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1.
The use of fireworks creates an unusual and distinctive anthropogenic atmospheric pollution event. We report on aerosol samples collected during Las Fallas in Valencia, a 6-day celebration famous for its firework displays, and add comparative data on firework- and bonfire-contaminated atmospheric aerosol samples collected from elsewhere in Spain (Barcelona, L’Alcora, and Borriana) and during the Guy Fawkes celebrations in London. Specific high-profile official firework events during Las Fallas included the afternoon Mascletà and the nightly aerial displays (especially in the climactic final 2 days of the fiesta) and were accompanied by pollution spikes in suspended particles, NO, SO2, and the creation and dispersal of an aerosol cloud enriched in a range of metallic elements. Notable metal aerosol concentration increases recorded during Las Fallas were potassium (from 500 to 5900 ng m−3), aluminium (as Al2O3 from around 600 to 2200 ng m−3), titanium (from 200 to 700 ng m−3), magnesium (from 100 to 500 ng m−3), lead (from 17 to 379 ng m−3), barium (from 39 to 322 ng m−3), strontium (from 3 to 112 ng m−3), copper (from 12 to 71 ng m−3), and antimony (from 1 to 52 ng m−3). Firework-contaminated aerosols of similarly metalliferous composition were also identified at the other monitoring sites, although different sites show variations attributable to other sources such as bonfires and local industry. Unusual levels of the trace elements Ba, Sr and (to a lesser extent) Cu, always in proportions with Ba dominant, along with strongly enhanced K, Pb, and Sb, are identified as being particularly characteristic of firework aerosols. Although firework-related recreational pollution episodes are transient in nature, they are highly concentrated, contribute significantly to total annual metal emissions, and are on average fine enough to be easily inhaled and a health risk to susceptible individuals.  相似文献   

2.
Fine particle (PM2.5) samples were collected, using a charcoal diffusion denuder, in two urban areas of Chile, Santiago and Temuco, during the winter and spring season of 1998. Molecular markers of the organic aerosol were determined using GC/MS. Diagnostic ratios and molecular tracers were used to investigate the origin of carbonaceous aerosols. As main sources, road and non-road engine emissions in Santiago, and wood burning in Temuco were identified. Cluster analysis was used to compare the chemical characteristics of carbonaceous aerosols between the two urban environments. Distinct differences between Santiago and Temuco samples were observed. High concentrations of isoprenoid (30–69 ng m−3) and unresolved complex mixture (UCM) of hydrocarbons (839–1369 ng m−3) were found in Santiago. High concentrations of polynuclear aromatic hydrocarbons (751±304 ng m−3) and their oxygenated derivatives (4±2 ng m−3), and of n-alk-1-enes (16±13 ng m−3) were observed in Temuco.  相似文献   

3.
PM2.5 aerosols were collected in Nanjing, a typical mega-city in China, during summer and winter 2004 and were characterized for aromatic and cyclic compounds using a GC/MS technique to understand the air pollution problem. They include polycyclic aromatic hydrocarbons (PAHs), hopanes, phthalates and hydroxy-PAHs (OH-PAHs). PAHs, hopanes and OH-PAHs presented higher concentrations in winter (26–178, 3.0–18, and 0.013–0.421 ng m−3, respectively) than in summer (12–96, 1.6–11, and 0.029–0.171 ng m−3, respectively) due to an enhanced coal burning for house heating and atmospheric inversion layers developed in the cold season. In contrast, phthalates are more abundant in summer (109–368 ng m−3, average 230 ng m−3) than in winter (33–390 ng m−3, average 170 ng m−3) due to an enhanced evaporation from plastics during the hot season and the subsequent deposition on the pre-existing particles. Generally, all the identified compounds showed higher concentrations in nighttime than in daytime due to inversion layers and increased emissions from heavy-duty trucks at night. PAHs, hopanes and phthalates in Nanjing aerosols are 5–100 times more abundant than those in Los Angeles, USA, indicating a serious air pollution problem in the city. Concentrations of OH-PAHs are 1–3 orders of magnitude less than their parent PAHs and comparable to those reported from other international cities. Source identification using diagnostic ratios of the organic tracers suggests that PAHs in Nanjing urban area are mainly derived from coal burning, whereas hopanes are more attributable to traffic emissions.  相似文献   

