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NASA NTRS2005

Lightning NO(x) Production and Its Consequences for Tropospheric Chemistry

Cloud-resolving case-study simulations of convective transport and lightning NO production have yielded results which are directly applicable to the design of lightning parameterizations for global chemical transport models. In this work we have used cloud-resolving models (the Goddard Cumulus Ensemble Model (GCE) and MMS) to drive an off-line cloud-scale chemical transport model (CSCTM). The CSCTM, in conjunction with aircraft measurements of NO(x) in thunderstorms and ground-based lightning observations, has been used to constrain the amount of NO produced per flash. Cloud and chemistry simulations for several case studies of storms in different environments will be presented. Observed lightning flash rates have been incorporated into the CSCTM, and several scenarios of NO production per intracloud (IC) and per cloud-to-ground (CG) flash have been tested for each storm. The resulting NO(x) mixing ratios are compared with aircraft measurements taken within the storm (typically the anvil region) to determine the most likely NO production scenario. The range of values of NO production per flash (or per meter of lightning channel length) that have been deduced from the model will be shown and compared with values of production in the literature that have been deduced from observed NO spikes and from anvil flux calculations. Results show that on a per flash basis, IC flashes are nearly as productive of NO as CG flashes. This result simplifies the lightning parameterization for global models (ie., an algorithm for estimating the ICKG ratio is not necessary). Vertical profiles of lightning NOx mass at the end of the 3-D storm simulations have been summarized to yield suggested profiles for use in global models. Estimates of mean NO production per flash vary by a factor of three from one simulated storm to another. When combined with the global flash rate of 44 flashes per second from NASA's Optical Transient Detector (OTD) measurements, these estimates and the results from other techniques yield global NO production rates of 2-9 TgN/year. Simulations of the photochemistry over the 24 hours following a storm has been performed to determine the additional ozone production which can be attributed to lightning NO. Convective transport of HO(x), precursors leads to the generation of a HO(x), plume which substantially aids the downstream ozone production.

Pickering, Kenneth E.↗
NASA NTRS2006

Improving Lightning NO(x) Parameterizations for Global Chemical Transport Models

Parameterization of lightning NO(x) in global chemical transport models requires a method to specify the temporal and geographic distribution of flash rates, an estimate of NO production per flash, and a method to specify the effective vertical distribution of NO production. Flash rate parameterizations using the upward convective cloud mass flux have been developed and tested for several GCM and assimilated meteorological data sets. This parameterization and others involving the cloud-top height and convective precipitation provide a generally acceptable climatological distribution of flashes after normalization with satellite data. However, considerable improvement in terms of geographic and temporal variability may be achieved in the future using cloud microphysics data available from next-generation GCMs. Cloud-resolving case-study simulations of convective transport and lightning NO production have yielded results which are directly applicable to the NO production per flash and the vertical NO distribution portions of the global model lightning parameterizations. In this work we have used cloud-resolving models (the Goddard Cumulus Ensemble Model (GCE) and MM5) to drive an off-line cloud-scale chemical transport model (CSCTM). The CSCTM, in conjunction with aircraft measurements of NO(x) in thunderstorms and ground-based lightning observations, has been used to constrain the amount of NO produced per flash. Observed lightning flash rates have been incorporated into the CSCTM, and several scenarios of NO production per intracloud (IC) and per cloud-to-ground (CG) flash have been tested in each of several case study storms. The resulting NO(x) mixing ratios are compared with aircraft measurements taken within the storm (typically the anvil region) to determine the most likely NO production scenario. The range of values of NO production per flash (or per meter of lightning channel length) that have been deduced from the model will be shown and compared with values of production in the literature that have been deduced from observed NO spikes and from anvil flux calculations. Results show that on a per flash basis, IC flashes are nearly as productive of NO as CG flashes. Estimates of mean NO production per flash vary by a factor of three from one simulated storm to another. Vertical profiles of lightning NOx mass at the end of the 3-D storm simulations have been summarized to yield suggested profiles for use in global models. These profiles show a larger percentage of the total lightning NO(x) mass in the free troposphere than those suggested by Pickering et al. (1998).

