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At least 127 records · Page 7

Application of Advanced Earth Observations and Model Simulations to Improve Air Quality Monitoring in the Hindu-Kush-Himalayan Region

Air pollution is a serious environmental health concern in the Hindu Kush Himalayan (HKH) region of south-central Asia, as rapid industrialization and population growth have led to increased anthropogenic emissions from transportation, residential, industrial, energy, and biomass burning sources. Natural emissions from dust and forest fires are additional sources of air pollutants that can exacerbate air quality in the region. The combination of the complex pollutant mixtures and atmospherically stable weather conditions during the winter monsoon can visibility reductions and hazardous air quality from persistent haze episodes. The Kathmandu Valley is especially vulnerable to extreme haze issues due to the surrounding mountains that restrict air movement and retains pollutants in the atmosphere. This study uses state-of-the-art satellite observations and modeling capabilities in conjunction with ground-based networks to provide a comprehensive data toolkit for advancing air quality monitoring and forecasting decisions in the HKH region. The toolkit includes new generation satellite observations from the TROPOspheric Monitoring Instrument (TROPOMI), Geostationary Environment Monitoring Spectrometer (GEMS), and Advanced Meteorological Imager, which provide high spatiotemporal information on NO2, HCHO, SO2, O3, and aerosol optical depth (AOD). Particulate matter with diameters less than 2.5 micrometers (PM2.5) are derived from the satellite-retrieved AOD using ground-based observations and forecast model data. The satellite observations are also used to initialize and constrain forecast model systems designed for the HKH region. This talk will highlight the performance of the air quality toolkit for enhancing decision-making processes during exceptional air quality events in the region. Note: Presentation includes additional attachment of full presentation with sound and animation (best when viewed as slide show) with runtime of 15 min 32 secs

Aaron Naeger↗

The Detection, Characterization and Tracking of Recent Aleutian Island Volcanic Ash Plumes and the Assessment of Their Impact on Aviation

The Aleutian Islands of Alaska are home to a number of major volcanoes which periodically present a significant hazard to aviation. During summer of 2008, the Okmok and Kasatochi volcanoes experienced moderate eruptive events. These were followed a dramatic, major eruption of Mount Redoubt in late March 2009. The Redoubt case is extensively covered in this paper. Volcanic ash and SO2 from each of these eruptions dispersed throughout the atmosphere. This created the potential for major problems for air traffic near the ash dispersions and at significant distances downwind. The NASA Applied Sciences Weather Program implements a wide variety of research projects to develop volcanic ash detection, characterization and tracking applications for NASA Earth Observing System and NOAA GOES and POES satellites. Chemistry applications using NASA AURA satellite Ozone Monitoring System (OMI) retrievals produced SO2 measurements to trace the dispersion of volcanic aerosol. This work was complimented by advanced multi-channel imager applications for the discrimination and height assignment of volcanic ash using NASA MODIS and NOAA GOES and POES imager data. Instruments similar to MODIS and OMI are scheduled for operational deployment on NPOESS. In addition, the NASA Calipso satellite provided highly accurate measurements of aerosol height and dispersion for the calibration and validation of these algorithms and for corroborative research studies. All of this work shortens the lead time for transition to operations and ensures that research satellite data and applications are operationally relevant and utilized quickly after the deployment of operational satellite systems. Introduction

Murray, John J.↗

Primary lithium battery technology and its application to NASA missions

A description is given of the components, overall cell reactions, and performance characteristics of promising new ambient temperature lithium primary systems based on the Li-V205, Li-SO2, and Li-SOC12 couples. Development status of these systems is described in regard to availability and uncertainties in the areas of safety and selected performance characteristics. Studies show that use of lithium batteries would enhance a variety of missions and applications by decreasing power sytems weight and thereby increasing payload weight. In addition, the lithium batteries could enhance cost effectiveness of the missions.

