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1.
In April 2000 atmospheric trace gas measurements were performed on the western Indian Ocean on a cruise of the Dutch research vessel Pelagia from the Seychelles (5°S, 55°E) to Djibouti (12°N, 43°E). The measurements included analysis of dimethyl sulfide (DMS), acetone and acetonitrile every 40 s using PTR-MS (proton-transfer-reaction mass spectrometry) and gas chromatographic analyses of C2–C7 hydrocarbons in air samples taken during the cruise. The measurements took place at the end of the winter monsoon season and the sampled air masses came predominantly from the Southern Hemisphere, resulting in low concentrations of some long-lived hydrocarbons, halocarbons, acetone (350 pptv) and acetonitrile (120 pptv). On three consecutive days a diurnal cycle in DMS concentration was observed, which was used to estimate the emission of DMS (1.5±0.7×1013 molecules m−2 s−1) and the 24 h averaged concentration of hydroxyl (OH) radicals (1.4±0.7×106 molecules cm−3). A strongly increased DMS concentration was found at a location where upwelling of deeper ocean waters took place, coinciding with a marked decrease in acetone and acetonitrile. In the northwestern Indian Ocean a slight increase of some trace gases was noticed showing a small influence of pollution from Asia and from northeast Africa as indicated with back trajectory calculations. The air masses from Asia had elevated acetonitrile concentrations showing some influence of biomass burning as was also found during the 1999 Indian Ocean Experiment, whereas the air masses from northeast Africa seemed to have other sources of pollution.  相似文献   

2.
Air–water exchange fluxes of polycyclic aromatic hydrocarbons (PAHs) were simultaneously measured in air and water samples from two sites on the Kenting coast, located at the southern tip of Taiwan, from January to December 2010. There was no significant difference in the total PAH (t-PAH) concentrations in both gas and dissolved phases between these two sites due to the less local input which also coincided to the low levels of t-PAH concentration; the gas and dissolved phases averaged 1.29 ± 0.59 ng m?3 and 2.17 ± 1.19 ng L?1 respectively. The direction and magnitude of the daily flux of PAHs were significantly influenced by wind speed and dissolved PAH concentrations. Individual PAH flux ranged from 627 ng m?2 d?1 volatilization of phenanthrene during the rainy season with storm–water discharges raising dissolved phase concentration, to 67 ng m?2 d?1 absorption of fluoranthene during high wind speed periods. Due to PAH annual fluxes through air–water exchange, Kenting seawater is a source of low molecular weight PAHs and a reservoir of high molecular weight PAHs. Estimated annual volatilization fluxes ranged from 7.3 μg m?2 yr?1 for pyrene to 50 μg m?2 yr?1 for phenanthrene and the absorption fluxes ranged from ?2.6 μg m?2 yr?1 for chrysene to ?3.5 μg m?2 yr?1 for fluoranthene.  相似文献   

3.
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   

4.
A fully automated twin ECD gas chromatograph system with sample enriching adsorption–desorption primary stage was deployed on two field campaigns – Ny-Ålesund, Svalbard, Arctic Norway (July–September 1997), and the RRS Discovery CHAOS cruise of the northeast Atlantic (April–May 1998). Concentrations of an extensive set of halocarbons were detected at hourly intervals at pptv levels. We present here the results obtained for the chlorinated solvents, tetrachloroethene (PCE) and trichloroethene (TCE). Average baseline PCE and TCE concentrations of 1.77 and 0.12 pptv, respectively, were recorded in Ny-Ålesund. During pollution incidences, concentrations rose to 5.61 (PCE) and 3.18 pptv (TCE). The cruise data showed average concentrations ranging from 4.26 (PCE) and 1.66 pptv (TCE) for air masses originating over the North Atlantic and Arctic open oceans, to maxima of 15.59 (PCE) and 17.51 pptv (TCE) for polluted air masses from Northern Europe. The data sets emphasise the difficulties in defining remote sites for background tropospheric halocarbon measurements, as Ny-Ålesund research station proved to be a source of tetrachloroethene. The data also suggest possible oceanic emissions of trichloroethene in the sub-tropical ocean.  相似文献   

