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1.
2.
During the 1999 summer field season at Summit, Greenland, we conducted several series of experiments to follow up on our 1998 discovery that NOx is released from the sunlit snowpack. The 1999 experiments included measurements of HONO in addition to NO and NO2, and were designed to confirm, for Greenland snow, that the processes producing reactive nitrogen oxides in the snow are largely photochemical. Long duration experiments (up to 48 h) in a flow-through chamber and in the natural snowpack revealed sun-synchronous diurnal variations of all three reactive nitrogen oxides. In a second set of experiments we alternately shaded or exposed snow (again in the natural snowpack and in the chamber) to ambient sunlight for short periods to reduce any temperature changes during variations in light intensity. All three N oxides increased (decreased) very rapidly when sunlit (shaded). In all experiments NO2 was approximately 3-fold more abundant than NO and HONO (which were at similar levels). Higher concentrations of NO3 in the snow resulted in higher mixing ratios of HONO, NO and NO2 in the snow pore air, consistent with our hypothesis that photolysis of NO3 is the source of the reactive N oxides.  相似文献   

3.
The mineral insoluble fraction of snowpit samples collected at Summit is investigated, representing deposition from summer 1987 to summer 1991. We attempt to describe the particles which are observed in the series, with very large seasonal variations. Elemental, mineralogical and size distribution studies are carried out on four samples selected according to the chemical profile of the snowpit (two samples from spring and two from winter) using X-ray fluorescence spectrometry and analytical transmission electron microscopy. Results indicate a large predominance of the soil-derived particles originating from arid or semi-arid regions of the Northern Hemisphere. The mineralogy clearly indicates a high contribution for the muscovite-illite associated with a low kaolinite/chlorite ratio, together with the rather lack of smectite. This supports the hypothesis of an Asian source. Several other factors are consistent with this Asian source, like the recent climatology and the good timing between the Asian dust storms period and the peak of dust concentration in the ice. The mineralogy of the insoluble particles in the snow is similar between winter and spring, suggesting that the change of concentration between the seasons is more strongly linked to changes of atmospheric parameters than changes of the source regions.  相似文献   

4.
A study of carbonaceous particulate matter (PM) was conducted in the Middle East at sites in Israel, Jordan, and Palestine. The sources and seasonal variation of organic carbon, as well as the contribution to fine aerosol (PM2.5) mass, were determined. Of the 11 sites studied, Nablus had the highest contribution of organic carbon (OC), 29%, and elemental carbon (EC), 19%, to total PM2.5 mass. The lowest concentrations of PM2.5 mass, OC, and EC were measured at southern desert sites, located in Aqaba, Eilat, and Rachma. The OC contribution to PM2.5 mass at these sites ranged between 9.4% and 16%, with mean annual PM2.5 mass concentrations ranging from 21 to 25 ug m?3. These sites were also observed to have the highest OC to EC ratios (4.1–5.0), indicative of smaller contributions from primary combustion sources and/or a higher contribution of secondary organic aerosol. Biomass burning and vehicular emissions were found to be important sources of carbonaceous PM in this region at the non-southern desert sites, which together accounted for 30%–55% of the fine particle organic carbon at these sites. The fraction of measured OC unapportioned to primary sources (1.4 μgC m?3 to 4.9 μgC m?3; 30%–74%), which has been shown to be largely from secondary organic aerosol, is relatively constant at the sites examined in this study. This suggests that secondary organic aerosol is important in the Middle East during all seasons of the year.  相似文献   

5.
The surface energy balance (SEB) is essential for understanding the coupled cryosphere–atmosphere system in the Arctic. In this study, we investigate the spatiotemporal variability in SEB across tundra, snow and ice. During the snow-free period, the main energy sink for ice sites is surface melt. For tundra, energy is used for sensible and latent heat flux and soil heat flux leading to permafrost thaw. Longer snow-free period increases melting of the Greenland Ice Sheet and glaciers and may promote tundra permafrost thaw. During winter, clouds have a warming effect across surface types whereas during summer clouds have a cooling effect over tundra and a warming effect over ice, reflecting the spatial variation in albedo. The complex interactions between factors affecting SEB across surface types remain a challenge for understanding current and future conditions. Extended monitoring activities coupled with modelling efforts are essential for assessing the impact of warming in the Arctic.  相似文献   

