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1.
The study of mercury (Hg) cycle in Arctic regions is a major subject of concern due to the dramatic increases of Hg concentrations in ecosystem in the last few decades. The causes of such increases are still in debate, and an important way to improve our knowledge on the subject is to study the exchanges of Hg between atmosphere and snow during springtime. We organized an international study from 10 April to 10 May 2003 in Ny-Ålesund, Svalbard, in order to assess these fluxes through measurements and derived calculations.Snow-to-air emission fluxes of Hg were measured using the flux chamber technique between ∼0 and 50 ng m−2 h−1. A peak in Gaseous Elemental Mercury (GEM) emission flux from the snow to the atmosphere has been measured just few hours after an Atmospheric Mercury Depletion Event (AMDE) recorded on 22 April 2004. Surprisingly, this peak in GEM emitted after this AMDE did not correspond to any increase in Hg concentration in snow surface. A peak in GEM flux after an AMDE was observed only for this single event but not for the four other AMDEs recorded during this spring period.In the snow pack which is seasonal and about 40 cm depth above permafrost, Hg is involved in both production and incorporation processes. The incorporation was evaluated to ∼5–40 pg m2 h. Outside of AMDE periods, Hg flux from the snow surface to the atmosphere was the consequence of GEM production in the air of snow and was about ∼15–50 ng m−2 h−1, with a contribution of deeper snow layers evaluated to ∼0.3–6.5 ng m−2 h−1. The major part of GEM production is then mainly a surface phenomenon. The internal production of GEM was largely increasing when snow temperatures were close to melting, indicating a chemical process occurring in the quasi-liquid layer at the surface of snow grains.  相似文献   

2.
Surface–atmosphere mercury fluxes are difficult to measure accurately. Current techniques include dynamic flux chambers and micrometeorological gradient and aerodynamic approaches, all of which have a number of intrinsic problems associated with them. We have adapted conditional sampling (relaxed eddy accumulation), a micrometeorological technique commonly used to measure other trace gas fluxes, to measure surface–air mercury fluxes. Our initial flux measurement campaign over an agricultural soil consisted of two 1-week measurement periods, and was longer in duration than previously reported mercury flux measurement periods. Fluxes during both measurement periods ranged between 190.5 (evolution) and –91.7 ng m−2 h−1 (deposition) with an average evolution of 9.67 ng m−2 h−1. The data showed significant diurnal trends, weakly correlated with shallow soil temperatures and solar radiation. This initial trial run indicates that conditional sampling has much promise for the accurate quantification of both short and long-term mercury fluxes.  相似文献   

3.
Canopy scale emissions of isoprene and monoterpenes from Amazonian rainforest were measured by eddy covariance and eddy accumulation techniques. The peak mixing ratios at about 10 m above the canopy occurred in the afternoon and were typically about 90 pptv of α-pinene and 4–5 ppbv of isoprene. α-pinene was the most abundant monoterpene in the air above the canopy comprising ≈50% of the total monoterpene mixing ratio. Measured isoprene fluxes were almost 10 times higher than α-pinene fluxes. Normalized conditions of 30°C and 1000 μmol m−2 s−1 were associated with an isoprene flux of 2.4 mg m−2 h−1 and a β-pinene flux of 0.26 mg m−2 h−1. Both fluxes were lower than values that have been specified for Amazon rainforests in global emission models. Isoprene flux correlated with a light- and temperature-dependent emission activity factor, and even better with measured sensible heat flux. The variation in the measured α-pinene fluxes, as well as the diurnal cycle of mixing ratio, suggest emissions that are dependent on both light and temperature. The light and temperature dependence can have a significant effect on the modeled diurnal cycle of monoterpene emission as well as on the total monoterpene emission.  相似文献   

