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1.
Two years of continuous measurements of SO2deposition fluxes to moorland vegetation are reported. The mean flux of 2.8 ng SO2 m-2 s-1 is regulated predominantly by surface resistance (r c) which, even for wet surfaces, was seldom smaller than 100 s m-1. The control of surface resistance is shown to be regulated by the ratio of NH3SO2 concentrations with an excess of NH3 generating the small surface resistances for SO2. A dynamic surface chemistry model is used to simulate the effects of NH3 on SO2 deposition flux and is able to capture responses to short-term changes in ambient concentrations of SO2, NH3 and meteorological conditions. The coupling between surface resistance and NH3/SO2 concentration ratios shows that the deposition velocity for SO2 is regulated by the regional pollution climate. Recent long-term SO2 flux measurements in a transect over Europe demonstrate the close link between NH3/SO2 concentrations and rc (SO2). The deposition velocity for SO2 is predicted to have increased with time since the 1970s and imply a 40% increase in v d at a site at which the annual mean ambient SO2 concentrations declined from 47 to 3 g m-3 between 1973 and 1998.  相似文献   

2.
Major sulphur emission control programs have been implemented in North America, resulting in current emissions being ~30% less than those in 1980. However, the level of acidic deposition remaining is still unlikely to promote widespread recovery of aquatic ecosystems. The First-order Acidity Balance (FAB) model has been applied to south-central Ontario (285 lakes in the Muskoka River Catchment) to evaluate the need for further reductions in emissions. As a result of the past decline in deposition, the proportion of lakes with critical loads exceedance has dropped substantially; however, further reductions in sulphur and nitrogen emissions are required to eliminate critical loads exceedance. Based on bulk deposition of sulphate and nitrogen (41.1 mmolc m-2 yr-1 and 62.5 mmolc m-2 yr-1, respectively) for the period 1995–1999, 166 lakes (58.3%) exceedcritical loads. Even with full implementation of SO2 abatementprograms in Canada (achieved in 1994) and the United States (legislated for 2010), critical loads will be exceeded in a large proportion (46.6%) of the study lakes.  相似文献   

3.
Most ammonia (NH3) emission inventories have been calculated on an annual basis and do not take into account the seasonal variability of emissions that occur as a consequence of climate and agricultural practices that change throughout the year. When used as input to atmospheric transport models to simulate concentration fields, these models therefore fail to capture seasonal variations in ammonia concentration and dry and wet deposition. In this study, seasonal NH3 emissions from agriculture were modelled on a monthly basis for the year 2000, by incorporating temporal aspects of farming practice. These monthly emissions were then spatially distributed using the AENEID model (Atmospheric Emissions for National Environmental Impacts Determination). The monthly model took the temporal variation in the magnitude of the ammonia emissions, as well as the fine scale (1-km) spatial variation of those temporal changes into account to provide improved outputs at 5-km resolution. The resulting NH3 emission maps showed a strong seasonal emission pattern, with the highest emissions during springtime (March and April) and the lowest emissions during summer (May to July). This emission pattern was mainly influenced by whether cattle were outside grazing or housed and by the application of manures and fertilizers to the land. When the modelled emissions were compared with measured NH3 concentrations, the comparison suggested that the modelled emission trend corresponds fairly well with the seasonal trend in the measurements. The remaining discrepancies point to the need to develop functional parametrisations of the interactions with climatic seasonal variation.  相似文献   

4.
This study presents the chemical composition of bulk deposition during the period of February 1996–May 1997 and the chemical composition of sub-event wet deposition on 13 August 1997 in Gebze. Samples were analyzed for SO4 2-, NO3 -, Cl-,Ca2+, Mg2+, K+, Na+, and NH4 + in addition to pH. The source of some ionic components in the bulk deposition such as K+ and Ca2+ were found to be the terrestrial regions, as expected. The (non-sea Cl-)/Cl- ratio of 0.05 suggests that the very large portion of Cl- in the bulkdeposition was of marine origin. The ratio of (non-sea SO4 2-)/SO4 2- varied between 0.86 and 0.99,indicating that the main source of sulfate was not the sea. It is found that the sulfate and calcium concentrations were highest in summer and lowest in fall. The analysis of bulk deposition also indicated that nearly 24% of the events were acidic (pH < 5.6). During sub-event wet deposition collectedon the same site pH decreased continually, and during the passageof cold front concentrations of Cl-, SO4 2- and NO3 - increased.  相似文献   

5.
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   

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+ 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   

