Responses of future air quality to emission controls over North Carolina,Part I: Model evaluation for current-year simulations

The prediction of future air quality and its responses to emission control strategies at national and state levels requires a reliable model that can replicate atmospheric observations. In this work, the Mesoscale Model (MM5) and the Community Multiscale Air Quality Modeling (CMAQ) system are applied at a 4-km horizontal grid resolution for four one-month periods, i.e., January, June, July, and August in 2002 to evaluate model performance and compare with that at 12-km. The evaluation shows skills of MM5/CMAQ that are overall consistent with current model performance. The large cold bias in temperature at 1.5 m is likely due to too cold soil initial temperatures and inappropriate snow treatments. The large overprediction in precipitation in July is due likely to too frequent afternoon convective rainfall and/or an overestimation in the rainfall intensity. The normalized mean biases and errors are ?1.6% to 9.1% and 15.3–18.5% in January and ?18.7% to ?5.7% and 13.9–20.6% in July for max 1-h and 8-h O₃ mixing ratios, respectively, and those for 24-h average PM_2.5 concentrations are 8.3–25.9% and 27.6–38.5% in January and ?57.8% to ?45.4% and 46.1–59.3% in July. The large underprediction in PM_2.5 in summer is attributed mainly to overpredicted precipitation, inaccurate emissions, incomplete treatments for secondary organic aerosols, and model difficulties in resolving complex meteorology and geography. While O₃ prediction shows relatively less sensitivity to horizontal grid resolutions, PM_2.5 and its secondary components, visibility indices, and dry and wet deposition show a moderate to high sensitivity. These results have important implications for the regulatory applications of MM5/CMAQ for future air quality attainment.     

Seasonal,Episodic and Targeted Control of Sulfate Deposition

The large differences in seasonal rates of wet sulfate deposition observed at many receptors in eastern North America imply that reducing SO₂ emissions only in the summer half of the year (April-September) would bring about greater annual wet sulfate deposition reductions than reducing emissions by the same amount year-round. Targeting the emission reductions to those source areas which contribute the bulk of summer depositions in ecologically sensitive areas would increase further the gain factor, defined as the ratio of annual fractional deposition decrement to annual fractional emission decrement. In the northeastern U.S., between 10 and 15 rain episodes deposit about 60 percent of the annual wet sulfate; reducing emissions in the dry periods preceding these heavy deposition episodes could further increase the gain factor. However, it is difficult to predict these episodes, and they do not occur simultaneously over large regions of the country.     

A simulation of sulfur wet deposition and its dependence on the inflow of sulfur species to storms

Numerical precipitation scavenging models are used to investigate the relationship between the inflow concentrations of sulfur species to precipitation systems and the resulting sulfur wet deposition. Simulations have been made for summer and winter seasons using concentration ranges of SO₂, aerosol SO₄²⁻, H₂O₂ and O₃ appropriate for the eastern U.S. summer simulations use one-dimensional timedependent convective cloud and scavenging models; winter simulations use two-dimensional steady-state warm-frontal models. Sulfur scavenging mechanisms include nucleation scavenging of aerosol, aqueous reactions of H₂O₂, O₃ and HCHO with S(IV), and nonreactive S(IV) scavenging. Over the wide range of conditions that have been examined, the relation between sulfur inflow and sulfur wet deposition varies from nearly linear to strongly nonlinear. The degree of nonlinearity is most affected by aerosol SO₄²⁻ levels and relative levels of SO₂ vs H₂O₂. Higher aerosol SO₄²⁻ levels (as found in summer) produce a more linear relation. The greatest nonlinearity occurs when SO₂ exceeds H₂O₂. Winter simulations show more nonlinearity than summer simulations.     

Summary of the 1991 EPRI/EPA/DOE SO2 Control Symposium

The 1991 SO₂ Control Symposium was held December 3-6, 1991, in Washington, D.C. The symposium, jointly sponsored by the Electric Power Research Institute (EPRI), the U.S. Environmental Protection Agency (EPA), and the U.S. Department of Energy (DOE), focused attention on recent improvements in conventional sulfur dioxide (SO₂) control technologies, emerging processes, and strategies for complying with the Clean Air Act Amendments of 1990. Its purpose was to provide a forum for the exchange of technical and regulatory information on SO₂ control technology. Over 800 representatives of 20 countries from government, academia, flue gas desulfurization (FGD) process suppliers, equipment manufacturers, engineering firms, and utilities attended. In all, 50 U.S. utilities and 10 utilities in other countries were represented. In 11 technical sessions, a diverse group of speakers presented 111 technical papers on development, operation, and commercialization of wet and dry FGD, Clean Coal Technologies, and combined sulfur dioxide/nitrogen oxides (SO₂/NO_x processes.     

