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

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At least 55 records · Page 3

Three Decades of Global Methane Sources and Sinks

Methane is an important greenhouse gas, responsible for about 20 of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios which differ in fossil fuel and microbial emissions to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.

periodic variations↗

Formation of Complex Organic Molecules (COMs) from Polycyclic Aromatic Hydrocarbons (PAHs): Top-Down Synthesis of organics in planetary systems

Complex, organic molecules have been found in many solar system objects (i.e., dust, comets, meteorites, moons, etc.); however, their origins and formation remain a mystery. Two chemical evolutionary pathways have been proposed to explain the organic inventory of our solar system. The first pathway, the top-down approach, suggests an interstellar (ISM) heritage whereby the organic material found in the solar system formed from the erosion and functionalization of large pre-solar carbon-bearing species (mainly large Polycyclic Aromatic Hydrocarbons or PAHs). The second pathway suggests that the origin of the Solar System prebiotic matter is the result of bottom-up synthesis from small reactive molecules (e.g., formaldehyde – H2CO, acetylene – H2C2, and similar species). In this second scenario, it is supposed that very few, if any, pre-solar large molecules could have survived due to the proto - solar nebula radiation environment. Polycyclic Aromatic Hydrocarbons or PAHs comprise ~20-30% of all available carbon in the Universe. The PAHs found within our Solar System tend to be smaller than those suspected to be in the ISM, comprised of only 14 to 18 carbon atoms in size whereas ISM PAHs are typically 50 to 100 carbon atoms. The disparity in PAH sizes between the ISM and Solar System environments is not understood, but may point to conversion of large ISM PAHs to Solar System Organics. This presentation details recent experiments regarding the stability of large PAHs to the various types of radiation found within a proto - solar disk and the production of smaller, complex, molecules from the degradation of the larger PAHs. The presentation will highlight differences and similarities in degradation products based on experimental conditions (e.g., radiation type) and discuss future work with a new experimental setup known as ICEE (Institute for Carbon Evolution Experiments).

molecukes↗

Cosmochemical trends of volatile elements in the solar system

Chemical interactions between gases and grains in the solar nebula played a central role in establishing the presently observed volatile element inventories of the planets, their satellites, and the other bodies in the solar system. Kinetic constraints relevant to gas-grain chemical interactions in the solar nebula are reviewed. The abundant, chemically active volatiles H, O, C, N, and S are emphasized; however, less abundant volatiles such as P, Cl, and F are discussed where appropriate.

Fegley, Bruce, Jr.↗

Model Evaluation of Methods for Estimating Surface Emissions and Chemical Lifetimes from Satellite Data

Column densities from satellite retrievals can provide valuable information for estimating emissions and chemical lifetimes objectively across the globe. To better understand the uncertainties associated with these estimates, we test four methods using simulated column densities from a point source: a box model approach, a 2D Gaussian fit, an Inverse Radius fit and an Exponentially-Modified Gaussian fit. The model results were simulated using the WRF and CAMx models for the year 2005, for a single point source outside Atlanta in Georgia, USA with specified emissions and three chemical scenarios: no chemical reactions, 12 h chemical lifetime and 1 h chemical lifetime. No other sources were included in the simulations. We find that the box model provides reliable estimates irrespective of plume speed and plume direction, if the plume speed and the chemical lifetime are known accurately. The 2D Gaussian fit was found to be sensitive to plume speed and direction, and requires omnidirectional dispersion in order to have a decent fit. However, the 2D Gaussian fit is only an approximate fit to the data, and the discrepancies mean that the results are dependent on the geographical domain used for the optimization. An Inverse Radius fit is introduced to correct this issue, which is found to provide improved emissions and lifetime estimates. The Exponentially-Modified Gaussian fit also gave improved estimates. It is however dependent on accurate plume rotation such that reported chemical lifetimes with this method could be significantly underestimated.

Emission inventory↗

Dust Spectroscopy and the Nature of Grains

Ground-based, air-borne and space-based, infrared spectra of a wide variety of objects have revealed prominent absorption and emission features due to large molecules and small dust grains. Analysis of this data reveals a highly diverse interstellar and circumstellar grain inventory, including both amorphous materials and highly crystalline compounds (silicates and carbon). This diversity points towards a wide range of physical and chemical birthsites as well as a complex processing of these grains in the interstellar medium. In this talk, I will review the dust inventory contrasting and comparing both the interstellar and circumstellar reservoirs. The focus will be on the processes that play a role in the lifecycle of dust in the interstellar medium.

