Atmospheric Deposition of Reactive Nitrogen on Turf Grassland in Central Japan: Comparison of the Contribution of Wet and Dry Deposition

The atmospheric deposition of reactive nitrogen on turf grassland in Tsukuba, central Japan, was investigated from July 2003 to December 2004. The target components were ammonium, nitrate, and nitrite ions for wet deposition and gaseous ammonia, nitric and nitrous acids, and particulate ammonium, nitrate, and nitrite for dry deposition. Organic nitrogen was also evaluated by subtracting the amount of inorganic nitrogen from total nitrogen. A wet-only sampler and filter holders were used to collect precipitation and the atmospheric components, respectively. An inferential method was applied to calculate the dry deposition velocity of gases and particles, which involved the effects of surface wetness and ammonia volatilization through stomata on the dry deposition velocity. The mean fraction of the monthly wet to total deposition was different among chemical species; 37, 77, and 1% for ammoniacal, nitrate-, and nitrite-nitrogen, respectively. The annual deposition of inorganic nitrogen in 2004 was 47 and 48 mmol m⁻² yr⁻¹ for wet and dry deposition, respectively; 51% of atmospheric deposition was contributed by dry deposition. The annual wet deposition in 2004 was 20, 27, and 0.07 mmol m⁻² yr⁻¹, and the annual dry deposition in 2004 was 35, 7.4, and 5.4 mmol m⁻² yr⁻¹ for ammoniacal, nitrate-, and nitrite-nitrogen, respectively. Ammoniacal nitrogen was the most important reactive nitrogen because of its remarkable contribution to both wet and dry deposition. The median ratio of the organic nitrogen concentration to total nitrogen was 9.8, 17, and 15% for precipitation, gases, and particles, respectively.     

Monitoring Long-term Trends in Sulfate and Ammonium in US Precipitation: Results from the National Atmospheric Deposition Program/National Trends Network

Data from the National Atmospheric Deposition Program/National Trends Network (NADP/NTN) indicate significant changes have occurred in precipitation chemistry and the chemical climate in the United States (US). A Seasonal Kendall Trend (SKT) analysis shows statistically significant increases in precipitation ammonium concentrations at 64% of 159 continental US NADP/NTN sites evaluated from Winter 1985 to Fall 2004 (Dec. 1984 – Nov. 2004). Sulfate decreases were widespread, with an SKT analysis indicating statistically significant decreases at 89% of sites evaluated. Ratios of chemical equivalent concentrations of ammonium to sulfate in precipitation have risen to the extent that ammonium now exceeds sulfate over more than half of the continental U.S. on a precipitation-weighted-mean annual basis. These trends in the concentrations of ammonium, sulfate, and other species have been accompanied by significant decreases in the frequency of acidic precipitation (pH < 5.0) in the last decade.     

Uncertainty in Estimation of Wet Deposition of Sulphur

A model is described for predicting wet deposition ofsulphur in Britain from rainfall and site measurementsof ion concentration in precipitation. This modelincludes orographic enhancement of both rainfall andion concentration. The model output is comparedagainst available measurement data. Sensitivity anduncertainty analyses are used to predict the outputuncertainty. If the stated assumptions can be shown tobe correct, the wet deposition for Britain at the 5 kmscale is accurate to ±35% across the country. Theanalyses show a larger uncertainty in central Englandand a possible bias towards underestimation of wetdeposition, the latter being of importance incalculating critical load exceedances in remote areas.     

