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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 91 records · Page 5

Microwave-Assisted Reactive CO 2 Capture with the SrCO 3 -Graphite System

This study details the initial development of a microwave heat-driven reactive CO 2 capture (RCC) process using the SrO/SrCO 3 cycle and graphitic carbon to absorb ppm-levels of CO 2 from humidified room temperature air and selectively convert it into CO. By combining first-principles density functional theory (DFT) simulations with thermogravimetric analysis (TGA) and X-ray diffraction (XRD) verification, it is demonstrated that SrO spontaneously absorbs moisture to generate Sr(OH) 2 followed by Sr(OH) 2 *1H 2 O, which then can spontaneously react with atmospheric levels of CO 2 to form SrCO 3 . The resulting SrCO 3 can then react with solid carbon at elevated temperatures to selectively produce CO and regenerate SrO. Graphitic carbon is an excellent microwave absorber that can quickly generate temperatures approaching 1000 °C and then cool to room temperature within minutes, potentially allowing for integration with intermittent electricity. It is shown that using microwaves to selectively heat a mixture of graphitic carbon and SrCO 3 produced CO with 85 ± 3% selectivity and stable performance over ten cycles. The rapid heating for release and room temperature CO 2 uptake processes appeared to prevent performance loss from particle sintering typically observed with traditional thermal systems. In conclusion, these results demonstrate a new RCC approach that adds to the growing number of potential technologies available for converting CO 2 to useful chemicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Polymer nanoparticle photocatalysts realized in non-aqueous solvents

Colloidal organic nanoparticles (oNPs) have emerged as a promising category of photocatalyst, thanks to their long-lived surface-bound charges, electronic tunability, and strong absorption in the visible spectrum. Our previous research has established a direct correlation between charge generation in oNPs and their photocatalytic activity, highlighting their effectiveness as a framework for stable, long-lived free carriers. However, oNPs have been restricted to use only in aqueous environments as a result of being synthesized via either nano-emulsion or nano-precipitation procedures. Herein, we present a method for transferring oNP photocatalysts from water into polar non-aqueous solvents while retaining their long-term colloidal stability. We observed that the polymer chains in the solvent-transferred oNPs rearrange from a predominantly H-aggregate structure in water to a combination of H- and J-aggregate characteristics in N,N-dimethylformamide, suggesting a dynamic rearrangement in response to the new solvent environment. Importantly, transient absorption and time-resolved microwave conductivity measurements confirm that the solvent-transferred oNPs maintain their ability to generate free charges at an internal heterojunction. This development opens unique opportunities for eventually leveraging light-generated, long-lived electrons and holes in synthetic redox chemistry across diverse solvent environments, a direction that will be explored in future studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Microwave-assisted ammonia synthesis over Ru/MgO catalysts at ambient pressure

Here, in this work, a fixed frequency (2.45 GHz) microwave (MW) was used to synthesis ammonia over Ru/MgO catalysts under ambient atmospheric pressure at 320 °C. The loading of Ru catalyst over MgO was varied at 4% and 10 wt %. The metal support interaction was found to play an important role not only catalytically but also altering the microwave-catalyst interaction affecting the ammonia formation rate. The higher metal loading (10 wt%) produced the most activity, stability, and energy efficiency. It was found the Ru was better dispersed at higher loading which decreased the sintering of the catalyst due to lower microwave energy needed to maintain the reaction temperature. Additional effects from the microwave can include enhanced electron movement and/or electric fields formed between the metal sites of the catalyst. The microwave reactor offers a quick on/off catalyst recovery, within 11 min, compared to thermal convectional Haber Bosch (HB) technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solar Occultation Satellite Data and Derived Meteorological Products: Sampling Issues and Comparisons with Aura MLS

Derived Meteorological Products (DMPs, including potential temperature (theta), potential vorticity, equivalent latitude (EqL), horizontal winds and tropopause locations) have been produced for the locations and times of measurements by several solar occultation (SO) instruments and the Aura Microwave Limb Sounder (MLS). DMPs are calculated from several meteorological analyses for the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer, Stratospheric Aerosol and Gas Experiment II and III, Halogen Occultation Experiment, and Polar Ozone and Aerosol Measurement II and III SO instruments and MLS. Time-series comparisons of MLS version 1.5 and SO data using DMPs show good qualitative agreement in time evolution of O3, N2O, H20, CO, HNO3, HCl and temperature; quantitative agreement is good in most cases. EqL-coordinate comparisons of MLS version 2.2 and SO data show good quantitative agreement throughout the stratosphere for most of these species, with significant biases for a few species in localized regions. Comparisons in EqL coordinates of MLS and SO data, and of SO data with geographically coincident MLS data provide insight into where and how sampling effects are important in interpretation of the sparse SO data, thus assisting in fully utilizing the SO data in scientific studies and comparisons with other sparse datasets. The DMPs are valuable for scientific studies and to facilitate validation of non-coincident measurements.

