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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

REDOTHERM: a thermodynamic modeling framework for redox-based thermochemical processes

Two-step thermochemical redox cycles are being developed as a potential pathway for the production of hydrogen and syngas. While there are many possible reactor and system configurations, moving oxide systems are considered promising in terms of the redox thermodynamics, due to the potential implementation of a countercurrent system that can achieve higher performance compared to other configurations. There is a lack of a robust thermodynamic modeling framework in the field, with multiple models incorporating incorrect thermodynamic assumptions that violate the second law of thermodynamics. We present in this work REDOTHERM, an open-source system model for moving oxides that incorporates the correct thermodynamic limits, as well as various options for the system auxiliary units including product separation, heat recovery, and oxygen removal. The model is agnostic to the energy source, and could be used for solar thermal or other configurations. We highlight the uses of this model, presenting some of the tradeoffs and challenges in redox-active material selection and how they affect the entire thermochemical hydrogen production process. This model could be easily adapted and used for material exploration, system/reactor design, and technoeconomic analysis.

08 HYDROGEN↗
DOE OSTI2026

Integrated Hydrogen Energy System Testing/Validation: Cooperative Research and Development Final Report, CRADA Number CRD-21-18272

Through the ARIES platform, this proposed project aims to bridge a gap and utilize the power hardware-in-the-loop (PHIL) and controller hardware-in-the-loop (CHIL) experiments and create open-source interconnection and interoperability information that can aid in faster and cheaper installation and operation of grid forming fuel cell inverters.

08 HYDROGEN↗
NASA NTRS2000

The Precambrian Biogeochemical Carbon Isotopic Record: Contributions of Thermal Versus Biological Processes

Superplumes offer a new approach for understanding global C cycles. Isotopes help to discern the impacts of geological, environmental and biological processes ujpun the evolution of these cycles. For example, C-13/C-12 values of coeval sedimentary organics and carbonates give global estimates of the fraction of C buried as organics (Forg), which today lies near 0.2. Before Oxygenic photosynthesis arose, our biosphere obtained reducing power for biosynthesis solely from thermal volatiles and rock alteration. Thus Forg was dominated by the mantle redox state, which has remained remarkably constant for greater than Gy. Recent data confirm that the long-term change in Forg had been small, indicating that the mantle redox buffer remains important even today. Oxygenic photosynthesis enabled life to obtain additional reducing power by splitting the water molecule. Accordingly, biological organic production rose above the level constrained by the mantle-derived flux of reduced species. For example, today, chemoautotrophs harvesting energy from hydrothermal emanations can synthesize at most between 0.2 x 10(exp 12) and 2x 10(exp 12) mol C yr-1 of organic C globally. In contrast, global photosynthetic productivity is estimated at 9000 x 10(exp 12) mol C yr-1. Occasionally photosynthetic productivity did contribute to dramatically -elevated Forg values (to 0.4 or more) as evidenced by very high carbonate C-13/C-12. The interplay between biological, tectonic and other environmental factors is illustrated by the mid-Archean to mid-Proterozoic isotopic record. The relatively constant C-13/C-12 values of Archean carbonates support the view that photosynthetically-driven Forg increases were not yet possible. In contrast, major excursions in C-13/C-12, and thus also in Forg, during the early Proterozoic confirmed the global importance of oxygenic photosynthesis by that time. Remarkably, the superplume event at 1.9 Ga did not trigger another major Forg increase, despite the favorable conditions for organic burial that were evidenced by elevated sea levels and higher black shale abundances. Perhaps those superplume-rated processes that favored enhanced organic burial were offset by the ability of mantle-derived redox buffering, which was enhanced during the superplume event, to limit excursions in Forg.

DesMarais, David J.↗
NASA NTRS1990

Precipitable water estimation from high-resolution split window radiance measurements

A technique that uses the spatial variance of image brightness temperature to derive total column precipitable water is applied to high-resolution multispectral aircraft scanner data for the June 19, 1986 COHMEX day. The technique has several advantages over other approaches in that it requires only relative calibration accuracy, is less susceptible to instrument error, and does not directly use a priori information. Results indicate significant horizontal variability of precipitable water at the mesoscale. Precipitable water gradients of 6 mm per 10 km are not uncommon. The results verify well against special rawinsonde measurements and the ensuing cloud field development. While only applied to this specialized aircraft data, the applicability of the technique to operational AVHRR and VAS data is discussed.

