Nitrogen Deposition and Strategies for the Control of Acidification and Eutrophication across Great Britain

It is now recognised that a multi-pollutant, multi-effect approach needsto be adopted to address the range of problems caused by atmosphericpollution. In this paper we use a relatively simple trajectory model (HARM)to explore the coupled behaviour of sulphur dioxide (SO₂),oxides of nitrogen (NO_x) and ammonia (NH₃) andthe possible effects of future reductions in emissions of these pollutantson depositions of S and N across Great Britain. The performance of HARM withrespect to concentrations and depositions of NO_y andNH_x is assessed by comparison with data from nationalmonitoring networks. A range of emissions scenarios are modelled and theeffects of these reductions on critical loads exceedance are explored usingthe critical loads function (CLF), which allows both the acidification andeutrophication effects of S and N deposition to be explored simultaneously.Spatial variations in the reductions of deposition of S and/or N required tomeet critical loads are described. Reductions in emissions of the precursorsof strong acids (SO₂ and NO_x) yield benefits interms of ammonium deposition as a result of their coupled chemistry. Thedevelopment of strategies to control nitrogen deposition will need to take this non-linearity in to account.     

Trends in Emissions of Acidifying Species in Asia, 1985–1997

Acid deposition is a serious problem throughout much of Asia. Emissions of sulfur dioxide (SO₂) and nitrogen oxides (NO_x) have been increasing steadily, as nations strive to increase their levels of economic development. Coal and fuel oil have been the main choices for powering industrial development; and, until recently, only a few countries had taken steps to avert the atmospheric emissions that accompany fuel combustion. This paper discusses trends in emissions of SO₂ and NO_x that have occurred in Asian countries in the period 1985–1997, using results from the RAINS-Asia computer model and energy-use trends from the IEA Energy Statistics and Balances database. Emissions of SO₂ in Asia grew from 26.6 Tg in 1985 to 33.7 Tg in 1990 and 39.2 Tg in 1997. Though SO₂ emissions used to grow as fast as fossil-fuel use, recent limitations on the sulfur content of coal and oil have slowed the growth. The annual-average emissions growth between 1990 and 1997 was only 2.2%, considerably less than the economic growth rate. Emissions of NO_x, on the other hand, continue to grow rapidly, from 14.1 Tg in 1985 to 18.7 Tg in 1990 and 28.5 Tg in 1997 (6.2% per year between 1990 and 1997), with no signs of abating. Thus, though SO₂ remains the major contributor to acidifying emissions in Asia, the role of NO_x will become more and more important in the future.     

Development of a Multi-Resolution Emission Inventory and Its Impact on Sulfur Distribution for Northeast Asia

Emissions in East Asia for 1993 by administrative units and source types are estimated to support regional emission assessments and transport modeling studies. Total emission of SO_x, NO_x, soil NO_x, N₂O, and NH₃ are 24 150, 12 610, 1963, 908, and 8263 kton yr^-1, respectively.China's emission contribution is the highest for every species.The area sources are the most significant source type for SO_x and NO_x, but the fraction due to mobile source is highest for NO_x. Major LPSs are located from the middle to the east part of China, south and middle-west part of South Korea, and the east part of Japan. The area sources of SO_x show a pattern similar to population density, whereas NH₃ shows a strong landuse dependency. Detail emissions analysis reveals higher SO_x emission `cores' within each province. The estimated emissions are used to estimate sulfur deposition in the regions. The seasonal average sulfur distribution amounts are estimated from the ATMOS2 chemical transport model. The results showed anti-correlation with temperature for sulfur (SO₂ + SO₄ ^-2) concentrations and a positive correlation with rainfall for deposition.     

