Dry deposition and internal circulation of nitrogen,sulphur and base cations to a coniferous forest

The dry deposition of sulphur, nitrogen and base cations to a spruce stand was estimated during a five year period using a surrogate surface resembling needles, throughfall and bulk deposition measurements. The deposition was calculated from the ratio between the deposition of an ion and sodium on the surrogate surface and the net throughfall of sodium to the forest. The dry deposition represented a large fraction of the total atmospheric input of base cations. For Na⁺, Mg²⁺, Ca²⁺, and K⁺ they were 66, 67, 53 and 42%, respectively. The internal circulation was 95% of non-marine net throughfall fro K⁺ and 76% for Ca²⁺. The dry deposition of SO₂ to the canopies regulates the internal circulation of Ca²⁺. The dry deposition of SO₂ to the canopies regulates the internal circulation of Ca²⁺. The dry depositions of ammonium and nitrate are close to the net throughfall of Kjeldahl-N and nitrate, respectively. The obtained deposition velocities are comparable to other studies. The calculated dry deposition of ammonium was compared to the net throughfall of ammonium at three nearby forest stands receiving different ammonium amounts on the soils. No correlation to nitrogen level was found, but most ammonium was lost and converted to organic nitrogen in the canopies of the wettest forest stand.     

Atmospheric deposition and canopy exchange processes in alpine forest ecosystems (northern Italy)

Throughfall and bulk precipitation chemistry were studied for five years (June 1994–May 1999) at two high elevation forest sites (Val Gerola and Val Masino) which were known to differ in terms of tree health, as assessed by live crown condition. The ion concentration of bulk precipitation samples did not differ significantly between sites, except for Mg²⁺, while the throughfall concentrations differed in the measured values of H⁺, N-NO₃⁻, Cl⁻, Na⁺, K⁺, DOC and weak organic acids. The results of the application of the canopy exchange model indicated a higher contribution from the dry deposition of N-NO₃⁻, N-NH₄⁺ and H⁺ at Val Gerola, where the damage symptoms were more evident. In addition, the canopy leaching of Ca²⁺, K⁺ and weak organic acids were 47%, 21% and 27% higher at Val Gerola than at Val Masino. Annual SO₄²⁻ deposition fluxes (21.3 kg ha⁻¹ yr⁻¹ at Val Masino and 23.6 kg ha⁻¹ yr⁻¹ at Val Gerola) were similar to those reported for moderately polluted European and U.S. sites. Annual N loads were 13.6 and 13.1 kg ha⁻¹ yr⁻¹ in the bulk input, and 15.0 and 18.0 kg ha⁻¹ yr⁻¹ in throughfall inputs, at Val Masino and Val Gerola, respectively. The contribution of the organic fraction to the total N atmospheric deposition load is significant, constituting 17% of the bulk flux and 40% of the throughfall flux. Measured nitrogen loads exceed the critical nutrient loads by several kg N ha⁻¹ at both stations. In particular the nitrogen throughfall load at Val Gerola was about 3 times higher than the critical values.     

Elevational patterns of sulfur deposition at a site in the Catskill Mountains,New York

In this paper we report measurements of SO^2-₄ fluxes in throughfall and bulk deposition across an elevational transect from 800 to 1275 m on Slide Mountain in the Catskill Mountains of southeastern New York State. The net throughfall flux of SO^2-₄ (throughfall-bulk deposition), which we attribute to cloud and dry deposition, increased by roughly a factor of 13 across this elevational range. Part of the observed increase results from the year-round exposure of evergreen foliage at the high-elevation sites, compared to the lack of foliage in the dormant season in the deciduous canopies at low elevations. Comparison of the net throughfall flux with estimates of cloud deposition suggests that both cloud deposition and dry deposition increased with elevation. Dry deposition estimates from a nearby monitoring site fall within the measured range of net throughfall flux for SO^2-₄. The between-site variation in net throughfall flux was very high at the high-elevation sites, and less so at the lower sites, suggesting that studies of atmospheric deposition at high-elevations will be complicated by extreme spatial variability in deposition rates. Studies of atmospheric deposition in mountainous areas of the eastern U.S. have often emphasized cloud water deposition, but these results suggest that elevational increases in dry deposition may also be important.     

