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At least 253 records · Page 14

Flame tube parametric studies for control of fuel bound nitrogen using rich-lean two-stage combustion

An experimental parametric study of rich-lean two-stage combustion in a flame tube is described and approaches for minimizing the conversion of fuel-bound nitrogen to nitrogen oxides in a premixed, homogeneous combustion system are evaluated. Air at 672 K and 0.48 MPa was premixed with fuel blends of propane, toluene, and pyridine at primary equivalence ratios ranging from 0.5 to 2.0 and secondary equivalence ratios of 0.5 to 0.7. Distillates of SRC-II, a coal syncrude, were also tested. The blended fuels were proportioned to vary fuel hydrogen composition from 9.0 to 18.3 weight percent and fuel nitrogen composition from zero to 1.5 weight percent. Rich-lean combustion proved effective in reducing fuel nitrogen to NO sub x conversion; conversion rates up to 10 times lower than those normally produced by single-stage combustion were achieved. The optimum primary equivalence ratio, where the least NO sub x was produced and combustion efficiency was acceptable, shifted between 1.4 and 1.7 with changes in fuel nitrogen content and fuel hydrogen content. Increasing levels of fuel nitrogen content lowered the conversion rate, but not enough to avoid higher NO sub x emissions as fuel nitrogen increased.

Schultz, D. F.↗

Bolide impacts, acid rain, and biospheric traumas at the Cretaceous-Tertiary boundary

Two plausible projectiles are considered: an ice-rich long-period comet and a much smaller rock-metal asteroid. In the framework of a proposal addressed by Lewis et al. (1982), it is shown that, while the impact projectiles themselves do not shock-heat the atmosphere very extensively, the supersonic plume of water vapor and rock produced on impact does shock the atmosphere up to global scales and the shock is of sufficient intensity to produce abundant nitric oxide. For example, an ice-rich long-period comet with a mass of 1.25 x 10 to the 16th kg and a velocity of 65 km/s striking the earth would produce about 7 x 10 to the 40th molecules NO through shock-heating of the atmosphere by the high-velocity ejecta plume fragments. Specific attention is given to the fraction of the atmosphere shock-heated, the global circulation of the nitrogen oxides, the effects of the ejecta plume water on acid rain (AR) predictions, the effects of AR on continental soils, the relationship between AR production rates and the total amount of acid needed to acidify the surface oceans, and the longevity of the oceanic acidity event and the exhaled CO2 event and their implications for the environment in the first millenia or so after the impact.

Prinn, Ronald G.↗

The Central Role of Air Quality Observations in NASA's GEOS Composition Forecasting Model

The NASA GEOS composition forecast model (GEOS-CF) provides global, high-resolution (25 km) air quality forecasts in near-real time. This system combines the operational GEOS-5 weather forecasting model with the state-of-the-science GEOS-Chem chemistry module to provide detailed chemical analysis of a wide range of air pollutants such as ozone, carbon monoxide, nitrogen oxides, and fine particulate matter (PM2.5). The resolution of the forecasts is the highest compared to current, publicly-available global composition forecasts.Air quality observations are an indispensable tool to evaluate the model's ability to capture the strong temporal and spatial gradients of air pollutants across the globe. We show how comparisons against near-real time observations available through OpenAQ (www.openaq.org) demonstrate the model's overall success in reproducing surface concentrations of ozone, nitrogen dioxide, and PM2.5. This analysis also helps identifying current limitations of the model, for example over South America. The model-observation mismatches are most likely caused by uncertainties in the emissions data. Using the example of Rio de Janeiro, we show how the model skill can be improved by using local, high-resolution emission inventories in combination with air quality data.

Keller, Christoph A.↗

Analytical methods for toxic gases from thermal degradation of polymers

Toxic gases evolved from the thermal oxidative degradation of synthetic or natural polymers in small laboratory chambers or in large scale fire tests are measured by several different analytical methods. Gas detector tubes are used for fast on-site detection of suspect toxic gases. The infrared spectroscopic method is an excellent qualitative and quantitative analysis for some toxic gases. Permanent gases such as carbon monoxide, carbon dioxide, methane and ethylene, can be quantitatively determined by gas chromatography. Highly toxic and corrosive gases such as nitrogen oxides, hydrogen cyanide, hydrogen fluoride, hydrogen chloride and sulfur dioxide should be passed into a scrubbing solution for subsequent analysis by either specific ion electrodes or spectrophotometric methods. Low-concentration toxic organic vapors can be concentrated in a cold trap and then analyzed by gas chromatography and mass spectrometry. The limitations of different methods are discussed.