Jedlovec, Gary J.↗
NASA NTRS1983

Low-level water vapor fields from the VAS split-window channels at 11 and 12 microns

Originally, the VAS split window channels were designed to use the differential water vapor absorption between 11 and 12 microns to estimate sea surface temperature by correcting for the radiometric losses caused by atmospheric moisture. It is shown that it is possible to reverse the procedure in order to estimate the vertically integrated low level moisture content with the background surface (skin) temperature removed, even over the bright, complex background of the land. Because the lower troposphere's water vapor content is an important factor in convective instability, the derived fields are of considerable value to mesoscale meteorology. Moisture patterns are available as quantitative fields (centimeters of precipitable water) at full VAS resolution (as fine as 7 kilometers horizontal resolution every 15 minutes), and are readily converted to image format for false color movies. The technique, demonstrated with GOES-5, uses a sequence of split window radiances taken once every 3 hours from dawn to dusk over the Eastern and Central United States. The algorithm is calibrated with the morning radiosonde sites embedded within the first VAS radiance field; then, entire moisture fields are calculated at all five observation times. Cloud contamination is removed by rejecting any pixel having a radiance less than the atmospheric brightness determined at the radiosonde sites.

Chesters, D.↗
NASA NTRS2002

Hydrogen Concentrations on C-class Asteroids from Remote Sensing

We present spectroscopic observations of 16 asteroids from 1.9-3.6 microns, collected from the United Kingdom Infrared Telescope (UKIRT) from 1996-2000. Of these 16 asteroids, 11 show some evidence of a 3-micron hydrated mineral absorption feature greater than 2 sigma at 2.9 microns. Using relations first recognized for carbonaceous chondrite powders by Miyamoto and Zolensky (1994) and Sato et al. (1997), we have determined the hydrogen/silicon ratio for these asteroids and calculated their equivalent water contents, assuming all the hydrogen was in water. The asteroids split into two groups, roughly defined as equivalent water contents of greater than approx. 7% (eight asteroids) and less than approx. 3 % (the remaining eight asteroids). This latter group includes some asteroids for which there is a small but statistically significant 3-micron band of non-zero depth. The G-class asteroids in the survey have higher water contents, consistent with CM chondrites. This strengthens the connection between CM chondrites and G asteroids that was proposed by Burbine (1998). We find that the 0.7-micron and 3-micron band depths are correlated for the population of target objects.

Rivkin, A. S.↗
NASA NTRS2003

Hydrogen Concentrations on C-Class Asteroids Derived from Remote Sensing

We present spectroscopic observations of 16 asteroids from 1.9-3.6 microns collected from the United Kingdom Infrared Telescope (UKIRT) from 1996-2000. Of these 16 asteroids, 11 show some evidence of a 3 microns hydrated mineral absorption feature greater than 2(sigma) at 2.9 microns. Using relations first recognized for carbonaceous chondrite powders by Miyamoto and Zolensky and Sato et al., we have determined the hydrogen to silicon ratio for these asteroids and calculated their equivalent water contents, assuming all the hydrogen was in water. The asteroids split into 2 groups, roughly defined as equivalent water contents approx. greater than 7% (8 asteroids, all with 3 microns band depths approx. greater than 20%) and approx. greater than 3% for the remaining 8 asteroids. This latter group includes some asteroids for which a weak but statistically significant 3 microns band of non-zero depth exists. The G-class asteroids in the survey have higher water contents, consistent with CM chondrites. This strengthens the connection between CM chondrites and G asteroids that was proposed by Burbine. We find that the 0.7 microns and 3 microns band depths are correlated for the population of target objects.

