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1.
F Nadim  C Perkins  S Liu  R J Carley  G E Hoag 《Chemosphere》2001,45(6-7):1033-1043
Atmospheric mercury was monitored from January 1997 through the end of December 1999 in eight sampling locations in Connecticut. Four sampling locations were chosen along the shores of Long Island Sound and four were chosen in interior sections of Connecticut. Sampling locations were chosen to represent both rural and urban sectors. Average concentrations of gaseous and particulate mercury were found to be 2.06 ng/m3 and 10.5 pg/m3, respectively. The weekly average wet deposition fluxes of mercury and methylmercury over the three-year sampling period were measured to be 611 and 11 microg/ha/week, respectively. Concentrations of gaseous, particulate and wet flux of mercury were found to be significantly higher in urban areas than the rural sampling locations. There was, however, no significant difference between the mean gaseous and particulate concentrations of mercury in coastal and inland sampling locations. No significant difference was observed either between the wet fluxes of total mercury in coastal and inland sampling locations and there was no spatial gradient for mercury concentration and deposition. The data of this study suggest that vehicular traffic and localized emission sources in urban areas play a significant role in determining the atmospheric concentration of mercury in Connecticut.  相似文献   

2.
This study applies a methodology for discriminating local and external contributions of atmospheric particulate matter (PM) at a rural background station in the North-western coast of Spain. The main inputs at the nearest scale have come from soil dust, marine aerosol and road traffic. At a larger scale, the highest contributions have come from fossil-fuel combustion sources, giving rise to relatively high ammonium sulphate background levels, mainly in summer. External contributions from long-range transport processes of African dust and nitrate have been detected. Morocco and Western Sahara have been identified as the main potential source regions of African dust, with a higher content of Al and Ti than other crustal components. Geographical areas from central and Eastern Europe have been identified as potential sources of particulate nitrate. The discrimination of the PM contribution from natural and anthropogenic sources at different geographical scales is a necessary information for establishing PM reduction strategies in specific areas.  相似文献   

3.
A network of eight monitoring stations was established to study the atmospheric nitrogen concentration and deposition in the State of Connecticut. The stations were classified into urban, rural, coastal and inland categories to represent the geographical location and land use characteristics surrounding the monitoring sites. Nitrogen species including nitrate, ammonium, nitric acid vapor and organic nitrogen in the air and precipitation were collected, analyzed and used to infer nitrogen concentrations and dry and wet deposition flux densities for the sampling period from 1997 through 1999, with independently collected meteorological data. Statistical analyses were conducted to evaluate the spatial variations of atmospheric concentration and deposition fluxes of total nitrogen in Connecticut. A slightly higher atmospheric concentration of total nitrogen was observed along the Connecticut coastline of Long Island Sound compared to inland areas, while the differences of nitrogen deposition fluxes were insignificant between coastal and inland sites. The land use characteristics surrounding the monitoring sites had profound effects on the atmospheric nitrogen concentration and dry deposition flux. The ambient nitrogen concentration over the four urban sites was averaged 38.9% higher than that over the rural sites, resulting a 58.0% higher dry deposition flux in these sites compared to their rural counterparts. The local industrial activities and traffic emissions of nitrogen at urban areas had significant effects on the spatial distribution of atmospheric nitrogen concentration and dry deposition flux in the State. Wet and total deposition fluxes appeared to be invariant between the monitoring sites, except for high flux densities measured at Old Greenwich, a monitoring station near to and downwind of the New York and New Jersey industrial complexes.  相似文献   