Hsu, M.-T. S.↗

Multi-model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation Historical and Projected Changes

We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice-core measurements. We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present-day (year 2000 ACCMIP time-slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multi-model mean deposition of 50 Tg(N) yr1 from nitrogen oxide emissions, 60 Tg(N) yr1 from ammonia emissions, and 83 Tg(S) yr1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards misrepresentation of 1980 NH3 emissions over North America. Based on ice-core records, the 1850 deposition fluxes agree well with Greenland ice cores but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double 2000 in some scenarios and reaching 1300 mg(N) m2 yr1 averaged over regional to continental scale regions in RCP 2.6 and 8.5, 3050 larger than the values in any region currently (2000). The new ACCMIP deposition dataset provides novel, consistent and evaluated global gridded deposition fields for use in a wide range of climate and ecological studies.

Lamarque, J.-F.↗

Has NO(2) in Metropolitan Areas Returned to Pre-COVID-19 Levels as Measured by OMI Satellite Data?

Nitrogen oxides (NOx = NO + NO2) are primarily emitted through the combustion of fossil fuels, such as automobiles and power plants. NOx can contribute to chemical reactions that produce ozone and fine particulate matter (PM2.5) pollution. Using tropospheric vertical column density (TVCD) NO2 data from satellite hyperspectral instruments, such as the Ozone Monitoring Instrument (OMI) on board NASA’s EOS Aura satellite, one can monitor changes in NO2 pollution during “black-swan” events, such as mobility restrictions during COVID-19 lockdowns. Our OMI team has created the Global Nitrogen Dioxide Monitoring Home Page (https://so2.gsfc.nasa.gov/no2/no2_index.html ) where we display NO2 TVCD time series, animated maps, and COVID-specific NO2 anomalies comparing to a pre-COVID five-year average for 317 cities and regions around the world. During the pandemic as a result of the widespread lockdowns, many areas saw low NO2 anomalies superimposed on the natural weather related NO2 changes, such as seasonal NO2 cycle. Has NO2 levels returned to pre-Covid-19 levels in large metropolitan areas? We analyze NO2 time series from March through September for the years 2020-2023 using as a reference the average NO2 from 2015-2019 for those months. We will present data from selected cities that represent all countries.

Keith D Evans↗

Multi-Model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation of Historical and Projected Future Changes

We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice core measurements.We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present day (year 2000 ACCMIP time slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multimodel mean deposition of approximately 50 Tg(N) yr−1 from nitrogen oxide emissions, 60 Tg(N) yr−1 from ammonia emissions, and 83 Tg(S) yr−1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards a potential misrepresentation of 1980 NH3 emissions over North America. Based on ice core records, the 1850 deposition fluxes agree well with Greenland ice cores, but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways (RCPs) to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double their 2000 counterpart in some scenarios and reaching >1300 mg(N)m−2 yr−1 averaged over regional to continental-scale regions in RCP 2.6 and 8.5, 30-50% larger than the values in any region currently (circa 2000). However, sulfur deposition rates in 2100 are in all regions lower than in 2000 in all the RCPs. The new ACCMIP multimodel deposition dataset provides state-of-the-science, consistent and evaluated time slice (spanning 1850-2100) global gridded deposition fields for use in a wide range of climate and ecological studies.

Lamarque, J.-F.↗

Global Ozone and Reactive Nitrogen : Composition, Chemistry and Sources

Ozone plays a central role in the chemistry of the atmosphere both as an ultraviolet shield and as a source of hydroxyl radicals (OH), a potent initiator of atmospheric chemistry. There is evidence to suggest that the ozone abundance in the troposphere (0-10 km) has doubled since the industrial revolution and continues to increase to date. The principle reason for this increase is thought to be the increasing emissions of nitrogen oxides (NO(x)) from anthropogenic activities. Although NO(x) is highly reactive and its products such as HN03 are easily removed by deposition, it now appears that its chemistry is quite complex and it can be transported over long distances via its conversion to a variety of nitrates and penetrates. The sources of atmospheric NO(x) include free tropospheric sources such as lightning and subsonic aircraft, as well as surface emissions which are transported to the free troposphere via convective processes. Recent experimental and theoretical studies have tried to unravel the chemistry of reactive nitrogen species, its sources, and their role in ozone formation. In this presentation we shall describe the results from these studies.