Research on the impact of forest stand structure on atmospheric deposition

Dry and wet deposition onto thirty forest stands in relation to stand structure is studied by sampling throughfall and bulk precipitation. Nine measurement sites are situated in Pseudotsuga menziesii stands, ten in Pinus sylvestris and eleven in Quercus robur stands. All stands are situated within a radius of 1.2 km to assure a more or less equal air pollution load. In each stand, detailed forest structure inventories are made to determine aerodynamic roughness, collecting efficiency and surface area parameters. Measurements to data cover a four month period (April-July 1990). First results show relatively high throughfall deposition in Pseudotsuga menziesii stands. Lowest throughfall fluxes are recorded for Quercus robur and intermediate values for Pinus sylvestris stands. There are indications of a relatively strong canopy exchange in Quercus robur stands during the measurement period. Many results from forest stand structure inventories are not available yet. However, a strong relation is observed between throughfall deposition in Pseudotsuga menziesii stands and total crown volume.     

Observation of SO2 dry deposition velocity at a high elevation flux tower over an evergreen broadleaf forest in Central Taiwan

A 60-m flux tower was built on a 2100 m mountain for the measurement of the air pollutant concentration and the evaluation of dry deposition velocity in Central Taiwan. The tower was constructed in an evergreen broadleaf forest, which is the dominant species of forest in the world. Multiple-level SO₂ concentrations and meteorological variables at the site were measured from February to April 2008. The results showed that the mean dry deposition velocities of SO₂ were 0.61 cm s^?1 during daytime and 0.27 cm s^?1 during nighttime. From the comparison of the monthly data, a tendency was observed that the dry deposition velocity increases with LAI and solar radiation. Furthermore, it was observed that the deposition velocity was larger over wet canopy than over dry canopy, and that higher deposition velocities in the wet season were mainly caused by non-stomatal uptake of wet canopy. Over wet canopy, the mean dry deposition velocities of SO₂ were estimated to be 0.83 cm s^?1 during daytime and 0.47 cm s^?1 during nighttime; and 0.44 cm s^?1 during daytime and 0.19 cm s^?1 during nighttime over dry canopy. There is good agreement between the results of this study and those in other studies and the predictions of Zhang et al. (2003a). The medians (geometric means) of derived r_c during daytime are 233 (266) m s^?1 over dry canopy and 147 (146) m s^?1 over wet canopy. It was found that solar radiation is the critical important meteorological variable determining stomatal resistance during daytime. For non-stomatal resistance, clear dependencies were observed on the friction velocity and relative humidity.     

Atmospheric deposition and canopy exchange processes in heathland ecosystems

The aims of the present study were to determine canopy exchange processes and to quantify total atmospheric deposition of sulphur and nitrogen in heathland. The study was carried out in dry inland heath vegetation, dominated by Calluna vulgaris, in two nature reserves in the eastern part of the Netherlands. Atmospheric deposition was determined with throughfall-stemflow measurements, adapted for low vegetation. Throughflow measurements (sum of throughfall and stemflow) in artificial Calluna canopies showed co-deposition of SOx and NHy upon heathland vegetation. In the real Calluna canopy, a significant part of the deposited ammonia/ammonium was directly assimilated by the Calluna shoots, especially in wet periods. The concentrations of potassium, calcium and magnesium in throughflow, after passage through the Calluna canopy, increased significantly compared with bulk precipitation. The amount of cations lost from the canopy were in good agreement with the observed ammonium uptake by the Calluna. A field experiment demonstrated that losses of the above-mentioned cations can be doubled by application of ammonium sulphate. It was shown that interception deposition is an important component of the atmospheric deposition of sulphur and nitrogen upon Calluna heathland; bulk precipitation amounted to only c. 35-40% of total atmospheric input. Total atmospheric deposition of sulphur and nitrogen in the investigated heathlands was 1.5-2.1 (27-33 kg S ha(-1) yr(-1)) and 2.1-3.1 kmolc ha(-1) yr(-1) (30-45 kg N ha(-1) yr(-1)), respectively. It is concluded that the present atmospheric nitrogen deposition is a continuous threat for the existence of heathlands in Western Europe.     

Comparison of throughfall and soil solution chemistry between a high-density Corsican pine stand and a naturally regenerated silver birch stand

In Flanders, critical loads for acidification and eutrophication are exceeded in the majority of the forest stands, and many previously nitrogen limited forest ecosystems have become nitrogen saturated. The present study investigates whether a naturally regenerated stand of silver birch (Betula pendula Roth) contributes less to the acidification and eutrophication of the forest soil than a high-density plantation of Corsican pine (Pinus nigra ssp. laricio Maire). Throughfall deposition of inorganic nitrogen was about 3.5 times higher in the Corsican pine stand than in the birch stand. Potassium throughfall deposition was significantly higher under birch due to higher canopy leaching. Magnesium throughfall deposition was significantly higher under the pine canopy due to higher dry deposition. The lower nitrogen throughfall deposition in the birch stand was reflected in a 60% lower nitrate percolation at 1m depth compared with pine. Nitrate soil percolation is linked to losses of aluminium and base cations.     

