Modelling the contribution of different sources of sulphur to atmospheric deposition in the United Kingdom

In order to understand relationships between sources and receptors of atmospheric deposition, computer models must be used. This paper describes a Lagrangian acid deposition model that represents emissions of trace species across Northern Europe. The chemistry of sulphur dioxide, dimethyl sulphide and hydrogen sulphide is represented and the model tested against estimates of UK wet and dry deposition. Mean UK wet and dry deposition for the period 1992–1994 was 206 and 145 ktonne S yr^-1, respectively. The model predicted wet and dry deposition of 222 and 166 ktonne S yr^-1, in good agreement with measurements. The model has been used to examine the sources of deposited S to the UK. For a base year of 1992, 86% of the UK's SO₂ emissions are exported. The S deposition attributable from mainland European sources was 36% of the UK total S deposition, in good agreement with other UK models but this differs substantially from the calculations of the EMEP model. Natural sources of S deposition from planktonic emissions of dimethyl sulphide, biological emissions of hydrogen sulphide and non-eruptive volcanic emissions of sulphur dioxide contributed approximately 1% of the modelled UK S deposition, of which 95% originated from dimethyl sulphide. The explicit chemical scheme for dimethyl sulphide incorporated into the model showed that 24% of the resultant deposited S was methane sulphonic acid. Boundary conditions of the model were tested and it was found that initialisation of sulphur dioxide and sulphate concentrations to representative ambient conditions had a very small effect. The modelled contribution of UK and European sources to UK S deposition was approximately 40 and 60%, respectively, showing the dramatic change arising from projected UK SO₂ emissions in 2010. This revised version was published online in July 2006 with corrections to the Cover Date.     

Treatment of Urban Areas within a Regional Transport Model of Sulphur and Nitrogen Oxides

The air pollution transport model UGEM (The University of Greenwich Evaluation Model) has been developed to evaluate medium-range transport and deposition of sulphur and oxidised nitrogen from all types of sources of emissions in the UK and to estimate their average annual deposition and concentrations across the UK. The model has been tested for its predictions against the available measurements.This study was focused on a possibility of applying the UGEM model to the assessment of air quality on a local scale. One parameter in the model is crucial, the local deposition fraction. The effect of this parameter on quality of the model predictions has been studied for different scales of UGEM output, such as the whole territory of the UK, a rural region and an urban area.The results of the study show that the magnitude of the local deposition fraction should be different for each grid square to reach the best agreement of predictions of concentrations with measurements. Applying a local value of the parameter to each grid square will improve the model predictions of the concentrations in urban areas in particular and will not affect the quality of model predictions of the wet deposition.     

Two high-speed, portable GC systems designed for the measurement of non-methane hydrocarbons and PAN: results from the Jungfraujoch High Altitude Observatory

Near real-time measurements of light non-methane hydrocarbons (NMHCs) and peroxyacetyl nitrate (PAN) have been performed in the free troposphere using two fast gas chromatography (GC) instruments designed for use on aircraft. A GC-helium ionisation detector (HID) system measured 15 C(2)-C(5) hydrocarbons with 5 min time resolution and a dual channel GC-Electron Capture Detector (ECD) measured PAN with 90 s resolution. Both instruments had low parts per trillion by volume (pptV) detection limits and ran continuously at the remote Jungfraujoch (JFJ) research station in the Swiss Alps (46.55[degree]N, 7.98[degree]E), 3580 m above mean sea level (AMSL), during February/March 2003. Carbon monoxide, ozone, nitrogen oxide and nitrogen dioxide and all odd nitrogen species (NO(y)) were also measured continuously. Hydrocarbons and CO were strongly correlated in all air-masses whilst PAN exhibited both positive and negative correlations with respect to O(3), dependent on age and origin of the air-mass sampled. PAN was found to contribute [similar]20% to the NO(y) sampled on average. The experiment, as well as providing interesting datasets from this remote location, also demonstrated that when optimised, GC techniques have the potential to measure at a time resolution significantly greater than is traditionally considered, with high sensitivity and low uncertainty.     

