Validation of model calculation of ammonia deposition in the neighbourhood of a poultry farm using measured NH3 concentrations and N deposition

Substantial emission of ammonia (NH₃) from animal houses and the related high local deposition of NH₃-N are a threat to semi-natural nitrogen-deficient ecosystems situated near the NH₃ source. In Denmark, there are regulations limiting the level of NH₃ emission from livestock houses near N-deficient ecosystems that are likely to change due to nitrogen (N) enrichment caused by NH₃ deposition. The models used for assessing NH₃ emission from livestock production, therefore, need to be precise, as the regulation will affect both the nature of the ecosystem and the economy of the farmer. Therefore a study was carried out with the objective of validating the Danish model used to monitor NH₃ transport, dispersion and deposition from and in the neighbourhood of a chicken farm. In the study we measured NH₃ emission with standard flux measuring methods, NH₃ concentrations at increasing distances from the chicken houses using passive diffusion samplers and deposition using ¹⁵N-enriched biomonitors and field plot studies. The dispersion and deposition of NH₃ were modelled using the Danish OML-DEP model. It was also shown that model calculations clearly reflect the measured NH₃ concentration and N deposition. Deposition of N measured by biomonitors clearly reflected the variation in NH₃ concentrations and showed that deposition was not significantly different from zero (P < 0.05) at distances greater than 150–200 m from these chicken houses. Calculations confirmed this, as calculated N deposition 320 m away from the chicken farm was only marginally affected by the NH₃ emission from the farm. There was agreement between calculated and measured deposition showing that the model gives true estimates of the deposition in the neighbourhood of a livestock house emitting NH₃.     

Modelling the atmospheric transport and deposition of sulphur and nitrogen over the United Kingdom and assessment of the influence of SO2 emissions from international shipping

A statistical Lagrangian atmospheric transport model was used to generate annual maps of deposition of sulphur and oxidised and reduced nitrogen for the UK at a 5×5 km² resolution. The model was run using emissions for the year 2002. The model was compared with measurements of gas concentrations (SO₂, NO_x, HNO₃ and NH₃) and of wet deposition and aerosol concentrations of SO₄²⁻, NO₃⁻ and NH₄⁺ from national monitoring networks. Good correlation was obtained, demonstrating that the model is capable of accurately estimating the mass balance and spatial distribution of sulphur and nitrogen compounds in the atmosphere. A future emissions scenario for the year 2020 was used to test the influence of shipping emissions on sulphur deposition in the UK. The results show that, if shipping emissions are assumed to increase at a rate of 2.5% per year, their relative contribution to sulphur deposition is expected to increase from 9% to 28% between 2002 and 2020. The model was compared to both a European scale and a global scale chemical transport model and found to give broad agreement with the magnitude and location of sulphur deposition associated with shipping emissions. Enforcement of the MARPOL convention to reduce the sulphur content in marine fuel to 1% was estimated to result in a 6% reduction in total sulphur deposition to the UK for the year 2020. The percentage area of sensitive habitats with exceedance of critical loads for acidity in the UK was predicted to decrease by 1% with the implementation of the MARPOL convention.     

Ammonia concentrations and modeling of inorganic particulate matter in the vicinity of an egg production facility in Southeastern USA

