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Atmospheric Environment (v.44, #26)
Study of a winter PM episode in Istanbul using the high resolution WRF/CMAQ modeling system by Ulas Im; Kostandinos Markakis; Alper Unal; Tayfun Kindap; Anastasia Poupkou; Selahattin Incecik; Orhan Yenigun; Dimitros Melas; Christina Theodosi; Nikos Mihalopoulos (pp. 3085-3094).
High winter-time PM10, sulfate, nitrate and ammonium levels in Istanbul were investigated using a high resolution WRF/CMAQ mesoscale model system. A model-ready anthropogenic emission inventory on 2 km spatial resolution was developed for the area and the present study is the first attempt to test these emissions. The results suggested that the system was capable of producing the magnitudes. PM10 levels calculated by the model underestimated the observations with an average of 10 per cent at Bogazici University sampling station, whereas an overestimation of 12 per cent is calculated for all stations. High uncertainties, particularly in traffic and coal combustion, led to over estimations around emission hot spots. Base case results together with the sensitivity studies pointed significant contribution of local sources, pointing to the need of control strategies focusing on primary particulate emissions.
Keywords: Air quality modeling; Aerosol; Chemical composition; Istanbul; WRF; CMAQ
Sources of fine particles in the South Coast area, California by Eugene Kim; Katarzyna Turkiewicz; Sylvia A. Zulawnick; Karen L. Magliano (pp. 3095-3100).
PM2.5 (particulate matter less than 2.5 μm in aerodynamic diameter) speciation data collected between 2003 and 2005 at two United State Environmental Protection Agency (US EPA) Speciation Trends Network monitoring sites in the South Coast area, California were analyzed to identify major PM2.5 sources as a part of the State Implementation Plan development. Eight and nine major PM2.5 sources were identified in LA and Rubidoux, respectively, through PMF2 analyses. Similar to a previous study analyzing earlier data (), secondary particles contributed the most to the PM2.5 concentrations: 53% in LA and 59% in Rubidoux. The next highest contributors were diesel emissions (11%) in LA and Gasoline vehicle emissions (10%) in Rubidoux. Most of the source contributions were lower than those from the earlier study. However, the average source contributions from airborne soil, sea salt, and aged sea salt in LA and biomass smoke in Rubidoux increased.To validate the apportioned sources in this study, PMF2 results were compared with those obtained from EPA PMF (). Both models identified the same number of major sources and the resolved source profiles and contributions were similar at the two monitoring sites. The minor differences in the results caused by the differences in the least square algorithm and non-negativity constraints between two models did not affect the source identifications.
Keywords: South Coast Basin; Speciation trends network; Source apportionment; PM; 2.5
Influence of uncertain reaction rates on ozone sensitivity to emissions by Daniel S. Cohan; Bonyoung Koo; Greg Yarwood (pp. 3101-3109).
Air quality models rely upon simplified photochemical mechanisms to efficiently represent the thousands of chemical species that interact to form air pollution. Uncertainties in the chemical reaction rate constants and photolysis frequencies that comprise those mechanisms can generate uncertainty in the estimation of pollutant concentrations and their responsiveness to emission controls. A high-order sensitivity analysis technique is applied to quantify the extent to which reaction rate uncertainties influence estimates of ozone concentrations and their sensitivities to precursor emissions during an air pollution episode in Houston, Texas. Several reactions were found to have much larger proportional effects on ozone’s sensitivities to emissions than on its concentrations. In particular, uncertainties in photolysis frequencies and in the rate of reaction between NO2 and OH to form nitric acid can significantly influence the magnitude and sign of peak ozone sensitivity to nitrogen oxide (NOx) emissions. Ozone sensitivity to VOCs exhibits a much more muted response to uncertainties in the reaction rate constants and photolysis frequencies considered here. The results indicate the importance of accurate reaction rate constants to predicting the ozone impacts resulting from NOx emission controls.
Keywords: Ozone; Reaction rate constants; Parametric uncertainty; Sensitivity analysis; Decoupled direct method; Houston; Texas
Characteristics of aerosol types from AERONET sunphotometer measurements by J. Lee; J. Kim; C.H. Song; S.B. Kim; Y. Chun; B.J. Sohn; B.N. Holben (pp. 3110-3117).
By using observations from the Aerosol Robotic Network (AERONET), aerosol types are classified according to dominant size mode and radiation absorptivity as determined by fine-mode fraction (FMF) and single-scattering albedo (SSA), respectively. The aerosol type from anthropogenic sources is significantly different with regard to location and season, while dust aerosol is observed persistently over North Africa and the Arabian Peninsula. For four reference locations where different aerosol types are observed, time series and optical properties for each aerosol type are investigated. The results show that aerosol types are strongly affected by their sources and partly affected by relative humidity. The analysis and methodology of this study can be used to compare aerosol classification results from satellite and chemical transport models, as well as to analyze aerosol characteristics on a global scale over land for which satellite observations need to be improved.
