Transport of nitrogen oxides, carbon monoxide and ozone to the Alpine Global Atmosphere Watch stations Jungfraujoch (Switzerland), Zugspitze and Hohenpeissenberg (Germany), Sonnblick (Austria) and Mt. Krvavec (Slovenia)

The Alpine stations Zugspitze, Hohenpeissenberg, Sonnblick, Jungfraujoch and Mt. Krvavec contribute to the Global Atmosphere Watch Programme (GAW) of the World Meteorological Organization (WMO). The aim of GAW is the surveillance of the large-scale chemical composition of the atmosphere. Thus, the detection of air pollutant transport from regional sources is of particular interest. In this paper, the origin of NO_x (measured with a photo-converter), CO and O₃ at the four Alpine GAW stations is studied by trajectory residence time statistics. Although these methods originated during the early 1980s, no comprehensive study of different atmospheric trace gases measured simultaneously at several background observatories in the Alps was conducted up to present.The main NO_x source regions detected by the trajectory statistics are the northwest of Europe and the region covering East Germany, Czech Republic and southeast Poland, whereas the main CO source areas are the central, north eastern and eastern parts of Europe with some gradient from low to high latitudes. Subsiding air masses from west and southwest are relatively poor in NO_x and CO.The statistics for ozone show strong seasonal effects. Near ground air masses are poor in ozone in winter but rich in ozone in summer. The main source for high ozone concentration in winter is air masses that subside from higher elevations, often enhanced by foehn effects at Hohenpeissenberg. During summer, the Mediterranean constitutes an important additional source for high ozone concentrations.Especially during winter, large differences between Hohenpeissenberg and the higher elevated stations are found. Hohenpeissenberg is frequently within the inversion, whereas the higher elevated stations are above the inversion.Jungfraujoch is the only station where the statistics detect an influence of air rich in CO and NO_x from the Po Basin.     

A study of the ozone formation by ensemble back trajectory-process analysis using the Eta–CMAQ forecast model over the northeastern U.S. during the 2004 ICARTT period

The integrated process rates (IPRs) estimated by the Eta–CMAQ model at grid cells along the trajectory of the air mass transport path were analyzed to quantitatively investigate the relative importance of physical and chemical processes for O₃ formation and evolution over the northeastern U.S. during the 2004 International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) period. The Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model is used to determine the back trajectory of air masses reaching the northeast by linking a downwind receptor to upwind source areas. The process analysis is applied to a high O₃ episode occurring on July 22, 2004 at three selected sites in the northeastern U.S. The process analysis at the location of the site shows that during the daytime, the O₃ concentrations in the surface layer are mainly enhanced by the vertical diffusion of O₃-rich air from aloft, followed by horizontal advection (HADV) and chemical production (CHEM), whereas dry deposition (DDEP) and vertical advection (ZADV) mainly deplete O₃ concentrations at the sites of Valley Central (VC), NY and Castle Spring (CS), NH. By integrating the effects of each process over the depth of the daytime planetary boundary layer (PBL), it was found that at the VC site, CHEM and HADV contributed about 53% and 41%, respectively, to O₃ levels within the PBL. This confirms the significance of regional transport of O₃ from the industrialized areas into the Northeast. On the other hand, the process analysis results for O₃ formation in moving air masses indicate that on July 22, large chemical production of O₃ along the transport path over the polluted urban regions leads to significant increase in O₃ in the air mass reaching the VC site, whereas the low chemical production of O₃ along the transport path over the low emission regions leads to the low O₃ concentration at the site of Belleayre Mountain (BM), NY. The dramatic buildup of O₃ concentration from 50 ppb to 102 ppb in the air masses before reaching the VC site after 12:00 EST on 7/22 indicates the significant impact of pollution from the northeastern urban corridor at this site. On the basis of the results at the CS site, it was found that high NO_x emissions along the transport path led to large chemical production of O₃ in the air mass reaching the CS site on July 22. In contrast, the low chemical production of O₃ associated with low emission (relatively clean conditions) along the transport path over the northern portions of the domain is responsible for the low O₃ concentration at the CS site on July 26.     