The Importance of Nitrogen Oxides for the Exceedance of Critical Thresholds in the Nordic Countries

Impacts of air pollutants and especially acidification in ecosystems have been of serious concern in the Nordic countries since the 1970s. The current approach to assess several pollutants (sulfur and nitrogen oxides, ammonia, volatile organic compounds) and their effects (acidification, eutrophication and ground-level ozone) simultaneously is extremely complex. This study explored the relative role of nitrogen oxides in environmental impacts in the Nordic countries. The share of NO_x in the exceedances of critical loads, the long-term ecosystem protection targets, was found to be roughly 25% in acidification and 50% in eutrophication. The contribution of NO_x emissions to ground-level ozone formation was considered important, as NO_x is the limiting precursor in ozone formation in the Nordic countries. The comparison of observed and modeled accumulated ozone concentrations (AOT40) for the early 1990s shows noticeable differences in the Nordic area, partly due to the sensitivity of the AOT40 indicator to the 40 ppb threshold value.     

Developing optimal abatement strategies for the effects of sulphur and nitrogen deposition at European scale

Integrated Assessment Models were successfully used to provide input to the negotiations for the Oslo Protocol on Further Reductions of Sulphur Emissions, finalized within the United Nations Economic Commission for Europe Convention on Long-range Transboundary Air Pollution in Oslo in June 1994. The techniques developed within this framework will be extended now to the simultaneous analysis of sulphur and nitrogen deposition. In addition to acidification, atmospheric deposition of nitrogen contributes to eutrophication of certain ecosystems, through a nutrient effect, and originates from the long-range transport of emissions of both oxidised and reduced nitrogen (NO_x and NH₃). Modelling reductions in nitrogen deposition thus introduces a need to establish multi-pollutant multi-effect modelling techniques. This paper investigates the development of a model set up to examine reductions of these pollutants in an economically and environmentally efficient manner. The control of nitrogen deposition encompasses action across several economic sectors, particularly the power, transport and agricultural sectors. Combining sulphur and nitrogen deposition limits on a European scale will require a flexible modelling approach and the issues governing possible approaches are presented.     

Acidification and nutrient imbalance in forest soils subjected to nitrogen deposition

Emission of nitrogen oxides (NO_x) and ammonia (NH₃) from a fertilizer factory and the resulting input of nitrates (NO₃ ^?) and ammonium (NH₄ ⁺) into the soil were the main reasons of nitrogen (N) cycle disturbance in forest ecosystems near Novgorod, North-Western Russia (50°31′ North, 31°17′ East). Total N atmospheric input was about 100 kg/ha annually. NH₃ was a dominant pollutant, causing the increase of atmospheric precipitation pH within the polluted region compared to background territories (6.0–6.5 and 4.5–5.0, respectively). Soil acidification through NH₄ ⁺ nitrification was observed. N-NO₃ ^? concentrations in soil solution reached 20–30 mg/l, and proton (H) production was equal to 4.1 keq/ha per warm season (from April to October). Compared with soil status in 1983, pH decrease by 0.2 pH units was found in A horizon. The content of exchangeable calcium (Ca) and magnesium (Mg) decreased by the factor of 2–3 and 1.5–2 in A and B horizons, respectively. Triple increase of exchangeable aluminium (Al) content was detected in A horizon. Through recent decrease of pollutant emission, the polluted territory is now a suitable subject for recovery studies.     

An Integrated Assessment Model for Fine Particulate Matter in Europe

Exposure to fine particles in the ambient air is recognized as a significant threat to human health. Two pathways contribute to the particle burden in the atmosphere: Fine particles originate from primary emissions, and secondary organic and inorganic particles are formed from the gas phase from the emissions of 'conventional' pollutants such as SO₂, NO_x, VOC and NH₃. Both types of particulate matter can be transported over long distances in the atmosphere. An integrated assessment model for particulate matter developed at IIASA addresses the relative importance of the different types of particulates, distinguishing primary and secondary particles and two size fractions. The model projects these emissions into the future and seeks cost-effective strategies for reducing health risks to population. The model integrates the control of primary emissions of fine particles with strategies to reduce the precursor emissions for the secondary aerosols. Preliminary results addressing the PM_2.5 fraction of both primary and secondary particulate matter indicate that in Europe the exposure to particulates will be significantly reduced as a side effect of the emission controls for conventional air pollutants (SO₂, NO_x, NH₃).     