Keywords: Aerosol; Type; Black carbon; Dust
Impact of roadside noise barriers on particle size distributions and pollutants concentrations near freeways by Zhi Ning; Neelakshi Hudda; Nancy Daher; Winnie Kam; Jorn Herner; Kathleen Kozawa; Steven Mara; Constantinos Sioutas (pp. 3118-3127).
Increasing epidemiological evidence has established an association between a host of adverse health effects and exposure to ambient particulate matter (PM) and co-pollutants, especially those emitted from motor vehicles. Although PM and their co-pollutants dispersion profiles near the open freeway have been extensively characterized by means of both experimental measurements and numerical simulations in recent years, such investigations near freeways with roadside barriers have not been well documented in the literature. A few previous studies suggested that the presence of roadside structures, such as noise barriers and vegetation, may impact the decay of pollutant concentrations downwind of the freeway by limiting the initial dispersion of traffic emissions and increasing their vertical mixing due to the upward deflection of airflow. Since the noise barriers are now common roadside features of the freeways, particularly those running through populated urban areas, it is pertinent to investigate the impact of their presence on the particles and co-pollutants concentrations in areas adjacent to busy roadways. This study investigated two highly trafficked freeways (I-710 and I-5) in Southern California, with two sampling sites for each freeway, one with and the other without the roadside noise barriers. Particle size distributions and co-pollutants concentrations were measured in the immediate proximity of freeways and at different distances downwind of the freeways. The results showed the formation of a “concentration deficit” zone in the immediate vicinity of the freeway with the presence of roadside noise barrier, followed by a surge of pollutant concentrations further downwind at 80–100 m away from freeway. The particle and co-pollutants concentrations reach background levels at farther distances of 250–400 m compared to 150–200 m at the sites without roadside noise barriers.
Keywords: Particle size distribution; Pollutants concentrations; Noise barrier; Freeway emissions; Roadway configurations
Assessment of the uncertainty of using an inverse-dispersion technique to measure methane emissions from animals in a barn and in a small pen by Zhiling Gao; Raymond L. Desjardins; Thomas K. Flesch (pp. 3128-3134).
Dispersion techniques are useful for assessing the effectiveness of management practices in mitigating methane (CH4) emissions from animal operations. In this paper, the accuracy of an inverse-dispersion technique was examined for two common situations: 1) emissions from animals in a barn and 2) emissions from animals in a pen. For both situations, the accuracy of emission estimates generally increased with increasing fetch (scaled to barn height, h, or to pen width, Xs) between the source and the concentration measurement. The gas recovery ratio increased from 0.66 at 5 h to 0.93–1.03 at 10 h–25 h for the barn, and decreased from 1.59 at 0 Xs to 0.99 at 5 Xs and from 1.54 at 0 Xs to 1.09 at 5 Xs for the two small pen scenarios, due to the declining sensitivity of the dispersion model to errors in wind complexity and errors in the assumed source configuration. However, the relative uncertainty of the measured concentration increased with fetch due to the decreasing gas concentrations. Hence, improving the accuracy of emission estimates is a compromise between the source configuration sensitivity and the concentration measurement sensitivity. Fetches of about twice the size of the pen and about 10 times the height of the barn are suggested.
Keywords: Inverse-dispersion technique; Pen; Barn; Open-path laser; Relative uncertainty
Variation of the mixing state of Saharan dust particles with atmospheric transport by Manuel Dall’Osto; Roy M. Harrison; Eleanor J. Highwood; Colin O’Dowd; Darius Ceburnis; Xavier Querol; Eric P. Achterberg (pp. 3135-3146).
Mineral dust is an important aerosol species in the Earth’s atmosphere and has a major source within North Africa, of which the Sahara forms the major part. Aerosol Time of Flight Mass Spectrometry (ATOFMS) is first used to determine the mixing state of dust particles collected from the land surface in the Saharan region, showing low abundance of species such as nitrate and sulphate internally mixed with the dust mineral matrix. These data are then compared with the ATOFMS single particle mass spectra of Saharan dust particles detected in the marine atmosphere in the vicinity of the Cape Verde islands, which are further compared with those from particles with longer atmospheric residence sampled at a coastal station at Mace Head, Ireland. Saharan dust particles collected near the Cape Verde Islands showed increased internally mixed nitrate but no sulphate, whilst Saharan dust particles collected on the coast of Ireland showed a very high degree of internally mixed secondary species including nitrate, sulphate and methanesulphonate. This uptake of secondary species will change the pH and hygroscopic properties of the aerosol dust and thus can influence the budgets of other reactive gases, as well as influencing the radiative properties of the particles and the availability of metals for dissolution.
