Transport of SO2 and aerosol over the Yellow sea

Aircraft measurements of air pollutants were made to investigate the characteristic features of long-range transport of sulfur compounds over the Yellow Sea for the periods of 26–27 April and 7–10 November in 1998, and 9–11 April and 19 June in 1999, together with aerosol measurements at the Taean background station in Korea. The overall mean concentrations of SO₂, O₃ and aerosol number in the boundary layer for the observation period ranged 0.1–7.4 ppb 32.1–64.1 ppb and 1.0–143.6 cm⁻³, respectively. It was found that the air mass over the Yellow Sea had a character of both the polluted continental air and clean background air, and the sulfur transport was mainly confined in the atmospheric boundary layer. The median of SO₂ concentration within the boundary layer was about 0.1–2.2 ppb. However, on 8 November, 1998, the mean concentrations of SO₂ and aerosol number increased up to 7.4 ppb and 109.5 cm⁻³, respectively, in the boundary layer, whereas O₃ concentration decreased remarkably. This enhanced SO₂ concentration occurred in low level westerly air stream from China to Korea. Aerosol analyses at the downstream site of Taean in Korea showed 2–3 times higher sulfate concentration than that of other sampling days, indicating a significant amount of SO₂ conversion to non sea-salt sulfate during the long-range transport.     

Effect of winds on SO2 and SPM concentrations in Delhi

A study of concentrations of sulfur dioxide (SO₂) and suspended particulate matter (SPM) has been performed in Delhi. The monthly and seasonal variations of concentrations and winds are analyzed. The monthly mean SO₂ concentrations were in the range of 16.15–34.44 μg m⁻³ and showed regular seasonal variations with the highest concentrations in winter and lowest in monsoon season. On the other hand, the monthly mean SPM concentrations reached the highest (465.68 μg m⁻³) in November and the lowest (150.07 μg m⁻³) in August. It was observed that high SO₂ concentrations were generally associated with the wind blowing from WNW–NW directions, and the high SPM concentrations were usually related to the wind blowing from W–NW directions.     

Long-term measurements of SO2 dry deposition over Gansu Province,China

Potassium carbonate sulfation plates, monitored monthly for 11 years from 48 sites in 11 cities in Gansu Province, China, provide a crude estimate of cumulative SO₂ dry depositions. Measured SO₂ dry deposition rates were 1.6–472 mg m⁻² day⁻¹ and had seasonal variations with maxima in winter and minima mainly during summer as a result of higher winter and lower summer SO₂ concentrations. The 11-year monthly average SO₂ dry deposition rates are 23.2–248.97 and 11.7–175.6 mg m⁻² day⁻¹ in the eleven cities in winter and summer, respectively. A monthly average SO₂ deposition velocity was also estimated from 0.06 to 9.72 cm s⁻² in the 11 cities studied with a 11-year average maximum value of about 1.1–2.7 cm s⁻² in April and July and a 11-year average minimum value of about 0.2–1.0 cm s⁻¹ in January. The SO₂ dry deposition velocity also exhibits an increasing with wind speed in basins of less than 500 mm annual precipitation. In contrast, due to influences of the relative humidity in valleys of more than 500 mm annual precipitation, it shows a decreasing trend with wind speed increasing.     

Broadband UV spectroscopy system used for monitoring of SO2 and NO emissions from thermal power plants

A gas monitoring system based on broadband absorption spectroscopic techniques in the ultraviolet region is described and tested. The system was employed in real-time continuous concentration measurements of sulfur dioxide (SO₂) and nitric oxide (NO) from a 220-ton h^?1 circulating fluidized bed (CFB) boiler in Shandong province, China. The emission coefficients (per kg of coal and per kWh of electricity) and the total emission of the two pollutant gases were evaluated. The measurement results showed that the emission concentrations of SO₂ and NO from the CFB boiler fluctuated in the range of 750–1300 mg m^?3 and 100–220 mg m^?3, respectively. Compared with the specified emission standards of air pollutants from thermal power plants in China, the values were generally higher for SO₂ and lower for NO. The relatively high emission concentrations of SO₂ were found to mainly depend on the sulfur content of the fuel and the poor desulfurization efficiency. This study indicates that the broadband UV spectroscopy system is suitable for industrial emission monitoring and pollution control.     

