Past and future trends in concentrations of sulphur and nitrogen compounds in the Arctic

Recent trends in nitrogen and sulphur compounds in air and precipitation from a range of Arctic monitoring stations are presented, with seasonal data from the late 70s to 2004 or 2005. Earlier findings of declining sulphur concentrations are confirmed for most stations, while the pattern is less clear for reduced and oxidized nitrogen. In fact there are positive trends for nitrogen compounds in air at several stations. Acidity is generally reduced at many stations while the precipitation amount is either increasing or stable. Variability of sulphate concentrations in air for the period 1991–2000 is reasonably well reproduced at most stations using an Eulerian, hemispherical model. Results for nitrogen compounds are weaker. Scenario studies show that even if large sulphur emission reductions take place in important source regions in South-East Asia in the coming decades, only small changes in Arctic deposition can be expected. This is because South-East Asian emissions have small influence north of the Arctic circle.     

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.     

Effects of nitrogen with and without acidified sulphur on an ectomycorrhizal community in a Sitka spruce (Picea sitchensis Bong. Carr) forest

This preliminary study investigated the effects of enhanced nitrogen (NH4NO3 at 48 kg ha(-1) y(-1)), sulphur (Na2SO4 at 50 kg ha(-1) y(-1)), acidified nitrogen and sulphur (H2SO4 + NH4NO3) at pre-stated doses (pH 2.5), and acidified nitrogen and sulphur deposition at double these doses on the ectomycorrhizal community associated with a 13-year-old Sitka spruce (Picea sitchensis) forest. Sulphur deposition had little impact on below ground ectomycorrhizal diversity, but stimulated sporocarp production. Nitrogen inputs increased below ground colonisation compared to acidified nitrogen and sulphur, largely due to an increase in Tylospora fibrillosa colonisation. Sporocarp production and ectomycorrhizal root colonisation by Lactarius rufus were reduced in the nitrogen treated plots. These observations suggest that nitrogen deposition to a young plantation may suppress ectomycorrhizal fungi producing large sporocarps. It is proposed that enhanced nitrogen deposition increases ectomycorrhizal nitrogen assimilation, consuming more carbon and leaving less for extrametrical mycelium and sporocarp development.     

Tracing sources of atmospheric sulphur using epiphytic lichens

The overall objective of this work was to measure the spatial variation of sulphur isotopic composition of lichens across the island of Newfoundland in order to assess the degree to which the atmosphere is being affected by long-range transport of anthropogenic sulphur from eastern North America, and/or local pollution sources. A contour map (based on over 80 composite samples of the lichen Alectoria sarmentosa) illustrates the spatial distribution of sulphur isotopic composition of the Newfoundland atmosphere. It shows a gradient of delta(34)S of sulphur in lichen, decreasing from the coast to the interior of the island. It also shows local anomalies corresponding to the city of St. John's, the Come-By-Chance Oil Refinery, mining areas and fossil-fuel powered pulp and paper mills in central and western Newfoundland. The study strongly suggests that the isotopic composition of sulphur in the Newfoundland atmosphere is influenced more by the ocean (sea salt sulphate) and local anthropogenic activities in the province, than by long-range transport of continental North American sulphate.     

Competitive diesel engine emissions of sulphur and nitrogen species

NO_x, nitrate and sulphate emissions from a typical European passenger car diesel engine have been measured testing eight different fuels under five steady operating conditions (reproducing modes of the European transient urban/extraurban certification cycle). It is confirmed that nitrogen species compete with sulphur compounds to be adsorbed by diesel particulate matter (DPM) before being emitted into the atmosphere. This competition is found to increase with engine load, and is explained on the basis of the different specific surface and adsorption capacity of soot particles under different operating modes. When a high specific surface is available, as occurs in low load modes, both nitrates and sulphates are adsorbed by soot particles. On the contrary when a small surface is accessible, like in high load modes, sulphates are selectively adsorbed. This is specially important since sulphates are responsible for hydrocarbon retention in DPM due to the scrubbing effect.     

