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NASA NTRS1989

Theory and observations: Model simulations of the period 1955-1985

The main objective of the theoretical studies presented here is to apply models of stratospheric chemistry and transport in order to understand the processes that control stratospheric ozone and that are responsible for the observed variations. The model calculations are intended to simulate the observed behavior of atmospheric ozone over the past three decades (1955-1985), for which there exists a substantial record of both ground-based and, more recently, satellite measurements. Ozone concentrations in the atmosphere vary on different time scales and for several different causes. The models described here were designed to simulate the effect on ozone of changes in the concentration of such trace gases as CFC, CH4, N2O, and CO2. Changes from year to year in ultraviolet radiation associated with the solar cycle are also included in the models. A third source of variability explicitly considered is the sporadic introduction of large amounts of NO sub x into the stratosphere during atmospheric nuclear tests.

Isaksen, Ivar S. A.↗

NASA NTRS1992

Ocean-atmospheric linkages

This chapter focuses on the role of the ocean in the global carbon cycle on the time scale of decades to centuries. The input rate of CO2 to the atmosphere due to fossil fuel burning and deforestation has continued to increase over the last century. To balance the global carbon budget, a sink is required whose magnitude is changing on similar time scales. We have sought to identify aspects of the ocean system that are capable of responding on decadal time scales, to examine our present ability to model such changes, and to pinpoint ways in which this ability could be improved. Many other important aspects of the ocean's role in global change are not addressed, including the importance of oceanic heat transport and thermal inertia to the climate system, biogeochemical cycling of elements other than carbon, and the importance of the ocean as a source or sink of trace gases.

Rintoul, Stephen R.↗

DOE OSTI2022

Airborne Lidar Measurements of XCO 2 in Synoptically Active Environment and Associated Comparisons With Numerical Simulations

Frontal boundaries have been shown to cause large changes in CO 2 mole-fractions, but clouds and the complex vertical structure of fronts make these gradients difficult to observe. It remains unclear how the column average CO 2 dry air mole-fraction (XCO 2 ) changes spatially across fronts, and how well airborne lidar observations, data assimilation systems, and numerical models without assimilation capture XCO 2 frontal contrasts (ΔXCO 2 , i.e., warm minus cold sector average of XCO 2 ). We demonstrated the potential of airborne Multifunctional Fiber Laser Lidar (MFLL) measurements in heterogeneous weather conditions (i.e., frontal environment) to investigate the ΔXCO 2 during four seasonal field campaigns of the Atmospheric Carbon and Transport-America (ACT-America) mission. Most frontal cases in summer (winter) reveal higher (lower) XCO 2 in the warm (cold) sector than in the cold (warm) sector. During the transitional seasons (spring and fall), no clear signal in ΔXCO 2 was observed. Intercomparison among the MFLL, assimilated fields from NASA's Global Modeling and Assimilation Office (GMAO), and simulations from the Weather Research and Forecasting-—Chemistry (WRF-Chem) showed that (a) all products had a similar sign of ΔXCO 2 though with different levels of agreement in ΔXCO 2 magnitudes among seasons; (b) ΔXCO 2 in summer decreases with altitude; and (c) significant challenges remain in observing and simulating XCO 2 frontal contrasts. A linear regression analyses between ΔXCO 2 for MFLL versus GMAO, and MFLL versus WRF-Chem for summer-2016 cases yielded a correlation coefficient of 0.95 and 0.88, respectively. The reported ΔXCO 2 variability among four seasons provide guidance to the spatial structures of XCO 2 transport errors in models and satellite measurements of XCO 2 in synoptically-active weather systems.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Canadian Oil Sands Extraction and Upgrading: A Synthesis of the Data on Energy Consumption, CO 2 Emissions, and Supply Costs