Frank, H. A.↗

A global anthropogenic emission inventory of atmospheric pollutants from sector- and fuel-specific sources (1970–2017): an application of the Community Emissions Data System (CEDS)

Global anthropogenic emission inventories remain vital for understanding the sources of atmospheric pollution and the associated impacts on the environment, human health, and society. Rapid changes in today's society require that these inventories provide contemporary estimates of multiple atmospheric pollutants with both source sector and fuel type information to understand and effectively mitigate future impacts. To fill this need, we have updated the open-source Community Emissions Data System (CEDS) (Hoesly et al., 2019) to develop a new global emission inventory, CEDSGBD-MAPS. This inventory includes emissions of seven key atmospheric pollutants (NOx; CO; SO2; NH3; non-methane volatile organic compounds, NMVOCs; black carbon, BC; organic carbon, OC) over the time period from 1970–2017 and reports annual country-total emissions as a function of 11 anthropogenic sectors (agriculture; energy generation; industrial processes; on-road and non-road transportation; separate residential, commercial, and other sectors (RCO); waste; solvent use; and international shipping) and four fuel categories (total coal, solid biofuel, the sum of liquid-fuel and natural-gas combustion, and remaining process-level emissions). The CEDSGBD-MAPS inventory additionally includes monthly global gridded (0.5°?×?0.5°) emission fluxes for each compound, sector, and fuel type to facilitate their use in earth system models. CEDSGBD-MAPS utilizes updated activity data, updates to the core CEDS default scaling procedure, and modifications to the final procedures for emissions gridding and aggregation. Relative to the previous CEDS inventory (Hoesly et al., 2018), these updates extend the emission estimates from 2014 to 2017 and improve the overall agreement between CEDS and two widely used global bottom-up emission inventories. The CEDSGBD-MAPS inventory provides the most contemporary global emission estimates to date for these key atmospheric pollutants and is the first to provide global estimates for these species as a function of multiple fuel types and source sectors. Dominant sources of global NOx and SO2 emissions in 2017 include the combustion of oil, gas, and coal in the energy and industry sectors as well as on-road transportation and international shipping for NOx. Dominant sources of global CO emissions in 2017 include on-road transportation and residential biofuel combustion. Dominant global sources of carbonaceous aerosol in 2017 include residential biofuel combustion, on-road transportation (BC only), and emissions from the waste sector. Global emissions of NOx, SO2, CO, BC, and OC all peak in 2012 or earlier, with more recent emission reductions driven by large changes in emissions from China, North America, and Europe. In contrast, global emissions of NH3 and NMVOCs continuously increase between 1970 and 2017, with agriculture as a major source of global NH3 emissions and solvent use, energy, residential, and the on-road transport sectors as major sources of global NMVOCs. Due to similar development methods and underlying datasets, the CEDSGBD-MAPS emissions are expected to have consistent sources of uncertainty as other bottom-up inventories. The CEDSGBD-MAPS source code is publicly available online through GitHub: https://github.com/emcduffie/CEDS/tree/CEDS_GBD-MAPS (last access: 1 December 2020). The CEDSGBD-MAPS emission inventory dataset (both annual country-total and monthly global gridded files) is publicly available under https://doi.org/10.5281/zenodo.3754964 (McDuffie et al., 2020c).

Mcduffie, Erin↗

Global SO 2 Data Record from OMPS Instruments on the JPSS Constellation

NASA’s Earth Observing System (EOS) SO 2 climate data record (CDR) started in 2004, with the launch of the Aura/Ozone Monitoring Instrument (OMI) and is now being continued with the SNPP/Ozone Mapping and Profiler Suite (OMPS) launched in 2011. Both OMI and SNPP/OMPS SO 2 CDRs are produced with the Goddard principal component analysis (PCA) spectral fitting algorithm. An advantage of the data-driven PCA retrieval technique is that it enables highly consistent retrievals from different instruments, by inherently accounting for various instrumental factors. To further extend the EOS SO 2 CDR, we are implementing the PCA SO 2 retrieval algorithm with the L1B measurements from OMPS instruments flying on the Joint Polar Satellite System (JPSS) constellation. In this presentation, we will provide an update on our progress in NOAA-20 (launched in 2017) and NOAA-21 (launched in 2022) PCA SO2 retrievals. We will focus on our new NOAA-20/OMPS PCA SO 2 EOS continuity product, to be publicly released in fall of 2023. We will present statistical analyses on the quality of NOAA-20 PCA SO 2 product, including retrieval noise, biases over background areas, and long-term stability. We will compare our PCA SO 2 retrievals from NOAA-20 with those from OMI, SNPP/OMPS, and S5P/TROPOMI (TROPOspheric Monitoring Instrument) for anthropogenic sources as well as large volcanic plumes. We will also discuss the application of a new machine learning technique that helps to further reduce the noise of NOAA-20 SO 2 retrievals. In addition, we will present preliminary PCA SO 2 retrievals from NOAA-21/OMPS, including those from direct readout implementation for aviation disaster avoidance. Finally, we will share some first results applying the PCA algorithm to NASA’s geostationary TEMPO (Tropospheric Emissions: Monitoring of Pollution) instrument to obtain hourly, high resolution SO 2 data over North America.