Will PM control undermine China's efforts to reduce soil acidification?

China’s strategies to control acidifying pollutants and particulate matter (PM) may be in conflict for soil acidification abatement. Acidifying pollutant emissions are estimated for 2005 and 2020 with anticipated control policies. PM emissions including base cations (BCs) are evaluated with two scenarios, a base case applying existing policy to 2020, and a control case including anticipated tightened measures. Depositions of sulfur (S), nitrogen (N) and BCs are simulated and their acidification risks are evaluated with critical load (CL). In 2005, the area exceeding CL covered 15.6% of mainland China, with total exceedance of 2.2 Mt S. These values decrease in the base scenario 2020, implying partial recovery from acidification. Under more realistic PM control, the respective estimates are 17.9% and 2.4 Mt S, indicating increased acidification risks due to abatement of acid-neutralizing BCs. China’s anthropogenic PM abatement will have potentially stronger chemical implications for acidification than developed countries.     

Wet and dry deposition of sulfur and nitrogen compounds in Ontario

Measurements have been made of sulfur and nitrogen compounds in precipitation since 1980 and in air since 1981 in Ontario. This paper presents results of the atmospheric deposition measurement program to the end of 1985. As is to be expected from the distribution of emission sources, annual concentrations of SO₄²⁻ andNO₃⁻ in precipitation, and of SO₂,SO₄²⁻ andNO₃⁻ in air are higher in southern Ontario than in northern Ontario. The corresponding distribution pattern for deposition is similar to that of concentration. A wet SO₄²⁻ deposition rate of 20 kg ha¹⁻ y¹⁻, a value considered critical for the acidification of sensitive water bodies, is exceeded in all of central and southern Ontario. On a province-wide basis, sulfur wet deposition is about four times higher than sulfur dry deposition. For nitrogen, wet and dry deposition are more comparable, though the former is still higher. The S- and N-species display different seasonal trends in concentration and deposition reflecting a dependence on meteorological factors, and on the associated chemical transformation rates. On the other hand, year to year variations are small.     

The Impact of Urban and Industrial Emissions on Mesoscale Precipitation Quality

Results from an acid rain field study around the city of Philadelphia are presented. The study involved the sampling of wet deposition at a network of 40 sites within a distance of 60 km from the Delaware River. Emphasis was placed on event-type rain sampling of frontal and primarily nonconvective storms which are responsible for most of the Northeast’s wet deposition. For most storms, meteorological conditions contributed to a predominant southeasterly transport. Since most of the area’s urban and industrial emissions occur along the Delaware River, the Pennsylvania sector of the network was identified as the downwind (target) region; the New Jersey sector was the upwind (control) region. Local emissions appear to impact the deposition of nitrate (NO₃?) which may register increases greater than 200%. It appears that this impact grows with distance from the river suggesting peaks beyond the 60 km boundary of the network. Comparisons with estimates of NO _x emissions reveal that a substantial fraction may be deposited as NO₃? on the mesoscale. The impact of local emissions on total sulfur is less striking; for some storms the sulfur excess is only in the form of dissolved SO₂. Storm-to-storm variabilities in meteorological conditions, emissions, and oxidant availabilities are probable causes of the variability in the magnitude of the local impact.     

Emissions of Sulfur Trioxide from Coal-Fired Power Plants

Abstract

Emissions of sulfur trioxide (SO₃) are a key component of plume opacity and acid deposition. Consequently, these emissions need to be low enough to not cause opacity violations and acid deposition. Generally, a small fraction of sulfur (S) in coal is converted to SO₃ in coal-fired combustion devices such as electric utility boilers. The emissions of SO₃ from such a boiler depend on coal S content, combustion conditions, flue gas characteristics, and air pollution devices being used. It is well known that the catalyst used in the selective catalytic reduction (SCR) technology for nitrogen oxides control oxidizes a small fraction of sulfur dioxide in the flue gas to SO₃. The extent of this oxidation depends on the catalyst formulation and SCR operating conditions. Gas-phase SO₃ and sulfuric acid, on being quenched in plant equipment (e.g., air preheater and wet scrubber), result in fine acidic mist, which can cause increased plume opacity and undesirable emissions. Recently, such effects have been observed at plants firing high-S coal and equipped with SCR systems and wet scrubbers. This paper investigates the factors that affect acidic mist production in coal-fired electric utility boilers and discusses approaches for mitigating emission of this mist.     