Aircraft Emissions: A Comparison of Methodologies Based on Different Data Availability

The impact of air traffic on the global atmosphere is characterised by a high degree of uncertainty, concerning both the physico-chemical phenomena involved and the extent of the forcing due to anthropogenic emissions. The different effects of these emissions (e.g. on climate change, stratospheric ozone depletion, acidification, tropospheric ozone formation) are dealt with by different international bodies and conventions (e.g. IPCC, EMEP. . .) which are trying to define a standard methodology allowing countries to evaluate their contributions to global aircraft emissions and to report these figures in a standardised way. The paper compares different methodologies proposed by the joint EMEP/CORINAIR 'Atmospheric Emission Inventory Guidebook' for estimating aircraft emissions. Adjustments to these methodologies have been proposed, in order to integrate some additional data such as the total amount of flight hours per aircraft type or fuel consumption per trip. In case detailed information is not available, we recommend the use of a VERY SIMPLE methodology which may yield acceptable results, provided that every country makes adequate assumptions on the average aircraft type.     

Transport of NO<Subscript>X</Subscript> Emissions from Sugarcane Fertilisation into the Great Barrier Reef Lagoon

The Great Barrier Reef World Heritage Area contains highly sensitive ecosystems that are threatened by the effects of anthropogenic activity including eutrophication. The nearby sugarcane plantations of tropical north Queensland are fertilised annually and there has been ongoing concern about the magnitude of the loss of applied nitrogen to the environment. Previous studies have considered the potential of rainwater run-off to deposit reactive nitrogen species into rivers and ultimately into the Great Barrier Reef Lagoon, but have neglected the possibility of transport via the atmosphere. This paper reports the results of a modelling study commissioned by Australia’s National Heritage Trust aimed at assessing whether or not atmospheric deposition of reactive nitrogen from Queensland’s sugarcane plantations posed a potential threat to the Great Barrier Reef Lagoon. Atmospheric dispersion modelling was undertaken using The Air Pollution Model, developed by Australia’s Commonwealth Scientific and Industrial Research Organisation. Despite the predominance of onshore southeasterly winds, the dispersion model results indicate that 9% of the time during the sugarcane fertilization season (in the modeled years 2001–2006) the meteorological conditions resulted in emissions from the coastal regions of north Queensland being transported out over the ocean around the Great Barrier Reef. The results suggest that there may be a greater efficiency for transport out over the reef during October than for November and December. For the 2 months that exhibited the greatest potential for transport of coastal pollution to the Great Barrier Reef, the modeled deposition of nitrogen oxides (NO_X) into the Great Barrier Reef lagoon was less than 1% of the total emissions from the sugarcane plantations, but was not zero. Our model has a simple chemical scheme that does not cover the full chemistry of all reactive nitrogen compounds and so the results are only indicative of the potential levels of deposition. Nevertheless, our study shows that small amounts of NO_X that originate from sugarcane fertilization may be transported and dry deposited into the Great Barrier Reef lagoon. Other pathways not included in the modeling scheme may provide a more efficient transport mechanism. Whilst modern practices for the application of fertilizer to sugarcane plantations have drastically reduced emissions, the potential efficiency of transport of pollutants via the atmosphere may be of concern for other more highly polluting agricultural industries.     

Modeling the Effects of Air Quality Policy Changes on Water Quality in Urban Areas

