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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

A High-Entropy Oxide as High-Activity Electrocatalyst for Water Oxidation

High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr 0.2 Mn 0.2 Fe 0.2 Co 0.2 Ni 0.2 O 3-δ with the parent compounds (single B-site in the ABO 3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition–function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono- or bimetallic oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2002

On the Pathways of the Return Flow of the Meridional Overturning Circulation in the Tropical Atlantic

A numerical model of the tropical Atlantic ocean is used to investigate the upper layer pathways of the Meridional Overturning Circulation (MOC) in the tropical Atlantic. The main focus of this thesis is on those parts of the tropical circulation that are thought to be important for the MOC return flow, but whose dynamics have not been understood yet. It is shown how the particular structure of the tropical gyre and the MOO act to inhibit the flow of North Atlantic water into the equatorial thermocline. As a result, the upper layers of the tropical Atlantic are mainly fed by water from the South Atlantic. The processes that carry the South Atlantic water across the tropical Atlantic into the North Atlantic as part of the MOO are described here, and three processes that were hitherto not understood are explained as follows: The North Brazil Current rings are created as the result of the reflection of Rossby waves at the South American coast. These Rossby waves are generated by the barotropically unstable North Equatorial Countercurrent. The deep structure of the rings can be explained by merger of the wave's anticyclones with the deeper intermediate eddies that are generated as the intermediate western boundary current crosses the equator. The bands of strong zonal velocity in intermediate depths along the equator have hitherto been explained as intermediate currents. Here, an alternative interpretation of the observations is offered: The Eulerian mean flow along the equator is negligible and the observations are the signature of strong seasonal Rossby waves. The previous interpretation of the observations can then be explained as aliasing of the tropical wave field. The Tsuchyia Jets are driven by the Eliassen-Palm flux of the tropical instability waves. The equatorial current system with its strong shears is unstable and generates tropical instability waves.

Jochum, Markus↗
NASA NTRS2000

Soil, Groundwater, Surface Water, and Sediments of Kennedy Space Center, Florida: Background Chemical and Physical Characteristics

This study documented background chemical composition of soils, groundwater, surface; water, and sediments of Kennedy Space Center. Two hundred soil samples were collected, 20 each in 10 soil classes. Fifty-one groundwater wells were installed in 4 subaquifers of the Surficial Aquifer and sampled; there were 24 shallow, 16 intermediate, and 11 deep wells. Forty surface water and sediment samples were collected in major watershed basins. All samples were away from sites of known contamination. Samples were analyzed for organochlorine pesticides, aroclors, chlorinated herbicides, polycyclic aromatic hydrocarbons (PAH), total metals, and other parameters. All aroclors (6) were below detection in all media. Some organochlorine pesticides were detected at very low frequencies in soil, sediment, and surface water. Chlorinated herbicides were detected at very low frequencies in soil and sediments. PAH occurred in low frequencies in soiL, shallow groundwater, surface water, and sediments. Concentrations of some metals differed among soil classes, with subaquifers and depths, and among watershed basins for surface water but not sediments. Most of the variation in metal concentrations was natural, but agriculture had increased Cr, Cu, Mn, and Zn.

Shmalzer, Paul A.↗
NASA NTRS1976

Studies of Current Circulation at Ocean Waste Disposal Sites

The author has identified the following significant results. Acid waste plume was observed in LANDSAT imagery fourteen times ranging from during dump up to 54 hours after dump. Circulation processes at the waste disposal site are highly storm-dominated, with the majority of the water transport occurring during strong northeasterlies. There is a mean flow to the south along shore. This appears to be due to the fact that northeasterly winds produce stronger currents than those driven by southeasterly winds and by the thermohaline circulation. During the warm months (May through October), the ocean at the dump site stratifies with a distinct thermocline observed during all summer cruising at depths ranging from 10 to 21 m. During stratified conditions, the near-bottom currents were small. Surface currents responded to wind conditions resulting in rapid movement of surface drogues on windy days. Mid-depth drogues showed an intermediate behavior, moving more rapidly as wind velocities increased.

