Wet and dry deposition monitoring in Southeastern Michigan

Wet and dry deposition as collected by a bucket were measured at two sites in southeastern Michigan for two years. The precipitation had an average pH of 4.27 and a SO²⁻₄ to NO⁻₃ ratio of 2.0. Particulate dry deposition velocities of 0.6 cm s⁻¹ for SO²⁻₄ and NO⁻₃ and > 2 cm s⁻¹ for Cl⁻, Ca²⁺, Mg²⁺,Na⁺ and K⁺ were calculated. The ambient particle composition, dry bucket collection and wet deposition were compared at two sites, one urban and the other rural. Higher ambient particle concentrations and dry deposition rates were measured at the urban site than the rural site, indicating the influence of local emissions. However, local emissions had no effect on the wet deposition concentrations. The influence of more distant source regions was examined by separating the precipitation events by wind direction. The events from the south and east had the highest SO²⁻₄ to NO⁻₃ ratios, which corresponded to the areas with the highest sulfur emissions. NO⁻₃ showed no directional dependence.Wet deposition was examined for the effect of storm type and seasonal trends. Contrary to a recent study on Long Island, we found higher concentrations of H⁺, SO²⁻₄ and NH⁺₄ in winter rain compared to snow. The wet deposition concentrations of H⁺, SO²⁻₄, and NH⁺₄ were highest in the summer, while only Na⁺ and Cl⁻ concentrations were highest in the winter, presumably due to winter road salting. The total deposition of acidic ions was highest in the summer and lowest in the winter, due both to lower concentrations and lower precipitation volumes in the winter. The dry deposition as collected by a bucket accounted for 1 % of total H⁺ deposition, 21 % of SO²⁻₄ deposition, 27% of NO⁻₃ deposition, 50% of Cl⁻ deposition and 61 % of Ca²⁺ deposition.     

Role of ammonia chemistry and coarse mode aerosols in global climatological inorganic aerosol distributions

We use an inorganic aerosol thermodynamic equilibrium model in a three-dimensional chemical transport model to understand the roles of ammonia chemistry and natural aerosols on the global distribution of aerosols. The thermodynamic equilibrium model partitions gas-phase precursors among modeled aerosol species self-consistently with ambient relative humidity and natural and anthropogenic aerosol emissions during the 1990s.Model simulations show that accounting for aerosol inorganic thermodynamic equilibrium, ammonia chemistry and dust and sea-salt aerosols improve agreement with observed SO₄, NO₃, and NH₄ aerosols especially at North American sites. This study shows that the presence of sea salt, dust aerosol and ammonia chemistry significantly increases sulfate over polluted continental regions. In all regions and seasons, representation of ammonia chemistry is required to obtain reasonable agreement between modeled and observed sulfate and nitrate concentrations. Observed and modeled correlations of sulfate and nitrate with ammonium confirm that the sulfate and nitrate are strongly coupled with ammonium. SO₄ concentrations over East China peak in winter, while North American SO₄ peaks in summer. Seasonal variations of NO₃ and SO₄ are the same in East China. In North America, the seasonal variation is much stronger for NO₃ than SO₄ and peaks in winter.Natural sea salt and dust aerosol significantly alter the regional distributions of other aerosols in three main ways. First, they increase sulfate formation by 10–70% in polluted areas. Second, they increase modeled nitrate over oceans and reduce nitrate over Northern hemisphere continents. Third, they reduce ammonium formation over oceans and increase ammonium over Northern Hemisphere continents. Comparisons of SO₄, NO₃ and NH₄ deposition between pre-industrial, present, and year 2100 scenarios show that the present NO₃ and NH₄ deposition are twice pre-industrial deposition and present SO₄ deposition is almost five times pre-industrial deposition.     