4.
Micrometeorological measurements and ambient air samples, analyzed for concentrations of NH3, HNO3, NH4+, and NO3, were collected at an alpine tundra site on Niwot Ridge, Colorado. The measured concentrations were extremely low and ranged between 5 and 70 ng N m−3. Dry deposition fluxes of these atmospheric species were calculated using the micrometeorological gradient method. The calculated mean flux for NH3 indicates a net deposition to the surface and indicates that NH3 contributed significantly to the total N deposition to the tundra during the August–September measurement period. Our pre-measurement estimate of the compensation point for NH3 in air above the tundra was 100–200 ng N m−3; thus, a net emission of NH3 was expected given the low ambient concentrations of NH3 observed. Based on our results, however, the NH3 compensation point at this alpine tundra site appears to have been at or below about 20 ng N m−3. Large deposition velocities (>2 cm s−1) were determined for nitrate and ammonium and may result from reactions with surface-derived aerosols.  相似文献   

5.
Estimates of the atmospheric deposition to Galveston Bay of polycyclic aromatic hydrocarbons (PAHs) are made using precipitation and meteorological data that were collected continuously from 2 February 1995 to 6 August 1996 at Seabrook, TX, USA. Particulate and vapor phase PAHs in ambient air and particulate and dissolved phases in rain samples were collected and analyzed. More than 95% of atmospheric PAHs were in the vapor phase and about 73% of PAHs in the rain were in the dissolved phase. Phenanthrene and napthalene were the dominant compounds in air vapor and rain dissolved phases, respectively, while 5 and 6 ring PAH were predominant in the particulate phase of both air and rain samples. Total PAH concentrations ranged from 4 to 161 ng m−3 in air samples and from 50 to 312 ng l−1 in rain samples. Temporal variability in total PAH air concentrations were observed, with lower concentrations in the spring and fall (4–34 ng m −3) compared to the summer and winter (37–161 ng m−3). PAHs in the air near Galveston Bay are derived from both combustion and petroleum vaporization. Gas exchange from the atmosphere to the surface water is estimated to be the major deposition process for PAHs (1211 μg m− 2 yr− 1), relative to wet deposition (130 μg m−2 yr− 1) and dry deposition (99 μg m−2 yr− 1). Annual deposition of PAHs directly to Galveston Bay from the atmosphere is estimated as 2  t yr−1.  相似文献   

6.
Concentrations of different species of mercury in arctic air and precipitation have been measured at Ny-Ålesund (Svalbard) and Pallas (Finland) during 1996–1997. Typical concentrations for vapour phase mercury measured at the two stations were in the range of 0.7–2 ng m−3 whereas particulate mercury concentrations were below 5 pg m−3. Total mercury in precipitation was in the range 3–30 ng l−1. In order to evaluate the transport and deposition of mercury to the arctic from European anthropogenic sources, the Eulerian transport model HMET has been modified and extended to also include mercury species. A scheme for chemical conversion of elemental mercury to other species of mercury and deposition characteristics of different mercury species have been included in the model. European emission inventories for three different forms of Hg (Hg0, HgCl2 and Hgp) have been implemented in the numerical grid system for the HMET model.  相似文献   

7.
The concentrations and size distributions of low molecular weight dicarboxylic acids in suburban particulate matter collected in early and mid-autumn 2002 and early and mid-summer 2003 in Tainan, Taiwan, were analyzed. PM2.5 contained, on average, 449.3 ng m−3 oxalic acid, 53.0 ng m−3 malic acid, 45.5 ng m−3 maleic acid, 29.6 ng m−3 succinic acid, 20.8 ng m−3 malonic acid, and 11.6 ng m−3 tartaric acid. Bar tartaric acid, concentrations were higher during the day, indicating that these acids are photochemical products. Furthermore, the malonic acid–succinic acid ratio of 0.79 during daytime and 0.60 during nighttime demonstrates that more succinic acid is converted to malonic acid during daytime, and that aerosol dicarboxylic acids predominantly originate from photochemical oxidation during daytime. The concentration peak of oxalic acid occurred in the condensation and droplet modes (0.32–1.0 μm), as did that of sulfate. In early summer, succinic acid, malonic acid, and oxalic acid major concentration peaks occurred at 0.32–0.54 μm, indicative of the relationship created by photochemical decomposition of succinc acid into malonic acid into oxalic acid. This photochemical decomposition accelerated in mid-summer such that most concentration peaks for succinic and malonic acids also occurred at 0.32–1.0 μm. Mid-summer is also the wettest period of the four in Tainan, with 85% RH. As a result of hygroscopic reactions in mid-summer, malonic acid and oxalic acid major concentration peaks shifted from 0.32–0.54 μm or 0.54–1.0 μm to 1.0–1.8 μm, thus extending the range in which these species were found to larger particle sizes, and this shift was highly correlated with a shift in succinic acid size distribution. This latter observation offers additional evidence that succinic acid is photochemically decomposed into malonic acid and oxalic acid and that the presence of malonic and oxalic acids in the wet mid-summer atmosphere is made more obvious via hygroscopic growth. Close correlation between succinic acid and Na+ and succinic acid and NO3 in the coarse mode is related to sea spray.  相似文献   

