The effects of atmospheric nitrogen deposition on the soil chemistry of coniferous forests in The Netherlands

Nitrogen fluxes, particularly those of ammonium, are extremely high in Dutch forests. In soils exposed to high ammonium deposition, acidification, eutrophication or a combination of both processes may occur. In addition to the amounts of ammonium deposited, the rate of soil nitrification determines which process takes place. A nation-wide investigation, in which three coniferous tree species were involved, was carried out to study the relation between deposition fluxes, measured by means of throughfall and bulk samplers, and the chemical composition of the soil. The ammonium deposition accounted directly for the high ammonium content and the high ammonium/cation ratios in the soil. In the top layer of most of the forest soils which were investigated nitrification rates were low. In these stands ammonium/cation ratios in the soil often reflected ammonium/cation ratios in throughfall water. Even in soils with relatively high nitrification rates, ammonium concentrations exceeded those of nitrate in the top layer of the mineral soil, indicating that ammonium deposition was more important than nitrification rate in determining the predominant form of nitrogen.     

Deposition to forests in Europe: most important factors influencing dry deposition and models used for generalisation

Dry deposition of gases and particles to forests is influenced by factors influencing the turbulent transport, such as wind speed, tree height, canopy closure, LAI, etc. as well as by factors influencing surface condition, such as precipitation, relative humidity, global radiation, etc. In this paper, an overview of these factors is given and it is shown which are the most important determining temporal and spatial variation of dry deposition of sodium and sulphur. Furthermore, it is evaluated how well current deposition models are able to describe the temporal and spatial variation in dry deposition. It is concluded that the temporal variation is not modelled well enough, because of limited surface-wetness exchange parameterisations. The influence of forest characteristics are modelled reasonably well, provided enough data describing the forests and the spatial variation in concentration is available. For Europe these data are not available. The means to decrease the atmospheric deposition through forest management is discussed.     

An experimental study of the dry deposition of gaseous nitric acid to snow

A chamber placed in a constant temperature freezing room was used to study the surface resistance during deposition of HNO₃ to a snow surface. The resistance decreased with increasing temperature from larger than 5 s mm⁻¹ at − 18°C to about l s mm⁻¹ at −3°C. Measurements of gaseous and particulate nitrate concentrations during winter at a rural site in south central Sweden gave concentrations in the range of 0.4–5 μg HNO₃ m⁻¹ and 0.3–3 μg NO⁻₃ m⁻³ with a mean value of 1.3 μg HNO₃ m⁻³ and 0.7 μg NO⁻₃ m⁻³, respectively. The results indicate that for periods with temperatures below − 2°C estimated dry deposition of HNO₃ to snow is at most 4 % of measured wet deposition of nitrate in the area.     

Dry deposition of sulfur dioxide or nitric acid to oak, elm and pine leaves

To improve our knowledge of atmospheric inputs to forests, experiments were performed in the field to measure the dry deposition of SO2 and HNO3 to oak, elm, and pine leaves. A tree branch was enclosed in a Teflon chamber, through which SO2 or HNO3 flowed. The dry deposition characteristics of SO2 and HNO3 were very different. The SO2 deposition occurred primarily through stomatal openings for the oak and pine leaves, and equal stomatal and cuticular deposition was observed for the elm leaves. The deposited SO2 could not be removed from the branch by extracting in water or by revolatilization. In contrast, over 90% of HNO3 dry deposition occurred to the cuticle. Most of the deposited HNO3 could be extracted from the leaves. Revolatilization of HNO3 was negligible from an active branch, but increased from a dormant or detached branch. A deposition velocity was derived from the ratio of the flux of the gas to the leaves and the gas concentration in the chamber. Deposition velocities ranged from 0.02 to 0.11 cm s(-1) for SO2 and from 0.2 to 1.2 cm s(-1) for HNO3 to individual leaf surfaces.     

