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1.
A continuous relaxed eddy accumulation system ispresented for the automated measurement of surface/atmosphere exchange fluxes of atmospheric ammonia (NH3) at a single height. The new system features sampling by parallel plate denuder inlets, online chemical analysis using the conductivity cell of a commercially available NH3 analyzer and online flux calculation. The effective detection limit of the system for air concentrations is 0.2 g m-3 and it is estimated to resolve fluxes > ± 20 ng m-2 s-1, depending on the NH3 concentration and turbulence. The performance of the system was tested in two measurement campaigns above agricultural grassland, in which it was compared with a 3-point continuous gradient system. During the first campaign, after urea application of 47 kg N ha-1 in autumn, the REA system derived fluxes which were on average twice as large as the gradient fluxes, while concentrations agreed closely (on average within 4%). Possible reasons include differences in the footprint and an over-correction of the gradient flux in stable conditions. Due to wet and cold conditions, only 0.3% of the fertilizer N was volatilized as NH3 during the first week. Results from the deployment of an improved system are presented for a summer day, 6 days after fertilization with calcium ammonium nitrate. The agreement of both concentrations (on average within 13%) and fluxes (26%) was very encouraging and similar to the agreement found between two state-of-the-art gradient systems with online analysis.  相似文献   

2.
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   

3.
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   

4.
Ammonia concentration gradients were measuredabove a grassland in an agricultural region fromJuly 1998 to July 2000 at the locationSchagerbrug in the Netherlands. They were used tocalculate the surface-atmosphere exchange ofammonia by means of the aerodynamic gradienttechnique. Measurements of the ammonia exchangewere also performed at a grass field that is partof a major wetland reserve in the centre of theNetherlands (Oostvaardersplassen), during theperiod June 1994–September 1995. At Schagerbrug,low net emissions or small depositions weremeasured during the winter months, and a netemission up to 5 kg NH3 ha-1 month-1 in summer. The net annual emission was 26 kgN ha-1, with manure application contributingabout 50% of this emission. AtOostvaardersplassen mainly deposition occurred,but large emissions were measured in autumn. Themeasured exchange fluxes are compared to modelevaluations that incorporate plant physiologicaldata, such as apoplastic NH4 +concentrations and pH. Results show a goodagreement between field observations and modelsimulations, although some improvements arenecessary during nighttime periods. Themeasurements are conducted within the GRAMINAEproject, a second tranche project of EC TERI.  相似文献   

5.
Field measurements of NH3 fluxes using an eddy covariance technique were made for a total of 60 days between July and September 2002 at an intensively managed grassland in Southern Scotland. The collected data demonstrate the suitability of a tuneable diode laser absorption spectroscopy (TDLAS) system coupled with a sonic anemometer for eddy covariance measurements. The novelty of these measurements is the application to ammonia, which has only become measurable using TDLAS techniques recently, because of its small ambient concentration. Data presented in this paper show typical features of the fluxes and concentration for the summer season. NH3 concentration and flux values are in a similar range to previous studies using flux gradient methods at the same field site, although the particularly wet season reduced the concentration of NH3 in the air. For an example day, measured NH3 fluxes ranged between ?11 and 44 ng m?2 s?1 with an average value of 3.78 ng m?2 s?1 indicating a small net emission from the vegetation. Spectral analysis executed on the data shows the percentage of flux carried by the small eddies (from 0.2 to 2 m) suggesting that high detection frequency instruments are particularly suitable for estimating NH3 fluxes between atmosphere and vegetation.  相似文献   

6.
Field measurements of NH3 fluxes using an eddy covariance technique were made for a total of 60 days between July and September 2002 at an intensively managed grassland in Southern Scotland. The collected data demonstrate the suitability of a tuneable diode laser absorption spectroscopy (TDLAS) system coupled with a sonic anemometer for eddy covariance measurements. The novelty of these measurements is the application to ammonia, which has only become measurable using TDLAS techniques recently, because of its small ambient concentration. Data presented in this paper show typical features of the fluxes and concentration for the summer season. NH3 concentration and flux values are in a similar range to previous studies using flux gradient methods at the same field site, although the particularly wet season reduced the concentration of NH3 in the air. For an example day, measured NH3 fluxes ranged between –11 and 44 ng m–2 s–1 with an average value of 3.78 ng m–2 s–1 indicating a small net emission from the vegetation. Spectral analysis executed on the data shows the percentage of flux carried by the small eddies (from 0.2 to 2 m) suggesting that high detection frequency instruments are particularly suitable for estimating NH3 fluxes between atmosphere and vegetation.  相似文献   

