WorldWideScience

Sample records for primary aerosol emissions

  1. Characterization of selenium in ambient aerosols and primary emission sources.

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    De Santiago, Arlette; Longo, Amelia F; Ingall, Ellery D; Diaz, Julia M; King, Laura E; Lai, Barry; Weber, Rodney J; Russell, Armistead G; Oakes, Michelle

    2014-08-19

    Atmospheric selenium (Se) in aerosols was investigated using X-ray absorption near-edge structure (XANES) spectroscopy and X-ray fluorescence (XRF) microscopy. These techniques were used to determine the oxidation state and elemental associations of Se in common primary emission sources and ambient aerosols collected from the greater Atlanta area. In the majority of ambient aerosol and primary emission source samples, the spectroscopic patterns as well as the absence of elemental correlations suggest Se is in an elemental, organic, or oxide form. XRF microscopy revealed numerous Se-rich particles, or hotspots, accounting on average for ∼16% of the total Se in ambient aerosols. Hotspots contained primarily Se(0)/Se(-II). However, larger, bulk spectroscopic characterizations revealed Se(IV) as the dominant oxidation state in ambient aerosol, followed by Se(0)/Se(-II) and Se(VI). Se(IV) was the only observed oxidation state in gasoline, diesel, and coal fly ash, while biomass burning contained a combination of Se(0)/Se(-II) and Se(IV). Although the majority of Se in aerosols was in the most toxic form, the Se concentration is well below the California Environmental Protection Agency chronic exposure limit (∼20000 ng/m(3)).

  2. Primary anthropogenic aerosol emission trends for China, 1990–2005

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    Y. Lei

    2011-02-01

    Full Text Available An inventory of anthropogenic primary aerosol emissions in China was developed for 1990–2005 using a technology-based approach. Taking into account changes in the technology penetration within industry sectors and improvements in emission controls driven by stricter emission standards, a dynamic methodology was derived and implemented to estimate inter-annual emission factors. Emission factors of PM2.5 decreased by 7%–69% from 1990 to 2005 in different industry sectors of China, and emission factors of TSP decreased by 18%–80% as well, with the measures of controlling PM emissions implemented. As a result, emissions of PM2.5 and TSP in 2005 were 11.0 Tg and 29.7 Tg, respectively, less than what they would have been without the adoption of these measures. Emissions of PM2.5, PM10 and TSP presented similar trends: they increased in the first six years of 1990s and decreased until 2000, then increased again in the following years. Emissions of TSP peaked (35.5 Tg in 1996, while the peak of PM10 (18.8 Tg and PM2.5 (12.7 Tg emissions occurred in 2005. Although various emission trends were identified across sectors, the cement industry and biofuel combustion in the residential sector were consistently the largest sources of PM2.5 emissions, accounting for 53%–62% of emissions over the study period. The non-metallic mineral product industry, including the cement, lime and brick industries, accounted for 54%–63% of national TSP emissions. There were no significant trends of BC and OC emissions until 2000, but the increase after 2000 brought the peaks of BC (1.51 Tg and OC (3.19 Tg emissions in 2005. Although significant improvements in the estimation of primary aerosols are presented here, there still exist large uncertainties. More accurate and detailed activity information and emission factors based on local tests are essential to further improve emission estimates

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

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    P. Q. Fu

    2013-02-01

    Full Text Available 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 for 1.8–11.0% (4.8% of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA tracers formed from the oxidation of biogenic volatile organic compounds (VOCs such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052–53.3 ng m−3 (9.2 ng m−3, followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC, we estimate that an average of 10.7% (up to 26.2% of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8% and α-pinene SOC (2.9%. In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.

  4. Global climate impacts of country-level primary carbonaceous aerosol from solid-fuel cookstove emissions

    International Nuclear Information System (INIS)

    Lacey, Forrest; Henze, Daven

    2015-01-01

    Cookstove use is globally one of the largest unregulated anthropogenic sources of primary carbonaceous aerosol. While reducing cookstove emissions through national-scale mitigation efforts has clear benefits for improving indoor and ambient air quality, and significant climate benefits from reduced green-house gas emissions, climate impacts associated with reductions to co-emitted black (BC) and organic carbonaceous aerosol are not well characterized. Here we attribute direct, indirect, semi-direct, and snow/ice albedo radiative forcing (RF) and associated global surface temperature changes to national-scale carbonaceous aerosol cookstove emissions. These results are made possible through the use of adjoint sensitivity modeling to relate direct RF and BC deposition to emissions. Semi- and indirect effects are included via global scaling factors, and bounds on these estimates are drawn from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. Absolute regional temperature potentials are used to estimate global surface temperature changes. Bounds are placed on these estimates, drawing from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. We estimate a range of 0.16 K warming to 0.28 K cooling with a central estimate of 0.06 K cooling from the removal of cookstove aerosol emissions. At the national emissions scale, countries’ impacts on global climate range from net warming (e.g., Mexico and Brazil) to net cooling, although the range of estimated impacts for all countries span zero given uncertainties in RF estimates and fuel characterization. We identify similarities and differences in the sets of countries with the highest emissions and largest cookstove temperature impacts (China, India, Nigeria, Pakistan, Bangladesh and Nepal), those with the largest temperature impact per carbon emitted (Kazakhstan, Estonia, and Mongolia), and those that would provide the

  5. Global climate impacts of country-level primary carbonaceous aerosol from solid-fuel cookstove emissions

    Science.gov (United States)

    Lacey, Forrest; Henze, Daven

    2015-11-01

    Cookstove use is globally one of the largest unregulated anthropogenic sources of primary carbonaceous aerosol. While reducing cookstove emissions through national-scale mitigation efforts has clear benefits for improving indoor and ambient air quality, and significant climate benefits from reduced green-house gas emissions, climate impacts associated with reductions to co-emitted black (BC) and organic carbonaceous aerosol are not well characterized. Here we attribute direct, indirect, semi-direct, and snow/ice albedo radiative forcing (RF) and associated global surface temperature changes to national-scale carbonaceous aerosol cookstove emissions. These results are made possible through the use of adjoint sensitivity modeling to relate direct RF and BC deposition to emissions. Semi- and indirect effects are included via global scaling factors, and bounds on these estimates are drawn from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. Absolute regional temperature potentials are used to estimate global surface temperature changes. Bounds are placed on these estimates, drawing from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. We estimate a range of 0.16 K warming to 0.28 K cooling with a central estimate of 0.06 K cooling from the removal of cookstove aerosol emissions. At the national emissions scale, countries’ impacts on global climate range from net warming (e.g., Mexico and Brazil) to net cooling, although the range of estimated impacts for all countries span zero given uncertainties in RF estimates and fuel characterization. We identify similarities and differences in the sets of countries with the highest emissions and largest cookstove temperature impacts (China, India, Nigeria, Pakistan, Bangladesh and Nepal), those with the largest temperature impact per carbon emitted (Kazakhstan, Estonia, and Mongolia), and those that would provide the

  6. A new physically-based quantification of marine isoprene and primary organic aerosol emissions

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    N. Meskhidze

    2009-07-01

    Full Text Available The global marine sources of organic carbon (OC are estimated here using a physically-based parameterization for the emission of marine isoprene and primary organic matter. The marine isoprene emission model incorporates new physical parameters such as light sensitivity of phytoplankton isoprene production and dynamic euphotic depth to simulate hourly marine isoprene emissions totaling 0.92 Tg C yr−1. Sensitivity studies using different schemes for the euphotic zone depth and ocean phytoplankton speciation produce the upper and the lower range of marine-isoprene emissions of 0.31 to 1.09 Tg C yr−1, respectively. Established relationships between sea spray fractionation of water-insoluble organic carbon (WIOC and chlorophyll-a concentration are used to estimate the total primary sources of marine sub- and super-micron OC of 2.9 and 19.4 Tg C yr−1, respectively. The consistent spatial and temporal resolution of the two emission types allow us, for the first time, to explore the relative contributions of sub- and super-micron organic matter and marine isoprene-derived secondary organic aerosol (SOA to the total OC fraction of marine aerosol. Using a fixed 3% mass yield for the conversion of isoprene to SOA, our emission simulations show minor (<0.2% contribution of marine isoprene to the total marine source of OC on a global scale. However, our model calculations also indicate that over the tropical oceanic regions (30° S to 30° N, marine isoprene SOA may contribute over 30% of the total monthly-averaged sub-micron OC fraction of marine aerosol. The estimated contribution of marine isoprene SOA to hourly-averaged sub-micron marine OC emission is even higher, approaching 50% over the vast regions of the oceans during the midday hours when isoprene emissions are highest. As it is widely believed that sub-micron OC has the potential to influence the cloud droplet activation of marine aerosols, our

  7. Quantitative evaluation of emission controls on primary and secondary organic aerosol sources during Beijing 2008 Olympics

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    S. Guo

    2013-08-01

    Full Text Available To assess the primary and secondary sources of fine organic aerosols after the aggressive implementation of air pollution controls during the 2008 Beijing Olympic Games, 12 h PM2.5 values were measured at an urban site at Peking University (PKU and an upwind rural site at Yufa during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region summer field campaign. The average PM2.5 concentrations were 72.5 ± 43.6 μg m−3 and 64.3 ± 36.2 μg m−3 (average ± standard deviation, below as the same at PKU and Yufa, respectively, showing the lowest concentrations in recent years. Combining the results from a CMB (chemical mass balance model and secondary organic aerosol (SOA tracer-yield model, five primary and four secondary fine organic aerosol sources were compared with the results from previous studies in Beijing. The relative contribution of mobile sources to PM2.5 concentrations was increased in 2008, with diesel engines contributing 16.2 ± 5.9% and 14.5 ± 4.1% and gasoline vehicles contributing 10.3 ± 8.7% and 7.9 ± 6.2% to organic carbon (OC at PKU and Yufa, respectively. Due to the implementation of emission controls, the absolute OC concentrations from primary sources were reduced during the Olympics, and the contributions from secondary formation of OC represented a larger relative source of fine organic aerosols. Compared with the non-controlled period prior to the Olympics, primary vehicle contributions were reduced by 30% at the urban site and 24% at the rural site. The reductions in coal combustion contributions were 57% at PKU and 7% at Yufa. Our results demonstrate that the emission control measures implemented in 2008 significantly alleviated the primary organic particle pollution in and around Beijing. However, additional studies are needed to provide a more comprehensive assessment of the emission control effectiveness on SOA formation.

  8. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996–2010

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    Z. Lu

    2011-09-01

    Full Text Available China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2 and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC emissions from these two countries for the period 1996–2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %–17 % due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs of SO2, BC, and OC emissions are estimated to be −16 %–17 %, −43 %–93 %, and −43 %–80 % for China, and −15 %–16 %, −41 %–87 %, and −44 %–92

  9. Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996-2010

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    Lu, Z.; Zhang, Q.; Streets, D. G.

    2011-09-01

    China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996-2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %-17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be -16 %-17 %, -43 %-93 %, and -43 %-80 % for China, and -15 %-16 %, -41 %-87 %, and -44 %-92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and

  10. Primary emissions and secondary aerosol production potential from woodstoves for residential heating: Influence of the stove technology and combustion efficiency

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    Bertrand, Amelie; Stefenelli, Giulia; Bruns, Emily A.; Pieber, Simone M.; Temime-Roussel, Brice; Slowik, Jay G.; Prévôt, André S. H.; Wortham, Henri; El Haddad, Imad; Marchand, Nicolas

    2017-11-01

    To reduce the influence of biomass burning on air quality, consumers are encouraged to replace their old woodstove with new and cleaner appliances. While their primary emissions have been extensively investigated, the impact of atmospheric aging on these emissions, including secondary organic aerosol (SOA) formation, remains unknown. Here, using an atmospheric smog chamber, we aim at understanding the chemical nature and quantify the emission factors of the primary organic aerosols (POA) from three types of appliances for residential heating, and to assess the influence of aging thereon. Two, old and modern, logwood stoves and one pellet burner were operated under typical conditions. Emissions from an entire burning cycle (past the start-up operation) were injected, including the smoldering and flaming phases, resulting in highly variable emission factors. The stoves emitted a significant fraction of POA (up to 80%) and black carbon. After ageing, the total mass concentration of organic aerosol (OA) increased on average by a factor of 5. For the pellet stove, flaming conditions were maintained throughout the combustion. The aerosol was dominated by black carbon (over 90% of the primary emission) and amounted to the same quantity of primary aerosol emitted by the old logwood stove. However, after ageing, the OA mass was increased by a factor of 1.7 only, thus rendering OA emissions by the pellet stove almost negligible compared to the other two stoves tested. Therefore, the pellet stove was the most reliable and least polluting appliance out of the three stoves tested. The spectral signatures of the POA and aged emissions by a High Resolution - Time of Flight - Aerosol Mass Spectrometer (Electron Ionization (EI) at 70 eV) were also investigated. The m/z 44 (CO2+) and high molecular weight fragments (m/z 115 (C9H7+), 137 (C8H9O2+), 167 (C9H11O3+) and 181 (C9H9O4+, C14H13+)) correlate with the modified combustion efficiency (MCE) allowing us to discriminate further

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

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    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

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

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    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

  13. Open burning of rice, corn and wheat straws: primary emissions, photochemical aging, and secondary organic aerosol formation

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    Fang, Zheng; Deng, Wei; Zhang, Yanli; Ding, Xiang; Tang, Mingjin; Liu, Tengyu; Hu, Qihou; Zhu, Ming; Wang, Zhaoyi; Yang, Weiqiang; Huang, Zhonghui; Song, Wei; Bi, Xinhui; Chen, Jianmin; Sun, Yele; George, Christian; Wang, Xinming

    2017-12-01

    Agricultural residues are among the most abundant biomass burned globally, especially in China. However, there is little information on primary emissions and photochemical evolution of agricultural residue burning. In this study, indoor chamber experiments were conducted to investigate primary emissions from open burning of rice, corn and wheat straws and their photochemical aging as well. Emission factors of NOx, NH3, SO2, 67 non-methane hydrocarbons (NMHCs), particulate matter (PM), organic aerosol (OA) and black carbon (BC) under ambient dilution conditions were determined. Olefins accounted for > 50 % of the total speciated NMHCs emission (2.47 to 5.04 g kg-1), indicating high ozone formation potential of straw burning emissions. Emission factors of PM (3.73 to 6.36 g kg-1) and primary organic carbon (POC, 2.05 to 4.11 gC kg-1), measured at dilution ratios of 1300 to 4000, were lower than those reported in previous studies at low dilution ratios, probably due to the evaporation of semi-volatile organic compounds under high dilution conditions. After photochemical aging with an OH exposure range of (1.97-4.97) × 1010 molecule cm-3 s in the chamber, large amounts of secondary organic aerosol (SOA) were produced with OA mass enhancement ratios (the mass ratio of total OA to primary OA) of 2.4-7.6. The 20 known precursors could only explain 5.0-27.3 % of the observed SOA mass, suggesting that the major precursors of SOA formed from open straw burning remain unidentified. Aerosol mass spectrometry (AMS) signaled that the aged OA contained less hydrocarbons but more oxygen- and nitrogen-containing compounds than primary OA, and carbon oxidation state (OSc) calculated with AMS resolved O / C and H / C ratios increased linearly (p < 0.001) with OH exposure with quite similar slopes.

  14. Time-resolved analysis of primary volatile emissions and secondary aerosol formation potential from a small-scale pellet boiler

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    Czech, Hendryk; Pieber, Simone M.; Tiitta, Petri; Sippula, Olli; Kortelainen, Miika; Lamberg, Heikki; Grigonyte, Julija; Streibel, Thorsten; Prévôt, André S. H.; Jokiniemi, Jorma; Zimmermann, Ralf

    2017-06-01

    Small-scale pellet boilers and stoves became popular as a wood combustion appliance for domestic heating in Europe, North America and Asia due to economic and environmental aspects. Therefore, an increasing contribution of pellet boilers to air pollution is expected despite their general high combustion efficiency. As emissions of primary organic aerosol (POA) and permanent gases of pellet boilers are well investigated, the scope of this study was to investigate the volatile organic emissions and the formation potential of secondary aerosols for this type of appliance. Fresh and aged emissions were analysed by a soot-particle aerosol time-of-flight mass spectrometry (SP-AMS) and the molecular composition of the volatile precursors with single-photon ionisation time-of-flight mass spectrometry (SPI-TOFMS) at different pellet boiler operation conditions. Organic emissions in the gas phase were dominated by unsaturated hydrocarbons while wood-specific VOCs, e.g. phenolic species or substituted furans, were only detected during the starting phase. Furthermore, organic emissions in the gas phase were found to correlate with fuel grade and combustion technology in terms of secondary air supply. Secondary organic aerosols of optimised pellet boiler conditions (OPT, state-of-the-art combustion appliance) and reduced secondary air supply (RSA, used as a proxy for pellet boilers of older type) were studied by simulating atmospheric ageing in a Potential Aerosol Mass (PAM) flow reactor. Different increases in OA mass (55% for OPT, 102% for RSA), associated with higher average carbon oxidation state and O:C, could be observed in a PAM chamber experiment. Finally, it was found that derived SOA yields and emission factors were distinctly lower than reported for log wood stoves.

  15. Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations.

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    Mohr, Claudia; Huffman, Alex; Cubison, Michael J; Aiken, Allison C; Docherty, Kenneth S; Kimmel, Joel R; Ulbrich, Ingrid M; Hannigan, Michael; Jimenez, Jose L

    2009-04-01

    Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS). High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning emissions contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to those from ambient hydrocarbon-like OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from these sources is unlikelyto be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/zs that may be useful for differentiating some of these sources. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, whereas motor vehicle emissions have very low signal at this m/z.

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

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    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.

  17. 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

  18. Primary emissions and secondary organic aerosol formation from the exhaust of a flex-fuel (ethanol) vehicle

    Science.gov (United States)

    Suarez-Bertoa, R.; Zardini, A. A.; Platt, S. M.; Hellebust, S.; Pieber, S. M.; El Haddad, I.; Temime-Roussel, B.; Baltensperger, U.; Marchand, N.; Prévôt, A. S. H.; Astorga, C.

    2015-09-01

    Incentives to use biofuels may result in increasing vehicular emissions of compounds detrimental to air quality. Therefore, regulated and unregulated emissions from a Euro 5a flex-fuel vehicle, tested using E85 and E75 blends (gasoline containing 85% and 75% of ethanol (vol/vol), respectively), were investigated at 22 and -7 °C over the New European Driving Cycle, at the Vehicle Emission Laboratory at the European Commission Joint Research Centre Ispra, Italy. Vehicle exhaust was comprehensively analyzed at the tailpipe and in a dilution tunnel. A fraction of the exhaust was injected into a mobile smog chamber to study the photochemical aging of the mixture. We found that emissions from a flex-fuel vehicle, fueled by E85 and E75, led to secondary organic aerosol (SOA) formation, despite the low aromatic content of these fuel blends. Emissions of regulated and unregulated compounds, as well as emissions of black carbon (BC) and primary organic aerosol (POA) and SOA formation were higher at -7 °C. The flex-fuel unregulated emissions, mainly composed of ethanol and acetaldehyde, resulted in very high ozone formation potential and SOA, especially at low temperature (860 mg O3 km-1 and up to 38 mg C kg-1). After an OH exposure of 10 × 106 cm-3 h, SOA mass was, on average, 3 times larger than total primary particle mass emissions (BC + POA) with a high O:C ratio (up to 0.7 and 0.5 at 22 and -7 °C, respectively) typical of highly oxidized mixtures. Furthermore, high resolution organic mass spectra showed high 44/43 ratios (ratio of the ions m/z 44 and m/z 43) characteristic of low-volatility oxygenated organic aerosol. We also hypothesize that SOA formation from vehicular emissions could be due to oxidation products of ethanol and acetaldehyde, both short-chain oxygenated VOCs, e.g. methylglyoxal and acetic acid, and not only from aromatic compounds.

  19. 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.

  20. 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...

  1. 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 ...

  2. 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

  3. 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.

  4. Local emission of primary air pollutants and its contribution to wet deposition and concentrations of aerosols and gases in ambient air in Japan

    Science.gov (United States)

    Aikawa, Masahide; Hiraki, Takatoshi; Tomoyose, Nobutaka; Ohizumi, Tsuyoshi; Noguchi, Izumi; Murano, Kentaro; Mukai, Hitoshi

    2013-11-01

    We studied wet deposition by precipitation and the concentrations of aerosols and gases in ambient air in relation to the primary air pollutants discharged from domestic areas. The concentrations of aerosols and gases were influenced by nearby emissions except for non-sea-salt SO, which is transported long distances. The area facing the Sea of Japan showed much larger wet deposition than other areas, although the domestic emissions of the primary air pollutants there were small and showed a peak in wet deposition from October to March, as distinct from April to September in other areas. We performed the correlation analyses between wet deposition of each component and the product of the concentrations of corresponding aerosols and gases in ambient air and the two-thirds power of the precipitation. From the results, following scavenging processes were suggested. • Sulfate and ammonium were scavenged in precipitation as particulate matter such as (NH4)2SO4 and NH4HSO4. • Nitrate was scavenged mainly in precipitation through gaseous HNO3. • Ammonium was complementarily scavenged in precipitation through aerosols such as (NH4)2SO4 and NH4HSO4 and through gaseous NH3.

  5. 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

  6. The primary volcanic aerosol emission from Mt Etna: Size-resolved particles with SO2 and role in plume reactive halogen chemistry

    Science.gov (United States)

    Roberts, T. J.; Vignelles, D.; Liuzzo, M.; Giudice, G.; Aiuppa, A.; Coltelli, M.; Salerno, G.; Chartier, M.; Couté, B.; Berthet, G.; Lurton, T.; Dulac, F.; Renard, J.-B.

    2018-02-01

    Volcanoes are an important source of aerosols to the troposphere. Within minutes after emission, volcanic plume aerosol catalyses conversion of co-emitted HBr, HCl into highly reactive halogens (e.g. BrO, OClO) through chemical cycles that cause substantial ozone depletion in the dispersing downwind plume. This study quantifies the sub-to-supramicron primary volcanic aerosol emission (0.2-5 μm diameter) and its role in this process. An in-situ ground-based study at Mt Etna (Italy) during passive degassing co-deployed an optical particle counter and Multi-Gas SO2 sensors at high time resolution (0.1 Hz) enabling to characterise the aerosol number, size-distribution and emission flux. A tri-modal volcanic aerosol size distribution was found, to which lognormal distributions are fitted. Total particle volume correlates to SO2 (as a plume tracer). The measured particle volume:SO2 ratio equates to a sulfate:SO2 ratio of 1-2% at the observed meteorological conditions (40% Relative Humidity). A particle mass flux of 0.7 kg s-1 is calculated for the measured Mt Etna SO2 flux of 1950 tonnes/day. A numerical plume atmospheric chemistry model is used to simulate the role of the hygroscopic primary aerosol surface area and its humidity dependence on volcanic plume BrO and OClO chemistry. As well as predicting volcanic BrO formation and O3 depletion, the model achieves OClO/SO2 in broad quantitative agreement with recently reported Mt Etna observations, with a predicted maximum a few minutes downwind. In addition to humidity - that enhances aerosols surface area for halogen cycling - background ozone is predicted to be an important control on OClO/SO2. Dependence of BrO/SO2 on ambient humidity is rather low near-to-source but increases further downwind. The model plume chemistry also exhibits strong across-plume spatial variations between plume edge and centre.

  7. 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.

  8. 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; 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.

  9. 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

  10. 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.

  11. Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

    Science.gov (United States)

    Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

    2018-04-01

    In the frame of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), we analyse the budget of primary aerosols and secondary inorganic aerosols over the Mediterranean Basin during the years 2012 and 2013. To do this, we use two year-long numerical simulations with the chemistry-transport model MOCAGE validated against satellite- and ground-based measurements. The budget is presented on an annual and a monthly basis on a domain covering 29 to 47° N latitude and 10° W to 38° E longitude. The years 2012 and 2013 show similar seasonal variations. The desert dust is the main contributor to the annual aerosol burden in the Mediterranean region with a peak in spring, and sea salt being the second most important contributor. The secondary inorganic aerosols, taken as a whole, contribute a similar level to sea salt. The results show that all of the considered aerosol types, except for sea salt aerosols, experience net export out of our Mediterranean Basin model domain, and thus this area should be considered as a source region for aerosols globally. Our study showed that 11 % of the desert dust, 22.8 to 39.5 % of the carbonaceous aerosols, 35 % of the sulfate and 9 % of the ammonium emitted or produced into the study domain are exported. The main sources of variability for aerosols between 2012 and 2013 are weather-related variations, acting on emissions processes, and the episodic import of aerosols from North American fires. In order to assess the importance of the anthropogenic emissions of the marine and the coastal areas which are central for the economy of the Mediterranean Basin, we made a sensitivity test simulation. This simulation is similar to the reference simulation but with the removal of the international shipping emissions and the anthropogenic emissions over a 50 km wide band inland along the coast. We showed that around 30 % of the emissions of carbonaceous aerosols and 35 to 60 % of the exported carbonaceous aerosols originates from the marine and

  12. 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.

  13. Dissecting Future Aerosol Emissions. Warming Tendencies and Mitigation Opportunities

    Energy Technology Data Exchange (ETDEWEB)

    Streets, D.G. [Decision and Information Sciences Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL, 60439 (United States)

    2007-04-15

    Future global emissions of aerosols will play an important role in governing the nature and magnitude of future anthropogenic climate change. We present in this paper a number of future scenarios of emissions of black carbon (BC) and organic carbon (OC) by world region, which we combine with sulfate (SO4) assessed in terms of the emissions of its precursor, SO2. We find that aerosol emissions from the household and industrial sectors are likely to decline along almost all future pathways. Transportation emissions, however, are subject to complex interacting forces that can lead to either increases or decreases. Biomass burning declines in many scenarios, but the Amazon rainforests remain vulnerable if unsustainable economic growth persists. East Asia is the key region for primary aerosols, and trends in China will have a major bearing on the direction and magnitude of releases of BC (expected reductions in the range of 640-1290 Gg), OC (reductions of 520-1900 Gg), and SO2 (ranging from an increase of 21 Tg to a reduction of 30 Tg). Analysis of joint BC, OC, and SO2 emission changes identifies a number of key world regions and economic sectors that could be effectively targeted for aerosol reductions.

  14. 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

  15. 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.

  16. 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

  17. 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

  18. 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

  19. 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

  20. 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.

