Atmospheric Aerosol Emissions Related to the Mediterranean Seawater Biogeochemistry

Science.gov (United States)

Sellegri, K.; Schwier, A.; Rose, C.; Gazeau, F. P. H.; Guieu, C.; D'anna, B.; Ebling, A. M.; Pey, J.; Marchand, N.; Charriere, B.; Sempéré, R.; Mas, S.

2016-02-01

Marine aerosols contribute significantly to the global aerosol load and consequently has an important impact on the Earth's climate. Different factors influence the way they are produced at the air/seawater interface. The sea state (whitecap coverage, temperature, etc. ) influence the size and concentration of primarily produced particles but also biogeochemical characteristics of the seawater influence both the physical and chemical primary fluxes to the atmosphere. An additional aerosol source of marine aerosol to the atmosphere is the formation of new particles by gaz-to-particle conversion, i.e. nucleation. How the seawater and surface microlayer biogeochemical compositions influences the aerosol emissions is still a large debate. In order to study marine emissions, one approach is to use semi-controlled environments such as mesocosms. Within the MedSea and SAM projects, we characterize the primary Sea Spray Aerosol (SSA) during mesocosms experiments performed during different seasons in the Mediteranean Sea. Mesocosms were either left unchanged as control or enriched by addition of nutriments in order to create different levels of phytoplanctonic activities. The mesocosms waters were daily analyzed for their chemical and biological composition (DOC, CDOM, TEP, Chl-a, virus, bacteria, phytoplankton and zooplankton concentrations). SSA production by bubble bursting was daily simulated in a dedicated set-up. The size segregated SSA number fluxes, cloud condensation nuclei (CCN) properties, and chemical composition were determined as a function of the seawater characteristics. We show that the SSA organic content was clearly correlated to the seawater Chl-a level, provided that the mesocosm was not enriched to create an artificial phytoplanctonic bloom. In our experiments, the enrichment of the seawater with natural surface microlayer did not impact the SSA organic content nor its CCN properties. At last, nucleation of secondary particles were observed to occur in

A simple parameterization of aerosol emissions in RAMS

Science.gov (United States)

Letcher, Theodore

Throughout the past decade, a high degree of attention has been focused on determining the microphysical impact of anthropogenically enhanced concentrations of Cloud Condensation Nuclei (CCN) on orographic snowfall in the mountains of the western United States. This area has garnered a lot of attention due to the implications this effect may have on local water resource distribution within the Region. Recent advances in computing power and the development of highly advanced microphysical schemes within numerical models have provided an estimation of the sensitivity that orographic snowfall has to changes in atmospheric CCN concentrations. However, what is still lacking is a coupling between these advanced microphysical schemes and a real-world representation of CCN sources. Previously, an attempt to representation the heterogeneous evolution of aerosol was made by coupling three-dimensional aerosol output from the WRF Chemistry model to the Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) (Ward et al. 2011). The biggest problem associated with this scheme was the computational expense. In fact, the computational expense associated with this scheme was so high, that it was prohibitive for simulations with fine enough resolution to accurately represent microphysical processes. To improve upon this method, a new parameterization for aerosol emission was developed in such a way that it was fully contained within RAMS. Several assumptions went into generating a computationally efficient aerosol emissions parameterization in RAMS. The most notable assumption was the decision to neglect the chemical processes in formed in the formation of Secondary Aerosol (SA), and instead treat SA as primary aerosol via short-term WRF-CHEM simulations. While, SA makes up a substantial portion of the total aerosol burden (much of which is made up of organic material), the representation of this process is highly complex and highly expensive within a numerical

Primary marine aerosol emissions from the Mediterranean Sea during pre-bloom and oligotrophic conditions: correlations to seawater chlorophyll a from a mesocosm study

Science.gov (United States)

Schwier, A. N.; Rose, C.; Asmi, E.; Ebling, A. M.; Landing, W. M.; Marro, S.; Pedrotti, M.-L.; Sallon, A.; Iuculano, F.; Agusti, S.; Tsiola, A.; Pitta, P.; Louis, J.; Guieu, C.; Gazeau, F.; Sellegri, K.

2015-07-01

The effect of ocean acidification and changing water conditions on primary (and secondary) marine aerosol emissions is not well understood on a regional or a global scale. To investigate this effect as well as the indirect effect on aerosol that changing biogeochemical parameters can have, ~ 52 m3 pelagic mesocosms were deployed for several weeks in the Mediterranean Sea during both winter pre-bloom and summer oligotrophic conditions and were subjected to various levels of CO2 to simulate the conditions foreseen in this region for the coming decades. After seawater sampling, primary bubble-bursting aerosol experiments were performed using a plunging water jet system to test both chemical and physical aerosol parameters (10-400 nm). Comparing results obtained during pre-bloom and oligotrophic conditions, we find the same four log-normal modal diameters (18.5 ± 0.6, 37.5 ± 1.4, 91.5 ± 2.0, 260 ± 3.2 nm) describing the aerosol size distribution during both campaigns, yet pre-bloom conditions significantly increased the number fraction of the second (Aitken) mode, with an amplitude correlated to virus-like particles, heterotrophic prokaryotes, TEPs (transparent exopolymeric particles), chlorophyll a and other pigments. Organic fractions determined from kappa closure calculations for the diameter, Dp ~ 50 nm, were much larger during the pre-bloom period (64 %) than during the oligotrophic period (38 %), and the organic fraction decreased as the particle size increased. Combining data from both campaigns together, strong positive correlations were found between the organic fraction of the aerosol and chlorophyll a concentrations, heterotrophic and autotrophic bacteria abundance, and dissolved organic carbon (DOC) concentrations. As a consequence of the changes in the organic fraction and the size distributions between pre-bloom and oligotrophic periods, we find that the ratio of cloud condensation nuclei (CCN) to condensation nuclei (CN) slightly decreased during the

Small global effect on terrestrial net primary production due to increased fossil fuel aerosol emissions from East Asia during the last decade.

Science.gov (United States)

O'Sullivan, Michael; Rap, Alex; Reddington, Carly; Spracklen, Dominick; Buermann, Wolfgang

2016-04-01

The global terrestrial carbon sink has increased since the start of this century at a time of rapidly growing carbon dioxide emissions from fossil fuel burning. Here we test the hypothesis that increases in atmospheric aerosols from fossil fuel burning have increased the diffuse fraction of incoming solar radiation and the efficiency of photosynthesis leading to increased plant carbon uptake. Using a combination of atmospheric and biospheric models, we find that changes in diffuse light associated with fossil fuel aerosol emission accounts for only 2.8% of the increase in global net primary production (1.221 PgC/yr) over the study period 1998 to 2007. This relatively small global signal is however a result of large regional compensations. Over East Asia, the strong increase in fossil fuel emissions contributed nearly 70% of the increased plant carbon uptake (21 TgC/yr), whereas the declining fossil fuel aerosol emissions in Europe and North America contributed negatively (-16% and -54%, respectively) to increased plant carbon uptake. At global scale, we also find the CO2 fertilization effect on photosynthesis to be the dominant driver of increased plant carbon uptake, in line with previous studies. These results suggest that further research into alternative mechanisms by which fossil fuel emissions could increase carbon uptake, such as nitrogen deposition and carbon-nitrogen interactions, is required to better understand a potential link between the recent changes in fossil fuel emissions and terrestrial carbon uptake.

Secondary organic aerosol formation from in-use motor vehicle emissions using a potential aerosol mass reactor.

Science.gov (United States)

Tkacik, Daniel S; Lambe, Andrew T; Jathar, Shantanu; Li, Xiang; Presto, Albert A; Zhao, Yunliang; Blake, Donald; Meinardi, Simone; Jayne, John T; Croteau, Philip L; Robinson, Allen L

2014-10-07

Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

Climate Impacts From a Removal of Anthropogenic Aerosol Emissions

Science.gov (United States)

Samset, B. H.; Sand, M.; Smith, C. J.; Bauer, S. E.; Forster, P. M.; Fuglestvedt, J. S.; Osprey, S.; Schleussner, C.-F.

2018-01-01

Limiting global warming to 1.5 or 2.0°C requires strong mitigation of anthropogenic greenhouse gas (GHG) emissions. Concurrently, emissions of anthropogenic aerosols will decline, due to coemission with GHG, and measures to improve air quality. However, the combined climate effect of GHG and aerosol emissions over the industrial era is poorly constrained. Here we show the climate impacts from removing present-day anthropogenic aerosol emissions and compare them to the impacts from moderate GHG-dominated global warming. Removing aerosols induces a global mean surface heating of 0.5-1.1°C, and precipitation increase of 2.0-4.6%. Extreme weather indices also increase. We find a higher sensitivity of extreme events to aerosol reductions, per degree of surface warming, in particular over the major aerosol emission regions. Under near-term warming, we find that regional climate change will depend strongly on the balance between aerosol and GHG forcing.

Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

Science.gov (United States)

Spracklen, D. V.; Carslaw, K. S.; Merikanto, J.; Mann, G. W.; Reddington, C. L.; Pickering, S.; Ogren, J. A.; Andrews, E.; Baltensperger, U.; Weingartner, E.; Boy, M.; Kulmala, M.; Laakso, L.; Lihavainen, H.; Kivekäs, N.; Komppula, M.; Mihalopoulos, N.; Kouvarakis, G.; Jennings, S. G.; O'Dowd, C.; Birmili, W.; Wiedensohler, A.; Weller, R.; Gras, J.; Laj, P.; Sellegri, K.; Bonn, B.; Krejci, R.; Laaksonen, A.; Hamed, A.; Minikin, A.; Harrison, R. M.; Talbot, R.; Sun, J.

2010-05-01

We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300-2000 cm-3 in the marine boundary layer and free troposphere (FT) and 1000-10 000 cm-3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2-10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=-88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=-25%). Simulated CN concentrations in the continental BL were also biased low (NMB=-74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation

Primary gas- and particle-phase emissions and secondary organic aerosol production from gasoline and diesel off-road engines.

Science.gov (United States)

Gordon, Timothy D; Tkacik, Daniel S; Presto, Albert A; Zhang, Mang; Jathar, Shantanu H; Nguyen, Ngoc T; Massetti, John; Truong, Tin; Cicero-Fernandez, Pablo; Maddox, Christine; Rieger, Paul; Chattopadhyay, Sulekha; Maldonado, Hector; Maricq, M Matti; Robinson, Allen L

2013-12-17

Dilution and smog chamber experiments were performed to characterize the primary emissions and secondary organic aerosol (SOA) formation from gasoline and diesel small off-road engines (SOREs). These engines are high emitters of primary gas- and particle-phase pollutants relative to their fuel consumption. Two- and 4-stroke gasoline SOREs emit much more (up to 3 orders of magnitude more) nonmethane organic gases (NMOGs), primary PM and organic carbon than newer on-road gasoline vehicles (per kg of fuel burned). The primary emissions from a diesel transportation refrigeration unit were similar to those of older, uncontrolled diesel engines used in on-road vehicles (e.g., premodel year 2007 heavy-duty diesel trucks). Two-strokes emitted the largest fractional (and absolute) amount of SOA precursors compared to diesel and 4-stroke gasoline SOREs; however, 35-80% of the NMOG emissions from the engines could not be speciated using traditional gas chromatography or high-performance liquid chromatography. After 3 h of photo-oxidation in a smog chamber, dilute emissions from both 2- and 4-stroke gasoline SOREs produced large amounts of semivolatile SOA. The effective SOA yield (defined as the ratio of SOA mass to estimated mass of reacted precursors) was 2-4% for 2- and 4-stroke SOREs, which is comparable to yields from dilute exhaust from older passenger cars and unburned gasoline. This suggests that much of the SOA production was due to unburned fuel and/or lubrication oil. The total PM contribution of different mobile source categories to the ambient PM burden was calculated by combining primary emission, SOA production and fuel consumption data. Relative to their fuel consumption, SOREs are disproportionately high total PM sources; however, the vastly greater fuel consumption of on-road vehicles renders them (on-road vehicles) the dominant mobile source of ambient PM in the Los Angeles area.

Regional aerosol emissions and temperature response: Local and remote climate impacts of regional aerosol forcing

Science.gov (United States)

Lewinschal, Anna; Ekman, Annica; Hansson, Hans-Christen

2017-04-01

Emissions of anthropogenic aerosols vary substantially over the globe and the short atmospheric residence time of aerosols leads to a highly uneven radiative forcing distribution, both spatially and temporally. Regional aerosol radiative forcing can, nevertheless, exert a large influence on the temperature field away from the forcing region through changes in heat transport or the atmospheric or ocean circulation. Moreover, the global temperature response distribution to aerosol forcing may vary depending on the geographical location of the forcing. In other words, the climate sensitivity in one region can vary depending on the location of the forcing. The surface temperature distribution response to changes in sulphate aerosol forcing caused by sulphur dioxide (SO2) emission perturbations in four different regions is investigated using the Norwegian Earth System Model (NorESM). The four regions, Europe, North America, East and South Asia, are all regions with historically high aerosol emissions and are relevant from both an air-quality and climate policy perspective. All emission perturbations are defined relative to the year 2000 emissions provided for the Coupled Model Intercomparison Project phase 5. The global mean temperature change per unit SO2 emission change is similar for all four regions for similar magnitudes of emissions changes. However, the global temperature change per unit SO2 emission in simulations where regional SO2 emission were removed is substantially higher than that obtained in simulations where regional SO2 emissions were increased. Thus, the climate sensitivity to regional SO2 emissions perturbations depends on the magnitude of the emission perturbation in NorESM. On regional scale, on the other hand, the emission perturbations in different geographical locations lead to different regional temperature responses, both locally and in remote regions. The results from the model simulations are used to construct regional temperature potential

Primary marine aerosol emissions from the Mediterranean Sea during pre-bloom and oligotrophic conditions: correlations to seawater chlorophyll a from a mesocosm study

OpenAIRE

Schwier , A. N.; Rose , C.; Asmi , E.; Ebling , A. M.; Landing , W. M.; Marro , S.; Pedrotti , M.-L.; Sallon , A.; Iuculano , F.; Agusti , S.; Tsiola , A.; Pitta , P.; Louis , J.; Guieu , C.; Gazeau , F.

2015-01-01

The effect of ocean acidification and changing water conditions on primary (and secondary) marine aerosol emissions is not well understood on a regional or a global scale. To investigate this effect as well as the indirect effect on aerosol that changing biogeochemical parameters can have, ~ 52 m3 pelagic mesocosms were deployed for several weeks in the Mediterranean Sea during both winter pre-bloom and summer oligotrophic conditions and were subjected to various levels of C...

Physico-Chemical Evolution of Organic Aerosol from Wildfire Emissions

Science.gov (United States)

Croteau, P.; Jathar, S.; Akherati, A.; Galang, A.; Tarun, S.; Onasch, T. B.; Lewane, L.; Herndon, S. C.; Roscioli, J. R.; Yacovitch, T. I.; Fortner, E.; Xu, W.; Daube, C.; Knighton, W. B.; Werden, B.; Wood, E.

2017-12-01

Wildfires are the largest combustion-related source of carbonaceous emissions to the atmosphere; these include direct emissions of black carbon (BC), primary organic aerosol (POA) and semi-volatile, intermediate-volatility, and volatile organic compounds (SVOCs, IVOCs, and VOCs). However, there are large uncertainties surrounding the evolution of these carbonaceous emissions as they are physically and chemically transformed in the atmosphere. To understand these transformations, we performed sixteen experiments using an environmental chamber to simulate day- and night-time chemistry of gas- and aerosol-phase emissions from 6 different fuels at the Fire Laboratory in Missoula, MT. Across the test matrix, the experiments simulated 2 to 8 hours of equivalent day-time aging (with the hydroxyl radical and ozone) or several hours of night-time aging (with the nitrate radical). Aging resulted in an average organic aerosol (OA) mass enhancement of 28% although the full range of OA mass enhancements varied between -10% and 254%. These enhancement findings were consistent with chamber and flow reactor experiments performed at the Fire Laboratory in 2010 and 2012 but, similar to previous studies, offered no evidence to link the OA mass enhancement to fuel type or oxidant exposure. Experiments simulating night-time aging resulted in an average OA mass enhancement of 10% and subsequent day-time aging resulted in a decrease in OA mass of 8%. While small, for the first time, these experiments highlighted the continuous nature of the OA evolution as the wildfire smoke cycled through night- and day-time processes. Ongoing work is focussed on (i) quantifying bulk compositional changes in OA, (ii) comparing the near-field aging simulated in this work with far-field aging simulated during the same campaign (via a mini chamber and flow tube) and (iii) integrating wildfire smoke aging datasets over the past decade to examine the relationship between OA mass enhancement ratios, modified

Semi-quantitative characterisation of ambient ultrafine aerosols resulting from emissions of coal fired power stations

International Nuclear Information System (INIS)

Hinkley, J.T.; Bridgman, H.A.; Buhre, B.J.P.; Gupta, R.P.; Nelson, P.F.; Wall, T.F.

2008-01-01

Emissions from coal fired power stations are known to be a significant anthropogenic source of fine atmospheric particles, both through direct primary emissions and secondary formation of sulfate and nitrate from emissions of gaseous precursors. However, there is relatively little information available in the literature regarding the contribution emissions make to the ambient aerosol, particularly in the ultrafine size range. In this study, the contribution of emissions to particles smaller than 0.3 μm in the ambient aerosol was examined at a sampling site 7 km from two large Australian coal fired power stations equipped with fabric filters. A novel approach was employed using conditional sampling based on sulfur dioxide (SO 2 ) as an indicator species, and a relatively new sampler, the TSI Nanometer Aerosol Sampler. Samples were collected on transmission electron microscope (TEM) grids and examined using a combination of TEM imaging and energy dispersive X-ray (EDX) analysis for qualitative chemical analysis. The ultrafine aerosol in low SO 2 conditions was dominated by diesel soot from vehicle emissions, while significant quantities of particles, which were unstable under the electron beam, were observed in the high SO 2 samples. The behaviour of these particles was consistent with literature accounts of sulfate and nitrate species, believed to have been derived from precursor emissions from the power stations. A significant carbon peak was noted in the residues from the evaporated particles, suggesting that some secondary organic aerosol formation may also have been catalysed by these acid seed particles. No primary particulate material was observed in the minus 0.3 μm fraction. The results of this study indicate the contribution of species more commonly associated with gas to particle conversion may be more significant than expected, even close to source

Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM): VOLCANIC AEROSOLS DERIVED FROM EMISSIONS

Energy Technology Data Exchange (ETDEWEB)

Mills, Michael J. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Schmidt, Anja [School of Earth and Environment, University of Leeds, Leeds UK; Easter, Richard [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Solomon, Susan [Department of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge Massachusetts USA; Kinnison, Douglas E. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Ghan, Steven J. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Neely, Ryan R. [School of Earth and Environment, University of Leeds, Leeds UK; National Centre for Atmospheric Science, University of Leeds, Leeds UK; Marsh, Daniel R. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Conley, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Bardeen, Charles G. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Gettelman, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA

2016-03-06

Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptions between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.

Climate and health implications of future aerosol emission scenarios

Science.gov (United States)

Partanen, Antti-Ilari; Landry, Jean-Sébastien; Damon Matthews, H.

2018-02-01

Anthropogenic aerosols have a net cooling effect on climate and also cause adverse health effects by degrading air quality. In this global-scale sensitivity study, we used a combination of the aerosol-climate model ECHAM-HAMMOZ and the University of Victoria Earth System Climate Model to assess the climate and health effects of aerosols emissions from three Representative Concentration Pathways (RCP2.6, RCP4.5, and RCP8.5) and two new (LOW and HIGH) aerosol emission scenarios derived from RCP4.5, but that span a wider spectrum of possible future aerosol emissions. All simulations had CO2 emissions and greenhouse gas forcings from RCP4.5. Aerosol forcing declined similarly in the standard RCP aerosol emission scenarios: the aerosol effective radiative forcing (ERF) decreased from -1.3 W m-2 in 2005 to between -0.1 W m-2 and -0.4 W m-2 in 2100. The differences in ERF were substantially larger between LOW (-0.02 W m-2 in 2100) and HIGH (-0.8 W m-2) scenarios. The global mean temperature difference between the simulations with standard RCP aerosol emissions was less than 0.18 °C, whereas the difference between LOW and HIGH reached 0.86 °C in 2061. In LOW, the rate of warming peaked at 0.48 °C per decade in the 2030s, whereas in HIGH it was the lowest of all simulations and never exceeded 0.23 °C per decade. Using present-day population density and baseline mortality rates for all scenarios, PM2.5-induced premature mortality was 2 371 800 deaths per year in 2010 and 525 700 in 2100 with RCP4.5 aerosol emissions; in HIGH, the premature mortality reached its maximum value of 2 780 800 deaths per year in 2030, whereas in LOW the premature mortality at 2030 was below 299 900 deaths per year. Our results show potential trade-offs in aerosol mitigation with respect to climate change and public health as ambitious reduction of aerosol emissions considerably increased warming while decreasing mortality.

Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

Directory of Open Access Journals (Sweden)

D. V. Spracklen

2010-05-01

Full Text Available We synthesised observations of total particle number (CN concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm⁻³ in the marine boundary layer and free troposphere (FT and 1000–10 000 cm⁻³ in the continental boundary layer (BL. Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R²=0.46 but fail to explain the observed seasonal cycle (R²=0.1. The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88% unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%. Simulated CN concentrations in the continental BL were also biased low (NMB=−74% unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one or kinetic-type mechanism (J proportional to sulfuric acid to the power two with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R²=0.3 than by increasing the number emission from primary anthropogenic sources (R²=0.18. The nucleation constants that resulted in best overall match between model and observed CN concentrations were

Potential sensitivity of photosynthesis and isoprene emission to direct radiative effects of atmospheric aerosol pollution

Science.gov (United States)

Strada, Susanna; Unger, Nadine

2016-04-01

A global Earth system model is applied to quantify the impacts of direct anthropogenic aerosol effective radiative forcing on gross primary productivity (GPP) and isoprene emission. The impacts of different pollution aerosol sources (anthropogenic, biomass burning, and non-biomass burning) are investigated by performing sensitivity experiments. The model framework includes all known light and meteorological responses of photosynthesis, but uses fixed canopy structures and phenology. On a global scale, our results show that global land carbon fluxes (GPP and isoprene emission) are not sensitive to pollution aerosols, even under a global decline in surface solar radiation (direct + diffuse) by ˜ 9 %. At a regional scale, GPP and isoprene emission show a robust but opposite sensitivity to pollution aerosols in regions where forested canopies dominate. In eastern North America and Eurasia, anthropogenic pollution aerosols (mainly from non-biomass burning sources) enhance GPP by +5-8 % on an annual average. In the northwestern Amazon Basin and central Africa, biomass burning aerosols increase GPP by +2-5 % on an annual average, with a peak in the northwestern Amazon Basin during the dry-fire season (+5-8 %). The prevailing mechanism varies across regions: light scattering dominates in eastern North America, while a reduction in direct radiation dominates in Europe and China. Aerosol-induced GPP productivity increases in the Amazon and central Africa include an additional positive feedback from reduced canopy temperatures in response to increases in canopy conductance. In Eurasia and northeastern China, anthropogenic pollution aerosols drive a decrease in isoprene emission of -2 to -12 % on an annual average. Future research needs to incorporate the indirect effects of aerosols and possible feedbacks from dynamic carbon allocation and phenology.

The role of reduced aerosol precursor emissions in driving near-term warming

International Nuclear Information System (INIS)

Gillett, Nathan P; Von Salzen, Knut

2013-01-01

The representative concentration pathway (RCP) scenarios all assume stringent emissions controls on aerosols and their precursors, and hence include progressive decreases in aerosol and aerosol precursor emissions through the 21st century. Recent studies have suggested that the resultant decrease in aerosols could drive rapid near-term warming, which could dominate the effects of greenhouse gas (GHG) increases in the coming decades. In CanESM2 simulations, we find that under the RCP 2.6 scenario, which includes the fastest decrease in aerosol and aerosol precursor emissions, the contribution of aerosol reductions to warming between 2000 and 2040 is around 30%. Moreover, the rate of warming in the RCP 2.6 simulations declines gradually from its present-day value as GHG emissions decrease. Thus, while aerosol emission reductions contribute to gradual warming through the 21st century, we find no evidence that aerosol emission reductions drive particularly rapid near-term warming in this scenario. In the near-term, as in the long-term, GHG increases are the dominant driver of warming. (letter)

Wintertime Arctic Ocean sea water properties and primary marine aerosol concentrations

Directory of Open Access Journals (Sweden)

J. Zábori

2012-11-01

Full Text Available Sea spray aerosols are an important part of the climate system through their direct and indirect effects. Due to the diminishing sea ice, the Arctic Ocean is one of the most rapidly changing sea spray aerosol source areas. However, the influence of these changes on primary particle production is not known.

In laboratory experiments we examined the influence of Arctic Ocean water temperature, salinity, and oxygen saturation on primary particle concentration characteristics. Sea water temperature was identified as the most important of these parameters. A strong decrease in sea spray aerosol production with increasing water temperature was observed for water temperatures between −1°C and 9°C. Aerosol number concentrations decreased from at least 1400 cm⁻³ to 350 cm⁻³. In general, the aerosol number size distribution exhibited a robust shape with one mode close to dry diameter D_p 0.2 μm with approximately 45% of particles at smaller sizes. Changes in sea water temperature did not result in pronounced change of the shape of the aerosol size distribution, only in the magnitude of the concentrations. Our experiments indicate that changes in aerosol emissions are most likely linked to changes of the physical properties of sea water at low temperatures. The observed strong dependence of sea spray aerosol concentrations on sea water temperature, with a large fraction of the emitted particles in the typical cloud condensation nuclei size range, provide strong arguments for a more careful consideration of this effect in climate models.

Potential sensitivity of photosynthesis and isoprene emission to direct radiative effects of atmospheric aerosol pollution

Directory of Open Access Journals (Sweden)

S. Strada

2016-04-01

Full Text Available A global Earth system model is applied to quantify the impacts of direct anthropogenic aerosol effective radiative forcing on gross primary productivity (GPP and isoprene emission. The impacts of different pollution aerosol sources (anthropogenic, biomass burning, and non-biomass burning are investigated by performing sensitivity experiments. The model framework includes all known light and meteorological responses of photosynthesis, but uses fixed canopy structures and phenology. On a global scale, our results show that global land carbon fluxes (GPP and isoprene emission are not sensitive to pollution aerosols, even under a global decline in surface solar radiation (direct + diffuse by  ∼ 9 %. At a regional scale, GPP and isoprene emission show a robust but opposite sensitivity to pollution aerosols in regions where forested canopies dominate. In eastern North America and Eurasia, anthropogenic pollution aerosols (mainly from non-biomass burning sources enhance GPP by +5–8 % on an annual average. In the northwestern Amazon Basin and central Africa, biomass burning aerosols increase GPP by +2–5 % on an annual average, with a peak in the northwestern Amazon Basin during the dry-fire season (+5–8 %. The prevailing mechanism varies across regions: light scattering dominates in eastern North America, while a reduction in direct radiation dominates in Europe and China. Aerosol-induced GPP productivity increases in the Amazon and central Africa include an additional positive feedback from reduced canopy temperatures in response to increases in canopy conductance. In Eurasia and northeastern China, anthropogenic pollution aerosols drive a decrease in isoprene emission of −2 to −12 % on an annual average. Future research needs to incorporate the indirect effects of aerosols and possible feedbacks from dynamic carbon allocation and phenology.

Laboratory Measurements of Biomass Cook-stove Emissions Aged in an Oxidation Flow Reactor: Influence of Combustion and Aging Conditions on Aerosols

Science.gov (United States)

Grieshop, A. P.; Reece, S. M.; Sinha, A.; Wathore, R.

2016-12-01

Combustion in rudimentary and improved cook-stoves used by billions in developing countries can be a regionally dominant contributor to black carbon (BC), primary organic aerosols (POA) and precursors for secondary organic aerosol (SOA). Recent studies suggest that SOA formed during photo-oxidation of primary emissions from biomass burning may make important contribution to its atmospheric impacts. However, the extent to which stove type and operating conditions affect the amount, composition and characteristics of SOA formed from the aging of cookstoves emissions is still largely undetermined. Here we present results from experiments with a field portable oxidation flow reactor (F-OFR) designed to assess aging of cook-stove emissions in both laboratory and field settings. Laboratory tests results are used to compare the quantity and properties of fresh and aged emissions from a traditional open fire and twp alternative stove designs operated on the standard and alternate testing protocols. Diluted cookstove emissions were exposed to a range of oxidant concentrations in the F-OFR. Primary emissions were aged both on-line, to study the influence of combustion variability, and sampled from batched emissions in a smog chamber to examine different aging conditions. Data from real-time particle- and gas-phase instruments and integrated filter samples were collected up and down stream of the OFR. The properties of primary emissions vary strongly with stove type and combustion conditions (e.g. smoldering versus flaming). Experiments aging diluted biomass emissions from distinct phases of stove operation (smoldering and flaming) showed peak SOA production for both phases occurred between 3 and 6 equivalent days of aging with slightly greater production observed in flaming phase emissions. Changing combustion conditions had a stronger influence than aging on POA+SOA `emission factors'. Aerosol Chemical Speciation Monitor data show a substantial evolution of aerosol

Effects of aerosol emission pathways on future warming and human health

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Partanen, Antti-Ilari; Matthews, Damon

2016-04-01

The peak global temperature is largely determined by cumulative emissions of long-lived greenhouse gases. However, anthropogenic emissions include also so-called short-lived climate forcers (SLCFs), which include aerosol particles and methane. Previous studies with simple models indicate that the timing of SLCF emission reductions has only a small effect on the rate of global warming and even less of an effect on global peak temperatures. However, these simple model analyses do not capture the spatial dynamics of aerosol-climate interactions, nor do they consider the additional effects of aerosol emissions on human health. There is therefore merit in assessing how the timing of aerosol emission reductions affects global temperature and premature mortality caused by elevated aerosol concentrations, using more comprehensive climate models. Here, we used an aerosol-climate model ECHAM-HAMMOZ to simulate the direct and indirect radiative forcing resulting from aerosol emissions. We simulated Representative Concentration Pathway (RCP) scenarios, and we also designed idealized low and high aerosol emission pathways based on RCP4.5 scenario (LOW and HIGH, respectively). From these simulations, we calculated the Effective Radiative Forcing (ERF) from aerosol emissions between 1850 and 2100, as well as aerosol concentrations used to estimate the premature mortality caused by particulate pollution. We then use the University of Victoria Earth System Climate Model to simulate the spatial and temporal pattern of climate response to these aerosol-forcing scenarios, in combination with prescribed emissions of both short and long-lived greenhouse gases according to the RCP4.5 scenario. In the RCP scenarios, global mean ERF declined during the 21st century from -1.3 W m-2 to -0.4 W m-2 (RCP8.5) and -0.2 W m-2 (RCP2.6). In the sensitivity scenarios, the forcing at the end of the 21st century was -1.6 W m-2 (HIGH) and practically zero (LOW). The difference in global mean temperature

Significance of Future Biogenic and Fire Emissions on Regional Aerosol Burden

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Lim, A.; Tai, A. P. K.; Val Martin, M.

2017-12-01

Land-use and land cover changes have been found to substantially affect atmospheric aerosols and climate worldwide1,2, but the complex mechanisms and pathways involved in the interactions between terrestrial processes and aerosols are not well understood. Here we use a global coupled aerosol chemistry-climate-land model (CESM with CAM5 using Modal Aerosol Module 3 and CLM4.5 in Satellite Phenology mode) to investigate how aerosols respond to future climate and land-use changes, and in turn, affects cloud cover and other hydrometeorological variables in the long term. Time-sliced simulations are conducted for a base year (2000) as a base case; then three future projected scenarios for year 2050 driven by land-use and climate projections following the Representative Concentration Pathways RCP8.53 are conducted. The first scenario considers future projected biogenic emissions, allowing us to investigate the effect of increased plant activity and enhanced biogenic emissions due to future land-use and climate on aerosol burden. The second scenario considers future biomass burning emissions, allowing us to investigate the effect of increased biomass burning emissions due to future land-use and climate on aerosol burden. The third scenario combines the projected changes in the two emissions. We find that both biogenic and biomass burning emissions contribute significantly to local aerosol and cloud condensation nuclei (CCN) concentrations. The contribution from biogenic emissions to local aerosol burden is smaller in magnitude (10% to 20%), but the effects are ubiquitous in many places globally. Meanwhile, the contribution from biomass burning emissions can be much higher in magnitude (63%)4, but concentrated in heavily burned regions and occurs only during burning season. Effects of both emissions are not additive since a larger flux of emissions causes greater deposition. The resulting further impacts of land-use change on regional hydrometeorology are also explored

Methods of analysis for complex organic aerosol mixtures from urban emission sources of particulate carbon

International Nuclear Information System (INIS)

Mazurek, M.A.; Hildemann, L.M.; Simoneit, B.R.T.

1990-10-01

Organic aerosols comprise approximately 30% by mass of the total fine particulate matter present in urban atmospheres. The chemical composition of such aerosols is complex and reflects input from multiple sources of primary emissions to the atmosphere, as well as from secondary production of carbonaceous aerosol species via photochemical reactions. To identify discrete sources of fine carbonaceous particles in urban atmospheres, analytical methods must reconcile both bulk chemical and molecular properties of the total carbonaceous aerosol fraction. This paper presents an overview of the analytical protocol developed and used in a study of the major sources of fine carbon particles emitted to an urban atmosphere. 23 refs., 1 fig., 2 tabs

Identification of the sources of primary organic aerosols at urban schools: A molecular marker approach

International Nuclear Information System (INIS)

Crilley, Leigh R.; Qadir, Raeed M.; Ayoko, Godwin A.; Schnelle-Kreis, Jürgen; Abbaszade, Gülcin; Orasche, Jürgen; Zimmermann, Ralf; Morawska, Lidia

2014-01-01

Children are particularly susceptible to air pollution and schools are examples of urban microenvironments that can account for a large portion of children's exposure to airborne particles. Thus this paper aimed to determine the sources of primary airborne particles that children are exposed to at school by analyzing selected organic molecular markers at 11 urban schools in Brisbane, Australia. Positive matrix factorization analysis identified four sources at the schools: vehicle emissions, biomass burning, meat cooking and plant wax emissions accounting for 45%, 29%, 16% and 7%, of the organic carbon respectively. Biomass burning peaked in winter due to prescribed burning of bushland around Brisbane. Overall, the results indicated that both local (traffic) and regional (biomass burning) sources of primary organic aerosols influence the levels of ambient particles that children are exposed at the schools. These results have implications for potential control strategies for mitigating exposure at schools. - Highlights: • Selected organic molecular markers at 11 urban schools were analyzed. • Four sources of primary organic aerosols were identified by PMF at the schools. • Both local and regional sources were found to influence exposure at the schools. • The results have implications for mitigation of children's exposure at schools. - The identification of the most important sources of primary organic aerosols at urban schools has implications for control strategies for mitigating children's exposure at schools

Updating Sea Spray Aerosol Emissions in the Community Multiscale Air Quality Model

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Gantt, B.; Bash, J. O.; Kelly, J.

2014-12-01

Sea spray aerosols (SSA) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. In this study, the Community Multiscale Air Quality (CMAQ) model is updated to enhance fine mode SSA emissions, include sea surface temperature (SST) dependency, and revise surf zone emissions. Based on evaluation with several regional and national observational datasets in the continental U.S., the updated emissions generally improve surface concentrations predictions of primary aerosols composed of sea-salt and secondary aerosols affected by sea-salt chemistry in coastal and near-coastal sites. Specifically, the updated emissions lead to better predictions of the magnitude and coastal-to-inland gradient of sodium, chloride, and nitrate concentrations at Bay Regional Atmospheric Chemistry Experiment (BRACE) sites near Tampa, FL. Including SST-dependency to the SSA emission parameterization leads to increased sodium concentrations in the southeast U.S. and decreased concentrations along the Pacific coast and northeastern U.S., bringing predictions into closer agreement with observations at most Interagency Monitoring of Protected Visual Environments (IMPROVE) and Chemical Speciation Network (CSN) sites. Model comparison with California Research at the Nexus of Air Quality and Climate Change (CalNex) observations will also be discussed, with particular focus on the South Coast Air Basin where clean marine air mixes with anthropogenic pollution in a complex environment. These SSA emission updates enable more realistic simulation of chemical processes in coastal environments, both in clean marine air masses and mixtures of clean marine and polluted conditions.

Modeling regional aerosol and aerosol precursor variability over California and its sensitivity to emissions and long-range transport during the 2010 CalNex and CARES campaigns

Science.gov (United States)

Fast, J. D.; Allan, J.; Bahreini, R.; Craven, J.; Emmons, L.; Ferrare, R.; Hayes, P. L.; Hodzic, A.; Holloway, J.; Hostetler, C.; Jimenez, J. L.; Jonsson, H.; Liu, S.; Liu, Y.; Metcalf, A.; Middlebrook, A.; Nowak, J.; Pekour, M.; Perring, A.; Russell, L.; Sedlacek, A.; Seinfeld, J.; Setyan, A.; Shilling, J.; Shrivastava, M.; Springston, S.; Song, C.; Subramanian, R.; Taylor, J. W.; Vinoj, V.; Yang, Q.; Zaveri, R. A.; Zhang, Q.

2014-09-01

The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using the extensive meteorological, trace gas, and aerosol measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The overall objective of the field campaigns was to obtain data needed to better understand processes that affect both climate and air quality, including emission assessments, transport and chemical aging of aerosols, aerosol radiative effects. Simulations were performed that examined the sensitivity of aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. We found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics quantifying the differences between observed and simulated quantities. Comparisons with lidar and in situ measurements indicate

Modelling of primary aerosols in the chemical transport model MOCAGE: development and evaluation of aerosol physical parameterizations

Directory of Open Access Journals (Sweden)

B. Sič

2015-02-01

Full Text Available This paper deals with recent improvements to the global chemical transport model of Météo-France MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle that consists of updates to different aerosol parameterizations. MOCAGE only contains primary aerosol species: desert dust, sea salt, black carbon, organic carbon, and also volcanic ash in the case of large volcanic eruptions. We introduced important changes to the aerosol parameterization concerning emissions, wet deposition and sedimentation. For the emissions, size distribution and wind calculations are modified for desert dust aerosols, and a surface sea temperature dependant source function is introduced for sea salt aerosols. Wet deposition is modified toward a more physically realistic representation by introducing re-evaporation of falling rain and snowfall scavenging and by changing the in-cloud scavenging scheme along with calculations of precipitation cloud cover and rain properties. The sedimentation scheme update includes changes regarding the stability and viscosity calculations. Independent data from satellites (MODIS, SEVIRI, the ground (AERONET, EMEP, and a model inter-comparison project (AeroCom are compared with MOCAGE simulations and show that the introduced changes brought a significant improvement on aerosol representation, properties and global distribution. Emitted quantities of desert dust and sea salt, as well their lifetimes, moved closer towards values of AeroCom estimates and the multi-model average. When comparing the model simulations with MODIS aerosol optical depth (AOD observations over the oceans, the updated model configuration shows a decrease in the modified normalized mean bias (MNMB; from 0.42 to 0.10 and a better correlation (from 0.06 to 0.32 in terms of the geographical distribution and the temporal variability. The updates corrected a strong positive MNMB in the sea salt representation at high latitudes (from 0.65 to 0.16, and a negative MNMB in

Aerosol emission during human speech

Science.gov (United States)

Asadi, Sima; Wexler, Anthony S.; Cappa, Christopher D.; Bouvier, Nicole M.; Barreda-Castanon, Santiago; Ristenpart, William D.

2017-11-01

We show that the rate of aerosol particle emission during healthy human speech is strongly correlated with the loudness (amplitude) of vocalization. Emission rates range from approximately 1 to 50 particles per second for quiet to loud amplitudes, regardless of language spoken (English, Spanish, Mandarin, or Arabic). Intriguingly, a small fraction of individuals behave as ``super emitters,'' consistently emitting an order of magnitude more aerosol particles than their peers. We interpret the results in terms of the eggressive flowrate during vocalization, which is known to vary significantly for different types of vocalization and for different individuals. The results suggest that individual speech patterns could affect the probability of airborne disease transmission. The results also provide a possible explanation for the existence of ``super spreaders'' who transmit pathogens much more readily than average and who play a key role in the spread of epidemics.

Highly-controlled, reproducible measurements of aerosol emissions from African biomass combustion

Science.gov (United States)

Haslett, Sophie; Thomas, J. Chris; Morgan, William; Hadden, Rory; Liu, Dantong; Allan, James; Williams, Paul; Sekou, Keïta; Liousse, Catherine; Coe, Hugh

2017-04-01

Particulate emissions from biomass burning can alter the atmosphere's radiative balance and cause significant harm to human health. However, the relationship between these emissions and fundamental combustion processes is, to date, poorly characterised. In atmospheric models, aerosol emissions are represented by emission factors based on mass loss, which are averaged over an entire combustion event for each particulate species. This approach, however, masks huge variability in emissions during different phases of the combustion period. Laboratory tests have shown that even small changes to the burning environment can lead to huge variation in observed aerosol emission factors (Akagi et al., 2011). In order to address this gap in understanding, in this study, small wood samples sourced from Côte D'Ivoire were burned in a highly-controlled laboratory environment. The shape and mass of samples, available airflow and surrounding heat were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real-time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. Both of these instruments are used regularly to measure aerosol concentrations in the field. This methodology produced remarkably repeatable results, allowing three different phases of combustion to be identified by their emissions. Black carbon was emitted predominantly during flaming combustion; organic aerosols were emitted during pyrolysis before ignition and from smouldering-dominated behaviour near the end of combustion. During the flaming period, there was a strong correlation between the emission of black carbon and the rate of mass loss, which suggests there is value in employing a mass-based emission factor for this species. However, very little correlation was seen between organic aerosol and mass loss throughout the tests. As such, results here suggest that emission factors averaged over an entire combustion event are unlikely to be

Exchanges in boundary layer and low troposphere and consequences on pollution of Fos-Berre-Marseille area (ESCOMPTE experiment); Les aerosols: emissions, formation d'aerosols organiques secondaires, transport longue distance. Zoom sur les aerosols carbones en Europe

Energy Technology Data Exchange (ETDEWEB)

Guillaume, B

2006-01-15

There are two types of 'carbonaceous aerosols': 'black carbon' (BC) and 'organic carbon'(OC). BC is directly emitted in the atmosphere while OC is either directly emitted (primary OC, OCp) or secondarily formed through oxidation processes in the atmosphere (secondary organic aerosols, SOA). Complexity of carbonaceous aerosols is still poorly represented in existing aerosol models and uncertainties appear mainly both in their emission inventories and in their complex atmospheric evolution (transport, gas-particle interactions, dry/wet deposition), making difficult the estimation of their radiative impact. In this framework, I developed during my PhD at Laboratoire d'Aerologie, a new approach to deal with this complexity, with implementation of both a new carbonaceous aerosol emission inventory and a new aerosol modelling tool at global scale. My work is divided in 5 different tasks: - better characterisation of BC and OCp emissions, achieved through the development of a new emission inventory from fossil fuel and biofuel combustion sources (industrial, domestic and mobile sources). This inventory provides BC and OCp emissions for Europe at 25 km * 25 km resolution for the years 1990, 1995, 2000, 2005 and 2010, with two additional regional zooms: on France, at 10 km * 10 km resolution for the years 2000 and 2010 with improved road traffic, and in Marseille region (Escompte campaign, 1999,-2001) at 1 km * 1 km resolution for the year 1999; - better modelling of carbonaceous aerosol complex atmospheric evolution, through coupling of a global scale gas transport/chemistry model (TM4) with an aerosol module (ORISAM) featuring size-distributed aerosols (on 8 diameter sections from 40 nm to 10 {mu}m) organic/inorganic chemical composition and explicit treatment of SOA formation; - simulations with this new aerosol model ORISAM-TM4 and model/measurements comparisons to study BC and OC long-range transport; - sensitivity tests on SOA

Evaluation of the Volatility Basis-Set Approach for Modeling Primary and Secondary Organic Aerosol in the Mexico City Metropolitan Area

Science.gov (United States)

Tsimpidi, A. P.; Karydis, V. A.; Pandis, S. N.; Zavala, M.; Lei, W.; Molina, L. T.

2007-12-01

Anthropogenic air pollution is an increasingly serious problem for public health, agriculture, and global climate. Organic material (OM) contributes ~ 20-50% to the total fine aerosol mass at continental mid-latitudes. Although OM accounts for a large fraction of PM2.5 concentration worldwide, the contributions of primary and secondary organic aerosol have been difficult to quantify. In this study, new primary and secondary organic aerosol modules were added to PMCAMx, a three dimensional chemical transport model (Gaydos et al., 2007), for use with the SAPRC99 chemistry mechanism (Carter, 2000; ENVIRON, 2006) based on recent smog chamber studies (Robinson et al., 2007). The new modeling framework is based on the volatility basis-set approach (Lane et al., 2007): both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The emission inventory, which uses as starting point the MCMA 2004 official inventory (CAM, 2006), is modified and the primary organic aerosol (POA) emissions are distributed by volatility based on dilution experiments (Robinson et al., 2007). Sensitivity tests where POA is considered as nonvolatile and POA and SOA as chemically reactive are also described. In all cases PMCAMx is applied in the Mexico City Metropolitan Area during March 2006. The modeling domain covers a 180x180x6 km region in the MCMA with 3x3 km grid resolution. The model predictions are compared with Aerodyne's Aerosol Mass Spectrometry (AMS) observations from the MILAGRO Campaign. References Robinson, A. L.; Donahue, N. M.; Shrivastava, M. K.; Weitkamp, E. A.; Sage, A. M.; Grieshop, A. P.; Lane, T. E.; Pandis, S. N.; Pierce, J. R., 2007. Rethinking organic aerosols: semivolatile emissions and photochemical aging. Science 315, 1259-1262. Gaydos, T. M.; Pinder, R. W.; Koo, B.; Fahey, K. M.; Pandis, S. N., 2007. Development and application of a three- dimensional aerosol

Primary Emission and the Potential of Secondary Aerosol Formation from Chinese Gasoline Engine Exhaust

Science.gov (United States)

Hu, Min; Peng, Jianfei; Qin, Yanhong; Du, Zhuofei; Li, Mengjin; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Lu, Sihua; Wu, Yusheng; Zeng, Limin; Guo, Song; Shao, Min; Wang, Yinhui; Shuai, Shijin

2017-04-01

Along with the urbanization and economic growth, vehicle population in China reached 269 million, ranked the second in the world in 2015. Gasoline vehicle is identified to be the main source for urban PM2.5 in China, accounting for 15%-31%. In this study the impact of fuel components on PM2.5 and volatile organic compounds (VOCs) emissions from a gasoline port fuel injection (PFI) engine and a gasoline direct injection (GDI) engine are discussed. Results show that, higher proportion of aromatics, alkenes or sulfur in gasoline fuel will lead to higher PM emissions. The PM from the PFI engine mainly consists of OC and a small amount of EC and inorganic ions, while the PM discharge from the GDI engine mainly consists of EC, OM and a small amount of inorganic ions. Since the GDI engines can reduce fuel consumption and CO2 emissions, and it would become more and more popular in the near future. The characteristics of POM component, emission factors and source profile were investigated from GDI engine, particularly focused on the effect of engine speed, load and the catalyst, which will be very much helpful for source identification as source indicators. Chamber experiments were conducted to quantify the potential of secondary aerosol formation from exhaust of a PFI gasoline engine and China V gasoline fuel. During 4-5 h simulation, equivalent to10 days of atmospheric photo-oxidation in Beijing, the extreme SOA production was 426 ± 85 mg/kg fuel, with high precursors and OH exposure. 14% of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatility organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reduction of emissions of aerosol precursor gases from vehicles is essential to mediate pollution in China.

Radiative effects of interannually varying vs. interannually invariant aerosol emissions from fires

Directory of Open Access Journals (Sweden)

B. S. Grandey

2016-11-01

Full Text Available Open-burning fires play an important role in the earth's climate system. In addition to contributing a substantial fraction of global emissions of carbon dioxide, they are a major source of atmospheric aerosols containing organic carbon, black carbon, and sulfate. These “fire aerosols” can influence the climate via direct and indirect radiative effects. In this study, we investigate these radiative effects and the hydrological fast response using the Community Atmosphere Model version 5 (CAM5. Emissions of fire aerosols exert a global mean net radiative effect of −1.0 W m−2, dominated by the cloud shortwave response to organic carbon aerosol. The net radiative effect is particularly strong over boreal regions. Conventionally, many climate modelling studies have used an interannually invariant monthly climatology of emissions of fire aerosols. However, by comparing simulations using interannually varying emissions vs. interannually invariant emissions, we find that ignoring the interannual variability of the emissions can lead to systematic overestimation of the strength of the net radiative effect of the fire aerosols. Globally, the overestimation is +23 % (−0.2 W m−2. Regionally, the overestimation can be substantially larger. For example, over Australia and New Zealand the overestimation is +58 % (−1.2 W m−2, while over Boreal Asia the overestimation is +43 % (−1.9 W m−2. The systematic overestimation of the net radiative effect of the fire aerosols is likely due to the non-linear influence of aerosols on clouds. However, ignoring interannual variability in the emissions does not appear to significantly impact the hydrological fast response. In order to improve understanding of the climate system, we need to take into account the interannual variability of aerosol emissions.

Time Resolved Measurements of Primary Biogenic Aerosol Particles in Amazonia

Science.gov (United States)

Wollny, A. G.; Garland, R.; Pöschl, U.