An experimental investigation of some methods of estimating turbulence parameters for use in dispersion models

The standard deviations of wind fluctuations in the horizontal and vertical directions, σ_θ and σ_φ, are now used in some pollution dispersion models to estimate the plume spread parameters σ_y and σ_z. Methods exist for estimating σ_θ and σ_φ when direct measurements are unavailable, using routine weather observations or wind measurements and temperature profiles from meteorological towers. In this paper such estimates are compared with direct measurements made at a height of 56 m, for a sampling time of 1 h, for a range of meteorological conditions. The work was carried out at a site in relatively irregular terrain. This was flat to rolling with a mixed surface cover within 1 km of the tower, with hills rising beyond that distance. Profile measurements were made with robust instruments rather than research grade sensors.Estimates of σ_φ made during the daytime agreed well with measurements, with a bias in the estimates of less than 0.4°. The r.m.s. differences between estimates and measurements were 1.1° (profile method) and less than 2° (routine weather observations method). Daytime σ_θ estimates were generally too low (bias 5–6°), although they were positively correlated with the measurements. At night σ_θ, was severely underestimated, and σ_φ was also underestimated.     

Measurement of the dry deposition flux of NH3 on to coniferous forest

The dry deposition flux of NH3 to coniferous forest was determined by the micrometeorological gradient method using a 36 m high tower. Aerodynamic characteristics of the site were studied, using a second tower erected in the forest 100 m from the first. Fluxes and gradients of heat and momentum measured on both towers indicated a fairly homogeneous turbulent flow field over the studied area of the forest. Site specific flux profile functions for heat were derived from continuous measurements of turbulent fluxes and gradients. These functions were used to derive fluxes from the observed gradients of NH3. In total, eighty 90-min NH3 flux runs were performed. The results indicate a strong nonstomatal uptake of NH3 by the forest. A representative dry deposition velocity for NH3 of 3.6 cm(-1) s was derived. The annual average flux was roughly estimated to be equivalent to 50 kg N ha(-1) yr, significantly higher than the critical load for coniferous forest.     

Measurements and modelling of cloudwater deposition to moorland and forests

The objective of the study was to measure the size dependence of cloudwater deposition and associated average ionic fluxes to vegetated surfaces. Measurements were made over a forest canopy at Dunslair heights in south Scotland and a moorland site, Great Dun Fell, in northern England. Measurements were made using the gradient and eddy correlation techniques. Eddy correlation measurements were made using an ultrasonic anemometer, a Knollenberg forward scattering spectrometer probe (to measure liquid water fluxes and fluxes of droplets in 1 microm size intervals) and a GSI particulate volume monitor (to measure liquid-water fluxes). Measurements were made at Great Dun Fell of the size dependence of droplet deposition velocity, using the gradient technique with two Knollenberg probes. Simultaneous gradient and eddy correlation measurements were also made at Great Dun Fell of average cloud-water fluxes, together with chemical analysis of cloud water composition, using a continuous analysis system. At Dunslair Heights, eddy correlation measurements were made using both the Knollenberg and Gerber Scientific Instruments (GSI) probes, while simultaneous gradient measurements using two GSI probes were also attempted. Samples of cloud water were collected at Dunslair Heights, using passive string collectors for chemical analysis by ion chromatography. The major findings of the study were: 1. The droplet deposition velocities measured by the two techniques were similar. 2. The deposition velocities were a strong function of droplet size. Considerable resistance to deposition was evident for droplets of less than 5 microm radius. Deposition velocities for particles from about 6 to 8 microm exceeded those for momentum. 3. Except when the droplets were very small or the winds very light, bulk cloud-water deposition velocities were about 80% or more of the momentum deposition velocities to forests.     

A laboratory investigation of the routes of HNO3 dry deposition to coniferous seedlings

White pine, Norway spruce and red spruce seedlings were exposed to nitric acid vapor concentrations of 10 to 120 ppb in constant stirred tank reactors. Nitric acid dry deposition rates were determined from both the change in nitric acid concentration in the reactor flow stream and from the amount of nitrogen recovered from the seedlings. Nitric acid labeled with 15N was used to distinguish dry-deposited nitrogen in the plant from the nitrogen that was already present. It was found that dry deposition occurs via three routes: surface deposition, trans-cuticular deposition, and stomatal deposition. Resistance to surface deposition is very low (< 4.8 m2-s mol(-1)) for a freshly washed surface, but increases as the surface adsorption sites are occupied. Resistance to trans-cuticular uptake averaged 206 m2-s mol(-1). Stomatal resistance can be calculated from the rate of water diffusion out of the plant. Eighty per cent of the nitric acid deposited via the trans-cuticular and stomatal routes was assimilated by the plant. However, none of the nitric acid deposited on the surface was assimilated. In rural areas with coniferous forests, the combination of low ambient nitric acid concentrations and low initial surface resistance means that most nitric acid will be dry deposited on the tree surface, and thus will not be directly assimilated.     