Pickering, Kenneth E.↗
NASA NTRS1995

Non-Thermal Removal of Gaseous Pollutants

The removal of fluorine based exhaust gases such as CFC's, PFC's, NF3, and SF6 used for plasma etching of and deposition on semi-conductors is a subject of increasing interest because of safety, air pollution, and global warming issues. Conventional treatment methods for removing exhaust gas pollutants are wet scrubbing, carbon and resin adsorption, catalytic oxidation, and thermal incineration. However, there are drawbacks associated with each of these methods which include difficulties in implementation, problems with the disposal of solid and liquid pollutant waste, large water and fuel consumption, and additional pollutants such as NOx emissions which are generated in thermal incineration processes.

exhaust gases↗
NASA NTRS2007

An Assessment of NASA Aeropropulsion Technologies: A System Study

Aviation industry s robust growth rate has given rise to growing concerns about the contribution that aviation emissions will make to local air quality and global climate change. Over the last several years, NASA has been engaged in the development of aeropropulsion technologies with specific objectives to reduce aircraft emissions. A system analysis was performed to evaluate the potential impact of these propulsion technologies on aircraft CO2 (directly proportional to fuel burn) and NOx reductions. A large subsonic aircraft, with two 396-kN thrust (85,000-pound) engines was chosen for the study. Performance benefit estimates are presented for each technology, with a summary of potential emissions reduction possible from the development of these technologies. The results show that NASA s aeropropulsion technologies have the potential to significantly reduce the CO2 and NO(x) emissions. The results are used to support informed decision-making on the development of aeropropulsion technology portfolio for CO2 and NO(x) reductions.

Tong, Michael T.↗
NASA NTRS2004

Activities of NASA's Global Modeling Initiative (GMI) in the Assessment of Subsonic Aircraft Impact

The Intergovernmental Panel on Climate Change estimated a peak increase in ozone ranging from 7-12 ppbv (zonal and annual average, and relative to a baseline with no aircraft), due to the subsonic aircraft in the year 2015, corresponding to aircraft emissions of 1.3 TgN/year. This range of values presumably reflects differences in model input (e.g., chemical mechanism, ground emission fluxes, and meteorological fields), and algorithms. The model implemented by the Global Modeling Initiative allows testing the impact of individual model components on the assessment calculations. We present results of the impact of doubling the 1995 aircraft emissions of NOx, corresponding to an extra 0.56 TgN/year, utilizing meteorological data from NASA's Data Assimilation Office (DAO), the Goddard Institute for Space Studies (GISS), and the Middle Atmosphere Community Climate Model, version 3 (MACCM3). Comparison of results to observations can be used to assess the model performance. Peak ozone perturbations ranging from 1.7 to 2.2 ppbv of ozone are calculated using the different fields. These correspond to increases in total tropospheric ozone ranging from 3.3 to 4.1 Tg/Os. These perturbations are consistent with the IPCC results, due to the difference in aircraft emissions. However, the range of values calculated is much smaller than in IPCC.

Rodriquez, J. M.↗
NASA NTRS2007

Land Surface Process and Air Quality Research and Applications at MSFC

This viewgraph presentation provides an overview of land surface process and air quality research at MSFC including atmospheric modeling and ongoing research whose objective is to undertake a comprehensive spatiotemporal analysis of the effects of accurate land surface characterization on atmospheric modeling results, and public health applications. Land use maps as well as 10 meter air temperature, surface wind, PBL mean difference heights, NOx, ozone, and O3+NO2 plots as well as spatial growth model outputs are included. Emissions and general air quality modeling are also discussed.

Quattrochi, Dale↗
NASA NTRS2007

An Overview of Snow Photochemistry: Evidence, Mechanisms and Impacts

It has been shown that sunlit snow and ice plays an important role in processing atmospheric species. Photochemical production of a variety of chemicals has recently been reported to occur in snow/ice and the release of these photochemically generated species may significantly impact the chemistry of the overlying atmosphere. Nitrogen oxide and oxidant precursor fluxes have been measured in a number of snow covered environments, where in some cases the emissions significantly impact the overlying boundary layer. For example, photochemical ozone production (such as that occurring in polluted mid-latitudes) of 3-4 ppbv/day has been observed at South Pole, due to high OH and NO levels present in a relatively small boundary layer. Field and laboratory experiments have determined that the origin of the observed NOx flux is the photochemistry of nitrate within the snowpack, however some details of the mechanism have not yet been elucidated. A variety of low molecular weight organic compounds have been shown to be emitted from sunlit snowpacks, the source of which has been proposed to be either direct or indirect photo-oxidation of natural organic materials present in the snow. Although myriad studies have observed active processing of species within irradiated snowpacks, the fundamental chemistry occurring remains poorly understood. Here we consider the nature of snow at a fundamental, physical level; photochemical processes within snow and the caveats needed for comparison to atmospheric photochemistry; our current understanding of nitrogen, oxidant, halogen and organic photochemistry within snow; the current limitations faced by the field and implications for the future.