5.
Concentrations of size fractionated particulate sodium and potassium were measured in both marine and urban air. Marine air sampling was conducted during a cruise on R/V Hakuho-maru in the northwestern North Pacific in the summer of 1998. Urban air sampling was performed in the central part of Tokyo in 1997 and 1998. The fine sodium concentration (D<1.1 μm) in “Urban” air (180 ng m−3) was 3 times higher than that in “Marine” air (56 ng m−3). In the urban air samples, the size distributions of sodium and potassium showed bimodal peaks in the fine particle range (D<1.1 μm) and in the coarse particle range (D>1.1 μm). The existence of anthropogenic sodium in the fine particle range was detected in the urban air. The K/Na weight ratios in the fine particle range of the urban air (1.8–2.7) was 50–75 times higher than that in seawater (0.036). Potassium in the urban air is thought to be derived largely from anthropogenic sources. In the urban air samples, a high correlation between fine sodium and fine potassium concentrations suggests that they have the same anthropogenic source. Reevaluating the K/Na ratios in marine air to be relatively higher than that in seawater, we can estimate that several percents of anthropogenic sodium can be transported from land to remote marine air.  相似文献   

6.
The soil/plant/atmosphere exchange of carbonyl sulfide (COS) was investigated in an open oak woodland ecosystem at a rural site in northern California. Measurements of atmospheric concentrations of COS were made in June and in December 1994. We found a significant diel cycle with a drop of COS levels by approximately 150 ppt during the night in both seasons. The mean COS daytime background mixing ratios showed a distinct seasonal difference with 465±77 ppt in summer and 375±56 ppt in winter. The nighttime bulk COS flux into the ecosystem was estimated using a micrometeorological model. To address the observed depletion of COS during stable nocturnal boundary layer conditions, the potential of various ecosystem compartments to act as a sink for COS was investigated. Studies using dynamic enclosures flushed with ambient air excluded vegetation as an important sink during nighttime due to high stomatal resistance. Results from soil chamber measurements indicate that the soil can act as a dominant sink for atmospheric COS.  相似文献   

7.
High volume air sampling in Bermuda, Sable Island (Nova Scotia) and along a cruise track from the Gulf of Mexico to northeast coast of the USA, was carried out to assess air concentrations, particle-gas partitioning and transport of polyfluorinated chemicals (PFCs) in this region. Samples were collected in the summer of 2007. Targeted compounds included the neutral PFCs: fluorotelomer alcohols (FTOHs), perfluoroalkyl sulfonamides (FOSAs) and perfluoroalkyl sulfonamido ethanols (FOSEs).Among the FTOHs, 8:2 FTOH was dominant in all samples. Sum of the concentration of FTOHs (gas+particle phase) were higher in Bermuda (mean, 34 pg m?3) compared to Sable Island (mean, 16 pg m?3). In cruise samples, sum of FTOHs were highly variable (mean, 81 pg m?3) reflecting contributions from land-based sources in the northeast USA with concentrations reaching as high as 156 pg m?3.Among the FOSAs and FOSEs, MeFOSE was dominant in all samples. In Bermuda, levels of MeFOSE were exceptionally high (mean, 62 pg m?3), exceeding the FTOHs. Sable Island samples also exhibited the dominance of MeFOSE but at a lower concentration (mean, 15 pg m?3). MeFOSE air concentrations (pg m?3) in cruise samples ranged from 1.6 to 73 and were not linked to land-based sources. In fact high concentrations of MeFOSE observed in Bermuda were associated with air masses that originated over the Atlantic Ocean.The partitioning to particles for 8:2 FTOH, 10:2 FTOH, MeFOSE and EtFOSE ranged from as high as 15 to 42% for cruise samples to 0.9 to 14% in Bermuda. This study provides key information for validating and developing partitioning and transport models for the PFCs.  相似文献   