Average critical loads for nitrogen and sulfur and its use in acidification abatement policy in the Netherlands

Atmospheric deposition of N and S on terrestrial and aquatic ecosystems causes effects induced by eutrophication and acidification. Effects of eutrophication include forest damage, NO₃ pollution of groundwater and vegetation changes in forests, heathlands and surface waters due to an excess of N. Effects of acidification include forest damage, groundwater pollution, and loss of fish populations due to Al mobilization. Critical loads (deposition levels) for N and S on terrestrial and aquatic ecosystems in the Netherlands related to these effects have been derived by empirical data and steady-state acidification models. Critical loads of N generally vary between 500 and 1500 mol _c ha^?1 yr^?1 for forests, heathlands and surface waters and between 1500 and 3600 for phreatic groundwaters. Critical loads of total acid (S and N) vary between 300 to 500 mol _c ha^?1 yr^?1 for phreatic groundwaters and surface waters and between 1100 to 1700 mol ha^?1 yr^?1 for forests. On the basis of the various critical loads a deposition target for total acid of 1400 mol _c ha^?1 yr^?1 has been set in the Netherlands from which the N input should be less than 1000 mol _c ha^?1 yr^?1. This level, to be reached in the year 2010, implies an emission reduction of 80–90% in SO₂, NO _x and NH₃ in the Netherlands and of about 30% in neighboring countries compared to 1980 emissions.     

Increasing contributions of nitrogen to the acidity of surface waters in Norway

The acidification of lakes in southern Norway is largely due to sulfate. Recent data from regional surveys of lakes and from monitoring stations indicates that nitrate concentrations have increased in many lakes and rivers in southernmost Norway. The ratio of NO₃ to NO₃ + SO₄ is still low for most areas, but is 0.54 on an equivalent basis in lakes and rivers in the area of high runoff in southwestern Norway. Here, concentrations of nitrate in the runoff are lower than for sites in Central Europe, but are higher than those in North America. The sites showing increases in NO₃ also increased in Al. Further increases in nitrate as a mobile anion which may be due to decreased uptake in the watershed, will contribute to acidification in the same manner as sulfate.     

A Global Analysis of Acidification and Eutrophication of Terrestrial Ecosystems

This paper presents an explorative, quantitative analysis of acidification and eutrophication of natural terrestrial ecosystems caused by excess sulfur (S) and nitrogen (N) deposition. The analysis is based on a steady-state approach, involving the comparison of deposition fluxes with critical loads to identify areas where critical loads are exceeded. Deposition fields for sulfur and nitrogen were obtained from the STOCHEM global chemistry-transport model, and they were combined with estimated base cation deposition to derive net acid deposition fluxes. The results indicate that the critical loads for acidification are exceeded in 7–17% of the global area of natural ecosystems. In addition, comparison of nitrogen deposition with critical loads for eutrophication yielded an exceedance in 7–18% of the global natural ecosystems. Apart from serious problems in the heavily industrialized regions of eastern USA, Europe, the former Soviet Union, and large parts of Asia, risks are also found in parts of South America, and West, East and Southern Africa. Both acidification and eutrophication risks could significantly increase in Asia, Africa and South America in the near future, and decrease in North America and Western Europe. Accounting for the effects of N in the analysis of acidification significantly enlarges the potentially affected areas and moves them away from highly industrialized areas compared to studies considering S deposition alone. Major uncertainties in the approach followed are associated with upscaling, the estimates of S, N and base cation emission and deposition fluxes, the critical loads to describe ecosystem vulnerability and the treatment of soil N immobilization and denitrification.     