4.
INTENTION, GOAL, SCOPE, BACKGROUND: The halogen bromine is far less abundant than chlorine, but it can be found at high concentrations in special materials like flame retarded plastics. The fate and effects of Br in waste incineration are not well understood. It may have similar implications like Cl for the volatilisation of heavy metals and the formation of low volatile organic compounds. Due to its lower oxidation potential, there is a risk of formation of elementary Br2 in the offgas. OBJECTIVE: Co-combustion tests of different types of Br containing plastic waste materials (up to 22%) and MSW in the TAMARA pilot plant for waste incineration were conducted to investigate the Br partitioning and the influence of Br on metal volatilisation. METHODS: The Br inventory of the fuel mix was elevated to approx. 1 wt-%. All input and output mass flows of the furnace have been sampled and the partitioning of Cl, Br, S, and a number of heavy metals, has been calculated on the basis of closed mass balances. RESULTS AND DISCUSSION: Organically-bound Br was typically released to more than 90% into the raw gas. Elementary Br2 was detected at high Br levels. Its presence was always analysed when all SO2 in the raw gas was oxidised to SO3. Br enhances the volatilisation of metals like K, Zn, Cd, Sn, Sb, and Pb out of the fuel bed principally in the same way as Cl. The tests gave strong indication that the promoting influence of the halogens on metal volatilisation is more pronounced than that of the fuel bed temperature. The volatilised metals are condensated on the fly ashes and are discharged along with the filter ashes. CONCLUSIONS: As long as a surplus of SO2 is present in the raw gas no Br2 is formed. Although the halogen induced transfer out of the fuel bed causes high concentrations of volatile metals in the filter ashes, a recovery is not economically feasible for the time being. The volatilisation gives no rise to metal emission problems as long as efficient dedusting is achieved. RECOMMENDATION AND OUTLOOK: If there is a risk of Br2 formation, in wet scrubbing a reducing agent has to be added to the neutral scrubber for efficient abatement. Filter ashes should be disposed of in a way that enables access for recovery in the future. The exact volatilisation characteristics of the various metals have to be studied in future using specifically tailored experiments.  相似文献   

5.
The temporal trends of major, minor and trace elements in the total atmospheric particulate sampled in the urban area of Turin (Italy) were determined for the following years: 1976, 1986, 1996 and 2001. The wavelength dispersive X-ray fluorescence (WD-XRF) technique was adopted to determine the concentrations of Ba, Br, Ca, Cl, Cr, Cu, Fe, K, Mg, Mn, Ni, Pb, S, Ti and Zn. A smaller number of samples was also analysed by ICP atomic emission spectroscopy (ICP-AES) and the results were compared with those obtained by WD-XRF to confirm their validity. A clear seasonal pattern with higher concentrations of the aforementioned elements in the cold periods was observed. Moreover, a change in the chemical composition of atmospheric particulate matter was evidenced, particularly between the first (1976 and 1986) and the last (1996 and 2001) years. This change can be attributed both to the greater contribution of Pb and Br to atmospheric pollution in the past and, in recent years, to the higher level of pollutants associated with increased vehicular traffic and industrial activities. The application of chemometric techniques (Principal Component Analysis and Cluster Analysis) allowed us to speculate about the main emitting sources influencing the total atmospheric particulate in these years.  相似文献   

6.
Median atmospheric concentrations of Pb, Br, S, As, Se, and particulate matter (PM) decreased, and median concentrations of Sb, Cu, Zn, Fe, Ca, Cr and Ba increased in urban aerosol in downtown Budapest between 1996 and 2002. The changes in Pb and Br concentrations were unambiguously attributed to the phasing out of leaded gasoline. The increments were mainly related to and explained by non-exhaust vehicular emissions. The mechanical wear of asbestos-free brake linings of road vehicles contributed to the concentration of Cu and Sb on average by 69% and 66%, respectively in the PM10 size fraction. Tire rubber abrasion was a major source for atmospheric Zn; on average, non-crustal sources accounted for 67% of Zn in the PM10 size fraction. Contribution of the tire wear component to the PM10 mass was estimated to be 6% at most, while its contribution to organic aerosol was of the order of 15%.  相似文献   

7.
The goal of the regional haze mitigation program in the United States is to attain "natural conditions" in national parks and wilderness areas by 2064. Results of research investigations on background concentrations of sea salt and biogenic organic matter, of episodic Saharan and Asian dust, and of carbon from natural fires were reviewed to provide a basis for making site-specific estimates of what the concentrations of atmospheric fine particulate matter components might be under natural conditions in the Southeastern United States. Based on this review, rough estimates were made of potential contributions of these aerosol components to natural background visibility. Natural organic particles were the dominant influence on the rate of visibility improvement required to reach natural conditions at an inland, mountainous location, and organic particles and sea salt were the dominant influences on the rate at a coastal location. African dust also had a large episodic effect, but the current regulatory approach is not designed to address episodic background variations. Insufficient data exist to quantify the contributions of wildfires with any detail, although global air pollution modeling provides insight, and their emissions can be locally dominant. Conservative regional refinements to the default natural background estimates do not greatly alter the region-wide rates of reduction of ambient particulate matter concentrations that will be needed to accomplish the first phase of the regional haze program. However, refinements at specific Class I areas may have considerable influence on defining the nature (magnitude and spatial and temporal distribution) of local emission reduction efforts there.  相似文献   

