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1.
Continuous data of the concentration measurements of respirable suspended particulates (PM10, particles with aerodynamic diameter smaller than or equal to 10 pm) were analyzed. These measurements were carried out at an urban and nearby industrial location in northern Greece for the 5-year period 1996-2000. The time series concentration trend was examined, the seasonal and diurnal variations were identified, and the lognormality of the daily mean concentration data sets was tested. Over the 5-year data-gathering period, the days on which the U.S. Environmental Protection Agency (EPA) 24-hr PM10 standard was exceeded (episode days) were identified and their relation to prevailing synoptic-scale meteorological conditions was studied. The analysis led to useful information concerning the air quality levels, the contribution of the main pollution sources in this area, as well as some of the mechanisms that influence the PM10 concentrations. It also was proved that the measured PM10 concentrations are a result of a combination of processes including local anthropogenic sources, mesoscale transport, and resuspension. A complex system of sources and meteorological conditions modulate the heavy particulate pollution in the area of interest.  相似文献   

2.
3.
A historic antimony smelter site at Endeavour Inlet, New Zealand has smelter residues with up to 17 wt.% antimony. Residues include coarse tailings (cm scale particles, poorly sorted), sand tailings (well sorted) and smelter slag (blocks up to 30 cm across). All of this material has oxidised to some degree over the ca. 100 years since the site was abandoned. Oxidation has resulted in acidification of the residues down to pH 2-5. Smelter slag contains pyrrhotite (FeS) and metallic antimony, and oxidation is restricted to surfaces only. The coarse tailings are the most oxidised, and few sulfide grains persist. Unoxidised sand tailings contain 10-20 vol.% stibnite (Sb2S3) containing up to 5% As, with subordinate arsenopyrite (FeAsS), and minor pyrite (FeS2). The sand tailings are variably oxidised on a scale of 2-10 cm, but original depositional layering is preserved during oxidation and formation of senarmontite (Sb2O3). Oxidation of sand tailings has resulted in localised mobility of both Sb and As on the cm scale, resulting in redistribution of these metalloids with iron oxyhydroxide around sand grain boundaries. Experiments demonstrate that Sb mobility decreases with time on a scale of days. Attenuation of both As and Sb occurs due to adsorption on to iron oxyhydroxides which are formed during oxidation of the smelter residues. There is no detectable loss of Sb or As from the smelter site into the adjacent river, <50 m away, which has elevated Sb (ca. 20 microg/l) and As (ca. 7 microg/l) from mineralised rocks upstream. Despite the high concentrations of Sb and As in the smelter residues, these metalloids are not being released into the environment.  相似文献   

4.
To evaluate the spatial variability of ozone concentrations, two studies were undertaken in the montane environment of Trentino region, northern Italy, in 2007. In the first study, a 225 km2 area was considered. Here, a randomized design was used to evaluate the variability of ozone concentration at 1 and 225 km2 scale. Measurements were carried out by passive samplers between May and June 2007. In a second study, the whole 6207 km2 area of Trentino was considered. The area is covered by five grid cells of the European Monitoring and Evaluation Programme (EMEP). A systematic 15 × 15 km grid was used to allocate 15 passive samplers over the entire province, resulting into 1–4 samplers for each of the 5 EMEP grid cells (2500 km2 each) overlapping the study area. Measurements were carried out between June and September 2007. Accuracy of passive samplers was checked by direct comparison with conventional ozone analysers. Significant differences (P = 0.034) were found in ozone concentration among 1 × 1 km quadrates within the 225 km2 study area, while variability within the 1 × 1 km grid cells (coefficient of variation, CV′ = 0.12) slightly exceed the measurement error (CV′ = 0.08). At larger scales (225, 2500 and 6207 km2), ozone concentration shows much higher variability (CV′ from 0.18 to 0.28, with peak values at 0.40). Reported differences lead to very different AOT40 estimates even within the same EMEP grid cell. These findings suggest that 1 × 1 km resolution seems appropriate for ozone concentration modelling. On the other hand, significant sub-grid variation may exist at the resolution adopted by the EMEP model. Coupled with the likely variability of other important meteorological, soil and vegetation variables, our findings suggest that ozone risk assessment for vegetation based on large-scale modelled AOT40 and flux needs to be considered with great caution. The evidence reported in this paper asks for more detailed national-scale modelling, and the development of methods to incorporate local scale variations into large-scale models.  相似文献   