Dry deposition and foliar leaching of mercury and selected trace elements in deciduous forest throughfall

The estimated annual throughfall deposition flux of Hg in a northern mixed-hardwood forest in the Lake Huron Watershed was 10.5±1.0 μg m⁻² compared to an annual precipitation Hg flux of 8.7±0.5 μg m⁻² (June 1996–June 1997). The source of this additional Hg in throughfall is often attributed to wash-off of dry deposition, but foliar leaching of Hg may also be important. To determine the influence of both dry deposition and foliar leaching of Hg and other elements in throughfall, we measured a suite of trace elements (Hg, Al, Mg, V, Mn, Cu, Zn, As, Rb, Sr, Cd, Ba, La, Ce, and Pb) in throughfall, precipitation, and ambient air samples from a northern mixed-hardwood forest. Based on a multiple linear regression model, dry deposition had the most important influence on Hg, Al, La, Ce, V, As, Cu, Zn, Cd, and Pb fluxes while foliar leaching strongly influenced Mg, Mn, Rb, Sr, and Ba fluxes in net throughfall. The Hg dry deposition flux was estimated using gaseous and aerosol Hg measurements and modeled deposition velocities. The calculated dry deposition flux (∼12–14 μg m⁻²) of Hg to the canopy indicated that atmospheric deposition of Hg could easily account for all of the Hg deposited in net throughfall (1.9±0.1 μg m⁻²). Although there is a large uncertainty associated with these techniques, the modeling estimates indicate that atmospheric Hg may account for all of the Hg deposited in litterfall (11.4±2.8 μg m⁻²).     

Base cation deposition in europe-part I. Model description, results and uncertainties

Deposition of base cations (Na⁺, Mg²⁺, Ca²⁺, K⁺) in Europe was mapped for 1989 with a spatial resolution of 10 x 20 km using the so-called inferential modeling technique. Deposition fields resembled the geographic variability of sources, land-use and climate. Dry deposition constituted on average 45% of the total base cation deposition in Europe. Modeled deposition estimates compared reasonably well with deposition estimates derived from throughfall and bulk-precipitation measurements made at 174 sites scattered over Europe. Using error propagation, the random and systematic error in total deposition for an average grid cell of 10 x 20 km was estimated to equal 35–50% and 25–40%, respectively. Within individual grids a relatively large variability in deposition is expected.     

Long term changes in atmospheric N and S throughfall deposition and effects on soil solution chemistry in a Scots pine forest in the Netherlands

In a Scots pine forest the throughfall deposition and the chemical composition of the soil solution was monitored since 1984. (Inter)national legislation measures led to a reduction of the deposition of nitrogen and sulphur. The deposition of sulphur has decreased by approximately 65%. The total mineral-nitrogen deposition has decreased by ca. 25%, which is mainly due to a reduction in ammonium-N deposition (−40%), since nitrate-N deposition has increased (+50%). The nitrogen concentration in the upper mineral soil solution at 10 cm depth has decreased, leading to an improved nutritional balance, which may result in improved tree vitality. In the drainage water at 90 cm depth the fluxes of NO₃⁻ and SO₄²⁻ have decreased, resulting in a reduced leeching of accompanying base cations, thus preserving nutrients in the ecosystem. It may take still several years, however, before this will meet the prerequisite of a sustainable ecosystem.     

Comparison of forest edge effects on throughfall deposition in different forest types

This study examined the influence of distance to the forest edge, forest type, and time on Cl⁻, SO₄²⁻, NO₃⁻, and NH₄⁺ throughfall deposition in forest edges. The forests were dominated by pedunculate oak, silver birch, or Corsican/Austrian pine, and were situated in two regions of Flanders (Belgium). Along transects, throughfall deposition was monitored at distances of 0-128 m from the forest edge. A repeated-measures analysis demonstrated that time, forest type, and distance to the forest edge significantly influenced throughfall deposition of the ions studied. The effect of distance to the forest edge depended significantly on forest type in the deposition of Cl⁻, SO₄²⁻, and NO₃⁻: the edge effect was significantly greater in pine stands than in deciduous birch and oak stands. This finding supports the possibility of converting pine plantations into oak or birch forests in order to mitigate the input of nitrogen and potentially acidifying deposition.     

