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1.
A Chronology of Nitrogen Deposition in the UK Between 1900 and 2000   总被引:2,自引:0,他引:2  
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.  相似文献   

2.
Simple bioenergetics models were used to derive annual nitrogen excretion rates of each seabird species occurring at colonies in the UK. These were combined with population distribution data and an estimated fraction of nitrogen volatilized to estimate the spatial distribution of NH3 emissions from seabird colonies at a 1 km resolution. The effect of these emissions on atmospheric NH3 concentrations and nitrogen deposition in the UK was assessed using the FRAME atmospheric chemistry and transport model. The total emission of NH3 from the UK seabird colonies is estimated at 2.7 kt yr?1. Emissions from seabirds are largely concentrated in remote parts of Britain, where agricultural and other anthropogenic emissions are minimal. Although seabirds account for less than 1% of total UK NH3 emissions (~370 kt yr?1), their occurrence in remote areas and frequently large colony sizes results in seabirds providing a major fraction of the atmospheric nitrogen deposition for many remote ecosystems.  相似文献   

3.
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+ 4and 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 Ndeposition+0.21, r 2 = 0.33, n = 43) was more robust than the relationship between N deposition and soil NO and N2O fluxes.  相似文献   

4.
Simple bioenergetics models were used to derive annual nitrogen excretion rates of each seabird species occurring at colonies in the UK. These were combined with population distribution data and an estimated fraction of nitrogen volatilized to estimate the spatial distribution of NH3 emissions from seabird colonies at a 1 km resolution. The effect of these emissions on atmospheric NH3 concentrations and nitrogen deposition in the UK was assessed using the FRAME atmospheric chemistry and transport model. The total emission of NH3 from the UK seabird colonies is estimated at 2.7 kt yr–1. Emissions from seabirds are largely concentrated in remote parts of Britain, where agricultural and other anthropogenic emissions are minimal. Although seabirds account for less than 1% of total UK NH3 emissions (370 kt yr–1), their occurrence in remote areas and frequently large colony sizes results in seabirds providing a major fraction of the atmospheric nitrogen deposition for many remote ecosystems.  相似文献   

5.
Spatial and temporal changes in mobility of N species have been studied for three UK upland river networks, the Etherow in the South Pennines, the Nether Beck in the Lake District and the Dee in NE Scotland. The catchments are subject to N deposition at 35.1, 22.0 and 10.8–15.6 kg N ha?1 yr?1, respectively. The NH+ 4 leaching appears to be predominantly regulated by flow path in more polluted upland catchments. It is greatest where water draining acidified peaty soils contributes more to total discharge. Soluble organic matter may provide the dominant counter anion. In the Etherow and Dee catchments, which are dominated by acid mineral and organic soils, at high discharge NO? 3 also appears to be associated with greater input of water from acidified soils. In contrast, for the Nether Beck, higher NO? 3 concentrations are associated with tributaries draining soils contributing water with higher alkalinity, suggesting nitrification is important. For the Etherow and Dee, dissolved organic N (DON) appears to originate predominantly from acidified, peaty soils. Spiking experiments with peat soil from the Etherow catchment confirmed the limited capacity of these soils to utilize inorganic N inputs, favouring equilibration with NH+ 4 inputs and leaching losses of inorganic N throughout the year.  相似文献   

6.
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 Ndeposition + 0.21, r 2 = 0.33, n = 43) was more robust than the relationship between N deposition and soil NO and N2O fluxes.  相似文献   

7.
Size resolved particle composition and nitric acid (HNO3)measurements from the ASEPS'98 experiment conducted in the BalticSea are used to provide observational evidence of substantialgas-particle transfer of oxidized nitrogen (N) compounds in themarine boundary layer. We then focus on the importance ofHNO3 reactions on sea salt particles in determining spatio-temporal patterns of N dry deposition to marine ecosystems.Modelling results obtained assuming no kinetic or chemical limiton HNO3 uptake and horizontally homogeneous conditions withnear-neutral stability, indicate that for wind speeds 3.5 – 10 ms-1 transfer of HNO3 to the particle phase to formparticle nitrate (NO3 -) may decrease the N depositionvelocity by 50%. We extend this research using the CHEM-COASTmodel to demonstrate that, in a sulphur poor environment undermoderate wind speeds with HNO3 concentrations representativeof those found in the marine boundary layer, inclusion ofheterogeneous reactions on sea spray significantly reducesmodelled NO3 - deposition in the near coastal zone.  相似文献   

