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At least 523 records · Page 29
All sourcesNASA NTRSDOE OSTI
NASA NTRS2018

Fundamental Study of a 7-Element Fuel Injector Configuration for Gas Turbine Combustors - A Look at Cold Flow and Burning Measurements

Lean direct injection (LDI) is a combustion concept to reduce oxides of nitrogen (NOx) for next generation aircraft gas turbine engines. These newer engines have cycles that increase fuel efficiency through increased operating pressures, which increase combustor inlet temperatures. NOx formation rates increase with higher temperatures, and the LDI strategy is to avoid high temperature by staying fuel lean and away from stoichiometric burning. Thus, LDI relies on rapid and uniform fuel/air mixing. Additionally, in combustors for smaller core engines, the area and volume bring about mixing and time scale challenges not found in larger engines. As part of our parametric study in which we vary swirler angle and orientation and look at their effect on fluid mixing and combustion, we examine one configuration of a 7-point lean direct injector by looking at the non-combusting 2-D velocity field using PIV, and combusting system for chemical species using chemiluminescent imaging and flame spectroscopy. The circular 7-point array consists of axial swirlers, with the center 60° swirler surrounded by six 52° swirlers. The velocity results for this configuration show that the outer swirlers serve to isolate the center flow field near the injector exit. A recirculation zone forms downstream of the center swirler, but not behind the outer swirlers. The combusting results also show an isolated zone directly downstream of the center injector. The flame spectra show variation in speciation of combustion species such as OH*, C3*, CH*, and C2* as a function of position within the combustor.

lean direct injection↗
NASA NTRS2017

Emissions Relationships Among Western Forest Fire Plumes: I. Emission Factors Free from Mixing Errors

Previous studies of emission factors from biomass burning are prone to largeerrors since they ignore the interplay of mixing and varying pre-fire backgroundCO2 levels. Such complications severely affected our studies of 446 forest fireplume samples measured in the Western US by the science teams of NASAsSEAC4RS and ARCTAS airborne missions. Consequently we propose a MixedEffects Regression Emission Technique (MERET) to check techniques like theNormalized Emission Ratio Method (NERM), where use of sequentialobservations cannot disentangle emissions and mixing. We also evaluate asimpler consensus technique. All techniques relate emissions to fuel burnedusing C burn = Δ Ctot added to the fire plume, where ≈ Ctot (CO2 + CO). Mixed-effectsregression can estimate pre-fire background values of Ctot (indexed byobservation j) simultaneously with emissions factors indexed by individual species i, δέλτα-xi (Cburn )i,j., MERET and consensus require more than twoemissions indicators. Our studies excluded samples where exogenous CO orCH4 might have been fed into a fire plume, mimicking emission.We sought to let the data on 13 gases and particulate properties suggest clustersof variables and plume types, using non-negative matrix factorization (NMF).While samples were mixtures, the NMF unmixing suggested purer burn types.Particulate properties (bscat, babs, SSA, AÅE) and gas-phase emissions were interrelated.Finally, we sought a simple categorization useful for modeling ozone productionin plumes. Two kinds of fires produced high ozone: those with large fuel nitrogenas evidenced by remnant CH3CN in the plumes, and also those from veryintense large burns. Fire types with optimal ratios of delta-NOydelta-HCHO associate with the highest additional ozone per unit Cburn, Perhaps theseplumes exhibit limited NOx binding to reactive organics. Perhaps these plumesexhibit limited NOx binding to reactive organics.

plumes↗
NASA NTRS2016

Emissions Relationships Among Western Forest Fire Plumes: II. Plume Typing for Sources of Ozone and Aerosol Absorption