Contribution of canopy leaching to sulphate deposition in a Scots pine forest

Radioactive sulphate (35SO4) was applied to the soil below a Scots pine forest on 23 June 1989, and its movement into the canopy and into throughfall and stemflow was measured over 4 months. The specific activity, Bq (mg S)(-1), of the canopy increased monotonically; uptake by current-year (1989) expanding needles was initially twice as fast as by older needles or live twigs. By 10 October the canopy average specific activity was 62 Bq (mg S)(-1). The specific activity of net throughfall (throughfall + stemflow - rain), deduced from measurements from six throughfall collectors, six stemflow collectors and two rain collectors, fell rapidly from 12.6 Bq (mg S)(-1) in late July to <1 Bq (mg S)(-1) in mid-August. The results suggest (assuming rapid equilibration of 35S with sulphate in soil) that root-derived sulphate contributed c. 3% of sulphate in net throughfall and that dry deposition of SO2 and sulphate particles contributed c. 97% of the 0.56 g S m(-2) measured in net throughfall over the period. Simultaneous measurements of SO2 at canopy height and of NH3 above and within the canopy gave mean concentrations of 5.9 and 0.86 microg m(-3), respectively, sufficient to account for the sulphate measured in net throughfall only if codeposition of NH3 and SO2 occurred to canopy surfaces. The large values of specific activity observed in July, however, indicate that throughfall composition may be closely related to recent soil input of sulphate, and that equilibrium cannot be safely assumed. The possibility of a significant contribution of soil-derived sulphate to sulphate deposition in net throughfall cannot be ruled out on the basis of this experiment.     

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.     

Base-cation deposition in Europe—part II. Acid neutralization capacity and contribution to forest nutrition

An assessment was made of the capacity of base cations to neutralize acid deposition and of the contribution of base cation deposition to forest nutrition in Europe. In large parts of southern Europe more than 50% of the potential acid deposition was found counteracted by deposition of non-sea salt Mg²⁺ + Ca²⁺ + K⁺. In central and northwestern Europe, base cation deposition usually amounted to less than 25% of the acid input. Smallest base cation deposition relative to potential acid deposition was found in southern Scandinavia, Denmark, northern Germany and The Netherlands. A similar spatial pattern was found for the neutralization of acid anions in precipitation. Whereas in Scandinavia weathering is the dominant supplier of base cation to forest soils, in eastern and southern Europe, forests mainly rely on atmospheric deposition for the supply of base cations. Using error propagation, the random and systematic error in acid neutralization capacity for an average grid cell of 10 × 20 km was estimated to equal 45–55% and 50–55%, respectively.     

The contribution of ammonia emissions from agriculture to the deposition of acidifying and eutrophying compounds onto forests

In the vicinity of a large ammonia emission area, dry and wet deposition of acidifying and eutrophying compounds onto Douglas Fir forests was studied by sampling throughfall, stemflow and bulk precipitation. Deposition amounts of NH(4)(+) and SO(4)(2-) were recognised to be among the highest of Central Europe, resulting in extremely high inputs of (potential) acid to the forest soils (13.1 kEq ha(-1) year(-1)). The contribution of NH(3) emissions from agriculture to the total acid deposition to the forests was 52%. The total nitrogen deposition amounted to 115.0 kg ha(-1) year(-1), 83% originating from NH(3) emissions and 17% from NO(x) emissions. Calculated mean dry deposition velocities of NH(3) and SO(2) were much larger than reported in the literature. A synergistic effect between NH(3) and SO(2) in the process of dry deposition is suggested and evidence for this effect is discussed. When deposition models do not take this interaction into account, they will underestimate NH(3) and SO(2) deposition amounts in areas with intensive animal husbandry.     

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.     

Effects of canopy-deposition interaction on H+ supply to soils in Pinus banksiana and Populus tremuloides ecosystems in the Athabasca oil sands region in Alberta, Canada

Soil acidification has been of concern in the oil sands region in Alberta due to increased acid deposition. Using the canopy budget model, and accounting for H⁺ canopy leaching by organic acids, we determined sources and sinks of H⁺ in throughfall in jack pine (Pinus banksiana) and trembling aspen (Populus tremuloides) stands in two watersheds from 2006 to 2009. In pine stands, H⁺ deposition was greater in throughfall than in bulk precipitation while the opposite was true in aspen stands. The annual H⁺ interception deposition was 148.8-193.8 and 49.7-70.0 mol_c ha⁻¹ in pine and aspen stands, respectively; while the annual H⁺ canopy leaching was 127.1-128.7 and 0.0-6.0 mol_c ha⁻¹, respectively. The greater H⁺ supply in pine stands was caused by greater interception deposition of SO₄²⁻ and organic acids released from the pine canopy. Such findings have significant implications for establishing critical loads for various ecosystems in the oil sands region.     

