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1.
Simultaneous chloroform (CHCl3) emission and ozone (O3) deposition are regularly observed under nocturnal inversions during the summer months from and to the peat bogs in the vicinity of the Mace Head Atmospheric Research Station, Connemara, Co Galway, Ireland. Emissions were estimated using the nocturnal box model applied to routine atmospheric observations collected over a 14-year period from 1995 to 2008. Strict criteria were applied in the selection of events of low wind speed, under a stable night-time inversion layer in baseline air conditions, with no transport from Europe. The mean peatland CHCl3 flux was 2.91 μg m?2 h?1 with highly variable fluxes ranging from 0.44 to 12.94 μg m?2 h?1. These fluxes are generally larger than those reported previously for similar biomes and if representative would make a significant contribution to the global estimated source of CHCl3. Fluxes were not strongly correlated with either atmospheric temperature or the level of precipitation. Over the 14-year period there appears to have been a small increase in overall CHCl3 emissions, although we stress that the nocturnal box model has a number of limitations and assumptions which should be taken into account.  相似文献   

2.
The present study focuses on the exceptional Saharan dust event that affected most of France in February 2004. Activity levels of various artificial radionuclides (90Sr, 137Cs, uranium, thorium and plutonium isotopes, 241Am) were examined. Activity or isotopic ratios are discussed in the context of atmospheric nuclear weapons tests, among them French tests performed in Sahara in the 1960s. The daily evolution of 137Cs activity levels in the atmosphere was compared to daily PM10 change. A link between airborne 137Cs and PM10, is given. It is estimated that this 2-day event deposited as much 137Cs as would be deposited on average over a 10-month period. The amount of deposited 137Cs and 239+240Pu represents respectively about 0.1 and 1% of the activity already present in the soil. Such Saharan dust events correspond to an extreme type of “feeder” process of artificial radionuclides in the atmosphere. Therefore, they contribute to the long term background level of artificial radionuclides kept at trace levels in the atmosphere.  相似文献   

3.
Abstract

Biofiltration of periodically fluctuating concentrations of an α-pinene-laden waste gas was investigated to treat both high-frequency and low-frequency fluctuations. The effects of periodic concentration fluctuations on biofilter performance were measured. Controlled variables of periodic operation included cycle period and amplitude. The cycle period ranged from 10 min to 6 days, with the inlet α-pinene concentration fluctuating between 0 and 100 parts per million volume. At high-frequency concentration cycling (i.e., on the order of minutes), both cyclic and constant concentration biofilters maintained similar long-term performance with an average removal efficiency of 77% at an averaged loading rate of 29 g α-pinene/m3 bed/hr. A first approximation suggests kinetics that are time-independent, indicating that steady-state data can be used to predict transient behavior at this time scale. Cyclic biofilter operation with a cycle period of 24 hr (with equal on/off time) was achievable for biofilters without a significant loss in performance. At longer time scales, cyclic biofilter performance decreased at the restart of the ON cycle. The recovery time to previous levels of performance increased with increasing cycle period; the recovery time was less than 1 hr for a cycle period of 24 hr and between 6 and 8 hr for a cycle period of 6 days.  相似文献   

4.
222Rn concentrations in the air in Nerja Cave (Spain) have been measured over 4 yr and at four sampling points. Concentrations average 168 Bq m-3 in the spring–summer when the temperature lapse rate provides a stable cave atmosphere. In the autumn–winter, the radon levels decrease to 48 Bq m-3. 222Rn flux has also been measured for soils in the cave, with an average value of 34 × 10-3 Bq m-2 s-1. The average natural flow rate in the spring–summer is about 0.70 m3 s-1 and the autumn–winter is approximately 3.6 m3 s-1 determined over 1992–1995. The radiation exposure levels for workers and tourists represent only a low percentage of the exposure guides for the general population.  相似文献   