Deposition of sulphur,nitrogen and acidity in precipitation over Ireland: chemistry,spatial distribution and long-term trends

The chemical composition of pollutant species in precipitation sampled daily or weekly at 10 sites in Ireland for the five-year period, 1994–1998, is presented. Sea salts accounted for 81% of the total ionic concentration. Approximately 50% of the SO₄²⁻ in precipitation was from sea-salt sources. The proportion of sea salts in precipitation decreased sharply eastwards. In contrast, the concentration of NO₃⁻ and the proportion of non-sea-salt SO₄²⁻ increased eastwards reflecting the closer proximity to major emission sources. The mean (mol_c) ratio of SO₄²⁻:NO₃⁻ was 1.6 for all sites, indicating that SO₄²⁻ was the major acid anion.The spatial correlation between SO₄²⁻, NO₃⁻ and NH₄⁺ concentrations in precipitation was statistically significant. The regional trend in NO₃⁻ concentration was best described by linear regression against easting. SO₄²⁻ concentration followed a similar pattern. However, the regression was improved by inclusion of elevation. Inclusion of northing in the regression did not significantly improve any of the relationships except for NH₄⁺, indicating a significant increase in concentrations from northwest to southeast.The spatial distribution of deposition fluxes showed similar gradients increasing from west and southwest to east and northeast. However, the pattern of deposition shows the influence of precipitation volume in determining the overall input. Mean depositions of sulphur and nitrogen in precipitation were ≈30 ktonnes S yr⁻¹ and 48 ktonnes N yr⁻¹ over the five-year period, 1994–1998, for Ireland.Least-squares linear regression analysis indicated a slight decreasing trend in precipitation concentrations for SO₄²⁻ (20%), NO₃⁻ (13%) and H⁺ (24%) and a slight increasing trend for NH₄⁺ (15%), over the period 1991–1998.     

Evaluation of a CMAQ simulation at high resolution over the UK for the calendar year 2003

A comprehensive ‘operational’ evaluation of the performance of the Community Multiscale Air Quality (CMAQ) modelling system version 4.6 was conducted in support of pollution assessment in the UK for the calendar year 2003. The model was run on multiple grids using one-way nests down to a horizontal resolution as fine as 5 km over the whole of the UK. The model performance was evaluated for pollutants with standards and limit values (e.g. O₃, PM₁₀) and species contributing to acidic and nitrogenous deposition (e.g. NH₃, SO₄^2–, NO₃^–, NH₄⁺) against data from operational national monitoring networks. The key performance characteristics of the modelling system were found to be variable according to acceptance criteria and to depend on the type (e.g. urban, rural) and location of the sites, as well as on the time of the year. As regards the techniques that were used for ‘operational’ evaluation, performance generally complied with expected levels and ranged from good (e.g. O₃, SO₄^2–) to moderate (e.g. PM₁₀, NO₃^–). At a few sites low correlations and large standard deviations for some species (e.g. SO₂) suggest that these sites are subject to local factors (e.g. topography, emission sources) that are not well described in the model. Overall, the model tends to over predict O₃ and under predict aerosol species (except SO₄^2–). Discrepancies between predicted and observed concentrations may be due to a variety of intertwined factors, which include inaccuracies in meteorological predictions, chemical boundary conditions, temporal variability in emissions, and uncertainties in the treatment of gas and aerosol chemistry. Further work is thus required to investigate the respective contributions of such factors on the predicted concentrations.     

Simulation of long-range transport of acidic pollutants in East Asia during the Yellow Sand event