Grannas, A. M.↗
NASA NTRS1994

Micro-grooved heat transfer combustor wall

A gas turbine engine hot section combustor liner is provided a non-film cooled portion of a heat transfer wall having a hot surface and a plurality of longitudinally extending micro-grooves disposed in the portion of the wall along the hot surface in a direction parallel to the direction of the hot gas flow. The depth of the micro-grooves is very small and on the order of magnitude of a predetermined laminar sublayer of a turbulent boundary layer. The micro-grooves are sized so as to inhibit heat transfer from the hot gas flow to the hot surface of the wall while reducing NOx emissions of the combustor relative to an otherwise similar combustor having a liner wall portion including film cooling apertures. In one embodiment the micro-grooves are about 0.001 inches deep and have a preferred depth range of from about 0.001 inches to 0.005 inches and which are square, rectangular, or triangular in cross-section and the micro-grooves are spaced about one width apart.

Ward, Steven D.↗
NASA NTRS2007

NASA 9-Point LDI Code Validation Experiment

This presentation highlights the experimental work to date to obtain validation data using a 9-point lean direct injector (LDI) in support of the National Combustion Code. The LDI is designed to supply fuel lean, Jet-A and air directly into the combustor such that the liquid fuel atomizes and mixes rapidly to produce short flame zones and produce low levels of oxides of nitrogen and CO. We present NOx and CO emission results from gas sample data that support that aspect of the design concept. We describe this injector and show high speed movies of selected operating points. We present image-based species maps of OH, fuel, CH and NO obtained using planar laser induced fluorescence and chemiluminescence. We also present preliminary 2-component, axial and vertical, velocity vectors of the air flow obtained using particle image velocimetry and of the fuel drops in a combusting case. For the same combusting case, we show preliminary 3-component velocity vectors obtained using a phase Doppler anemometer. For the fueled, combusting cases especially, we found optical density is a technical concern that must be addressed, but that in general, these preliminary results are promising. All optical-based results confirm that this injector produces short flames, typically on the order of 5- to-7-mm long at typical cruise and high power engine cycle conditions.

Hicks, Yolanda R.↗
NASA NTRS2007

Fabrication and Characterization of Diffusion Bonds for Silicon Carbide

Diffusion bonds of silicon carbide (SiC) were fabricated using several different types of titanium (Ti) based interlayers between the SiC substrates. The interlayers were an alloyed Ti foil, a pure Ti foil, and a physically vapor deposited (PVD) Ti coating. Microscopy was conducted to evaluate the cross-sections of the resulting bonds. Microprobe analysis identified reaction formed phases in the diffusion bonded region. Uniform and well adhered bonds were formed between the SiC substrates. In the case where the alloyed Ti foil or a thick Ti coating (i.e. 20 micron) was used as the interlayer, microcracks and several phases were present in the diffusion bonds. When a thinner interlayer was used (i.e. 10 micron PVD Ti), no microcracks were observed and only two reaction formed phases were present. The two phases were preferred and fully reacted phases that did not introduce thermal stresses or microcracks during the cool-down stage after processing. Diffusion bonded samples were evaluated with the non-destructive evaluation (NDE) methods of pulsed thermography and immersion ultrasonic testing. Joined SiC substrates that were fully bonded and that had simulated bond flaws in the interlayer were also evaluated using immersion ultrasound. Pull testing was conducted on the bonds to determine the tensile strength. To demonstrate the joining approach for a complex multilayered component for a low NOx injector application, the diffusion bonding approach was used to join three 4" diameter SiC discs that contained complex fuel and air flow channels.

Halbig, Michael↗
NASA NTRS2007

Nitric Acid Particles in Cold Thick Ice Clouds Observed at Global Scale: Link with Lightning, Temperature, and Upper Tropospheric Water Vapor

Signatures of nitric acid particles (NAP) in cold thick ice clouds have been derived from satellite observations. Most NAP are detected in the Tropics (9 to 20% of clouds with T less than 202.5 K). Higher occurrences were found in the rare mid-latitudes very cold clouds. NAP occurrence increases as cloud temperature decreases and NAP are more numerous in January than July. Comparisons of NAP and lightning distributions show that lightning is the main source of the NOx, which forms NAP in cold clouds. Qualitative comparisons of NAP with upper tropospheric humidity distributions suggest that NAP play a role in the dehydration of the upper troposphere when the tropopause is colder than 195K.