Klemas, V.↗
NASA NTRS1993

Constraints on the rate of discharge and duration of the Mangala Valles flood

Interest in Mangala Valles remains high within the planetary science community. This is justified because the survey mission images provide us with nearly complete coverage of the system at high resolution. Upcoming high resolution topography from the Mars Observer Laser Altimeter will enable the application of flood discharge models with an unprecedented level of detail. Previous work on the Mangala Valles problem has relied on the available low resolution topography. This has limited the ability of workers to constrain discharge calculations to only within several-order-of-magnitude estimates. Local determinations of channel depths via shadow length measurements and photoclinometric profiling are much more accurate, but can only be applied to steep slopes (and/or low sun elevations) in the case of shadow measurements, or across relatively short distances (to avoid changes in albedo along asymmetric photoclinometric profiles). We are taking stereo parallax measurements from medium resolution Viking Orbiter images, which provide a valuable intermediate check of the topography between those measurements made thus far and the upcoming Mars Observer data. The images used are from orbits 034A and 637A, and cover Mangala Valles from the source graben in Memnonia Fossae to the beginning of the bifurcated reach (at 9.5 deg lat., 151.5 deg lon.). These images are about 300 m/pixel and 250 m/pixel, respectively. Both sets of images were orthographically projected to 250 m/pixel. The separation angle between left-right pairs is approximately 52 degrees. This results in a vertical accuracy on the order of plus or minus 260 m. Though this is still somewhat coarse, the channel relief is clearly resolved. Preliminary profiles across Mangala Valles and the large topographic ridge to the east are shown on the following page. An east-west regional tilt that resulted from slight scaling differences in the digital data has been 'removed' by visually estimating a regional datum on the stereo pairs. North-south variations in scale have not yet been adjusted for, so the zero datum for each profile was simply taken to be the high water line of the channel itself. Our depth measurement for the source breach of about 750 m agrees reasonably well with values of 700-1000 m determined from shadow measurements.

Parker, T. J.↗
NASA NTRS1987

Seasonal cycling of sulfur and iron in porewaters of a Delaware salt marsh

An extensive pore water data set has been gathered in the Great Marsh, Delaware over various seasons, salinities, and tides. The data all point to a complimentary redox cycle for sulfur and iron which operates seasonally and tidally. Surface oxidizing conditions prevail in summer, with more reducing conditions at depth during the winter. During the spring tides which flood the marsh, pyrite oxidation occurs releasing excess dissolved iron (II) and sulfate to the porewaters, and precipitating authigenic solid iron phases. The redox conditions in the porewaters of the upper zone during the summer is poised between mildly oxidizing and mildly reducing conditions as shown by pE calculations. This redox environment and intermediate iron-sulfur redox species may be important for the stimulation of plant growth (photosynthesis) and sustenance of a viable microbial community (heterotrophy and chemoautropy).

Luther, George W., III↗
DOE OSTI2022

More Realistic Intermediate Depth Dry Firn Densification in the Energy Exascale Earth System Model (E3SM)

Abstract Earth system models account for seasonal snow cover, but many do not accommodate the deeper snowpack on ice sheets (aka firn) that slowly transforms to ice under accumulating snowfall. To accommodate and resolve firn depths of up to 60 m in the Energy Exascale Earth System Model's land surface model (ELM), we add 11 layers to its snowpack and evaluate three dry snow compaction equations in multi‐century simulations. After comparing results from ELM simulations (forced with atmospheric reanalysis) with empirical data, we find that implementing into ELM a two‐stage firn densification model produces more accurate dry firn densities at intermediate depths of 20–60 m. Compared to modeling firn using the equations in the (12 layer) Community Land Model (version 5), switching to the two‐stage firn densification model (with 16 layers) significantly decreases root‐mean‐square errors in upper 60 m dry firn densities by an average of 41 kg m −3 (31%). Simulations with three different firn density parameterizations show that the two‐stage firn densification model should be used for applications that prioritize accurate upper 60 m firn air content (FAC) in regions where the mean annual surface temperature is greater than roughly −31°C. Because snow metamorphism, firn density, and FAC are major components in modeling ice sheet surface albedo, melt water retention, and climatic mass balance, these developments advance broader efforts to simulate the response of land ice to atmospheric forcing in Earth system models.

