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1.
Croplands contribute to atmospheric nitric oxide (NO), but very limited data are available about NO fluxes from intensively managed croplands in China. In this study, NO fluxes were measured in a typical vegetable field planted with flowering Chinese cabbage (Brassica campestris L. ssp. Chinensis var. utilis Tsen et Lee), which is the most widely cultivated vegetable in Guangdong province, south China. NO emission drastically increased after nitrogen fertilizer application, and other practices involving loosening the soil also enhanced NO emission. Mean NO emission flux was 47.5 ng N m−2 s–1 over a complete growth cycle. Annual NO emission from the vegetable field was about 10.1 kg N ha−1 yr−1. Fertilizer-induced NO emission factor was estimated to be 2.4%. Total NO emission from vegetable fields in Guangdong province was roughly estimated to be 11.7 Gg N yr−1 based on the vegetable field area and annual NO emission rate, and to be 13.3 Gg N yr−1 based on fertilizer-induced NO emission factor and background NO emission. This means that NO emission from vegetable fields was approximately 6% of NOx from commercial energy consumption in Guangdong province.  相似文献   

2.
Static chamber method was adopted to measure the surface exchanges of NO and NO2 between three kinds of agricultural lands and the atmosphere during spring–summer period in the Yangtze Delta, China. The average NO fluxes were 20.9, 27.4 and 21.4 ng N m−2 s−1, respectively, for cabbage (CA, cultivation of celery occurred along with cabbage), potato (PO) and soybean (SY) fields. The average NO2 fluxes were −1.12, 0.93 and −0.68 ng N m−2 s−1, respectively, for the cabbage, potato and soybean fields. Apparently, negative linear correlation was found between the NO2 fluxes from the CK plot (tilled conventionally but did not cultivate any seeds) and its ambient concentrations, and the compensation point was calculated to be 0.92 ppbv. The total NO emission from the vegetable lands and SY land in this region during spring–summer period was roughly estimated to be 15.9 Gg N, which accounted for about 11.2% of the estimated value of total NO emissions in the July of 1999 from Chinese agricultural fields.  相似文献   

3.
In China, vegetable croplands are characterized by intensive fertilization and cultivation, which produce significant nitrogenous gases to the atmosphere. In this study, nitric oxides (NOX) and nitrous oxide (N2O) emissions from the croplands cultivated with three typical vegetables had been measured in Yangtze River Delta of China from September 2 to December 16, 2006. The NO fluxes varied in the ranges of 1.6–182.4, 1.4–2901 and 0.5–487 ng Nm?2 s?1 with averages of 33.8 ± 44.2, 360 ± 590 and 76 ± 112 (mean ± SD) ngNm?2 s?1 for cabbage, garlic, and radish fields (n = 88), respectively. N2O fluxes from the three vegetable fields were found to occur in pulses and significantly promoted by tillage with average values of 5.8, 8.8, and 4.3 ng Nm?2 h?1 for cabbage, garlic, and radish crops, respectively. Influence of vegetables canopy on the NO emission was investigated and quantified. It was found that on cloudy days the canopy can only shield NO emission from croplands soil while on sunny days it cannot only prevent NO emission but also assimilate NO through the open leaves stomas. Multiple linear regression analysis indicated that soil temperature was the most important factor in controlling NO emission, followed by fertilizer amount and gravimetric soil water content. About 1.2%, 11.56% and 2.56% of applied fertilizers N were emitted as NO–N and N2O–N from the cabbage, garlic and radish plots, respectively.  相似文献   