  1. Evaluating Simulated Primary Anthropogenic and Biomass Burning Organic Aerosols during MILAGRO: Implications for Assessing Treatments of Secondary Organic Aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Fast, Jerome D.; Aiken, Allison; Allan, James D.; Alexander, M. L.; Campos, Teresa; Canagaratna, Manjula R.; Chapman, Elaine G.; DeCarlo, Peter; de Foy, B.; Gaffney, Jeffrey; de Gouw, Joost A.; Doran, J. C.; Emmons, L.; Hodzic, Alma; Herndon, Scott C.; Huey, L. G.; Jayne, John T.; Jimenez, Jose L.; Kleinman, Lawrence I.; Kuster, W. C.; Marley, Nancy A.; Russell, Lynn M.; Ochoa, Carlos; Onasch, Timothy B.; Pekour, Mikhail S.; Song, Chen; Ulbrich, Ingrid M.; Warneke, Carsten; Welsh-Bon, Daniel; Wiedinmyer, Christine; Worsnop, Douglas R.; Yu, Xiao-Ying; Zaveri, Rahul A.

    2009-08-31

    Simulated primary organic aerosols (POA), as well as other particulates and trace gases, in the vicinity of Mexico City are evaluated using measurements collected during the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaigns. Since the emission inventories and dilution will affect predictions of total organic matter and consequently total particulate matter, our objective is to assess the uncertainties in predicted POA before testing and evaluating the performance of secondary organic aerosol (SOA) treatments. Carbon monoxide (CO) is well simulated on most days both over the city and downwind, indicating that transport and mixing processes were usually consistent with the meteorological conditions observed during MILAGRO. Predicted and observed elemental carbon (EC) in the city was similar, but larger errors occurred at remote locations since the CO/EC emission ratios in the national emission inventory were lower than in the metropolitan emission inventory. Components of organic aerosols derived from Positive Matrix Factorization and data from several Aerodyne Aerosol Mass Spectrometer instruments deployed both at ground sites and on research aircraft are used to evaluate the model. Predicted POA was consistently lower than the measured organic matter at the ground sites, which is consistent with the expectation that SOA should be a large fraction of the total organic matter mass. A much better agreement was found when predicted POA was compared with the sum of "primary anthropogenic" and "primary biomass burning" components on days with relatively low biomass burning, suggesting that the overall magnitude of primary organic particulates released was reasonable. The predicted POA was greater than the total observed organic matter when the aircraft flew directly downwind of large fires, suggesting that biomass burning emission estimates from some large fires may be too high. Predicted total observed organic carbon (TOOC) was

  2. 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

  3. 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

  4. 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.

  5. 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.

  6. 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.

  7. 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

  8. 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.

  9. 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

  10. 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

  11. 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 Dp 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.

  12. 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

  13. 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

  14. Gas phase emissions from cooking processes and their secondary aerosol production potential

    Science.gov (United States)

    Klein, Felix; Platt, Stephen; Bruns, Emily; Termime-roussel, Brice; Detournay, Anais; Mohr, Claudia; Crippa, Monica; Slowik, Jay; Marchand, Nicolas; Baltensperger, Urs; Prevot, Andre; El Haddad, Imad

    2014-05-01

    Long before the industrial evolution and the era of fossil fuels, high concentrations of aerosol particles were alluded to in heavily populated areas, including ancient Rome and medieval London. Recent radiocarbon measurements (14C) conducted in modern megacities came as a surprise: carbonaceous aerosol (mainly organic aerosol, OA), a predominant fraction of particulate matter (PM), remains overwhelmingly non-fossil despite extensive fossil fuel combustion. Such particles are directly emitted (primary OA, POA) or formed in-situ in the atmosphere (secondary OA, SOA) via photochemical reactions of volatile organic compounds (VOCs). Urban levels of non-fossil OA greatly exceed the levels measured in pristine environments strongly impacted by biogenic emissions, suggesting a contribution from unidentified anthropogenic non-fossil sources to urban OA. Positive matrix factorization (PMF) techniques applied to ambient aerosol mass spectrometer (AMS, Aerodyne) data identify primary cooking emissions (COA) as one of the main sources of primary non-fossil OA in major cities like London (Allan et al., 2010), New York (Sun et al., 2011) and Beijing (Huang et al., 2010). Cooking processes can also emit VOCs that can act as SOA precursors, potentially explaining in part the high levels of oxygenated OA (OOA) identified by the AMS in urban areas. However, at present, the chemical nature of these VOCs and their secondary aerosol production potential (SAPP) remain virtually unknown. The approach adopted here involves laboratory quantification of PM and VOC emission factors from the main primary COA emitting processes and their SAPP. Primary emissions from deep-fat frying, vegetable boiling, vegetable frying and meat cooking for different oils, meats and vegetables were analysed under controlled conditions after ~100 times dilution. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a high resolution proton transfer time-of-flight mass spectrometer (PTR

  15. 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

  16. 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

  17. 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.

  18. 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

  19. Could aerosol emissions be used for regional heat wave mitigation?

    Directory of Open Access Journals (Sweden)

    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

  20. 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

  1. 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

  2. Continental anthropogenic primary particle number emissions

    Directory of Open Access Journals (Sweden)

    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

  3. 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

  4. 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

  5. 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.

  6. Photochemical production of aerosols from real plant emissions

    Directory of Open Access Journals (Sweden)

    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.

  7. 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.

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

    Science.gov (United States)

    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.

  9. 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

  10. 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

  11. 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.

  12. 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

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

    Science.gov (United States)

    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.

  14. 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

  15. 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.

  16. 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

  17. 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)

  18. 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.

  19. Microbiology and atmospheric processes: chemical interactions of primary biological aerosols

    Directory of Open Access Journals (Sweden)

    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.

  20. Significance of Future Biogenic and Fire Emissions on Regional Aerosol Burden

    Science.gov (United States)

    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

  1. 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)

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

    Science.gov (United States)

    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.

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

    Directory of Open Access Journals (Sweden)

    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

  4. 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

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

    Directory of Open Access Journals (Sweden)

    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.

  6. 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.

  7. 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.

  8. 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

  9. 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.

  10. 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.

  11. 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.

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

    Science.gov (United States)

    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

  13. 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.

  14. 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

  15. 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...

  16. 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,...

  17. Effects of aerosol emission pathways on future warming and human health

    Science.gov (United States)

    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

  18. 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

  19. 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

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

    Science.gov (United States)

    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

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

    Science.gov (United States)

    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.

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

    Directory of Open Access Journals (Sweden)

    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.

  3. 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 NOx 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

  4. 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.

  5. 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...

  6. 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.

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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.

  9. 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

  10. 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.

  11. 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.

  12. 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.

  13. Secondary emission electron gun using external primaries

    Science.gov (United States)

    Srinivasan-Rao, Triveni [Shoreham, NY; Ben-Zvi, Ilan [Setauket, NY

    2009-10-13

    An electron gun for generating an electron beam is provided, which includes a secondary emitter. The secondary emitter includes a non-contaminating negative-electron-affinity (NEA) material and emitting surface. The gun includes an accelerating region which accelerates the secondaries from the emitting surface. The secondaries are emitted in response to a primary beam generated external to the accelerating region. The accelerating region may include a superconducting radio frequency (RF) cavity, and the gun may be operated in a continuous wave (CW) mode. The secondary emitter includes hydrogenated diamond. A uniform electrically conductive layer is superposed on the emitter to replenish the extracted current, preventing charging of the emitter. An encapsulated secondary emission enhanced cathode device, useful in a superconducting RF cavity, includes a housing for maintaining vacuum, a cathode, e.g., a photocathode, and the non-contaminating NEA secondary emitter with the uniform electrically conductive layer superposed thereon.

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

    Directory of Open Access Journals (Sweden)

    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

  15. 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

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

    Directory of Open Access Journals (Sweden)

    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.

  17. 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

  18. 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

  19. Aerosol Emissions from Great Lakes Harmful Algal Blooms

    Energy Technology Data Exchange (ETDEWEB)

    May, Nathaniel W. [Department; Olson, Nicole E. [Department; Panas, Mark [Department; Axson, Jessica L. [Department; Tirella, Peter S. [Department; Kirpes, Rachel M. [Department; Craig, Rebecca L. [Department; Gunsch, Matthew J. [Department; China, Swarup [William; Laskin, Alexander [William; Ault, Andrew P. [Department; Department; Pratt, Kerri A. [Department; Department

    2017-12-20

    In freshwater lakes, harmful algal blooms (HABs) of Cyanobacteria (blue-green algae) produce toxins that impact human health. However, little is known about the chemical species present in lake spray aerosol (LSA) produced from wave-breaking in freshwater HABs. In this study, a laboratory LSA generator produced aerosols from freshwater samples collected from Lake Michigan and Lake Erie during HAB and non-bloom conditions. Particles were analyzed for size and chemical composition by single particle mass spectrometry, electron microscopy, and fluorescence microscopy, with three distinct types of LSA identified with varying levels of organic carbon and biological material associated with calcium salts. LSA autofluorescence increases with blue-green algae concentration, showing that organic molecules of biological origin are incorporated in LSA from HABs. The number fraction of LSA with biological mass spectral markers also increases with particle diameter (greater than 0.5 μm), showing that HABs have size-dependent impacts on aerosol composition. The highest number fraction of LSA enriched in organic carbon were observed in particles less than 0.5 μm in diameter. Understanding the transfer of organic and biogenic material from freshwater to the atmosphere via LSA particles is crucial for determining health and climate effects due to HABs.

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

    Directory of Open Access Journals (Sweden)

    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.

  1. 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.

  2. 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

  3. Characterization of fresh and aged organic aerosol emissions from meat charbroiling

    Directory of Open Access Journals (Sweden)

    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.

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

    Science.gov (United States)

    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.

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

    Directory of Open Access Journals (Sweden)

    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

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

    Directory of Open Access Journals (Sweden)

    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

  7. 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

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

    Directory of Open Access Journals (Sweden)

    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.

  9. 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

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

    Directory of Open Access Journals (Sweden)

    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.

  11. 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.

  12. 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

  13. 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.)

  14. 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.

  15. Laboratory investigation of fire radiative energy and smoke aerosol emissions

    Science.gov (United States)

    Charles Ichoku; J. Vanderlei Martins; Yoram J. Kaufman; Martin J. Wooster; Patrick H. Freeborn; Wei Min Hao; Stephen Baker; Cecily A. Ryan; Bryce L. Nordgren

    2008-01-01

    Fuel biomass samples from southern Africa and the United States were burned in a laboratory combustion chamber while measuring the biomass consumption rate, the fire radiative energy (FRE) release rate (Rfre), and the smoke concentrations of carbon monoxide (CO), carbon dioxide (CO2), and particulate matter (PM). The PM mass emission rate (RPM) was quantified from...

  16. Secondary organic aerosol production from modern diesel engine emissions

    Directory of Open Access Journals (Sweden)

    S. Samy

    2010-01-01

    Full Text Available Secondary organic aerosol (SOA production was observed at significant levels in a series of modern diesel exhaust (DE aging experiments conducted at the European Outdoor Photoreactor/Simulation Chamber (EUPHORE. The greatest production occurred in DE with toluene addition experiments (>40%, followed by DE with HCHO (for OH radical generation experiments. A small amount of SOA (3% was observed for DE in dark with N2O5 (for NO3 radical production experiments. The analysis for a limited number (54 of polar organic compounds (POC was conducted to assess the composition of modern DE and the formation of photochemical transformation products. Distinct POC formation in light versus dark experiments suggests the role of OH initiated reactions in these chamber atmospheres. A trend of increasing concentrations of dicarboxylic acids in light versus dark experiments was observed when evaluated on a compound group basis. The four toluene addition experiments in this study were performed at different [tol]o/[NOx]o ratios and displayed an average SOA %yield (in relation to toluene of 5.3±1.6%, which is compared to past chamber studies that evaluated the impact of [tol]o/[NOx]o on SOA production in more simplified mixtures.

  17. 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

  18. 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

  19. 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)

  20. 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

  1. Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties

    Directory of Open Access Journals (Sweden)

    J. Zábori

    2013-05-01

    Full Text Available Primary marine aerosols (PMAs are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent, will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (Tw range between −1°C and 15°C. A sharp decrease in PMA emissions for a Tw increase from −1°C to 4°C was followed by a lower rate of change in PMA emissions for Tw up to about 6°C. Near constant number concentrations for water temperatures between 6°C to 10°C and higher were recorded. Even though the total particle number concentration changes for overlapping Tw ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for a dry diameter (DpDp > 0.125μm, the particle number concentrations during winter were mostly higher than in summer (up to 50%. The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in Tw from −1°C to 10°C during winter measurements showed a decrease in the peak of relative particle number concentration at about a Dp of 0.180μm, while an increase was observed for particles with Dp > 1μm. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of Tw in the range

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

    Directory of Open Access Journals (Sweden)

    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.

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

    Directory of Open Access Journals (Sweden)

    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.

  4. 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.)

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

    Directory of Open Access Journals (Sweden)

    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.

  6. 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.

  7. 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

  8. 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

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

    Science.gov (United States)

    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

  10. 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.

  11. 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

  12. 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

  13. 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

  14. 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

  15. 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.

  16. 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

  17. 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.

  18. 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

  19. 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.

  20. 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

  1. 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.

  2. 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.

  3. 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.

  4. 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

  5. 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

  6. 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).

  7. 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

  8. 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

  9. 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...

  10. 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

  11. 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

  12. 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)

  13. 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.

  14. Atmospheric emitted radiance interferometer (AERI): Status and the aerosol explanation for extra window region emissions

    Energy Technology Data Exchange (ETDEWEB)

    Revercomb, H.E.; Knuteson, R.O.; Best, F.A.; Dirkx, T.P. [Univ. of Wisconsin, Madison, WI (United States)] [and others

    1996-04-01

    High spectral resolution observations of downwelling emission from 3 to 19 microns have been made by the Atmospheric Emitted Radiance Interferometer (AERI) Prototype at the Southern Great Plains (SGP) Cloud and Radiative Testbed (CART) site for over two years. The spectral data set from AERI provides a basis for improving clear sky radiative transfer; determining the radiative impact of clouds, including the derivation of cloud radiative properties; defining the influences of aerosols in the window regions; and retrieving boundary layer state properties, including temperature, water vapor, and other trace gases. The data stream of radiometrically and spectrally calibrated radiances is routinely provided by Pacific Northwest Laboratory (PNL) to those science teams requesting it, and further information on the instrument and data characteristics is available in the ARM Science Team proceedings for 1993 and 1994 and in several conference publications. This paper describes the AERI status, calibration, field experiment wit a new AERI-01 and schedule, window region emissions, and future AERI plans.

  15. 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

  16. 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.

  17. 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.

  18. Evaluation of hierarchical agglomerative cluster analysis methods for discrimination of primary biological aerosol

    Directory of Open Access Journals (Sweden)

    I. Crawford

    2015-11-01

    Full Text Available In this paper we present improved methods for discriminating and quantifying primary biological aerosol particles (PBAPs by applying hierarchical agglomerative cluster analysis to multi-parameter ultraviolet-light-induced fluorescence (UV-LIF spectrometer data. The methods employed in this study can be applied to data sets in excess of 1 × 106 points on a desktop computer, allowing for each fluorescent particle in a data set to be explicitly clustered. This reduces the potential for misattribution found in subsampling and comparative attribution methods used in previous approaches, improving our capacity to discriminate and quantify PBAP meta-classes. We evaluate the performance of several hierarchical agglomerative cluster analysis linkages and data normalisation methods using laboratory samples of known particle types and an ambient data set. Fluorescent and non-fluorescent polystyrene latex spheres were sampled with a Wideband Integrated Bioaerosol Spectrometer (WIBS-4 where the optical size, asymmetry factor and fluorescent measurements were used as inputs to the analysis package. It was found that the Ward linkage with z-score or range normalisation performed best, correctly attributing 98 and 98.1 % of the data points respectively. The best-performing methods were applied to the BEACHON-RoMBAS (Bio–hydro–atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen–Rocky Mountain Biogenic Aerosol Study ambient data set, where it was found that the z-score and range normalisation methods yield similar results, with each method producing clusters representative of fungal spores and bacterial aerosol, consistent with previous results. The z-score result was compared to clusters generated with previous approaches (WIBS AnalysiS Program, WASP where we observe that the subsampling and comparative attribution method employed by WASP results in the overestimation of the fungal spore concentration by a factor of 1.5 and the

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

    Energy Technology Data Exchange (ETDEWEB)

    Annette Rohr

    2005-09-30

    This report documents progress made on the subject project during the period of March 1, 2005 through August 31, 2005. 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 performance and analysis of field experiments at the first TERESA plant, located in the Upper Midwest and henceforth referred to as Plant 0, and at two additional coal-fired power plants (Plants 1 and 2) utilizing different coal types and with different plant configurations. During this reporting period, fieldwork was completed at Plant 1, located in the Southeast. Stage I toxicological assessments were carried out in normal Sprague-Dawley rats, and Stage II assessments were carried out in a compromised model (myocardial infarction-MI-model). Normal rats were exposed to the following atmospheric scenarios: (1) primary particles; (2) oxidized emissions; (3) oxidized emissions + secondary organic aerosol (SOA)--this scenario was repeated; and (4) oxidized emissions + ammonia + SOA. Compromised animals were exposed to oxidized emissions + SOA (this scenario was also conducted in replicate). Stage I assessment endpoints included breathing pattern/pulmonary function; in vivo chemiluminescence (an indicator of oxidative stress); blood cytology; bronchoalveolar lavage (BAL) fluid analysis; and histopathology. Stage II assessments included continuous ECG monitoring via

  20. 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.

  1. 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

  2. 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.; hide

    2016-01-01

    Emissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC-8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for 1.2 h. A Lagrangian plume cross-section model was used to simulate the evolution of ozone (O3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO2 and fine particles, especially primary OA and chloride. Filter-based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O3, peroxyacetyl nitrate (PAN), and nitrate was observed with (Delta)O3/(Delta)CO, (Delta)PAN/(Delta)NOy, and (Delta)nitrate/(Delta)NOy reaching approx. 0.1, approx. 0.3, and approx.0.3. For five selected cases, the model reasonably simulated O3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen-to-carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO2, NOx, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of approx. 2) to be equivalent to approx. 2% SO2 from coal combustion and approx. 1% NOx and approx. 9% CO from mobile sources.

  3. 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, ...

  4. 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...

  5. 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

  6. Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory

    Energy Technology Data Exchange (ETDEWEB)

    McMeeking, Gavin R.; Kreidenweis, Sonia M.; Baker, Stephen; Carrico, Christian M.; Chow, Judith C.; Collett, Jr., Jeffrey L.; Hao, Wei Min; Holden, Amanda S.; Kirchstetter, Thomas W.; Malm, William C.; Moosmuller, Hans; Sullivan, Amy P.; Wold, Cyle E.

    2009-05-15

    We characterized the gas- and speciated aerosol-phase emissions from the open combustion of 33 different plant species during a series of 255 controlled laboratory burns during the Fire Laboratory at Missoula Experiments (FLAME). The plant species we tested were chosen to improve the existing database for U.S. domestic fuels: laboratory-based emission factors have not previously been reported for many commonly-burned species that are frequently consumed by fires near populated regions and protected scenic areas. The plants we tested included the chaparral species chamise, manzanita, and ceanothus, and species common to the southeastern US (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, and wax myrtle). Fire-integrated emission factors for gas-phase CO{sub 2}, CO, CH{sub 4}, C{sub 2-4} hydrocarbons, NH{sub 3}, SO{sub 2}, NO, NO{sub 2}, HNO{sub 3} and particle-phase organic carbon (OC), elemental carbon (EC), SO{sub 4}{sup 2-}, NO{sub 3}{sup -}, Cl{sup -}, Na{sup +}, K{sup +}, and NH{sub 4}{sup +} generally varied with both fuel type and with the fire-integrated modified combustion efficiency (MCE), a measure of the relative importance of flaming- and smoldering-phase combustion to the total emissions during the burn. Chaparral fuels tended to emit less particulate OC per unit mass of dry fuel than did other fuel types, whereas southeastern species had some of the largest observed EF for total fine particulate matter. Our measurements often spanned a larger range of MCE than prior studies, and thus help to improve estimates for individual fuels of the variation of emissions with combustion conditions.

  7. 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.

  8. Improved identification of primary biological aerosol particles using single-particle mass spectrometry

    Directory of Open Access Journals (Sweden)

    M. A. Zawadowicz

    2017-06-01

    Full Text Available Measurements of primary biological aerosol particles (PBAP, especially at altitudes relevant to cloud formation, are scarce. Single-particle mass spectrometry (SPMS has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols (PBAP and particles containing fragments of PBAP as part of an internal mixture using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodology to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to two sets of ambient data collected at Storm Peak Laboratory and a forested site in Central Valley, California to show that 0.04–2 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol. In addition, 36–56 % of particles identified as biological also contained spectral features consistent with mineral dust, suggesting internal dust–biological mixtures.

  9. Aerosol emissions from forest and grassland burnings in the southern amazon basin and central Brazil

    Science.gov (United States)

    Leslie, Alistair C. D.

    1981-03-01

    Forest and grassland clearing by means of prescribed fires in tropical areas of the world may be responsible for large inputs of fine particulates to the global atmosphere besides being a major source of trace gases. The major continents on which extensive biomass burning takes place are Africa and South America. Such agricultural practices of burning have been employed throughout man's existence, but the importance and significance of such burning relative to anthropogenic industrial emissions to the atmosphere has not until extremely recently been seriously studied. In August-September 1979 project "Brushfire 1979" took place based in Brasília, Brazil. The Air Quality Division of the National Center for Atmospheric Research made ground level and aircraft measurements of trace gases (e.g. CO 2, CO, CH 4, N 2O, H 2, CH 3Cl, COS, NO, NO 2, O 3) and Florida State University sampled ground level aerosol emissions from grass and forest burnings. Aerosols were sampled using plastic 7-stage single orifice cascade impactors and FSU type linear and circular "streakers". Long term sampling was made of regional background for total particulates (8 μmad). Short term sampling within grass or forest fires was made using impactors incorporated into portable kits containing 4 miniature 12-18 V dc Brailsford pumps and a disposable dry cell power pack. Sampling times of 5-15 min were found optimal under these conditions. Grass fires were sampled in the savannah area northeast of Brasília and forest fires in the state of Mato Grosso on the southern edge of the dryland forest of the Amazon basin. Residual ash samples were collected. All of the samples were analyzed at Florida State University using PIXE for 15-20 elements including Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Pb and Sr. Computer reduction of the X-ray spectra was made using the "HEXB" program. One of the prominent features found was the large flux of small particles (<2.0 μm) from both fire

  10. 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

  11. Influences of Scavenging and Removal of Surfactants by Bubble Processing on Primary Marine Aerosol Production from North Atlantic Seawater

    Science.gov (United States)

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

    2017-12-01

    Primary marine aerosol particles (PMA) are produced by bursting bubbles from breaking waves at the air-sea interface and significantly modulate atmospheric chemical transformations and cloud properties. Surfactants in bulk seawater rapidly (seconds) adsorb onto fresh bubble surfaces forming organic films that influence size, rise velocity, bursting behavior, and associated PMA emissions. During a cruise on the R/V Endeavor in September and October 2016, PMA production from biologically productive and oligotrophic seawater was investigated at four stations in the western North Atlantic Ocean. PMA were produced in a high-capacity generator via turbulent mixing of seawater and clean air in a Venturi nozzle. When the flow of fresh seawater through the generator was turned off, surfactant depletion via bubble processing resulted in greater PMA mass production efficiencies per unit air detrained but had no consistent influence on number production efficiencies. The greater (factor of 3) production efficiencies of organic matter associated with PMA generated with the Venturi relative to those generated with frits during previous campaigns contributed to a faster depletion of surfactants from the seawater reservoir and corresponding divergence in response.

  12. Local source impacts on primary and secondary aerosols in the Midwestern United States

    Science.gov (United States)

    Jayarathne, Thilina; Rathnayake, Chathurika M.; Stone, Elizabeth A.

    2016-04-01

    Atmospheric particulate matter (PM) exhibits heterogeneity in composition across urban areas, leading to poor representation of outdoor air pollutants in human exposure assessments. To examine heterogeneity in PM composition and sources across an urban area, fine particulate matter samples (PM2.5) were chemically profiled in Iowa City, IA from 25 August to 10 November 2011 at two monitoring stations. The urban site is the federal reference monitoring (FRM) station in the city center and the peri-urban site is located 8.0 km to the west on the city edge. Measurements of PM2.5 carbonaceous aerosol, inorganic ions, molecular markers for primary sources, and secondary organic aerosol (SOA) tracers were used to assess statistical differences in composition and sources across the two sites. PM2.5 mass ranged from 3 to 26 μg m-3 during this period, averaging 11.2 ± 4.9 μg m-3 (n = 71). Major components of PM2.5 at the urban site included organic carbon (OC; 22%), ammonium (14%), sulfate (13%), nitrate (7%), calcium (2.9%), and elemental carbon (EC; 2.2%). Periods of elevated PM were driven by increases in ammonium, sulfate, and SOA tracers that coincided with hot and dry conditions and southerly winds. Chemical mass balance (CMB) modeling was used to apportion OC to primary sources; biomass burning, vegetative detritus, diesel engines, and gasoline engines accounted for 28% of OC at the urban site and 24% of OC at the peri-urban site. Secondary organic carbon from isoprene and monoterpene SOA accounted for an additional 13% and 6% of OC at the urban and peri-urban sites, respectively. Differences in biogenic SOA across the two sites were associated with enhanced combustion activities in the urban area and higher aerosol acidity at the urban site. Major PM constituents (e.g., OC, ammonium, sulfate) were generally well-represented by a single monitoring station, indicating a regional source influence. Meanwhile, nitrate, biomass burning, food cooking, suspended dust, and

  13. 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.

  14. 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

  15. 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

  16. 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

  17. 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.