58 GEOSCIENCES↗
DOE OSTI2023

Spatial Study 2022: Water Column, Sediment, and Total Ecosystem Respiration Rates across the Yakima River Basin, Washington, USA (v2)

This dataset supports a broader study examining the drivers of spatial variability in sediment respiration rates in the Yakima River Basin and is associated with the manuscript “Sediment-associated processes account for most of the spatial variation in ecosystem respiration in the Yakima River basin” submitted to Nature Communications Earth & Environment (Garayburu-Caruso et al., in review). The dataset provides ecosystem metabolism estimates generated from streamMetabolizer (Appling et al.; 2018) using data collected during the same five-week period at 48 sites within multiple rivers throughout the Yakima River Basin in Washington, USA. Additionally, it includes the scripts used for the analysis and producing the figures in the manuscript. The contents include streamMetabolizer inputs and outputs and additional relevant data needed to generate the main manuscript results. The data included are: total ecosystem respiration, water respiration, calculated sediment-associated respiration, gross primary production outputs from the river corridor model for the Yakima River Basin, median grain size (d50), depth, dissolved oxygen, water temperature, pressure, and annual oxygen consumption. The associated GitHub repository can be found at https://github.com/river-corridors-sfa/SSS_metabolism. Samples collected during this study were labeled as “Second Spatial Study” or “SSS.” Raw time series sensor data, total suspended solids, and depth data from SSS were published at https://data.ess-dive.lbl.gov/datasets/doi:10.15485/1969566. A subset of data from the SSS samples were published in the contiguous United States (CONUS)-Scale Model-Sample (CM) study data package available at https://data.ess-dive.lbl.gov/view/doi:10.15485/1923689 that presents data from across the CONUS. They include dissolved organic carbon (DOC, measured as non-purgeable organic carbon, NPOC), total nitrogen (TN), grain size, aerobic sediment respiration, dissolved oxygen (DO), and temperature. Parent IDs and Site IDs are consistent between the SSS and CM data packages, and they can be mapped directly so data across packages can be used together. Field metadata for the samples in this da This dataset is comprised of one main data folder with four subfolders. The main data folder contains of (1) file-level metadata; (2) data dictionary; (3) total/water column/sediment respiration; (4) gross primary production (GPP); (5) median grain size (d50); and (6) annual oxygen consumption. The “Figures” subfolder contains the figures used in the paper and all intermediate files (including geospatial files). The “Published_Data” contains a readme directing the user to download the public data to reproduce analyses and figures. The “Scripts” folder contains all scripts used in the analyses that were not part of running StreamMetabolizer. Lastly, the “Stream_Metabolizer” folder contains all files associated with running StreamMetabolizer including (1) model input files, (2) model output files, (3) processing scripts, (4) histogram plots of the outputs, and (5) an R project. All files are .csv, .pdf, .R, .Rmd, .Rproj, .html, .png, .txt, .qgz, .cpg, .dbf, .prj, .shp, .shp.ea.iso.xml, .shp.iso.xml, .shx, .sbn. ta package can be found at either link. We acknowledge the Yakama Nation as owners and caretakers of the lands where we collected these data. We thank the Confederated Tribes and Bands of the Yakama Nation Tribal Council and Yakama Nation Fisheries for working with us to facilitate sample collection and optimization of data usage according to their values and worldview.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Oxygen Evolution on Iron Oxide Nanoparticles: The Impact of Crystallinity and Size on the Overpotential

The oxygen evolution reaction (OER) is a critical reaction in electrolysis and photoelectrolysis of water to generate and store clean energy. Therefore, the development of low-cost and efficient electrocatalysts for the OER is of great scientific and technological importance. Although promising iron oxide-based electrocatalysts have been recently developed for the OER, an in-depth experimental and theoretical analysis of the OER mechanism on iron oxide-based electrocatalysts is still needed to provide guidelines to optimize the performance of iron oxide-based electrocatalysts further. To address this need, we synthesized a series of monodisperse iron oxide nanoparticles to analyze their intrinsic OER activities. Using nanoparticles of the same size but different crystallinity, we show that amorphous iron oxide nanoparticles have better OER activity than crystalline ones. The size effect studies further revealed that the edge/defect sites are the active sites for the OER. Density functional theory calculations demonstrated that the edge/defect sites provide bridge sites to adsorb OER intermediates, resulting in low OER overpotential. These calculations confirm that the high OER activity of amorphous nanoparticles results from a high concentration of defect sites on their surface. These results provide novel strategies to increase the performance of iron oxide-based and likely other oxide-based OER electrocatalysts.