5.
Plant species release appreciable quantities of volatile organic substances to the atmosphere. The major compounds emitted are monoterpenes (C10) like α-pinene, β-pinene, and limonene and the hemiterpene (C5) isoprene. The rate of emission of isoprene is light dependent and ranges between 0.04 to 2.4 ppb/cm2/min/l for oak, cottonwood, and eucalyptus foliage. The rate of emission of a- and/3-pinene and limonene is dependent on the rate of transpiration, structural integrity of the oil cells and resin glands, and temperature of the foliage. Rates of emission for conifer foliage range from 0.4 to 3.5 ppb/g/min/l. An inventory of North American forest regions for the frequency of occurrence of these chemicals released by different tree species showed that 15% was the lowest value for a specific forest-type that emitted terpenes to the atmosphere. More commonly 100% of the trees of a given forest-type emitted terpenes to the atmosphere. An average of 70% is typical of the United States forested regions as a whole. The annual contribution of forest hydrocarbon emissions to the air pollution problem on a global basis is reflected in the 175 × 106 tons of reactive hydrocarbons from tree foliage sources compared to the 27 × 106 tons from man’s activities; in other words, there is a 6.2-fold greater emission level from natural sources than from man made sources. The fate of these gaseous olefins in the atmosphere is undetermined.  相似文献   

6.
During Fall 1996, epiphytic lichens were collected along altitudinal sections in two areas of France (the Vosges mountains in the North-East, and the Alps, in Haute-Savoie) in order to verify any geographic distribution of atmospheric metals on a small scale. These lichens have various Pb isotopic compositions (206Pb/207Pb=1.126–1.147) which are correlated with the altitude of sampling. Lichens sampled near valleys display isotopic ratios significantly less radiogenic than those sampled at several hundred to thousand meters of altitude. In the Vosges sections, Pb concentrations and isotopic compositions of lichens may be used to define three zones: (1) valley: Pb-rich and non-radiogenic ratios, (2) transition: low-Pb and intermediate isotopic compositions, (3) mountain: heterogeneous Pb concentrations but more radiogenic and homogeneous Pb isotopic composition. Other metals (Zn, Cu, Cd, As), when normalised one to another, are not fractionated between these zones and display homogeneous relative abundance along the altitudinal sections of both sites. Variation of 206Pb/207Pb ratios with altitude is interpreted in terms of mixing of at least two pollution sources: one being the petrol (leaded and/or unleaded) combustion, and the other being of industrial origin. The latter is characterised by a more radiogenic isotopic composition. The Pb isotopic composition of flue gas residues from different municipal solid waste combustors in the Rhine valley and in other areas of France would suggest that these plants might be an important source of industrial Pb in the atmosphere. If the average industrial Pb in France has a 206Pb/207Pb close to 1.15, between 60 and 80% of the total Pb in lichens from the Rhine valley would come from gasoline combustion, whereas 85–90% of the Pb would have an industrial origin in lichens from higher altitude in the Vosges mountains. Although lichens from the Alps were collected at higher altitude, the percentage of industrial Pb for these lichens would be slightly lower (65%). Major winds and convection winds in the different valleys must then play an important role in term of distribution of atmospheric Pb in function of altitude.  相似文献   