4.
Seasonal patterns of atmospheric mercury (Hg) fluxes measured over vegetated terrestrial systems can provide insight into the underlying process controlling emission and deposition of Hg to vegetated surfaces. Gaseous elemental Hg fluxes were measured for week-long periods in each season (spring, summer, fall, and winter) over an uncontaminated high-elevation wetland meadow in Shenandoah National Park, Virginia using micrometeorological methods. Mean net deposition was observed in the spring (?4.8 ng m?2 h?1), emission in the summer (2.5 ng m?2 h?1), near zero flux in the fall (0.3 ng m?2 h?1), and emission in the winter (4.1 ng m?2 h?1). Nighttime deposition (when stomata are closed) and the poor correlation between Hg fluxes and canopy conductance during periods of active vegetation growth suggest that stomatal processes are not the dominant mechanism for ecosystem-level GEM exchange at this site. The strong springtime deposition relative to summer implies that young vegetation is better at scavenging Hg, with the highest deposition occurring at night possibly via a cuticular pathway. These results suggest that spring is a period of GEM deposition while other seasons exhibit net emission, emphasizing the importance of capturing GEM flux seasonality when determining total Hg budgets.  相似文献   

5.
Agricultural soils may account for 10% of anthropogenic emissions of NO, a precursor of tropospheric ozone with potential impacts on air quality and global warming. However, the estimation of this biogenic source strength and its relationships to crop management is still challenging because of the spatial and temporal variability of the NO fluxes.Here, we present a combination of new laboratory- and field-scale methods to characterise NO emissions and single out the effects of environmental drivers.First, NO fluxes were continuously monitored over the growing season of a maize-cropped field located near Paris (France), using 6 automatic chambers. Mineral fertilizer nitrogen was applied from May to October 2005. An additional field experiment was carried out in October to test the effects of N fertilizer form on the NO emissions. The automatic chambers were designed to measure simultaneously the NO and N2O gases. Laboratory measurements were carried out in parallel using soil cores sampled at same site to test the response of NO fluxes to varying soil N–NH4 and water contents, and temperatures. The effects of soil core thickness were also analysed.The highest NO fluxes occurred during the first 5 weeks following fertilizer application. The cumulative loss of NO–N over the growing season was estimated at 1.5 kg N ha?1, i.e. 1.1% of the N fertilizer dose (140 kg N ha?1). All rainfall events induced NO peak fluxes, whose magnitude decreased over time in relation to the decline of soil inorganic N. In October, NO emissions were enhanced with ammonium forms of fertilizer N. Conversely, the application of nitrate-based fertilizers did not significantly increase NO emissions compared to an unfertilized control. The results of the subsequent laboratory experiments were in accordance with the field observations in magnitude and time variations. NO emissions were maximum with a water soil content of 15% (w w?1), and with a NH4–N content of 180 mg NH4–N kg soil?1. The response of NO fluxes to soil temperature was fitted with two exponential functions, involving a Q10 of 2.0 below 20 °C and a Q10 of 1.4 above. Field and laboratory experiments indicated that most of the NO fluxes originated from the top 10 cm of soil. The characterisation of this layer in terms of mean temperature, NH4 and water contents is thus paramount to explaining the variations of NO fluxes.  相似文献   

6.
Aerosol samples (TSP and PM10) during each season were collected at a national monitoring point in Shanghai in 2008. Halogens (Br, I) were determined in samples along with sodium (Na) by ICP-MS and ICP-OES after microwave digestion. In this report we focused on the concentration characteristics of halogen elements Br and I and their seasonal distributions. The mean annual concentrations of total Br and I were 24 ng m?3 and 12 ng m?3 for TSP, 21 ng m?3 and 9 ng m?3 for PM10, respectively. Concentrations of Br and I in TSP and PM10 were lowest in summer but an increase occurred in autumn and winter. Water-soluble Br and I accounted for about 32% of the total Br and I in aerosols, and about 68% of Br and I was non soluble which may be non-soluble organic species. These non-soluble organic species are present in aerosols in the possible binding forms as mineral dust, natural organic matter, and adsorption to black carbon or mineral material such as iron oxides. Soluble Br and I in PM10 extracted by a dilute acid solution (HNO3 + H2SO4) increased by 22% and 18%, respectively, compared with water-soluble Br and I. A positive correlation with Na and sea water enrichment factors for Br and I indicated that bromine and iodine in aerosols originated mostly from marine sources in Shanghai.  相似文献   