4.
Five weeks of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle bound mercury (Hgp) concentrations as well as fluxes of GEM were measured at Maryhill, Ontario, Canada above a biosolids amended field. The study occurred during the autumn of 2004 (October–November) to capture the effects of cool weather conditions on the behaviour of mercury in the atmosphere. The initial concentration of total mercury (Hg) in the amended soil was relatively low (0.4 μg g−1±10%).A micrometeorological approach was used to infer the flux of GEM using a continuous two-level sampling system with inlets at 0.40 and 1.25 m above the soil surface to measure the GEM concentration gradient. The required turbulent transfer coefficients were derived from meteorological parameters measured on site. The average GEM flux over the study was 0.1±0.2 ng m−2 h−1(±one standard deviation). The highest averaged hourly GEM fluxes occurred when the averaged net radiation was highest, although the slight diurnal patterns observed were not statistically significant for the complete flux data series. GEM emission fluxes responded to various local events including the passage of a cold front when the flux increased to 2 ng m−2 h−1 and during a biosolids application event at an adjacent field when depositional fluxes peaked at −3 ng m−2 h−1. Three substantial rain events during the study kept the surface soil moisture near field capacity and only slightly increased the GEM flux. Average concentrations of RGM (2.3±3.0 pg m−3), Hgp (3.0±6.2 pg m−3) and GEM (1.8±0.2 ng m−3) remained relatively constant throughout the study except when specific local events resulted in elevated concentrations. The application of biosolids to an adjacent field produced large increases in Hgp (25.8 pg m−3) and RGM (21.7 pg m−3) concentrations only when the wind aligned to impact the experimental equipment. Harvest events (corn) in adjacent fields also corresponded to higher concentrations of GEM and Hgp but with no elevated peaks in RGM concentrations. Diurnal patterns were not statistically significant for RGM and Hgp at Maryhill.  相似文献   

5.
Gaseous methane (CH4) emissions from a swine waste holding lagoon were determined periodically during the year. Micrometeorological techniques were used in order that emission rates from the lagoon were measured under ambient conditions with little disturbance to the natural environment. During the cold winter measurement period, CH4 fluxes were linearly related to lagoon water temperature below 22°C (r=0.87). During warmer measurement periods, both water and air temperatures and windspeed affected emissions rates. In general, flux rates followed a diurnal pattern with greater fluxes during the day when both temperature and windspeed were greatest. Mathematical models using air and water temperature and windspeed factors could explain 47 to 75% of the variation in fluxes. Daily emission rates ranged from 1 to 500 kg CH4 ha−1 d−1. The average flux for the year was 52.3 kg CH4 ha−1 d−1 which corresponded to about 5.6 kg CH4 animal−1 yr−1 from the primary lagoon.  相似文献   

6.
A water surface sampler (WSS) was employed in combination with greased knife-edge surface deposition plates (KSSs) to measure the vapor phase deposition rates of PCBs to the sampler at an urban site, Chicago, IL. This sampler employed a water circulation system that continuously removed deposited PCBs. Total (gas+particle) and particulate PCB fluxes were collected with the WSS and KSSs, respectively. Gas phase PCB fluxes were then calculated by subtracting the KSS fluxes (particulate) from the WSS fluxes (gas+particle). The calculated gas phase PCB fluxes averaged 830±910 ng m−2d−1. This flux value is, in general, higher than the fluxes determined using simultaneously measured air–water concentrations in natural waters and is in the absorption direction. This difference is primarily because the PCBs were continuously removed from the WSS water keeping the water PCB concentration near zero.Concurrently, ambient air samples were collected using a modified high volume air sampler. The gas phase PCB concentrations ranged between 1.10 and 4.46 ng m−3 (average±SD, 2.29±1.28 ng m−3). The gas phase fluxes were divided by the simultaneously measured gas phase ambient concentrations to determine the overall gas phase mass transfer coefficients (MTCs) for PCBs. The average gas phase overall MTCs (Kg) for each homolog group ranged between 0.22 and 1.32 cm s−1 (0.54±0.47 cm s−1). The average MTC was in good agreement with those determined using similar techniques.  相似文献   