Tielens, A. G. G. M.↗

Evaluating Global Emission Inventories of Biogenic Bromocarbons

Emissions of halogenated very short-lived substances (VSLS) are poorly constrained. However, their inclusion in global models is required to simulate a realistic inorganic bromine (Bry) loading in both the troposphere, where bromine chemistry perturbs global oxidizing capacity, and in the stratosphere, where it is a major sink for ozone (O3). We have performed simulations using a 3-D chemical transport model (CTM) including three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform (CHBr3) and dibromomethane (CH2Br2). We perform the first concerted evaluation of these inventories, comparing both the magnitude and spatial distribution of emissions. For a quantitative evaluation of each inventory, model output is compared with independent long-term observations at National Oceanic and Atmospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF (National Science Foundation) HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 (38 %) to 0.78 (115 %) parts per trillion (ppt) in the tropics, depending on emission inventory. For CH2Br2, the range is 0.17 (24 %) to 1.25 (167 %) ppt. We also use aircraft observations made during the 2011 Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere (SHIVA) campaign, in the tropical western Pacific. Here, the performance of the various inventories also varies significantly, but overall the CTM is able to reproduce observed CHBr3 well in the free troposphere using an inventory based on observed sea-to-air fluxes. Finally, we identify the range of uncertainty associated with these VSLS emission inventories on stratospheric bromine loading due to VSLS (Br(VSLS/y)). Our simulations show Br(VSLS/y) ranges from approximately 4.0 to 8.0 ppt depending on the inventory. We report an optimized estimate at the lower end of this range (approximately 4 ppt) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.

bromocarbons↗

Database for Safety-Oriented Tracking of Chemicals

SafetyChem is a computer program that maintains a relational database for tracking chemicals and associated hazards at Johnson Space Center (JSC) by use of a Web-based graphical user interface. The SafetyChem database is accessible to authorized users via a JSC intranet. All new chemicals pass through a safety office, where information on hazards, required personal protective equipment (PPE), fire-protection warnings, and target organ effects (TOEs) is extracted from material safety data sheets (MSDSs) and recorded in the database. The database facilitates real-time management of inventory with attention to such issues as stability, shelf life, reduction of waste through transfer of unused chemicals to laboratories that need them, quantification of chemical wastes, and identification of chemicals for which disposal is required. Upon searching the database for a chemical, the user receives information on physical properties of the chemical, hazard warnings, required PPE, a link to the MSDS, and references to the applicable International Standards Organization (ISO) 9000 standard work instructions and the applicable job hazard analysis. Also, to reduce the labor hours needed to comply with reporting requirements of the Occupational Safety and Health Administration, the data can be directly exported into the JSC hazardous- materials database.

Stump, Jacob↗

Processing and Synthesis of Pre-Biotic Chemicals in Hypervelocity Impacts

Hypervelocity impacts (HVIs) may have played a significant role in establishing the initial organic inventory for pre-biotic chemistry on the Earth and other planetary bodies. In addition to the delivery of organic compounds intact to planetary surfaces, generally at velocities below approx.20 km/s, HVIs also enable synthesis of new molecules. The cooling post-impact plasma plumes of HVIs in the interstellar medium (ISM), the protosolar nebula (PSN), and the early solar system comprise pervasive conditions for organic synthesis. Such plasma synthesis (PS) can operate over many length scales (from nm-scale dust to planets) and energy scales (from molecular rearrangement to atomization and recondensation). HVI experiments with the flexibility to probe the highest velocities and distinguish synthetic routes are a high priority to understand the relevance of PS to exobiology. We describe here recent studies of PS at small spatial scales and extremely high velocities with pulsed laser ablation (PLA). PLA can simulate the extreme plasma conditions generated in impacts of dust particles at speeds of up to 100 km/s or more. When applied to carbonaceous solids, new and pre-biotically relevant molecular species are formed with high efficiency [1,2].