Process analysis of a regional air pollution episode over Pearl River Delta Region,China, using the MM5-CMAQ model

This study focuses on the influences of a warm high-pressure meteorological system on aerosol pollutants, employing the simulations by the Models-3/CMAQ system and the observations collected during October 10–12, 2004, over the Pearl River Delta (PRD) region. The results show that the spatial distributions of air pollutants are generally circular near Guangzhou and Foshan, which are cities with high emissions rates. The primary pollutant is particulate matter (PM) over the PRD. MM5 shows reasonable performance for major meteorological variables (i.e., temperature, relative humidity, wind direction) with normalized mean biases (NMB) of 4.5–38.8% and for their time series. CMAQ can capture one peak of all air pollutant concentrations on October 11, but misses other peaks. The CMAQ model systematically underpredicts the mass concentrations of all air pollutants. Compared with chemical observations, SO₂ and O₃ are predicted well with a correlation coefficient of 0.70 and 0.65. PM_2.5 and NO are significantly underpredicted with an NMB of 43% and 90%, respectively. The process analysis results show that the emission, dry deposition, horizontal transport, and vertical transport are four main processes affecting air pollutants. The contributions of each physical process are different for the various pollutants. The most important process for PM₁₀ is dry deposition, and for NO_x it is transport. The contributions of horizontal and vertical transport processes vary during the period, but these two processes mostly contribute to the removal of air pollutants at Guangzhou city, whose emissions are high. For this high-pressure case, the contributions of the various processes show high correlations in cities with the similar geographical attributes. According to the statistical results, cities in the PRD region are divided into four groups with different features. The contributions from local and nonlocal emission sources are discussed in different groups.

Implications: The characteristics of aerosol pollution episodes are intensively studied in this work using the high-resolution modeling system MM5/SMOKE/CMAQ, with special efforts on examining the contributions of different physical and chemical processes to air concentrations for each city over the PRD region by a process analysis method, so as to provide a scientific basis for understanding the formation mechanism of regional aerosol pollution under the high-pressure system over PRD.     

Measurements and analyses of nitrogen oxides and ozone in the yard and on the roof of a street-canyon in Suzhou

The concentrations of air pollutants such as nitrogen oxides and ozone characterised by very fast chemical reactions can significantly vary within urban street-canyon due to the short distances between sources and receptor. With the primary objective to analyse this issue, NO, NO₂, NO_x, O₃, BTX, and wind flow field were continuously measured for 1 week at two heights (a street-level yard and a 25-m-high rooftop) in an urban canyon in Suzhou (China). The yard ozone concentrations were found to be up to six times lower than on the roof. Different frequency distributions (FD), dynamical and chemical processes of the pollutant variations from yard to roof are discussed to explain the findings. The predominant factors for the dissimilar pollutant vertical diffusion at the two measurement locations were associated to dissimilar fluid-dynamic and heterogeneous removal effects that likely induced dissimilar ozone chemical processes relative to NO_x and BTX precursors.     

Identification of redundant air quality measurements through the use of principal component analysis

This study aims to show how principal component analysis (PCA) can be used to identify redundant measurements in air quality monitoring networks. The minimum number of air quality monitoring sites in Oporto Metropolitan Area (Oporto-MA) was evaluated using PCA and then compared to the one settled by the legislation. Nine sites, monitoring NO₂, O₃ and PM₁₀, were selected and the air pollutant concentrations were analysed from January 2003 to December 2005. PCA was applied to the data corresponding to the first two years that were divided into annual quarters to verify the persistence of the PCA results. The number of principal components (PCs) was selected by applying two criteria: Kaiser (PCs with eigenvalues greater than 1) and ODV₉₀ (PCs representing at least 90% of the original data variance). Each pollutant was analysed separately. The two criteria led to different results. Using Kaiser criterion for the eight analysed periods, two PCs were selected in: (i) five periods for O₃ and PM₁₀; and (ii) six periods for NO₂. These PCs had important contributions of the same groups of monitoring sites. The percentage of the original data variance contained in the selected PCs using this criterion was always below 90%. Thus, the results obtained using ODV₉₀ were considered with more confidence. Using this criterion, only five monitoring sites for NO₂, three for O₃ and seven for PM₁₀ were needed to characterize the region. The number of monitoring sites for NO₂ and O₃ was in agreement with what was established by the legislation. However, for PM₁₀, Oporto-MA needed two more monitoring sites. To validate PCA results, statistical models were determined to estimate air pollutant concentrations at removed monitoring sites using the concentrations measured at the remaining monitoring sites. These models were applied to a year's data. The good performance obtained by the models showed that the monitoring sites selected by the procedure presented in this study were enough to infer the air pollutant concentrations in the region defined by the initial monitoring sites. Additionally, the air pollutant analysers corresponding to the redundant measurements can be installed in non-monitored regions, allowing the enlargement of the air quality monitoring network.     