This paper describes the development and application of an integrated modeling framework composed of an urban air chemistry model, an urban runoff model, and a water-quality model. The models were linked to simulate the fate and transport of air emissions of nitrogen compounds in the air, urban watershed, surface water runoff, and in a coastal receiving-water body. The model linkage is demonstrated by evaluating the potential water quality implications of reducing NO _x emissions by 32%, volatile organic compound emissions by 51%, and ammonia emissions by 30%, representing changes from 1987 levels to proposed 2000 target levels in Los Angeles, California, USA. Simulations of the Los Angeles dry season during the summer of 1987 (June 1 to August 31) indicated that by reducing emissions from 1987 to proposed year 2000 levels, the dry deposition nitrogen loads to Santa Monica Bay and the Ballona Creek watershed were reduced 21.4% and 15.0%, respectively. Water quality modeling results indicated that dry season atmospheric load reductions to the Ballona Creek Estuary did not reduce chlorophyll-a levels or significantly raise nighttime dissolved oxygen levels because the magnitude of the reductions was negligible compared to non-atmospheric inputs of nitrogen compounds. Simulations of the time period from November 18, 1987 to December 4, 1987 during the Los Angeles wet season indicated that air emissions reductions produced an 18.6% reduction in the dry deposition nitrogen load to Santa Monica Bay, a 15.5% reduction in the dry deposition nitrogen load to the Ballona Creek watershed, a 16.8% reduction in the wet deposition nitrogen load to the Ballona Creek watershed, and a 16.1% reduction in the stormwater discharge load from the Ballona Creek watershed. Although the wet season load reductions are significant, modeling results of the ultimate effect on the Ballona Creek Estuary water quality were inconclusive.     

Deposition Monitoring in Europe

A monitoring station for atmospheric deposition was designed and constructed. Three such stations were applied in a pilot project for a year on three sites (Speulder forest in The Netherlands, Auchencorth in Scotland and Melpitz in Germany) in different regions in Europe to estimate local inputs and to validate deposition models which are currently used or developed to estimate ecosystem specific deposition in Europe. Fluxes at Auchencorth Moss are lowest for all components, except for those much influenced by the sea as a source. As Melpitz is located far away from seas, these components are lowest at this site. Wet deposition is the dominant source of input at Auchencorth, whereas at Speulder forest, through its roughness and pollution climate, dry deposition is dominant. At this site dry deposition velocities are highest. Melpitz is a polluted site. Particularly sulphur deposition is high. It is recommended to equip several locations in Europe with intensive deposition monitoring methods. Such a network will be an extension of existing monitoring programmes on air pollution, such as that run by Eurepean Monitoring and Evaluation Programme for the long-range transmission of air pollutants in Europe (EMEP). The intensive monitoring locations should be selected based on pollution climates and type of vegetation, common in Europe.     

Requirements for developing a regional monitoring capacity for aerosols in Europe within EMEP

The European Monitoring and Evaluation Programme (EMEP) has been established to provide information to Parties to the Convention on Long Range Transboundary Air Pollution on deposition and concentration of air pollutants, as well as on the quantity and significance of long-range transmission of pollutants and transboundary fluxes. To achieve its objectives with the required scientific credibility and technical underpinning, a close integration of the programme's main elements is performed. These elements are emission inventories, chemical transport modelling, and the monitoring of atmospheric chemistry and deposition fluxes, which further are integrated towards abatement policy development. A critical element is the air pollution monitoring that is performed across Europe with a focus not only on health effect aspects and compliance monitoring, but also on process studies and source receptor relationships. Without a strong observational basis a predictive modelling capacity cannot be developed and validated. Thus the modelling success strongly depends on the quality and quantity of available observations. Particulate matter (PM) is a relatively recent addition to the EMEP monitoring programme, and the network for PM mass observations is still evolving. This article presents the current status of EMEP aerosol observations, followed by a critical evaluation in view of EMEP's main objectives and its model development requirements. Specific recommendations are given for improving the PM monitoring programme within EMEP.     

A Global Overview of Atmospheric Acid Deposition Fluxes

This paper presents a summary of globalacid deposition flux data taken from a globalassessment report on acid deposition prepared forUNEP/WMO (Whelpdale and Kaiser, 1996). There is a largevariation in the spacial coverage and reliability ofmonitoring around the world. Many more stationsmeasure wet deposition than collect appropriate datafor estimating dry deposition. The widespread regionswith highest precipitation concentrations anddeposition fluxes of sulphate and nitrate coincideclosely with the regions of highest density ofSO₂ and NO_x precursor emissions occurringprimarily in the mid-latitude, northern hemispherebelt where a large fraction of the worlds fossilfuels is consumed. Organic acids in precipitation makea minor contribution to acidity (<20%) inindustrial regions, but in the rest of the world theyare of same order, or even exceed, inorganic acids.Less is known about dry deposition, but it appears topredominate near strong emission sources with wetdeposition predominating farther downwind. The molarratio of the N/S contribution to acidic deposition isclose to 1.0 over large areas of Europe and NorthAmerica, but is highly variable elsewhere, beinghighest in equatorial regions due to biomass burningand lowest near smelters and other large sources of SO₂.     