Sing, Hanwant B.↗

Impact of stratospheric aircraft emissions on ozone: A two dimensional model study

Atmospheric perturbations caused by the emission of nitrogen oxides from a projected fleet of stratospheric aircraft are studied with a two dimensional chemistry, transport model. Photochemistry of the lower stratosphere, the region where these aircraft may fly, is now known to be influenced by heterogeneous reactions involving sulfuric acid aerosols. This study examines the sensitivity of the atmospheric effects of aircraft to heterogeneous reactions. Information of background aerosols based on the SAGE 2 measurements have been used in the parameterization of the heterogeneous conversion rates. It is found that heterogeneous reactions make the lower stratospheric ozone less sensitive to perturbations in the odd nitrogen level. The calculated reduction in global ozone due to NO(x) injection from a fleet of Mach 2.4 aircraft is 1.28 percent if gas phase reactions only are considered in the model, and 0.06 percent if heterogeneous reactions are included.

Natarajan, M.↗

Impact of Regional Northern Hemisphere Mid-latitude Anthropogenic Sulfur Dioxide Emissions on Local and Remote Tropospheric Oxidants

The unintended consequences of reductions in regional anthropogenic sulfur dioxide (SO2) emissions implemented to protect human health are poorly understood. SO2 decreases began in the 1970s in the US and Europe and are expected to continue into the future, while recent emissions decreases in China are also projected to continue. In addition to the well-documented climate effects (warming) from reducing aerosols, tropospheric oxidation is impacted via aerosol modification of photolysis rates and radical sinks. Impacts on the hydroxyl radical and other trace constituents directly affect climate and air quality metrics such as surface ozone levels. We use the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 nudged towards National Centers for Environmental Prediction (NCEP) reanalysis wind velocities to estimate the impact of SO2 emissions from the US, Europe, and China by differencing a control simulation with an otherwise identical simulation in which 2015 anthropogenic SO2 emissions are set to zero over one of the regions. Springtime sulfate aerosol changes occur both locally to the emission region and also throughout the Northern Hemispheric troposphere, including remote oceanic regions and the Arctic. Hydroperoxy (HO2) radicals are directly removed via heterogeneous chemistry on aerosol surfaces, including sulfate, in the model, and we find that sulfate aerosol produced by SO2 emissions from the three individual northern mid-latitude regions strongly reduces both HO2 and hydroxyl (OH) by up to 10 % year-round throughout most of the troposphere north of 30∘ N latitude. Regional SO2 emissions significantly increase nitrogen oxides (NOx) by about 5 %–8 % throughout most of the free troposphere in the Northern Hemisphere by increasing the NOx lifetime as the heterogeneous sink of HO2 on sulfate aerosol declines. Despite the NOx increases, tropospheric ozone decreases at northern mid-latitudes by 1 %–4 % zonally averaged and by up to 5 ppbv in summertime surface air over China, where the decreases in HO2 and OH suppress O3 production. Since 2015 anthropogenic SO2 emissions in China exceed those in the US or Europe, the oxidative response is greatest for the China perturbation simulation. Chemical effects of aerosols on oxidation (reactive uptake) dominate over radiative effects (photolysis rates), the latter of which are only statistically significant locally for the large perturbation over China. We find that the SO2 emissions decrease in China, which has yet to be fully realized, will have the largest impact on oxidants and related species in the Northern Hemisphere free troposphere compared to future decreases in Europe or the US. Our results bolster previous calls for a multipollutant strategy for air pollution mitigation to avoid the unintended consequence of aerosol removal leading to surface ozone increases that offset or mask surface ozone gains achieved by regulation of other pollutants, especially in countries where current usage of high-sulfur emitting fuels may be phased out in the future.

anthropogenic sulfur dioxide emissions↗

Measurements and Modeling of Nitric Oxide Formation in Counterflow, Premixed CH4/O2/N2 Flames