Acid deposition and the element composition of pine tree rings

The element contents of pine tree rings (Pinus sylvestris L.) were analyzed in five areas differing in the level of sulphur deposition. The elements studied and their average content in xylem were as follows:

aluminium 4.2, manganese 65, zinc 8.4, potassium 390, rubidium 2.2, calcium 930, magnesium 131, phosphorus 38, sulphur 56, nitrogen 0.65, boron 4.3 and molybdenum 0.03 mg/kg.

The contents of aluminium, potassium and rubidium were higher in tree rings from the 1950's on, particularly in southern Finland. The increase is probably due to acid deposition in the soil.     

Indications for changing deposition patterns in central Europe

The German Federal Environmental Agency (Umweltbundesamt) currently runs a network of 17 air pollution monitoring stations in rural areas within the Federal Republic of Germany. Since 1982, daily bulk precipitation samples have been collected and analysed at five of these stations. As no changes in sampling and chemical analysis techniques have been introduced in this time period, an interpretation with respect to trends is possible. An increase in pH is most obvious at Deuselbach in the western part of Germany. It is related to a decrease in sulphate ions. Reduced SO2 emissions in the western part of Europe have resulted in decreasing ambient air concentrations mainly in the western part of Germany, whereas changes in concentrations close to the eastern border of West Germany were not as pronounced. Part of the decrease, however, was a consequence of three mild winters in sequence at the end of the period, with little easterly air flow. Estimated dry deposition fluxes of sulphur at 3 rural stations in West Germany were lower in 1988/1989 compared to 1980-1987 by 44-69%. Wet deposition showed between 8% increase and 25% decrease. The resulting reduction in total sulphur deposition ranged from 17-54%. Deposition via interception of fog droplets was not measured.     

Changes in the atmospheric deposition of acidifying compounds in the UK between 1986 and 2001

Emissions of a precursor of acidity in precipitation, sulphur dioxide (SO2), declined in the UK and the EU (15) by 71% and 72%, respectively, between 1986 and 2001, while nitrous oxide emissions declined by about 40%. Acidity in UK precipitation and the deposition of sulphate in precipitation halved during this period, but reductions were larger in the English Midlands than at the west coast and in high rainfall areas (>2000 mm). There is evidence that the smaller reductions in sulphur deposition in the west and south are due in part to shipping sources of SO2. Reductions in sulphur dry deposition (74%) are larger than in wet deposition (45%), due to changes in the canopy resistance to dry deposition. For reduced nitrogen, there has been a small (10%) reduction in emissions and deposition, while for oxidized nitrogen, a substantial reduction in emissions (40%) occurred but wet deposition of nitrate changed by less than 10%.     

Influence of air pollution on the foliar nutrition of conifers in Great Britain

The nutritional status of needles from Sitka spruce, Norway spruce and Scots pine in a total of 108 stands was assessed. There was little evidence of nutritional deficiency, although potassium levels were frequently quite low. Analysis of some heavy metals (lead and copper) failed to reveal any likely toxicity problems. Sulphur, nitrogen and iron levels in/on the foliage were all related to various measures of sulphur and nitrogen pollution, determined using improved deposition models that take into account cloud deposition and the seeder-feeder mechanism. The analysis strongly suggested that direct air pollution has a greater effect on sulphur, nitrogen and iron foliar analyses than indirect pollution (wet deposition). The relationships were identified for levels of pollution that were generally lower than those seen in traditional gradient studies.     