Strategic guidelines for street canyon geometry to achieve sustainable street air quality

This paper is concerned with the motion of air within the urban street canyon and is directed towards a deeper understanding of pollutant dispersion with respect to various simple canyon geometries and source positions. Taking into account the present days typical urban configurations, three principal flow regimes “isolated roughness flow”, “skimming flow” and “wake interference flow” (Boundary Layer Climates, 2nd edition, Methuen, London) and their corresponding pollutant dispersion characteristics are studied for various canopies aspect ratios, namely relative height (h₂/h₁), canyon height to width ratio (h/w) and canyon length to height ratio (l/h). A field-size canyon has been analyzed through numerical simulations using the standard k-ε turbulence closure model. It is found that the pollutant transport and diffusion is strongly dependent upon the type of flow regime inside the canyon and exchange between canyon and the above roof air. Some rules of thumbs have been established to get urban canyon geometries for efficient dispersion of pollutants.     

Strategic guidelines for street canyon geometry to achieve sustainable street air quality

This paper is concerned with the motion of air within the urban street canyon and is directed towards a deeper understanding of pollutant dispersion with respect to various simple canyon geometries and source positions. Taking into account the present days typical urban configurations, three principal flow regimes “isolated roughness flow”, “skimming flow” and “wake interference flow” (Boundary Layer Climates, 2nd edition, Methuen, London) and their corresponding pollutant dispersion characteristics are studied for various canopies aspect ratios, namely relative height (h₂/h₁), canyon height to width ratio (h/w) and canyon length to height ratio (l/h). A field-size canyon has been analyzed through numerical simulations using the standard k-ε turbulence closure model. It is found that the pollutant transport and diffusion is strongly dependent upon the type of flow regime inside the canyon and exchange between canyon and the above roof air. Some rules of thumbs have been established to get urban canyon geometries for efficient dispersion of pollutants.     

Effect of typhoon on atmospheric particulates in autumn in central Taiwan

Previous studies have suggested that the ongoing global climate change will likely increase the intensity and frequency of extreme weather, such as typhoons. Since the beginning of global warming, it has become necessary to understand the influence of typhoons on air quality. Rare data, especially particulate measurements data could be used to establish the relationship between the air pollution and typhoons. One of main limiting factors is that most of the previous chemical analyses of particulates used a relatively long sampling time, which could dilute the temporal impact of particulate characteristics and their sources. This work, depending more time-resolved measurements, focus on the characteristics and sources of high particulate matter levels and the influence of typhoons and the Pacific high system. Depending on the measurements, two pollutant groups were clearly identified in this work. The first pollutant group was the emissions from neighboring riverbeds under the strong circulation of the typhoon in the driest season and characterized as high coarse particle concentrations with high mass fraction of Ca²⁺. The second pollutant group was characterized as the formation and transport of secondary particles with prevalent ions of NH₄⁺, NO₃^?, and SO₄^2? and occurred in the sea-land breeze circulation under the influence the Pacific high system.     