Electrochemistry↗
DOE OSTI2020

Pervasive low-velocity layer atop the 410-km discontinuity beneath the northwest Pacific subduction zone: Implications for rheology and geodynamics

Regional triplication waveforms of five intermediate-depth events are modeled to simultaneously obtain the compressional (P) and shear (SH) wave velocity structure beneath northwestern Pacific subduction zone. Both the P- and SH-wave velocity models for three different sub-regions show a low-velocity layer (LVL) with a thickness of ~55-80 km lying above the 410-km discontinuity with a ~900 km lateral extent from the Japan Sea to the northeastern Asian continental margin. With the dihedral angle approaching to zero around 400 km, a minute amount of melt atop the 410-km discontinuity caused by the hydrous slab might completely wet olivine grain boundaries and result in a low seismic velocity layer in this specific subduction zone. This mechanism suggests that the 410-LVL is a low viscosity zone that would partially decouple the upper mantle from the transition zone. We infer that the widespread 410-LVL provides evidence for a water-bearing mantle transition zone beneath the western Pacific subduction zone.

58 GEOSCIENCES↗
NASA NTRS2013

The MJO Transition from Shallow to Deep Convection in CloudSat/CALIPSO Data and GISS GCM Simulations

The relationship between convective penetration depth and tropospheric humidity is central to recent theories of the Madden-Julian oscillation (MJO). It has been suggested that general circulation models (GCMs) poorly simulate the MJO because they fail to gradually moisten the troposphere by shallow convection and simulate a slow transition to deep convection. CloudSat and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) data are analyzed to document the variability of convection depth and its relation to water vapor during the MJO transition from shallow to deep convection and to constrain GCM cumulus parameterizations. Composites of cloud occurrence for 10MJO events show the following anticipatedMJO cloud structure: shallow and congestus clouds in advance of the peak, deep clouds near the peak, and upper-level anvils after the peak. Cirrus clouds are also frequent in advance of the peak. The Advanced Microwave Scanning Radiometer for EarthObserving System (EOS) (AMSR-E) columnwater vapor (CWV) increases by;5 mmduring the shallow- deep transition phase, consistent with the idea of moisture preconditioning. Echo-top height of clouds rooted in the boundary layer increases sharply with CWV, with large variability in depth when CWV is between;46 and 68 mm. International Satellite Cloud Climatology Project cloud classifications reproduce these climatological relationships but correctly identify congestus-dominated scenes only about half the time. A version of the Goddard Institute for Space Studies Model E2 (GISS-E2) GCM with strengthened entrainment and rain evaporation that produces MJO-like variability also reproduces the shallow-deep convection transition, including the large variability of cloud-top height at intermediate CWV values. The variability is due to small grid-scale relative humidity and lapse rate anomalies for similar values of CWV. 1.

DelGenio, Anthony G.↗
NASA NTRS2015

Evolution of the Oxidation State of the Earth's Mantle: Challenges of High Pressure Quenching

The oxidation state of the Earth's mantle during formation remains an unresolved question, whether it was constant throughout planetary accretion, transitioned from reduced to oxidized, or from oxidized to reduced. We investigate the stability of Fe3+ at depth, in order to constrain processes (water, late accretion, dissociation of FeO) which may reduce or oxidize the Earth's mantle. Experiments of more mafic compositions and at higher pressures commonly form a polyphase quench intergrowth composed primarily of pyroxenes, with interstitial glass which hosts nearly all of the more volatile minor elements. In our previous experiments on shergottite compositions, variable fO2, T, and P is less than 4 GPa, Fe3+/TotFe decreased slightly with increasing P, similar to terrestrial basalt. For oxidizing experiments less than 7GPa, Fe3+/TotFe decreased as well, but it's unclear from previous modelling whether the deeper mantle could retain significant Fe3+. Our current experiments expand our pressure range deeper into the Earth's mantle and focus on compositions and conditions relevant to the early Earth. Experiments with Knippa basalt as the starting composition were conducted at 1-8 GPa and 1800 C, using a molybdenum capsule to set the fO2 near IW, by buffering with Mo-MoO3. TEM and EELS analyses revealed the run products from 7-8 GPa quenched to polycrystalline phases, with the major phase pyroxene containing approximately equal Fe3+/2+. A number of different approaches have been employed to produce glassy samples that can be measured by EELS and XANES. A more intermediate andesite was used in one experiment, and decompression during quenching was attempted after, but both resulted in a finer grained polyphase texture. Experiments are currently underway to test different capsule materials may affect quench texture. A preliminary experiment using liquid nitrogen to greatly enhance the rate of cooling of the assembly has also been attempted and this technique will be refined in further experiments.