7.
Continuous micrometorological measurements of ammonia (NH3)exchange were made for a period of 19 months (May 1998–November 1999) over intensively managed grassland in southern Scotland. This study focused on the influence of management activities, such as cutting and fertilising, on vegetation-atmosphere exchange of NH3. Measurements were conducted within the European project GRAMINAE (GRassland AMmonia INteractions Across Europe) within which the Scottish site forms one of 6 sites in an E–W transect across Europe. NH3 emissions were enhanced (up to 300 ng m-2 s-1) after cutting followed by larger emissions after fertilising (up to 1400 ng m-2 s-1). Annual budget calculations show the intensive grassland acted as a net source (1.8 kg N ha-1 yr1) although fluxes were bi-directional with deposition dominating in the winter and emission in the summer. Initial modelling of the NH3 exchange using a `canopy compensation point' model has been conducted for key periods. The dynamics of the fluxes during these key periods, such as before and after cutting and fertilising, may be reproduced by introducing different values of the apoplastic ratio, = [NH4 +]/[H+].  相似文献   

8.
Temporal trends of non-sea salt (nss-) sulfate and nitrate were analyzed from nationwide precipitation chemistry measurements provided by the Ministry of the Environment (MOE) for the 1988–2002 fiscal years (April–March). The concentrations and deposition of nss-sulfate were found to be decreasing, and those of nitrate were stable or slightly increasing at most sites. These deposition trends were discussed from the viewpoint of emissions of SO2 and NOX during the period of interest. Because monitoring techniques have changed in the number of active sites, samplers, and analytical methods during the operation period, the median of all annual depositions measured in Japan in a specific year was selected as the annual representative. The contribution of specific emission sources was also calculated for 1990 on the basis of the nss-sulfate and nitrate deposition in Japan obtained with a model simulation in which the model did not include volcanic emissions from Mt. Oyama, Miyakejima Island, which began to erupt suddenly and violently in 2000. For nss-sulfate, the calculated deposition agrees well with the intensity and trends of the median up to 1999. After 2000, a higher deposition than calculated in the preceding years was evident, which is attributable to the volcanic SO2 from Mt. Oyama. For nitrate, both the calculated and observed depositions were slightly increasing; however, the calculation was found to exceed the observation.  相似文献   

9.
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   

10.
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   

11.
Ammonia emissions from two contrasting seabird colonies in Scotland were measured, based on the determination of atmospheric concentrations downwind of the colonies. Atmospheric concentrations of ammonia (NH3) across the downwind plume were compared with the inverse application of a Gaussian dispersion model (ID) to calculate the modelled NH3 emission that would generate the measured cross-wind-integrated plume concentration. In parallel, a tracer gas (sulphur hexafluoride, SF6) was released from the colonies with air samples taken to allow determination of SF6 concentrations. On the basis of the known emission rate of SF6, the magnitude of ammonia emissions was estimated by the cross-wind-integrated tracer ratio (TR) of NH3/SF6 concentrations. Coupled with data on annual bird attendance, the measurements indicate annual emissions from the Isle of May and the Bass Rock of 18 and 132 tonnes NH3-N year?1, respectively. The measured NH3 emissions were compared with estimates of seabird nitrogen excretion to estimate the proportion of excreted N that is volatilised as NH3 (F Nr). The emission estimates of the two methods compared favourably, giving 4 and 6 kg NH3-N h?1 (F Nr = 15%) for the Isle of May for the ID and TR methods, respectively, and 21 and 25 kg NH3-N h?1 (F Nr = 50%) for the Bass Rock for the ID and TR methods, respectively. The results provide the first measurement-based estimates to allow regional up scaling of ammonia emissions from seabirds.  相似文献   

12.
Ammonia emissions from two contrasting seabird colonies in Scotland were measured, based on the determination of atmospheric concentrations downwind of the colonies. Atmospheric concentrations of ammonia (NH3) across the downwind plume were compared with the inverse application of a Gaussian dispersion model (ID) to calculate the modelled NH3 emission that would generate the measured cross-wind-integrated plume concentration. In parallel, a tracer gas (sulphur hexafluoride, SF6) was released from the colonies with air samples taken to allow determination of SF6 concentrations. On the basis of the known emission rate of SF6, the magnitude of ammonia emissions was estimated by the cross-wind-integrated tracer ratio (TR) of NH3/SF6 concentrations. Coupled with data on annual bird attendance, the measurements indicate annual emissions from the Isle of May and the Bass Rock of 18 and 132 tonnes NH3-N year–1, respectively. The measured NH3 emissions were compared with estimates of seabird nitrogen excretion to estimate the proportion of excreted N that is volatilised as NH3 (FNr). The emission estimates of the two methods compared favourably, giving 4 and 6 kg NH3-N h–1 (FNr = 15%) for the Isle of May for the ID and TR methods, respectively, and 21 and 25 kg NH3-N h–1 (FNr = 50%) for the Bass Rock for the ID and TR methods, respectively. The results provide the first measurement-based estimates to allow regional up scaling of ammonia emissions from seabirds.  相似文献   