As Canadian crude bitumen production from oil sands has increased in recent decades, the nation’s oil and gas industry has become a significant contributor to national greenhouse gas emissions. Canada has developed carbon emission reduction targets to meet its Nationally Determined Contributions and Mid-Century Strategy goals. A detailed profile of energy consumption pathways in the oil sands industry is necessary to identify potential areas of improvement and to monitor progress toward meeting emissions reduction targets. Much of the existing literature for oil sands modeling provides input assumptions with different technological boundaries. For a set of oil sands extraction and upgrading technologies, this study first reviews the literature and then quantifies energy input requirements, CO 2 emissions, and operating costs for a set of consistent technological boundaries and energy units. Summary results refer to requirements and costs at the production facility, excluding transportation and blending costs. An energy system diagram of oil sands production that matches these boundaries is provided, which can be used by integrated assessment models, oil sands companies, and government ministries to evaluate the present and future energy consumption and emissions pathways of the oil sands industry.

02 PETROLEUM↗

DOE OSTI2022

Simulation and Optimization of Volatile Fatty Acid Upgrading Strategies for Sustainable Transportation Fuel Production

Underutilized wet waste is a promising feedstock for production of carbon-neutral or carbon-negative liquid transportation fuels. Arrested methanogenesis of wet wastes by microbes, which produces mixtures of C2-C8 carboxylic acids (volatile fatty acids, VFAs), is practiced industrially at a pilot scale and the VFA products can be catalytically upgraded to molecules suitable for use as transportation fuels (alcohols and alkanes) via sequential ketonization and hydrogenation, both steps of which have been demonstrated with high (>90%) yield at the lab scale. We present in this work a simulation-based decision-making framework which evaluates upgrading strategies of VFAs to alcohol- and hydrocarbon-based neat and blended diesel, jet, and gasoline fuels. The processes utilize sequential upgrading steps (ketonization and hydrogenation) accompanied by one distillation step (either separating VFAs before ketonization or alcohols after ketone hydrogenation) to form two liquid streams: a light alcohol stream best suited as a light-duty fuel and a heavy alcohol or hydrocarbon stream best suited as a diesel or jet fuel. Suitability of the liquid products as transportation fuels and maximum blending levels with petrofuels comes from simulation of critical fuel properties (boiling point, flash point, lower heating value, viscosity, melting point, water solubility, and cetane/octane number). Catalytic upgrading steps and fuel property mixing models used by the simulation are experimentally validated. We demonstrate the flexibility of the decision-making algorithm by evaluating processing scenarios for experimentally-observed VFA profiles with varied carbon chain length distributions. Processing scenarios are optimized for either maximum total renewable carbon utilization or production of heavy-duty (jet or diesel) fuels. We evaluate the economic viability and CO2 emissions of each proposed upgrading scenario using techno-economic and life cycle analyses. The decision-making framework developed in this work can also be used to down-select promising strategies for upgrading of other bio-based feedstocks to sustainable fuels and chemicals.

aviation fuel↗

NASA NTRS2000

Candle Flames in Non-Buoyant Atmospheres

This paper addresses the behavior of a candle flame in a long-duration, quiescent microgravity environment both on the space Shuttle and the Mir Orbiting Station. On the Shuttle, the flames became dim blue after an initial transient where there was significant yellow (presumably soot) in the flame. The flame lifetimes were typically less than 60 seconds. The safety-mandated candlebox that contained the candle flame inhibited oxygen transport to the flame and thus limited the flame lifetime. The flames on the Mir were similar, except that the yellow luminosity persisted longer into the flame lifetime because of a higher initial oxygen concentration, The Mir flames burned for as long as 45 minutes. The difference in the flame lifetime between the Shuttle and Mir flames was primarily the redesigned candlebox that did not inhibit oxygen transport to the flame. In both environments, the flame intensity and the height-to-width ratio gradually decreased as the ambient oxygen content in the sealed chamber slowly decreased. Both sets of experiments showed spontaneous, axisymmetric flame oscillations just prior to extinction. The paper also presents a numerical model of a candle flame. The formulation is two-dimensional and time-dependent in the gas phase with constant specific heats, thermal conductivity and Lewis number (although different species can have different Lewis numbers), one-step finite-rate kinetics, and gas-phase radiative losses from CO2 and H2O. The treatment of the liquid/wick phase assumes that the, fuel evaporates from a constant diameter sphere connected to an inert cone. The model predicts a steady flame with a shape and size quantitatively similar to the Shuttle and Mir flames. The computation predicts that the flame size will increase slightly with increasing ambient oxygen mole fraction. The model also predicts pre-extinction flame oscillations if the rate of decrease in ambient oxygen is small enough, such as that which would occur for a flame burning in a sealed ambient.

