Search Results
Diurnal variations of ambient particulate wood burning emissions and their contribution to the concentration of Polycyclic Aromatic Hydrocarbons (PAHs) in Seiffen, Germany
2011, Poulain, L., Iinuma, Y., Müller, K., Birmili, W., Weinhold, K., Brüggemann, E., Gnauk, T., Hausmann, A., Löschau, G., Wiedensohler, A., Herrmann, H.
Residential wood burning is becoming an increasingly important cause of air quality problems since it has become a popular source of alternative energy to fossil fuel. In order to characterize the contribution of residential wood burning to local particle pollution, a field campaign was organized at the village of Seiffen (Saxony, Germany). During this campaign, an Aerosol Mass Spectrometer (AMS) was deployed in parallel to a PM1 high volume filter sampler. The AMS mass spectra were analyzed using Positive Matrix Factorization (PMF) to obtain detailed information about the organic aerosol (OA). Biomass-burning organic aerosol (BBOA), Hydrocarbon-like organic aerosol (HOA), and Oxygenated Organic Aerosol (OOA) were identified and represented 20%, 17% and 62% of total OA, respectively. Additionally, Polycyclic Aromatic Hydrocarbons (PAH) were measured by the AMS with an average concentration of 10 ng m−3 and short term events of extremely high PAH concentration (up to 500 ng m−3) compared to the mean PAH value were observed during the whole measurement period. A comparison with the results from PM1 filter samples showed that the BBOA factor and the AMS PAH are good indicators of the total concentration of the different monosaccharide anhydrides and PAH measured on the filter samples. Based on its low correlation with CO and the low car traffic, the HOA factor was considered to be related to residential heating using liquid fuel. An influence of the time of the week (week vs. weekend) on the diurnal profiles of the different OA components was observed. The weekdays were characterized by two maxima; a first one early in the morning and a stronger one in the evening. During the weekend days, the different OA components principally reached only one maximum in the afternoon. Finally, the PAH emitted directly from residential wood combustion was estimated to represent 1.5% of the total mass of the BBOA factor and around 62% of the total PAH concentration measured at Seiffen. This result highlights the important contribution of residential wood combustion to air quality and PAH emissions at the sampling place, which might have a significant impact on human health. Moreover, it also emphasizes the need for a better time resolution of the chemical characterization of toxic particulate compounds in order to provide more information on variations of the different sources through the days as well as to better estimate the real human exposure.
Long-range and local air pollution: What can we learn from chemical speciation of particulate matter at paired sites?
2020, Pandolfi, Marco, Mooibroek, Dennis, Hopke, Philip, van Pinxteren, Dominik, Querol, Xavier, Herrmann, Hartmut, Alastuey, Andrés, Favez, Olivier, Hüglin, Christoph, Perdrix, Esperanza, Riffault, Véronique, Sauvage, Stéphane, van der Swaluw, Eric, Tarasova, Oksana, Colette, Augustin
Here we report results of a detailed analysis of the urban and non-urban contributions to particulate matter (PM) concentrations and source contributions in five European cities, namely Schiedam (the Netherlands, NL), Lens (France, FR), Leipzig (Germany, DE), Zurich (Switzerland, CH) and Barcelona (Spain, ES). PM chemically speciated data from 12 European paired monitoring sites (one traffic, five urban, five regional and one continental background) were analysed by positive matrix factorisation (PMF) and Lenschow's approach to assign measured PM and source contributions to the different spatial levels. Five common sources were obtained at the 12 sites: sulfate-rich (SSA) and nitrate-rich (NSA) aerosols, road traffic (RT), mineral matter (MM), and aged sea salt (SS). These sources explained from 55 % to 88 % of PM mass at urban low-traffic-impact sites (UB) depending on the country. Three additional common sources were identified at a subset of sites/countries, namely biomass burning (BB) (FR, CH and DE), explaining an additional 9 %-13 % of PM mass, and residual oil combustion (V-Ni) and primary industrial (IND) (NL and ES), together explaining an additional 11 %-15 % of PM mass. In all countries, the majority of PM measured at UB sites was of a regional+continental (R+C) nature (64 %-74 %). The R+C PM increments due to anthropogenic emissions in DE, NL, CH, ES and FR represented around 66 %, 62 %, 52 %, 32 % and 23 %, respectively, of UB PM mass. Overall, the R+C PM increments due to natural and anthropogenic sources showed opposite seasonal profiles with the former increasing in summer and the latter increasing in winter, even if exceptions were observed. In ES, the anthropogenic R+C PM increment was higher in summer due to high contributions from regional SSA and V-Ni sources, both being mostly related to maritime shipping emissions at the Spanish sites. Conversely, in the other countries, higher anthropogenic R+C PM increments in winter were mostly due to high contributions from NSA and BB regional sources during the cold season. On annual average, the sources showing higher R+C increments were SSA (77 %-91 % of SSA source contribution at the urban level), NSA (51 %-94 %), MM (58 %-80 %), BB (42 %-78 %) and IND (91 % in NL). Other sources showing high R+C increments were photochemistry and coal combustion (97 %-99 %; identified only in DE). The highest regional SSA increment was observed in ES, especially in summer, and was related to ship emissions, enhanced photochemistry and peculiar meteorological patterns of the Western Mediterranean. The highest R+C and urban NSA increments were observed in NL and associated with high availability of precursors such as NOx and NH3. Conversely, on average, the sources showing higher local increments were RT (62 %-90 % at all sites) and V-Ni (65 %-80 % in ES and NL). The relationship between SSA and V-Ni indicated that the contribution of ship emissions to the local sulfate concentrations in NL has strongly decreased since 2007 thanks to the shift from high-sulfur-to low-sulfur-content fuel used by ships. An improvement of air quality in the five cities included here could be achieved by further reducing local (urban) emissions of PM, NOx and NH3 (from both traffic and non-traffic sources) but also SO2 and PM (from maritime ships and ports) and giving high relevance to non-urban contributions by further reducing emissions of SO2 (maritime shipping) and NH3 (agriculture) and those from industry, regional BB sources and coal combustion. © 2020 Copernicus GmbH. All rights reserved.
Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: Evaluation of the volatility-basis-set approach within the CHIMERE model
2013, Zhang, Q.J., Beekmann, M., Drewnick, F., Freutel, F., Schneider, J., Crippa, M., Prevot, A.S.H., Baltensperger, U., Poulain, L., Wiedensohler, A., Sciare, J., Gros, V., Borbon, A., Colomb, A., Michoud, V., Doussin, J.-F., Denier Van Der Gon, H.A.C., Haeffelin, M., Dupont, J.-C., Siour, G., Petetin, H., Bessagnet, B., Pandis, S.N., Hodzic, A., Sanchez, O., Honoré, C., Perrussel, O.
Simulations with the chemistry transport model CHIMERE are compared to measurements performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer campaign in the Greater Paris region in July 2009. The volatility-basis-set approach (VBS) is implemented into this model, taking into account the volatility of primary organic aerosol (POA) and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations with a modified treatment of POA volatility and modified secondary organic aerosol (SOA) formation schemes. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated, and four pollution regimes are defined according to the air mass origin. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC) shows the best correlation with measurements. High-concentration events observed mostly after long-range transport are well reproduced by the model. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization), to emission input data, and to simulated OH levels can be responsible for this behavior. Despite these uncertainties, the implementation of the VBS scheme into the CHIMERE model allowed for much more realistic organic aerosol simulations for Paris during summertime. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from northeast (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during periods with advection from Southern France and Spain.