Artificial intelligence modeling to evaluate field performance of photocatalytic asphalt pavement for ambient air purification

In recent years, the application of titanium dioxide (TiO₂) as a photocatalyst in asphalt pavement has received considerable attention for purifying ambient air from traffic-emitted pollutants via photocatalytic processes. In order to control the increasing deterioration of ambient air quality, urgent and proper risk assessment tools are deemed necessary. However, in practice, monitoring all process parameters for various operating conditions is difficult due to the complex and non-linear nature of air pollution-based problems. Therefore, the development of models to predict air pollutant concentrations is very useful because it can provide early warnings to the population and also reduce the number of measuring sites. This study used artificial neural network (ANN) and neuro-fuzzy (NF) models to predict NO_x concentration in the air as a function of traffic count (T_r) and climatic conditions including humidity (H), temperature (T), solar radiation (S), and wind speed (W) before and after the application of TiO₂ on the pavement surface. These models are useful for modeling because of their ability to be trained using historical data and because of their capability for modeling highly non-linear relationships. To build these models, data were collected from a field study where an aqueous nano TiO₂ solution was sprayed on a 0.2-mile of asphalt pavement in Baton Rouge, LA. Results of this study showed that the NF model provided a better fitting to NO_x measurements than the ANN model in the training, validation, and test steps. Results of a parametric study indicated that traffic level, relative humidity, and solar radiation had the most influence on photocatalytic efficiency.     

Multiple regression analysis in modeling of columnar ozone in Peninsular Malaysia

This study aimed to predict monthly columnar ozone (O₃) in Peninsular Malaysia by using data on the concentration of environmental pollutants. Data (2003–2008) on five atmospheric pollutant gases (CO₂, O₃, CH₄, NO₂, and H₂O vapor) retrieved from the satellite Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) were employed to develop a model that predicts columnar ozone through multiple linear regression. In the entire period, the pollutants were highly correlated (R?=?0.811 for the southwest monsoon, R?=?0.803 for the northeast monsoon) with predicted columnar ozone. The results of the validation of columnar ozone with column ozone from SCIAMACHY showed a high correlation coefficient (R?=?0.752–0.802), indicating the model’s accuracy and efficiency. Statistical analysis was utilized to determine the effects of each atmospheric pollutant on columnar ozone. A model that can retrieve columnar ozone in Peninsular Malaysia was developed to provide air quality information. These results are encouraging and accurate and can be used in early warning of the population to comply with air quality standards.     

Tree bark as a passive air sampler to indicate atmospheric polybrominated diphenyl ethers (PBDEs) in southeastern China

The different barks were sampled to discuss the influence of the tree species, trunk circumference, and bark thickness on the accumulation processes of polybrominated diphenyl ethers (PBDEs) from air into the bark. The results of different PBDE concentrations indicated that barks with a thickness of 0–3 mm collected from weeping willow, Camphor tree, and Masson pine, the trunk circumferences of which were 100 to 150 cm, were better PBDEs passive samplers. Furthermore, tree bark and the corresponding air samples were collected at Anji (AJ), Hangzhou (HZ), Shanghai (SH), and Wenling (WL) to investigate the relationship between the PBDE concentrations in bark and those in air. In addition, the significant correlation (r ²?=?0.906; P?<?0.05) indicated that atmospheric PBDEs were the principle source for the accumulation of PBDEs in the barks. In this study, the log K _BA (bark–air partition coefficient) of individual PBDE congeners at the four sites were in the range from 5.69 to 6.79. Finally, the total PBDE concentration in WL was 5 to 20 times higher than in the other three cities. The result indicated that crude household workshops contributed a heavy amount of PBDEs pollution to the environment, which had been verified by the spatial distribution of PBDEs levels in barks collected at Wenling (range, 26.53–1317.68 ng/g dw). The good correlation between the PBDE concentrations in the barks and the air samples and the variations of the PBDE concentrations in tree barks collected from different sites reflected that the bark could be used as a passive sampler to indicate the atmospheric PBDEs.     