A review of models for estimating terrestrial ecological receptor exposure to chemical contaminants

In instances where empirical measurements are not practicable, ecological risk assessments may rely on site-specific exposure models for estimating uptake of chemical contaminants. This paper presents, based on a review of the literature, a compilation of relatively simple quantitative models that can be combined to produce site- and species-specific first-order estimates of uptake of chemicals from abiotic media. These models have proved useful in providing order-of-magnitude estimates for screening and sample program design purposes. This paper intended as both a practical guide for choosing models to estimate terrestrial wildlife exposures and as a step toward development of a more comprehensive and standard approach to exposure assessment in terrestrial ecological receptors.     

Atmospheric concentrations and the deposition velocity to snow of nitric acid,sulfur dioxide and various particulate species

A study of deposition velocities to snow was conducted during the 1982–1983 and 1983–1984 winters at the University of Michigan Biological Station in northern Michigan. Weekly measurements were made of dry deposition rates to snow and the atmospheric concentrations of the depositing species. SO₂, with an average concentration of 2.2 ppb, was the dominant atmospheric sulfur containing species. NO₂, with an average concentration of 1.8 ppb, was the dominant atmospheric nitrogenous species. NO⁻₃ deposition was due primarily to HNO₃, which averaged 0.2 ppb. The HNO₃ deposition velocity averaged 1.4cm s⁻¹. The SO₂ deposition velocity varied with temperature, averaging 0.15 cm s⁻¹ for samples with appreciable exposure time above − 3°C, and 0.06 cm s⁻¹ for samples which remained below an ambient temperature of −3°C. Deposition velocities of Ca²⁺, Mg²⁺ , Na⁺, K⁺ and NH⁺₄ were 2.1, 1.5, 0.44, 0.51 and 0.10cm s⁻¹, respectively. The mass median diameters of these species were 4.4, 2.7, 1.8, 0.9 and 0.46 μm, respectively.     

The surface radiative forcing of nitric acid for northern mid-latitudes

Ground-based, high-resolution measurements of downward atmospheric thermal emission spectra are reported for a northern mid-latitude location for summer and winter conditions. These measurements clearly show the presence of the 11.3-μm thermal emission band of nitric acid situated between 850–920 cm⁻¹. By using the FASCOD3 line-by-line radiation code to simulate the background thermal emission, the measured seasonally averaged surface radiative forcing due to nitric acid is determined to be 0.055 W m⁻²±15%. The zenith column amounts of nitric acid are found to vary between 7.9×10¹⁵ and 1.1×10¹⁶ molecules cm⁻²±15%. An estimation is made of the contribution of nitric acid to the direct radiative forcing of the Earth's surface since pre-industrial times for northern mid-latitudes. This work suggests that nitric acid may play a role that is comparable to that of other greenhouse gases, such as CFC-11, in the forcing of the Earth's climate system. Under polluted conditions, nitric acid may contribute about half of the radiative forcing that is currently associated with tropospheric ozone.     

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.     

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.     

Changed vegetation composition in coniferous forests near to motorways in Southern Germany: the effects of traffic-born pollution

To estimate the effect of traffic emissions on the vegetation composition of coniferous forests near to motorways, three transects of 520 m length were studied by analysing vegetation composition, soil parameters and deposition data in the Munich-area, Southern Germany. The detected patterns suggest that motorways have an impact on the vegetation composition in the neighbourhood of roads. Depending on the wind direction, the influences of the motorways reaches up to 230 m on downwind side and up to 80 m on upwind side. The vegetation is mainly affected by the deposition of nitrogen deriving from fuel combustion and by basic substances added to road salt. By monitoring vegetation changes near to motorways, it is possible to estimate the areas where harmful alterations of the ecosystem can be expected.     