Transport impacts on atmosphere and climate: Shipping

Emissions of exhaust gases and particles from oceangoing ships are a significant and growing contributor to the total emissions from the transportation sector. We present an assessment of the contribution of gaseous and particulate emissions from oceangoing shipping to anthropogenic emissions and air quality. We also assess the degradation in human health and climate change created by these emissions. Regulating ship emissions requires comprehensive knowledge of current fuel consumption and emissions, understanding of their impact on atmospheric composition and climate, and projections of potential future evolutions and mitigation options. Nearly 70% of ship emissions occur within 400 km of coastlines, causing air quality problems through the formation of ground-level ozone, sulphur emissions and particulate matter in coastal areas and harbours with heavy traffic. Furthermore, ozone and aerosol precursor emissions as well as their derivative species from ships may be transported in the atmosphere over several hundreds of kilometres, and thus contribute to air quality problems further inland, even though they are emitted at sea. In addition, ship emissions impact climate. Recent studies indicate that the cooling due to altered clouds far outweighs the warming effects from greenhouse gases such as carbon dioxide (CO₂) or ozone from shipping, overall causing a negative present-day radiative forcing (RF). Current efforts to reduce sulphur and other pollutants from shipping may modify this. However, given the short residence time of sulphate compared to CO₂, the climate response from sulphate is of the order decades while that of CO₂ is centuries. The climatic trade-off between positive and negative radiative forcing is still a topic of scientific research, but from what is currently known, a simple cancellation of global mean forcing components is potentially inappropriate and a more comprehensive assessment metric is required. The CO₂ equivalent emissions using the global temperature change potential (GTP) metric indicate that after 50 years the net global mean effect of current emissions is close to zero through cancellation of warming by CO₂ and cooling by sulphate and nitrogen oxides.     

Atmospheric deposition and canopy exchange processes in heathland ecosystems

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

Crown condition of Norway spruce in relation to sulphur and nitrogen deposition and soil properties in southeast Norway

Atmospheric deposition of sulphur and nitrogen compounds may lead to enhanced leaching of base cations, accumulation of nitrogen in organic matter, lowered pH and increased concentration of toxic aluminium in soil, which in turn may affect the vitality of forest trees. A general monitoring of forest condition has been initiated in many European countries, partly in order to reveal stresses caused by acidification. However, forest condition is also affected by many other factors. This paper examines a seven-year series of crown-condition data from Local County Monitoring Plots in Norway spruce stands in Norway. Average, time trend and lability variables were calculated for crown density and crown colour for each plot. Wet deposition of sulphate, ammonium and nitrate for each plot were estimated using data from the national air and precipitation monitoring programmes. Soil data are based on soil sampling within the plots. The analysis gave no evident support for the hypothesized negative effect on crown condition from sulphur and nitrogen deposition and related alterations in soil.     

Short-term variability in biogenic sulphur emissions from a florida spartina alterniflora marsh

Emissions of biogenic sulphur gases from a Florida Spartina alterniflora zone were measured over several tidal and diel cycles using a dynamic flow chamber technique, corroborating recently published information in the literature. The flux of hydrogen sulfide from individual measurements is shown to vary by over four orders of magnitude, and correlates primarily with the stage of the tidal cycle. In contrast, the fluxes of dimethyl sulphide, carbon disulphide and dimethyl disulphide vary by less than an order of magnitude and correlate primarily with the diurnal temperature changes in the sediment surface. These differences are discussed in terms of the various biological and physical parameters which may regulate the release of reduced sulphur compounds to the atmosphere.     

Phenolic compounds content in Pinus halepensis Mill. needles: a bioindicator of air pollution

Foliar phenol concentrations (total and simple phenols) were determined in Aleppo pine (Pinus halepensis Mill.) needles collected in June 2000, from 6 sites affected by various forms of atmospheric pollutants (NO, NO(2), NO(x), O(3) and SO(2)) monitored during two months. Results show an increase in total phenol content with exposure to sulphur dioxide and a reduction with exposure to nitrogen oxide pollution. p-Coumaric acid, syringic acid and 4-hydroxybenzoic acid concentrations increase with exposure to nitrogen oxide pollution, whereas gallic acid and vanillin decrease in the presence respectively of sulphur dioxide and ozone. This in situ work confirms the major interest of using total and simple phenolic compounds of P. halepensis as biological indicators of air quality.     

Evidence of sulphur and nitrogen deposition signals at the United Kingdom Acid Waters Monitoring Network sites

Some recent studies of trends in sulphate in surface waters have alluded to possible lag effects imposed by catchment soils, resulting in discrepancies between trends in deposition and run-off. To assess the extent of these possible effects in the UK, sulphate concentration data from the United Kingdom Acid Waters Monitoring Network (AWMN) sites are compared with estimates of sulphur deposition at each site. From these data, input-output budgets are computed at an annual time scale. The estimated budgets suggest a close association between catchment sulphur inputs and outputs at an annual scale, with well-balanced annual budgets at most sites, indicative of only minor lag effects. A similar analysis of the AWMN site nitrogen budget shows little evidence of an association between nitrogen inputs and outputs at this time scale.     