Rivkin, A. S.↗
NASA NTRS2003

Hydrogen Concentrations on C-class Asteroids Derived from Remote Sensing

We present spectroscopic observations of 16 asteroids from 1.9-3.6 microns collected from the United Kingdom Infrared Telescope (UKIRT) from 1996-2000. Of these 16 asteroids, 11 show some evidence of a 3 micron hydrated mineral absorption feature greater than 2 sigma at 2.9 microns. Using relations first recognized for carbonaceous chondrite powders by Miyamoto and Zolensky (1994) and Sato et al. (1997), we have determined the hydrogen to silicon ratio for these asteroids and calculated their equivalent water contents, assuming all the hydrogen was in water. The asteroids split into 2 groups, roughly defined as equivalent water contents greater than approximately 7% (8 asteroids, all with 3 micron band depths greater than approximately 20%) and less than approximately 3% for the remaining 8 asteroids. This latter group includes some asteroids for which a weak but statistically significant 3 micron band of non-zero depth exists. The G-class asteroids in the survey have higher water contents, consistent with CM chondrites. This strengthens the connection between CM chondrites and G asteroids that was proposed by Burbine (1998). We find that the 0.7 micron and 3 micron band depths are correlated for the population of target objects.

Rivkin, A. S.↗
NASA NTRS1983

Low-level water vapor fields from the VISSR Atmospheric Sounder (VAS) 'split window' channels

A simple physical algorithm is presented which calculates the water vapor content of the lower troposphere from the 11 and 12 micron (split window) channels on the VISSR Atmospheric Sounder (VAS) on the Geostationary Operational Environmental Satellites. The algorithm is used to analyze a time series of VAS split window radiances observed at 15 km horizontal resolution over eastern North America during a 12 hr period on 13 July 1981. Results of the color coded images of the derived precipitable water fields are found to show vivid water vapor features whose broad structure and evolution are verified by the radiosonde and surface networks. The satellite moisture fields also show significant mesoscale features and rapid developments which are not resolved by the conventional networks. The VAS split window is determined to clearly differentiate those areas in which water vapor extends over a deep layer and is more able to support convective cells from those areas in which water vapor is confined to a shallow layer and is therefore less able to support convection. It is concluded that the VAS split windows can be used operationally to monitor mesoscale developments in the low-level moisture fields over relatively cloud-free areas of the United States.

Chesters, D.↗
NASA NTRS2017

Regenerative Gas Dryer for In-Situ Propellant Production

Rocket propellant can be produced anywhere that water is found by splitting it into hydrogen and oxygen, potentially saving several tons of mass per mission and enabling the long term presence of humans in space beyond LEO. When water is split into hydrogen and oxygen, the gaseous products can be very humid (several thousand ppm). Propellant-grade gases need to be extremely dry before being converted into cryogenic liquids (less than 26 ppm water for grade B Oxygen). The primary objective of this project is to design, build and test a regenerative gas drying system that can take humid gas from a water electrolysis system and provide dry gas (less than 26ppm water) to the inlet of a liquefaction system for long durations. State of the art work in this area attempted to use vacuum as a means to regenerate desiccant, but it was observed that water would migrate to the dry zone without a sweep gas present to direct the desorbed vapor. Further work attempted to use CO2 as a sweep gas, but this resulted in a corrosive carbonic acid. In order for in-situ propellant production to work, we need a way to continuously dry humid gas that addresses these issues.

Paz, Aaron↗
NASA NTRS1982

Low-level water vapor fields from the VISSR atmospheric sounder (VAS) split window channels at 11 and 12 microns

A series of high-resolution water vapor fields were derived from the 11 and 12 micron channels of the VISSR Atmospheric Sounder (VAS) on GOES-5. The low-level tropospheric moisture content was separated from the surface and atmospheric radiances by using the differential adsorption across the 'split window' along with the average air temperature from imbedded radiosondes. Fields of precipitable water are presented in a time sequence of five false color images taken over the United States at 3-hour intervals. Vivid subsynoptic and mesoscale patterns evolve at 15 km horizontal resolution over the 12-hour observing period. Convective cloud formations develop from several areas of enhanced low-level water vapor, especially where the vertical water vapor gradient relatively strong. Independent verification at radiosonde sites indicates fairly good absolute accuracy, and the spatial and temporal continuity of the water vapor features indicates very good relative accuracy. Residual errors are dominated by radiometer noise and unresolved clouds.