The atmospheric chemical process was simulated using the Carbon Bond 4 (CB-4) model, the aqueous-phase chemistry in Regional Acid Deposition Model and the thermodynamic equilibrium relation of aerosols with the emission inventories of the Emission Database for Global Atmospheric Research, the database of China and South Korea and the Mesoscale Model version 2 (MM5) meteorological fields to examine the spatial distributions of the acidic pollutant concentrations in East Asia for the case of the long-lasting Yellow Sand event in April 1998. The present models simulate quite well the observed general trend and the diurnal variation of concentrations of gaseous pollutants, especially for O₃ concentration. However, the model underestimates SO₂ and NO_x concentration but overestimates O₃ concentration largely due to uncertainty in NO_x and VOC emissions. It is found that the simulated gaseous pollutants such as SO₂, NO_x, and NH₃ are not transported far away from the source regions but show significant diurnal variations of their concentrations. However, the daily variations of the concentrations are not significant due to invariant emission rates. On the other hand, concentrations of the transformed pollutants including SO₄²⁻, NH₄⁺, and NO₃⁻ are found to have significant daily variations but little diurnal variations. The model-estimated deposition indicates that dry deposition is largely contributed by gaseous pollutants while wet deposition of pollutants is mainly contributed by the transformed pollutants.     

Current and future emission estimates of exhaust gases and particles from shipping at the largest port in Korea

The emissions of exhaust gases (NO _x , SO₂, VOCs, and CO₂) and particles (e.g., PM) from ships traversing Busan Port in Korea were estimated over three different years (the years 2006, 2008, and 2009). This analysis was performed according to the ship operational modes (“at sea,” “maneuvering,” and “in port”) and ship types based on an activity-based method. The ship emissions for current (base year 2009) and future scenarios (years 2020 and 2050) were also compared. The annual emissions of SO₂, VOCs, PM, and CO₂ were highest (9.6?×?10³, 374, 1.2?×?10³, and 5.6?×?10⁵ ton year^?1, respectively) in 2008. In contrast, the annual NO _x emissions were highest (11.7?×?10³ ton year^?1) in 2006 due mainly to the high NO _x emission factor. The emissions of air pollutants for each ship operational mode differed considerably, with the largest emission observed in “in port” mode. In addition, the largest fraction (approximately 45–67 %) of the emissions of all air pollutants during the study period was emitted from container ships. The future ship emissions of most pollutants (except for SO₂ and PM) in 2020 and 2050 are estimated to be 1.4–1.8 and 4.7–6.1 times higher than those in 2009 (base year), respectively.     

Non-linear response of wet deposition to emissions reduction: A model study

An Eulerian atmospheric model with complex chemistry (Acidic Deposition and Oxidant Model) and a Lagrangian model with linear chemistry (Ontario Ministry of the Environment Trajectory Model) were used to simulate the wet SO₄²⁻ deposition pattern over eastern North America for 16 days during April 1981.The two model results agree reasonably well with each other when the 16 day average values are compared. They also show reasonable agreement with observed data. Having established the ability of the models to predict deposition patterns for 1981 emissions, reduction scenarios with 50% SO_x and 50% SO_x and NO_x of the 1981 emissions were studied through the Eulerian model. Near the heavy emissions area, the reduction in SO₄²⁻ wet deposition is only about 30–40%. In this respect the linear Lagrangian model departs significantly from the Eulerian model. This non-linearity in response is attributed to the role of oxidants in controlling the conversion of SO₂ to SO₄²⁻.     

Sensitivity analyses of factors influencing CMAQ performance for fine particulate nitrate

Improvement of air quality models is required so that they can be utilized to design effective control strategies for fine particulate matter (PM_2.5). The Community Multiscale Air Quality modeling system was applied to the Greater Tokyo Area of Japan in winter 2010 and summer 2011. The model results were compared with observed concentrations of PM_2.5 sulfate (SO₄^2-), nitrate (NO₃^?) and ammonium, and gaseous nitric acid (HNO₃) and ammonia (NH₃). The model approximately reproduced PM_2.5 SO₄^2? concentration, but clearly overestimated PM_2.5 NO₃^? concentration, which was attributed to overestimation of production of ammonium nitrate (NH₄NO₃). This study conducted sensitivity analyses of factors associated with the model performance for PM_2.5 NO₃^? concentration, including temperature and relative humidity, emission of nitrogen oxides, seasonal variation of NH₃ emission, HNO₃ and NH₃ dry deposition velocities, and heterogeneous reaction probability of dinitrogen pentoxide. Change in NH₃ emission directly affected NH₃ concentration, and substantially affected NH₄NO₃ concentration. Higher dry deposition velocities of HNO₃ and NH₃ led to substantial reductions of concentrations of the gaseous species and NH₄NO₃. Because uncertainties in NH₃ emission and dry deposition processes are probably large, these processes may be key factors for improvement of the model performance for PM_2.5 NO₃^?.