  18. 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

  19. Secondary organic aerosol from sesquiterpene and monoterpene emissions in the United States.

    Science.gov (United States)

    Sakulyanontvittaya, Tanarit; Guenther, Alex; Helmig, Detlev; Milford, Jana; Wiedinmyer, Christine

    2008-12-01

    Emissions of volatile organic compounds (VOC) from vegetation are believed to be a major source of secondary organic aerosol (SOA), which in turn comprises a large fraction of fine particulate matter in many areas. Sesquiterpenes are a class of biogenic VOC with high chemical reactivity and SOA yields. Sesquiterpenes have only recently been quantified in emissions from a wide variety of plants. In this study, a new sesquiterpene emission inventory is used to provide input to the Models-3 Community Multiscale Air Quality (CMAQ) model. CMAQ is used to estimate the contribution of sesquiterpenes and monoterpenes to SOA concentrations over the contiguous United States. The gas-particle partitioning module of CMAQ was modified to include condensable products of sesquiterpene oxidation and to update values of the enthalpy of vaporization. The resulting model predicts July monthly average surface concentrations of total SOA in the eastern U.S. ranging from about 0.2-0.8 microg m(-3). This is roughly double the amount of SOA produced in this region when sesquiterpenes are not included. Even with sesquiterpenes included, however, the model significantly underpredicts surface concentrations of particle-phase organic matter compared to observed values. Treating all SOA as capable of undergoing polymerization increases predicted monthly average surface concentrations in July to 0.4-1.2 microg m(-3), in closer agreement with observations. Using the original enthalpy of vaporization value in CMAQ in place of the values estimated from the recent literature results in predicted SOA concentrations of about 0.3-1.3 microg m(-3).

  20. 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.

  1. 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

  2. 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.

  3. 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

  4. 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.

  5. Laboratory studies of the chemical composition and cloud condensation nuclei (CCN activity of secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA

    Directory of Open Access Journals (Sweden)

    A. T. Lambe

    2011-09-01

    Full Text Available Secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA were produced in laboratory experiments from the oxidation of fourteen precursors representing atmospherically relevant biogenic and anthropogenic sources. The SOA and OPOA particles were generated via controlled exposure of precursors to OH radicals and/or O3 in a Potential Aerosol Mass (PAM flow reactor over timescales equivalent to 1–20 days of atmospheric aging. Aerosol mass spectra of SOA and OPOA were measured with an Aerodyne aerosol mass spectrometer (AMS. The fraction of AMS signal at m/z = 43 and m/z = 44 (f43, f44, the hydrogen-to-carbon (H/C ratio, and the oxygen-to-carbon (O/C ratio of the SOA and OPOA were obtained, which are commonly used to characterize the level of oxidation of oxygenated organic aerosol (OOA. The results show that PAM-generated SOA and OPOA can reproduce and extend the observed f44f43 composition beyond that of ambient OOA as measured by an AMS. Van Krevelen diagrams showing H/C ratio as a function of O/C ratio suggest an oxidation mechanism involving formation of carboxylic acids concurrent with fragmentation of carbon-carbon bonds. Cloud condensation nuclei (CCN activity of PAM-generated SOA and OPOA was measured as a function of OH exposure and characterized as a function of O/C ratio. CCN activity of the SOA and OPOA, which was characterized in the form of the hygroscopicity parameter κorg, ranged from 8.4×10−4 to 0.28 over measured O/C ratios ranging from 0.05 to 1.42. This range of κorg and O/C ratio is significantly wider than has been previously obtained. To first order, the κorg-to-O/C relationship is well represented by a linear function of the form κorg = (0.18±0.04 ×O/C + 0.03, suggesting that a simple, semi-empirical parameterization of OOA hygroscopicity and

  6. A high-resolution emission inventory of primary pollutants for the Huabei region, China

    Directory of Open Access Journals (Sweden)

    B. Zhao

    2012-01-01

    Full Text Available Huabei, located between 32° N and 42° N, is part of eastern China and includes administratively the Beijing and Tianjin Municipalities, Hebei and Shanxi Provinces, and Inner-Mongolia Autonomous Region. Over the past decades, the region has experienced dramatic changes in air quality and climate, and has become a major focus of environmental research in China. Here we present a new inventory of air pollutant emissions in Huabei for the year 2003 developed as part of the project Influence of Pollution on Aerosols and Cloud Microphysics in North China (IPAC-NC.

    Our estimates are based on data from the statistical yearbooks of the state, provinces and local districts, including major sectors and activities of power generation, industrial energy consumption, industrial processing, civil energy consumption, crop straw burning, oil and solvent evaporation, manure, and motor vehicles. The emission factors are selected from a variety of literature and those from local measurements in China are used whenever available. The estimated total emissions in the Huabei administrative region in 2003 are 4.73 Tg SO2, 2.72 Tg NOx (in equivalent NO2, 1.77 Tg VOC, 24.14 Tg CO, 2.03 Tg NH3, 4.57 Tg PM10, 2.42 Tg PM2.5, 0.21 Tg EC, and 0.46 Tg OC.

    For model convenience, we consider a larger Huabei region with Shandong, Henan and Liaoning Provinces included in our inventory. The estimated total emissions in the larger Huabei region in 2003 are: 9.55 Tg SO2, 5.27 Tg NOx (in equivalent NO2, 3.82 Tg VOC, 46.59 Tg CO, 5.36 Tg NH3, 10.74 Tg PM10, 5.62 Tg PM2.5, 0.41 Tg EC, and 0.99 Tg OC. The estimated emission rates are projected into grid cells at a horizontal resolution of 0.1° latitude by 0.1° longitude. Our gridded emission inventory consists of area sources, which are classified into industrial, civil, traffic, and

  7. 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.; hide

    2011-01-01

    Reliable assessment of the impact of aerosols emitted from boreal forest fires on the Arctic climate necessitates improved understanding of emissions and the microphysical properties of carbonaceous (black carbon (BC) and organic aerosols (OA)) and inorganic aerosols. The size distributions of BC were measured by an SP2 based on the laser-induced incandescence technique on board the DC-8 aircraft during the NASA ARCTAS campaign. Aircraft sampling was made in fresh plumes strongly impacted by wildfires in North America (Canada and California) in summer 2008 and in those transported from Asia (Siberia in Russia and Kazakhstan) in spring 2008. We extracted biomass burning plumes using particle and tracer (CO, CH3CN, and CH2Cl2) data. OA constituted the dominant fraction of aerosols mass in the submicron range. The large majority of the emitted particles did not contain BC. We related the combustion phase of the fire as represented by the modified combustion efficiency (MCE) to the emission ratios between BC and other species. In particular, we derived the average emission ratios of BC/CO = 2.3 +/- 2.2 and 8.5 +/- 5.4 ng/cu m/ppbv for BB in North America and Asia, respectively. The difference in the BC/CO emission ratios is likely due to the difference in MCE. The count median diameters and geometric standard deviations of the lognormal size distribution of BC in the BB plumes were 136-141 nm and 1.32-1.36, respectively, and depended little on MCE. These BC particles were thickly coated, with shell/core ratios of 1.3-1.6. These parameters can be used directly for improving model estimates of the impact of BB in the Arctic.

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

    Directory of Open Access Journals (Sweden)

    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.

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

    Directory of Open Access Journals (Sweden)

    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.

  10. Methodology for assessing the concentrations of the primary marine aerosol in coastal areas

    International Nuclear Information System (INIS)

    Barsanti, P.; Briganti, G.; Cappelletti, A.; Marri, P.

    2009-01-01

    European and Italian regulations (DM 60/2002) fix for atmospheric particulate matter PM10 the threshold of 50 μg/m 3 as limit not to be exceeded more than 35 times per year (24 hour mean); unfortunately, such prescriptions do not distinguish anthropic contributions from natural ones (sea salt, Saharan sand, coastal erosion, volcanic ashes, etc.). The aim of this study is to set up a methodology in order to estimate sea salt emissions, both from open sea and surf zone, and to model atmospheric dispersion of marine aerosols. The proposed methodology, applied to the coastal zone between Massa Carrara and Viareggio (Tuscany, Italy), shows specific open sea emissions are generally very low in comparison with the surf zone ones: they are not negligible only with strong winds, but such meteorological conditions are neither persistent nor very frequent in the selected area. On the contrary, sea surf contributions are much more strong (at least 1 order of magnitude), peak-shaped and persistent then the first ones, and can lead to high PM10 concentration fields up to few kilometres inland. The comparison between model outputs and observations, in two points placed at 2000 and 4000 m from the shoreline, has shown an amount of sea salt in total PM10 even greater then 70% in mass. The existence of a surf zone, which can persist many hours or days even after a storm, can produce both elevated PM concentrations and gradients, mainly for light winds perpendicular to the shoreline. This work, supported by MINNI Project (www.minni.org), is suitable for other coastal areas as well and it is aimed to furnish an overview of marine particulate production and atmospheric dispersion processes; it is the starting point of an experimental investigation program, supported by institutional air quality authorities [it

  11. The polonium 210 in aerosols: contribution to the study of savannah fires and volcano emissions

    International Nuclear Information System (INIS)

    Nho-Kim, E.Y.

    1996-01-01

    Natural sources plan a fundamental role on the emission of the species causing climatic variations. The aim of this study is, on the one hand, to estimate fluxes of different components emitted by biomass burning and volcanoes, and on the other hand, to trace these components in time and space. We used 210 Po, last decay product in the 238 U series, as a tracer, as it is one of the characteristic species emitted by these sources: it is highly enriched in these plumes compared to the usual atmosphere and the 210 Po radioactivity is not affected by chemical transformation. We have shown that the contribution of biomass burning on the 210 Po concentration in local background atmosphere is minor during the dry season, compared to that of Saharan soil dusts despite of the importance of this source in the global budget of 210 Po (10%). However, the good correlation observed between the 210 Po concentration and that of carbonaceous aerosols and of CO 2 in biomass burning plumes reveals that 210 Po can be used as a reference of the components emitted by biomass burning. We have estimated the contribution of the Indonesian volcanoes which represent about 5 to 30 % of the global volcanic budget of trace metals. Atmospheric transport of these volcanic plumes was simulated using the 210 Po as a tracer. Due to the characteristic atmospheric circulation in this region, vertical transport is predominant over meridian dispersion, which is moderated by the convergence of the trade winds. The impact of these volcanic emissions on the atmospheric concentration of the trace metals remains a local effect when the volcanic activity is out of cataclysmal eruptions. (author)

  12. 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

  13. 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

  14. Effects of emission reductions on organic aerosol in the southeastern United States

    Directory of Open Access Journals (Sweden)

    C. L. Blanchard

    2016-01-01

    Full Text Available Long-term (1999 to 2013 data from the Southeastern Aerosol Research and Characterization (SEARCH network are used to show that anthropogenic emission reductions led to important decreases in fine-particle organic aerosol (OA concentrations in the southeastern US On average, 45 % (range 25 to 63 % of the 1999 to 2013 mean organic carbon (OC concentrations are attributed to combustion processes, including fossil fuel use and biomass burning, through associations of measured OC with combustion products such as elemental carbon (EC, carbon monoxide (CO, and nitrogen oxides (NOx. The 2013 mean combustion-derived OC concentrations were 0.5 to 1.4 µg m−3 at the five sites operating in that year. Mean annual combustion-derived OC concentrations declined from 3.8 ± 0.2 µg m−3 (68 % of total OC to 1.4 ± 0.1 µg m−3 (60 % of total OC between 1999 and 2013 at the urban Atlanta, Georgia, site (JST and from 2.9 ± 0.4 µg m−3 (39 % of total OC to 0.7 ± 0.1 µg m−3 (30 % of total OC between 2001 and 2013 at the urban Birmingham, Alabama (BHM, site. The urban OC declines coincide with reductions of motor vehicle emissions between 2006 and 2010, which may have decreased mean OC concentrations at the urban SEARCH sites by > 2 µg m−3. BHM additionally exhibits a decline in OC associated with SO2 from 0.4 ± 0.04 µg m−3 in 2001 to 0.2 ± 0.03 µg m−3 in 2013, interpreted as the result of reduced emissions from industrial sources within the city. Analyses using non-soil potassium as a biomass burning tracer indicate that biomass burning OC occurs throughout the year at all sites. All eight SEARCH sites show an association of OC with sulfate (SO4 ranging from 0.3 to 1.0 µg m−3 on average, representing  ∼  25 % of the 1999 to 2013 mean OC concentrations. Because the mass of OC identified with SO4 averages 20 to 30 % of the SO4 concentrations, the mean SO4

  15. The impact of biogenic carbon emissions on aerosol absorption inMexico City

    Energy Technology Data Exchange (ETDEWEB)

    Marley, N; Gaffney, J; Tackett, M J; Sturchio, N; Hearty, L; Martinez, N; Hardy, K D; Machany-Rivera, A; Guilderson, T P; MacMillan, A; Steelman, K

    2009-02-24

    In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbing secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.

  16. The size distribution of marine atmospheric aerosol with regard to primary biological aerosol particles over the South Atlantic Ocean

    Science.gov (United States)

    Matthias-Maser, Sabine; Brinkmann, Jutta; Schneider, Wilhelm

    The marine atmosphere is characterized by particles which originate from the ocean and by those which reached the air by advection from the continent. The bubble-burst mechanism produces both sea salt as well as biological particles. The following article describes the determination of the size distribution of marine aerosol particles with special emphasis on the biological particles. Th data were obtained on three cruises with the German Research Vessel "METEOR" crossing the South Atlantic Ocean. The measurements showed that biological particles amount to 17% in number and 10% in volume concentration. Another type of particle became obvious in the marine atmosphere, the biologically contaminated particle, i.e. particles which consist partly (approximately up to one-third) of biological matter. Their concentration in the evaluated size class ( r>2 μm) is higher than the concentration of the pure biological particles. The concentrations vary over about one to two orders of magnitude during all cruises.

  17. 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

  18. 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

  19. 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,...

  20. Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

    Science.gov (United States)

    Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

    2017-12-01

    The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

  1. 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...

  2. Assessment of Atmospheric heavy metal deposition in North Egypt aerosols using neutron activation analysis and optical emission inductively coupled plasma

    International Nuclear Information System (INIS)

    El-Araby, E.H.; Abd El-Wahab, M.; Diab, H.M.; El-Desouky, T.M.; Mohsen, M.

    2011-01-01

    The aim of the present study is to assess the current level of atmospheric heavy metal pollution of aerosols in different cities of North Egypt using the neutron activation analysis and optical emission inductively coupled plasma techniques. The results revealed that the highest concentrations of particulate matter PM 10 and total suspended particulate matter were close to industrial areas. From the results of the enrichment factor calculations, the most significant elements of anthropogenic origin are Ba, Sb, Ce and Zn. - Highlights: → Average concentration of Cd using OE-ICP is below detection limit for all the samples. → Maximum average concentration of Pb in PM10 and TSP is 5425 and 570.3, respectively. → Concentration of 20 elements in PM 10 and TSP aerosols are determined using the NAA. → EF revealed that Pb, Ba, Br, Ce, Hf, La Sb and Zn are of anthropogenic origin.

  3. Geophysical applicability of aerosol size distribution measurements using cascade impactors and proton induced X-ray emission

    International Nuclear Information System (INIS)

    Van Grieken, R.E.; Johansson, T.B.; Akselsson, K.R.; Winchester, J.W.; Nelson, J.W.; Chapman, K.R.

    1976-01-01

    Proton Induced X-ray Emission, (PIXE), is capable of high precision analysis for trace element components of aerosol particle size fractions sampled by cascade impactor. A statistical evaluation of data quality has been carried out in order to distinguish between analytical uncertainties in the PIXE procedure, errors caused by cascade impactor performance and by other factors in the sampling procedure, and geophysical causes of differences in composition and particle size distributions of the elements in aerosols. Replicate analyses and simultaneous samplings taken in north Florida and St. Louis have been used for the data evaluation. In addition to the analytical error the sampling procedure contributes an error of approximately 10% to be added quadratically. The resulting precision is sufficient to evaluate the data in geophysical terms. This is illustrated by means of sample sets taken simultaneously in an urban, forest and coastal environment of the same region. (author)

  4. 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...

  5. 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.

  6. 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...

  7. 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

  8. Qualitative Analysis of E-Liquid Emissions as a Function of Flavor Additives Using Two Aerosol Capture Methods.

    Science.gov (United States)

    Eddingsaas, Nathan; Pagano, Todd; Cummings, Cody; Rahman, Irfan; Robinson, Risa; Hensel, Edward

    2018-02-13

    This work investigates emissions sampling methods employed for qualitative identification of compounds in e-liquids and their resultant aerosols to assess what capture methods may be sufficient to identify harmful and potentially harmful constituents present. Three popular e-liquid flavors (cinnamon, mango, vanilla) were analyzed using qualitative gas chromatography-mass spectrometry (GC-MS) in the un-puffed state. Each liquid was also machine-puffed under realistic-use flow rate conditions and emissions were captured using two techniques: filter pads and methanol impingers. GC-MS analysis was conducted on the emissions captured using both techniques from all three e-liquids. The e-liquid GC-MS analysis resulted in positive identification of 13 compounds from the cinnamon flavor e-liquid, 31 from mango, and 19 from vanilla, including a number of compounds observed in all e-liquid experiments. Nineteen compounds were observed in emissions which were not present in the un-puffed e-liquid. Qualitative GC-MS analysis of the emissions samples identify compounds observed in all three samples: e-liquid, impinge, and filter pads, and each subset thereof. A limited number of compounds were observed in emissions captured with impingers, but were not observed in emissions captured using filter pads; a larger number of compounds were observed on emissions collected from the filter pads, but not those captured with impingers. It is demonstrated that sampling methods have different sampling efficiencies and some compounds might be missed using only one method. It is recommended to investigate filter pads, impingers, thermal desorption tubes, and solvent extraction resins to establish robust sampling methods for emissions testing of e-cigarette emissions.

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

    Directory of Open Access Journals (Sweden)

    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.

  10. 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.

  11. 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.

  12. 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

  13. 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

  14. Herbivory by an Outbreaking Moth Increases Emissions of Biogenic Volatiles and Leads to Enhanced Secondary Organic Aerosol Formation Capacity.

    Science.gov (United States)

    Yli-Pirilä, Pasi; Copolovici, Lucian; Kännaste, Astrid; Noe, Steffen; Blande, James D; Mikkonen, Santtu; Klemola, Tero; Pulkkinen, Juha; Virtanen, Annele; Laaksonen, Ari; Joutsensaari, Jorma; Niinemets, Ülo; Holopainen, Jarmo K

    2016-11-01

    In addition to climate warming, greater herbivore pressure is anticipated to enhance the emissions of climate-relevant biogenic volatile organic compounds (VOCs) from boreal and subarctic forests and promote the formation of secondary aerosols (SOA) in the atmosphere. We evaluated the effects of Epirrita autumnata, an outbreaking geometrid moth, feeding and larval density on herbivore-induced VOC emissions from mountain birch in laboratory experiments and assessed the impact of these emissions on SOA formation via ozonolysis in chamber experiments. The results show that herbivore-induced VOC emissions were strongly dependent on larval density. Compared to controls without larval feeding, clear new particle formation by nucleation in the reaction chamber was observed, and the SOA mass loadings in the insect-infested samples were significantly higher (up to 150-fold). To our knowledge, this study provides the first controlled documentation of SOA formation from direct VOC emission of deciduous trees damaged by known defoliating herbivores and suggests that chewing damage on mountain birch foliage could significantly increase reactive VOC emissions that can importantly contribute to SOA formation in subarctic forests. Additional feeding experiments on related silver birch confirmed the SOA results. Thus, herbivory-driven volatiles are likely to play a major role in future biosphere-vegetation feedbacks such as sun-screening under daily 24 h sunshine in the subarctic.

  15. Estimation of the aerosol optical thickness distribution in the Northeast Asian forest fire episode in May 2003: Possible missing emissions

    Science.gov (United States)

    In, Hee-Jin; Kim, Yong Pyo

    2010-11-01

    During the study of the enhancement of aerosol optical thickness (AOT) which was derived by Community Multi-scale Air Quality (CMAQ) model for an active forest fire episode in Northeast Asia for May 2003 (In et al., 2009), it was found that CMAQ underestimated and overestimated AOT sporadically compared to the multiple satellite observations. Based on the AERONET surface AOT observation result, the WMO Global Telecommunications System (GTS) SYNOP system smoke/fire reports, and surface aerosol concentration data in Korea, it was found that these errors were resulted from missing of biomass burning emissions and coarse aerosols originating from soil. An inconsistency between surface observed and CMAQ estimate AOT and MODIS hot spot detects was found, which suggests that accuracy of MODIS fire products needs to be assessed in East Russian, China, and Korea in order to utilize them for national scale fire management in the region. The implement of origin and transport process of wind blown dust in current CMAQ is necessary to extend CMAQ capability in Northeast Asia.

  16. CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: seasonal and diel variations and impact of anthropogenic emissions

    Science.gov (United States)

    Thalman, Ryan; de Sá, Suzane S.; Palm, Brett B.; Barbosa, Henrique M. J.; Pöhlker, Mira L.; Lizabeth Alexander, M.; Brito, Joel; Carbone, Samara; Castillo, Paulo; Day, Douglas A.; Kuang, Chongai; Manzi, Antonio; Ng, Nga Lee; Sedlacek, Arthur J., III; Souza, Rodrigo; Springston, Stephen; Watson, Thomas; Pöhlker, Christopher; Pöschl, Ulrich; Andreae, Meinrat O.; Artaxo, Paulo; Jimenez, Jose L.; Martin, Scot T.; Wang, Jian

    2017-10-01

    During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60 km downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ˜ 0. 15 is consistent with the largely uniform and high O : C value (˜ 0. 8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF (positive matrix factorization) analysis of AMS (aerosol mass spectrometry) spectra, were estimated through

  17. CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: seasonal and diel variations and impact of anthropogenic emissions

    Directory of Open Access Journals (Sweden)

    R. Thalman

    2017-10-01

    Full Text Available During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5 campaign, size-resolved cloud condensation nuclei (CCN spectra were characterized at a research site (T3 60 km downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015. Particle hygroscopicity (κCCN and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ∼ 0. 15 is consistent with the largely uniform and high O : C value (∼ 0. 8, indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF (positive matrix factorization analysis of AMS (aerosol mass

  18. 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

  19. 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

    Directory of Open Access Journals (Sweden)

    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

  20. 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

  1. Model studies of the effect of aerosol wastewater emissions on terrestrial mollusks Achatina fulica

    Directory of Open Access Journals (Sweden)

    Kamardin Nikolaj Nikolaevich

    2016-12-01

    Full Text Available The laboratory experiments were carried on using the juvenile mollusk Achatina fulica as a bioindicator of soil contamination and air pollution. It is shown that when experimental animals breathed and had dermal contact with the aerosols prepared from the wastewater and those prepared from two solutions of Ni in distilled water at two concentrations they weighed significantly less than controls . According to the results of AAS, heavy metals (HM, in particular Cd, Cu, Ni of sewage accumulated in the digestive gland of the shell. In model experiments mollusks were contained in the chamber periodically (2 hours of input and 2 hours of pause filled with aerosol containing Ni at concentrations of 30 and 50 mg / dm3 nickel for two weeks It resulted in accumulation of Ni in the digestive gland of mollusks with concentrations 6 to 10 times exceeding controls, respectively. At that the experimental animals gained weight reliably slower than the controls contained in aquatic aerosol without Ni. The subsequent one week exposure of shells in aerosol, prepared from the distilled water without Ni reduced the concentration of nickel in the tissue of the digestive gland. Thus, bioavailability of HM and nickel solutions prepared from untreated wastewaters in breathing aerosol and possibly by skin contact was demonstrated. The toxicant delivery seems to occur apart from food intake.

  2. Primary organic pollutants in New Zealand urban aerosol in winter during high PM1 episodes

    International Nuclear Information System (INIS)

    Krivacsy, Zoltan; Blazso, Marianne; Shooter, David

    2006-01-01

    In the two biggest New Zealand cities, Auckland and Christchurch, the mass concentration of the PM 1 atmospheric aerosol can exceed the 50 μg m -3 24 h health guideline in winter. This high pollution level is thought to be caused mainly by old-fashioned domestic heating systems based on wood combustion. Therefore the chemistry of the carbonaceous aerosol has been investigated in several high-pollution level urban situations in order to assess the origin of the pollution. All the high concentration organic tracers, including levoglucosan and dehydroabietic acid, were characteristic for biomass burning. The findings have confirmed via advanced chemical analytical methods that domestic heating can be the main contributor to the high level of wintertime pollution, especially in Christchurch. The results are of great importance in supporting the ambition of authorities and environmental associations to change the domestic heating regimes. - PM 1 aerosol concentrations can exceed air quality guidelines during winter in Christchurch, New Zealand

  3. 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.

  4. 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.

  5. 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)

  6. 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

  7. Organic tracers of primary biological aerosol particles at subtropical Okinawa Island in the western North Pacific Rim

    Science.gov (United States)

    Zhu, Chunmao; Kawamura, Kimitaka; Kunwar, Bhagawati

    2015-06-01

    Primary biological aerosol particles (PBAPs) play an important role in affecting atmospheric physical and chemical properties. Aerosol samples were collected at Cape Hedo, Okinawa Island, Japan, from October 2009 to February 2012 and analyzed for five primary saccharides and four sugar alcohols as PBAP tracers. We detected high levels of sucrose in spring when blossoming of plants happens and prolifically emits pollen to the air. Concentrations of glucose, fructose, and trehalose showed levels higher than the other saccharides in spring in 2010. In comparison, primary saccharide levels were mutually comparable in spring, summer, and autumn in 2011, indicating the interannual variability of their local production in subtropical forests, which is driven by local temperature and radiation. High trehalose events were found to be associated with Asian dust outflows, indicating that Asian dust also contributes to PBAPs at Okinawa. Sugar alcohols peaked in summer and correlated with local precipitation and temperature, indicating high microbial activities. Positive matrix factorization analysis confirmed that the PBAPs are mainly derived from local vegetation, pollen, and fungal spores. A higher contribution of PBAP tracers to water-soluble organic carbon (WSOC) was found in summer (14.9%). The annual mean ambient loadings of fungal spores and PBAPs were estimated as 0.49 µg m-3 and 4.12 µg m-3, respectively, using the tracer method. We report, for the first time, year-round biomarkers of PBAP and soil dust and their contributions to WSOC in the subtropical outflow region of the Asian continent.

  8. 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.