Dry deposition of ammonia,nitric acid,ammonium, and nitrate to alpine tundra at Niwot Ridge,Colorado

Micrometeorological measurements and ambient air samples, analyzed for concentrations of NH₃, HNO₃, NH₄⁺, and NO₃⁻, were collected at an alpine tundra site on Niwot Ridge, Colorado. The measured concentrations were extremely low and ranged between 5 and 70 ng N m⁻³. Dry deposition fluxes of these atmospheric species were calculated using the micrometeorological gradient method. The calculated mean flux for NH₃ indicates a net deposition to the surface and indicates that NH₃ contributed significantly to the total N deposition to the tundra during the August–September measurement period. Our pre-measurement estimate of the compensation point for NH₃ in air above the tundra was 100–200 ng N m⁻³; thus, a net emission of NH₃ was expected given the low ambient concentrations of NH₃ observed. Based on our results, however, the NH₃ compensation point at this alpine tundra site appears to have been at or below about 20 ng N m⁻³. Large deposition velocities (>2 cm s⁻¹) were determined for nitrate and ammonium and may result from reactions with surface-derived aerosols.     

A procedure for use in estimating human exposure to particulate matter of ambient origin

Modern epidemiology has shown that fluctuations of mortality data are statistically significantly correlated with fluctuations of ambient particulate matter (PM) concentration data. This relation cannot be confounded by exposure to PM of indoor origin because the concentrations of ambient PM are not correlated with concentrations of PM of indoor origin. It has been suggested, given the above understanding, that modern PM exposure measurements and analysis should create separate estimates of exposure to all PM of ambient origin and exposure to all PM of nonambient origin (primarily of indoor origin), and not exposure to total PM. This paper reviews the developments of the form of the general microenvironmental mass balance equation that can be utilized for estimating human exposure to PM of ambient origin and for estimating the portion of total PM exposure that is attributable to nonambient origin PM. The equation is perfectly general and can be applied to conditions of time-varying factors that influence exposure, such as rapidly changing air-exchange rates in a home as doors and windows are opened and closed, and turning on and off air cleaners in a home. It is suggested that this procedure be applied in exposure assessment studies and validated using independent techniques of estimating exposure to PM of ambient origin available in the literature.     

Acid precipitation: The importance of nitric acid

Acid precipitation is caused by H₂SO₄ and HNO₃. Currently, in the north-eastern United States on an annual basis, the maximum contributions of H₂SO₄ and HNO₃ to the acidity of precipitation in summer are 73 and 31% and in winter are 59 and 61%, respectively. Based on statistical analyses of the 15-y record of precipitation composition from the Hubbard Brook Experimental Forest during 1964–1979, the importance of H₂SO₄ has decreased by about 30% relative to HNO₃ and HNO₃ has increased by about 50% relative to H₂SO₄.     

The weight method: a new screening method for estimating pesticide deposition from knapsack sprayers in developing countries

Investigations of occupational and environmental risk caused by the use of agrochemicals have received considerable interest over the last decades. And yet, in developing countries, the lack of staff and analytical equipment as well the costs of chemical analyses make it difficult, if not impossible, to monitor pesticide contamination and residues in humans, air, water, and soils. A new and simple method is presented here for estimation of pesticide deposition in humans and soil after application. The estimate is derived on the basis of water mass balance measured in a given number of high absorbent papers under low evaporative conditions and unsaturated atmosphere. The method is presented as a suitable, rapid, low cost screening tool, complementary to toxicological tests, to assess occupational and environmental exposure caused by knapsack sprayers, where there is a lack of analytical instruments. This new method, called the “weight method”, was tested to obtain drift deposition on the neighbouring field and the clothes of the applicator after spraying water with a knapsack sprayer in one of the largest areas of potato production in Colombia. The results were confirmed by experimental data using a tracer and the same set up used for the weight method. The weight method was able to explain 86% of the airborne drift and deposition variance.