5.
During the June 1996 eruption of Mt Ruapehu, New Zealand, traces of fine particulate volcanic ash were observed in or near the cities of Hamilton and Auckland, 166–282 km from the volcano. Although no health impacts in these cities were attributed to the eruption, hospital records at both cities for the following month show the highest rates of respiratory mortality for the 1990s. Alternative explanations for this increase in respiratory mortality were investigated, including urban air pollution, adverse weather conditions and influenza. Comparable records from Wellington city, assumed to be outside the zone of ash dispersal, were used as a ‘control’. Our results suggest that at Hamilton, where non-volcanic factors can largely be eliminated as making a significant contribution, diffuse volcanic ashfall may have been an important factor in respiratory mortality during the weeks following the eruption. At Auckland, further away from the volcano but with a much larger population than Hamilton, a case for a weaker volcanic contribution can be made, but is more equivocal because of coincidentally high urban air pollution and cold, stable weather.These findings support the concept that diffuse fine volcanic ash poses a risk to respiratory health at greater distances from an eruption than is currently perceived. This is because the finest ‘respirable’ fraction of erupted material with potentially hazardous physico-chemical properties is likely to be ejected highest into the atmosphere and dispersed the greatest distance. If significant amounts reach large cities, then large numbers of individuals may be at risk, especially those already suffering poor respiratory health. This work has important implications for environmental health and hazard management in New Zealand and in other regions that may be susceptible to a similar volcanic threat.  相似文献   

6.
This paper examines the inter-suburb dispersion of particulate air pollution in Christchurch, New Zealand, during a wintertime particulate pollution episode. The dispersion is simulated using the RAMS/CALMET/CALPUFF modelling system, with data from a detailed emissions inventory of home heating, motor vehicles and industry. During the period 27 July–1 August 1995, peak 1 h and 24 h PM10 concentrations of 368 and 107 μg m−3, respectively, were observed. Peak concentrations occurred at night, when particulate emissions from wood- and coal-burning domestic heating appliances were at a maximum and emitted into a stable boundary layer. The model is generally able to reproduce the observed PM10 time series recorded at surface monitors located throughout the urban area. For this simulation, the fractional gross error ranges between 0.69 and 0.99, and the fractional bias ranges between −0.17 and 0.30. Strong horizontal concentration gradients of 100 μg m−3 km−1, both in the observational record and model predictions, are apparent. Three emission reduction options, designed to reduce the severity of particulate pollution episodes in Christchurch, are simulated. When both domestic open-hearth fires and all coal burning are removed, the 24 h average peak concentration is reduced by 55%. The number of guideline exceedences of PM10 in the modelled period is reduced from five to one. Removing open-hearth fires results in 42% reduction in PM10 concentration, resulting in three exceedences of the guideline, and removing coal-burning fires yields a 32% reduction in PM10, resulting in four exceedences of the guideline.  相似文献   

7.
A numerical model, Mesoscale Model version 5 (MM5), is used in conjunction with a three-dimensional Eulerian/Lagrangian dispersion model (CAMx4) to model PM10 dispersion for a period of 48 h for the city of Christchurch, New Zealand. In a typical winter, Christchurch usually experiences severe degradation in air quality. The formation of a nocturnal temperature inversion layer during stagnant synoptic conditions, and the emissions of particulate matter (PM10) mainly from solid fuel home heating appliances (the ‘Domestic’ factor) leads to severe smog episodes on about 30 nights each winter. The modelling results from the highest resolution computational grid are compared with observed meteorology and air pollution dispersion for winter 2000, when the Christchurch Air Pollution Study (CAPS2000) was underway. The numerical modelling system is able to simulate surface-layer meteorology and PM10 spatial distribution with a good level of skill, with the Index of Agreement and Pearson's correlation coefficient greater than 0.8 for PM10.  相似文献   

