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1.
We use the global mercury model published by Bergan et al. (1999) to evaluate the potential role of ozone and the hydroxyl radical as gas phase oxidants for the oxidation of elemental mercury in the atmosphere. The magnitude of natural and man-made mercury emissions are taken from recent literature estimates. We consider only two mercury reservoirs, elemental mercury, Hg0, and the more soluble divalent form, HgII. Wet and dry deposition of HgII is explicitly treated.Applying monthly mean fields of ozone for the oxidation of gas phase Hg0 and using the reaction rate by Hall (1995) yields a global transformation of Hg0 to HgII which is too slow to keep the simulated concentration of Hg0 near observed values. This shows that there must be additional important removal processes for Hg0 or that the reaction rate proposed by Hall (1995) is too slow. A simulation in which the oxidation rate was artificially increased, so that the global turn-over time of Hg0 is one year and the simulated average concentration of Hg0 realistic, produces latitudinal and seasonal variations in Hg0 that do not support the hypothesis that gas phase reaction with O3 is the major oxidation process for Hg0.Recent studies indicate that OH may be an important gas phase oxidant for Hg0 (Sommar et al., 2001). Using OH as the sole oxidantand applying the oxidation rate by Sommar et al., we calculate aconcentration of Hg0 well below (about a factor of three) the observations. By prescribing a slower rate, corresponding to a turn-over time of Hg0 of one year, we calculate concentrations of both Hg0 in surface air and HgII in precipitation which correspond reasonably well, both in magnitude and temporal variation, with seasonal observations in Europe and North America. This result supports the suggestion that the oxidation by OH is an important pathway for the removal of Hg0. In view of the uncertainties associated with our calculations, this conclusion should still be regarded as tentative.  相似文献   

2.
During the spring of 2005, the total particle concentrations and the submicron aerosol size distributions were measured on board the research vessel over the south sea of Korea and the Korean sector of the Yellow Sea. Similar measurements were made over the East China Sea in autumn 2005. The aerosol properties varied dynamically according to the meteorological conditions, the proximity to the land masses and the air mass back trajectories. The average total particle concentration was the lowest over the East China Sea, 4335 ± 2736 cm 3, but the instantaneous minimum, 837 cm 3, for the entire ship measurement was recorded during the Yellow Sea cruise. There was also a long (more than 6 h) stretch of low total particle concentrations that fell as low as 1025 cm 3 during the East China Sea cruise when the ship was the farthest from the shores and the air mass back trajectories resided long hours over the sea. These observations lead to the suggestion of ~ 1000 cm 3 as the background total particle concentration over the marine boundary layer in the studied region of the Yellow Sea and the East China Sea, implying significant anthropogenic influence even for the background value. In the mean time, average aerosol size distributions were unimodal and the mode diameter ranged between 52 and 86 nm, excluding the fog periods, which suggests that the aerosols measured in this study experienced relatively less aging processes within the marine boundary layer.  相似文献   

3.
Presented are the results of mercury content measurements in the surface air layer in the Sea of Japan in the period from October 27 to November 11, 2010. It is revealed that the mercury content varied from 0.6 to 3.8 ng/m3. It is demonstrated that the mercury concentration distribution has geographical zoning and depends on the movement of air masses and on the closeness of anthropogenic sources. The maximum mercury concentration is detected in the central part of the sea at the southwestern and southern directions of the wind, that is associated with the industrial emissions of East Asia countries. The minimum mercury concentration corresponding to the concentration in the surface air layer of the Arctic, Atlantic Ocean (Northern Hemisphere), and the Sea of Okhotsk and Bering Sea was observed along the coast of Primorye at the northwestern wind direction.  相似文献   

4.
Measurements of carbon dioxide (CO2) concentration were made at a coastal land station, Goa, on the west coast of India from March to June 2003 as part of the ARMEX (ARabian sea Monsoon Experiment) campaign. The observations show a systematic reduction (~120?mg?m?3) of CO2 concentration during the pre-monsoon months, March–May, during which no significant change in anthropogenic emissions takes place. CO2 shoots up from 520 to 635?mg?m?3 in June with the onset of the South West monsoon. Back trajectories show that the source of air mass gradually shifts from the coastal land mass to the open southern Arabian Sea during the pre-monsoon period. The observed reduction in CO2 is explained in terms of earlier measurements in the Arabian Sea indicating maximum chlorophyll a (Sarupria and Bhargava in J Mar Sci 27:292–297, 1998) and minimum partial pressure of CO2 (Sarma in J Geophys Res 108:3225, 2003) in the sea waters off the west coast of India during the pre-monsoon period, cleaner marine air mass advection from the open sea, and negligible local vertical CO2 flux.  相似文献   