Dietrich, D. L.↗

NASA NTRS2017

An ISRU Propellant Production System to Fully Fuel a Mars Ascent Vehicle

In-Situ Resource Utilization (ISRU) will enable the long term presence of humans beyond low earth orbit. Since 2009, oxygen production from the Mars atmosphere has been baselined as an enabling technology for Mars human exploration by NASA. However, using water from the Martian regolith in addition to the atmospheric CO2 would enable the production of both liquid Methane and liquid Oxygen, thus fully fueling a Mars return vehicle. A case study was performed to show how ISRU can support NASA's Evolvable Mars Campaign (EMC) using methane and oxygen production from Mars resources. A model was built and used to generate mass and power estimates of an end-to-end ISRU system including excavation and extraction water from Mars regolith, processing the Mars atmosphere, and liquefying the propellants. Even using the lowest yield regolith, a full ISRU system would weigh 1.7 mT while eliminating the need to transport 30 mT of ascent propellants from earth.

Mars Surface↗

NASA NTRS2022

Nuclear Power Concepts and Development Strategies for High-Power Electric Propulsion Missions to Mars

Under the Mars Transportation Assessment Study (MTAS), NASA and the Department of Energy are performing analyses and generating concepts for crewed nuclear electric propulsion (NEP) missions to Mars. This report presents the results of trade studies and concept development for the nuclear electric power system, consisting of the fission reactor, radiation shielding, power conversion, heat rejection, and power management and distribution (PMAD). The nuclear power team completed trade studies to evaluate different reactor and power conversion technologies and developed preliminary concepts for the crew shielding, waste heat radiators, and PMAD. The initial results suggest that a modified terrestrial microreactor combined with supercritical CO2 Brayton conversion could be used to perform the crew and cargo missions with satisfactory performance and modest risk. The report includes preliminary development strategies that could bring the NEP technology to fruition for Mars missions in the late 2030s or early 2040s.

Lee S. Mason↗

DOE OSTI2023

Evaluation of Additively Manufactured Monolithic SiC and SiC Ceramic Matrix Composites for CSP- Fabrication and Testing of Receiver Design Feature Specimens in a Simulating Lab Test via Laser Heating

Critical to the creation of a multi-component SiC receiver design concept capable of meeting the SETO CST cost goal objectives of <$150/kWth is the optimal utilization of material for solar absorption and heat transfer to transport fluid. This is to maximize the solar-thermal efficiency in the techno-economic analysis of derived use case. As a first step in preparation of sub-component design for on-sun test evaluations we use different proposed SiC absorber element in a customized laser heat flux test to assess an effective heat transfer coefficient characteristic of the design. The test results are analyzed to extract the effective heat transfer coefficient, thus enable optimization of the geometry of receiver components for heat transfer, efficiency attributes and the thermo-structural management of the components. High intensity CO2 laser is used in combination with air flow through the test specimen to assess the effective heat transfer coefficient under heat flux conditions corresponding to high solar concentrations in the range of 1000-2000 suns.

14 SOLAR ENERGY↗

NASA NTRS1992

Intercomparison of eddy correlation carbon dioxide sensors during FIFE 1989

An intercomparison was made of the infrared gas analyzers used in the First ISLSCP Field Experiment (FIFE) 1989 to measure surface fluxes of carbon dioxide immediately following intensive field campaign 5. Fluxes of CO2 agreed to within 15 percent when all instruments are compared; when models of the same type of analyzer were compared, the agreement was within 5 percent. The stability of the calibration coefficients is examined, and it is shown that frequent calibration of the gas analyzers is required. Differences in the physical design of the analyzer models discussed here, such as sampling volume and sensitivity of the electronics to thermal drift, influence the precision of the flux estimates. Spectra and cospectra reveal the degree to which instrumental noise limits the complete sampling of all frequencies of eddies contributing to flux transport.