  9. Simulated nutrient dissolution of Asian aerosols in various atmospheric waters: Potential links to marine primary productivity

    Science.gov (United States)

    Wang, Lingyan; Bi, Yanfeng; Zhang, Guosen; Liu, Sumei; Zhang, Jing; Xu, Zhaomeng; Ren, Jingling; Zhang, Guiling

    2017-09-01

    To probe the bioavailability and environmental mobility of aerosol nutrient elements (N, P, Si) in atmospheric water (rainwater, cloud and fog droplets), ten total suspended particulate (TSP) samples were collected at Fulong Mountain, Qingdao from prevailing air mass trajectory sources during four seasons. Then, a high time-resolution leaching experiment with simulated non-acidic atmospheric water (non-AAW, Milli-Q water, pH 5.5) and subsequently acidic atmospheric water (AAW, hydrochloric acid solution, pH 2) was performed. We found that regardless of the season or source, a monotonous decreasing pattern was observed in the dissolution of N, P and Si compounds in aerosols reacted with non-AAW, and the accumulated dissolved curves of P and Si fit a first-order kinetic model. No additional NO3- + NO2- dissolved out, while a small amount of NH4+ in Asian dust (AD) samples was released in AAW. The similar dissolution behaviour of P and Si from non-AAW to AAW can be explained by the Transition State Theory. The sources of aerosols related to various minerals were the natural reasons that affected the amounts of bioavailable phosphorus and silicon in aerosols (i.e., solubility), which can be explained by the dissolution rate constant of P and Si in non-AAW with lower values in mineral aerosols. The acid/particle ratio and particle/liquid ratio also have a large effect on the solubility of P and Si, which was implied by Pearson correlation analysis. Acid processing of aerosols may have great significance for marine areas with limited P and Si and post-acidification release increases of 1.1-10-fold for phosphorus and 1.2-29-fold for silicon. The decreasing mole ratio of P and Si in AAW indicates the possibility of shifting from a Si-limit to a P-limit in aerosols in the ocean, which promotes the growth of diatoms prior to other algal species.

  10. 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...

  11. CO_2 emission trends of China's primary aluminum industry: A scenario analysis using system dynamics model

    International Nuclear Information System (INIS)

    Li, Qiang; Zhang, Wenjuan; Li, Huiquan; He, Peng

    2017-01-01

    China announced its promise on CO_2 emission peak. When and what level of CO_2 emission peak China's primary aluminum industry will reach is in suspense. In this paper, a system dynamic model is established, with five subsystems of economy development, primary aluminum production, secondary aluminum production, CO_2 emission intensity and policies making involved. The model is applied to examine potential CO_2 emission trends of China's primary aluminum industry in next fifteen years with three scenarios of “no new policies”, “13th five-year plan” and “additional policies”. Simulation results imply that: merely relying on rapid expansion of domestic scarps recycling and reuse could not mitigate CO_2 emission continuously. Combination of energy-saving technology application and electrolytic technology innovation, as well as promoting hydropower utilization in primary aluminum industry are necessary for long term low-carbon development. From a global prospective, enhancing international cooperation on new primary aluminum capacity construction in other countries, especially with rich low-carbon energy, could bring about essential CO_2 emission for both China's and global primary aluminum industry. - Highlights: • A system dynamic model is established for future CO_2 emission trend of China's primary aluminum industry. • Three potential policy scenarios are simulated. • The impacts of potential policies implication on the CO_2 emission trend are discussed.

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

    Science.gov (United States)

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

    2015-11-01

    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 fine-mode size distribution, include sea surface temperature (SST) dependency, and reduce surf-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several coastal and national observational data sets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for coastal sites in the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST dependency to the SSA emission parameterization led to increased sodium concentrations in the southeastern US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in a modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This update of SSA emissions enabled a more realistic simulation of the atmospheric chemistry in coastal environments where marine air mixes with urban pollution.

  13. 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.

  14. A new nebulization device with exchangeable aerosol generation mode as a useful tool to investigate sample introduction processes in inductively coupled plasma atomic emission spectrometry

    International Nuclear Information System (INIS)

    Grotti, Marco; Lagomarsino, Cristina; Frache, Roberto

    2004-01-01

    A new sample introduction device has been designed in order to differentiate between the effects of the aerosol production and its following desolvation on analytical performances of an inductively coupled plasma optical spectrometer. This research tool allows to easily switch between the pneumatic and ultrasonic aerosol generation mode and to use a joint desolvation chamber. In this way, a real comparison between aerosol production systems may be attained and the influence of aerosol generation process on analytical figures clearly distinguished from that of the desolvation process. In this work, the separate effects of the aerosol generation and desolvation processes on analytical sensitivity and tolerance towards matrix effects have been investigated. Concerning sensitivity, it was found that both the processes play an important role in determining emission intensities, being the increase in sensitivity due to desolvation higher than that due to the improved aerosol generation efficiency. Concerning the matrix effects, a predominant role of the desolvation system was found, while the influence of the aerosol generation mode was much less important. For nitric acid, the decreasing effect was mitigated by the presence of a desolvation system, due to partial removal of the acid. On the contrary, the depressive effect of sulfuric acid was enhanced by the presence of a desolvation system, due to degradation of the solvent removal efficiency and to further decrease in the analyte transport rate caused by clustering phenomena. Concerning the interferences due to sodium and calcium, a depressive effect was observed, which is enhanced by desolvation

  15. A Systematic Exploration of the Local and Remote Climate Effects of Anthropogenic Aerosol Emissions from Key Regions

    Science.gov (United States)

    Voulgarakis, A.; Kasoar, M.; Shawki, D.; Lamarque, J. F.; Shindell, D. T.; Faluvegi, G.; Bellouin, N.; Collins, W.; Tsigaridis, K.

    2016-12-01

    The radiative forcing of short-lived pollutants such as aerosols and tropospheric ozone is highly inhomogeneous and can therefore affect regional temperature, circulation and precipitation in a much more complicated way than the forcing of well-mixed greenhouse gases. Such effects have only recently started to be examined thoroughly and systematically from a global point of view, to understand regional interactions. Here, after outlining some key past work in this area, results from recent simulations with the UK Met Office's HadGEM3 global composition-climate model will be presented in which anthropogenic emissions of sulfur dioxide (SO2) and black carbon in key regions (East Asia, South Asia, Europe, the US, and the northern mid-latitudes as a whole) have been removed. The linkages between emissions, concentrations, radiative forcing, temperature and precipitation responses will be discussed. A particular emphasis will be placed on non-local effects, i.e. how emissions over a certain region can affect other areas remotely. Finally, we will contrast our results with those from similar experiments pursued using the NASA GISS-E2 and the NCAR CESM1 models for US and East Asian SO2 emissions, and will discuss the large differences in the models' behaviour.

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

    Directory of Open Access Journals (Sweden)

    C. A. Stroud

    2012-09-01

    Full Text Available 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 rural sites (Harrow and Bear Creek, ON to derive hydrocarbon-like organic aerosol (HOA factors. A novel diagnostic model evaluation was performed by investigating model POA bias as a function of HOA mass concentration and indicator ratios (e.g. BC/HOA. Eight case studies were selected based on factor analysis and back trajectories to help classify model bias for certain POA source types. By considering model POA bias in relation to co-located BC and CO biases, a plausible story is developed that explains the model biases for all three species.

    At the rural sites, daytime mean PM1 POA mass concentrations were under-predicted compared to observed HOA concentrations. POA under-predictions were accentuated when the transport arriving at the rural sites was from the Detroit/Windsor urban complex and for short-term periods of biomass burning influence. Interestingly, the daytime CO concentrations were only slightly under-predicted at both rural sites, whereas CO was over-predicted at the urban Windsor site with a normalized mean bias of 134%, while good agreement was observed at Windsor for the comparison of daytime PM1 POA and HOA mean values, 1.1 μg m−3 and 1.2 μg m−3, respectively. Biases in model POA predictions also trended from positive to negative with increasing HOA values. Periods of POA over-prediction were most evident at the urban site on calm nights due to an overly-stable model surface layer

  17. Evidence of aqueous secondary organic aerosol formation from biogenic emissions in the North American Sonoran Desert.

    Science.gov (United States)

    Youn, Jong-Sang; Wang, Zhen; Wonaschütz, Anna; Arellano, Avelino; Betterton, Eric A; Sorooshian, Armin

    2013-07-16

    This study examines the role of aqueous secondary organic aerosol formation in the North American Sonoran Desert as a result of intense solar radiation, enhanced moisture, and biogenic volatile organic compounds (BVOCs). The ratio of water-soluble organic carbon (WSOC) to organic carbon (OC) nearly doubles during the monsoon season relative to other seasons of the year. When normalized by mixing height, the WSOC enhancement during monsoon months relative to preceding dry months (May-June) exceeds that of sulfate by nearly a factor of 10. WSOC:OC and WSOC are most strongly correlated with moisture parameters, temperature, and concentrations of O 3 and BVOCs. No positive relationship was identified between WSOC or WSOC:OC and anthropogenic tracers such as CO over a full year. This study points at the need for further work to understand the effect of BVOCs and moisture in altering aerosol properties in understudied desert regions.

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

    Directory of Open Access Journals (Sweden)

    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

  19. 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

  20. Improved Near Real Time WRF-Chem Volcanic Emission Prediction and Impacts of Ash Aerosol on Weather.

    Science.gov (United States)

    Stuefer, M.; Webley, P. W.; Hirtl, M.

    2017-12-01

    We use the numerical Weather Research Forecasting (WRF) model with online Chemistry (WRF-Chem) to investigate the regional effects of volcanic aerosol on weather. A lot of observational data have become available since the Icelandic eruption of Eyjafjallajökull in spring 2010. The observed plume characteristics and meteorological data have been exploited for volcanic WRF-Chem case studies. We concluded that the Eyjafjallajökull ash plume resulted in significant direct aerosol effects altering the state of the atmosphere over large parts of Europe. The WRF-Chem model runs show near surface temperature differences up to 3ºC, altered vertical stability, changed pressure- and wind fields within the atmosphere loaded with ash aerosol. The modeled results have been evaluated with lidar network data, and ground and balloon based observations all over Europe. Besides case studies, we use WRF-Chem to build an improved volcanic ash decision support system that NOAA can use within the Volcanic Ash Advisory Center (VAAC) system. Realistic eruption source parameter (ESP) estimates are a main challenge in predicting volcanic emission dispersion in near real time. We implemented historic ESP into the WRF-Chem preprocessing routine, which can be used as a first estimate to assess a volcanic plume once eruption activity is reported. In a second step, a range of varying plume heights has been associated with the different ash variables within WRF-Chem, resulting in an assembly of different plume scenarios within one WRF-Chem model run. Once there is plume information available from ground or satellite observations, the forecaster has the option to select the corresponding ash variable that best matches the observations. In addition we added an automatic domain generation tool to create near real time WRF-Chem model runs anywhere on the globe by reducing computing expenses at the same time.

  1. 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

  2. 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.

  3. Review: The Use of Real-Time Fluorescence Instrumentation to Monitor Ambient Primary Biological Aerosol Particles (PBAP

    Directory of Open Access Journals (Sweden)

    Mehael J. Fennelly

    2017-12-01

    Full Text Available Primary biological aerosol particles (PBAP encompass many particle types that are derived from several biological kingdoms. These aerosol particles can be composed of both whole living units such as pollen, bacteria, and fungi, as well as from mechanically formed particles, such as plant debris. They constitute a significant proportion of the overall atmospheric particle load and have been linked with adverse health issues and climatic effects on the environment. Traditional methods for their analysis have focused on the direct capture of PBAP before subsequent laboratory analysis. These analysis types have generally relied on direct optical microscopy or incubation on agar plates, followed by time-consuming microbiological investigation. In an effort to address some of these deficits, real-time fluorescence monitors have come to prominence in the analysis of PBAP. These instruments offer significant advantages over traditional methods, including the measurement of concentrations, as well as the potential to simultaneously identify individual analyte particles in real-time. Due to the automated nature of these measurements, large data sets can be collected and analyzed with relative ease. This review seeks to highlight and discuss the extensive literature pertaining to the most commonly used commercially available real-time fluorescence monitors (WIBS, UV-APS and BioScout. It discusses the instruments operating principles, their limitations and advantages, and the various environments in which they have been deployed. The review provides a detailed examination of the ambient fluorescent aerosol particle concentration profiles that are obtained by these studies, along with the various strategies adopted by researchers to analyze the substantial data sets the instruments generate. Finally, a brief reflection is presented on the role that future instrumentation may provide in revolutionizing this area of atmospheric research.

  4. Size distribution and concentrations of heavy metals in atmospheric aerosols originating from industrial emissions as predicted by the HYSPLIT model

    Science.gov (United States)

    Chen, Bing; Stein, Ariel F.; Maldonado, Pabla Guerrero; Sanchez de la Campa, Ana M.; Gonzalez-Castanedo, Yolanda; Castell, Nuria; de la Rosa, Jesus D.

    2013-06-01

    This study presents a description of the emission, transport, dispersion, and deposition of heavy metals contained in atmospheric aerosols emitted from a large industrial complex in southern Spain using the HYSPLIT model coupled with high- (MM5) and low-resolution (GDAS) meteorological simulations. The dispersion model was configured to simulate eight size fractions (17 μm) of metals based on direct measurements taken at the industrial emission stacks. Twelve stacks in four plants were studied and the stacks showed considerable differences for both emission fluxes and size ranges of metals. We model the dispersion of six major metals; Cr, Co, Ni, La, Zn, and Mo, which represent 77% of the total mass of the 43 measured elements. The prediction shows that the modeled industrial emissions produce an enrichment of heavy metals by a factor of 2-5 for local receptor sites when compared to urban and rural background areas in Spain. The HYSPLIT predictions based on the meteorological fields from MM5 show reasonable consistence with the temporal evolution of concentrations of Cr, Co, and Ni observed at three sites downwind of the industrial area. The magnitude of concentrations of metals at two receptors was underestimated for both MM5 (by a factor of 2-3) and GDAS (by a factor of 4-5) meteorological runs. The model prediction shows that heavy metal pollution from industrial emissions in this area is dominated by the ultra-fine (<0.66 μm) and fine (<2.5 μm) size fractions.

  5. Modeling organic aerosols in a megacity: potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol formation

    Directory of Open Access Journals (Sweden)

    A. Hodzic

    2010-06-01

    Full Text Available It has been established that observed local and regional levels of secondary organic aerosols (SOA in polluted areas cannot be explained by the oxidation and partitioning of anthropogenic and biogenic VOC precursors, at least using current mechanisms and parameterizations. In this study, the 3-D regional air quality model CHIMERE is applied to estimate the potential contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic precursors (S/IVOC in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to include explicitly the volatility distribution of primary organic aerosols (POA, their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007 ("ROB" and Grieshop et al. (2009 ("GRI" are compared and evaluated against surface and aircraft measurements. The 3-D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS data, and for the first time also with oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (2–4 times with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009, both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The predicted production from anthropogenic and biomass burning S/IVOC represents 40–60% of the total measured SOA at the surface during the day and is somewhat larger than that from commonly measured aromatic VOCs, especially at the T1 site at the edge of the city. The SOA production from the continued multi-generation S/IVOC oxidation products continues actively

  6. PREP-CHEM-SRC – 1.0: a preprocessor of trace gas and aerosol emission fields for regional and global atmospheric chemistry models

    Directory of Open Access Journals (Sweden)

    S. R. Freitas

    2011-05-01

    Full Text Available The preprocessor PREP-CHEM-SRC presented in the paper is a comprehensive tool aiming at preparing emission fields of trace gases and aerosols for use in atmospheric-chemistry transport models. The considered emissions are from the most recent databases of urban/industrial, biogenic, biomass burning, volcanic, biofuel use and burning from agricultural waste sources. For biomass burning, emissions can be also estimated directly from satellite fire detections using a fire emission model included in the tool. The preprocessor provides emission fields interpolated onto the transport model grid. Several map projections can be chosen. The inclusion of these emissions in transport models is also presented. The preprocessor is coded using Fortran90 and C and is driven by a namelist allowing the user to choose the type of emissions and the databases.

  7. Primary Aluminum Reduction Industry - National Emission Standards for Hazardous Air Pollutants (NESHAP)

    Science.gov (United States)

    National emission standards for each new or existing potline, paste production operation, and anode bake furnace associated with a primary aluminum reduction plant. Includes rule history, implementation information and additional resources.

  8. Submicrometer aerosol in rural and urban backgrounds in southern Poland: primary and secondary components of PM1.

    Science.gov (United States)

    Rogula-Kozłowska, Wioletta; Klejnowski, Krzysztof

    2013-01-01

    Diurnal samples of PM(1) (submicrometer particles, having aerodynamic diameters not greater than 1 μm) were collected at an urban background site in Zabrze (from 01.08. to 31.12.2009) and a rural background site in Racibórz (from 01.08. to 31.12.2010). The samples were analyzed for carbon (organic and elemental), water soluble ions (Na(+), NH(4) (+), K(+), Mg(2+), Ca(2+), Cl(-), NO(3)(-), SO(4)(2-)) and concentrations of 21 elements by using, respectively, a Sunset Laboratory carbon analyzer, a Herisau Metrohm AG ion chromatograph, a PANalitycal Epsilon 5 spectrometer. To perform the monthly mass closure calculations for PM(1), the chemical components were categorized into organic matter (OM), elemental carbon (EC), secondary inorganic aerosol (SIA), crustal matter (CM), marine components (MC), other elements (OE) and unidentified matter (UM). The mass contributions of secondary (SOM) and primary (POM) organic matter to PM(1) were also estimated. In average, 50 % of PM(1) in Zabrze and 40 % in Racibórz were secondary aerosol coming from the transformations of its gaseous precursors. High concentrations and mass contributions of EC and OM to PM, and probable PM acidic nature in Zabrze, indicate particularly high hazard from the ambient submicrometer particles to the inhabitants of southern Poland.

  9. Oxidative aging and secondary organic aerosol formation from simulated wildfire emissions

    Science.gov (United States)

    C. J. Hennigan; M. A. Miracolo; G. J. Engelhart; A. A. May; Cyle Wold; WeiMin Hao; T. Lee; A. P. Sullivan; J. B. Gilman; W. C. Kuster; J. A. de Gouw; J. L. Collett; S. M. Kreidenweis; A. L. Robinson

    2010-01-01

    Wildfires are a significant fraction of global biomass burning and a major source of trace gas and particle emissions in the atmosphere. Understanding the air quality and climate implications of wildfires is difficult since the emissions undergo complex transformations due to aging processes during transport away from the source. As part of the third Fire Lab at...

  10. Experimental determination of the dynamic shape factor of primary sodium peroxide aerosols

    International Nuclear Information System (INIS)

    Barbe, M.

    1985-09-01

    A hypothetical accident in a fast breeeder reactor could cause aerosols to be generated in a sodium fire. The computer codes relative to the modeling of such accidents make it necessary to use various input parameters among which the dynamic shape factor kappa of the aerosols produced. This study concerns the shape factor of sodium peroxide; the discrepancies between the values of this parameter given in the literature justifies the usefulness of our work. We have tried to use the simplest method. The dynamic shape factor is proportional to the ratio of the equivalent volume diameter to the aerodynamic diameter for a given particle. Therefore, these two quantities must be determined. The particles are classified by means of a centrifuge as a function of their aerodynamic diameter; the equivalent volume diameter of the particles thus selected can then be determined by assessing the mass (neutron activation) and the number (electron microscope) on the same sample of particles. Our results show that the dynamic shape factor of sodium peroxide submicronic particles generated by a fire is nearly 1 and the values of this parameter increase with the particles size [fr

  11. Aerosol modelling and validation during ESCOMPTE 2001

    Science.gov (United States)

    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

  12. Monitoring of PM10 and PM2.5 around primary particulate anthropogenic emission sources

    Science.gov (United States)

    Querol, Xavier; Alastuey, Andrés; Rodriguez, Sergio; Plana, Felicià; Mantilla, Enrique; Ruiz, Carmen R.

    Investigations on the monitoring of ambient air levels of atmospheric particulates were developed around a large source of primary anthropogenic particulate emissions: the industrial ceramic area in the province of Castelló (Eastern Spain). Although these primary particulate emissions have a coarse grain-size distribution, the atmospheric transport dominated by the breeze circulation accounts for a grain-size segregation, which results in ambient air particles occurring mainly in the 2.5-10 μm range. The chemical composition of the ceramic particulate emissions is very similar to the crustal end-member but the use of high Al, Ti and Fe as tracer elements as well as a peculiar grain-size distribution in the insoluble major phases allow us to identify the ceramic input in the bulk particulate matter. PM2.5 instead of PM10 monitoring may avoid the interference of crustal particles without a major reduction in the secondary anthropogenic load, with the exception of nitrate. However, a methodology based in PM2.5 measurement alone is not adequate for monitoring the impact of primary particulate emissions (such as ceramic emissions) on air quality, since the major ambient air particles derived from these emissions are mainly in the range of 2.5-10 μm. Consequently, in areas characterised by major secondary particulate emissions, PM2.5 monitoring should detect anthropogenic particulate pollutants without crustal particulate interference, whereas PM10 measurements should be used in areas with major primary anthropogenic particulate emissions.

  13. 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

  14. Properties and Fluxes of Primary Marine Aerosol Generated Via Detrainment of Turbulence-Modulated Bubble Plumes from Fresh North Atlantic Seawater

    Science.gov (United States)

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

    2017-12-01

    During a September-October 2016 cruise of the R/V Endeavor in the western North Atlantic Ocean, primary marine aerosol (PMA) was produced in a high capacity generator during day and night via detrainment of bubbles from biologically productive and oligotrophic seawater. The turbulent mixing of clean air and seawater in a Venturi nozzle produced bubble plumes with tunable size distributions. Physicochemical characteristics of size-resolved PMA and seawater were measured. PMA number production efficiencies per unit air detrained (PEnum) increased with increasing detainment rate. For given conditions, PEnum values summed over size distributions were roughly ten times greater than those for frits whereas normalized size distributions were similar. Results show that bubble size distributions significantly modulated number production fluxes but not relative shapes of corresponding size distributions. In contrast, mass production efficiencies (PEmass) decreased with increasing air detrainment and were similar to those for frits, consistent with the hypothesis that bubble rafts on the seawater surface modulate emissions of larger jet droplets that dominate PMA mass production. Production efficiencies of organic matter were about three times greater than those for frits whereas organic enrichment factors integrated over size distributions were similar.

  15. Impact of Wildfire Emissions on Chloride and Bromide Depletion in Marine Aerosol Particles.

    Science.gov (United States)

    Braun, Rachel A; Dadashazar, Hossein; MacDonald, Alexander B; Aldhaif, Abdulamonam M; Maudlin, Lindsay C; Crosbie, Ewan; Aghdam, Mojtaba Azadi; Hossein Mardi, Ali; Sorooshian, Armin

    2017-08-15

    This work examines particulate chloride (Cl - ) and bromide (Br - ) depletion in marine aerosol particles influenced by wildfires at a coastal California site in the summers of 2013 and 2016. Chloride exhibited a dominant coarse mode due to sea salt influence, with substantially diminished concentrations during fire periods as compared to nonfire periods. Bromide exhibited a peak in the submicrometer range during fire and nonfire periods, with an additional supermicrometer peak in the latter periods. Chloride and Br - depletions were enhanced during fire periods as compared to nonfire periods. The highest observed %Cl - depletion occurred in the submicrometer range, with maximum values of 98.9% (0.32-0.56 μm) and 85.6% (0.56-1 μm) during fire and nonfire periods, respectively. The highest %Br - depletion occurred in the supermicrometer range during fire and nonfire periods with peak depletion between 1.8-3.2 μm (78.8% and 58.6%, respectively). When accounting for the neutralization of sulfate by ammonium, organic acid particles showed the greatest influence on Cl - depletion in the submicrometer range. These results have implications for aerosol hygroscopicity and radiative forcing in areas with wildfire influence owing to depletion effects on composition.

  16. Experimental study of radioactive aerosols emission during the thermal degradation of organic materials in nuclear facilities

    International Nuclear Information System (INIS)

    Fernandez, Yvette

    1993-01-01

    Radioactive products may be released during a fire in nuclear fuel cycles facilities. These products must be confined to avoid a contamination spread in the environment. It is therefore necessary to be able to predict the amount and the physico-chemical forms of radioactive material that may be airborne. The aim of this study is to determine experimentally the release of contamination aerosols in a typical fire scenario involving plutonium oxide in a glove box. Firstly, this phenomenon has been studied in a small scale test chamber where samples of polymethylmethacrylate (Plexiglas) contaminated by cerium oxide (used as a substitute for plutonium oxide) were submitted to thermal degradation (pyrolysis and combustion). The release of radioactive material is determined by the quantity of contaminant emitted, the kinetics of the release and the particle size distribution of aerosols. Secondly, the development of an experimental procedure allowed to realize large scale fires in more realistic conditions. The experimental tools developed in the course of this study allow to consider application to other scenarios. (author) [fr

  17. Impacts of Siberian biomass burning on organic aerosols over the North Pacific Ocean and the Arctic: primary and secondary organic tracers.

    Science.gov (United States)

    Ding, Xiang; Wang, Xinming; Xie, Zhouqing; Zhang, Zhou; Sun, Liguang

    2013-04-02

    During the 2003 Chinese Arctic Research Expedition (CHINARE2003) from the Bohai Sea to the high Arctic (37°N-80°N), filter-based particle samples were collected and analyzed for tracers of primary and secondary organic aerosols (SOA) as well as water-soluble organic carbon (WSOC). Biomass burning (BB) tracer levoglucosan had comparatively much higher summertime average levels (476 ± 367 pg/m(3)) during our cruise due to the influence of intense forest fires then in Siberia. On the basis of 5-day back trajectories, samples with air masses passing through Siberia had organic tracers 1.3-4.4 times of those with air masses transporting only over the oceans, suggesting substantial contribution of continental emissions to organic aerosols in the marine atmosphere. SOA tracers from anthropogenic aromatics were negligible or not detected, while those from biogenic terpenenoids were ubiquitously observed with the sum of SOA tracers from isoprene (623 ± 414 pg/m(3)) 1 order of magnitude higher than that from monoterpenes (63 ± 49 pg/m(3)). 2-Methylglyceric acid as a product of isoprene oxidation under high-NOx conditions was dominant among SOA tracers, implying that these BSOA tracers were not formed over the oceans but mainly transported from the adjacent Siberia where a high-NOx environment could be induced by intense forest fires. The carbon fractions shared by biogenic SOA tracers and levoglucosan in WSOC in our ocean samples were 1-2 orders of magnitude lower than those previously reported in continental samples, BB emissions or chamber simulation samples, largely due to the chemical evolution of organic tracers during transport. As a result of the much faster decline in levels of organic tracers than that of WSOC during transport, the trace-based approach, which could well reconstruct WSOC using biogenic SOA and BB tracers for continental samples, only explained ∼4% of measured WSOC during our expedition if the same tracer-WSOC or tracer-SOC relationships were

  18. 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.