Laser-induced fluorescence (LIF) measurements of NO concentration in a variety of CH4/O2/N2 flames are used to evaluate the chemical kinetics of NO formation. The analysis begins with previous measurements in flat, laminar, premixed CH4/O2/N2 flames stabilized on a water-cooled McKenna burner at pressures ranging from 1 to 14.6 atm, equivalence ratios from 0.5 to 1.6, and volumetric nitrogen/oxygen dilution ratios of 2.2, 3.1 and 3.76. These measured results are compared to predictions to determine the capabilities and limitations of the comprehensive kinetic mechanism developed by the Gas Research Institute (GRI), version 2.11. The model is shown to predict well the qualitative trends of NO formation in lean-premixed flames, while quantitatively underpredicting NO concentration by 30-50%. For rich flames, the model is unable to even qualitatively match the experimental results. These flames were found to be limited by low temperatures and an inability to separate the flame from the burner surface. In response to these limitations, a counterflow burner was designed for use in opposed premixed flame studies. A new LIF calibration technique was developed and applied to obtain quantitative measurements of NO concentration in laminar, counterflow premixed, CH4/O2/N2 flames at pressures ranging from 1 to 5.1 atm, equivalence ratios of 0.6 to 1.5, and an N2/O2 dilution ratio of 3.76. The counterflow premixed flame measurements are combined with measurements in burner-stabilized premixed flames and counterflow diffusion flames to build a comprehensive database for analysis of the GRI kinetic mechanism. Pathways, quantitative reaction path and sensitivity analyses are applied to the GRI mechanism for these flame conditions. The prompt NO mechanism is found to severely underpredict the amount of NO formed in rich premixed and nitrogen-diluted diffusion flames. This underprediction is traced to uncertainties in the CH kinetics as well as in the nitrogen oxidation chemistry. Suggestions are made which significantly improve the predictive capability of the GRI mechanism in near-stoichiometric, rich, premixed flames and in atmospheric-pressure, diffusion flames. However, the modified reaction mechanism is unable to model the formation of NO in ultra-rich, premixed or in high-pressure, nonpremixed flames, thus indicating the need for additional study under these conditions.

Thomsen, D. Douglas↗

Future Lightning Instruments for Weather and Climate Monitoring From LEO

Lightning is not only a natural hazard, but it also holds information about physical processes at work in deep convection and influences atmospheric oxidants that modulate ozone and methane. Hence, spaceborne lightning observations are essential for monitoring extreme events and feedbacks in Earth’s climate system. Low-Earth orbiting (LEO) lightning mapping instruments established a 25-year record of global lightning activity and resulted in a wealth of studies that motivated its designation as an Essential Climate Variable by the World Meteorological Organization. Although geostationary observations of lightning have become increasingly available since 2017, LEO lightning mappers continue to serve critical needs given their unique vantage point and acceptance as a unifying reference for geostationary lightning mapper and ground-based global lightning datasets. At the close of 2023, the Lightning Imaging Sensor (LIS) will cease operations on the International Space Station, which introduces a critical gap in LEO-based monitoring of global lightning activity. To address this need, NASA is developing new lightning mapping technology that enables future LEO-based satellite missions. Existing LEO-based lightning mappers rely on narrowband optical emissions centered on 777.4-nm and detectors that capture 500 images per second to detect lightning both day and night. Lightning can also produce optical emissions in a narrowband centered on 337-nm without any corresponding emissions at the traditionally used near-infrared (NIR) wavelength. These near-ultraviolet (UV) emissions are associated with earlier stage electrical breakdown (e.g., streamers), may frequent intense regions of deep convective storms, and may be a significant source of nitrogen oxide production in the upper atmosphere. A new lightning mapping instrument called the CubeSat Lightning Imaging and Detection Experiment (CLIDE) is being designed at NASA Marshall Space Flight Center to use high-speed, scientific CMOS image sensors capable of detecting lightning’s transient optical emissions in the near-UV and NIR during both daylit and nighttime scenes. This will extend the record of global lightning activity and help pave the way for future small satellite missions that combine radio and optical lightning detectors to obtain novel three-dimensional maps of lightning on a global scale, which can revolutionize the way lightning is used to monitor weather and understand changes in climate.