7.
The concentrations of total gaseous mercury (TGM) in air over the southern Baltic Sea and dissolved gaseous mercury (DGM) in the surface seawater were measured during summer and winter. The summer expedition was performed on 02–15 July 1997, and the winter expedition on 02–15 March 1998. Average TGM and DGM values obtained were 1.70 and 17.6 ng m−3 in the summer and 1.39 and 17.4 ng m−3 in the winter, respectively. Based on the TGM and DGM data, surface water saturation and air-water fluxes were calculated. The results indicate that the seawater was supersaturated with gaseous mercury during both seasons, with the highest values occurring in the summer. Flux estimates were made using the thin film gas-exchange model. The average Hg fluxes obtained for the summer and winter measurements were 38 and 20 ng m−2 d−1, respectively. The annual mercury flux from this area was estimated by a combination of the TGM and DGM data with monthly average water temperatures and wind velocities, resulting in an annual flux of 9.5 μg m−2 yr−1. This flux is of the same order of magnitude as the average wet deposition input of mercury in this area. This indicates that reemissions from the water surface need to be considered when making mass-balance estimates of mercury in the Baltic Sea as well as modelling calculations of long-range transboundary transport of mercury in northern Europe.  相似文献   

8.
Micrometeorological flux-gradient and nocturnal boundary layer methods were combined with Fourier transform infrared (FTIR) spectroscopy for high-precision trace gas analysis to measure fluxes of the trace gases CO2, CH4 and N2O between agricultural fields and the atmosphere. The FTIR measurements were fully automated and routinely obtained a precision of 0.1–0.2% for several weeks during a measurement campaign in October 1995. In flux-gradient measurements, vertical profiles of the trace gases were measured every 30 min from the ground to 22 m. When combined with independent micrometeorological measurements of water vapour fluxes, trace gas fluxes from the underlying surface could be determined. In the nocturnal boundary layer method the rate of change in mass storage in the 0–22 m layer was combined with fluxes measured at 22 m to estimate surface fluxes. Daytime fluxes for CO2 were −0.78±0.40 (1σ) mg CO2 m−2 s−1. Daytime fluxes of N2O and CH4 were very small and difficult to measure reliably using the flux-gradient technique, despite the high precision of the concentration measurements. Mean daytime flux for N2O was 17±48 ng N m−2 s−1, while the corresponding flux for CH4 was 47±410 ng CH4 m−2 s−1. The mean nighttime flux of CO2 estimated using the nocturnal boundary layer method was +0.15±0.05 mg CO2 m−2 s−1, in good agreement with chamber measurements of respiration rates. Nighttime fluxes of CH4 and N2O from the nocturnal boundary layer method were 109±69 ng CH4 m−2 s−1 and 2±3.2 ng N m−2 s−1, respectively, in good agreement with chamber measurements and inventory estimates based on the sheep and cattle stocking rates in the region. The suitability of FTIR-based methods for long term monitoring of spatially and temporally averaged flux measurements is discussed.  相似文献   

9.
In order to assess the importance of mercury emissions from naturally enriched sources relative to anthropogenic point sources, data must be collected that characterizes mercury emissions from representative areas and quantifies the influence of various environmental parameters that control emissions. With this information, we will be able to scale up natural source emissions to regional areas. In this study in situ mercury emission measurements were used, along with data from laboratory studies and statistical analysis, to scale up mercury emissions for the naturally enriched Ivanhoe Mining District, Nevada. Results from stepwise multi-variate regression analysis indicated that lithology, soil mercury concentration, and distance from the nearest fault were the most important factors controlling mercury flux. Field and lab experiments demonstrated that light and precipitation enhanced mercury emissions from alluvium with background mercury concentrations. Diel mercury emissions followed a Gaussian distribution. The Gaussian distribution was used to calculate an average daily emission for each lithologic unit, which were then used to calculate an average flux for the entire area of 17.1 ng Hg m−2 h−1. An annual emission of ∼8.7×104 g of mercury to the atmosphere was calculated for the 586 km2 area. The bulk of the Hg released into the atmosphere from the district (∼89%) is from naturally enriched non-point sources and ∼11% is emitted from areas of anthropogenic disturbance where mercury was mined. Mercury emissions from this area exceed the natural emission factor applied to mercury rich belts of the world (1.5 ng m−2 h−1) by an order of magnitude.  相似文献   