Study of Bulk and Sub-Event Wet Deposition in Gebze,Turkey

This study presents the chemical composition of bulk deposition during the period of February 1996–May 1997 and the chemical composition of sub-event wet deposition on 13 August 1997 in Gebze. Samples were analyzed for SO₄ ^2-, NO₃ ^-, Cl^-,Ca²⁺, Mg²⁺, K⁺, Na⁺, and NH₄ ⁺ in addition to pH. The source of some ionic components in the bulk deposition such as K⁺ and Ca²⁺ were found to be the terrestrial regions, as expected. The (non-sea Cl^-)/Cl^- ratio of 0.05 suggests that the very large portion of Cl^- in the bulkdeposition was of marine origin. The ratio of (non-sea SO₄ ^2-)/SO₄ ^2- varied between 0.86 and 0.99,indicating that the main source of sulfate was not the sea. It is found that the sulfate and calcium concentrations were highest in summer and lowest in fall. The analysis of bulk deposition also indicated that nearly 24% of the events were acidic (pH < 5.6). During sub-event wet deposition collectedon the same site pH decreased continually, and during the passageof cold front concentrations of Cl^-, SO₄ ^2- and NO₃ ^- increased.     

Long Term Trends in Sulphur and Nitrogen Deposition in Europe and the Cause of Non-linearities

Emissions of sulphur and oxidized nitrogen compounds in Europe have been reduced following a series of control measures during the last two decades. These changes have taken place during a period in which the primary gases and the wet deposition throughout Europe were extensively monitored. Since the end of the 1970s, for example land based sulphur emissions declined by between 90 and 70% depending on the region. Over the same period the total deposition of sulphur and its partitioning into wet and dry deposition have declined, but the spatial pattern in the reduction in deposition differs from that of emission and has changed with time. Such non-linearities in the emission-deposition relationship are important to understand as they complicate the process of assessing the effects of emission reduction strategies. Observed non-linearities in terrestrial sulphur emission-deposition patterns have been identified in north west Europe due to increases in marine emissions, and are currently slowing the recovery of freshwater ecosystems. Changes in the relative amounts of SO₂ and NH₃ in air over the last two decades have also changed the affinity of terrestrial surfaces for SO₂ and have therefore changed the deposition velocity of SO₂ over substantial areas. The consequence of this effect has been the very rapid reduction in ambient SO₂ concentration in some of the major source areas of Europe, where NH₃ did not change much. Interactions between the different pollutants, generating non-linearities are now being incorporated in long-range transport models to simulate the effects of historical emission trends and to provide projections into the future. This paper identifies non-linearities in emission deposition relationships for sulphur and nitrogen compounds in Europe using data from the EMEP long-rang transport model and measured concentration fields of the major ions in precipitation and of SO₂ and NO₂ in surface air.     

Long-term Trends in Surface Water Quality of Five Lakes in Japan

Since 1983, the Ministry of the Environment of Japan has conducted nation-wide acid deposition surveys. To investigate the effects of acid deposition on surface water, we used the nonparametric Mann–Kendall test to find temporal trends in pH, alkalinity, and electrical conductivity (EC) in more than 10 years of data collected from five lakes and their catchments (Lake Kuttara: northernmost; Lake Kamakita: near Tokyo; Lake Ijira: central; Lake Banryu: western; and Lake Unagiike: southernmost). The pH of Lake Ijira water has declined slightly since the mid-1990s, corresponding with the downward trends seen in the pH and alkalinity of the river water flowing into the lake. There were significant upward trends in the EC of both the lake and stream water; the same trends were also found for concentrations. These trends show evidence of acidification due to atmospheric deposition, and this is the first such finding in Japan based on significant long-term trends. Lake Ijira is located about 40 km north of the Chukyo industrial area near Nagoya. The annual depositions of H⁺, nss-, and in Lake Ijira were among the highest of all deposition monitoring sites, suggesting that this is the main cause of the significant acidification observed in Lake Ijira. No significant trends suggesting acidification were observed in any of the other lake catchments in spite of the significant upward trends in EC. Upward trends in pH and alkalinity at Lake Banryu and upward trends in alkalinity at Lake Kamakita were detected, but no change in pH or alkalinity at Lake Kuttara and Lake Unagiike was observed.     