2009-04-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the Amazonian Aerosol Characterization Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. This presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 µm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as "viable aerosols" or "fluorescent bioparticles" (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. Data from the UVAPS were averaged over 5 minute time intervals. The presence of bioparticles in the observed size range has been

Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer

Directory of Open Access Journals (Sweden)

M. F. Heringa

2011-06-01

Full Text Available A series of photo-oxidation smog chamber experiments were performed to investigate the primary emissions and secondary aerosol formation from two different log wood burners and a residential pellet burner under different burning conditions: starting and flaming phase. Emissions were sampled from the chimney and injected into the smog chamber leading to primary organic aerosol (POA concentrations comparable to ambient levels. The composition of the aerosol was measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS and black carbon (BC instrumentation. The primary emissions were then exposed to xenon light to initiate photo-chemistry and subsequent secondary organic aerosol (SOA production. After correcting for wall losses, the average increase in organic matter (OM concentrations by SOA formation for the starting and flaming phase experiments with the two log wood burners was found to be a factor of 4.1±1.4 after five hours of aging. No SOA formation was observed for the stable burning phase of the pellet burner. The startup emissions of the pellet burner showed an increase in OM concentration by a factor of 3.3. Including the measured SOA formation potential, average emission factors of BC+POA+SOA, calculated from CO₂ emission, were found to be in the range of 0.04 to 3.9 g/kg wood for the stable burning pellet burner and an old log wood burner during startup respectively. SOA contributed significantly to the ion C₂H₄O₂⁺ at mass to charge ratio m/z 60, a commonly used marker for primary emissions of wood burning. This contribution at m/z 60 can overcompensate for the degradation of levoglucosan leading to an overestimation of the contribution of wood burning or biomass burning to the total OM. The primary organic emissions from the three different burners showed a wide range in O:C atomic ratio (0.19−0.60 for the starting and flaming

The impact of aerosol emissions on the 1.5 °C pathways

Science.gov (United States)

Hienola, Anca; Partanen, Antti-Ilari; Pietikäinen, Joni-Pekka; O’Donnell, Declan; Korhonen, Hannele; Damon Matthews, H.; Laaksonen, Ari

2018-04-01

To assess the impact of anthropogenic aerosol emission reduction on limiting global temperature increase to 1.5 °C or 2 °C above pre-industrial levels, two climate modeling approaches have been used (MAGICC6, and a combination of ECHAM-HAMMOZ and the UVic ESCM), with two aerosol control pathways under two greenhouse gas (GHG) reduction scenarios. We found that aerosol emission reductions associated with CO2 co-emissions had a significant warming effect during the first half of the century and that the near-term warming is dependent on the pace of aerosol emission reduction. The modeling results show that these aerosol emission reductions account for about 0.5 °C warming relative to 2015, on top of the 1 °C above pre-industrial levels that were already reached in 2015. We found also that the decreases in aerosol emissions lead to different decreases in the magnitude of the aerosol radiative forcing in the two models. By 2100, the aerosol forcing is projected by ECHAM–UVic to diminish in magnitude by 0.96 W m‑2 and by MAGICC6 by 0.76 W m‑2 relative to 2000. Despite this discrepancy, the climate responses in terms of temperature are similar. Aggressive aerosol control due to air quality legislation affects the peak temperature, which is 0.2 °C–0.3 °C above the 1.5 °C limit even within the most ambitious CO2/GHG reduction scenario. At the end of the century, the temperature differences between aerosol reduction scenarios in the context of ambitious CO2 mitigation are negligible.

Where and What Is Pristine Marine Aerosol?

Science.gov (United States)

Russell, L. M.; Frossard, A. A.; Long, M. S.; Burrows, S. M.; Elliott, S.; Bates, T. S.; Quinn, P.

2014-12-01

The sources and composition of atmospheric marine aerosol particles have been measured by functional group composition (from Fourier transform infrared spectroscopy) to identify the organic composition of the pristine primary marine (ocean-derived) particles as 65% hydroxyl, 21% alkane, 6% amine, and 7% carboxylic acid functional groups [Frossard et al., 2014a,b]. Pristine but non-primary components from photochemical reactions (likely from biogenic marine vapor emissions) add carboxylic acid groups. Non-pristine contributions include shipping effluent in seawater and ship emissions, which add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. The pristine primary marine (ocean-derived) organic aerosol composition is nearly identical to model generated primary marine aerosol particles from bubbled seawater, indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the generated primary marine aerosol particles remained nearly constant over a broad range of chlorophyll-a concentrations, the generated primary marine aerosol particle alkane group fraction increased with chlorophyll-a concentrations. In addition, the generated primary marine aerosol particles have a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater hydroxyl group peak location is closer to that of polysaccharides. References Cited Frossard, Amanda A., Lynn M. Russell, Paola Massoli, Timothy S. Bates, and Patricia K. Quinn, "Side-by-Side Comparison of Four Techniques Explains the Apparent Differences in the Organic Composition of Generated and Ambient Marine Aerosol Particles," Aerosol Science and Technology - Aerosol Research Letter

The Influence of Emission Location on the Magnitude and Spatial Distribution of Aerosols' Climate Effects

Science.gov (United States)

Persad, G.; Caldeira, K.

2017-12-01

The global distribution of anthropogenic aerosol emissions has evolved continuously since the preindustrial era - from 20th century North American and Western European emissions hotspots to present-day South and East Asian ones. With this comes a relocation of the regional radiative, dynamical, and hydrological impacts of aerosol emissions, which may influence global climate differently depending on where they occur. A lack of understanding of this relationship between aerosol emissions' location and their global climate effects, however, obscures the potential influence that aerosols' evolving geographic distribution may have on global and regional climate change—a gap which we address in this work. Using a novel suite of experiments in the CESM CAM5 atmospheric general circulation model coupled to a slab ocean, we systematically test and analyze mechanisms behind the relative climate impact of identical black carbon and sulfate aerosol emissions located in each of 8 past, present, or projected future major emissions regions. Results indicate that historically high emissions regions, such as North America and Western Europe, produce a stronger cooling effect than current and projected future high emissions regions. Aerosol emissions located in Western Europe produce 3 times the global mean cooling (-0.34 °C) as those located in East Africa or India (-0.11 °C). The aerosols' in-situ radiative effects remain relatively confined near the emissions region, but large distal cooling results from remote feedback processes - such as ice albedo and cloud changes - that are excited more strongly by emissions from certain regions than others. Results suggest that aerosol emissions from different countries should not be considered equal in the context of climate mitigation accounting, and that the evolving geographic distribution of aerosol emissions may have a substantial impact on the magnitude and spatial distribution of global climate change.

Smoke aerosol chemistry and aging of Siberian biomass burning emissions in a large aerosol chamber

Science.gov (United States)

Kalogridis, A.-C.; Popovicheva, O. B.; Engling, G.; Diapouli, E.; Kawamura, K.; Tachibana, E.; Ono, K.; Kozlov, V. S.; Eleftheriadis, K.

2018-07-01

Vegetation open fires constitute a significant source of particulate pollutants on a global scale and play an important role in both atmospheric chemistry and climate change. To better understand the emission and aging characteristics of smoke aerosols, we performed small-scale fire experiments using the Large Aerosol Chamber (LAC, 1800 m3) with a focus on biomass burning from Siberian boreal coniferous forests. A series of burn experiments were conducted with typical Siberian biomass (pine and debris), simulating separately different combustion conditions, namely, flaming, smoldering and mixed phase. Following smoke emission and dispersion in the combustion chamber, we investigated aging of aerosols under dark conditions. Here, we present experimental data on emission factors of total, elemental and organic carbon, as well as individual organic compounds, such as anhydrosugars, phenolic and dicarboxylic acids. We found that total carbon accounts for up to 80% of the fine mode (PM2.5) smoke aerosol. Higher PM2.5 emission factors were observed in the smoldering compared to flaming phase and in pine compared to debris smoldering phase. For low-temperature combustion, organic carbon (OC) contributed to more than 90% of total carbon, whereas elemental carbon (EC) dominated the aerosol composition in flaming burns with a 60-70% contribution to the total carbon mass. For all smoldering burns, levoglucosan (LG), a cellulose decomposition product, was the most abundant organic species (average LG/OC = 0.26 for pine smoldering), followed by its isomer mannosan or dehydroabietic acid (DA), an important constituent of conifer resin (DA/OC = 0.033). A levoglucosan-to-mannosan ratio of about 3 was observed, which is consistent with ratios reported for coniferous biomass and more generally softwood. The rates of aerosol removal for OC and individual organic compounds were investigated during aging in the chamber in terms of mass concentration loss rates over time under dark

Primary and secondary aerosols in Beijing in winter: sources, variations and processes

Science.gov (United States)

Sun, Yele; Du, Wei; Fu, Pingqing; Wang, Qingqing; Li, Jie; Ge, Xinlei; Zhang, Qi; Zhu, Chunmao; Ren, Lujie; Xu, Weiqi; Zhao, Jian; Han, Tingting; Worsnop, Douglas R.; Wang, Zifa

2016-07-01

Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size

Primary and secondary aerosols in Beijing in winter: sources, variations and processes

Directory of Open Access Journals (Sweden)

Y. Sun

2016-07-01

Full Text Available Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %, sulfate (15 % and nitrate (11 %. Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA factors from traffic, cooking, biomass burning (BBOA and coal combustion (CCOA emissions as well as two secondary OA (SOA factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %. Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 % and biomass burning emissions (18 %. BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93, and made a considerable contribution to OA in winter (9 %. An aqueous-phase-processed SOA (aq-OOA that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+ was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %. Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on

Primary and secondary organic aerosols in summer 2016 in Beijing

Science.gov (United States)

Tang, Rongzhi; Wu, Zepeng; Li, Xiao; Wang, Yujue; Shang, Dongjie; Xiao, Yao; Li, Mengren; Zeng, Limin; Wu, Zhijun; Hallquist, Mattias; Hu, Min; Guo, Song

2018-03-01

To improve air quality, the Beijing government has employed several air pollution control measures since the 2008 Olympics. In order to investigate organic aerosol sources after the implementation of these measures, ambient fine particulate matter was collected at a regional site in Changping (CP) and an urban site at the Peking University Atmosphere Environment Monitoring Station (PKUERS) during the Photochemical Smog in China field campaign in summer 2016. Chemical mass balance (CMB) modeling and the tracer yield method were used to apportion primary and secondary organic sources. Our results showed that the particle concentration decreased significantly during the last few years. The apportioned primary and secondary sources explained 62.8 ± 18.3 and 80.9 ± 27.2 % of the measured OC at CP and PKUERS, respectively. Vehicular emissions served as the dominant source. Except for gasoline engine emissions, the contributions of all the other primary sources decreased. In addition, the anthropogenic SOC, i.e., toluene SOC, also decreased, implying that deducting primary emissions can reduce anthropogenic SOA. In contrast to the SOA from other regions in the world where biogenic SOA was dominant, anthropogenic SOA was the major contributor to SOA, implying that deducting anthropogenic VOC emissions is an efficient way to reduce SOA in Beijing. Back-trajectory cluster analysis results showed that high mass concentrations of OC were observed when the air mass was from the south. However, the contributions of different primary organic sources were similar, suggesting regional particle pollution. The ozone concentration and temperature correlated well with the SOA concentration. Different correlations between day and night samples suggested different SOA formation pathways. Significant enhancement of SOA with increasing particle water content and acidity was observed in our study, suggesting that aqueous-phase acid-catalyzed reactions may be the important SOA formation

Future aerosols of the southwest - Implications for fundamental aerosol research

International Nuclear Information System (INIS)

Friedlander, S.K.

1980-01-01

It is shown that substantial increases in the use of coal in the U.S. will lead to substantial increases in emissions of particulate matter, SO/sub x/, and NO/sub x/ in the part of the U.S. west of the Mississippi. A shift in the primary particulate emissions from coarse to submicron particles is predicted. Attention is given to the nature of the submicron aerosol in the southwest, the distribution of sulfur with respect to particle size, the formation of new particles in the atmosphere, and the ammonium nitrate equilibrium. It is concluded that increased coal use will result in a 50% increase in SO/sub x/ emissions and a doubling of NO/sub x/ emissions in the western U.S. by the year 2000, that ambient levels of aerosol sulfates and nitrates will increase, and that a large increase in submicron aerosol mass is likely

Numerical simulations of Aerosol and Trace Gas Emissions and Transformations over the North China Plain

Science.gov (United States)

He, H.; Ren, X.; Li, Z.; Dickerson, R. R.

2016-12-01

The North China Plain (NCP) is one of the most populated and polluted regions on Earth. In the past decades the rapid economic development has resulted in heavy atmospheric aerosol loadings in this region. The high aerosol concentrations induce severe environmental and climate problems, and aerosols can also affect human health and visibility. So there is a continued need to understand air quality in this region and transport of air pollutants from this region as populations grow, energy use increases, and industrial activity evolves. The unique mix of species over the NCP makes understanding the processes leading to transformations of primary pollutants and formation of secondary pollutants essential to predicting regional and global impacts. WRF-Chem simulations were performed for the NCP to investigate the emissions and transformations of air pollutants. MIX emission inventory of year 2010 (developed for MICS-Asia III and HTAP projects) was used to drive the WRF-Chem model. Modeling results were evaluated with observation data including OMI SO2/NO2 and MODIS AOD products to improve our knowledge of emission changes in the NCP between 2010 and 2016. We also estimated the regional transport of air pollutants from the NCP to downwind areas such as South Korea and Japan with WRF-Chem simulations constrained by these observations.

Molecular characterization of urban organic aerosol in tropical India: contributions of primary emissions and secondary photooxidation

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P. Q. Fu

2010-03-01

Full Text Available Organic molecular composition of PM₁₀ samples, collected at Chennai in tropical India, was studied using capillary gas chromatography/mass spectrometry. Fourteen organic compound classes were detected in the aerosols, including aliphatic lipids, sugar compounds, lignin products, terpenoid biomarkers, sterols, aromatic acids, hydroxy-/polyacids, phthalate esters, hopanes, Polycyclic Aromatic Hydrocarbons (PAHs, and photooxidation products from biogenic Volatile Organic Compounds (VOCs. At daytime, phthalate esters were found to be the most abundant compound class; however, at nighttime, fatty acids were the dominant one. Di-(2-ethylhexyl phthalate, C₁₆ fatty acid, and levoglucosan were identified as the most abundant single compounds. The nighttime maxima of most organics in the aerosols indicate a land/sea breeze effect in tropical India, although some other factors such as local emissions and long-range transport may also influence the composition of organic aerosols. However, biogenic VOC oxidation products (e.g., 2-methyltetrols, pinic acid, 3-hydroxyglutaric acid and β-caryophyllinic acid showed diurnal patterns with daytime maxima. Interestingly, terephthalic acid was maximized at nighttime, which is different from those of phthalic and isophthalic acids. A positive relation was found between 1,3,5-triphenylbenzene (a tracer for plastic burning and terephthalic acid, suggesting that the field burning of municipal solid wastes including plastics is a significant source of terephthalic acid. Organic compounds were further categorized into several groups to clarify their sources. Fossil fuel combustion (24–43% was recognized as the most significant source for the total identified compounds, followed by plastic emission (16–33%, secondary oxidation (8.6–23%, and microbial/marine sources (7.2–17%. In contrast, the contributions of terrestrial plant waxes (5.9–11% and biomass burning (4.2–6.4% were relatively

Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

Science.gov (United States)

Lee, Alex K. Y.; Chen, Chia-Li; Liu, Jun; Price, Derek J.; Betha, Raghu; Russell, Lynn M.; Zhang, Xiaolu; Cappa, Christopher D.

2017-12-01

Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the -log(NOx / NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7-20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

Transient Climate Impacts for Scenarios of Aerosol Emissions from Asia: A Story of Coal versus Gas

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Grandey, B. S.; Cheng, H.; Wang, C.

2014-12-01

Projections of anthropogenic aerosol emissions are uncertain. In Asia, it is possible that emissions may increase if business continues as usual, with economic growth driving an increase in coal burning. But it is also possible that emissions may decrease rapidly due to the widespread adoption of cleaner technology or a shift towards non-coal fuels, such as natural gas. In this study, the transient climate impacts of three aerosol emissions scenarios are investigated: an RCP4.5 (Representative Concentration Pathway 4.5) control; a scenario with reduced Asian anthropogenic aerosol emissions; and a scenario with enhanced Asian anthropogenic aerosol emissions. A coupled atmosphere-ocean configuration of CESM (Community Earth System Model), including CAM5 (Community Atmosphere Model version 5), is used. Enhanced Asian aerosol emissions are found to delay global mean warming by one decade at the end of the century. Aerosol-induced suppression of the East Asian and South Asian summer monsoon precipitation occurs. The enhanced Asian aerosol emissions also remotely impact precipitation in other parts of the world: over the Sahel, West African monsoon precipitation is suppressed; and over Australia, austral summer monsoon precipitation is enhanced. These remote impacts on precipitation are associated with a southward shift of the ITCZ. The aerosol-induced sea surface temperature (SST) response appears to play an important role in the precipitation changes over South Asia and Australia, but not over East Asia. These results indicate that energy production in Asia, through the consequent aerosol emissions and associated radiative effects, might significantly influence future climate both locally and globally.

Accessing the Impact of Sea-Salt Emissions on Aerosol Chemical Formation and Deposition Over Pearl River Delta, China

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Fan, Q.; Wang, X.; Liu, Y.; Wu, D.; Chan, P. W.; Fan, S.; Feng, Y.

2015-12-01

Sea-salt aerosol (SSA) emissions have a significant impact on aerosol pollution and haze formation in the coastal areas. In this study, Models-3/CMAQ modeling system was utilized to access the impact of SSA emissions on aerosol chemical formation and deposition over Pearl River Delta (PRD), China in July 2006. More SSAs were transported inland from the open-ocean under the southeast wind in summertime. Two experiments (with and without SSA emissions in the CMAQ model) were set up to compare the modeling results with each other. The results showed that the increase of sulfate concentrations were more attributable to the primary emissions of coarse SO42- particles in SSA, while the increase of nitrate concentrations were more attributable to secondary chemical formations, known as the mechanisms of chloride depletion in SSA. In the coastal areas, 17.62 % of SO42-, 26.6% of NO3- and 38.2% of PM10 were attributed to SSA emissions, while those portions were less than 1% in the inland areas. The increases of PM10 and its components due to SSA emissions resulted in higher deposition fluxes over PRD, particularly in the coastal areas, except for the wet deposition of nitrate. Nitrate was more sensitive to SSA emissions in chemical formations than sulfate and dry deposition of aerosol was also more sensitive than that for wet deposition. Process analysis of sulfate and nitrate was applied to find out the difference of physical and chemical mechanisms between Guangzhou (the inland areas) and Zhuhai (the coastal areas). The negative contributions of dry deposition process to both sulfate and nitrate concentrations increased if SSA emissions were taken into account in the model, especially for Zhuhai. The negative contributions of cloud process also increased due to cloud scavenging and wet deposition process. In the coastal area, the gas-to-particle conversions became more active with high contributions of aerosol process to nitrate concentrations.

Continental anthropogenic primary particle number emissions

Science.gov (United States)

Paasonen, Pauli; Kupiainen, Kaarle; Klimont, Zbigniew; Visschedijk, Antoon; Denier van der Gon, Hugo A. C.; Amann, Markus

2016-06-01

Atmospheric aerosol particle number concentrations impact our climate and health in ways different from those of aerosol mass concentrations. However, the global, current and future anthropogenic particle number emissions and their size distributions are so far poorly known. In this article, we present the implementation of particle number emission factors and the related size distributions in the GAINS (Greenhouse Gas-Air Pollution Interactions and Synergies) model. This implementation allows for global estimates of particle number emissions under different future scenarios, consistent with emissions of other pollutants and greenhouse gases. In addition to determining the general particulate number emissions, we also describe a method to estimate the number size distributions of the emitted black carbon particles. The first results show that the sources dominating the particle number emissions are different to those dominating the mass emissions. The major global number source is road traffic, followed by residential combustion of biofuels and coal (especially in China, India and Africa), coke production (Russia and China), and industrial combustion and processes. The size distributions of emitted particles differ across the world, depending on the main sources: in regions dominated by traffic and industry, the number size distribution of emissions peaks in diameters range from 20 to 50 nm, whereas in regions with intensive biofuel combustion and/or agricultural waste burning, the emissions of particles with diameters around 100 nm are dominant. In the baseline (current legislation) scenario, the particle number emissions in Europe, Northern and Southern Americas, Australia, and China decrease until 2030, whereas especially for India, a strong increase is estimated. The results of this study provide input for modelling of the future changes in aerosol-cloud interactions as well as particle number related adverse health effects, e.g. in response to tightening

Primary and secondary organic aerosols in summer 2016 in Beijing

Directory of Open Access Journals (Sweden)

R. Tang

2018-03-01

Full Text Available To improve air quality, the Beijing government has employed several air pollution control measures since the 2008 Olympics. In order to investigate organic aerosol sources after the implementation of these measures, ambient fine particulate matter was collected at a regional site in Changping (CP and an urban site at the Peking University Atmosphere Environment Monitoring Station (PKUERS during the Photochemical Smog in China field campaign in summer 2016. Chemical mass balance (CMB modeling and the tracer yield method were used to apportion primary and secondary organic sources. Our results showed that the particle concentration decreased significantly during the last few years. The apportioned primary and secondary sources explained 62.8 ± 18.3 and 80.9 ± 27.2 % of the measured OC at CP and PKUERS, respectively. Vehicular emissions served as the dominant source. Except for gasoline engine emissions, the contributions of all the other primary sources decreased. In addition, the anthropogenic SOC, i.e., toluene SOC, also decreased, implying that deducting primary emissions can reduce anthropogenic SOA. In contrast to the SOA from other regions in the world where biogenic SOA was dominant, anthropogenic SOA was the major contributor to SOA, implying that deducting anthropogenic VOC emissions is an efficient way to reduce SOA in Beijing. Back-trajectory cluster analysis results showed that high mass concentrations of OC were observed when the air mass was from the south. However, the contributions of different primary organic sources were similar, suggesting regional particle pollution. The ozone concentration and temperature correlated well with the SOA concentration. Different correlations between day and night samples suggested different SOA formation pathways. Significant enhancement of SOA with increasing particle water content and acidity was observed in our study, suggesting that aqueous-phase acid-catalyzed reactions may be

Highly controlled, reproducible measurements of aerosol emissions from combustion of a common African biofuel source

Science.gov (United States)

Haslett, Sophie L.; Thomas, J. Chris; Morgan, William T.; Hadden, Rory; Liu, Dantong; Allan, James D.; Williams, Paul I.; Keita, Sekou; Liousse, Cathy; Coe, Hugh

2018-01-01

Particulate emissions from biomass burning can both alter the atmosphere's radiative balance and cause significant harm to human health. However, due to the large effect on emissions caused by even small alterations to the way in which a fuel burns, it is difficult to study particulate production of biomass combustion mechanistically and in a repeatable manner. In order to address this gap, in this study, small wood samples sourced from Côte D'Ivoire in West Africa were burned in a highly controlled laboratory environment. The shape and mass of samples, available airflow and surrounding thermal environment were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. This methodology produced remarkably repeatable results, allowing aerosol emissions to be mapped directly onto different phases of combustion. Emissions from pyrolysis were visible as a distinct phase before flaming was established. After flaming combustion was initiated, a black-carbon-dominant flame was observed during which very little organic aerosol was produced, followed by a period that was dominated by organic-carbon-producing smouldering combustion, despite the presence of residual flaming. During pyrolysis and smouldering, the two phases producing organic aerosol, distinct mass spectral signatures that correspond to previously reported variations in biofuel emissions measured in the atmosphere are found. Organic aerosol emission factors averaged over an entire combustion event were found to be representative of the time spent in the pyrolysis and smouldering phases, rather than reflecting a coupling between emissions and the mass loss of the sample. Further exploration of aerosol yields from similarly carefully controlled fires and a careful comparison with data from macroscopic fires and real-world emissions will help to deliver greater constraints on the

Aerosol exposure versus aerosol cooling of climate: what is the optimal emission reduction strategy for human health?

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J. Löndahl

2010-10-01

Full Text Available Particles, climate change, and health have thought-provoking interactions. Air pollution is one of the largest environmental problems concerning human health. On the other hand, aerosol particles can have a cooling effect on climate and a reduction of those emissions may result in an increased temperature globally, which in turn may have negative health effects. The objective of this work was to investigate the "total health effects" of aerosol emissions, which include both exposure to particles and consequences for climate change initiated by particles. As a case study the "total health effect" from ship emissions was derived by subtracting the number of deaths caused by exposure with the estimated number of lives saved from the cooling effect of the emissions. The analysis showed that, with current level of scientific understanding, it could not be determined whether ship emissions are negative or positive for human health on a short time scale. This first attempt to approximate the combined effect of particle emissions on health shows that reductions of particulate air pollution will in some cases (black carbon have win-win effects on health and climate, but sometimes also cause a shift from particle exposure-related health effects towards an increasing risk of health consequences from climate change. Thus, measures to reduce aerosol emissions have to be coupled with climate change mitigation actions to achieve a full health benefit on a global level.

A Simple Model of Global Aerosol Indirect Effects

Science.gov (United States)

Ghan, Steven J.; Smith, Steven J.; Wang, Minghuai; Zhang, Kai; Pringle, Kirsty; Carslaw, Kenneth; Pierce, Jeffrey; Bauer, Susanne; Adams, Peter

2013-01-01

Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth's energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically based model expresses the aerosol indirect effect (AIE) using analytic representations of cloud and aerosol distributions and processes. Although the simple model is able to produce estimates of AIEs that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates by the simple model are sensitive to preindustrial cloud condensation nuclei concentration, preindustrial accumulation mode radius, width of the accumulation mode, size of primary particles, cloud thickness, primary and secondary anthropogenic emissions, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Estimates of present-day AIEs as low as 5 W/sq m and as high as 0.3 W/sq m are obtained for plausible sets of parameter values. Estimates are surprisingly linear in emissions. The estimates depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models, which adds to understanding of the dependence on AIE uncertainty on uncertainty in parameter values.

Global radiative effects of solid fuel cookstove aerosol emissions

Science.gov (United States)

Huang, Yaoxian; Unger, Nadine; Storelvmo, Trude; Harper, Kandice; Zheng, Yiqi; Heyes, Chris

2018-04-01

We apply the NCAR CAM5-Chem global aerosol-climate model to quantify the net global radiative effects of black and organic carbon aerosols from global and Indian solid fuel cookstove emissions for the year 2010. Our assessment accounts for the direct radiative effects, changes to cloud albedo and lifetime (aerosol indirect effect, AIE), impacts on clouds via the vertical temperature profile (semi-direct effect, SDE) and changes in the surface albedo of snow and ice (surface albedo effect). In addition, we provide the first estimate of household solid fuel black carbon emission effects on ice clouds. Anthropogenic emissions are from the IIASA GAINS ECLIPSE V5a inventory. A global dataset of black carbon (BC) and organic aerosol (OA) measurements from surface sites and aerosol optical depth (AOD) from AERONET is used to evaluate the model skill. Compared with observations, the model successfully reproduces the spatial patterns of atmospheric BC and OA concentrations, and agrees with measurements to within a factor of 2. Globally, the simulated AOD agrees well with observations, with a normalized mean bias close to zero. However, the model tends to underestimate AOD over India and China by ˜ 19 ± 4 % but overestimate it over Africa by ˜ 25 ± 11 % (± represents modeled temporal standard deviations for n = 5 run years). Without BC serving as ice nuclei (IN), global and Indian solid fuel cookstove aerosol emissions have net global cooling radiative effects of -141 ± 4 mW m-2 and -12 ± 4 mW m-2, respectively (± represents modeled temporal standard deviations for n = 5 run years). The net radiative impacts are dominated by the AIE and SDE mechanisms, which originate from enhanced cloud condensation nuclei concentrations for the formation of liquid and mixed-phase clouds, and a suppression of convective transport of water vapor from the lower troposphere to the upper troposphere/lower stratosphere that in turn leads to reduced ice cloud formation. When BC is allowed

The impact of residential combustion emissions on atmospheric aerosol, human health, and climate

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E. W. Butt

2016-01-01

Full Text Available Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC and organic carbon (OC mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5 concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (>  30 years of age premature mortality (due to both cardiopulmonary disease and lung cancer to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range for monthly varying residential emissions and 517 000 (192 000–827 000 when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the

Aerosol Emissions from Fuse-Deposition Modeling 3D Printers in a Chamber and in Real Indoor Environments.

Science.gov (United States)

Vance, Marina E; Pegues, Valerie; Van Montfrans, Schuyler; Leng, Weinan; Marr, Linsey C

2017-09-05

Three-dimensional (3D) printers are known to emit aerosols, but questions remain about their composition and the fundamental processes driving emissions. The objective of this work was to characterize the aerosol emissions from the operation of a fuse-deposition modeling 3D printer. We modeled the time- and size-resolved emissions of submicrometer aerosols from the printer in a chamber study, gained insight into the chemical composition of emitted aerosols using Raman spectroscopy, and measured the potential for exposure to the aerosols generated by 3D printers under real-use conditions in a variety of indoor environments. The average aerosol emission rates ranged from ∼10 8 to ∼10 11 particles min -1 , and the rates varied over the course of a print job. Acrylonitrile butadiene styrene (ABS) filaments generated the largest number of aerosols, and wood-infused polylactic acid (PLA) filaments generated the smallest amount. The emission factors ranged from 6 × 10 8 to 6 × 10 11 per gram of printed part, depending on the type of filament used. For ABS, the Raman spectra of the filament and the printed part were indistinguishable, while the aerosol spectra lacked important peaks corresponding to styrene and acrylonitrile, which are both present in ABS. This observation suggests that aerosols are not a result of volatilization and subsequent nucleation of ABS or direct release of ABS aerosols.

A new oxidation flow reactor for measuring secondary aerosol formation of rapidly changing emission sources

Science.gov (United States)

Simonen, Pauli; Saukko, Erkka; Karjalainen, Panu; Timonen, Hilkka; Bloss, Matthew; Aakko-Saksa, Päivi; Rönkkö, Topi; Keskinen, Jorma; Dal Maso, Miikka

2017-04-01

Oxidation flow reactors (OFRs) or environmental chambers can be used to estimate secondary aerosol formation potential of different emission sources. Emissions from anthropogenic sources, such as vehicles, often vary on short timescales. For example, to identify the vehicle driving conditions that lead to high potential secondary aerosol emissions, rapid oxidation of exhaust is needed. However, the residence times in environmental chambers and in most oxidation flow reactors are too long to study these transient effects ( ˜ 100 s in flow reactors and several hours in environmental chambers). Here, we present a new oxidation flow reactor, TSAR (TUT Secondary Aerosol Reactor), which has a short residence time ( ˜ 40 s) and near-laminar flow conditions. These improvements are achieved by reducing the reactor radius and volume. This allows studying, for example, the effect of vehicle driving conditions on the secondary aerosol formation potential of the exhaust. We show that the flow pattern in TSAR is nearly laminar and particle losses are negligible. The secondary organic aerosol (SOA) produced in TSAR has a similar mass spectrum to the SOA produced in the state-of-the-art reactor, PAM (potential aerosol mass). Both reactors produce the same amount of mass, but TSAR has a higher time resolution. We also show that TSAR is capable of measuring the secondary aerosol formation potential of a vehicle during a transient driving cycle and that the fast response of TSAR reveals how different driving conditions affect the amount of formed secondary aerosol. Thus, TSAR can be used to study rapidly changing emission sources, especially the vehicular emissions during transient driving.

Emission of intermediate, semi and low volatile organic compounds from traffic and their impact on secondary organic aerosol concentrations over Greater Paris

Science.gov (United States)

Sartelet, K.; Zhu, S.; Moukhtar, S.; André, M.; André, J. M.; Gros, V.; Favez, O.; Brasseur, A.; Redaelli, M.

2018-05-01

Exhaust particle emissions are mostly made of black carbon and/or organic compounds, with some of these organic compounds existing in both the gas and particle phases. Although emissions of volatile organic compounds (VOC) are usually measured at the exhaust, emissions in the gas phase of lower volatility compounds (POAvapor) are not. However, these gas-phase emissions may be oxidised after emission and enhance the formation of secondary organic aerosols (SOA). They are shown here to contribute to most of the SOA formation in Central Paris. POAvapor emissions are usually estimated from primary organic aerosol emissions in the particle phase (POA). However, they could also be estimated from VOC emissions for both gasoline and diesel vehicles using previously published measurements from chamber measurements. Estimating POAvapor from VOC emissions and ageing exhaust emissions with a simple model included in the Polyphemus air-quality platform compare well to measurements of SOA formation performed in chamber experiments. Over Greater Paris, POAvapor emissions estimated using POA and VOC emissions are compared using the HEAVEN bottom-up traffic emissions model. The impact on the simulated atmospheric concentrations is then assessed using the Polyphemus/Polair3D chemistry-transport model. Estimating POAvapor emissions from VOC emissions rather than POA emissions lead to lower emissions along motorway axes (between -50% and -70%) and larger emissions in urban areas (up to between +120% and +140% in Central Paris). The impact on total organic aerosol concentrations (gas plus particle) is lower than the impact on emissions: between -8% and 25% along motorway axes and in urban areas respectively. Particle-phase organic concentrations are lower when POAvapor emissions are estimated from VOC than POA emissions, even in Central Paris where the total organic aerosol concentration is higher, because of different assumptions on the emission volatility distribution, stressing the

Characterization of fresh and aged organic aerosol emissions from meat charbroiling

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C. Kaltsonoudis

2017-06-01

Full Text Available Cooking emissions can be a significant source of fine particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. Greek souvlakia with pork were cooked using a commercial charbroiler and a fraction of the emissions were introduced into a smog chamber where after a characterization phase they were exposed to UV illumination and oxidants. The particulate and gas phases were characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS and a proton-transfer-reaction mass spectrometer (PTR-MS correspondingly. More than 99 % of the aerosol emitted was composed of organic compounds, while black carbon (BC contributed 0.3 % and the inorganic species less than 0.5 % of the total aerosol mass. The initial O  :  C ratio was approximately 0.09 and increased up to 0.30 after a few hours of chemical aging (exposures of 1010 molecules cm−3 s for OH and 100 ppb h for ozone. The initial and aged AMS spectra differed considerably (θ =  27°. Ambient measurements were also conducted during Fat Thursday in Patras, Greece, when traditionally meat is charbroiled everywhere in the city. Positive matrix factorization (PMF revealed that cooking organic aerosol (COA reached up to 85 % of the total OA from 10:00 to 12:00 LST that day. The ambient COA factor in two major Greek cities had a mass spectrum during spring and summer similar to the aged meat charbroiling emissions. In contrast, the ambient COA factor during winter resembled strongly the fresh laboratory meat charbroiling emissions.

Primary sources of PM2.5 organic aerosol in an industrial Mediterranean city, Marseille

Science.gov (United States)

El Haddad, I.; Marchand, N.; Wortham, H.; Piot, C.; Besombes, J.-L.; Cozic, J.; Chauvel, C.; Armengaud, A.; Robin, D.; Jaffrezo, J.-L.

2011-03-01

Marseille, the most important port of the Mediterranean Sea, represents a challenging case study for source apportionment exercises, combining an active photochemistry and multiple emission sources, including fugitive emissions from industrial sources and shipping. This paper presents a Chemical Mass Balance (CMB) approach based on organic markers and metals to apportion the primary sources of organic aerosol in Marseille, with a special focus on industrial emissions. Overall, the CMB model accounts for the major primary anthropogenic sources including motor vehicles, biomass burning and the aggregate emissions from three industrial processes (heavy fuel oil combustion/shipping, coke production and steel manufacturing) as well as some primary biogenic emissions. This source apportionment exercise is well corroborated by 14C measurements. Primary OC estimated by the CMB accounts on average for 22% of total OC and is dominated by the vehicular emissions that contribute on average for 17% of OC mass concentration (vehicular PM contributes for 17% of PM2.5). Even though industrial emissions contribute only 2.3% of the total OC (7% of PM2.5), they are associated with ultrafine particles (Dpheavy metals such as Pb, Ni and V. On one hand, given that industrial emissions governed key primary markers, their omission would lead to substantial uncertainties in the CMB analysis performed in areas heavily impacted by such sources, hindering accurate estimation of non-industrial primary sources and secondary sources. On the other hand, being associated with bursts of submicron particles and carcinogenic and mutagenic components such as PAH, these emissions are most likely related with acute ill-health outcomes and should be regulated despite their small contributions to OC. Another important result is the fact that 78% of OC mass cannot be attributed to the major primary sources and, thus, remains un-apportioned. We have consequently critically investigated the uncertainties

Changes in future air quality, deposition, and aerosol-cloud interactions under future climate and emission scenarios

Energy Technology Data Exchange (ETDEWEB)

Glotfelty, Timothy; Zhang, Yang; Karamchandani, Prakash; Streets, David G.

2016-08-01

The prospect of global climate change will have wide scale impacts, such as ecological stress and human health hazards. One aspect of concern is future changes in air quality that will result from changes in both meteorological forcing and air pollutant emissions. In this study, the GU-WRF/Chem model is employed to simulate the impact of changing climate and emissions following the IPCC AR4 SRES A1B scenario. An average of 4 future years (2020, 2030, 2040, and 2050) is compared against an average of 2 current years (2001 and 2010). Under this scenario, by the Mid-21st century global air quality is projected to degrade with a global average increase of 2.5 ppb in the maximum 8-hr O₃ level and of 0.3 mg m³ in 24-hr average PM2.5. However, PM2.5 changes are more regional due to regional variations in primary aerosol emissions and emissions of gaseous precursor for secondary PM2.5. Increasing NOx emissions in this scenario combines with a wetter climate elevating levels of OH, HO₂, H₂O₂, and the nitrate radical and increasing the atmosphere’s near surface oxidation state. This differs from findings under the RCP scenarios that experience declines in OH from reduced NOx emissions, stratospheric recovery of O₃, and increases in CH₄ and VOCs. Increasing NO_x and O₃ levels enhances the nitrogen and O₃ deposition, indicating potentially enhanced crop damage and ecosystem stress under this scenario. The enhanced global aerosol level results in enhancements in aerosol optical depth, cloud droplet number concentration, and cloud optical thickness. This leads to dimming at the Earth’s surface with a global average reduction in shortwave radiation of 1.2 W m² . This enhanced dimming leads to a more moderate warming trend and different trends in radiation than those found in NCAR’s CCSM simulation, which does not include the advanced chemistry and aerosol

Secondary organic aerosol formation from road vehicle emissions

Science.gov (United States)

Pieber, Simone M.; Platt, Stephen M.; El Haddad, Imad; Zardini, Alessandro A.; Suarez-Bertoa, Ricardo; Slowik, Jay G.; Huang, Ru-Jin; Hellebust, Stig; Temime-Roussel, Brice; Marchand, Nicolas; Drinovec, Luca; Mocnik, Grisa; Baltensperger, Urs; Astorga, Covadogna; Prévôt, André S. H.

2014-05-01

Organic aerosol particles (OA) are a major fraction of the submicron particulate matter. OA consists of directly emitted primary (POA) and secondary OA (SOA). SOA is formed in-situ in the atmosphere via the reaction of volatile organic precursors. The partitioning of SOA species depends not only on the exposure to oxidants, but for instance also on temperature, relative humidity (RH), and the absorptive mass chemical composition (presence of inorganics) and concentration. Vehicle exhaust is a known source of POA and likely contributes to SOA formation in urban areas [1;2]. This has recently been estimated by (i) analyzing ambient data from urban areas combined with fuel consumption data [3], (ii) by examining the chemical composition of raw fuels [4], or (iii) smog chamber studies [5, 6]. Contradictory and thus somewhat controversial results in the relative quantity of SOA from diesel vs. gasoline vehicle exhaust were observed. In order to elucidate the impact of variable ambient conditions on the potential SOA formation of vehicle exhaust, and its relation to the emitted gas phase species, we studied SOA formed from the exhaust of passenger cars and trucks as a function of fuel and engine type (gasoline, diesel) at different temperatures (T 22 vs. -7oC) and RH (40 vs. 90%), as well as with different levels of inorganic salt concentrations. The exhaust was sampled at the tailpipe during regulatory driving cycles on chassis dynamometers, diluted (200 - 400x) and introduced into the PSI mobile smog chamber [6], where the emissions were subjected to simulated atmospheric ageing. Particle phase instruments (HR-ToF-AMS, aethalometers, CPC, SMPS) and gas phase instruments (PTR-TOF-MS, CO, CO2, CH4, THC, NH3 and other gases) were used online during the experiments. We found that gasoline emissions, because of cold starts, were generally larger than diesel, especially during cold temperatures driving cycles. Gasoline vehicles also showed the highest SOA formation

Assessment of Biomass Burning Smoke Influence on Environmental Conditions for Multi-Year Tornado Outbreaks by Combining Aerosol-Aware Microphysics and Fire Emission Constraints

Science.gov (United States)

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; Da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2016-01-01

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRFChem for its use in applications such as NWP and cloud-resolving simulations.

Highly controlled, reproducible measurements of aerosol emissions from combustion of a common African biofuel source

Directory of Open Access Journals (Sweden)

S. L. Haslett

2018-01-01

Full Text Available Particulate emissions from biomass burning can both alter the atmosphere's radiative balance and cause significant harm to human health. However, due to the large effect on emissions caused by even small alterations to the way in which a fuel burns, it is difficult to study particulate production of biomass combustion mechanistically and in a repeatable manner. In order to address this gap, in this study, small wood samples sourced from Côte D'Ivoire in West Africa were burned in a highly controlled laboratory environment. The shape and mass of samples, available airflow and surrounding thermal environment were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. This methodology produced remarkably repeatable results, allowing aerosol emissions to be mapped directly onto different phases of combustion. Emissions from pyrolysis were visible as a distinct phase before flaming was established. After flaming combustion was initiated, a black-carbon-dominant flame was observed during which very little organic aerosol was produced, followed by a period that was dominated by organic-carbon-producing smouldering combustion, despite the presence of residual flaming. During pyrolysis and smouldering, the two phases producing organic aerosol, distinct mass spectral signatures that correspond to previously reported variations in biofuel emissions measured in the atmosphere are found. Organic aerosol emission factors averaged over an entire combustion event were found to be representative of the time spent in the pyrolysis and smouldering phases, rather than reflecting a coupling between emissions and the mass loss of the sample. Further exploration of aerosol yields from similarly carefully controlled fires and a careful comparison with data from macroscopic fires and real-world emissions will help to deliver

Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols

Energy Technology Data Exchange (ETDEWEB)

Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.

2013-05-10

Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of SOA generated from two monoterpenes, limonene and a-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ~100 ppb ammonia vapor in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (~0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for excitation = 420+- 50 nm and emission = 475 +- 38 nm. The window of the strongest fluorescence shifted to excitation = 320 +- 25 nm and emission = 425 +- 38 nm for the a-pinene-derived SOA. Both regions overlap with the excitation-emission matrix (EEM) spectra of some of the fluorophores found in primary biological aerosols. Our study suggests that, despite the low quantum yield, the aged SOA particles should have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

Wildland fire emissions, carbon, and climate: Emission factors

Science.gov (United States)

Shawn Urbanski

2014-01-01

While the vast majority of carbon emitted by wildland fires is released as CO2, CO, and CH4, wildland fire smoke is nonetheless a rich and complex mixture of gases and aerosols. Primary emissions include significant amounts of CH4 and aerosol (organic aerosol and black carbon), which are short-lived climate forcers. In addition to CO2 and short-lived climate forcers,...

Time-resolved characterization of primary emissions from residential wood combustion appliances.

Science.gov (United States)

Heringa, M F; DeCarlo, P F; Chirico, R; Lauber, A; Doberer, A; Good, J; Nussbaumer, T; Keller, A; Burtscher, H; Richard, A; Miljevic, B; Prevot, A S H; Baltensperger, U

2012-10-16

Primary emissions from a log wood burner and a pellet boiler were characterized by online measurements of the organic aerosol (OA) using a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and of black carbon (BC). The OA and BC concentrations measured during the burning cycle of the log wood burner, batch wise fueled with wood logs, were highly variable and generally dominated by BC. The emissions of the pellet burner had, besides inorganic material, a high fraction of OA and a minor contribution of BC. However, during artificially induced poor burning BC was the dominating species with ∼80% of the measured mass. The elemental O:C ratio of the OA was generally found in the range of 0.2-0.5 during the startup phase or after reloading of the log wood burner. During the burnout or smoldering phase, O:C ratios increased up to 1.6-1.7, which is similar to the ratios found for the pellet boiler during stable burning conditions and higher than the O:C ratios observed for highly aged ambient OA. The organic emissions of both burners have a very similar H:C ratio at a given O:C ratio and therefore fall on the same line in the Van Krevelen diagram.

Factors Affecting Aerosol Radiative Forcing

Science.gov (United States)

Wang, J.; Lin, J.; Ni, R.

2016-12-01

Rapid industrial and economic growth has meant large amount of aerosols in the atmosphere with strong radiative forcing (RF) upon the climate system. Over parts of the globe, the negative forcing of aerosols has overcompensated for the positive forcing of greenhouse gases. Aerosol RF is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. In this study, we analyze the major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA), and black carbon (BC). We analyze the RFof aerosols produced by 11 major regions across the globe, including but not limited to East Asia, Southeast Asia, South Asia, North America, and Western Europe. Factors analyzed include population size, per capita gross domestic production (GDP), emission intensity (i.e., emissionsper unit GDP), chemical efficiency (i.e., mass per unit emissions) and radiative efficiency (i.e., RF per unit mass). We find that among the 11 regions, East Asia produces the largest emissions and aerosol RF, due to relatively high emission intensity and a tremendous population size.South Asia produce the second largest RF of SIOA and BC and the highest RF of POA, in part due to its highest chemical efficiency among all regions. Although Southeast Asia also has large emissions,its aerosol RF is alleviated by its lowest chemical efficiency.The chemical efficiency and radiative efficiency of BC produced by the Middle East-North Africa are the highest across the regions, whereas its RF is loweredbyasmall per capita GDP.Both North America and Western Europe have low emission intensity, compensating for the effects on RF of large population sizes and per capita GDP. There has been a momentum to transfer industries to Southeast Asia and South Asia, and such transition is expected to continue in the coming years. The resulting

Contribution of fungi to primary biogenic aerosols in the atmosphere: wet and dry discharged spores, carbohydrates, and inorganic ions

Directory of Open Access Journals (Sweden)

W. Elbert

2007-09-01

Full Text Available Biogenic aerosols play important roles in atmospheric chemistry physics, the biosphere, climate, and public health. Here, we show that fungi which actively discharge their spores with liquids into the air, in particular actively wet spore discharging Ascomycota (AAM and actively wet spore discharging Basidiomycota (ABM, are a major source of primary biogenic aerosol particles and components. We present the first estimates for the global average emission rates of fungal spores.

Measurement results and budget calculations based on investigations in Amazonia (Balbina, Brazil, July 2001 indicate that the spores of AAM and ABM may account for a large proportion of coarse particulate matter in tropical rainforest regions during the wet season (0.7–2.3 μg m⁻³. For the particle diameter range of 1–10 μm, the estimated proportions are ~25% during day-time, ~45% at night, and ~35% on average. For the sugar alcohol mannitol, the budget calculations indicate that it is suitable for use as a molecular tracer for actively wet discharged basidiospores (ABS. ABM emissions seem to account for most of the atmospheric abundance of mannitol (10–68 ng m⁻³, and can explain the observed diurnal cycle (higher abundance at night. ABM emissions of hexose carbohydrates might also account for a significant proportion of glucose and fructose in air particulate matter (7–49 ng m⁻³, but the literature-derived ratios are not consistent with the observed diurnal cycle (lower abundance at night. AAM emissions appear to account for a large proportion of potassium in air particulate matter over tropical rainforest regions during the wet season (17–43 ng m⁻³, and they can also explain the observed diurnal cycle (higher abundance at night. The results of our investigations and budget calculations for tropical rainforest aerosols are consistent with measurements performed at other locations.

Based on

Modeling Secondary Organic Aerosol Formation From Emissions of Combustion Sources

Science.gov (United States)

Jathar, Shantanu Hemant

Atmospheric aerosols exert a large influence on the Earth's climate and cause adverse public health effects, reduced visibility and material degradation. Secondary organic aerosol (SOA), defined as the aerosol mass arising from the oxidation products of gas-phase organic species, accounts for a significant fraction of the submicron atmospheric aerosol mass. Yet, there are large uncertainties surrounding the sources, atmospheric evolution and properties of SOA. This thesis combines laboratory experiments, extensive data analysis and global modeling to investigate the contribution of semi-volatile and intermediate volatility organic compounds (SVOC and IVOC) from combustion sources to SOA formation. The goals are to quantify the contribution of these emissions to ambient PM and to evaluate and improve models to simulate its formation. To create a database for model development and evaluation, a series of smog chamber experiments were conducted on evaporated fuel, which served as surrogates for real-world combustion emissions. Diesel formed the most SOA followed by conventional jet fuel / jet fuel derived from natural gas, gasoline and jet fuel derived from coal. The variability in SOA formation from actual combustion emissions can be partially explained by the composition of the fuel. Several models were developed and tested along with existing models using SOA data from smog chamber experiments conducted using evaporated fuel (this work, gasoline, fischertropschs, jet fuel, diesels) and published data on dilute combustion emissions (aircraft, on- and off-road gasoline, on- and off-road diesel, wood burning, biomass burning). For all of the SOA data, existing models under-predicted SOA formation if SVOC/IVOC were not included. For the evaporated fuel experiments, when SVOC/IVOC were included predictions using the existing SOA model were brought to within a factor of two of measurements with minor adjustments to model parameterizations. Further, a volatility

Effect of aircraft exhaust sulfur emissions on near field plume aerosols

Energy Technology Data Exchange (ETDEWEB)

Brown, R.C.; Miake-Lye, R.C.; Anderson, M.R.; Kolb, C.E. [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

1997-12-31

Based on estimated exit plane sulfur speciation, a two dimensional, axisymmetric flow field model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the engine on the formation and growth of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols in the near field plume. The conversion of fuel sulfur to sulfur trioxide and sulfuric acid in the engine is predicted to significantly increase the number density and surface area density of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols and the chemical activation of exhaust soot particulates. This analysis indicates the need for experimental measurements of exhaust SO{sub x} emissions to fully assess the atmospheric impact of aircraft emissions. (author) 18 refs.; Submitted to Geophysical Research Letters

Effect of aircraft exhaust sulfur emissions on near field plume aerosols

Energy Technology Data Exchange (ETDEWEB)

Brown, R C; Miake-Lye, R C; Anderson, M R; Kolb, C E [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

1998-12-31

Based on estimated exit plane sulfur speciation, a two dimensional, axisymmetric flow field model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the engine on the formation and growth of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols in the near field plume. The conversion of fuel sulfur to sulfur trioxide and sulfuric acid in the engine is predicted to significantly increase the number density and surface area density of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols and the chemical activation of exhaust soot particulates. This analysis indicates the need for experimental measurements of exhaust SO{sub x} emissions to fully assess the atmospheric impact of aircraft emissions. (author) 18 refs.; Submitted to Geophysical Research Letters

A global perspective on aerosol from low-volatility organic compounds

Directory of Open Access Journals (Sweden)

H. O. T. Pye

2010-05-01

Full Text Available Global production of organic aerosol from primary emissions of semivolatile (SVOCs and intermediate (IVOCs volatility organic compounds is estimated using the global chemical transport model, GEOS-Chem. SVOC oxidation is predicted to be a larger global source of net aerosol production than oxidation of traditional parent hydrocarbons (terpenes, isoprene, and aromatics. Using a prescribed rate constant and reduction in volatility for atmospheric oxidation, the yield of aerosol from SVOCs is predicted to be about 75% on a global, annually-averaged basis. For IVOCs, the use of a naphthalene-like surrogate with different high-NO_x and low-NO_x parameterizations produces a global aerosol yield of about 30%, or roughly 5 Tg/yr of aerosol. Estimates of the total global organic aerosol source presented here range between 60 and 100 Tg/yr. This range reflects uncertainty in the parameters for SVOC volatility, SVOC oxidation, SVOC emissions, and IVOC emissions, as well as wet deposition. The highest estimates result if SVOC emissions are significantly underestimated (by more than a factor of 2 or if wet deposition of the gas-phase semivolatile species is less effective than previous estimates. A significant increase in SVOC emissions, a reduction of the volatility of the SVOC emissions, or an increase in the enthalpy of vaporization of the organic aerosol all lead to an appreciable reduction of prediction/measurement discrepancy. In addition, if current primary organic aerosol (POA inventories capture only about one-half of the SVOC emission and the Henrys Law coefficient for oxidized semivolatiles is on the order of 10³ M/atm, a global estimate of OA production is not inconsistent with the top-down estimate of 140 Tg/yr by (Goldstein and Galbally, 2007. Additional information is needed to constrain the emissions and treatment of SVOCs and IVOCs, which have traditionally not been included in models.