Influence of ozone, relative humidity, and flow rate on the deposition and oxidation of sulfur dioxide on yellow sand

To evaluate the influences of O₃, relative humidity (RH), and flow rate on the reaction between yellow sand and SO₂, the SO₂ deposition velocity and the oxidation state of sulfur were investigated by means of exposure experiments in a cylindrical flow reactor. Early in the reaction, the deposition velocity was not influenced by the RH or the presence of O₃; as the reaction progressed, however, the deposition velocity increased in the presence of O₃ and at high humidity. The oxidation of sulfur from S(IV) to S(VI) was also enhanced under these conditions. The amount of sulfur oxidation was positively correlated with the amount of deposited O₃. Furthermore, the SO₂ deposition velocity increased with increasing flow rate. However, changes in the flow rate had no noticeable effect on the amount of SO₂ oxidation.     

Spatial patterns in wet and dry deposition of atmospheric mercury and trace elements in central Illinois,USA

An intensive 1-month atmospheric sampling campaign was conducted concurrently at eight monitoring sites in central Illinois, USA, from June 9 to July 3, 2011 to assess spatial patterns in wet and dry deposition of mercury and other trace elements. Summed wet deposition of mercury ranged from 3.1 to 5.4 μg/m² across sites for the total study period, while summed dry deposition of reactive mercury (gaseous oxidized mercury plus particulate bound mercury) ranged from 0.7 to 1.6 μg/m², with no statistically significant differences found spatially between northern and southern sites. Ratios of summed wet to summed dry mercury deposition across sites ranged from 2.2 to 4.9 indicating that wet deposition of mercury was dominant during the study period. Volume-weighted mean mercury concentrations in precipitation were found to be significantly higher at northern sites, while precipitation depth was significantly higher at southern sites. These results showed that substantial amounts of mercury deposition, especially wet deposition, occurred during the study period relative to typical annual wet deposition levels. Summed wet deposition of anthropogenic trace elements was much higher, compared to summed dry deposition, for sulfur, selenium, and copper, while at some sites summed dry deposition dominated summed wet deposition for lead and zinc. This study highlights that while wet deposition of Hg was dominant during this spring/summer-season study, Hg dry deposition also contributed an important fraction and should be considered for implementation in future Hg deposition monitoring studies.     

A Computer Plot for a High Temperature Psychrometric Chart

This paper presents results of multivariate regression models developed to estimate the properties and cost of U.S. coals washed for varying degrees of sulfur removal using commercially available physical coal preparation processes. The models allow washed coal characteristics to be predicted from information on coal origin, heating value, ash, and sulfur content. The models were developed by first "processing" each of the 710 coals in the U.S. Bureau of Mines (USBM) coal washability data base through a coal preparation plant computer model which optimizes plant performance to achieve a desired washed coal quality. Washability data are adjusted to account for the inefficiencies of coal washing equipment, and the actual coal sizes treated by various plant wash streams. Since different plant designs may be capable of achieving a given level of sulfur removal, three nominal levels of plant complexity (Levels 2, 3, 4) were included to identify the most economical alternative. The washed coal characteristics thus derived were then analyzed using standard statistical techniques to develop regression equations linking washed coal properties and cost to raw coal properties for each of 18 geographical regions encompassing the entire U.S. These regression models are incorporated in the Advanced Utility Simulation Model (AUSM) to estimate the economic potential of coal washing as a sulfur abatement strategy, in conjunction with other options available to coal-fired power plants. Modeling results for Pennsylvania showed that washed coals frequently were selected as part of a cost-effective control strategy, accounting for 10 to 30 percent of the total emissions reduction, and that "local coal" restrictions significantly increase the use of washed coal as an SO₂ control strategy. Hypothetical requirements for mandatory coal cleaning, however, were found to be costly and ineffective.     

