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1.

A total of 47 passive air samples and 25 soil samples were collected to study the temporal trend, distribution, and air–soil exchange of polychlorinated naphthalenes (PCNs) in Shanghai, China. Atmospheric PCNs ranged from 3.44 to 44.1 pg/m3 (average of 21.9 pg/m3) in summer and 13.6 to 153 pg/m3 (average of 40.0 pg/m3) in winter. In the soil samples, PCN concentrations were 54.7–1382 pg/g dry weight (average of 319 pg/g). Tri-CNs and tetra-CNs were two dominant homolog groups in air samples, while di-CNs were also found at comparable proportions to tri-CNs and tetra-CNs in soil samples. Most air and soil samples from the industrial and urban areas showed higher PCN concentrations than those from suburban areas. However, some soil samples in urban centers presented higher PCN concentrations than industrial areas. Analysis of PCN sources indicated that both industrial thermal process and historical usage of commercial PCN mixtures contributed to the PCN burden in most areas. The fugacity fraction results indicated a strong tendency of volatilization for lighter PCNs (tri- to hexa-CNs) in both seasons, and air–soil deposition for octa-CNs. Moreover, air–soil exchange fluxes indicate that soil was an important source of atmospheric PCNs in some areas. The results of this study provide information for use in the evaluation of the potential impact and human health risk of PCNs around the study areas.

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In 1997, the United States National Ambient Air Quality Standard (NAAQS) for ozone was revised from a 1-h average of 0.12 parts per million (ppm) to an 8-h average of 0.08 ppm. Analysis of ozone data for the ensemble of the contiguous United States and for the period 1980–1998 shows that the average number of summer days per year in exceedance of the new standard is in the range 8–24 in the Northeast and in Texas, and 12–73 in southern California. The probability of exceedance increases with temperature and exceeds 20% in the Northeast for daily maximum temperatures above 305 K. We present the results of several different approaches to analyzing the long-term trends in the old and new standards over the continental United States from 1980 to 1998. Daily temperature data are used to resolve meteorological variability and isolate the effects of changes in anthropogenic emissions. Significant negative trends are found in the Northeast urban corridor, in the Los Angeles Basin and on the western bank of Lake Michigan. Temperature segregation enhances the detection of negative trends. Positive trends occur at isolated sites, mostly in the Southeast; a strong positive trend is found in Nashville (Tennessee). There is some evidence that, except in the Southwest, air quality improvements from the 1980s to the 1990s have leveled off in the past decade.  相似文献   

4.
Knowledge of the characteristics of Pb and its isotopic transfer in different compartments is scant, especially for the mobility of Pb isotopes in the geochemical cycle. The present study characterizes differential Pb transport mechanism and the mobility of Pb isotopes in the pedogenic parent rock–pedosphere–irrigated riverwater–cereal–atmosphere system in the Yangtze River delta region, by determining Pb concentration and Pb isotopic ratios of pedogenic parent rocks, fluvial suspended particle matter, tillage soils, soil profiles, irrigated riverwater, fertilizer, Pb ore, cereal roots and grains. The results show that Pb isotopes in the geochemical cycle generally follow the equation of 208Pb/206Pb = −1.157 × 206Pb/207Pb + 3.46 (r2 = 0.941). However, Pb isotopes have different mobility in different environmental matrixes. Whereas in the pedosphere, the heavier Pb (208Pb) usually shows stronger mobility relative to the lighter Pb, and is more likely to transfer into soil exchangeable Pb fraction and carbonates phase. The lighter Pb shows stronger transfer ability from soil to cereal grain via root compared to the heavier Pb. However, the cereal grains have lower 206Pb/207Pb and higher 208Pb/206Pb ratios than root and tillage soil, similar to the airborne Pb and anthropogenic Pb, implying that a considerable amount of Pb in cereal grains comes from the atmosphere. The estimate model shows that 16.7–52.6% (average: 33.5%) of Pb in rice grain is the airborne Pb.  相似文献   

5.
The photodegradation processes of fenpropathrin and λ-cyhalothrin were studied in hexane, methanol/water (1:1, v/v), and acetone in both ultraviolet light and simulated sunlight. Intermediates in the photodegradation process were identified using gas chromatography/mass spectrometry (GC/MS), and the analysis of intermediates was used to speculate on possible photodegradation pathways. The photodegradation processes of fenpropathrin and λ-cyhalothrin followed pseudo first-order kinetics. The photodegradation rates varied according to the solvent in decreasing order: hexane?>?methanol/water (1:1, v/v)?>?acetone. The effects of substances coexisting in the environment on the photodegradation of pyrethroids were also investigated in the research. Acetone, humic acid, and riboflavin increased photodegradation rates while l-ascorbic acid slowed the process. This study provides a theoretical basis for the removal of pyrethroid pollution from the natural environment.  相似文献   