Implications: The Community Multiscale Air Quality modeling system clearly overestimated the concentration of fine particulate nitrate in the Greater Tokyo Area of Japan, which was attributed to overestimation of production of ammonium nitrate. Sensitivity analyses were conducted for factors associated with the model performance for nitrate. Ammonia emission and dry deposition of nitric acid and ammonia may be key factors for improvement of the model performance.     

The contribution of dry deposited ammonia and sulphur dioxide to the composition of precipitation from continuously open gauges

A series of experiments using bulk precipitation collectors of the type used in the UK precipitation chemistry network measured the amounts of NH₄⁺, SO₄²⁻ and other ions that could be washed from funnels (diameter 15 cm) exposed to a wide range of NH₃ and SO₂ concentrations over periods from hours to days. In dry conditions, the average deposition flux of NH₃ was between 50 and 120 nmol NH₄⁺ funnel⁻¹ d⁻¹ (0.1–0.3 kg N ha⁻¹ yr⁻¹), and was independent of the concentration of NH₃. Dry deposition of NH₃ to wet funnels at small NH₃ concentrations was almost 5 times that to dry funnels under the same conditions (average 240 nmol funnel⁻¹ d⁻¹; 0.7 kg ha⁻¹ yr⁻¹), and increased with increasing NH₃ concentrations. The amount of NH₄⁺ ions remaining on the funnel surface was inversely proportional to the vapour pressure deficit during the experiment. This result was interpreted as a dependence on the duration of surface wetness, with greater deposition of NH₄⁺ when evaporation rates of surface water were small.The amount of SO₂ deposited on funnel surfaces was closely related to the amount of NH₃ deposited, in both wet and dry conditions, but was not strongly correlated with the SO₂ concentration. At low NH₃ and SO₂ concentrations the average deposition to dry funnels was 70 nmol SO₄²⁻ funnel⁻¹ d⁻¹ (0.5 kg ha⁻¹ yr⁻¹), and to wet funnels was approximately 2.5 times larger. The results are interpreted in terms of the balance between the rate of evaporation of surface water, and the rate of oxidation of SO₂, which leads to the ‘fixing’ of NH₄⁺ ions on the surface as involatile salts.It is predicted that dry deposition of NH₃ to funnel surfaces across the UK Secondary Network could account for as much as one-half of the measured bulk wet deposition at sites where wet deposition of NH₄–N is small. The amount of dry deposition depends on how long and how often funnel surfaces are wetted by rain or dew, and on the air concentrations of NH₃. These predictions are based on funnels being wetted only once per day. More frequent wetting would increase the contribution from dry deposition, and the consequent overestimate of wet deposition of NH₄–N across the UK by using data obtained from bulk collectors. To some extent this overestimate may be offset by microbial degradation and loss of NH₄–N in weekly bulk precipitation samples during collection and storage.     