Previous studies of emission factors from biomass burning are prone to largeerrors since they ignore the interplay of mixing and varying pre-fire backgroundCO2 levels. Such complications severely affected our studies of 446 forest fireplume samples measured in the Western US by the science teams of NASAs SEAC4RS and ARCTAS airborne missions. Consequently we propose a MixedEffects Regression Emission Technique (MERET) to check techniques like theNormalized Emission Ratio Method (NERM), where use of sequentialobservations cannot disentangle emissions and mixing. We also evaluate asimpler consensus technique. All techniques relate emissions to fuel burnedusing Cburn Ctot added to the fire plume, where Ctot (CO2 + CO). Mixed-effectsregression can estimate pre-fire background values of Ctot (indexed byobservation j) simultaneously with emissions factors indexed by individualspecies i, xi (Cburn )i,j., MERET and consensus require more than twoemissions indicators. Our studies excluded samples where exogenous CO orCH4 might have been fed into a fire plume, mimicking emission.We sought to let the data on 13 gases and particulate properties suggest clustersof variables and plume types, using non-negative matrix factorization (NMF).While samples were mixtures, the NMF unmixing suggested purer burn types.Particulate properties (bscat, babs, SSA, AE) and gas-phase emissions were interrelated.Finally, we sought a simple categorization useful for modeling ozone productionin plumes. Two kinds of fires produced high ozone: those with large fuel nitrogenas evidenced by remnant CH3CN in the plumes, and also those from veryintense large burns. Fire types with optimal ratios of delta-NOydelta-HCHO associate with the highest additional ozone per unit Cburn, Perhaps theseplumes exhibit limited NOx binding to reactive organics. Perhaps these plumesexhibit limited NOx binding to reactive organics.

ozone↗
NASA NTRS2018

Fuel Sensitivity of Gas Emissions, Lean Blowout and Combustion Dynamics for a 9-Point LDI Combustor

Fuel sensitivity of gaseous emissions, approach to lean blowout and combustion dynamics are evaluated in this study. Experiments were conducted at the NASA Glenn Research Center's CE-5 flame tube test facility with a 9-point Swirl-Venturi Lean Direct Injection (SV-LDI) combustor. A reference jet fuel (A2) and two test fuels (C1 and C3) from were provided by the National Jet Fuels Combustion Program (NJFCP). C1 is essentially a 2-component iso-paraffin test fuel with a low cetane number of 17, and C3 is a high viscosity test fuel. Approach to lean blowout was monitored in terms of the rapid increase in CO emissions index as equivalence ratio decreased, but testing did not proceed all the way to lean blowout (LBO). Burning C1 was found to produce lower NOx emissions, but C1 flame temperatures were about 25 K higher relative to A2 at near LBO points (where CO emissions increased very rapidly). The NOx emissions of C3 were similar to A2. At low power conditions where fuel injector performance is not optimized for this 9-point LDI combustor, C3 had higher CO emissions than A2 and C1, likely due to C3's higher viscosity relative to A2 and C1. No discernable difference in combustion dynamics was observed between the three fuels tested in the 9-point LDI combustor. While a systematic ignition test campaign was not conducted, it was observed that C1 required a higher equivalence ratio and inlet air temperature for test rig ignition compared to A2 and C3.

Combustion dynamics↗
NASA NTRS2019

Long Term Biological Treatment of Space Habitation Waste Waters in a One Stage MABR: Comparison of Operation for N and C Oxidation With and Without Simultaneous Denitrification

Aerobic biological stabilization has been previously demonstrated for full size MABR?s (CoMANDR 1.0, CoMANDR 2.0, and R-CoMANDR) over operating periods of ~1 year. These systems have successfully treated a variety of possible habitation waste streams including an ISS (urine + flush and humidity condensate) and Early Planetary Base (EPB) wastewater (urine, flush water, hygiene wastewater, and laundry). Biological stabilization has a number of advantages including: 1) elimination of hazardous pre-treat chemicals; 2) production of NOx species (that can be easily rejected by evaporative or membrane systems); 3) elimination of volatile organic constituents; 4) a low pH effluent that facilitates membrane and distillation processes; and 5) a effluent that produces a better quality and less hazardous brine for water recovery. Previous work has primarily evaluated aerobic operation in which organic carbon and nitrogen is converted to CO2 and NOx-, respectively. An alternative to aerobic operation would be to include anoxic operation to promote denitrification and production of N2 gas. This allows for production of make-up gas as well as reduces the O2 demand and can increase ammonia oxidation efficiency. We evaluated the operation of a full scale (2 crew/day) MABR operated to perform oxidation of organic carbon and nitrogen with and without simultaneous reduction of oxidized N to N2 gas, simultaneous nitrification denitrification (SNDN). The system was challenged with a variety of space habitation wastewaters ranging from an ISS composition to a possible EPB waste stream under both continuous and on-production feeding modes. The system has been operated for over 2.5 years. We report on an overall comparison of aerobic oxidation and SNDN operational regimes to evaluate the system with the best overall attributes to support recycling of space habitation waste streams.