5.
Recent field investigations in polar regions, and over the ocean, have suggested that elemental mercury (Hg0) can be photochemically oxidized in the presence of reactive halogen species that are formed in the presence of salt particles, typically through a reactive catalytic cycle involving ozone destruction. Furthermore, these studies have suggested that the Hg0 oxidation reaction involves the reaction with reactive bromine species such as Br, BrO, and Br2. To investigate these reactions in more detail, we performed experiments using a quartz reactive chamber so that the oxidation of Hg0, and the formation of ionic Hg products, could be examined in detail under different reaction scenarios, but at realistic levels of Hg. To examine if the reactions were enhanced by the presence of deliquescent salt surfaces, as has been postulated to be the case for the formation of reactive halogens, one surface of the cell was coated with either NaCl or NaBr for some experiments. In addition to laboratory experiments with a Xenon lamp, outdoor experiments under natural light were also conducted. The results of these studies showed that oxidation of Hg0 did not occur in the dark, except in the presence of a deliquescent NaBr salt surface. The rate of oxidation was slow in the absence of salt surfaces, and in the absence of low wavelength light (<324 nm). In the presence of NaCl surfaces, oxidation rates were at least two orders of magnitude faster, but the rate was further increased in the presence of NaBr, by a further factor of 25. With outdoor light, while the rates of oxidation were lower, the results were similar overall. The results are discussed in terms of the reactions occurring and the mechanisms of Hg0 oxidation. Finally, the implications of these reactions to the overall global Hg cycle are discussed.  相似文献   

6.
Dimethylsulfide (DMS) in surface seawater and the air, methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2–) in aerosol, and radon-222 (Rn-222) were measured in the northern North Pacific, including the Bering Sea, during summer (13 July – 6 September 1997). The mean atmospheric DMS concentrations in the eastern region (21.0 ± 5.8 nmole/m3 (mean ± S.D.), n=30) and Bering Sea (19.9 ± 9.8 nmole/m3, n=10) were higher than that in the western region (11.1 ± 6.4 nmole/m3, n=31) (p<0.05), although these regions did not significantly differ in the mean DMS concentration in surface seawater. Mean sea-to-air DMS flux in the eastern region (21.0 ± 10.4 mole/m2/day, n=19) was larger than those in the western region (11.3 ± 16.9 mole /m2/day, n=22) and Bering Sea (11.2 ± 7.8 mole/m2/day, n=7) (p<0.05). This suggests that the longitudinal difference in atmospheric DMS was produced by that in DMS flux owing to wind speed, while the possible causes of the higher DMS concentrations in the Bering Sea include (1) later DMS oxidation rates, (2) lower heights of the marine boundary layer, and (3) more inactive convection. The mean MSA concentrations in the eastern region (1.18 ± 0.84 nmole/m3, n=35) and Bering Sea (1.17 ± 0.87 nmole/m3, n=13) were higher than that in the western region (0.49 ± 0.25 nmole/m3, n=28) (p < 0.05). Thus the distribution of MSA was similar to that of DMS, while the nss-SO4 2– concentrations were higher near the continent. This suggests that nss-SO4 2– concentrations were regionally influenced by anthropogenic sulfur input, because the distribution of nss-SO4 2– was similar to that of Rn-222 used as a tracer of continental air masses.  相似文献   