Measurements of Primary Biogenic Aerosol Particles with an Ultraviolet Aerodynamic Particle Sizer (UVAPS) During AMAZE-08

Science.gov (United States)

Wollny, A. G.; Garland, R.; Pöschl, U.

2008-12-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the AMazonian Aerosol CharacteriZation Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. The presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 μm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as 'viable aerosols' or 'fluorescent bioparticles' (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. First data analyses show a pronounced peak of FBAP at diameters around 2-3 μm. In this size range the biogenic particle fraction was

Impacts of controlling biomass burning emissions on wintertime carbonaceous aerosol in Europe

NARCIS (Netherlands)

Fountoukis, C.; Butler, T.; Lawrence, M.G.; Denier van der Gon, H.A.C.; Visschedijk, A.J.H.; Charalampidis, P.; Pilinis, C.; Pandis, S.N.

2014-01-01

We use a 3-D regional chemical transport model, with the latest advancements in the organic aerosol (OA) treatment, and an updated emission inventory for wood combustion to study the organic aerosol change in response to the replacement of current residential wood combustion technologies with pellet

Long term atmospheric aerosol characterization in the Amazon Basin

Science.gov (United States)

Artaxo, Paulo; Gerab, Fábio; Yamasoe, Marcia A.

This chapter presents a characterization of atmospheric aerosols collected in different places in the Amazon Basin. Both the biogenic aerosol emission from the forest and the particulate material which is emitted to the atmosphere due to the large scale man-made burns during the dry season were studied. The samples were collected during a three year period at three different locations in the Amazon (Cuiabá, Alta Floresta and Serra do Navio), using stacked filter units. Aerosol samples were also collected directly over fires of cerrado vegetation and tropical primary forest burns The samples were analyzed using several techniques for a number of elements. Gravimetric analyses were used to determine the total atmospheric aerosol concentration. Multivariate statistical analysis was used in order to identify and characterize the sources of the atmospheric aerosol present in the sampled regions. Cerrado burning emissions were enriched compared to forest ones, specially for Cl, K and Zn. High atmospheric aerosol concentrations were observed in large amazonian areas due to emissions from man-made burns in the period from June to September. The emissions from burns dominate the fine fraction of the atmospheric aerosol with characteristic high contents of black carbon, S and K. Aerosols emitted in biomass burning process are correlated to the increase in the aerosol optical thickness of the atmosphere during the Amazonian dry season. The Serra do Navio aerosol is characterized by biogenic emissions with strong marine influence. The presence of trace elements characteristic of soil particulate associated with this marine contribution indicates the existence of aerosol transport from Africa to South America. Similar composition characteristics were observed in the biogenic emission aerosols from Serra do Navio and Alta Floresta.

Carbonaceous aerosols over China--review of observations, emissions, and climate forcing.

Science.gov (United States)

Wang, Linpeng; Zhou, Xuehua; Ma, Yujie; Cao, Zhaoyu; Wu, Ruidong; Wang, Wenxing

2016-01-01

Carbonaceous aerosols have been attracting attention due to the influence on visibility, air quality, and regional climate. Statistical analyses based on concentration levels, spatial-temporal variations, correlations, and organic carbon (OC) to element carbon (EC) ratios from published data of OC and EC in particulate matter (PM2.5 and PM10) were carried out in order to give a carbonaceous aerosol profile in China. The results showed maxima for OC of 29.5 ± 18.2 μg C m(-3) and for EC of 8.4 ± 6.3 μg C m(-3) in winter and minima for OC of 12.9 ± 7.7 μg C m(-3) in summer and for EC of 4.6 ± 2.8 μg C m(-3) in spring. In addition, OC and EC both had higher concentrations in urban than those in rural sites. Carbonaceous aerosol levels in China are about three to seven times higher compared to those in the USA and Europe. OC and EC occupied 20 ± 6 and 7 ± 3% of PM2.5 mass and 17 ± 7 and 5 ± 3% of PM10 mass, respectively, implying that carbonaceous aerosols are the main component of PM, especially OC. Secondary organic carbon (SOC) was a significant portion of PM and contributed 41 ± 26% to OC and 8 ± 6% to PM2.5 mass. The OC/EC ratio was 3.63 ± 1.73, which, along with the good correlation between OC and EC and the OC to EC slope of 2.29, signifies that coal combustion and/or vehicular exhaust is the dominated carbonaceous aerosol source in China. These provide a primary observation-based understanding of carbonaceous aerosol pollution in China and have a great significance in improving the emission inventory and climate forcing evaluation.

Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass

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Bahreini, R.; Middlebrook, A. M.; de Gouw, J. A.; Warneke, C.; Trainer, M.; Brock, C. A.; Stark, H.; Brown, S. S.; Dube, W. P.; Gilman, J. B.; Hall, K.; Holloway, J. S.; Kuster, W. C.; Perring, A. E.; Prevot, A. S. H.; Schwarz, J. P.; Spackman, J. R.; Szidat, S.; Wagner, N. L.; Weber, R. J.; Zotter, P.; Parrish, D. D.

2012-03-01

Although laboratory experiments have shown that organic compounds in both gasoline fuel and diesel engine exhaust can form secondary organic aerosol (SOA), the fractional contribution from gasoline and diesel exhaust emissions to ambient SOA in urban environments is poorly known. Here we use airborne and ground-based measurements of organic aerosol (OA) in the Los Angeles (LA) Basin, California made during May and June 2010 to assess the amount of SOA formed from diesel emissions. Diesel emissions in the LA Basin vary between weekdays and weekends, with 54% lower diesel emissions on weekends. Despite this difference in source contributions, in air masses with similar degrees of photochemical processing, formation of OA is the same on weekends and weekdays, within the measurement uncertainties. This result indicates that the contribution from diesel emissions to SOA formation is zero within our uncertainties. Therefore, substantial reductions of SOA mass on local to global scales will be achieved by reducing gasoline vehicle emissions.

Evolution of aerosol downwind of a major highway

Science.gov (United States)

Liggio, J.; Staebler, R. M.; Brook, J.; Li, S.; Vlasenko, A. L.; Sjostedt, S. J.; Gordon, M.; Makar, P.; Mihele, C.; Evans, G. J.; Jeong, C.; Wentzell, J. J.; Lu, G.; Lee, P.

2010-12-01

Primary aerosol from traffic emissions can have a considerable impact local and regional scale air quality. In order to assess the effect of these emissions and of future emissions scenarios, air quality models are required which utilize emissions representative of real world conditions. Often, the emissions processing systems which provide emissions input for the air quality models rely on laboratory testing of individual vehicles under non-ambient conditions. However, on the sub-grid scale particle evolution may lead to changes in the primary emitted size distribution and gas-particle partitioning that are not properly considered when the emissions are ‘instantly mixed’ within the grid volume. The affect of this modeling convention on model results is not well understood. In particular, changes in organic gas/particle partitioning may result in particle evaporation or condensation onto pre-existing aerosol. The result is a change in the particle distribution and/or an increase in the organic mass available for subsequent gas-phase oxidation. These effects may be missing from air-quality models, and a careful analysis of field data is necessary to quantify their impact. A study of the sub-grid evolution of aerosols (FEVER; Fast Evolution of Vehicle Emissions from Roadways) was conducted in the Toronto area in the summer of 2010. The study included mobile measurements of particle size distributions with a Fast mobility particle sizer (FMPS), aerosol composition with an Aerodyne aerosol mass spectrometer (AMS), black carbon (SP2, PA, LII), VOCs (PTR-MS) and other trace gases. The mobile laboratory was used to measure the concentration gradient of the emissions at perpendicular distances from the highway as well as the physical and chemical evolution of the aerosol. Stationary sites at perpendicular distances and upwind from the highway also monitored the particle size distribution. In addition, sonic anemometers mounted on the mobile lab provided measurements of

Modelling carbonaceous aerosol from residential solid fuel burning with different assumptions for emissions

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R. Ots

2018-04-01

Full Text Available Evidence is accumulating that emissions of primary particulate matter (PM from residential wood and coal combustion in the UK may be underestimated and/or spatially misclassified. In this study, different assumptions for the spatial distribution and total emission of PM from solid fuel (wood and coal burning in the UK were tested using an atmospheric chemical transport model. Modelled concentrations of the PM components were compared with measurements from aerosol mass spectrometers at four sites in central and Greater London (ClearfLo campaign, 2012, as well as with measurements from the UK black carbon network.The two main alternative emission scenarios modelled were Base4x and combRedist. For Base4x, officially reported PM2.5 from the residential and other non-industrial combustion source sector were increased by a factor of four. For the combRedist experiment, half of the baseline emissions from this same source were redistributed by residential population density to simulate the effect of allocating some emissions to the smoke control areas (that are assumed in the national inventory to have no emissions from this source. The Base4x scenario yielded better daily and hourly correlations with measurements than the combRedist scenario for year-long comparisons of the solid fuel organic aerosol (SFOA component at the two London sites. However, the latter scenario better captured mean measured concentrations across all four sites. A third experiment, Redist – all emissions redistributed linearly to population density, is also presented as an indicator of the maximum concentrations an assumption like this could yield.The modelled elemental carbon (EC concentrations derived from the combRedist experiments also compared well with seasonal average concentrations of black carbon observed across the network of UK sites. Together, the two model scenario simulations of SFOA and EC suggest both that residential solid fuel emissions may be higher than

Modelling carbonaceous aerosol from residential solid fuel burning with different assumptions for emissions

Science.gov (United States)

Ots, Riinu; Heal, Mathew R.; Young, Dominique E.; Williams, Leah R.; Allan, James D.; Nemitz, Eiko; Di Marco, Chiara; Detournay, Anais; Xu, Lu; Ng, Nga L.; Coe, Hugh; Herndon, Scott C.; Mackenzie, Ian A.; Green, David C.; Kuenen, Jeroen J. P.; Reis, Stefan; Vieno, Massimo

2018-04-01

Evidence is accumulating that emissions of primary particulate matter (PM) from residential wood and coal combustion in the UK may be underestimated and/or spatially misclassified. In this study, different assumptions for the spatial distribution and total emission of PM from solid fuel (wood and coal) burning in the UK were tested using an atmospheric chemical transport model. Modelled concentrations of the PM components were compared with measurements from aerosol mass spectrometers at four sites in central and Greater London (ClearfLo campaign, 2012), as well as with measurements from the UK black carbon network.The two main alternative emission scenarios modelled were Base4x and combRedist. For Base4x, officially reported PM2.5 from the residential and other non-industrial combustion source sector were increased by a factor of four. For the combRedist experiment, half of the baseline emissions from this same source were redistributed by residential population density to simulate the effect of allocating some emissions to the smoke control areas (that are assumed in the national inventory to have no emissions from this source). The Base4x scenario yielded better daily and hourly correlations with measurements than the combRedist scenario for year-long comparisons of the solid fuel organic aerosol (SFOA) component at the two London sites. However, the latter scenario better captured mean measured concentrations across all four sites. A third experiment, Redist - all emissions redistributed linearly to population density, is also presented as an indicator of the maximum concentrations an assumption like this could yield.The modelled elemental carbon (EC) concentrations derived from the combRedist experiments also compared well with seasonal average concentrations of black carbon observed across the network of UK sites. Together, the two model scenario simulations of SFOA and EC suggest both that residential solid fuel emissions may be higher than inventory

Long-term trends in California mobile source emissions and ambient concentrations of black carbon and organic aerosol.

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McDonald, Brian C; Goldstein, Allen H; Harley, Robert A

2015-04-21

A fuel-based approach is used to assess long-term trends (1970-2010) in mobile source emissions of black carbon (BC) and organic aerosol (OA, including both primary emissions and secondary formation). The main focus of this analysis is the Los Angeles Basin, where a long record of measurements is available to infer trends in ambient concentrations of BC and organic carbon (OC), with OC used here as a proxy for OA. Mobile source emissions and ambient concentrations have decreased similarly, reflecting the importance of on- and off-road engines as sources of BC and OA in urban areas. In 1970, the on-road sector accounted for ∼90% of total mobile source emissions of BC and OA (primary + secondary). Over time, as on-road engine emissions have been controlled, the relative importance of off-road sources has grown. By 2010, off-road engines were estimated to account for 37 ± 20% and 45 ± 16% of total mobile source contributions to BC and OA, respectively, in the Los Angeles area. This study highlights both the success of efforts to control on-road emission sources, and the importance of considering off-road engine and other VOC source contributions when assessing long-term emission and ambient air quality trends.

Could aerosol emissions be used for regional heat wave mitigation?

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D. N. Bernstein

2013-07-01

Full Text Available Geoengineering applications by injection of sulfate aerosols into the stratosphere are under consideration as a measure of last resort to counter global warming. Here a potential regional-scale application to offset the impacts of heat waves is critically examined. Using the Weather Research and Forecasting model with fully coupled chemistry (WRF-Chem, the effect of regional-scale sulfate aerosol emission over California in each of two days of the July 2006 heat wave is used to quantify potential reductions in surface temperature as a function of emission rates in a layer at 12 km altitude. Local meteorological factors yield geographical differences in surface air temperature sensitivity. For emission rates of approximately 30 μg m−2 s−1 of sulfate aerosols (with standard WRF-Chem size distribution over the region, temperature decreases of around 7 °C result during the middle part of the day over the Central Valley, one of the areas hardest hit by the heat wave. Regions more ventilated with oceanic air such as Los Angeles have slightly smaller reductions. The length of the hottest part of the day is also reduced. Advection effects on the aerosol cloud must be more carefully forecast for smaller injection regions. Verification of the impacts could be done via measurements of differences in reflected and surface downward shortwave. Such regional geoengineering applications with specific near-term target effects but smaller cost and side effects could potentially provide a means of testing larger scale applications. However, design considerations for regional applications, such as a preference for injection at a level of relatively low wind speed, differ from those for global applications. The size of the required injections and the necessity of injection close to the target region raise substantial concerns. The evaluation of this regional-scale application is thus consistent with global model evaluations, emphasizing that mitigation via

Aerosol modelling and validation during ESCOMPTE 2001

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Cousin, F.; Liousse, C.; Cachier, H.; Bessagnet, B.; Guillaume, B.; Rosset, R.

The ESCOMPTE 2001 programme (Atmospheric Research. 69(3-4) (2004) 241) has resulted in an exhaustive set of dynamical, radiative, gas and aerosol observations (surface and aircraft measurements). A previous paper (Atmospheric Research. (2004) in press) has dealt with dynamics and gas-phase chemistry. The present paper is an extension to aerosol formation, transport and evolution. To account for important loadings of primary and secondary aerosols and their transformation processes in the ESCOMPTE domain, the ORISAM aerosol module (Atmospheric Environment. 35 (2001) 4751) was implemented on-line in the air-quality Meso-NH-C model. Additional developments have been introduced in ORganic and Inorganic Spectral Aerosol Module (ORISAM) to improve the comparison between simulations and experimental surface and aircraft field data. This paper discusses this comparison for a simulation performed during one selected day, 24 June 2001, during the Intensive Observation Period IOP2b. Our work relies on BC and OCp emission inventories specifically developed for ESCOMPTE. This study confirms the need for a fine resolution aerosol inventory with spectral chemical speciation. BC levels are satisfactorily reproduced, thus validating our emission inventory and its processing through Meso-NH-C. However, comparisons for reactive species generally denote an underestimation of concentrations. Organic aerosol levels are rather well simulated though with a trend to underestimation in the afternoon. Inorganic aerosol species are underestimated for several reasons, some of them have been identified. For sulphates, primary emissions were introduced. Improvement was obtained too for modelled nitrate and ammonium levels after introducing heterogeneous chemistry. However, no modelling of terrigeneous particles is probably a major cause for nitrates and ammonium underestimations. Particle numbers and size distributions are well reproduced, but only in the submicrometer range. Our work points out

Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks

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Th. F. Mentel

2013-09-01

Full Text Available Atmospheric aerosols impact climate by scattering and absorbing solar radiation and by acting as ice and cloud condensation nuclei. Biogenic secondary organic aerosols (BSOAs comprise an important component of atmospheric aerosols. Biogenic volatile organic compounds (BVOCs emitted by vegetation are the source of BSOAs. Pathogens and insect attacks, heat waves and droughts can induce stress to plants that may impact their BVOC emissions, and hence the yield and type of formed BSOAs, and possibly their climatic effects. This raises questions of whether stress-induced changes in BSOA formation may attenuate or amplify effects of climate change. In this study we assess the potential impact of stress-induced BVOC emissions on BSOA formation for tree species typical for mixed deciduous and Boreal Eurasian forests. We studied the photochemical BSOA formation for plants infested by aphids in a laboratory setup under well-controlled conditions and applied in addition heat and drought stress. The results indicate that stress conditions substantially modify BSOA formation and yield. Stress-induced emissions of sesquiterpenes, methyl salicylate, and C17-BVOCs increase BSOA yields. Mixtures including these compounds exhibit BSOA yields between 17 and 33%, significantly higher than mixtures containing mainly monoterpenes (4–6% yield. Green leaf volatiles suppress SOA formation, presumably by scavenging OH, similar to isoprene. By classifying emission types, stressors and BSOA formation potential, we discuss possible climatic feedbacks regarding aerosol effects. We conclude that stress situations for plants due to climate change should be considered in climate–vegetation feedback mechanisms.

Characterizing the influence of anthropogenic emissions and transport variability on sulfate aerosol concentrations at Mauna Loa Observatory

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Potter, Lauren E.

Sulfate aerosol in the atmosphere has substantial impacts on human health and environmental quality. Most notably, atmospheric sulfate has the potential to modify the earth's climate system through both direct and indirect radiative forcing mechanisms (Meehl et al., 2007). Emissions of sulfur dioxide, the primary precursor of sulfate aerosol, are now globally dominated by anthropogenic sources as a result of widespread fossil fuel combustion. Economic development in Asian countries since 1990 has contributed considerably to atmospheric sulfur loading, particularly China, which currently emits approximately 1/3 of global anthropogenic SO2 (Klimont et al., 2013). Observational and modeling studies have confirmed that anthropogenic pollutants from Asian sources can be transported long distances with important implications for future air quality and global climate change. Located in the remote Pacific Ocean (19.54°N, 155.58°W) at an elevation of 3.4 kilometers above sea level, Mauna Loa Observatory (MLO) is an ideal measurement site for ground-based, free tropospheric observations and is well situated to experience influence from springtime Asian outflow. This study makes use of a 14-year data set of aerosol ionic composition, obtained at MLO by the University of Hawaii at Manoa. Daily filter samples of total aerosol concentrations were made during nighttime downslope (free-tropospheric) transport conditions, from 1995 to 2008, and were analyzed for aerosol-phase concentrations of the following species: nitrate (NO3-), sulfate (SO42-), methanesulfonate (MSA), chloride (Cl-), oxalate, sodium (Na+), ammonium (NH 4+), potassium (K+), magnesium (Mg 2+), and calcium (Ca2+). An understanding of the factors controlling seasonal and interannual variations in aerosol speciation and concentrations at this site is complicated by the relatively short lifetimes of aerosols, compared with greenhouse gases which have also been sampled over long time periods at MLO. Aerosol filter

Future premature mortality due to O3, secondary inorganic aerosols and primary PM in Europe--sensitivity to changes in climate, anthropogenic emissions, population and building stock.

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Geels, Camilla; Andersson, Camilla; Hänninen, Otto; Lansø, Anne Sofie; Schwarze, Per E; Skjøth, Carsten Ambelas; Brandt, Jørgen

2015-03-04

Air pollution is an important environmental factor associated with health impacts in Europe and considerable resources are used to reduce exposure to air pollution through emission reductions. These reductions will have non-linear effects on exposure due, e.g., to interactions between climate and atmospheric chemistry. By using an integrated assessment model, we quantify the effect of changes in climate, emissions and population demography on exposure and health impacts in Europe. The sensitivity to the changes is assessed by investigating the differences between the decades 2000-2009, 2050-2059 and 2080-2089. We focus on the number of premature deaths related to atmospheric ozone, Secondary Inorganic Aerosols and primary PM. For the Nordic region we furthermore include a projection on how population exposure might develop due to changes in building stock with increased energy efficiency. Reductions in emissions cause a large significant decrease in mortality, while climate effects on chemistry and emissions only affects premature mortality by a few percent. Changes in population demography lead to a larger relative increase in chronic mortality than the relative increase in population. Finally, the projected changes in building stock and infiltration rates in the Nordic indicate that this factor may be very important for assessments of population exposure in the future.

Light absorption by primary particle emissions from a lignite burning plant

International Nuclear Information System (INIS)

Bond, T.C.; Bussemer, M.; Wehner, B.; Keller, S.; Charlson, R.J.; Heintzenberg, J.

1999-01-01

Anthropogenic aerosols from the burning of fossil fuels contribute to climate forcing by both scattering and absorbing solar radiation, and estimates of climate forcing by light-absorbing primary particles have recently been published. While the mass and optical properties of emissions are needed for these studies, the available measurements do not characterize the low-technology burning that is thought to contribute a large fraction of light-absorbing material to the global budget. The authors have measured characteristics of particulate matter (PM) emitted from a small, low-technology lignite-burning plant. The PM emission factor is comparable to those used to calculate emission inventories of light-absorbing particles. However, the fine fraction, the absorbing fraction, and the absorption efficiency of the emissions are substantially below assumptions that have been made in inventories of black carbon emissions and calculations of climate forcing. The measurements suggest that nonblack, light-absorbing particles are emitted from low-technology coal burning. As the burning rate increases, the emitted absorption cross-section decreases, and the wavelength dependence of absorption becomes closer to that of black particles

The role of anthropogenic aerosol emission reduction in achieving the Paris Agreement's objective

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Hienola, Anca; Pietikäinen, Joni-Pekka; O'Donnell, Declan; Partanen, Antti-Ilari; Korhonen, Hannele; Laaksonen, Ari

2017-04-01

The Paris agreement reached in December 2015 under the auspices of the United Nation Framework Convention on Climate Change (UNFCCC) aims at holding the global temperature increase to well below 2◦C above preindustrial levels and "to pursue efforts to limit the temperature increase to 1.5◦C above preindustrial levels". Limiting warming to any level implies that the total amount of carbon dioxide (CO2) - the dominant driver of long-term temperatures - that can ever be emitted into the atmosphere is finite. Essentially, this means that global CO2 emissions need to become net zero. CO2 is not the only pollutant causing warming, although it is the most persistent. Short-lived, non-CO2 climate forcers also must also be considered. Whereas much effort has been put into defining a threshold for temperature increase and zero net carbon emissions, surprisingly little attention has been paid to the non-CO2 climate forcers, including not just the non-CO2 greenhouse gases (methane (CH4), nitrous oxide (N2O), halocarbons etc.) but also the anthropogenic aerosols like black carbon (BC), organic carbon (OC) and sulfate. This study investigates the possibility of limiting the temperature increase to 1.5◦C by the end of the century under different future scenarios of anthropogenic aerosol emissions simulated with the very simplistic MAGICC climate carbon cycle model as well as with ECHAM6.1-HAM2.2-SALSA + UVic ESCM. The simulations include two different CO2 scenarios- RCP3PD as control and a CO2 reduction leading to 1.5◦C (which translates into reaching the net zero CO2 emissions by mid 2040s followed by negative emissions by the end of the century); each CO2 scenario includes also two aerosol pollution control cases denoted with CLE (current legislation) and MFR (maximum feasible reduction). The main result of the above scenarios is that the stronger the anthropogenic aerosol emission reduction is, the more significant the temperature increase by 2100 relative to pre

Continental anthropogenic primary particle number emissions

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P. Paasonen

2016-06-01

Full Text Available Atmospheric aerosol particle number concentrations impact our climate and health in ways different from those of aerosol mass concentrations. However, the global, current and future anthropogenic particle number emissions and their size distributions are so far poorly known. In this article, we present the implementation of particle number emission factors and the related size distributions in the GAINS (Greenhouse Gas–Air Pollution Interactions and Synergies model. This implementation allows for global estimates of particle number emissions under different future scenarios, consistent with emissions of other pollutants and greenhouse gases. In addition to determining the general particulate number emissions, we also describe a method to estimate the number size distributions of the emitted black carbon particles. The first results show that the sources dominating the particle number emissions are different to those dominating the mass emissions. The major global number source is road traffic, followed by residential combustion of biofuels and coal (especially in China, India and Africa, coke production (Russia and China, and industrial combustion and processes. The size distributions of emitted particles differ across the world, depending on the main sources: in regions dominated by traffic and industry, the number size distribution of emissions peaks in diameters range from 20 to 50 nm, whereas in regions with intensive biofuel combustion and/or agricultural waste burning, the emissions of particles with diameters around 100 nm are dominant. In the baseline (current legislation scenario, the particle number emissions in Europe, Northern and Southern Americas, Australia, and China decrease until 2030, whereas especially for India, a strong increase is estimated. The results of this study provide input for modelling of the future changes in aerosol–cloud interactions as well as particle number related adverse health effects, e.g. in response

a Study of the Origin of Atmospheric Organic Aerosols

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Hildemann, Lynn Mary

1990-01-01

The sources of ambient organic particulate matter in urban areas are investigated through a program of emission source measurements, atmospheric measurements, and mathematical modeling of source/receptor relationships. A dilution sampler intended to collect fine organic aerosol from combustion sources is designed to simulate atmospheric cooling and dilution processes, so that organic vapors which condense under ambient conditions will be collected as particulate matter. This system is used to measure the emissions from a boiler burning distillate oil, a home fireplace, catalyst and noncatalyst automobiles, heavy-duty diesel trucks, natural gas home appliances, and meat cooking operations. Alternate techniques are used to sample the particulate matter emitted from cigarette smoking, a roofing tar pot, paved road dust, brake lining wear, tire wear, and vegetative detritus. The bulk chemical characteristics of the fine aerosol fraction are presented for each source. Over half of the fine aerosol mass emitted from automobiles, wood burning, meat cooking, home appliances, cigarettes, and tar pots is shown to consist of organic compounds. The organic material collected from these sources is analyzed using high-resolution gas chromatography. Using a simple analytical protocol, a quantitative, 50-parameter characterization of the elutable fine organic aerosol emitted from each source type is obtained, which proves to be a unique fingerprint that can be used to distinguish most sources from each other. A mathematical model is used to predict the characteristics of fine ambient organic aerosol in the Los Angeles area that would prevail if the primary organic emissions are transported without chemical reaction. The model is found to track the seasonal variations observed in the ambient aerosol at the three sites studied. Emissions from vehicles and fireplaces are identified as significant sources of solvent-extractable organic aerosol. Differences between the model

Formation of secondary organic aerosols from gas-phase emissions of heated cooking oils

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T. Liu

2017-06-01

Full Text Available Cooking emissions can potentially contribute to secondary organic aerosol (SOA but remain poorly understood. In this study, formation of SOA from gas-phase emissions of five heated vegetable oils (i.e., corn, canola, sunflower, peanut and olive oils was investigated in a potential aerosol mass (PAM chamber. Experiments were conducted at 19–20 °C and 65–70 % relative humidity (RH. The characterization instruments included a scanning mobility particle sizer (SMPS and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS. The efficiency of SOA production, in ascending order, was peanut oil, olive oil, canola oil, corn oil and sunflower oil. The major SOA precursors from heated cooking oils were related to the content of monounsaturated fat and omega-6 fatty acids in cooking oils. The average production rate of SOA, after aging at an OH exposure of 1. 7 × 1011 molecules cm−3 s, was 1. 35 ± 0. 30 µg min−1, 3 orders of magnitude lower compared with emission rates of fine particulate matter (PM2. 5 from heated cooking oils in previous studies. The mass spectra of cooking SOA highly resemble field-derived COA (cooking-related organic aerosol in ambient air, with R2 ranging from 0.74 to 0.88. The average carbon oxidation state (OSc of SOA was −1.51 to −0.81, falling in the range between ambient hydrocarbon-like organic aerosol (HOA and semi-volatile oxygenated organic aerosol (SV-OOA, indicating that SOA in these experiments was lightly oxidized.

The global impact of the transport sectors on atmospheric aerosol: simulations for year 2000 emissions

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M. Righi

2013-10-01

Full Text Available We use the EMAC (ECHAM/MESSy Atmospheric Chemistry global model with the aerosol module MADE (Modal Aerosol Dynamics model for Europe, adapted for global applications to quantify the impact of transport emissions (land transport, shipping and aviation on the global aerosol. We consider a present-day (2000 scenario according to the CMIP5 (Climate Model Intercomparison Project Phase 5 emission data set developed in support of the IPCC (Intergovernmental Panel on Climate Change Fifth Assessment Report. The model takes into account particle mass and number emissions: The latter are derived from mass emissions under different assumptions on the size distribution of particles emitted by the three transport sectors. Additional sensitivity experiments are performed to quantify the effects of the uncertainties behind such assumptions. The model simulations show that the impact of the transport sectors closely matches the emission patterns. Land transport is the most important source of black carbon (BC pollution in the USA, Europe and the Arabian Peninsula, contributing up to 60–70% of the total surface-level BC concentration in these regions. Shipping contributes about 40–60% of the total aerosol sulfate surface-level concentration along the most-traveled routes of the northern Atlantic and northern Pacific oceans, with a significant impact (~ 10–20% along the coastlines. Aviation mostly affects aerosol number, contributing about 30–40% of the particle number concentration in the northern midlatitudes' upper troposphere (7–12 km, although significant effects are also simulated at the ground, due to the emissions from landing and take-off cycles. The transport-induced perturbations to the particle number concentrations are very sensitive to the assumptions on the size distribution of emitted particles, with the largest uncertainties (about one order of magnitude obtained for the land transport sector. The simulated climate impacts, due to

Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

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Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

2015-06-01

Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

Cloud-Resolving Model Simulations of Aerosol-Cloud Interactions Triggered by Strong Aerosol Emissions in the Arctic

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Wang, H.; Kravitz, B.; Rasch, P. J.; Morrison, H.; Solomon, A.

2014-12-01

Previous process-oriented modeling studies have highlighted the dependence of effectiveness of cloud brightening by aerosols on cloud regimes in warm marine boundary layer. Cloud microphysical processes in clouds that contain ice, and hence the mechanisms that drive aerosol-cloud interactions, are more complicated than in warm clouds. Interactions between ice particles and liquid drops add additional levels of complexity to aerosol effects. A cloud-resolving model is used to study aerosol-cloud interactions in the Arctic triggered by strong aerosol emissions, through either geoengineering injection or concentrated sources such as shipping and fires. An updated cloud microphysical scheme with prognostic aerosol and cloud particle numbers is employed. Model simulations are performed in pure super-cooled liquid and mixed-phase clouds, separately, with or without an injection of aerosols into either a clean or a more polluted Arctic boundary layer. Vertical mixing and cloud scavenging of particles injected from the surface is still quite efficient in the less turbulent cold environment. Overall, the injection of aerosols into the Arctic boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. The pure liquid clouds are more susceptible to the increase in aerosol number concentration than the mixed-phase clouds. Rain production processes are more effectively suppressed by aerosol injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. Aerosol injection into a clean boundary layer results in a greater cloud albedo increase than injection into a polluted one, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, the impact of dynamical feedback due to precipitation changes is small. According to these results, which are dependent upon the representation of ice nucleation

The effect of harmonized emissions on aerosol properties in global models – an AeroCom experiment

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C. Textor

2007-08-01

Full Text Available The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA and one with unified emissions, injection heights, and particle sizes at the source (ExpB. Surprisingly, harmonization of aerosol sources has only a small impact on the simulated inter-model diversity of the global aerosol burden, and consequently global optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols and parameterizations of aerosol microphysics (e.g., the split between deposition pathways and to a lesser extent by the spatial and temporal distributions of the (precursor emissions.

The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversities for these two species were caused by a few outliers. The experiment also showed that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences.

These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies.

Future Premature Mortality Due to O3, Secondary Inorganic Aerosols and Primary PM in Europe — Sensitivity to Changes in Climate, Anthropogenic Emissions, Population and Building Stock

Science.gov (United States)

Geels, Camilla; Andersson, Camilla; Hänninen, Otto; Lansø, Anne Sofie; Schwarze, Per E.; Ambelas Skjøth, Carsten; Brandt, Jørgen

2015-01-01

Air pollution is an important environmental factor associated with health impacts in Europe and considerable resources are used to reduce exposure to air pollution through emission reductions. These reductions will have non-linear effects on exposure due, e.g., to interactions between climate and atmospheric chemistry. By using an integrated assessment model, we quantify the effect of changes in climate, emissions and population demography on exposure and health impacts in Europe. The sensitivity to the changes is assessed by investigating the differences between the decades 2000–2009, 2050–2059 and 2080–2089. We focus on the number of premature deaths related to atmospheric ozone, Secondary Inorganic Aerosols and primary PM. For the Nordic region we furthermore include a projection on how population exposure might develop due to changes in building stock with increased energy efficiency. Reductions in emissions cause a large significant decrease in mortality, while climate effects on chemistry and emissions only affects premature mortality by a few percent. Changes in population demography lead to a larger relative increase in chronic mortality than the relative increase in population. Finally, the projected changes in building stock and infiltration rates in the Nordic indicate that this factor may be very important for assessments of population exposure in the future. PMID:25749320

Future Premature Mortality Due to O3, Secondary Inorganic Aerosols and Primary PM in Europe — Sensitivity to Changes in Climate, Anthropogenic Emissions, Population and Building Stock

Directory of Open Access Journals (Sweden)

Camilla Geels

2015-03-01

Full Text Available Air pollution is an important environmental factor associated with health impacts in Europe and considerable resources are used to reduce exposure to air pollution through emission reductions. These reductions will have non-linear effects on exposure due, e.g., to interactions between climate and atmospheric chemistry. By using an integrated assessment model, we quantify the effect of changes in climate, emissions and population demography on exposure and health impacts in Europe. The sensitivity to the changes is assessed by investigating the differences between the decades 2000–2009, 2050–2059 and 2080–2089. We focus on the number of premature deaths related to atmospheric ozone, Secondary Inorganic Aerosols and primary PM. For the Nordic region we furthermore include a projection on how population exposure might develop due to changes in building stock with increased energy efficiency. Reductions in emissions cause a large significant decrease in mortality, while climate effects on chemistry and emissions only affects premature mortality by a few percent. Changes in population demography lead to a larger relative increase in chronic mortality than the relative increase in population. Finally, the projected changes in building stock and infiltration rates in the Nordic indicate that this factor may be very important for assessments of population exposure in the future.

Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

Science.gov (United States)

Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

2012-04-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the

Simulating secondary organic aerosol from missing diesel-related intermediate-volatility organic compound emissions during the Clean Air for London (ClearfLo campaign

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R. Ots

2016-05-01

Full Text Available We present high-resolution (5 km  ×  5 km atmospheric chemical transport model (ACTM simulations of the impact of newly estimated traffic-related emissions on secondary organic aerosol (SOA formation over the UK for 2012. Our simulations include additional diesel-related intermediate-volatility organic compound (IVOC emissions derived directly from comprehensive field measurements at an urban background site in London during the 2012 Clean Air for London (ClearfLo campaign. Our IVOC emissions are added proportionally to VOC emissions, as opposed to proportionally to primary organic aerosol (POA as has been done by previous ACTM studies seeking to simulate the effects of these missing emissions. Modelled concentrations are evaluated against hourly and daily measurements of organic aerosol (OA components derived from aerosol mass spectrometer (AMS measurements also made during the ClearfLo campaign at three sites in the London area. According to the model simulations, diesel-related IVOCs can explain on average  ∼  30 % of the annual SOA in and around London. Furthermore, the 90th percentile of modelled daily SOA concentrations for the whole year is 3.8 µg m−3, constituting a notable addition to total particulate matter. More measurements of these precursors (currently not included in official emissions inventories is recommended. During the period of concurrent measurements, SOA concentrations at the Detling rural background location east of London were greater than at the central London location. The model shows that this was caused by an intense pollution plume with a strong gradient of imported SOA passing over the rural location. This demonstrates the value of modelling for supporting the interpretation of measurements taken at different sites or for short durations.

Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

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Gunsch, Matthew J.; May, Nathaniel W.; Wen, Miao; Bottenus, Courtney L. H.; Gardner, Daniel J.; VanReken, Timothy M.; Bertman, Steven B.; Hopke, Philip K.; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5-2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5-2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon-organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

Tar balls are processed, weakly absorbing, primary aerosol particles formed downwind of boreal forest fires

Science.gov (United States)

Sedlacek, A. J., III; Buseck, P. R.; Adachi, K.; Kleinman, L. I.; Onasch, T. B.; Springston, S. R.

2017-12-01

Biomass burning is a major source of light-absorbing black and brown carbonaceous aerosols Brown carbon is a poorly characterized mixture that includes tar balls (TBs), a type of carbonaceous particle unique to biomass burning. Here we describe the first atmospheric observations of the formation and evolution of TBs Aerosol particles were collected on TEM grids during individual aircraft transects at varying downwind distances from the Colockum Tarp wildland fire. The TEM images show primary particles transforming from viscous, impact-deformed particles to spherical TBs. The number fraction of TBs in the wildfire smoke plume increased from less than 5% in samples collected close to the emission source to greater than 40% after 3 hours of aging, with little change in downwind TB diameters. The TB mass fraction increased from 2% near the fire to 23±9% downwind. Single-scatter albedo determined from scattering and absorption measurements increased slightly with downwind distance. Mie calculations show this observation is consistent with weak light absorbance by TBs (m=1.56 - 0.02i) but not consistent with order-of-magnitude stronger absorption observed in different settings. The field-derived TB mass fractions reported here indicate that this particle type should be accounted for in biomass-burn emission inventories.

Diurnal cycling of urban aerosols under different weather regimes

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Gregorič, Asta; Drinovec, Luka; Močnik, Griša; Remškar, Maja; Vaupotič, Janja; Stanič, Samo

2016-04-01

A one month measurement campaign was performed in summer 2014 in Ljubljana, the capital of Slovenia (population 280,000), aiming to study temporal and spatial distribution of urban aerosols and the mixing state of primary and secondary aerosols. Two background locations were chosen for this purpose, the first one in the city center (urban background - KIS) and the second one in the suburban background (Brezovica). Simultaneous measurements of black carbon (BC) and particle number size distribution of submicron aerosols (PM1) were conducted at both locations. In the summer season emission from traffic related sources is expected to be the main local contribution to BC concentration. Concentrations of aerosol species and gaseous pollutants within the planetary boundary layer are controlled by the balance between emission sources of primary aerosols and gases, production of secondary aerosols, chemical reactions of precursor gases under solar radiation and the rate of dilution by mixing within the planetary boundary layer (PBL) as well as with tropospheric air. Only local emission sources contribute to BC concentration during the stable PBL with low mixing layer height, whereas during the time of fully mixed PBL, regionally transported BC and other aerosols can contribute to the surface measurements. The study describes the diurnal behaviour of the submicron aerosol at the urban and suburban background location under different weather regimes. Particles in three size modes - nucleation (humidity, wind speed and direction), diurnal profile differs for sunny, cloudy and rainy days. Nucleation mode particles were found to be subjected to lower daily variation and only slightly influenced by weather, as opposed to Aitken and accumulation mode particles. The highest correlation between BC and particle number concentration is observed during stable atmospheric conditions in the night and morning hours and is attributed to different particle size modes, depending on the

Photochemical production of aerosols from real plant emissions

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Th. F. Mentel

2009-07-01

Full Text Available Emission of biogenic volatile organic compounds (VOC which on oxidation form secondary organic aerosols (SOA can couple the vegetation with the atmosphere and climate. Particle formation from tree emissions was investigated in a new setup: a plant chamber coupled to a reaction chamber for oxidizing the plant emissions and for forming SOA. Emissions from the boreal tree species birch, pine, and spruce were studied. In addition, α-pinene was used as reference compound. Under the employed experimental conditions, OH radicals were essential for inducing new particle formation, although O₃ (≤80 ppb was always present and a fraction of the monoterpenes and the sesquiterpenes reacted with ozone before OH was generated. Formation rates of 3 nm particles were linearly related to the VOC carbon mixing ratios, as were the maximum observed volume and the condensational growth rates. For all trees, the threshold of new particle formation was lower than for α-pinene. It was lowest for birch which emitted the largest fraction of oxygenated VOC (OVOC, suggesting that OVOC may play a role in the nucleation process. Incremental mass yields were ≈5% for pine, spruce and α-pinene, and ≈10% for birch. α-Pinene was a good model compound to describe the yield and the growth of SOA particles from coniferous emissions. The mass fractional yields agreed well with observations for boreal forests. Despite the somewhat enhanced VOC and OH concentrations our results may be up-scaled to eco-system level. Using the mass fractional yields observed for the tree emissions and weighting them with the abundance of the respective trees in boreal forests SOA mass concentration calculations agree within 6% with field observations. For a future VOC increase of 50% we predict a particle mass increase due to SOA of 19% assuming today's mass contribution of pre-existing aerosol and oxidant levels.

Influences of natural emission sources (wildfires and Saharan dust) on the urban organic aerosol in Barcelona (Western Mediterranean Basis) during a PM event.

Science.gov (United States)

van Drooge, Barend L; Lopez, Jordi F; Grimalt, Joan O

2012-11-01

The urban air quality in Barcelona in the Western Mediterranean Basin is characterized by overall high particulate matter (PM) concentrations, due to intensive local anthropogenic emissions and specific meteorological conditions. Moreover, on several days, especially in summer, natural PM sources, such as long-range transported Saharan dust from Northern Africa or wildfires on the Iberian Peninsula and around the Mediterranean Basin, may influence the levels and composition of the organic aerosol. In the second half of July 2009, daily collected PM(10) filter samples in an urban background site in Barcelona were analyzed on organic tracer compounds representing several emission sources. During this period, an important PM peak event was observed. Individual organic compound concentrations increased two to five times during this event. Although highest increase was observed for the organic tracer of biomass burning, the contribution to the organic aerosol was estimated to be around 6 %. Organic tracers that could be related to Saharan dust showed no correlation with the PM and OC levels, while this was the case for those related to fossil fuel combustion from traffic emissions. Moreover, a change in the meteorological conditions gave way to an overall increase of the urban background contamination. Long-range atmospheric transport of organic compounds from primary emissions sources (i.e., wildfires and Saharan dust) has a relatively moderate impact on the organic aerosol in an urban area where the local emissions are dominating.

Multi-Model Simulations of Aerosol and Ozone Radiative Forcing Due to Anthropogenic Emission Changes During the Period 1990-2015

Science.gov (United States)

Myhre, Gunnar; Aas, Wenche; Ribu, Cherian; Collins, William; Faluvegi, Gregory S.; Flanner, Mark; Forster, Piers; Hodnebrog, Oivind; Klimont, Zbigniew; Lund, Marianne T.

2017-01-01

Over the past few decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and air pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing using recently updated emission data for the period 1990-2015, as simulated by seven global atmospheric composition models. The models broadly reproduce large-scale changes in surface aerosol and ozone based on observations (e.g. 1 to 3 percent per year in aerosols over the USA and Europe). The global mean radiative forcing due to ozone and aerosol changes over the 1990-2015 period increased by 0.17 plus or minus 0.08 watts per square meter, with approximately one-third due to ozone. This increase is more strongly positive than that reported in IPCC AR5 (Intergovernmental Panel on Climate Change Fifth Assessment Report). The main reasons for the increased positive radiative forcing of aerosols over this period are the substantial reduction of global mean SO2 emissions, which is stronger in the new emission inventory compared to that used in the IPCC analysis, and higher black carbon emissions.

Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

Science.gov (United States)

Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

2007-12-01

Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

Primary and secondary organic aerosol origin by combined gas-particle phase source apportionment

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M. Crippa

2013-08-01

Full Text Available Secondary organic aerosol (SOA, a prominent fraction of particulate organic mass (OA, remains poorly constrained. Its formation involves several unknown precursors, formation and evolution pathways and multiple natural and anthropogenic sources. Here a combined gas-particle phase source apportionment is applied to wintertime and summertime data collected in the megacity of Paris in order to investigate SOA origin during both seasons. This was possible by combining the information provided by an aerosol mass spectrometer (AMS and a proton transfer reaction mass spectrometer (PTR-MS. A better constrained apportionment of primary OA (POA sources is also achieved using this methodology, making use of gas-phase tracers. These tracers made possible the discrimination between biogenic and continental/anthropogenic sources of SOA. We found that continental SOA was dominant during both seasons (24–50% of total OA, while contributions from photochemistry-driven SOA (9% of total OA and marine emissions (13% of total OA were also observed during summertime. A semi-volatile nighttime component was also identified (up to 18% of total OA during wintertime. This approach was successfully applied here and implemented in a new source apportionment toolkit.

Analysis of aerosol emission and hazard evaluation of electrical discharge machining (EDM) process.

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Jose, Mathew; Sivapirakasam, S P; Surianarayanan, M

2010-01-01

The safety and environmental aspects of a manufacturing process are important due to increased environmental regulations and life quality. In this paper, the concentration of aerosols in the breathing zone of the operator of Electrical Discharge Machining (EDM), a commonly used non traditional manufacturing process is presented. The pattern of aerosol emissions from this process with varying process parameters such as peak current, pulse duration, dielectric flushing pressure and the level of dielectric was evaluated. Further, the HAZOP technique was employed to identify the inherent safety aspects and fire risk of the EDM process under different working conditions. The analysis of aerosol exposure showed that the concentration of aerosol was increased with increase in the peak current, pulse duration and dielectric level and was decreased with increase in the flushing pressure. It was also found that at higher values of peak current (7A) and pulse duration (520 micros), the concentration of aerosols at breathing zone of the operator was above the permissible exposure limit value for respirable particulates (5 mg/m(3)). HAZOP study of the EDM process showed that this process is vulnerable to fire and explosion hazards. A detailed discussion on preventing the fire and explosion hazard is presented in this paper. The emission and risk of fire of the EDM process can be minimized by selecting proper process parameters and employing appropriate control strategy.

Final Report, The Influence of Organic-Aerosol Emissions and Aging on Regional and Global Aerosol Size Distributions and the CCN Number Budget

Energy Technology Data Exchange (ETDEWEB)

Donahue, Neil M. [Carnegie Mellon Univ., Pittsburgh, PA (United States)

2015-12-23

We conducted laboratory experiments and analyzed data on aging of organic aerosol and analysis of field data on volatility and CCN activity. With supplemental ASR funding we participated in the FLAME-IV campaign in Missoula MT in the Fall of 2012, deploying a two-chamber photochemical aging system to enable experimental exploration of photochemical aging of biomass burning emissions. Results from that campaign will lead to numerous publications, including demonstration of photochemical production of Brown Carbon (BrC) from secondary organic aerosol associated with biomass burning emissions as well as extensive characterization of the effect of photochemical aging on the overall concentrations of biomass burning organic aerosol. Excluding publications arising from the FLAME-IV campaign, project research resulted in 8 papers: [11, 5, 3, 10, 12, 4, 8, 7], including on in Nature Geoscience addressing the role of organic compounds in nanoparticle growth [11

High Altitude Emissions of Black Carbon Aerosols: Potential Climate Implications

Science.gov (United States)

Satheesh, S. K.

2017-12-01

Synthesizing a series of ground-based and airborne measurements of aerosols over the Indian region during summer and pre-monsoon seasons have revealed the persistence of elevated absorbing aerosol layers over most of the Indian region; more than 50% of which located above clouds. Subsequent, in situ measurements of black carbon (BC) using high-altitude balloons, showed surprising layers with high concentrations in the middle and upper troposphere even at an altitude of 8 to 10 kms. Simultaneous measurements of the vertical thermal structure have shown localized warming due to BC absorption leading to large reduction in lapse rate and sharp temperature inversion, which in turn increases the atmospheric stability. This aerosol-induced stable layer is conducive for maintaining the black carbon layer longer at that level, leading thereby to further solar absorption and subsequently triggering dry convection. These observations support the `solar escalator' concept through which absorption-warming-convection cycles lead to self-lifting of BC to upper troposphere or even to lower stratosphere under favorable conditions in a matter of a few days. Employing an on-line regional chemistry transport model (WRF-Chem), incorporating aircraft emissions, it is shown that emissions from high-flying aircrafts as the most likely source of these elevated black carbon layers. These in-situ injected particles, produce significant warming of the thin air in those heights and lift these layers to even upper tropospheric/lower stratospheric heights, aided by the strong monsoonal convection occurring over the region, which are known to overshoot the tropical tropopause leading to injection of tropospheric air mass (along with its constituent aerosols) into the stratosphere, especially during monsoon season when the tropical tropopause layer is known to be thinnest. These simulations are further supported by the CALIPSO space-borne LIDAR derived extinction coefficient profiles. Based on

Refined Use of Satellite Aerosol Optical Depth Snapshots to Constrain Biomass Burning Emissions in the GOCART Model

Science.gov (United States)

Petrenko, Mariya; Kahn, Ralph; Chin, Mian; Limbacher, James

2017-10-01

Simulations of biomass burning (BB) emissions in global chemistry and aerosol transport models depend on external inventories, which provide location and strength for BB aerosol sources. Our previous work shows that to first order, satellite snapshots of aerosol optical depth (AOD) near the emitted smoke plume can be used to constrain model-simulated AOD, and effectively, the smoke source strength. We now refine the satellite-snapshot method and investigate where applying simple multiplicative emission adjustment factors alone to the widely used Global Fire Emission Database version 3 emission inventory can achieve regional-scale consistency between Moderate Resolution Imaging Spectroradiometer (MODIS) AOD snapshots and the Goddard Chemistry Aerosol Radiation and Transport model. The model and satellite AOD are compared globally, over a set of BB cases observed by the MODIS instrument during the 2004, and 2006-2008 biomass burning seasons. Regional discrepancies between the model and satellite are diverse around the globe yet quite consistent within most ecosystems. We refine our approach to address physically based limitations of our earlier work (1) by expanding the number of fire cases from 124 to almost 900, (2) by using scaled reanalysis-model simulations to fill missing AOD retrievals in the MODIS observations, (3) by distinguishing the BB components of the total aerosol load from background aerosol in the near-source regions, and (4) by including emissions from fires too small to be identified explicitly in the satellite observations. The small-fire emission adjustment shows the complimentary nature of correcting for source strength and adding geographically distinct missing sources. Our analysis indicates that the method works best for fire cases where the BB fraction of total AOD is high, primarily evergreen or deciduous forests. In heavily polluted or agricultural burning regions, where smoke and background AOD values tend to be comparable, this approach

Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

Data.gov (United States)

U.S. Environmental Protection Agency — The uploaded data consists of the BRACE Na aerosol observations paired with CMAQ model output, the updated model's parameterization of sea salt aerosol emission size...

