Meissner effect in superconductors. Spontaneous symmetry-breaking yields massless phase modes representing the low-energy excitations of the Mexican-Hat potential. Only in superconductors the phase mode is shifted towards higher energies owing to the gauge field of the charged condensate. This results in a low-energy excitation spectrum governed by the Higgs mode. Consequently, the Bardeen-Cooper-Schrieffer-like Meissner effect signifies a macroscopic quantum condensate in which a photon acquires mass, representing a one-to-one analogy to high-energy physics. We report on an innovative spectroscopic technique to study symmetries and energies of the Higgs modes in the high-temperature superconductor Bi 2 Sr 2 CaCu 2 O 8 after a soft quench of the Mexican-Hat potential. Population inversion induced by an initial laser pulse leads to an additional anti-Stokes Raman-scattering signal, which is consistent with polarization-dependent Higgs modes. Within Ginzburg-Landau theory, the Higgs-mode energy is connected to the Cooper-pair coherence length. Within a Bardeen-Cooper-Schrieffer weak-coupling model we develop a quantitative and coherent description of single-particle and two-particle channels. This opens the avenue for Higgs Spectroscopy in quantum condensates and provides a unique pathway to control and explore Higgs physics.

Science & Technology - Other Topics↗
DOE OSTI2025

Atomic-scale frustrated Josephson coupling and multicondensate visualization in FeSe

In a Josephson junction involving multiband superconductors, competition between interband and interjunction Josephson couplings gives rise to frustration and spatial disjunction of superfluid densities among superconducting condensates. Such frustrated coupling manifests as the quantum interference of Josephson currents from different tunnelling channels and becomes tunable if channel transparency can be varied. To explore these unconventional effects in the prototypical s ± -wave superconductor FeSe, we use atomic-resolution scanned Josephson tunnelling microscopy for condensate-resolved imaging and junction tuning—capabilities unattainable in macroscopic Josephson devices with fixed characteristics. We quantitatively demonstrate frustrated Josephson tunnelling by examining two tunnelling inequalities. The relative transparency of two parallel tunnelling pathways is found tunable, revealing a tendency towards a 0–π transition with decreasing scanned Josephson tunnelling microscopy junction resistance. Here, the simultaneous visualization of both superconducting condensates reveals anticorrelated superfluid modulations, highlighting the role of interband scattering. Our study establishes scanned Josephson tunnelling microscopy as a powerful tool enabling new research frontiers of multicondensate superconductivity.

Scanning probe microscopy↗
DOE OSTI2025

Topological excitonic insulator with tunable momentum order

Correlated topological materials often maintain a delicate balance among physical symmetries. Many topological orders are symmetry protected, whereas most correlated phenomena arise from spontaneous symmetry breaking. Cases where symmetry breaking induces a non-trivial topological phase are rare. Here we demonstrate the presence of two such phases in Ta 2 Pd 3 Te 5 , where Coulomb interactions form excitons that condense below 100 K, one with zero and the other with finite momentum. We observed a full spectral bulk gap, which stems from exciton condensation. This topological excitonic insulator state spontaneously breaks mirror symmetries but involves a weak structural coupling. Scanning tunnelling microscopy shows gapless boundary modes in the bulk insulating phase. Their magnetic field response, together with theoretical modelling, indicates a topological origin. These observations establish Ta 2 Pd 3 Te 5 as a topological excitonic insulator in a three-dimensional crystal. Finally, our results manifest a unique sequence of topological exciton condensations in a bulk crystal, offering exciting opportunities to study critical behaviour and excitations.

36 MATERIALS SCIENCE↗