Dilution and aerosol dynamics within a diesel car exhaust plume—CFD simulations of on-road measurement conditions

Vehicle particle emissions are studied extensively because of their health effects, contribution to ambient PM levels and possible impact on climate. The aim of this work was to obtain a better understanding of secondary particle formation and growth in a diluting vehicle exhaust plume using 3-d information of simulations together with measurements. Detailed coupled computational fluid dynamics (CFD) and aerosol dynamics simulations have been conducted for H₂SO₄–H₂O and soot particles based on measurements within a vehicle exhaust plume under real conditions on public roads.Turbulent diffusion of soot and nucleation particles is responsible for the measured decrease of number concentrations within the diesel car exhaust plume and decreases coagulation rates. Particle size distribution measurements at 0.45 and 0.9 m distance to the tailpipe indicate a consistent soot mode (particle diameter D_p∼50 nm) at variable operating conditions. Soot mode number concentrations reached up to 10¹³ m⁻³ depending on operating conditions and mixing.For nucleation particles the simulations showed a strong sensitivity to the spatial dilution pattern, related cooling and exhaust H₂SO_4(g). The highest simulated nucleation rates were about 0.05–0.1 m from the axis of the plume. The simulated particle number concentration pattern is in approximate accordance with measured concentrations, along the jet centreline and 0.45 and 0.9 m from the tailpipe. Although the test car was run with ultralow sulphur fuel, high nucleation particle (D_p⩽15 nm) concentrations (>10¹³ m⁻³) were measured under driving conditions of strong acceleration or the combination of high vehicle speed (>140 km h⁻¹) and high engine rotational speed (>3800 revolutions per minute (rpm)).Strong mixing and cooling caused rapid nucleation immediately behind the tailpipe, so that the highest particle number concentrations were recorded at a distance, x=0.45 m behind the tailpipe. The simulated growth of H₂SO₄–H₂O nucleation particles was unrealistically low compared with measurements. The possible role of low and semi-volatile organic components on the growth processes is discussed. Simulations for simplified H₂SO₄–H₂O–octane–gasoil aerosol resulted in sufficient growth of nucleation particles.     

An analysis of seasonal surface dust aerosol concentrations in the western US (2001–2004): Observations and model predictions

Long-term surface observations indicate that soil dust represents over 30% of the annual fine (particle diameter less than 2.5 μm) particulate mass in many areas of the western US; in spring and summer, it represents an even larger fraction. There are numerous dust-producing playas in the western US, but surface dust aerosol concentrations in this region are also influenced by dust of Asian origin. This study examines the seasonality of surface soil dust concentrations at 15 western US sites using observations from the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network from 2001 to 2004. Average soil concentrations in particulate matter less than 10 μm in diameter (PM₁₀) were lowest in winter and peaked during the summer months at these sites; however, episodic higher-concentration events (>10 μg m⁻³) occurred in the spring, the time of maximum Asian dust transport to the western US. Simulated surface dust concentrations from the Navy Aerosol Analysis and Prediction System (NAAPS) suggested that long-range transport from Asia dominates surface dust concentrations in the western US in the spring, and that, although some long-range transport does occur throughout the year (1–2 μg m⁻³), locally generated dust plays a larger role in the region in summer and fall. However, NAAPS simulated some anomalously high concentrations (>50 μg m⁻³) of local dust in the fall and winter months over portions of the western US. Differences between modeled and observed dust concentrations were attributed to overestimation of total observed soil dust concentrations by the assumptions used to convert IMPROVE measurements into PM₁₀ soil concentrations, lack of inhibition of model dust production in snow-covered regions, and lack of seasonal agricultural sources in the model.     