Ammonia (NH₃) is an important base gas and can react with acidic species to form atmospheric aerosols. Due to the rapid growth of poultry and swine production in the North Carolina Coastal Plain, atmospheric NH₃ concentrations across the region have subsequently increased. Ammonia concentrations and inorganic particulate matter (PM) at four ambient stations in the vicinity of an egg production facility were measured for 1 year using PM_2.5 speciation samplers with honeycomb denuders and ion chromatography (IC). Meanwhile, concentrations of NH₃ and inorganic PM in one of the egg production houses were also simultaneously measured using a gas analyzer for NH₃ and the filter pack plus IC method for inorganic PM. An equilibrium model-ISORROPIA II was applied to predict the behavior of inorganic aerosols in response to precursor gas concentrations and environmental parameters. Average ambient NH₃ concentrations varied from 10.0 to 27.0 μg/m³, and they were negatively correlated with the distances from the ambient location to the nearest egg production house exhausts. Ambient NH₃ concentrations were higher in warm seasons than in cold seasons. Measured NH₃ concentrations agreed well with ISORROPIA II model predictions at all sampling stations. For the ambient stations, there was a good agreement in particle phase NH₄ ⁺ between the model simulation and observations. For the in-house station, the model simulation was applied to correct the overestimation of particle phase NH₄ ⁺ due to gas phase NH₃ breaking through the denuders. Changes in SO₄ ^2?, NO₃ ^?, and Cl^? yield proportional changes in inorganic PM mass. Due to the abundance of NH₃ gas in the vicinity area of the monitored farm, changes in NH₃ concentrations had a small effect on inorganic PM mass. Aerosol equilibrium modeling may be used to assess the influence of precursor gas concentrations on inorganic PM formation when the measurements for some species are unavailable.     

Changes in soil inorganic nitrogen as related to atmospheric nitrogenous pollutants in southern California

The deposition of nitrogenous pollutants has serious implications for ecosystem function and stability. Research in temperate ecosystems has indicated a wide range of ecological responses, yet very little is known about arid ecosystems. In this study, measurements of atmospheric and soil concentrations of the plant-available NO^-₃ and NH⁺₄ were evaluated to identify a potential gradient in nitrogen (N) deposition. The evaluations were conducted in coastal sage scrub, a semi-arid vegetation type native to the lower elevations of southern California.The summer atmospheric concentrations of nitrate (NO^-₃) and ammonium (NH⁺₄) were determined at five locations on the Perris Plain of southern California. The atmospheric influences varied from direct interception of pollution generated in the Los Angeles Basin at the northern end of the gradient to a site 70 km south lacking any direct Los Angeles influence. The summer atmospheric concentrations of NO^-₃ varied more than three-fold along the gradient. Ammonium concentrations followed a similar pattern, but the gradient was less steep. Winter concentrations were very low for both compounds. The summer soil surface NO^-₃ concentrations were near the detection limits at low pollution sites but in the range of 50–60 μg N g^-1 soil under highly polluted conditions. Wet deposition was found to be a minor contributor of plant-available N, suggesting that dry deposition may be a consequential source of plant-available N.The detection of significant changes in inorganic, plant-available N in the upper layer of soils is enhanced by the unique environmental conditions and vegetation of southern California. This study suggests that the coastal sage scrub ecosystem is experiencing significant changes in N fertility that may contribute to changes in plant species composition. The data also show that this semi-arid ecosystem provides a unique opportunity to assess many physical, chemical and biological responses to dry deposition alone.     

Concentration-dependent NH3 deposition processes for mixed moorland semi-natural vegetation

Dry deposition modelling typically assumes that canopy resistance (R_c) is independent of ammonia (NH₃) concentration. An innovative flux chamber system was used to provide accurate continuous measurements of NH₃ deposition to a moorland composed of a mixture of Calluna vulgaris (L.) Hull, Eriophorum vaginatum L. and Sphagnum spp. Ammonia was applied at a wide range of concentrations (1–100 μg m⁻³). The physical and environmental properties and the testing of the chamber are described, as well as results for the moorland vegetation using the ‘canopy resistance’ and ‘canopy compensation point’ interpretations of the data.Results for moorland plant species demonstrate that NH₃ concentration directly affects the rate of NH₃ deposition to the vegetation canopy, with R_c and cuticular resistance (R_w) increasing with increasing NH₃ concentrations. Differences in R_c were found between night and day: during the night R_c increases from 17 s m⁻¹ at 10 μg m⁻³ to 95 s m⁻¹ at 80 μg m⁻³, whereas during the day R_c increases from 17 s m⁻¹ at 10 μg m⁻³ to 48 s m⁻¹ at 80 μg m⁻³. The lower resistance during the day is caused by the stomata being open and available as a deposition route to the plant. R_w increased with increasing NH₃ concentrations and was not significantly different between day and night (at 80 μg m⁻³ NH₃ day R_w=88 s m⁻¹ and night R_w=95 s m⁻¹). The results demonstrate that assessments using fixed R_c will over-estimate NH₃ deposition at high concentrations (over ∼15 μg m⁻³).     