Emission Inventory for an Industrial Area of India

The paper presents an emission inventory for Cochin, which is a highly industrialized area situated in the southern part of India. A proper emission inventory is very important for planning pollution control programmes, particularly in coastal sites like Cochin, where environmental situations are of growing concern owing to their typical meterorological conditions. In a systematic way the sources are broadly classified as point, line and area sources. The data on emissions from industries, fuel consumption for vehicular and domestic activities along with the respective emission factors are used for estimating the emissions. The study reveals that industrial sources are mainly responsible for emissions of particulate matter, oxides of sulphur and ammonia in the region. Automobiles are the prime sources of hydrocarbons, oxides of nitrogen and carbon monoxide emitting 95%, 77% and 70% respectively of their total emissions, while the contribution from domestic sources is not very significant.     

太湖氮磷大气干湿沉降时空特征

为了探索太湖氮磷营养盐干湿沉降特征及对太湖营养盐输入的贡献,于2011年不同季节采集太湖不同位点的大气干湿沉降样品,分析干湿沉降中氮（N）和磷（P）的形态和沉降量。研究结果表明,输入太湖的磷以干沉降为主,而氮以湿沉降为主。在太湖干沉降中总无机氮（TIN）占总氮（TN）的77.1%,溶解性磷（DIP）占总磷（TP）的77.9%。干沉降中TIN主要以NH+4-N为主。西太湖是TN与TP通过大气干湿沉降输入太湖的最高湖区。太湖全年大气TN沉降总量为20 978 t,TP沉降总量为1 268 t,因此,氮磷大气干湿沉降是太湖营养盐输入的重要来源之一。     

Nitrate Leaching by Atmospheric N Deposition to Upper Groundwater in the Sandy Regions of The Netherlands in 1990

Anthropogenic increase in atmospheric nitrogen (N) deposition in nature areas results in nitrate leaching to groundwater, threatening its quality. Member states of the European Union are obliged to reduce groundwater nitrate concentrations and to monitor this reduction. The relationship between N deposition and groundwater nitrate concentrations is quantified using a field survey and geographical information. Nitrate concentrations of the uppermost metre of groundwater in nature areas in the sandy regions in 1990 were related to geographical data by means of regression analysis. In this way nitrate concentrations could be explained by potential ammonia deposition, soil type, vegetation and land use. We found that about 35% of 54 kg ha(-1) a(-1) atmospheric N deposition was leached to the upper groundwater as nitrate, resulting in a mean NO3 concentration of about 30 mg L(-1). The critical N load for exceeding the EC limit value (50 mg L(-1)) in the sandy regions of The Netherlands composed of natural vegetation will be about 80 kg ha(-1) a(-1). Leaching is less than expected for nature areas but comparable with leaching of N surpluses in pastures in The Netherlands. A reduction in nitrate leaching by 25% or more can currently be detected via a new field survey.     