Keywords: Saharan dust; Single particle; ATOFMS; Mixing state; Iron
Road traffic impact on urban atmospheric aerosol loading at Oporto, Portugal by César Oliveira; Casimiro Pio; Alexandre Caseiro; Patrícia Santos; Teresa Nunes; Hongjun Mao; Lakhumal Luahana; Ranjeet Sokhi (pp. 3147-3158).
At urban areas in south Europe atmospheric aerosol levels are frequently above legislation limits as a result of road traffic and favourable climatic conditions for photochemical formation and dust suspension. Strategies for urban particulate pollution control have to take into account specific regional characteristics and need correct information concerning the sources of the aerosol.With these objectives, the ionic and elemental composition of the fine (PM2.5) and coarse (PM2.5–10) aerosol was measured at two contrasting sites in the centre of the city of Oporto, roadside (R) and urban background (UB), during two campaigns, in winter and summer.Application of Spatial Variability Factors, in association with Principal Component/Multilinear Regression/Inter-site Mass Balance Analysis, to aerosol data permitted to identify and quantify 5 main groups of sources, namely direct car emissions, industry, photochemical production, dust suspension and sea salt transport. Traffic strongly influenced PM mass and composition. Direct car emissions and road dust resuspension contributed with 44–66% to the fine aerosol and with 12 to 55% to the coarse particles mass at both sites, showing typically highest loads at roadside. In fine particles secondary origin was also quite important in aerosol loading, principally during summer, with 28–48% mass contribution, at R and UB sites respectively. Sea spray has an important contribution of 18–28% to coarse aerosol mass in the studied area, with a highest relative contribution at UB site.Application of Spatial Variability/Mass Balance Analysis permitted the estimation of traffic contribution to soil dust in both size ranges, across sites and seasons, demonstrating that as much as 80% of present dust can result from road traffic resuspension.
Keywords: Urban aerosol; Source apportionment; Road dust; South-Europe
A new methodology development for the regulatory forecasting of PM10. Application in the Greater Athens Area, Greece by A. Sfetsos; D. Vlachogiannis (pp. 3159-3172).
The paper introduces a new methodology for the prediction of daily PM10 concentrations, in line with the regulatory framework introduced through the EU Directive 2008/50/EC. The proposed approach is based on the efficient utilisation of the data collected over short time intervals (hourly) rather than the daily values used to derive the daily regulatory threshold. It is sufficiently simple and easily applicable in operational forecasting systems with the ability to accept as inputs both historical data and exogenous paraeters, such as meteorological variables. The application of the proposed methodology is demonstrated using data from five monitoring stations of air pollutants located in Athens, over a five year period (2000–2004) as well as compatible meteorological data from the NCEP (National Centers for Environmental Protection). A set of different models have been tested at the same time to reveal the effectiveness of the proposed approach, both univariate and multivariate, and linear and non-linear models. The analysis of all examined datasets has shown conclusive evidence that the introduction of the newly developed procedure which utilises data collected over a shorter horizon can significantly increase the forecasting ability of any developed model using daily historic PM10 data, under all examined metrics.
Keywords: PM10 exceedances; Forecasting; Subsampling; Regulatory limit
Polychlorinated biphenyls (PCB) and dichlorodiphenyltrichloroethane (DDE) air concentrations in the Lake Ontario region: Trends and potential sources by Hyun-Deok Choi; James J. Pagano; Michael S. Milligan; Philip K. Hopke; Steven Skubis; Thomas M. Holsen (pp. 3173-3178).
Airborne particle and gas samples were collected approx every 12 days from April 2002 to June 2006 at the Sterling Nature Center located near the southeast corner of Lake Ontario. These samples were analyzed for polychlorinated biphenyls (PCBs) and dichlorodiphenyltrichloroethane (DDE). Clausius-Clapeyron (C–C) regression analyses of PCBs and DDE yielded moderate correlations (r 2 = 0.54, p < 0.001;r 2 = 0.74, p < 0.001, respectively) indicating that much of the variations in concentrations can be explained by temperature. Back trajectory analysis indicated that the most important factors driving unusually high PCB partial pressures relative to those predicted by the C–C regression were slow wind speeds and winds generally from the southwest. This combination, which occurred frequently in 2004, increased contact of the air with contaminated upwind surfaces with minimum dilution. Hybrid receptor modeling (Potential Source Contribution Function (PSCF)) results for the total PCBs identified the midwestern US region that contains the urban areas of southern Indiana (IN), southwestern Ohio (OH), and northern Kentucky (KY) having the highest PSCF values. In general urban areas like Chicago (IL), Detroit (MI), Cleveland (OH), St. Louis (MO), and Nashville (TN) also had significant possibilities. In contrast, the PSCF modeling for DDE identified northern Alabama as the area with the highest probability where DDT was applied to cotton fields.