8.
Several collocated semicontinuous instruments measuring particulate matter with particle sizes < or =2.5 microm (PM2.5) sulfate (SO4(2-)) and nitrate (NO3-) were intercompared during two intensive field campaigns as part of the PM2.5 Technology Assessment and Characterization Study. The summer 2001 urban campaign in Queens, NY, and the summer 2002 rural campaign in upstate New York (Whiteface Mountain) hosted an operation of an Aerosol Mass Spectrometer, Ambient Particulate Sulfate and Nitrate Monitors, a Continuous Ambient Sulfate Monitor, and a Particle-Into-Liquid Sampler with Ion Chromatographs (PILS-IC). These instruments provided near real-time particulate SO4(2-) and NO3- mass concentration data, allowing the study of particulate SO4(2-)/NO3- diurnal patterns and detection of short-term events. Typical particulate SO4(2-) concentrations were comparable at both sites (ranging from 0 to 20 microg/m3), while ambient urban particulate NO3- concentrations ranged from 0 to 11 microg/m3 and rural NO3- concentration was typically less than 1 microg/m3. Results of the intercomparisons of the semicontinuous measurements are presented, as are results of the comparisons between the semicontinuous and time-integrated filter-based measurements. The comparisons at both sites, in most cases, indicated similar performance characteristics. In addition, charge balance calculations, based on major soluble ionic components of atmospheric aerosol from the PILS-IC and the filter measurements, indicated slightly acidic aerosol at both locations.  相似文献   

9.
During 1993-1996 and 2001-2003, we evaluated the percentage of plants (incidence) exhibiting ozone-induced foliar symptoms on vegetation within a National Wildlife Refuge located along the Atlantic Ocean coast of New Jersey, USA. Incidence varied among plant species and years. Bioindicator plants most sensitive to ozone, across all years, included native common milkweed (Asclepias syriaca) and wild grape (Vitis spp.), as well as introduced tree-of-heaven (Ailanthus altissima). Less sensitive bioindicators included Virginia creeper (Parthenocissus quinquefolia) and winged sumac (Rhus coppolina). Black cherry (Prunus serotina) and sassafras (Sassafras albidum) were least sensitive. The greatest incidence of ozone symptoms, across all plant species, occurred in 1996, followed by 2001>1995>1994>1993>2003>2002. A model was developed that showed a statistically significant relationship between incidence of ozone symptoms and the following parameters: plant species, Palmer Drought Severity Index, and the interaction of W126 x N100 measures of ambient ozone.  相似文献   

10.
Hourly measurements of baseline ozone at the Mace Head Atmospheric Research Station on the Atlantic Ocean coast of Ireland are observed when unpolluted air masses are advected to the station from across the North Atlantic Ocean. Monthly mean ozone mixing ratios in baseline air masses have risen steadily during the 1980s and 1990s reaching unprecedented levels during the early months of 1999. During the 2000s, baseline ozone mixing ratios have shown evidence of decline and stabilisation. Over the entire 20-year 1987–2007 period, the trend in annual baseline ozone has been +0.31±0.12(2−σ) ppb year−1 and is highly statistically significant. Trends have been highest in the spring months and lowest in the summer months, producing a significant increase in the amplitude of the seasonal cycle. Over the shorter 1995–2007 period, we demonstrate how the growth to peak in 1999 and the subsequent decline have been driven by boreal biomass burning events during 1998/1999 and 2002/2003. The 2000s have been characterised by relatively constant baseline ozone and CH4 levels and these may be a reasonable guide to future prospects, at least in the short term.  相似文献   