Effects of missing seasonal data on estimates of period means of dry and wet deposition

The current study uses resampling to investigate the impacts of cyclic seasonal behavior on 1- and 5-year period means composed from seasonal mean values in the presence of missing data. This is an empirical study using complete years of seasonal monitoring data collected in the eastern US and extracted from the clean air status and trends network (CASTNET) dry and the National Atmospheric Deposition Program/National Trends Network (NADP/NTN) wet deposition data archives. Estimators of period means with missing seasonal data are determined using means of the non-missing values as estimates of the missing data. Estimates are evaluated in terms of 95% inclusion intervals (e.g., estimates are within ±X% of the true value ⩾95% of the time). For dry deposition, missing transition seasons (i.e., spring or fall) usually yield estimates of annual means that are within ±20% of the true annual mean ⩾95% of the time. Missing summers or winters usually have larger impacts on estimates of annual means of dry deposited species than missing transition seasons. A missing summer has the largest impact on estimates of annual means of dry deposition for all constituents, except SO₂, where winter is especially important. For wet deposition, a missing season yields estimates of annual means that are within ±30% of the true annual mean ⩾95% of the time. A missing summer has the largest impact on estimates of annual means of wet deposition for all constituents, except NH₄⁺, where spring and fall are important. A strategy requiring at least 3 years of seasonal representation for three seasons with the fourth season having at least two seasonal values, yields estimates of wet deposition that are within ±17% of the true 5-year means ⩾95% of the time for all species. Corresponding confidence statements for dry deposition results are considerably stronger, with estimates that are within ±10% of the true 5-year mean ⩾95% of the time.     

An assessment of sulfur deposition pathways in Asia

The acid deposition model is developed and applied to assess the sulfur deposition pathways in Asia. Simulations for four seasons are conducted: February, April, August, and October. The predicted results of summer and winter are compared to measured concentration of SO₂, sulfate, and sulfate wet deposition in Japan. Further comparison of sulfate wet deposition to observations in China is made to assess the general performance of the model. The study shows that wet deposition is more important than dry deposition. It is the predominant factor in each of these four months. It is also found that rainout process, compared to washout process, make a larger contribution to sulfate wet deposition in summer and spring than in the dry months, such as October. The total sulfur wet to dry deposition ratio is 1.6 in February, 1.2 in April, 2.9 in August, and 1.9 in October.     

Source attribution for mercury deposition in the contiguous United States: regional difference and seasonal variation

Quantifying the contribution of emission sources responsible for mercury deposition in specific receptor regions helps develop emission control strategies that alleviate the impact on ecosystem and human health. In light of the maximum available control technology (MACT) rules proposed by U.S. Environmental Protection Agency (EPA) and the ongoing intergovernmental negotiation coordinated by United Nations Environmental Programme (UNEP) for mercury, the Community Multiscale Air Quality Modeling System (CMAQ-Hg) was applied to estimate the source contribution in six subregions of the contiguous United States (CONUS). The considered source categories include electric generating units (EGU), iron and steel industry (IRST), other industrial point sources excluding EGU and IRST (OIPM), the remaining anthropogenic sources (RA), natural processes (NAT), and out-of-boundary transport (BC). It is found that, on an annual basis, dry deposition accounts for two-thirds of total annual deposition in CONUS (474 Mg yr(-1)), mainly contributed by reactive gaseous mercury (about 60% of total deposition). The contribution from large point sources can be as high as 75% near the emission sources (< 100 km), indicating that emission reduction may result in direct deposition decrease near the source locations. Out-of-boundary transport contributes from 68% (Northeast) to 91% (West Central) of total deposition. Excluding the contribution from out-of boundary transport, EGU contributes to about 50% of deposition in the Northeast, Southeast, and East Central regions, whereas emissions from natural processes are more important in the Pacific and West Central regions (contributing up to 40% of deposition). This suggests that the implementation of the new EPA MACT standards will significantly benefit only these three regions. Emission speciation is a key factor for local deposition. The source contribution exhibits strong seasonal variation. Deposition is greater in warm seasons due to stronger Hg0 oxidation. However, the contribution from anthropogenic sources is smaller in warm seasons because of larger emissions from natural processes and stronger vertical mixing that facilitates transport.     

Temporal variations and bioaccumulation of heavy metals in different Suaeda salsa marshes of the Yellow River estuary,China