Moncrieff, J. B.↗

NASA NTRS1999

A Southern California Perspective of the April, 1998 Trans-Pacific Asian Dust Event

The Jet Propulsion Laboratory (JPL) coherent CO2 backscatter lidar has been in almost continuous operation since 1984 and has now accumulated a significant time-series database tracking the long-term and seasonal variability of backscatter from the atmospheric column above the Pasadena, Calif. locale. A particularly noteworthy episode observed by the lidar in 1998 was a particularly extreme instance of incursion by Asian-sourced dust during the closing days of April. Such events are not uncommon during the northern spring, when strong cold fronts and convection over the Asian interior deserts loft crustal material into the mid-troposphere whence it can be transported across the Pacific Ocean, occasionally reaching the continental US. However, the abnormal strength of the initiating storm in this case generated an atypically dense cloud of material which resulted in dramatically reduced visibility along the length of the Western Seaboard. These dust events are now recognized as a potentially significant, non-negligible radiative forcing influence. The progress of the April 1998 dust cloud eastward across the Pacific Ocean was initially observed in satellite imagery and transmitted to the broader atmospheric research community via electronic communications. The use of Internet technology in this way was effective in facilitating a rapid response correlative measurement exercise by numerous atmospheric observation stations throughout the western US and its success has resulted in the subsequent establishment of an ad hoc communications environment, data exchange medium, and mechanism for providing early-warning alert of other significant atmospheric phenomena in the future.

Tratt, David M.↗

NASA NTRS1995

Obliquity Experiments with a Mars General Circulation Model

We have simulated the seasonal variation of the general circulation on Mars for obliquities of 0deg and 60deg. These obliquities represent the minimum and maximum values the planet has experienced during the past 10(exp 7) years (e.g., Laskar and Robutel, 1993, Nature, 361, 608-614). The model we use is the NASA/Ames Mars General Circulation Model (Pollack et al., 1993, J. Geophys. Res. 98, 3149-3181). We vary only the obliquity; all other model parameters are as in Pollack et al. At high obliquity, the model shows dramatic seasonal variations in the polar caps and in the structure and intensity of the circulation. At the solstices the winter cap extends to the equator. Thus, surface temperatures throughout the entire winter hemisphere are fixed at the CO2 frost point. During summer surface temperatures at the poles reach 269K in the north and 295K in the south. The most notable changes to the circulation at solstice compared to our standard runs are a general weakening of the winter westerlies, a Hadley cell of greater latitudinal extent, and the development of very strong, possibly unstable, low-level jets in midlatitudes of the summer hemisphere. Surface stresses associated with these jets are sufficient to raise dust continuously. Thus, dust storms should be frequent features of the high obliquity climate. This result is independent of any desorbed regolith CO2 which would raise mean surface pressures. At zero obliquity the structure of the circulation resembles that of present day equinox conditions modulated by the varying insolation associated with orbital eccentricity. Notable features include equatorial superrotation, asymmetric Hadley cells, and stronger poleward heat fluxes in the northern hemisphere. Since the poles do not receive solar energy at any time of year, permanent caps form which extend to about 70deg in each hemisphere. However, the north permanent cap is growing at a rate 40% faster than the south cap. This is due to the differences in topography, albedo, emissivity, and heat transport in each hemisphere. Thus the zero obliquity climate system appears to be evolving toward a state in which the north cap is the dominant cap.