Size partitioning of particulate inorganic nitrogen species between the fine and coarse mode ranges and its implication to their deposition on the surface ocean

In order to discuss the dry deposition fluxes of atmospheric fixed nitrogen species, observations of aerosol chemistry including nitrate (NO₃^?) and ammonium (NH₄⁺) were conducted at two islands, Rishiri Island and Sado Island, over the Sea of Japan. Although the atmospheric concentrations of particulate NH₄⁺–N showed higher values than those of particulate NO₃^?–N at both sites, the dry deposition fluxes of the particulate NO₃^?–N were estimated to be higher than those of the particulate NH₄⁺–N. This was caused by the difference of particle sizes between the particulate NO₃^? and NH₄⁺; NH₄⁺ was almost totally contained in fine particles (d < 2.5 μm) with smaller deposition velocity, whereas NO₃^? was mainly contained in coarse particles (d > 2.5 μm) with greater deposition velocity. Fine mode NO₃^? was strongly associated with fine mode sea-salt and mineral particles, of which higher concentrations shifted the size of particulate NO₃^? toward the fine mode range. This size shift would decrease the dry deposition flux of the fixed nitrogen species on coastal waters and accelerate atmospheric transport of them to the remote oceanic areas.     

Ammonia in the atmosphere: a review on emission sources, atmospheric chemistry and deposition on terrestrial bodies

Gaseous ammonia (NH₃) is the most abundant alkaline gas in the atmosphere. In addition, it is a major component of total reactive nitrogen. The largest source of NH₃ emissions is agriculture, including animal husbandry and NH₃-based fertilizer applications. Other sources of NH₃ include industrial processes, vehicular emissions and volatilization from soils and oceans. Recent studies have indicated that NH₃ emissions have been increasing over the last few decades on a global scale. This is a concern because NH₃ plays a significant role in the formation of atmospheric particulate matter, visibility degradation and atmospheric deposition of nitrogen to sensitive ecosystems. Thus, the increase in NH₃ emissions negatively influences environmental and public health as well as climate change. For these reasons, it is important to have a clear understanding of the sources, deposition and atmospheric behaviour of NH₃. Over the last two decades, a number of research papers have addressed pertinent issues related to NH₃ emissions into the atmosphere at global, regional and local scales. This review article integrates the knowledge available on atmospheric NH₃ from the literature in a systematic manner, describes the environmental implications of unabated NH₃ emissions and provides a scientific basis for developing effective control strategies for NH₃.     

Analysis of the uptake of atmospheric ammonia by leaves of Phaseolus vulgaris L.

Individual leaves of Phaseolus vulgaris L. were exposed for 9 h in a leaf chamber to different NH₃ concentrations at different light intensities. The rates of NH₃-uptake, transpiration and photosynthesis were measured simultaneously. The flux density of NH₃ increased linearly with concentration in the range of 4–400μg m⁻³. Flux densities also increased with light intensity. Resistance analysis indicated that NH₃ transport into the leaf is via the stomata: transport via the cuticle is negligible under the experimental conditions. There is no internal resistance against NH₃ transport. The NH₃ flux was found not to influence the photosynthesis.     

Vertical distribution of gases and aerosols: The behaviour of ammonia and related components in the lower atmosphere

Vertical concentration profiles for NH₃, HNO₃ and HCl-gas and for NH₄⁺, NO₃⁻, SO²⁻₄, Cl⁻ and Na⁺ aerosol were obtained from a meteorological tower in the central part of the Netherlands. An upward NH₃ flux of 0.12 μgm⁻² s⁻¹ was calculated from the NH₃ profiles and meteorological data. From the HNO₃ profiles a maximum HNO₃ dry deposition velocity of 4 cm s⁻¹ was calculated. Good agreement was found between the measured concentration products [NH₃]_(g) × [HNO₃]_(g) and the theoretical values at temperatures above 0°C and relative humidities below 80%. In other cases, higher NH₃ and/or HNO concentrations in the gas phase were measured than theoretically predicted.     