Biological water processing↗
NASA NTRS2014

Aircraft Trajectory Design Based on Reducing the Combined Effects of Carbon-di-oxide, Nitrogen and Contrails

Aircraft operations need to meet the combined requirements of safety, efficiency, capacity and reduced environmental impact. Aircraft routes can be made efficient by flying wind optimal routes. However, the desire to reduce the impact of aviation emissions and contrails may result in trajectories, which deviate from wind optimal trajectories leading to extra fuel use. The lifetime associated with different emissions and contrails varies from a few hours to several hundred years. The impact of certain gases depends on the amount and location of the emission, and the decision-making horizon, in years, when the impact is estimated. The Absolute Global Temperature Potential (AGTP) is used as a metric to measure the combined effects of emissions and contrails. This paper extends earlier work by the authors to include the effect of oxides of nitrogen in the development of aircraft trajectories to reduce the combined effects of carbon dioxide, oxides of nitrogen (NOX) and contrails. The methodology is applied to air traffic in the continental US. The paper shows the trade-offs between reducing emissions and the cost of extra fuel using a fuel sensitivity index, defined as the reduction in AGTP per kg of fuel. The paper shows the performance of the optimization strategy for decision intervals of 10, 25 and 100 years. Based on the simplified models, the inclusion of NOX emissions has a slight influence on the minimal climate impact trajectories when the decision horizons are around 25 years.

Sridhar, Banavar↗
NASA NTRSDate not supplied

Biomass burning declines lead to large net reductions in NO2 concentrations over north equatorial Africa in spite of growing fossil fuel emissions

Socio-economic development in low and middle-income countries has been accompanied by increased emissions of air pollutants such as nitrogen oxides (NOx: nitrogen dioxide (NO2) + nitric oxide (NO)), which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, biomass burning—another important NOx source—has declined in Africa’s northern biomass burning region, attributed to changes in climate and anthropogenic fire management associated with agricultural development. Here we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to over 350 million people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the biomass burning season of November through February. Reductions in burned area explained the majority of these change in NO2 VCDs, but there were also weaker relationships between changes in NO2 VCDs and fossil fuel emissions over parts of West Africa, which were stronger during rainy season. Over Africa’s biomass burning regions, NO2 VCDs tended to decrease with increasing population density up to a threshold of approximately 180 people per km2, suggesting that anthropogenic activity causes a net reduction in NO2 emissions across roughly 90% of the continent’s biomass burning regions. In contrast to the widely-held perception that socio-economic development worsens air quality in low and middle-income nations, our results suggest that countries in Africa’s northern biomass burning region are following a different pathway, resulting in regional air quality benefits. However, these benefits may be lost with increasing fossil fuel use.

Biomass burning↗
NASA NTRSDate not supplied

Isotopically Tracking Nitrogen Oxides, Nitrous Acid, And Nitric Acid, Particulate Nitrate from Wildfire During FIREX-AQ