EURODELTA III exercise: An evaluation of air quality models’ capacity to reproduce the carbonaceous aerosol
2019, Mircea, Mihaela, Bessagnet, Bertrand, D'Isidoro, Massimo, Pirovano, Guido, Aksoyoglu, Sebnem, Ciarelli, Giancarlo, Tsyro, Svetlana, Manders, Astrid, Bieser, Johannes, Stern, Rainer, Vivanco, Marta García, Cuvelier, Cornelius, Aas, Wenche, Prévôt, André S.H., Aulinger, Armin, Briganti, Gino, Calori, Giuseppe, Cappelletti, Andrea, Colette, Augustin, Couvidat, Florian, Fagerli, Hilde, Finardi, Sandro, Kranenburg, Richard, Rouïl, Laurence, Silibello, Camillo, Spindler, Gerald, Poulain, Laurent, Herrmann, Hartmut, Jimenez, Jose L., Day, Douglas A., Tiitta, Petri, Carbone, Samara
The carbonaceous aerosol accounts for an important part of total aerosol mass, affects human health and climate through its effects on physical and chemical properties of the aerosol, yet the understanding of its atmospheric sources and sinks is still incomplete. This study shows the state-of-the-art in modelling carbonaceous aerosol over Europe by comparing simulations performed with seven chemical transport models (CTMs) currently in air quality assessments in Europe: CAMx, CHIMERE, CMAQ, EMEP/MSC-W, LOTOS-EUROS, MINNI and RCGC. The simulations were carried out in the framework of the EURODELTA III modelling exercise and were evaluated against field measurements from intensive campaigns of European Monitoring and Evaluation Programme (EMEP) and the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI). Model simulations were performed over the same domain, using as much as possible the same input data and covering four seasons: summer (1–30 June 2006), winter (8 January – 4 February 2007), autumn (17 September- 15 October 2008) and spring (25 February - 26 March 2009). The analyses of models’ performances in prediction of elemental carbon (EC) for the four seasons and organic aerosol components (OA) for the last two seasons show that all models generally underestimate the measured concentrations. The maximum underestimation of EC is about 60% and up to about 80% for total organic matter (TOM). The underestimation of TOM outside of highly polluted area is a consequence of an underestimation of secondary organic aerosol (SOA), in particular of its main contributor: biogenic secondary aerosol (BSOA). This result is independent on the SOA modelling approach used and season. The concentrations and daily cycles of total primary organic matter (TPOM) are generally better reproduced by the models since they used the same anthropogenic emissions. However, the combination of emissions and model formulation leads to overestimate TPOM concentrations in 2009 for most of the models. All models capture relatively well the SOA daily cycles at rural stations mainly due to the spatial resolution used in the simulations. For the investigated carbonaceous aerosol compounds, the differences between the concentrations simulated by different models are lower than the differences between the concentrations simulated with a model for different seasons. © 2019 The Authors
Ozone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke
2022, Ansmann, Albert, Ohneiser, Kevin, Chudnovsky, Alexandra, Knopf, Daniel A., Eloranta, Edwin W., Villanueva, Diego, Seifert, Patric, Radenz, Martin, Barja, Boris, Zamorano, Félix, Jimenez, Cristofer, Engelmann, Ronny, Baars, Holger, Griesche, Hannes, Hofer, Julian, Althausen, Dietrich, Wandinger, Ulla
A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019-May 2020) and over Punta Arenas in southern Chile at 53.2°S (January 2020-November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10-12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10-12 km, smoke particle surface area (SA) concentrations of 5-7 μm2 cm-3 (Antarctica, spring 2021) and 6-10 μm2 cm-3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4-1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2-3.5 mPa (Arctic, 20 %-30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1-2 mPa (10 %-20 % contribution to the total ozone loss over Antarctica) was observed in the 14-23 km PSC height range in September-October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm-3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26-30 Dobson units (9 %-10 %, September 2020, 2021) and 52-57 Dobson units (17 %-20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70-80°S. Copyright:
Influx of African biomass burning aerosol during the Amazonian dry season through layered transatlantic transport of black carbon-rich smoke
2020, Holanda, Bruna A., Pöhlker, Mira L., Walter, David, Saturno, Jorge, Sörgel, Matthias, Ditas, Jeannine, Ditas, Florian, Schulz, Christiane, Aurélio Franco, Marco, Wang, Qiaoqiao, Donth, Tobias, Artaxo, Paulo, Barbosa, Henrique M.J., Borrmann, Stephan, Braga, Ramon, Brito, Joel, Cheng, Yafang, Dollner, Maximilian, Kaiser, JohannesW., Klimach, Thomas, Knote, Christoph, Krüger, Ovid O., Fütterer, Daniel, Lavrič, Jošt V., Ma, Nan, Machado, Luiz A.T., Ming, Jing, Morais, Fernando G., Paulsen, Hauke, Sauer, Daniel, Schlager, Hans, Schneider, Johannes, Su, Hang, Weinzierl, Bernadett, Walser, Adrian, Wendisch, Manfred, Ziereis, Helmut, Zöger, Martin, Pöschl, Ulrich, Andreae, Meinrat O., Pöhlker, Christopher