Brickerhoff, W. B.↗

Interstellar Precursors of Meteoritic Organics

The organic inventory initially available to protostellar disks is the first step on the long chemical path to the development of Life. The early earth may have obtained most its volatile material from the arrival of meteorites and comets at its surface. Determining the most likely distribution of meteoritic and cometary organic molecules that could seed primitive planets is a major goal since it sets the initial conditions for, at least part of, the phase of prebiotic chemical evolution. Observations and measurements of the chemical composition of primitive Solar System organics, and of dense molecular clouds, should allow the construction of coherent theoretical picture of the development of organic complexity from interstellar biogenic material to the beginning of prebiotic evolution.

Charnley, S. B.↗

How emissions uncertainty influences the distribution and radiative impacts of smoke from fires in North America

Fires and the aerosols that they emit impact air quality, health, and climate, but the abundance and properties of carbonaceous aerosol (both black carbon and organic carbon) from biomass burning (BB) remain uncertain and poorly constrained. We aim to explore the uncertainties associated with fire emissions and their air quality and radiative impacts from underlying dry matter consumed and emissions factors. To investigate this, we compare model simulations from a global chemical transport model, GEOS-Chem, driven by a variety of fire emission inventories with surface and airborne observations of black carbon (BC) and organic aerosol (OA) concentrations and satellite-derived aerosol optical depth (AOD). We focus on two fire-detection-based and/or burned-area-based (FD-BA) inventories using burned area and active fire counts, respectively, i.e., the Global Fire Emissions Database version 4 (GFED4s) with small fires and the Fire INventory from NCAR version 1.5 (FINN1.5), and two fire radiative power (FRP)-based approaches, i.e., the Quick Fire Emission Dataset version 2.4 (QFED2.4) and the Global Fire Assimilation System version 1.2 (GFAS1.2). We show that, across the inventories, emissions of BB aerosol (BBA) differ by a factor of 4 to 7 over North America and that dry matter differences, not emissions factors, drive this spread. We find that simulations driven by QFED2.4 generally overestimate BC and, to a lesser extent, OA concentrations observations from two fire-influenced aircraft campaigns in North America (ARCTAS and DC3) and from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, while simulations driven by FINN1.5 substantially underestimate concentrations. The GFED4s and GFAS1.2-driven simulations provide the best agreement with OA and BC mass concentrations at the surface (IMPROVE), BC observed aloft (DC3 and ARCTAS), and AOD observed by MODIS over North America. We also show that a sensitivity simulation including an enhanced source of secondary organic aerosol (SOA) from fires, based on the NOAA Fire Lab 2016 experiments, produces substantial additional OA; however, the spread in the primary emissions estimates implies that this magnitude of SOA can be neither confirmed nor ruled out when comparing the simulations against the observations explored here. Given the substantial uncertainty in fire emissions, as represented by these four emission inventories, we find a sizeable range in 2012 annual BBA PM2.5 population-weighted exposure over Canada and the contiguous US (0.5 to 1.6 µg/cu. m). We also show that the range in the estimated global direct radiative effect of carbonaceous aerosol from fires (−0.11 to −0.048 W/sq. m) is large and comparable to the direct radiative forcing of OA (−0.09 W/sq. m) estimated in the Fifth Assessment Report (AR5) of the Intergovernmental Panel on Climate Change (IPCC). Our analysis suggests that fire emissions uncertainty challenges our ability to accurately characterize the impact of smoke on air quality and climate.

North America↗

Self assembly properties of primitive organic compounds

A central event in the origin of life was the self-assembly of amphiphilic, lipid-like compounds into closed microenvironments. If a primitive macromolecular replicating system could be encapsulated within a vesicular membrane, the components of the system would share the same microenvironment, and the result would be a step toward true cellular function. The goal of our research has been to determine what amphiphilic molecules might plausibly have been available on the early Earth to participate in the formation of such boundary structures. To this end, we have investigated primitive organic mixtures present in carbonaceous meteorites such as the Murchison meteorite, which contains 1-2 percent of its mass in the form of organic carbon compounds. It is likely that such compounds contributed to the inventory of organic carbon on the prebiotic earth, and were available to participate in chemical evolution leading to the emergence of the first cellular life forms. We found that Murchison components extracted into non-polar solvent systems are surface active, a clear indication of amphiphilic character. One acidic fraction self-assembles into vesicular membranes that provide permeability barriers to polar solutes. Other evidence indicates that the membranes are bimolecular layers similar to those formed by contemporary membrane lipids. We conclude that bilayer membrane formation by primitive amphiphiles on the early Earth is feasible. However, only a minor fraction of acidic amphiphiles assembles into bilayers, and the resulting membranes require narrowly defined conditions of pH and ionic composition to be stable. It seems unlikely, therefore, that meteoritic infall was a direct source of membrane amphiphiles. Instead, the hydrocarbon components and their derivatives more probably would provide an organic stock available for chemical evolution. Our current research is directed at possible reactions which would generate substantial quantities of membranogenic amphiphiles. One possibility is photochemical oxidation of hydrocarbons.