The water-soluble ionic composition of PM2.5 in Shanghai and Beijing,China

A year-long field study to characterize the ionic species in PM2.5 was carried out in Shanghai and Beijing, China, in 1999–2000. Weekly samples of PM2.5 were collected using a special low flow rate (0.4 l min⁻¹) sampler. In Shanghai, SO₄²⁻ NO₃⁻ and NH₄⁺ were the dominant ionic species, which accounted for 46%, 18% and 17% of the total mass of ions, respectively. Local SO₂ emissions were an important source of SO₄²⁻ in PM2.5 because the SO₄²⁻ concentration was correlated with the SO₂ concentration (r=0.66). The relatively stable SO₄²⁻/SO₂ mass ratio over a large range of temperatures suggests that gas-phase oxidation of SO₂ played a minor role in the formation of SO₄²⁻. The sum of SO₄²⁻ and NO₃⁻ was highly correlated with NH₄⁺ (r=0.96), but insufficient ammonium was present to totally neutralize the aerosol. In Beijing, SO₄²⁻, NO₃⁻ and NH₄⁺ were also the dominant ionic species, constituting 44%, 25% and 16% of the total mass of water-soluble ions, respectively. Local SO₂ emissions were an important source of SO₄²⁻ in the winter since SO₄²⁻ was correlated with SO₂ (r=0.83). The low-mass SO₄²⁻/SO₂ ratio (0.27) during winter, which had low humidity, suggests that gas-phase oxidation of SO₂ was a major route of sulfate formation. In the summer, however, much higher mass ratios of SO₄²⁻/SO₂ (5.6) were observed and were ascribed to in-cloud sulfate formation. The annual average ratio of NO₃⁻/SO₄²⁻ was 0.4 and 0.6 in Shanghai and in Beijing, respectively, suggesting that stationary emissions were still a dominant source in these two cities.     

Spatial distribution of wet deposition of nitrogen in South Korea

A method is developed to estimate wet deposition of nitrogen in a 11×14 km (0.125°Lon.×0.125°Lat.) grid scale using the precipitation chemistry monitored data at 10 sites scattered over South Korea supplemented by the routinely available precipitation rate data at 65 sites and the estimated emissions of NO₂ and NH₃ at each precipitation monitoring site. This approach takes into account the contributions of local NO₂ and NH₃ emissions and precipitation rates on wet deposition of nitrogen. Wet deposition of nitrogen estimated by optimum regression equations for NO₃⁻ and NH₄⁺ derived from annual total monitored wet deposition and that of emissions of NO₂ and NH₃ is incorporated to normalize wet deposition of nitrogen at each precipitation rate class, which is divided into 6 classes. The optimum regression equations for the estimation of wet deposition of nitrogen at precipitation monitoring sites are developed using the normalized wet deposition of nitrogen and the precipitation rate at 10 precipitation chemistry monitoring sites. The estimated average annual total wet depositions of NO₃⁻ and NH₄⁺ are found to be 260 and 500 eq ha⁻¹ yr⁻¹ with the maximum values of 400 and 930 eq ha⁻¹ yr⁻¹, respectively. The annual mean total wet deposition of nitrogen is found to be about 760 eq ha⁻¹ yr⁻¹, of which more than 65% is contributed by wet deposition of ammonium while, the emission of NH₃ is about half of that of NO₂, suggesting the importance of NH₃ emission for wet deposition of nitrogen in South Korea.     

A Comprehensive Inventory of the Ship Traffic Exhaust Emissions in the Baltic Sea from 2006 to 2009

This study addresses the exhaust emissions of CO₂, NO_x, SO_x, CO, and PM_2.5 originated from Baltic Sea shipping in 2006–2009. Numerical results have been computed using the Ship Traffic Emissions Assessment Model. This model is based on the messages of the automatic identification system (AIS), which enable the positioning of ships with a high spatial resolution. The NO_x emissions in 2009 were approximately 7 % higher than in 2006, despite the economic recession. However, the SO_x emissions in 2009 were approximately 14 % lower, when compared to those in 2006, mainly caused by the fuel requirements of the SO_x emission control area (SECA) which became effective in May 2006, but affected also by changes in ship activity. Results are presented on the differential geographic distribution of shipping emissions before (Jan–April 2006) and after (Jan–April 2009) the SECA regulations. The predicted NO_x emissions in 2009 substantially exceeded the emissions in 2006 along major ship routes and at numerous harbors, mostly due to the continuous increase in the number of small vessels that use AIS transmitters. Although the SO_x emissions have been reduced in 2009 in most major ship routes, these have increased in the vicinity of some harbors and on some densely trafficked routes. A seasonal variation of emissions is also presented, as well as the distribution of emissions in terms of vessel flag state, type, and weight.     