Manney, Gloria↗

Microwave-assisted ammonia synthesis over Cs-Ru/CeO 2 catalyst at ambient pressure: Effects of metal loading and support particle size

Industrially, ammonia is produced by Haber-Bosch process under high temperatures and pressures, consuming more than >2% of the world's energy production. This paper presents microwave-assisted catalytic synthesis of ammonia operated at atmospheric pressure and temperatures from 260 to 360 °C. A Cs-promoted Ru catalyst supported on cerium oxide with different metal loading (4–24 wt% Ru) and support particle size (25nm, 50nm and 5μm) was investigated. The small size cerium oxide support resulted in the highest activity while the large cerium oxide support was less favorable, leading to lower activity associated to large Ru particle size and lower dispersion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultra-Wideband Microwave Imaging System for Root Phenotyping

The roots are a vital organ for plant growth and health. The opaque surrounding environment of the roots and the complicated growth process means that in situ and non-destructive root phenotyping face great challenges, which thus spur great research interests. The existing methods for root phenotyping are either unable to provide high-precision and high accuracy in situ detection, or they change the surrounding root environment and are destructive to root growth and health. Thus,we propose and develop an ultra-wideband microwave scanning method that uses time reversal to achieve in situ root phenotyping nondestructively. To verify the method’s feasibility, we studied an electromagnetic numerical model that simulates the transmission signal of two ultra-wideband microwave antennas. The simulated signal of roots with different shapes shows the proposed system’s capability to measure the root size in the soil. Experimental validations were conducted considering three sets of measurements with different sizes, numbers and locations, and the experimental results indicate that the developed imaging system was able to differentiate root sizes and numbers with high contrast. The reconstruction from both simulations and experimental measurements provided accurate size estimation of the carrots in the soil, which indicates the system’s potential for root imaging.

59 BASIC BIOLOGICAL SCIENCES↗

Quantifying Variability and Controls of Riverine Dissolved Organic Carbon Exported to Arctic Coastal Margins of North America (Final Report)

This project involved implementation and application of a coupled permafrost hydrology and dissolved organic carbon process models to investigate how spatial and seasonal variations in terrestrial hydrology and soil freeze/thaw dynamics influence the mobilization, loading, and export of organic carbon to the stream network for selected arctic basins across northern Alaska and northwest Canada. The model simulations were constrained by detailed observations of in- stream chemistry, soil active layer profile moisture and temperature dynamics, streamflow, soil carbon inventories and satellite microwave remote sensing based assessments of surface soil freeze-thaw dynamics. We developed and applied the numerical modeling and data analysis, incorporating observed data for calibration and validation, in order to investigate the terrestrial hydrology, permafrost dynamics, and associated DOC production and loading to rivers across a region encompassing watersheds draining to the coast. The project produced six publications and three datasets archived in public repositories.