7.
In the United States, fertilized corn fields, which make up approximately 5% of the total land area, account for approximately 45% of total soil NOx emissions. Leaf chamber measurements were conducted of NO and NO2 fluxes between individual corn leaves and the atmosphere in (1) field-grown plants near Champaign, IL (USA) in order to assess the potential role of corn canopies in mitigating soil–NOx emissions to the atmosphere, and (2) greenhouse-grown plants in order to study the influence of various environmental variables and physiological factors on the dynamics of NO2 flux. In field-grown plants, fluxes of NO were small and inconsistent from plant to plant. At ambient NO concentrations between 0.1 and 0.3 ppbv, average fluxes were zero. At ambient NO concentrations above 1 ppbv, NO uptake occurred, but fluxes were so small (14.3±0.0 pmol m−2 s−1) as to be insignificant in the NOx inventory for this site. In field-grown plants, NO2 was emitted to the atmosphere at ambient NO2 concentrations below 0.9 ppbv (the NO2 compensation point), with the highest rate of emission being 50 pmol m−2 s−1 at 0.2 ppbv. NO2 was assimilated by corn leaves at ambient NO2 concentrations above 0.9 ppbv, with the maximum observed uptake rate being 643 pmol m−2 s−1 at 6 ppbv. When fluxes above 0.9 ppbv are standardized for ambient NO2 concentration, the resultant deposition velocity was 1.2±0.1 mm s−1. When scaled to the entire corn canopy, NO2 uptake rates can be estimated to be as much as 27% of the soil-emitted NOx. In greenhouse-grown and field-grown leaves, NO2 deposition velocity was dependent on incident photosynthetic photon flux density (PPFD; 400–700 nm), whether measured above or below the NO2 compensation point. The shape of the PPFD dependence, and its response to ambient humidity in an experiment with greenhouse-grown plants, led to the conclusion that stomatal conductance is a primary determinant of the PPFD response. However, in field-grown leaves, measured NO2 deposition velocities were always lower than those predicted by a model solely dependent on stomatal conductance. It is concluded that NO2 uptake rate is highest when N availability is highest, not when the leaf deficit for N is highest. It is also concluded that the primary limitations to leaf-level NO2 uptake concern both stomatal and mesophyll components.  相似文献   

8.
We present here a novel instrument for measuring surface–atmosphere exchange fluxes of ammonia. The instrument is the upgraded version of a recently developed near-infrared diode laser based photoacoustic ammonia concentration monitoring instrument, i.e. the original instrument is supplemented with two additional sampling lines, an appropriate gas handling system and an advanced software controlling gradient measurements. As a result of these developments, ammonia concentration can be measured simultaneously at three different heights above the ground and ammonia fluxes can be calculated from these data using the aerodynamic gradient method. The instrument operates fully automatically, requires minimal maintenance and has a temperature controlled, waterproof housing which makes it suitable for measurements even under harsh field conditions. Preliminary tests on stability and accuracy were carried out during two two-week field measurement campaigns, with the three sampling inlets being placed at the same height together with the inlet of a reference instrument. The readings of the three channels agreed well (with correlation coefficients above 0.96). Comparison to reference instruments showed good stability of the photoacoustic instrument, there was no measurable zero-drift or change in sensitivity during the tests. Flux measurements were carried out during a three-week field campaign in southern Scotland over fertilized grassland with reference to a wet-chemical AMANDA instrument in gradient configuration. Ammonia fluxes calculated from the data of the two instruments agreed well. Fluxes up to 2500 ng m?2 s?1 were observed after fertilization. The minimum detectable ammonia flux was calculated on the basis of “virtual ammonia fluxes”, from measurements carried out with all inlets at the same height and was found to be ±60 ng m?2 s?1 which ensures reliable measurements above intensively managed grasslands or agricultural fields.  相似文献   