SO2↗

The effect of plasma heating on sublimation-driven flow in Io's atmosphere

The atmospheric flow on Io is numerically computed in a flat 2-D axisymmetric geometry for a sublimation atmosphere on the trailing hemisphere subjected to plasma bombardment, UV heating, and IR cooling. Calculations are performed for subsolar vapor pressures of approximately 6.5 x 10(exp -3) Pa (approximately 3 x 10(exp 18) SO2/sq cm) and 6.8 x 10(exp -4) Pa (approximately 4 x 10(exp 17) SO2/sq cm); the latter approximates the vapor pressure of F. P. Fanale et al. (1982). The amount of plasma energy deposited in the atmosphere is 20% of the plasma flow energy due to corotation (J. A. Linker et al., 1988). It is found that plasma heating significantly inflates the upper atmosphere, increasing both the exobase altitude and the amount of surface covered by more than an exospheric column of gas. This in turn controls the supply of the Io plasma torus (M. A. McGrath and R. E. Johnson, 1987). The horizontal flow of mass and energy is also important in determining the exobase altitude; and it is shown that IR cooling can be important, although our use of the equilibrium, cool-to-space approximation for a pure SO2 gas (E. Lellouch et al., 1992) may overestimate this effect. The calculated exobase altitudes are somewhat lower than those suggested by McGrath and Johnson (1987) for supplying the torus, indicating the details of the plasma energy deposition and sputter ejection rate near the exobase, as well as the IR emission from this region need to be examined. In addition, the molecules sublimed (or sputtered) from the surface are transported to the exobase in times short compared to the molecular photodissociation time. Therefore, the exobase is dominated by molecular species and the exobase is supplied by a small region of the surface.

Wong, Mau C.↗

Toba volcano super eruption destroyed the ozone layer and caused a human population bottleneck

Volcanic eruptions trigger a broad spectrum of climatic responses. For example, the Mount Pinatubo eruption in 1991 forced an El Niño and global cooling, and the Tambora eruption in 1815 caused the "Year Without a Summer." Especially grand eruptions such as Toba around 74,000 years ago can push the Earth's climate into a volcanic winter state, significantly lowering the surface temperature and precipitation globally. Here we present a new, previously overlooked element of the volcanic effects spectrum: the radiative mechanism of stratospheric ozone depletion. We found that the volcanic plume of Toba enhanced the UV optical depth and suppressed the primary formation of stratospheric ozone from O2 photolysis. Sulfate aerosols additionally reflect the photons needed to break the O2 bond (λ < 242 nm), otherwise controlled by ozone absorption and Rayleigh scattering alone during volcanically quiescent conditions. Our NASA GISS ModelE simulations of the Toba eruption reveal up to 50% global ozone loss due to the overall photochemistry perturbations of the sulfate aerosols. We also consider and quantify the radiative effects of SO2, which partially compensated for the ozone loss by inhibiting the photolytic O3 sink. Our analysis shows that the magnitude of the ozone loss and UV-induced health-hazardous effects after the Toba eruption are similar to those in the aftermath of a potential nuclear conflict. These findings suggest a “Toba ozone catastrophe" as a likely contributor to the historic population decline in this period, consistent with a genetic bottleneck in human evolution.