54 ENVIRONMENTAL SCIENCES↗

Examples of X-Ray Characterization Techniques in Energy Storage Research

Lithium-ion batteries have revolutionized the portable electronics and transportation sectors. Their performance is often critically dependent on the crystal structures of the anode and cathode electrode materials, which must enable the transport and reversible storage of lithium ions into and out of the lattice. Because lithium is a low-Z element, characterization of materials for lithium-ion batteries can be particularly challenging. Regardless, X-ray techniques enable analysis of material structures to better understand how battery materials perform and degrade, particularly when combined with other materials characterization and electrochemical characterization techniques. While X-ray techniques are most often used in battery research for phase identification of crystal structures, X-ray characterization techniques are also used for a wide variety of other purposes. I will discuss several examples from my research with various collaborators on several projects that highlight the impact that X-ray characterization techniques can have on battery research. The first example will focus on low-temperature microwave-assisted solvothermal synthesis of vanadium-doped LiFePO4 cathode materials for lithium-ion batteries. (1,2) Through a combination of electrochemical and materials characterization, we determined that low temperature synthesis resulted in metastable phases that enabled incorporation of higher dopant levels than resulting from high-temperature synthesis of thermodynamically stable phases. Rietveld refinement of X-ray diffraction data enabled understanding of how lattice parameters changed with doping levels and synthesis temperature. X-ray absorption near edge spectroscopy enabled understanding of the vanadium and iron oxidation states to confirm how vacancies in the structure caused by doping were charge compensated. This was important to understand because the literature suggests doping can improve LiFePO4 electrical conductivity, which improves battery charge and discharge rates. The second example will focus on understanding residual strain in lithium metal anodes. Lithium-ion batteries typically use graphite anodes, but the charge-storage capacity can be theoretically improved ~10x by using lithium metal as the anode material instead. However, lithium anodes suffer from growth of high-aspect-ratio features, such as dendrites, that can pierce nanoporous polymer separators and lead to short circuits and fires. External pressure is commonly applied to cells to enable better morphological control. We hypothesized that applied pressure may promote strain and possibly work hardening during electrochemical cycling, which motivated us to look for evidence of residual strain in lithium metal cycled under applied pressure using X-ray diffraction and sin2(..psi..) analysis. We found that lithium electrodeposited under high pressure exhibited in-plane compressive strain and that that lithium electrodeposited under low pressure did not. (3) The residual strain that accompanies electrodeposition under high pressure may lead to work hardening, which may explain how a soft metal like lithium can puncture separators and why higher pressure does not always decrease short circuits. (4-6) References: 1) Harrison, K. L.; Manthiram, A. Microwave-Assisted Solvothermal Synthesis and Characterization of Metastable LiFe1- x (VO) x PO4 Cathodes. Inorganic chemistry 2011, 50(8), 3613-3620. 2) Harrison, K. L.; Bridges, C. A.; Paranthaman, M. P.; Segre, C. U.; Katsoudas, J.; Maroni, V. A.; Idrobo, J. C.; Goodenough, J. B.; Manthiram, A. Temperature Dependence of Aliovalent-Vanadium Doping in LiFePO4 Cathodes. Chemistry of Materials 2013, 25(5), 768-781. 3) Rodriguez, M. A.; Harrison, K. L.; Goriparti, S.; Griego, J. J.; Boyce, B. L.; Perdue, B. R. Use of a Be-Dome Holder for Texture and Strain Characterization of Li Metal Thin Films via Sin2 (..psi..) Methodology. Powder Diffraction 2020, 35(2), 89-97. 4) Jungjohann, K. L.; Gannon, R. N.; Goriparti, S.; Randolph, S. J.; Merrill, L. C.; Johnson, D. C.; Zavadil, K. R.; Harris, S. J.; Harrison, K. L. Cryogenic Laser Ablation Reveals Short-Circuit Mechanism in Lithium Metal Batteries. ACS Energy Letters 2021, 6(6), 2138-2144. 5) Harrison, K. L.; Merrill, L. C.; Long, D. M.; Randolph, S. J.; Goriparti, S.; Christian, J.; Warren, B.; Roberts, S. A.; Harris, S. J.; Perry, D. L. Cryogenic Electron Microscopy Reveals That Applied Pressure Promotes Short Circuits in Li Batteries. Iscience 2021, 24(12). 6) Harrison, K. L.; Goriparti, S.; Merrill, L. C.; Long, D. M.; Warren, B.; Roberts, S. A.; Perdue, B. R.; Casias, Z.; Cuillier, P.; Boyce, B. L. Effects of Applied Interfacial Pressure on Li-Metal Cycling Performance and Morphology in 4 M LiFSI in DME. ACS Applied Materials & Interfaces 2021, 13(27), 31668-31679.

batteries↗

Influence of Annealing Temperature on the OER Activity of NiO(111) Nanosheets Prepared via Microwave and Solvothermal Synthesis Approaches