Inorganic aerosols responses to emission changes in Yangtze River Delta, China.

Science.gov (United States)

Dong, Xinyi; Li, Juan; Fu, Joshua S; Gao, Yang; Huang, Kan; Zhuang, Guoshun

2014-05-15

The new Chinese National Ambient Air Quality standards (CH-NAAQS) published on Feb. 29th, 2012 listed PM2.5 as criteria pollutant for the very first time. In order to probe into PM2.5 pollution over Yangtze River Delta, the integrated MM5/CMAQ modeling system is applied for a full year simulation to examine the PM2.5 concentration and seasonality, and also the inorganic aerosols responses to precursor emission changes. Total PM2.5 concentration over YRD was found to have strong seasonal variation with higher values in winter months (up to 89.9 μg/m(3) in January) and lower values in summer months (down to 28.8 μg/m(3) in July). Inorganic aerosols were found to have substantial contribution to PM2.5 over YRD, ranging from 37.1% in November to 52.8% in May. Nocturnal production of nitrate (NO3(-)) through heterogeneous hydrolysis of N2O5 was found significantly contribute to high NO3(-) concentration throughout the year. In winter, NO3(-) was found to increase under nitrogen oxides (NOx) emission reduction due to higher production of N2O5 from the excessive ozone (O3) introduced by attenuated titration, which further lead to increase of ammonium (NH4(+)) and sulfate (SO4(2-)), while other seasons showed decrease response of NO3(-). Sensitivity responses of NO3(-) under anthropogenic VOC emission reduction was examined and demonstrated that in urban areas over YRD, NO3(-) formation was actually more sensitive to VOC than NOx due to the O3-involved nighttime chemistry of N2O5, while a reduction of NOx emission may have counter-intuitive effect by increasing concentrations of inorganic aerosols. Copyright © 2014 Elsevier B.V. All rights reserved.

Optical, physical and chemical properties of aerosols transported to a coastal site in the western Mediterranean: a focus on primary marine aerosols

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M. Claeys

2017-06-01

Full Text Available As part of the ChArMEx-ADRIMED campaign (summer 2013, ground-based in situ observations were conducted at the Ersa site (northern tip of Corsica; 533 m a.s.l. to characterise the optical, physical and chemical properties of aerosols. During the observation period, a major influence of primary marine aerosols was detected (22–26 June, with a mass concentration reaching up to 6.5 µg m−3 and representing more than 40 % of the total PM10 mass concentration. Its relatively low ratio of chloride to sodium (average of 0.57 indicates a fairly aged sea salt aerosol at Ersa. In this work, an original data set, obtained from online real-time instruments (ATOFMS, PILS-IC has been used to characterise the ageing of primary marine aerosols (PMAs. During this PMA period, the mixing of fresh and aged PMAs was found to originate from both local and regional (Gulf of Lion emissions, according to local wind measurements and FLEXPART back trajectories. Two different aerosol regimes have been identified: a dust outbreak (dust originating from Algeria/Tunisia, and a pollution period with aerosols originating from eastern Europe, which includes anthropogenic and biomass burning sources (BBP. The optical, physical and chemical properties of the observed aerosols, as well as their local shortwave (SW direct radiative effect (DRE in clear-sky conditions, are compared for these three periods in order to assess the importance of the direct radiative impact of PMAs compared to other sources above the western Mediterranean Basin. As expected, AERONET retrievals indicate a relatively low local SW DRF during the PMA period with mean values of −11 ± 4 at the surface and −8 ± 3 W m−2 at the top of the atmosphere (TOA. In comparison, our results indicate that the dust outbreak observed at our site during the campaign, although of moderate intensity (AOD of 0.3–0.4 at 440 nm and column-integrated SSA of 0.90–0.95, induced a local

Primary and Secondary Organic Marine Aerosol and Oceanic Biological Activity: Recent Results and New Perspectives for Future Studies

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Matteo Rinaldi

2010-01-01

Full Text Available One of the most important natural aerosol systems at the global level is marine aerosol that comprises both organic and inorganic components of primary and secondary origin. The present paper reviews some new results on primary and secondary organic marine aerosol, achieved during the EU project MAP (Marine Aerosol Production, comparing them with those reported in the recent literature. Marine aerosol samples collected at the coastal site of Mace Head, Ireland, show a chemical composition trend that is influenced by the oceanic biological activity cycle, in agreement with other observations. Laboratory experiments show that sea-spray aerosol from biologically active sea water can be highly enriched in organics, and the authors highlight the need for further studies on the atmospheric fate of such primary organics. With regard to the secondary fraction of organic aerosol, the average chemical composition and molecular tracer (methanesulfonic-acid, amines distribution could be successfully characterized by adopting a multitechnique analytical approach.

Organic aerosol formation in citronella candle plumes

OpenAIRE

Bothe, Melanie; Donahue, Neil McPherson

2010-01-01

Citronella candles are widely used as insect repellants, especially outdoors in the evening. Because these essential oils are unsaturated, they have a unique potential to form secondary organic aerosol (SOA) via reaction with ozone, which is also commonly elevated on summer evenings when the candles are often in use. We investigated this process, along with primary aerosol emissions, by briefly placing a citronella tealight candle in a smog chamber and then adding ozone to the chamber. In rep...

Aerosol vertical distribution, new particle formation, and jet aircraft particle emissions in the free troposhere and tropopause region; Vertikalverteilung und Neubildungsprozesse des Aerosols und partikelfoermige Flugzeugemissionen in der freien Troposphaere und Tropopausenregion

Energy Technology Data Exchange (ETDEWEB)

Schroeder, F P

2000-07-01

A contribution to the understanding of natural and anthropogenously induced particle formation as well as aerosol physical transformation processes within the free troposphere (FT) is introduced. Documentation and interpretation of empirical data relevant with respect to possible climatologic impact of anthropogenous aerosol emissions into the atmosphere is presented. The first section describes new technique for high spatial resolution measurements of ultrafine aerosol particles by condensation nucleus counters (CNCs), a necessary prerequisite for the observation of natural particle formation and jet aircraft emissions. The second section illustrates vertical distribution and variability ranges of the aerosol in the FT and the tropopause region (TP). Typical microphysical states of the atmospheric aerosol within the Northern Hemisphere are documented by means of systematic measurements during more than 60 flight missions. Simple mathematical parameterizations of the aerosol vertical distribution and aerosol size distributions are developed. Important aerosol sources within the FT are localized and possible aerosol formation processes are discussed. The third section is focussed on jet-engine particle emissions within the FT and TP. A unique inflight experiment for detection of extremely high concentrations (>10{sup 6} cm{sup -3}) of extremely small (donw to <3 nm) aerosols inside the exhaust plumes of several jet aircraft is described. Particle emission indices and emission-controlling parameters are deduced. Most important topic is the impact of fuel sulfur content of kerosine on number, size and chemical composition of jet particle emissions. Generalized results are parameterized in form of lognormal aerosol particle size distributions. (orig.) [German] Ein Beitrag zum Verstaendnis natuerlicher und anthropogen induzierter Aerosolneubildung sowie physikalischer Aerosolumwandlung in der freien Troposphaere wird vorgestellt. Empirisch gewonnenes Datenmaterial wird

Aerosol and monsoon climate interactions over Asia: AEROSOL AND MONSOON CLIMATE INTERACTIONS

Energy Technology Data Exchange (ETDEWEB)

Li, Zhanqing [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Lau, W. K. -M. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Ramanathan, V. [Department of Atmospheric and Climate Sciences, University of California, San Diego California USA; Wu, G. [Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing China; Ding, Y. [National Climate Center, China Meteorological Administration, Beijing China; Manoj, M. G. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Liu, J. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Qian, Y. [Pacific Northwest National Laboratory, Richland Washington USA; Li, J. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Zhou, T. [Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing China; Fan, J. [Pacific Northwest National Laboratory, Richland Washington USA; Rosenfeld, D. [Institute of Earth Sciences, Hebrew University, Jerusalem Israel; Ming, Y. [Geophysical Fluid Dynamic Laboratory, NOAA, Princeton New Jersey USA; Wang, Y. [Jet Propulsion Laboratory, California Institute of Technology, Pasadena California USA; Huang, J. [College of Atmospheric Sciences, Lanzhou University, Lanzhou China; Wang, B. [Department of Atmospheric Sciences, University of Hawaii, Honolulu Hawaii USA; School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing China; Xu, X. [Chinese Academy of Meteorological Sciences, Beijing China; Lee, S. -S. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Cribb, M. [Department of Atmospheric and Oceanic Science and ESSIC, University of Maryland, College Park Maryland USA; Zhang, F. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Yang, X. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Zhao, C. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Takemura, T. [Research Institute for Applied Mechanics, Kyushu University, Fukuoka Japan; Wang, K. [State Key Laboratory of Earth Surface Processes and Resource Ecology and College of Global Change and Earth System Science, Beijing Normal University, Beijing China; Xia, X. [Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing China; Yin, Y. [School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing China; Zhang, H. [National Climate Center, China Meteorological Administration, Beijing China; Guo, J. [Chinese Academy of Meteorological Sciences, Beijing China; Zhai, P. M. [Chinese Academy of Meteorological Sciences, Beijing China; Sugimoto, N. [National Institute for Environmental Studies, Tsukuba Japan; Babu, S. S. [Space Physics Laboratory, Vikram Sarabhai Space Centre, Thiruvananthapuram India; Brasseur, G. P. [Max Planck Institute for Meteorology, Hamburg Germany

2016-11-15

Asian monsoons and aerosols have been studied extensively which are intertwined in influencing the climate of Asia. This paper provides a comprehensive review of ample studies on Asian aerosol, monsoon and their interactions. The region is the primary source of aerosol emissions of varies species, influenced by distinct weather and climatic regimes. On continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulation. The atmospheric thermodynamic state may also be altered by the aerosol serving as cloud condensation nuclei or ice nuclei. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of numerous monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcings of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.

Natural and Anthropogenic Influences on Atmospheric Aerosol Variability

Energy Technology Data Exchange (ETDEWEB)

Asmi, A.

2012-07-01

several drivers for these changes in the number concentrations are likely. The IPCC representative emission pathways prognose radical reductions of anthropogenic emissions in the next decades, especially of sulphur dioxide, that will most likely cause strong reduction in the present-day cooling effect of the atmospheric aerosols. The model simulations of this thesis show that effect will cause strong additional positive forcing on the atmosphere, possibly causing further increase in the near-surface mean temperatures. The effect was further magnified when new particle formation in atmosphere was also considered in the model calculations. Strong reductions in primary aerosol emissions and especially secondary aerosol precursors should be thus considered with caution. (orig.)

Origin of surface and columnar Indian Ocean Experiment (INDOEX) aerosols using source- and region-tagged emissions transport in a general circulation model

Science.gov (United States)

Verma, S.; Venkataraman, C.; Boucher, O.

2008-12-01

We study the relative influence of aerosols emitted from different sectors and geographical regions on aerosol loading in south Asia. Sectors contributing aerosol emissions include biofuel and fossil fuel combustion, open biomass burning, and natural sources. Geographical regions include India (the Indo-Gangetic plain, central India, south India, and northwest India), southeast Asia, east Asia, Africa-west Asia, and the rest of the world. Simulations of the Indian Ocean Experiment (INDOEX), from January to March 1999, are made in the general circulation model of Laboratoire de Météorologie Dynamique (LMD-ZT GCM) with emissions tagged by sector and geographical region. Anthropogenic emissions dominate (54-88%) the predicted aerosol optical depth (AOD) over all the receptor regions. Among the anthropogenic sectors, fossil fuel combustion has the largest overall influence on aerosol loading, primarily sulfate, with emissions from India (50-80%) and rest of the world significantly influencing surface concentrations and AOD. Biofuel combustion has a significant influence on both the surface and columnar black carbon (BC) in particular over the Indian subcontinent and Bay of Bengal with emissions largely from the Indian region (60-80%). Open biomass burning emissions influence organic matter (OM) significantly, and arise largely from Africa-west Asia. The emissions from Africa-west Asia affect the carbonaceous aerosols AOD in all receptor regions, with their largest influence (AOD-BC: 60%; and AOD-OM: 70%) over the Arabian Sea. Among Indian regions, the Indo-Gangetic Plain is the largest contributor to anthropogenic surface mass concentrations and AOD over the Bay of Bengal and India. Dust aerosols are contributed mainly through the long-range transport from Africa-west Asia over the receptor regions. Overall, the model estimates significant intercontinental incursion of aerosol, for example, BC, OM, and dust from Africa-west Asia and sulfate from distant regions (rest

Simultaneous reductions in emissions of black carbon and co-emitted species will weaken the aerosol net cooling effect

Science.gov (United States)

Wang, Z. L.; Zhang, H.; Zhang, X. Y.

2015-04-01

Black carbon (BC), a distinct type of carbonaceous material formed from the incomplete combustion of fossil and biomass based fuels under certain conditions, can interact with solar radiation and clouds through its strong light-absorption ability, thereby warming the Earth's climate system. Some studies have even suggested that global warming could be slowed down in the short term by eliminating BC emission due to its short lifetime. In this study, we estimate the influence of removing some sources of BC and other co-emitted species on the aerosol radiative effect by using an aerosol-climate atmosphere-only model BCC_AGCM2.0.1_CUACE/Aero with prescribed sea surface temperature and sea ice cover, in combination with the aerosol emissions from the Representative Concentration Pathways (RCPs) scenarios. We find that the global annual mean aerosol net cooling effect at the top of the atmosphere (TOA) will be enhanced by 0.12 W m-2 compared with recent past year 2000 levels if the emissions of only BC are reduced to the level projected for 2100 based on the RCP2.6 scenario. This will be beneficial~for the mitigation of global warming. However, both aerosol negative direct and indirect radiative effects are weakened when BC and its co-emitted species (sulfur dioxide and organic carbon) are simultaneously reduced. Relative to year 2000 levels, the global annual mean aerosol net cooling effect at the TOA will be weakened by 1.7-2.0 W m-2 if the emissions of all these aerosols are decreased to the levels projected for 2100 in different ways based on the RCP2.6, RCP4.5, and RCP8.5 scenarios. Because there are no effective ways to remove the BC exclusively without influencing the other co-emitted components, our results therefore indicate that a reduction in BC emission can lead to an unexpected warming on the Earth's climate system in the future.

Variability in the primary emissions and secondary gas and particle formation from vehicles using bioethanol mixtures.

Science.gov (United States)

Gramsch, E; Papapostolou, V; Reyes, F; Vásquez, Y; Castillo, M; Oyola, P; López, G; Cádiz, A; Ferguson, S; Wolfson, M; Lawrence, J; Koutrakis, P

2018-04-01

Bioethanol for use in vehicles is becoming a substantial part of global energy infrastructure because it is renewable and some emissions are reduced. Carbon monoxide (CO) emissions and total hydrocarbons (THC) are reduced, but there is still controversy regarding emissions of nitrogen oxides (NO x ), aldehydes, and ethanol; this may be a concern because all these compounds are precursors of ozone and secondary organic aerosol (SOA). The amount of emissions depends on the ethanol content, but it also may depend on the engine quality and ethanol origin. Thus, a photochemical chamber was used to study secondary gas and aerosol formation from two flex-fueled vehicles using different ethanol blends in gasoline. One vehicle and the fuel used were made in the United States, and the others were made in Brazil. Primary emissions of THC, CO, carbon dioxide (CO 2 ), and nonmethane hydrocarbons (NMHC) from both vehicles decreased as the amount of ethanol in gasoline increased. NO x emissions in the U.S. and Brazilian cars decreased with ethanol content. However, emissions of THC, CO, and NO x from the Brazilian car were markedly higher than those from the U.S. car, showing high variability between vehicle technologies. In the Brazilian car, formation of secondary nitrogen dioxide (NO 2 ) and ozone (O 3 ) was lower for higher ethanol content in the fuel. In the U.S. car, NO 2 and O 3 had a small increase. Secondary particle (particulate matter [PM]) formation in the chamber decreased for both vehicles as the fraction of ethanol in fuel increased, consistent with previous studies. Secondary to primary PM ratios for pure gasoline is 11, also consistent with previous studies. In addition, the time required to form secondary PM is longer for higher ethanol blends. These results indicate that using higher ethanol blends may have a positive impact on air quality. The use of bioethanol can significantly reduce petroleum use and greenhouse gas emissions worldwide. Given the extent of

Uncertainty in Predicting CCN Activity of Aged and Primary Aerosols

Science.gov (United States)

Zhang, Fang; Wang, Yuying; Peng, Jianfei; Ren, Jingye; Collins, Don; Zhang, Renyi; Sun, Yele; Yang, Xin; Li, Zhanqing

2017-11-01

Understanding particle CCN activity in diverse atmospheres is crucial when evaluating aerosol indirect effects. Here aerosols measured at three sites in China were categorized as different types for attributing uncertainties in CCN prediction in terms of a comprehensive data set including size-resolved CCN activity, size-resolved hygroscopic growth factor, and chemical composition. We show that CCN activity for aged aerosols is unexpectedly underestimated 22% at a supersaturation (S) of 0.2% when using κ-Kohler theory with an assumption of an internal mixture with measured bulk composition that has typically resulted in an overestimate of the CCN activity in previous studies. We conclude that the underestimation stems from neglect of the effect of aging/coating on particle hygroscopicity, which is not considered properly in most current models. This effect enhanced the hygroscopicity parameter (κ) by between 11% (polluted conditions) and 30% (clean days), as indicated in diurnal cycles of κ based on measurements by different instruments. In the urban Beijing atmosphere heavily influenced by fresh emissions, the CCN activity was overestimated by 45% at S = 0.2%, likely because of inaccurate assumptions of particle mixing state and because of variability of chemical composition over the particle size range. For both fresh and aged aerosols, CCN prediction exhibits very limited sensitivity to κSOA, implying a critical role of other factors like mixing of aerosol components within and between particles in regulating CCN activity. Our findings could help improving CCN parameterization in climate models.

Characterization of Wildfire-Induced Aerosol Emissions From the Maritime Continent Peatland and Central African Dry Savannah with MISR and CALIPSO Aerosol Products

Science.gov (United States)

Lee, Huikyo; Jeong, Su-Jong; Kalashnikova, Olga; Tosca, Mika; Kim, Sang-Woo; Kug, Jong-Seong

2018-03-01

Aerosol plumes from wildfires affect the Earth's climate system through regulation of the radiative budget and clouds. However, optical properties of aerosols from individual wildfire smoke plumes and their resultant impact on regional climate are highly variable. Therefore, there is a critical need for observations that can constrain the partitioning between different types of aerosols. Here we present the apparent influence of regional ecosystem types on optical properties of wildfire-induced aerosols based on remote sensing observations from two satellite instruments and three ground stations. The independent observations commonly show that the ratio of the absorbing aerosols is significantly lower in smoke plumes from the Maritime Continent than those from Central Africa, so that their impacts on regional climate are different. The observed light-absorbing properties of wildfire-induced aerosols are explained by dominant ecosystem types such as wet peatlands for the Maritime Continent and dry savannah for Central Africa, respectively. These results suggest that the wildfire-aerosol-climate feedback processes largely depend on the terrestrial environments from which the fires originate. These feedbacks also interact with climate under greenhouse warming. Our analysis shows that aerosol optical properties retrieved based on satellite observations are critical in assessing wildfire-induced aerosols forcing in climate models. The optical properties of carbonaceous aerosol mixtures used by state-of-the-art chemistry climate models may overestimate emissions for absorbing aerosols from wildfires over the Maritime Continent.

Aerosol characterization during project POLINAT

Energy Technology Data Exchange (ETDEWEB)

Hagen, D.E.; Hopkins, A.R.; Paladino, J.D.; Whitefield, P.D. [Missouri Univ., Rolla, MO (United States). Cloud and Aerosol Sciences Lab.; Lilenfeld, H.V. [McDonnell Douglas Aerospace-East, St. Louis, MO (United States)

1997-12-31

The objectives of the aerosol/particulate characterization measurements of project POLINAT (POLlution from aircraft emissions In the North ATlantic flight corridor) are: to search for aerosol/particulate signatures of air traffic emissions in the region of the North Atlantic Flight Corridor; to search for the aerosol/particulate component of large scale enhancement (`corridor effects`) of air traffic related species in the North Atlantic region; to determine the effective emission indices for the aerosol/particulate component of engine exhaust in both the near and far field of aircraft exhaust plumes; to measure the dispersion and transformation of the aerosol/particulate component of aircraft emissions as a function of ambient condition; to characterize background levels of aerosol/particulate concentrations in the North Atlantic Region; and to determine effective emission indices for engine exhaust particulates for regimes beyond the jet phase of plume expansion. (author) 10 refs.

Aerosol characterization during project POLINAT

Energy Technology Data Exchange (ETDEWEB)

Hagen, D E; Hopkins, A R; Paladino, J D; Whitefield, P D [Missouri Univ., Rolla, MO (United States). Cloud and Aerosol Sciences Lab.; Lilenfeld, H V [McDonnell Douglas Aerospace-East, St. Louis, MO (United States)

1998-12-31

The objectives of the aerosol/particulate characterization measurements of project POLINAT (POLlution from aircraft emissions In the North ATlantic flight corridor) are: to search for aerosol/particulate signatures of air traffic emissions in the region of the North Atlantic Flight Corridor; to search for the aerosol/particulate component of large scale enhancement (`corridor effects`) of air traffic related species in the North Atlantic region; to determine the effective emission indices for the aerosol/particulate component of engine exhaust in both the near and far field of aircraft exhaust plumes; to measure the dispersion and transformation of the aerosol/particulate component of aircraft emissions as a function of ambient condition; to characterize background levels of aerosol/particulate concentrations in the North Atlantic Region; and to determine effective emission indices for engine exhaust particulates for regimes beyond the jet phase of plume expansion. (author) 10 refs.

Determination of the power of multielement aerosol composition emission from distant industrial sources

International Nuclear Information System (INIS)

Popova, S.A.; Kutsenogij, K.P.; Chankina, O.V.

2008-01-01

The results from the monitoring of the temporal variability of the multielement composition of atmospheric aerosols are presented. They are used to determine the emission power of a series of elements from distant sources.

Mass yields of secondary organic aerosols from the oxidation of α-pinene and real plant emissions

Directory of Open Access Journals (Sweden)

J. N. Smith

2011-02-01

Full Text Available Biogenic volatile organic compounds (VOCs are a significant source of global secondary organic aerosol (SOA; however, quantifying their aerosol forming potential remains a challenge. This study presents smog chamber laboratory work, focusing on SOA formation via oxidation of the emissions of two dominant tree species from boreal forest area, Scots pine (Pinus sylvestris L. and Norway spruce (Picea abies, by hydroxyl radical (OH and ozone (O3. Oxidation of α-pinene was also studied as a reference system. Tetramethylethylene (TME and 2-butanol were added to control OH and O3 levels, thereby allowing SOA formation events to be categorized as resulting from either OH-dominated or O3-initiated chemistry. SOA mass yields from α-pinene are consistent with previous studies while the yields from the real plant emissions are generally lower than that from α-pinene, varying from 1.9% at an aerosol mass loading of 0.69 μg m−3 to 17.7% at 26.0 μg m−3. Mass yields from oxidation of real plant emissions are subject to the interactive effects of the molecular structures of plant emissions and their reaction chemistry with OH and O3, which lead to variations in condensable product volatility. SOA formation can be reproduced with a two-product gas-phase partitioning absorption model in spite of differences in the source of oxidant species and product volatility in the real plant emission experiments. Condensable products from OH-dominated chemistry showed a higher volatility than those from O3-initiated systems during aerosol growth stage. Particulate phase products became less volatile via aging process which continued after input gas-phase oxidants had been completely consumed.

Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

Science.gov (United States)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-12-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation

Formation of secondary inorganic aerosols by power plant emissions exhausted through cooling towers in Saxony.

Science.gov (United States)

Hinneburg, Detlef; Renner, Eberhard; Wolke, Ralf

2009-01-01

The fraction of ambient PM10 that is due to the formation of secondary inorganic particulate sulfate and nitrate from the emissions of two large, brown-coal-fired power stations in Saxony (East Germany) is examined. The power stations are equipped with natural-draft cooling towers. The flue gases are directly piped into the cooling towers, thereby receiving an additionally intensified uplift. The exhausted gas-steam mixture contains the gases CO, CO2, NO, NO2, and SO2, the directly emitted primary particles, and additionally, an excess of 'free' sulfate ions in water solution, which, after the desulfurization steps, remain non-neutralized by cations. The precursor gases NO2 and SO2 are capable of forming nitric and sulfuric acid by several pathways. The acids can be neutralized by ammonia and generate secondary particulate matter by heterogeneous condensation on preexisting particles. The simulations are performed by a nested and multi-scale application of the online-coupled model system LM-MUSCAT. The Local Model (LM; recently renamed as COSMO) of the German Weather Service performs the meteorological processes, while the Multi-scale Atmospheric Transport Model (MUSCAT) includes the transport, the gas phase chemistry, as well as the aerosol chemistry (thermodynamic ammonium-sulfate-nitrate-water system). The highest horizontal resolution in the inner region of Saxony is 0.7 km. One summer and one winter episode, each realizing 5 weeks of the year 2002, are simulated twice, with the cooling tower emissions switched on and off, respectively. This procedure serves to identify the direct and indirect influences of the single plumes on the formation and distribution of the secondary inorganic aerosols. Surface traces of the individual tower plumes can be located and distinguished, especially in the well-mixed boundary layer in daytime. At night, the plumes are decoupled from the surface. In no case does the resulting contribution of the cooling tower emissions to PM10

The effect of South American biomass burning aerosol emissions on the regional climate

Science.gov (United States)

Thornhill, Gillian D.; Ryder, Claire L.; Highwood, Eleanor J.; Shaffrey, Len C.; Johnson, Ben T.

2018-04-01

The impact of biomass burning aerosol (BBA) on the regional climate in South America is assessed using 30-year simulations with a global atmosphere-only configuration of the Met Office Unified Model. We compare two simulations of high and low emissions of biomass burning aerosol based on realistic interannual variability. The aerosol scheme in the model has hygroscopic growth and optical properties for BBA informed by recent observations, including those from the recent South American Biomass Burning Analysis (SAMBBA) intensive aircraft observations made during September 2012. We find that the difference in the September (peak biomass emissions month) BBA optical depth between a simulation with high emissions and a simulation with low emissions corresponds well to the difference in the BBA emissions between the two simulations, with a 71.6 % reduction from high to low emissions for both the BBA emissions and the BB AOD in the region with maximum emissions (defined by a box of extent 5-25° S, 40-70° W, used for calculating mean values given below). The cloud cover at all altitudes in the region of greatest BBA difference is reduced as a result of the semi-direct effect, by heating of the atmosphere by the BBA and changes in the atmospheric stability and surface fluxes. Within the BBA layer the cloud is reduced by burn-off, while the higher cloud changes appear to be responding to stability changes. The boundary layer is reduced in height and stabilized by increased BBA, resulting in reduced deep convection and reduced cloud cover at heights of 9-14 km, above the layer of BBA. Despite the decrease in cloud fraction, September downwelling clear-sky and all-sky shortwave radiation at the surface is reduced for higher emissions by 13.77 ± 0.39 W m-2 (clear-sky) and 7.37 ± 2.29 W m-2 (all-sky), whilst the upwelling shortwave radiation at the top of atmosphere is increased in clear sky by 3.32 ± 0.09 W m-2, but decreased by -1.36±1.67 W m-2 when cloud changes are

Distinguishing the roles of meteorology, emission control measures, regional transport, and co-benefits of reduced aerosol feedbacks in ;APEC Blue;

Science.gov (United States)

Gao, Meng; Liu, Zirui; Wang, Yuesi; Lu, Xiao; Ji, Dongsheng; Wang, Lili; Li, Meng; Wang, Zifa; Zhang, Qiang; Carmichael, Gregory R.

2017-10-01

Air quality are strongly influenced by both emissions and meteorological conditions. During the Asia Pacific Economic Cooperation (APEC) week (November 5-11, 2014), the Chinese government implemented unprecedented strict emission control measures in Beijing and surrounding provinces, and then a phenomenon referred to as ;APEC Blue; (rare blue sky) occurred. It is challenging to quantify the effectiveness of the implemented strict control measures solely based on observations. In this study, we use the WRF-Chem model to distinguish the roles of meteorology, emission control measures, regional transport, and co-benefits of reduced aerosol feedbacks during APEC week. In general, meteorological variables, PM2.5 concentrations and PM2.5 chemical compositions are well reproduced in Beijing. Positive weather conditions (lower temperature, lower relative humidity, higher wind speeds and enhanced boundary layer heights) play important roles in ;APEC Blue;. Applying strict emission control measures in Beijing and five surrounding provinces can only explain an average decrease of 17.7 μg/m3 (-21.8%) decreases in PM2.5 concentrations, roughly more than half of which is caused by emission controls that implemented in the five surrounding provinces (12.5 μg/m3). During the APEC week, non-local emissions contributed to 41.3% to PM2.5 concentrations in Beijing, and the effectiveness of implementing emission control measures hinges on dominant pathways and transport speeds. Besides, we also quantified the contribution of reduced aerosol feedbacks due to strict emission control measures in this study. During daytime, co-benefits of reduced aerosol feedbacks account for about 10.9% of the total decreases in PM2.5 concentrations in urban Beijing. The separation of contributions from aerosol absorption and scattering restates the importance of controlling BC to accelerate the effectiveness of aerosol pollution control.

A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

Directory of Open Access Journals (Sweden)

D. V. Spracklen

2005-01-01

Full Text Available A GLObal Model of Aerosol Processes (GLOMAP has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN>3nm vary between about 250–500 cm-3 in remote marine boundary layer regions and are generally in good agreement with observations. Modelled continental CN concentrations are lower than observed, which may be due to lack of some primary aerosol sources or the neglect of nucleation mechanisms other than binary homogeneous nucleation of sulfuric acid-water particles. Remote marine CN concentrations increase to around 2000–10 000 cm (at standard temperature and pressure in the upper troposphere, which agrees with typical observed vertical profiles. Cloud condensation nuclei (CCN at 0.2% supersaturation vary between about 1000 cm-3 in polluted regions and between 10 and 500 cm-3 in the remote marine boundary layer. New particle formation through sulfuric acid-water binary nucleation occurs predominantly in the upper troposphere, but the model results show that these particles contribute greatly to aerosol concentrations in the marine boundary layer. For this sulfur-sea salt system it is estimated that sea spray emissions account for only ~10% of CCN in the tropical marine boundary layer, but between 20 and 75% in the mid-latitude Southern Ocean. In a run with only natural sulfate and sea salt emissions the global mean surface CN concentration is more than 60% of that from a run with 1985 anthropogenic

Study of radioactive aerosols emissions and establishment of a model in a nuclear medicine environment during the use of a technetium generator

International Nuclear Information System (INIS)

Bombardier, Pierre

2012-01-01

This work deals with the control of radioactive aerosols emissions inside the nuclear medicine facilities. These emissions occur during pulmonary scintigraphy examinations using aerosols marked with 99m Tc. Using a test chamber, we have developed a method permitting to quantify these emissions around the aerosol generator. A method dedicated to emissions measurement coming from the patient during the pulmonary ventilation is also described. The results obtained on one patient are exposed in this thesis. We characterized and modelled the ventilation of a complete nuclear medicine department with a CFD (Computational Fluid Dynamics) software. This permitted us to study the dissemination of the radioactive aerosol and to compare it with measures of ambient air activity. The numerical model of this department was then employed to test containment solutions and to help defining the best location for air contaminations sensors. An original method combining staff position information and the simulation of the dissemination for the aerosol released has been used to confirm the exposure levels for several professional groups and enhance the workplace studies. (author)

Characterization of organic aerosols in Beirut, Lebanon

International Nuclear Information System (INIS)

Waked, Antoine

2012-01-01

The chemical composition of PM2.5 includes both organic and inorganic compounds. Organic compounds, which constitute a significant fraction of the PM2.5 mass, can be emitted directly as primary aerosol from sources such as fossil-fuel combustion, biomass burning, and natural biogenic emissions, or formed in the atmosphere via chemical reactions leading to secondary organic aerosol (SOA) formation. SOA, which account for 20 - 80 % of total organic aerosol, are currently a major source of uncertainty in air quality modeling. The identification and quantification of the chemical composition of the organic fraction of PM2.5 and its source apportionment are of great interest, especially in the Middle East region where data on organic aerosols are currently lacking. Lebanon, a small developing country in the Middle East region located on the eastern shore of the Mediterranean basin represents a good example for characterizing organic aerosols in this region. To address this issue, the air quality in Beirut (the capital city of Lebanon) was investigated with a focus on organic aerosols. First, an air pollutant emission inventory was developed for Lebanon with a spatial resolution of 5 km x 5 km and for Beirut with a spatial resolution of 1 km x 1 km. The results obtained show that the road transport sector is the major contributor to carbon monoxide (CO), nitrogen oxides (NO x ) and non-methane volatile organic compounds (VOC) emissions, whereas fossil fuel-fired power plants and large industrial plants are the major contributors to sulfur dioxide (SO 2 ) and primary particulate matter (PM) emissions. Then, two intensive 15-day measurement campaigns were conducted at a semi-urban site located in a Beirut suburb to characterize air pollutant concentrations. The first measurement campaign took place in July 2011 and the second in February 2012. Measurements included PM2.5, organic carbon (OC) and elemental carbon (EC) mass concentrations as well as a molecular

Nitrous Oxide Emissions from Biofuel Crops and Atmospheric Aerosols: Associations with Air Quality and Regional Climate

Science.gov (United States)

Pillai, Priya Ramachandran

Emissions of greenhouse gases (GHG) and primary release and secondary formation of aerosols alter the earth's radiative balance and therefore have important climatic implications. Savings in carbon dioxide (CO2) emissions accomplished by replacing fossil fuels with biofuels may increase the nitrous oxide (N2O) emissions. Among various atmospheric trace gases, N2O, irrespective of its low atmospheric concentration, is the fourth most important gas in causing the global greenhouse effect. Major processes, those affect the concentration of atmospheric N2O, are soil microbial activities leading to nitrification and denitrification. Therefore, anthropogenic activities such as industrial emissions, and agricultural practices including application of nitrogenous fertilizers, land use changes, biomass combustion all contribute to the atmospheric N2O concentration. The emission rates of N2O related to biofuel production depend on the nitrogen (N) fertilizer uptake efficiency of biofuel crops. However, crops with less N demand, such as switchgrass may have more favorable climate impacts when compared to crops with high N demands, such as corn. Despite its wide environmental tolerance, the regional adaptability of the potential biofuel crop switch grass varies considerably. Therefore, it is important to regionally quantify the GHG emissions and crop yield in response to N-fertilization. A major objective of this study is to quantify soil emissions of N2O from switchgrass and corn fields as a function of N-fertilization. The roles of soil moisture and soil temperature on N2O fluxes were analyzed. These N2O observations may be used to parameterize the biogeochemical models to better understand the impact of different N2O emission scenarios. This study allows for improvements in climate models that focus on understanding the environmental impacts of the climate change mitigation strategy of replacing fossil fuels with biofuels. As a second major objective, the top of the

Estimate of biogenic VOC emissions in Japan and their effects on photochemical formation of ambient ozone and secondary organic aerosol

Science.gov (United States)

Chatani, Satoru; Matsunaga, Sou N.; Nakatsuka, Seiji

2015-11-01

A new gridded database has been developed to estimate the amount of isoprene, monoterpene, and sesquiterpene emitted from all the broadleaf and coniferous trees in Japan with the Model of Emissions of Gases and Aerosols from Nature (MEGAN). This database reflects the vegetation specific to Japan more accurately than existing ones. It estimates much lower isoprene emitted from other vegetation than trees, and higher sesquiterpene emissions mainly emitted from Cryptomeria japonica, which is the most abundant plant type in Japan. Changes in biogenic emissions result in the decrease in ambient ozone and increase in organic aerosol simulated by the air quality simulation over the Tokyo Metropolitan Area in Japan. Although newly estimated biogenic emissions contribute to a better model performance on overestimated ozone and underestimated organic aerosol, they are not a single solution to solve problems associated with the air quality simulation.

Aerosol measurements over Southern Africa using LIDAR, satellite and sun-photometer

CSIR Research Space (South Africa)

Sivakumar, V

2009-08-01

Full Text Available .csir.co.za Dust Sea Salt Giant nuclei Natural Particles Chemical chemical condensables : SOA, H2SO4, HNO3 … nucleation condensation Aerosol Formation and processes Health Aerosols Solar Radiation Clouds Slide 3 © CSIR 2008 www....csir.co.za Emissions from Industries, vechicle and urban Volatile Components SO2, NOx, NH3, VOC Transformation Humidity and deposition of particules Primary Aerosols, BC, OC, Marine Salts, Natural resources 0 - 16 k m U p t o 50 k m 26 – 29...

A study of photochemical againg of ambient air using Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions

Science.gov (United States)

Lee, T.; Son, J.; Kim, J.; Kim, S.; Sung, K.; Park, G.; Link, M.; Park, T.; Kim, K.; Kang, S.; Ban, J.; Kim, D. S.

2016-12-01

Recent research proposed that Secondary Aerosol (SA) is important class of predicting future climate change scenarios, health effect, and a general air quality. However, there has been lack of studies to investigate SA formation all over the world. This study tried to focus on understanding potential secondary aerosol formation and its local impact by the photochemical aging of inorganic and organic aerosols in the ambient air using the Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions. PAM chamber manufactured by Aerodyne make an oxidizing environment that simulates oxidation processes on timescales of 12-15 hrs in the atmosphere. Chemical compositions of ambient aerosol and aerosol that was aged in the PAM chamber were alternately measured every 2-minutes using the High Resolution-Time of Flight-Aerosol Mass Spectrometer (HR-ToF-AMS). HR-ToF-AMS provides non-refractory aerosol mass concentrations including nitrate, sulfate, hydrocarbon-like and oxygenated organic aerosol in real time. This study includes a residence area of mixture of sources, a forest site of dominant source of biogenic VOCs, an underground parking lot of dominant vehicle emission, and laboratory experiment of vehicle emissions under different fuels and speeds using the chassis dynamometer. As a result, it was revealed that gasoline and LPG vehicle relatively made more potential SA than diesel vehicle.

Aerosol numerical modelling at local scale

International Nuclear Information System (INIS)

Albriet, Bastien

2007-01-01

At local scale and in urban areas, an important part of particulate pollution is due to traffic. It contributes largely to the high number concentrations observed. Two aerosol sources are mainly linked to traffic. Primary emission of soot particles and secondary nanoparticle formation by nucleation. The emissions and mechanisms leading to the formation of such bimodal distribution are still badly understood nowadays. In this thesis, we try to provide an answer to this problematic by numerical modelling. The Modal Aerosol Model MAM is used, coupled with two 3D-codes: a CFD (Mercure Saturne) and a CTM (Polair3D). A sensitivity analysis is performed, at the border of a road but also in the first meters of an exhaust plume, to identify the role of each process involved and the sensitivity of different parameters used in the modelling. (author) [fr

Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

Science.gov (United States)

Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

2010-03-01

This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source

Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

Science.gov (United States)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-08-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidative properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosols (SIA = sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosols (OA) indicated that highly oxidized secondary OA (SOA) showed decreases similar to those of SIA during APEC. However, primary OA (POA) from cooking, traffic, and biomass burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging

Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

Science.gov (United States)

Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles,...

Secondary organic aerosol formation from primary aliphatic amines with NO3 radical

Science.gov (United States)

Malloy, Q. G. J.; Qi, Li; Warren, B.; Cocker, D. R., III; Erupe, M. E.; Silva, P. J.

2009-03-01

Primary aliphatic amines are an important class of nitrogen containing compounds emitted from automobiles, waste treatment facilities and agricultural animal operations. A series of experiments conducted at the UC-Riverside/CE-CERT Environmental Chamber is presented in which oxidation of methylamine, ethylamine, propylamine, and butylamine with O3 and NO3 have been investigated. Very little aerosol formation is observed in the presence of O3 only. However, after addition of NO, and by extension NO3, large aerosol mass yields (~44% for butylamine) are seen. Aerosol generated was determined to be organic in nature due to the small fraction of NO and NO2 in the total signal (tested) as detected by an aerosol mass spectrometer (AMS). We propose a reaction mechanism between carbonyl containing species and the parent amine leading to formation of particulate imine products. These findings can have significant impacts on rural communities with elevated nighttime PM loadings, when significant levels of NO3 exist.

Secondary organic aerosol formation from primary aliphatic amines with NO3 radical

Directory of Open Access Journals (Sweden)

P. J. Silva

2009-03-01

Full Text Available Primary aliphatic amines are an important class of nitrogen containing compounds emitted from automobiles, waste treatment facilities and agricultural animal operations. A series of experiments conducted at the UC-Riverside/CE-CERT Environmental Chamber is presented in which oxidation of methylamine, ethylamine, propylamine, and butylamine with O3 and NO3 have been investigated. Very little aerosol formation is observed in the presence of O3 only. However, after addition of NO, and by extension NO3, large aerosol mass yields (~44% for butylamine are seen. Aerosol generated was determined to be organic in nature due to the small fraction of NO and NO2 in the total signal (<1% for all amines tested as detected by an aerosol mass spectrometer (AMS. We propose a reaction mechanism between carbonyl containing species and the parent amine leading to formation of particulate imine products. These findings can have significant impacts on rural communities with elevated nighttime PM loadings, when significant levels of NO3 exist.

Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area

Directory of Open Access Journals (Sweden)

A. P. Tsimpidi

2010-01-01

Full Text Available New primary and secondary organic aerosol modules have been added to PMCAMx, a three dimensional chemical transport model (CTM, for use with the SAPRC99 chemistry mechanism based on recent smog chamber studies. The new modelling framework is based on the volatility basis-set approach: both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. This new framework with the use of the new volatility basis parameters for low-NO_x and high-NO_x conditions tends to predict 4–6 times higher anthropogenic SOA concentrations than those predicted with the older generation of models. The resulting PMCAMx-2008 was applied in Mexico City Metropolitan Area (MCMA for approximately a week during April 2003 during a period of very low regional biomass burning impact. The emission inventory, which uses as a starting point the MCMA 2004 official inventory, is modified and the primary organic aerosol (POA emissions are distributed by volatility based on dilution experiments. The predicted organic aerosol (OA concentrations peak in the center of Mexico City, reaching values above 40 μg m⁻³. The model predictions are compared with the results of the Positive Matrix Factorization (PMF analysis of the Aerosol Mass Spectrometry (AMS observations. The model reproduces both Hydrocarbon-like Organic Aerosol (HOA and Oxygenated Organic Aerosol (OOA concentrations and diurnal profiles. The small OA underprediction during the rush-hour periods and overprediction in the afternoon suggest potential improvements to the description of fresh primary organic emissions and the formation of the oxygenated organic aerosols, respectively, although they may also be due to errors in the simulation of dispersion and vertical mixing. However, the AMS OOA data are not specific enough to prove that the model reproduces the organic aerosol

Historical (1750-2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS)

Science.gov (United States)

Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang; Klimont, Zbigniew; Janssens-Maenhout, Greet; Pitkanen, Tyler; Seibert, Jonathan J.; Vu, Linh; Andres, Robert J.; Bolt, Ryan M.; Bond, Tami C.; Dawidowski, Laura; Kholod, Nazar; Kurokawa, June-ichi; Li, Meng; Liu, Liang; Lu, Zifeng; Moura, Maria Cecilia P.; O'Rourke, Patrick R.; Zhang, Qiang

2018-01-01

We present a new data set of annual historical (1750-2014) anthropogenic chemically reactive gases (CO, CH4, NH3, NOx, SO2, NMVOCs), carbonaceous aerosols (black carbon - BC, and organic carbon - OC), and CO2 developed with the Community Emissions Data System (CEDS). We improve upon existing inventories with a more consistent and reproducible methodology applied to all emission species, updated emission factors, and recent estimates through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estimated using the same activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These estimates are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission estimates, estimating emissions' uncertainty, and publication of the system as open-source software.

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

Directory of Open Access Journals (Sweden)

D. E. Young

2016-05-01

Full Text Available The San Joaquin Valley (SJV in California experiences persistent air-quality problems associated with elevated particulate matter (PM concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ campaign. The average submicron aerosol (PM1 concentration was 31.0 µg m−3 and the total mass was dominated by organic aerosols (OA, 55 %, followed by ammonium nitrate (35 %. High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C, hydrogen-to-carbon (H / C, and nitrogen-to-carbon (N / C ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C  =  0.09 associated with local traffic, cooking OA (COA; 18 % of total OA, O / C  =  0.19 associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C  =  0.33; BBOA2: 20 % of total OA, O / C  =  0.60 most likely

Factors influencing the outdoor concentration of carbonaceous aerosols at urban schools in Brisbane, Australia: Implications for children's exposure

International Nuclear Information System (INIS)

Crilley, L.R.; Ayoko, G.A.; Mazaheri, M.; Morawska, L.

2016-01-01

This comprehensive study aimed to determine the sources and driving factors of organic carbon (OC) and elemental carbon (EC) concentrations in ambient PM 2.5 in urban schools. Sampling was conducted outdoors at 25 schools in the Brisbane Metropolitan Area, Australia. Concentrations of primary and secondary OC were quantified using the EC tracer method, with secondary OC accounting for an average of 60%. Principal component analysis distinguished the contributing sources above the background and identified groups of schools with differing levels of primary and secondary carbonaceous aerosols. Overall, the results showed that vehicle emissions, local weather conditions and secondary organic aerosols (SOA) were the key factors influencing concentrations of carbonaceous component of PM 2.5 at these schools. These results provide insights into children's exposure to vehicle emissions and SOA at such urban schools. - Highlights: • We aimed to find the contributing sources to children's exposure at school. • Measured outdoor organic carbon and elemental carbon at 25 urban schools. • Schools varied in exposure to primary and secondary sources. • Secondary organic carbon the largest component of carbonaceous aerosols. • Vehicle emission levels at schools are primarily dependent on local traffic counts. - Key factors influencing concentrations of carbonaceous component of PM 2.5 at urban schools were found to be vehicle emissions, secondary organic aerosols and local weather conditions.

New aerosol particles formation in the Sao Paulo Metropolitan Area

Science.gov (United States)

Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

2016-04-01

The Sao Paulo Metropolitan Area (SPMA), in the southeast region of Brazil, is considered a megalopolis comprised of Sao Paulo city and more 38 municipalities. The air pollutant emissions in the SPMA are related to the burning of the fuels: etanol, gasohol (gasoline with 25% ethanol) and diesel. According to CETESB (2013), the road vehicles contributed up to about 97, 87, and 80% of CO, VOCs and NOx emissions in 2012, respectively, being most of NOx associated to diesel combustion and most of CO and VOCs from gasohol and ethanol combustion. Studies conducted on ambient air pollution in the SPMA have shown that black carbon (BC) explains 21% of mass concentration of PM2.5 compared with 40% of organic carbon (OC), 20% of sulfates, and 12% of soil dust (Andrade et al., 2012). Most of the observed ambient PM2.5 mass concentration usually originates from precursors gases such as sulphur dioxide (SO2), ammonia (NH3), nitrogen oxides (NOx) and VOCs as well as through the physico-chemical processes such as the oxidation of low volatile hydrocarbons transferring to the condensed phase (McMurry et al., 2004). The Weather Research and Forecasting with Chemistry model (WRF-Chem; Grell et al. 2005), configured with three nested grid cells: 75, 15, and 3 km, is used as photochemical modeling to describe the physico-chemical processes leading to evolution of particles number and mass size distribution from a vehicular emission model developed by the IAG-USP laboratory of Atmospheric Processes and based on statistical information of vehicular activity. The spatial and temporal distributions of emissions in the finest grid cell are based on road density products compiled by the OpenStreetMap project and measurements performed inside tunnels in the SPMA, respectively. WRF-Chem simulation with coupled primary aerosol (dust and sea-salt) and biogenic emission modules and aerosol radiative effects turned on is conducted as the baseline simulation (Case_0) to evaluate the model

Chemical apportionment of aerosol optical properties during the Asia-Pacific Economic Cooperation summit in Beijing, China

Science.gov (United States)

Han, Tingting; Xu, Weiqi; Chen, Chen; Liu, Xingang; Wang, Qingqing; Li, Jie; Zhao, Xiujuan; Du, Wei; Wang, Zifa; Sun, Yele

2015-12-01

We have investigated the chemical and optical properties of aerosol particles during the 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing, China, using the highly time-resolved measurements by a high-resolution aerosol mass spectrometer and a cavity attenuated phase shift extinction monitor. The average (±σ) extinction coefficient (bext) and absorption coefficient (bap) were 186.5 (±184.5) M m-1 and 23.3 (±21.9) M m-1 during APEC, which were decreased by 63% and 56%, respectively, compared to those before APEC primarily due to strict emission controls. The aerosol composition and size distributions showed substantial changes during APEC; as a response, the mass scattering efficiency (MSE) of PM1 was decreased from 4.7 m2 g-1 to 3.5 m2 g-1. Comparatively, the average single-scattering albedo (SSA) remained relatively unchanged, illustrating the synchronous reductions of bext and bap during APEC. MSE and SSA were found to increase as function of the oxidation degree of organic aerosol (OA), indicating a change of aerosol optical properties during the aging processes. The empirical relationships between chemical composition and particle extinction were established using a multiple linear regression model. Our results showed the largest contribution of ammonium nitrate to particle extinction, accounting for 35.1% and 29.3% before and during APEC, respectively. This result highlights the important role of ammonium nitrate in the formation of severe haze pollution during this study period. We also observed very different optical properties of primary and secondary aerosol. Owing to emission controls in Beijing and surrounding regions and also partly the influences of meteorological changes, the average bext of secondary aerosol during APEC was decreased by 71% from 372.3 M m-1 to 108.5 M m-1, whereas that of primary aerosol mainly from cooking, traffic, and biomass burning emissions showed a smaller reduction from 136.7 M m-1 to 71.3 M m-1. As a result

Retrieving global aerosol sources from satellites using inverse modeling

Directory of Open Access Journals (Sweden)

O. Dubovik

2008-01-01

Full Text Available Understanding aerosol effects on global climate requires knowing the global distribution of tropospheric aerosols. By accounting for aerosol sources, transports, and removal processes, chemical transport models simulate the global aerosol distribution using archived meteorological fields. We develop an algorithm for retrieving global aerosol sources from satellite observations of aerosol distribution by inverting the GOCART aerosol transport model.