Wildfires are an important source of reactive nitrogen species including nitrogen oxides (NOx = NO + NO2) and nitrous acid (HONO), as well as products such as nitric acid (HNO3) and particulate nitrate (p-NO3-). These species have strongly influence air quality and climate. In summer of 2019 (July 25 —August 21), as part of the FIREX-AQ ground mission, we drove ~3000 miles and sampled smoke of different ages in both daytime and nighttime from 5 different wildfires in the western US. Using recently developed methods that have been validated in both laboratory and field settings, we conducted high time resolution collection of NOx, NO2, HONO, HNO3, and p-NO3- for off-line characterization of isotopic composition δ15N, δ18O and Δ17O (=δ17O−0.52 δ18O). δ15N serves as a potential tracer for tracking sources and reactive nitrogen cycling pathways, δ18O and Δ17O provide key information about oxidation pathways (i.e. O3 versus RO2). Our measured δ15N for HONO ranges from -4.9‰ to +5.2‰ and -8‰ to +5.2‰ respectively, in the majority overlapping with our prior lab controlled burning results, which suggests the capability of δ15N for tracing the biomass burning emissions against other sources including vehicular emissions and soil emissions. In addition, our measurements show δ18O and Δ17O for NO2 and HONO vary significantly day vs night, as well as in young smoke vs aged smoke, likely reflecting different oxidizing mechanisms under different smoke conditions. Preliminary results of isotopic signatures of all the above reactive nitrogen species will be presented, and their relationships will be explored to identify wildfire derived reactive nitrogen source signatures and to constrain atmospheric processing pathways (e.g. secondary formation of HONO) for different fires under various smoke conditions depending on fuel types, fire conditions and meteorological conditions.

Jiajue Chai↗
NASA NTRS2020

Global Environmental Impact of Supersonic Cruise Aircraft in the Stratosphere

We analyze the climate and ozone impacts of commercial supersonic aircraft using state-of-the-science modeling capabilities ranging from plume to global scale. A scenario-based approach captures variability and uncertainty in the impacts with market adoption, aircraft design choices and regulatory scenarios, focusing on different overland flight restrictions. We find that the notional aircraft considered could attract a market of up to 2.5% of year-2035 seat-kilometers. Overland flight restrictions reduce this market by 80–100%. In comparison to subsonic aircraft, contrails are found to be∼10 times less likely to form behind supersonic jets. A Mach 1.6 jet cruising at 17 km altitude causes 0.85 mDU of depletion per billion seat-km, with 54% of this impact attributable to sulfur emissions and 35% to NOx emissions. Asa result, we find a net non-CO2, non-contrail radiative forcing of−0.020 mW m−2per billion seat-km. Long-term adjoint simulations show that net ozone-neutral cruise can be achieved by flying near 14 km, subject to fuel sulfur content and NOx emissions index.

supersonic, Stratosphere, environment↗
NASA NTRS2021

Global Environmental Impact of Supersonic Cruise Aircraft in the Stratosphere

We analyze the climate and ozone impacts of commercial supersonic aircraft using state-of-the-science modeling capabilities ranging from plume to global scale. A scenario-based approach captures variability and uncertainty in the impacts with market adoption, aircraft design choices and regulatory scenarios, focusing on different overland flight restrictions. We find that the notional aircraft considered could attract a market of up to 2.5% of year-2035 seat-kilometers. Overland flight restrictions reduce this market by 80–100%. In comparison to subsonic aircraft, contrails are found to be ∼ 10 times less likely to form behind supersonic jets. A Mach 1.6 jet cruising at 17 km altitude causes 0.85 mDU of depletion per billion seat-km, with 54% of this impact attributable to sulfur emissions and 35% to NOx emissions. As a result, we find a net non-CO2, non-contrail radiative forcing of −0.020mWm−2 per billion seat-km. Long-term adjoint simulations show that net ozone-neutral cruise can be achieved by flying near 14 km, subject to fuel sulfur content and NOx emissions index.

Raymond L Speth↗
NASA NTRS2021

Effective radiative forcing from emissions of reactive gases and aerosols - a multi-model comparison