Trends in the Water Chemistry of High Altitude Lakes in Europe

Here we present the chemical trends of seven high altitude lakes, analysed within the AL:PE and MOLAR Projects of the EU (1999) and selected on the basis of the availability of complete and reliable data for the period 1984–1999. The lakes are representative of the Scandinavian Alps, the Cairngorm Mountains in Scotland, the Alps and the Pyrenees. Significant trends were identified for some indicators of acidification, for instance pH and alkalinity, but not all lakes reacted similarly to decreasing depositions of sulphate and base cations. Differences in lake response are discussed in relation to recent variations of atmospheric deposition chemistry and associated changes in climatic conditions. Beside individual variations of the studied lakes, depending, among other things, on altitude and morphology, catchment characteristics and climate trends play a major role for the reaction of high altitude lakes on changes in atmospheric depositions.     

An Automated Wet Deposition System to Compare the Effects of Reduced and Oxidised N on Ombrotrophic Bog Species: Practical Considerations

Critical N loads for ombrotrophic bogs, which often contain rare and N-sensitive plants (especially those in lower plant groups: lichens, mosses and liverworts), are based on very few experimental data from measured, low background N deposition areas. Additionally the relative effects of reduced versus oxidised N are largely unknown. This paper describes an automated field exposure system (30 km S. of Edinburgh, Scotland) for treating ombrotrophic bog vegetation with fine droplets of oxidised N (NaNO₃) and reduced N (NH₄Cl). Whim Moss exists in an area of low ambient N deposition (ca. 8 kg N ha^–1 y^–1), the sources and quantification of which are described. The wet N treatment system is run continuously, and is controlled/activated by wind speed and rainfall to provide a unique simulation of real world treatment patterns (no rain=no treatment). Simulated precipitation is supplied at ionic concentrations below4mMin rainwater collected on site. Treatments provide a replicated dose response to 16, 32 and 64 kg N ha^–1 y^–1 adjusted for ambient deposition (8 kg N ha^–1 y^–1). The 16 and 64 kg N ha^–1 y^–1 are duplicated with a P+K supplement. Baseline soil chemistry and foliar nutrient status was established for all 44 plots for Calluna vulgaris, Sphagnum capillifolium, Hypnum jutlandicum and Cladonia portentosa.     

Comparisons of Measured and Modelled Ozone Deposition to Forests in Northern Europe

The performance of a new dry deposition module, developedfor the European-scale mapping and modelling of ozone flux to vegetation, was tested against micrometeorological ozone and water vapour flux measurements. The measurement data are for twoconiferous (Scots pine in Finland, Norway spruce in Denmark) and one deciduous forest (mountain birch in Finland). On average, themodel performs well for the Scots pine forest, if local inputdata are used. The daytime deposition rates are somewhat over-predicted at the Danish site, especially in the afternoon. The mountain birch data indicate that the generic parameterisationof stomatal responses is not very representative of this northernspecies. The module was also tested by using modelled meteorological data that constitute the input for a photochemical transport model.     

Deposition Loads of Sulphur and Nitrogen in Germany

High spatial resolution maps of deposition loads in Germanyare produced as an input for abatement strategy research andfor critical loads exceedance calculations on a nationalscale. In this paper methods ofmapping total deposition loads in Germany and preliminarymaps of nitrogen and sulphur deposition loads for the year1993 are presented. A comparison of these mapping resultswith EMEP deposition mapping results has been carried out.The differences in the results of the German national and theEuropean EMEP mapping, due to different databases anddifferent methods, are quantified and discussed. Highresolution maps of deposition loads are compared to Europeanlow resolution maps on the same temporal and spatial scale,assuming that on average both should lead to similar results.However, the average differencescalculated for 23 EMEP 150 × 150 km² grid cells over Germanywere found to be 33% higher for sulphur (S) total depositionby the German method 65% higher for S dry deposition and1% lower for S wet deposition. The German results fornitrogen (N) total deposition are 2% higher than the EMEPresult 22% higher for N dry deposition and 10% lower for Nwet deposition.     