The inversion is based on a generalized, multi-term least-squares-type fitting, allowing flexible selection and refinement of a priori algorithm constraints. For example, limitations can be placed on retrieved quantity partial derivatives, to constrain global aerosol emission space and time variability in the results. Similarities and differences between commonly used inverse modeling and remote sensing techniques are analyzed. To retain the high space and time resolution of long-period, global observational records, the algorithm is expressed using adjoint operators.

Successful global aerosol emission retrievals at 2°×2.5 resolution were obtained by inverting GOCART aerosol transport model output, assuming constant emissions over the diurnal cycle, and neglecting aerosol compositional differences. In addition, fine and coarse mode aerosol emission sources were inverted separately from MODIS fine and coarse mode aerosol optical thickness data, respectively. These assumptions are justified, based on observational coverage and accuracy limitations, producing valuable aerosol source locations and emission strengths. From two weeks of daily MODIS observations during August 2000, the global placement of fine mode aerosol sources agreed with available independent knowledge, even though the inverse method did not use any a priori information about aerosol sources, and was initialized with a "zero aerosol emission" assumption. Retrieving coarse mode aerosol emissions was less successful

How important is organic aerosol hygroscopicity to aerosol indirect forcing?

International Nuclear Information System (INIS)

Liu Xiaohong; Wang Jian

2010-01-01

Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR community atmospheric model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (represented by a single parameter 'κ' ) of POA and SOA. Our model simulation indicates that in the present-day (PD) condition changing the 'κ' value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S = 0.1% by 40-80% over the POA source regions, while changing the 'κ' value of SOA by ± 50% (from 0.14 to 0.07 and 0.21) changes the CCN concentration within 40%. There are disproportionally larger changes in CCN concentration in the pre-industrial (PI) condition. Due to the stronger impact of organics hygroscopicity on CCN and cloud droplet number concentration at PI condition, global annual mean anthropogenic aerosol indirect forcing (AIF) between PD and PI conditions reduces with the increase of the hygroscopicity of organics. Global annual mean AIF varies by 0.4 W m -2 in the sensitivity runs with the control run of - 1.3 W m -2 , highlighting the need for improved understanding of organics hygroscopicity and its representation in global models.

Aerosol emissions from prescribed fires in the United States: A synthesis of laboratory and aircraft measurements

Science.gov (United States)

A. A. May; G. R. McMeeking; T. Lee; J. W. Taylor; J. S. Craven; I. Burling; A. P. Sullivan; S. Akagi; J. L. Collett; M. Flynn; H. Coe; S. P. Urbanski; J. H. Seinfeld; R. J. Yokelson; S. M. Kreidenweis

2014-01-01

Aerosol emissions from prescribed fires can affect air quality on regional scales. Accurate representation of these emissions in models requires information regarding the amount and composition of the emitted species. We measured a suite of submicron particulate matter species in young plumes emitted from prescribed fires (chaparral and montane ecosystems in California...

Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

Science.gov (United States)

Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

2015-10-06

Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

Applications of particle induced X-ray emission analysis to ambient aerosol studies

International Nuclear Information System (INIS)

Lannefors, H.

1982-01-01

The characteristics of Particle Induced X-ray Emission (PIXE) analysis in conjunction with different ambient aerosol samplers have been studied. Correction factors have been calculated for homogeneous and inhomogeneous rural and urban aerosol samples. The Nuclepore two stage filter sampler provided the most useful combination of the resolution and particle size fractionation in urban, rural and remote environments. The PIXE-analysis technique in combination with different samplers was employed in aerosol composition studies in rural and remote environments. Particular emphasis was laid on studies of aerosol long range transport. Based on air mass trajectory analysis and aerosol composition measurements the foreign contribution in southern Sweden was estimated to be 70 - 80% for S and Pb but only 30 - 50% for V and Ni. The spatial and temporal extension of a long range transport episode was studied using high time resolution continuous filter samplers in a network in southern Sweden. The variation in the concentration levels of sulphur agreed well with changes in the air mass history. Arctic summer elemental concentration levels as measured during the Swedish YMER-80 icebreaker expedition were typically one order of magnitude lower than Arctic winter levels. The combination of chemical information, optical properties and size distribution data supports the hypothesis of long range transport of air pollution into the Arctic especially during the winter. This takes place during the winter season because the Polar front is further south making conditions for long range transport up to the Arctic more favourable. (Auth.)

Large contribution of fossil fuel derived secondary organic carbon to water soluble organic aerosols in winter haze in China

Science.gov (United States)

Zhang, Yan-Lin; El-Haddad, Imad; Huang, Ru-Jin; Ho, Kin-Fai; Cao, Jun-Ji; Han, Yongming; Zotter, Peter; Bozzetti, Carlo; Daellenbach, Kaspar R.; Slowik, Jay G.; Salazar, Gary; Prévôt, André S. H.; Szidat, Sönke

2018-03-01

Water-soluble organic carbon (WSOC) is a large fraction of organic aerosols (OA) globally and has significant impacts on climate and human health. The sources of WSOC remain very uncertain in polluted regions. Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time-of-flight aerosol mass spectrometer measurements. Fossil emissions on average accounted for 32-47 % of WSOC. Secondary organic carbon (SOC) dominated both the non-fossil and fossil derived WSOC, highlighting the importance of secondary formation to WSOC in severe winter haze episodes. Contributions from fossil emissions to SOC were 61 ± 4 and 50 ± 9 % in Shanghai and Beijing, respectively, significantly larger than those in Guangzhou (36 ± 9 %) and Xi'an (26 ± 9 %). The most important primary sources were biomass burning emissions, contributing 17-26 % of WSOC. The remaining primary sources such as coal combustion, cooking and traffic were generally very small but not negligible contributors, as coal combustion contribution could exceed 10 %. Taken together with earlier 14C source apportionment studies in urban, rural, semi-urban and background regions in Asia, Europe and the USA, we demonstrated a dominant contribution of non-fossil emissions (i.e., 75 ± 11 %) to WSOC aerosols in the Northern Hemisphere; however, the fossil fraction is substantially larger in aerosols from East Asia and the eastern Asian pollution outflow, especially during winter, due to increasing coal combustion. Inclusion of our findings can improve a modelling of effects of WSOC aerosols on climate, atmospheric chemistry and public health.

Historical (1750–2014 anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS

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R. M. Hoesly

2018-01-01

Full Text Available We present a new data set of annual historical (1750–2014 anthropogenic chemically reactive gases (CO, CH4, NH3, NOx, SO2, NMVOCs, carbonaceous aerosols (black carbon – BC, and organic carbon – OC, and CO2 developed with the Community Emissions Data System (CEDS. We improve upon existing inventories with a more consistent and reproducible methodology applied to all emission species, updated emission factors, and recent estimates through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estimated using the same activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These estimates are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission estimates, estimating emissions' uncertainty, and publication of the system as open-source software.

Assessment of Bacterial Aerosol in a Preschool, Primary School and High School in Poland

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Ewa Brągoszewska

2018-02-01

Full Text Available The issue of healthy educational buildings is a global concern because children are particularly at risk of lung damage and infection caused by poor indoor air quality (IAQ. This article presents the results of a preliminary study of the concentration and size distribution of bacterial aerosol in three educational buildings: a preschool, primary school, and high school. Sampling was undertaken in the classrooms with an Andersen six-stage impactor (with aerodynamic cut-off diameters of 7.0, 4.7, 3.3, 2.1, 1.1 and 0.65 μm during spring 2016 and 2017, as well as the outside of the buildings. After incubation, bioaerosol particles captured on nutrient media on Petri dishes were quantitatively evaluated and qualitatively identified. The highest average concentration of bacterial aerosol was inside the primary school building (2205 CFU/m3, whereas the lowest average concentration of indoor culturable bacteria was observed in the high school building (391 CFU/m3. Using the obtained data, the exposure dose (ED of the bacterial aerosol was estimated for children attending each educational level. The most frequently occurring species in the sampled bacterial aerosol were Gram-positive cocci in the indoor environment and Gram-positive rod-forming endospores in the outdoor environment.

Global-scale combustion sources of organic aerosols: sensitivity to formation and removal mechanisms

Science.gov (United States)

Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos

2017-06-01

Organic compounds from combustion sources such as biomass burning and fossil fuel use are major contributors to the global atmospheric load of aerosols. We analyzed the sensitivity of model-predicted global-scale organic aerosols (OA) to parameters that control primary emissions, photochemical aging, and the scavenging efficiency of organic vapors. We used a computationally efficient module for the description of OA composition and evolution in the atmosphere (ORACLE) of the global chemistry-climate model EMAC (ECHAM/MESSy Atmospheric Chemistry). A global dataset of aerosol mass spectrometer (AMS) measurements was used to evaluate simulated primary (POA) and secondary (SOA) OA concentrations. Model results are sensitive to the emission rates of intermediate-volatility organic compounds (IVOCs) and POA. Assuming enhanced reactivity of semi-volatile organic compounds (SVOCs) and IVOCs with OH substantially improved the model performance for SOA. The use of a hybrid approach for the parameterization of the aging of IVOCs had a small effect on predicted SOA levels. The model performance improved by assuming that freshly emitted organic compounds are relatively hydrophobic and become increasingly hygroscopic due to oxidation.

Agricultural Fires in the Southeastern U.S. During SEAC4RS: Emissions of Trace Gases and Particles and Evolution of Ozone, Reactive Nitrogen, and Organic Aerosol

Science.gov (United States)

Liu, X.; Zhang, Y.; Huey, L. G.; Yokelson, R. J.; Wang, Y.; Jimenez, J. L.; Campuzano-Jost, P.; Beyersdorf, A. J.; Blake, D. R.; Choi, Y.;

Program GICC, final report (March 2005), inventory of carbonaceous aerosol particles from 1860 to 2100 or which carbonaceous aerosol for a significant climatic regional/global impact?; Programme GICC, RAPPORT DEFINITIF (Mars 2005), inventaire d'emissions d'aerosol carbone de 1860 a 2100 ou quelles emissions d'aerosol carbone pour un impact climatique regional/global significatif?

Energy Technology Data Exchange (ETDEWEB)

Cachier, H.; Guinot, B. [Laboratoire des Sciences du Climat et de l' Environnment, UMR CEA/CNRS 1572 - CEA Saclay, 91 - Gif sur Yvette (France); Criqui, P.; Mima, S. [IEPE, 38 - Grenoble (France); Brignon, J.M. [INERIS, 60 - Verneuil-en-Halatte (France); Penner, J. [Michigan Univ., Ann Arbor, MI (United States); Carmichael, G. [Iowa Univ., Iowa City, IA (United States); Gadi, R. [National Physical Lab., New Delhi (India); Denier Van der Gon, H. [TNO Hollande (Netherlands); Gregoire, J.M. [JRC, Ispra (Italy); Liousse, C.; Michel, C.; Guillaume, B.; Junker, C

2007-07-01

The aim of our program is to determine past, present and future emission inventories of carbonaceous particles from 1860 to 2100 for fossil fuel and biofuel sources. Emission inventories for savannah and forest fires have been developed by using burnt area products given by satellite for Asia and Africa. The strong collaboration with the different groups attending this GICC program has allowed to develop the following results. 1- With the improvement of algorithms and new choices for emission factors, emission inventories for black carbon (BC), primary organic carbon (OCp) and total organic carbon (OCtot) have been constructed for the period 1950 to 1997 for fossil fuel and biofuel sources. With these new development, biofuel sources have been seen to be significant, especially in the developing countries. 2- Past inventories have been developed for fossil fuel and biofuel sources from 1860 to 1997 by taking into account the evolution of fuel consumption, fuel use and emission factors. 3- Savannah and forest fire inventories have been constructed based on burnt area products, for Africa (1981-1991, 2000) and Asia (2000-2001). These results show the importance of using real time data instead of statistics. 4-Future emission inventory of black carbon by fossil fuel sources has been constructed for 2100 following the IPCC scenario A2 (catastrophic case) and B1 (perfect world). 5-Characterization of biofuel emissions has been realized by organizing an experiment in a combustion chamber where indian and chinese biofuels (fuelwood, agricultural wastes, dung-cake etc..). were burnt, reproducing the burning methods used in these countries. 6-Finally, the differences between the existing inventories of carbonaceous aerosols has been explained. (A.L.B.)

Organic aerosol formation in citronella candle plumes.

Science.gov (United States)

Bothe, Melanie; Donahue, Neil McPherson

2010-09-01

Citronella candles are widely used as insect repellants, especially outdoors in the evening. Because these essential oils are unsaturated, they have a unique potential to form secondary organic aerosol (SOA) via reaction with ozone, which is also commonly elevated on summer evenings when the candles are often in use. We investigated this process, along with primary aerosol emissions, by briefly placing a citronella tealight candle in a smog chamber and then adding ozone to the chamber. In repeated experiments, we observed rapid and substantial SOA formation after ozone addition; this process must therefore be considered when assessing the risks and benefits of using citronella candle to repel insects.

Attribution of aerosol radiative forcing over India during the winter monsoon to emissions from source categories and geographical regions

Science.gov (United States)

Verma, S.; Venkataraman, C.; Boucher, O.

2011-08-01

We examine the aerosol radiative effects due to aerosols emitted from different emission sectors (anthropogenic and natural) and originating from different geographical regions within and outside India during the northeast (NE) Indian winter monsoon (January-March). These studies are carried out through aerosol transport simulations in the general circulation (GCM) model of the Laboratoire de Météorologie Dynamique (LMD). The model estimates of aerosol single scattering albedo (SSA) show lower values (0.86-0.92) over the region north to 10°N comprising of the Indian subcontinent, Bay of Bengal, and parts of the Arabian Sea compared to the region south to 10°N where the estimated SSA values lie in the range 0.94-0.98. The model estimated SSA is consistent with the SSA values inferred through measurements on various platforms. Aerosols of anthropogenic origin reduce the incoming solar radiation at the surface by a factor of 10-20 times the reduction due to natural aerosols. At the top-of-atmosphere (TOA), aerosols from biofuel use cause positive forcing compared to the negative forcing from fossil fuel and natural sources in correspondence with the distribution of SSA which is estimated to be the lowest (0.7-0.78) from biofuel combustion emissions. Aerosols originating from India and Africa-west Asia lead to the reduction in surface radiation (-3 to -8 W m -2) by 40-60% of the total reduction in surface radiation due to all aerosols over the Indian subcontinent and adjoining ocean. Aerosols originating from India and Africa-west Asia also lead to positive radiative effects at TOA over the Arabian Sea, central India (CNI), with the highest positive radiative effects over the Bay of Bengal and cause either negative or positive effects over the Indo-Gangetic plain (IGP).

New trajectory-driven aerosol and chemical process model Chemical and Aerosol Lagrangian Model (CALM

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P. Tunved

2010-11-01

Full Text Available A new Chemical and Aerosol Lagrangian Model (CALM has been developed and tested. The model incorporates all central aerosol dynamical processes, from nucleation, condensation, coagulation and deposition to cloud formation and in-cloud processing. The model is tested and evaluated against observations performed at the SMEAR II station located at Hyytiälä (61° 51' N, 24° 17' E over a time period of two years, 2000–2001. The model shows good agreement with measurements throughout most of the year, but fails in reproducing the aerosol properties during the winter season, resulting in poor agreement between model and measurements especially during December–January. Nevertheless, through the rest of the year both trends and magnitude of modal concentrations show good agreement with observation, as do the monthly average size distribution properties. The model is also shown to capture individual nucleation events to a certain degree. This indicates that nucleation largely is controlled by the availability of nucleating material (as prescribed by the [H₂SO₄], availability of condensing material (in this model 15% of primary reactions of monoterpenes (MT are assumed to produce low volatile species and the properties of the size distribution (more specifically, the condensation sink. This is further demonstrated by the fact that the model captures the annual trend in nuclei mode concentration. The model is also used, alongside sensitivity tests, to examine which processes dominate the aerosol size distribution physical properties. It is shown, in agreement with previous studies, that nucleation governs the number concentration during transport from clean areas. It is also shown that primary number emissions almost exclusively govern the CN concentration when air from Central Europe is advected north over Scandinavia. We also show that biogenic emissions have a large influence on the amount of potential CCN observed

Distinct high molecular weight organic compound (HMW-OC) types in aerosol particles collected at a coastal urban site

Science.gov (United States)

Dall'Osto, M.; Healy, R. M.; Wenger, J. C.; O'Dowd, C.; Ovadnevaite, J.; Ceburnis, D.; Harrison, Roy M.; Beddows, D. C. S.

2017-12-01

Organic oligomers were discovered in laboratory-generated atmospheric aerosol over a decade ago. However, evidence for the presence of oligomers in ambient aerosols is scarce and mechanisms for their formation have yet to be fully elucidated. In this work, three unique aerosol particle types internally mixed with High molecular weight organic compounds (HMW-OC) species - likely oligomers - were detected in ambient air using single particle Aerosol Time-Of-Flight Mass Spectrometry (ATOFMS) in Cork (Ireland) during winter 2009. These particle types can be described as follows: (1) HMW-OCs rich in organic nitrogen - possibly containing nitrocatechols and nitroguaiacols - originating from primary emissions of biomass burning particles during evening times; (2) HMW-OCs internally mixed with nitric acid, occurring in stagnant conditions during night time; and (3) HMW-OCs internally mixed with sea salt, likely formed via photochemical reactions during day time. The study exemplifies the power of methodologies capable of monitoring the simultaneous formation of organic and inorganic particle-phase reaction products. Primary emissions and atmospheric aging of different types of HMW-OC contributes to aerosol with a range of acidity, hygroscopic and optical properties, which can have different impacts on climate and health.

Potential of secondary aerosol formation from Chinese gasoline engine exhaust.

Science.gov (United States)

Du, Zhuofei; Hu, Min; Peng, Jianfei; Guo, Song; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Qin, Yanhong; Niu, He; Li, Mengren; Yang, Yudong; Lu, Sihua; Wu, Yusheng; Shao, Min; Shuai, Shijin

2018-04-01

Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds (VOCs). However, little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4-5hr simulation, which was estimated to represent more than 10days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol (SOA) production was 426±85mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China. Copyright © 2017. Published by Elsevier B.V.

Brown carbon aerosols from burning of boreal peatlands: microphysical properties, emission factors, and implications for direct radiative forcing

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R. K. Chakrabarty

2016-03-01

Full Text Available The surface air warming over the Arctic has been almost twice as much as the global average in recent decades. In this region, unprecedented amounts of smoldering peat fires have been identified as a major emission source of climate-warming agents. While much is known about greenhouse gas emissions from these fires, there is a knowledge gap on the nature of particulate emissions and their potential role in atmospheric warming. Here, we show that aerosols emitted from burning of Alaskan and Siberian peatlands are predominantly brown carbon (BrC – a class of visible light-absorbing organic carbon (OC – with a negligible amount of black carbon content. The mean fuel-based emission factors for OC aerosols ranged from 3.8 to 16.6 g kg−1. Their mass absorption efficiencies were in the range of 0.2–0.8 m2 g−1 at 405 nm (violet and dropped sharply to 0.03–0.07 m2 g−1 at 532 nm (green, characterized by a mean Ångström exponent of  ≈  9. Electron microscopy images of the particles revealed their morphologies to be either single sphere or agglomerated “tar balls”. The shortwave top-of-atmosphere aerosol radiative forcing per unit optical depth under clear-sky conditions was estimated as a function of surface albedo. Only over bright surfaces with albedo greater than 0.6, such as snow cover and low-level clouds, the emitted aerosols could result in a net warming (positive forcing of the atmosphere.

Updated African biomass burning emission inventories in the framework of the AMMA-IDAF program, with an evaluation of combustion aerosols

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C. Liousse

2010-10-01

Full Text Available African biomass burning emission inventories for gaseous and particulate species have been constructed at a resolution of 1 km by 1km with daily coverage for the 2000–2007 period. These inventories are higher than the GFED2 inventories, which are currently widely in use. Evaluation specifically focusing on combustion aerosol has been carried out with the ORISAM-TM4 global chemistry transport model which includes a detailed aerosol module. This paper compares modeled results with measurements of surface BC concentrations and scattering coefficients from the AMMA Enhanced Observations period, aerosol optical depths and single scattering albedo from AERONET sunphotometers, LIDAR vertical distributions of extinction coefficients as well as satellite data. Aerosol seasonal and interannual evolutions over the 2004–2007 period observed at regional scale and more specifically at the Djougou (Benin and Banizoumbou (Niger AMMA/IDAF sites are well reproduced by our global model, indicating that our biomass burning emission inventory appears reasonable.

Arctic Aerosols and Sources

DEFF Research Database (Denmark)

Nielsen, Ingeborg Elbæk

2017-01-01

Since the Industrial Revolution, the anthropogenic emission of greenhouse gases has been increasing, leading to a rise in the global temperature. Particularly in the Arctic, climate change is having serious impact where the average temperature has increased almost twice as much as the global during......, ammonium, black carbon, and trace metals. This PhD dissertation studies Arctic aerosols and their sources, with special focus on black carbon, attempting to increase the knowledge about aerosols’ effect on the climate in an Arctic content. The first part of the dissertation examines the diversity...... of aerosol emissions from an important anthropogenic aerosol source: residential wood combustion. The second part, characterizes the chemical and physical composition of aerosols while investigating sources of aerosols in the Arctic. The main instrument used in this research has been the state...

Real time measurements of submicrometer aerosols in Seoul, Korea: Sources, characteristics, and processing of organic aerosols during winter time.

Science.gov (United States)

Kim, H.; Zhang, Q.

2016-12-01

Highly time-resolved chemical characterization of non-refractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter when persistent air quality problems associated with elevated PM concentrations were observed. The average NR-PM1 concentration was 27.5 µg m-3 and the average mass was dominated by organics (44%), followed by nitrate (24%) and sulfate (10%). Five distinct sources of organic aerosol (OA) were identified from positive matrix factorization (PMF) analysis of the AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA), cooking represented by a cooking OA factor (COA), wood combustion represented by a biomass burning OA factor (BBOA), and secondary aerosol formation in the atmosphere that is represented by a semi-volatile oxygenated OA factor (SVOOA) and a low volatile oxygenated OA factor (LVOOA). These factors, on average, contributed 16, 20, 23, 15 and 26% to the total OA mass, respectively, with primary organic aerosol (POA = HOA + COA + BBOA) accounting for 59% of the OA mass. On average, both primary emissions and secondary aerosol formation are important factors affecting air quality in Seoul during winter, contributing approximately equal. However, differences in the fraction of PM source and properties were observed between high and low loading PM period. For example, during stagnant period with low wind speed (WS) (0.99 ± 0.7 m/s) and high RH (71%), high PM loadings (43.6 ± 12.4 µg m-3) with enhanced fractions of nitrate (27%) and SVOOA (8%) were observed, indicating a strong influence from locally generated secondary aerosol. On the other hand, when low PM loadings (12.6 ± 7.1 µg m-3), which were commonly associated with high WS (1.8 ± 1.1 m/s) and low RH (50 %), were observed, the fraction of regional sources, such as sulfate (12%) and LVOOA (21

Inventory of aerosol and sulphur dioxide emissions from India. Part 1 - Fossil fuel combustion

International Nuclear Information System (INIS)

Shekar Reddy, M.; Venkataraman, C.

2002-01-01

A comprehensive, spatially resolved (0.25 o x 0.25 o ) fossil fuel consumption database and emissions inventory was constructed, for India, for the first time. Emissions of sulphur dioxide and aerosol chemical constituents were estimated for 1996-1997 and extrapolated to the Indian Ocean Experiment (INDOEX) study period (1998-1999). District level consumption of coal/lignite, petroleum and natural gas in power plants, industrial, transportation and domestic sectors was 9411 PJ, with major contributions from coal (54%) followed by diesel (18%). Emission factors for various pollutants were derived using India specific fuel characteristics and information on combustion/air pollution control technologies for the power and industrial sectors. Domestic and transportation emission factors, appropriate for Indian source characteristics, were compiled from literature. SO 2 emissions from fossil fuel combustion for 1996-1997 were 4.0Tg SO 2 yr -1 , with 756 large point sources (e.g. utilities, iron and steel, fertilisers, cement, refineries and petrochemicals and non-ferrous metals), accounting for 62%. PM 2.5 emitted was 0.5 and 2.0Tgyr -1 for the 100% and the 50% control scenario, respectively, applied to coal burning in the power and industrial sectors. Coal combustion was the major source of PM 2.5 (92%) primarily consisting of fly ash, accounting for 98% of the 'inorganic fraction' emissions (difference between PM 2.5 and black carbon + organic matter) of 1.6Tgyr -1 . Black carbon emissions were estimated at 0.1Tgyr -1 , with 58% from diesel transport, and organic matter emissions at 0.3Tgyr -1 , with 48% from brick-kilns. Fossil fuel consumption and emissions peaked at the large point industrial sources and 22 cities, with elevated area fluxes in northern and western India. The spatial resolution of this inventory makes it suitable for regional-scale aerosol-climate studies. These results are compared to previous studies and differences discussed. Measurements of

Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls

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E. A. Marais

2016-02-01

Full Text Available Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA, but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (γ for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC4RS and ground-based (SOAS observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx  ≡  NO + NO2 over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2 react significantly with both NO (high-NOx pathway and HO2 (low-NOx pathway, leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA and formaldehyde (a product of isoprene oxidation. Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58 % of isoprene SOA from the low-NOx pathway and glyoxal (28 % from both low- and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation, but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate on aerosol acidity and volume. The US Environmental Protection Agency (EPA projects 2013–2025 decreases in

Aerosols from biomass combustion

Energy Technology Data Exchange (ETDEWEB)

Nussbaumer, T

2001-07-01

This report is the proceedings of a seminar on biomass combustion and aerosol production organised jointly by the International Energy Agency's (IEA) Task 32 on bio energy and the Swiss Federal Office of Energy (SFOE). This collection of 16 papers discusses the production of aerosols and fine particles by the burning of biomass and their effects. Expert knowledge on the environmental impact of aerosols, formation mechanisms, measurement technologies, methods of analysis and measures to be taken to reduce such emissions is presented. The seminar, visited by 50 participants from 11 countries, shows, according to the authors, that the reduction of aerosol emissions resulting from biomass combustion will remain a challenge for the future.

Aerosols from biomass combustion

Energy Technology Data Exchange (ETDEWEB)

Nussbaumer, T.

2001-07-01

This report is the proceedings of a seminar on biomass combustion and aerosol production organised jointly by the International Energy Agency's (IEA) Task 32 on bio energy and the Swiss Federal Office of Energy (SFOE). This collection of 16 papers discusses the production of aerosols and fine particles by the burning of biomass and their effects. Expert knowledge on the environmental impact of aerosols, formation mechanisms, measurement technologies, methods of analysis and measures to be taken to reduce such emissions is presented. The seminar, visited by 50 participants from 11 countries, shows, according to the authors, that the reduction of aerosol emissions resulting from biomass combustion will remain a challenge for the future.

Physical and chemical characterization of residential oil boiler emissions.

Science.gov (United States)

Hays, Michael D; Beck, Lee; Barfield, Pamela; Lavrich, Richard J; Dong, Yuanji; Vander Wal, Randy L

2008-04-01

The toxicity of emissions from the combustion of home heating oil coupled with the regional proximity and seasonal use of residential oil boilers (ROB) is an important public health concern. Yet scant physical and chemical information about the emissions from this source is available for climate and air quality modeling and for improving our understanding of aerosol-related human health effects. The gas- and particle-phase emissions from an active ROB firing distillate fuel oil (commonly known as diesel fuel) were evaluated to address this deficiency. Ion chromatography of impactor samples showed that the ultrafine ROB aerosol emissions were approximately 45% (w/w) sulfate. Gas chromatography-mass spectrometry detected various n-alkanes at trace levels, sometimes in accumulation mode particles, and out of phase with the size distributions of aerosol mass and sulfate. The carbonaceous matter in the ROB aerosol was primarily light-adsorbing elemental carbon. Gas chromatography-atomic emission spectroscopy measured a previously unrecognized organosulfur compound group in the ROB aerosol emissions. High-resolution transmission electron microscopy of ROB soot indicated the presence of a highly ordered primary particle nanostructure embedded in larger aggregates. Organic gas emissions were measured using EPA Methods TO-15 and TO-11A. The ROB emitted volatile oxygenates (8 mg/(kg of oil burned)) and olefins (5 mg/(kg of oil burned)) mostly unrelated to the base fuel composition. In the final analysis, the ROB tested was a source of numerous hazardous air pollutants as defined in the Clean Air Act Amendments. Approximations conducted using emissions data from the ROB tests show relatively low contributions to a regional-level anthropogenic emissions inventory for volitile organic compounds, PM2.5, and SO2 mass.

Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

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C. J. Hennigan

2011-08-01

Full Text Available Smog chamber experiments were conducted to investigate the chemical and physical transformations of organic aerosol (OA during photo-oxidation of open biomass burning emissions. The experiments were carried out at the US Forest Service Fire Science Laboratory as part of the third Fire Lab at Missoula Experiment (FLAME III. We investigated emissions from 12 different fuels commonly burned in North American wildfires. The experiments feature atmospheric and plume aerosol and oxidant concentrations; aging times ranged from 3 to 4.5 h. OA production, expressed as a mass enhancement ratio (ratio of OA to primary OA (POA mass, was highly variable. OA mass enhancement ratios ranged from 2.9 in experiments where secondary OA (SOA production nearly tripled the POA concentration to 0.7 in experiments where photo-oxidation resulted in a 30 % loss of the OA mass. The campaign-average OA mass enhancement ratio was 1.7 ± 0.7 (mean ± 1σ; therefore, on average, there was substantial SOA production. In every experiment, the OA was chemically transformed. Even in experiments with net loss of OA mass, the OA became increasingly oxygenated and less volatile with aging, indicating that photo-oxidation transformed the POA emissions. Levoglucosan concentrations were also substantially reduced with photo-oxidation. The transformations of POA were extensive; using levoglucosan as a tracer for POA, unreacted POA only contributed 17 % of the campaign-average OA mass after 3.5 h of exposure to typical atmospheric hydroxyl radical (OH levels. Heterogeneous reactions with OH could account for less than half of this transformation, implying that the coupled gas-particle partitioning and reaction of semi-volatile vapors is an important and potentially dominant mechanism for POA processing. Overall, the results illustrate that biomass burning emissions are subject to extensive chemical processing in the atmosphere, and the timescale for these transformations is rapid.

Atmospheric aerosols in Rome, Italy: sources, dynamics and spatial variations during two seasons

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C. Struckmeier

2016-12-01

Full Text Available Investigations on atmospheric aerosols and their sources were carried out in October/November 2013 and May/June 2014 consecutively in a suburban area of Rome (Tor Vergata and in central Rome (near St Peter's Basilica. During both years a Saharan dust advection event temporarily increased PM10 concentrations at ground level by about 12–17 µg m−3. Generally, in October/November the ambient aerosol was more strongly influenced by primary emissions, whereas higher relative contributions of secondary particles (sulfate, aged organic aerosol were found in May/June. Absolute concentrations of anthropogenic emission tracers (e.g. NOx, CO2, particulate polycyclic aromatic hydrocarbons, traffic-related organic aerosol were generally higher at the urban location. Positive matrix factorization was applied to the PM1 organic aerosol (OA fraction of aerosol mass spectrometer (HR-ToF-AMS data to identify different sources of primary OA (POA: traffic, cooking, biomass burning and (local cigarette smoking. While biomass burning OA was only found at the suburban site, where it accounted for the major fraction of POA (18–24 % of total OA, traffic and cooking were more dominant sources at the urban site. A particle type associated with cigarette smoke emissions, which is associated with a potential characteristic marker peak (m∕z 84, C5H10N+, a nicotine fragment in the mass spectrum, was only found in central Rome, where it was emitted in close vicinity to the measurement location. Regarding secondary OA, in October/November, only a very aged, regionally advected oxygenated OA was found, which contributed 42–53 % to the total OA. In May/June total oxygenated OA accounted for 56–76 % of the OA. Here a fraction (18–26 % of total OA of a fresher, less oxygenated OA of more local origin was also observed. New particle formation events were identified from measured particle number concentrations and size distributions in May/June 2014 at

Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis

Directory of Open Access Journals (Sweden)

K. Tsigaridis

2003-01-01

Full Text Available A global 3-dimensional chemistry/transport model able to describe O3, NOx, Volatile Organic Compounds (VOC, sulphur and NH3 chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere focusing on Secondary Organic Aerosol (SOA formation. A number of global simulations have been performed to determine a possible range of annual global SOA production and investigate uncertainties associated with the model results. The studied uncertainties in the SOA budget have been evaluated to be in decreasing importance: the potentially irreversible sticking of the semi-volatile compounds on aerosols, the enthalpy of vaporization of these compounds, the partitioning of SOA on non-carbonaceous aerosols, the conversion of aerosols from hydrophobic to hydrophilic, the emissions of primary carbonaceous aerosols, the chemical fate of the first generation products and finally the activity coefficient of the condensable species. The large uncertainties associated with the emissions of VOC and the adopted simplification of chemistry have not been investigated in this study. Although not all sources of uncertainties have been investigated, according to our calculations, the above factors within the experimental range of variations could result to an overall uncertainty of about a factor of 20 in the global SOA budget. The global annual SOA production from biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or sea-salt, together with the partitioning and the dissociation of the semi-volatile products in aerosol water has been neglected. Comparison of model results to observations, where available, shows a better agreement for the upper budget estimates than for the

Modeling and Evaluation of the Global Sea-Salt Aerosol Distribution: Sensitivity to Emission Schemes and Resolution Effects at Coastal/Orographic Sites

Science.gov (United States)

Spada, M.; Jorba, O.; Perez Garcia-Pando, C.; Janjic, Z.; Baldasano, J. M.

2013-01-01

One of the major sources of uncertainty in model estimates of the global sea-salt aerosol distribution is the emission parameterization. We evaluate a new sea-salt aerosol life cycle module coupled to the online multi-scale chemical transport model NMMB/BSC-CTM. We compare 5 year global simulations using five state-of-the-art sea-salt open-ocean emission schemes with monthly averaged coarse aerosol optical depth (AOD) from selected AERONET sun photometers, surface concentration measurements from the University of Miami's Ocean Aerosol Network, and measurements from two NOAA/PMEL cruises (AEROINDOEX and ACE1). Model results are highly sensitive to the introduction of sea-surface-temperature (SST)-dependent emissions and to the accounting of spume particles production. Emission ranges from 3888 teragrams per year to 8114 teragrams per year, lifetime varies between 7.3 hours and 11.3 hours, and the average column mass load is between 5.0 teragrams and 7.2 teragrams. Coarse AOD is reproduced with an overall correlation of around 0.5 and with normalized biases ranging from +8.8 percent to +38.8 percent. Surface concentration is simulated with normalized biases ranging from minus 9.5 percent to plus 28 percent and the overall correlation is around 0.5. Our results indicate that SST-dependent emission schemes improve the overall model performance in reproducing surface concentrations. On the other hand, they lead to an overestimation of the coarse AOD at tropical latitudes, although it may be affected by uncertainties in the comparison due to the use of all-sky model AOD, the treatment of water uptake, deposition and optical properties in the model and/or an inaccurate size distribution at emission.

TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

Energy Technology Data Exchange (ETDEWEB)

Annette Rohr

2005-03-31

to oxidized emissions were performed. Stage I toxicological assessments were carried out in Sprague-Dawley rats. Biological endpoints included breathing pattern/pulmonary function; in vivo chemiluminescence (an indicator of oxidative stress); blood cytology; bronchoalveolar lavage (BAL) fluid analysis; and histopathology. No significant differences between exposed animals and sham animals (exposed to filtered air) were observed for any of the endpoints; histopathological results are pending and will be reported in the next semiannual report. The scenarios evaluated during this reporting period were slightly modified from those originally proposed. We substituted a new scenario, secondary aerosol + SOA, to investigate the effects of a strongly acidic aerosol with a biogenic component. Since we did not observe any biological response to this scenario, the neutralized secondary aerosol scenario (i.e., oxidized emissions + ammonia) was deemed unnecessary. Moreover, in light of the lack of response observed in the Stage I assessment, it was decided that a Stage II assessment (evaluation of cardiac function in a compromised rat model) was unlikely to provide useful information. However, this model will be employed at Plant 1 and/or 2. During this reporting period, significant progress was made in planning for fieldwork at Plant 1. Stack sampling was carried out at the plant in mid-December to determine the concentration of primary particles. It was found that PM{sub 2.5} mass concentrations were approximately three times higher than those observed at Plant 0. In mid-February, installation and setup for the mobile laboratories began. Animal exposures are scheduled to begin at this plant on March 21, 2005. During the next reporting period, we will initiate fieldwork at Plant 1. At either or both Plants 1 and 2, a detailed Stage II assessment will be performed, even if no significant findings are observed in Stage I. The next semiannual report is expected to include a

A GCM study of organic matter in marine aerosol and its potential contribution to cloud drop activation

Directory of Open Access Journals (Sweden)

G. J. Roelofs

2008-02-01

Full Text Available With the global aerosol-climate model ECHAM5-HAM we investigate the potential influence of organic aerosol originating from the ocean on aerosol mass and chemical composition and the droplet concentration and size of marine clouds. We present sensitivity simulations in which the uptake of organic matter in the marine aerosol is prescribed for each aerosol mode with varying organic mass and mixing state, and with a geographical distribution and seasonality similar to the oceanic emission of dimethyl sulfide. Measurements of aerosol mass, aerosol chemical composition and cloud drop effective radius are used to assess the representativity of the model initializations. Good agreement with the measurements is obtained when organic matter is added to the Aitken, accumulation and coarse modes simultaneously. Representing marine organics in the model leads to higher cloud drop number concentrations and thus smaller cloud drop effective radii, and this improves the agreement with measurements. The mixing state of the organics and the other aerosol matter, i.e. internal or external depending on the formation process of aerosol organics, is an important factor for this. We estimate that globally about 75 Tg C yr⁻¹ of organic matter from marine origin enters the aerosol phase, with comparable contributions from primary emissions and secondary organic aerosol formation.

Contribution of Seawater Surfactants to Generated Primary Marine Aerosol Particles

Science.gov (United States)

Frossard, A. A.; Gerard, V.; Duplessis, P.; Kinsey, J. D.; Lu, X.; Zhu, Y.; Bisgrove, J.; Maben, J. R.; Long, M. S.; Chang, R.; Beaupre, S. R.; Kieber, D. J.; Keene, W. C.; Noziere, B.; Cohen, R. C.

2017-12-01

Surfactants account for minor fractions of total organic carbon in the ocean but may have major impacts on the surface tension of bursting bubbles at the sea surface that drive the production of primary marine aerosol particles (PMA). Surfactants associated with marine aerosol may also significantly reduce the surface tension of water thereby increasing the potential for cloud droplet activation and growth. During September and October 2016, PMA were produced from bursting bubbles in seawater using a high capacity generator at two biologically productive and two oligotrophic stations in the western North Atlantic, as part of a cruise on the R/V Endeavor. Surfactants were extracted from paired PMA and seawater samples, and their ionic compositions, total concentrations, and critical micelle concentrations (CMC) were quantified and compared for the four hydrographic stations. Higher surfactant concentrations were determined in the aerosol produced from biologically productive seawater compared to oligotrophic seawater, and the surfactants extracted from productive seawater were stronger (had lower CMCs) than those in the oligotrophic seawater. Surfactants associated with PMA and seawater in productive regions also varied over diel cycles, whereas those in the oligotrophic regions did not. This work demonstrates a direct link between surfactants in seawater and those in PMA.

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

Science.gov (United States)

Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

2017-01-01

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

Enhanced marine sulphur emissions offset global warming and impact rainfall.

Science.gov (United States)

Grandey, B S; Wang, C

2015-08-21

Artificial fertilisation of the ocean has been proposed as a possible geoengineering method for removing carbon dioxide from the atmosphere. The associated increase in marine primary productivity may lead to an increase in emissions of dimethyl sulphide (DMS), the primary source of sulphate aerosol over remote ocean regions, potentially causing direct and cloud-related indirect aerosol effects on climate. This pathway from ocean fertilisation to aerosol induced cooling of the climate may provide a basis for solar radiation management (SRM) geoengineering. In this study, we investigate the transient climate impacts of two emissions scenarios: an RCP4.5 (Representative Concentration Pathway 4.5) control; and an idealised scenario, based on RCP4.5, in which DMS emissions are substantially enhanced over ocean areas. We use mini-ensembles of a coupled atmosphere-ocean configuration of CESM1(CAM5) (Community Earth System Model version 1, with the Community Atmosphere Model version 5). We find that the cooling effect associated with enhanced DMS emissions beneficially offsets greenhouse gas induced warming across most of the world. However, the rainfall response may adversely affect water resources, potentially impacting human livelihoods. These results demonstrate that changes in marine phytoplankton activity may lead to a mixture of positive and negative impacts on the climate.

Emissions of Black Carbon, Organic, and Inorganic Aerosols From Biomass Burning in North America and Asia in 2008

Science.gov (United States)

Kondo, Y.; Matsui, H.; Moteki, N.; Sahu, L.; Takegawa, N.; Kajino, M.; Zhao, Y.; Cubison, M. J.; Jimenez, J. L.; Vay, S.;

Monsoon sensitivity to aerosol direct radiative forcing in the ...

Indian Academy of Sciences (India)

to the total, scattering aerosols and black carbon aerosols. ... acts as an internal damping mechanism spinning down the regional hydrological cycle and leading to sig- ... tion and emission of longwave radiation. ... effect of aerosols over India, where the emission of .... that aerosol effects on monsoon water cycle dynam-.

Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols. Part 1; Aerosol Trends and Radiative Forcing

Science.gov (United States)

Leibensperger, E. M.; Mickley, L. J.; Jacob, D. J.; Chen, W.-T.; Seinfeld, J. H.; Nenes, A.; Adams, P. J.; Streets, D. G.; Kumar, N.; Rind, D.

2012-01-01

We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950-2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980-2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970-1990, with values over the eastern US (east of 100 deg W) of -2.0Wm(exp-2 for direct forcing including contributions from sulfate (-2.0Wm-2), nitrate (-0.2Wm(exp-2), organic carbon (-0.2Wm(exp-2), and black carbon (+0.4Wm(exp-2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50 %. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8Wm(exp-2) direct and 1.0Wm(exp-2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3Wm(exp-2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.

Modelling African aerosol using updated fossil fuel and biofuel emission inventories for 2005 and 2030

Science.gov (United States)

Liousse, C.; Penner, J. E.; Assamoi, E.; Xu, L.; Criqui, P.; Mima, S.; Guillaume, B.; Rosset, R.

2010-12-01

A regional fossil fuel and biofuel emission inventory for particulates has been developed for Africa at a resolution of 0.25° x 0.25° for the year 2005. The original database of Junker and Liousse (2008) was used after modification for updated regional fuel consumption and emission factors. Consumption data were corrected after direct inquiries conducted in Africa, including a new emitter category (i.e. two-wheel vehicles including “zemidjans”) and a new activity sector (i.e. power plants) since both were not considered in the previous emission inventory. Emission factors were measured during the 2005 AMMA campaign (Assamoi and Liousse, 2010) and combustion chamber experiments. Two prospective inventories for 2030 are derived based on this new regional inventory and two energy consumption forecasts by the Prospective Outlook on Long-term Energy Systems (POLES) model (Criqui, 2001). The first is a reference scenario, where no emission controls beyond those achieved in 2003 are taken into account, and the second is for a "clean" scenario where possible and planned policies for emission control are assumed to be effective. BC and OCp emission budgets for these new inventories will be discussed and compared to the previous global dataset. These new inventories along with the most recent open biomass burning inventory (Liousse et al., 2010) have been tested in the ORISAM-TM5 global chemistry-climate model with a focus over Africa at a 1° x 1° resolution. Global simulations for BC and primary OC for the years 2005 and 2030 are carried out and the modelled particulate concentrations for 2005 are compared to available measurements in Africa. Finally, BC and OC radiative properties (aerosol optical depths and single scattering albedo) are calculated and the direct radiative forcing is estimated using an off line model (Wang and Penner, 2009). Results of sensitivity tests driven with different emission scenarios will be presented.

Study of emission episodes of urban aerosol by ion beam analytical techniques

International Nuclear Information System (INIS)

Angyal, A.; Kertesz, Zs.; Szikszai, Z.; Szoboszlai, Z.; Furu, E.; Csedreki, L.; Daroczi, L.

2010-01-01

Complete text of publication follows. Aerosol pollution has impact on the climate and on human health. Thus investigation of atmospheric aerosol is important in urban environment such as Debrecen. One of the main goals of our study was to define the sources of the particles. The hourly evolution of atmospheric aerosol concentration was used to identify sources of fine (aerodynamic diameter < 2,5 μm) and coarse (10 μm ≥ aerodynamic diameter ≥ 2.5 μm) urban particulate matter in Debrecen. In both size fractions sources were found which were characterized by high heavy metal content. In this study we provide accurate information of the sources of coarse mode heavy metals by using nuclear and scanning electron microscopy. Single particle analysis of chosen samples was carried out on the ATOMKI Scanning Nuclear Microprobe Facility. Elemental composition for Z ≥ 6, morphology and size of around 500 coarse mode particles were determined by Scanning Transmission Ion Microscopy, light-element PIXE and PIXE analytical methods. Furthermore Scanning Electron Microscopy (SEM) was used to investigate particles morphology. The main components of the particles were Na, K, Ca, S, P and Fe with traces of Ti, V, Cr, Mn, Ni, Cu, Zn, Co, Pb. S-rich particles were enriched in one or more of the following elements: Na, Ca, K, Fe, Zn. Trace metals (Mn, Cu, Zn, Cr) occurred together Fe supposedly originated from industrial emission or traffic. P appeared in the Ca-rich particles. Particles with high concentration of Ni were rich in V, Fe and S. Thus this source was identified as residual combustion. V-rich particles occurred together with Fe, Mn and Cr. Their possible source was industry. Pb was attached to Ca, Fe, S containing particles. As result of the SEM study the following particle types (Figure 1.) were identified: semitransparent material (S-K-rich, S-Zn-rich, PCa-rich), spherical (FeO, Fe-Ni-Cr-V-rich), cubic (KCl, CaCl) and crystalline (S-Ca-rich). The main sources of

Temperature and burning history affect emissions of greenhouse gases and aerosol particles from tropical peatland fire

Science.gov (United States)

Kuwata, Mikinori; Kai, Fuu Ming; Yang, Liudongqing; Itoh, Masayuki; Gunawan, Haris; Harvey, Charles F.

2017-01-01

Tropical peatland burning in Asia has been intensifying over the last decades, emitting huge amounts of gas species and aerosol particles. Both laboratory and field studies have been conducted to investigate emission from peat burning, yet a significant variability in data still exists. We conducted a series of experiments to characterize the gas and particulate matter emitted during burning of a peat sample from Sumatra in Indonesia. Heating temperature of peat was found to regulate the ratio of CH4 to CO2 in emissions (ΔCH4/ΔCO2) as well as the chemical composition of particulate matter. The ΔCH4/ΔCO2 ratio was larger for higher temperatures, meaning that CH4 emission is more pronounced at these conditions. Mass spectrometric analysis of organic components indicated that aerosol particles emitted at higher temperatures had more unsaturated bonds and ring structures than that emitted from cooler fires. The result was consistently confirmed by nuclear magnetic resonance analysis. In addition, CH4 emitted by burning charcoal, which is derived from previously burned peat, was lower by at least an order of magnitude than that from fresh peat. These results highlight the importance of both fire history and heating temperature for the composition of tropical peat-fire emissions. They suggest that remote sensing technologies that map fire histories and temperatures could provide improved estimates of emissions.

Impact of primary and secondary air supply intensity in stove on emissions of size-segregated particulate matter and carbonaceous aerosols from apple tree wood burning

Science.gov (United States)

Sun, Jian; Shen, Zhenxing; Zhang, Leiming; Zhang, Qian; Lei, Yali; Cao, Junji; Huang, Yu; Liu, Suixin; Zheng, Chunli; Xu, Hongmei; Liu, Hongxia; Pan, Hua; Liu, Pingping; Zhang, Renjian

2018-04-01

In order to assess emission factors (EF) more accurately from household biomass burning, a series of laboratory-controlled apple tree wood burning tests were conducted to measure the EFs of size-segregated particulate matter (PM) and carbonaceous aerosols. The controlled burning experiments were conducted with designed primary air (PA) and secondary air (SA) supply intensity. An optimum value of 7 m3·h- 1 was found for SA, resulting the highest modified combustion efficiency (92.4 ± 2.5%) as well as the lowest EFs of PM2.5 (0.13 ± 0.01 g·MJ- 1), OC (0.04 ± 0.03 g·MJ- 1) and EC (0.03 ± 0.01 g·MJ- 1). SA values of 7 and 10 m3·h- 1 resulted the lowest EFs for all the different PM sizes. In a test with PA of 6 m3·h- 1 and SA of 7 m3·h- 1, very low EFs were observed for OC1 (8.2%), OC2 (11.2%) and especially OP (Pyrolyzed OC) (0%, not detected), indicating nearly complete combustion under this air supply condition. Besides SA, higher PA was proved to have positive effects on PM and carbonaceous fraction emission reduction. For example, with a fixed SA of 1.5 m3·h- 1, EFs of PM2.5 decreased from 0.64 to 0.27 g·MJ- 1 when PA increased from 6 to 15 m3·h- 1 (P < 0.05). Similar reductions were also observed in EFs of OC, EC and size segregated PM.