This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NOX, volatile organic compounds (VOCs; including CO), SO2, NH3, black carbon, organic carbon, and concentrations of methane, N2O and ozone-depleting halocarbons, using CMIP6 models. Concentration and emission changes of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, stratospheric water vapour, secondary inorganic and organic aerosol, and methane. Where possible we break down the ERFs from each emitted species into the contributions from the composition changes. The ERFs are calculated for each of the models that participated in the AerChemMIP experiments as part of the CMIP6 project, where the relevant model output was available. The 1850 to 2014 multi-model mean ERFs (± standard deviations) are −1.03 ± 0.37 W/sq.m for SO2 emissions, −0.25 ± 0.09 W/sq.m for organic carbon (OC), 0.15 ± 0.17 W/sq.m for black carbon (BC) and −0.07 ± 0.01 W/sq.m for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W/sq.m. The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W/sq.m for methane (CH4), 0.26 ± 0.07 W/sq.m for nitrous oxide (N2O) and 0.12 ± 0.2 W/sq.m for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NOx), volatile organic compounds and both together (O3) lead to ERFs of 0.14 ± 0.13, 0.09 ± 0.14 and 0.20 ± 0.07 W/sq.m respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.

radiative forcing↗
NASA NTRS2021

Reductions in NO2 Burden Over North Equatorial Africa from Decline in Biomass Burning in Spite of Growing Fossil Fuel Use, 2005 to 2017

Socioeconomic development in low- and middle-income countries has been accompanied by increased emissions of air pollutants, such as nitrogen oxides [NOx: nitrogen dioxide (NO2) + nitric oxide (NO)], which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, landscape biomass burning—another important NOx source—has declined in north equatorial Africa, attributed to changes in climate and anthropogenic fire management. Here, we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to hundreds of millions of people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the dry season of November through February. Reductions in burned area explained the majority of variation in NO2 VCDs, though changes in fossil fuel emissions also explained some variation. Over Africa’s biomass burning regions, raising mean GDP density (USD·km−2) above its lowest levels is associated with lower NO2 VCDs during the dry season, suggesting that economic development mitigates net NO2 emissions during these highly polluted months. In contrast to the traditional notion that socioeconomic development increases air pollutant concentrations in low- and middle-income nations, our results suggest that countries in Africa’s northern biomass-burning region are following a different pathway during the fire season, resulting in potential air quality benefits. However, these benefits may be lost with increasing fossil fuel use and are absent during the rainy season.

air pollution↗
NASA NTRS2021

Evaluating Drought Responses of Surface Ozone Precursor Proxies: Variations With Land Cover Type, Precipitation, and Temperature

Prior work suggests drought exacerbates US air quality by increasing surface ozone concentrations. We analyze 2005–2015 tropospheric column concentrations of two trace gases that serve as proxies for surface ozone precursors retrieved from the OMI/Aura satellite: Nitrogen dioxide (ΩNO2; NOx proxy) and formaldehyde (ΩHCHO; VOC proxy). We find 3.5% and 7.7% summer drought enhancements (classified by SPEI) for ΩNO2 and ΩHCHO, respectively, corroborating signals previously extracted from ground‐level observations. When we subset by land cover type, the strongest ΩHCHO drought enhancement (10%) occurs in the woody savannas of the Southeast US. By isolating the influences of precipitation and temperature, we infer that enhanced biogenic VOC emissions in this region increase ΩHCHO independently with both high temperature and low precipitation during drought. The strongest ΩNO2 drought enhancement (6.0%) occurs over Midwest US croplands and grasslands, which we infer to reflect the sensitivity of soil NOx emissions to temperature.

drought↗
NASA NTRS2021

Extreme Ozone Loss Following Nuclear War Results in Enhanced Surface Ultraviolet Radiation

For the first time, we use a modern climate model with interactive chemistry including the effects of aerosols on photolysis rates to simulate the consequences of regional and global scale nuclear wars (injecting 5 and 150 Tg of soot respectively) for the ozone layer and surface ultraviolet (UV) light. For a global nuclear war, heating in the stratosphere, reduced photolysis, and an increase in catalytic loss from the Hox cycle cause a 15 year-long reduction in the ozone column, with a peak loss of 75% globally and 65% in the tropics. This is larger than predictions from the 1980s, which assumed large injections of nitrogen oxides (NOx),but did not include the effects of smoke. NOx from the fireball and the fires provide a small (5%) Increase to the global average ozone loss for the first few years. Initially, soot would shield the surface from UV-B, but UV Index values would become extreme: greater than 35in the tropics for 4years, and greater than 45during the summer in the southern polar regions for 3 years. For a regional war, global column ozone would be reduced by 25% with recovery taking 12 years. This is similar to previous simulations, but with a faster recovery time due to a shorter lifetime for soot in our simulations. In-line photolysis provides process specific action spectra enabling future integration with biogeochemistry models and allows output that quantifies the potential health impacts from changes in surface UV for this and other larger aerosol injections.