8.
Mercury (Hg) emissions from gasoline, diesel, and liquefied petroleum gas (LPG) vehicles were measured and speciated (particulate, oxidized, and elemental mercury). First, three different fuel types were analyzed for their original Hg contents; 571.1±4.5 ng L−1 for gasoline, 185.7±2.6 ng L−1 for diesel, and 1230.3±23.5 ng L−1 for LPG. All three vehicles were then tested at idling and driving modes. Hg in the exhaust gas was mostly in elemental form (Hg0), and no detectable levels of particulate (Hgp) or oxidized (Hg2+) mercury were measured. At idling modes, Hg concentrations in the exhaust gas of gasoline, diesel, and LPG vehicles were 1.5–9.1, 1.6–3.5, and 10.2–18.6 ng m−3, respectively. At driving modes, Hg concentrations were 3.8–16.8 ng m−3 (gasoline), 2.8–8.5 ng m−3 (diesel), and 20.0–26.9 ng m−3 (LPG). For all three vehicles, Hg concentrations at driving modes were higher than at idling modes. Furthermore, Hg emissions from LPG vehicle was highest of all three vehicle types tested, both at idling and driving modes, as expected from the fact that it had the highest original fuel Hg content.  相似文献   

9.
A few copper and gold smelters in Chile are behind a large fraction of global arsenic emissions, raising concerns for increased concentrations of arsenic in PM10 in Central and Northern Chile. This concern is amplified by the fact that Northern Chile soils and rivers in general are characterized by a high arsenic content. A monitoring and modeling study has been performed to quantify the regional impact of the smelter emissions. Measured atmospheric arsenic concentrations from 2.4 to 30.7 ng m−3 were found at seven rural stations, located tens to hundreds of kilometers away from the nearest smelter. Analyses of topsoil and subsoil samples taken from PM10 monitoring stations revealed levels up to 291 mg kg−1, the highest values found in the northern Atacama desert in Chile. An absolute principal component analysis of selected trace elements in PM10 shows that the regional impact of anthropogenic smelter emissions on airborne arsenic concentrations is more important than the effect of soil dust resuspension. The dominance of the smelter emissions is larger in Central Chile than in the northern parts. The impact of resuspended soil dust on airborne arsenic levels in rural areas was estimated not to exceed 5 ng m−3. The model calculations support the dominant role of anthropogenic emissions and give spatial and temporal variations in atmospheric concentrations consistent with the monitored levels at five of the seven stations. At two of the northernmost stations indications were found of unidentified sources other than the smelters and the resuspended soil dust, contributing to about 5 ng m−3 of total arsenic levels. The study confirms that a strong control or elimination of arsenic emissions from the smelters would lead to arsenic in PM10 levels in Northern and Central Chile comparable to non-polluted areas in other countries.  相似文献   