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

Science.gov (United States)

Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray

TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

Energy Technology Data Exchange (ETDEWEB)

Annette Rohr

2004-12-02

This report documents progress made on the subject project during the period of March 1, 2004 through August 31, 2004. The TERESA Study is designed to investigate the role played by specific emissions sources and components in the induction of adverse health effects by examining the relative toxicity of coal combustion and mobile source (gasoline and/or diesel engine) emissions and their oxidative products. The study involves on-site sampling, dilution, and aging of coal combustion emissions at three coal-fired power plants, as well as mobile source emissions, followed by animal exposures incorporating a number of toxicological endpoints. The DOE-EPRI Cooperative Agreement (henceforth referred to as ''the Agreement'') for which this technical progress report has been prepared covers the analysis and interpretation of the field data collected at the first power plant (henceforth referred to as Plant 0, and located in the Upper Midwest), followed by the performance and analysis of similar field experiments at two additional coal-fired power plants (Plants 1 and 2) utilizing different coal types and with different plant configurations. Significant progress was made on the Project during this reporting period, with field work being initiated at Plant 0. Initial testing of the stack sampling system and reaction apparatus revealed that primary particle concentrations were lower than expected in the emissions entering the mobile chemical laboratory. Initial animal exposures to primary emissions were carried out (Scenario 1) to ensure successful implementation of all study methodologies and toxicological assessments. Results indicated no significant toxicological effects in response to primary emissions exposures. Exposures were then carried out to diluted, oxidized, neutralized emissions with the addition of secondary organic aerosol (Scenario 5), both during the day and also at night when primary particle concentrations in the sampled stack emissions

Large contribution of fossil fuel derived secondary organic carbon to water soluble organic aerosols in winter haze in China

Directory of Open Access Journals (Sweden)

Y.-L. Zhang

2018-03-01

Full Text Available Water-soluble organic carbon (WSOC is a large fraction of organic aerosols (OA globally and has significant impacts on climate and human health. The sources of WSOC remain very uncertain in polluted regions. Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C and offline high-resolution time-of-flight aerosol mass spectrometer measurements. Fossil emissions on average accounted for 32–47 % of WSOC. Secondary organic carbon (SOC dominated both the non-fossil and fossil derived WSOC, highlighting the importance of secondary formation to WSOC in severe winter haze episodes. Contributions from fossil emissions to SOC were 61 ± 4 and 50 ± 9 % in Shanghai and Beijing, respectively, significantly larger than those in Guangzhou (36 ± 9 % and Xi'an (26 ± 9 %. The most important primary sources were biomass burning emissions, contributing 17–26 % of WSOC. The remaining primary sources such as coal combustion, cooking and traffic were generally very small but not negligible contributors, as coal combustion contribution could exceed 10 %. Taken together with earlier 14C source apportionment studies in urban, rural, semi-urban and background regions in Asia, Europe and the USA, we demonstrated a dominant contribution of non-fossil emissions (i.e., 75 ± 11 % to WSOC aerosols in the Northern Hemisphere; however, the fossil fraction is substantially larger in aerosols from East Asia and the eastern Asian pollution outflow, especially during winter, due to increasing coal combustion. Inclusion of our findings can improve a modelling of effects of WSOC aerosols on climate, atmospheric chemistry and public health.

Identification of secondary aerosol precursors emitted by an aircraft turbofan

Science.gov (United States)

Kılıç, Doğuşhan; El Haddad, Imad; Brem, Benjamin T.; Bruns, Emily; Bozetti, Carlo; Corbin, Joel; Durdina, Lukas; Huang, Ru-Jin; Jiang, Jianhui; Klein, Felix; Lavi, Avi; Pieber, Simone M.; Rindlisbacher, Theo; Rudich, Yinon; Slowik, Jay G.; Wang, Jing; Baltensperger, Urs; Prévôt, Andre S. H.

2018-05-01

Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM) chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs) and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS) for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS) for nonrefractory particulate matter (NR-PM1) were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5-7 %), more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

Time evolution and emission factors of aerosol particles from day and night time savannah fires

Science.gov (United States)

Vakkari, Ville; Beukes, Johan Paul; Tiitta, Petri; Venter, Andrew; Jaars, Kerneels; Josipovic, Miroslav; van Zyl, Pieter; Kulmala, Markku; Laakso, Lauri

2013-04-01

The largest uncertainties in the current global climate models originate from aerosol particle effects (IPCC, 2007) and at the same time aerosol particles also pose a threat to human health (Pope and Dockery, 2006). In southern Africa wild fires and prescribed burning are one of the most important sources of aerosol particles, especially during the dry season from June to September (e.g. Swap et al., 2003; Vakkari et al., 2012). The aerosol particle emissions from savannah fires in southern Africa have been studied in several intensive campaigns such as SAFARI 1992 and 2000 (Swap et al., 2003). However, all previous measurements have been carried out during the daytime, whereas most of the prescribed fires in southern Africa are lit up only after sunset. Furthermore, the previous campaigns followed the plume evolution for up to one hour after emission only. In this study, combining remote sensing fire observations to ground-based long-term measurements of aerosol particle and trace gas properties at the Welgegund measurement station (www.welgegund.org), we have been able to follow the time evolution of savannah fire plumes up to several hours in the atmosphere. For the first time the aerosol particle size distribution measurements in savannah fire plumes cover both day and night time plumes and also the ultrafine size range below 100 nm. During the period from May 20th 2010 to April 15th 2012 altogether 61 savannah fire plumes were observed at Welgegund. The evolution of the aerosol size distribution remained rapid for at least five hours after the fire: during this period the growth rate of the aerosol particle count mean diameter (size range 12 to 840 nm) was 24 nm h-1 for daytime plumes and 8 nm h-1 for night time plumes. The difference in the day and night time growth rate shows that photochemical reactions significantly increase the condensable vapour concentration in the plume. Furthermore, the condensable vapour concentration was found to affect both the

Secondary Organic Aerosol Production from Gasoline Vehicle Exhaust: Effects of Engine Technology, Cold Start, and Emission Certification Standard.

Science.gov (United States)

Zhao, Yunliang; Lambe, Andrew T; Saleh, Rawad; Saliba, Georges; Robinson, Allen L

2018-02-06

Secondary organic aerosol (SOA) formation from dilute exhaust from 16 gasoline vehicles was investigated using a potential aerosol mass (PAM) oxidation flow reactor during chassis dynamometer testing using the cold-start unified cycle (UC). Ten vehicles were equipped with gasoline direct injection engines (GDI vehicles) and six with port fuel injection engines (PFI vehicles) certified to a wide range of emissions standards. We measured similar SOA production from GDI and PFI vehicles certified to the same emissions standard; less SOA production from vehicles certified to stricter emissions standards; and, after accounting for differences in gas-particle partitioning, similar effective SOA yields across different engine technologies and certification standards. Therefore the ongoing, dramatic shift from PFI to GDI vehicles in the United States should not alter the contribution of gasoline vehicles to ambient SOA and the natural replacement of older vehicles with newer ones certified to stricter emissions standards should reduce atmospheric SOA levels. Compared to hot operations, cold-start exhaust had lower effective SOA yields, but still contributed more SOA overall because of substantially higher organic gas emissions. We demonstrate that the PAM reactor can be used as a screening tool for vehicle SOA production by carefully accounting for the effects of the large variations in emission rates.

Long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometer

Science.gov (United States)

Xu, J.; Zhang, X.; Liu, Y.; Shichang, K.; Ma, Y.

2017-12-01

An intensive measurement was conducted at a remote, background, and high-altitude site (Qomolangma station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from April 12 to May 12, 2016 to chemically characterize high time-resolved submicron particulate matter (PM1) and obtain the influence of biomass burning emissions to the Himalayas, frequently transported from south Asia during pre-monsoon season. Two high aerosol loading periods were observed during the study. Overall, the average (± 1σ) PM1 mass concentration was 4.44 (± 4.54) µg m-3 for the entire study, comparable with those observed at other remote sites worldwide. Organic aerosols (OA) was the dominant PM1 species (accounting for 54.3% of total PM1 mass on average) and its contribution increased with the increase of total PM1 mass loading. The average size distributions of PM1 species all peaked at an overlapping accumulation mode ( 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transportations. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a biomass burning related OA (BBOA, 43.7%) and two oxygenated OA (Local-OOA and LRT-OOA; 13.9% and 42.4%) represented sources from local emissions and long-range transportations, respectively. Two polluted air mass origins (generally from the west and southwest of QOMS) and two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions were observed, respectively, suggesting the important sources of wildfires from south Asia. One of polluted aerosol plumes was investigated in detail to illustrate the evolution of aerosol characteristics at QOMS driving by different impacts of wildfires, air mass origins, meteorological conditions and

Climate Implications of the Heterogeneity of Anthropogenic Aerosol Forcing

Science.gov (United States)

Persad, Geeta Gayatri

Short-lived anthropogenic aerosols are concentrated in regions of high human activity, where they interact with radiation and clouds, causing horizontally heterogeneous radiative forcing between polluted and unpolluted regions. Aerosols can absorb shortwave energy in the atmosphere, but deplete it at the surface, producing opposite radiative perturbations between the surface and atmosphere. This thesis investigates climate and policy implications of this horizontal and vertical heterogeneity of anthropogenic aerosol forcing, employing the Geophysical Fluid Dynamics Laboratory's AM2.1 and AM3 models, both at a global scale and using East Asia as a regional case study. The degree of difference between spatial patterns of climate change due to heterogeneous aerosol forcing versus homogeneous greenhouse gas forcing deeply impacts the detection, attribution, and prediction of regional climate change. This dissertation addresses a gap in current understanding of these two forcings' response pattern development, using AM2.1 historical forcing simulations. The results indicate that fast atmospheric and land-surface processes alone substantially homogenize the global pattern of surface energy flux response to heterogeneous aerosol forcing. Aerosols' vertical redistribution of energy significantly impacts regional climate, but is incompletely understood. It is newly identified here, via observations and historical and idealized forcing simulations, that increased aerosol-driven atmospheric absorption may explain half of East Asia's recent surface insolation decline. Further, aerosols' surface and atmospheric effects counteract each other regionally---atmospheric heating enhances summer monsoon circulation, while surface dimming suppresses it---but absorbing aerosols' combined effects reduce summer monsoon rainfall. This thesis constitutes the first vertical decomposition of aerosols' impacts in this high-emissions region and elucidates the monsoonal response to aerosols

Temporal variability in aerosol characteristics and its radiative properties over Patiala, northwestern part of India: Impact of agricultural biomass burning emissions.

Science.gov (United States)

Sharma, D; Srivastava, A K; Ram, K; Singh, A; Singh, D

2017-12-01

A comprehensive measurements of aerosol optical depth (AOD), particulate matter (PM) and black carbon (BC) mass concentrations have been carried out over Patiala, a semi-urban site in northwest India during October 2008 to September 2010. The measured aerosol data was incorporated in an aerosol optical model to estimate various aerosol optical parameters, which were subsequently used for radiative forcing estimation. The measured AOD at 500 nm (AOD 500 ) shows a significant seasonal variability, with maximum value of 0.81 during post-monsoon (PoM) and minimum of 0.56 during winter season. The Ångström exponent (α) has higher values (i.e. more fine-mode fraction) during the PoM/winter periods, and lower (i.e. more coarse-mode fraction) during pre-monsoon (PrM). In contrast, turbidity coefficient (β) exhibits an opposite trend to α during the study period. BC mass concentration varies from 2.8 to 13.9 μg m -3 (mean: 6.5 ± 3.2 μg m -3 ) during the entire study period, with higher concentrations during PoM/winter and lower during PrM/monsoon seasons. The average single scattering albedo (SSA at 500 nm) values are 0.70, 0.72, 0.82 and 0.75 during PoM, winter, PrM and monsoon seasons, respectively. However, inter-seasonal and inter-annual variability in measured aerosol parameters are statistically insignificant at Patiala. These results suggest strong changes in emission sources, aerosol composition, meteorological parameters as well as transport of aerosols over the station. Higher values of AOD, α and BC, along with lower SSA during PoM season are attributed to agriculture biomass burning emissions over and around the station. The estimated aerosol radiative forcing within the atmosphere is positive (i.e. warming) during all the seasons with higher values (∼60 Wm -2 ) during PoM-08/PoM-09 and lower (∼40 Wm -2 ) during winter-09/PrM-10. The present study highlights the role of BC aerosols from agricultural biomass burning emissions during post

Secondary organic aerosol importance in the future atmosphere

International Nuclear Information System (INIS)

Tsigaridis, K.; Kanakidou, M.

2007-01-01

In order to investigate the secondary organic aerosol (SOA) response to changes in biogenic volatile organic compounds (VOC) emissions in the future atmosphere and how important will SOA be relative to the major anthropogenic aerosol component (sulfate), the global three-dimensional chemistry/transport model TM3 has been used. Emission estimates of biogenic VOC (BVOC) and anthropogenic gases and particles from the literature for the year 2100 have been adopted. According to our present-day model simulations, isoprene oxidation produces 4.6 Tg SOA yr -1 , that is less than half of the 12.2 Tg SOA yr -1 formed by the oxidation of other BVOC. In the future, nitrate radicals and ozone become more important than nowadays, but remain minor oxidants for both isoprene and aromatics. SOA produced by isoprene is estimated to almost triple, whereas the production from other BVOC more than triples. The calculated future SOA burden change, from 0.8 Tg at present to 2.0 Tg in the future, is driven by changes in emissions, oxidant levels and pre-existing particles. The non-linearity in SOA formation and the involved chemical and physical feedbacks prohibit the quantitative attribution of the computed changes to the above-mentioned individual factors. In 2100, SOA burden is calculated to exceed that of sulfate, indicating that SOA might become more important than nowadays. These results critically depend on the biogenic emissions and thus are subject to the high uncertainty associated with these emissions estimated due to the insufficient knowledge on plant response to carbon dioxide changes. Nevertheless, they clearly indicate that the change in oxidants and primary aerosol caused by human activities can contribute as much as the change in BVOC emissions to the increase of the biogenic SOA production in the future atmosphere. (authors)

Impact of Emissions and Long-Range Transport on Multi-Decadal Aerosol Trends: Implications for Air Quality and Climate

Science.gov (United States)

Chin, Mian

2012-01-01

We present a global model analysis of the impact of long-range transport and anthropogenic emissions on the aerosol trends in the major pollution regions in the northern hemisphere and in the Arctic in the past three decades. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to analyze the multi-spatial and temporal scale data, including observations from Terra, Aqua, and CALIPSO satellites and from the long-term surface monitoring stations. We will analyze the source attribution (SA) and source-receptor (SR) relationships in North America, Europe, East Asia, South Asia, and the Arctic at the surface and free troposphere and establish the quantitative linkages between emissions from different source regions. We will discuss the implications for regional air quality and climate change.

Chemical interactions between aerosols and vapors in the primary circuit of an LWR during a severe accident

International Nuclear Information System (INIS)

Wheatley, C.J.

1988-01-01

Aerosol formation, agglomeration, convection and deposition within the primary circuit of an LWR during a severe accident significantly affect the transport of fission products, even though they may compose only a small fraction of the aerosol material. Intra-particle and vapor chemical interactions are important to this through mass transfer between the aerosol and vapor. The authors will describe a model that attempts to account for these processes and of the two-way coupling that exists with the thermal hydraulics. They will discuss what agglomeration and deposition mechanisms must be included, alternatives for treating intra-particle chemical interactions, mechanisms of aerosol formation, and methods for solving the resulting equations. Results will be presented that illustrate the importance of treating the two-way coupling and the extent to which disequilibrium between the aerosol and vapor affects fission product behavior

Impact of anthropogenic emissions and open biomass burning on regional carbonaceous aerosols in South China

Energy Technology Data Exchange (ETDEWEB)

Zhang Gan, E-mail: zhanggan@gig.ac.c [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Li Jun [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Li Xiangdong [Department of Civil and Structural Engineering, Hong Kong Polytechnic University, Hung Hom, Kowloon (Hong Kong); Xu Yue; Guo Lingli [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Tang Jianhui [Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003 (China); Lee, Celine S.L. [Department of Civil and Structural Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon (Hong Kong); Liu Xiang [State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640 (China); Chen Yingjun [Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003 (China)

2010-11-15

Carbonaceous aerosols were studied at three background sites in south and southwest China. Hok Tsui in Hong Kong had the highest concentrations of carbonaceous aerosols (OC = 8.7 {+-} 4.5 {mu}g/m{sup 3}, EC = 2.5 {+-} 1.9 {mu}g/m{sup 3}) among the three sites, and Jianfeng Mountains in Hainan Island (OC = 5.8 {+-} 2.6 {mu}g/m{sup 3}, EC = 0.8 {+-} 0.4 {mu}g/m{sup 3}) and Tengchong mountain over the east edge of the Tibetan Plateau (OC = 4.8 {+-} 4.0 {mu}g/m{sup 3}, EC = 0.5 {+-} 0.4 {mu}g/m{sup 3}) showed similar concentration levels. Distinct seasonal patterns with higher concentrations during the winter, and lower concentrations during the summertime were observed, which may be caused by the changes of the regional emissions, and monsoon effects. The industrial and vehicular emissions in East, Southeast and South China, and the regional open biomass burning in the Indo-Myanmar region of Asia were probably the two major potential sources for carbonaceous matters in this region. - Anthropogenic emissions in China and open biomass burning in the Indo-Myanmar region were the two major potential sources for carbonaceous matters in South China region.

The possible influence of volcanic emissions on atmospheric aerosols in the city of Colima, Mexico

International Nuclear Information System (INIS)

Miranda, Javier; Zepeda, Francisco; Galindo, Ignacio

2004-01-01

An elemental composition study of atmospheric aerosols from the City of Colima, in the Western Coast of Mexico, is presented. Samples of PM 15 -PM 2.5 and PM 2.5 were collected with Stacked Filter Units (SFU) of the Davis design, in urban and rural sites, the latter located between the City of Colima and the Volcan de Colima, an active volcano. Elemental analyses were carried out using Particle Induced X-ray Emission (PIXE). The gravimetric mass concentrations for the fine fraction were slightly higher in the urban site, while the mean concentrations in the coarse fraction were equal within the uncertainties. High Cl contents were determined in the coarse fraction, a fact also observed in emissions from the Volcan de Colima by other authors. In addition to average elemental concentrations, cluster analysis based on elemental contents was performed, with wind speed and direction data, showing that there is an industrial contributor to aerosols North of the urban area. Moreover, a contribution from the volcanic emissions was identified from the grouping of S, Cl, Cu, and Zn, elements associated to particles emitted by the Volcan de Colima. - Elemental analyses of PM 15 in the City of Colima, Mexico, were done to identify possible contributions from the Volcan de Colima, an active volcano

Impact of anthropogenic emissions and open biomass burning on regional carbonaceous aerosols in South China

International Nuclear Information System (INIS)

Zhang Gan; Li Jun; Li Xiangdong; Xu Yue; Guo Lingli; Tang Jianhui; Lee, Celine S.L.; Liu Xiang; Chen Yingjun

2010-01-01

Carbonaceous aerosols were studied at three background sites in south and southwest China. Hok Tsui in Hong Kong had the highest concentrations of carbonaceous aerosols (OC = 8.7 ± 4.5 μg/m 3 , EC = 2.5 ± 1.9 μg/m 3 ) among the three sites, and Jianfeng Mountains in Hainan Island (OC = 5.8 ± 2.6 μg/m 3 , EC = 0.8 ± 0.4 μg/m 3 ) and Tengchong mountain over the east edge of the Tibetan Plateau (OC = 4.8 ± 4.0 μg/m 3 , EC = 0.5 ± 0.4 μg/m 3 ) showed similar concentration levels. Distinct seasonal patterns with higher concentrations during the winter, and lower concentrations during the summertime were observed, which may be caused by the changes of the regional emissions, and monsoon effects. The industrial and vehicular emissions in East, Southeast and South China, and the regional open biomass burning in the Indo-Myanmar region of Asia were probably the two major potential sources for carbonaceous matters in this region. - Anthropogenic emissions in China and open biomass burning in the Indo-Myanmar region were the two major potential sources for carbonaceous matters in South China region.

Temporal variability in aerosol characteristics and its radiative properties over Patiala, northwestern part of India: Impact of agricultural biomass burning emissions

International Nuclear Information System (INIS)

Sharma, D.; Srivastava, A.K.; Ram, K.; Singh, A.; Singh, D.

2017-01-01

A comprehensive measurements of aerosol optical depth (AOD), particulate matter (PM) and black carbon (BC) mass concentrations have been carried out over Patiala, a semi-urban site in northwest India during October 2008 to September 2010. The measured aerosol data was incorporated in an aerosol optical model to estimate various aerosol optical parameters, which were subsequently used for radiative forcing estimation. The measured AOD at 500 nm (AOD 500 ) shows a significant seasonal variability, with maximum value of 0.81 during post-monsoon (PoM) and minimum of 0.56 during winter season. The Ångström exponent (α) has higher values (i.e. more fine-mode fraction) during the PoM/winter periods, and lower (i.e. more coarse-mode fraction) during pre-monsoon (PrM). In contrast, turbidity coefficient (β) exhibits an opposite trend to α during the study period. BC mass concentration varies from 2.8 to 13.9 μg m −3 (mean: 6.5 ± 3.2 μg m −3 ) during the entire study period, with higher concentrations during PoM/winter and lower during PrM/monsoon seasons. The average single scattering albedo (SSA at 500 nm) values are 0.70, 0.72, 0.82 and 0.75 during PoM, winter, PrM and monsoon seasons, respectively. However, inter-seasonal and inter-annual variability in measured aerosol parameters are statistically insignificant at Patiala. These results suggest strong changes in emission sources, aerosol composition, meteorological parameters as well as transport of aerosols over the station. Higher values of AOD, α and BC, along with lower SSA during PoM season are attributed to agriculture biomass burning emissions over and around the station. The estimated aerosol radiative forcing within the atmosphere is positive (i.e. warming) during all the seasons with higher values (∼60 Wm −2 ) during PoM–08/PoM–09 and lower (∼40 Wm −2 ) during winter–09/PrM–10. The present study highlights the role of BC aerosols from agricultural biomass burning

TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

Energy Technology Data Exchange (ETDEWEB)

Annette C. Rohr; Petros Koutrakis; John Godleski

2011-03-31

Determining the health impacts of different sources and components of fine particulate matter (PM2.5) is an important scientific goal, because PM is a complex mixture of both inorganic and organic constituents that likely differ in their potential to cause adverse health outcomes. The TERESA (Toxicological Evaluation of Realistic Emissions of Source Aerosols) study focused on two PM sources - coal-fired power plants and mobile sources - and sought to investigate the toxicological effects of exposure to realistic emissions from these sources. The DOE-EPRI Cooperative Agreement covered the performance and analysis of field experiments at three power plants. The mobile source component consisted of experiments conducted at a traffic tunnel in Boston; these activities were funded through the Harvard-EPA Particulate Matter Research Center and will be reported separately in the peer-reviewed literature. TERESA attempted to delineate health effects of primary particles, secondary (aged) particles, and mixtures of these with common atmospheric constituents. The study involved withdrawal of emissions directly from power plant stacks, followed by aging and atmospheric transformation of emissions in a mobile laboratory in a manner that simulated downwind power plant plume processing. Secondary organic aerosol (SOA) derived from the biogenic volatile organic compound {alpha}-pinene was added in some experiments, and in others ammonia was added to neutralize strong acidity. Specifically, four scenarios were studied at each plant: primary particles (P); secondary (oxidized) particles (PO); oxidized particles + secondary organic aerosol (SOA) (POS); and oxidized and neutralized particles + SOA (PONS). Extensive exposure characterization was carried out, including gas-phase and particulate species. Male Sprague Dawley rats were exposed for 6 hours to filtered air or different atmospheric mixtures. Toxicological endpoints included (1) breathing pattern; (2) bronchoalveolar lavage

Climatic effects of 1950–2050 changes in US anthropogenic aerosols – Part 1: Aerosol trends and radiative forcing

Directory of Open Access Journals (Sweden)

D. G. Streets

2012-04-01

Full Text Available We calculate decadal aerosol direct and indirect (warm cloud radiative forcings from US anthropogenic sources over the 1950–2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980–2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970–1990, with values over the eastern US (east of 100° W of −2.0 W m−2 for direct forcing including contributions from sulfate (−2.0 W m−2, nitrate (−0.2 W m−2, organic carbon (−0.2 W m−2, and black carbon (+0.4 W m−2. The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50%. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8 W m−2 direct and 1.0 W m−2 indirect, mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3 W m−2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide suggests that a US emission control strategy focused on BC would have only limited climate benefit.

Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

Science.gov (United States)

Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

2016-07-01

Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

Field study of a Brownian Demister Unit to reduce aerosol based emission from a Post Combustion CO2 Capture plant

NARCIS (Netherlands)

Khakharia, P.M.; Kvamsdal, H.M.; Da Silva, E.F.; Vlugt, T.J.H.; Goetheer, E.L.V.

2014-01-01

Emission of solvent and its degradation products from a typical absorption-desorption based Post Combustion CO2 Capture (PCCC) process is inevitable and thus, an area of growing concern. Recently, it has been pointed out that emissions can also occur by means of aerosol droplets. Conventional

Contribution to the study of nuclear aerosol: looking for the dynamic form factor of the aerosol of primary particles of sodium oxide

International Nuclear Information System (INIS)

Barbe, M.

1982-09-01

The dynamical form factor describes the entrainment of any non spherical particle, of inhomogeneous density, in relation to the entrainment of a spherical particle with the same volume and some sedimentation speed. Experimental study of the form factor and particle size distribution of sodium peroxide primary aerosols [fr

Will Aerosol Hygroscopicity Change with Biodiesel, Renewable Diesel Fuels and Emission Control Technologies?

Science.gov (United States)

Vu, Diep; Short, Daniel; Karavalakis, Georgios; Durbin, Thomas D; Asa-Awuku, Akua

2017-02-07

The use of biodiesel and renewable diesel fuels in compression ignition engines and aftertreatment technologies may affect vehicle exhaust emissions. In this study two 2012 light-duty vehicles equipped with direct injection diesel engines, diesel oxidation catalyst (DOC), diesel particulate filter (DPF), and selective catalytic reduction (SCR) were tested on a chassis dynamometer. One vehicle was tested over the Federal Test Procedure (FTP) cycle on seven biodiesel and renewable diesel fuel blends. Both vehicles were exercised over double Environmental Protection Agency (EPA) Highway fuel economy test (HWFET) cycles on ultralow sulfur diesel (ULSD) and a soy-based biodiesel blend to investigate the aerosol hygroscopicity during the regeneration of the DPF. Overall, the apparent hygroscopicity of emissions during nonregeneration events is consistently low (κ diesel vehicles. As such, the contribution of regeneration emissions from a growing fleet of diesel vehicles will be important.

Development of a United States-Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study.

Science.gov (United States)

Kuhns, Hampden; Knipping, Eladio M; Vukovich, Jeffrey M

2005-05-01

The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was commissioned to investigate the sources of haze at Big Bend National Park in southwest Texas. The modeling domain of the BRAVO Study includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The first regional-scale Mexican emissions inventory designed for air-quality modeling applications was developed for 10 northern Mexican states, the Tula Industrial Park in the state of Hidalgo, and the Popocatépetl volcano in the state of Puebla. Emissions data were compiled from numerous sources, including the U.S. Environmental Protection Agency (EPA), the Texas Natural Resources Conservation Commission (now Texas Commission on Environmental Quality), the Eastern Research Group, the Minerals Management Service, the Instituto Nacional de Ecología, and the Instituto Nacional de Estadistica Geografía y Informática. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) < 10 microm in aerodynamic diameter, and PM < 2.5 microm in aerodynamic diameter. Wind-blown dust and biomass burning were not included in the inventory, although high concentrations of dust and organic PM attributed to biomass burning have been observed at Big Bend National Park. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions

Plutonium-aerosol emission rates and human pulmonary deposition calculations for Nuclear Site 201, Nevada Test Site

International Nuclear Information System (INIS)

Shinn, J.H.; Homan, D.N.

1982-01-01

This study determined the plutonium-aerosol fluxes from the soil to quantify (1) the extent of potential human exposure by deep-lung retention of alpha-emitting particles; (2) the source term should there be any significant, long-term, transport of plutonium aerosols; and (3) the resuspension factor and rate so that, for the first time at any nuclear site, one may calculate how long it will take for wind erosion to carry away a significant amount of the contaminated soil. High-volume air samplers and cascade impactors were used to characterize the plutonium aerosols. Meteorological flux-profile methods were used to calculate dust and plutonium aerosol emission rates. A floorless wind tunnel (10-m long) was used to examine resuspension under steady-state, high wind speed. The resuspension factor was two orders of magnitude lower than the other comparable sites at NTS and elsewhere, and the average resuspension rate of 5.3 x 10 -8 /d was also very low, so that the half-time for resuspension by wind erosion was about 36,000 y

Fractional iron solubility of aerosol particles enhanced by biomass burning and ship emission in Shanghai, East China.

Science.gov (United States)

Fu, H B; Shang, G F; Lin, J; Hu, Y J; Hu, Q Q; Guo, L; Zhang, Y C; Chen, J M

2014-05-15

In terms of understanding Fe mobilization from aerosol particles in East China, the PM2.5 particles were collected in spring at Shanghai. Combined with the backtrajectory analysis, the PM2.5/PM10 and Ca/Al ratios, a serious dust-storm episode (DSE) during the sampling was identified. The single-particle analysis showed that the major iron-bearing class is the aluminosilicate dust during DSE, while the Fe-bearing aerosols are dominated by coal fly ash, followed by a minority of iron oxides during the non-dust storm days (NDS). Chemical analyses of samples showed that the fractional Fe solubility (%FeS) is much higher during NDS than that during DSE, and a strong inverse relationship of R(2)=0.967 between %FeS and total atmospheric iron loading were found, suggested that total Fe (FeT) is not controlling soluble Fe (FeS) during the sampling. Furthermore, no relationship between FeS and any of acidic species was established, suggesting that acidic process on aerosol surfaces are not involved in the trend of iron solubility. It was thus proposed that the source-dependent composition of aerosol particles is a primary determinant for %FeS. Specially, the Al/Fe ratio is poorly correlated (R(2)=0.113) with %FeS, while the apparent relationship between %FeS and the calculated KBB(+)/Fe ratio (R(2)=0.888) and the V/Fe ratio (R(2)=0.736) were observed, reflecting that %FeS could be controlled by both biomass burning and oil ash from ship emission, rather than mineral particles and coal fly ash, although the latter two are the main contributors to the atmospheric Fe loading during the sampling. Such information can be useful improving our understanding on iron solubility on East China, which may further correlate with iron bioavailability to the ocean, as well as human health effects associated with exposure to fine Fe-rich particles in densely populated metropolis in China. Copyright © 2014 Elsevier B.V. All rights reserved.

Aerosol composition and source apportionment in Santiago de Chile

Science.gov (United States)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dpsource apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of several heavy metals such as Zn, Cu and others. A factor with molybdenum, arsenic, copper and sulfur was observed frequently, and it results from emissions of copper smelters.

Historical gaseous and primary aerosol emissions in the United States from 1990 to 2010

Directory of Open Access Journals (Sweden)

J. Xing

2013-08-01

Full Text Available An accurate description of emissions is crucial for model simulations to reproduce and interpret observed phenomena over extended time periods. In this study, we used an approach based on activity data to develop a consistent series of spatially resolved emissions in the United States from 1990 to 2010. The state-level anthropogenic emissions of SO2, NOx, CO, NMVOC (non-methane volatile organic compounds, NH3, PM10 and PM2.5 for a total of 49 sectors were estimated based on several long-term databases containing information about activities and emission controls. Activity data for energy-related stationary sources were derived from the State Energy Data System. Corresponding emission factors reflecting implemented emission controls were calculated back from the National Emissions Inventory (NEI for seven years (i.e., 1990, 1995, 1996, 1999, 2001, 2002 and 2005, and constrained by the AP-42 (US EPA's Compilation of Air Pollutant Emissions Factors dataset. Activity data for mobile sources including different types of highway vehicles and non-highway equipment were obtained from highway statistics reported by the Federal Highway Administration. The trends in emission factors for highway mobile source were informed by the 2011 National Transportation Statistics. Emissions for all non-energy-related sources were either scaled by the growth ratio of activity indicators or adjusted based on the NEI trends report. Because of the strengthened control efforts, particularly for the power sector and mobile sources, emissions of all pollutants except NH3 were reduced by half over the last two decades. The emission trends developed in this study are comparable with the NEI trend report and EDGAR (Emissions Database for Global Atmospheric Research data, but better constrained by trends in activity data. Reductions in SO2, NOx, CO and EC (speciation of PM2.5 by SMOKE, Sparse Matrix Operator Kernel Emissions emissions agree well with the observed changes in

Determination of light elements concentration in aerosols by X emission induced by deuteron

International Nuclear Information System (INIS)

Morales, J.R.; Romo, C.

1983-01-01

Absolute concentrations for Al, Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe and Cu were obtained in the range from 10 ng/m 3 to 10 4 ng/m 3 in aerosols from Santiago. A 4,2 MeV deuteron beam was used to induce characteristic X-ray emission. It was found that relative abundance of these elements is maintained for days of high and low total suspended particulates. (Author)

Polar and non-polar organic aerosols from large-scale agricultural-waste burning emissions in Northern India: Implications to organic mass-to-organic carbon ratio.

Science.gov (United States)

Rajput, Prashant; Sarin, M M

2014-05-01

This study focuses on characteristics of organic aerosols (polar and non-polar) and total organic mass-to-organic carbon ratio (OM/OC) from post-harvest agricultural-waste (paddy- and wheat-residue) burning emissions in Northern India. Aerosol samples from an upwind location (Patiala: 30.2°N, 76.3°E) in the Indo-Gangetic Plain were analyzed for non-polar and polar fractions of organic carbon (OC1 and OC2) and their respective mass (OM1 and OM2). On average, polar organic aerosols (OM2) contribute nearly 85% of the total organic mass (OM) from the paddy- and wheat-residue burning emissions. The water-soluble-OC (WSOC) to OC2 ratio, within the analytical uncertainty, is close to 1 from both paddy- and wheat-residue burning emissions. However, temporal variability and relatively low WSOC/OC2 ratio (Av: 0.67±0.06) is attributed to high moisture content and poor combustion efficiency during paddy-residue burning, indicating significant contribution (∼30%) of aromatic carbon to OC2. The OM/OC ratio for non-polar (OM1/OC1∼1.2) and polar organic aerosols (OM2/OC2∼2.2), hitherto unknown for open agricultural-waste burning emissions, is documented in this study. The total OM/OC ratio is nearly identical, 1.9±0.2 and 1.8±0.2, from paddy- and wheat-residue burning emissions. Copyright © 2013 Elsevier Ltd. All rights reserved.

Identification of secondary aerosol precursors emitted by an aircraft turbofan

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D. Kılıç

2018-05-01

Full Text Available Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS for nonrefractory particulate matter (NR-PM1 were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5–7 %, more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

Prevention of PCDD/Fs emission from a municipal wastewater sludge incinerator through enhanced control of copper aerosol

Directory of Open Access Journals (Sweden)

Peña, E.

2012-10-01

Full Text Available Municipal wastewater sludge incineration (MWSI leads to products of incomplete combustion, including chlorinated species such as dioxins and furans (PCDD/Fs. Other pollutants, such as heavy metals (HM, are released too as a consequence of feed traces, which depend on the specific activities of each area. The main aim of this work is to determine whether the early separation of the potential catalysts on the PCDD/Fs formation –HM as copper or zinc– offers a promising way to prevent the emission of these trace pollutants, considering that the current end-of-pipe measures don’t ensure their stable emission. Experimental results cover the size distributed target metal contents along the incineration line. These results show a high concentration of copper in the most penetrating aerosol size range of the electrostatic precipitator (0.6 μm - 1.0 μm, and how low emission values of both, total and metallic aerosol (mass basis, are compatible with irregular and unexplained outliers of PCDD/Fs emission.

La incineración de lodos de aguas residuales urbanas acarrea la formación de compuestos derivados de combustiones incompletas, incluyendo especies cloradas como dioxinas y furanos (PCDD/Fs. Otros contaminantes, como metales pesados, se emiten como consecuencia de las trazas del lodo, las cuales dependen de las actividades del entorno. El objetivo principal es determinar si la separación de catalizadores potenciales en reacciones de formación de PCDD/Fs (cobre o zinc puede abrir vías para prevenir la emisión de contaminantes traza, considerando que ninguna de las técnicas de prevención actuales aseguran emisiones estables de metales pesados o PCDD/Fs. Se determinan concentraciones de metales pesados segregados por tamaño de partícula a lo largo de la línea de incineración. Los resultados muestran concentraciones elevadas de cobre en el aerosol de máxima penetración del electrofiltro (0,6 μm - 1,0 μm, y cómo concentraciones

Microbiology and atmospheric processes: chemical interactions of primary biological aerosols

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L. Deguillaume

2008-07-01

Full Text Available This paper discusses the influence of primary biological aerosols (PBA on atmospheric chemistry and vice versa through microbiological and chemical properties and processes. Several studies have shown that PBA represent a significant fraction of air particulate matter and hence affect the microstructure and water uptake of aerosol particles. Moreover, airborne micro-organisms, namely fungal spores and bacteria, can transform chemical constituents of the atmosphere by metabolic activity. Recent studies have emphasized the viability of bacteria and metabolic degradation of organic substances in cloud water. On the other hand, the viability and metabolic activity of airborne micro-organisms depend strongly on physical and chemical atmospheric parameters such as temperature, pressure, radiation, pH value and nutrient concentrations. In spite of recent advances, however, our knowledge of the microbiological and chemical interactions of PBA in the atmosphere is rather limited. Further targeted investigations combining laboratory experiments, field measurements, and modelling studies will be required to characterize the chemical feedbacks, microbiological activities at the air/snow/water interface supplied to the atmosphere.

The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite, Taiwan

Science.gov (United States)

Chang, Shih-Yu; Lee, Chung-Te; Chou, Charles C.-K.; Liu, Shaw-Chen; Wen, Tian-Xue

The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas-aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl -, NO 2-, NO 3-, SO 42-, Na +, NH 4+, K +, Mg 2+ and Ca 2+). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m -3 for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.

Impacts of Future Climate, Emission, and Land Use Changes on Aerosols and Air Quality over the Continental

Science.gov (United States)

Changes in climate, emission, and land use in the U.S. over the next century are imminent. The response of geologic, biogenic, and anthropogenic aerosol to interactions between these changes, however, are more uncertain and difficult to quantify. To explore these interactions, ...

Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

OpenAIRE

Gantt, B.; Kelly, J. T.; Bash, J. O.

2015-01-01

Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the...

Organic molecular composition of marine aerosols over the Arctic Ocean in summer: contributions of primary emission and secondary aerosol formation

OpenAIRE

P. Q. Fu; K. Kawamura; J. Chen; B. Charrière; R. Sempéré

2013-01-01

Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m⁻³ (mean 47.6 ng m⁻³), accounting ...

Evaluation of the health impact of aerosols emitted from different combustion sources: Comprehensive characterization of the aerosol physicochemical properties as well as the molecular biological and toxicological effects of the aerosols on human lung cells and macrophages.

Science.gov (United States)

Zimmermann, R.; Dittmar, G.; Kanashova, T.; Buters, J.; Öder, S.; Paur, H. R.; Mülhopt, S.; Dilger, M.; Weiss, C.; Harndorf, H.; Stengel, B.; Hirvonen, M. R.; Jokiniemi, J.; Hiller, K.; Sapcariu, S.; Sippula, O.; Streibel, T.; Karg, E.; Weggler, B.; Schnelle-Kreis, J.; Lintelmann, J.; Sklorz, M.; Orasche, J.; Müller, L.; Passig, J.; Gröger, T.; Jalava, P. I.; Happo, M.; Uski, O.

2017-12-01

A novel approach to evaluate the health effects of anthropogenic combustion emissions is the detailed comparison of comprehensive physicochemical data on the combustion aerosol properties with the biological response of aerosol-exposed lung cells. In this context the "HICE-Aerosol and Health" project consortium studies the properties as well as the biological and toxicological effects on lung cells induced by different combustion aerosol emissions (e.g. ship diesel exhaust, wood combustion effluents or automobile aerosol). Human alveolar epithelial cells (e.g. A549 cells) as well as murine macrophages were exposed to diluted emissions, using field deployable ALI-exposition systems in a mobile S2-biological laboratory. This allows a realistic lung-cell exposure by simulation of the lung situation. The cellular effects were then comprehensively characterized (cytotoxicology, transcriptomics, proteomics etc.) effects monitoring and put in context with the chemical and physical aerosol data. Emissions of wood combustion, a ship engine as well as diesel and gasoline engines were investigated. Furthermore for some experiments the atmospheric aging of the emission was simulated in a flow tube reactor using UV-light and ozone. Briefly the following order of cellular response-strength was observed: A relatively mild cellular effect is observed for the diluted wood combustion emissions, regardless if log-wood and pellet burner emissions are investigated. Similarly mild biological effects are observed for gasoline car emissions. The ship diesel engine emissions and construction machine diesel engine induced much more intense biological responses. A surprising result in this context is, that heavy fuel oil (HFO)-emissions show lower biological effect strengths than the supposedly cleaner diesel fuel emissions (DF). The HFO-emissions contain high concentrations of known toxicants (metals, polycyclic aromatics). This result was confirmed by experiments with murine macrophages

Aerosol composition and source apportionment in Santiago de Chile

International Nuclear Information System (INIS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-01-01

Santiago de Chile, Sao Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3 . Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10 ). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2 . In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of

Characterizing the Sources and Processing of Submicron Aerosols at a Coastal Site near Houston, TX, with a Specific Focus on the Impact of Regional Shipping Emissions

Science.gov (United States)

Schulze, B.; Wallace, H. W., IV; Bui, A.; Flynn, J. H., III; Erickson, M. H.; Griffin, R. J.

2017-12-01

The Texas Gulf Coast region historically has been influenced heavily by regional shipping emissions. However, the effects of the recent establishment of the North American Emissions Control Area (ECA) on aerosol properties in this region are presently unknown. In order to understand better the current sources and processing mechanisms influencing coastal aerosol near Houston, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed for three weeks at a coastal location during May-June 2016. Total mass loadings of organic and inorganic non-refractory aerosol components during onshore flow periods were similar to those published before establishment of the regulations. Using estimated methanesulfonic acid (MSA) mass loadings and published biogenic MSA:non-sea-salt-sulfate (nss-SO4) ratios, we determined that over 70% of nss-SO4 over the Gulf was from anthropogenic sources, predominantly shipping emissions. Mass spectral analysis indicated that for periods with similar backward-trajectory-averaged meteorological conditions, air masses influenced by shipping emissions have an increased mass fraction of ions related to carboxylic acids and a significantly larger oxygen-to-carbon (O:C) ratio than air masses that stay within the ECA boundary, suggesting that shipping emissions impact marine organic aerosol (OA) oxidation state. Amine fragment mass loadings were positively correlated with anthropogenic nss-SO4 during onshore flow, implying anthropogenic-biogenic interaction in marine OA production. Five OA factors were resolved by positive matrix factorization, corresponding to a hydrocarbon-like OA, a semi-volatile OA, and three different oxygenated organic aerosols ranked by their O:C ratio (OOA-1, OOA-2, and OOA-3). OOA-1 constituted the majority of OA mass during a period likely influenced by aqueous-phase processing and may be linked to local glyoxal/methylglyoxal-related sources. OOA-2 was produced within the Houston urban region and was

Secondary organic aerosol formation from biomass burning intermediates: phenol and methoxyphenols

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L. D. Yee

2013-08-01

Full Text Available The formation of secondary organic aerosol from oxidation of phenol, guaiacol (2-methoxyphenol, and syringol (2,6-dimethoxyphenol, major components of biomass burning, is described. Photooxidation experiments were conducted in the Caltech laboratory chambers under low-NOx (2O2 as the OH source. Secondary organic aerosol (SOA yields (ratio of mass of SOA formed to mass of primary organic reacted greater than 25% are observed. Aerosol growth is rapid and linear with the primary organic conversion, consistent with the formation of essentially non-volatile products. Gas- and aerosol-phase oxidation products from the guaiacol system provide insight into the chemical mechanisms responsible for SOA formation. Syringol SOA yields are lower than those of phenol and guaiacol, likely due to novel methoxy group chemistry that leads to early fragmentation in the gas-phase photooxidation. Atomic oxygen to carbon (O : C ratios calculated from high-resolution-time-of-flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS measurements of the SOA in all three systems are ~ 0.9, which represent among the highest such ratios achieved in laboratory chamber experiments and are similar to that of aged atmospheric organic aerosol. The global contribution of SOA from intermediate volatility and semivolatile organic compounds has been shown to be substantial (Pye and Seinfeld, 2010. An approach to representing SOA formation from biomass burning emissions in atmospheric models could involve one or more surrogate species for which aerosol formation under well-controlled conditions has been quantified. The present work provides data for such an approach.

Biological Particle Emissions From a South-East Asian Tropical Rainforest Using a Real- Time Dual Channel UV Fluorescence Bio-Aerosol Spectrometer

Science.gov (United States)

Gabey, A.; Coe, H.; Gallagher, M.; McFiggans, G.; Kaye, P.; Stanley, W.; Foot, V.

2008-12-01

Primary biogenic aerosols (PBA) contribute typically up to half of coarse mode particulate loading in tropical regions (e.g. Elbert et al. 2007). PBA contribute to the spread of genetic material and hence biodiversity within the biosphere either directly by transport of the organisms or their reproductive components. This spread via various vectors contributes to disease both animal and plant. Many studies have suggested PBA might be important for initiation of cloud formation and subsequent precipitation evolution by acting as cloud condensation nuclei (CCN) or possibly as ice nuclei (IN). This link is inferred from laboratory studies demonstrating the high activation efficiency of PBA at warm temperatures, coupled with observations that biological particles are ubiquitous in the atmosphere. Despite more than two hundred years of research, e.g. Ehrenberg (1830), information on the abundance, composition and more importantly the sources and heterogeneity of PBA on global scales are still poorly understood. The first realistic estimates of global average emission rates of PBA based on observations (mainly in Amazonia) and budget calculations, were provided by Elbert et al. (2007). They demonstrate that fungi, which have evolved many passive and active spore dispersal mechanisms, contribute a major fraction of the observed PBA and coarse particulate mass (particles with diameters between 1-10 μ m) in many, but in particular, tropical regions. Two major classes of fungal spores are commonly identified, these being AAM and ABM, Acomycota and Basidiomycota respectively (we will adopt the nomenclature used by Elbert et al. 2007, in this study). These species discharge their spores via wet spore active discharge mechanisms. Elbert et al. (2007) estimate a global average spore emission rate for ABM of ~17-50 Tg yr-1. This is consistent with observed typical concentrations of ABS which range from ~103 to 104 m- 3; and ~0.1-1 μ g m-3 by mass. The global average abundance

Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

OpenAIRE

Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

2014-01-01

Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as d...

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

Science.gov (United States)

Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

2015-12-01

The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi-volatile oxygenated OA (SV-OOA; 16 % of total OA; O / C = 0.63) and low volatility oxygenated OA (LV-OOA; 24 % of total OA; O / C = 0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a~previous wintertime campaign (winter 2010), most notably that PM1 concentrations were nearly three times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 to 12:00 PST. This is an indication that nighttime chemistry might also be

Global distribution and climate forcing of marine organic aerosol: 1. Model improvements and evaluation

Directory of Open Access Journals (Sweden)

N. Meskhidze

2011-11-01

Full Text Available Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR's Community Atmosphere Model (CAM5 with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7. Emissions of marine primary organic aerosols (POA, phytoplankton-produced isoprene- and monoterpenes-derived secondary organic aerosols (SOA and methane sulfonate (MS⁻ are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr⁻¹, for the Gantt et al. (2011 and Vignati et al. (2010 emission parameterizations, respectively. Marine sources of SOA and particulate MS⁻ (containing both sulfur and carbon atoms contribute an additional 0.2 and 5.1 Tg yr⁻¹, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ng m⁻³, with values up to 400 ng m⁻³ over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2, both Gantt et al. (2011 and Vignati et al. (2010 formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011 parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN. The largest increases (up to 20% in CCN (at a supersaturation (S of 0.2% number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming

Regional modeling of carbonaceous aerosols over Europe-focus on secondary organic aerosols

International Nuclear Information System (INIS)

Bessagnet, B.; Menut, L.; Curci, G.; Hodzic, A.; Guillaume, B.; Liousse, C.; Moukhtar, S.; Pun, B.; Seigneur, C.; Schulz, M.

2008-01-01

In this study, an improved and complete secondary organic aerosols (SOA) chemistry scheme was implemented in the CHIMERE model. The implementation of isoprene chemistry for SOA significantly improves agreement between long series of simulated and observed particulate matter concentrations. While simulated organic carbon concentrations are clearly improved at elevated sites by adding the SOA scheme, time correlation are impaired at low level sites in Portugal, Italy and Slovakia. At several sites a clear underestimation by the CHIMERE model is noticed in wintertime possibly due to missing wood burning emissions as shown in previous modeling studies. In Europe, the CHIMERE model gives yearly average SOA concentrations ranging from 0.5 μg m -3 in the Northern Europe to 4 μg m -3 over forested regions in Spain, France, Germany and Italy. In addition, our work suggests that during the highest fire emission periods, fires can be the dominant source of primary organic carbon over the Mediterranean Basin, but the SOA contribution from fire emissions is low. Isoprene chemistry has a strong impact on SOA formation when using current available kinetic schemes. (authors)

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris during the MEGAPOLI summer and winter campaigns

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C. Fountoukis

2016-03-01

Full Text Available We use a three-dimensional regional chemical transport model (PMCAMx with high grid resolution and high-resolution emissions (4 × 4 km2 over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009 and a winter (January/February 2010 period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 % of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA concentrations is also encouraging (mean bias = 0.1 µg m−3 during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m−3 mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d−1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00–14:00 LT and 20 % during dinner time (20:00–22:00 LT. Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias =  −2.3 µg m−3 pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

Science.gov (United States)

Fountoukis, Christos; Megaritis, Athanasios G.; Skyllakou, Ksakousti; Charalampidis, Panagiotis E.; Denier van der Gon, Hugo A. C.; Crippa, Monica; Prévôt, André S. H.; Fachinger, Friederike; Wiedensohler, Alfred; Pilinis, Christodoulos; Pandis, Spyros N.