Earth-abundant transition metal oxides are promising alternatives to precious metal oxides as electrocatalysts for the oxygen evolution reaction (OER) and are intensively investigated for alkaline water electrolysis. OER electrocatalysis, like most other catalytic reactions, is surface-initiated, and the catalyst performance is fundamentally determined by the surface properties. Most transition metal oxide catalysts show OER activities that depend on the predominantly exposed crystal facets/surface structure. Therefore, the design of synthetic strategies to obtain the most active crystal facets is of significant research interest. In this work, rock salt NiO OER catalysts with (111) predominantly exposed facets were synthesized by a solvothermal (ST) method either heated under supercritical or microwave-assisted (MW) conditions. Particular emphasis was placed on the influence of the post annealing temperature on the structural configuration and OER activity to compare their catalytic performances. The as-prepared electrocatalysts are pure α-Ni hydroxides which were converted to rock salt NiO (111) nanosheets with hexagonal pores after heat treatment at different temperatures. The OER activity of the electrodes has been evaluated in 0.1 M KOH using geometric and intrinsic current densities via normalization by the disk area and BET area, respectively. The lowest overpotential at a geometric current density of 10 mA/cm 2 is found for samples pretreated by heating between 400 and 500 °C with a catalyst loading of 115 μg/cm 2 . Despite the very similar nature of the catalysts obtained from the two methods, the ST electrodes show a higher geometric and intrinsic current density for 500 °C pretreatment. The MW electrodes, however, achieve an optimal geometric current density for 400 °C pretreatment, while their intrinsic current density requires pretreatment over 600 °C. Interestingly, pretreated electrodes show consistently higher OER activity as compared to the poorly crystalline/less ordered hydroxide as-prepared electrocatalysts. Thus, our study highlights the importance of the synthesis method and pretreatment at an optimal temperature.

36 MATERIALS SCIENCE↗

Spaceborne SAR sensor architecture

Spaceborne imaging radars for the decade of the '90s will be called upon to provide increased illumination parameter flexibility, polar orbital coverage, and to operate from the same platform with other advanced sensors such as multilinear arrays. The potential information content in accurately merged microwave infrared, or microwave visible images is enormous by comparison to either radar images alone or visible/infrared images alone, since microwave images are principally responsive to surface geometry whereas visible/infrared images are highly sensitive to surface chemistry. A strawman system concept in which a SAR and multilinear array (MLA) are flown on a polar orbiting free flyer at 800 km altitude is discussed. Data would be relayed to ground via the TDRSS (or equivalent).

Carver, K. R.↗

The Aura Mission and the "A-Train"

By the end of 2004 the A-Train will have been assembled in orbit. The A-Train consists of five low earth orbit satellites flying within 15 minutes of each other. The first in the train is Aqua, launched early this year, in an ascending node orbit with 1 :30 PM crossing time. In January 2004, Aura will be launched, following 15 minutes behind Aqua. Aura's focus is atmospheric chemistry, with both forward looking, and backward looking instruments along with nadir sounders. Aura's limb microwave instrument will also be able to make temperature and humidity measurements into the troposphere. By mid-2004, CALIPSO, a cloud lidar mission and CloudSat, a cloud radar mission will be co-manifested. These two spacecraft will follow, and maneuver about 1 minute behind Aqua. The lidar on CALIPSO will provide aerosol and cloud height information which can enhance the aerosol information from Aqua s MODIS instrument. CloudSat s radar will enhance the information from AMSR-E, AIRS and HSB on Aqua. The fifth satellite to be launched in 2004 is PARASOL which will use the POLDER instrument to provide polarization information which can be used to determine aerosol composition and size distribution.

Schoeberl, Mark R.↗

NASA Perspectives on Earth Observations from Satellite or 50 Years of Meteorological Satellite Experiments-The NASA Perspective

The NASA was established in 1959. From those very eady days to the present NASA has been intimately involved with NOAA and the scientific community in the development and operation of satellite and sensor experiments. The early efforts included experiments on the TIROS and geostationary Applications Technology Satellites (ATS) series. In the latter case the spin-scan cameras conceived by Verner Suomi, along with the TIROS cameras, opened new vistas at what could be done in meteorological studies with the daily, nearly global, synoptic views from space-borne sensors As the years passed and the Nimbus series of satellites came into being in the 1960's, more quantitative observations with longer-lifetime, increasingly capable, better calibrated instruments came into being. NASA, in collaboration with and in support of NOAA, implemented operational systems that we now know as the Polar Operational Environmental Satellite (POES) series and the Geostationary Operational Environmental Satellite (GOES) series that provided dependable, continuous, dedicated satellite observations for use by the weather and atmospheric science communities. Through the 1970's, 1980's, and 1990's improved, well-calibrated instruments with more spectral bands extending into the thermal and the microwave portions of the electromagnetic spectrum were provided to obtain accurate soundings of the atmosphere, atmospheric chemistry constituents such as ozone, global sea surface temperature, snow and ice extent, vegetation dynamics, etc. In the 1990's and up to the present the NASA/Earth Observing System (EOS) has been developed, implemented, and operated over many years to provide a very comprehensive suite of observations of the atmosphere, as well as land and ocean parameters. The future looks bright wherein the development of new systems, broadly described by the National Academy of Science Decadal Study, is now underway. NASA, along with collaborations with NOAA, other agencies, and the scientific and applications communities looks forward to achieving in the years to come goals possible with the global information provided by satellites and continuously improved with technology development, joint data assimilation efforts, and attendant research studies.