Chesters, D.↗
NASA NTRS1983

Low level water vapor fields from the VISSR Atmospheric Sounder (VAS) 'split window' channels

The use of the 11 and 12-micron IR-radiometer channels of the VISSR Atmosphere Sounder (VAS) on the GOES to detect water vapor in the lowest 300-400 mb of the troposphere is reported. An algorithm is developed to eliminate the background temperature, allowing the calculation of precipitable water (PW) over both land and water via a single-layer radiative model. This 'split-window' method is demonstrated in a case study, covering the US on July 13, 1981. PW values were calculated from five VAS images and compared with those from radiosonde data and surface measurements. It is shown that the VAS PW images have good resolution (15 km), reveal vivid, continuously evolving details, and differentiate deep, convection-supporting layers from shallow ones. PW ranged from 1.7 to 5.5 g/sq cm (+ or - 1.0 g/sq cm), in good agreement with other measurements. Since this method can detect mesoscale water-vapor fields in relatively clear air, it is considered of great potential value for numerical forecasting.

Robinson, W. D.↗
DOE OSTI2025

Approaches for Water Removal in Direct-Fired sCO 2 Power Cycles

There is interest in investigation of water removal processes in direct fired sCO 2 flows, as this may potentially lead to greater system efficiency as the removal of this contaminant will result in sCO 2 behaving close to idealized behaviors. Water removal should be split into a two-step process, condensation of the water, followed by separation of the liquid phase water from the sCO 2 . The two main avenues of condensation are manipulation of pressure and temperature for phase change. For this paper, temperature-based phase change is the primary focus through the implementation of heat exchangers. Of the heat exchangers investigated it was found that printed circuit heat exchangers (PCHEs) could be an alternative for this use case, though the specific design of flow channel geometry and flow direction depends on the specific system case and cannot be determined at this point. For water separation there were four processes identified, all of which already assume water is in liquid phase at that point in the system. Of these separation avenues the best candidate is the hydrocyclone as it has a proven history of separating liquid-liquid phase mixtures with small density differences in oilfield use, in addition they have been investigated and modeled specifically for water separation for sCO 2 flows and the footprint is relatively small.

20 FOSSIL-FUELED POWER PLANTS↗
NASA NTRS2005

Evidence for Liquid Water on Comets

We have reexamined the arguments for the existence of liquid water on comets, and believe that recent cometary flybys along with pre-Giotto data support its presence on short-period comets. Liquid water would affect cometary dynamics, leaving distinct signatures in precession, orbital dynamics, and potential splitting of comets. Liquid water geysers would affect cometary atmosphere, dust evolution, and non-gravitational forces that perturb the orbit. Liquid water would affect the composition of both the interior and exterior of the comet, producing geologic effects consistent with recent flyby photographs. And most importantly, liquid water suppork the growth of lifeforms, which would make a comet a biofriendly incubator for interplanetary transport. The major objection against liquid water is the necessity of a pressure vessel to prevent sublimation into space. We discuss how such a pressure vessel could naturally evolve as a pristine comet makes its first journey inside the orbit of Mars, and suggest that this type of vessel was observed by Giotto, Deep Space I, and Stardust.

Sheldon, Robert↗
NASA NTRS1996

A technique for determining cloud free vs cloud contaminated pixels in satellite imagery