INCREASING ROLE OF NITROGEN IN THE ACIDIFICATION OF SURFACE WATERS IN THE ADIRONDACK MOUNTAINS,NEW YORK

Assessments of the aquatic effects of acidic deposition have focused on sulfur, as have recent efforts to control the emissions of acidifying compounds. Nitrogen dynamics were excluded from most acidic deposition modeling studies because it was believed that terrestrial ecosystems strongly retain N and because modeling N is a more formidable task than modeling S due to the influence of complex biological processes on N cycling. Re-examination of available data for the Adirondack Mountains of New York suggests that N deposition may be contributing to both chronic and episodic acidification of freshwaters to a greater extent than is generally believed. Previous research concluded that N has played a limited role in acidification processes in these lakes, based on regional averages of chronic chemistry. However, it is now known that historic acidification responses have been spatially variable within the Adirondack Mountains and that the declines in lakewater pH have been less than previously believed. Lakewater NO₃ ^- concentrations are commonly in the range of 5 to 25 μeq L^-1 on a chronic basis in portions of the Adirondack region that have experienced significant chronic acidification. These NO₃ ^- concentrations correspond in magnitude to inferred historical acidification. Furthermore, the relative importance of NO₃ ^- as an agent of acidification increases dramatically during snowmelt when conditions are most toxic to fish. The consequence of not addressing N in formulating acidification recovery strategies for the Adirondacks includes the likelihood that we will overestimate the response of surface water to the mandated sulfur emissions reductions.     

Projections of SO2, NOx,NH3 and VOC Emissions in East Asia Up to 2030

Starting from an inventory of SO₂, NO_x, VOC and NH₃ emissions for the years 1990 and 1995 in East Asia (Japan, South and North Korea, China, Mongolia and Taiwan), the temporal development of the emissions of the four air pollutants is projected to the year 2030 based on scenarios of economic development. The projections are prepared at a regional level (prefectures or provinces of individual countries) and distinguish more than 100 source categories for each region. The emission estimates are presented with a spatial resolution of 1×1 degree longitude/latitude. First results suggest that, due to the emission control legislation taken in the region, SO₂ emissions would only grow by about 46 percent until 2030. Emissions of NO_x and VOC may increase by 95 and 65 percent, respectively, mainly driven by the expected increase in road traffic volume. Ammonia, mainly emitted from agriculture, is projected to double by 2030.     

Effect of nitrite accumulation on nitrous oxide emission and total nitrogen loss during swine manure composting

Abstract

The present study investigated the nitrogen balance in swine manure composting to evaluate the effect of nitrite (NO^? ₂) accumulation, which induces nitrogenous emissions, such as N₂O, during compost maturation. During active composting, most N losses result from NH₃ emission, which was 9.5% of the initial total nitrogen (TN_initial), after which, NO^? ₂ began to accumulate as only ammonia-oxidizing bacteria proliferated. After active composting, the addition of mature swine compost (MSC), including nitrite-oxidizing bacteria (NOB), could prevent NO^? ₂ accumulation and reduce N₂O emission by 70% compared with the control in which NO^? ₂ accumulated as a result of delayed growth of indigenous NOB. Total N₂O emissions in the control and in the treatment of MSC addition (MA) were 9.3% and 3.0% of TN_initial, respectively, whereas N losses as the sum total of NH₃ and N₂O over the whole period were 19.0% (control) and 12.8% (MA) of TN_initial, respectively. However, the difference in total N losses was markedly greater than that measured as NH₃ and N₂O, which were 27.8% (control) and 13.3% (MA) of TN_initial, respectively. These results demonstrated that the magnitude of nitrogen losses induced by NO^? ₂ accumulation is too large to ignore in the composting of swine manure.     

Precipitation Composition in the Ohio River Valley: Spatial Variability and Temporal Trends

Sulfate (SO₄ ^2?), nitrate (NO₃ ^?) and ammonium (NH₄ ⁺) concentrations in precipitation as measured at NADP sites within the Ohio River Valley of the Midwestern USA between 1985 and 2002 are quantified and temporal trends attributed to changes/ variations in (i) the precipitation regime, (ii) emission patterns and (iii) air mass trajectories. The results indicate that mean SO₄ ^2? concentrations in precipitation declined by 37–43% between 1985 and 2002, while NO₃ ^? concentrations decreased by 1–32%, and NH₄ ⁺ concentrations exhibited declining concentrations at some sites and increasing concentrations at others. The change in SO₄ ^2? concentrations is in broad agreement with estimated reductions in sulfur dioxide emissions. Changes in NO₃ ^? concentrations appear to be less closely related to variations in emissions of oxides of nitrogen and exhibit a stronger dependence on weekly precipitation volume. Up to one quarter of the variability in log-transformed weekly NO₃ ^? concentrations in precipitation is explicable by variations in precipitation volume. Trends in annual average log-transformed SO₄ ^2? concentrations exhibit only a relatively small influence of variability in weekly precipitation amount but at each of the sites considered the variance explanation of annual average log-transformed SO₄ ^2? by sampling year was increased by removing the influence of precipitation volume. Annual mean log-transformed ion concentrations detrended for precipitation volume (by week) and emission changes (by year) exhibit positive correlations at all sites, indicating that the residual variability of SO₄ ^2?, NO₃ ^? and NH₄ ⁺ may have a common source which is postulated to be linked to synoptic scale variability and air mass trajectories.     