The Influence of Atmospheric N Deposition on Nitrous Oxide and Nitric Oxide Fluxes and Soil Ammonium and Nitrate Concentrations

The deposition of atmospheric N to soils provides sources of available N to the nitrifying and denitrifying microbial community and subsequently influences the rate of NO and N₂O emissions from soil. We have investigated the influence of three different sources of enhanced N deposition on NO and N₂O emissions 1) elevated NH₃ deposition to woodlands downwind of poultry and pig farms, 2) increased wet cloud and occult N deposition to upland forest and moorland and 3) enhanced N deposition to trees as NO ₃ ^– and NH ₄ ⁺ aerosol. Flux measurements of NO and N₂O were made using static chambers in the field or intact and repacked soil cores in the laboratory and determination of N₂O by gas chromatography and of NO by chemiluminescence analysis. Rates of N deposition to our study sites were derived from modelled estimates of N deposition, NH₃ concentrations measured by passive diffusion and inference from measurements of the ²¹⁰Pb inventory of soils under tree canopies compared with open grassland. NO and N₂O emissions and KCl-extractable soil NH ₄ ⁺ and NO ₃ ^– concentrations all increased with increasing N deposition rate. The extent of increase did not appear to be influenced by the chemical form of the N deposited. Systems dominated by dry-deposited NH₃ downwind of intensive livestock farms or wet-deposited NH ₄ ⁺ and NO ₃ ^– in the upland regions of Britain resulted in approximately the same linear response. Emissions of NO and N₂O from these soils increased with both N deposition and KCl extractable NH ₄ ⁺ , but the relationship between NH ₄ ⁺ and N deposition (ln NH ₄ ⁺ = 0.62 ln N_deposition + 0.21, r ² = 0.33, n = 43) was more robust than the relationship between N deposition and soil NO and N₂O fluxes.     

A Chronology of Nitrogen Deposition in the UK Between 1900 and 2000

Measurements of the concentrations of nitrogen compounds in air and precipitation in the UK have been made since the mid-19th century, but no networks operating to common protocols and having traceable analytical procedures were established until the 1950s. From 1986 onwards, a high-quality network of sampling stations for precipitation chemistry was established across the UK. In the following decade, monitoring networks provided measurement of NO₂, NH₃, HNO₃ and a satisfactory understanding of the dry deposition process for these gases allowed dry deposition to be quantified. Maps of N deposition for oxidized and reduced compounds at a spatial scale of 5 km × 5 km are available from 1986 to 2000. Between 1950 and 1985, the more limited measurements, beginning with those of the European Air Chemistry Network (EACN) provide a reasonable basis to estimate wet deposition of NO ₃ ^– –N and NH ₄ ⁺ –N. For the first half of the century, estimates of deposition were scaled with emissions assuming a constant relationship between emission and deposition for each of the components of the wet and dry deposition budget at the country scale. Emissions of oxidized N, which dominated total nitrogen emissions throughout the century, increased from 312 kt N annually in 1900 to a peak of 787 kt for the decade 1980–1990 and then declined to 460 kt in 2000. Emissions of reduced N, largely from coal combustion were about 168 kt N in 1900, increasing to a peak of 263 kt N in 2000 and by now dominated by agricultural sources. Reduced N dominated the deposition budget at the country scale, increasing from 163 kt N in 1900 to 211 kt N in 2000, while deposition of oxidized N was 66 kt N in 1900 and 191 kt N in 2000. Over the century, 68 Mt (Tg) of fixed N was emitted within the UK, 78% as NO _x , while 29 Mt of nitrogen was deposited (43% of emissions), equivalent to 1.2 t N ha^–1, on average, with 60% in the reduced form. Deposition to semi-natural ecosystems is approximately 15 Tg N, equivalent to between 1 and 5 t N ha^–1, over the century and appears to be accumulating in soil. The N deposition over the century is similar in magnitude to the total soil N inventory in surface horizons.     