8.
The impact of nitrogen fertilizers on gaseous emissions duringwinter and spring-thaw is not well understood and was the objective of this research. Using a micrometeorological method,N2O, NO and NOx fluxes from ryegrass were measured from November 1997 to March 1998. Three different mineralfertilizers were applied in November: urea (U), slow-release urea(SRU) and ammonium nitrate (AN). N2O emissions during the winter were small, increasing significantly in March. Total losses of N2O-N were significantly higher from SRU and U plots, with winter N2O emissions accounting for 50% of annual losses. Nitric oxide fluxes from all plots weresmall during the measurement period (<0.9 ng N m-2 s-1). The NO fluxes from U and AN fertilized plots were significantly higher than from SRU and control plots. NO2 fluxes were always negative (–6 ng N m-2 s-1)indicating deposition, but decreased to –2 ng N m-2s-1 when snow was present on the soil surface. Our resultsindicate that the form of inorganic N applied has an effect on NO+ N2O emissions but not on NO2 fluxes.Sponsored by CAPES – Brasília, Brazil  相似文献   

9.
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.  相似文献   

10.
Estimates of soil N2O and NOemissions at regional and country scales arehighly uncertain, because the most widely usedmethodologies are based on few data, they do notinclude all sources and do not account forspatial and seasonal variability. To improveunderstanding of the spatial distribution of soilNO and N2O emissions we have developedsimple multi-linear regression models based onpublished field studies from temperate climates.The models were applied to create spatialinventories at the 5 km2 scale of soil NOand N2O emissions for Great Britain. The N2O regression model described soilN2O emissions as a function of soil N input,soil water content, soil temperature and land useand provided an annual N2O emission of 128 kt N2O-N yr-1. Emission rates largerthan 12 kg N2O-N ha-1 yr-1 werecalculated for the high rainfall grassland areasin the west of Great Britain.Soil NO emissions were calculated using tworegression models, which described NO emissionsas a function of soil N input with and without afunction for the water filled pore space. Thetotal annual emissions from both methods, 66 and7 kt NO-N yr-1, respectively, span the rangeof previous estimates for Great Britain.  相似文献   

11.
Nitrate leaching was measured over seven years of nitrogen (N) addition in a paired-catchment experiment in Alptal, central Switzerland (altitude: 1200 m, bulk N deposition: 12 kg ha-1 a-1). Two forested catchments (1500 m2 each) dominated by Picea abies) were delimited by trenches in the Gleysols. NH4NO3 was added to one of the catchments using sprinklers. During the first year, the N addition was labelled with 15N. Additionally, soil N transformationswere studied in replicated plots. Pre-treatment NO3 --N leaching was 4 kg ha-1 a-1 from both catchments, and remained between 2.5 and 4.8 kg ha-1 a-1 in the control catchment. The first year of treatment induced an additional leaching of 3.1 kg ha-1, almost 90% of which was labelled with 15N, indicating that it did not cycle through the large N pools of the ecosystem (soil organic matter and plants). These losses partly correspond to NO3 - from precipitation bypassing the soil due to preferential flow. During rain or snowmelt events, NO3 - concentration peaks as the water table is rising, indicating flushing from the soil. Nitrification occurs temporarily along the water flow paths in the soil and can be the source of NO3 - flushing. Its isotopic signature however, shows that this release mainly affects recently applied N, stored only between runoff events or up to a few weeks. At first, the ecosystem retained 90% of the added N (2/3 in the soil), but NO3 - losses increased from 10 to 30% within 7 yr, indicating that the ecosystem became progressively N saturated.  相似文献   

12.
The purpose of this study is to evaluate cost-effective reduction strategies for nitrogen oxides (NO x ) in the Asian region. The source-receptor relationships of the Lagrangian “puff” model of long-range transportation, ATMOS-N, were used to calculate the wet/dry deposition of the nitrogen (N) in Asia. Critical loads of N deposition in Asia were calculated from the relationships between the critical load of sulfur (S) and balance of N in and out using the data of S critical load of RAINS-ASIA. The cost functions of N reduction of Asian countries were derived by the regression analysis with the data of cost functions of European countries used in RAINS. In order to assess the environmental impact, the gaps between N deposition and critical load of N were calculated. The emission of NO x was reduced in some cases of this model, and the changes of gaps between N deposition and critical load were observed as well as the changes of the reduction cost. It is shown that a uniform reduction of NO x emissions by countries in Asia is not cost-effective strategy.  相似文献   