8.
While the existence of black carbon as part of dissolved organic matter (DOM) has been confirmed, quantitative determinations of dissolved black carbon (DBC) in freshwater ecosystem and information on factors controlling its concentration are scarce. In this study, stream surface water samples from a series of watersheds subject to different burn frequencies in Konza Prairie (Kansas, USA) were collected in order to determine if recent fire history has a noticeable effect on DBC concentration. The DBC levels detected ranged from 0.04 to 0.11 mg L?1, accounting for ca. 3.32 ± 0.51% of dissolved organic carbon (DOC). No correlation was found between DBC concentration and neither fire frequency nor time since last burn. We suggest that limited DBC flux is related to high burning efficiency, possibly greater export during periods of high discharge and/or the continuous export of DBC over long time scales. A linear correlation between DOC and DBC concentrations was observed, suggesting the export mechanisms determining DOC and DBC concentrations are likely coupled. The potential influence of fire history was less than the influence of other factors controlling the DOC and DBC dynamics in this ecosystem. Assuming similar conditions and processes apply in grasslands elsewhere, extrapolation to a global scale would suggest a global grasslands flux of DBC on the order of 0.14 Mt carbon year?1.  相似文献   

9.
Estimates of the atmospheric deposition to Galveston Bay of polycyclic aromatic hydrocarbons (PAHs) are made using precipitation and meteorological data that were collected continuously from 2 February 1995 to 6 August 1996 at Seabrook, TX, USA. Particulate and vapor phase PAHs in ambient air and particulate and dissolved phases in rain samples were collected and analyzed. More than 95% of atmospheric PAHs were in the vapor phase and about 73% of PAHs in the rain were in the dissolved phase. Phenanthrene and napthalene were the dominant compounds in air vapor and rain dissolved phases, respectively, while 5 and 6 ring PAH were predominant in the particulate phase of both air and rain samples. Total PAH concentrations ranged from 4 to 161 ng m−3 in air samples and from 50 to 312 ng l−1 in rain samples. Temporal variability in total PAH air concentrations were observed, with lower concentrations in the spring and fall (4–34 ng m −3) compared to the summer and winter (37–161 ng m−3). PAHs in the air near Galveston Bay are derived from both combustion and petroleum vaporization. Gas exchange from the atmosphere to the surface water is estimated to be the major deposition process for PAHs (1211 μg m− 2 yr− 1), relative to wet deposition (130 μg m−2 yr− 1) and dry deposition (99 μg m−2 yr− 1). Annual deposition of PAHs directly to Galveston Bay from the atmosphere is estimated as 2  t yr−1.  相似文献   

10.
Produced water samples from the Bacia de Campos oil field offshore Pargo andPampo platforms were analyzed for Ba, 226Ra, 228Ra, V, Ni and Pb. The activity concentrations measured were in the range of 1.6–6.0 Bq/L for 226Ra and 0.7–8.2 Bq/L for 228Ra for both platforms. For Ba, V, Ni and Pb the concentrations measured were in the range of 5.6–25.7 mg/L, 0.15–0.46 μg/L, 4.85–12.14 μg/L and 4.04–12.37 μg/L. A strong correlation between barium and radium isotopes concentration was observed (226Ra: R2 = 0.897;228 Ra: R2 = 0.737). In order to evaluate the environmental impact from discharges of produced water into the sea, the seawater and sediment samples were collected at distances from 250 to 1000 m around the platforms. The seawater samples were analyzed for dissolved and particulate material and the sediment samples for total and leachable fraction. The results show that even for the shortest sampling distance (250 m) from the discharge point, Ba, 226Ra, 228Ra, V, Ni and Pb concentrations in seawater and sediment were similar to the local background, indicating that dispersion by local currents minimizes any environmental impact involving these parameters.  相似文献   