11.
Twenty-four to forty-eight-hour ozone air quality forecasts are increasingly being used in metropolitan areas to inform the public about potentially harmful air quality conditions. The forecasts are also behind "ozone action day" programs in which the public and private sectors are encouraged or mandated to alter activities that contribute to the formation of ground-level ozone. Presented here is a low-cost application of the Urban Airshed Model (UAM), an Eulerian 3-dimensional photochemical-transport grid model for generating next-day peak ozone concentration forecasts. During the summer of 1997, next-day peak ozone concentrations in Atlanta, GA, were predicted both by a team of eight forecasters and by the Urban Airshed Model in Forecast Mode (UAM-FM). Results are presented that compare the accuracy of the team and the UAM-FM. The results for the summer of 1997 indicate that the UAM-FM may be a better predictor of peak ozone concentrations when concentrations are high (> 0.095 ppmv), and the team may be a better predictor of ozone concentrations when concentrations are low (< or = 0.095 ppmv). The UAM-FM is also discussed in the context of other forecasting tools, primarily linear regression models and a no-skill, persistence-based technique.  相似文献   

12.
The growth of 1-year-old aspen was simulated using TREGRO, a computer simulation model of individual tree growth, to assess potential effects of ozone (O3). TREGRO was parameterized using information from a field experiment conducted at Ithaca, NY, USA; the model was then applied using environmental information from Suwon, Korea, where O3 exposures of aspen had not been conducted. In the parameterization at Ithaca, the simulated and measured total biomass differed by about 3% and the differences between measured and simulated biomass gain of leaf, shoot, and root were 15.4, 8.3, and 4.4%, respectively. Simulating growth at Suwon required adjustment in growth rates to match measured growth due to the different weather conditions at the two cities. The assimilated carbon was evenly distributed to each tissue (foliage, branch, stem, coarse, fine roots) in Suwon, whereas it was mainly allocated to vigorous stem growth in Ithaca. The vigorous growth under Suwon conditions resulted in less total non-structural carbon and perhaps trees more vulnerable to O3 stress. Although the ambient O3 in Suwon (1.2 ppm.h of sum of the hourly concentrations greater than 0.06 ppm [SUM06]) was lower than that in Ithaca (2.1 ppm.h of SUM06), a reduction of 8% of total assimilated carbon was found compared to simulation without O3. Severe effects on root growth at elevated O3 (1.7 times ambient) were predicted; however, the effects on leaf growth would not be as severe.  相似文献   

13.
Continuous specific measurements of sulphur dioxide, nitric oxide, nitrogen dioxide and ozone have been made for over 2y at Bottesford, a rural site in central England, 20 km away from town and industry sources and 1 km from traffic sources. Statistics of hourly, daily, monthly, seasonal and yearly values are given.On an annual basis, there was 50% more oxides of nitrogen (nitric oxide plus nitrogen dioxide) than sulphur dioxide, and more ozone than either. The nitric oxide and nitrogen dioxide were approximately equal. No other published annual values of nitric oxide, nitrogen dioxide and ozone at U.K. rural sites are known. The summer nitric oxide values were greater at this site than at three other rural sites in the British Isles for which summer nitric oxide values have been reported, but so was the sulphur dioxide, and the amounts of both these gases probably reflect the size and distance of combustion sources.Diurnal variations of the four gases during summer months at Bottesford were similar to those published for a site in southern England. The diurnal variations for winter months at Bottesford were somewhat different, especially for nitrogen dioxide. No other published winter patterns are known.Usually nitrogen dioxide and ozone concentrations were in opposition, both short and long term, but on rare occasions, for example in relatively clean winter air, the ozone concentration rose and fell directly with the nitrogen dioxide. Hourly ozone values exceeded 50 ppb (10−9, by volume) for several hours a month in 22 months out of 24. The World Health Organisation guideline for public health exposure limits is given as 50–100 ppb h−1, not to be exceeded more than once per month.  相似文献   