To understand the temporal variations and bioaccumulation of heavy metals in the coastal marshes, the concentrations of heavy metals (Cr, Ni, Pb, and Cu) in the two Suaeda salsa marshes [middle S. salsa marsh (MM) and low S. salsa marsh (LM)] of the Yellow River estuary were determined from May to November in 2008 by in situ sampling and inductively coupled plasma mass spectrometry (ICP-MS) analysis. Results showed that heavy metal concentrations in S. salsa of MM and LM were generally in the order of Cu?>?Cr?>?Pb?>?Ni, while those in sediments fell in the order of Cr?>?Ni?>?Cu?>?Pb. Heavy metal concentrations of S. salsa in MM and LM were different, and significant differences were observed in stems (F?=?4.797, p?=?0.046) and litters (F?=?6.799, p?=?0.026) for Ni. Litter was the main stock of heavy metals, and the allocations of Cr, Ni, and Pb reached 31.25–51.31, 28.49–42.58, and 29.55–66.79 % (in MM) and 36.73–48.60, 41.70–57.87, and 33.30–60.64 % (in LM), respectively. The ratios of roots/leaves (R/L) and roots/stems (R/S) for Cr and Ni in MM were mostly greater than 1, while those ratios in LM were mostly less than 1, indicating that Cr and Ni in S. salsa at LM had greater mobility compared with those at MM. Moreover, the [accumulation factor, AF]_plant of Cr, Ni, Cu, and Pb in LM, especially [AF]_root and [AF]_stem of Cr and [AF]_litter of Ni, was also higher than that in MM. These indicated that S. salsa grown in LM was more suitable for potential biomonitor or phytoremediation of Cr, Ni, Cu, and Pb if intertidal sediments were seriously contaminated with an increase of pollutant loading (especially heavy metals) in the Yellow River estuary. The use of biomonitor (S. salsa) living and growing in LM could yield valuable information not only on the presence of anthropogenic stressors, but, more importantly, on the adverse influence the stressors are having on the environment.     

A diagnostic evaluation of modeled mercury wet depositions in Europe using atmospheric speciated high-resolution observations

This study is part of the Global Mercury Observation System (GMOS), a European FP7 project dedicated to the improvement and validation of mercury models to assist in establishing a global monitoring network and to support political decisions. One key question about the global mercury cycle is the efficiency of its removal out of the atmosphere into other environmental compartments. So far, the evaluation of modeled wet deposition of mercury was difficult because of a lack of long-term measurements of oxidized and elemental mercury. The oxidized mercury species gaseous oxidized mercury (GOM) and particle-bound mercury (PBM) which are found in the atmosphere in typical concentrations of a few to a few tens pg/m³ are the relevant components for the wet deposition of mercury. In this study, the first European long-term dataset of speciated mercury taken at Waldhof/Germany was used to evaluate deposition fields modeled with the chemistry transport model (CTM) Community Multiscale Air Quality (CMAQ) and to analyze the influence of the governing parameters. The influence of the parameters precipitation and atmospheric concentration was evaluated using different input datasets for a variety of CMAQ simulations for the year 2009. It was found that on the basis of daily and weekly measurement data, the bias of modeled depositions could be explained by the bias of precipitation fields and atmospheric concentrations of GOM and PBM. A correction of the modeled wet deposition using observed daily precipitation increased the correlation, on average, from 0.17 to 0.78. An additional correction based on the daily average GOM and PBM concentration lead to a 50 % decrease of the model error for all CMAQ scenarios. Monthly deposition measurements were found to have a too low temporal resolution to adequately analyze model deficiencies in wet deposition processes due to the nonlinear nature of the scavenging process. Moreover, the general overestimation of atmospheric GOM by the CTM in combination with an underestimation of low precipitation events in the meteorological models lead to a good agreement of total annual wet deposition besides the large error in weekly deposition estimates. Moreover, it was found that the current speciation profiles for GOM emissions are the main factor for the overestimation of atmospheric GOM concentrations and might need to be revised in the future. The assumption of zero emissions of GOM lead to an improvement of the mean normalized bias for three-hourly observations of atmospheric GOM from 9.7 to 0.5, Furthermore, the diurnal correlation between model and observation increased from 0.01 to 0.64. This is a strong indicator that GOM is not directly emitted from primary sources but is mainly created by oxidation of GEM.     

Estimates of regional contributions to wet acid deposition in western Massachusetts during the summer of 1984