11.
Even though dry deposition and air–water exchange of semivolatile organic compounds (SOCs) are important for surfaces in and around the urban areas, there is still no generally accepted direct measurement technique for dry deposition. In this study, a modified water surface sampler (WSS) configuration, including a filter holder and an XAD-2 resin column, was employed to investigate the polycyclic aromatic hydrocarbon (PAH) dry deposition in an urban area. The measured total (particle+dissolved) PAH fluxes to the WSS averaged to be 34 960±16 540 ng m−2 d−1. Average particulate PAH flux, determined by analyzing the filter in the WSS, was about 8% of the total PAH flux. Temporal flux variations indicated that colder months (October–April) had the highest PAH fluxes. This increase could be attributed to the residential heating as well as meteorological effects including lower mixing height. A high volume air sampler was concurrently employed to collect ambient air concentrations. The average total (gas+particle) atmospheric PAH concentration (456±524 ng m−3) was within the range of previously measured values at different urban locations. PAH concentrations in urban areas are more than two orders of magnitude higher than those measured in pristine areas and this result may indicate that urban areas have major source sectors and greater deposition rates are expected near to these areas. The average contribution of particle phase was about 10% in total concentration. Simultaneous particulate phase dry deposition and ambient air samples were collected in this study. Then, particulate phase apparent dry deposition velocities were calculated using the fluxes and concentrations for each PAH compound and they ranged from 0.1 to 1.2 cm s−1. These values are in good agreement with previously reported values.  相似文献   

12.
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   

13.
Regional haze from biomass burning in SE Asia is a recurring air pollution phenomenon with a potential impact on the health of several hundred million people. Air quality data in Brunei Darussalam during the 1998 haze episode revealed that only particulate matter is a significant pollutant. The WHO guideline of 70 μg m−3 for PM10 (24 h average) was exceeded on 54 days during the haze episode which lasted from 1 February to 30 April 1998. Concentrations of SO2, NO2, and O3 were all below WHO guidelines and the 8 h guideline for CO was exceeded on only seven occasions. Average daily PM10 concentrations were below 450 μg m−3 but concentrations greater than 600 μg m−3 persisted for several hours at a time and total exposure to such high concentrations could add up to several days over the course of a haze episode. Airborne particles exhibited diurnal variation, typically rising through the night to very high levels in the early morning and thereafter decreasing due largely to meteorological factors. The pollutant standards index (PSI), widely used to report urban air quality, may not be suitable for haze from forest fires as it does not take into account short-term exposure to extremely high particle concentrations of up to 1 mg m−3.  相似文献   

14.
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   

15.
Seawater, atmospheric dimethylsulfide (DMS) and aerosol compounds, potentially linked with DMS oxidation, such as methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO42?) were determined in the North Yellow Sea, China during July–August, 2006. The concentrations of seawater and atmospheric DMS ranged from 2.01 to 11.79 nmol l?1 and from 1.68 to 8.26 nmol m?3, with average values of 6.20 nmol l?1 and 5.01 nmol m?3, respectively. Owing to the appreciable concentration gradient, DMS accumulated in the surface water was transferred into the atmosphere, leading to a net sea-to-air flux of 6.87 μmol m?2 d?1 during summer. In the surface seawater, high DMS values corresponded well with the concurrent increases in chlorophyll a levels and a significant correlation was observed between integrated DMS and chlorophyll a concentrations. In addition, the concentrations of MSA and nss-SO42? measured in the aerosol samples ranged from 0.012 to 0.079 μg m?3 and from 3.82 to 11.72 μg m?3, with average values of 0.039 and 7.40 μg m?3, respectively. Based on the observed MSA, nss-SO42? and their ratio, the relative biogenic sulfur contribution was estimated to range from 1.2% to 11.5%, implying the major contribution of anthropogenic source to sulfur budget in the study area.  相似文献   

16.
To investigate the characteristics of mercury exchange between soil and air in the heavily air-polluted area, total gaseous mercury (TGM) concentration in air and Hg exchange flux were measured in Wanshan Hg mining area (WMMA) in November, 2002 and July–August, 2004. The results showed that the average TGM concentrations in the ambient air (17.8–1101.8 ng m−3), average Hg emission flux (162–27827 ng m−2 h−1) and average Hg dry deposition flux (0–9434 ng m−2 h−1) in WMMA were 1–4 orders of magnitude higher than those in the background area. It is said that mercury-enriched soil is a significant Hg source of the atmosphere in WMMA. It was also found that widely distributed roasted cinnabar banks are net Hg sources of the atmosphere in WMMA. Relationships between mercury exchange flux and environmental parameters were investigated. The results indicated that the rate of mercury emission from soil could be accelerated by high total soil mercury concentration and solar irradiation. Whereas, highly elevated TGM concentrations in the ambient air can restrain Hg emission from soil and even lead to strongly atmospheric Hg deposition to soil surface. A great amount of gaseous mercury in the heavily polluted atmosphere may cycle between soil and air quickly and locally. Vegetation can inhibit mercury emission from soil and are important sinks of atmospheric mercury in heavily air-polluted area.  相似文献   