A study of seasonal and yearly modulation of carbon dioxide sources and sinks,with a particular attention to the Boreal Atlantic Ocean

With the intention of identifying and monitoring space and time patterns of carbon dioxide sources and sinks, the seasonal fields of atmospheric CO₂ concentration over an area covering Europe, the Boreal Atlantic, and North Africa have been computed by using CO₂ observations measured at one or two remote sites in conjunction with the backward air trajectories crossing the same observation sites.The air trajectories have been calculated by means of the wind speed fields provided by the ECMWF (European Centre of Medium-range Weather Forecast, of Reading, UK) analyses (T213/L31 model) on a regular grid, while the atmospheric CO₂ concentrations have been measured at two alpine European stations, located in the free atmosphere, far from the influence of local industrial pollution.A modified version of the statistical receptor-to-source-oriented-model (hereafter, source-oriented model) of Stohl (Atmos. Environ. 30 (1998) 947), using the above-mentioned air trajectories, has then been applied to reconstruct the spatial distribution fields of atmospheric CO₂.This source-oriented methodology belongs to a family of models which are simpler and easier to use than the more powerful and widespread inverse models and can allow a reliable deduction of the location of sources and sinks of gas tracers.We have applied this kind of model in order to identify source and sink macro-regions of CO₂ over the above-mentioned area in the period 1993–1998. The CO₂ observing stations of Plateau Rosà (3480 m a.s.l., in the western Alps) and Zugspitze (2937 m, in the eastern Alps) have been considered particularly fit for this purpose, because of their location in high orography areas, allowing to monitor values of atmospheric CO₂ concentrations representative of fairly well-mixed air, not affected by some local influences (industries, urban emissions, etc.). In this way, it can be assumed that possible maxima or minima observed in the trend of measured gas concentration can be due to contaminations of the air mass during its whole travel, at some specific locations identified by the source-oriented model.The most interesting result obtained in this study is the seasonal cycle of the atmospheric CO₂ concentration found over the mid- and sub-tropical latitudes of the Boreal Atlantic Ocean and evident in all simulations. This cycle appears to be clearly related to the seasonal trend of the SST, particularly in the tropical and subtropical Atlantic regions, and is particularly evident during the warmest months (during Spring, Autumn and particularly in Summer).     

Ambient air pollution and term birth weight in Texas from 1998 to 2004

Previous studies have explored the association between air pollution levels and adverse birth outcomes such as lower birth weight. Existing literature suggests an association, although results across studies are not consistent. Additional research is needed to confirm the effect, investigate the exposure window of importance, and distinguish which pollutants cause harm.

We assessed the association between ambient pollutant concentrations and term birth weight for 1,548,904 births in TX from 1998 to 2004. Assignment of prenatal exposure to air pollutants was based on maternal county of residence at the time of delivery. Pollutants examined included particulate matter with aerodynamic diameter ≤10 and ≤2.5 µm (PM₁₀ and PM_2.5), sulfur dioxide (SO₂), nitrogen dioxide (NO₂), carbon monoxide (CO), and ozone (O₃). We applied a linear model with birth weight as a continuous variable. The model was adjusted for known risk factors and region. We assessed pollutant effects by trimester to identify biological exposure window of concern, and explored interaction due to race/ethnicity.

An interquartile increase in ambient pollutant concentrations of SO₂ and O₃ was associated with a 4.99-g (95% confidence interval [CI], 1.87–8.11) and 2.72-g (95% CI, 1.11–4.33) decrease in birth weight, respectively. Lower birth weight was associated with exposure to O₃ in the first and second trimester, whereas results were not significant for other pollutants by trimester. A positive association was exhibited for PM_2.5 in the first trimester. Effects estimates for PM₁₀ and PM_2.5 were inconsistent across race/ethnic groups.

Current ambient air pollution levels may be increasing the risk of lower birth weight for some pollutants. These risks may be increased for certain racial/ethnic groups. Additional research including consideration of improved methodology is needed to investigate these findings. Future studies should examine the influence of residual confounding.

Implications: This is one of the most comprehensive studies examining criteria air pollutants and lower birth weight in Texas. Our findings confirm results found previously for adverse effects of the air pollutant SO₂ on lower birth weight. Results from our study suggest that adverse pregnancy outcomes such as lower birth weight can occur even while maintaining air pollution levels below regulatory standards. Future studies should incorporate the assessment of differential pollutant exposure as well as effect estimates by race/ethnicity with individual and community-level social factors in order to enhance our understanding of how physical, social, and host factors influence birth outcomes.

Supplemental Materials: Supplementary information relating to characteristics of excluded births, distribution of air pollutant monitors by pollutant, and correlation coefficients of the air pollutants is available in the publisher's online edition of the Journal of the Air & Waste Management Association.     