7.
Total gaseous mercury (TGM) in the lower atmosphere of northern Wisconsin exhibits strong annual and diurnal cycles similar to those previously reported for other rural monitoring sites across mid-latitude North America. Annually, TGM was highest in late winter and then gradually declined until late summer. During 2002–04, the average TGM concentration was 1.4 ± 0.2 (SD) ng m?3, and the amplitude of the annual cycle was 0.4 ng m?3 (~30% of the long-term mean). The diurnal cycle was characterized by increasing TGM concentrations during the morning followed by decreases during the afternoon and night. The diurnal amplitude was variable but it was largest in spring and summer, when daily TGM oscillations of 20–40% were not uncommon. Notably, we also observed a diurnal cycle for TGM indoors in a room ventilated through an open window. Even though TGM concentrations were an order of magnitude higher indoors, (presumably due to historical practices within the building: e.g. latex paint, fluorescent lamps, thermometers), the diurnal cycle was remarkably similar to that observed outdoors. The indoor cycle was not directly attributable to human activity, the metabolic activity of vegetation or diurnal atmospheric dynamics; but it was related to changes in temperature and oxidants in outdoor air that infiltrated the room. Although there was an obvious difference in the proximal source of indoor and outdoor TGM, similarities in behavior suggest that common TGM cycles may be driven largely by adsorption/desorption reactions involving solid surfaces, such as leaves, snow, dust and walls. Such behavior would imply a short residence time for Hg in the lower atmosphere and intense recycling – consistent with the “ping-pong ball” or “multi-hop” conceptual models proposed by others.  相似文献   

8.
Abstract

An airborne lidar was used to study the smoke plume from the burning of a controlled oil spill on the ocean. The ratio of the amount of light (at a wavelength, λ, of 0.532 u.m) backscattered by the smoke to the amount of light extinguished by the smoke was determined by measuring the strength of a laser beam after it had passed through the smoke plume, been reflected from the ocean, and passed through the smoke plume again, and comparing this to the strength of the laser beam reflected directly from the ocean. The optical depth of the smoke (at λ = 0.532 µm) was typically between 0.2 and 0.5. The mass fluxes of smoke particles that passed through four vertical cross sections of the (nonsteady state) smoke plume were estimated from lidar measurements to be 142, 175, 423, and 414 g s-1, compared to an average smoke mass production rate of ~770 g s-1. The spatial distribution of smoke mass along the long axis of the plume was also estimated from the lidar measurements; derived smoke mass concentrations were generally <300 µg m-3, with a few isolated values up to ~800 µg m-3.  相似文献   

9.
Isoprene is one of the most important biogenic volatile organic compounds with large terrestrial emissions and comparatively a small oceanic source on a global scale. This marine source seems to strongly depend on environmental parameters such as phytoplankton abundance, light, temperature, wind speed, and thus, to be highly variable. However, this source can consequently affect the chemistry of the marine boundary layer on a local or mesoscale. The present study investigates the factors that control isoprene levels and estimates the marine source of isoprene and its role in the oxidizing capacity of the atmosphere at a coastal site in the East Mediterranean. More than 2000 measurements of isoprene have been conducted at Finokalia sampling station on the island of Crete over an 8-month period from February to October 2004. Isoprene varies between 5 and 1200 pptv with the highest values observed in summer. The origin of the air masses determines the atmospheric abundance and the prevailing source of isoprene. According to chemical box model calculations, during daytime the isoprene observed under marine conditions is reducing hydroxyl (OH) and hydroperoxy (HO2) radicals by up to 26% and 13%, respectively, whereas, it can increase the sum of peroxy radicals by a factor of 4. At night, isoprene of marine origin is depressing nitrate radicals by up to 25% and increases the low nighttime levels of OH and HO2 radicals by up to 25% and 30%, respectively. The seawater emissions of isoprene in the area are estimated between 108 and 6×109 molecules cm−2 s−1 with a strong seasonal variability.  相似文献   

10.
The ambient air in Northern Italy is characterised by relatively high PAH and PM10 concentrations in relation to calm wind and intensive temperature inversions, especially during cold periods. These stagnant conditions are occasionally interrupted by North-Föhn events, which cause a drop in relative humidity and an increase in O3 levels, indicating the mixing of local and free troposphere air flows. In this study the influence of the North-Föhn on concentrations of tracer organic compounds, including polycyclic aromatic hydrocarbons (PAHs), PM10, O3 and black carbon (BC) was studied during a North-Föhn event in November 2007. Large fluctuations in the concentration of these compounds, as well as changes in PM10 composition due to daytime and night-time variations of local source emissions were observed. Although these events occur at low frequencies (6-10%) they can for short periods, strongly affect the regional air quality by quickly decreasing the concentrations of these tracer organic compounds.  相似文献   