17.
The spatial and temporal variability of sulfur gas fluxes (H2S, COS, CH3SH, DMS, and CS2) at the sediment–air interface were studied in the intertidal Wadden Sea area of Sylt-Rømø (Germany/Denmark) during eight measuring campaigns between June 1991 and September 1994. Measurements were performed mainly at four sites in a sheltered intertidal bay of approximately 6 km2 (Königshafen) and discontinuously in a wider range of the 400 km2 Sylt-Rømø tidal flat area. In situ fluxes of the S-gases were determined by a dynamic chamber technique focusing on dry sediment periods. Additional experiments were conducted in order to determine changes in S-gas concentrations in the sediment between the surface and 70 cm depth.In most cases H2S was the dominant S-gas emitted from the sediment to the atmosphere, contributing up to 70% of the total S-emission at this interface. Mean H2S emission rates ranged between 0.07 and 9.95 μg S m-2 h-1. Both emission rates and relative contribution of H2S were lowest from fine sand and highest from muddy sites. Diurnal variation of H2S emission was evident in summer and fall with up to 10-fold higher rates during night than during the day. Distinct seasonal variation of H2S-transfer between the sediment and the atmosphere was observed with higher emission rates in the summer than in spring or fall. The emission of H2S to the atmosphere was smaller by a factor of 1600–26 000 than the H2S produced from sulfate reduction. Apparently, the efficiency by which H2S produced in the sediment is retained and reoxidized by biogeochemical sediment processes is extremely high. Carbonyl sulfide (COS) was emitted with relatively constant rates in space and time with mean flux rates ranging between 0.24 and 2.0 μg S m-2 h-1. Carbon disulfide emission rates were comparable to those of COS and varied between 0.3 and 2.23 μg S m-2 h-1. DMS played a minor role in the S-gas transfer from uncovered sediment areas contributing between 3.1 and 23% to total S-emission from the sediment to the atmosphere.  相似文献   

18.
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   

19.
Neutral volatile and semi-volatile polyfluorinated organic compounds (PFC) and ionic perfluorinated compounds were determined in air samples collected at two sites in the vicinity of Hamburg, Germany, and onboard the German research vessel Atair during a cruise in the German Bight, North Sea, in early November 2007. PUF/XAD-2/PUF cartridges and glass fiber filters as sampling media were applied to collect several fluorotelomer alcohols (FTOH), fluorotelomer acrylates (FTA), perfluoroalkyl sulfonamides (FASA), and perfluoroalkyl sulfonamido ethanols (FASE) in the gas- and particle-phase as well as a set of perfluorinated carboxylates (PFCA) and sulfonates (PFSA) in the particle-phase. This study presents the distribution of PFC in ambient air of the German North Sea and in the vicinity of Hamburg for the first time. Average total PFC concentrations in and around Hamburg (180 pg m?3) were higher than those observed in the German Bight (80 pg m?3). In the German Bight, minimum–maximum gas-phase concentrations of 17–82 pg m?3 for ΣFTOH, 2.6–10 pg m?3 for ΣFTA, 10–15 pg m?3 for ΣFASA, and 2–4.4 pg m?3 for ΣFASE were determined. In the vicinity of Hamburg, minimum–maximum gas-phase concentrations of 32–204 pg m?3 for ΣFTOH, 3–26 pg m?3 for ΣFTA, 3–18 pg m?3 for ΣFASA, and 2–15 pg m?3 for ΣFASE were detected. Concentrations of perfluorinated acids were in the range of 1–11 pg m?3. FTOH clearly dominated the substance spectrum; 8:2 FTOH occurred in maximum proportions. Air mass back trajectories, cluster, and correlation analyses revealed that the air mass origin and thus medium to long range atmospheric transport was the governing parameter for the amount of PFC in ambient air. Southwesterly located source regions seemed to be responsible for elevated PFC concentrations, local sources appeared to be of minor importance.  相似文献   

20.
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   

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