Seasonal and spatial variation of organic tracers for biomass burning in PM1 aerosols from highly insolated urban areas

PM₁ aerosol characterization on organic tracers for biomass burning (levoglucosan and its isomers and dehydroabietic acid) was conducted within the AERTRANS project. PM₁ filters (N?=?90) were sampled from 2010 to 2012 in busy streets in the urban centre of Madrid and Barcelona (Spain) at ground-level and at roof sites. In both urban areas, biomass burning was not expected to be an important local emission source, but regional emissions from wildfires, residential heating or biomass removal may influence the air quality in the cities. Although both areas are under influence of high solar radiation, Madrid is situated in the centre of the Iberian Peninsula, while Barcelona is located at the Mediterranean Coast and under influence of marine atmospheres. Two extraction methods were applied, i.e. Soxhlet and ASE, which showed equivalent results after GC-MS analyses. The ambient air concentrations of the organic tracers for biomass burning increased by an order of magnitude at both sites during winter compared to summer. An exception was observed during a PM event in summer 2012, when the atmosphere in Barcelona was directly affected by regional wildfire smoke and levels were four times higher as those observed in winter. Overall, there was little variation between the street and roof sites in both cities, suggesting that regional biomass burning sources influence the urban areas after atmospheric transport. Despite the different atmospheric characteristics in terms of air relative humidity, Madrid and Barcelona exhibit very similar composition and concentrations of biomass burning organic tracers. Nevertheless, levoglucosan and its isomers seem to be more suitable for source apportionment purposes than dehydroabietic acid. In both urban areas, biomass burning contributions to PM were generally low (2 %) in summer, except on the day when wildfire smoke arrive to the urban area. In the colder periods the contribution increase to around 30 %, indicating that regional biomass burning has a substantial influence on the urban air quality.     

Evaluation of aerosol sources at European high altitude background sites with trajectory statistical methods

This study has investigated the influence of synoptic weather patterns and long-range transport episodes on the concentrations of several compounds related to different aerosol sources (EC, OC, SO₄^2?, Ca²⁺, Na⁺, K⁺, ²¹⁰Pb, levoglucosan and dicarboxylic acids) registered in PM10 or PM2.5 aerosol samples collected at three remote background sites in central Europe. Air mass back-trajectories arriving at these sites have been analysed by statistical methods. Firstly, air mass back-trajectories have been grouped into clusters. Each cluster corresponds to specific meteorological scenarios, which were extracted and discussed. Finally, redistributed concentration fields have been computed to identify the main potential source regions of the different key aerosol components. A marked seasonal pattern is observed in the occurrence of the different clusters, with fast westerly and northerly Atlantic flows during winter and weak circulation flows in summer. Spring and fall were characterised by advection of moderate flows from northeastern and eastern Europe. Significant inter-cluster differences were observed for concentrations of receptor aerosol components, with the highest concentrations of EC, OC, SO₄^2?, K⁺ and ²¹⁰Pb associated with local and mesoscale aerosol sources located over central Europe related to enhanced photochemical processes. Emissions produced by fossil fuel and biomass burning processes from the Baltic countries, Byelorussia, western regions of Russia and Kazakhstan in spring and fall also contribute to elevated levels of EC, OC, SO₄^2?, K⁺ and ²¹⁰Pb. In the summer period long-range transport episodes of mineral dust from North-African deserts were also frequently detected, which caused elevated concentrations of coarse Ca²⁺ at sites. The baseline aerosol concentrations in central Europe at the high altitude background sites were registered in winter, with the exception of coarse Na⁺. While the relatively high concentrations of Na⁺ can be explained by sea salt advected from the Atlantic, the low levels of other aerosol components are caused by efficient aerosol scavenging associated to advections of Atlantic air masses, as well as lower emissions of these species over the Atlantic compared to those over the European continent and very limited vertical air mass exchange over the continent.     