7.
To study the effects of elevated inputs of acidity and nitrogen (N), 1000 mmol m-2 a-1 of ammonium sulphate (NH4NO3) equivalent to an input of potential acidity of 2000 mmol m-2 a-1 was applied annually for 11 yr between 1983 and 1993 in a beech forest at Solling, Germany. Most of the applied NH4 + was nitrified in the litter layer and in the upper mineral soil. N in soil leachate quickly responded to the elevated input, but most of the applied N was stored in the soil or left the ecosystem via pathways other than soil output. Leaching of N from the soil increased until the last year of N addition. After the last N application, N fluxes decreased rapidly to low values. The buffering of acidity produced by the nitrification of the applied NH4 + was caused mainly by three different processes: (i) sulphur (S) retention, (ii) release of aluminium, (iii) release of base cations. Retention of S took place mostly in the subsoil. 72% of the S input was recovered in output after 14 years of the experiment. Due to the increased fluxes of mobile anions with soil solution, outputs of cations increased drastically.  相似文献   

8.
In order to assess nitrous oxide (N2O) emissions from typical intensively managed grassland in northern Britain fluxes were measured by eddy covariance using tuneable diode laser absorption spectroscopy from June 2002 to June 2003 for a total period of 4000 h. With micrometeorological techniques it is possible to obtain a very detailed picture of the fluxes of N2O at field scale (103–104 m2), which are valuable for extrapolation to regional scales. In this paper three of the four fertilizer applications were investigated in detail. N2O emissions did not always show a clear response. Hourly fluxes were very large immediately after the June 2002 nitrogen fertilizer application, peaking at 2.5 mg N2O–N m?2 s?1. Daily fluxes were averaging about 300 ng N2O m?2 s?1 over the 4 days following fertilizer application. The response of N2O emissions was less evident after the August fertilization, although 2 days after fertilizer application an hourly maximum flux of 554 ng N2O–N m?2 s?1 was registered. For the rest of August the flux was undetectable. The differences between fertilization events can be explained by different environmental conditions, such as soil temperature and rainfall. A fertiliser-induced N2O emission was not observed after fertilizer application in March 2003, due to lack of rainfall. The total N2O flux from June 2002 to June 2003 was 5.5 kg N2O–N ha?1y?1, which is 2.8% of the total annual N fertilizer input.  相似文献   

9.
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 g m–3 to 30 s m–1 at 30 g 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   

10.
Extremely high emissions of S and N compounds in Central Europe (both 280 mmol m-2 yr-1) declined by 70and 35%, respectively, during the last decade. Decreaseddeposition rates of SO4 -2, NO3 -, and NH4 + in the region paralleled emission declines. The reduction in atmospheric inputs of S and N to mountain ecosystemshas resulted in a pronounced reversal of acidification in the Tatra Mountains and Bohemian Forest lakes. Between the 1987–1990and 1997–1999 periods, concentrations of SO4 -2 and NO3 - decreased (average ± standard deviation) by 22±7 and 12±7 mol L-1, respectively, in theTatra Mountains, and by 19±7 and 15±10 mol L-1, respectively, in the Bohemian Forest. Their decrease was compensated in part (1) by a decrease in Ca2+ + Mg2+ (17±7 mol L-1) and H+ (4±6 mol L-1), and an increase in HCO3 -(10±10 mol L-1) in the Tatra Mountains lakes, and (2) by a decrease in Al (7±4 mol L-1), Ca2+ + Mg2+ (9±6 mol L-1), and H+ (6±5 mol L-1), in Bohemian Forest lakes. Despite the rapid decline in lake water concentrations of SO4 -2 and NO3 - in response to reduced S and N emissions, their present concentrations in some lakes are higher than predictionsbased on observed concentrations at comparable emission rates during development of acidification. This hysteresis in chemical reversal from acidification has delayed biological recovery of the lakes. The only unequivocal sign of biological recovery hasbeen observed in erné Lake (Bohemian Forest) where a cladoceran species Ceriodaphnia quadrangular has recentlyreached its pre-acidification abundance.  相似文献   