9.
From September 2006 to October 2007 turbulent fluxes of carbon dioxide were measured at an urban tower station (26 m above ground level, z/zh = 1.73) in Essen, Germany, using the eddy covariance technique. The site was located at the border between a public park area (70 ha) in the south–west of the station and suburban/urban residential as well as light commercial areas in the north and east of the tower. Depending on the land-use two different sectors (park and urban) were identified showing distinct differences in the temporal evolution of the surface-atmosphere exchange of CO2. While urban fluxes appear to be governed by anthropogenic emissions from domestic heating and traffic (average flux 9.3 μmol m?2 s?1), the exchange of CO2 was steered by biological processes when the park contributed to the flux footprint. The diurnal course during the vegetation period exhibited negative daytime fluxes up to ?10 μmol m?2 s?1 on average in summer. Nevertheless, with a mean of 0.8 μmol m?2 s?1 park sector fluxes were slightly positive, thus no net carbon uptake by the surface occurred throughout the year.In order to sum the transport of CO2 a gap-filling procedure was performed by means of artificial neural network generalisation. Using additional meteorological inputs the daily exchange of CO2 was reproduced using radial basis function networks (RBF). The resulting yearly sum of 6031 g m?2 a?1 indicates the entire study site to be a considerable source of CO2.  相似文献   

10.
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   

11.
During a measurement period from June till November 2004, ammonia fluxes above non-fertilized managed grassland in The Netherlands were measured with a Gradient Ammonia—High Accuracy—Monitor (GRAHAM). Compared with earlier ammonia measurement systems, the GRAHAM has higher accuracy and a quality control system.Flux measurements are presented for two different periods, i.e. a warm, dry summer period (from 18 July till 15 August) and a wet, cool autumn period (23 September till 23 October). From these measurements canopy compensation points were derived. The canopy compensation point is defined as the effective surface concentration of ammonia. In the summer period (negative) deposition fluxes are observed in the evening, night and early morning due to leaf surface wetness, while in the afternoon emission fluxes are observed due to high canopy compensation points. The mean NH3-flux in this period was 4 ng m−2 s−1, which corresponds to a net emission of 0.10 kg N ha−1 over the 28 day sampling period. The NH3-flux in the autumn period mainly shows (negative) deposition fluxes due to small canopy compensation points caused by low temperatures and a generally wet surface. The mean NH3-flux in this period is −24 ng m−2 s−1, which corresponds to a net deposition of 0.65 kg N ha−1 over the 31 day sampling period.Frequency distributions of the NH3-concentration and flux show that despite higher average ambient NH3-concentrations (13.3 μg m−3 in the summer period vs. 6.4 μg m−3 in the autumn period) there are more emission events in the summer period than in the autumn period (about 50% of the time in summer vs. 20% in autumn). This is caused by the high canopy compensation points in summer due to high temperatures and a dry surface. In autumn, deposition dominates due to a generally wet surface that induces low canopy compensation points.For our non-fertilized agricultural grassland site, the derived canopy compensation points (at temperatures between 7 and 29 °C) varied from 0.5 to 29.7 μg m−3 and were on an average 7.0 μg m−3, which is quite high for non-fertilized conditions and probably caused by high nitrogen inputs in the past or high dry deposition amounts from local sources. The average value for the ratio between NH4+ and H+ concentration in the canopy, Γc, that was derived from our data was 2200.  相似文献   

12.
Simultaneous daily measurements of water-soluble organic nitrogen (WSON), ammonium and nitrate were made between July and November 2008 at a rural location in south-east Scotland, using a ‘Cofer’ nebulizing sampler for the gas phase and collection on an open-face PTFE membrane for the particle phase. Average concentrations of NH3 were 82 ± 17 nmol N m?3 (error is s.d. of triplicate samples), while oxidised N concentrations in the gas phase (from trapping NO2 and HNO3) were smaller, at 2.6 ± 2.2 nmol N m?3, and gas-phase WSON concentrations were 18 ± 11 nmol N m?3. The estimated collection efficiency of the nebulizing samplers for the gas phase was 88 (±8) % for NH3, 37 (±16) % for NO2 and 57 (±7) % for WSON; reported average concentrations have not been corrected for sampling efficiency. Concentrations in the particle phase were smaller, except for nitrate, at 21 ± 9, 10 ± 6 and 8 ± 9 nmol N m?3, respectively. The absence of correlation in either phase between WSON and either (NH3 + NH4+) or NO3? concentrations suggests atmospheric WSON has diverse sources. During wet days, concentrations of gas and particle-phase inorganic N were lower than on dry days, whereas the converse was true for WSON. These data represent the first reports of simultaneous measurements of gas and particle phase water-soluble nitrogen compounds in rural air on a daily basis, and show that WSON occurs in both phases, contributing 20–25% of the total water-soluble nitrogen in air, in good agreement with earlier data on the contribution of WSON to total dissolved N in rainfall in the UK.  相似文献   