13.
Soil- and stream-water data from the Plynlimon research area, mid-Wales, have been used to develop a conceptual model of spatial variations in nitrogen (N) leaching within moorland catchments. Extensive peats, in both hilltop and valley locations, are considered near-complete sinks for inorganic N, but leach the most dissolved organic nitrogen (DON). Peaty mineral soils on hillslopes also retain inorganic N within upper organic horizons, but a proportion percolates into mineral horizons as nitrate (NO? 3), either through incomplete immobilisation in the organic layer, or in water bypassing the organic soil matrix via macropores. This NO? 3 reaches the stream where mineral soilwaters discharge (via matrix throughflow or pipeflow) directly to the drainage network, or via small N-enriched flush wetlands. NO? 3 in hillslope waters discharging into larger valley wetlands will be removed before reaching the stream. A concept of catchment ‘nitrate leaching zones’ is proposed, whereby most stream NO? 3 derives from localised areas of mineral soil hillslope draining directly to the stream; the extent of these zones within a catchment may thus determine its overall susceptibility to elevated surface water NO? 3 concentrations.  相似文献   

14.
Providing an accurate estimate of the dry component of N deposition to low N background, semi-natural habitats, such as bogs and upland moors dominated by Calluna vulgaris is difficult, but essential to relate nitrogen deposition to effects in these communities. To quantify the effects of NH3 inputs to moorland vegetation growing on a bog at a field scale, a field release NH3 fumigation system was established at Whim Moss (Scottish Borders) in 2002. Gaseous NH3 from a line source was released along of a 60 m transect, when meteorological conditions (wind speed >2.5 m s?1 and wind direction in the sector 180–215°) were met, thereby providing a profile of decreasing NH3 concentration with distance from the source. In a complementary study, using a NH3 flux chamber system, the relationships between NH3 concentrations and cuticular resistances were quantified for a range of NH3 concentrations and micrometeorological conditions for moorland vegetation. Cuticular resistances increased with NH3 concentration from 11 s m?1 at 3.0 μg m?3 to 30 s m?1 at 30 μg m?3. The NH3 concentration data and the concentration-dependent canopy resistance are used to calculate NH3 deposition taking into account leaf surface wetness. The implications of using an NH3 concentration-dependent cuticular resistance and the importance for refining critical loads are discussed.  相似文献   

15.
This paper reports data from a field study investigating the impacts of elevated ammonia (NH3) deposition on Calluna vulgaris growing on an ombrotrophic peat bog in S.E. Scotland. Shoot extension, foliar N concentrations, chlorophyll concentration and chlorophyll fluorescence were measured during the second growing season of exposure to a gradient of ammonia concentrations. Results indicate that NH3 increases growth between 150–200 kg N ha?1y?1 cumulative deposition. Foliar N content increased significantly in response to NH3 cumulative deposition up to 400 kg N ha?1 y?1 whereas chlorophyll a content significantly decreased. Measurements of Fv/Fm suggest that although NH3 exposure altered the growth and reduced chlorophyll a, the efficiency of photosystem II was insensitive to NH3–N deposition at this stage.  相似文献   

16.
Concentrations of NO2, NO, and O3 from a rooftop monitoring station in Gothenburg, Sweden (2002–2006) were analysed to characterise NO2 pollution. [NO2] was shown to correlate strongly and non-linearly with [NO x ] (NO x ?=?NO?+?NO2), in line with observations in other cities. The [NO2] to [NO x ] fraction fell initially with increasing [NO x ]. At [NO x ] levels >200 ppb, the decline in [NO2]/[NO x ] with increasing [NO x ] levelled out and [NO2]/[NO x ] converged towards approximately 0.15–0.16, independent of [NO x ]. Data from a traffic route site showed the same pattern. This value of [NO2]/[NO x ] at high [NO x ] can be interpreted as the NO2 fraction of the NO x emissions from vehicle exhaust. Situations with high NO x pollution and minimum [NO2]/[NO x ] were always associated with [O3] close to zero. Plotting [Ox] (Ox?=?NO2?+?O3) vs. [NO x ] provided a strong linear correlation for situations dominated by local pollution ([NO]/[NO2]>1). The slope of the regression, a measure of the primary NO2 fraction in NO x emissions, was 0.13 during the day and 0.14 during the night. With stronger winds, the rooftop monitoring station became more similar, in terms of NO2 pollution, to a city street site and a traffic route site, although [NO2] was almost always higher at the street/traffic route locations. The EU standard for the annual average of [NO2] (40 μg m?3) was exceeded, while the hourly standard (200 μg m?3, not to be exceeded more than 18 times per year by 2010) was not exceeded at any of the sites.  相似文献   