11.
Estimating regional patterns in concentrations of atmosphericammonia (NH3) gas and ammonium (NH4 +) in aerosolis essential to assess dry deposition, as well as to test theperformance of long-range transport models. Until now, methods for monitoring NH3 and NH4 + (collectively NHx) have focused on either passive sampling, which does not sample aerosol NH4 +, or active sampling techniquessuitable for sampling over several minutes to 24 hr. The classicalactive sampling approach is the diffusion denuder, which typically involves either a complex annular denuder or a long(0.5 m) and fragile glass tube. A new denuder implementationis reported here that has been designed for long-term samplingof NH3 and NH4 +. By sampling at just 0.35 L min-1, the method is suitable for monthly measurementsand uses 0.1 m long glass denuders, which may be sent safelyby the normal postal service to monitoring sites. Two denudersare applied in series to test for adequate NH3 captureefficiency in each sample, while a subsequent acidified paperfilter collects NH4 +. The method has been implementedat over 50 sites across the U.K. as part of a new national monitoring network. The detection limit is <0.01 μg m-3 and the sampling is sufficiently accurate to show theseasonal patterns at different sites. This low-cost method willbe useful to address future trends in NH3 and NH4 +, especially in relation to compliance with international agreements to reduce NH3 emissions.  相似文献   

12.
In order to assess nitrous oxide (N2O) emissions from typical intensively managed grassland in northern Britain fluxes were measured by eddy covariance using tuneable diode laser absorption spectroscopy from June 2002 to June 2003 for a total period of 4000 h. With micrometeorological techniques it is possible to obtain a very detailed picture of the fluxes of N2O at field scale (103–104 m2), which are valuable for extrapolation to regional scales. In this paper three of the four fertilizer applications were investigated in detail. N2O emissions did not always show a clear response. Hourly fluxes were very large immediately after the June 2002 nitrogen fertilizer application, peaking at 2.5 mg N2O–N m–2 s–1. Daily fluxes were averaging about 300 ng N2O m–2 s–1 over the 4 days following fertilizer application. The response of N2O emissions was less evident after the August fertilization, although 2 days after fertilizer application an hourly maximum flux of 554 ng N2O–N m–2 s–1 was registered. For the rest of August the flux was undetectable. The differences between fertilization events can be explained by different environmental conditions, such as soil temperature and rainfall. A fertiliser-induced N2O emission was not observed after fertilizer application in March 2003, due to lack of rainfall. The total N2O flux from June 2002 to June 2003 was 5.5 kg N2O–N ha–1y–1, which is 2.8% of the total annual N fertilizer input.  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+ 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   

14.
In order to study the effect of thevegetation structure on atmospheric ammonia(NH3) dispersion and deposition, anexperiment was set up near Paris, in July 1997.Between 12 and 162 m downwind of a 200 m line-source releasing 600 to 1200 g NH3hr-1placed at the top of a maize canopy, NH3concentration was measured, within and above thecanopy, with a set of 30 active, acid-coateddenuders over periods of 2 to 3 hr. Eight datasets were collected over a one-month period.NH3 concentration decreased sharply withdistance to the source, from up to800 g NH3 m-3 at 12 m, to lessthan 10 g NH3 m-3 at 162 m andshowed strong vertical gradients. Within thecanopy, the concentration scaled using thefriction velocity, the canopy height, and thesource strength, exhibited a universal power lawrelationship as a function of the normaliseddownwind distance from the source. A mass balancemethod and a resistance model approach were usedas independent estimates of the cumulateddeposition at 162 m downwind from the source,which range between 1 and 29% of the emittedNH3. Both methods agreed approximately inmagnitude. A sensitivity analysis showed that thecuticular uptake and the compensation point aremajor parameters that needs to be bettercharacterised under high NH3 concentrationif one wants to improve NH3 short-rangedeposition modelling.  相似文献   