Chepfer, H.↗
NASA NTRS2007

Chemical Data Assimilation Estimates of Continental US Ozone and Nitrogen Budgets during INTEX-A

Global ozone analyses, based on assimilation of stratospheric profile and ozone column measurements, and NOy predictions from the Real-time Air Quality Modeling System (RAQMS) are used to estimate the ozone and NOy budget over the Continental US during the July-August 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A). Comparison with aircraft, satellite, surface, and ozonesonde measurements collected during the INTEX-A show that RAQMS captures the main features of the global and Continental US distribution of tropospheric ozone, carbon monoxide, and NOy with reasonable fidelity. Assimilation of stratospheric profile and column ozone measurements is shown to have a positive impact on the RAQMS upper tropospheric/lower stratosphere ozone analyses, particularly during the period when SAGE III limb scattering measurements were available. Eulerian ozone and NOy budgets during INTEX-A show that the majority of the Continental US export occurs in the upper troposphere/lower stratosphere poleward of the tropopause break, a consequence of convergence of tropospheric and stratospheric air in this region. Continental US photochemically produced ozone was found to be a minor component of the total ozone export, which was dominated by stratospheric ozone during INTEX-A. The unusually low photochemical ozone export is attributed to anomalously cold surface temperatures during the latter half of the INTEX-A mission, which resulted in net ozone loss during the first 2 weeks of August. Eulerian NOy budgets are shown to be very consistent with previously published estimates. The NOy export efficiency was estimated to be 24 percent, with NOx+PAN accounting for 54 percent of the total NOy export during INTEX-A.

Pierce, Robert B.↗
NASA NTRS2007

Reactive Nitrogen Distribution and Partitioning in the North American Troposphere and Lowermost Stratosphere

A comprehensive group of reactive nitrogen species (NO, NO2, HNO3, HO2NO2, PANs, alkyl nitrates, and aerosol-NO3) were measured in the troposphere and lowermost stratosphere over North America and the Atlantic during July/August 2004 (INTEX-A) from the NASA DC-8 platform (0.1-12 km). Less reactive nitrogen species (HCN and CH3CN), that are also unique tracers of biomass combustion, were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, and stratosphere was sampled both over continental U. S., Atlantic and Pacific. The North American upper troposphere was found to be greatly influenced by both lightning NO(x) and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO(x). Under polluted conditions PAN was a dominant carrier of reactive nitrogen in the upper troposphere while nitric acid dominated in the lower troposphere. Peroxynitric acid (HO2NO2) was present in sizable concentrations always peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the lower troposphere. Plumes from Alaskan fires contained large amounts of PAN and very little enhancement in ozone. Observational data suggest that lightning was a far greater contributor to NO(x) in the upper troposphere than previously believed. NO(x) and NO(y) reservoir appeared to be in steady state only in the middle troposphere where NO(x)/NO(y) was independent of air mass age. A first comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. These uncertainties likely propagate themselves in satellites derived NOx data. Observed data are interpreted to suggest that soil sinks of HCN/CH3CN are at best very small. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.

Singh, H. B.↗
NASA NTRS2006

Workshop on the Impacts of Aviation on Climate Change

Projections indicate that demand for aviation transportation will increase by more than two fold over the next few decades. Timely action is needed to understand and quantify the potential climate impacts of aviation emissions particularly given the sustained lapse over the last several years in U.S. research activities in this area. In response to the stated needs, a group of international experts participated in the Workshop on the Impacts of Aviation on Climate Change during June 7-9, 2006 in Boston, MA. The workshop focus was on the impacts of subsonic aircraft emissions in the UT/LS region and on the potential response of the climate system. The goals of the workshop were to assess and document the present state of scientific knowledge, to identify the key underlying uncertainties and gaps, to identify ongoing and further research needed, to explore the development of climate impact metrics, and to help focus the scientific community on the aviation-climate change research needs. The workshop concluded that the major ways that aviation can affect climate, in agreement with the 1999 assessment by the Intergovernmental Panel on Climate Change (IPCC), are the direct climate effects from CO2 and water vapor emissions, the indirect forcing on climate resulting from changes in the distributions and concentrations of ozone and methane as a primary consequence of aircraft nitrogen oxide (NOx) emissions, the direct effects (and indirect effects on clouds) from emitted aerosols and aerosol precursors, and the climate effects associated with contrails and cirrus cloud formation. The workshop was organized in three subgroups: (1) Effects of aircraft emissions on the UT/LS chemical composition, (2) Effects of water and particle emissions on contrails and on cirrus clouds, and (3) Impacts on climate from aircraft emissions and identification of suitable metrics to measure these impacts. The workshop participants acknowledged the need for focused research specifically to address the uncertainties and gaps in our understanding of current and projected impacts of aviation on climate and to develop metrics to better characterize these impacts. This may entail coordination and/or expansion of existing and planned climate research programs, or new activities. Such efforts should include strong and continuing interactions among the science and aviation communities as well as policymakers to develop well-informed decisions.