6.
The chemical composition of pollutant species in precipitation sampled daily or weekly at 10 sites in Ireland for the five-year period, 1994–1998, is presented. Sea salts accounted for 81% of the total ionic concentration. Approximately 50% of the SO42− in precipitation was from sea-salt sources. The proportion of sea salts in precipitation decreased sharply eastwards. In contrast, the concentration of NO3 and the proportion of non-sea-salt SO42− increased eastwards reflecting the closer proximity to major emission sources. The mean (molc) ratio of SO42−:NO3 was 1.6 for all sites, indicating that SO42− was the major acid anion.The spatial correlation between SO42−, NO3 and NH4+ concentrations in precipitation was statistically significant. The regional trend in NO3 concentration was best described by linear regression against easting. SO42− concentration followed a similar pattern. However, the regression was improved by inclusion of elevation. Inclusion of northing in the regression did not significantly improve any of the relationships except for NH4+, indicating a significant increase in concentrations from northwest to southeast.The spatial distribution of deposition fluxes showed similar gradients increasing from west and southwest to east and northeast. However, the pattern of deposition shows the influence of precipitation volume in determining the overall input. Mean depositions of sulphur and nitrogen in precipitation were ≈30 ktonnes S yr−1 and 48 ktonnes N yr−1 over the five-year period, 1994–1998, for Ireland.Least-squares linear regression analysis indicated a slight decreasing trend in precipitation concentrations for SO42− (20%), NO3 (13%) and H+ (24%) and a slight increasing trend for NH4+ (15%), over the period 1991–1998.  相似文献   

7.
Organic pollutants, especially polychlorinated hydrocarbons, phenols, guaiacols and catechols have been studied by analyses of snow samples from North Pole, May 1984. All of these pollutants were below the limit of determination which was estimated to be as fallout 0.1–0.05 μg/m2 for individual compounds. For comparison, snow samples from Central Finland and South Finland 1983–1985 also showed non-detectable levels of chlorinated hydrocarbons but well measurable levels of chlorophenol compounds which were significantly higher at urban (heavy traffic) than rural and higher at South than Central Finnish places, respectively. One sample from Lapland, North Finland 1985, however, had no measurable amounts of chlorophenols like the North Pole sample.  相似文献   

8.
Sonic anemometer turbulence measurements were made at Summit, Greenland during summer 2004 and spring 2005. These measurements allow for the characterization of the variability of the atmospheric boundary layer at this site by describing seasonal and diurnal changes in sensible heat flux and boundary layer stability as well as providing estimates of mixing layer height. Diurnal sensible heat fluxes at Summit ranged from −18 to −2 W m−2 in the spring and from −7 to +10 W m−2 in the summer. Sustained stable surface layer conditions and low wind speeds occured during the spring but not during the summer months. Unstable conditions were not observed at Summit until late April. Diurnal cycles of convective conditions during the daytime (0700–1700 h local time) were observed throughout July and August. Boundary layer heights, which were estimated for neutral to stable conditions, averaged 156 m for the spring 2005 observations. Comparisons of the boundary layer characteristics of Summit with those from South Pole, Antarctica, provide possible explanations for the significant differences in snowpack and surface-layer chemistry between the two sites.  相似文献   

9.
Atmospheric monitoring data for selected polynuclear aromatic hydrocarbons (PAHs) were compiled from remote, rural and urban locations in the UK, Sweden, Finland and Arctic Canada. The objective was to examine the seasonal and temporal trends, to shed light on the factors which exert a dominant influence over ambient PAH levels. Urban centres in the UK have concentrations 1-2 orders of magnitude higher than in rural Europe and up to 3 orders of magnitude higher than Arctic Canada. Interpretation of the data suggests that proximity to primary sources 'drives' PAH air concentrations. Seasonality, with winter (W) > summer (S), was apparent for most compounds at most sites; high molecular weight compounds (e.g. benzo[a]pyrene) showed this most clearly and consistently. Some low molecular weight compounds (e.g. phenanthrene) sometimes displayed S>W seasonality at some rural locations. Strong W>S seasonality is linked to seasonally-dependent sources which are greater in winter. This implicates inefficient combustion processes, notably the diffusive domestic burning of wood and coal. However, sometimes seasonality can also be strongly influenced by broad changes in meteorology and air mass origin (e.g. in the Canadian Arctic). The datasets examined here suggest a downward trend for many PAHs at some sites, but this is not apparent for all sites and compounds. The inherent noise in ambient air monitoring data makes it difficult to derive unambiguous evidence of underlying declines, to confirm the effectiveness of international source reduction measures.  相似文献   