2016-03-01

We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 × 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 µg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 µg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Aerosol emissions factors from traditional biomass cookstoves in India: insights from field measurements

Directory of Open Access Journals (Sweden)

A. Pandey

2017-11-01

Full Text Available Residential solid biomass cookstoves are important sources of aerosol emissions in India. Cookstove emissions rates are largely based on laboratory experiments conducted using the standard water-boiling test, but real-world emissions are often higher owing to different stove designs, fuels, and cooking methods. Constraining mass emissions factors (EFs for prevalent cookstoves is important because they serve as inputs to bottom-up emissions inventories used to evaluate health and climate impacts. Real-world EFs were measured during winter 2015 for a traditional cookstove (chulha burning fuel wood, agricultural residue, and dung from different regions of India. Average (±95 % confidence interval EFs for fuel wood, agricultural residue, and dung were (1 PM2.5 mass: 10.5 (7.7–13.4 g kg−1, 11.1 (7.7–15.5 g kg−1, and 22.6 (14.9–32.9 g kg−1, respectively; (2 elemental carbon (EC: 0.9 (0.6–1.4 g kg−1, 1.6 (0.6–3.0 g kg−1, and 1.0 (0.4–2.0 g kg−1, respectively; and (3 organic carbon (OC: 4.9 (3.2–7.1 g kg−1, 7.0 (3.5–12.5 g kg−1, and 12.9 (4.2–15.01 g kg−1, respectively. The mean (±95 % confidence interval OC ∕ EC mass ratios were 6.5 (4.5–9.1, 7.6 (4.4–12.2, and 12.7 (6.5–23.3, respectively, with OC and EC quantified by the IMPROVE_A thermal-optical reflectance protocol. These real-world EFs are higher than those from previous laboratory-based measurements. Combustion conditions have larger effects on EFs than the fuel types. We also report the carbon mass fractions of our aerosol samples determined using the thermal-optical reflectance method. The mass fraction profiles are consistent between the three fuel categories but markedly different from those reported in past literature – including the source profiles for wood stove PM2.5 emissions developed as inputs to receptor modeling studies conducted by the Central Pollution Control Board of India. Thermally

Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber

Science.gov (United States)

C. J. Hennigan; M. A. Miracolo; G. J. Engelhart; A. A. May; A. A. Presto; T. Lee; A. P. Sullivan; G. R. McMeeking; H. Coe; C. E. Wold; W.-M. Hao; J. B. Gilman; W. C. Kuster; J. de Gouw; B. A. Schichtel; J. L. Collett; S. M. Kreidenweis; A. L. Robinson

2011-01-01

Smog chamber experiments were conducted to investigate the chemical and physical transformations of organic aerosol (OA) during photo-oxidation of open biomass burning emissions. The experiments were carried out at the US Forest Service Fire Science Laboratory as part of the third Fire Lab at Missoula Experiment (FLAME III). We investigated emissions from 12 different...

Investigating smoke's influence on primary production throughout the Amazon

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Flanner, M. G.; Mahowald, N. M.; Zender, C. S.; Randerson, J. T.; Tosca, M. G.

2007-12-01

Smoke from annual burning in the Amazon causes large reduction in surface insolation and increases the diffuse fraction of photosynthetically-active radiation (PAR). These effects have competing influence on gross primary production (GPP). Recent studies indicate that the sign of net influence depends on aerosol optical depth, but the magnitude of smoke's effect on continental-scale carbon cycling is very poorly constrained and may constitute an important term of fire's net impact on carbon storage. To investigate widespread effects of Amazon smoke on surface radiation properties, we apply a version of the NCAR Community Atmosphere Model with prognostic aerosol transport, driven with re-analysis winds. Carbon aerosol emissions are derived from the Global Fire Emissions Database (GFED). We use AERONET observations to identify model biases in aerosol optical depth, single-scatter albedo, and surface radiative forcing, and prescribe new aerosol optical properties based on field observations to improve model agreement with AERONET data. Finally, we quantify a potential range of smoke-induced change in large-scale GPP based on: 1) ground measurements of GPP in the Amazon as a function of aerosol optical depth and diffuse fraction of PAR, and 2) empirical functions of ecosystem-scale photosynthesis rates currently employed in models such as the Community Land Model (CLM).

Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

Science.gov (United States)

Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

2014-09-15

aerosol factor (AMS_PMF_COA) to oxidized organic aerosol, chloride and locally produced nitrate, indicating that AMS_PMF_COA cannot be attributed to primary cooking emissions only. Overall, there are clear benefits from factor analysis applied to results obtained from multiple techniques, which allows better association of aerosols with sources and atmospheric processes. Copyright © 2014 Elsevier B.V. All rights reserved.

In-situ studies on volatile jet exhaust particle emissions - impacts of fuel sulfur content and environmental conditions on nuclei-mode aerosols

Energy Technology Data Exchange (ETDEWEB)

Schroeder, F.; Baumann, R.; Petzold, A.; Busen, R.; Schulte, P.; Fiebig, M. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Brock, C.A. [Denver Univ., CO (United States). Dept. of Engineering

2000-02-01

In-situ measurements of ultrafine aerosol particle emissions were performed at cruise altitudes behind the DLR ATTAS research jet (RR M45H M501 engines) and a B737-300 aircraft (CFM56-3B1 engines). Measurements were made 0.15-20 seconds after emission as the source aircraft burned fuel with sulfur contents (FSC) of 2.6, 56 or 118 mg kg{sup -1}. Particle size distributions of from 3 to 60 nm diameter were determined using CN-counters with varying lower size detection limits. Volatile particle concentrations in the aircraft plumes strongly increased as diameter decreased toward the sizes of large molecular clusters, illustrating that apparent particle emissions are extremely sensitive to the smallest particle size detectable by the instrument used. Environmental conditions and plume age alone could influence the number of detected ultrafine (volatile) aerosols within an order of magnitude, as well. The observed volatile particle emissions decreased nonlinearly as FSC decreased to 60 mg kg{sup -1}, reaching minimum values of about 2 x 10{sup 17} kg{sup -1} and 2 x 10{sup 16} kg{sup -1} for particles >3 nm and >5 nm, respectively. Volatile particle emissions did not change significantly as FSCs were further reduced below 60 mg kg{sup -1}. Volatile particle emissions did not differ significantly between the two studied engine types. In contrast, soot particle emissions from the modern CFM56-3B1 engines were 4-5 times less (4 x 10{sup 14} kg{sup -1}) than from the older RR M45H M501 engines (1.8 x 10{sup 15} kg{sup -1}). Contrail processing has been identified as an efficient sink/quenching parameter for ultrafine particles and reduces the remaining interstitial aerosol by factors 2-10 depending on particle size.

Emission and chemistry of organic carbon in the gas and aerosol phase at a sub-urban site near Mexico City in March 2006 during the MILAGRO study

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J. A. de Gouw

2009-05-01

Full Text Available Volatile organic compounds (VOCs and carbonaceous aerosol were measured at a sub-urban site near Mexico City in March of 2006 during the MILAGRO study (Megacity Initiative: Local and Global Research Objectives. Diurnal variations of hydrocarbons, elemental carbon (EC and hydrocarbon-like organic aerosol (HOA were dominated by a high peak in the early morning when local emissions accumulated in a shallow boundary layer, and a minimum in the afternoon when the emissions were diluted in a significantly expanded boundary layer and, in case of the reactive gases, removed by OH. In comparison, diurnal variations of species with secondary sources such as the aldehydes, ketones, oxygenated organic aerosol (OOA and water-soluble organic carbon (WSOC stayed relatively high in the afternoon indicating strong photochemical formation. Emission ratios of many hydrocarbon species relative to CO were higher in Mexico City than in the U.S., but we found similar emission ratios for most oxygenated VOCs and organic aerosol. Secondary formation of acetone may be more efficient in Mexico City than in the U.S., due to higher emissions of alkane precursors from the use of liquefied petroleum gas. Secondary formation of organic aerosol was similar between Mexico City and the U.S. Combining the data for all measured gas and aerosol species, we describe the budget of total observed organic carbon (TOOC, and find that the enhancement ratio of TOOC relative to CO is conserved between the early morning and mid afternoon despite large compositional changes. Finally, the influence of biomass burning is investigated using the measurements of acetonitrile, which was found to correlate with levoglucosan in the particle phase. Diurnal variations of acetonitrile indicate a contribution from local burning sources. Scatter plots of acetonitrile versus CO suggest that the contribution of biomass burning to the enhancement of most gas and aerosol species was not dominant and perhaps

Emission and Chemistry of Organic Carbon in the Gas and Aerosol Phase at a Sub-Urban Site Near Mexico City in March 2006 During the MILAGRO Study

Energy Technology Data Exchange (ETDEWEB)

de Gouw, Joost A.; Welsh-Bon, Daniel; Warneke, Carsten; Kuster, W. C.; Alexander, M. L.; Baker, Angela K.; Beyersdorf, Andreas J.; Blake, D. R.; Canagaratna, Manjula R.; Celada, A. T.; Huey, L. G.; Junkermann, W.; Onasch, Timothy B.; Salcido, A.; Sjostedt, S. J.; Sullivan, Amy; Tanner, David J.; Vargas-Ortiz, Leroy; Weber, R. J.; Worsnop, Douglas R.; Yu, Xiao-Ying; Zaveri, Rahul A.

2009-05-28

Volatile organic compounds (VOCs) and carbonaceous aerosol were measured at a sub-urban site near Mexico City in March of 2006 during the MILAGRO study (Megacity Initiative: Local and Global Research Objectives). Diurnal variations of hydrocarbons, elemental carbon (EC) and hydrocarbon-like organic aerosol (HOA) were dominated by a high peak in the early morning when local emissions accumulated in a shallow boundary layer, and a minimum in the afternoon when the emissions were diluted in a significantly expanded boundary layer and, in case of the reactive gases, removed by OH. In comparison, diurnal variations of species with secondary sources such as the aldehydes, ketones, oxygenated organic aerosol (OOA) and water-soluble organic carbon (WSOC) stayed relatively high in the afternoon indicating strong photochemical formation. Emission ratios of many hydrocarbon species relative to CO were higher in Mexico City than in the U.S., but we found similar emission ratios for most oxygenated VOCs and organic aerosol. Secondary formation of acetone may be more efficient in Mexico City than in the U.S., due to higher emissions of alkane precursors from the use of liquefied petroleum gas. Secondary formation of organic aerosol was similar between Mexico City and the U.S. Combining the data for all measured gas and aerosol species, we describe the budget of total observed organic carbon (TOOC), and find that the enhancement ratio of TOOC relative to CO is conserved between the early morning and mid afternoon despite large compositional changes. Finally, the influence of biomass burning is investigated using the measurements of acetonitrile, which was found to correlate with levoglucosan in the particle phase. Diurnal variations of acetonitrile indicate a contribution from local burning sources. Scatter plots of acetonitrile versus CO suggest that the contribution of biomass burning to the enhancement of most gas and aerosol species was not dominant and perhaps not dissimilar

Wintertime aerosol chemical composition and source apportionment of the organic fraction in the metropolitan area of Paris

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M. Crippa

2013-01-01

Full Text Available The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30–36% and nitrate (28–29%, with lower contributions from sulfate (14–16%, ammonium (12–14% and black carbon (7–13%.

Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11–15% of organic mass, biomass burning (13–15% and cooking (up to 35% during meal hours. Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings.

Effect of Pellet Boiler Exhaust on Secondary Organic Aerosol Formation from α-Pinene.

Science.gov (United States)

Kari, Eetu; Hao, Liqing; Yli-Pirilä, Pasi; Leskinen, Ari; Kortelainen, Miika; Grigonyte, Julija; Worsnop, Douglas R; Jokiniemi, Jorma; Sippula, Olli; Faiola, Celia L; Virtanen, Annele

2017-02-07

Interactions between anthropogenic and biogenic emissions, and implications for aerosol production, have raised particular scientific interest. Despite active research in this area, real anthropogenic emission sources have not been exploited for anthropogenic-biogenic interaction studies until now. This work examines these interactions using α-pinene and pellet boiler emissions as a model test system. The impact of pellet boiler emissions on secondary organic aerosol (SOA) formation from α-pinene photo-oxidation was studied under atmospherically relevant conditions in an environmental chamber. The aim of this study was to identify which of the major pellet exhaust components (including high nitrogen oxide (NO x ), primary particles, or a combination of the two) affected SOA formation from α-pinene. Results demonstrated that high NO x concentrations emitted by the pellet boiler reduced SOA yields from α-pinene, whereas the chemical properties of the primary particles emitted by the pellet boiler had no effect on observed SOA yields. The maximum SOA yield of α-pinene in the presence of pellet boiler exhaust (under high-NO x conditions) was 18.7% and in the absence of pellet boiler exhaust (under low-NO x conditions) was 34.1%. The reduced SOA yield under high-NO x conditions was caused by changes in gas-phase chemistry that led to the formation of organonitrate compounds.

Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

Science.gov (United States)

Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

2014-12-01

Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photo-oxidation under a range of controlled conditions (relative humidity or RH ~65-89%, volatile organic compound-to-NOx or VOC / NOx ~3-9 and NOx ~2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene but low isoprene emitter, and its emissions were observed to produce measurable amounts of secondary organic aerosol (SOA) via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e. in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photo-oxidation products of the minor volatile organic compounds (VOCs) co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally isoprene-emitting landscapes in Southeast

Toward a minimal representation of aerosols in climate models: description and evaluation in the Community Atmosphere Model CAM5

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X. Liu

2012-05-01

Full Text Available A modal aerosol module (MAM has been developed for the Community Atmosphere Model version 5 (CAM5, the atmospheric component of the Community Earth System Model version 1 (CESM1. MAM is capable of simulating the aerosol size distribution and both internal and external mixing between aerosol components, treating numerous complicated aerosol processes and aerosol physical, chemical and optical properties in a physically-based manner. Two MAM versions were developed: a more complete version with seven lognormal modes (MAM7, and a version with three lognormal modes (MAM3 for the purpose of long-term (decades to centuries simulations. In this paper a description and evaluation of the aerosol module and its two representations are provided. Sensitivity of the aerosol lifecycle to simplifications in the representation of aerosol is discussed.

Simulated sulfate and secondary organic aerosol (SOA mass concentrations are remarkably similar between MAM3 and MAM7. Differences in primary organic matter (POM and black carbon (BC concentrations between MAM3 and MAM7 are also small (mostly within 10%. The mineral dust global burden differs by 10% and sea salt burden by 30–40% between MAM3 and MAM7, mainly due to the different size ranges for dust and sea salt modes and different standard deviations of the log-normal size distribution for sea salt modes between MAM3 and MAM7. The model is able to qualitatively capture the observed geographical and temporal variations of aerosol mass and number concentrations, size distributions, and aerosol optical properties. However, there are noticeable biases; e.g., simulated BC concentrations are significantly lower than measurements in the Arctic. There is a low bias in modeled aerosol optical depth on the global scale, especially in the developing countries. These biases in aerosol simulations clearly indicate the need for improvements of aerosol processes (e.g., emission fluxes of anthropogenic aerosols and

The economics and ethics of aerosol geoengineering strategies

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Goes, Marlos; Keller, Klaus; Tuana, Nancy

2010-05-01

Anthropogenic greenhouse gas emissions are changing the Earth's climate and impose substantial risks for current and future generations. What are scientifically sound, economically viable, and ethically defendable strategies to manage these climate risks? Ratified international agreements call for a reduction of greenhouse gas emissions to avoid dangerous anthropogenic interference with the climate system. Recent proposals, however, call for a different approach: geoengineering climate by injecting aerosol precursors into the stratosphere. Published economic studies typically neglect the risks of aerosol geoengineering due to (i) a potential failure to sustain the aerosol forcing and (ii) due to potential negative impacts associated with aerosol forcings. Here we use a simple integrated assessment model of climate change to analyze potential economic impacts of aerosol geoengineering strategies over a wide range of uncertain parameters such as climate sensitivity, the economic damages due to climate change, and the economic damages due to aerosol geoengineering forcings. The simplicity of the model provides the advantages of parsimony and transparency, but it also imposes considerable caveats. For example, the analysis is based on a globally aggregated model and is hence silent on intragenerational distribution of costs and benefits. In addition, the analysis neglects the effects of future learning and is based on a simple representation of climate change impacts. We use this integrated assessment model to show three main points. First, substituting aerosol geoengineering for the reduction of greenhouse gas emissions can fail the test of economic efficiency. One key to this finding is that a failure to sustain the aerosol forcing can lead to sizeable and abrupt climatic changes. The monetary damages due to such a discontinuous aerosol geoengineering can dominate the cost-benefit analysis because the monetary damages of climate change are expected to increase with

Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

Science.gov (United States)

Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

2008-12-01

The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

Secondary inorganic aerosols in Europe: sources and the significant influence of biogenic VOC emissions, especially on ammonium nitrate

Science.gov (United States)

Aksoyoglu, Sebnem; Ciarelli, Giancarlo; El-Haddad, Imad; Baltensperger, Urs; Prévôt, André S. H.

2017-06-01

Contributions of various anthropogenic sources to the secondary inorganic aerosol (SIA) in Europe as well as the role of biogenic emissions on SIA formation were investigated using the three-dimensional regional model CAMx (comprehensive air quality model with extensions). Simulations were carried out for two periods of EMEP field campaigns, February-March 2009 and June 2006, which are representative of cold and warm seasons, respectively. Biogenic volatile organic compounds (BVOCs) are known mainly as precursors of ozone and secondary organic aerosol (SOA), but their role on inorganic aerosol formation has not attracted much attention so far. In this study, we showed the importance of the chemical reactions of BVOCs and how they affect the oxidant concentrations, leading to significant changes, especially in the formation of ammonium nitrate. A sensitivity test with doubled BVOC emissions in Europe during the warm season showed a large increase in secondary organic aerosol (SOA) concentrations (by about a factor of two), while particulate inorganic nitrate concentrations decreased by up to 35 %, leading to a better agreement between the model results and measurements. Sulfate concentrations decreased as well; the change, however, was smaller. The changes in inorganic nitrate and sulfate concentrations occurred at different locations in Europe, indicating the importance of precursor gases and biogenic emission types for the negative correlation between BVOCs and SIA. Further analysis of the data suggested that reactions of the additional terpenes with nitrate radicals at night were responsible for the decline in inorganic nitrate formation, whereas oxidation of BVOCs with OH radicals led to a decrease in sulfate. Source apportionment results suggest that the main anthropogenic source of precursors leading to formation of particulate inorganic nitrate is road transport (SNAP7; see Table 1 for a description of the categories), whereas combustion in energy and

Laboratory and field measurements of organic aerosols with the photoionization aerosol mass spectrometer

Science.gov (United States)

Dreyfus, Matthew A.

. The high-time resolution data shows that rapid concentration changes of a common individual species can be lost with traditional bulk sampling, and a time resolution of 30 minutes is suggested to accurately represent these changes. Using the mass spectra collected from the extended sampling campaign, source apportionment was performed with positive matrix factorization (PMF). The resulting model features six factors either correlated to specific sources (meat cooking, car emissions/road dust, diesel exhaust) or types of compounds (phthalates, alkanes/alkanoic acids, PAHs). The high-time resolution data allowed for the observation of specific trends in each factor's behavior as a function of time and wind direction relative to the receptor site. Elemental carbon/organic carbon (EC/OC) data is used to calculate the percentages of primary and secondary organic aerosol. Primary organic aerosol (POA) constituted the vast majority of the total carbon at 91% (an average of 2.8 +/- 1.1mug/m 3); 30% of which came from combustion, and 70% from non-combustion sources. These results can be explained by the PIAMS data: the diesel factor contributes to the combustion-related POA; the car/road dust, meat cooking, and alkane/alkanoic acid factors contribute the majority of non-combustion POA. The remaining factors represent products from the ozonolysis of various monoterpenes. The product ion peaks observed indicates that both the stabilized Criegee intermediate pathway and the hydroperoxide channel are both active pathways in yielding dimers and high-order oligomer.

Particulate emissions from a mid-latitude prescribed chaparral fire

Science.gov (United States)

Cofer, Wesley R., III; Levine, Joel S.; Sebacher, Daniel I.; Winstead, Edward L.; Riggin, Philip J.; Brass, James A.; Ambrosia, Vincent G.

1988-01-01

Particulate emission from a 400-acre prescribed chaparral fire in the San Dimas Experimental Forest was investigated by collecting smoke aerosol on Teflon and glass-fiber filters from a helicopter, and using SEM and EDAX to study the features of the particles. Aerosol particles ranged in size from about 0.1 to 100 microns, with carbon, oxygen, magnesium, aluminum, silicon, calcium, and iron as the primary elements. The results of ion chromatographic analysis of aerosol-particle extracts (in water-methanol) revealed the presence of significant levels of NO2(-), NO3(-), SO4(2-), Cl(-), PO4(3-), C2O4(2-), Na(+), NH4(+), and K(+). The soluble ionic portion of the aerosol was estimated to be about 2 percent by weight.

Effect of selective catalytic reduction (SCR) on fine particle emission from two coal-fired power plants in China

Science.gov (United States)

Li, Zhen; Jiang, Jingkun; Ma, Zizhen; Wang, Shuxiao; Duan, Lei

2015-11-01

Nitrogen oxides (NOx) emission abatement of coal-fired power plants (CFPPs) requires large-scaled installation of selective catalytic reduction (SCR), which would reduce secondary fine particulate matter (PM2.5) (by reducing nitrate aerosol) in the atmosphere. However, our field measurement of two CFPPs equipped with SCR indicates a significant increase of SO42- and NH4+ emission in primary PM2.5, due to catalytic enhancement of SO2 oxidation to SO3 and introducing of NH3 as reducing agent. The subsequent formation of (NH4)2SO4 or NH4HSO4 aerosol is commonly concentrated in sub-micrometer particulate matter (PM1) with a bimodal pattern. The measurement at the inlet of stack also showed doubled primary PM2.5 emission by SCR operation. This effect should therefore be considered when updating emission inventory of CFPPs. By rough estimation, the enhanced primary PM2.5 emission from CFPPs by SCR operation would offset 12% of the ambient PM2.5 concentration reduction in cities as the benefit of national NOx emission abatement, which should draw attention of policy-makers for air pollution control.

Factors Affecting Aerosol Radiative Forcing from Both Production-based and Consumption-based View

Science.gov (United States)

Wang, J.; Lin, J.; Ni, R.

2017-12-01

Aerosol radiative forcing (RF) is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. This problem becomes more complicated when taking into account the role of international trade, which means reallocated aerosol RF due to separation of regions producing goods and emissions and regions consuming those goods. Here we analyze major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA) and black carbon (BC), extending the work of Lin et al. (2016, Nature Geoscience). We contrast five factors determining production-based (RFp, due to a region's production of goods) and consumption-based (RFc, due to a region's consumption) forcing by 11 major regions, including population size, per capita output, emission intensity (emission per output), chemical efficiency (mass per unit emission) and radiative efficiency (RF per unit mass). Comparing across the 11 regions, East Asia produces the strongest RFp and RFc of SIOA and BC and the second largest RFp and RFc of POA primarily due to its high emission intensity. Although Middle East and North Africa has low emissions, its RFp is strengthened by its largest chemical efficiency for POA and BC and second largest chemical efficiency for SIOA. However, RFp of South-East Asia and Pacific is greatly weakened by its lowest chemical efficiency. Economic trade means that net importers (Western Europe, North America and Pacific OECD) have higher RFc than RFp by 50-100%. And such forcing difference is mainly due to the high emission intensity of the exporters supplying these regions. For North America, SIOA's RFc is 50% stronger than RFp, for that emission intensity of SIOA is 5.2 times in East Asia and 2.5 times in Latin America and Caribbean compared with that in North America, and the chemical efficiency in the top four exporters are

Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the volatility-basis-set approach within the CHIMERE model

Directory of Open Access Journals (Sweden)

Q. J. Zhang

2013-06-01

Full Text Available Simulations with the chemistry transport model CHIMERE are compared to measurements performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation summer campaign in the Greater Paris region in July 2009. The volatility-basis-set approach (VBS is implemented into this model, taking into account the volatility of primary organic aerosol (POA and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations with a modified treatment of POA volatility and modified secondary organic aerosol (SOA formation schemes. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated, and four pollution regimes are defined according to the air mass origin. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC shows the best correlation with measurements. High-concentration events observed mostly after long-range transport are well reproduced by the model. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization, to emission input data, and to simulated OH levels can be responsible for

Characterization of carbonaceous aerosol emissions from selected combustion sources

International Nuclear Information System (INIS)

Martinez, J.P.G.; Espino, M.P.M.; Pabroa, P.C.B.; Bautista, A.T. VII

2015-01-01

Carbonaceous Particulates are carbon-containing solid or liquid matter which form a significant portion of the fine particulate mass (PM2.5) and these have known profound adverse effects on health, climate and visibility. This study aims to characterize carbonaceous aerosol emissions from different combustion sources to establish fingerprints for these for use in the refinement of improvement of the resolution of sources apportionment studies being done by the Philippine Nuclear Research Institute (PNRI), i.e. to resolve vehicular emission sources. Fine air particulate sample were collected in pre-baked Quartz filters using an improvised collection set-up with a Gent sampler. Concentrations of organic and elemental carbon (OC and EC, respectively) in PM2.5 were measured for the different combustion sources—vehicular emissions, tire pyrolysis, and biomass burning, using a thermal-optical method of analysis following the IMPROVE_A protocol. Measured OC ad EC concentrations are shown as percentages with respect to the total carbon (TC) and are illustrated in a 100% stacked chart. Predominance of the EC2 fraction is exhibited in both the diesel fuelled vehicle and tire pyrolysis emissions with EC2/OC2 ratio distinguishing one from the other, EC2/OC2 is 1.63 and 8.41, respectively. Predominance of either OC2 or OC3 fraction is shown in the unleaded gasoline and LPG Fuelled vehicles and in biomass burning with the OC2/OC3 ratio distinguishing one from the others. OC2/OC3 ratios are 1.33 for unleaded gasoline fuelled vehicle, 1.89 for LPG-fuelled vehicle, 0.55 for biomass burning (leaves) and 0.82 biomass burning (wood). The study has shown probable use of the EC2/OC2 and OC2/OC3 ratios to distinguish fingerprints for combustion sources covered in this study. (author)

Light absorption of biomass burning and vehicle emission-sourced carbonaceous aerosols of the Tibetan Plateau.

Science.gov (United States)

Hu, Zhaofu; Kang, Shichang; Li, Chaoliu; Yan, Fangping; Chen, Pengfei; Gao, Shaopeng; Wang, Zhiyong; Zhang, Yulan; Sillanpää, Mika

2017-06-01

Carbonaceous aerosols over the Tibetan Plateau originate primarily from biomass burning and vehicle emissions (BB and VEs, respectively). The light absorption characteristics of these carbonaceous aerosols are closely correlated with the burning conditions and represent key factors that influence climate forcing. In this study, the light absorption characteristics of elemental carbon (EC) and water-soluble organic carbon (WSOC) in PM 2.5 (fine particulate matter smaller than 2.5 μm) generated from BB and VEs were investigated over the Tibetan Plateau (TP). The results showed that the organic carbon (OC)/EC ratios from BB- and VE-sourced PM 2.5 were 17.62 ± 10.19 and 1.19 ± 0.36, respectively. These values were higher than the ratios in other regions, which was primarily because of the diminished amount of oxygen over the TP. The mass absorption cross section of EC (MAC EC ) at 632 nm for the BB-sourced PM 2.5 (6.10 ± 1.21 m 2 .g -1 ) was lower than that of the VE-sourced PM 2.5 (8.10 ± 0.98 m 2 .g -1 ), indicating that the EC content of the BB-sourced PM 2.5 was overestimated because of the high OC/EC ratio. The respective absorption per mass (α/ρ) values at 365 nm for the VE- and BB-sourced PM 2.5 were 0.71 ± 0.17 m 2 .g -1 and 0.91 ± 0.18 m 2 .g -1 . The α/ρ value of the VEs was loaded between that of gasoline and diesel emissions, indicating that the VE-sourced PM 2.5 originated from both types of emissions. Because OC and WSOC accounts for most of the carbonaceous aerosols at remote area of the TP, the radiative forcing contributed by the WSOC should be high, and requires further investigation.

Aerosol Optical Properties and Trace Gas Emissions From Laboratory-Simulated Western US Wildfires

Science.gov (United States)

Selimovic, V.; Yokelson, R. J.; Warneke, C.; Roberts, J. M.; De Gouw, J. A.; Reardon, J.; Griffith, D. W. T.

2017-12-01

Western wildfires have a major impact on air quality in the US. In the fall of 2016, 107 fires were burned in the large-scale combustion facility at the US Forest Service Missoula Fire Sciences Laboratory as part of the Fire Influence on Regional and Global Environments Experiment (FIREX). Canopy, litter, duff, dead wood, and other fuels from various widespread coniferous and chaparral ecosystems were burned in combinations to represent relevant configurations in the field and as pure components to investigate the effects of individual fuels. The smoke emissions were characterized by a large suite of state-of-the-art instruments. In this study we report emission factor (EF, g compound emitted per kg fuel burned) measurements in fresh smoke of a diverse suite of critically-important trace gases measured by open-path Fourier transform infrared spectroscopy (OP-FTIR). We also report aerosol optical properties (absorption EF, single scattering albedo (SSA) and Ångström absorption exponent (AAE)) as well as black carbon (BC) EF measured by photoacoustic extinctiometers (PAX) at 870 and 401 nm. A careful comparison with available field measurements of wildfires confirms that representative data can be extracted from the lab fire data. The OP-FTIR data show that ammonia (1.65 g kg-1), acetic acid (2.44 g kg-1), and other trace gases are significant emissions not previously measured for US wildfires. The PAX measurements show that brown carbon (BrC) absorption is most dominant for combustion of duff (AAE 7.13) and rotten wood (AAE 4.60): fuels that are consumed in greater amounts during wildfires than prescribed fires. We confirm that about 86% of the aerosol absorption at 401 nm in typical fresh wildfire smoke is due to BrC.

Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

Science.gov (United States)

Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

2017-06-01

A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S

The economics (or lack thereof) of aerosol geoengineering

Science.gov (United States)

Goes, M.; Keller, K.; Tuana, N.

2009-04-01

Anthropogenic greenhouse gas emissions are changing the Earth's climate and impose substantial risks for current and future generations. What are scientifically sound, economically viable, and ethically defendable strategies to manage these climate risks? Ratified international agreements call for a reduction of greenhouse gas emissions to avoid dangerous anthropogenic interference with the climate system. Recent proposals, however, call for the deployment of a different approach: to geoengineer climate by injecting aerosol precursors into the stratosphere. Published economic studies typically suggest that substituting aerosol geoengineering for abatement of carbon dioxide emissions results in large net monetary benefits. However, these studies neglect the risks of aerosol geoengineering due to (i) the potential for future geoengineering failures and (ii) the negative impacts associated with the aerosol forcing. Here we use a simple integrated assessment model of climate change to analyze potential economic impacts of aerosol geoengineering strategies over a wide range of uncertain parameters such as climate sensitivity, the economic damages due to climate change, and the economic damages due to aerosol geoengineering forcing. The simplicity of the model provides the advantages of parsimony and transparency, but it also imposes severe caveats on the interpretation of the results. For example, the analysis is based on a globally aggregated model and is hence silent on the question of intragenerational distribution of costs and benefits. In addition, the analysis neglects the effects of endogenous learning about the climate system. We show that the risks associated with a future geoengineering failure and negative impacts of aerosol forcings can cause geoenginering strategies to fail an economic cost-benefit test. One key to this finding is that a geoengineering failure would lead to dramatic and abrupt climatic changes. The monetary damages due to this failure can

Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics

Science.gov (United States)

Alanen, Jenni; Simonen, Pauli; Saarikoski, Sanna; Timonen, Hilkka; Kangasniemi, Oskari; Saukko, Erkka; Hillamo, Risto; Lehtoranta, Kati; Murtonen, Timo; Vesala, Hannu; Keskinen, Jorma; Rönkkö, Topi

2017-07-01

Natural gas usage in the traffic and energy production sectors is a growing trend worldwide; thus, an assessment of its effects on air quality, human health and climate is required. Engine exhaust is a source of primary particulate emissions and secondary aerosol precursors, which both contribute to air quality and can cause adverse health effects. Technologies, such as cleaner engines or fuels, that produce less primary and secondary aerosols could potentially significantly decrease atmospheric particle concentrations and their adverse effects. In this study, we used a potential aerosol mass (PAM) chamber to investigate the secondary aerosol formation potential of natural gas engine exhaust. The PAM chamber was used with a constant UV-light voltage, which resulted in relatively long equivalent atmospheric ages of 11 days at most. The studied retro-fitted natural gas engine exhaust was observed to form secondary aerosol. The mass of the total aged particles, i.e., particle mass measured downstream of the PAM chamber, was 6-268 times as high as the mass of the emitted primary exhaust particles. The secondary organic aerosol (SOA) formation potential was measured to be 9-20 mg kgfuel-1. The total aged particles mainly consisted of organic matter, nitrate, sulfate and ammonium, with the fractions depending on exhaust after-treatment and the engine parameters used. Also, the volatility, composition and concentration of the total aged particles were found to depend on the engine operating mode, catalyst temperature and catalyst type. For example, a high catalyst temperature promoted the formation of sulfate particles, whereas a low catalyst temperature promoted nitrate formation. However, in particular, the concentration of nitrate needed a long time to stabilize - more than half an hour - which complicated the conclusions but also indicates the sensitivity of nitrate measurements on experimental parameters such as emission source and system temperatures. Sulfate was

Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics

Directory of Open Access Journals (Sweden)

J. Alanen

2017-07-01

Full Text Available Natural gas usage in the traffic and energy production sectors is a growing trend worldwide; thus, an assessment of its effects on air quality, human health and climate is required. Engine exhaust is a source of primary particulate emissions and secondary aerosol precursors, which both contribute to air quality and can cause adverse health effects. Technologies, such as cleaner engines or fuels, that produce less primary and secondary aerosols could potentially significantly decrease atmospheric particle concentrations and their adverse effects. In this study, we used a potential aerosol mass (PAM chamber to investigate the secondary aerosol formation potential of natural gas engine exhaust. The PAM chamber was used with a constant UV-light voltage, which resulted in relatively long equivalent atmospheric ages of 11 days at most. The studied retro-fitted natural gas engine exhaust was observed to form secondary aerosol. The mass of the total aged particles, i.e., particle mass measured downstream of the PAM chamber, was 6–268 times as high as the mass of the emitted primary exhaust particles. The secondary organic aerosol (SOA formation potential was measured to be 9–20 mg kgfuel−1. The total aged particles mainly consisted of organic matter, nitrate, sulfate and ammonium, with the fractions depending on exhaust after-treatment and the engine parameters used. Also, the volatility, composition and concentration of the total aged particles were found to depend on the engine operating mode, catalyst temperature and catalyst type. For example, a high catalyst temperature promoted the formation of sulfate particles, whereas a low catalyst temperature promoted nitrate formation. However, in particular, the concentration of nitrate needed a long time to stabilize – more than half an hour – which complicated the conclusions but also indicates the sensitivity of nitrate measurements on experimental parameters such as emission

Formation of the natural sulfate aerosol

Energy Technology Data Exchange (ETDEWEB)

Kerminen, V M; Hillamo, R; Maekinen, M; Virkkula, A; Maekelae, T; Pakkanen, T [Helsinki Univ. (Finland). Dept. of Physics

1997-12-31

Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

Formation of the natural sulfate aerosol

Energy Technology Data Exchange (ETDEWEB)

Kerminen, V.M.; Hillamo, R.; Maekinen, M.; Virkkula, A.; Maekelae, T.; Pakkanen, T. [Helsinki Univ. (Finland). Dept. of Physics

1996-12-31

Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

Is the aerosol emission detectable in the thermal infrared?

Science.gov (United States)

Hollweg, H.-D.; Bakan, S.; Taylor, J. P.

2006-08-01

The impact of aerosols on the thermal infrared radiation can be assessed by combining observations and radiative transfer calculations. Both have uncertainties, which are discussed in this paper. Observational uncertainties are obtained for two FTIR instruments operated side by side on the ground during the LACE 1998 field campaign. Radiative transfer uncertainties are assessed using a line-by-line model taking into account the uncertainties of the HITRAN 2004 spectroscopic database, uncertainties in the determination of the atmospheric profiles of water vapor and ozone, and differences in the treatment of the water vapor continuum absorption by the CKD 2.4.1 and MT_CKD 1.0 algorithms. The software package OPAC was used to describe the optical properties of aerosols for climate modeling. The corresponding radiative signature is a guideline to the assessment of the uncertainty ranges of observations and models. We found that the detection of aerosols depends strongly on the measurement accuracy of atmospheric profiles of water vapor and ozone and is easier for drier conditions. Within the atmospheric window, only the forcing of downward radiation at the surface by desert aerosol emerges clearly from the uncertainties of modeling and FTIR measurement. Urban and polluted continental aerosols are only partially detectable depending on the wave number and on the atmospheric water vapor amount. Simulations for the space-borne interferometer IASI show that only upward radiation above transported mineral dust aloft emerges out of the uncertainties. The detection of aerosols with weak radiative impact by FTIR instruments like ARIES and OASIS is made difficult by noise as demonstrated by the signal to noise ratio for clean continental aerosols. Altogether, the uncertainties found suggest that it is difficult to detect the optical depths of nonmineral and unpolluted aerosols.

Impact of anthropogenic aerosols on present and future climate

International Nuclear Information System (INIS)

Deandreis, C.

2008-03-01

Aerosols influence the Earth radiative budget both through their direct effect (scattering and absorption of solar radiation) and their indirect effect (impacts on cloud microphysics). The role of anthropogenic aerosol in climate change has been recognized to be significant when compared to the one of greenhouse gases. Despite many studies on this topic, the assessments of both anthropogenic aerosol radiative forcing and their impacts on meteorological variables are still very uncertain. Major reasons for these uncertainties stem from the insufficient knowledge of the emissions sources and of the processes of formation, transformation and deposition. Models used to study climate are often inadequate to study aerosol processes because of coarse spatial and temporal scales. Uncertainties due to the parameterization of the aerosol are added to the uncertainties in the representation of large scale dynamics and physical processes such as transport, hydrological cycle and radiative budget. To predict, the role of the anthropogenic aerosol impact in the future climate change, I have addressed some of these key uncertainties. In this study, I simulate interactively aerosols processes in a climate model in order to improve the estimation of their direct and indirect effects. I estimate a modification of the top of the atmosphere net flux of 60% for the present period. I also show that, for future projection, the representation of the emissions source is an other important source of error. I assess that aerosols radiative forcing differ by 40% between simulations performed with 2 different emissions inventories. These inventories are representative for a high and a low limit in term of carbonaceous aerosols emissions for the 2050 horizon. (author)

0D-modelling of carbonaceous aerosols; L'aerosol de combustion dans une region en grande mutation, l'Asie

Energy Technology Data Exchange (ETDEWEB)

Michel, Ch.

2005-06-15

One of the main uncertainties in the estimate of the climatic impact of aerosols is linked to our knowledge of gases and aerosols emissions. This is particularly crucial over Asia, where a strong regional fingerprint is observed, with different emission types, depending on the various vegetation and climate conditions (biomass burning emissions) and on the very fast changes of the population and industrialization (biofuel and fossil fuel emissions). The main goal of this work was first to derive a biomass burning inventory for gases and particles over Asia for the 2001 ACE-Asia (Aerosol Characterization Experiment) and TRACE-P (Transport and Chemical Evolution over the Pacific) campaigns (March to May 2001). I implemented a methodology that is the most adapted to my study, and based on the burnt area cartography (GBA-2000 project (Global Burnt Area 2000) [Tansey et al., 2005]). The results of this study, ABBI (Asian Biomass Burning Inventory) [Michel et al., 2005] have been compared with another biomass burning emission inventory (ACESS: ACE-Asia and TRACE-P Modelling and Emission Support System) [Streets et al., 2003], built from fire counts and not from burnt areas. This comparison shows the limits of the use of fire counts in the emission inventory maps and underlines the importance and the relevance of the method used in my study. A comparison with the year 2000 emission inventory, obtained with the same method, underlines the importance of the inter-annual variations. The ABBI inventory has been introduced in the Meso-NH-C mesoscale model combined with an aerosol module: ORISAM (ORganic and Inorganic Spectral Aerosol Module) Bessagnet, 2000]. I have focused in particular on the impact of the burnt vegetation emissions over the asian continent. Comparisons between simulated and ground and airborne measured data showed satisfactory results in some cases, but showed also some limits. Sensitivity tests have been carried out firstly to test the impact of fire

Regional modeling of carbonaceous aerosols over Europe-focus on secondary organic aerosols

Energy Technology Data Exchange (ETDEWEB)

Bessagnet, B. [INERIS, Inst Nat Env Indust Risques, F-60550 Verneuil en Halatte, (France); Menut, L. [Ecole Poltechnique, Inst Pierre Simon Laplace, Lab Meteorol Dyn, F-91128 Palaiseau, (France); Curci, G. [Univ degli Studi dell' Aquila, CETEMPS, 67010 Coppito - L' Aquila, (Italy); Hodzic, A. [NCAR, Nat Center for Atmosph Research, Boulder, 80301, CO, (United States); Guillaume, B.; Liousse, C. [LA/OMP, Lab Aerol/Observ Midi-Pyrenees, F-31400 Toulouse, (France); Moukhtar, S. [York Univ, Centre Atmosph Chem, Toronto, (Italy); Pun, B.; Seigneur, C. [Atmosph and Environ Research, San Ramon, CA 94583, (United States); Schulz, M. [CEA-CNRS-UVSQ, IPSL, Lab Sciences Climat et Environm, F-91191 Gif sur Yvette, (France)

2008-07-01

In this study, an improved and complete secondary organic aerosols (SOA) chemistry scheme was implemented in the CHIMERE model. The implementation of isoprene chemistry for SOA significantly improves agreement between long series of simulated and observed particulate matter concentrations. While simulated organic carbon concentrations are clearly improved at elevated sites by adding the SOA scheme, time correlation are impaired at low level sites in Portugal, Italy and Slovakia. At several sites a clear underestimation by the CHIMERE model is noticed in wintertime possibly due to missing wood burning emissions as shown in previous modeling studies. In Europe, the CHIMERE model gives yearly average SOA concentrations ranging from 0.5 {mu}g m{sup -3} in the Northern Europe to 4 {mu}g m{sup -3} over forested regions in Spain, France, Germany and Italy. In addition, our work suggests that during the highest fire emission periods, fires can be the dominant source of primary organic carbon over the Mediterranean Basin, but the SOA contribution from fire emissions is low. Isoprene chemistry has a strong impact on SOA formation when using current available kinetic schemes. (authors)

Tracing Primary PM2.5 emissions via Chinese supply chains

Science.gov (United States)

Meng, Jing; Liu, Junfeng; Xu, Yuan; Tao, Shu

2015-05-01

In this study, we examine a supply-chain approach to more effectively mitigate primary PM2.5 emissions in China from the perspectives of production, consumption and their linkages using structural path analysis. We identify the pattern of all supply chain paths using principal component analysis. To address the severe haze problems in China, it is important to understand how final demand purchase initiates production processes and ultimately leads to primary PM2.5 emission. We found that consumers’ demands on power and transportation mainly induce direct emissions, quite different from the demands on construction, industry and service products which largely drive emissions in upstream activities. We also found that nearly 80% of the economic sectors in China follow a similar pattern in generating primary PM2.5 emissions in electricity, cement and the ferrous metal industries; but only the construction sector increases the release of PM2.5 due to the production of non-metallic mineral products. These findings indicate that further reduction of end-of-pipe emissions in the power and transportation sectors will facilitate cleaner production in almost all the economic sectors. However, for urbanization induced emissions, China should mitigate PM2.5 emissions through the supply chain of construction, either severely reducing its life-cycle intensity or carefully planning to avoid extensive, unnecessary building activity.

Tracing Primary PM2.5 emissions via Chinese supply chains

International Nuclear Information System (INIS)

Meng, Jing; Liu, Junfeng; Tao, Shu; Xu, Yuan

2015-01-01

In this study, we examine a supply-chain approach to more effectively mitigate primary PM 2.5 emissions in China from the perspectives of production, consumption and their linkages using structural path analysis. We identify the pattern of all supply chain paths using principal component analysis. To address the severe haze problems in China, it is important to understand how final demand purchase initiates production processes and ultimately leads to primary PM 2.5 emission. We found that consumers’ demands on power and transportation mainly induce direct emissions, quite different from the demands on construction, industry and service products which largely drive emissions in upstream activities. We also found that nearly 80% of the economic sectors in China follow a similar pattern in generating primary PM 2.5 emissions in electricity, cement and the ferrous metal industries; but only the construction sector increases the release of PM 2.5 due to the production of non-metallic mineral products. These findings indicate that further reduction of end-of-pipe emissions in the power and transportation sectors will facilitate cleaner production in almost all the economic sectors. However, for urbanization induced emissions, China should mitigate PM 2.5 emissions through the supply chain of construction, either severely reducing its life-cycle intensity or carefully planning to avoid extensive, unnecessary building activity. (letter)

Atmospheric acidification of mineral aerosols: a source of bioavailable phosphorus for the oceans

Directory of Open Access Journals (Sweden)

A. Nenes

2011-07-01

Full Text Available Primary productivity of continental and marine ecosystems is often limited or co-limited by phosphorus. Deposition of atmospheric aerosols provides the major external source of phosphorus to marine surface waters. However, only a fraction of deposited aerosol phosphorus is water soluble and available for uptake by phytoplankton. We propose that atmospheric acidification of aerosols is a prime mechanism producing soluble phosphorus from soil-derived minerals. Acid mobilization is expected to be pronounced where polluted and dust-laden air masses mix. Our hypothesis is supported by the soluble compositions and reconstructed pH values for atmospheric particulate matter samples collected over a 5-yr period at Finokalia, Crete. In addition, at least tenfold increase in soluble phosphorus was observed when Saharan soil and dust were acidified in laboratory experiments which simulate atmospheric conditions. Aerosol acidification links bioavailable phosphorus supply to anthropogenic and natural acidic gas emissions, and may be a key regulator of ocean biogeochemistry.

BVOC-aerosol-climate interactions in the global aerosol-climate model ECHAM5.5-HAM2

Directory of Open Access Journals (Sweden)

R. Makkonen

2012-11-01

Full Text Available The biosphere emits volatile organic compounds (BVOCs which, after oxidation in the atmosphere, can partition on the existing aerosol population or even form new particles. The large quantities emitted provide means for a large potential impact on both aerosol direct and indirect effects. Biogenic responses to atmospheric temperature change can establish feedbacks even in rather short timescales. However, due to the complexity of organic aerosol partitioning, even the sign of these feedbacks is of large uncertainty. We use the global aerosol-climate model ECHAM5.5-HAM2 to explore the effect of BVOC emissions on new particle formation, clouds and climate. Two BVOC emission models, MEGAN2 and LPJ-GUESS, are used. MEGAN2 shows a 25% increase while LPJ-GUESS shows a slight decrease in global BVOC emission between years 2000 and 2100. The change of shortwave cloud forcing from year 1750 to 2000 ranges from −1.4 to −1.8 W m⁻² with 5 different nucleation mechanisms. We show that the change in shortwave cloud forcing from the year 2000 to 2100 ranges from 1.0 to 1.5 W m⁻². Although increasing future BVOC emissions provide 3–5% additional CCN, the effect on the cloud albedo change is modest. Due to simulated decreases in future cloud cover, the increased CCN concentrations from BVOCs can not provide significant additional cooling in the future.

Large contribution of natural aerosols to uncertainty in indirect forcing

Science.gov (United States)

Carslaw, K. S.; Lee, L. A.; Reddington, C. L.; Pringle, K. J.; Rap, A.; Forster, P. M.; Mann, G. W.; Spracklen, D. V.; Woodhouse, M. T.; Regayre, L. A.; Pierce, J. R.

2013-11-01

The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.

Large contribution of natural aerosols to uncertainty in indirect forcing.

Science.gov (United States)

Carslaw, K S; Lee, L A; Reddington, C L; Pringle, K J; Rap, A; Forster, P M; Mann, G W; Spracklen, D V; Woodhouse, M T; Regayre, L A; Pierce, J R

2013-11-07

The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.

Importance of Sulfate Aerosol in Evaluating the Relative Contributions of Regional Emissions to the Historical Global Temperature Change

International Nuclear Information System (INIS)

Andronova, N.; Schlesinger, M.

2004-01-01

During the negotiations of the Kyoto Protocol the delegation of Brazil presented an approach for distributing the burden of emissions reductions among the Parties based on the effect of their cumulative historical emissions on the global-average near-surface temperature. The Letter to the Parties does not limit the emissions to be considered to be only greenhouse gas (GHG) emissions. Thus, in this paper we explore the importance of anthropogenic SOx emissions that are converted to sulfate aerosol in the atmosphere, together with the cumulative greenhouse gas emissions, in attributing historical temperature change. We use historical emissions and our simple climate model to estimate the relative contributions to global warming of the regional emissions by four Parties: OECD90, Africa and Latin America, Asia, and Eastern Europe and the Former Soviet Union. Our results show that for most Parties the large warming contributed by their GHG emissions is largely offset by the correspondingly large cooling by their SOx emissions. Thus, OECD90 has become the dominant contributor to recent global warming following its large reduction in SOx emissions after 1980

Aerosols CFA 97

International Nuclear Information System (INIS)

Anon.

1998-01-01

During the thirteen congress on aerosols several papers were presented about the behaviour of radioactive aerosols and their impact on environment, or the exposure to radon and to its daughters, the measurement of the size of the particulates of the short-lived radon daughters and two papers about the behaviour of aerosols in containment during a fission products release in the primary circuit and susceptible to be released in atmosphere in the case of containment failure. (N.C.)

Comparison of two different dust emission mechanisms over the Horqin Sandy Land area: Aerosols contribution and size distributions

Science.gov (United States)

Ju, Tingting; Li, Xiaolan; Zhang, Hongsheng; Cai, Xuhui; Song, Yu

2018-03-01

Dust aerosols (PM10) emission fluxes due to convective turbulent dust emissions (CTDE) and saltation-bombardment and/or aggregation-disintegration dust emissions (SADE) events were comparatively studied using the data obtained from the Naiman station over the Horqin Sandy Land area in Inner Mongolia, China from 2011 to 2015. The annual cumulative dust fluxes released by CTDE events was about one third of that by SADE events, with the order of 103∼104 μg m-2 s-1. The particle size distributions (PSDs) with diameter between 0.1 and 20 μm during CTDE and SADE events over the Horqin Sandy Land area were simulated based on the fragmentation theory, respectively. The results indicated that an improved equation based on fragmentation theory could be applied to describe the PSDs over the Horqin site which may be because the scale-invariant fragmentation theory mainly explains the PSDs of free dust particles on the surface, which differ from the PSDs of suspend airborne dust and the improved equation was more applicable to the PSDs of SADE events because the dust emission mechanism of SADE are saltation bombardment and aggregation disintegration. The number-related mean aerosol diameters (DN) barely varied under different friction velocity (u*) for SADE events, while the volume-related mean aerosol diameters (DV) changed distinctly with the change of u*. For CTDE events, the DN and DV had no obvious relationship with the change of u* because the dominating influence factor during CTDE event was thermal convection rather than u*. The mass-related PSDs usually exhibited a peak between 0.45 and 0.70 μm during SADE events, while for CTDE events there was a wide peak in the range of 0.10 0.70 μm. The results suggest that DN should be not be recommended as an individual parameter to describe the PSDs. The mass-related PSDs can effectively distinguish the SADE and CTDE events.

Aerosol typing - key information from aerosol studies

Science.gov (United States)

Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

2016-04-01

Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

Aerosols in Northern Morocco: Input pathways and their chemical fingerprint

Science.gov (United States)

Benchrif, A.; Guinot, B.; Bounakhla, M.; Cachier, H.; Damnati, B.; Baghdad, B.