Production and removal of aerosol in a polluted fog layer: model evaluation and fog effect on PM

A radiation fog physics, gas- and aqueous-phase chemistry model is evaluated against measurements in three sites in the San Joaquin Valley of California (SJV) during the winter of 1995. The measurements include for the first time vertically resolved fog chemical composition measurements. Overall the model is successful in reproducing the fog dynamics as well as the temporal and spatial variability of the fog composition (pH, sulfate, nitrate, and ammonium concentrations) in the area. Sulfate production in the fog layer is relatively slow (1–4 μg m⁻³ per fog episode) compared to the episodes in the early 1980s because of the low SO₂ concentrations in the area and the lack of oxidants inside the fog layer. Sulfate production inside the fog layer is limited by the availability of oxidants in the urban areas of the valley and by SO₂ in the more remote areas. Nitrate is produced in the rural areas of the valley by the heterogeneous reaction of N₂O₅ on fog droplets, but this reaction is of secondary importance for the more polluted urban areas. The gas-phase production of HNO₃ during the daytime is sufficient to balance the nitrate removed during the nighttime fog episodes. Entrainment of air from the layer above the fog provides another source of reactants for the fog layer. Wet removal is one of most important processes inside the fog layer in SJV. We estimate based on the three episodes investigated during IMS95 that a typical fog episode removes 500–2000 μg m⁻² of sulfate, 2500–6500 μg m⁻² of nitrate, and 2000–3500 μg m⁻² of ammonium. For the winter SJV valley the net fog effect corresponds to reductions in ground ambient concentrations of 0.05–0.2 μg m⁻³ for sulfate, 3–6 μg m⁻³ for total nitrate, and 1–3 μg m⁻³ for total ammonium.     

Biases in Clean Air Status and Trends Network filter pack results associated with sampling protocol

Network filter pack sampling protocol changed in 1989 from requiring a week-long daytime sample and a week-long nighttime sample to requiring a single week-long sample per week at each monitoring site. In the current study, single-filter pack weekly results are compared with weekly results aggregated from separate daytime and nighttime weekly filter pack samples collected at the monitoring site located at Egbert, Ontario, Canada. Comparisons of the concentrations resulting from the two sampling protocols for all major chemical species (SO₄²⁻, NO₃⁻, NH₄⁺, HNO₃, and SO₂) show median biases of <5 nmol m⁻³ (0.1 ppb) and median relative biases of <10%. Median relative biases have the same sign for each species, suggesting biases in the same direction. Based on median differences, composite day–night weekly sampler results generally exceed the single-sampler weekly results (in all cases except for the summer nylon filter HNO₃), and the magnitude depends on the constituent and on the season. Examination of seasonal results reveals large discrepancies in some cases, especially during summer. To use Clean Air Status and Trends Network results for trends analyses over time periods encompassing the 1989 protocol change, it may be useful to put all of the data on the same basis of sampler protocol. Algorithms derived from linear regression analyses using paired bootstrap sampling are offered to convert the recent results to the pre-1989 basis; however, they may only be appropriate for sites in the eastern US. Chemical and statistical reasoning suggests that the results of day–night weekly sampling are usually consistent with higher accuracy than single-sampler weekly results. Adjustments are indicated for summer Teflon NO₃ and nylon HNO₃, for summer and fall Teflon NH₄, and for Total SO₂ in each season. Nylon filters are also shown to have variable collection characteristics for SO₂ that are consistent with a humidity effect. A network-wide change in the SO₂ collection and/or retention characteristics of the nylon filters is found in April 1997.     