Gas/solid partitioning of semivolatile organic compounds (SOCs) to air filters. 2. Partitioning of polychlorinated dibenzodioxins,polychlorinated dibenzofurans,and polycyclic aromatic hydrocarbons to quartz fiber filters

Gas/particle distributions of atmospheric semi-volatile organic compounds (SOCs) are often measured using filter/sorbent samplers. Unfortunately, the adsorption of gaseous SOCs onto a filter can cause positive biases in the measured particle-phase concentrations, and negative biases in the measured gas-phase concentrations. When quartz fiber filters (QFFs) are used, surface-area-normalized gas/quartz partition coefficient (K_p,s, m³ m⁻²) values will be useful when estimating the magnitudes of these errors. Gas/QFF K_p,s values have been reported in the literature only for polycyclic aromatic hydrocarbons (PAHs) and n-alkanes. Gas/QFF K_p,s values were measured here for a series of polychlorinated dibenzodioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs), and also for a range of PAHs. Within each of the three individual compound classes, plots of log K_p,s vs. log p_L^o (sub-cooled liquid vapor pressure) were found to be linear with slopes of approximately −1. At relative humidity (RH)=25%, the pooled log K_p,s data at 25°C for the three compound classes were correlated with log p_L^o nearly as well (r²=0.95) as were the data for the individual compound classes (r²≈0.97). In general, the K_p,s values for the PAHs and PCDD/PCDFs studied were found to be about a factor of 2 larger for partitioning to clean QFFs at RH=25% than for TMFs at RH=21–52%. Backup QFFs used in filter/sorbent sampling in a suburban area yielded K_p,s values for PAHs at RH=37% that were significantly lower than for clean QFFs at the same RH. (This may have been the result of the adsorption of ambient organic compounds that at least partially blocked the direct adsorption of the SOCs to the QFF surface). Therefore, when QFFs are used to separate atmospheric gas- and particle-phase SOCs, corrections for compound-dependent gas adsorption artifacts for QFFs may need to be carried out using K_p,s values that were obtained with ambient backup QFFs.     

Impact of building facades and ground heating on wind flow and pollutant transport in street canyons

This paper investigates the impacts of building facades and ground heating on the wind flow and pollutant transport in street canyons using the computational fluid dynamic (CFD) technique. Street canyons of H/W (H representing the building height and W the street width) varied from 0.1 to 2, which covered the basic flow regimes of skimming flow (H/W=1 or 2), wake interference flow (H/W=0.5), and isolated roughness flow (H/W=0.1), were examined in a series of sensitivity tests. Heating that occurred on different surfaces, including ground surface and building façades, posed considerable effects on the street canyon wind flow and pollutant transport compared with those under isothermal conditions. The CFD results showed that the mechanically induced wind flow and pollutant transport were complicated by the buoyancy under temperature stratification. Individual street canyons of different H/W and surface-heating scenarios exhibited their unique wind flow structure and pollutant transport behaviors. Two counter-rotating vortices were calculated in the street canyons of H/W=1, in which the zone of higher pollutant concentration under isothermal conditions was switched from the leeward side to the windward side. In the street canyon of H/W=2, the recirculating wind pattern was perturbed by surface heating that led to the development of either one primary vortex or three closely coupled vortices. Because of the complicated wind structure, the zones of higher pollutant concentration located either on the leeward or windward ground level were subjected to the surface-heating scenarios. Only two vortices were developed inside the street canyon of H/W=0.5. The large primary vortex, centered inside the street canyon, extended above the roof level of the street canyon. Meanwhile, a small secondary vortex was found at the ground-level windward corner whose size results as a function of surface-heating configurations. Finally, in the street canyon of H/W=0.1, an isolated clockwise-rotating vortex was developed beside the leeward building while the wind in the windward side blew in the prevailing wind direction. As a result, air pollutant emitted at the street centerline was unlikely to be carried into the leeward vortex. Instead, it was dispersed rapidly on the windward side before being removed from the street canyon.     