7.
This paper presents samples of Saharan dust outbreak affecting the Mediterranean Tunisian coasts and its impact on PM10 (Particles with an aerodynamic diameter below 10 µm) surface concentrations measured at seven monitoring stations during summer 2006. During the events, the daily PM10 levels at all stations exceeded EU and Tunisian air quality standard limits which are equal to 50 µg/m3. The maximum values ranged from 200 µg/m3 to 300 µg/m3 depending on the monitoring station. The impact is even more dramatic on PM10 hourly concentrations leading to maximum hourly peaks ranging from 400 µg/m3 to 850 µg/m3 again depending on the monitoring station (industrial or residential, traffic and commercial). Comparison between backward air masses trajectories reaching Tunisian coasts and satellite imageries vis-à-vis the PM10 hourly concentrations measured at the monitoring stations during 2006 evidenced the influence of the Saharan dust outbreaks on surface concentrations. The origin of the air masses is found to be from South-West direction under the influence of air masses from the Algerian Saharan desert.  相似文献   

8.
The sorption studies of Hg2+, CH3Hg+ and elemental mercury (Hg0) were carried out on lichen (Parmelia sulcata) and moss (Funaria hygrometrica) samples under laboratory conditions. Desorption studies with HCl indicate that inorganic mercury (Hg+2) and methyl mercury could be completely desorbed with 1 M HCl and 0.5 M HCl, respectively. Samples loaded with elemental mercury, however, needed 4–5 M HCl concentration for complete desorption of the adsorbed elemental mercury. When similar desorption studies were carried out with field samples collected around a thermometer factory with elevated levels of mercury (8 mg/kg), it was found that only about 10–15% of total mercury was desorbed with 1M HCl, while 4–5 M acid was required for complete desorption. We have tried to correlate this information to understand the transformations of mercury species that may occur either in the atmosphere or on the biomonitors. The results indicated that the elemental mercury, the principal form of mercury contamination around the thermometer factory, is converted into a strongly held form by some chemical binding agents on the surface of lichen/moss, or elemental mercury could diffuse into the cells of the lichen/moss, which then needs the stronger acid to release it. Sorption capacity studies suggest that the lichens and mosses can also be used as sorbent material for the decontamination of inorganic and methyl mercury from aqueous solutions.  相似文献   

9.
The potential resources on the ion-stimulated syntheses effects of aerosol particles of lower troposphere in test sites in the arctic, mountain, arid and forest areas as the function of irradiation time and gas-precursor concentration were experimentally and theoretically evaluated. The dust-free outdoor air was irradiated with an ionization current of 10− 6 A by α-rays from isotope 239Pu. The total output of radiolytic aerosols (RA) with a diameter of 3–1000 nm was found to be 0.05–0.1 molecules per 1 eV of absorbed radiation, while the physical upper limit is 0.25–0.4 molecules/eV. In an interval of exposition time from 6 to 800 s (adsorbed energy is 3 · 1012–1014 eV/cm3) the RA mass concentration at different sites was increased from 1–10 to 50–500 μg/m3. According to the liquid chromatography data the major RA material is the H2O/HNO3 solution with acid concentration  25%. The used physical model presents new aerosols as a product from small and intermediate ion association through formation of neutral clusters and describes adequately some of the peculiarities in field experiment data. Introducing SO2, NH3, and also hydrochloric, nitric and sulphuric acid vapours with concentration 0.1–1 mg/m3 in the irradiated air stimulated an increase of mass aerosol concentration by a factor of 8–30. The mean size also decreased by a factor of 3–5. These facts allowed us to expect that the chemical composition of radiolytic aerosols generated in outdoor air would noticeably differ after addition of the gas-precursors.  相似文献   

10.
Currents and atmospheric parameters were measured in the East China Sea in February, 1975, as part of the AMTEX'75 program. These data were used to describe outbreaks of cold continental air over this warm and shallow sea. Particular emphasis was placed on describing the structure of mesoscale atmospheric cells embedded in the outbreaks and the effects of these cells on the water column.Two cold air outbreaks were recorded. Heat fluxes (latent plus sensible) as high as 1270 cal/cm2 day were calculated. Evidence of mesoscale atmospheric cells was found during outbreaks in satellite imagery and in solarimeter data. The development of mesoscale cells was described by correlating fluctuations in the air temperature and absolute humidity records. The cells were found to be best developed when satellite imagery showed that they were of the closed variety. The data suggest that cellular activity matures from open to closed cell types.During the period of greatest development, a representative closed cell was 24–30 km in diameter, moved at 8 m s-1 over the spar buoy, had a temperature fluctuation of 0.4 °C, an absolute humidity fluctuation of 0.4 g kg-1, and wind speed and heat flux fluctuations of - 12.5%.A non-dimensional index, formed from the fluctuations of the air temperature and absolute humidity records, was used to indicate the passage of mesoscale atmospheric cells over the measuring site. Using this index as input and the fluctuations in the oceanic parameters at a depth of 20 m as output, it was found that the passage of mature cells was significantly correlated with temperature fluctuations and current fluctuations aligned 25 ° to the right of the wind about 45 min later.  相似文献   