10.
Atmospheric concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) were measured in southeastern Korea during the spring of 2002. During this period, severe Asian dust events (ADs) occurred throughout Korea. Total suspended particulates (TSP) of ADs (456.8 μg m−3) increased approximately 3.6-fold compared with non-Asian dust events (NADs; 128.5 μg m−3). However, the concentrations of PCDD/Fs (average concentration, 3.34 pg m−3) did not increase as much as TSP; there was not a significant difference in the concentrations of particle-bound PCDD/Fs collected between ADs (2.45 pg m−3) and NADs (2.05 pg m−3). Meanwhile, according to TSP levels, the concentrations during NADs were 2.8-fold higher than ADs (16.73 and 5.98 ng g−1-TSP, respectively). High TSP levels during sand storms without an increase in PCDD/Fs reflected an increase in coarse and accumulation mode particles. Gas/particle partitioning studies revealed the additional inputs of particulate matters to the air during ADs which did not relate with the increase of PCDD/Fs. Furthermore, emissions from ADs may consist of relatively complex atmospheric particles; back trajectories showed air masses moving at low altitudes over Korea, but there were no differences in PCDD/Fs or atmospheric pollutants regardless of air movements. The study area, which is located in southeastern Korea, might be affected by both marine and regional anthropogenic sources, which do not appear to cause clear differences in PCDD/F concentrations or congener profiles between different air trajectories.  相似文献   

11.
《Chemosphere》2007,66(11):2477-2484
Atmospheric Hg transfer to the forest soil through litterfall was investigated in a primary rainforest at Ilha Grande (Southeast Brazil) from January to December 1997. Litter mass deposition reached 10.0 t ha−1 y−1, with leaves composing 50–84% of the total litter mass. Concentrations of Hg in the total fallen litter varied from 20 to 244 ng g−1, with higher concentrations during the dry season, between June and August (225 ± 17 ng g−1), and lower concentrations during the rainy season (99 ± 54 ng g−1). This seasonal variability was reflected in the Hg flux through litterfall, which corresponded to a Hg input to the forest floor of 122 μg m−2 y−1, with average Hg deposition of 16.5 ± 1.5 μg m−2 month−1 during and just after the dry season (June–September) and 7.0 ± 3.6 μg m−2 month−1 in the rest of the year. The variability in meteorological conditions (determining atmospheric Hg availability to foliar scavenging) may explain the pulsed pattern of Hg deposition, since litterfall temporal variability was generally unrelated with such deposition, except by a peak in litterfall production in September. Comparisons with regional data on Hg atmospheric deposition show that litterfall promotes Hg deposition at Ilha Grande two to three orders of magnitude higher than open rainfall deposition in non-industrialized areas and approximately two times higher than open rainfall deposition in industrialized areas in Rio de Janeiro State. The observed input suggests that atmospheric Hg transfer through litterfall may explain a larger fraction of the total Hg input to forest soils in Southeast Brazil than those recorded at higher latitudes.  相似文献   

12.
To investigate the characteristics of mercury exchange between soil and air in the heavily air-polluted area, total gaseous mercury (TGM) concentration in air and Hg exchange flux were measured in Wanshan Hg mining area (WMMA) in November, 2002 and July–August, 2004. The results showed that the average TGM concentrations in the ambient air (17.8–1101.8 ng m−3), average Hg emission flux (162–27827 ng m−2 h−1) and average Hg dry deposition flux (0–9434 ng m−2 h−1) in WMMA were 1–4 orders of magnitude higher than those in the background area. It is said that mercury-enriched soil is a significant Hg source of the atmosphere in WMMA. It was also found that widely distributed roasted cinnabar banks are net Hg sources of the atmosphere in WMMA. Relationships between mercury exchange flux and environmental parameters were investigated. The results indicated that the rate of mercury emission from soil could be accelerated by high total soil mercury concentration and solar irradiation. Whereas, highly elevated TGM concentrations in the ambient air can restrain Hg emission from soil and even lead to strongly atmospheric Hg deposition to soil surface. A great amount of gaseous mercury in the heavily polluted atmosphere may cycle between soil and air quickly and locally. Vegetation can inhibit mercury emission from soil and are important sinks of atmospheric mercury in heavily air-polluted area.  相似文献   