Danielson, L. R.↗
DOE OSTI2020

Thermocatalytic Heat Pipes for Geothermal Resource Recovery

Heat pipes are an important technology that allow orders of magnitude faster heat transfer than simple conduction. However, operating principles in heat pipes place fundamental bounds on their performance (critical heat flux and efficiency). Conventional heat pipe functionality is inherently tied to vaporization and condensation of the working fluid charged in the heat pipe. These fluids each have different operating temperature ranges based on the capillary, entrainment, sonic, and boiling limits of the heat pipe design. These limits, typically the capillary limit, dictate the maximum heat flux a heat pipe can carry, and most importantly for geothermal systems, the distance over which the pipes can operate (100 to 200 m maximum under optimum conditions). A thermocatalytic heat pipe breaks the inherent limitations of phase change thermo- and hydrodynamics and can transform heat pipe technology as a potentially more efficient means of extracting heat from a geothermal resource. The thermocatalytic heat pipe uses a working fluid to transport both sensible and chemical heat. An endothermic chemical reaction at depth removes heat from the reservoir and produces reactive intermediates, which are transported to the surface and used to run a reverse exothermic reaction that releases heat for use in power generation or other useful purposes. This technology offers two distinct advantages over conventional geothermal heat recovery technologies: (1) lower heat loss to the rock outside of the geothermal reservoir, and (2) higher heat transfer rates to the well field within the geothermal reservoir. Both advantages offer opportunity to reduce risks and lower costs of geothermal energy recovery. In this report, we discuss an initial effort to assess the efficacy and limitations of this technology for extracting heat from both porous/permeable and nominally impermeable geothermal reservoirs. Numerical simulation capabilities of the STOMP-GT code were enhanced to enable simulations of thermochemical heat pipes traversing geothermal reservoirs. An array of potential thermochemical reaction systems was evaluated and screened. Of these, an ethanol dehydration reaction was most promising in the vapor-liquid reaction set. A solid-phase dehydration reaction (CuSO4·5H2O) showed the highest reaction enthalpy per unit volume but would require development of a nonaqueous carrier fluid to implement it in a heat pipe. Subsurface reservoir simulations predicted long-term performance of the heat pipes for each geothermal reservoir type. The performance of U-shaped wells and coaxial wells was evaluated for a suite of reactions for both hydrothermal and hot dry rock reservoirs and was compared with a baseline case of simply pumping water through the wells. The heat pipe technology was additionally evaluated for an enhanced geothermal system (EGS) with an injection borehole, production borehole, and intervening hydraulically conductive fracture. All reservoir types showed significant improvement in heat recovered over a 20-year operating period ranging from a 1.8X increase for the hot dry rock case to more than 2.5X more energy recovered for the EGS case.

15 GEOTHERMAL ENERGY↗
DOE OSTI2024

Water foraging with dynamic roots in E3SM; The role of roots in terrestrial ecosystem memory on intermediate timescales (Final Technical Report)