8.
Concentrations of Pb in livers of willow grouse (Lagopus lagopus), black grouse (Tetrao tetrix), and hare (Lepus timidus) were determined in samples collected during the period 1990-92 from 77 locations distributed across Norway. Our objective was to elucidate the impact of long-range atmospheric transport on the Pb exposure of the animals. The moss Hylocomium splendens was measured for atmospheric Pb deposition and Pb in soil at 60-cm depth was determined to reflect the natural geochemical background at the study locations. Strong positive relationships were found between Pb in liver and atmospheric deposition of Pb for all species and age groups studied. Results indicate that long-range atmospheric transport was the main source of Pb in the animals studied. This conclusion was supported by Pb analysis of typical food plants for the animals. Correlation between Pb in liver and Pb in soil mineral matter was observed only when considering sites with very low impact of atmospheric deposition. Even though the observed liver Pb concentrations may seem low (< or =12 microg g(-1) dw) they approach levels where sub-lethal effects cannot be ignored.  相似文献   

9.
Rapid urbanization and industrialization in South China has placed great strain on the environment and on human health. In the present study, the total suspended particulate matter (TSP) in the urban and suburban areas of Hong Kong and Guangzhou, the two largest urban centres in South China, was sampled from December 2003 to January 2005. The samples were analysed for the concentrations of major elements (Al, Fe, Mg and Mn) and trace metals (Cd, Cr, Cu, Pb, V and Zn), and for Pb isotopic composition. Elevated concentrations of metals, especially Cd, Pb, V and Zn, were observed in the urban and suburban areas of Guangzhou, showing significant atmospheric trace element pollution. Distinct seasonal patterns were observed in the heavy metal concentrations of aerosols in Hong Kong, with higher metal concentrations during the winter monsoon period, and lower concentrations during summertime. The seasonal variations in the metal concentrations of the aerosols in Guangzhou were less distinct, suggesting the dominance of local sources of pollution around the city. The Pb isotopic composition in the aerosols of Hong Kong had higher 206Pb/207Pb and 208Pb/207Pb ratios in winter, showing the influence of Pb from the northern inland areas of China and the Pearl River Delta (PRD) region, and lower 206Pb/207Pb and 208Pb/207Pb ratios in summer, indicating the influence of Pb from the South Asian region and from marine sources. The back trajectory analysis showed that the enrichment of heavy metals in Hong Kong and Guangzhou was closely associated with the air mass from the north and northeast that originated from northern China, reflecting the long-range transport of heavy metal contaminants from the northern inland areas of China to the South China coast.  相似文献   

10.
The ongoing program Clean Air for Europe (CAFE) is an initiative from the EU Commission to establish a coordinated effort to reach better air quality in the EU. The focus is on particulate matter as it has been shown to have large impact on human health. CAFE requested that WHO make a review of the latest findings on air pollutants and health to facilitate assessments of the different air pollutants and their health effects. The WHO review project on health aspects of air pollution in Europe confirmed that exposure to particulate matter (PM), despite the lower levels we face today, still poses a significant risk to human health. Using the recommended uniform risk coefficients for health impact assessment of PM, regardless of sources, premature mortality related to long-range transported anthropogenic particles has been estimated to be about 3500 deaths per year for the Swedish population, corresponding to a reduction in life expectancy of up to about seven months. The influence of local sources is more difficult to estimate due to large uncertainties when linking available risk coefficients to exposure data, but the estimates indicate about 1800 deaths brought forward each year with a life expectancy reduction of about 2-3 months. However, some sectors of the population are exposed to quite high locally induced concentrations and are likely to suffer excessive reductions in life expectancy. Since the literature increasingly supports assumptions that combustion related particles are associated with higher relative risks, further studies may shift the focus for abatement strategies. CAFE sets out to establish a general cost effective abatement strategy for atmospheric particles. Our results, based on studies of background exposure, show that long-range transported sulfate rich particles dominate the health effects of PM in Sweden. The same results would be found for the whole of Scandinavia and many countries influenced by transboundary air pollution. However, several health studies, including epidemiological studies with a finer spatial resolution, indicate that engine exhaust particles are more damaging to health than other particles. These contradictory findings must be understood and source specific risk estimates have to be established by expert bodies, otherwise it will not be possible to find the most cost effective abatement strategy for Europe. We are not happy with today's situation where every strategy to reduce PM concentrations is estimated to have the same impact per unit change in the mass concentration. Obviously there is a striking need to introduce more specific exposure variables and a higher geographical resolution in epidemiology as well as in health impact assessments.  相似文献   