Size-resolved sulfate and ammonium measurements in marine boundary layer over the North and South Pacific

Marine background levels of non-sea-salt- (nss-) SO₄²⁻ (5.0–9.7 neq m⁻³), NH₄⁺ (2.1–4.4 neq m⁻³) and elemental carbon (EC) (40–80 ngC m⁻³) in aerosol samples were measured over the equatorial and South Pacific during a cruise by the R/V Hakuho-maru from November 2001 to March 2002. High concentrations of nss-SO₄²⁻ (47–94 neq m⁻³), NH₄⁺ (35–94 neq m⁻³) and EC (130–460 ngC m⁻³) were found in the western North Pacific near the coast of the Asian continent under the influence of the Asian winter monsoon. Particle size distributions of ionic components showed that the equivalent concentrations of nss-SO₄²⁻ were balanced with those of NH₄⁺ in the size range of 0.06<D<0.22 μm, whereas the concentration ratios of NH₄⁺ to nss-SO₄²⁻ in the size range of D>0.22 μm were decreased with increase in particle size. We estimated the source contributions of those aerosol components in the marine background air over the equatorial and South Pacific. Biomass burning accounted for the large fraction (80–98% in weight) of EC and the minor fraction (2–4% in weight) of nss-SO₄²⁻. Marine biogenic source accounted for several tens percents of NH₄⁺ and nss-SO₄²⁻. In the accumulation mode, 70% of particle number existed in the size range of 0.1<D<0.2 μm. In the size rage of 0.06<D<0.22 μm, the dominant aerosol component of (NH₄)₂SO₄ would be mainly derived from the marine biogenic sources.     

Influence of air mass trajectories on the chemical composition of precipitation in India

Chemical composition of precipitation was measured with wet-only samplers at a rural site at Bhubaneswar in eastern India during 1997–1998. All rain events were compared with trajectories and precipitation fields from the ECMWF. The pH and ionic concentrations were found to vary systematically with the origin of air and the amount of rainfall along the trajectory. A seasonal cycle for pH was found with a monthly median pH below 5.0 during October–December. The highest monthly median concentration of Ca²⁺ was found in May with 20 μmol l⁻¹ and for SO₄²⁻ in January with 52 μmol l⁻¹. Samples with trajectories within 400 km from Bhubaneswar during the last 5 days were found to have a median pH slightly below 5.0 as an average. These samples also had the highest concentration for all measured ions, indicating large pollution sources within the region. Samples with continental origin showed a decrease of ∼70% in concentration if there had been rain during >50% of the last 5 days compared to rain during <50% of the last 5 days. High concentrations of Na⁺ and Cl⁻ were also found in continental samples. Resuspension of previously deposited sea salt is believed to be the reason. The data were compared with data from three other sites in western India and higher concentrations of almost all ions (NH₄⁺ being the exception) compared to Bhubaneswar were found at the west coast in monsoon samples.     

Absence of trends in relative risk estimates for the association between Black Smoke and daily mortality over a 34 years period in The Netherlands