The Role of Cloud Processing in the Relationship Between Wet Deposited Sulphur and Sulphur Dioxide Emissions

It is well established that wet deposition of sulphate in the UKhas fallen by a much smaller fraction than have emissions of sulphur dioxide. Dry deposition of sulphur has decreased in proportion to the decline in emissions. A number of suggestionshave been made which offer possible explanations for this non-linearity between emissions and wet deposition. In this paper amodel of the processing of sulphur dioxide by aqueous phase cloudchemistry in a cloudy boundary layer is presented. This work doesnot simulate all the details of the mechanisms by which sulphate is incorporated into precipitation. It does, however, explorethe non-linearity of this oxidation process. It is shown that theoxidation of sulphur dioxide, in these conditions, over the UK isdominated by oxidation by ozone. The rate of sulphate productionis then controlled by the availability of the one basic trace gasin the atmosphere ammonia. Using realistic concentrations of thereacting species this is found to simulate well the observed non-linearity. The model predicts that sulphate and sulphur dioxideconcentrations will be uncorrelated in the cloudy boundary layerbut that ammonium and sulphate will be well correlated. Fieldobservations at a cloudy site in Northern England are consistentwith these predictions.     

Climatology and Trends of the Temporal and Spatial Distribution of Sandstorms in Inner Mongolia

The temporal and spatial distribution of sandstorms have been investigated statistically for a period of 40 years (1961–2000),using data from 118 observatories in Inner Mongolia, P.R. of China. In terms of climate variations, the effects of changes in climate(affecting parameters such as precipitation, temperature, ENSO activities, etc.), ecological systems and human behavior on the space-time distribution of sandstorms have been studied. It is shown that in Inner Mongolia nearly all sandstorms occurred inthe central-western region during 1961–2000. Their frequency decreased from the 1960s to the 1990s. The mean annual variationshows that spring is the main sandstorm season, especially April. In view of connection with climate variations, dry and cold periods correspond with a high frequency of sandstorms,wet and warm periods with a low frequency. With respect to thespatial distribution, sandstorms hit preferably dry and warm regions. There are some relations between ENSO activities andthe sandstorm frequency. The sandstorm rate was relatively higher in most of the El Niño years, and in most of the La Niña years the rate was relatively lower.     

What Anthropogenic Radionuclides (90Sr and 137Cs in Atmospheric Deposition, Surface Soils and Aeolian Dusts Suggest for Dust Transport over Japan

Currently, atmospheric anthropogenic radionuclides (particulate) are controlled by suspension of the surface dust containing those radionuclides (resuspension). We have found, therefore, that such radionuclides can be used as tracers of the surface dust suspension, transport and its subsequent deposition in distant areas. The ¹³⁷Cs/⁹⁰Sr activity ratios in the atmospheric deposition, without the direct influence of nuclear tests and accidents, at the Meteorological Research Institute (MRI, Tsukuba, Japan) during the 1990s were fairly low (average: 2.1). This value is not in agreement with the ratios in Japanese surface soils (range of averages: 4–7), which had been considered as the primary source of the deposited dust. This suggests that the current atmospheric dust deposition in Japan is a mixture of local and remote components. The remote component could be an aeolian dust that has been transported long distances from arid areas. The major component is most likely to be Asian dust. It was further hypothesized that other remote source may exist beyond the Asian domain, based on accumulated observations and model results. To obtain more information about the dust transport, Sahara dust deposited in Monaco in 2002 and a suspended dust collected in the Taklamakan area in 2001 were analyzed for ⁹⁰Sr and ¹³⁷Cs. The Taklamakan dust exhibited a ¹³⁷Cs/⁹⁰Sr ratio of about 4, which is within the range of atmospheric deposition observed at the MRI, while the Sahara dust exhibited a higher ¹³⁷Cs/⁹⁰Sr ratio (about 13). Although the present Sahara datum was negative for our hypothesis of ‘hyper-range transport’, the seasonal change of the ¹³⁷Cs/⁹⁰Sr ratio in the atmospheric deposition observed at the MRI requires an aeolian dust source having a low ¹³⁷Cs/⁹⁰Sr ratio, other than Asian dust.     