Einaudi, Franco↗

Hemispheric Differences in Tropical Lower Stratospheric Transport and Tracers Annual Cycle

Transport of long-lived tracers (such as O, CO, and N O) in the lower stratosphere largely determines the composition of the entire stratosphere. Stratospheric transport includes the mean residual circulation (with air rising in the tropics and sinking in the polar and middle latitudes), plus two-way isentropic (quasi-horizontal) mixing by eddies. However, the relative importance of two transport components remains uncertain. Previous studies quantified the relative role of these processes based on tropics-wide average characteristics under common assumption of well-mixed tropics. However, multiple instruments provide us with evidence that show significant differences in the seasonal cycle of ozone between the Northern (0-20N) and Southern (0-20S) tropical (NT and ST respectively) lower stratosphere. In this study we investigate these differences in tracer seasonality and quantify transport processes affecting tracers annual cycle amplitude using simulations from Goddard Earth Observing System Chemistry Climate Model (GEOSCCM) and Whole Atmosphere Community Climate Model (WACCM) and compare them to observations from the Microwave Limb Sounder (MLS) on the Aura satellite. We detect the observed contrast between the ST and NT in GEOSCCM and WACCM: annual cycle in ozone and other chemical tracers is larger in the NT than in the ST but opposite is true for the annual cycle in vertical advection. Ozone budgets in the models, analyzed based on the Transformed Eulerian Mean (TEM) framework, demonstrate a major role of quasi-horizontal mixing vertical advection in determining the NTST ozone distribution and behavior. Analysis of zonal variations in the NT and ST ozone annual cycles further suggests important role of North American and Asian Summer Monsoons (associated with strong isentropic mixing) on the lower stratospheric ozone in the NT. Furthermore, multi model comparison shows that most CCMs reproduce the observed characteristic of ozone annual cycle quite well. Thus, latitudinal variations within the tropics have to be considered in order to understand the balance between upwelling and quasi- horizontal mixing in the tropical lower stratosphere and the paradigm of well mixed tropics has to be reconsidered.

Chemistry-Climate Models↗

A Model and Satellite-Based Analysis of the Tropospheric Ozone Distribution in Clear Versus Convectively Cloudy Conditions

Satellite observations of in-cloud ozone concentrations from the Ozone Monitoring Instrument and Microwave Limb Sounder instruments show substantial differences from background ozone concentrations. We develop a method for comparing a free-running chemistry-climate model (CCM) to in-cloud and background ozone observations using a simple criterion based on cloud fraction to separate cloudy and clear-sky days. We demonstrate that the CCM simulates key features of the in-cloud versus background ozone differences and of the geographic distribution of in-cloud ozone. Since the agreement is not dependent on matching the meteorological conditions of a specific day, this is a promising method for diagnosing how accurately CCMs represent the relationships between ozone and clouds, including the lower ozone concentrations shown by in-cloud satellite observations. Since clouds are associated with convection as well as changes in chemistry, we diagnose the tendency of tropical ozone at 400 hPa due to chemistry, convection and turbulence, and large-scale dynamics. While convection acts to reduce ozone concentrations at 400 hPa throughout much of the tropics, it has the opposite effect over highly polluted regions of South and East Asia.

Ozone Monitoring and Microwave Limb Sounder instru↗

Indirect observation of unobservable interstellar molecules

It is suggested that the abundances of neutral non-polar interstellar molecules unobservable by radio astronomy can be systematically determined by radio observation of the protonated ions. As an example, observed N2H(+) column densities are analyzed to infer molecular nitrogen abundances in dense interstellar clouds. The chemistries and expected densities of the protonated ions of O2, C2, CO2, C2H2 and CH4 are then discussed. Microwave transition frequencies fo HCO2(+) and C2H3(+) are estimated, and a preliminary astronomical search for HCO2(+) is described.

Herbst, E.↗