13.
Improved measurements of ammonia losses from cattle feedlots are needed to quantify the national NH3 emissions inventory and evaluate management techniques for reducing emissions. Speciation cartridges composed of glass honeycomb denuders and filter packs were adapted to measure gaseous NH3 and aerosol NH4+ fluxes using relaxed eddy accumulation (REA). Laboratory testing showed that a cartridge equipped with four honeycomb denuders had a total capture capacity of 1800 μg of NH3. In the field, a pair of cartridges was deployed adjacent to a sonic anemometer and an open-path gas analyzer on a mobile tower. High-speed valves were attached to the inlets of the cartridges and controlled by a datalogger so that up- and down-moving eddies were independently sampled based on direction of the vertical wind speed and a user-defined deadband. Air flowed continuously through the cartridges even when not sampling by means of a recirculating air handling system. Eddy covariance measurement of CO2 and H2O, as measured by the sonic and open-path gas analyzer, were used to determine the relaxation factor needed to compute REA-based fluxes. The REA system was field tested at the Beef Research Unit at Kansas State University in the summer and fall of 2007. Daytime NH3 emissions ranged between 68 and 127 μg m?2 s?1; fluxes tended to follow a diurnal pattern correlated with latent heat flux. Daily fluxes of NH3 were between 2.5 and 4.7 g m?2 d?1 and on average represented 38% of fed nitrogen. Aerosol NH4+ fluxes were negligible compared with NH3 emissions. An REA system designed around the high-capacity speciation cartridges can be used to measure NH3 fluxes from cattle feedlots and other strong sources. The system could be adapted to measure fluxes of other gases and aerosols.  相似文献   

14.
Measurements of NO and NO2 were made at a surface site (55.28 °N, 77.77 °W) near Kuujjuarapik, Canada during February and March 2008. NOx mixing ratios ranged from near zero to 350 pptv with emission from snow believed to be the dominant source. The amount of NOx was observed to be dependent on the terrain over which the airmass has passed before reaching the measurement site. The 24 h average NOx emission rates necessary to reproduce observations were calculated using a zero-dimensional box model giving rates ranging from 6.9 × 108 molecule cm?2 s?1 to 1.2 × 109 molecule cm?2 s?1 for trajectories over land and from 3.8 × 108 molecule cm?2 s?1 to 6.6 × 108 molecule cm?2 s?1 for trajectories over sea ice. These emissions are higher than those suggested by previous studies and indicate the importance of lower latitude snowpack emissions. The difference in emission rate for the two types of snow cover shows the importance of snow depth and underlying surface type for the emission potential of snow-covered areas.  相似文献   

15.
In Brazil, sugarcane fields are often burned to facilitate manual harvesting, and this burning causes environmental pollution from the large amounts of soot released into the atmosphere. This material contains numerous organic compounds such as PAHs. In this study, the concentrations of PAHs in two particulate-matter fractions (PM2.5 and PM10) in the city of Araraquara (SE Brazil, with around 200,000 inhabitants and surrounded by sugarcane plantations) were determined during the sugarcane harvest (HV) and non-harvest (NHV) seasons in 2008 and 2009. The sampling strategy included four campaigns, with 60 samples in the NHV season and 220 samples in the HV season. The PM2.5 and PM10 fractions were collected using a dichotomous sampler (10 L min?1, 24 h) with Teflon? filters. The filter sets were extracted (ultrasonic bath with hexane/acetone (1:1 v/v)) and analyzed by HPLC/Fluorescence. The median concentration for total PAHs (PM2.5 in 2009) was 0.99 ng m?3 (NHV) and 3.3 ng m?3 (HV). In the HV season, the total concentration of carcinogenic PAHs (benz(a)anthracene, benzo(b)fluoranthene, benzo(k)fluoranthene, and benzo(a)pyrene) was 5 times higher than in the NHV season. B(a)P median concentrations were 0.017 ng m?3 and 0.12 ng m?3 for the NHV and HV seasons, respectively. The potential cancer risk associated with exposure through inhalation of these compounds was estimated based on the benzo[a]pyrene toxic equivalence (BaPeq), where the overall toxicity of a PAH mixture is defined by the concentration of each compound multiplied by its relative toxic equivalence factor (TEF). BaPeq median (2008 and 2009 years) ranged between 0.65 and 1.0 ng m?3 and 1.2–1.4 ng m?3 for the NHV and HV seasons, respectively. Considering that the maximum permissible BaPeq in ambient air is 1 ng m?3, related to the increased carcinogenic risk, our data suggest that the level of human exposure to PAHs in cities surrounded by sugarcane crops where the burning process is used is cause for concern.  相似文献   