10.
Due to the high temporal and spatial variability of N2O fluxes, estimates of N2O emission from temperate forest ecosystems are still highly uncertain, particularly at larger scales. Although highest N2O emissions with up to 7.0 kg N ha−1 yr−1 were mainly reported for soils affected by stagnant water, most of the reported gas flux measurements were performed at forest sites with well-aerated soils yielding mostly to low mean annual emission rates less than 1.0 kg N ha−1 yr−1. This study compares N2O fluxes from upland (Cambisols) and temporally water-logged (Gleysols, Histosols) soils of the Central Black Forest (South-West Germany) over a period of 2 yr. Mean annual N2O fluxes from investigated soils ranged between 0.2 and 3.9 kg N ha−1 yr−1. The fluxes showed a large variability between the different soil types. Emissions could be clearly ranked in the following order: Cambisols (0.26–0.75 kg N ha−1 yr−1)<Gleysols (1.37–2.68 kg N ha−1 yr−1)<Histosol (3.66–3.95 kg N ha−1 yr−1). Although the Cambisols cover two-thirds of the investigated area, only about half of the overall N2O is emitted from this soil type. Therefore, regional or national N2O fluxes from temperate forest soils are underestimated if soils characterised by intermediate aeration conditions are disregarded.  相似文献   

11.
Emissions of nitric oxide (NO) were determined during late spring and summer 1995 and the spring of 1996 from four agricultural soils on which four different crops were grown. These agricultural soils were located at four different sites throughout North Carolina. Emission rates were calculated using a dynamic flow-through chamber system coupled to a mobile laboratory for in-situ analysis. Average NO fluxes during late spring 1995 were: 50.9±47.7 ng N m−2 s−1 from soil planted with corn in the lower coastal plain. Average NO fluxes during summer 1995 were: 6.4±4.6 and 20.2±19.0 ng N m−2 s−1, respectively, from soils planted with corn and soybean in the coastal region; 4.2±1.7 ng N m−2 s−1 from soils planted with tobacco in the piedmont region; and 8.5±4.9 ng N m−2 s−1 from soils planted with corn in the upper piedmont region. Average NO fluxes for spring 1996 were: 66.7±60.7 ng N m−2 s−1 from soils planted with wheat in the lower coastal plain; 9.5±2.9 ng N m−2 s−1 from soils planted with wheat in the coastal plain; 2.7±3.4 ng N m−2 s−1 from soils planted with wheat in the piedmont region; and 56.1±53.7 ng N m−2 s−1 from soils planted with corn in the upper piedmont region. An apparent increase in NO flux with soil temperature was present at all of the locations. The composite data from all the research sites revealed a general positive trend of increasing NO flux with soil water content. In general, increases in total extractable nitrogen (TEN) appeared to be related to increased NO emissions within each site, however a consistent trend was not evident across all sites.  相似文献   

12.
To evaluate the tropical wetlands contribution to the methane (CH4) burden better, field campaigns were performed during 2004 and 2005 near the Miranda River, in five sites inside the Brazilian Pantanal region. The CH4 fluxes were determined using the static chamber technique. Environmental variables that may affect CH4 emissions, as the water depth, the water and air temperatures were also measured. The overall average of the 320 individual CH4 flux measurements made between March/2004 and March/2005 was 142±314 mg CH4 m−2 d−1, which is a value near the ones observed in other tropical flooded regions. About 47% of the fluxes measurements presented nonlinear increases in the chamber concentrations, which were assumed to be linked to CH4 losses through bubbles. The bubble flux represented about 90% of the total CH4 losses in the measurements and ranged from 1 to 2187 mg CH4 m−2 d−1 with an average of 292±410 mg CH4 m−2 d−1 (median: 153 mg CH4 m−2 d−1). The diffusive flux ranged from 1 to 124 mg CH4 m−2 d−1, with an average of 10±17 mg CH4 m−2 d−1 (median: 5 mg CH4 m−2 d−1). The fluxes from lakes were smaller than those observed in the floodplains, where the flooding was more dependent on the seasonal cycle. The diffusive flux showed a slight, but not statistically significant seasonal variation, following the seasonal variation of the flooding of the Pantanal region. A rough estimative of the total annual CH4 emission shows that the contribution of the Pantanal is about 3.3 Tg CH4 yr−1, which represents about 3.3% of the total CH4 emissions estimated to be originated in wetlands ecosystems. It may be a conservative estimate, which may present a large interannual variation, since it was obtained during one of the lowest flood of the Pantanal in recent years.  相似文献   