Harberle, R. M.↗

NASA NTRS2002

Chemistry and Transport In a Multi-Dimensional Model

The focus of the work funded under this proposal is the exchange between the stratosphere and the troposphere, and between the troposphere and the blaspheme. These two interfaces represent the frontiers of atmospheric chemistry. It is the combination of exchange processes at both interfaces that ultimately controls how the blaspheme (including human activities) affects the ozone layer. The modeling work was motivated by and attempts to integrate information obtained by aircraft, spacecraft, shuttle and oceanic measurements. The model development and research activities accomplished in the past three years provide a technical and intellectual basis for the research in this group. The innovative part of our research program is related to the IAV of ozone and the hydrological cycle. Other related but independently supported work include the study of isotopic fractionation of atmospheric species, e.g., N2O and CO2. Our theory suggests that we now have the ability to probe the middle atmosphere at a level of sensitivity where subtle details such as the isotopic composition of simple molecules can yield measurable systematic effects. This creates the possibility for probing the chemistry and dynamics of the middle atmosphere using all of the N2O and CO2 isotopologues. In the following we will briefly describe the model development and review the highlights of recent accomplishments.

Yung, Yuk L.↗

DOE OSTI2023

Organic Additive–derived Films on Cu Electrodes Promote Electrochemical CO 2 Reduction to C 2+ Products Under Strongly Acidic Conditions

Electrochemical CO 2 reduction (CO 2 R) at low pH is desired for high CO 2 utilization; the competing hydrogen evolution reaction (HER) remains a challenge. High alkali cation concentration at a high operating current density has recently been used to promote electrochemical CO 2 R at low pH. Herein we report an alternative approach to selective CO2R (>70 % Faradaic efficiency for C 2+ products, FE C2+ ) at low pH (pH 2; H 3 PO 4 /KH 2 PO 4 ) and low potassium concentration ([K + ]=0.1 M) using organic film-modified polycrystalline copper (Modified-Cu). Furthermore, such an electrode effectively mitigates HER due to attenuated proton transport. Modified-Cu still achieves high FE C2+ (45 % with Cu foil /55 % with Cu GDE) under 1.0 M H 3 PO 4 (pH≈1) at low [K + ] (0.1 M), even at low operating current, conditions where HER can otherwise dominate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Tuning Alkaline Anion Exchange Membranes through Crosslinking: A Review of Synthetic Strategies and Property Relationships

Alkaline anion exchange membranes (AAEMs) are an enabling component for next-generation electrochemical devices, including alkaline fuel cells, water and CO2 electrolyzers, and flow batteries. While commercial systems, notably fuel cells, have traditionally relied on proton-exchange membranes, hydroxide-ion conducting AAEMs hold promise as a method to reduce cost-per-device by enabling the use of non-platinum group electrodes and cell components. AAEMs have undergone significant material development over the past two decades; however, challenges remain in the areas of durability, water management, high temperature performance, and selectivity. In this review, we survey crosslinking as a tool capable of tuning AAEM properties. While crosslinking implementations vary, they generally result in reduced water uptake and increased transport selectivity and alkaline stability. We survey synthetic methodologies for incorporating crosslinks during AAEM fabrication and highlight necessary precautions for each approach.

08 HYDROGEN↗

NASA NTRS2023

Unraveling the Mechanisms and Implications of a Stronger Mid-Pliocene Atlantic Meridional Overturning Circulation (AMOC) in PlioMIP2