Black carbon (BC) aerosols influence the Earth's atmosphere and climate, but their microphysical properties, spatiotemporal distribution, and long-range transport are not well constrained. This study presents airborne observations of the transatlantic transport of BC-rich African biomass burning (BB) smoke into the Amazon Basin using a Single Particle Soot Photometer (SP2) as well as several complementary techniques. We base our results on observations of aerosols and trace gases off the Brazilian coast onboard the HALO (High Altitude and LOng range) research aircraft during the ACRIDICON-CHUVA campaign in September 2014. During flight AC19 over land and ocean at the northeastern coastline of the Amazon Basin, we observed a BCrich layer at ∼ 3:5 km altitude with a vertical extension of ∼ 0:3 km. Backward trajectories suggest that fires in African grasslands, savannas, and shrublands were the main source of this pollution layer and that the observed BB smoke had undergone more than 10 d of atmospheric transport and aging over the South Atlantic before reaching the Amazon Basin. The aged smoke is characterized by a dominant accumulation mode, centered at about 130 nm, with a particle concentration of Nacc D 850±330 cm-3. The rBC particles account for ∼ 15 % of the submicrometer aerosol mass and ∼ 40 % of the total aerosol number concentration. This corresponds to a mass concentration range from 0.5 to 2 μ g m-3 (1st to 99th percentiles) and a number concentration range from 90 to 530 cm-3. Along with rBC, high cCO (150 ± 30 ppb) and cO3 (56 ± 9 ppb) mixing ratios support the biomass burning origin and pronounced photochemical aging of this layer. Upon reaching the Amazon Basin, it started to broaden and to subside, due to convective mixing and entrainment of the BB aerosol into the boundary layer. Satellite observations show that the transatlantic transport of pollution layers is a frequently occurring process, seasonally peaking in August/September. By analyzing the aircraft observations together with the long-term data from the Amazon Tall Tower Observatory (ATTO), we found that the transatlantic transport of African BB smoke layers has a strong impact on the northern and central Amazonian aerosol population during the BBinfluenced season (July to December). In fact, the early BB season (July to September) in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season (October to December) appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes in aerosol optical properties such as the single scattering albedo (increasing from 0.85 in August to 0.90 in November) and the BC-to-CO enhancement ratio (decreasing from 11 to 6 ng m-3 ppb-1). Our results suggest that, despite the high fraction of BC particles, the African BB aerosol acts as efficient cloud condensation nuclei (CCN), with potentially important implications for aerosol-cloud interactions and the hydrological cycle in the Amazon. © 2020 Author(s).
Overview of the synoptic and pollution situation over Europe during the EUCAARI-LONGREX field campaign
2011, Hamburger, T., McMeeking, G., Minikin, A., Birmili, W., Dall'Osto, M., O'Dowd, C., Flentje, H., Henzing, B., Junninen, H., Kristensson, A., de Leeuw, G., Stohl, A., Burkhart, J.F., Coe, H., Krejci, R., Petzold, A.
In May 2008 the EUCAARI-LONGREX aircraft field campaign was conducted within the EUCAARI intensive observational period. The campaign aimed at studying the distribution and evolution of air mass properties on a continental scale. Airborne aerosol and trace gas measurements were performed aboard the German DLR Falcon 20 and the British FAAM BAe-146 aircraft. This paper outlines the meteorological situation over Europe during May 2008 and the temporal and spatial evolution of predominantly anthropogenic particulate pollution inside the boundary layer and the free troposphere. Time series data of six selected ground stations are used to discuss continuous measurements besides the single flights. The observations encompass total and accumulation mode particle number concentration (0.1–0.8 μm) and black carbon mass concentration as well as several meteorological parameters. Vertical profiles of total aerosol number concentration up to 10 km are compared to vertical profiles probed during previous studies. During the first half of May 2008 an anticyclonic blocking event dominated the weather over Central Europe. It led to increased pollutant concentrations within the centre of the high pressure inside the boundary layer. Due to long-range transport the accumulated pollution was partly advected towards Western and Northern Europe. The measured aerosol number concentrations over Central Europe showed in the boundary layer high values up to 14 000 cm−3 for particles in diameter larger 10 nm and 2300 cm−3 for accumulation mode particles during the high pressure period, whereas the middle free troposphere showed rather low concentrations of particulates. Thus a strong negative gradient of aerosol concentrations between the well mixed boundary layer and the clean middle troposphere occurred.
Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China
2018, Chen, Jie, Wu, Zhijun, Augustin-Bauditz, Stefanie, Grawe, Sarah, Hartmann, Markus, Pei, Xiangyu, Liu, Zirui, Ji, Dongsheng, Wex, Heike
Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.
Mercury plumes in the global upper troposphere observed during flights with the CARIBIC observatory from may 2005 until june 2013
2014, Slemr, Franz, Weigelt, Andreas, Ebinghaus, Ralf, Brenninkmeijer, Carl, Baker, Angela, Schuck, Tanja, Rauthe-Schöch, Armin, Riede, Hella, Leedham, Emma, Hermann, Markus, van Velthoven, Peter, Oram, David, O'Sullivan, Debbie, Dyroff, Christoph, Zahn, Andreas, Ziereis, Helmut
Tropospheric sections of flights with the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrumented Container) observatory from May 2005 until June 2013, are investigated for the occurrence of plumes with elevated Hg concentrations. Additional information on CO, CO2, CH4, NOy, O3, hydrocarbons, halocarbons, acetone and acetonitrile enable us to attribute the plumes to biomass burning, urban/industrial sources or a mixture of both. Altogether, 98 pollution plumes with elevated Hg concentrations and CO mixing ratios were encountered, and the Hg/CO emission ratios for 49 of them could be calculated. Most of the plumes were found over East Asia, in the African equatorial region, over South America and over Pakistan and India. The plumes encountered over equatorial Africa and over South America originate predominantly from biomass burning, as evidenced by the low Hg/CO emission ratios and elevated mixing ratios of acetonitrile, CH3Cl and particle concentrations. The backward trajectories point to the regions around the Rift Valley and the Amazon Basin, with its outskirts, as the source areas. The plumes encountered over East Asia and over Pakistan and India are predominantly of urban/industrial origin, sometimes mixed with products of biomass/biofuel burning. Backward trajectories point mostly to source areas in China and northern India. The Hg/CO2 and Hg/CH4 emission ratios for several plumes are also presented and discussed.
No Evidence for a Significant Impact of Heterogeneous Chemistry on Radical Concentrations in the North China Plain in Summer 2014
2020, Tan, Zhaofeng, Hofzumahaus, Andreas, Lu, Keding, Brown, Steven S., Holland, Frank, Huey, Lewis Gregory, Kiendler-Scharr, Astrid, Li, Xin, Liu, Xiaoxi, Ma, Nan, Min, Kyung-Eun, Rohrer, Franz, Shao, Min, Wahner, Andreas, Wang, Yuhang, Wiedensohler, Alfred, Wu, Yusheng, Wu, Zhijun, Zeng, Limin, Zhang, Yuanhang, Fuchs, Hendrik
The oxidation of nitric oxide to nitrogen dioxide by hydroperoxy (HO2) and organic peroxy radicals (RO2) is responsible for the chemical net ozone production in the troposphere and for the regeneration of hydroxyl radicals, the most important oxidant in the atmosphere. In Summer 2014, a field campaign was conducted in the North China Plain, where increasingly severe ozone pollution has been experienced in the last years. Chemical conditions in the campaign were representative for this area. Radical and trace gas concentrations were measured, allowing for calculating the turnover rates of gas-phase radical reactions. Therefore, the importance of heterogeneous HO2 uptake on aerosol could be experimentally determined. HO2 uptake could have suppressed ozone formation at that time because of the competition with gas-phase reactions that produce ozone. The successful reduction of the aerosol load in the North China Plain in the last years could have led to a significant decrease of HO2 loss on particles, so that ozone-forming reactions could have gained importance in the last years. However, the analysis of the measured radical budget in this campaign shows that HO2 aerosol uptake did not impact radical chemistry for chemical conditions in 2014. Therefore, reduced HO2 uptake on aerosol since then is likely not the reason for the increasing number of ozone pollution events in the North China Plain, contradicting conclusions made from model calculations reported in the literature. © 2020 American Chemical Society.