11.
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   

12.
Recent studies suggest that dairy operations may be a major source of non-methane volatile organic compounds in dairy-intensive regions such as Central California, with short chain carboxylic acids (volatile fatty acids or VFAs) as the major components. Emissions of four VFAs (acetic acid, propanoic acid, butanoic acid and hexanoic acid) were measured from two feed sources (silage and total mixed rations (TMR)) at six Central California Dairies over a fifteen-month period. Measurements were made using a combination of flux chambers, solid phase micro-extraction fibers coupled to gas chromatography mass spectrometry (SPME/GC–MS) and infra-red photoaccoustic detection (IR-PAD for acetic acid only). The relationship between acetic acid emissions, source surface temperature and four sample composition factors (acetic acid content, ammonia-nitrogen content, water content and pH) was also investigated. As observed previously, acetic acid dominates the VFA emissions. Fluxes measured by IR-PAD were systematically lower than SPME/GC–MS measurements by a factor of two. High signals in field blanks prevented emissions from animal waste sources (flush lane, bedding, open lot) from being quantified. Acetic acid emissions from feed sources are positively correlated with surface temperature and acetic acid content. The measurements were used to derive a relationship between surface temperature, acetic acid content and the acetic acid flux. The equation derived from SPME/GC–MS measurements predicts estimated annual average acetic acid emissions of (0.7 + 1/?0.4) g m?2 h?1 from silage and (0.2 + 0.3/?0.1) g m?2 h?1 from TMR using annually averaged acetic acid content and meteorological data. However, during the summer months, fluxes may be several times higher than these values.  相似文献   

13.
Under the National Ambient Air Quality Standards (NAAQS), put in place as a result of the Clean Air Amendments of 1990, three regions in the state of Utah are in violation of the NAAQS for PM10 and PM2.5 (Salt Lake County, Ogden City, and Utah County). These regions are susceptible to strong inversions that can persist for days to weeks. This meteorology, coupled with the metropolitan nature of these regions, contributes to its violation of the NAAQS for PM during the winter. During January–February 2009, 1-hr averaged concentrations of PM10-2.5, PM2.5, NOx, NO2, NO, O3, CO, and NH3 were measured. Particulate-phase nitrate, nitrite, and sulfate and gas-phase HONO, HNO3, and SO2 were also measured on a 1-hr average basis. The results indicate that ammonium nitrate averages 40% of the total PM2.5 mass in the absence of inversions and up to 69% during strong inversions. Also, the formation of ammonium nitrate is nitric acid limited. Overall, the lower boundary layer in the Salt Lake Valley appears to be oxidant and volatile organic carbon (VOC) limited with respect to ozone formation. The most effective way to reduce ammonium nitrate secondary particle formation during the inversions period is to reduce NOx emissions. However, a decrease in NOx will increase ozone concentrations. A better definition of the complete ozone isopleths would better inform this decision.

Implications: Monitoring of air pollution constituents in Salt Lake City, UT, during periods in which PM2.5 concentrations exceeded the NAAQS, reveals that secondary aerosol formation for this region is NOx limited. Therefore, NOx emissions should be targeted in order to reduce secondary particle formation and PM2.5. Data also indicate that the highest concentrations of sulfur dioxide are associated with winds from the north-northwest, the location of several small refineries.  相似文献   