Deamer, D. W.↗

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite NO2 Data Assimilation and Improvements in Background NOx Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

V. Shah↗

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite Data Assimilation and Improvements in Background NO x Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NO x =NO+NO 2 ) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO 2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

Viral Shah↗

Planetary atmospheres program

Chemical and physical models of the Jovian subnebula are addressed. Halide cloud condensation and volatile element inventories on Venus and considered. Computation methods for isolated grain condensation behavior are examined.

Source record↗

Parameterization of Aerosol Sinks in Chemical Transport Models

The modelers point of view is that the aerosol problem is one of sources, evolution, and sinks. Relative to evolution and sink processes, enormous attention is given to the problem of aerosols sources, whether inventory based (e.g., fossil fuel emissions) or dynamic (e.g., dust, sea salt, biomass burning). On the other hand, aerosol losses in models are a major factor in controlling the aerosol distribution and lifetime. Here we shine some light on how aerosol sinks are treated in modern chemical transport models. We discuss the mechanisms of dry and wet loss processes and the parameterizations for those processes in a single model (GEOS-5). We survey the literature of other modeling studies. We additionally compare the budgets of aerosol losses in several of the ICAP models.

Colarco, Peter↗

Volatiles in the Martian regolith

An inventory of released volatiles on Mars has been derived based upon Viking measurements of atmospheric and surface chemical composition, and upon the inferred mineralogy of a ubiquitous regolith, assumed to average 200m in depth. This model is consistent with the relative abundances of volatiles (except for S) on the earth's surface, but implies one-fifteenth of the volatile release of earth if starting materials were comparable. All constituents are accommodated as chemical components of, or absorbed phases on, regolith materials - without the necessity of invoking unobservable deposits of carbonates, nitrates, or permafrost ice.

Clark, B. C.↗

Discovery of Presolar Corundum (and SiC?) in an Interplanetary Dust Particle

This work is part of an ongoing investigation [1-3] of isotopically anomalous phases in interplanetary dust particles (IDPs) on a scale of 100 nm. Previously, such NanoSIMS studies have found sub-micrometer sized, isotopically distinct presolar grains in IDPs at higher abundances than in primitive meteorites [1-5], which demonstrates the unique and primitive nature of IDPs. Although not all presolar grains found so far in IDPs have been chemically or petrographically characterized, the majority appear to be silicate stardust. Conspicuously absent from the presolar grain inventory in IDPs have been other grain types, which are commonly found in primitive meteorites, such as SiC and corundum (Al2O3).

Stadermann, F. J.↗

Monitoring and Testing the Parts Cleaning Stations, Abrasive Blasting Cabinets, and Paint Booths

I have the opportunity to work in the Environmental Management Office (EMO) this summer. One of the EMO's tasks is to make sure the Environmental Management System is implemented to the entire Glenn Research Center (GRC). The Environmental Management System (EMS) is a policy or plan that is oriented toward minimizing an organization's impact to the environment. Our EMS includes the reduction of solid waste regeneration and the reduction of hazardous material use, waste, and pollution. With the Waste Management Team's (WMT) help, the EMS can be implemented throughout the NASA Glenn Research Center. The WMT is responsible for the disposal and managing of waste throughout the GRC. They are also responsible for the management of all chemical waste in the facility. My responsibility is to support the waste management team by performing an inventory on parts cleaning stations, abrasive cabinets, and paint booths through out the entire facility. These booths/stations are used throughout the center and they need to be monitored and tested for hazardous waste and material. My job is to visit each of these booths/stations, take samples of the waste, and analyze the samples.

Jordan, Tracee M.↗