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.     

Precision of atmospheric dry deposition data from the Clean Air Status and Trends Network

A collocated, dry deposition sampling program was begun in January 1987 by the US Environmental Protection Agency to provide ongoing estimates of the overall precision of dry deposition and supporting data entering the Clean Air Status and Trends Network (CASTNet) archive. Duplicate sets of dry deposition sampling instruments were installed adjacent to existing instruments and have been operated for various periods at 11 collocated field sites. All sampling and operations were performed using standard CASTNet procedures. The current study documents the bias-corrected precision of CASTNet data based on collocated measurements made at paired sampling sites representative of sites across the network. These precision estimates include the variability for all operations from sampling to data storage in the archive. Precision estimates are provided for hourly, instrumental ozone (O₃) concentration and meteorological measurements, hourly model estimates of deposition velocity (V_d) from collocated measurements of model inputs, hourly O₃ deposition estimates, weekly filter pack determinations of selected atmospheric chemical species, and weekly estimates of V_d and deposition for each monitored filter pack chemical species and O₃.Estimates of variability of weekly pollutant concentrations, expressed as coefficients of variation, depend on chemical species: NO₃⁻∼8.1%; HNO₃∼6.4%; SO₂∼4.3%; NH₄⁺∼3.7%; SO₄²⁻∼2.3%; and O₃∼1.3%. Precision of estimates of weekly V_d from collocated measurements of model inputs also depends on the chemical species: aerosols ∼2.8%; HNO₃∼2.6%; SO₂∼3.0%; and O₃∼2.0%. Corresponding precision of weekly deposition estimates are: NO₃⁻∼8.6%; HNO₃⁻∼5.2%; SO₂∼5.6%; NH₄⁺∼3.9%; SO₄²⁻∼3.5%; and O₃∼3.3%. Precision of weekly concentration, V_d estimates, and deposition estimates are comparable in magnitude and slightly smaller than the corresponding hourly values. Annual precision estimates, although uncertain due to their small sample size in the current study, are consistent with the corresponding weekly values.     

Analysis of emission databases for regional models

General procedures for adapting emission inventories to regional models and for studying the impact of differences in inventories on model predictions are outlined. To illustrate the methods, analysis of two inventories which are still being validated is presented. The inventories together satisfy current requirements for the NCAR regional acid deposition model (RADM). These include anthropogenic emissions of SO₂, sulfate aerosol, NO, NO₂, NH₃ and volatile organic compounds (VOC) in 10 reactivity classes, from United States and Canadian point and area sources on 80-km grid resolutions, for weekend and weekday seasonally representative days on a diurnal basis during the 1980–1982 period. Application of checking procedures, designed by our group to screen for subtle anomalies not identified at previous stages of quality assurance employed by the inventory developers, resulted in adjustments primarily to VOC emissions. Comparisons of the modified inventories, which provide an indication of uncertainties in emissions due to variations in inventory development procedures, revealed differences in the eastern United States total daily emissions to be at most on the order of 5 % for SO_x, and NO_x, 20% for VOC and 85% for NH₃. Studies of the impact of inventory differences on predictions of RADM were conducted for the 22–24 April 1981 period, which was monitored as part of the Oxidation and Scavenging Characteristics of April Rains program. Event total wet sulfate deposition differed by 10% or less while midday O₃ concentrations differed by 1% or less for individual grids over the modeling domain.     