11.
Radon daughters are produced as free ions, but they become attached to aerosol particles at a rate depending on the particle concentration. In the lower marine boundary layer, most of those which do not become attached plate out on the ocean surface. In this paper a simple model is used to examine the influence of several parameters on radon/radon daughter disequilibria in maritime air. The model is compared with experimental data from Cape Grim.The radon daughter to radon ratio, f, decreases from 0.86 to 0.1 as the particle concentration falls from 1000 to 10 cm-3. Estimates of radon concentration at sea level, based on daughter measurements may therefore be in error by as much as a factor of 10 unless allowance is made for particle concentration. At 100 cm-3, the standard deviation of the distribution of measured f values is about 30%, indicating that the particle concentration is not the only factor influencing the loss of radon daughters. The implication is that radon daughters can be used to measure radon concentrations at sea level with an accuracy of about 30%, provided the particle concentration is known.The measurements show that there is a very low proportion of unattached daughers in the air between about 30 and 165 m above sea level. According to the model, this implies that mixing of air up to about 200 m is usually rapid enough to result in plate-out of radon daughters on the ocean on a time scale of less than 100 s.  相似文献   

12.
This paper examines the potential for the use of artificial neural networks (ANNs) to estimate the reference crop evapotranspiration (ET0) based on air temperature data under humid subtropical conditions on the southern coast of the Caspian Sea situated in the north of Iran. The input variables for the networks were the maximum and minimum air temperature and extraterrestrial radiation. The temperature data were obtained from eight meteorological stations with a range of latitude, longitude, and elevation throughout the study area. A comparison of the estimates provided by the ANNs and by Hargreaves equation was also conducted. The FAO-56 Penman–Monteith model was used as a reference model for assessing the performance of the two approaches. The results of this study showed that ANNs using air temperature data successfully estimated the daily ET0 and that the ANNs with an R 2 of 0.95 and a root mean square error (RMSE) of 0.41 mm day?1 simulated ET0 better than the Hargreaves equation, which had an R 2 of 0.91 and a RMSE of 0.51 mm day?1.  相似文献   

13.
A heavy rainfall event during the period from 30th of March to 2nd of April 2009 has been studied using upper air and surface data as well as NOAA HYSPLIT model. This observational study attempts to determine factors responsible for the occurrence of heavy rainfall over Iran induced by Mediterranean cyclone, a western severe sub-tropical storm that made rainfall on most regions of the country. On the surface chart, cyclones, anticyclones and weather fronts were identified. The positions of the cold and warm fronts, which extended from a two-core low pressure center, were quite in good agreements with directions of winds i.e., westerly, southerly and easterly flows as well as the regions of precipitation. The heavy rain event occurred due to a Mediterranean cyclone’s activity over the study area, while other conditions were also responsible for this event such as an unstable atmosphere condition with abundant low-level moisture, which the warm and moist air parcels were brought by the southwesterly low-level jet into the country from Persian Gulf, Oman Sea, Indian Ocean and Caspian Sea at lower levels as well as Mediterranean Sea, Red Sea and Persian Gulf at upper levels over the examined period. A strong low-level convergence zone was observed along the wind-shift line between the southwesterly flow because of the low-level jet and the northeasterly flow due to the Russian high pressure. The amount of precipitable water varied between 20 and 24 kg m?2, surface moisture convergence exceeded 2.5 g kg?1 s?1 and the highest CAPE value in the sounding profiles was observed in Birjand site with 921 J kg?1 during the study period. The HYSPLIT model outputs confirmed the observed synoptic features for the examined system over the country.  相似文献   