13.
Isoprene fluxes from a Salix viminalis (willow) plantation in western Sweden were measured using the relaxed eddy accumulation (REA) technique. Fluxes of up to 0.23 μg m−2 s−1 could be observed. A standard emission factor at 303 K and a PAR flux of 1000 μ mol m−2 s−1 was estimated to 0.98 μg m−2 s−1 by using the G93 algorithm. The chemistry of an air parcel passing over a willow coppice plantation was investigated utilising a Lagrangian box model in which the measured isoprene fluxes were used as input data. Dispersion after the field was accounted for by a procedure based on the Gaussian plume model. The calculations indicate that, in most cases, the isoprene emissions have a small effect on the local air quality.  相似文献   

14.
We present measurements of ammonia (NH3) over a deciduous forest in southern Indiana collected during four field campaigns; two in the spring during the transition to leaf-out and two during the winter. Above canopy NH3 concentrations measured continuously using two Wet Effluent Diffusion Denuders indicate mean concentrations of 0.6–1.2 μg m−3 during the spring and 0.3 μg m−3 during the winter. Measurements suggest that on average the forest act as a sink of NH3, with a representative daily deposition flux of 1.8 mg-NH3 m−2 during the spring. However, on some days during the spring inverted concentration gradients of NH3 were observed resulting in an apparent upward flux of nearly 0.2 mg-NH3 m−2 h−1. Analyses suggest that this apparent emission flux may be due to canopy emission but evaporation of ammonium nitrate particles may also be partly responsible for the observed inverted concentration gradients.  相似文献   

15.
The effects of natural compounds on reducing formaldehyde emission from plywood were investigated. Urea, catechin and vanillin were examined as the natural formaldehyde reducers. The microemission cell, with an internal volume of 35 ml, the maximum exposed test surface area of 177 cm2 and an air purge flow rate of 50 ml min−1, was used to measure specific emission rate (SER). In the case of no reducer treatment, formaldehyde emission from plywood was fast and SERs were 4.4 mg m−2 h−1 at 30 °C and 15 mg m−2 h−1 at 60 °C. When this plywood was treated with the natural compounds, the SERs of formaldehyde were decreased at all temperatures. In the case of urea treatment, the SERs of formaldehyde decreased to 0.30 mg m−2 h−1 at 30 °C and 0.65 mg m−2 h−1 at 60 °C. When the urea treatment was applied to the inside of kitchen cabinet (made from plywood; 270 cm wide, 60 cm deep, 250 cm high), the concentration of formaldehyde was reduced substantially from 1600 to 130 μg m−3. The reducing effect of formaldehyde continued during the observation period (6 months), with a mean concentration of 100 μg m−3. Reducers in the plywood would react with released formaldehyde. Application of natural compounds such as urea, catechin and vanillin could provide a simple and effective approach for suppressing formaldehyde emission from plywood.  相似文献   

16.
The sea-to-air flux of the biogenic volatile sulphur compound dimethyl sulphide was assessed with the relaxed eddy accumulation (REA) and the gradient flux (GF) techniques from a stationary platform in the coastal Atlantic Ocean. Fluxes varied between 2 and 16 μmol m−2 d−1. Fluxes derived from REA were on average 7.1±5.03 μmol m−2 d−1, not significantly different from the average flux of 5.3±2.3 μmol m−2 d−1 derived from GF measurements. Gas transfer velocities were calculated from the fluxes and seawater DMS concentrations. They were within the range of gas transfer rates derived from the commonly used parameterizations that relate gas transfer to wind speed.  相似文献   