13.
Trace elements and metals in the ultrafine (<0.18 μm) and accumulation (0.18–2.5 μm) particulate matter (PM) modes were measured during the winter season, next to a busy Southern California freeway with significant (∼20%) diesel traffic. Both ambient and concentrated size-segregated impactor samples were taken in order to collect enough mass for chemical analysis. Data at this location were compared to a site located 1 mile downwind of the freeway, which was reflective of urban background. The most abundant trace elements in the accumulation mode detected by inductively coupled plasma mass spectroscopy (ICPMS) were S (138 ng m−3), Na (129 ng m−3), and Fe (89 ng m−3) while S (35 ng m−3) and Fe (35 ng m−3) were the most abundant in the ultrafine mode. The concentrations of several trace elements, including Mg, Al, and Zn, and in particular Ca, Cu, and Pb, did not uniformly increase with size within fine PM, an indication that various roadway sources exist for these elements. Calculation of crustal enrichment factors for the two sites indicates that the freeway traffic contributed to enriched levels of ultrafine Cu, Ba, P and Fe and possibly Ca. The results of this study show that trace elements constitute a small fraction of PM mass in the nanoparticle size range, but these can and should be characterized due to their likely importance to human health.  相似文献   

14.
15.
PM10 aerosols at McMurdo Station, Antarctica were sampled continuously during the austral summers of 1995–1996 and 1996–1997. PM10 (particles with aerodynamic diameters less than 10 μm) mass concentrations at Hut Point, located less than 1 km from downtown McMurdo, averaged 3.4 μg m−3, more than an order of magnitude lower than the USEPA annual average National Ambient Air Quality Standard (NAAQS) of 50 μg m−3. Concentrations of methanesulfonate and nitrate were similar to those measured at other Antarctic coastal sites. Non-sea-salt sulfate (NSS) concentrations on Ross Island were higher than those found at other coastal locations. The average elemental carbon concentration (129 ng m−3) downwind of the station was two orders of magnitude higher than those measured at remote coastal and inland Antarctic sites during summer. Average sulfur dioxide concentrations (746 ng m−3) were 3–44 times higher than those reported for coastal Antarctica. Concentrations of Pb and Zn were 17 and 46 times higher than those reported for the South Pole. A methanesulfonate to biogenic sulfate ratio (R) of 0.47 was derived that is consistent with the proposed temperature dependence of R.  相似文献   

16.
Five weeks of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle bound mercury (Hgp) concentrations as well as fluxes of GEM were measured at Maryhill, Ontario, Canada above a biosolids amended field. The study occurred during the autumn of 2004 (October–November) to capture the effects of cool weather conditions on the behaviour of mercury in the atmosphere. The initial concentration of total mercury (Hg) in the amended soil was relatively low (0.4 μg g−1±10%).A micrometeorological approach was used to infer the flux of GEM using a continuous two-level sampling system with inlets at 0.40 and 1.25 m above the soil surface to measure the GEM concentration gradient. The required turbulent transfer coefficients were derived from meteorological parameters measured on site. The average GEM flux over the study was 0.1±0.2 ng m−2 h−1(±one standard deviation). The highest averaged hourly GEM fluxes occurred when the averaged net radiation was highest, although the slight diurnal patterns observed were not statistically significant for the complete flux data series. GEM emission fluxes responded to various local events including the passage of a cold front when the flux increased to 2 ng m−2 h−1 and during a biosolids application event at an adjacent field when depositional fluxes peaked at −3 ng m−2 h−1. Three substantial rain events during the study kept the surface soil moisture near field capacity and only slightly increased the GEM flux. Average concentrations of RGM (2.3±3.0 pg m−3), Hgp (3.0±6.2 pg m−3) and GEM (1.8±0.2 ng m−3) remained relatively constant throughout the study except when specific local events resulted in elevated concentrations. The application of biosolids to an adjacent field produced large increases in Hgp (25.8 pg m−3) and RGM (21.7 pg m−3) concentrations only when the wind aligned to impact the experimental equipment. Harvest events (corn) in adjacent fields also corresponded to higher concentrations of GEM and Hgp but with no elevated peaks in RGM concentrations. Diurnal patterns were not statistically significant for RGM and Hgp at Maryhill.  相似文献   

17.
Higher plant waxes are the predominant natural components in the lipid fractions (> C15) of aerosols sampled over rural and oceanic regions. Hydrocarbon, fatty acid, ketone and fatty alcohol fractions of the lipids were characterized in terms of their contents of homologous compound series and specific biogenic molecular markers. Particulate samples from the rural western United States have been analyzed and compared with samples from urban Los Angeles and remote areas over the Atlantic Ocean. The samples from rural sites contained predominantly vascular plant wax and lesser amounts of higher plant sterols and resin residues. Urban samples and, to varying degrees, some rural samples contained primarily higher weight residues of petroleum products. The loadings of hydrocarbons derived from higher plant waxes ranged approximately from 10 to 160 ng m−3 of air (for fatty acids, 10–100 ng m−3 and for fatty alcohols, 10–200 ng m−3). Higher molecular weight lipids (i.e. plant epicuticular wax, terpenes, etc.) from flora comprise a significant component of the organic carbon in rural aerosols. Primary biogenic residues are major components of aerosols in all areas and they are important components in the global cycling of organic carbon.  相似文献   