A major issue in air pollution epidemiology is whether the associations that are found in the statistical analyses on the health effects of air pollution reflect real causal associations of single components or mixtures thereof, or just reflect statistical associations that are mainly the result of the high correlation between the separate components, one of them being the true causal factor.In a previous analysis on the relationship between daily SO₂ levels and daily mortality in The Netherlands [Buringh, E., Fischer, P., Hoek, G., 2000. Is SO₂ a causative factor for the PM-associated mortality risks in The Netherlands? Inhal. Toxicol. 12 (Suppl. 1), 55–60.], it was shown that the statistical significant association between daily variation in SO₂ and daily mortality did not reflect a causal relation. Black Smoke levels in The Netherlands have decreased 4-fold during the 34 years in the period 1972–2006 (annual average from 27 μg m^?3 to 6 μg m^?3). This large decrease in concentrations enabled us to use the same approach for this component as was done earlier for SO₂ to assess whether a decreasing trend in Black Smoke levels in The Netherlands is associated with an increasing trend in mortality relative risks or not.We used daily averaged Black Smoke (BS) data from 1972 to 2006. In the first two decades (1970–1990) only sparse data were available. Based on the availability of the data, we selected data from 1972 to 1974 and from 1982 to 1984 because during these two periods continuous daily measurement series were available. For the later years (1989–2006) data covering the whole of The Netherlands were available, giving a total of 24 years of daily data. Data on daily total mortality counts (excluding external causes), cardiovascular mortality and respiratory mortality for the whole population of The Netherlands were analyzed with regard to daily Black Smoke levels using generalized additive Poisson regression models (GAM). Period specific relative risk estimates were compared and differences in estimates between periods were evaluated.We found no consistent increase in relative risks for daily total and cause-specific mortality over time, despite the decreasing trend in the Black Smoke levels in The Netherlands. Average relative risks for total mortality varied over the different periods from 0.997 per 10 μg m^?3 daily Black Smoke to 1.010 per 10 μg m^?3. Average relative risks for cardiovascular mortality varied from 0.988 per 10 μg m^?3 to 1.010 per 10 μg m^?3 and for respiratory mortality from 1.000 to 1.010 per 10 μg m^?3. For weekly averaged concentrations the average relative risks for total mortality varied over the different periods from 1.004 per 10 μg m^?3 Black Smoke to 1.018 per 10 μg m^?3. Average relative risks for cardiovascular mortality varied from 1.003 per 10 μg m^?3 to 1.016 per 10 μg m^?3 and for respiratory mortality from 1.000 to 1.050 per 10 μg m^?3.The result of our analyses suggests that Black Smoke cannot be excluded as a potential causal agent because relative risks over time show no increasing trend despite the decreasing trend in Black Smoke concentrations.     

Assessment of air quality benefits from national air pollution control policies in China. Part II: Evaluation of air quality predictions and air quality benefits assessment

Following the meteorological evaluation in Part I, this Part II paper presents the statistical evaluation of air quality predictions by the U.S. Environmental Protection Agency (U.S. EPA)’s Community Multi-Scale Air Quality (Models-3/CMAQ) model for the four simulated months in the base year 2005. The surface predictions were evaluated using the Air Pollution Index (API) data published by the China Ministry of Environmental Protection (MEP) for 31 capital cities and daily fine particulate matter (PM_2.5, particles with aerodiameter less than or equal to 2.5 μm) observations of an individual site in Tsinghua University (THU). To overcome the shortage in surface observations, satellite data are used to assess the column predictions including tropospheric nitrogen dioxide (NO₂) column abundance and aerosol optical depth (AOD). The result shows that CMAQ gives reasonably good predictions for the air quality.The air quality improvement that would result from the targeted sulfur dioxide (SO₂) and nitrogen oxides (NO_x) emission controls in China were assessed for the objective year 2010. The results show that the emission controls can lead to significant air quality benefits. SO₂ concentrations in highly polluted areas of East China in 2010 are estimated to be decreased by 30–60% compared to the levels in the 2010 Business-As-Usual (BAU) case. The annual PM_2.5 can also decline by 3–15 μg m^?3 (4–25%) due to the lower SO₂ and sulfate concentrations. If similar controls are implemented for NO_x emissions, NO_x concentrations are estimated to decrease by 30–60% as compared with the 2010 BAU scenario. The annual mean PM_2.5 concentrations will also decline by 2–14 μg m^?3 (3–12%). In addition, the number of ozone (O₃) non-attainment areas in the northern China is projected to be much lower, with the maximum 1-h average O₃ concentrations in the summer reduced by 8–30 ppb.     