Since the first earth orbiting satellite sent pictures of the earth back to them, atmospheric scientists have been focused on the possibilities of using that information as both a forecasting tool and as a meteorological research tool. With the latest generation of Geostationary Operational Environmental Satellites (GOES) now entering service, that view of the earth yields views at a frequency and resolution never before available. These satellites have imagers with a five band multi-spectral capability with high spatial resolution. In addition, the sounder has eighteen thermal infrared (IR) channels plus one low-resolution visible band. With a resolution as small as one kilometer, GOES provides scientists with a powerful eye on the atmosphere. Menzel and Purdom (1994) detail both the imager and sounder capability as well as other systems on the GOES satellites. Immediately apparent in the visible channel are the patterns of clouds swirling over both oceans and continents. These clouds range in size from huge planetary systems covering thousands of kilometers to puffy fair weather cumulus clouds on the order of half a kilometer in size. With the IR sensors temperature patterns are observed. High clouds appear very cold, while low stratus field show temperatures near that of the surface. The surface, in turn, generally appears warmer than the clouds. It would seem then a simple manner to determine cloud and surface temperature from the imagery, but such is not the case. While most of the atmospheric constituents are well mixed and homogeneous, water vapor is not. The water molecule, because of its unique structure and vibration modes, affects the transmittance of the atmosphere most notably in the infrared regions. There are regions of the IR spectrum where water vapor acts as a strong absorber, and at others it is nearly transparent. The transparent wavelengths are called windows, and one such window occurs at 11.2 microns. Adjacent to this window at 12.7 microns which is strongly absorbed by water vapor. These two wavelengths form what is known as a split window, the utility of which was used. Using the linearized form of the radiative transfer equation, they were able to use the split window to determine the amount of water vapor present in the atmosphere. Jedlovec developed the physical split-window (PSW) technique which determines the integrated water content (IWC). The PSW method using Visible Infrared Spin Scan Radiometer (VISSR) Atmospheric Sounder (VAS) found on the older versions of the GOES satellites was used. Recently, Jedlovec and colleagues have been attempting to apply the PSW method using full disk IR imagery obtained by the new generation of GOES satellites. IWC is essential for improved analysis and prediction of convective storms which have been observed to develop in regions of both strong and rapidly evolving moisture gradients. It has also been used in the prediction of clouds and precipitation.

Wohlman, Richard A.↗
DOE OSTI2025

Perovskite-driven solar C 2 hydrocarbon synthesis from CO 2

Photoelectrochemistry (PEC) presents a direct pathway to solar fuel synthesis by integrating light absorption and catalysis into compact electrodes. Yet, PEC hydrocarbon production remains elusive due to high catalytic overpotentials and insufficient semiconductor photovoltage. Here we demonstrate ethane and ethylene synthesis by interfacing lead halide perovskite photoabsorbers with suitable copper nanoflower electrocatalysts. The resulting perovskite photocathodes attain a 9.8% Faradaic yield towards C 2 hydrocarbon production at 0 V against the reversible hydrogen electrode. The catalyst and perovskite geometric surface areas strongly influence C 2 photocathode selectivity, which indicates a role of local current density in product distribution. The thermodynamic limitations of water oxidation are overcome by coupling the photocathodes to Si nanowire photoanodes for glycerol oxidation. These unassisted perovskite–silicon PEC devices attain partial C 2 hydrocarbon photocurrent densities of 155 µA cm -2 , 200-fold higher than conventional perovskite–BiVO 4 artificial leaves for water and CO 2 splitting. These insights establish perovskite semiconductors as a versatile platform towards PEC multicarbon synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2014

Recent Advances in Water Analysis with Gas Chromatograph Mass Spectrometers

We report on progress made in developing a water sampling system for detection and analysis of volatile organic compounds in water with a gas chromatograph mass spectrometer (GCMS). Two approaches are described herein. The first approach uses a custom water pre-concentrator for performing trap and purge of VOCs from water. The second approach uses a custom micro-volume, split-splitless injector that is compatible with air and water. These water sampling systems will enable a single GC-based instrument to analyze air and water samples for VOC content. As reduced mass, volume, and power is crucial for long-duration, manned space-exploration, these water sampling systems will demonstrate the ability of a GCMS to monitor both air and water quality of the astronaut environment, thereby reducing the amount of required instrumentation for long duration habitation. Laboratory prototypes of these water sampling systems have been constructed and tested with a quadrupole ion trap mass spectrometer as well as a thermal conductivity detector. Presented herein are details of these water sampling system with preliminary test results.

quadrupole ion trap↗
NASA NTRSDate not supplied

Soluble Organic Matter (SOM) analysis of the Hayabusa2 samples: The first results