  19. Mutagenicity assessment of aerosols in emissions from wood combustion in Portugal

    International Nuclear Information System (INIS)

    Vu, B.; Alves, C.A.; Gonçalves, C.; Pio, C.; Gonçalves, F.; Pereira, R.

    2012-01-01

    Polycyclic aromatic hydrocarbon (PAH) extracts of fine particles (PM 2.5 ) collected from combustion of seven wood species and briquettes were tested for mutagenic activities using Ames test with Salmonella typhimurium TA98 and TA100. The woods were Pinus pinaster (maritime pine), Eucalyptus globulus (eucalypt), Quercus suber (cork oak), Acacia longifolia (golden wattle), Quercus faginea (Portuguese oak), Olea europea (olive), and Quercus ilex rotundifolia (Holm oak). Burning experiments were done using woodstove and fireplace, hot start and cold start conditions. A mutagenic response was recorded for all species except golden wattle, maritime pine, and briquettes. The mutagenic extracts were not correlated with high emission factors of carcinogenic PAHs. These extracts were obtained both from two burning appliances and start-up conditions. However, fireplace seemed to favour the occurrence of mutagenic emissions. The negative result recorded for golden wattle was interesting, in an ecological point of view, since after confirmation, this invasive species, can be recommended for domestic use. - Highlights: ► Both woodstove and fireplace, either with a cold or hot start, produce emissions with mutagenic potential. ► The high level of carcinogenic PAHs in combustion emissions was not correlated with mutagenicity. ► The golden wattle, an invasive species, produced no mutagenic emissions. - Wood smoke from fireplace burning of dominant forest species displayed strong mutagenic activity without a significant correlation with carcinogenic PAHs emission factors.

  20. Relationship between trace gases and aerosols from biomass burning in Southeast Asia using satellite and emission data

    Science.gov (United States)

    Azuma, Yoshimi; Nakamura, Maya; Kuji, Makoto

    2012-11-01

    Southeast Asia is one of the biggest regions of biomass burning with forest fires and slash-and-burn farming. From the fire events, a large amount of air pollutants are emitted such as carbon monoxide (CO), nitrogen oxide (NOx) and aerosol (black carbon; BC). Biomass burning generally causes not only local, but also transboundary air pollution, and influences the atmospheric environment in the world accordingly. However, impact of air pollutants' emissions from large-scale fire in Southeast Asia is not well investigated compared to other regions such as South America and Africa. In this study, characteristics of the atmospheric environment were investigated with correlative analyses among several satellite data (MOPITT, OMI, and MODIS) and emission inventory (GFEDv3) in Southeast Asia from October 2004 to June 2008 on a monthly basis. As a result, it is suggested that the transboundary air pollution from the biomass burning regions occurred over Southeast Asia, which caused specifically higher air pollutants' concentration at Hanoi, Vietnam in spring dry season.

  1. Globalization and pollution: tele-connecting local primary PM2.5 emissions to global consumption

    Science.gov (United States)

    Meng, Jing; Liu, Junfeng; Xu, Yuan; Guan, Dabo; Liu, Zhu; Huang, Ye; Tao, Shu

    2016-11-01

    Globalization pushes production and consumption to geographically diverse locations and generates a variety of sizeable opportunities and challenges. The distribution and associated effects of short-lived primary fine particulate matter (PM2.5), a representative of local pollution, are significantly affected by the consumption through global supply chain. Tele-connection is used here to represent the link between production and consumption activity at large distances. In this study, we develop a global consumption-based primary PM2.5 emission inventory to track primary PM2.5 emissions embodied in the supply chain and evaluate the extent to which local PM2.5 emissions are triggered by international trade. We further adopt consumption-based accounting and identify the global original source that produced the emissions. We find that anthropogenic PM2.5 emissions from industrial sectors accounted for 24 Tg globally in 2007; approximately 30% (7.2 Tg) of these emissions were embodied in export of products principally from Brazil, South Africa, India and China (3.8 Tg) to developed countries. Large differences (up to 10 times) in the embodied emissions intensity between net importers and exporters greatly increased total global PM2.5 emissions. Tele-connecting production and consumption activity provides valuable insights with respect to mitigating long-range transboundary air pollution and prompts concerted efforts aiming at more environmentally conscious globalization.

  2. 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.

  3. 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)

  4. Globalization and pollution: tele-connecting local primary PM2.5 emissions to global consumption

    Science.gov (United States)

    Meng, Jing; Xu, Yuan; Guan, Dabo; Liu, Zhu; Huang, Ye; Tao, Shu

    2016-01-01

    Globalization pushes production and consumption to geographically diverse locations and generates a variety of sizeable opportunities and challenges. The distribution and associated effects of short-lived primary fine particulate matter (PM2.5), a representative of local pollution, are significantly affected by the consumption through global supply chain. Tele-connection is used here to represent the link between production and consumption activity at large distances. In this study, we develop a global consumption-based primary PM2.5 emission inventory to track primary PM2.5 emissions embodied in the supply chain and evaluate the extent to which local PM2.5 emissions are triggered by international trade. We further adopt consumption-based accounting and identify the global original source that produced the emissions. We find that anthropogenic PM2.5 emissions from industrial sectors accounted for 24 Tg globally in 2007; approximately 30% (7.2 Tg) of these emissions were embodied in export of products principally from Brazil, South Africa, India and China (3.8 Tg) to developed countries. Large differences (up to 10 times) in the embodied emissions intensity between net importers and exporters greatly increased total global PM2.5 emissions. Tele-connecting production and consumption activity provides valuable insights with respect to mitigating long-range transboundary air pollution and prompts concerted efforts aiming at more environmentally conscious globalization. PMID:27956874

  5. Globalization and pollution: tele-connecting local primary PM2.5 emissions to global consumption.

    Science.gov (United States)

    Meng, Jing; Liu, Junfeng; Xu, Yuan; Guan, Dabo; Liu, Zhu; Huang, Ye; Tao, Shu

    2016-11-01

    Globalization pushes production and consumption to geographically diverse locations and generates a variety of sizeable opportunities and challenges. The distribution and associated effects of short-lived primary fine particulate matter (PM 2.5 ), a representative of local pollution, are significantly affected by the consumption through global supply chain. Tele-connection is used here to represent the link between production and consumption activity at large distances. In this study, we develop a global consumption-based primary PM 2.5 emission inventory to track primary PM 2.5 emissions embodied in the supply chain and evaluate the extent to which local PM 2.5 emissions are triggered by international trade. We further adopt consumption-based accounting and identify the global original source that produced the emissions. We find that anthropogenic PM 2.5 emissions from industrial sectors accounted for 24 Tg globally in 2007; approximately 30% (7.2 Tg) of these emissions were embodied in export of products principally from Brazil, South Africa, India and China (3.8 Tg) to developed countries. Large differences (up to 10 times) in the embodied emissions intensity between net importers and exporters greatly increased total global PM 2.5 emissions. Tele-connecting production and consumption activity provides valuable insights with respect to mitigating long-range transboundary air pollution and prompts concerted efforts aiming at more environmentally conscious globalization.

  6. Measurement of particle emission in automobil exhaust - application of continuous radiometric aerosol measurement to the emission of diesel engines

    International Nuclear Information System (INIS)

    Krasenbrink, A.; Georgi, B.

    1989-01-01

    The well-known method of measuring continuously dust by β-absorption is transferred to the problem of particle emission in automobile exhaust. With two similar dust-monitors FH62 having different sampling air flow rates and two low-pressure impactors the reliability of radiometric mass determination was verified. First static experiments with diesel soot showed the necessity of a dilution system, a new mass calibration with regard to the changed β-absorptivity and a quicker calculation of concentration for realtime measurements. (orig.) [de

  7. Inventory of primary particulates emissions; Inventaire des emissions de particules primaires

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2001-12-01

    CITEPA carried out a national inventory on particulate emissions. This report presents the results of this study for a great number of sectors and it covers a larger number of sources than the previous CITEPA inventories on particles and some other inventories carried out by International organisms (TNO, IIASA). In particular, at the present time, fugitive dust emissions for some sources are rarely taken into account in inventories because of poor knowledge and they are still the subject of researches in order to validate the emission results. (author)

  8. 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

  9. Primary sources of selected POPs: regional and global scale emission inventories

    Energy Technology Data Exchange (ETDEWEB)

    Breivik, Knut; Alcock, Ruth; Li Yifan; Bailey, Robert E.; Fiedler, Heidelore; Pacyna, Jozef M

    2004-03-01

    During the last decade, a number of studies have been devoted to the sources and emissions of Persistent Organic Pollutants (POPs) at regional and global scales. While significant improvements in knowledge have been achieved for some pesticides, the quantitative understanding of the emission processes and emission patterns for 'non-pesticide' POPs are still considered limited. The key issues remaining for the non-pesticide POPs are in part determined by their general source classification. For industrial chemicals, such as the polychlorinated biphenyls (PCBs), there is considerable uncertainty with respect to the relative importance of atmospheric emissions from various source categories. For PCBs, temperature is discussed as a potential key factor influencing atmospheric emission levels and patterns. When it comes to the unintentional by-products of combustion and industrial processes (PCDD/Fs), there is still a large uncertainty with respect to the relative contribution of emissions from unregulated sources such as backyard barrel burning that requires further consideration and characterisation. For hexachlorobenzene (HCB), the relative importance of primary and secondary atmospheric emissions in controlling current atmospheric concentrations remains one of the key uncertainties. While these and other issues may remain unresolved, knowledge concerning the emissions of POPs is a prerequisite for any attempt to understand and predict the distribution and fate of these chemicals on a regional and global scale as well as to efficiently minimise future environmental burdens. - Knowledge of primary emissions is a prerequisite for understanding and predicting POPs on a regional/global scale.

  10. Primary sources of selected POPs: regional and global scale emission inventories

    International Nuclear Information System (INIS)

    Breivik, Knut; Alcock, Ruth; Li Yifan; Bailey, Robert E.; Fiedler, Heidelore; Pacyna, Jozef M.

    2004-01-01

    During the last decade, a number of studies have been devoted to the sources and emissions of Persistent Organic Pollutants (POPs) at regional and global scales. While significant improvements in knowledge have been achieved for some pesticides, the quantitative understanding of the emission processes and emission patterns for 'non-pesticide' POPs are still considered limited. The key issues remaining for the non-pesticide POPs are in part determined by their general source classification. For industrial chemicals, such as the polychlorinated biphenyls (PCBs), there is considerable uncertainty with respect to the relative importance of atmospheric emissions from various source categories. For PCBs, temperature is discussed as a potential key factor influencing atmospheric emission levels and patterns. When it comes to the unintentional by-products of combustion and industrial processes (PCDD/Fs), there is still a large uncertainty with respect to the relative contribution of emissions from unregulated sources such as backyard barrel burning that requires further consideration and characterisation. For hexachlorobenzene (HCB), the relative importance of primary and secondary atmospheric emissions in controlling current atmospheric concentrations remains one of the key uncertainties. While these and other issues may remain unresolved, knowledge concerning the emissions of POPs is a prerequisite for any attempt to understand and predict the distribution and fate of these chemicals on a regional and global scale as well as to efficiently minimise future environmental burdens. - Knowledge of primary emissions is a prerequisite for understanding and predicting POPs on a regional/global scale

  11. 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.

  12. The impact of biogenic, anthropogenic, and biomass burning volatile organic compound emissions on regional and seasonal variations in secondary organic aerosol

    Science.gov (United States)

    Kelly, Jamie M.; Doherty, Ruth M.; O'Connor, Fiona M.; Mann, Graham W.

    2018-05-01

    The global secondary organic aerosol (SOA) budget is highly uncertain, with global annual SOA production rates, estimated from global models, ranging over an order of magnitude and simulated SOA concentrations underestimated compared to observations. In this study, we use a global composition-climate model (UKCA) with interactive chemistry and aerosol microphysics to provide an in-depth analysis of the impact of each VOC source on the global SOA budget and its seasonality. We further quantify the role of each source on SOA spatial distributions, and evaluate simulated seasonal SOA concentrations against a comprehensive set of observations. The annual global SOA production rates from monoterpene, isoprene, biomass burning, and anthropogenic precursor sources is 19.9, 19.6, 9.5, and 24.6 Tg (SOA) a-1, respectively. When all sources are included, the SOA production rate from all sources is 73.6 Tg (SOA) a-1, which lies within the range of estimates from previous modelling studies. SOA production rates and SOA burdens from biogenic and biomass burning SOA sources peak during Northern Hemisphere (NH) summer. In contrast, the anthropogenic SOA production rate is fairly constant all year round. However, the global anthropogenic SOA burden does have a seasonal cycle which is lowest during NH summer, which is probably due to enhanced wet removal. Inclusion of the new SOA sources also accelerates the ageing by condensation of primary organic aerosol (POA), making it more hydrophilic, leading to a reduction in the POA lifetime. With monoterpene as the only source of SOA, simulated SOA and total organic aerosol (OA) concentrations are underestimated by the model when compared to surface and aircraft measurements. Model agreement with observations improves with all new sources added, primarily due to the inclusion of the anthropogenic source of SOA, although a negative bias remains. A further sensitivity simulation was performed with an increased anthropogenic SOA reaction

  13. Quantifying Sulphur Emissions and Atmospheric Aerosol Loading From the 1730-36 Lanzarote Eruption

    Science.gov (United States)

    Sharma, K.; Blake, S.; Self, S.

    2005-12-01

    The AD 1730-36 eruption of Lanzarote (Canary Islands) is the third largest basaltic fissure eruption known to have occurred in the last 1000 years, after the Icelandic events of Laki (AD 1783-84) and Eldgja (AD 934). Our new volume estimates suggest that the Lanzarote eruption produced ~6 km3 of alkali basalt magma along a 15-km long, E-W trending fissure. Eruptive activity occurred in five distinct phases. Each phase began with Strombolian fire fountain activity, building large spatter and scoria cones. This was accompanied and followed by effusive aa and pahoehoe lava flow emplacement. As studies in Iceland have shown, this type of sustained fissure eruption can release large amounts of SO2 to the upper atmosphere, leading to the formation of sulphate aerosol clouds and causing widespread environmental damage and human suffering. Matrix glasses in scoria and surface lava samples have 80-300 ppm S (EMPA) and 300-600 ppm H2O (FTIR), whereas glass inclusions in olivine have 420-2650 ppm S and 1000-5000 ppm H2O. Low sulphur inclusions are believed to be partially degassed, representing melt that was trapped during degassing-induced crystallization that occurred as a result of shallow decompression. The inclusions with the highest sulphur contents trap the original un-degassed melt, as indicated by their consistent S/K2O ratio (0.22). The high sulphur contents are also consistent with our finding, from olivine-spinel equilibria, that the magma was relatively oxidized (log fO2 -4.8) therefore favouring the formation of sulphate species and preventing sulphide saturation. Our glass analyses indicate that 40 Mt of SO2 was injected into the upper troposphere - lower stratosphere via 12-16-km-high eruption plumes and that over half this amount was released during the first year of activity. This figure correlates with published Greenland ice-core (GISP-2) data that shows an acidity spike in 1731, suggesting stratospheric transport of sulphate aerosol to the North during

  14. 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.

  15. Aerosol-based emission, solvent degradation, and corrosion in post combustion CO2 capture

    NARCIS (Netherlands)

    Khakharia, P.

    2015-01-01

    Global greenhouse gas emissions, especially of CO2, have been increasing tremendously over the past century. This is known to cause not only an increase of temperature, but also a change in our climate. Along with a shift to renewable sources of energy, Carbon Capture and Storage is necessary to

  16. Aerosol and NOx emission factors and submicron particle number size distributions in two road tunnels with different traffic regimes

    Directory of Open Access Journals (Sweden)

    D. Imhof

    2006-01-01

    Full Text Available Measurements of aerosol particle number size distributions (18–700 nm, mass concentrations (PM2.5 and PM10 and NOx were performed in the Plabutsch tunnel, Austria, and in the Kingsway tunnel, United Kingdom. These two tunnels show different characteristics regarding the roadway gradient, the composition of the vehicle fleet and the traffic frequency. The submicron particle size distributions contained a soot mode in the diameter range D=80–100 nm and a nucleation mode in the range of D=20–40 nm. In the Kingsway tunnel with a significantly lower particle number and volume concentration level than in the Plabutsch tunnel, a clear diurnal variation of nucleation and soot mode particles correlated to the traffic density was observed. In the Plabutsch tunnel, soot mode particles also revealed a diurnal variation, whereas no substantial variation was found for the nucleation mode particles. During the night a higher number concentration of nucleation mode particles were measured than soot mode particles and vice versa during the day. In this tunnel with very high soot emissions during daytime due to the heavy-duty vehicle (HDV share of 18% and another 40% of diesel driven light-duty vehicles (LDV semivolatile species condense on the pre-existing soot surface area rather than forming new particles by homogeneous nucleation. With the low concentration of soot mode particles in the Kingsway tunnel, also the nucleation mode particles exhibit a diurnal variation. From the measured parameters real-world traffic emission factors were estimated for the whole vehicle fleet as well as differentiated into the two categories LDV and HDV. In the particle size range D=18–700 nm, each vehicle of the mixed fleet emits (1.50±0.08×1014 particles km-1 (Plabutsch and (1.26±0.10×1014 particles km-1 (Kingsway, while particle volume emission factors of 0.209±0.008 cm3 km-1 and 0.036±0.004 cm3 km-1, respectively, were obtained. PM1 emission factors of 104±4 mg

  17. 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.

  18. The polonium 210 in aerosols: contribution to the study of savannah fires and volcano emissions; Le polonium 210 dans les aerosols: contribution a l`etude des feux de savanes et des emissions volcaniques

    Energy Technology Data Exchange (ETDEWEB)

    Nho-Kim, E.Y

    1996-06-27

    Natural sources plan a fundamental role on the emission of the species causing climatic variations. The aim of this study is, on the one hand, to estimate fluxes of different components emitted by biomass burning and volcanoes, and on the other hand, to trace these components in time and space. We used {sup 210}Po, last decay product in the {sup 238}U series, as a tracer, as it is one of the characteristic species emitted by these sources: it is highly enriched in these plumes compared to the usual atmosphere and the {sup 210}Po radioactivity is not affected by chemical transformation. We have shown that the contribution of biomass burning on the {sup 210}Po concentration in local background atmosphere is minor during the dry season, compared to that of Saharan soil dusts despite of the importance of this source in the global budget of {sup 210}Po (10%). However, the good correlation observed between the {sup 210}Po concentration and that of carbonaceous aerosols and of CO{sub 2} in biomass burning plumes reveals that {sup 210}Po can be used as a reference of the components emitted by biomass burning. We have estimated the contribution of the Indonesian volcanoes which represent about 5 to 30 % of the global volcanic budget of trace metals. Atmospheric transport of these volcanic plumes was simulated using the {sup 210}Po as a tracer. Due to the characteristic atmospheric circulation in this region, vertical transport is predominant over meridian dispersion, which is moderated by the convergence of the trade winds. The impact of these volcanic emissions on the atmospheric concentration of the trace metals remains a local effect when the volcanic activity is out of cataclysmal eruptions. (author)

  19. 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.

  20. 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.

  1. Correlations between water-soluble organic aerosol and water vapor: a synergistic effect from biogenic emissions?

    Science.gov (United States)

    Hennigan, Christopher J; Bergin, Michael H; Weber, Rodney J

    2008-12-15

    Ground-based measurements of meteorological parameters and water-soluble organic carbon in the gas(WSOCg) and particle (WSOCp) phases were carried out in Atlanta, Georgia, from May to September 2007. Fourteen separate events were observed throughout the summer in which WSOCp and water vapor concentrations were highly correlated (average WSOCp-water vapor r = 0.92); however, for the entire summer, no well-defined relationship existed between the two. The correlation events, which lasted on average 19 h, were characterized by a wide range of WSOCp and water vapor concentrations. Several hypotheses for the correlation are explored, including heterogeneous liquid phase SOA formation and the co-emission of biogenic VOCs and water vapor. The data provide supporting evidence for contributions from both and suggest the possibility of a synergistic effect between the co-emission of water vapor and VOCs from biogenic sources on SOA formation. Median WSOCp concentrations were also correlated with elemental carbon (EC), although this correlation extended over the entire summer. Despite the emission of water vapor from anthropogenic mobile sources and the WSOCp-EC correlation, mobile sources were not considered a potential cause for the WSOCp-water vapor correlations because of their low contribution to the water vapor budget. Meteorology could perhaps have influenced the WSOCp-EC correlation, but other factors are implicated as well. Overall, the results suggest that the temperature-dependent co-emission of water vapor through evapotranspiration and SOA precursor-VOCs by vegetation may be an important process contributing to SOA in some environments.

  2. On the Link Between Ocean Biota Emissions, Aerosol, and Maritime Clouds: Airborne, Ground, and Satellite Measurements Off the Coast of California

    Science.gov (United States)

    2009-10-14

    Simpson, 1948; Lovelock et al., 1972; Andreae, 1990; Leck et al., 1990). Facchini et al. (2008a) have also shown that biogenic emissions are a...fastigiata, Dimethyl-2- carboxy-ethylsulphonium hydroxide and its salts, J. Chem. Soc., 3, 1591-1597. Charlson, R. J., Lovelock , J. E., Andreae...aerosols for pristine Arctic clouds, Tellus, 57B, 261-268. Lovelock , J. E., Maggs, R. J., and R. A. Rasmussen (1972). Atmospheric dimethyl sulfide and

  3. 76 FR 70833 - National Emission Standards for Hazardous Air Pollutant Emissions for Primary Lead Processing

    Science.gov (United States)

    2011-11-15

    ... INFORMATION: For specific information regarding the modeling methodology, contact Dr. Michael Stewart, Office... there is a malfunction, the emission limitation is still enforceable through injunctive relief. While... (GEP) stack height of 330 feet (as was done in the SIP and in modeling submitted by the Doe Run Company...

  4. Complementary online aerosol mass spectrometry and offline FT-IR spectroscopy measurements: Prospects and challenges for the analysis of anthropogenic aerosol particle emissions

    Science.gov (United States)

    Faber, Peter; Drewnick, Frank; Bierl, Reinhard; Borrmann, Stephan

    2017-10-01

    The aerosol mass spectrometer (AMS) is well established in investigating highly time-resolved dynamics of submicron aerosol chemical composition including organic aerosol (OA). However, interpretation of mass spectra on molecular level is limited due to strong fragmentation of organic substances and potential reactions inside the AMS ion chamber. Results from complementary filter-based FT-IR absorption measurements were used to explain features in high-resolution AMS mass spectra of different types of OA (e.g. cooking OA, cigarette smoking OA, wood burning OA). Using this approach some AMS fragment ions were validated in this study as appropriate and rather specific markers for a certain class of organic compounds for all particle types under investigation. These markers can therefore be used to get deeper insights in the chemical composition of OA based on AMS mass spectra in upcoming studies. However, the specificity of other fragment ions such as C2H4O2+ (m/z 60.02114) remains ambiguous. In such cases, complementary FT-IR measurements allow the interpretation of highly time-resolved AMS mass spectra at the level of molecular functional groups. Furthermore, this study discusses the challenges in reducing inorganic interferences (e.g. from water and ammonium salts) in FT-IR spectra of atmospheric aerosols to decrease spectral uncertainties for better comparisons and, thus, to get more robust results.

  5. Mutagenicity assessment of aerosols in emissions from wood combustion in Portugal.

    Science.gov (United States)

    Vu, B; Alves, C A; Gonçalves, C; Pio, C; Gonçalves, F; Pereira, R

    2012-07-01

    Polycyclic aromatic hydrocarbon (PAH) extracts of fine particles (PM(2.5)) collected from combustion of seven wood species and briquettes were tested for mutagenic activities using Ames test with Salmonella typhimurium TA98 and TA100. The woods were Pinus pinaster (maritime pine), Eucalyptus globulus (eucalypt), Quercus suber (cork oak), Acacia longifolia (golden wattle), Quercus faginea (Portuguese oak), Olea europea (olive), and Quercus ilex rotundifolia (Holm oak). Burning experiments were done using woodstove and fireplace, hot start and cold start conditions. A mutagenic response was recorded for all species except golden wattle, maritime pine, and briquettes. The mutagenic extracts were not correlated with high emission factors of carcinogenic PAHs. These extracts were obtained both from two burning appliances and start-up conditions. However, fireplace seemed to favour the occurrence of mutagenic emissions. The negative result recorded for golden wattle was interesting, in an ecological point of view, since after confirmation, this invasive species, can be recommended for domestic use. Copyright © 2012 Elsevier Ltd. All rights reserved.

  6. Tropospheric Aerosols

    Science.gov (United States)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  7. 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.

  8. Emission characteristics of refractory black carbon aerosols from fresh biomass burning: a perspective from laboratory experiments

    Science.gov (United States)

    Pan, Xiaole; Kanaya, Yugo; Taketani, Fumikazu; Miyakawa, Takuma; Inomata, Satoshi; Komazaki, Yuichi; Tanimoto, Hiroshi; Wang, Zhe; Uno, Itsushi; Wang, Zifa

    2017-11-01

    The emission characteristics of refractory black carbon (rBC) from biomass burning are essential information for numerical simulations of regional pollution and climate effects. We conducted combustion experiments in the laboratory to investigate the emission ratio and mixing state of rBC from the burning of wheat straw and rapeseed plants, which are the main crops cultivated in the Yangtze River Delta region of China. A single particle soot photometer (SP2) was used to measure rBC-containing particles at high temporal resolution and with high accuracy. The combustion state of each burning case was indicated by the modified combustion efficiency (MCE), which is calculated using the integrated enhancement of carbon dioxide and carbon monoxide concentrations relative to their background values. The mass size distribution of the rBC particles showed a lognormal shape with a mode mass equivalent diameter (MED) of 189 nm (ranging from 152 to 215 nm), assuming an rBC density of 1.8 g cm-3. rBC particles less than 80 nm in size (the lower detection limit of the SP2) accounted for ˜ 5 % of the total rBC mass, on average. The emission ratios, which are expressed as ΔrBC / ΔCO (Δ indicates the difference between the observed and background values), displayed a significant positive correlation with the MCE values and varied between 1.8 and 34 ng m-3 ppbv-1. Multi-peak fitting analysis of the delay time (Δt, or the time of occurrence of the scattering peak minus that of the incandescence peak) distribution showed that rBC-containing particles with rBC MED = 200 ± 10 nm displayed two peaks at Δt = 1.7 µs and Δt = 3.2 µs, which could be attributed to the contributions from both flaming and smoldering combustion in each burning case. Both the Δt values and the shell / core ratios of the rBC-containing particles clearly increased as the MCE decreased from 0.98 (smoldering-dominant combustion) to 0.86 (flaming-dominant combustion), implying the great importance of the

  9. Application of Recent Advances in Forward Modeling of Emissions from Boreal and Temperate Wildfires to Real-time Forecasting of Aerosol and Trace Gas Concentrations

    Science.gov (United States)

    Hyer, E. J.; Reid, J. S.; Kasischke, E. S.; Allen, D. J.