Relation between estimated dry deposition and throughfall in a coniferous forest exposed to controlled levels of SO2 and NO2

Throughfall was collected in a Scots pine forest exposed to about 14 microg m(-3) of both SO2 and NO2, and in a control forest with 1 microg m(-3) SO2 and < 1 microg m(-3) NO2. Precipitation was collected in a nearby open field. Collection was performed on an event basis during the whole vegetation period. Exposure was made by an open-air release system during the vegetation period, except during rain and at night. Additional sulfate deposition in the exposed forest (compared to control forest) was nearly equal to dry deposition of sulfur dioxide, as estimated with a stomatal conductance model adapted for the particular forest. It is thus concluded that essentially all of the dry deposited sulfur dioxide is eventually extracted and appears in throughfall-including the fraction that has been deposited through stomata. Attempts to relate net throughfall deposition to dry deposition of sulfate in the control forest were inconclusive, since a minor (10%) uncertainty in the water balance had a major influence on calculated deposition velocity for particulate sulfate. Nitrate throughfall deposition is about half of the open field wet deposition, both for the exposed and control forest. Thus, a long-term exposure with about 14 microg m(-3) NO2 decreased nitrate throughfall deposition.     

Description and evaluation of a model of deposition velocities for routine estimates of air pollutant dry deposition over North America.: Part I: model development

This paper describes the development of a detailed dry deposition model for routine computation of dry deposition velocities of SO₂, O₃, HNO₃ and fine particle SO₄²⁻ across much of North America. Four different dry deposition/surface exchange sub-models have been combined with the current Canadian weather forecast model (Global Environmental Multiscale model) with a 3 h time resolution and a horizontal spatial resolution of 35 km. The present model uses the US Geological Survey North American Land Cover Characteristics data to obtain fourteen different land use and five seasonal categories. The four sub-models used are a multi-layer model for gaseous species over taller canopy land-use types, a big-leaf model for gaseous species over lower canopies (including bare soil and water) and for HNO₃ under all surface types and, two different models for SO₄²⁻, one for tall canopies and the other for short canopies. All necessary parameters for each sub-model, chemical species, land-use and seasonal categories have been selected from available data libraries or from the values reported in the literature. The purpose for developing this model (referred to as the Routine Deposition Model (RDM)), when coupled with air concentration data, is to provide estimates of seasonal dry deposition, which can be combined with wet deposition to produce total deposition estimates. Model theory is discussed in this paper and model sensitivity tests and results will be presented in a companion paper.     

Atmospheric deposition of phthalate esters in a subtropical city

In Chinese cities, air pollution has become a serious and aggravating environmental problem undermining the sustainability of urban ecosystems and the quality of urban life. Bulk atmospheric deposition samples were collected two-weekly, from February 2007 to January 2008, at three representative areas, one suburban and two urbanized, in the subtropical city, Guangzhou, China, to assess the deposition fluxes and seasonal variations of phthalate esters (PAEs). Sixteen PAE congeners in bulk deposition samples were measured and the depositional fluxes of ∑₁₆PAEs ranged from 3.41 to 190 μg m^?2 day^?1, and were highly affected by local anthropogenic activities. The significant relationship between PAEs and particulate depositional fluxes (correlation coefficient R² = 0.72, P < 0.001) showed PAEs are associated primarily with particles. Temporal flux variations of PAEs were influenced by seasonal changes in meteorological parameters, and the deposition fluxes of PAEs were obviously higher in wet season than in dry season. Diisobutyl phthalate (DiBP), Di-n-butyl phthalate (DnBP), and Di(2-ethylhexyl) phthalate (DEHP) dominated the PAE pattern in bulk depositions, which is consistent with a high consumption of the plasticizer market in China. PAE profiles in bulk deposition showed similarities exhibited in both time and space, and a weak increase of high molecular weight PAE (HMW PAE) contribution in the wet season compared to those in the dry season. Average atmospheric deposition fluxes of PAEs in the present study were significantly higher than those from other studies, reflecting strong anthropogenic inputs as a consequence of rapid industrial and urban development in the region.