Toba volcano↗

Computing rovibrational, vibrational, and cascade emission spectra for comparison to astronomical observations

Over the last several years, our group has been involved in developing approaches to compute highly accurate spectroscopic constants and vibrational frequencies for small transient molecules that may be used in the interpretation and assignment of high-resolution laboratory experiments as well as high-resolution astronomical spectra. Additionally, we have used the computed spectroscopic constants to simulate purely rotational and rovibrational spectra so that these may be compared directly with high-resolution astronomical observations, and we have worked on developing approaches that can be applied to much larger molecules, such as polycyclic aromatic hydrocarbon (PAH) molecules, where we can explicitly determine anharmonic corrections to vibrational frequencies as well as take into account intensity sharing due to resonances. In addition, for PAH molecules we have used the anharmonic data to compute a library of temperature-dependent anharmonic vibrational spectra, with proper inclusion of polyad resonances, which can then be used to model the cascade emission spectra of PAH molecules – the type of spectra directly observed by astronomers. Another part of our work in spectroscopic signatures involves computing highly accurate line lists for common molecules, such as CO2, SO2, and NH3, which occur in many astrophysical environments, including the atmospheres of exoplanents, and often need to have their lines identified in high-resolution observations in order to determine which lines are due to other molecules. In order to characterize the atmospheres of hot exoplanets, these line lists need to be very accurate and extend to very high energies. I will discuss our latest work in these areas of astrochemical spectroscopy research.

Timothy J Lee↗

SO3/H2SO4 continuous real-time sensor demonstration at a power plant

We present results from field testing of a new, innovative sensor developed to measure SO3/H2SO4 continuously and in real time at a coal-fired power plant. The system utilizes the sensitivity, specificity, and real-time capabilities of mid-infrared (Mid-IR) laser-based sensor technology, along with a heated, close-coupled cell mounted directly to a power plant duct. Measurements were made by the laser sensor over a 2-day period and compared to results from the accepted method, EPA 8A, which requires a 30-minute collection, labor intensive processing, and off-site analysis at a lab. In contrast to the condensation method, the laser sensor continuously samples flue gas and reports measurements of the concentration of SO3/H2SO4, SO2 ever second with unattended operation. This initial demonstration proved the sensor concept and paves the way for its use for optimizing sorbent injection used to neutralize SO3/H2SO4. Optimized sorbent injection will enable significant cost savings associated with efforts to mitigate the presence and effects of SO3/H2SO4 such as “Blue Plume”, air heater fouling, and duct corrosion. In particular, the real-time, actionable information will enable better control of additive injection in flex conditions and variable fuels.

20 FOSSIL-FUELED POWER PLANTS↗

Tunable-diode laser absorption spectrometry

Tunable-diode laser absorption spectrometry (TDLAS) affords a number of advantages for atmospheric measurements. It is a universal method, applicable, in principle, to all gases of atmospheric interest. Because of its extremely high spectral resolution it provides unequivocal identification of the target species, with no interferences from other gases. It provides real-time, in situ measurements with time resolutions better than 1 minute. The sensitivity of the current TDLAS system is marginally capable of measuring HO2. This species exists in the troposphere at concentrations which are up to 2 orders of magnitude higher than those of HO and, in addition, is much less susceptible to removal by the surfaces of the instrument and its sampling system. HO2 is an important HO sub x species in its own right but can also give direct information on the HO concentration by virtue of the rapid partitioning between these two species. The addition of the high-frequency modulation technique to the TDLAS system would ensure its ability to measure HO2 under most atmospheric conditions. The ability of the TDLAS to measure hydrogen peroxide (H2O2) in the ambient atmosphere was also demonstrated. H2O2 measurements give a clear indication of HO sub x mixing ratios and are also important as a photolytic source of HO and as an important oxidant for other atmospheric consitituents such as SO2.

Schiff, H. I.↗

Atmospheric Infrared Sounder Version 7 Near-Real-Time Product and Imagery Released by NASA GES DISC

The NASA Goddard Earth Sciences Data and Information Services Center (GES DISC) has been the home of data processing, archive, and distribution services for data from the Atmospheric Infrared Sounder (AIRS) mission since its launch in 2002. The GES DISC provides service to both AIRS routine and Near Real-Time (NRT) products. The AIRS NRT products are an important element in the Land, Atmosphere Near real-time Capability for EOS (LANCE). In collaboration with AIRS Project, the GES DISC has just released products from the Version 7 algorithm. The new version algorithm provides significant improvements over the previous version. The most substantial advances are: improved consistency between day and night water vapor; improved total column ozone and temperature; improved infrared-only (IR-only) retrievals, especially in high latitude regions; an improved Stochastic Cloud Clearing Neural Network used as a first guess at the initial value in the iterative retrieval process; and removal of ambiguity in surface classification in the IR-only retrieval algorithm. In addition, the GES DISC produces AIRS NRT imagery. The AIRS NRT imagery are generated by mosaicking and mapping the available AIRS 6-minute retrieval granules to a global projection. The images are constantly refreshed when new granules are produced. The AIRS NRT Viewer and LANCE Worldview provide visualization services to online users for AIRS NRT imagery. The data products used to generate this imagery include atmospheric temperature, humidity, precipitation, cloud, Dust Score, CO, and SO2. In this presentation, we will demonstrate visualization of the AIRS NRT imagery from the new Version 7, and demonstrate some improvements over the previous version. Progress on improving the AIRS NRT imagery, a collaboration project with the AIRS Applications Development Team at NASA Jet Propulsion Laboratory (JPL), will also be presented.