An investigation of the assumptions of linear chemistry and superposition in LRTAP models

Most current LRTAP models assume a linear relationship between sulphur emissions and predicted acidic concentrations, as well as the ability to superpose concentrations from different emission sources. This paper uses a non-linear chemistry model and control scenarios of 50% reductions in S, N and hydrocarbon (HC) emissions to examine the validity of these two assumptions at various downwind receptors. The model predicts that a 50% reduction in S emissions will lead to a 60–65% reduction in SO₂ concentrations and a 25–40% reduction in H₂SO₄ concentrations, depending upon whether or not NO_x and/or HC emissions are reduced by 50% at the same time. The non-linearities in the model predictions are due to complex interactions between NO_x, HC, OH and HO₂. Even when there was non-linearity in the individual S species (SO₂ and SO₄), there was little non-linearity in total airborne S. Adding the results of independent model predictions for different sources (superposition) might introduce errors due to

• 1.(1) chemical interactions between the emissions from the various sources
• 2.(2) overestimates of physical processes such as mixing in of ambient air.

The model was also used to examine trends in regional air quality in eastern North Amierica.     

Ship emissions and their externalities for Greece

The existing and emerging international and European policy framework for the reduction of ship exhaust emissions dictates the need to produce reliable national, regional and global inventories in order to monitor emission trends and consequently provide the necessary support for future policy making. Furthermore, the inventories of ship exhaust emissions constitute the basis upon which their external costs are estimated in an attempt to highlight the economic burden they impose upon the society and facilitate the cost–benefit analysis of the proposed emission abatement technologies, operational measures and market-based instruments prior to their implementation.The case of Greece is of particular interest mainly because the dense ship traffic within the Greek seas directly imposes the impact of its exhaust emission pollutants (NO_x, SO₂ and PM) upon the highly populated, physically sensitive and culturally precious Greek coastline, as well as upon the land and seas of Greece in general, whereas the contribution of Greece in the global CO₂ inventory at a time of climatic change awareness cannot be ignored. In this context, this paper presents the contribution of Greece in ship exhaust emissions of CO₂, NO_x, SO₂ and PM from domestic and international shipping over the last 25 years (1984–2008), utilizing the fuel-based (fuel sales) emission methodology. Furthermore, the ship exhaust emissions generated within the Greek seas and their externalities are estimated for the year 2008, through utilizing the fuel-based (fuel sales) approach for domestic shipping and the activity-based (ship traffic) approach for international shipping.On this basis, it was found that during the 1984 to 2008 period the fuel-based (fuel sales) ship emission inventory for Greece increased at an average annual rate of 2.85%. In 2008, the CO₂, NO_x, SO₂ and PM emissions reached 12.9 million tons (of which 12.4 million tons of CO₂) and their externalities were found to be around 3.1 billion euro. With regard to shipping within the Greek seas, the utilization of the fuel-based (fuel sales) analysis for domestic shipping and the activity-based (ship traffic) analysis for international shipping shows that the ship-generated emissions reached 7.4 million tons (of which 7 million tons of CO₂) and their externalities were estimated at 2.95 billion euro. Finally, the internalization of external costs for domestic shipping was found to produce an increase of 12.96 and 2.71 euro per passenger and transported ton, respectively.     

Wintertime wet and dry deposition in northern Michigan

Wet and dry deposition were monitored at the University of Michigan Biological Station in rural northern Michigan for three winters. Dry deposition was measured by both the conventional bucket method and by measuring increases in concentration in exposed, elevated snow samples. Average results of the two methods were in reasonable agreement. The cumulative wet and dry deposition quantities are in good agreement with snowpack accumulations until the first thaw period. Dry deposition to snow accounts for less than 15% of the total H⁺, SO²⁻₄, NO⁻₃ and NH⁺₄ and approximately 25% of the Ca ²⁺, Mg ²⁺, Na⁺, K⁺ and Cl⁻ during an average precipitation year. Snowpack measurements were also made under deciduous and red pine canopies. Decreases in H⁺ and NO⁻₃ were observed under the red pine canopy.     