14.
The extent of the exceedance of the EU limit values for nitrogen dioxide (NO2) and particulate matter (PM10) concentrations within the Netherlands is expected to decrease significantly, in the coming years. Whether limit values will actually be exceeded, in the next decade, depends not only on European, national and local policies, but also on the effects of inevitable interannual meteorological fluctuations. An analysis of model calculations and measurements yields variations (1 sigma) in the annual average concentration of about 5% for NO2 and 9% for PM10, due to meteorological fluctuations. These deviations from long-term average concentrations affect assessments of future levels, set against limit values. For instance, an NO2 concentration of 39 μg m?3, estimated for a given year with long-term average meteorology, indicates that it is likely (chance >66%) that the limit value of 40 μg m?3 will not be exceeded in that particular year. At the same time, the estimation also indicates, for example, that this situation is unlikely (change <33%) to continue for three years in a row. However, with an estimated concentration of 38 μg m?3, it is likely that the limit value will not be exceeded for three years in a row. The limit value for the daily average PM10 concentration is equivalent to an annual average of about 32 μg m?3. This threshold is unlikely to be exceeded for three years in a row, when an annual average concentration of 29 μg m?3 is estimated. Interannual variations in concentrations of NO2 and PM10 are linked to large-scale meteorological fluctuations. Therefore, similar results can be expected for other European countries.  相似文献   

15.
Effects of climate change on surface-water photochemistry: a review   总被引:2,自引:0,他引:2  
Information concerning the link between surface-water photochemistry and climate is presently very scarce as only a few studies have been dedicated to the subject. On the basis of the limited knowledge that is currently available, the present inferences can be made as follows: (1) Warming can cause enhanced leaching of ionic solutes from the catchments to surface waters, including cations and more biologically labile anions such as sulphate. Preferential sulphate biodegradation followed by removal as organic sulphides in sediment could increase alkalinity, favouring the generation of the carbonate radical, CO3 ·?. However, this phenomenon would be easily offset by fluctuations of the dissolved organic carbon (DOC), which is strongly anticorrelated with CO3 ·?. Therefore, obtaining insight into DOC evolution is a key issue in understanding the link between photochemistry and climate. (2) Climate change could exacerbate water scarcity in the dry season in some regions. Fluctuations in the water column could deeply alter photochemistry that is usually favoured in shallower waters. However, the way water is lost would strongly affect the prevailing photoinduced processes. Water outflow without important changes in solute concentration would mostly favour reactions induced by the hydroxyl and carbonate radicals (·OH and CO3 ·?). In contrast, evaporative concentration would enhance reactions mediated by singlet oxygen (1O2) and by the triplet states of chromophoric dissolved organic matter (3CDOM*). (3) In a warmer climate, the summer stratification period of lakes would last longer, thereby enhancing photochemical reactions in the epilimnion but at the same time keeping the hypolimnion water in the dark for longer periods.  相似文献   

16.
Polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) were measured in bulk deposition at three Danish rural forest sites with a mutual maximum distance of 450 km. At one of the forest sites concentrations in the ambient atmosphere were sampled from a 12 m high tower. Sampling was carried out within a period of 3 years with sampling intervals of 1–2 months. Mean bulk deposition fluxes were 1 ng m−2 yr−1 I-TEQ and deviated less than 30% between the sites. Yearly average PCDD/F concentrations in the atmosphere were 24 fg m−3 I-TEQ with maximum values in the winter period. During winter months atmospheric concentrations of PCDD/F and oxidized sulphur compounds showed a positive correlation, furthermore seasonal bulk deposition showed correlation between PCDD/F and sulphate.  相似文献   