6.
Aerosol samples were collected from Northwest China desert region (Minqin), coastal suburb (Qingdao) and interior of the Yellow Sea (Qianliyan) in spring and summer of 1995 and 1996. Samples were analysed for major components, carbon and sulphur. The results show that concentrations of aerosols change considerably in time and space. The crustal materials carried by cold front system increase notably the aerosol concentration (mass/unit vol.) over the Yellow Sea but reduce the percentage contribution of pollutants and sea-salt. The sea-salt and regional aerosols become dominant fractions in coastal atmosphere in summer when the dust storms are expired in source region and the Southeast monsoon starts in the Pacific Ocean.  相似文献   

7.
The Bulgarian dispersion model 'Eulerian Model for Air Pollution' (EMAP) is used to estimate the sulphur pollution over the Balkan region for the period 1995–2000. A subdomain of the European Monitoring and Evaluation Programme (EMEP) grid is chosen containing 12 countries. The computational grid in this domain has a space step of 25 km, twice as fine as the EMEP grid. The former operational DWD 'Europa-Model' is used as meteorological driver. The source input is the official EMEP emission data. Monthly calculations are made having the last moment fields from the previous month as initial conditions for the next one. The boundary conditions are set to zero, so the influence of other European sources is not accounted for in this study. According to the EMEP methodology, multiple runs are made setting every time the sources of various countries to zero. The impact of every country in the pollution of all others is estimated.  相似文献   

8.
This study focused on establishing trends in the period 1988–2001 in PM2.5, PM10 and ozone concentrations in Santiago, Chile, and linking those to population exposure. There is strong seasonality in the concentration levels, driven by prevailing meteorological conditions, with the concentration of particulates peaking at the beginning of winter, whereas the ozone concentration is highest during the summer. The levels of PM2.5 and PM10 have substantially decreased since the late 1980s and so has the population exposure. Nevertheless, the majority of the population is still exposed to annual average levels that are above standard values. The situation with ozone exposure is different; no substantial decrease can be observed in the data. If anything, certain parts of Santiago, notably the south-east, have shown increased levels of ozone. Overall population exposure indicates that the average person was more at risk of ozone in the year 2000 than they were in 1993.  相似文献   

9.
The air-sea gas exchange of alpha-hexachlorocyclohexane (α-HCH) in the Canadian Arctic was estimated using a micrometeorological approach and the commonly used Whitman two-film model. Concurrent shipboard measurements of α-HCH in air at two heights (1 and 15 m) and in surface seawater were conducted during the Circumpolar Flaw Lead study in 2008. Sampling was carried out during eight events in the early summer time when open water was encountered. The micrometeorological technique employed the vertical gradient in air concentration and the wind speed to estimate the flux; results were corrected for atmospheric stability using the Monin-Obukhov stability parameter. The Whitman two-film model used the concentrations of α-HCH in surface seawater, in bulk air at 1 and 15 m above the surface, and the Henry's law constant adjusted for temperature and salinity to derive the flux. Both approaches showed that the overall net flux of α-HCH was from water to air. Mean fluxes calculated using the micrometeorological technique ranged from -3.5 to 18 ng m(-2) day(-1) (mean 7.4), compared to 3.5 to 14 ng m(-2) day(-1) (mean 7.5) using the Whitman two-film model. Flux estimates for individual events agreed in direction and within a factor of two in magnitude for six of eight events. For two events, fluxes estimated by micrometeorology were zero or negative, while fluxes estimated with the two-film model were positive, and the reasons for these discrepancies are unclear. Improvements are needed to shorten air sampling times to ensure that stationarity of meteorological conditions is not compromised over the measurement periods. The micrometeorological technique could be particularly useful to estimate fluxes of organic chemicals over water in situations where no water samples are available.  相似文献   