The General Motors mobile Atmospheric Research Laboratory was situated in rural western Massachusetts in the Berkshire Mountains for 62 days during the summer of 1984. One purpose of this study was to determine the source regions of wet acid deposition for this northeastern U.S. location. First, to apportion the precursors (sulfate, sulfur dioxide and nitrate) to source regions, daily ambient air samples were analyzed for the precursors as well as for tracer species that are associated with particular sources. Factor and trajectory analyses were then used to deduce the contributions of the Midwest and the Northeast to these precursors. Finally, the contribution of the precursors to precipitation acidity was estimated by analyzing the chemical constituents in the rain during seven precipitation events. Averaged over the entire duration of the study, the data show that Northeast sources accounted for about 60% of the precipitation sulfate and nitrate, while Midwest sources accounted for about 30%. The balance (~ 10%) was accounted for by background sulfate. A more useful way of examining the data is according to the type of storm that caused the wet deposition. The site was affected by two basic types of storms: coastal low-pressure systems that traveled up the Atlantic Coast, and cold fronts that approached from the west. During the coastal lowpressure events, the Midwestern contribution to precipitation acidity was zero, as easterly flows from the Atlantic Ocean dominated. The cold front events, however, were all associated with southwesterly flows, and the Midwest contributions exceeded the Northeast contributions. During these events, the average Midwest contribution to precipitation acidity was about 50%. For all events, the ratio of sulfate to nitrate was approximately 2:1 on an equivalent basis. During the coastal lows, the relative nitrate contributions were the highest. It was estimated that particulate sulfate scavenging was responsible for about half of the sulfate in the rain, while the other half was due to in-cloud oxidation of gaseous sulfur dioxide.     

Do We Understand Trends in Atmospheric Sulfur Species?

ABSTRACT

Anomalies appear to exist in our understanding of atmospheric sulfur compounds, specifically as evidenced in the time trends of the different chemical forms of these compounds. Trends determined at a number of locations by several different groups seem to indicate that, responding to emission reductions across North America, the concentration of SO₂ in the atmosphere is declining more rapidly than that of aerosol SO₄ ^2-. A number of possible reasons for this discrepancy are examined, but it is not possible to provide a definitive answer at this stage. The intent is to stimulate debate, because shortcomings in our understanding of the processes involved could have profound implications for the credibility of abatement strategies and policies for both acid deposition and fine particulate matter (PM).     

Long-term relationships between mercury wet deposition and meteorology

Daily-event precipitation samples collected in Underhill, VT from 1995 to 2006 were analyzed for total mercury and results suggest that there were no statistically significant changes in annual mercury wet deposition over time, despite significant emissions reductions in the Northeast United States. Meteorological analysis indicates that mercury deposition has not decreased as transport of emissions from major source regions in the Midwest and East Coast have consistently contributed to the largest observed mercury wet deposition amounts over the period. In contrast, annual volume-weighted mean (VWM) mercury concentration declined slightly over the 12-years, and a significant decrease was observed from CY 2001 to 2006. An increase in the total annual precipitation amount corresponded with the decline in annual VWM mercury concentration. Analysis suggests that the increase in precipitation observed was strongly related to changes in the amount and type of precipitation that fell seasonally, and this departure was attributed to a response in meteorological conditions to climate variability and the El Niño-Southern Oscillation (ENSO) cycle. Increased amounts of rainfall and mixed precipitation (mixture of rainfall and snowfall), particularly in the spring and fall seasons, enhanced annual precipitation amounts and resulted in declining VWM mercury concentrations during these periods. Thus, declines in concentration at the more remote Underhill site appear to be more directly linked to local scale meteorological and climatological variability than to a reduction in emissions of mercury to the atmosphere.     

Dry deposition of particles and canopy exchange: Comparison of wet,bulk and throughfall deposition at five forest sites in Italy

The contribution of dry deposition to the total atmospheric input of acidifying compounds and base cations is of overwhelming importance. Throughfall measurements provide an estimate of the total deposition to forest soils, including dry deposition, but some uncertainties, related to the canopy interaction processes, affect this approach. We compared the concentrations and the fluxes of the main ions determined in wet-only, bulk and throughfall samples collected at five forest sites in Italy. The contribution of coarse particles deposited onto the bulk samplers was of prime importance for base cations, representing on average from 16% to 46% of the bulk deposition. The extent of this dry deposition depended on some geographical features of the sites, such as the distance from the sea and the annual rainfall. The possibility of applying specific bulk/wet ratios to estimate the wet deposition proved to be limited by the temporal variability of these ratios, which must be considered together with the spatial variability. A direct comparison of the dry contribution deriving from the bulk–wet and the throughfall–wet demonstrated that an extensive natural surface (forest canopy) performs better than a small synthetic surface (funnel of the bulk sampler) in collecting dry deposition of SO₄²⁻, NO₃⁻ and Na⁺. The canopy exchange model was applied to both bulk and wet data to estimate the contribution of dry deposition to the total input of base cations, and the uncertainty associated to the model discussed. The exclusive use of bulk data led to a considerable underestimation of base cation dry deposition, which varies among the study sites.