Atmospheric concentrations of ammonia and ammonium at an agricultural site in the southeast United States

In this study, we present ∼1 yr (October 1998–September 1999) of 12-hour mean ammonia (NH₃), ammonium (NH₄⁺), hydrochloric acid (HCl), chloride (Cl⁻), nitrate (NO₃⁻), nitric acid (HNO₃), nitrous acid (HONO), sulfate (SO₄²⁻), and sulfur dioxide (SO₂) concentrations measured at an agricultural site in North Carolina's Coastal Plain region. Mean gas concentrations were 0.46, 1.21, 0.54, 5.55, and 4.15 μg m⁻³ for HCl, HNO₃, HONO, NH₃, and SO₂, respectively. Mean aerosol concentrations were 1.44, 1.23, 0.08, and 3.37 μg m⁻³ for NH₄⁺, NO₃⁻, Cl⁻, and SO₄²⁻, respectively. Ammonia, NH₄⁺, HNO₃, and SO₄²⁻ exhibit higher concentrations during the summer, while higher SO₂ concentrations occur during winter. A meteorology-based multivariate regression model using temperature, wind speed, and wind direction explains 76% of the variation in 12-hour mean NH₃ concentrations (n=601). Ammonia concentration increases exponentially with temperature, which explains the majority of variation (54%) in 12-hour mean NH₃ concentrations. Dependence of NH₃ concentration on wind direction suggests a local source influence. Ammonia accounts for >70% of NH_x (NH_x=NH₃+NH₄⁺) during all seasons. Ammonium nitrate and sulfate aerosol formation does not appear to be NH₃ limited. Sulfate is primarily associated ammonium sulfate, rather than bisulfate, except during the winter when the ratio of NO₃⁻–NH₄⁺ is ∼0.66. The annual average NO₃⁻–NH₄⁺ ratio is ∼0.25.     

Evaluation of the DMS flux and its conversion to SO2 over the southern ocean

A total of 16 boundary layer (BL) DMS flux values were derived from flights over the Southern Ocean. DMS flux values were derived from airborne observations recorded during the Aerosol Characterization Experiment (ACE 1). The latitude range covered was 55°S–40°S. The method of evaluation was based on the mass-balance photochemical-modeling (MBPCM) approach. The estimated flux for the above latitude range was 0.4–7.0 μmol m⁻² d⁻¹. The average value from all data analyzed was 2.6±1.8 μmol m⁻² d⁻¹. A comparison of the MBPCM methodology with several other DMS flux methods (e.g., ship and airborne based) revealed reasonably good agreement in some cases and significant disagreement in other cases. Considering the limited number of cases compared and the fact that conditions for the comparisons were far from ideal, it is not possible to conclude that major agreement or differences have been established between these methods. A major result from this study was the finding that DMS oxidation is a major source of BL SO₂ over the Southern Ocean. Model simulations suggest that, on average, the conversion efficiency is 0.7 or higher, given a lifetime for SO₂ of ∼1 d. A comparison of two sulfur case studies, one based on DMS–SO₂ data generated on the NCAR C-130 aircraft, the other based on data recorded on the NOAA ship Discoverer, revealed qualitative agreement in finding that DMS was a major source of Southern Ocean SO_2. On the other hand, significant disagreement was found regarding the DMS/SO₂ conversion efficiency (e.g., 0.3–0.5 versus 0.7–0.9). Although yet unknown factors, such as vertical mixing, may be involved in reducing the level of disagreement, it does appear at this time that some significant portion of this difference may be related to systematic differences in the two different techniques employed to measure SO₂. It would seem prudent, therefore, that further instrument intercomparison SO₂ studies be considered. It also would be desirable to stage new intercomparison activity between the MBPCM flux approach and the air-to-sea gradient as well as other flux methods, but under far more favorable conditions.     

Transport and evolution of a winter-time Yellow sand observed in Korea

Long-range transport of mineral dust such as Yellow sand (YS) is not restricted to the springtime periods in Northeast Asia. A YS phenomenon was observed during 25–27 January 1999, which was a remarkably distinctive episode in the occurrence time and intensity that had ever observed in the wintertime in Korea. This YS event was traced to be originated from the arid region of central and eastern Asia; the Gobi desert and Loess plateau. The traveling speed of the dust storm was found to be about 70 km h⁻¹ with it's horizontal size of larger than the whole Korean peninsula during this episode. Aerosol mass loadings changed by an order of magnitude within a few hours. The dominant ion components were SO₄²⁻, NO₃⁻, Ca²⁺ and Na⁺ during the passage of YS. The mode diameter of these compounds of YS was around 4 μm, compared to 0.4–0.9 μm after the passage of YS. SO₄²⁻ and NO₃⁻ concentrations were found to be well correlated with Ca²⁺ concentration in the coarse mode during the YS event, whereas they were well correlated with NH₄⁺ concentration during the non-YS period, indicating a significant amount of SO₄²⁻ and NO₃⁻ formations on the Ca²⁺-rich coarse aerosol during the long-range transport of YS.     