Terrestrial ecosystems can show sustained responses to stress events that may last for years after the initial perturbation. This phenomenon is referred to as legacy or memory and it emerges from a set of ecosystem processes that are poorly captured by Earth System and Land Surface Models. Consequently, these models struggle to predict the impact that extreme climate events have on surface energy, carbon and hydrological exchange once a stressor such as drought has relaxed or in response to repeated exposure to stress. In this project, we set out to test how the addition of dynamic root profiles in land surface models impact the capacity for Earth System Models, such as the Department of Energy’s E3SM, to capture realistic legacy effects. Observations have shown that vegetation shifts their root profiles during stress events to forage for water and these altered root profiles may take years to relax back to the initial state. We hypothesized that the alteration of the belowground root structures may be a source of terrestrial ecosystem legacy that is missing from models. To test this idea we undertook three core activities. (1) We developed a global-scale analysis of the impact of dynamic roots on ecosystem legacy building from a recently developed dynamic root module. (2) We developed new root dynamics in the DOE’s Energy Land Model (ELM) that allowed not only root profiles to shift their profile but also simultaneously alter carbon allocation to fine root pools. We then tested the impact of these new dynamics with intensive sensitivity analysis at four long-term AmeriFlux sites. (3) We undertook detailed isotopic analysis of tree rings from these AmeriFlux sites to assess ecophysiological and ecohydrological legacy to stress events that can be used to benchmark the sensitivity experiments with ELM. From these core activities, we report the following key findings. Firstly, on a global scale, the addition of dynamic roots led to chronically water-stressed ecosystems recovering faster to climate stress while wetter ecosystem showed enhanced legacy. This is because across ecosystems, stress events were almost universally associated with water shortages that led to the development of deeper root profiles. These deeper root profiles proved beneficial for recovery from drought stress. While the root dynamics did not universally improve the modeled representation of legacy it showed complex transient dynamics that emerge from the addition of dynamic roots. Secondly, the sensitivity analysis illustrated long term shifts in rooting depths away from the prescribed default profile suggesting that initializing of root profiles could benefit from spin-up simulations that converge on locally optimized root profiles. In addition, by enabling dynamic allocation some of the sites predicted unrealistically low allocation to roots (and high allocation to leaves). While these changes did not dramatically alter modeled gross primary productivity, they illustrated that without more sophisticated root processes in models, there is little penalty to dramatically disinvest in roots. Thirdly, the isotopic analysis of tree rings showed highly distinct legacy responses across species and sites. For example, T. canadensis showed reduced transpiration the year after stress events illustrated by sustained elevated $\delta^{18}$O. In contrast, A saccharum displayed elevated $\delta^{13}$C associated with reduced stomatal conductance in response to the previous years’ stress event. These geochemical signatures of legacy were present despite tree growth returning to normal the year after the stress. The results show the importance of species-level dynamics in legacy that are absent in modeling that assumes common traits within plant functional types. In summary, the work here established new avenues to explore root dynamics in models while illustrating how additional root processes are needed before dynamic carbon allocation can be implemented. Lastly, this project provided mentorship to a postdoctoral fellow, training for an early career scientist and multiple undergraduate students recruited from a minority serving institution.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Influence of covariance of aerosol and meteorology on co-located precipitating and non-precipitating clouds over the Indo-Gangetic Plain

Aerosol–cloud–precipitation interaction (ACPI) plays a pivotal role in the global and regional water cycle and the earth's energy budget; however, it remains highly uncertain due to the different underlying physical mechanisms. Therefore, this study aims to systematically analyze the effects of aerosols and meteorological factors on ACPI in the co-located precipitating clouds (PCs) and non-precipitating clouds (NPCs) in winter and summer seasons by employing the long-term (2001–2021) retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Tropical Rainfall Measuring Mission (TRMM) coupled with the National Center for Environmental Prediction/National Center for Atmospheric Research (NCEP/NCAR) reanalysis-II datasets over the Indo-Gangetic Plain (IGP). The results exhibit a decadal increase in aerosol optical depth (AOD) over Lahore (5.2 %), Delhi (9 %), Kanpur (10.7 %), and Gandhi College (22.7 %) and a decrease over Karachi (-1.9 %) and Jaipur (-0.5 %). The most stable meteorology with high values of lower-tropospheric stability (LTS) is found in both seasons over Karachi. In the summer season, the occurrence frequency of clouds is high (74 %) over Gandhi College, 60 % of which are PCs. Conversely, the lowest number of PCs is found over Karachi. Similarly, in the winter season, the frequency of cloud occurrence is low over Karachi and high over Lahore and Gandhi College. The analysis of cloud top pressure (CTP) and cloud optical thickness (COT) indicates high values of cloud fraction (CF) for thick and high-level clouds over all study areas except Karachi. The microphysical properties such as cloud effective radius (CER) and cloud droplet number concentration (CDNC) bear high values (CER ≳ 15 µm and CDNC ≳ 50 cm -3 ) for both NPCs and PCs in summer. The AOD–CER correlation is good (weak) for PCs (NPCs) in winter. Similarly, the sensitivity value of the first indirect effect (FIE) is high (ranging from 0.2 ± 0.13 to 0.3 ± 0.01 in winter and from 0.19 ± 0.03 to 0.32 ± 0.05 in summer) for PCs and low for NPCs. The sensitivity value for the second indirect effect (SIE) is relatively higher (such as 0.6 ± 0.14 in winter and 0.4 ± 0.04 in summer) than FIE. Sensitivity values of the aerosol-cloud interaction (ACI) are low (i.e., -0.06 ± 0.09) for PCs in summer. Furthermore, the precipitation rate (PR) exhibits high values in the summer season, primarily due to the significant contribution from optically thick clouds with lower CDNC (≲ 50 cm -3 ) and larger CER and the intermediate contribution from optically thick clouds with higher CDNC ( ≳ 50 cm -3 ).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Cell Free and Immobilization Technologies (CFIT)