17.
The average total (wet plus dry) nitrogen deposition to the Tampa Bay Estuary was 7.3 (±1.3) kg-N ha−1 yr−1 or 760 (±140) metric tons-N yr−1 for August 1996–July 1999, estimated as a direct deposition rate to the 104,000-ha water surface. This nitrogen flux estimate accounted for ammonia exchange at the air–sea interface. The uncertainty estimate was based on measurement error. Wet deposition was 56% of the total nitrogen deposition over this period, with an average 0.78 ratio of dry-to-wet deposition. Wet nitrogen deposition rates varied considerably, from near zero to 1.3 kg-N ha−1 month−1. About 40% of the total nitrogen flux occurred during the summer months of June, July and August when rainfall was the highest, except for 1997–1998 when the El Niño phenomenon brought unseasonal rainfall. Ammonia/ammonium contributed to 58%, and nitric acid/nitrate 42%, of the total nitrogen deposition over the 3-yr period. In one summer as waters of Tampa Bay warmed above 28°C and ammonium concentrations reached 0.03 mg l−1, the estimated net flux of ammonia was from the Bay waters to the atmosphere.  相似文献   

18.
Ammonia-nitrogen flux (NH3-N=(14/17)NH3) was determined from six anaerobic swine waste storage and treatment lagoons (primary, secondary, and tertiary) using the dynamic chamber system. Measurements occurred during the fall of 1998 through the early spring of 1999, and each lagoon was examined for approximately one week. Analysis of flux variation was made with respect to lagoon surface water temperature (∼15 cm below the surface), lagoon water pH, total aqueous phase NHx(=NH3+NH4+) concentration, and total Kjeldahl nitrogen (TKN). Average lagoon temperatures (across all six lagoons) ranged from approximately 10.3 to 23.3°C. The pH ranged in value from 6.8 to 8.1. Aqueous NHx concentration ranged from 37 to 909 mg N l−1, and TKN varied from 87 to 950 mg N l−1. Fluxes were the largest at the primary lagoon in Kenansville, NC (March 1999) with an average value of 120.3 μg N m−2 min−1, and smallest at the tertiary lagoon in Rocky Mount, NC (November 1998) at 40.7 μg N m−2 min−1. Emission rates were found to be correlated with both surface lagoon water temperature and aqueous NHx concentration. The NH3-N flux may be modeled as ln(NH3-N flux)=1.0788+0.0406TL+0.0015([NHx]) (R2=0.74), where NH3-N flux is the ammonia flux from the lagoon surface in μg N m−2 min−1, TL is the lagoon surface water temperature in °C, and [NHx] is the total ammonia-nitrogen concentration in mg N l−1.  相似文献   

19.
Concentrations of a suite of trace elements (Al, Ag, As, Cd, Co, Cr, Cu, Fe, Ni, Pb, Sr, V, Zn) were measured in aerosol and precipitation samples collected at a coastal site in New Castle, NH, from August 1996, through July 1997. Metal concentrations in aerosol and precipitation exhibit a high degree of temporal variability over the annual cycle, varying by approximately one order of magnitude or less for aerosol metals and by ∼2–3 orders of magnitude in precipitation. Estimates of the total annual atmospheric deposition of metals to the Gulf of Maine range from ∼103 kg yr−1 for Ag, ∼104–105 kg yr−1 for the majority of metals, and ∼106 kg yr−1 for the crustal elements Al and Fe.  相似文献   

20.
About 42 Asian-dust storms influenced the mainland and China during 2000–2002. Based on the Micaps meteorology data provided by China Meteorological Administration, the basic characteristics, including the source, movement route and influenced areas were studied for each case. It was shown that about 70% Asian-dust storms that influence China came from Mongolia, and were strengthened during the way from west to east. In 2000–2002, there was about 63.9% Asian-dust weather that might have affected China seas through three different routes. The probability is affecting the Bohai Sea was 27.4%, the Yellow Sea 30.9%, the East China Sea 12.3%, the Korea Channel 20.2% and the Japan Sea 9.2%. Annual dry deposition flux to the Yellow Sea was about 0.13 g m−2 d−1, and in spring was ∼0.20 g m−2 d−1. The total amount of dry deposition to the Yellow Sea was ∼17.9 Tg yr−1.  相似文献   

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