10.
Long Ye  Hong You  Jie Yao  Xi Kang  Lu Tang 《Chemosphere》2013,90(10):2493-2498
Seasonal variation and influencing factors of perchlorate in snow, surface soil, rain, surface water, groundwater and corn were studied. Seven hundreds and seventy samples were collected in different periods in Harbin and its vicinity, China. Perchlorate concentrations were analyzed by ion chromatography–electrospray mass spectrometry. Results indicate that fireworks and firecrackers display from the Spring Festival to the Lantern Festival (February 2, 2011–February 17, 2011) can result in the occurrence of perchlorate in surface soil and snow. Perchlorate distribution is affected by wind direction in winter. Melting snow which contained perchlorate can dissolve perchlorate in surface soil, and then perchlorate can percolate into groundwater so that perchlorate concentrations in groundwater increased in spring. Perchlorate concentrations in groundwater and surface water decrease after rainy season in summer. Groundwater samples collected in the floodplain areas of the Songhua River and the Ashi River contained higher perchlorate concentrations than that far away with the rivers. The corns have the ability to accumulate perchlorate.  相似文献   

11.
Li Z  Li D  Oh JR  Je JG 《Chemosphere》2004,56(6):611-618
Alkylphenols (APs) have been known as endocrine disruptors and consequently received much environmental concern. This study focused on seasonal variation and spatial distribution of nonylphenol (NP) in various matrixes including dissolved water, particulates, surface sediment, sediment trap and sediment core taken from Shihwa Lake and its adjacent areas. A total of 11 phenolic compounds including nonylphenol, t-octylphenol (t-OP) and bisphenol A (BPA) were measured in February, June and October 2002. NP is the most abundant chemical among the phenolic compounds and its concentrations in dissolved water, particulates and surface sediments from Shihwa Lake were measured as 17.4-1533.1 ng/l, 4.3-831.2 ng/l and 10.4-5054.1 ng/g dw, respectively. NP concentration in dissolved water varied with seasons and generally showed a decreasing order of June > October > February, while the seasonal trend was hardly found in sediment. High levels of NP were measured in surrounding industrial complexes, the concentrations was decreased gradually with distance from the industrial areas. NP in core samples showed an increasing trend toward the core depth. There exists a reasonable correlation between NP in dissolved water and in particulates, whereas the correlation between NP in dissolved water and in sediments is not significant. APs concentrations in Shihwa Lake were comparable to other highly polluted areas of the world and their possible effects on various organisms in the lake are discussed.  相似文献   

12.
Gannet (Sula bassana) eggs collected from Ailsa Craig, Western Scotland between 1977-1998 have been analyzed retrospectively for several PCB congeners. Concentrations of a range of congeners were determined in 8-10 eggs analyzed separately for several individual years. All congeners declined in concentrations throughout the time period, but the rates of decline differed for different congeners. Declines were first order and half-lives varied between 5.4 years for PCB-101 to 10.1 years for PCB-180. Egg concentrations reflect the maternal body burden, which itself is controlled by the birds rate of intake (principally via the diet) and losses (via metabolism and other clearance mechanisms). The declining concentrations in eggs, therefore, broadly reflect reductions in prey concentrations (principally herring and mackerel) and--in turn--water column concentrations. Rates of change in PCB concentrations from this study were similar to those noted in fish-eating birds from the Baltic Sea and North American Great Lakes, and ambient air in the UK. This provides indirect evidence that gannet eggs are broadly reflecting regional/global scale clearance/removal mechanisms which are controlling ambient PCB concentrations.  相似文献   