17.
The anaerobic activities in swine slurry storage and treatment generate biogas containing gaseous ammonia component which is a chemical agent that can cause adverse environmental impacts when released to the atmosphere. The aim of this pilot plant study was to remove ammonia from biogas generated in a covered lagoon, using a sulfuric acid wet scrubber. The data showed that, on average, the biogas contained 43.7 ppm of ammonia and its concentration was found to be exponentially related to the air temperature inside the lagoon. When the air temperature rose to 35°C and the biogas ammonia concentration reached 90 ppm, the mass transfer of ammonia/ammonium from the deeper liquid body to the interface between the air and liquid became a limiting factor. The biogas velocity was critical in affecting ammonia removal efficiency of the wet scrubber. A biogas flow velocity of 8 to 12 mm s?1 was recommended to achieve a removal efficiency of greater than 60%. Stepwise regression revealed that the biogas velocity and air temperature, not the inlet ammonia concentration in biogas, affected the ammonia removal efficiency. Overall, when 73 g L?1 (or 0.75 M) sulfuric acid solution was used as the scrubber solution, removal efficiencies varied from 0% to 100% with an average of 55% over a 40‐d measurement period. Mass balance calculation based on ammonium–nitrogen concentration in final scrubber liquid showed that about 21.3 g of ammonia was collected from a total volume of 1169 m3 of biogas, while the scrubber solution should still maintain its ammonia absorbing ability until its concentration reaches up to 1 M. These results showed promising use of sulfuric acid wet scrubber for ammonia removal in the digester biogas.  相似文献   

18.
Weather modification activities are performed mostly by cloud seeding. Some operational projects have been conducted for more than a half century and cover planetary scales. These activities have led to large amounts of seeding agents being deposited on the ground in precipitation. The main intent of this paper is to identify the spatial pattern of silver iodide deposits after hail suppression. The spatial pattern of silver iodide deposits is determined using the weather modification project measurements from seeding agent reports, two weather radars and 316 launching sites during a 5-year period. The estimated spatial distribution of the deposits is not uniform, with the maximum silver iodide amount located in the southern part of the study area (up to 140 μg m?2). Our results are comparable with the measurements performed by chemical analyses during other cloud seeding experiments. The maximum location coincides well with that of the maximum seeded hailstorm precipitation frequency. A new method for identifying the spatial pattern of wet-deposited material has been established. The location with the maximum amount is found. This method would be important as a means of placing samplers and monitoring at the representative sites because those are where most weather modification projects would be performed in the future.  相似文献   

19.
Carbonyl compounds exist in the atmosphere as either gases or aerosols. Some of them are water soluble and known as oxidation products of biogenic and/or anthropogenic hydrocarbons. Five carbonyl compounds, glyoxal (GO), 4-oxopentanal (4-OPA), glycolaldehyde (GA), hydroxyacetone (HA) and methylglyoxal (MG) have been identified in a temporal series of 12 rain samples. The concentrations of the compounds in the samples were high at the beginning of the rain event and decreased with time to relatively low and fairly constant levels, indicating that the compounds were washed out from the atmosphere at the start of the rain event. Possibly, these compounds also existed in the cloud condensation nuclei (CCN). Wet deposition rates of the carbonyl compounds were calculated for nine samples collected during a 20 h period. The deposition rates ranged from 0 (4-OPA) to 1.2×10−1 mg C m−2 h−1 (MG) with the average of 2.9×10−2 mg C m−2 h−1. Production rates of isoprene oxidation products (GA, HA and MG) in the area surrounding the sampling site were estimated with a chemical box model. The deposition rates exceeded the production rates in most samples. This indicates that the rainfall causes a large net flux of the water soluble compounds from the atmosphere to the ground. Insoluble carbonyl compounds such as n-nonanal and n-decanal were expected to be present in the atmosphere, but were not detected in the rain during the sampling period, suggesting that an aerosol containing these insoluble compounds does not effectively act as a CCN.  相似文献   

20.
A global atmospheric transport model is used to calculate lead concentrations in the atmosphere. The model performance is evaluated through comparisons with observations in Europe. The model results of lead concentrations in surface air were compared with measurements in East Asia. The detailed comparisons showed generally good agreement for recent decades, although systematic underestimation was found in China. Anthropogenic lead emissions in China are estimated from economic statistics to be 56 000 t yr?1, which is not small considering the economic scale of China. The underestimations suggest a hidden source of lead emissions. The emissions in Japan and Korea are derived from optimization by the model. The magnitude is about 2000 t yr?1, which is much greater than that reported by the Pollutant Release and Transfer Register in Japan and Toxics Release Inventory in Korea.  相似文献   

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