Feng Ding↗

Lidar Observations of the Pinatubo Volcanic Cloud over Hampton, Virginia

A series of eruptions of Mt. Pinatubo climaxed in a cataclysmic eruption on June 15-16, which greatly perturbed the stratospheric aerosol layer. These eruptions yielded an estimated 20 megatons of SO2, which is three times the amount produced by El Chichon. Lidar measurements taken by the 48-inch lidar system at Langley Research Center show the vertical distribution, intensity and spread of the Pinatubo aerosol layers over the middle latitude locations. A few observations have also been made using an airborne lidar system which measures scattering and depolarization. The magnitude and transport time of the volcanic aerosols following Pinatubo and El Chichon are compared. In addition, comparisons are made between the ground-based lidar measurements and near-coincident Stratospheric Aerosol and Gas Experiment (SAGE) 2 satellite observations of the Pinatubo aerosol layers.

Osborn, M. T.↗

Cleaned 5-Minute Resolution Air Quality and Meteorological Data from Nine TCEQ CAMS Sites in Houston, Texas (Nov 2021 – Oct 2022)

These data encompass 5-minute air monitoring and meteorological observations collected in the greater Houston, Texas metropolitan region, at nine (9) Continuous Ambient Monitoring Stations (CAMS) operated by the Texas Commission on Environmental Quality (TCEQ) between November 1, 2021 and October 31, 2022. The CAMS sites (CAMS 1, 8, 35, 45, 148, 403, 405, 410, and 1052) were chosen because their instrumentation includes measurements of PM2.5. These sites also provide continuous multi-parameter air-quality and meteorological measurements. Particulate matter (PM2.5, PM10) was sampled along with several trace gases, including ozone (O3), nitrogen oxides (NO, NO2, NOx), sulfur dioxide (SO2), and carbon monoxide (CO). The data set also contains standard surface meteorological parameters (temperature, humidity, pressure, wind speed, and wind direction). Several sites also include AutoGC-based measurements of volatile organic compounds (VOCs). Air monitoring instruments deployed at the selected sites comprise the following systems: BAM-1020 or TEOM (PM2.5), Thermo Scientific TEI 49i (O3), TEI 42i (NOx), and AutoGCs (VOCs). This data set is similar to the data included within the houairq5mX1.00 datastream, except for a few additional quality control steps. A systematic data cleaning and verification process was performed on the data set to ensure its quality and preparation for analysis. Removal of non-numeric status flags (e.g., [LIM], [QAS], [SPZ], [CAL], [PMA], [AQI], [SPN], [MAL]) was accomplished by employing rule-based string parsing to extract valid numerical values. Missing entries were set to -9999; however, invalid or anomalous values (e.g., 99999) were retained as originally reported by the TCEQ to preserve data provenance. The time sequence was verified for completeness, removal of duplicates, and uniformity at 5-minute intervals. Column labeling was standardized, and corresponding values were assessed for physical plausibility. All timestamps in the data set were reported in Coordinated Universal Time (UTC) as provided by the TCEQ. Further, the latitude and longitude coordinates were added for each CAMS site. A subset of the data (June 1–September 30, 2022) has been used in the following publication: Subba et al. 2025. “Implications of sea breeze circulations on boundary layer aerosols in the southern coastal Texas region.” EGUsphere 2025: 1–49, https://doi.org/10.5194/egusphere-2025-2659.

latitude↗

Towards a Global Aerosol Climatology: Preliminary Trends in Tropospheric Aerosol Amounts and Corresponding Impact on Radiative Forcing between 1950 and 1990