Keywords: Polychlorinated biphenyls (PCB); Dichlorodiphenyltrichloroethane (DDE); Potential source contribution function (PSCF); Lake Ontario
Linear and non-linear relationships mapping the Henry’s law parameters of organic pesticides by Mohammad Goodarzi; Erlinda V. Ortiz; Leandro dos S. Coelho; Pablo R. Duchowicz (pp. 3179-3186).
This work aims to predict the air to water partitioning for 96 organic pesticides by means of the Quantitative Structure–Property Relationships Theory. After performing structural feature selection with Genetics Algorithms and Replacement Method linear approaches, it is found that among the most important molecular features appears the Moriguchi octanol–water partition coefficient, and higher lipophilicities would lead to compounds having higher Henry’s law constants. We also compare the statistical performance achieved by four fully-connected Feed-Forward Multilayer Perceptrons Artificial Neural Networks. The statistical results found reveal that the best performing model uses the Levenberg–Marquardt with Bayesian regularization (BR) weighting function for achieving the most accurate predictions.
Keywords: QSPR-QSAR Theory; Replacement method; Artificial neural networks; Henry’s law constant; Dragon molecular descriptors
Chemical speciation, transport and contribution of biomass burning smoke to ambient aerosol in Guangzhou, a mega city of China by Zhisheng Zhang; Guenter Engling; Chuan-Yao Lin; Charles C.-K. Chou; Shih-Chun C. Lung; Shih-Yu Chang; Shaojia Fan; Chuen-Yu Chan; Yuan-Hang Zhang (pp. 3187-3195).
Intensive measurements of aerosol (PM10) and associated water-soluble ionic and carbonaceous species were conducted in Guangzhou, a mega city of China, during summer 2006. Elevated levels of most chemical species were observed especially at nighttime during two episodes, characterized by dramatic build-up of the biomass burning tracers levoglucosan and non-sea-salt potassium, when the prevailing wind direction had changed due to two approaching tropical cyclones. High-resolution air mass back trajectories based on the MM5 model revealed that air masses with high concentrations of levoglucosan (43–473 ng m−3) and non-sea-salt potassium (0.83–3.2 μg m−3) had passed over rural regions of the Pearl River Delta and Guangdong Province, where agricultural activities and field burning of crop residues are common practices. The relative contributions of biomass burning smoke to organic carbon in PM10 were estimated from levoglucosan data to be on average 7.0 and 14% at daytime and nighttime, respectively, with maxima of 9.7 and 32% during the episodic transport events, indicating that biomass and biofuel burning activities in the rural parts of the Pearl River Delta and neighboring regions could have a significant impact on ambient urban aerosol levels.
Keywords: Biomass combustion; PM; 10; Levoglucosan; Non-sea-salt potassium; Pearl River Delta
Changes in the wet precipitation of sodium and chloride over the continental United States, 1984–2006 by Philip J. Lloyd (pp. 3196-3206).
Data on wet-only precipitation from the National Atmospheric Deposition Program/National Trends Network were analysed for trends in the sodium and chloride fluxes over the United States between 1 January 1984 and 31 December 2006. The data were first checked for consistency and for ionic balance. It was necessary to correct for changes in bicarbonate due to changes in atmospheric CO2 levels over the study period, in order to obtain a balance. The fluxes were calculated and the trends determined by linear regression in the log domain. The significance of the trends was checked using both F- and t-tests. At 154 sites having reasonably continuous records over the assessment period, the sodium flux fell significantly at 139 and increased significantly at only one. The chloride flux similarly fell significantly at 140 and increased significantly at the same one as the sodium flux increased. At coastal sites the chloride to sodium ratio was the same as that in sea water, within experimental limits. Further from the coast the ratio changed apparently due to changes in the entire aerosol chemistry. The findings are discussed in terms of the simplicity and robustness of the methodology employed to determine the trends; the oceanic origin of most observable sodium even in the interior of the continent, probably because it occurs as a fine (<1 micron) aerosol which is poorly scavenged by precipitation; and the possibility that the drop in sodium and chloride fluxes might be driven by climate change.