The Hayabusa2 spacecraft successfully collected the surface and possible sub-surface materials of the asteroid 162173 Ryugu. Ryugu is a C-type asteroid characterized by a low-albedo surface probably consisting of hydrous minerals and carbonaceous materials. [1] The direct optical and spectral analysis of the returned samples indicates that Ryugu material is dominated by hydrous carbonaceous chondrite-like matter (similar to CI chondrites) [2]. Since carbonaceous chondrites have generally yielded various types of organic matter, the collected Ryugu grains are expected to contain diverse types of organic compounds including bio-related molecules. The occurrence of organic compounds in the Ryugu surface will provide clues to the evolution of prebiotic molecules and their preservations associated with aqueous alteration of the primitive asteroid. The initial analysis of soluble organic matter (SOM) of the Hayabusa2-returned samples has been performed by an international team consisting of 32 members. Because the sample amount available for comprehensive SOM analyses is limited, and because the SOM is expected to be present as a complex mixture of various types of organic compounds with very small concentrations of each compound, high-sensitivity and high-resolution analytical techniques have been developed using carbonaceous meteorites [e.g. 3]. Two aggregate samples of the Ryugu grains (A106 and C107) were allocated for the solvent extractions and bulk carbon (C), hydrogen (H), nitrogen (N), sulfur (S) and oxygen (O) measurements. The A106 sample was collected during the 1st sampling in February 2019 and the C107 sample was collected during the 2nd sampling in July 2019 after the Small Carry Impactor (SCI) operation. They consist mainly of particles smaller than 1 mm in diameter, and each sample mass was 38-39 mg. They were firstly investigated spectroscopically in the near infrared wavelength range by the Stone Team prior to the solvent extractions. Other small grains (A0080 and C0057) were also allocated for this study to investigate the spatial distribution of organic compounds on the sample surface. The extraction and analytical measurements implemented by the SOM Team are summarized in Figure 1. Each powder sample was extracted sequentially with non-polar to polar solvents, i.e., hexane, dichloromethane (DCM), methanol (MeOH) and H2O, for non-targeted analysis to reveal the compound composition. Each solvent extract was analyzed by solution state nuclear magnetic resonance (NMR) spectroscopy [4], Fourier transform- ion cyclotron resonance/mass spectrometry (FT-ICR/MS) with ESI and APPI ionization [5] and by high-resolution mass spectroscopy using Orbitrap MS coupled with nano-liquid chromatography (nanoLC/Orbitrap MS) [6], and using two dimensional gas chromatography/mass spectrometry (GC×GC/MS). The extracted residues were passed to the Chemistry Team for further inorganic element analysis. The other powder sample was subjected to the hot water extraction for amino acid analyses including chiral isomer separation, which was performed by three-dimensional (3D) high-performance liquid chromatography (HPLC) with high-sensitivity fluorescence detection (FD) [7] and by HPLC/FD coupled with quadrupole-time of flight/mass spectrometry (QToF/MS) [8]. After the hot water extraction, the residue was split into two halves. One half was further extracted with hydrochloric acid (HCl) to analyze for amino acids in bound-form. The other half was sequentially extracted with DCM/MeOH (1/1) to analyze semi-polar compounds such as polycyclic aromatic hydrocarbons (PAHs) by GC/MS, followed by further extraction with formic acid to analyze polar heterocyclic compounds, and subsequent extraction with HCl to detect bound-form polar compounds. The extracted residues were passed to the IOM Team for the analysis of insoluble organic matter (IOM). Compound-specific stable isotope analyses will be performed using GC/combustion/isotope ratio mass spectrometry (GC/C/IRMS) if the compound concentration is high enough to enable such an isotopic measurement. All extraction procedures were performed on an ISO 6 (Class 100) clean bench inside an ISO 5 (Class 1000) clean room. Baked serpentine powder was also analyzed as a procedural blank. In situ organic compound analysis with the molecular imaging was performed using desorption electrospray ionization (DESI) equipped with Orbitrap MS [9, 10], followed by spatial imaging of organic compounds using ToF/secondary ion mass spectrometry (ToF/SIMS) [11]. The bulk chemical and isotopic compositions of CNS and HO were determined using nano-elemental analysis/isotope ratio mass spectrometry (nanoEA/IRMS) [12] and EA/pyrolysis/IRMS, respectively. We have identified a variety of indigenous organic compounds in the extracts of both A106 and C107 samples. The Ryugu grains host organic molecules under the high-vacuum and cosmic-ray irradiation environment of the asteroid surface. The analysis of extracted molecules is in progress, and the first results will be presented at the symposium.

Hiroshi Naraoka↗