Nitrogen multitemporal monitoring through mosses in urban areas affected by mud volcanoes around Mt. Etna, Italy

Nitrogen emissions were assessed by using mosses as bioindicators in a densely inhabited area affected by mud volcanoes. Such volcanoes, locally called Salinelle, are phenomena that occur around Mt. Etna (Sicily, Italy), and are interpreted as the surface outflow of a hydrothermal system located below Mt. Etna, which releases sedimentary fluids (hydrocarbons and Na-Cl brines) along with magmatic gases (mainly CO₂ and He). To date, N emissions from such mud volcanoes have been only quantitatively assessed, and no biomonitoring campaigns are reported about the cumulative effects of these emissions. This study analyzed N concentrations in moss, water and soil samples, collected in a 4-year monitoring campaign. The bryophyte Bryum argenteum, a species widely adopted in surveys of atmospheric pollution, was used as a biological indicator. N concentrations in biomonitors showed relatively low values in the study sites. However, the results of this study suggest that N emissions from Salinelle may have an impact on surrounding ecosystems because N values in moss and water showed a significant correlation. N oxides, in particular, contribute to acidification of ecosystems, thus multitemporal biomonitoring is recommended, especially in those areas where N emitting sources are anthropogenic and natural.     

Differences in the Spatial Distribution and Chemical Composition of PM10 Between the UK and Poland

The Fine Resolution Atmospheric Multi-pollutant Exchange Model was used to calculate the spatial distribution and chemical composition of PM₁₀ concentrations for two geographically remote countries in Europe—the UK and Poland—for the year 2007. These countries are diverse in terms of pollutant emissions as well as climate conditions. Information on the contribution of natural and anthropogenic as well as national and imported particles in total PM₁₀ concentrations in both countries is presented. The paper shows that the modelled national annual average PM₁₀ concentrations, calculated for the entire country area, are similar for the UK and Poland and close to 12 μg m^?3. Secondary inorganic aerosols dominate the total PM₁₀ concentrations in Poland. Primary particulate matter has the greatest contribution to total PM₁₀ in the UK, with large contribution of base cations. Anthropogenic sources predominate (81 %) in total PM₁₀ concentrations in Poland, whereas natural prevail in the UK—hence, the future reduction of PM₁₀ air concentrations by emissions reduction could be more difficult in the UK than in Poland.     

Changes in Nutrient Emissions, Fluxes and Retention in a North-Eastern European Lowland Drainage Basin

Despite dramatic reductions in the 1990s of N and P emissions in the drainage basin, Lake Peipsi/Chudskoe (Estonia/Russia) is still suffering from algal blooms, probably caused by low N:P ratios of the lake water. To quantify the sources and changes of N and P inputs to the lake as a result of economic changes, we modelled emissions, transfer and in-stream retention using a GIS model. The model was calibrated using river monitoring data from the 1985–1989 period, and used to simulate emissions and loads for five future scenarios for 2015–2019. During the 1985–1999 period, diffuse P emissions decreased relatively more than N diffuse emissions, but this was not reflected in the loads to the lake. P loads decreased relatively less than N loads, which caused a decrease in the N:P ratio of the rivers. About 30–45% of diffuse N emissions and only 3–10% of diffuse P emissions reaches the river network. In-stream retention reduces N and P loads to the lake by about 62% and 72%, respectively. Point sources contribute negligibly to the N load to the lake, but form about one-third of the P load. A target/fast development scenario is the most likely scenario for the 2015–2019 period, resulting in higher nutrient loads than in recent years. We conclude that effective load reductions can be achieved by focussing on diffuse N and P emissions close ( < 50 km²) to the lake and by upgrading P removal capacity in wastewater treatment plants of towns.     

Using Measurements of Nitrogen Oxides to Estimate the Emission Controls Required to Meet the UK Nitrogen Dioxide Standard

In this paper we introduce a new method of analysing the relationship between nitrogen dioxide (NO₂) and oxides of nitrogen (NO_x) concentrations using data from the UK National Air Quality Archive. The study includes analyses of measurements from two different types of site in London, a kerbside site: Cromwell Rd, and three background sites: Bridge Place, London Bloomsbury and West London, over several years (1991–7). The data in some years showed that hourly NO₂ concentrations exceeded the UK Standard of 150 ppb. Data were binned, averaged, and polynomials fitted at each site. Analysis of the resulting polynomials was used to estimate reductions in NO_x emission required to achieve the National Air Quality Strategy Objective. Examination of the empirical ratio NO₂:NO_x (the 'yield') gives an indication of the sensitivity of the NO₂ to NO_x controls and the amount of NO₂ that would arise from modelled values of total oxides of nitrogen. The response of NO₂ to emission changes is very non-linear, implying 30–45% controls on NO_x may be required.     