Stability Studies of Waste Produced in Pilot-Plant Testing using Ferrous-EDTA and Magnesium-Enhanced Lime for Combined Sulfur-Dioxide/Nitrogen Oxides Removal

A pilot-plant-scale study of combined sulfur dioxide/nitrogen oxides (SO₂/NO_x) removal has been performed by the Dravo Lime Company at the Cincinnati Gas and Electric Company's Miami Fort Station in North Bend, Ohio. This study used Dravo's patented Thiosorbic® lime process along with Argonne National Laboratory's (ANL's) patented process for combined SO₂/NO_x removal using the chelate ferrous·ethylenediaminetetraacetate (Fe·EDTA). For approximately nine months, scrubbing tests were carried out, and waste samples were collected. Waste testing at ANL involved two types of long-term chemical stability experiments. In one test, the gas-phase composition above several different samples was studied by mass spectrometry over 22 months. Unexpectedly, production of carbon dioxide and hydrogen sulfide was observed in some of the samples. The other experiment involved solid-phase leaching. Samples were stored for up to 14 months before leaching. Each leachate was tested for total Kjeldahl nitrogen and for the nitrogen-containing ions nitrite, nitrate, and ammonium. Significant amounts of ammonium ions were found in two of the samples. Total leachable nitrogen was found to stabilize after about the first 7 months of storage.     

Long-term modelling of airborne pollution within the Northern Hemisphere

A long-term modelling (1991–1994) of oxidised sulphur, bound nitrogen and some heavy metals has been carried out by MSC-E/EMEP for the Northern Hemisphere. The transport unit of the model is an Eulerian scheme which could be classified as Pseudo-Lagrangian one. Vertical distribution described by means of Gaussian approximation and the exchange with the free troposphere are taken into account. Vertical movement is calculated proceeding from local mixing conditions, state of the surface, its height (topography) etc. The chemical unit for acid compounds contains 25 reactions and 14 compounds including sulphur and nitrogen compounds peroxyacetylnitrate, tropospheric ozone, volatile hydrocarbons (but methane) are considered as a whole via ozone creation potential. The model time step is 1 hour, meteorological data (winds, temperature, precipitation etc.) cover 6-hour intervals. The model results show that very significant part of the Arctic and West Asian acid pollution is produced by European countries. On the whole the Arctic pollution by SO_x, NO_x and NH_x comes from sources of Old World. The main source of sulphur pollution is located in Russia and of nitrogen compound — in Central and Northern Europe. About 50% SO_x, 70% NO_x and 40% NH_x deposition in Central Asia and Kazakhstan is-imported from external sources. A similar situation is observed in European and Asian parts of Russia.     

氮肥对镉在土壤-芥菜系统中迁移转化的影响

以芥菜为研究对象, 采用盆栽试验, 探讨了不同用量的5种氮肥对污染农田土壤中镉(Cd)在土壤–根系–地上部迁移累积的影响。结果表明: 5种氮肥均促进了芥菜根系对Cd的吸收, 且根系Cd含量随施氮量的增加而增加; 但根系吸收转运Cd的能力随氮肥施用量的增加呈先降后增的变化趋势。在≤200 mg(N)·kg^-1(土)的施氮水平下, CO(NH₂)₂和Ca(NO₃)₂处理能显著降低芥菜地上部Cd含量, 降低幅度分别为13%~29%和24%~30%。在施氮量相同的条件下, NH₄Cl和(NH₄)₂SO₄显著降低了土壤pH, 增加了土壤DTPA-Cd含量, 促进了芥菜对Cd的吸收。本试验条件下, 200 mg(N)·kg^-1(土)的CO(NH₂)₂在增加芥菜产量和降低芥菜地上部Cd含量等方面优于其他氮肥处理。     