11.
The occurrence of selected nitro-polycyclic aromatic hydrocarbons (nitro-PAHs) associated with atmospheric particulate matter has been investigated at an urban site and at a semi-rural site. For this purpose an analysis method based on gas chromatography and tandem ion trap mass spectrometry has been developed and applied. The nitro-PAH levels have been compared with levels of other air pollutants including unsubstituted PAHs, inorganic gases and particulate matter, as well as with meteorological parameters. Correlations and concentration ratios suggest that the dominant source of 9-nitroanthracene at the urban site is direct emissions, whereas at the semirural site its dominant source is atmospheric formation. The atmospheric formation of 2-nitrofluoranthene and 2-nitropyrene generally seems to be initiated by OH radicals during the day rather than by NO3 radicals at night. The average contribution of the OH initiated formation is estimated to be in the range of 90–100%. However, under wintertime conditions with cloudy weather implying low OH radical production, NO3 radicals may also be important as initiators of nitro-PAH formation. Samples influenced by transport of polluted air masses from the European continent have significantly elevated concentrations of atmospherically formed nitro-PAHs. The directly emitted nitro-PAHs, 1-nitropyrene and 3-nitrofluoranthene, do not exhibit elevated levels during such long-range transport episodes.  相似文献   

12.
Aerosol samples collected in three characteristic Chilean cities-including urban and remote zones-have been analyzed by the PIXE spectroscopic technique. Elemental composition, total suspended particulate matter (TSP), particle size distribution, and the peculiar geographic and meteorological parameters have been included in this study. Santiago--the polluted capital of Chile--registered high TSP indexes and important amounts of hazardous elements in air such as S, V, Cr, Zn, Br and Pb. The atmosphere of Antofagasta city showed marine and mineral activity influence. Results from Chillán city are similar to those from rural environments. Protons and deuterons-provided by the isochronous cyclotron of the University of Chile-were used to excite X-ray radiation from the sample. Signals were processed by an energy dispersive detection system, including a cryogenic Si(Li) detector, electronic for pulse amplification and an analog to digital converter. The absolute elemental concentration of the particulate matter in air was obtained through a fundamental parameter equation. Samples consist of particulate material collected directly on Nuclepore filters or deposited over Kapton foils. Typical elements analyzed were Mg, Al, Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Cu, Zn, As, Br and Pb.  相似文献   

13.
The objective of this study was to describe the ambient levels of particulate matter (PM) and its influence to air quality situation on the dry Mediterranean island of Cyprus. From October 2002 to August 2003 PM10 and PM2.5 samples were collected at 31 different sampling sites in Cyprus. In addition, continuous measurements of PM10 were carried out from 2003 to 2007 at a traffic and a rural site. It can be recognised that at all traffic and at some residential and urban background sites, the actual EU limit values have been exceeded. Special events e.g. long-range transport of Sahara dust storms were recorded over urban as well as rural areas in the order of 6–8 events per year, with a major frequency in summer and spring periods. The comparison of the PM10 concentrations in Cyprus cities with values of other European cities demonstrates the PM10 problem in Cyprus, especially in the dry summer season, when no rain is cleaning the air and the dry surfaces. This underlines the necessity of PM abatement strategies.  相似文献   