Deposition and Storage of Spheroidal Carbonaceous Fly-Ash Particles in European Mountain Lake Sediments and Catchment Soils

Spheroidal carbonaceous particles(SCPs) are produced only from high temperaturecombustion of fossil-fuels. In mountain lakesystems, they provide an unambiguous indicator ofatmospheric deposition. In order to comparedepositional fluxes of SCPs between mountainareas experiencing various pollutant regimes,intensive bulk deposition sampling was undertakenat five sites across Europe. Catchment soil coresand lake sediment cores were also taken at eachsite to compare SCP storage over the post-industrial period. Atmospheric, sediment and soilSCP data showed similar patterns. Highestcontamination was found in Scotland, Slovakia andSpain with the Austrian site intermediate and themid-Norwegian site least contaminated. A highproportion of accumulated SCPs were found to bestored in catchment soils at each site.Therefore, a significant increase in soilerosion, possibly as a result of future climatechange, could lead to the input of largequantities of catchment stored SCPs and, byimplication, other atmospherically depositedcontaminants to the lake ecosystem.     

Model Evaluation of Dry Deposition to Vegetation for Volatile and Semi-Volatile Organic Compounds in a Multimedia Environment

Gas-phase atmospheric deposition wasevaluated in a screening level model of themultimedia environmental distribution of toxics(MEND-TOX). Algorithmic additions to MEND-TOXfor the estimation of gas-phase depositionvelocity over vegetated surfaces were analyzedusing recently published dry deposition fluxmeasurements for nitric acid. Model outputs arecompared to similar estimates from the NOAAmultilayer dry deposition model. Results of theevaluation indicate that MEND-TOX performs wellas a screening level model for the estimation ofgas-phase dry deposition velocity of nitric acidover soybeans. The present study expandsprevious laboratory results for organic speciesto include an inorganic species and open fieldand dry leaf, conditions.(On assignment to the National Exposure Research Laboratory, U.S. Environmental Protection Agency); (author for correspondence, e-mail     

Experimental Assessment of Atmospheric Ammonia Dispersion and Short Range Dry Deposition in a Maize Canopy

In order to study the effect of thevegetation structure on atmospheric ammonia(NH₃) dispersion and deposition, anexperiment was set up near Paris, in July 1997.Between 12 and 162 m downwind of a 200 m line-source releasing 600 to 1200 g NH₃hr^-1placed at the top of a maize canopy, NH₃concentration was measured, within and above thecanopy, with a set of 30 active, acid-coateddenuders over periods of 2 to 3 hr. Eight datasets were collected over a one-month period.NH₃ concentration decreased sharply withdistance to the source, from up to800 g NH₃ m^-3 at 12 m, to lessthan 10 g NH₃ m^-3 at 162 m andshowed strong vertical gradients. Within thecanopy, the concentration scaled using thefriction velocity, the canopy height, and thesource strength, exhibited a universal power lawrelationship as a function of the normaliseddownwind distance from the source. A mass balancemethod and a resistance model approach were usedas independent estimates of the cumulateddeposition at 162 m downwind from the source,which range between 1 and 29% of the emittedNH₃. Both methods agreed approximately inmagnitude. A sensitivity analysis showed that thecuticular uptake and the compensation point aremajor parameters that needs to be bettercharacterised under high NH₃ concentrationif one wants to improve NH₃ short-rangedeposition modelling.     

Effects of Decreased Atmospheric Heavy Metal Deposition in South Sweden on Terrestrial Birds and Small Mammals in Natural Populations

In southern Sweden, where exposure to long range distributedheavy metals is about the highest in Scandinavia, depositionsof cadmium (Cd) and lead (Pb) decreased about 20 and 70%,respectively, between mid-1980s and mid-1990s, as estimated bytheir concentrations in moss. Concentrations of Cd and Pb in tissues of the pied flycatcher (Ficedula hypoleuca) and bank vole (Clethrionomys glareolus) were also lower in 1996and 1997 compared to 1981 and 1982. It is concluded that the decreased deposition rate of these elements in southern Sweden had caused decreased exposure, and thus also to decreased potential risk of detrimental effects on insectivorous birds andherbivorous mammals. There was no indication that breeding results of pied flycatcher was influenced by the decreased deposition of toxic metals.