The mid-Pliocene warm period (3.264–3.025 Ma) is the most recent geological period in which the atmospheric CO2 concentration was approximately equal to the concentration we measure today (ca. 400 ppm). Sea surface temperature (SST) proxies indicate above-average warming over the North Atlantic in the mid-Pliocene with respect to the pre-industrial period, which may be linked to an intensified Atlantic Meridional Overturning Circulation (AMOC). Earlier results from the Pliocene Model Intercomparison Project Phase 2 (PlioMIP2) show that the ensemble simulates a stronger AMOC in the mid-Pliocene than in the pre-industrial. However, no consistent relationship between the stronger mid-Pliocene AMOC and either the Atlantic northward ocean heat transport (OHT) or average North Atlantic SSTs has been found. In this study, we look further into the drivers and consequences of a stronger AMOC in mid-Pliocene compared to pre-industrial simulations in PlioMIP2. We find that all model simulations with a closed Bering Strait and Canadian Archipelago show reduced freshwater transport from the Arctic Ocean into the North Atlantic. This contributes to an increase in salinity in the subpolar North Atlantic and Labrador Sea that can be linked to the stronger AMOC in the mid-Pliocene. To investigate the dynamics behind the ensemble's variable response of the total Atlantic OHT to the stronger AMOC, we separate the Atlantic OHT into two components associated with either the overturning circulation or the wind-driven gyre circulation. While the ensemble mean of the overturning component is increased significantly in magnitude in the mid-Pliocene, it is partly compensated by a reduction in the gyre component in the northern subtropical gyre region. This indicates that the lack of relationship between the total OHT and AMOC is due to changes in OHT by the subtropical gyre. The overturning and gyre components should therefore be considered separately to gain a more complete understanding of the OHT response to a stronger mid-Pliocene AMOC. In addition, we show that the AMOC exerts a stronger influence on North Atlantic SSTs in the mid-Pliocene than in the pre-industrial, providing a possible explanation for the improved agreement of the PlioMIP2 ensemble mean SSTs with reconstructions in the North Atlantic.

AMOC↗

NASA NTRS1987

The doubled CO2 climate - Impact of the sea surface temperature gradient

The Goddard Institute for Space Studies (GISS) GCM of Hansen et al. (1983) was run, with 4 deg x 5 deg resolution, with doubled CO2 and two sets of sea surface temperature gradient distributions. One set was derived from the equilibrium doubled CO2 run of the 8 deg x 10 deg GISS GCM, with minimal high latitude amplification. The other set resembled closely the GFDL model results, with greater amplification. Both experiments had the same global mean surface air temperature change. The two experiments were often found to produce substantially different climate characteristics. With reduced high latitude amplification (set one), and thus, more equatorial warming, there was a greater increase in specific humidity and the greenhouse capacity of the atmosphere, resulting in a warmer atmosphere in general. Features such as the low-latitude precipitation, Hadley cell intensity, jet stream magnitude, and atmospheric energy transports all increased in comparison with the control run. In contrast, these features all decreased in the experiment with greater high latitude amplification (set two).

Rind, David↗

DOE OSTI2025

Hestia-SWIFL: hourly anthropogenic fossil fuel CO2 and heat on the 2km WRF grid, version 1.1

The Hestia-SWIFL version 1.1 anthropogenic heat (AH) and fossil fuel CO2 (FFCO2) emissions data product represent emissions due to the combustion of fossil fuel and cement production within the state of Arizona from 2019 to 2022. This product was developed as part of the Southwest Urban Corridor Integrated Field Laboratory (SW-IFL) project, which aims to provide new knowledge and tools that address extreme heat, air quality, climate change and related urban environmental issues by integrating high-resolution observations, modeling, and civic engagement. The emissions are generated using a bottom-up/engineering approach and are tied to results generated by the Vulcan Project version 4, an effort to quantify space/time-resolved FFCO2 & AH emissions for the entire United States landscape. A large number of data sources are combined to best estimate the emissions at fine scales such as air quality emissions data, traffic flow data, building information, sociodemographic information, and fuel statistics. The AH product provides emissions for two emissions sources (transportation and point source emissions) in units of Watts per hour per square meter (W/m2) per year (annual files) or per hour (hourly files). The FFCO2 product provides emissions from nine individual emission sectors as well as the total, and in units of tons of carbon (tC) per grid cell per year or per hour. The output made available here places the native spatial resolution of the Hestia FFCO2 & AH emissions data product (points, lines, and polygons) into a regularized 2km x 2km grid at hourly and annual temporal resolutions, and stored in netCDF files. The exact spatial extent is defined by the ASU Weather Research Forecast (WRF) simulation grid. All data are processed using R/Python pm high-performance computing system. 2-27-2026 updates: Bugs in airport hourly profile (both AH and FFCO2) and building spatial patterns (FFCO2 only) were fixed. Hourly emissions are reprocessed for all years to reflect those changes.

54 ENVIRONMENTAL SCIENCES↗