On the correlation of air and pollutant exchange for street canyons in combined wind-buoyancy-driven flow

The ventilation and pollutant transport in a two-dimensional (2D) street canyon of building-height-to-street-width (aspect) ratio h/b = 1 under different unstable stratifications were examined. To characterize the combined wind-buoyancy-driven flow and pollutant transport at different Richardson number Ri, a computational fluid dynamics (CFD) model based on the Reynolds-averaged Navier–Stokes (RANS) equations with the Renormalization Group (RNG) k ? ε turbulence model was adopted. Unlike the isothermal condition, a secondary recirculation is initiated at the ground-level windward corner of the street canyon once the unstable stratification is switched on (Ri < 0). It traps the ground-level pollutant leading to elevated pollutant concentration there. As Ri further decreases, the enlarging secondary recirculation enables direct pollutant removal from its core to the shear layer that offsets the ground-level pollutant accumulation. The ventilation and pollutant removal performance under different unstable stratifications are compared by the air (ACH) and pollutant (PCH) exchange rates, and pollutant retention time (τ). Both the mean and turbulent components of ACH are found to increase with decreasing Ri, suggesting that unstable stratification promotes ventilation in street canyons. Moreover, the CFD results agree well with our theoretical model that ACH² varies linearly with Ri. Turbulent transport originally dominates the pollutant removal under isothermal condition. However, progressive domination of pollutant removal by mean wind can be observed with decreasing stability (decreasing Ri from 0 to ?10.6). The critical value is estimated to be Ri = ?8, below which mean wind is the major pollutant removal carrier. Reduction in τ is also observed with decreasing Ri. Hence, in unstable stratification, pollutant resides shorter time in the street canyon compared with its isothermal counterpart, and the ventilation and pollutant removal are more favorable.     

Mesoscale modelling of vertical atmospheric transport in the Alps associated with the advection of a tropopause fold – a winter ozone episode

The role of vertical atmospheric transport (VAT) for a winter ozone episode (January 1988) in the Alps, observed both on the mountain crest (3580 m asl) and in the lee of the Alps (209 m asl), is investigated. Numerical simulations were carried out with a doubly nested mesoscale model (14 km horizontal resolution), characterised by a refined orography scheme. A comparison between the modelled vertical profiles with features observed in the aerological soundings over Payerne indicated that the model is able to reproduce the fold in the Alps down to 650 hPa. Frictional processes are found to be responsible for the fragmentation of the lower parts of the fold when it is advected over the mountains, thus enhancing ozone concentrations at the mountain crest with likely cross-tropopause mixing. Vertically propagating gravity waves and strong mesoscale vertical winds (nordfoehn) are responsible for the further downward transport of ozone-rich air to the lower troposphere. This mechanism leads to ozone concentrations up to 70 ppb(v) in the leeside. The study is important because tropospheric ozone trends in the lee of the Alps have been inferred, in the past, from ozone peaks associated with such nordfoehn conditions. It is now shown that nordfoehn may entrain air which has been recently exchanged across the tropopause.     

Air pollution “holiday effect” resulting from the Chinese New Year

Our study was an attempt to conduct a comprehensive and systematical examination of the holiday effect, defined as the difference in air pollutant concentrations between holiday and non-holiday periods. This holiday effect can be applied to other countries with similar national or cultural holidays. Hourly and daily surface measurements of six major air pollutants from thirteen air quality monitoring stations of the Taiwan Environmental Protection Administration during the Chinese New Year (CNY) and non-Chinese New Year (NCNY) periods were used. We documented evidence of a “holiday effect”, where air pollutant concentrations were significantly different between holidays (CNY) and non-holidays (NCNY), in the Taipei metropolitan area over the past thirteen years (1994–2006).The concentrations of NO_x, CO, NMHC, SO₂ and PM₁₀ were lower in the CNY than in the NCNY period, while the variation in the concentration of O₃ was reversed, which was mainly due to the NO titration effect. Similar differences in these six air pollutants between the CNY and NCNY periods were also found in the diurnal cycle and in the interannual variation. For the diurnal cycle, a common traffic-related double-peak variation was observed in the NCNY period, but not in the CNY period. Impacts of dust storms were also observed, especially on SO₂ and PM₁₀ in the CNY period. In the 13-year period of 1994–2006, decreasing trends of NO_x and CO in the NCNY period implied a possible reduction of local emissions. Increasing trends of SO₂ and PM₁₀ in the CNY period, on the other hand, indicated a possible enhancement of long-range transport. These two mechanisms weakened the holiday effect.