13.
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   

14.
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   

15.
A dry deposition model (RDM) for operational application has beenevaluated and modified in the present study. Field measurements of friction velocity and dry deposition velocity of SO2 andO3 over a mixed forest have been used to evaluate RDM. It was found that RDM predicts friction velocities very close to measurements and thus it can predict reasonable aerodynamic resistance. RDM overestimated O3 deposition during dry nighttime conditions and underestimated both O3 andSO2deposition for early morning hours. It could not predict the mean diurnal variation in deposition velocity for either O3 or SO2 deposition under wet surface conditions. Modifications have been made for O3 and SO2 dry deposition based on the comparison of results and based upon additional published data. Compared to an earlier version of RDM, the modified versionpredicts better results for O3 and SO2 dry deposition,especially under rain and dew conditions.  相似文献   

16.
Previously, it has been observed that the internal circulation (ion leakage) of calcium from a coniferous forest is caused by uptake of sulphur dioxide (SO2). Here we show that this correlation was not changed when the forest floor is covered with a roof. The reaction takes place in the canopy and is not influenced by deposition and root uptake of calcium and sulphate. The ion leakage of calcium is linked to the loss of acidity in throughfall. The process can, for one of the catchments, schematically be written: SO2 + H2O + 0.5 O2 + 0.58 CaA2→ SO4 2- + 0.94 H+ + 0.58 Ca2+ + 1.16 HA, in which A denotes the anion to a weak acid. This reaction also takes place today when the SO2 concentration is very low, but when the precipitation is still acidic. The ion leakage of manganese also is caused by the uptake of SO2, but only 0.12 manganese ions are released per SO2 molecule.  相似文献   

17.
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   

18.
The Turkey Lakes Watershed (TLW) was established in 1980 as asite for study of the ecosystem effects of acidic deposition, andsince then there has been 40% reduction in North AmericanSO2 emissions. Monitoring records for bulk deposition,shallow and deep ground water, two headwater streams and two lakeoutflows have been tested to identify statistically significantmonotonic trends. The TLW appears to be responding to decliningacidifying emissions because the most prevalent chemical trendacross sample types/stations was decreasing SO4 2-. Increasing pH was detected in four of the seven data sets, butonly the H+ decrease in bulk deposition was of a magnitudeto be an important ionic compensation for the SO4 2-decline. There is little evidence of acidification recovery inTLW waters however. Increasing alkalinity was found only in theoutflow of the penultimate lake of the basin, and in fact, deepground water and the other lake outflow had decreasing alkalinitytrends (i.e., continuing acidification). For the surface waterstations, the greater part of the ionic compensation fordeclining SO4 2- was decreasing base cations, and as aresult, these waters are probably becoming more dilute with time,although only the headwater streams exhibited decliningconductivity. Five of seven data sets had increasing dissolvedorganic carbon concentrations. Increasing NO3 - wasimportant in ground waters. Drought has strongly influencedtrends and delayed recovery by mobilizing S stored in catchmentwetlands and/or soils.  相似文献   

19.
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   

20.
Models are needed that predict both spatial and temporal improvements to ecosystems following reductions of acidifying emissions that produce `acid rain'. Logistic regression models were developed for the occurrence of fish and two fish-eatingbirds, common loons (Gavia immer) and common mergansers(Mergus merganser), using monitoring data collected onlakes across Ontario. These models were applied in the Algomaregion, including the Turkey Lakes Watershed (TLW). Using theWaterfowl Acidification Response Modeling System (WARMS), severalSO2 emission reduction scenarios were simulated, i.e. thosecontributing to measured 1982–1986 sulphate deposition levels, 1994levels (corresponding to full implementation of Canadian SO2emission reductions as stipulated in the 1991 Canada/U.S. AirQuality Agreement), 2010 levels (1994 plus full U.S. reductions),and both a 50% and a 75% further reduction beyond 2010 levels. Some habitat improvements in Algoma were predicted under the 2010scenario for all biota, but substantial increases in habitatquality, especially for mergansers, would occur only under further reductions. The TLW showed little change in chemistry orbiota, while lakes near the Montreal River were predicted toimprove substantially.  相似文献   

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