    2005-12-01

    The magnitude of trace gas and aerosol emissions from wildfires is a scientific problem with important implications for atmospheric composition, and is also integral to understanding carbon cycling in terrestrial ecosystems. Recent ecological research on modeling wildfire emissions has integrated theoretical advances derived from ecological fieldwork with improved spatial and temporal databases to produce "post facto" estimates of emissions with high spatial and temporal resolution. These advances have been shown to improve agreement with atmospheric observations at coarse scales, but can in principle be applied to applications, such as forecasting, at finer scales. However, several of the approaches employed in these forward models are incompatible with the requirements of real-time forecasting, requiring modification of data inputs and calculation methods. Because of the differences in data inputs used for real-time and "post-facto" emissions modeling, the key uncertainties in the forward problem are not necessarily the same for these two applications. However, adaptation of these advances in forward modeling to forecasting applications has the potential to improve air quality forecasts, and also to provide a large body of experimental data which can be used to constrain crucial uncertainties in current conceptual models of wildfire emissions. This talk describes a forward modeling method developed at the University of Maryland and its application to the Fire Locating and Modeling of Burning Emissions (FLAMBE) system at the Naval Research Laboratory. Methods for applying the outputs of the NRL aerosol forecasting system to the inverse problem of constraining emissions will also be discussed. The system described can use the feedback supplied by atmospheric observations to improve the emissions source description in the forecasting model, and can also be used for hypothesis testing regarding fire behavior and data inputs.

  10. Projected effect of 2000-2050 changes in climate and emissions on aerosol levels in China and associated transboundary transport

    Science.gov (United States)

    We investigate projected 2000–2050 changes in concentrations of aerosols in China and the associated transboundary aerosol transport by using the chemical transport model GEOS-Chem driven by the Goddard Institute for Space Studies (GISS) general circulation model (GCM) 3 at 4° × ...

  11. Primary and Aggregate Size Distributions of PM in Tail Pipe Emissions form Diesel Engines

    Science.gov (United States)

    Arai, Masataka; Amagai, Kenji; Nakaji, Takayuki; Hayashi, Shinji

    Particulate matter (PM) emission exhausted from diesel engine should be reduced to keep the clean air environment. PM emission was considered that it consisted of coarse and aggregate particles, and nuclei-mode particles of which diameter was less than 50nm. However the detail characteristics about these particles of the PM were still unknown and they were needed for more physically accurate measurement and more effective reduction of exhaust PM emission. In this study, the size distributions of solid particles in PM emission were reported. PMs in the tail-pipe emission were sampled from three type diesel engines. Sampled PM was chemically treated to separate the solid carbon fraction from other fractions such as soluble organic fraction (SOF). The electron microscopic and optical-manual size measurement procedures were used to determine the size distribution of primary particles those were formed through coagulation process from nuclei-mode particles and consisted in aggregate particles. The centrifugal sedimentation method was applied to measure the Stokes diameter of dry-soot. Aerodynamic diameters of nano and aggregate particles were measured with scanning mobility particle sizer (SMPS). The peak aggregate diameters detected by SMPS were fallen in the same size regime as the Stokes diameter of dry-soot. Both of primary and Stokes diameters of dry-soot decreased with increases of engine speed and excess air ratio. Also, the effects of fuel properties and engine types on primary and aggregate particle diameters were discussed.

  12. Toxicological Evaluation of Realistic Emissions of Source Aerosols (TERESA): Application to Power Plant-Derived PM2.5

    Energy Technology Data Exchange (ETDEWEB)

    Annette Rohr

    2007-02-28

    This report documents progress made on the subject project during the period of September 1, 2007 through February 28, 2007. 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 performance and analysis of field experiments at the first TERESA plant, located in the Upper Midwest and henceforth referred to as Plant 0, and at two additional coal-fired power plants (Plants 1 and 2) utilizing different coal types and with different plant configurations. During this reporting period, fieldwork was completed at Plant 2, located in the Midwest. The following scenarios were completed: (1) July 19-22: POS (oxidized + SOA); (2) July 25-28: PONS (oxidized + neutralized + SOA); (3) August 8-13: P (primary); (4) August 14-15: POS; (5) August 16-17: POS (MI rats); (6) August 28-31: OS (oxidized + SOA, without primary particles); (7) September 1-4: O (oxidized, no primary particles); (8) September 6-9: S (SOA, no primary particles); and (9) September 19-22: PO (oxidized). Results indicated some biological effects with some scenarios. Also during this reporting period, the annual meeting of the TERESA Technical Advisory Committee was held at the Harvard School of Public Health in Boston. During the next reporting period, data analyses will continue for Plant 2 as well as for pooled data from all three plants. Manuscripts documenting the overall

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

    Science.gov (United States)

    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.

  14. Emission characteristics of refractory black carbon aerosols from fresh biomass burning: a perspective from laboratory experiments

    Directory of Open Access Journals (Sweden)

    X. Pan

    2017-11-01

    Full Text Available The emission characteristics of refractory black carbon (rBC from biomass burning are essential information for numerical simulations of regional pollution and climate effects. We conducted combustion experiments in the laboratory to investigate the emission ratio and mixing state of rBC from the burning of wheat straw and rapeseed plants, which are the main crops cultivated in the Yangtze River Delta region of China. A single particle soot photometer (SP2 was used to measure rBC-containing particles at high temporal resolution and with high accuracy. The combustion state of each burning case was indicated by the modified combustion efficiency (MCE, which is calculated using the integrated enhancement of carbon dioxide and carbon monoxide concentrations relative to their background values. The mass size distribution of the rBC particles showed a lognormal shape with a mode mass equivalent diameter (MED of 189 nm (ranging from 152 to 215 nm, assuming an rBC density of 1.8 g cm−3. rBC particles less than 80 nm in size (the lower detection limit of the SP2 accounted for ∼ 5 % of the total rBC mass, on average. The emission ratios, which are expressed as ΔrBC ∕ ΔCO (Δ indicates the difference between the observed and background values, displayed a significant positive correlation with the MCE values and varied between 1.8 and 34 ng m−3 ppbv−1. Multi-peak fitting analysis of the delay time (Δt, or the time of occurrence of the scattering peak minus that of the incandescence peak distribution showed that rBC-containing particles with rBC MED  =  200 ± 10 nm displayed two peaks at Δt  =  1.7 µs and Δt  =  3.2 µs, which could be attributed to the contributions from both flaming and smoldering combustion in each burning case. Both the Δt values and the shell / core ratios of the rBC-containing particles clearly increased as the MCE decreased from 0.98 (smoldering

  15. 76 FR 76259 - National Emissions Standards for Hazardous Air Pollutants: Primary Aluminum Reduction Plants

    Science.gov (United States)

    2011-12-06

    ... Emissions From Maleic Anhydride Plants, Ethylbenzene/Styrene Plants, Benzene Storage Vessels, Benzene...). The rule is applicable to facilities with affected sources associated with the production of aluminum... are subject to the requirements of this NESHAP: 14 primary aluminum production plants and one carbon...

  16. 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.

  17. 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.

  18. 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.)

  19. Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

    Directory of Open Access Journals (Sweden)

    Y. Wang

    2013-03-01

    Full Text Available We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3 from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60% and 80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC and Sichuan Basin (SCB, while nitrate and sulfate contribute equally over North China (NC. Based on emission reduction targets in the 12th (2011–2015 Five-Year Plan (FYP, China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. The amount of NH3 emissions in 2015 is uncertain, given the lack of sufficient information on the past and present levels of NH3 emissions in China. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their 2006 levels, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC, for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

  20. A national day with near zero emissions and its effect on primary and secondary pollutants

    Science.gov (United States)

    Levy, Ilan

    2013-10-01

    Traffic related air pollution is a major health concern in many countries. The potential costs and benefits of different abatement policies are usually estimated by either models, case studies or previously implemented intervention measures. Such estimations have, however, limited ability to predict the effect of a reduction in primary pollutants' emissions on secondary pollutants such as ozone, because of the nonlinear nature of the photochemical reactions. This study examines the short term effects of a drastic change in emissions on a national scale during the Jewish holiday of Day of Atonement (DA) in Israel. During the holiday nearly all anthropogenic emission sources are ceased for a period of 25 h, including all vehicles, commercial, industrial and recreational activities. DAs during the 15 years period of 1998-2012 are analyzed at three sites with respect to primary and secondary air pollutants, and in greater details for 2001. A dramatic decrease in primary pollutants emissions (83-98% in NO) causes an 8 ppbv increase in ozone at the urban core. Downwind (27 km), ozone decreases by only 5 ppbv. Nighttime O3 is shown to increase to 20 ppbv at the urban sites and 30 ppbv downwind. In spite of the striking reduction in emissions, changes in ozone are not greater than what is reported in the literature about less significant events like the ozone weekend effect. Changes in ambient pollution levels observed during DA provide some indication to the possible outcomes of a major change in anthropogenic emissions. These may be considered as the best case scenario for emissions reduction intervention measures and thus aid policy makers in evaluating potential benefits of such measures.

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

    Energy Technology Data Exchange (ETDEWEB)

    Annette Rohr

    2006-03-31

    This report documents progress made on the subject project during the period of September 1, 2005 through February 28, 2006. 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 performance and analysis of field experiments at the first TERESA plant, located in the Upper Midwest and henceforth referred to as Plant 0, and at two additional coal-fired power plants (Plants 1 and 2) utilizing different coal types and with different plant configurations. During this reporting period, data processing and analyses were completed for exposure and toxicological data collected during the field campaign at Plant 1, located in the Southeast. To recap from the previous progress report, Stage I toxicological assessments were carried out in normal Sprague-Dawley rats, and Stage II assessments were carried out in a compromised model (myocardial infarction-MI-model). Normal rats were exposed to the following atmospheric scenarios: (1) primary particles; (2) oxidized emissions; (3) oxidized emissions + SOA--this scenario was repeated; and (4) oxidized emissions + ammonia + SOA. Compromised animals were exposed to oxidized emissions + SOA (this scenario was also conducted in replicate). Mass concentrations in exposure atmospheres ranged from 13.9 {micro}g/m{sup 3} for the primary particle scenario (P) to 385 {micro}g/m{sup 3} for one of the oxidized

  2. Primary and secondary contributions to aerosol light scattering and absorption in Mexico City during the MILAGRO 2006 campaign

    Directory of Open Access Journals (Sweden)

    G. Paredes-Miranda

    2009-06-01

    Full Text Available A photoacoustic spectrometer, a nephelometer, an aethalometer, and an aerosol mass spectrometer were used to measure at ground level real-time aerosol light absorption, scattering, and chemistry at an urban site located in North East Mexico City (Instituto Mexicano del Petroleo, Mexican Petroleum Institute, denoted by IMP, as part of the Megacity Impact on Regional and Global Environments field experiment, MILAGRO, in March 2006. Photoacoustic and reciprocal nephelometer measurements at 532 nm accomplished with a single instrument compare favorably with conventional measurements made with an aethalometer and a TSI nephelometer. The diurnally averaged single scattering albedo at 532 nm was found to vary from 0.60 to 0.85 with the peak value at midday and the minimum value at 07:00 a.m. local time, indicating that the Mexico City plume is likely to have a net warming effect on local climate. The peak value is associated with strong photochemical generation of secondary aerosol. It is estimated that the photochemical production of secondary aerosol (inorganic and organic is approximately 75% of the aerosol mass concentration and light scattering in association with the peak single scattering albedo. A strong correlation of aerosol scattering at 532 nm and total aerosol mass concentration was found, and an average mass scattering efficiency factor of 3.8 m2/g was determined. Comparisons of photoacoustic and aethalometer light absorption with oxygenated organic aerosol concentration (OOA indicate a very small systematic bias of the filter based measurement associated with OOA and the peak aerosol single scattering albedo.

  3. Primary and secondary contributions to aerosol light scattering and absorption in Mexico City during the MILAGRO 2006 campaign

    Science.gov (United States)

    Paredes-Miranda, G.; Arnott, W. P.; Jimenez, J. L.; Aiken, A. C.; Gaffney, J. S.; Marley, N. A.

    2009-06-01

    A photoacoustic spectrometer, a nephelometer, an aethalometer, and an aerosol mass spectrometer were used to measure at ground level real-time aerosol light absorption, scattering, and chemistry at an urban site located in North East Mexico City (Instituto Mexicano del Petroleo, Mexican Petroleum Institute, denoted by IMP), as part of the Megacity Impact on Regional and Global Environments field experiment, MILAGRO, in March 2006. Photoacoustic and reciprocal nephelometer measurements at 532 nm accomplished with a single instrument compare favorably with conventional measurements made with an aethalometer and a TSI nephelometer. The diurnally averaged single scattering albedo at 532 nm was found to vary from 0.60 to 0.85 with the peak value at midday and the minimum value at 07:00 a.m. local time, indicating that the Mexico City plume is likely to have a net warming effect on local climate. The peak value is associated with strong photochemical generation of secondary aerosol. It is estimated that the photochemical production of secondary aerosol (inorganic and organic) is approximately 75% of the aerosol mass concentration and light scattering in association with the peak single scattering albedo. A strong correlation of aerosol scattering at 532 nm and total aerosol mass concentration was found, and an average mass scattering efficiency factor of 3.8 m2/g was determined. Comparisons of photoacoustic and aethalometer light absorption with oxygenated organic aerosol concentration (OOA) indicate a very small systematic bias of the filter based measurement associated with OOA and the peak aerosol single scattering albedo.

  4. Environmental exposure of primary care personnel to ribavirin aerosol when supervising treatment of infants with respiratory syncytial virus infections.

    Science.gov (United States)

    Rodriguez, W J; Bui, R H; Connor, J D; Kim, H W; Brandt, C D; Parrott, R H; Burch, B; Mace, J

    1987-01-01

    The potential exposure to ribavirin aerosol in the environment was assessed in nurses caring for infants and children with severe lower respiratory tract infections due to respiratory syncytial virus. Ribavirin aerosol was administered via a ventilator, oxygen tent, or oxygen hood. Participants worked directly with infants receiving ribavirin for 20.0 to 35.0 h over a 3-day period. No toxic or adverse effects of ribavirin aerosol were observed in any of the 19 nurses studied, and ribavirin was not detected in erythrocytes, plasma, or urine collected after the potential exposure period. PMID:3662474

  5. Simulation of the interannual variations of biogenic emissions of volatile organic compounds in China: Impacts on tropospheric ozone and secondary organic aerosol

    Science.gov (United States)

    Fu, Y.; Liao, H.

    2012-12-01

    We use the MEGAN (Model of emissions of Gases and Aerosols from Nature) module embedded within the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to simulate the interannual variations in biogenic volatile organic compound (BVOC) emissions and concentrations of ozone and secondary organic aerosols (SOA) in China over years 2001-2006. To have better representation of biogenic emissions, we have updated in the model the land cover and leaf area index in China using Moderate Resolution Imaging Spectroradiometer (MODIS) satellite measurements, and we have developed a new classification of vegetation with 21 plant functional types. Estimated annual BVOC emission in China averaged over 2001-2006 is 18.85 Tg C yr-1, in which emissions of isoprene, monoterpenes, and other reactive volatile organic compounds account for 50.9%, 15.0%, and 34.1%, respectively. The simulated BVOC emissions in China have large interannual variations. The values of regionally averaged absolute percent departure from the mean (APDM) of isoprene emissions are in the range of 21-42% in January and 15-28% in July. The APDM values of monoterpene emissions are 14-32% in January and 10-21% in July, which are generally smaller than those of isoprene emissions. Model results indicate that the interannual variations in isoprene emissions are more dependent on variations in meteorological fields, whereas the interannual variations in monoterpene emissions are more sensitive to changes in vegetation parameters. With fixed anthropogenic emissions, as a result of the variations in both meteorological parameters and vegetation, simulated O3 concentrations show interannual variations of 0.8-5 ppbv (or largest APDM values of 4-15%), and simulated SOA shows APDM values of 5-15% in southwestern China in January as well as 10-25% in southeastern and 20-35% in northeastern China in July. On a regional mean basis, the interannual variations in BVOCs alone can lead to 2

  6. Interannual variation in the fine-mode MODIS aerosol optical depth and its relationship to the changes in sulfur dioxide emissions in China between 2000 and 2010

    Directory of Open Access Journals (Sweden)

    S. Itahashi

    2012-03-01

    Full Text Available Anthropogenic SO2 emissions increased alongside economic development in China at a rate of 12.7% yr−1 from 2000 to 2005. However, under new Chinese government policy, SO2 emissions declined by 3.9% yr−1 between 2005 and 2009. Between 2000 and 2010, we found that the variability in the fine-mode (submicron aerosol optical depth (AOD over the oceans adjacent to East Asia increased by 3–8% yr−1 to a peak around 2005–2006 and subsequently decreased by 2–7% yr−1, based on observations by the Moderate Resolution Imaging Spectroradiometer (MODIS on board NASA's Terra satellite and simulations by a chemical transport model. This trend is consistent with ground-based observations of aerosol particles at a mountainous background observation site in central Japan. These fluctuations in SO2 emission intensity and fine-mode AOD are thought to reflect the widespread installation of fuel-gas desulfurization (FGD devices in power plants in China, because aerosol sulfate is a major determinant of the fine-mode AOD in East Asia. Using a chemical transport model, we confirmed that the contribution of particulate sulfate to the fine-mode AOD is more than 70% of the annual mean and that the abovementioned fluctuation in fine-mode AOD is caused mainly by changes in SO2 emission rather than by other factors such as varying meteorological conditions in East Asia. A strong correlation was also found between satellite-retrieved SO2 vertical column density and bottom-up SO2 emissions, both of which were also consistent with observed fine-mode AOD trends. We propose a simplified approach for evaluating changes in SO2 emissions in China, combining the use of modeled sensitivity coefficients that describe the variation of fine-mode AOD with changes in SO2 emissions and satellite retrieval. Satellite measurements of fine-mode AOD

  7. 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-NOx and low-NOx 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.

  8. he Impact of Primary Marine Aerosol on Atmospheric Chemistry, Radiation and Climate: A CCSM Model Development Study

    Energy Technology Data Exchange (ETDEWEB)

    Keene, William C. [University of Virginia; Long, Michael S. [University of Virginia

    2013-05-20

    This project examined the potential large-scale influence of marine aerosol cycling on atmospheric chemistry, physics and radiative transfer. Measurements indicate that the size-dependent generation of marine aerosols by wind waves at the ocean surface and the subsequent production and cycling of halogen-radicals are important but poorly constrained processes that influence climate regionally and globally. A reliable capacity to examine the role of marine aerosol in the global-scale atmospheric system requires that the important size-resolved chemical processes be treated explicitly. But the treatment of multiphase chemistry across the breadth of chemical scenarios encountered throughout the atmosphere is sensitive to the initial conditions and the precision of the solution method. This study examined this sensitivity, constrained it using high-resolution laboratory and field measurements, and deployed it in a coupled chemical-microphysical 3-D atmosphere model. First, laboratory measurements of fresh, unreacted marine aerosol were used to formulate a sea-state based marine aerosol source parameterization that captured the initial organic, inorganic, and physical conditions of the aerosol population. Second, a multiphase chemical mechanism, solved using the Max Planck Institute for Chemistry's MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) system, was benchmarked across a broad set of observed chemical and physical conditions in the marine atmosphere. Using these results, the mechanism was systematically reduced to maximize computational speed. Finally, the mechanism was coupled to the 3-mode modal aerosol version of the NCAR Community Atmosphere Model (CAM v3.6.33). Decadal-scale simulations with CAM v.3.6.33, were run both with and without reactive-halogen chemistry and with and without explicit treatment of particulate organic carbon in the marine aerosol source function. Simulated results were interpreted (1) to evaluate influences

  9. Radiocarbon (14C) Constraints On The Fraction Of Refractory Dissolved Organic Carbon In Primary Marine Aerosol From The Northwest Atlantic

    Science.gov (United States)

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

    2017-12-01

    Nearly all organic carbon in seawater is dissolved (DOC), with more than 95% considered refractory based on modeled average lifetimes ( 16,000 years) and characteristically old bulk radiocarbon (14C) ages (4000 - 6000 years) that exceed the timescales of overturning circulation. Although this refractory dissolved organic carbon (RDOC) is present throughout the oceans as a major reservoir of the global carbon cycle, its sources and sinks are poorly constrained. Recently, RDOC was proposed to be removed from the oceans through adsorption onto the surfaces of rising bubble plumes produced by breaking waves, ejection into the atmosphere via bubble bursting as a component of primary marine aerosol (PMA), and subsequent oxidation in the atmosphere. To test this mechanism, we used natural abundance 14C (5730 ± 40 yr half-life) to trace the fraction of RDOC in PMA produced in a high capacity generator at two biologically-productive and two oligotrophic hydrographic stations in the Northwest Atlantic Ocean during a research cruise aboard the R/V Endeavor (Sep - Oct 2016). The 14C signatures of PMA separately generated day and night from near-surface (5 m) and deep (2500 m) seawater were compared with corresponding 14C signatures in seawater of near-surface dissolved inorganic carbon (DIC, a proxy for recently produced organic matter), bulk deep DOC (a proxy for RDOC), and near-surface bulk DOC. Results constrain the selectivity of PMA formation from RDOC in natural mixtures of recently produced and refractory DOC. The implications of these results for PMA formation and RDOC biogeochemistry will be discussed.

  10. Current and future emissions of primary pollutants from coal-fired power plants in Shaanxi, China.

    Science.gov (United States)

    Xu, Yong; Hu, Jianlin; Ying, Qi; Hao, Hongke; Wang, Dexiang; Zhang, Hongliang

    2017-10-01

    A high-resolution inventory of primary atmospheric pollutants from coal-fired power plants in Shaanxi in 2012 was built based on a detailed database compiled at unit level involving unit capacity, boiler size and type, commission time, corresponding control technologies, and average coal quality of 72 power plants. The pollutants included SO 2 , NO x , fine particulate matter (PM 2.5 ), inhalable particulate matter (PM 10 ), organic carbon (OC), elemental carbon (EC), carbon monoxide (CO) and non-methane volatile organic compounds (NMVOC). Emission factors for SO 2 , NO x , PM 2.5 and PM 10 were adopted from standardized official promulgation, supplemented by those from local studies. The estimated annual emissions of SO 2 , NO x , PM 2.5 , PM 10 , EC, OC, CO and NMVOC were 152.4, 314.8, 16.6, 26.4, 0.07, 0.27, 64.9 and 2.5kt, respectively. Small units (emission rates compared to medium (≥100MW and emissions were decontamination efficiency, sulfur content and ash content of coal. Weinan and Xianyang were the two cities with the highest emissions, and Guanzhong Plain had the largest emission density. Despite the projected growth of coal consumption, emissions would decrease in 2030 due to improvement in emission control technologies and combustion efficiencies. SO 2 and NO x emissions would experience significant reduction by ~81% and ~84%, respectively. PM 2.5 , PM 10 , EC and OC would be decreased by ~43% and CO and NMVOC would be reduced by ~16%. Copyright © 2017 Elsevier B.V. All rights reserved.

  11. 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

  12. 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.

  13. 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.)

  14. 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.

  15. 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...

  16. Black carbon aerosol properties measured by a single particle soot photometer in emissions from biomass burning in the laboratory and field

    Science.gov (United States)

    G. R. McMeeking; J. W. Taylor; A. P. Sullivan; M. J. Flynn; S. K. Akagi; C. M. Carrico; J. L. Collett; E. Fortner; T. B. Onasch; S. M. Kreidenweis; R. J. Yokelson; C. Hennigan; A. L. Robinson; H. Coe

    2010-01-01

    We present SP2 observations of BC mass, size distributions and mixing state in emissions from laboratory and field biomass fires in California, USA. Biomass burning is the primary global black carbon (BC) source, but understanding of the amount emitted and its physical properties at and following emission are limited. The single particle soot photometer (SP2) uses a...

  17. Comparison of Gasoline Direct-Injection (GDI) and Port Fuel Injection (PFI) Vehicle Emissions: Emission Certification Standards, Cold-Start, Secondary Organic Aerosol Formation Potential, and Potential Climate Impacts.