Use of stationary and mobile measurements to study power plant emissions

This paper presents a technique to study air pollution by combining high spatial resolution data obtained by a mobile platform and those measured by conventional stationary stations. Conventional stations provide time-series point data but cannot yield information that is distant from the sites. This can be complemented or supplemented by mobile measurements in the vicinity of the conventional sites. Together, the combined dataset yields a clearer and more precise picture of the dispersion and the transformation of pollutants in the atmosphere in a fixed time frame. Several experiments were conducted in the years 2002-2003 to track the impact of power plant plumes on ground receptors in the immediate vicinity (within a radius of 30 km) of the plants, using a combined mobile and stationary dataset. The mobile data allowed the identification of emissions from coal-fired and gas-fired power plants. Coal-fired power plants were the major source of sulfur dioxide (SO2), whereas nitrogen oxides (NOx) emitted from the gas-fired power plant played an important role in the formation of ozone (O3) at ground level. The mobile data showed that two particle size distribution regimes were detected: one had a dominant accumulation mode at 0.40-0.65 microm and the other at 0.65-1 microm. The existence of particles characterized by their mode at 0.65-1 microm and formed by in-cloud processes suggests that vehicular emissions were not the important source. Other local sources, such as power plants (elevated emission), were the likely sources, because Hong Kong does not have much manufacturing industry.     

The effect of variable sub-grid deposition factors on the results of the lagrangian long-range transport model of EMEP

The EMEP/MSC-W routine model for long-range atmospheric transport of sulphur and nitrogen includes a correction for the unresolved sub-grid-scale deposition in emission grid-squares. A constant fraction of the emissions is assumed to be directly deposited inside the first grid-square. Experiments have been performed to estimate the effects of using factors which vary with emission height and meteorological conditions. Results indicate that the constant local deposition factor used for sulphur dioxide in the routine model, is an overestimate, in particular for high-level emission sources. The change in annual deposition caused by the new local deposition factor for sulphur dioxide, is most clearly seen as a decreased deposition in the grid-squares with the largest emissions such as due for the former German Democratic Republic. The amount of this decrease strongly depends on the source height distribution. With the presently available emission data, a decrease of maximum 36% can be expected in individual grid squares. In grid-squares dominated by transboundary deposition, the increase is typically lower than 10%.     

Study on the aerosol optical properties and their relationship with aerosol chemical compositions over three regional background stations in China

The special and temporal characteristics of aerosol optical depth (AOD) and Angstrom wavelength exponent (Alpha) and their relationship with aerosol chemical compositions were analyzed by using the data of CE318 sun-photometer and aerosol sampling instruments at Lin'an, Shangdianzi and Longfengshan regional atmospheric background stations. Having the highest AOD among the three stations, Lin'an shows two peaks in a year. The AOD at Shangdianzi station shows a single annual peak with an obvious seasonal variation. The AOD at Longfengshan station has obvious seasonal variation which peaks in spring. The Alpha analysis suggests that the aerosol sizes in Lin'an, Longfengshan and Shangdianzi change from fine to coarse categories. The relationship between the aerosol optical depths of the Lin'an and Longfengshan stations and their chemical compositions is not significant, which suggests that there is not a simple linear relationship between column aerosol optical depth and the near surface chemical compositions of atmospheric aerosols. The aerosol optical depth may be affected by the chemical composition, the particle size and the shape of aerosol as well as the water vapor in the atmosphere.     

固定源氮氧化物排放及控制技术应用

固定源是氮氧化物排放的一个主要来源。通过对主要固定源氮氧化物生成机理及现有的排放控制技术进行论述，分析我国固定源氮氧化物排放的实际情况，提出我国固定源氮氧化物排放控制还处于起步阶段，氮氧化物排放标准相对宽松，氮氧化物排放控制技术有待进一步普及，并提出固定源氮氧化物排放治理的一些建议。