lightning↗

Impact of the 2008 Global Recession on Air Quality over the United States: Implications for Surface Ozone Levels from Changes in NOx Emissions

Satellite and ground observations detected large variability in nitrogen oxides (NOx) during the 2008 economic recession, but the impact of the recession on air quality has not been quantified. This study combines observed NOx trends and a regional chemical transport model to quantify the impact of the recession on surface ozone (O3) levels over the continental United States. The impact is quantified by simulating O3 concentrations under two emission scenarios: business-as-usual (BAU) and recession. In the BAU case, the emission projection from the Cross-State Air Pollution Rule is used to estimate the would-be NOx emission level in 2011. In the recession case, the actual NO2 trends observed from Air Quality System ground monitors and the Ozone Monitoring Instrument on the Aura satellite are used to obtain realistic changes in NOx emissions. The model prediction with the recession effect agrees better with ground O3 observations over time and space than the prediction with the BAU emission. The results show that the recession caused a 12ppbv decrease in surface O3 concentration over the eastern United States, a slight increase (0.51ppbv) over the Rocky Mountain region, and mixed changes in the Pacific West. The gain in air quality benefits during the recession, however, could be quickly offset by the much slower emission reduction rate during the post-recession period.

NOx emissions↗

Inverse Modeling of Texas NOx Emissions Using Space-Based and Ground-Based NO2 Observations

Inverse modeling of nitrogen oxide (NOx) emissions using satellite-based NO2 observations has become more prevalent in recent years, but has rarely been applied to regulatory modeling at regional scales. In this study, OMI satellite observations of NO2 column densities are used to conduct inverse modeling of NOx emission inventories for two Texas State Implementation Plan (SIP) modeling episodes. Addition of lightning, aircraft, and soil NOx emissions to the regulatory inventory narrowed but did not close the gap between modeled and satellite observed NO2 over rural regions. Satellitebased top-down emission inventories are created with the regional Comprehensive Air Quality Model with extensions (CAMx) using two techniques: the direct scaling method and discrete Kalman filter (DKF) with Decoupled Direct Method (DDM) sensitivity analysis. The simulations with satellite-inverted inventories are compared to the modeling results using the a priori inventory as well as an inventory created by a ground-level NO2 based DKF inversion. The DKF inversions yield conflicting results: the satellite based inversion scales up the a priori NOx emissions in most regions by factors of 1.02 to 1.84, leading to 3-55% increase in modeled NO2 column densities and 1-7 ppb increase in ground 8 h ozone concentrations, while the ground-based inversion indicates the a priori NOx emissions should be scaled by factors of 0.34 to 0.57 in each region. However, none of the inversions improve the model performance in simulating aircraft-observed NO2 or ground-level ozone (O3) concentrations.

Nitrogen dioxide↗

Tracking NO2 Pollution Changes Over Texas: Synthesis of In Situ and Satellite Observations

Nitrogen oxides (NO x ) are major air pollutants that play a crucial role in atmospheric chemistry. We compare Ozone Measuring Instrument's (OMI) NO 2 records with the in situ surface measurements from the Air Quality System of the US Environmental Protection Agency and the Texas Commission on Environmental Quality network in the state of Texas with the goal of understanding the correspondence of satellite and in situ surface observations and identifying the potential synergies between the two observing systems. Our analysis of over 40 in situ daily surface site observations, mostly from urban areas, and OMI daily observed data suggests a correlation ( r ) ranging between 0.2 and 0.8. The correlation improves considerably ( r > 0.5) for monthly average data. Weekly variation of surface NO 2 with a Sunday minimum is well captured by OMI tropospheric NO 2 column observations with similar weekend reductions. NO 2 trend in Texas during 2005–2019 is characterized by significant reductions of 20%–36% in highly populated cities and urban centers. However, a significant (up to 80%) increase was observed in oil and gas producing regions of the Permian and Eagle Ford Basins over the same period. In March–April of 2020, like the other US and global cities, Texas experienced up to 60% reduction in NO 2 levels in major cities due to travel restrictions imposed at local and national levels to contain the spread of COVID-19. Though such reduction is temporary, these reductions were significantly larger than those achieved in the past 16 years of OMI record suggesting that technological advancement can curtail NO x emissions.

Nitrogen dioxide (NO2)↗