    Science.gov (United States)

    Saliba, Georges; Saleh, Rawad; Zhao, Yunliang; Presto, Albert A; Lambe, Andrew T; Frodin, Bruce; Sardar, Satya; Maldonado, Hector; Maddox, Christine; May, Andrew A; Drozd, Greg T; Goldstein, Allen H; Russell, Lynn M; Hagen, Fabian; Robinson, Allen L

    2017-06-06

    Recent increases in the Corporate Average Fuel Economy standards have led to widespread adoption of vehicles equipped with gasoline direct-injection (GDI) engines. Changes in engine technologies can alter emissions. To quantify these effects, we measured gas- and particle-phase emissions from 82 light-duty gasoline vehicles recruited from the California in-use fleet tested on a chassis dynamometer using the cold-start unified cycle. The fleet included 15 GDI vehicles, including 8 GDIs certified to the most-stringent emissions standard, superultra-low-emission vehicles (SULEV). We quantified the effects of engine technology, emission certification standards, and cold-start on emissions. For vehicles certified to the same emissions standard, there is no statistical difference of regulated gas-phase pollutant emissions between PFIs and GDIs. However, GDIs had, on average, a factor of 2 higher particulate matter (PM) mass emissions than PFIs due to higher elemental carbon (EC) emissions. SULEV certified GDIs have a factor of 2 lower PM mass emissions than GDIs certified as ultralow-emission vehicles (3.0 ± 1.1 versus 6.3 ± 1.1 mg/mi), suggesting improvements in engine design and calibration. Comprehensive organic speciation revealed no statistically significant differences in the composition of the volatile organic compounds emissions between PFI and GDIs, including benzene, toluene, ethylbenzene, and xylenes (BTEX). Therefore, the secondary organic aerosol and ozone formation potential of the exhaust does not depend on engine technology. Cold-start contributes a larger fraction of the total unified cycle emissions for vehicles meeting more-stringent emission standards. Organic gas emissions were the most sensitive to cold-start compared to the other pollutants tested here. There were no statistically significant differences in the effects of cold-start on GDIs and PFIs. For our test fleet, the measured 14.5% decrease in CO 2 emissions from GDIs was much greater than

  18. Analysis of aerosol composition data for western United States wildfires between 2005 and 2015: Dust emissions, chloride depletion, and most enhanced aerosol constituents

    Science.gov (United States)

    Schlosser, Joseph S.; Braun, Rachel A.; Bradley, Trevor; Dadashazar, Hossein; MacDonald, Alexander B.; Aldhaif, Abdulmonam A.; Aghdam, Mojtaba Azadi; Mardi, Ali Hossein; Xian, Peng; Sorooshian, Armin

    2017-08-01

    This study examines major wildfires in the western United States between 2005 and 2015 to determine which species exhibit the highest percent change in mass concentration on day of peak fire influence relative to preceding nonfire days. Forty-one fires were examined using the Environmental Protection Agency (EPA) Interagency Monitoring of Protected Visual Environments (IMPROVE) data set. Organic carbon (OC) and elemental carbon (EC) constituents exhibited the highest percent change increase. The sharpest enhancements were for the volatile (OC1) and semivolatile (OC2) OC fractions, suggestive of secondary organic aerosol formation during plume transport. Of the noncarbonaceous constituents, Cl, P, K, NO3-, and Zn levels exhibited the highest percent change. Dust was significantly enhanced in wildfire plumes, based on significant enhancements in fine soil components (i.e., Si, Ca, Al, Fe, and Ti) and PMcoarse (i.e., PM10-PM2.5). A case study emphasized how transport of wildfire plumes significantly impacted downwind states, with higher levels of fine soil and PMcoarse at the downwind state (Arizona) as compared to the source of the fires (California). A global model (Navy Aerosol Analysis and Prediction System, NAAPS) did not capture the dust influence over California or Arizona during this case event because it is not designed to resolve dust dynamics in fires, which motivates improved treatment of such processes. Significant chloride depletion was observed on the peak EC day for almost a half of the fires examined. Size-resolved measurements during two specific fires at a coastal California site revealed significant chloride reductions for particle aerodynamic diameters between 1 and 10 μm.

  19. 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

  20. C1-C2 alkyl aminiums in urban aerosols: Insights from ambient and fuel combustion emission measurements in the Yangtze River Delta region of China

    International Nuclear Information System (INIS)

    Shen, Wenchao; Ren, Lili; Zhao, Yi; Zhou, Luyu; Dai, Liang; Ge, Xinlei; Kong, Shaofei; Yan, Qin; Xu, Honghui; Jiang, Yujun; He, Jun; Chen, Mindong; Yu, Huan

    2017-01-01

    We measured low molar-mass alkyl aminiums (methylaminium, dimethylaminium, ethylaminium and diethylaminium) in urban aerosols in the Yangtze River Delta region of eastern China in August 2014 and from November 2015 to May 2016. After examining artifact formation on sample filters, methylaminium, dimethylaminium and ethylaminium concentrations were quantified. The three C1-C2 aminiums exhibited a unimodal size distribution that maximized between 0.56 and 1.0 μm. Their concentrations in PM 2.5 were 5.7 ± 3.2 ng m −3 , 7.9 ± 5.4 ng m −3 and 20.3 ± 16.6 ng m −3 , respectively, with higher concentrations during the daytime and in warm seasons. On new particle growth days, amine uptake to particles larger than 56 nm was barely enhanced. The molar ratios of individual aminium/NH 4 + in PM 2.5 were on the order of 10 −4 and 10 −3 . Aminiums were thus far less to out-compete ammonium (NH 4 + ) in neutralizing acidic species in particle sizes down to 56 nm. Abundant nitrate (NO 3 − /SO 4 2− molar ratio = ∼3) and its correlation to methylaminium and ethylaminium implied that nitrate might be more important aminium salt than sulfate in urban aerosols of this area. Direct measurement of particle-phase amine emission from coal and biomass burning showed that coal burning is an important atmospheric amine source, considering coal burning is top-ranked particulate matter source in China. - Highlights: • Aminium concentration showed seasonal and diurnal variations in urban aerosols of our area. • Nitrate was more important aminium salt than sulfate in urban aerosols of our area. • Particle-phase amine emission from coal burning is an important atmospheric amine source. • Amine uptake to particles larger than 56 nm was barely enhanced on new particle growth events. • Aminiums cannot out-compete ammonium in neutralizing acidic species in urban aerosols with particle sizes down to 56 nm. - Aminiums cannot out-compete ammonium in

  1. Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

    Science.gov (United States)

    Zhang, Xinghua; Xu, Jianzhong; Kang, Shichang; Liu, Yanmei; Zhang, Qi

    2018-04-01

    An intensive field measurement was conducted at a remote, background, 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 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1) and obtain the dynamic processes (emissions, transport, and chemical evolution) of biomass burning (BB), frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ) PM1 mass concentration was 4.44 (±4.54) µg m-3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA) was the dominant PM1 species (accounting for 54.3 % of total PM1 on average) followed by black carbon (BC) (25.0 %), sulfate (9.3 %), ammonium (5.8 %), nitrate (5.1 %), and chloride (0.4 %). 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 transport. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %), a nitrogen-containing OA (NOA, 13.9 %) and a more-oxidized oxygenated OA (MO-OOA, 42.4 %). Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

  2. Diurnal cycling of urban aerosols under different weather regimes

    Science.gov (United States)

    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

  3. Fluorine-18 fluorodeoxyglucose positron emission tomography/computed tomography in the detection of primary pulmonary angiosarcomas

    International Nuclear Information System (INIS)

    Krishnamurthy, Arvind; Nayak, Deepika; Ramshankar, Vijayalakshmi; Majhi, Urmila

    2015-01-01

    Angiosarcoma is a malignant vascular tumor that originates from the mesenchymal cells which have undergone angioblastic differentiation. Pulmonary angiosarcomas are invariably (>90%) metastatic tumors form primaries of the skin, bone, liver, breast, or heart. Primary pulmonary angiosarcomas are exceedingly rare, with just about 20 cases being reported in the literature. We report an additional case with a brief review of the literature of a primary pulmonary angiosarcoma in a 26-year-old lady who presented with intractable hemoptysis. In addition, we highlight the potential of fluorine-18 fluorodeoxyglucose positron emission tomography/computed tomography as an important diagnostic tool in the evaluation of this tumor and thus contribute to the existing sparse literature on this fascinating yet devastating disease

  4. a Study of the Origin of Atmospheric Organic Aerosols

    Science.gov (United States)

    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

  5. GHG AND AEROSOL EMISSION FROM FIRE PIXEL DURING CROP RESIDUE BURNING UNDER RICE AND WHEAT CROPPING SYSTEMS IN NORTH-WEST INDIA

    Directory of Open Access Journals (Sweden)

    P. Acharya

    2016-10-01

    Full Text Available Emission of smoke and aerosol from open field burning of crop residue is a long-standing subject matter of atmospheric pollution. In this study, we proposed a new approach of estimating fuel load in the fire pixels and corresponding emissions of selected GHGs and aerosols i.e. CO2, CO, NO2, SO2, and total particulate matter (TPM due to burning of crop residue under rice and wheat cropping systems in Punjab in north-west India from 2002 to 2012. In contrasts to the conventional method that uses RPR ratio to estimate the biomass, fuel load in the fire pixels was estimated as a function of enhanced vegetation index (EVI. MODIS fire products were used to detect the fire pixels during harvesting seasons of rice and wheat. Based on the field measurements, fuel load in the fire pixels were modelled as a function of average EVI using second order polynomial regression. Average EVI for rice and wheat crops that were extracted through Fourier transformation were computed from MODIS time series 16 day EVI composites. About 23 % of net shown area (NSA during rice and 11 % during wheat harvesting seasons are affected by field burning. The computed average fuel loads are 11.32 t/ha (±17.4 during rice and 10.89 t/ha (±8.7 during wheat harvesting seasons. Calculated average total emissions of CO2, CO, NO2, SO2 and TPM were 8108.41, 657.85, 8.10, 4.10, and 133.21 Gg during rice straw burning and 6896.85, 625.09, 1.42, 1.77, and 57.55 Gg during wheat burning. Comparison of estimated values shows better agreement with the previous concurrent estimations. The method, however, shows its efficiency parallel to the conventional method of estimation of fuel load and related pollutant emissions.

  6. Distortion product otoacoustic emissions: comparison of sequential vs. simultaneous presentation of primary tones.

    Science.gov (United States)

    Kumar, U Ajith; Maruthy, Sandeep; Chandrakant, Vishwakarma

    2009-03-01

    Distortion product otoacoustic emissions are one form of evoked otoacoustic emissions. DPOAEs provide the frequency specific information about the hearing status in mid and high frequency regions. But in most screening protocols TEOAEs are preferred as it requires less time compared to DPOAE. This is because, in DPOAE each stimulus is presented one after the other and responses are analyzed. Grason and Stadler Incorporation 60 (GSI-60) offer simultaneous presentation of four sets of primary tones at a time and checks for the DPOAE. In this mode of presentation, all the pairs are presented at a time and following that response is extracted separately whereas, in sequential mode primaries are presented in orderly fashion one after the other. In this article simultaneous and sequential protocols were used to compare the Distortion product otoacoustic emission amplitude, noise floor and administration time in individuals with normal hearing and mild sensori-neural (SN) hearing loss. In simultaneous protocols four sets of primary tones (i.e. 8 tones) were presented together whereas, in sequential presentation mode one set of primary tones was presented each time. Simultaneous protocol was completed in less than half the time required for the completion of sequential protocol. Two techniques yielded similar results at frequencies above 1000 Hz only in normal hearing group. In SN hearing loss group simultaneous presentation yielded signifi cantly higher noise floors and distortion product amplitudes. This result challenges the use of simultaneous presentation technique in neonatal hearing screening programmes and on other pathologies. This discrepancy between two protocols may be due to some changes in biomechanical process in the cochlear and/or due to higher distortion/noise produced by the system during the simultaneous presentation mode.

  7. 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.

  8. Untangling the primary drivers of pinyon monoterpene production and emissions under predicted drought

    Science.gov (United States)

    Trowbridge, A. M.; Adams, H. D.; Breshears, D. D.; Monson, R. K.

    2012-04-01

    Climate and insect herbivory have important consequences for plant function, atmospheric composition, and the functioning of ecosystems and ecological communities. Within the last decade, pinyon-juniper woodlands throughout the southwestern U.S. have suffered large-scale mortality, especially of pinyon pine, due to drought and associated insect outbreaks. While much research has focused on the primary metabolic mechanisms underlying pinyon's sensitivity to drought, there remains a gap in our knowledge concerning how the resulting shift in carbon allocation toward plant secondary compounds, particularly monoterpenes, affects atmospheric process and ecological interactions. Monoterpenes are the principal constituents of pinyon resin. Because of their large global emission rates and effect on atmospheric chemistry, particularly ozone creation, identifying controls over emissions and sensitivities to environmental change is critical for global emission models. Furthermore, monoterpenes are known to impact insect behavior and act as defense compounds against herbivores, contributing to insect population fluctuations either directly through toxicity, or indirectly by influencing parasitism susceptibility. Pinyon mortality events are thought to be exacerbated by their susceptibility to herbivores resulting from weakened secondary chemical defenses, but the impact of current and predicted drought on the chemical defense status of pinyons and subsequent atmospheric and ecological consequences remain unknown. A field study was developed to examine the impact of seasonality and climate, particularly drought, on pinyon pine physiology and chemistry in the context of tiger moth (Lophocampa ingens) herbivory in pinyon-juniper woodlands. We demonstrate the importance of geography and seasonality, particularly mid-summer drought and late summer monsoons, in driving physiology and monoterpene concentrations and emissions. Emission rates significantly decreased throughout the summer

  9. Life cycle primary energy use and carbon emission of an eight-storey wood-framed apartment building

    Energy Technology Data Exchange (ETDEWEB)

    Gustavsson, Leif; Joelsson, Anna; Sathre, Roger [Ecotechnology, Department of Engineering and Sustainable Development, Mid Sweden University, 83125 Oestersund (Sweden)

    2010-02-15

    In this study the life cycle primary energy use and carbon dioxide (CO{sub 2}) emission of an eight-storey wood-framed apartment building are analyzed. All life cycle phases are included, including acquisition and processing of materials, on-site construction, building operation, demolition and materials disposal. The calculated primary energy use includes the entire energy system chains, and carbon flows are tracked including fossil fuel emissions, process emissions, carbon stocks in building materials, and avoided fossil emissions due to biofuel substitution. The results show that building operation uses the largest share of life cycle energy use, becoming increasingly dominant as the life span of the building increases. The type of heating system strongly influences the primary energy use and CO{sub 2} emission; a biomass-based system with cogeneration of district heat and electricity achieves low primary energy use and very low CO{sub 2} emissions. Using biomass residues from the wood products chain to substitute for fossil fuels significantly reduces net CO{sub 2} emission. Excluding household tap water and electricity, a negative life cycle net CO{sub 2} emission can be achieved due to the wood-based construction materials and biomass-based energy supply system. This study shows the importance of using a life cycle perspective when evaluating primary energy and climatic impacts of buildings. (author)

  10. 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-.

  11. 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

  12. Inhalation of primary motor vehicle emissions: Effects of urbanpopulation and land area

    Energy Technology Data Exchange (ETDEWEB)

    Marshall, Julian D.; McKone, Thomas E.; Nazaroff, William W.

    2004-06-14

    Urban population density can influence transportation demand, as expressed through average daily vehicle-kilometers traveled per capita (VKT). In turn, changes in transportation demand influence total passenger vehicle emissions. Population density can also influence the fraction of total emissions that are inhaled by the exposed urban population. Equations are presented that describe these relationships for an idealized representation of an urban area. Using analytic solutions to these equations, we investigate the effect of three changes in urban population and urban land area (infill, sprawl, and constant-density growth) on per capita inhalation intake of primary pollutants from passenger vehicles. The magnitude of these effects depends on density-emissions elasticity ({var_epsilon}{sub e}), a normalized derivative relating change in population density to change in vehicle emissions. For example, if urban population increases, per capita intake is less with infill development than with constant-density growth if {var_epsilon}{sub e} is less than -0.5, while for {var_epsilon}{sub e} greater than -0.5 the reverse is true.

  13. Development and Characterization of a Thermodenuder for Aerosol Volatility Measurements

    Energy Technology Data Exchange (ETDEWEB)

    Dr. Timothy Onasch

    2009-09-09

    This SBIR Phase I project addressed the critical need for improved characterization of carbonaceous aerosol species in the atmosphere. The proposed work focused on the development of a thermodenuder (TD) system capable of systematically measuring volatility profiles of primary and secondary organic aerosol species and providing insight into the effects of absorbing and nonabsorbing organic coatings on particle absorption properties. This work provided the fundamental framework for the generation of essential information needed for improved predictions of ambient aerosol loadings and radiative properties by atmospheric chemistry models. As part of this work, Aerodyne Research, Inc. (ARI) continued to develop and test, with the final objective of commercialization, an improved thermodenuder system that can be used in series with any aerosol instrument or suite of instruments (e.g., aerosol mass spectrometers-AMS, scanning mobility particle sizers-SMPS, photoacoustic absorption spectrometers-PAS, etc.) to obtain aerosol chemical, physical, and optical properties as a function of particle volatility. In particular, we provided the proof of concept for the direct coupling of our improved TD design with a full microphysical model to obtain volatility profiles for different organic aerosol components and to allow for meaningful comparisons between different TD-derived aerosol measurements. In a TD, particles are passed through a heated zone and a denuding (activated charcoal) zone to remove semi-volatile material. Changes in particle size, number concentration, optical absorption, and chemical composition are subsequently detected with aerosol instrumentation. The aerosol volatility profiles provided by the TD will strengthen organic aerosol emission inventories, provide further insight into secondary aerosol formation mechanisms, and provide an important measure of particle absorption (including brown carbon contributions and identification, and absorption enhancements

  14. Organic aerosols and inorganic species from post-harvest agricultural-waste burning emissions over northern India: impact on mass absorption efficiency of elemental carbon.

    Science.gov (United States)

    Rajput, Prashant; Sarin, M M; Sharma, Deepti; Singh, Darshan

    2014-01-01

    Atmospheric PM2.5 (particulate matter with aerodynamic diameter of ≤ 2.5 μm), collected from a source region [Patiala: 30.2 °N; 76.3 °E; 250 m above mean sea level] of emissions from post-harvest agricultural-waste (paddy-residue) burning in the Indo-Gangetic Plain (IGP), North India, has been studied for its chemical composition and impact on regional atmospheric radiative forcing. On average, organic aerosol mass accounts for 63% of PM2.5, whereas the contribution of elemental carbon (EC) is ∼3.5%. Sulphate, nitrate and ammonium contribute up to ∼85% of the total water-soluble inorganic species (WSIS), which constitutes ∼23% of PM2.5. The potassium-to-organic carbon ratio from paddy-residue burning emissions (KBB(+)/OC: 0.05 ± 0.01) is quite similar to that reported from Amazonian and Savanna forest-fires; whereas non-sea-salt-sulphate-to-OC ratio (nss-SO4(2-)/OC: 0.21) and nss-SO4(2-)/EC ratio of 2.6 are significantly higher (by factor of 5 to 8). The mass absorption efficiency of EC (3.8 ± 1.3 m(2) g(-1)) shows significant decrease with a parallel increase in the concentrations of organic aerosols and scattering species (sulphate and nitrate). A cross plot of OC/EC and nss-SO4(2-)/EC ratios show distinct differences for post-harvest burning emissions from paddy-residue as compared to those from fossil-fuel combustion sources in south-east Asia.

  15. 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.

  16. 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.

  17. Estimating Landscape Fire Particulate Matter (PM) Emissions over Southern Africa using MSG-SEVIRI Fire Radiative Power (FRP) and MODIS Aerosol Optical Thickness Observations

    Science.gov (United States)

    Mota, Bernardo; Wooster, Martin J.

    2016-04-01

    The approach to estimating landscape fire fuel consumption based on the remotely sensed fire radiative power (FRP) thermal energy release rate, as opposed to burned area, is now relatively widely used in studies of fire emissions, including operationally within the Copernicus Atmosphere Monitoring Service (CAMS). Nevertheless, there are still limitations to the approach, including uncertainties associated with using only the few daily overpasses typically provided by polar orbiting satellite systems, the conversion between FRP and smoke emissions, and the increased likelihood that the more frequent data from geostationary systems fails to detect the (probably highly numerous) smaller (i.e. low FRP) component of a regions fire regime. In this study, we address these limitations to directly estimate fire emissions of Particular Matter (PM; or smoke aerosols) by presenting an approach combining the "bottom-up" FRP observations available every 15 minutes across Africa from the Meteosat Spinning Enhanced Visible and Infrared Imager (SEVIRI) Fire Radiative Product (FRP) processed at the EUMETSAT LSA SAF, and the "top-down" aerosol optical thickness (AOT) measures of the fire plumes themselves as measured by the Moderate-resolution Imaging Spectro-radiometer (MODIS) sensors aboard the Terra (MOD04_L2) and Aqua (MYD04_L2) satellites. We determine PM emission coefficients that relate directly to FRP measures by combining these two datasets, and the use of the almost continuous geostationary FRP observations allows us to do this without recourse to (uncertain) data on wind speed at the (unknown) height of the matching plume. We also develop compensation factors to address the detection limitations of small/low intensity (low FRP) fires, and remove the need to estimate fuel consumption by going directly from FRP to PM emissions. We derive the smoke PM emissions coefficients per land cover class by comparing the total fire radiative energy (FRE) released from individual fires

  18. 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.

  19. Long-term implications of alternative light-duty vehicle technologies for global greenhouse gas emissions and primary energy demands

    International Nuclear Information System (INIS)

    Kyle, Page; Kim, Son H.

    2011-01-01

    This study assesses global light-duty vehicle (LDV) transport in the upcoming century, and the implications of vehicle technology advancement and fuel-switching on greenhouse gas emissions and primary energy demands. Five different vehicle technology scenarios are analyzed with and without a CO 2 emissions mitigation policy using the GCAM integrated assessment model: a reference internal combustion engine vehicle scenario, an advanced internal combustion engine vehicle scenario, and three alternative fuel vehicle scenarios in which all LDVs are switched to natural gas, electricity, or hydrogen by 2050. The emissions mitigation policy is a global CO 2 emissions price pathway that achieves 450 ppmv CO 2 at the end of the century with reference vehicle technologies. The scenarios demonstrate considerable emissions mitigation potential from LDV technology; with and without emissions pricing, global CO 2 concentrations in 2095 are reduced about 10 ppmv by advanced ICEV technologies and natural gas vehicles, and 25 ppmv by electric or hydrogen vehicles. All technological advances in vehicles are important for reducing the oil demands of LDV transport and their corresponding CO 2 emissions. Among advanced and alternative vehicle technologies, electricity- and hydrogen-powered vehicles are especially valuable for reducing whole-system emissions and total primary energy. - Highlights: → Alternative-fuel LDVs reduce whole-system CO 2 emissions, even without carbon pricing. → Alternative-fuel LDVs enhance the CO 2 mitigation capacity of the transportation sector. → Electric and hydrogen vehicles reduce whole-system primary energy supporting LDV transport.

  20. Aerosol optical properties observation and its relationship to meteorological conditions and emission during the Chinese National Day and Spring Festival holiday in Beijing

    Science.gov (United States)

    Zheng, Yu; Che, Huizheng; Zhao, Tianliang; Zhao, Hujia; Gui, Ke; Sun, Tianze; An, Linchang; Yu, Jie; Liu, Chong; Jiang, Yongcheng; Zhang, Lei; Wang, Hong; Wang, Yaqiang; Zhang, Xiaoye

    2017-11-01

    The reduction of traffic flow in downtown areas during the Chinese National Day holiday and the fireworks during the Spring Festival provide a unique opportunity for investigating the impact of urban anthropogenic activities on aerosol optical properties during these important Chinese festivals in Beijing. The National Day in 2014 and 2015 and Spring Festival in 2015 and 2016 were selected as study periods. The aerosol optical depth (AOD) at 440 nm increased over the all holiday periods and the average AODs during the 2015 National Day, 2015 Spring Festival and 2016 Spring Festival were about 81%, 21% and 36% higher than the background levels, respectively. The average AOD in 2014 National Day holiday was lower than background level partly influenced by precipitation event. The absorption AOD (AAOD) at 440 nm showed consistent variations with the AOD and the average AAODs during the 2015 National Day, 2015 Spring Festival and 2016 Spring Festival holidays were about 75%, 19% and 23% higher than the background level, respectively. The mean values of single scattering albedo were greater than the background level during the Spring Festival holidays, whereas the values during the National Day holiday in 2015 were lower partly due to the reduction of vehicular emissions in downtown areas. Fine- and coarse-mode particle volumes during pollution periods in holidays were 0.04-0.25 μm3 and 0.03-0.15 μm3 larger than background level, respectively. The results of potential source contribution function and concentration-weighted trajectory analyses identified the areas south of Beijing as the main source regions of PM2.5 and were responsible for the extremely high PM2.5 concentrations in Beijing during the holiday periods. The findings of this study may aid understanding the effects of human activities on aerosol optical properties over Beijing area and contribute to improving regional air quality.

  1. 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...

  2. 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.

  3. Trends in European background air reflect reductions in primary emissions of PCBs and PBDEs.

    Science.gov (United States)

    Schuster, Jasmin K; Gioia, Rosalinda; Breivik, Knut; Steinnes, Eiliv; Scheringer, Martin; Jones, Kevin C

    2010-09-01

    Data are presented for polychlorinated biphenyls (PCBs) and polybrominated diphenyls ethers (PBDEs) in passive air samplers (PAS) collected along a rural/remote latitudinal transect from southern UK to northern Norway during 2004-2008. This study is part of an ongoing campaign, using semipermeable membrane devices (SPMDs) as PAS over two year intervals since 1994. Absolute sequestered amounts of selected PCB congeners have decreased in a first order fashion between 1994-2008, with the average time of 8.4+/-3.2 years for atmospheric concentrations to decline by 50%. PCBs have continued to fractionate with latitude during this period. PBDE concentrations declined by 50% between 2000 and 2008 every 2.2+/-0.4 years. Results are discussed in terms of sources, long-range atmospheric transport, global fractionation, and clearance processes. It is concluded that the spatial and temporal trends in background European air mainly reflect the strength of primary diffusive emissions of these compounds and subsequently their ongoing declines. The direct evidence for this is similar rates of decline at all the sites; similar rates of decline for all congeners; no systematic change in the fractionation pattern since 1994. The latest results indicate a reduction in the rate of decline for PCBs (and hence in primary emissions).

  4. Cost-effective reduction of fine primary particulate matter emissions in Finland

    International Nuclear Information System (INIS)

    Karvosenoja, Niko; Klimont, Zbigniew; Tohka, Antti; Johansson, Matti

    2007-01-01

    Policies to reduce adverse health impacts of fine particulate matter (PM 2.5 ) require information on costs of abatement and associated costs. This paper explores the potential for cost-efficient control of anthropogenic primary PM 2.5 emissions in Finland. Based on a Kyoto-compliant energy projection, two emission control scenarios for 2020 were developed. 'Baseline' assumes implementation of PM controls in compliance with existing legislation. 'Reduction' assumes ambitious further reductions. Emissions for 2020 were estimated at 26 and 18.6 Gg a -1 for 'Baseline' and 'Reduction', respectively. The largest abatement potential, 3.0 Gg a -1 , was calculated for power plants and industrial combustion. The largest potential with marginal costs below 5000 Euro MG(PM 2.5 ) -1 was for domestic wood combustion, 1.7 Gg a -1 . For traffic the potential was estimated at 1.0 Gg a -1 , but was associated with high costs. The results from this paper are used in the policy-driven national integrated assessment modeling that explores cost-efficient reductions of the health impacts of PM

  5. 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

  6. Consideration of black carbon and primary organic carbon emissions in life-cycle analysis of Greenhouse gas emissions of vehicle systems and fuels.