nuclear war↗
NASA NTRS2022

Faster Tropical Upper Stratospheric Upwelling Drives Changes in Ozone Chemistry

Tropospheric trends in long-lived source gases N2O and the chlorofluorocarbons (CFCs) cause trends in O3 through changes in their reactive product gases. Transport affects the product gases because it controls the distribution of the long-lived source gases. We find that large changes in tropical upwelling 10-5 hPa since 2012 have strengthened the northern branch of the upper stratospheric (UpS) transport circulation, dramatically altering the abundances of N2O and its odd nitrogen product gases, NOx and HNO3. Increased upwelling is connected to stronger and more frequent Quasi-Biennial Oscillation easterly winds at 10 hPa and above. We use simulations with and without time varying MERRA2 meteorology to quantify the impact of dynamical changes on O3 loss via the NOx and ClOx cycles. We find that dynamical impacts on these cycles explain the mid-stratospheric tropical O3 increase and Arctic UpS O3 decrease since 2005.

Middle atmosphere chemistry and composition↗
NASA NTRS2023

Heterogeneity and Chemical Reactivity of the Remote Troposphere Defined By Aircraft Measurements - Corrected

The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O3 and CH4 (O3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O3 and CH4. Models distinctly underestimate O3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation.

Tropospheric Chemistry↗
NASA NTRS2023

Arctic Tropospheric Ozone: Assessment of Current Knowledge and Model Performance

As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.

Arctic↗
NASA NTRS2022

Secondary Inorganic Aerosol Chemistry and Its Impact on Atmospheric Visibility Over an Ammonia-Rich Urban Area in Central Taiwan

This study investigated the hourly inorganic aerosol chemistry and its impact on atmospheric visibility over an urban area in Central Taiwan, by relying on measurements of aerosol light extinction, inorganic gases, and PM 2.5 water-soluble ions (WSIs), and simulations from a thermodynamic equilibrium model. On average, the sulfate (SO 4 2− ), nitrate (NO 3 − ), and ammonium (NH 4 + ) components (SNA) contributed ∼90% of WSI concentrations, which in turn made up about 50% of the PM 2.5 mass. During the entire observation period, PM 2.5 and SNA concentrations, aerosol pH, aerosol liquid water content (ALWC), and sulfur and nitrogen conversion ratios all increased with decreasing visibility. In particular, the NO 3 − contribution to PM 2.5 increased, whereas the SO 4 2− contribution decreased, with decreasing visibility. The diurnal variations of the above parameters indicate that the interaction and likely mutual promotion between NO 3 − and ALWC enhanced the hygroscopicity and aqueous-phase reactions conducive for NO 3 − formation, thus led to severely impaired visibility. The high relative humidity (RH) at the study area (average 70.7%) was a necessary but not sole factor leading to enhanced NO 3 − formation, which was more directly associated with elevated ALWC and aerosol pH. Simulations from the thermodynamic model depict that the inorganic aerosol system in the study area was characterized by fully neutralized SO 4 2− (i.e. a saturated factor in visibility reduction) and excess NH 4 + amidst a NH 3 -rich environment. As a result, PM 2.5 composition was most sensitive to gas-phase HNO 3 , and hence NOx, and relatively insensitive to NH 3 . Consequently, a reduction of NOx would result in instantaneous cuts of NO 3 − , PM 2.5 , and ALWC, and hence improved visibility. On the other hand, a substantial amount of NH 3 reduction (>70%) would be required to lower the aerosol pH, driving more than 50% of the particulate phase NO 3 − to the gas phase, thereby making NH 3 a limiting factor in shifting PM 2.5 composition.

aerosol chemistry↗