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.     

Quantifying local traffic contributions to NO2 and NH3 concentrations in natural habitats

NO₂ and NH₃ concentrations were measured across a Special Area for Conservation in southern England, at varying distances from the local road network. Exceedances of the critical levels for these pollutants were recorded at nearly all roadside locations, extending up to 20 m away from roads at some sites. Further, paired measurements of NH₃ and NO₂ concentrations revealed differences between ground and tree canopy levels. At “background” sites, away from the direct influence of roads, concentrations were higher within tree canopies than at ground level; the reverse pattern was, however, seen at roadside locations. Calculations of pollutant deposition rates showed that nitrogen inputs are dominated by NH₃ at roadside sites. This study demonstrates that local traffic emissions contribute substantially to the exceedance of critical levels and critical loads, and suggests that on-site monitoring is needed for sites of nature conservation value which are in close proximity to local transport routes.     

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 use of inferential models for estimating nitric acid vapor deposition to semi-arid coniferous forests

Urban areas emit significant amounts of pollutants that impact forest ecosystems. One of the most important of these is nitric acid vapor (HNO₃), a nitrogen-containing gas that deposits efficiently to forest canopies. Since measuring HNO₃ fluxes directly is often impractical and costly in remote forest locales, inferential techniques are most often used to estimate HNO₃ flux. Given the highly efficient deposition of HNO₃, many of these inferential models assume that leaf surfaces are a ‘perfect sink’ for HNO₃ (i.e., that resistance to HNO₃ deposition is negligibly small or zero). This study tests the ‘perfect sink’ assumption in an open gas exchange system by exposing Abies magnifica, Abies concolor, and Pinus jeffreyi seedlings to concentrations of 1–13 ppb at 4–20% relative humidity. We find that, at these humidities and concentrations, cuticles are not perfect sinks for HNO₃, with cuticular resistance values ranging from 20 to 184 s m⁻¹. In addition, our results indicate that accumulating HNO₃ on leaf cuticles at these concentrations leads to higher cuticular resistance over 8–12 h exposure periods. Based on this laboratory data, we then parameterized cuticular resistance using a single-layer inferential model for semi-arid forests in the Lake Tahoe Basin. Modeled fluxes using this modification were 33% lower during well-mixed daytime conditions than the fluxes from an identical model run using the perfect sink assumption. Since HNO₃ can often account for more than half of atmospheric deposition, we conclude that inferential models that assume foliage to be perfect HNO₃ sinks are inaccurate, especially in semi-arid forests where significant amounts of HNO₃ can accumulate on leaf surfaces during dry periods.     

Determination of Atmospheric Nitrogen Input to Lake Greenwood,South Carolina: Part 2—Gaseous Measurements and Modeling

Abstract

The Reedy River branch of Lake Greenwood, SC, has repeatedly experienced summertime algal blooms, upsetting the natural system. A series of experiments were carried out to investigate atmospheric nitrogen (N) input into the lake. N was examined because of the insignificant phosphorus dry atmospheric flux and the unique nutrient demands of the dominant algae (Pithophora oedogonia) contributing to the blooms. Episodic atmospheric measurements during January and March 2001 have shown that the dry N flux onto the lake ranged from 0.9 to 17.4 kg N/ha-yr, and on average is caused by nitric acid (HNO₃; 31%), followed by nitrogen dioxide (NO₂; 23%), fine ammonium (NH₄ ⁺; 20%), coarse nitrate (NO₃ ^?; 16%), fine NO₃ ⁺ (5%), and coarse NH₄ ⁺ (5%). Similar measurements in Greenville, SC (the upper watershed of the Reedy River), showed that the dry N deposition flux there ranged from 1.4 to 9.7 kg N/ha-yr and was mostly caused by gaseous deposition (40% NO₂ and 40% HNO₃). The magnitude of this dry N deposition flux is comparable to wet N flux as well as other point sources in the area. Thermodynamic modeling showed low concentrations of ammonia, relative to the particulate NH₄ ⁺ concentrations.     

Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models

Methods for estimating the dry deposition velocities of atmospheric gases in the U.S. and surrounding areas have been improved and incorporated into a revised computer code module for use in numerical models of atmospheric transport and deposition of pollutants over regional scales. The key improvement is the computation of bulk surface resistances along three distinct pathways of mass transfer to sites of deposition at the upper portions of vegetative canopies or structures, the lower portions, and the ground (or water surface). This approach replaces the previous technique of providing simple look-up tables of bulk surface resistances. With the surface resistances divided explicitly into distinct pathways, the bulk surface resistances for a large number of gases in addition to those usually addressed in acid deposition models (SO₂, O₃ NO_x, and HNO₃) can be computed, if estimates of the effective Henry's Law constants and appropriate measures of the chemical reactivity of the various substances are known. This has been accomplished successfully for H₂O₂, HCHO₃ CH₃CHO (to represent other aldehvdes), CH₃O₂H (to represent organic peroxides), CH₃C(O)O₂H, HCOOH (to represent organic acids), NH₃, CH₃C(O)O₂NO₂ and HNO₂. Other factors considered include surface temperature, stomata1 response to environmental parameters, the wetting of surfaces by dew and rain, and the covering of surfaces by snow. Surface emission of gases and variations of uptake characteristics by individual plant species within the landuse types are not considered explicitly.     

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.     

A Predictive Mechanism for Mercury Oxidation on Selective Catalytic Reduction Catalysts under Coal-Derived Flue Gas

Abstract

This paper introduces a predictive mechanism for elemental mercury (Hg⁰) oxidation on selective catalytic reduction (SCR) catalysts in coal-fired utility gas cleaning systems, given the ammonia (NH₃)/nitric oxide (NO) ratio and concentrations of Hg⁰ and HCl at the monolith inlet, the monolith pitch and channel shape, and the SCR temperature and space velocity. A simple premise connects the established mechanism for catalytic NO reduction to the Hg⁰ oxidation behavior on SCRs: that hydrochloric acid (HCl) competes for surface sites with NH₃ and that Hg⁰ contacts these chlorinated sites either from the gas phase or as a weakly adsorbed species. This mechanism explicitly accounts for the inhibition of Hg⁰ oxidation by NH₃, so that the monolith sustains two chemically distinct regions. In the inlet region, strong NH₃ adsorption minimizes the coverage of chlorinated surface sites, so NO reduction inhibits Hg⁰ oxidation. But once NH₃ has been consumed, the Hg⁰ oxidation rate rapidly accelerates, even while the HCl concentration in the gas phase is uniform. Factors that shorten the length of the NO reduction region, such as smaller channel pitches and converting from square to circular channels, and factors that enhance surface chlorination, such as higher inlet HCl concentrations and lower NH₃/NO ratios, promote Hg⁰ oxidation.

This mechanism accurately interprets the reported tendencies for greater extents of Hg⁰ oxidation on honeycomb monoliths with smaller channel pitches and hotter temperatures and the tendency for lower extents of Hg⁰ oxidation for hotter temperatures on plate monoliths. The mechanism also depicts the inhibition of Hg⁰ oxidation by NH₃ for NH₃/NO ratios from zero to 0.9. Perhaps most important for practical applications, the mechanism reproduces the reported extents of Hg⁰ oxidation on a single catalyst for four coals that generated HCl concentrations from 8 to 241 ppm, which covers the entire range encountered in the U.S. utility industry. Similar performance is also demonstrated for full-scale SCRs with diverse coal types and operating conditions.     

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.     

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.