10.
We use GEOS-Chem chemical transport model simulations of sulfate–ammonium aerosol data from the NASA ARCTAS and NOAA ARCPAC aircraft campaigns in the North American Arctic in April 2008, together with longer-term data from surface sites, to better understand aerosol sources in the Arctic in winter–spring and the implications for aerosol acidity. Arctic pollution is dominated by transport from mid-latitudes, and we test the relevant ammonia and sulfur dioxide emission inventories in the model by comparison with wet deposition flux data over the source continents. We find that a complicated mix of natural and anthropogenic sources with different vertical signatures is responsible for sulfate concentrations in the Arctic. East Asian pollution influence is weak in winter but becomes important in spring through transport in the free troposphere. European influence is important at all altitudes but never dominant. West Asia (non-Arctic Russia and Kazakhstan) is the largest contributor to Arctic sulfate in surface air in winter, reflecting a southward extension of the Arctic front over that region. Ammonium in Arctic spring mostly originates from anthropogenic sources in East Asia and Europe, with added contribution from boreal fires, resulting in a more neutralized aerosol in the free troposphere than at the surface. The ARCTAS and ARCPAC data indicate a median aerosol neutralization fraction [NH4+]/(2[SO42?] + [NO3?]) of 0.5 mol mol?1 below 2 km and 0.7 mol mol?1 above. We find that East Asian and European aerosol transported to the Arctic is mostly neutralized, whereas West Asian and North American aerosol is highly acidic. Growth of sulfur emissions in West Asia may be responsible for the observed increase in aerosol acidity at Barrow over the past decade. As global sulfur emissions decline over the next decades, increasing aerosol neutralization in the Arctic is expected, potentially accelerating Arctic warming through indirect radiative forcing and feedbacks.  相似文献   

11.
The response of Pinus maximartinezii Rzedowski to photochemical oxidant air pollution was examined using 100 trees, during a 1 year cycle, at Vivero de Coyoacán, a tree nursery located in the south central part of México City, where exposure to polluted air masses has been continuous. The tree response assessment method was based upon documented symptoms of pollutant injury on the foliage. The results showed a homogeneous pattern of health and vigor and only medium sensitivity (based on foliar injury) to photochemical oxidants, although the trees maintained their needles through a three and not the normal 5 year period as at its geographic location of origin (different habitat or environment). Nevertheless, these data suggest that this species of pine could be proposed as good planting material for reforestation in the urban metropolitan area of México city.  相似文献   

12.
The emission of isoprene has been studied from a forest of Abies Borisii-regis, a Mediterranean fir species previously thought to emit only monoterpenes. Emission studies from two independent enclosure experiments indicated a standardised isoprene emission rate of (18.4±3.8) μg gdry-weight−1 h−1, similar in magnitude to species such as eucalyptus and oak which are considered to be strong isoprene emitters. Isoprene emission depended strongly on both leaf temperature (2°C–34°C) and photosynthetically active radiation (PAR) below 250 μmol m−2 s−1, becoming saturated with respect to PAR above this value. The annual isoprene emission rate was estimated to be (132±29) kT yr−1 for those trees growing within Greece, comparable to current estimates of the total isoprene budget of Greece as a whole, and contributing significantly to regional ozone and carbon monoxide budgets. Monoterpene emission exhibited exponential temperature dependence, with 1,8-cineole, α-pinene, β-pinene and limonene forming the primary emissions. A standardised total monoterpene emission rate of (2.7±1.1) μg gdry-weight−1 h−1 was calculated, corresponding to an annual monoterpene emission rate of (24±12) kT yr−1. Research was conducted as part of the AEROBIC’97 (AEROsol formation from BIogenic organic Carbon) series of field campaigns.  相似文献   

13.
Environmental Science and Pollution Research - Feedback between hydrologic variations and chemical weathering is thought to play a crucial role in modulating global carbon cycling. The mechanisms...  相似文献   

14.
In this paper the process by which a distributional model may be identified from a range of alternative models is examined. An assessment of the methods by which goodness-of-fit may be evaluated is presented. A procedure for selecting amongst the exponential, gamma, lognormal and Weibull distributions has been applied to 24-h average suspended particulates (β-scattering), ozone, carbon monoxide, sulphur dioxide, oxides of nitrogen, nitrogen dioxide and nitrogen oxide observations recorded in Melbourne, Australia. It is shown that
  • 1.(a) lognormal distribution is appropriate for particulate data and the majority of the nitric oxide, oxides of nitrogen and sulphur dioxide data sets
  • 2.(b) gamma distribution is best for both carbon monoxide, nitrogen dioxide and ozone
  • 3.(c) Weibull distribution is appropriate for a significant number of carbon monoxide and ozone data sets.
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In Part I of this series Taylor, Jakeman and Simpson (1986, Atmospheric Environment, 20, 1781–1789) examined the problem of identifying the appropriate distributional form for air pollution concentration data. In this paper we examine the parameter estimation problem. Monte Carlo simulation is used to compare methods for fitting statistical distributions to such data where the distributional form is known. Three methods are investigated for estimating the parameters of the lognormal distribution, two methods for the exponential distribution, three methods for the γ-distribution and four methods for the Weibull distribution. For all distributions and for each method we examine the accuracy with which the upper percentiles of the distribution are evaluated as it is these percentiles which are referred to by air quality standards. For each distribution a simple empirical model, which yields approximations to the relative root mean square error of the percentile estimates against sample size and parameter values, is developed and demonstrated. Thus for each distributional model an estimate of the relative error associated with evaluating high pollutant levels may be readily determined.  相似文献   