Seasonal variations of acidic air pollutants in Seoul,South Korea

The annular denuder system (ADS) was used to characterize seasonal variations of acidic air pollutants in Seoul, South Korea. Fifty- four 24 h samples were collected over four seasons from October 1996 to September 1997. The annual mean concentrations of HNO₃, HNO₂, SO₂ and NH₃ in the gas phase were 1.09, 4.51, 17.3 and 4.34 μg m^-3, respectively. The annual mean concentrations of PM_2.5(d_p≤2.5 μm in aerodynamic diameter, 50% cutoff), SO^2-₄, NO^-₃ and NH⁺₄ in the particulate phase were 56.9, 8.70, 5.97 and 4.19 μg m^-3, respectively. All chemical species monitored from this study showed statistical seasonal variations. Nitric acid (HNO₃) and ammonia (NH₃) exhibited substantially higher concentrations during the summer, while nitrous acid (HNO₂) and sulfur dioxide(SO₂) were higher during the winter. Concentrations of PM_2.5, SO^2-₄, NO^-₃ and NH⁺₄ in the particulate phase were higher during the winter months. SO^2-₄, NO^-₃ and NH⁺₄ accounted for 26–38% of PM_2.5. High correlations were found among PM_2.5, SO^2-₄, NO^-₃ and NH⁺₄. The mean H⁺ concentration measured only in the fall was 5.19 nmole m^-3.     

Chemical and strontium isotope characterization of rainwater in Beijing,China

Major ion concentrations and Sr isotope ratios (⁸⁷Sr/⁸⁶Sr) were measured in rainwater samples collected at an urban site in Beijing over a period of one year. The pH value and major ion concentrations of samples varied considerably, and about 50% of the rainwater studied here were acidic rain with pH values less than 5.0. Ca²⁺ and NH₄⁺ were the dominant cations in rainwaters and their volume weighted mean (VWM) values were 608 μeq l^?1 (14–1781 μeq l^?1) and 186 μeq l^?1 (48–672 μeq l^?1), respectively. SO₄^2? was the predominant anion with VWM value of 316 μeq l^?1 (65–987 μeq l^?1), next was NO₃^? with VWM value of 109 μeq l^?1 (30–382 μeq l^?1).Using Na as an indicator of marine origin, and Al for the terrestrial inputs, the proportions of sea salt and terrestrial elements were estimated from elemental ratios. More than 99% of Ca²⁺ and 98% of SO₄^2? in rainwater samples are non-sea-salt origin. The ⁸⁷Sr/⁸⁶Sr ratios were used to characterize the different sources based on the data sets of this study and those from literatures. Such sources include sea salts (⁸⁷Sr/⁸⁶Sr～0.90917), soluble soil dust minerals originating from either local or the desert and loess areas (～0.7111), and anthropogenic sources (fertilizers, coal combustion and automobile exhausts). The high concentrations of alkaline ions (mainly Ca²⁺) in Beijing atmosphere have played an important role to neutralize the acidity of rainwater. However, it is worth noting that there is a remarkable acidification trend of rainwater in Beijing recent years.     