2018-02-01

The Mediterranean basin is one of the most sensitive regions in the world regarding climate change and air quality. Deserts and marine aerosols combine with combustion aerosols from maritime traffic, large urban centers, and at a larger scale from populated industrialized regions in Europe. From Tetouan city located in the North of Morocco, we attempted to better figure out the main aerosol transport pathways and their respective aerosol load and chemical profile by examining air mass back trajectory patterns and aerosol chemical compositions from May 2011 to April 2012. The back trajectory analysis throughout the sampling period led to four clusters, for which meteorological conditions and aerosol chemical characteristics have been investigated. The most frequent cluster (CL3: 39%) corresponds to polluted air masses coming from the Mediterranean Basin, characterized by urban and marine vessels emissions out of Spain and of Northern Africa. Two other polluted clusters were characterized. One is of local origin (CL1: 22%), with a marked contribution from urban aerosols (Rabat, Casablanca) and from biomass burning aerosols. The second (CL2: 32%) defines air masses from the near Atlantic Ocean, affected by pollutants emitted from the Iberian coast. A fourth cluster (CL4: 7%) is characterized by rather clean, fast and rainy oceanic air masses, influenced during their last 24 h before reaching Tetouan by similar sources with those affecting CL2, but to a lesser extent. The chemical data show that carbonaceous species are found in the fine aerosols fraction and are generally from local primary sources (low OC/EC) rather than long-range transported. In addition to fresh traffic and maritime vessel aerosols, our results suggest the contribution of local biomass burning.

Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

Science.gov (United States)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2015-05-01

. Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.

Investigating the Linear Dependence of Direct and Indirect Radiative Forcing on Emission of Carbonaceous Aerosols in a Global Climate Model

Energy Technology Data Exchange (ETDEWEB)

Chen, Yanju [Department of Civil and Environmental Engineering, University of Illinois at Urbana-Champaign, Urbana IL USA; Wang, Hailong [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Singh, Balwinder [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Ma, Po-Lun [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Rasch, Philip J. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Bond, Tami C. [Department of Civil and Environmental Engineering, University of Illinois at Urbana-Champaign, Urbana IL USA

2018-02-02

The linearity of dependence of aerosol direct and indirect radiative forcing (DRF and IRF) on emissions is essential to answer the policy-relevant question on how the change in forcing would result from a change in emission. In this study, the forcing-to-emission relationship is investigated for black carbon (BC) and primary organic carbon (OC) emitted from North America and Asia. Direct and indirect radiative forcing of BC and OC are simulated with the Community Atmosphere Model (CAM5.1). Two diagnostics are introduced to aid in policy-relevant discussion: emission-normalized forcing (ENF) and linearity (R). DRF is linearly related to emission for both BC and OC from the two regions and emission-normalized DRF is similar, within 15%. IRF is linear to emissions for weaker sources and regions far from source (North American BC and OC), while for large emission sources and near source regions (Asian OC) the response of forcing to emission is sub-linear. In North America emission-normalized IRF (ENIRF) is 2-4 times higher than that in Asia. The difference among regions and species is primarily caused by failure of accumulation mode particles to become CCN, and then to activate into CDNC. Optimal aggregation area (30ºx 30º) has been used to communicate the regional variation of forcing-to-emission relationship. For IRF, only 15-40% of the Earth’s surface is significantly affected by the two emission regions, but the forcing in these regions comprises most of the global impact. Linearity of IRF occurs in about two-thirds of the significant regions except for Asian OC. ENF is an effective tool to estimate forcing changes due to reduction of surface emissions, as long as there is sufficient attention to the causes of nonlinearity in the simulations used to derive ENIRF (emission into polluted regions and emission elevation). The differences in ENIRF have important implications for policy decisions. Lower ENIRF in more polluted region like Asia means that reductions of

TOXICOLOGICAL EVALUATION OF REALISTIC EMISSIONS OF SOURCE AEROSOLS (TERESA): APPLICATION TO POWER PLANT-DERIVED PM2.5

Energy Technology Data Exchange (ETDEWEB)

Annette Rohr

2006-03-01

TERESA (Toxicological Evaluation of Realistic Emissions of Source Aerosols) involves exposing laboratory rats to realistic coal-fired power plant and mobile source emissions to help determine the relative toxicity of these PM sources. There are three coal-fired power plants in the TERESA program; this report describes the results of fieldwork conducted at the first plant, located in the Upper Midwest. The project was technically challenging by virtue of its novel design and requirement for the development of new techniques. By examining aged, atmospherically transformed aerosol derived from power plant stack emissions, we were able to evaluate the toxicity of PM derived from coal combustion in a manner that more accurately reflects the exposure of concern than existing methodologies. TERESA also involves assessment of actual plant emissions in a field setting--an important strength since it reduces the question of representativeness of emissions. A sampling system was developed and assembled to draw emissions from the stack; stack sampling conducted according to standard EPA protocol suggested that the sampled emissions are representative of those exiting the stack into the atmosphere. Two mobile laboratories were then outfitted for the study: (1) a chemical laboratory in which the atmospheric aging was conducted and which housed the bulk of the analytical equipment; and (2) a toxicological laboratory, which contained animal caging and the exposure apparatus. Animal exposures were carried out from May-November 2004 to a number of simulated atmospheric scenarios. Toxicological endpoints included (1) pulmonary function and breathing pattern; (2) bronchoalveolar lavage fluid cytological and biochemical analyses; (3) blood cytological analyses; (4) in vivo oxidative stress in heart and lung tissue; and (5) heart and lung histopathology. Results indicated no differences between exposed and control animals in any of the endpoints examined. Exposure concentrations for the

Quantification of regional radiative impacts and climate effects of tropical fire aerosols

Science.gov (United States)

Tosca, M. G.; Zender, C. S.; Randerson, J. T.

2011-12-01

Regionally expansive smoke clouds originating from deforestation fires in Indonesia can modify local precipitation patterns via direct aerosol scattering and absorption of solar radiation (Tosca et al., 2010). Here we quantify the regional climate impacts of fire aerosols for three tropical burning regions that together account for about 70% of global annual fire emissions. We use the Community Atmosphere Model, version 5 (CAM5) coupled to a slab ocean model (SOM) embedded within the Community Earth System Model (CESM). In addition to direct aerosol radiative effects, CAM5 also quantifies indirect, semi-direct and cloud microphysical aerosol effects. Climate impacts are determined using regionally adjusted emissions data that produce realistic aerosol optical depths in CAM5. We first analyzed a single 12-year transient simulation (1996-2007) forced with unadjusted emissions estimates from the Global Fire Emissions Database, version 3 (GFEDv3) and compared the resulting aerosol optical depths (AODs) for 4 different burning regions (equatorial Asia, southern Africa, South America and boreal North America) to observed MISR and MODIS AODs for the same period. Based on this analysis we adjusted emissions for each burning region between 150 and 300% and forced a second simulation with the regionally adjusted emissions. Improved AODs from this simulation are compared to AERONET observations available at 15 stations throughout the tropics. We present here two transient simulations--one with the adjusted fire emissions and one without fires--to quantify the cumulative fire aerosol climate impact for three major tropical burning regions (equatorial Asia, southern Africa and South America). Specifically, we quantify smoke effects on radiation, precipitation, and temperature. References Tosca, M.G., J.T. Randerson, C.S. Zender, M.G. Flanner and P.J. Rasch (2010), Do biomass burning aerosols intensify drought in equatorial Asia during El Nino?, Atmos. Chem. Phys., 10, 3515

The composition and variability of atmospheric aerosol over Southeast Asia during 2008

Directory of Open Access Journals (Sweden)

W. Trivitayanurak

2012-01-01

Full Text Available We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands was a net exporter of primary organic aerosol (42 kT and black carbon aerosol (11 kT. We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA, with Borneo being a net exporter of SOA (15 kT. SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%, with smaller contributions from gas-phase oxidation (15% and advection into the regions (14%. We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where

The composition and variability of atmospheric aerosol over Southeast Asia during 2008

Science.gov (United States)

Trivitayanurak, W.; Palmer, P. I.; Barkley, M. P.; Robinson, N. H.; Coe, H.; Oram, D. E.

2012-01-01

We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands) was a net exporter of primary organic aerosol (42 kT) and black carbon aerosol (11 kT). We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA), with Borneo being a net exporter of SOA (15 kT). SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%), with smaller contributions from gas-phase oxidation (15%) and advection into the regions (14%). We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD) data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where the model

Sampling and chemical analysis by TXRF of size-fractionated ambient aerosols and emissions

International Nuclear Information System (INIS)

John, A.C.; Kuhlbusch, T.A.J.; Fissan, H.; Schmidt, K.-G-; Schmidt, F.; Pfeffer, H.-U.; Gladtke, D.

2000-01-01

Results of recent epidemiological studies led to new European air quality standards which require the monitoring of particles with aerodynamic diameters ≤ 10 μm (PM 10) and ≤ 2.5 μm (PM 2.5) instead of TSP (total suspended particulate matter). As these ambient air limit values will be exceeded most likely at several locations in Europe, so-called 'action plans' have to be set up to reduce particle concentrations, which requires information about sources and processes of PMx aerosols. For chemical characterization of the aerosols, different samplers were used and total reflection x-ray fluorescence analysis (TXRF) was applied beside other methods (elemental and organic carbon analysis, ion chromatography, atomic absorption spectrometry). For TXRF analysis, a specially designed sampling unit was built where the particle size classes 10-2.5 μm and 2.5-1.0 μm were directly impacted on TXRF sample carriers. An electrostatic precipitator (ESP) was used as a back-up filter to collect particles <1 μm directly on a TXRF sample carrier. The sampling unit was calibrated in the laboratory and then used for field measurements to determine the elemental composition of the mentioned particle size fractions. One of the field campaigns was carried out at a measurement site in Duesseldorf, Germany, in November 1999. As the composition of the ambient aerosols may have been influenced by a large construction site directly in the vicinity of the station during the field campaign, not only the aerosol particles, but also construction material was sampled and analyzed by TXRF. As air quality is affected by natural and anthropogenic sources, the emissions of particles ≤ 10 μm and ≤ 2.5 μm, respectively, have to be determined to estimate their contributions to the so called coarse and fine particle modes of ambient air. Therefore, an in-stack particle sampling system was developed according to the new ambient air quality standards. This PM 10/PM 2.5 cascade impactor was

Aerosol impacts on regional trends in atmospheric stagnation

Science.gov (United States)

Mascioli, N. R.; Fiore, A. M.; Previdi, M. J.

2017-12-01

Extreme pollution events pose a significant threat to human health and are a leading cause of premature mortality worldwide. While emissions of atmospheric pollutants and their precursors are projected to decrease in the future due to air quality legislation, future climate change may affect the underlying meteorological conditions that contribute to extreme pollution events. Stagnation events, characterized by weak winds and an absence of precipitation, contribute to extreme pollution by halting the removal of pollutants via advection and wet deposition. Here, we use a global climate model (GFDL-CM3) to show that regional stagnation trends over the historical period (1860-2005) are driven by changes in anthropogenic aerosol emissions, rather than rising greenhouse gases. In the northeastern and central United States, aerosol-induced changes in surface and upper level winds have produced significant decreases in the number of stagnant summer days, while decreasing precipitation in the southeast US has increased the number of stagnant summer days. Significant drying over eastern China in response to aerosol forcing contributed to increased stagnation. Additionally, this region was found to be particularly sensitive to changes in local emissions, indicating that improving air quality will also lessen stagnation. In Europe, we find a dipole pattern wherein stagnation decreases over southern Europe and increases over northern Europe in response to global increases in aerosol emissions. We hypothesize that this is due to changes in the large-scale circulation patterns associated with a poleward shift of the North Atlantic storm track. We find that in the future, the combination of declining aerosol emissions and the continued rise of greenhouse gas emissions will lead to a reversal of the historical stagnation trends.

Coupling aerosol-cloud-radiative processes in the WRF-Chem model: Investigating the radiative impact of elevated point sources

Directory of Open Access Journals (Sweden)

E. G. Chapman

2009-02-01

resolution model domain (the extent of which corresponds to the typical size of a single global climate model grid cell and temporally over a three day analysis period, total rainfall in the sensitivity simulation increased by 31% over that in the baseline simulation. Fewer optically thin clouds, arbitrarily defined as a cloud exhibiting an optical depth less than 1, formed in the sensitivity simulation. Domain-averaged AODs dropped from 0.46 in the baseline simulation to 0.38 in the sensitivity simulation. The overall net effect of additional aerosols attributable to primary particulates and aerosol precursors from point source emissions above the surface was a domain-averaged reduction of 5 W m⁻² in mean daytime downwelling shortwave radiation.

Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

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D. V. Spracklen

2011-09-01

Full Text Available Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (CCN so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to CCN has not been evaluated on the global scale. By combining extensive observations of CCN concentrations with the GLOMAP global aerosol model, we find that the model is biased low (normalised mean bias = −77 % unless carbonaceous combustion aerosol act as CCN. We show that carbonaceous combustion aerosol accounts for more than half (52–64 % of global CCN with the range due to uncertainty in the emitted size distribution of carbonaceous combustion particles. The model predicts that wildfire and pollution (fossil fuel and biofuel carbonaceous combustion aerosol causes a global mean cloud albedo aerosol indirect effect of −0.34 W m⁻², with stronger cooling if we assume smaller particle emission size. We calculate that carbonaceous combustion aerosol from pollution sources cause a global mean aerosol indirect effect of −0.23 W m⁻². The small size of carbonaceous combustion particles from fossil fuel sources means that whilst pollution sources account for only one-third of the emitted mass they cause two-thirds of the cloud albedo aerosol indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for, along with other cloud effects not studied here, to ensure that black carbon emissions controls that reduce the high number concentrations of fossil fuel particles have the desired net effect on climate.

GHG emissions from primary aluminum production in China: Regional disparity and policy implications

International Nuclear Information System (INIS)

Hao, Han; Geng, Yong; Hang, Wen

2016-01-01

Highlights: • GHG emissions from primary aluminum production in China were accounted. • The impact of regional disparity of power generation was considered for this study. • GHG emissions factor of China’s primary aluminum production was 16.5 t CO_2e/t Al ingot in 2013. • Total GHG emissions from China’s primary aluminum production were 421 mt CO_2e in 2013. - Abstract: China is the world-leading primary aluminum production country, which contributed to over half of global production in 2014. Primary aluminum production is power-intensive, for which power generation has substantial impact on overall Greenhouse Gas (GHG) emissions. In this study, we explore the impact of regional disparity of China’s power generation system on GHG emissions for the sector of primary aluminum production. Our analysis reveals that the national GHG emissions factor (GEF) of China’s primary aluminum production was 16.5 t CO_2e/t Al ingot in 2013, with province-level GEFs ranging from 8.2 to 21.7 t CO_2e/t Al ingot. There is a high coincidence of provinces with high aluminum productions and high GEFs. Total GHG emissions from China’s primary aluminum production were 421 mt CO_2e in 2013, approximately accounting for 4% of China’s total GHG emissions. Under the 2020 scenario, GEF shows a 13.2% reduction compared to the 2013 level, but total GHG emissions will increase to 551 mt CO_2e. Based on our analysis, we recommend that the government should further promote energy efficiency improvement, facilitate aluminum industry redistribution with low-carbon consideration, promote secondary aluminum production, and improve aluminum industry data reporting and disclosure.

Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: meteorology and air mass origin dominate aerosol particle composition and size distribution

Directory of Open Access Journals (Sweden)

F. Freutel

2013-01-01

Full Text Available During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m⁻³, 2 μg m⁻³, 2 μg m⁻³, and 7 μg m⁻³, respectively were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m⁻³, 0.2 μg m⁻³, 0.4 μg m⁻³, and 1–3 μg m⁻³, respectively. For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NO_x it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be

Dust-wind interactions can intensify aerosol pollution over eastern China.

Science.gov (United States)

Yang, Yang; Russell, Lynn M; Lou, Sijia; Liao, Hong; Guo, Jianping; Liu, Ying; Singh, Balwinder; Ghan, Steven J

2017-05-11

Eastern China has experienced severe and persistent winter haze episodes in recent years due to intensification of aerosol pollution. In addition to anthropogenic emissions, the winter aerosol pollution over eastern China is associated with unusual meteorological conditions, including weaker wind speeds. Here we show, based on model simulations, that during years with decreased wind speed, large decreases in dust emissions (29%) moderate the wintertime land-sea surface air temperature difference and further decrease winds by -0.06 (±0.05) m s -1 averaged over eastern China. The dust-induced lower winds enhance stagnation of air and account for about 13% of increasing aerosol concentrations over eastern China. Although recent increases in anthropogenic emissions are the main factor causing haze over eastern China, we conclude that natural emissions also exert a significant influence on the increases in wintertime aerosol concentrations, with important implications that need to be taken into account by air quality studies.

Chemical compositions, sources and evolution processes of the submicron aerosols in Nanjing, China during wintertime

Science.gov (United States)

Wu, Y.; He, Y.; Ge, X.; Wang, J.; Yu, H.; Chen, M.

2016-12-01

Elevated atmospheric particulate matter pollution is one of the most significant environmental issues in the Yangtze River Delta (YRD), China. Thus it is important to unravel the characteristics, sources and evolution processes of the ambient aerosols in order to improve the air quality. In this study, we report the real-time monitoring results on submicron aerosol particles (PM1) in suburban Nanjing during wintertime of 2015, using an Aerodyne soot particle aerosol mass spectrometer (SP-AMS). This instrument allows the fast measurement of refractory black carbon simultaneously with other aerosol components. Results show that organics was on average the most abundant species of PM1 (25.9%), but other inorganic species, such as nitrate (23.7%) and sulfate (23.3%) also comprised large mass fractions. As the sampling site is heavily influenced by various sources including industrial, traffic and other anthropogenic emissions, etc., six organic aerosol (OA) factors were identified from Positive matrix factorization (PMF) analysis of the SP-AMS OA mass spectra. These factors include three primary OA factors - a hydrocarbon-like OA, an industry-related OA (IOA) and a cooking OA (COA), and three secondary OA factors, i.e., a local OOA (LSOA), a semi-volatile OOA (SV-OOA) and a low-volatility OOA (LV-OOA). Overall, the primary organic aerosol (POA) (HOA, IOA and COA) dominated the total OA mass. Behaviors and evolution processes of these OA factors will be discussed in combining with the other supporting data.

Spacetime Distributions of Wildfire Areas and Emissions of Carbon-Containing Gases and Aerosols in Northern Eurasia according to Satellite-Monitoring Data

Science.gov (United States)

Bondur, V. G.; Gordo, K. A.; Kladov, V. L.

2017-12-01

Based on online wildfire satellite-monitoring data, distributions of burned-out areas, as well as emission volumes of carbon-containing gases (CO and CO2) and fine aerosols (PM2.5), for different regions and months in 2005-2016 (across the territory of Russia) and in 2010-2016 (northern Eurasia) are analyzed. Distinctive features of the seasonal behavior of wildfires and emission volumes of carbon-containing gases and fine aerosols for different regions of northern Eurasia are determined. It is shown that between 2005 and 2016 the annual area of territories burned out during wildfires in Russia decreased by almost a factor of 2.6 owing to early detection and suppression of fire sources. It is determined that in 2014-2016 the relative size of burned-out areas in Ukraine increased 6-9-fold and volumes of CO, CO2, and PM2.5 emissions by more than a factor of 6.5-7.5 times when compared to earlier years and these characteristics for other European countries.

Trace elements in aerosols from background air pollution monitoring stations in the Amazon Basin using nuclear-related techniques

International Nuclear Information System (INIS)

Artaxo, P.; Martins, J.V.; Yamasoe, M.A.; Gerab, F.; Kocinas, S.

1994-01-01

In order to study the natural release of aerosol particles by the Amazon Basin tropical rain forest, the composition and size distribution of biogenic aerosol particles were analyzed. The role of the atmospheric emissions from the Amazon Basin rain forest in the global atmosphere will be investigated. The atmosphere was studied in long-term sampling stations in three different locations. The elemental composition of aerosol particles released during biomass burning was also measured in several different ecosystems, from primary forest to Savannah. One of the main focuses was to identify and quantify important physical and chemical processes in the generation, transformation and deposition of aerosol particles. Also important was to obtain a better understanding of natural aerosol sources concerning identification, their characteristics and strength, to be able to understand the natural chemistry in the atmosphere on a global scale. 36 refs, 3 figs, 3 tabs

Evidence of a reduction in cloud condensation nuclei activity of water-soluble aerosols caused by biogenic emissions in a cool-temperate forest.

Science.gov (United States)

Müller, Astrid; Miyazaki, Yuzo; Tachibana, Eri; Kawamura, Kimitaka; Hiura, Tsutom

2017-08-16

Biogenic organic aerosols can affect cloud condensation nuclei (CCN) properties, and subsequently impact climate change. Large uncertainties exist in how the difference in the types of terrestrial biogenic sources and the abundance of organics relative to sulfate affect CCN properties. For the submicron water-soluble aerosols collected for two years in a cool-temperate forest in northern Japan, we show that the hygroscopicity parameter κ CCN (0.44 ± 0.07) exhibited a distinct seasonal trend with a minimum in autumn (κ CCN  = 0.32-0.37); these κ CCN values were generally larger than that of ambient particles, including water-insoluble fractions. The temporal variability of κ CCN was controlled by the water-soluble organic matter (WSOM)-to-sulfate ratio (R 2  > 0.60), where the significant reduction of κ CCN in autumn was linked to the increased WSOM/sulfate ratio. Positive matrix factorization analysis indicates that α-pinene-derived secondary organic aerosol (SOA) substantially contributed to the WSOM mass (~75%) in autumn, the majority of which was attributable to emissions from litter/soil microbial activity near the forest floor. These findings suggest that WSOM, most likely α-pinene SOA, originated from the forest floor can significantly suppress the aerosol CCN activity in cool-temperate forests, which have implications for predicting climate effects by changes in biogenic emissions in future.

Landscape fires dominate terrestrial natural aerosol - climate feedbacks

Science.gov (United States)

Scott, C.; Arnold, S.; Monks, S. A.; Asmi, A.; Paasonen, P.; Spracklen, D. V.

2017-12-01

The terrestrial biosphere is an important source of natural aerosol including landscape fire emissions and secondary organic aerosol (SOA) formed from biogenic volatile organic compounds (BVOCs). Atmospheric aerosol alters the Earth's climate by absorbing and scattering radiation (direct radiative effect; DRE) and by perturbing the properties of clouds (aerosol indirect effect; AIE). Natural aerosol sources are strongly controlled by, and can influence, climate; giving rise to potential natural aerosol-climate feedbacks. Earth System Models (ESMs) include a description of some of these natural aerosol-climate feedbacks, predicting substantial changes in natural aerosol over the coming century with associated radiative perturbations. Despite this, the sensitivity of natural aerosols simulated by ESMs to changes in climate or emissions has not been robustly tested against observations. Here we combine long-term observations of aerosol number and a global aerosol microphysics model to assess terrestrial natural aerosol-climate feedbacks. We find a strong positive relationship between the summertime anomaly in observed concentration of particles greater than 100 nm diameter and the anomaly in local air temperature. This relationship is reproduced by the model and driven by variability in dynamics and meteorology, as well as natural sources of aerosol. We use an offline radiative transfer model to determine radiative effects due to changes in two natural aerosol sources: landscape fire and biogenic SOA. We find that interannual variability in the simulated global natural aerosol radiative effect (RE) is negatively related to the global temperature anomaly. The magnitude of global aerosol-climate feedback (sum of DRE and AIE) is estimated to be -0.15 Wm-2 K-1 for landscape fire aerosol and -0.06 Wm-2 K-1 for biogenic SOA. These feedbacks are comparable in magnitude, but opposite in sign to the snow albedo feedback, highlighting the need for natural aerosol feedbacks to

Aerosol climate effects and air quality impacts from 1980 to 2030

International Nuclear Information System (INIS)

Menon, Surabi; Sednev, Igor; Unger, Nadine; Koch, Dorothy; Shindell, Drew; Francis, Jennifer; Garrett, Tim; Streets, David

2008-01-01

We investigate aerosol effects on climate for 1980, 1995 (meant to reflect present day) and 2030 using the NASA Goddard Institute for Space Studies climate model coupled to an on-line aerosol source and transport model with interactive oxidant and aerosol chemistry. Aerosols simulated include sulfates, organic matter (OM), black carbon (BC), sea-salt and dust and, additionally, the amount of tropospheric ozone is calculated, allowing us to estimate both changes to air quality and climate for different time periods and emission amounts. We include both the direct aerosol effect and indirect aerosol effects for liquid-phase clouds. Future changes for the 2030 A1B scenario are examined, focusing on the Arctic and Asia, since changes are pronounced in these regions. Our results for the different time periods include both emission changes and physical climate changes. We find that the aerosol indirect effect (AIE) has a large impact on photochemical processing, decreasing ozone amount and ozone forcing, especially for the future (2030-1995). Ozone forcings increase from 0 to 0.12 W m -2 and the total aerosol forcing decreases from -0.10 to -0.94 W m -2 (AIE decreases from -0.13 to -0.68 W m -2 ) for 1995-1980 versus 2030-1995. Over the Arctic we find that compared to ozone and the direct aerosol effect, the AIE contributes the most to net radiative flux changes. The AIE, calculated for 1995-1980, is positive (1.0 W m -2 ), but the magnitude decreases (-0.3 W m -2 ) considerably for the future scenario. Over Asia, we evaluate the role of biofuel- and transportation-based emissions (for BC and OM) via a scenario (2030A) that includes a projected increase (factor of 2) in biofuel- and transport-based emissions for 2030 A1B over Asia. Projected changes from present day due to the 2030A emissions versus 2030 A1B are a factor of 4 decrease in summertime precipitation in Asia. Our results are sensitive to emissions used. Uncertainty in present-day emissions suggests that

Carbonyl Emissions in E-cigarette Aerosol: A Systematic Review and Methodological Considerations

Directory of Open Access Journals (Sweden)

Konstantinos E. Farsalinos

2018-01-01

Full Text Available Carbonyl emissions from tobacco cigarettes represent a substantial health risk contributing to smoking-related morbidity and mortality. As expected, this is an important research topic for tobacco harm reduction products, in an attempt to compare the relative risk of these products compared to tobacco cigarettes. In this study, a systematic review of the literature available on PubMed was performed analyzing the studies evaluating carbonyl emissions from e-cigarettes. A total of 32 studies were identified and presented. We identified a large diversity of methodologies, with substantial discrepancies in puffing patterns, aerosol collection and analytical methods as well as reported units of measurements. Such discrepancies make comparisons difficult, and in some cases the accuracy of the findings cannot be determined. Importantly, control for the generation of dry puffs was not performed in the vast majority of studies, particularly in studies using variable power devices, which could result in testing conditions and reported carbonyl levels that have no clinical relevance or context. Some studies have been replicated, verifying the presence of dry puff conditions. Whenever realistic use conditions were ensured, carbonyl emissions from e-cigarettes were substantially lower than tobacco cigarette smoke, while newer generation (bottom-coil, cotton wick atomizers appeared to emit minimal levels of carbonyls with questionable clinical significance in terms of health risk. However, extremely high levels of carbonyl emissions were reported in some studies, and all these studies need to be replicated because of potentially important health implications.

Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

International Nuclear Information System (INIS)

Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

2010-01-01

Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m 2 between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m 2 depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

Evaluation of chemical transport model predictions of primary organic aerosol for air masses classified by particle-component-based factor analysis

OpenAIRE

C. A. Stroud; M. D. Moran; P. A. Makar; S. Gong; W. Gong; J. Zhang; J. G. Slowik; J. P. D. Abbatt; G. Lu; J. R. Brook; C. Mihele; Q. Li; D. Sills; K. B. Strawbridge; M. L. McGuire

2012-01-01

Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in Southern Ontario, Canada, were used to evaluate predictions of primary organic aerosol (POA) and two other carbonaceous species, black carbon (BC) and carbon monoxide (CO), made for this summertime period by Environment Canada's AURAMS regional chemical transport model. Particle component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two...

Organic compounds in aerosols from selected European sites - Biogenic versus anthropogenic sources

Science.gov (United States)

Alves, Célia; Vicente, Ana; Pio, Casimiro; Kiss, Gyula; Hoffer, Andras; Decesari, Stefano; Prevôt, André S. H.; Minguillón, María Cruz; Querol, Xavier; Hillamo, Risto; Spindler, Gerald; Swietlicki, Erik

2012-11-01

Atmospheric aerosol samples from a boreal forest (Hyytiälä, April 2007), a rural site in Hungary (K-puszta, summer 2008), a polluted rural area in Italy (San Pietro Capofiume, Po Valley, April 2008), a moderately polluted rural site in Germany located on a meadow (Melpitz, May 2008), a natural park in Spain (Montseny, March 2009) and two urban background locations (Zurich, December 2008, and Barcelona, February/March 2009) were collected. Aliphatics, polycyclic aromatic hydrocarbons, carbonyls, sterols, n-alkanols, acids, phenolic compounds and anhydrosugars in aerosols were chemically characterised by gas chromatography-mass spectrometry, along with source attribution based on the carbon preference index (CPI), the ratios between the unresolved and the chromatographically resolved aliphatics, the contribution of wax n-alkanes, n-alkanols and n-alkanoic acids from plants, diagnostic ratios of individual target compounds and source-specific markers to organic carbon ratios. In spite of transboundary pollution episodes, Hyytiälä registered the lowest levels among all locations. CPI values close to 1 for the aliphatic fraction of the Montseny aerosol suggest that the anthropogenic input may be associated with the transport of aged air masses from the surrounding industrial/urban areas, which superimpose the locally originated hydrocarbons with biogenic origin. Aliphatic and aromatic hydrocarbons in samples from San Pietro Capofiume reveal that fossil fuel combustion is a major source influencing the diel pattern of concentrations. This source contributed to 25-45% of the ambient organic carbon (OC) at the Po Valley site. Aerosols from the German meadow presented variable contributions from both biogenic and anthropogenic sources. The highest levels of vegetation wax components and biogenic secondary organic aerosol (SOA) products were observed at K-puszta, while anthropogenic SOA compounds predominated in Barcelona. The primary vehicular emissions in the Spanish

A study of regional-scale aerosol assimilation using a Stretch-NICAM

Science.gov (United States)

Misawa, S.; Dai, T.; Schutgens, N.; Nakajima, T.

2013-12-01

Although aerosol is considered to be harmful to human health and it became a social issue, aerosol models and emission inventories include large uncertainties. In recent studies, data assimilation is applied to aerosol simulation to get more accurate aerosol field and emission inventory. Most of these studies, however, are carried out only on global scale, and there are only a few researches about regional scale aerosol assimilation. In this study, we have created and verified an aerosol assimilation system on regional scale, in hopes to reduce an error associated with the aerosol emission inventory. Our aerosol assimilation system has been developed using an atmospheric climate model, NICAM (Non-hydrostaric ICosahedral Atmospheric Model; Satoh et al., 2008) with a stretch grid system and coupled with an aerosol transport model, SPRINTARS (Takemura et al., 2000). Also, this assimilation system is based on local ensemble transform Kalman filter (LETKF). To validate this system, we used a simulated observational data by adding some artificial errors to the surface aerosol fields constructed by Stretch-NICAM-SPRINTARS. We also included a small perturbation in original emission inventory. This assimilation with modified observational data and emission inventory was performed in Kanto-plane region around Tokyo, Japan, and the result indicates the system reducing a relative error of aerosol concentration by 20%. Furthermore, we examined a sensitivity of the aerosol assimilation system by varying the number of total ensemble (5, 10 and 15 ensembles) and local patch (domain) size (radius of 50km, 100km and 200km), both of which are the tuning parameters in LETKF. The result of the assimilation with different ensemble number 5, 10 and 15 shows that the larger the number of ensemble is, the smaller the relative error become. This is consistent with ensemble Kalman filter theory and imply that this assimilation system works properly. Also we found that assimilation system

MATRIX (Multiconfiguration Aerosol TRacker of mIXing state: an aerosol microphysical module for global atmospheric models

Directory of Open Access Journals (Sweden)

S. E. Bauer

2008-10-01

Full Text Available A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS climate model (ModelE are described. This module, which is based on the quadrature method of moments (QMOM, represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations.

A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment

Testing Re-entrained Aerosol Kinetic Emissions from Roads : a new approach to infer silt loading on roadways

Science.gov (United States)

Kuhns, H.; Etyemezian, V.; Landwehr, D.; MacDougall, C.; Pitchford, M.; Green, M.

PM 10 and PM 2.5 emissions from roadways are currently estimated using the silt loading on the road surface as a surrogate for the emissions potential of road dust. While the United States Environmental Protection Agency prescribes this method in AP-42, there is considerable cost associated with silt loading measurements; it is feasible to sample only a small portion of a roadway network. A new approach for measuring the concentration of suspendable PM 10 above road surfaces has been developed to obtain a more spatially representative estimate of a road's potential to emit dust. The Testing Re-entrained Aerosols Kinetic Emissions from Roads (TRAKER) system uses real-time aerosol sensors mounted on a vehicle to measure the concentration of dust suspended from the road while the vehicle is in motion. When coupled with a Global Positioning System (GPS) instrument, TRAKER can be used to efficiently survey the changes in suspendable particles due to varying road conditions over a large spatial domain. In a recent study on paved roads in Las Vegas, the TRAKER system was compared with collocated silt loading measurements. The TRAKER system was also used to survey the relative amounts of suspendable road dust on approximately 300 miles of paved roads. The system provides a unique perspective on road dust sources and their spatial distribution. Results of this study indicated that the difference of the PM 10 concentrations measured behind the tire and on the hood is exponentially related to vehicle speed. This was an interesting finding because current AP-42 road dust emissions estimation methods do not include vehicle speed as a factor in the emissions calculations. The experiment also demonstrated that the distribution of suspendable material on roadways is highly variable and that a large number of samples are needed to represent road dust emissions potential on an urban scale for a variety of road and activity conditions.

76 FR 9409 - National Emission Standards for Hazardous Air Pollutants: Primary Lead Smelting

Science.gov (United States)

2011-02-17

... National Emission Standards for Hazardous Air Pollutants: Primary Lead Smelting; Proposed Rule #0;#0... Emission Standards for Hazardous Air Pollutants: Primary Lead Smelting AGENCY: Environmental Protection... standards for hazardous air pollutants (NESHAP) for Primary Lead Smelting to address the results of the...

Light absorbing organic aerosols (brown carbon) over the tropical Indian Ocean: impact of biomass burning emissions

International Nuclear Information System (INIS)

Srinivas, Bikkina; Sarin, M M

2013-01-01

The first field measurements of light absorbing water-soluble organic carbon (WSOC), referred as brown carbon (BrC), have been made in the marine atmospheric boundary layer (MABL) during the continental outflow to the Bay of Bengal (BoB) and the Arabian Sea (ARS). The absorption signal measured at 365 nm in aqueous extracts of aerosols shows a systematic linear increase with WSOC concentration, suggesting a significant contribution from BrC to the absorption properties of organic aerosols. The mass absorption coefficient (b abs ) of BrC shows an inverse hyperbolic relation with wavelength (from ∼300 to 700 nm), providing an estimate of the Angstrom exponent (α P , range: 3–19; Av: 9 ± 3). The mass absorption efficiency of brown carbon (σ abs−BrC ) in the MABL varies from 0.17 to 0.72 m 2  g −1 (Av: 0.45 ± 0.14 m 2  g −1 ). The α P and σ abs−BrC over the BoB are quite similar to that studied from a sampling site in the Indo-Gangetic Plain (IGP), suggesting the dominant impact of organic aerosols associated with the continental outflow. A comparison of the mass absorption efficiency of BrC and elemental carbon (EC) brings to focus the significant role of light absorbing organic aerosols (from biomass burning emissions) in atmospheric radiative forcing over oceanic regions located downwind of the pollution sources. (letter)

Time-resolved analysis of particle emissions from residential biomass combustion - Emissions of refractory black carbon, PAHs and organic tracers

Science.gov (United States)

Nielsen, Ingeborg E.; Eriksson, Axel C.; Lindgren, Robert; Martinsson, Johan; Nyström, Robin; Nordin, Erik Z.; Sadiktsis, Ioannis; Boman, Christoffer; Nøjgaard, Jacob K.; Pagels, Joakim

2017-09-01

Time-resolved particle emissions from a conventional wood stove were investigated with aerosol mass spectrometry to provide links between combustion conditions, emission factors, mixing state of refractory black carbon and implications for organic tracer methods. The addition of a new batch of fuel results in low temperature pyrolysis as the fuel heats up, resulting in strong, short-lived, variable emission peaks of organic aerosol-containing markers of anhydrous sugars, such as levoglucosan (fragment at m/z 60). Flaming combustion results in emissions dominated by refractory black carbon co-emitted with minor fractions of organic aerosol and markers of anhydrous sugars. Full cycle emissions are an external mixture of larger organic aerosol-dominated and smaller thinly coated refractory black carbon particles. A very high burn rate results in increased full cycle mass emission factors of 66, 2.7, 2.8 and 1.3 for particulate polycyclic aromatic hydrocarbons, refractory black carbon, total organic aerosol and m/z 60, respectively, compared to nominal burn rate. Polycyclic aromatic hydrocarbons are primarily associated with refractory black carbon-containing particles. We hypothesize that at very high burn rates, the central parts of the combustion zone become air starved, leading to a locally reduced combustion temperature that reduces the conversion rates from polycyclic aromatic hydrocarbons to refractory black carbon. This facilitates a strong increase of polycyclic aromatic hydrocarbons emissions. At nominal burn rates, full cycle emissions based on m/z 60 correlate well with organic aerosol, refractory black carbon and particulate matter. However, at higher burn rates, m/z 60 does not correlate with increased emissions of polycyclic aromatic hydrocarbons, refractory black carbon and organic aerosol in the flaming phase. The new knowledge can be used to advance source apportionment studies, reduce emissions of genotoxic compounds and model the climate impacts of

Mathematical modeling of atmospheric fine particle-associated primary organic compound concentrations

Science.gov (United States)

Rogge, Wolfgang F.; Hildemann, Lynn M.; Mazurek, Monica A.; Cass, Glen R.; Simoneit, Bernd R. T.

1996-08-01

An atmospheric transport model has been used to explore the relationship between source emissions and ambient air quality for individual particle phase organic compounds present in primary aerosol source emissions. An inventory of fine particulate organic compound emissions was assembled for the Los Angeles area in the year 1982. Sources characterized included noncatalyst- and catalyst-equipped autos, diesel trucks, paved road dust, tire wear, brake lining dust, meat cooking operations, industrial oil-fired boilers, roofing tar pots, natural gas combustion in residential homes, cigarette smoke, fireplaces burning oak and pine wood, and plant leaf abrasion products. These primary fine particle source emissions were supplied to a computer-based model that simulates atmospheric transport, dispersion, and dry deposition based on the time series of hourly wind observations and mixing depths. Monthly average fine particle organic compound concentrations that would prevail if the primary organic aerosol were transported without chemical reaction were computed for more than 100 organic compounds within an 80 km × 80 km modeling area centered over Los Angeles. The monthly average compound concentrations predicted by the transport model were compared to atmospheric measurements made at monitoring sites within the study area during 1982. The predicted seasonal variation and absolute values of the concentrations of the more stable compounds are found to be in reasonable agreement with the ambient observations. While model predictions for the higher molecular weight polycyclic aromatic hydrocarbons (PAH) are in agreement with ambient observations, lower molecular weight PAH show much higher predicted than measured atmospheric concentrations in the particle phase, indicating atmospheric decay by chemical reactions or evaporation from the particle phase. The atmospheric concentrations of dicarboxylic acids and aromatic polycarboxylic acids greatly exceed the contributions that

Recent changes in particulate air pollution over China observed from space and the ground: effectiveness of emission control.

Science.gov (United States)

Lin, Jintai; Nielsen, Chris P; Zhao, Yu; Lei, Yu; Liu, Yang; McElroy, Michael B

2010-10-15

The Chinese government has moved aggressively since 2005 to reduce emissions of a number of pollutants including primary particulate matter (PM) and sulfur dioxide (SO(2)), efforts inadvertently aided since late 2008 by economic recession. Satellite observations of aerosol optical depth (AOD) and column nitrogen dioxide (NO(2)) provide independent indicators of emission trends, clearly reflecting the sharp onset of the recession in the fall of 2008 and rebound of the economy in the latter half of 2009. Comparison of AOD with ground-based observations of PM over a longer period indicate that emission-control policies have not been successful in reducing concentrations of aerosol pollutants at smaller size range over industrialized regions of China. The lack of success is attributed to the increasing importance of anthropogenic secondary aerosols formed from precursor species including nitrogen oxides (NO(x)), non-methane volatile organic compounds (NMVOC), and ammonia (NH(3)).

Sources and atmospheric processing of winter aerosols in Seoul, Korea: insights from real-time measurements using a high-resolution aerosol mass spectrometer

Science.gov (United States)

Kim, Hwajin; Zhang, Qi; Bae, Gwi-Nam; Kim, Jin Young; Bok Lee, Seung

2017-02-01

Highly time-resolved chemical characterization of nonrefractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital and largest metropolis of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter, when elevated particulate matter (PM) pollution events are often observed. This is the first time that detailed real-time aerosol measurement results have been reported from Seoul, Korea, and they reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicron aerosol (PM1 = NR-PM1+ black carbon (BC)) was 27.5 µg m-3, and the total mass was dominated by organics (44 %), followed by nitrate (24 %) and sulfate (10 %). The average atomic ratios of oxygen to carbon (O / C), hydrogen to carbon (H / C), and nitrogen to carbon (N / C) of organic aerosols (OA) were 0.37, 1.79, and 0.018, respectively, which result in an average organic mass-to-carbon (OM / OC) ratio of 1.67. The concentrations (2.6-90.7 µg m-3) and composition of PM1 varied dynamically during the measurement period due to the influences of different meteorological conditions, emission sources, and air mass origins. Five distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA, O / C = 0.06), cooking activities represented by a cooking OA factor (COA, O / C = 0.14), wood combustion represented by a biomass burning OA factor (BBOA, O / C = 0.34), and secondary organic aerosol (SOA) represented by a semivolatile oxygenated OA factor (SV-OOA, O / C = 0.56) and a low-volatility oxygenated OA factor (LV-OOA, O / C = 0.68). On average, primary OA (POA = HOA + COA + BBOA) accounted for 59 % the OA mass, whereas SV-OOA and LV-OOA contributed 15 and 26 %, respectively. Our results indicate that air

The impact of bark beetle infestations on monoterpene emissions and secondary organic aerosol formation in western North America

Directory of Open Access Journals (Sweden)

A. R. Berg

2013-03-01

Full Text Available Over the last decade, extensive beetle outbreaks in western North America have destroyed over 100 000 km2 of forest throughout British Columbia and the western United States. Beetle infestations impact monoterpene emissions through both decreased emissions as trees are killed (mortality effect and increased emissions in trees under attack (attack effect. We use 14 yr of beetle-induced tree mortality data together with beetle-induced monoterpene emission data in the National Center for Atmospheric Research (NCAR Community Earth System Model (CESM to investigate the impact of beetle-induced tree mortality and attack on monoterpene emissions and secondary organic aerosol (SOA formation in western North America. Regionally, beetle infestations may have a significant impact on monoterpene emissions and SOA concentrations, with up to a 4-fold increase in monoterpene emissions and up to a 40% increase in SOA concentrations in some years (in a scenario where the attack effect is based on observed lodgepole pine response. Responses to beetle attack depend on the extent of previous mortality and the number of trees under attack in a given year, which can vary greatly over space and time. Simulated enhancements peak in 2004 (British Columbia and 2008 (US. Responses to beetle attack are shown to be substantially larger (up to a 3-fold localized increase in summertime SOA concentrations in a scenario based on bark-beetle attack in spruce trees. Placed in the context of observations from the IMPROVE network, the changes in SOA concentrations due to beetle attack are in most cases small compared to the large annual and interannual variability in total organic aerosol which is driven by wildfire activity in western North America. This indicates that most beetle-induced SOA changes are not likely detectable in current observation networks; however, these changes may impede efforts to achieve natural visibility conditions in the national parks and wilderness

MODIS Observation of Aerosols over Southern Africa During SAFARI 2000: Data, Validation, and Estimation of Aerosol Radiative Forcing

Science.gov (United States)

Ichoku, Charles; Kaufman, Yoram; Remer, Lorraine; Chu, D. Allen; Mattoo, Shana; Tanre, Didier; Levy, Robert; Li, Rong-Rong; Kleidman, Richard; Lau, William K. M. (Technical Monitor)

2001-01-01

Aerosol properties, including optical thickness and size parameters, are retrieved operationally from the MODIS sensor onboard the Terra satellite launched on 18 December 1999. The predominant aerosol type over the Southern African region is smoke, which is generated from biomass burning on land and transported over the southern Atlantic Ocean. The SAFARI-2000 period experienced smoke aerosol emissions from the regular biomass burning activities as well as from the prescribed burns administered on the auspices of the experiment. The MODIS Aerosol Science Team (MAST) formulates and implements strategies for the retrieval of aerosol products from MODIS, as well as for validating and analyzing them in order to estimate aerosol effects in the radiative forcing of climate as accurately as possible. These activities are carried out not only from a global perspective, but also with a focus on specific regions identified as having interesting characteristics, such as the biomass burning phenomenon in southern Africa and the associated smoke aerosol, particulate, and trace gas emissions. Indeed, the SAFARI-2000 aerosol measurements from the ground and from aircraft, along with MODIS, provide excellent data sources for a more intensive validation and a closer study of the aerosol characteristics over Southern Africa. The SAFARI-2000 ground-based measurements of aerosol optical thickness (AOT) from both the automatic Aerosol Robotic Network (AERONET) and handheld Sun photometers have been used to validate MODIS retrievals, based on a sophisticated spatio-temporal technique. The average global monthly distribution of aerosol from MODIS has been combined with other data to calculate the southern African aerosol daily averaged (24 hr) radiative forcing over the ocean for September 2000. It is estimated that on the average, for cloud free conditions over an area of 9 million square kin, this predominantly smoke aerosol exerts a forcing of -30 W/square m C lose to the terrestrial

Real-Time Observations of Secondary Aerosol Formation and Aging from Different Emission Sources and Environments

Science.gov (United States)

Ortega, A. M.; Palm, B. B.; Hayes, P. L.; Day, D. A.; Cubison, M.; Brune, W. H.; Hu, W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Rappenglueck, B.; Bon, D.; Graus, M.; Warneke, C.; Gilman, J.; Kuster, W.; De Gouw, J. A.; Jimenez, J. L.

2013-12-01

To investigate atmospheric processing of direct urban and wildfire emissions, we deployed a photochemical flow reactor (Potential Aerosol Mass, PAM) with submicron aerosol size and chemical composition measurements during FLAME-3, a biomass-burning study at USDA Fire Sciences Laboratory in Missoula, MT, and CalNex, a field study investigating the nexus of air quality and climate change at a receptor site in the LA-Basin at Pasadena, CA. The reactor produces OH concentrations up to 4 orders of magnitude higher than in ambient air, achieving equivalent aging of ~2 weeks in 5 minutes of processing. The OH exposure (OHexp) was stepped every 20 min in both field studies. Results show the value of this approach as a tool for in-situ evaluation of changes in OA concentration and composition due to photochemical processing. In FLAME-3, the average OA enhancement factor was 1.42 × 0.36 of the initial POA. Reactive VOCs, such as toluene, monoterpenes, and acetaldehyde, decreased with increased OHexp; however, formic acid, acetone, and some unidentified OVOCs increased after significant exposure. Net SOA formation in the photochemical reactor increased with OHexp, typically peaking around 3 days of equivalent atmospheric photochemical age (OHexp ~3.9e11 molecules cm-3 s), then leveling off at higher exposures. Unlike other studies, no decrease in OA is observed at high exposure, likely due to lower max OHexp in this study due to very high OH reactivity. The amount of additional OA mass added from aging is positively correlated with initial POA concentration, but not with the total VOC concentration or the concentration of known SOA precursors. The mass of SOA formed often exceeded the mass of the known VOC precursors, indicating the likely importance of primary semivolatile/intermediate volatility species, and possibly of unidentified VOCs as SOA precursors in biomass burning smoke. Results from CalNex show enhancement of OA and inorganic aerosol from gas-phase precursors

Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability.

Science.gov (United States)

Ghan, Steven; Wang, Minghuai; Zhang, Shipeng; Ferrachat, Sylvaine; Gettelman, Andrew; Griesfeller, Jan; Kipling, Zak; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Zhang, Kai

2016-05-24

A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing.

The European aerosol budget in 2006

Directory of Open Access Journals (Sweden)

J. M. J. Aan de Brugh

2011-02-01

Full Text Available This paper presents the aerosol budget over Europe in 2006 calculated with the global transport model TM5 coupled to the size-resolved aerosol module M7. Comparison with ground observations indicates that the model reproduces the observed concentrations quite well with an expected slight underestimation of PM₁₀ due to missing emissions (e.g. resuspension. We model that a little less than half of the anthropogenic aerosols emitted in Europe are exported and the rest is removed by deposition. The anthropogenic aerosols are removed mostly by rain (95% and only 5% is removed by dry deposition. For the larger natural aerosols, especially sea salt, a larger fraction is removed by dry processes (sea salt: 70%, mineral dust: 35%. We model transport of aerosols in the jet stream in the higher atmosphere and an import of Sahara dust from the south at high altitudes. Comparison with optical measurements shows that the model reproduces the Ångström parameter very well, which indicates a correct simulation of the aerosol size distribution. However, we underestimate the aerosol optical depth. Because the surface concentrations are close to the observations, the shortage of aerosol in the model is probably at higher altitudes. We show that the discrepancies are mainly caused by an overestimation of wet-removal rates. To match the observations, the wet-removal rates have to be scaled down by a factor of about 5. In that case the modelled ground-level concentrations of sulphate and sea salt increase by 50% (which deteriorates the match, while other components stay roughly the same. Finally, it is shown that in particular events, improved fire emission estimates may significantly improve the ability of the model to simulate the aerosol optical depth. We stress that discrepancies in aerosol models can be adequately analysed if all models would provide (regional aerosol budgets, as presented in the current study.

Uncertainties in modelling the spatial and temporal variations in aerosol concentrations

NARCIS (Netherlands)

Meij, de A.

2009-01-01

Aerosols play a key role in air quality (health aspects) and climate. In this thesis atmospheric chemistry transport models are used to study the uncertainties in aerosol modelling and to evaluate the effects of emission reduction scenarios on air quality. Uncertainties in: the emissions of gas and

Secondary organic aerosol in the global aerosol – chemical transport model Oslo CTM2

Directory of Open Access Journals (Sweden)

I. S. A. Isaksen

2007-11-01

Full Text Available The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA. Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics. A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr−1 by allowing semi-volatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA is the dominant OA component than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%–60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for β-pinene is used for NO3 oxidation of all terpenes