Stream ecosystem response to chronic deposition of N and acid at the Bear Brook Watershed, Maine

The Bear Brook Watershed in Maine (BBWM) is a long-term, paired watershed experiment that addresses the effects of acid and nitrogen (N) deposition on whole watersheds. To examine stream response at BBWM, we synthesized data on organic matter dynamics, including leaf breakdown rates, organic matter inputs and standing stocks, macroinvertebrate secondary production, and nutrient uptake in treated and reference streams at the BBWM. While N concentrations in stream water and leaves have increased, the input, standing stocks, and breakdown rates of leaves, as well as macroinvertebrate production, were not responsive to acid and N deposition. Both chronic and acute increases of N availability have saturated uptake of nitrate in the streams. Recent experimental increases in phosphorus (P) availability enhanced stream capacity to take up nitrate and altered the character of N saturation. These results show how the interactive effects of multiple factors, including environmental flow regime, acidification, and P availability, may constrain stream response to chronic N deposition.     

Air pollution associated with airports

Air quality in the vicinity of airports is examined with particular reference to a detailed study of Gatwick Airport (UK). Ambient air concentrations of carbon monoxide, hydrocarbons (total and non-methane), oxides of nitrogen, smoke and airborne particulate lead have been measured at seven locations around the airport. The results obtained have been compared with ambient air quality guidelines, where available, and with results from other monitoring sites in the UK. It is concluded that the airport cannot be considered to be a significantly more important contributor to average pollutant ground-level concentrations than other sources in the area.     

An observational case study of ozone and precursors inflow to South East England during an anticyclone

Summertime photochemical air pollution episodes within the United Kingdom have been proposed via modelling studies to be strongly influenced by regional scale inflow of air from the continental European boundary layer. We present a vertically resolved case study using measurements made from the NERC/Met Office BAe 146 research aircraft on 18th August 2005 over the South East of England and the North Sea during a weak anticyclone centred over Northern Europe. The vertical distribution of ozone, CO, NO(x), peroxyacetyl nitrate (PAN) and a wide range of both nonmethane hydrocarbons (NMHC) and oxygenated volatile organic compounds (OVOCs) were determined between 500 ft (approximately 152 m) and 7000 ft (approximately 2134 m) over the East Anglia coastline and 50 km inland. In excess of 80 ppbV ozone was observed within inflowing boundary layer air over the North Sea coast in a broad N-S sloping feature around 60 km wide. The inflowing feature of European origin was also observed further inland within the boundary layer albeit with lower, more variable, ozone mixing ratios. The increased variability in ozone over land was a product of titration by fresh surface emissions of NO via rapid upward transport in thermals, a hypothesis supported by the observed vertical wind speed component. Fast boundary layer mixing over land was further illustrated by a uniform distribution in reactive alkenes. A comparison between aircraft and surface O(3) UK AUN (Automatic Urban Network) measurements showed good agreement with the inland site, Sibton, but marked differences with the coastal monitoring site at Weybourne, potentially due to gradients established by ocean deposition in stably stratified marine air.     

Sources of lead and zinc associated with metal smelting activities in the Trail area,British Columbia,Canada

The spatial distribution and deposition of lead and zinc emitted from the Trail smelter, British Columbia, Canada, was studied by strategically locating moss bags in the area surrounding the smelter and monitoring the deposition of elements every three months. A combined diffusion/distribution model was applied to estimate the relative contribution of stack-emitted material and material emitted from the secondary sources (e.g., wind-blown dust from ore/slag storage piles, uncovered transportation/trucking of ore, and historical dust). The results indicate that secondary sources are the major contributor of lead and zinc deposited within a short distance from the smelter. Gradually, the stack emissions become the main source of Pb and Zn at greater distances from the smelter. Typical material originating from each source was characterized by SEM/EDX, which indicated a marked difference in their morphology and chemical composition.