PM2.5–10, PM2.5 and associated water-soluble inorganic species at a coastal urban site in the metropolitan region of Rio de Janeiro

The concentrations of PM_2.5−10, PM_2.5 and associated water-soluble inorganic species (WSIS) were determined in a coastal site of the metropolitan region of Rio de Janeiro, Southeastern Brazil, from October 1998 to September 1999 (n=50). Samples were dissolved in water and analyzed for major inorganic ions. The mean (± standard deviation; median) concentrations of PM_2.5−10 and PM_2.5 were, respectively, 26 (± 16; 21) μg m⁻³ and 17 (± 13; 14) μg m⁻³. Their mean concentrations were 1.7–1.8 times higher in dry season (May–October) than in rainy season (November–April). The WSIS comprised, respectively, 34% and 28% of the PM_2.5−10 and PM_2.5 masses. Chloride, Na⁺ and Mg²⁺ were the predominant ions in PM_2.5−10, indicating a significant influence of sea-salt aerosols. In PM_2.5, SO₄²⁻ (∼97% nss-SO₄²⁻) and NH₄⁺ were the most abundant ions and their equivalent concentration ratio (SO₄²⁻/NH₄⁺ ∼1.0) suggests that they were present as (NH₄)₂SO₄ particles. The mean concentration of (NH₄)₂SO₄ was 3.4 μg m⁻³. The mean equivalent PM_2.5 NO₃⁻ concentration was eight times smaller than those of SO₄²⁻ and NH₄⁺. The PM_2.5 NO₃⁻ concentration in dry season was three times higher than in rainy season, probably due to reaction of NaCl (sea salt) with HNO₃ as a result of higher levels of NO_y during the dry season and/or reduced volatilization of NH₄NO₃ due to lower wintertime temperature. Chloride depletion was observed in both size ranges, although more pronouncely in PM_2.5.     

Application of a Lagrangian particle model to assess the impact of harbour,industrial and urban activities on air quality in the Taranto area,Italy

This paper evaluates the relative impact on air quality of harbour emissions, with respect to other emission sources located in the same area. The impact assessment study was conducted in the city of Taranto, Italy. This area was considered as representative of a typical Mediterranean harbour region, where shipping, industries and urban activities co-exist at a short distance, producing an ideal case to study the interaction among these different sources. Chemical and meteorological field campaigns were carried out to provide data to this study. An emission inventory has been developed taking into account industrial sources, traffic, domestic heating, fugitive and harbour emissions. A 3D Lagrangian particle dispersion model (SPRAY) has then been applied to the study area using reconstructed meteorological fields calculated by the diagnostic meteorological model MINERVE. 3D short term hourly concentrations have been computed for both all and specific sources. Industrial activities are found to be the main contributor to SO₂. Industry and traffic emissions are mainly responsible for NO_x simulated concentrations. CO concentrations are found to be mainly related to traffic emissions, while primary PM₁₀ simulated concentrations tend to be linked to industrial and fugitive emissions. Contributions of harbour activities to the seasonal average concentrations of SO₂ and NO_x are predicted to be up to 5 and 30 μg m⁻³, respectively to be compared to a overall peak values of 60 μg m⁻³ for SO₂ and 70 μg m⁻³ for NO_x. At selected urban monitoring stations, SO₂ and NO_x average source contributions are predicted to be both of about 9% from harbour activities, while 87% and 41% respectively of total concentrations are predicted to be of industrial origin.     

A simple technique for measuring power station SO2 and NO2 emissions

Emissions of SO₂ and NO₂ from fossil fuel power stations can have serious environmental consequences via conversion to sulphuric and nitric acids and subsequent deposition. Consequently, there is considerable interest in techniques capable of monitoring these emissions, in order to ensure compliance with environmental legislation. Here we present a novel approach to measuring power station SO₂ and NO₂ emissions by traversing underneath the plume by car or on-foot or scanning the power station's plume from a fixed position with a compact and lightweight UV spectrometer. This work was performed at a power station in eastern England during January, February and June 2003, resulting in a SO₂ flux of 5.2 kg s⁻¹, which is in close correspondence with the in-stack measured value of 5.3 kg s⁻¹. This technique is considerably simpler and cheaper than other remote sensing approaches to monitoring these emissions.