18.
In order to assess the temporal variabilities of atmospheric mercury (Hg) from an area moderately impacted by man-made source processes, the concentrations of total gaseous mercury were measured routinely from an urban monitoring station during January 1999–August 2000. The mean hourly concentration of Hg from overall measurements was computed to be 5.26±3.27 ng m−3 (N=11, 572). Using these measurement data, we inspected various aspects on the temporal distribution of Hg. When analyzed over 24 h scale, the pattern was characterized by high concentration during nighttime relative to daytime (e.g., values approaching 9 ng m−3). This pattern was prominent during winter and seen persistently across fall, spring, and summer. When divided seasonally, the highest mean of 6.01 ng m−3 was observed during winter. It appears that such wintertime dominance is most likely to come from the anthropogenic sources such as household heating systems from late fall to early spring. A close inspection of the Hg data however indicated that the seasonal variation proceeded quite dynamically. Inspection of seasonally divided data groups generally showed substantial variabilities among different months. In order to analyze the factors affecting Hg distributions over different time scale, we conducted the correlation analysis. Whereas Hg generally exhibited strong correlations with such parameters as PM, SO2, and NO2, its relationship varied diurnally and seasonally. The overall results of the present study suggest that changes in its source signatures can vary over varying time scale under the influence of strong man-made source processes.  相似文献   

19.
Concentrations of size fractionated particulate sodium and potassium were measured in both marine and urban air. Marine air sampling was conducted during a cruise on R/V Hakuho-maru in the northwestern North Pacific in the summer of 1998. Urban air sampling was performed in the central part of Tokyo in 1997 and 1998. The fine sodium concentration (D<1.1 μm) in “Urban” air (180 ng m−3) was 3 times higher than that in “Marine” air (56 ng m−3). In the urban air samples, the size distributions of sodium and potassium showed bimodal peaks in the fine particle range (D<1.1 μm) and in the coarse particle range (D>1.1 μm). The existence of anthropogenic sodium in the fine particle range was detected in the urban air. The K/Na weight ratios in the fine particle range of the urban air (1.8–2.7) was 50–75 times higher than that in seawater (0.036). Potassium in the urban air is thought to be derived largely from anthropogenic sources. In the urban air samples, a high correlation between fine sodium and fine potassium concentrations suggests that they have the same anthropogenic source. Reevaluating the K/Na ratios in marine air to be relatively higher than that in seawater, we can estimate that several percents of anthropogenic sodium can be transported from land to remote marine air.  相似文献   

20.
Improvements in measurement technology are permitting development of a more detailed scientific understanding of the cycling of mercury in the global atmospheric environment. Critical to advancing the state of knowledge is the acquisition of accurate measurement of speciated mercury (gaseous and particulate) at ground research stations in a variety of settings located around the globe. This paper describes one such research effort conducted at TVA's Look Rock air quality monitoring site in Tennessee—a mountain top site (813 m elevation) just west of the Great Smoky Mountains National Park. The Great Smoky Mountains National Park is the largest National Park in the eastern US and it receives environmental protection under a variety of US statutes. Gaseous and particle mercury species along with some additional trace gases were measured at Look Rock during two field studies totaling 84 days in the spring and summer of 2004. Average results for the entire sampling period are: gaseous elemental mercury Hg(0): 1.65 ng m−3, reactive gaseous mercury RGM: 0.005 ng m−3, particulate mercury Hg(p): 0.007 ng m−3. Literature review indicates that these levels are within the range found for other rural/remote sites in North America and worldwide. Reactive and particulate mercury comprised together less than 1%, on average, of total airborne mercury at Look Rock. When compared to the global background mercury literature, the Look Rock measurements demonstrate that the atmospheric mercury levels in the vicinity of the Great Smoky Mountains National Park are clearly dominated by the global atmospheric pool, not by local or regional sources.  相似文献   

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