The sensitivity of the CHIMERE model to emissions reduction scenarios on air quality in Northern Italy

The sensitivity of the CHIMERE model to emission reduction scenarios on particulate matter PM2.5 and ozone (O₃) in Northern Italy is studied. The emissions of NO_x, PM2.5 SO₂, VOC or NH₃ were reduced by 50% for different source sectors for the Lombardy region, together with 5 additional scenarios to estimate the effect of local measures on improving the air quality for the Po valley area. Firstly, we evaluate the model performance by comparing calculated surface aerosol concentrations for the standard case (no emission reductions) with observations for January and June 2005. Calculated monthly mean PM10 concentrations are in general underestimated. For June, modelled PM10 concentrations slightly overestimate the measurements. Calculated monthly mean SO₄, NO₃^?, NH₄⁺ concentrations are in good agreement with the observations for January and June. Secondly, the model sensitivity of emission reduction scenarios on PM2.5 and O₃ calculated concentrations for the Po valley area is evaluated. The most effective scenarios to abate PM2.5 concentration are based on the SNAP2 (non-industrial combustion plants) and SNAP7 (road traffic) sectors, for which the NO_x and PM2.5 emissions are reduced by 50%. The number of days that the 2015 PM2.5 limit value of 25 μg m^?3 in Milan is exceeded by reducing primary PM2.5 and NO_x emissions for SNAP2 and 7 by 50%, does not change in January when compared to the standard case for the Milan area. It appears that 40% of the PM2.5 concentration in the greater Milan area is caused by the emissions surrounding the Lombardy region and from the model boundary conditions.This study also showed that a more effective pollutant reduction (emissions) per ton of pollutant reduced (concentrations) for the greater Milan area is obtained by reducing the primary PM2.5 emissions for SNAP7 by 50%. The most effective scenario on PM2.5 decrease for which precursor emissions are reduced is achieved by reducing SO₂ emissions by 50% for SNAP7.Our study showed that during summer time, the largest reductions in O₃ concentrations are achieved for SNAP7 emission reductions, when volatile organic compounds (VOCs) are reduced by 50%.     

Major ionic compositions of fine particulate matter in an animal feeding operation facility and its vicinity

Animal feeding operations (AFOs) produce particulate matter (PM) and gaseous pollutants. Investigation of the chemical composition of PM_2.5 inside and in the local vicinity of AFOs can help to understand the impact of the AFO emissions on ambient secondary PM formation. This study was conducted on a commercial egg production farm in North Carolina. Samples of PM_2.5 were collected from five stations, with one located in an egg production house and the other four located in the vicinity of the farm along four wind directions. The major ions of NH₄⁺, Na⁺, K⁺, SO₄^2?, Cl^?, and NO₃^? were analyzed using ion chromatography (IC). In the house, the mostly abundant ions were SO₄^2?, Cl^?, and K⁺. At ambient stations, SO₄^2?, and NH₄⁺ were the two most abundant ions. In the house, NH₄⁺, SO₄^2?, and NO₃^? accounted for only 10% of the PM_2.5 mass; at ambient locations, NH₄⁺, SO₄^2?, and NO₃^? accounted for 36–41% of the PM_2.5 mass. In the house, NH₄⁺ had small seasonal variations indicating that gas-phase NH₃ was not the only major force driving its gas–particle partitioning. At the ambient stations, NH₄⁺ had the highest concentrations in summer. In the house, K⁺, Na⁺, and Cl^? were highly correlated with each other. In ambient locations, SO₄^2? and NH₄⁺ had a strong correlation, whereas in the house, SO₄^2? and NH₄⁺ had a very weak correlation. Ambient temperature and solar radiation were positively correlated with NH₄⁺ and SO₄^2?. This study suggests that secondary PM formation inside the animal house was not an important source of PM_2.5. In the vicinity, NH₃ emissions had greater impact on PM_2.5 formation.

ImplicationsThe chemical composition of PM_2.5 inside and in the local vicinity of AFOs showed the impact of the AFO emissions on ambient secondary PM_2.5 formation, and the fate and transport of air pollutants associated with AFOs. The results may help to manage in-house animal facility air quality, and to develop regional air quality control strategies and policies, especially in animal agriculture-concentrated areas.