Today, several key factors negatively impact the production of fuels and chemicals from renewable sources. Common hindrances in the biological production of biochemicals are: (1) end-product or intermediate toxicity to the microbial biocatalyst, (2) the diversion of carbon to biomass formation, and (3) co-production of undesired byproducts. A particularly attractive alternative is to eliminate the biocatalyst entirely and instead operate the desired metabolic pathways in isolation, thus circumventing the roadblocks of biological toxicity, lower yields, and lack of specificity. However, cell-free enzyme systems still suffer from low productivities owing in part to the effects of free diffusion of intermediates, lack of long term enzyme stability, cofactor cost or inefficient recycling rates, and finally, the cost of enzyme production/purification. This project represents a new effort to propose innovative and cost competitive routes to producing biochemicals from a variety of feedstocks using cell free approaches. These routes will help reduce the current risk and cost associated with classical cell free production. Cell free technologies show promise for application to the production of toxic/inhibitory products or products difficult to separate from microbial growth media and can help reduce the production barriers in multiple areas of biological conversion of feedstocks to biochemicals. More specifically, we are developing new technologies and routes that could be used to produce high value biochemicals such as 2,3 BDO and terpenes (among many others) from biomass derived C5/C6 sugars or lignin but also from waste byproducts such as glycerol. This project will lead to significant innovation and also lead to new concepts and rational design of pathways and enzymes. Within this project, we will develop new metabolic enzyme cascades that will represent natural or artificial combinations of enzymes to produce the desired biochemicals from a variety of feedstocks. We are also developing basic design principals for constructing synthetic metabolons, using fusion proteins and synthetic protein scaffolds, to promote substrate channeling and stability while conserving peak activity. Additionally, our efforts include a techno economic analysis (TEA) of cell free approaches to provide the sensitivities of the process to enzyme loading, activity, pH, reactor volumes, cofactor recycling rates. Finally, we are focusing on further increasing stability, operating lifetime and efficiency of the pathway enzymes by immobilization on support surfaces. We are also focus on immobilizing pathway enzymes or combinations of enzymes on several different conducting polymers and evaluate the effect on stability and operating lifetime. As more combinations become available we will conduct a more systematic study of the means of immobilizing these enzymes. This preliminary work will enable the in-depth study of cofactor recycling at these interfaces using mediators for electron transfer. Taken together, these approaches will enable process intensification, continuous operation, lower capital and separations costs and end-product flexibility, and thus has the potential to contribute significantly to BETO's goals of cost competitive biofuels and bioproducts. To date we have demonstrated 1) the conversion of pyruvate to 2,3 BDO (4 enzymes with cofactor recycling, no additional cofactors needed) at >100g/L (>3g/L/h) using our enzyme tethering approach, 2) Generated mutants of a key redox enzyme with >180- fold improvement in NADH utilization over WT to >85% of NADPH utilization. 3) Produced mevalonate at >10g/L from glucose, limonene at >10g/L from mevalonate and more than >5g/L from glucose with crude enzyme preparations and complete cofactor recycling. 4) successfully generated fully active cross-linked aggregates (CLEAs) of NOX, a cofactor-regenerating water-forming oxidase that is key to our process with increased stability 5) Engineered and identified enzymes able to use the biomimetic cofactor NMN and synthesized new synthetic cofactors.

biocatalysis↗