Keywords: Sodium chloride; Rain; Precipitation chemistry; Atmospheric deposition; Aerosols; Trend analysis
Reconstructing historical trends of polycyclic aromatic hydrocarbon deposition in a remote area of Spain using herbarium moss material by L. Foan; C. Sablayrolles; D. Elustondo; E. Lasheras; L. González; A. Ederra; V. Simon; J.M. Santamaría (pp. 3207-3214).
Herbarium mosses from 1879–1881, 1973–1975 and 2006–2007 were used to investigate the historical changes of atmospheric deposition of polycyclic aromatic hydrocarbons (PAHs) at a remote site in Northern Spain. Natural abundance of nitrogen and carbon isotopes was also measured in order to assess the evolution of emissions from anthropogenic sources. Nitrogen and PAH concentrations as well as δ13C and δ15N ratios were significantly higher in 19th century samples compared to present century samples. Moreover, PAH distribution varied over the centuries, with the trend towards enrichment in light PAHs. The carbon, nitrogen and PAH concentrations measured in the mosses tally with the historical evolution of anthropogenic emissions in the area, mainly influenced by changes in economic activities, domestic heating and road traffic density. Mosses provided by herbaria seem to offer the possibility of studying long-term temporal evolution of atmospheric PAH deposition.
Keywords: Atmospheric deposition; Biomonitoring; Herbarium moss; PAH; N and C isotope signatures
Central power generation versus distributed generation – An air quality assessment in the South Coast Air Basin of California by Marc Carreras-Sospedra; Satish Vutukuru; Jacob Brouwer; Donald Dabdub (pp. 3215-3223).
This study assesses the air quality impacts of central power generation and compares them with the impacts of distributed generation (DG). The central power plant emissions factors used are from a newly installed combined cycle gas turbine system. Because location of power plants is a key parameter affecting air quality impacts, this study considers three potential locations for the installation of central power plants. Air quality impacts are evaluated for the South Coast Air Basin of California, in the year 2010, using a three-dimensional air quality model. Results are compared to air quality impacts from two potential DG scenarios to meet the same power demand as that of the central power plant case.Even though emissions from central generation are lower than emissions from the DG technology mix considered herein, central generation concentrates emissions in a small area, whereas DG spreads emissions throughout a larger cross-section of the air basin. As a result, air quality impacts from central generation are more significant than those from DG. The study also shows that assessment of air quality impacts from distributed and central generation should not only consider emissions levels, but also the spatial and temporal distribution of emissions and the air quality that results from atmospheric chemistry and transport – highly non-linear processes.Finally, analysis of population exposure to ozone and PM2.5 shows that central generation located in coastal areas upwind from populated areas would cause the highest population exposure and even though emissions from central generation are considerably lower than DG emissions spread throughout the basin, results show that central generation causes a higher pollutant exposure than DG.
Keywords: Distributed generation; Central generation; Air quality modeling; Reactivity
Exposure to ultrafine particles and PM2.5 in four Sydney transport modes by Luke D. Knibbs; Richard J. de Dear (pp. 3224-3227).
Concentrations of ultrafine (<0.1 μm) particles (UFPs) and PM2.5 (<2.5 μm) were measured whilst commuting along a similar route by train, bus, ferry and automobile in Sydney, Australia. One trip on each transport mode was undertaken during both morning and evening peak hours throughout a working week, for a total of 40 trips. Analyses comprised one-way ANOVA to compare overall (i.e. all trips combined) geometric mean concentrations of both particle fractions measured across transport modes, and assessment of both the correlation between wind speed and individual trip means of UFPs and PM2.5, and the correlation between the two particle fractions. Overall geometric mean concentrations of UFPs and PM2.5 ranged from 2.8 (train) to 8.4 (bus) × 104 particles cm−3 and 22.6 (automobile) to 29.6 (bus) μg m−3, respectively, and a statistically significant difference ( p < 0.001) between modes was found for both particle fractions. Individual trip geometric mean concentrations were between 9.7 × 103 (train) and 2.2 × 105 (bus) particles cm−3 and 9.5 (train) to 78.7 (train) μg m−3. Estimated commuter exposures were variable, and the highest return trip mean PM2.5 exposure occurred in the ferry mode, whilst the highest UFP exposure occurred during bus trips. The correlation between fractions was generally poor, and in keeping with the duality of particle mass and number emissions in vehicle-dominated urban areas. Wind speed was negatively correlated with, and a generally poor determinant of, UFP and PM2.5 concentrations, suggesting a more significant role for other factors in determining commuter exposure.
Keywords: Commuter; Exposure; Transport; Ultrafine particles; PM; 2.5