17.
In this analysis, we characterize urban and rural ozone (O3) trends across the US for the periods 1980–2008 (29 years) and 1994–2008 (15 years) using three exposure metrics, which summarize daily O3 concentrations to reflect different ways O3 may affect human health and vegetation. We observe that a statistically significant trend at a specific monitoring site, using one exposure metric, does not necessarily result in a similar trend using the other two metrics. The two most common trends among the monitoring sites are either a continuation of negative trending over the 29-year period or a shift from negative to no trend status, indicating a leveling off of the trending. Very few sites exhibit statistically significant increases in the exposure indices. In characterizing the statistically significant changes in the distribution of hourly average O3, we observe subtle statistically significant changes in the lower part of the distribution (i.e., below 50 ppb) that are not necessarily captured by the trending patterns associated with the three exposure metrics. Using multisite data from 12 metropolitan cities, we find that as the frequency of higher hourly average concentrations is reduced, the lower hourly average concentrations also move upward toward the mid-level values. The change in the number of the hourly average concentrations in the lower range is consistent with decreased NO scavenging. We recommend assessing possible subtle shifts in O3 concentrations by characterizing changes in the distribution of hourly average concentrations by month. Identifying statistically significant monthly changes in the mid- and low-level hourly average concentrations may provide important information for assessing changes in physical processes associated with global climate change, long-range transport, and the efficacy of models used for emission and risk reductions. Our results indicate that it is important to investigate the change in the trending pattern with time (e.g., moving 15-year trending) in order to assess how year-to-year variability may influence the trend calculation.  相似文献   

18.
Ambient air concentrations of specific C2–C6 hydrocarbons (HCs) are reported for various days during the summer months of 1983. The samples are classified as either urban, rural or polluted rural according to the sampling site, meteorological conditions and ozone levels. Generally, both the concentrations and HC/acetylene ratios are similar to those reported by other workers for comparable sites. The alkane/alkene ratio at the rural site exceeded that for the urban site and it is concluded that the major contribution to HCs at the former site is advection from distant sources. It appears that the main source of propane in rural areas is natural gas, with about 4.5–9 ppbC unaccounted for by this source.  相似文献   

19.
Environmental Science and Pollution Research - Ground level ozone is a major air pollutant with known toxic effects on humans. The research field is well established with many scientists from...  相似文献   

20.
Polychlorinated dibenzo-p-dioxin and dibenzofuran (PCDD/PCDF) were overall measured and compared in ambient air, water, soils, and sediments along the upper reaches of the Haihe River of North China, so as to evaluate their concentrations, profiles, and to understand the processes of gas–particle partitioning and air–water/soil exchange. The following results were obtained: (1) The average concentrations (toxic equivalents, TEQs) of 2,3,7,8-PCDD/PCDF in air, water, sediment, and soil samples were 4,855 fg/m3, 9.5 pg/L, 99.2 pg/g dry weight (dw), and 56.4 pg/g (203 fg TEQ/m3, 0.46 pg TEQ/L, 2.2 pg TEQ/g dw, and 1.3 pg TEQ/g, respectively), respectively. (2) Although OCDF, 1,2,3,4,6,7,8-HpCDF, OCDD, and 1,2,3,4,6,7,8-HpCDD were the dominant congeners among four environmental sinks, obvious discrepancies of these congener and homologue patterns of PCDD/PCDF were observed still. (3) Significant linear correlations for PCDD/PCDF were observed between the gas–particle partition coefficient (K p) and the subcooled liquid vapor pressure (P L 0) and octanol–air partition coefficient (K oa). (4) Fugacity fraction values of air–water exchange indicated that most of PCDD/PCDF homologues were dominated by net volatilization from water into air. The low-chlorinated PCDD/PCDF (tetra- to hexa-) presented a strong net volatilization from the soil into air, while high-chlorinated PCDD/PCDF (hepta- to octa-) were mainly close to equilibrium for air–soil exchange.  相似文献   

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