15.
Amounts of readily soluble nutrients on asphalt parking lot surfaceswere measured at four locations in metropolitan Phoenix, Arizona, U.S.A. Using a rainfall simulator, short intense rainfall events were generated to simulate `first flush' runoff. Samples were collected from 0.3 m2 sections of asphalt at 8 to 10 sites on each of four parkinglots, during the pre-monsoon season in June-July 1998 and analyzed for dissolved NO3 --N, NH4 +-N, soluble reactive phosphate (SRP), and dissolved organic carbon (DOC). Runoff concentrations varied considerably for NO3 --N and NH4 +-N (between 0.1 and 115.8 mg L-1) and DOC (26.1 to 295.7 mg L-1), but less so for SRP (0.1 to 1.0 mg L-1), representing average surface loadings of 191.3, 532.2, and 1.8 mg m-2 respectively. Compared with similar data collected from undeveloped desert soil surfaces outside the city, loadings of NO3 --N and NH4 +-N on asphalt surfaces were greater by factors of 91 and 13, respectively. In contrast, SRP loads showed little difference between asphalt and desert surfaces. Nutrient fluxes in runoff from a storm that occurred shortly after the experiments were used to estimate input-output budgets for 3 of the lots under study. Measured outputs of DOC and SRP were similar to those predicted using rainfall and experimentally determined surface loadings, but for NH4 +-N and particularly for NO3 --N, estimated rainfall inputs and surface runoff were significantly higher than exports in runoff. This suggests that parking lots may be important sites for nutrient accumulation and temporary storage in arid urban catchments.  相似文献   

16.
Air-sea exchange rates for ozone were measured by the eddy correlation technique at a site on the north Norfolk coast in the UK. The average surface resistance to ozone uptake was found to be, rs(O3) = 1,000 ± 100 s m-1. Micrometeorological measurements of trace gas fluxes to ocean surfaces are rare but a review of available measurements suggests that we can constrain sea water surface resistance for ozone to between 1,000 (Regener (1974), and this work) and 1,890 s m-1 (Lenschow et al., 1982), yielding surface deposition velocities between 0.53 and 1.0 mm s-1. These values are more than an order of magnitude greater than can be explained by laboratory determined mass accommodation coefficients for ozone to water. The importance of dry deposition with respect to process air-sea exchange models is highlighted. A trend in surface deposition velocity with wind speed was also observed supporting a surface chemical enhancement mechanism of ozone uptake which in turn is enhanced by near surface mixing processes.  相似文献   

17.
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   

18.
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   

19.
In April 1998, two intense dust storms were generated in CentralAsia and transported eastward across East Asia (15 and 19 April). This article presents the chemical characterization ofHong Kong (HK) aerosols during the dust storms. During the 15 Aprildust storm, hourly respiratory suspended particles (RSP)(particle diameter smaller than 10 m) concentrationsmonitored at 7 sites in Hong Kong reached the peak valuessynchronously between 9 and 11 a.m. on 17 April, in which thehighest concentration was 267 g m-3. Analysis ofthe RSP samples showed that concentrations of crustalelements (Ba, Ca, Cd, Cr, Fe, Mg, K+) and anthropogenicspecies (As, Ni, Pb, Zn, NH4 +, NO3 -,SO4 2- and total carbon) were substantiallyenhanced. Enhancement of these species was more than afactor of 2 to 14 relative to the non dust period. The totalcarbon content was high, at 59 g m-3 (notincluding carbonate), and the enrichment factors of Asand Pb on 17 April were 122 and 117, respectively. Thisimplied that anthropogenic materials together with mineraldust were transported to HK from Mainland China. Based onmaterial balance calculations, mineral dust contributed41% to the observed RSP mass on 17 April, which was 2 times thatof the nondust sample (22%). From the 5-day backwardtrajectory analysis, this storm was transported directlyfrom Northwest China to HK. However, there was nocorresponding observation for the 19 April dust stormaerosol. Consequently, 15 April storm had stronger impact onHK's atmosphere than 19 April storm. Compared to the HK AirQuality Objective, 15 April dust storm did not cause seriousair pollution in HK.  相似文献   

20.
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   

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