14.
Emissions of marine biogenic sulfur to the atmosphere of northern Europe   总被引:1,自引:0,他引:1  
Measurements of DMS and other reduced sulfur compounds in surface waters have been carried out from a helicopter in the seas surrounding Scandinavia. Average summer time concentrations of DMS ranged from 70 to 150 ngS L-1. Simultaneous measurements of biological and physical parameters revealed no correlation between DMS and phytoplankton species, species assemblages, total phytoplankton biomass, chlorophyll a, temperature, and salinity. The only exception was a correlation between DMS concentration, Chrysochromulina spp. belonging to the Prymnesiophyceae, and salinity over a narrow range of salinity in the Baltic Sea.The flux of reduced sulfur to the atmosphere in July in this region is estimated to be 120–170 gS m-2 d-1 from the Baltic, 240–810 in the Kattegat/Skagerrak, and 120–690 in the North Sea. Annual fluxes are roughly 100 times higher than these daily fluxes. On an annual basis, biogenic sulfur emissions from the coastal seas are negligible (<1%) compared to the anthropogenic emissions in northern Europe. However, during the summer months, the biogenic sulfur emissions from the seas surrounding the Scandinavian peninsula are estimated to be as high as 20–70% of the anthropogenic emissions in Scandinavia. This makes it of interest to incorporate the biogenic emissions in calculations of long-range transport and deposition of sulfur within the region.Other volatile sulfur species, mainly methyl mercaptan, contribute about 10% of the total flux of reduced sulfur. Estimated fluxes of CS2 to the atmosphere ranged from 1 gS m-2 d-1 in the Baltic Sea to 6 gS m-2 d-1 in the North Sea. No emissions for H2S or COS were detected.  相似文献   

15.
Synoptic conditions of extreme rainwater pollution episodes, evidenced by maximum values of parameters measured in the protected area of Wielkopolski National Park (western-central Poland), were analysed in this study. Precipitation samples were tested for the following parameters: pH, electrical conductivity and the concentration of the following elements: F-, Cl-, NO2-, NO3-, PO43-, SO42- and Na+, NH4+, K+, Mg2+, Ca2+. It was assumed, that in winter, western advection of Atlantic air masses was the most frequent aerosol and pollution transport scenario for the investigated area. In summer the most heavily pollution occur at the intensified meridional flow over the central Europe, indicating advection of cooler air from northern Europe and the North Sea. In most of cases, the weather conditions causing extreme concentration of examined pollutants, were determined by the movement of weather fronts over considerable parts of Poland and by precipitation caused by those fronts.  相似文献   

16.
In situ aircraft measurements of O3, CO,HNO3, and aerosol particles are presented,performed over the North Sea region in the summerlower stratosphere during the STREAM II campaign(Stratosphere Troposphere Experiments by AircraftMeasurements) in July 1994. Occasionally, high COconcentrations of 200-300 pbbv were measured in thelowermost stratosphere, together with relatively highHNO3 concentrations up to 1.6 ppbv. The particlenumber concentration (at standard pressure andtemperature) between 0.018-1 m decreased acrossthe tropopause, from >1000 cm-3 in the uppertroposphere to <500 cm-3 in the lowermoststratosphere. Since the CO sources are found in thetroposphere, the elevated CO mixing ratios areattributed to mixing of polluted tropospheric air intothe lowermost extratropical stratosphere. Further wehave used a chemical model to illustrate that nitrogenoxide reservoir species (mainly HNO3) determinethe availability of NOx (=NO + NO2) andtherefore largely control the total net O3production in the lower kilometers of thestratosphere. Model simulations, applying additionalNOx perturbations from aircraft, show that theO3 production efficiency of NOx is smallerthan previously assumed, under conditions withrelatively high HNO3 mixing ratios, as observedduring STREAM II. The model simulations furthersuggest a relatively high O3 productionefficiency from CO oxidation, as a result of therelatively high ambient HNO3 and NOxconcentrations, implying that upward transport of COrich air enhances O3 production in the lowermoststratosphere. Analysis of the measurements and themodel calculations suggest that the lowermoststratosphere is a transition region in which thechemistry deviates from both the upper troposphere andlower stratosphere.  相似文献   