Wuebbles, Don↗
NASA NTRS2008

Catalyst for treatment and control of post-combustion emissions

The present invention utilizes two precious metals with two to five different metal-oxides in a layered matrix to convert CO, HCs, and NOx to CO.sub.2, and N.sub.2 by oxidation of two components and reduction of the other in a moderately high temperature gaseous environment containing excess oxygen.

Upchurch, legal representative, Wilhelmina H.↗
NASA NTRS2008

Global Radiative Forcing of Coupled Tropospheric Ozone and Aerosols in a Unified General Circulation Model

Global simulations of sea salt and mineral dust aerosols are integrated into a previously developed unified general circulation model (GCM), the Goddard Institute for Space Studies (GISS) GCM II', that simulates coupled tropospheric ozone-NOx-hydrocarbon chemistry and sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon aerosols. The fully coupled gas-aerosol unified GCM allows one to evaluate the extent to which global burdens, radiative forcing, and eventually climate feedbacks of ozone and aerosols are influenced by gas-aerosol chemical interactions. Estimated present-day global burdens of sea salt and mineral dust are 6.93 and 18.1 Tg with lifetimes of 0.4 and 3.9 days, respectively. The GCM is applied to estimate current top of atmosphere (TOA) and surface radiative forcing by tropospheric ozone and all natural and anthropogenic aerosol components. The global annual mean value of the radiative forcing by tropospheric ozone is estimated to be +0.53 W m(sup -2) at TOA and +0.07 W m(sup -2) at the Earth's surface. Global, annual average TOA and surface radiative forcing by all aerosols are estimated as -0.72 and -4.04 W m(sup -2), respectively. While the predicted highest aerosol cooling and heating at TOA are -10 and +12 W m(sup -2) respectively, surface forcing can reach values as high as -30 W m(sup -2), mainly caused by the absorption by black carbon, mineral dust, and OC. We also estimate the effects of chemistry-aerosol coupling on forcing estimates based on currently available understanding of heterogeneous reactions on aerosols. Through altering the burdens of sulfate, nitrate, and ozone, heterogeneous reactions are predicted to change the global mean TOA forcing of aerosols by 17% and influence global mean TOA forcing of tropospheric ozone by 15%.

Liao, Hong↗
NASA NTRS2008

Improving Air Quality Forecasts with AURA Observations

Past studies have identified model initial and boundary conditions as sources of reducible errors in air-quality simulations. In particular, improving the initial condition improves the accuracy of short-term forecasts as it allows for the impact of local emissions to be realized by the model and improving boundary conditions improves long range transport through the model domain, especially in recirculating anticyclones. During the August 2006 period, we use AURA/OMI ozone measurements along with MODIS and CALIPSO aerosol observations to improve the initial and boundary conditions of ozone and Particulate Matter. Assessment of the model by comparison of the control run and satellite assimilation run to the IONS06 network of ozonesonde observations, which comprise the densest ozone sounding campaign ever conducted in North America, to AURA/TES ozone profile measurements, and to the EPA ground network of ozone and PM measurements will show significant improvement in the CMAQ calculations that use AURA initial and boundary conditions. Further analyses of lightning occurrences from ground and satellite observations and AURA/OMI NO2 column abundances will identify the lightning NOx signal evident in OMI measurements and suggest pathways for incorporating the lightning and NO2 data into the CMAQ simulations.

Newchurch, M. J.↗
NASA NTRS2006

Role of Climate Change in Global Predictions of Future Tropospheric Ozone and Aerosols

A unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies general circulation model II is applied to simulate an equilibrium CO2-forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5-20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2-driven climate change alone is predicted to reduce the global O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate-sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate-induced changes in burdens and different climatological conditions; with full gas-aerosol coupling and accounting for ozone and direct radiative forcings by the O2, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, -0.72, -1.0, +1.26, and -0.56 W m(exp -2), respectively, using present-day climate and year 2100 emissions, while they are predicted to be +0.76, -0.72, 0.74, +0.97, and -0.58 W m(exp -2), respectively, with year 2100 climate and emissions.

Liao, Hong↗