14.
In order to improve our knowledge of the surface ozone in the south of the Iberian Peninsula, annual, monthly, weekly and daily ozone concentrations have been closely monitored in the Seville metropolitan area highlighting those episodes that exceed the European Ozone Directive. A three-year period (2003-2005) and eight ozone stations were used; five of them located in the city's busiest areas and the rest in adjacent zones ( approximately 25km). In addition, the wind regime was also studied in order to understand the main characteristics of the surface atmospheric dynamics. The lowest ozone concentrations 17-33microgm(-3) took place in January while the highest 57-95microgm(-3) occurred in June. The ozone concentration week-weekend differences from May to September indicate that this phenomenon does not affect the ozone stations analysed. Daily cycles show minimum values between 7:00 and 8:00 UTC and maximum at noon, exceeding 90microgm(-3) during summer months. From March to October the ozone concentrations were above the target value for the protection of human health, especially during the summer months, with values up to 30% over the limit. The information threshold has been exceeded at all ozone stations studied but with greater frequency in the stations far from the city centre. In addition, at these latter stations the alert threshold was also exceeded on six occasions. This study in the city of Seville indicates that the high ozone levels are due to local atmospheric effects, mainly since the ozone air masses may undergo recirculation processes. The ozone is transported to the city from the S-SW, having a major impact in the NE areas.  相似文献   

15.
We investigated variations in the relative sensitivity of surface ozone formation in summer to precursor species concentrations of volatile organic compounds (VOCs) and nitrogen oxides (NOx) as inferred from the ratio of the tropospheric columns of formaldehyde to nitrogen dioxide (the “Ratio”) from the Aura Ozone Monitoring Instrument (OMI). Our modeling study suggests that ozone formation decreases with reductions in VOCs at Ratios <1 and NOx at Ratios >2; both NOx and VOC reductions may decrease ozone formation for Ratios between 1 and 2. Using this criteria, the OMI data indicate that ozone formation became: 1. more sensitive to NOx over most of the United States from 2005 to 2007 because of the substantial decrease in NOx emissions, primarily from stationary sources, and the concomitant decrease in the tropospheric column of NO2, and 2. more sensitive to NOx with increasing temperature, in part because emissions of highly reactive, biogenic isoprene increase with temperature, thus increasing the total VOC reactivity. In cities with relatively low isoprene emissions (e.g., Chicago), the data clearly indicate that ozone formation became more sensitive to NOx from 2005 to 2007. In cities with relatively high isoprene emissions (e.g., Atlanta), we found that the increase in the Ratio due to decreasing NOx emissions was not obvious as this signal was convolved with variations in the Ratio associated with the temperature dependence of isoprene emissions and, consequently, the formaldehyde concentration.  相似文献   

16.
The authors analyze the sensitivities of source regions in East Asia to PM2.5 (particulate matter with an aerodynamic diameter of ≤2.5 µm) concentration at Fukue Island located in the western part of Japan by using a regional chemical transport model with emission sensitivity simulations for the year 2010. The temporal variations in PM2.5 concentration are generally reproduced, but the absolute concentration is underestimated by the model. Chemical composition of PM2.5 in the model is compared with filter sampling data in spring; simulated sulfate, ammonium, and elemental carbon are consistent with observations, but mass concentration of particulate organic matters is underestimated. The relative contribution from each source region shows the seasonal variation, especially in summer. The contribution from central north China (105°E–124°E, 34°N–42°N) accounts for 50–60% of PM2.5 at Fukue Island except in summer; it significantly decreases in summer (18%). Central south China (105°E–123°E, 26°N–34°N) has the relative contribution of 15–30%. The contribution from the Korean Peninsula is estimated at about 10% except in summer. The domestic contribution accounts for about 7% in spring and autumn and increases to 19% in summer. We also estimate the relative contribution to daily average concentration in high PM2.5 days (>35 μg m?3). Central north China has a significant contribution of 60–70% except in summer. The relative contribution from central south China is estimated at 46% in summer and about 30% in the other seasons. The contributions from central north and south China on high PM2.5 days are generally larger than those of their seasonal mean contributions. The domestic contribution is smaller than the seasonal mean value in every season; it is less than 10% even in summer. These model results suggest that foreign anthropogenic sources have a substantial impact on attainment of the atmospheric environmental standard of Japan at Fukue Island.
Implications: The contribution from several source regions in East Asia to PM2.5 concentration at Fukue Island, a remote island located in the western part of Japan and close to the Asian continent, is estimated using a three-dimensional chemical transport model. The model results suggest that PM2.5 that is attributed to foreign anthropogenic sources have a larger contribution than that of domestic pollution and have a substantial impact on attainment of the atmospheric environmental standard of Japan at Fukue Island.  相似文献   