16.
Land spreading nitrogen-rich municipal waste biosolids (NO3-N<256 mg N kg−1 dry weight, NH3-N∼23,080 mg N kg−1 dry weight, Total Kjeldahl N∼41,700 mg N kg−1 dry weight) to human food and non-food chain land is a practice followed throughout the US. This practice may lead to the recovery and utilization of the nitrogen by vegetation, but it may also lead to emissions of biogenic nitric oxide (NO), which may enhance ozone pollution in the lower levels of the troposphere. Recent global estimates of biogenic NO emissions from soils are cited in the literature, which are based on field measurements of NO emissions from various agricultural and non-agricultural fields. However, biogenic emissions of NO from soils amended with biosolids are lacking. Utilizing a state-of-the-art mobile laboratory and a dynamic flow-through chamber system, in-situ concentrations of nitric oxide (NO) were measured during the spring/summer of 1999 and winter/spring of 2000 from an agricultural soil which is routinely amended with municipal waste biosolids. The average NO flux for the late spring/summer time period (10 June 1999–5 August 1999) was 69.4±34.9 ng N m−2 s−1. Biosolids were applied during September 1999 and the field site was sampled again during winter/spring 2000 (28 February 2000–9 March 2000), during which the average flux was 3.6±1.7 ng N m−2 s−1. The same field site was sampled again in late spring (2–9 June 2000) and the average flux was 64.8±41.0 ng N m−2 s−1. An observationally based model, developed as part of this study, found that summer accounted for 60% of the yearly emission while fall, winter and spring accounted for 20%, 4% and 16% respectively. Field experiments were conducted which indicated that the application of biosolids increases the emissions of NO and that techniques to estimate biogenic NO emissions would, on a yearly average, underestimate the NO flux from this field by a factor of 26. Soil temperature and % water filled pore space (%WFPS) were observed to be significant variables for predicting NO emissions, however %WFPS was found to be most significant during high soil temperature conditions. In the range of pH values found at this site (5.8±0.3), pH was not observed to be a significant parameter in predicting NO emissions.  相似文献   

17.
Multi-year hourly measurements of PM2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m?3 with peak hourly values of several μg m?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NOx showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m?3 with maximum hourly concentrations of 7–11 μg m?3 predominantly in summer or winter months. OC concentrations generally correlated with PM2.5 total mass and aerosol sulfate and with NOx during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NOx indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.  相似文献   