13.
14.
Time-series of perfluorinated alkylated substances (PFASs) in East Greenland polar bears and East and West Greenland ringed seals were updated in order to deduce whether a response to the major reduction in perfluoroalkyl production in the early 2000s had occurred. Previous studies had documented an exponential increase of perfluorooctane sulphonate (PFOS) in liver tissue from both species. In the present study, PFOS was still the far most dominant compound constituting 92% (West Greenland ringed seals), 88% (East Greenland ringed seals) and 85% (East Greenland polar bears). The PFOS concentrations increased up to 2006 with doubling times of approximately 6 years for the ringed seal populations and 14 years in case of polar bears. Since then a rapid decrease has occurred with clearing half-lives of approximately 1, 2 and 4 years, respectively. In polar bears perfluorohexane sulphonate (PFHxS) and perfluorooctane sulphonamide (PFOSA) also showed decreasing trends in recent years as do perfluorodecanoic acid (PFDA) and perfluoroundecanoic acid (PFUnA). For the West Greenland ringed seal population perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), PFDA and PFUnA peaked in the mid 2000s, whereas PFNA, PFDA and PFUnA in the East Greenland population have been stable or increasing in recent years. The peak of PFASs in Greenland ringed seals and polar bears occurred at a later time than in Canadian seals and polar bears and considerably later than observed in seal species from more southern latitudes. We suggest that this could be explained by the distance to emission hot-spots and differences in long-range transport to the Arctic.  相似文献   

15.
A continuous, 19-year record (1963–1982) of weekly, bulk precipitation chemistry at the Hubbard Brook Experimental Forest in West Thornton, New Hampshire shows no statistically significant trend in annual volume-weighted concentrations of hydrogen ion and nitrate, but a 34% decrease in sulfate, a 34% decrease in ammonium, a 63% decrease in chloride, a 79% decrease in magnesium and an 86% decrease in calcium during the period. Nitrate concentrations increased from 1964 to 1971 and H-ion concentrations decreased after 1970. Frequency distributions of the concentrations of the chemical components of precipitation are skewed. The range of H-ion concentrations in weekly samples has narrowed, and the frequency distribution has shifted toward higher concentrations (lower pH) during the last 19 years. Highest concentrations generally occur with lowest amounts of precipitation for most ions, but low concentrations can occur with either low or high amounts of precipitation. Time trends in deposition generally parallel trends in concentration over the 19-year period. Chemical deposition generally increases with increasing amount of precipitation in weekly samples.  相似文献   

16.
Mercury in the Mediterranean,part I: spatial and temporal trends   总被引:1,自引:0,他引:1  
The present paper provides an overview of mercury studies performed in the Mediterranean Sea region in the framework of several research projects funded by the European Commission and on-going national programmes carried out during the last 15 years. These studies investigated the temporal and spatial distribution of mercury species in air, in the water column and sediments, and the transport mechanisms connecting them. It was found that atmospheric concentrations of Hg compounds, particularly oxidised Hg species observed at five coastal sites in the Mediterranean Sea Basin, are significantly higher compared with those recorded at five coastal sites distributed across N Europe, most probably due to natural emissions. Hg levels in water are comparable to other oceans. Anthropogenic and natural point sources show locally limited enrichments, while natural diffusive sources influence Hg speciation over larger areas. Results and statistic comparison of mercury species concentrations within Mediterranean compartments will be presented and discussed.  相似文献   

17.
Aquatic pollution by metals is of concern because of various toxic effects to marine life. The Tolka Estuary, Co. Dublin, Ireland, is a typical Irish urban estuary. It has a significant metal loading originating from the urban environment. Results of a 25month analysis of cadmium, copper, lead and zinc spatial and temporal distribution over 10 sample locations in this estuary are presented in this paper. Metal concentrations were analysed using differential pulse polarography. Significant seasonal and spatial trends in metal distribution were observed over the 25months. Sediment metal concentrations gradually increased (30-120%) in spring to a maximum at the end of summer which was followed by a decrease in winter months (30-60%). Sediment organic matter (OM) concentrations exhibited similar seasonal trends and a positive correlation between OM and metal distributions was observed, implying OM had an influence on metal distributions over time.  相似文献   