A global aerosol climatology is needed in the study of decadal temperature change due to natural and anthropogenic forcing of global climate change. A preliminary aerosol climatology has been developed from global transport models for a mixture of sulfate and carbonaceous aerosols from fossil fuel burning, including also contributions from other major aerosol types such as soil dust and sea salt. The aerosol distributions change for the period of 1950 to 1990 due to changes in emissions of SO2 and carbon particles from fossil fuel burning. The optical thickness of fossil fuel derived aerosols increased by nearly a factor of 3 during this period, with particularly strong increase in eastern Asia over the whole time period. In countries where environmental laws came into effect since the early 1980s (e.g. US and western Europe), emissions and consequently aerosol optical thicknesses did not increase considerably after 1980, resulting in a shift in the global distribution pattern over this period. In addition to the optical thickness, aerosol single scattering albedos may have changed during this period due to different trends in absorbing black carbon and reflecting sulfate aerosols. However, due to the uncertainties in the emission trends, this change cannot be determined with any confidence. Radiative forcing of this aerosol distribution is calculated for several scenarios, resulting in a wide range of uncertainties for top-of-atmosphere (TOA) forcings. Uncertainties in the contribution of the strongly absorbing black carbon aerosol leads to a range in TOA forcings of ca. -0.5 to + 0.1 Wm (exp. -2), while the change in aerosol distributions between 1950 to 1990 leads to a change of -0.1 to -0.3 Wm (exp. -2), for fossil fuel derived aerosol with a "moderate" contribution of black carbon aerosol.

Tegen, Ina↗

Exploring NASA OMI Level 2 Data With Visualization

Satellite data products are important for a wide variety of applications that can bring far-reaching benefits to the science community and the broader society. These benefits can best be achieved if the satellite data are well utilized and interpreted, such as model inputs from satellite, or extreme events (such as volcano eruptions, dust storms, etc.).Unfortunately, this is not always the case, despite the abundance and relative maturity of numerous satellite data products provided by NASA and other organizations. Such obstacles may be avoided by allowing users to visualize satellite data as images, with accurate pixel-level (Level-2) information, including pixel coverage area delineation and science team recommended quality screening for individual geophysical parameters. We present a prototype service from the Goddard Earth Sciences Data and Information Services Center (GES DISC) supporting Aura OMI Level-2 Data with GIS-like capabilities. Functionality includes selecting data sources (e.g., multiple parameters under the same scene, like NO2 and SO2, or the same parameter with different aggregation methods, like NO2 in OMNO2G and OMNO2D products), user-defined area-of-interest and temporal extents, zooming, panning, overlaying, sliding, and data subsetting, reformatting, and reprojection. The system will allow any user-defined portal interface (front-end) to connect to our backend server with OGC standard-compliant Web Mapping Service (WMS) and Web Coverage Service (WCS) calls. This back-end service should greatly enhance its expandability to integrate additional outside data-map sources.

Level 2↗

Exploring NASA OMI Level 2 Data With Visualization

Satellite data products are important for a wide variety of applications that can bring far-reaching benefits to the science community and the broader society. These benefits can best be achieved if the satellite data are well utilized and interpreted, such as model inputs from satellite, or extreme events (such as volcano eruptions, dust storms,... etc.). Unfortunately, this is not always the case, despite the abundance and relative maturity of numerous satellite data products provided by NASA and other organizations. Such obstacles may be avoided by allowing users to visualize satellite data as "images", with accurate pixel-level (Level-2) information, including pixel coverage area delineation and science team recommended quality screening for individual geophysical parameters. We present a prototype service from the Goddard Earth Sciences Data and Information Services Center (GES DISC) supporting Aura OMI Level-2 Data with GIS-like capabilities. Functionality includes selecting data sources (e.g., multiple parameters under the same scene, like NO2 and SO2, or the same parameter with different aggregation methods, like NO2 in OMNO2G and OMNO2D products), user-defined area-of-interest and temporal extents, zooming, panning, overlaying, sliding, and data subsetting, reformatting, and reprojection. The system will allow any user-defined portal interface (front-end) to connect to our backend server with OGC standard-compliant Web Mapping Service (WMS) and Web Coverage Service (WCS) calls. This back-end service should greatly enhance its expandability to integrate additional outside data/map sources.