18.
Daily and seasonal variations in dry and wet atmospheric nitrogen fluxes have been studied during four campaigns between 2004 and 2006 at a coastal site of the Southern North Sea at De Haan (Belgium) located at coordinates of 51.1723° N and 3.0369° E. Concentrations of inorganic N-compounds were determined in the gaseous phase, size-segregated aerosol (coarse, medium, and fine), and rainwater samples. Dissolved organic nitrogen (DON) was quantified in rainwater. The daily variations in N-fluxes of compounds were evaluated with air-mass backward trajectories, classified into the main air-masses arriving at the sampling site (i.e., continental, North Sea, and Atlantic/UK/Channel).The three, non-episodic campaigns showed broadly consistent fluxes, but during the late summer campaign exceptionally high episodic N-deposition was observed. The average dry and wet fluxes for non-episodic campaigns amounted to 2.6 and 4.0 mg N m?2 d?1, respectively, whereas during the episodic late summer period these fluxes were as high as 5.2 and 6.2 mg N m?2 d?1, respectively.Non-episodic seasons/campaigns experienced average aerosol fluxes of 0.9–1.4 mg N m?2 d?1. Generally, the contribution of aerosol NH4+ was more significant in the medium and fine particulate fractions than that of aerosol NO3?, whereas the latter contributed more in the coarse fraction, especially in continental air-masses. During the dry mid-summer campaign, the DON contributed considerably (~15%) to the total N-budget.Exceptionally high episodic aerosol-N inputs have been observed for the late summer campaign, with especially high deposition rates of 3.6 and 2.9 mg N m?2 d?1 for Atlantic/UK/Channel and North Sea-continental (mixed) air-masses, respectively. During this pollution episode, the flux of NH4+ was dominating in each aerosol fraction/air-mass, except for coarse continental aerosols. High deposition of gaseous-N was also observed in this campaign with an average total N-flux of 2–2.5-times higher than in other campaigns.  相似文献   

19.

From simultaneous air and water polychlorinated biphenyl (PCB) measurements collected in September 2010, we re-evaluated the direction and magnitude of net air-water exchange of PCBs in southwest Lake Michigan and compared them with estimations made using similar approaches 15 years prior. Air and water samples were collected during a research expedition on Lake Michigan at 5 km off the coast of Chicago, with prevailing winds from the southwest of our location. Gas-phase ΣPCB concentrations ranged from 190 to 1100 pg m?3 with a median of 770 pg m?3, which is similar to the concentrations measured in the City of Chicago at the same time and similar to concentrations measured in this part of the lake over the last 20 years. Water dissolved-phase ΣPCB concentrations ranged from 150 to 170 pg L?1 with a median of 160 pg L?1, which is one-tenth of that measured in the 1990s. ?PCB net fluxes showed a slightly absorptive behavior, with a median of (?) 21 ng m?2 day?1 and an interquartile range of (?) 47 to (+) 5 ng m?2 day?1, where (?) and (+) fluxes indicate absorption and volatilization, respectively. Airborne PCB concentrations were higher when the winds were coming from Chicago and drive the deposition. Our fluxes are not significantly different from estimations from 1994 and 1995 and suggest that absorption of PCBs into the waters is slightly more prevalent than 15 years ago. It was confirmed that Chicago remains an important atmospheric source of PCBs to Lake Michigan.

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20.
During the summertime of 2007/2008, carbon dioxide (CO2) and methane (CH4) fluxes across air–water interface were investigated in the littoral zones of Lake Mochou and Lake Tuanjie, east Antarctica, using a static chamber technique. The mean fluxes of CO2 and CH4 were ?70.8 mgCO2 m?2 h?1 and 144.6 μgCH4 m?2 h?1, respectively, in the littoral zone of Lake Mochou; The mean fluxes were ?36.9 mgCO2 m?2 h?1 and 109.8 μgCH4 m?2 h?1, respectively, in the littoral zone of Lake Tuanjie. Their fluxes showed large temporal and spatial dynamics. The CO2 fluxes showed a significantly negative correlation with daily total radiation (DTR) and a weakly negative correlation with air temperature and water temperature, indicating that sunlight intensity controlled the magnitude of CO2 fluxes from the open lakes. The CH4 fluxes significantly correlated with local air temperature, water table and total dissolved solids (TDS), indicating that they were the predominant factors influencing CH4 fluxes. Summertime CO2 budgets in the littoral zones of Lake Mochou and Lake Tuanjie were estimated to be ?152.9 gCO2 m?2 and ?79.7 gCO2 m?2, respectively, and net CH4 emissions were estimated to be 312.3 mgCH4 m?2 and 237.2 mgCH4 m?2, respectively. Our results show that shallow, open, alga-rich lakes might be strong summertime CO2 absorbers and small CH4 emitters during the open water in coastal Antarctica.  相似文献   

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