17.
This paper provides the background to this special issue, outlining the extent to which the global atmospheric nitrogen cycle has been modified by human activity and outlining the range of effects. The global total emissions of reduced and oxidized nitrogen, amount to 124 Tg N, and exceed those from natural sources (34 Tg N) by almost a factor of four showing the extent to which anthropogenic activity has taken over the global N cycle. Of the 124 Tg N, 70 Tg N is emitted in the oxidized form, largely as NO and 70% of which results directly from anthropogenic activity. The remaining 54 Tg N is emitted as NH3, (66% anthropogenic). The enhanced nitrogen emissions are associated with a range of local, regional and global issues including, acidification, eutrophication, climate change, human health and tropospheric O3. The paper also places the Global Nitrogen Enrichment (GaNE) research programme in the UK in a wider perspective.  相似文献   

18.
This paper provides the background to this special issue, outlining the extent to which the global atmospheric nitrogen cycle has been modified by human activity and outlining the range of effects. The global total emissions of reduced and oxidized nitrogen, amount to 124 Tg N, and exceed those from natural sources (34 Tg N) by almost a factor of four showing the extent to which anthropogenic activity has taken over the global N cycle. Of the 124 Tg N, 70 Tg N is emitted in the oxidized form, largely as NO and 70% of which results directly from anthropogenic activity. The remaining 54 Tg N is emitted as NH3, (66% anthropogenic). The enhanced nitrogen emissions are associated with a range of local, regional and global issues including, acidification, eutrophication, climate change, human health and tropospheric O3. The paper also places the Global Nitrogen Enrichment (GaNE) research programme in the UK in a wider perspective.  相似文献   

19.
Regular additions of NH4NO3 (35–140 kg N ha−1 yr−1) and (NH4)2SO4 (140 kg N ha−1 yr−1) to a calcareous grassland in northern England over a period of 12 years have resulted in a decline in the frequency of the indigenous bryophyte species and the establishment of non-indigenous calcifuge species, with implications for the structure and composition of this calcareous bryophyte community. The lowest NH4NO3 additions of 35 kg N ha−1 yr−1 produced significant declines in frequency of Hypnum cupressiforme, Campylium chrysophyllum, and Calliergon cuspidatum. Significant reductions in frequency at higher NH4NO3 application rates were recorded for Pseudoscleropodium purum, Ctenidum molluscum, and Dicranum scoparium. The highest NH4NO3 and (NH4)2SO4 additions provided conditions conducive for the establishment of two typical calcifuges – Polytrichum spp. and Campylopus introflexus, respectively. Substrate-surface pH measurements showed a dose-related reduction in pH with increasing NH4NO3 deposition rates of 1.6 pH units between the control and highest deposition rate, and a further significant fall in pH, of >1 pH unit, between the NH4NO3 and (NH4)2SO4 treatments. These results suggest that indigenous bryophyte composition may be at risk from nitrogen deposition rates of 35 kg N ha−1 yr−1 or less. These effects are of particular concern for rare or endangered species of low frequency.  相似文献   

20.
As a first step to work out an abatement plan against air pollution, a local emission inventory with 1 hr temporal and 1 km spatial resolution in the city of Izmir and its surroundings was prepared. The study area consisted of a 200 × 170 km2 rectangle having the city of Izmir at the centre. The studied pollutants were total particulate matter (PM), sulfur oxides (SOx), nitrogen oxides (NOx), volatile organic compounds (VOC) and carbon monoxide (CO). Emissions of these pollutants were determined by estimation methods making use of suitable emission factors. Emission sources were evaluated in three categories; point, area and line sources. For year 2000 total emissions in the study area on an average day were estimated as 173 tons PM, 299 tons SOx, 136 tons NOx, 68 tons VOC and 320 tons CO. At the second part of the study, calculated emissions were transformed into air quality predictions in the area by using the Industrial Source Complex – Short Term (ISCST3) dispersion model. Model results were tested with monitoring data from urban air quality stations obtained during the year 2000. Results of the past, present and future air quality estimates in the region were discussed. In order to do so, future scenarios including various control technology applications were formulated and tested to see their effect on the future air quality.  相似文献   

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