14.
There is still a long-term debate concerning the relative contributions of naturally emitted and anthropogenic Se at the regional and local scales. Here, Se and heavy metal concentrations are reported for epiphytic lichens collected in coastal and inland areas from the USA, Canada and France for assessing atmospheric Se source. Correlations found between Se and Cl in lichens confirmed the major marine biogenic source for atmospheric Se. Continental samples do not show systematic relationships between Se and other metal (Pb, Cu, In …) contents, even for lichens collected in the vicinity of smelters or close to urban areas. Our results suggest that, although anthropogenic Se may be present, the marine biogenic Se source is a major contributor to atmospheric Se for our sampling locations. The contribution of naturally emitted atmospheric Se may be significant in urban and industrial areas and should be taken into account for further studies.  相似文献   

15.
The oceans are a major source for particles that play an important role in many atmospheric processes. In Europe sea salt may contribute significantly to particulate matter concentrations. We have compiled sodium concentration data as a tracer for sea salt for 89 sites in Europe to provide more insight in the distribution of sea salt across Europe. The annual average sea salt concentrations above land were estimated to range between 0.3 and almost 13 μg m?3. Maximum concentrations are found at the Irish coast. At coastal sites along the Atlantic and North Sea coast concentrations tend to be around 5 μg m?3. More inland locations up to about 300 km away from the coast tend to show concentrations between 2 and 5 μg m?3, whereas sites further away from the coast are characterized by lower concentrations. An analysis of the representativity of the data with respect to a long term average showed that the long average is associated with a standard deviation of around 15%. The compilation of observations provides an improved overview of sea salt concentrations in Europe as well as an improved basis for model validation. Verification of the results of the LOTOS-EUROS model learned that the model represents well the spatial variability of the observed sea salt concentrations very well. However, the absolute concentrations are significantly overestimated due to large uncertainties in the emission and dry deposition parameterizations. Using the high explained variability in the gradients across Europe, the bias-corrected modelled distribution serves as a best estimate of the sea salt distribution across Europe for 2005.  相似文献   

16.
The chemistry of high mountain snowpacks is a result of the long-range atmospheric transport and deposition of elements. Pyrenean snowpacks contain information about the fluxes of elements over SW Europe in winter. Here we analysed Al, Ti, Mn, Fe, Ni, Cu, Zn, As, Se, Cd and Pb in the 2004–05 winter snowpack in the Central Pyrenees, at an altitude range of 1820–3200 m a.s.l. Ni, As, Se and Cd were not detected in most cases. The concentrations of the remaining elements were comparable to those found in other high mountain areas in Europe and North America considered representative of regional background of atmospheric deposition in populated areas. In contrast, our measurements were higher than those of polar areas, which represent the global background. Single measurements of concentrations and snow accumulation were subject to considerable spatial variability, which may be attributable to strong wind drift and other post-depositional processes. The major ions chemistry of the snow indicated three possible origins for the solutes: terrigenous dust, sea salt spray and polluting S and N aerosols. We found no association between Cu, Zn and Pb and any of these possible sources. This observation therefore indicates that these elements were not preferentially bound to any particular kind of aerosol. Snow collected at altitudes of up to 2050 m a.s.l. presented higher concentrations of several elements than snow above this altitude, thereby indicating a local influence. Snow collected above 2300 m a.s.l. was therefore more representative of broad regional inputs. At these higher altitudes, snow was not enriched in Al, Ti, Mn, Fe or As compared with the composition of the upper continental crust and the local lithology, and these elements (except Mn) appeared almost exclusively in the particulate fraction. This observation indicates that Al, Ti, Mn, Fe and As were present mainly as part of dust particles of terrigenous origin. In contrast, Cu, Zn, and Pb presented medium to high enrichment factors and showed a higher proportion of soluble forms, thereby indicating their polluting character.  相似文献   

17.
The results of trace element content analysed in Sphagnum capillifolium and Pseudevernia furfuracea exposed in bags in 1999 are reconsidered to evaluate the reliability of moss and lichen transplants to detect urban trace element atmospheric pollution, using Naples as a case example. After 4 months' exposure, trace element concentrations were at least twice as high as the pre-exposure values and in general higher in Sphagnum than in Pseudevernia. Moss samples were enriched in the following order: As=Cu>Mo>Pb>V>Co>Cr>Zn; lichen samples in the order: Mo>Cu>As=Co=Ni>V>Pb. Based on the calculation of a cumulative load factor, all sites located along the coast had higher trace element loads compared to sites in the hilly inland area. Complementary SEM, TEM and EDS observations showed, despite significant damage to tissue and cell integrity, the recurrent presence of particulate matter in moss and lichen, indicating the considerable presence of dust in the urban atmosphere which, according to chemical composition, may be due both to anthropogenic and natural sources such as volcanic rock and soil and sea salts.  相似文献   