17.
The chemical product diaryl-p-phenylene diamine (DAPD), produced by The Goodyear Tire & Rubber Company as POLYSTAY 100® (CAS 68953-84-4), is employed as an antidegradant in polymers used in tires and industrial rubber products. Previous evaluations pertaining to the ecological fate of DAPD indicated a lack of biodegradative activity in aquatic media. In order to further pursue the biodegradation potential of DAPD, it was deemed necessary to enhance the sensitivity of the aquatic biodegradation assay through (a) employment of a radiotracer of the test substance, and (b) optimisation of conditions for achieving maximal solubilisation of test material in the aquatic media of the incubation vessels. Test vessels were prepared according to the OECD ready biodegradability test guidelines, with DAPD added on silica gel at concentrations of 10 or 100 μg L−1, together with a surfactant to aid solubilisation. After 63 d incubation up to 37% mineralisation was measured and up to 29% of the applied radioactivity was incorporated into cell biomass. Also, after 28 d no DAPD could be measured in solution by radio-TLC and HPLC–MS. These three results demonstrate that the antioxidant DAPD undergoes microbiologically mediated biodegradation and is highly unlikely to persist in the environment.  相似文献   

18.
Ozone uptake was studied in a pine forest in Tenerife, Canary Islands, an ecotone with strong seasonal changes in climate. Ambient ozone concentration showed a pronounced seasonal course with high concentrations during the dry and warm period and low concentrations during the wet and cold season. Ozone uptake by contrast showed no clear seasonal trend. This is because canopy conductance significantly decreased with soil water availability and vapour pressure deficit. Mean daily ozone uptake averaged 1.9 nmol m(-2) s(-1) during the wet and cold season, and 1.5 nmol m(-2) s(-1) during the warm and dry period. The corresponding daily mean ambient ozone concentrations were 42 and 51 nl l(-1), respectively. Thus we conclude that in Mediterranean type forest ecosystems the flux based approach is more capable for risk assessment than an external, concentration based approach.  相似文献   

19.
Micro-climatic and ambient ozone data were combined with measurements of sap flow through tree trunks in order to estimate whole-tree ozone uptake of adult Norway spruce (Picea abies), cembran pine (Pinus cembra), and European larch (Larix decidua) trees. Sap flow was monitored by means of the heat balance approach in two trees of each species during the growing season of 1998. In trees making up the stand canopy, the ozone uptake by evergreen foliages was significantly higher than by deciduous ones, when scaled to the ground area. However, if expressed per unit of whole-tree foliage area, ozone flux through the stomata into the needle mesophyll was 1.09, 1.18 and 1.40 nmol m(-2) s(-1) in Picea abies, Pinus cembra and Larix decidua, respectively. These fluxes are consistent with findings from measurements of needle gas exchange, published from the same species at the study site. It is concluded that the sap flow-based approach offers an inexpensive, spatially and temporally integrating way for estimating ozone uptake at the whole-tree and stand level, intrinsicly covering the effect of boundary layers on ozone flux.  相似文献   

20.
The Positive Matrix Factorization (PMF) receptor model and the Observation Based Model (OBM) were combined to analyze volatile organic compound (VOC) data collected at a suburban site (WQS) in the PRD region. The purposes are to estimate the VOC source apportionment and investigate the contributions of these sources and species of these sources to the O3 formation in PRD. Ten VOC sources were identified. We further applied the PMF-extracted concentrations of these 10 sources into the OBM and found "solvent usage 1", "diesel vehicular emissions" and "biomass/biofuel burning" contributed most to the O3 formation at WQS. Among these three sources, higher Relative Incremental Reactivity (RIR)-weighted values of ethene, toluene and m/p-xylene indicated that they were mainly responsible for local O3 formation in the region. Sensitivity analysis revealed that the sources of "diesel vehicular emissions", "biomass/biofuel burning" and "solvent usage 1" had low uncertainties whereas "gasoline evaporation" showed the highest uncertainty.  相似文献   

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