    Science.gov (United States)

    Cai, Hao; Wang, Michael Q

    2014-10-21

    The climate impact assessment of vehicle/fuel systems may be incomplete without considering short-lived climate forcers of black carbon (BC) and primary organic carbon (POC). We quantified life-cycle BC and POC emissions of a large variety of vehicle/fuel systems with an expanded Greenhouse gases, Regulated Emissions, and Energy use in Transportation model developed at Argonne National Laboratory. Life-cycle BC and POC emissions have small impacts on life-cycle greenhouse gas (GHG) emissions of gasoline, diesel, and other fuel vehicles, but would add 34, 16, and 16 g CO2 equivalent (CO2e)/mile, or 125, 56, and 56 g CO2e/mile with the 100 or 20 year Global Warming Potentials of BC and POC emissions, respectively, for vehicles fueled with corn stover-, willow tree-, and Brazilian sugarcane-derived ethanol, mostly due to BC- and POC-intensive biomass-fired boilers in cellulosic and sugarcane ethanol plants for steam and electricity production, biomass open burning in sugarcane fields, and diesel-powered agricultural equipment for biomass feedstock production/harvest. As a result, life-cycle GHG emission reduction potentials of these ethanol types, though still significant, are reduced from those without considering BC and POC emissions. These findings, together with a newly expanded GREET version, help quantify the previously unknown impacts of BC and POC emissions on life-cycle GHG emissions of U.S. vehicle/fuel systems.

  7. Real-time analysis of organic compounds in ship engine aerosol emissions using resonance-enhanced multiphoton ionisation and proton transfer mass spectrometry.

    Science.gov (United States)

    Radischat, Christian; Sippula, Olli; Stengel, Benjamin; Klingbeil, Sophie; Sklorz, Martin; Rabe, Rom; Streibel, Thorsten; Harndorf, Horst; Zimmermann, Ralf

    2015-08-01

    Organic combustion aerosols from a marine medium-speed diesel engine, capable to run on distillate (diesel fuel) and residual fuels (heavy fuel oil), were investigated under various operating conditions and engine parameters. The online chemical characterisation of the organic components was conducted using a resonance-enhanced multiphoton ionisation time-of-flight mass spectrometer (REMPI TOF MS) and a proton transfer reaction-quadrupole mass spectrometer (PTR-QMS). Oxygenated species, alkenes and aromatic hydrocarbons were characterised. Especially the aromatic hydrocarbons and their alkylated derivatives were very prominent in the exhaust of both fuels. Emission factors of known health-hazardous compounds (e.g. mono- and poly-aromatic hydrocarbons) were calculated and found in higher amounts for heavy fuel oil (HFO) at typical engine loadings. Lower engine loads lead in general to increasing emissions for both fuels for almost every compound, e.g. naphthalene emissions varied for diesel fuel exhaust between 0.7 mg/kWh (75 % engine load, late start of injection (SOI)) and 11.8 mg/kWh (10 % engine load, late SOI) and for HFO exhaust between 3.3 and 60.5 mg/kWh, respectively. Both used mass spectrometric techniques showed that they are particularly suitable methods for online monitoring of combustion compounds and very helpful for the characterisation of health-relevant substances. Graphical abstract Three-dimensional REMPI data of organic species in diesel fuel and heavy fuel oil exhaust.

  8. Aerosol in the containment

    International Nuclear Information System (INIS)

    Lanza, S.; Mariotti, P.

    1986-01-01

    The US program LACE (LWR Aerosol Containment Experiments), in which Italy participates together with several European countries, Canada and Japan, aims at evaluating by means of a large scale experimental activity at HEDL the retention in the pipings and primary container of the radioactive aerosol released following severe accidents in light water reactors. At the same time these experiences will make available data through which the codes used to analyse the behaviour of the aerosol in the containment and to verify whether by means of the codes of thermohydraulic computation it is possible to evaluate with sufficient accuracy variable influencing the aerosol behaviour, can be validated. This report shows and compares the results obtained by the participants in the LACE program with the aerosol containment codes NAVA 5 and CONTAIN for the pre-test computations of the test LA 1, in which an accident called containment by pass is simulated

  9. Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

    Directory of Open Access Journals (Sweden)

    X. Zhang

    2018-04-01

    Full Text Available An intensive field measurement was conducted at a remote, background, 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 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1 and obtain the dynamic processes (emissions, transport, and chemical evolution of biomass burning (BB, frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ PM1 mass concentration was 4.44 (±4.54 µg m−3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA was the dominant PM1 species (accounting for 54.3 % of total PM1 on average followed by black carbon (BC (25.0 %, sulfate (9.3 %, ammonium (5.8 %, nitrate (5.1 %, and chloride (0.4 %. 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 transport. Positive matrix factorization (PMF analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %, a nitrogen-containing OA (NOA, 13.9 % and a more-oxidized oxygenated OA (MO-OOA, 42.4 %. Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

  10. Intelligent emissions controller for substance injection in the post-primary combustion zone of fossil-fired boilers

    Science.gov (United States)

    Reifman, Jaques; Feldman, Earl E.; Wei, Thomas Y. C.; Glickert, Roger W.

    2003-01-01

    The control of emissions from fossil-fired boilers wherein an injection of substances above the primary combustion zone employs multi-layer feedforward artificial neural networks for modeling static nonlinear relationships between the distribution of injected substances into the upper region of the furnace and the emissions exiting the furnace. Multivariable nonlinear constrained optimization algorithms use the mathematical expressions from the artificial neural networks to provide the optimal substance distribution that minimizes emission levels for a given total substance injection rate. Based upon the optimal operating conditions from the optimization algorithms, the incremental substance cost per unit of emissions reduction, and the open-market price per unit of emissions reduction, the intelligent emissions controller allows for the determination of whether it is more cost-effective to achieve additional increments in emission reduction through the injection of additional substance or through the purchase of emission credits on the open market. This is of particular interest to fossil-fired electrical power plant operators. The intelligent emission controller is particularly adapted for determining the economical control of such pollutants as oxides of nitrogen (NO.sub.x) and carbon monoxide (CO) emitted by fossil-fired boilers by the selective introduction of multiple inputs of substances (such as natural gas, ammonia, oil, water-oil emulsion, coal-water slurry and/or urea, and combinations of these substances) above the primary combustion zone of fossil-fired boilers.

  11. Source apportionment of secondary organic aerosol in China using a regional source-oriented chemical transport model and two emission inventories.

    Science.gov (United States)

    Wang, Peng; Ying, Qi; Zhang, Hongliang; Hu, Jianlin; Lin, Yingchao; Mao, Hongjun

    2018-06-01

    A Community Multiscale Air Quality (CMAQ) model with source-oriented lumped SAPRC-11 (S11L) photochemical mechanism and secondary organic aerosol (SOA) module was applied to determine the contributions of anthropogenic and biogenic sources to SOA concentrations in China. A one-year simulation of 2013 using the Multi-resolution Emission Inventory for China (MEIC) shows that summer SOA are generally higher (10-15 μg m -3 ) due to large contributions of biogenic (country average 60%) and industrial sources (17%). In winter, SOA formation was mostly due to anthropogenic emissions from industries (40%) and residential sources (38%). Emissions from other countries in southeast China account for approximately 14% of the SOA in both summer and winter, and 46% in spring due to elevated open biomass burning in southeast Asia. The Regional Emission inventory in ASia v2.1 (REAS2) was applied in this study for January and August 2013. Two sets of simulations with the REAS2 inventory were conducted using two different methods to speciate total non-methane carbon into model species. One approach uses total non-methane hydrocarbon (NMHC) emissions and representative speciation profiles from the SPECIATE database. The other approach retains the REAS2 speciated species that can be directly mapped to S11L model species and uses source specific splitting factors to map other REAS2 lumped NMHC species. Biogenic emissions are still the most significant contributor in summer based on these two sets of simulations. However, contributions from the transportation sector to SOA in January are predicted to be much more important based on the two REAS2 emission inventories (∼30-40% vs. ∼5% by MEIC), and contributions from residential sources according to REAS2 was much lower (∼21-24% vs. ∼42%). These discrepancies in source contributions to SOA need to be further investigated as the country seeks for optimal emission control strategies to fight severe air pollution. Copyright

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

    Science.gov (United States)

    Rajan K. Chakrabarty; Madhu Gyawali; Reddy L. N. Yatavelli; Apoorva Pandey; Adam C. Watts; Joseph Knue; Lung-Wen A. Chen; Robert R. Pattison; Anna Tsibart; Vera Samburova; Hans Moosmuller

    2016-01-01

    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...

  13. Temporal trends and spatial variation characteristics of primary air pollutants emissions from coal-fired industrial boilers in Beijing, China

    International Nuclear Information System (INIS)

    Xue, Yifeng; Tian, Hezhong; Yan, Jing; Zhou, Zhen; Wang, Junling; Nie, Lei; Pan, Tao; Zhou, Junrui; Hua, Shenbing; Wang, Yong; Wu, Xiaoqing

    2016-01-01

    Coal-fired combustion is recognized as a significant anthropogenic source of atmospheric compounds in Beijing, causing heavy air pollution events and associated deterioration in visibility. Obtaining an accurate understanding of the temporal trends and spatial variation characteristics of emissions from coal-fired industrial combustion is essential for predicting air quality changes and evaluating the effectiveness of current control measures. In this study, an integrated emission inventory of primary air pollutants emitted from coal-fired industrial boilers in Beijing is developed for the period of 2007–2013 using a technology-based approach. Future emission trends are projected through 2030 based on current energy-related and emission control policies. Our analysis shows that there is a general downward trend in primary air pollutants emissions because of the implementation of stricter local emission standards and the promotion by the Beijing municipal government of converting from coal-fired industrial boilers to gas-fired boilers. However, the ratio of coal consumed by industrial boilers to total coal consumption has been increasing, raising concerns about the further improvement of air quality in Beijing. Our estimates indicate that the total emissions of PM 10 , PM 2.5 , SO 2 , NO x , CO and VOCs from coal-fired industrial boilers in Beijing in 2013 are approximately 19,242 t, 13,345 t, 26,615 t, 22,965 t, 63,779 t and 1406 t, respectively. Under the current environmental policies and relevant energy savings and emission control plans, it may be possible to reduce NO x and other air pollutant emissions by 94% and 90% by 2030, respectively, if advanced flue gas purification technologies are implemented and coal is replaced with natural gas in the majority of existing boilers. - Highlights: • A unit-based emission inventory of coal-fired industrial boilers is developed. • Temporal trend of historical period 2007–2013 and the future till 2030 is

  14. Seasonality of isoprenoid emissions from a primary rainforest in central Amazonia

    Directory of Open Access Journals (Sweden)

    E. G. Alves

    2016-03-01

    Full Text Available Tropical rainforests are an important source of isoprenoid and other volatile organic compound (VOC emissions to the atmosphere. The seasonal variation of these compounds is however still poorly understood. In this study, vertical profiles of mixing ratios of isoprene, total monoterpenes and total sesquiterpenes, were measured within and above the canopy, in a primary rainforest in central Amazonia, using a proton transfer reaction – mass spectrometer (PTR-MS. Fluxes of these compounds from the canopy into the atmosphere were estimated from PTR-MS measurements by using an inverse Lagrangian transport model. Measurements were carried out continuously from September 2010 to January 2011, encompassing the dry and wet seasons. Mixing ratios were higher during the dry (isoprene – 2.68 ± 0.9 ppbv, total monoterpenes – 0.67 ± 0.3 ppbv; total sesquiterpenes – 0.09 ± 0.07 ppbv than the wet season (isoprene – 1.66 ± 0.9 ppbv, total monoterpenes – 0.47 ± 0.2 ppbv; total sesquiterpenes – 0.03 ± 0.02 ppbv for all compounds. Ambient air temperature and photosynthetically active radiation (PAR behaved similarly. Daytime isoprene and total monoterpene mixing ratios were highest within the canopy, rather than near the ground or above the canopy. By comparison, daytime total sesquiterpene mixing ratios were highest near the ground. Daytime fluxes varied significantly between seasons for all compounds. The maximums for isoprene (2.53 ± 0.5 µmol m−2 h−1 and total monoterpenes (1.77 ± 0.05 µmol m−2 h−1 were observed in the late dry season, whereas the maximum for total sesquiterpenes was found during the dry-to-wet transition season (0.77 ± 0.1 µmol m−2 h−1. These flux estimates suggest that the canopy is the main source of isoprenoids emitted into the atmosphere for all seasons. However, uncertainties in turbulence parameterization near the ground could affect estimates of fluxes that come from the ground. Leaf

  15. Seasonality of isoprenoid emissions from a primary rainforest in central Amazonia

    Science.gov (United States)

    Alves, Eliane G.; Jardine, Kolby; Tota, Julio; Jardine, Angela; Yãnez-Serrano, Ana Maria; Karl, Thomas; Tavares, Julia; Nelson, Bruce; Gu, Dasa; Stavrakou, Trissevgeni; Martin, Scot; Artaxo, Paulo; Manzi, Antonio; Guenther, Alex

    2016-03-01

    Tropical rainforests are an important source of isoprenoid and other volatile organic compound (VOC) emissions to the atmosphere. The seasonal variation of these compounds is however still poorly understood. In this study, vertical profiles of mixing ratios of isoprene, total monoterpenes and total sesquiterpenes, were measured within and above the canopy, in a primary rainforest in central Amazonia, using a proton transfer reaction - mass spectrometer (PTR-MS). Fluxes of these compounds from the canopy into the atmosphere were estimated from PTR-MS measurements by using an inverse Lagrangian transport model. Measurements were carried out continuously from September 2010 to January 2011, encompassing the dry and wet seasons. Mixing ratios were higher during the dry (isoprene - 2.68 ± 0.9 ppbv, total monoterpenes - 0.67 ± 0.3 ppbv; total sesquiterpenes - 0.09 ± 0.07 ppbv) than the wet season (isoprene - 1.66 ± 0.9 ppbv, total monoterpenes - 0.47 ± 0.2 ppbv; total sesquiterpenes - 0.03 ± 0.02 ppbv) for all compounds. Ambient air temperature and photosynthetically active radiation (PAR) behaved similarly. Daytime isoprene and total monoterpene mixing ratios were highest within the canopy, rather than near the ground or above the canopy. By comparison, daytime total sesquiterpene mixing ratios were highest near the ground. Daytime fluxes varied significantly between seasons for all compounds. The maximums for isoprene (2.53 ± 0.5 µmol m-2 h-1) and total monoterpenes (1.77 ± 0.05 µmol m-2 h-1) were observed in the late dry season, whereas the maximum for total sesquiterpenes was found during the dry-to-wet transition season (0.77 ± 0.1 µmol m-2 h-1). These flux estimates suggest that the canopy is the main source of isoprenoids emitted into the atmosphere for all seasons. However, uncertainties in turbulence parameterization near the ground could affect estimates of fluxes that come from the ground. Leaf phenology seemed to be an important driver of seasonal

  16. Global Scale Attribution of Anthropogenic and Natural Dust Sources and their Emission Rates Based on MODIS Deep Blue Aerosol Products

    Science.gov (United States)

    Ginoux, Paul; Prospero, Joseph M.; Gill, Thomas E.; Hsu, N. Christina; Zhao, Ming

    2012-01-01

    Our understanding of the global dust cycle is limited by a dearth of information about dust sources, especially small-scale features which could account for a large fraction of global emissions. Here we present a global-scale high-resolution (0.1 deg) mapping of sources based on Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue estimates of dust optical depth in conjunction with other data sets including land use. We ascribe dust sources to natural and anthropogenic (primarily agricultural) origins, calculate their respective contributions to emissions, and extensively compare these products against literature. Natural dust sources globally account for 75% of emissions; anthropogenic sources account for 25%. North Africa accounts for 55% of global dust emissions with only 8% being anthropogenic, mostly from the Sahel. Elsewhere, anthropogenic dust emissions can be much higher (75% in Australia). Hydrologic dust sources (e.g., ephemeral water bodies) account for 31% worldwide; 15% of them are natural while 85% are anthropogenic. Globally, 20% of emissions are from vegetated surfaces, primarily desert shrublands and agricultural lands. Since anthropogenic dust sources are associated with land use and ephemeral water bodies, both in turn linked to the hydrological cycle, their emissions are affected by climate variability. Such changes in dust emissions can impact climate, air quality, and human health. Improved dust emission estimates will require a better mapping of threshold wind velocities, vegetation dynamics, and surface conditions (soil moisture and land use) especially in the sensitive regions identified here, as well as improved ability to address small-scale convective processes producing dust via cold pool (haboob) events frequent in monsoon regimes.

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

    Directory of Open Access Journals (Sweden)

    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

  18. 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

  19. 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

  20. 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

  1. Aerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment: Case study of Metro Manila, Philippines

    Science.gov (United States)

    Kecorius, Simonas; Madueño, Leizel; Vallar, Edgar; Alas, Honey; Betito, Grace; Birmili, Wolfram; Cambaliza, Maria Obiminda; Catipay, Grethyl; Gonzaga-Cayetano, Mylene; Galvez, Maria Cecilia; Lorenzo, Genie; Müller, Thomas; Simpas, James B.; Tamayo, Everlyn Gayle; Wiedensohler, Alfred

    2017-12-01

    Ultrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM10 and PM2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm3. That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM2.5. The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authors' knowledge, no other

  2. 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.

  3. Identification of secondary aerosol precursors emitted by an aircraft turbofan

    Directory of Open Access Journals (Sweden)

    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.

  4. 18F-fluorodeoxyglucose positron emission tomography in colorectal cancer: value in primary staging and follow-up

    International Nuclear Information System (INIS)

    Joerg, L.; Heinisch, M.; Rechberger, E.; Kurz, F.; Klug, R.; Aufschnaiter, M; Hammer, J.; Langsteger, W.

    2002-01-01

    Positron emission tomography using 18 F-fluorodeoxyglucose (FDG-PET) is a encouraging imaging techniques allowing a highly sensitive whole-body search for malignant foci detected by their increased glucose metabolism compared with benign tissues. Several studies are now available that indicate its added value for diagnosis and staging of colorectal cancer. In all, patient management seems to be changed in 20-30 % of patients who undergo fluorodeoxyglucose positron emission tomography in addition to standard staging procedures. Fluorodeoxyglucose positron emission tomography is also useful in monitoring radiation therapy and chemotherapy. Regarding preoperative staging of primary colorectal cancer the literature is very limited. (author)

  5. Influence of the aquatic environment on release behavior of fission products. Experimental study of aerosol emission during a PWR severe accident

    International Nuclear Information System (INIS)

    Monfort, M.

    1989-06-01

    This experimental study concerns the consequences on the environment of a PWR severe accident. A preliminary bibliographical survey has been undertaken in order to determine the elements to study, and the experimental protocols to use. 4 fission products (Cs, Sr, Ru, Ce) and 3 structure materials (Ag, Fe, In) have been chosen. Tests of cations (Cs + ) retention by soils have been done. They showed up the great variability of the results according to experimental procedures (contact time, agitation, solid phase concentration...). The adoption of a standard procedure which would enable the different results comparison is suggested. Then, the dissolution of powders from the 7 elements has been studied in different solutions. Two different phenomena occurs for some elements. We observed a partial dissolution of Ag, In and Ce, according to solution compositions, but fine particles or colloid presence may contribute to the solution total activity. The Cs dissolution is more important but never complete, because of an amalgam formation during calcination with structure materials. Ru doesn't dissolve, and fine particles presence is the reason of solution activity. Soils retention is minimal for the elements that are neutral, like Ru, and maximal for cations, especially Cs + . High contents of organic matter and clay in soils enhance retention. Thanks to the new theoretical source term values, plurielementary aerosols fabrication has debuted. The installation we used (Inducing oven with an aerosol maturation enclosure) allows the obtention of temperatures as high as 2800 - 3000 0 C and the volatilization of 13 elements between the 16 presents. Suggestions are done that may increase the Ru, Ce and Zr emissions [fr

  6. Concentrations of nitrous acid, nitric acid, nitrite and nitrate in the gas and aerosol phase at a site in the emission zone during ESCOMPTE 2001 experiment

    Science.gov (United States)

    Acker, K.; Möller, D.; Auel, R.; Wieprecht, W.; Kalaß, D.

    2005-03-01

    Ground-based measurements were performed at the "Expérience sur Site pour COntraindre les Modèles de Pollution atmosphérique et de Transport d`Emissions" (ESCOMPTE) field site E3 (Realtor) about 30 km north of the urban environment of Marseille and east of the industrial centre Berre pond to investigate the formation of nitrous and nitric acid and to detect the distribution of reactive N-species between the gas and particle phase during photochemical pollution events. A wet denuder sampling for gases followed by a steam jet collection for aerosols was both coupled to anion chromatographic analysis. The analytical system provided data continuously with 30-min time resolution between June 13 and July 13, 2001. Indications for heterogeneous formation of nitrous acid during nighttime and daytime on ground and aerosol surfaces were found, the average HNO 2/NO 2 ratio was 6%. Highest concentrations were observed during two episodes of strong pollution accumulation when sea breeze transported industrial, traffic and urban pollution land-inwards. After nocturnal heterogeneous formation (about 0.1 ppb v h -1 were estimated corresponding to increasing HNO 2/NO 2 ratios) and accumulation processes up to 1.2 ppb v HNO 2 were observed. Their photolysis produces up to 5-9×10 6 OH cm -3 s -1 and will contribute significantly to initiation of the daily photochemistry in the lowest part of the troposphere. For the key tropospheric species, HNO 3 daily peaks up to 4 ppb v were detected.

  7. Aerosol optical properties and trace gas emissions by PAX and OP-FTIR for laboratory-simulated western US wildfires during FIREX

    Directory of Open Access Journals (Sweden)

    V. Selimovic

    2018-03-01

    Full Text Available Western wildfires have a major impact on air quality in the US. In the fall of 2016, 107 test 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 fuel components were burned in combinations that represented realistic fuel complexes for several important western US coniferous and chaparral ecosystems including ponderosa pine, Douglas fir, Engelmann spruce, lodgepole pine, subalpine fir, chamise, and manzanita. In addition, dung, Indonesian peat, and individual coniferous ecosystem fuel components were burned alone to investigate the effects of individual components (e.g., duff and fuel chemistry on emissions. The smoke emissions were characterized by a large suite of state-of-the-art instruments. In this study we report emission factor (EF, grams of compound emitted per kilogram of fuel burned measurements in fresh smoke of a diverse suite of critically important trace gases measured using 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 (PAXs at 870 and 401 nm. The average trace gas emissions were similar across the coniferous ecosystems tested and most of the variability observed in emissions could be attributed to differences in the consumption of components such as duff and litter, rather than the dominant tree species. Chaparral fuels produced lower EFs than mixed coniferous fuels for most trace gases except for NOx and acetylene. A careful comparison with available field measurements of wildfires confirms that several methods can be used to extract data representative of real wildfires from the FIREX laboratory fire data. This is especially

  8. Aerosol optical properties and trace gas emissions by PAX and OP-FTIR for laboratory-simulated western US wildfires during FIREX

    Science.gov (United States)

    Selimovic, Vanessa; Yokelson, Robert J.; Warneke, Carsten; Roberts, James M.; de Gouw, Joost; Reardon, James; Griffith, David W. T.

    2018-03-01

    Western wildfires have a major impact on air quality in the US. In the fall of 2016, 107 test 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 fuel components were burned in combinations that represented realistic fuel complexes for several important western US coniferous and chaparral ecosystems including ponderosa pine, Douglas fir, Engelmann spruce, lodgepole pine, subalpine fir, chamise, and manzanita. In addition, dung, Indonesian peat, and individual coniferous ecosystem fuel components were burned alone to investigate the effects of individual components (e.g., duff) and fuel chemistry on emissions. The smoke emissions were characterized by a large suite of state-of-the-art instruments. In this study we report emission factor (EF, grams of compound emitted per kilogram of fuel burned) measurements in fresh smoke of a diverse suite of critically important trace gases measured using 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 (PAXs) at 870 and 401 nm. The average trace gas emissions were similar across the coniferous ecosystems tested and most of the variability observed in emissions could be attributed to differences in the consumption of components such as duff and litter, rather than the dominant tree species. Chaparral fuels produced lower EFs than mixed coniferous fuels for most trace gases except for NOx and acetylene. A careful comparison with available field measurements of wildfires confirms that several methods can be used to extract data representative of real wildfires from the FIREX laboratory fire data. This is especially valuable for

  9. Organic aerosols

    International Nuclear Information System (INIS)

    Penner, J.E.

    1994-01-01

    Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN

  10. A synergetic approach for estimating the local direct aerosol forcing: Application to an urban zone during the Expérience sur Site pour Contraindre les Modèles de Pollution et de Transport d'Emission (ESCOMPTE) experiment

    Science.gov (United States)

    Roger, J. C.; Mallet, M.; Dubuisson, P.; Cachier, H.; Vermote, E.; Dubovik, O.; Despiau, S.

    2006-07-01

    A method dedicated to the investigation of direct radiative forcing of the main anthropogenic aerosol species (ammonium sulfate, black carbon, particulate organic matter) is presented. We computed the direct radiative aerosol forcing at the top of atmosphere (TOA), at the bottom of atmosphere (BOA), and into the atmospheric layer (ATM). The methodology is based on chemical, photometric, and satellite measurements. We first determined the optical properties of the main aerosol species and then computed their direct radiative impact at local scale. The method was applied to a periurban zone during the Expérience sur Site pour Contraindre les Modèles de Pollution et de Transport d'Emission experiment. Optical computations indicate that the single scattering albedo, for the total aerosol population in the external mixture, is equal to 0.83 ± 0.04 at 550 nm, indicative of a strong absorption of the solar radiation. At the same time the mean asymmetry parameter is equal to 0.59 ± 0.04, and the mean aerosol optical thickness is equal to 0.30 ± 0.02, at 550 nm. The anthropogenic urban aerosol layer reduces significantly the daily surface illumination (-24 W m-2 > ΔFBOA > -47.5 W m-2) by reflection to space (-6 W m-2 > ΔFTOA > -9 W m-2) and by absorption of the solar radiation into the atmosphere (17 W m-2 < ΔFATM < 39 W m-2). The available resulting energy in the atmospheric column heats the lowermost part of the atmosphere from 1.1°K d-1 to 2.8°K d-1. Our study shows that the black carbon particles have a large contribution to the BOA forcing (almost 50% of the total daily forcing), whereas the ammonium sulfate particles contribute only to about 10%. Conversely, the TOA daily forcing is mostly driven by the ammonium sulfate aerosol (around 50%).

  11. 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

  12. Spatially Refined Aerosol Direct Radiative Forcing Efficiencies

    Science.gov (United States)

    Global aerosol direct radiative forcing (DRF) is an important metric for as