18.
A trajectory statistics method has been used to examine the causes of variability and seasonality of sulphur dioxide, particulate sulphate and non-sea-salt sulphate in precipitation measured at a French rural site. This methodology has permitted to define the likely contributing sources for two seasons, a warm and a cold, that show different patterns. The general results suggest the impact of the long-range transport of SO2 and SO2 secondary species from high anthropogenic sources. The increase of photochemical activity during the warm period, the seasonal large-scale wind movements responsible for precipitation and the removal processes during atmospheric transport may also significantly influence sulphur concentrations at Morvan.  相似文献   

19.
Moon HB  Kannan K  Lee SJ  Choi M 《Chemosphere》2007,66(4):585-593
Atmospheric bulk samples were collected monthly, for one year, from urban, suburban, and rural sites located in the coastal areas of Korea, for the assessment of depositional fluxes and seasonal variations in atmospheric concentrations of PBDEs. Twenty individual PBDE congeners were found in atmospheric samples, and their depositional fluxes varied from 10.1 to 89.0 microg/m2/year. The highest depositional fluxes were found in two urbanized areas, with a strong urban-rural gradient. The relationship between PBDE and particulate depositional fluxes showed significant correlation for all locations, which suggested the association of PBDEs to particulate phase. Deca-BDE (BDE 209) was the predominant congener (>93%) in all deposition samples, which is consistent with a high consumption of deca-BDE for the flame-retardant market in Korea. Seasonal variability was observed in PBDE concentrations for the two urban sites, whereas no seasonal trend was found for either the suburban or the rural location.  相似文献   

20.
In June 1996–June 1997 Berner impactors were used in the Helsinki area to measure size distributions of atmospheric aerosols simultaneously at an urban and at a rural site. Ten sample pairs were collected in the size range of 0.03–15.7 μm of equivalent aerodynamic diameter (EAD). Average size distributions at the two sites were calculated for 29 elements, particulate mass, and sulphate. At both sites especially sulphate, As, B, Bi, Cd, Ni, Tl, and V were enriched in fine particles (EAD<2.3 μm). In order to estimate local fine-particle sources of the various chemical components, the similarities and dissimilarities in the accumulation-mode parameters were studied separately for both sites. It was observed that often in different samples, different components had similar accumulation modes. At both sites, particulate mass, As, and Pb had similar accumulation modes to sulphate which suggests that long-range transport (LRT) is important for these components. V, Ni, Mo, and Co formed another group of similar accumulation modes at both sites suggesting that these elements largely originated from local and regional oil combustion. In addition, other groups of similar accumulation modes were observed but these groups were different between the sites. The meteorological parameters indicated that seven sample pairs formed a subset of the data in which the local emissions of the Helsinki area were transported to the urban site but not to the rural site. For this subset the rural fine-particle concentrations were considered to represent an upper limit estimate for the LRT. These upper limit LRT estimations were further improved by utilising the quantitative relative size distributions (QRSD) method at the rural site. The QRSD method supposes that in the fine-particle size range the LRT fractions of all chemical components have a similar shape in their size distributions. Fine-particle sulphate is typically long-range transported, and was therefore selected as the model component that represents the shape of LRT material. Sulphate size distribution was then scaled to give an estimation of the LRT contribution of each component at the rural site. These rural “sulphate scaled” LRT estimates were subtracted from the corresponding urban concentrations to give the local contributions (ng/m3) downwind of the Helsinki area. In particles with EAD below 2.3 μm, the highest absolute and relative downwind local contributions were observed for several common sea-salt and road-dust components. Also the combustion-related elements Ni and V showed fairly high downwind local contributions. Because of the limited number of samples, the local and LRT contributions were not estimated for different wind directions.  相似文献   

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