Aura↗

Importance of formaldehyde in cloud chemistry

A physical-chemical model which is an extension of that of Hong and Carmichael (1983) is used to investigate the role of formaldehyde in cloud chemistry. This model takes into account the mass transfer of SO2, O3, NH3, HNO3, H2O2, CO2, HCl, HCHO, O2, OH and HO2 into cloud droplets and their subsequent chemical reactions. The model is used to assess the importance of S(IV)-HCHO adduct formation, the reduction of H2O2 by HCHO, HCHO-free radical interactions, and the formation of HCOOH in the presence of HCHO in cloud droplets. Illustrative calculations indicate that the presence of HCHO inhibits sulfate production rate in cloud droplets. The direct inhibition of sulfate production rate in cloudwater due to nucleophilic addition of HSO3(-) to HCHO(aq) to form hydroxymethanesulfonate is generally low for concentrations of HCHO typical of ambient air. However, inhibition of sulfate production due to formaldehyde-free radical interactions in solution can be important. These formaldehyde-free radical reactions can also generate appreciable quantities of formic acid.

Adewuyi, Y. G.↗

Trace Chemistry

The goals of the trace chemistry group were to identify the processes relevant to aerosol and aerosol precursor formation occurring within aircraft gas turbine engines; that is, within the combustor, turbine, and nozzle. The topics of discussion focused on whether the chemistry of aerosol formation is homogeneous or heterogeneous; what species are important for aerosol and aerosol precursor formation; what modeling/theoretical activities to pursue; what experiments to carry out that both support modeling activities and elucidate fundamental processes; and the role of particulates in aerosol and aerosol precursor formation. The consensus of the group was that attention should be focused on SO2, SO3, and aerosols. Of immediate concern is the measurement of the concentration of the species SO3, SO2, H2SO4 OH, HO2, H2O2, O, NO, NO2, HONO, HNO3, CO, and CO2 and particulates in various engines, both those currently in use and those in development. The recommendation was that concentration measurements should be made at both the combustor exit and the engine exit. At each location the above species were classified into one of four categories of decreasing importance, Priority I through IV, as follows: Combustor exit: Priority I species - SO3:SO2 ratio, SO3, SO2, and particulates; Priority II species: OH and O; Priority III species - NO and NO2; and Priority IV species - CO and CO2. For the Engine exit: Priority I species - SO3:SO2 ratio, SO3, SO2,H2SO4, and particulates; Priority II species: OH,HO2, H2O2, and O; Priority III species - NO, NO2, HONO, and HNO3; and Priority IV species - CO and CO2. Table I summarizes the anticipated concentration range of each of these species. For particulate matter, the quantities of interest are the number density, size distribution, and composition. In order to provide data for validating multidimensional reacting flow models, it would be desirable to make 2-D, time-resolved measurements of the concentrations of the above species and, in addition, of the pressure, temperature, and velocity. A near term goal of the experimental program should be to confirm the nonlinear effects of sulfur speciation, and if present, to provide an explanation for them. It is also desirable to examine if the particulate matter retains any sulfur. The recommendation is to examine the effects on SOx production of variations in fuel-bound sulfur and aromatic content (which may affect the amount of particulates formed). These experiments should help us to understand if there is a coupling between particulate formation and SO, concentration. Similarly, any coupling with NOx can be examined either by introducing NOx into the combustion air or by using fuel-bound nitrogen. Also of immediate urgency is the need to establish and validate a detailed mechanism for sulfur oxidation/aerosol formation, whose chemistry is concluded to be homogeneous, because there is not enough surface area for heterogeneous effects. It is envisaged that this work will involve both experimental and theoretical programs. The experimental work will require, in addition to the measurements described above, fundamental studies in devices such as flow reactors and shock tubes. Complementing this effort should be modeling and theoretical activities. One impediment to the successful modeling of sulfur oxidation is the lack of reliable data for thermodynamic and transport properties for several species, such as aqueous nitric acid, sulfur oxides, and sulfuric acid. Quantum mechanical calculations are recommended as a convenient means of deriving values for these properties. Such calculations would also help establish rate constants for several important reactions for which experimental measurements are inherently fraught with uncertainty. Efforts to implement sufficiently detailed chemistry into computational fluid dynamic codes should be continued. Zero- and one-dimensional flow models are also useful vehicles for elucidating the minimal set of species and reactions that must be included in two- and three-dimensional modeling studies.

Radhakrishnan, Krishnan↗