Natural and anthropogenic components of soil acidification

The following 8 theses are theoretically founded and experimentally quantified. 1. Rocks contain only bases and no acid precursors. Therefore, with the exception of sulfide containing rocks, soils cannot acidify as a result of atmospheric rock weathering. 2. A consumption of protons in rocks and soils results in a decrease of their acid neutralizing capacity (ANC) and can result in the buildup of a base neutralizing capacity (BNC). Strong soil acidification leads to the formation of stronger acids from weaker acids in the solid phase; this may be connected with a decrease in the BNC. 3. Weak acids (carbonic acid) lead in geological times to the depletion of bases without a larger accumulation of labile cation acids. Strong acids (HNO₃, organic acids, H₂SO₄) can lead within a few decades to soil acidification, i.e. to leaching of nutrient cations and the accumulation of labile cation acids. 4. The acid input caused by the natural emission of SO₂ and NO_x can be buffered by silicate weathering even in soils low in silicates. 5. The cause of soil impoverishment and soil acidification is a decoupling of the ion cycle in the ecosystem. 6. Acid deposition in forest ecosystems which persists over decades leads to soil acidification. 7. Formation and deposition of strong acids with conservative anions (SO₄, NO₃) shifts soil chemistry into the Al or Al/Fe buffer range up to great soil depth. In such soils eluvial conditions prevail throughout the solum and even in upper part of the C horizon: in connection with the decomposition of clay minerals, Al and eventually Fe are being eluviated. The present soil classification does not include this soil forming process. 8. In the long run, soil acidification by acid deposition results in the retraction of the root system of acid tolerant tree species from the mineral soil, and in water acidification.     

A regional scale model for the calculation of episodic concentrations and depositions of acidifying components

An eulerian long-range transport model for the calculation of concentrations of SO₂, SO₄, NO _x , and NO₃ and wet and dry depositions of SO _x (sum of SO₂ and SO₄) and NO _y (sum of NO, NO₂ and NO₃) over Europe is presented. The model is developed in such a way that only routinely available, analyzed or prognostic meteorological fields are required as input data. In this way it is possible to obtain a forecast of the air quality during smog episodes. For evaluation of smog episodes the model provides a way to estimate the contributions of different sources and the effect of emission scenarios. The model has been evaluated for four winter and three summer episodes. The modeled concentrations of SO₂ and SO, are in agreement with the available measurements. A less good agreement is found for NO₂ and NO _x (sum of NO and NO₂) concentrations. For these components the model tends to underpredict the measured values.     

The acidifying potential of atmospheric deposition in Canada

It is proposed that the value of ([SO₄ ^??] - [Ca⁺⁺ + Mg⁺⁺]) in precipitation is a suitable way to describe the acidifying potential (AP) of the wet desposition. In eastern North America, the AP of precipitation varies from 20 to 85% of the total sulphate, the remainder of the sulphate being neutralized H₂SO₄, sulphate from salts in dust or from sea salt. The AP ranges from 20 to 80% of the H⁺ in the wet deposition. The rest of the H⁺ is contributed by the net effect of N compounds. Ammonium and nitrate ions from ammonia and NO_Xemissions do not represent a net acidic loading to the terrestrial ecosystem if they are taken up by vegetation. However, when N leaches from watersheds in the form nitrate, it constitutes an acidifying demand on the ecosystem. Therefore, the overall net acidifying potential (NAP) applied to the terrestrial ecosystem is defined by the value of ([SO₄ ^??] - [Ca⁺⁺ + Mg⁺⁺]) in precipitation plus [NO₃ ^??] in runoff from the watershed.