18.
Xu J  Wang P  Guo W  Dong J  Wang L  Dai S 《Chemosphere》2006,65(9):1445-1451
Nonylphenol (NP) is known as an endocrine disruptor and consequently has drawn much environmental concern. This study focused on seasonal variation and spatial distribution of NP in various matrices including water, suspended particles, and sediment taken from Lanzhou Reach of Yellow River in China. NP was measured in July and November in 2004. Concentrations of NP in water ranged from 34.2 to 599.0 ng/l, in suspended particles from 49.6 to 2835.2 ng/g dry wt, and in sediment from 38.4 to 863.0 ng/g dry wt. In terms of most water and suspended particles samples, concentrations were higher in warmer seasons than in colder seasons. Good linear correlations (R(2)=0.90 in July, R(2)=0.97 in November) were obtained for NP concentrations between water and suspended particles. In terms of sediment samples, concentrations were higher in November than in July, probably due to greater deposition of suspended particles. Reasonable linear correlations (R(2)=0.60 in July, R(2)=0.79 in November) were obtained for NP concentrations between water and sediment.  相似文献   

19.
Site and regional trends in seasonally averaged particle SO4(2-) concentrations were examined for a large portion of the United States using data collected by the CASTNet air monitoring network. Trends were analyzed for overlapping periods of 1988-1999 and 1992-1999. The largest absolute SO4(2-) decreases--approximately -0.4 microg/m3/yr--between 1988 and 1999 occurred in summer for sites in the Ohio River Valley and areas to the east. Generally, the largest SO4(2-) reductions were found for summer, but larger relative reductions often occurred for spring and autumn. Sulfate changes during 1992-1999 were quite different from those found for 1988-1999 and were not entirely consistent with changes in SO2 emissions. In some locations, the 1992-1999 period saw smaller declines in SO4(2-), while in other places seasonal SO4(2-) actually increased. Increases were mostly confined to summer and autumn across the southern and southwestern states. Multivariate analysis of ambient sulfur levels, by region, versus SO2 emissions reveals that annual emissions are associated with more than 80% of the variance in seasonal sulfur (SO2 and SO4(2-)) in more than three-quarters of the cases examined. The weakest associations were found for the southeastern United States.  相似文献   

20.
There is a need for a robust and accurate technique to measure ammonia (NH3) emissions from animal feeding operations (AFOs) to obtain emission inventories and to develop abatement strategies. Two consecutive seasonal studies were conducted to measure NH3 emissions from an open-lot dairy in central Texas in July and December of 2005. Data including NH3 concentrations were collected and NH3 emission fluxes (EFls), emission rates (ERs), and emission factors (EFs) were calculated for the open-lot dairy. A protocol using flux chambers (FCs) was used to determine these NH3 emissions from the open-lot dairy. NH3 concentration measurements were made using chemiluminescence-based analyzers. The ground-level area sources (GLAS) including open lots (cows on earthen corrals), separated solids, primary and secondary lagoons, and milking parlors were sampled to estimate NH3 emissions. The seasonal NH3 EFs were 11.6 +/- 7.1 kg-NH3 yr(-1)head(-1) for the summer and 6.2 +/- 3.7 kg-NH3 yr(-1)head(-1) for the winter season. The estimated annual NH3 EF was 9.4 +/- 5.7 kg-NH3 yr(-1)head(-1) for this open-lot dairy. The estimated NH3 EF for winter was nearly 47% lower than summer EF. Primary and secondary lagoons (approximately 37) and open-lot corrals (approximately 63%) in summer, and open-lot corrals (approximately 95%) in winter were the highest contributors to NH3 emissions for the open-lot dairy. These EF estimates using the FC protocol and real-time analyzer were lower than many previously reported EFs estimated based on nitrogen mass balance and nitrogen content in manure. The difference between the overall emissions from each season was due to ambient temperature variations and loading rates of manure on GLAS. There was spatial variation of NH3 emission from the open-lot earthen corrals due to variable animal density within feeding and shaded and dry divisions of the open lot. This spatial variability was attributed to dispirit manure loading within these areas.  相似文献   

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