17.
The main objective of this study is to investigate the chemical characteristics of biomass burning aerosol and its impact on regional air quality during an agricultural waste burning period in early summer in the rural areas of Korea. A 12-h integrated intensive sampling of biomass burning aerosol in the fine and coarse modes was conducted on 2–20 June 2003 in Gwangju, Korea. The collected samples were analyzed for concentrations of mass, ionic, elemental, and carbonaceous species. Average concentrations of fine and coarse mass were measured to be 67.9 and 18.7 μg m− 3 during the biomass burning period, 41.9 and 18.8 μg m− 3 during the haze period, and 35.6 and 13.3 μg m− 3 during the normal period, respectively. An exceptionally high PM2.5 concentration of 110.3 μg m− 3 with a PM2.5/PM10 ratio of 0.79 was observed on 6 June 2003 during the biomass burning period. The potassium ratio method was used to identify biomass burning samples. The average ratio of potassium in the fine mode to the coarse mode (FK/CK) was 23.8 during the biomass burning period, 6.0 during the haze period, and 4.7 during the normal period, respectively. A FK/CK ratio above 9.2 was considered a criterion for biomass burning event in this study. Particulate matter from the open field burning of agricultural waste has an adverse impact on visibility, human health, and regional air quality.  相似文献   

18.
The concentrations of DMS were simultaneously measured in both water and air at the sea surface on board a vessel during a trans-Pacific cruise around 40° N in August 1988. Those in the surface seawater varied widely with a mean of 162 ng S/1 and a standard deviation of 134 ng S/1 (n=37), but the variation was not a mere fluctuation and the high concentration (376 ng S/1) was found in the area between 145° W and 170° W. The atmospheric DMS concentration varied more widely with a mean value of 177 ng S/m3 and a standard deviation of 203 ng S/m3 (n=23). The diurnal variation of DMS was not significant in the air near the sea surface. However, the concentrations in the surface water was fairly well correlated with those in the surface air. The correlation coefficient (r 2=0.86) was larger than that between the atmospheric concentration and outflux of DMS (r 2=0.64). These findings mean that the turnover time of DMS in the atmosphere is not extremely short. Based on the linear relation between the atmospheric and seawater DMS, the turnover time of the atmospheric DMS has been calculated to be 0.9 days with an uncertainty of around 50%. The oxidation rate agrees fairly well with that expected from the OH radical concentration in the marine atmosphere.  相似文献   

19.
Ambient particulate sulfate measurements have been intermittently performed at a rural site in Israel over a period of more than two years. Concurrent measurements of ambient pollutants (SO2, NO–NOx, and O3), as well as meteorological data, were also carried out. The daily data included four particulate sulfate samples representing four successive 6 h accumulating periods. The measured concentrations of sulfate ions ranged from a low 2 g m-3 observed during the winter season to a high of >50 g m-3 obtained during the summer. Little correlation was obtained between the sulfate concentration and either O3 or SO2, although sulfate and O3 showed a similar diurnal and annual trend. Based on the data distribution and on a photochemical model, it was concluded that a large part of the particulate sulfate observed at the eastern coast of the Mediterranean Sea must be related to long-range transport from distant sources.  相似文献   

20.
PM10 samples were collected over three years at Monzenmachi, the Japan Sea coast, the Noto Peninsula, Ishikawa, Japan from January 17, 2001 to December 18, 2003, using a high volume air sampler with quartz filters. The concentrations of the water-soluble inorganic ions in PM10 were determined with using ion chromatography. By analyzing the characteristics of these, the evidences were found that the Asian outflow had an obviously influence on the air quality at our study site. The results were as follows: the secondary pollutants SO42−, NO3 and NH4+ were the primary water-soluble inorganic ions at our study site. The monthly mean concentrations of SO42−, NH4+, NO3 and Ca2+ have prominent peak in spring due to the strong influence of the Asian continent outflow—these according to backward air trajectory analysis, the maximum of which were 6.09 for nss-SO42− in May, 2.87 for NO3 and 0.68 μg m−3 for nss-Ca2+ in April, respectively. Comparable to similar data reported from various points around East Asia, it had the characteristics of a polluted coastal area at our study site. The concentration of nss-Ca2+ in PM10 drastically increased when the Asian dust invaded, the mean value during the Asian dust days(AD) was 0.86 μg m−3, about 4 times higher than those of normal days (NAD). Meanwhile, the mean concentrations of nss-SO42−, NO3 and NH4+ in AD periods were higher than those in NAD periods which were 5.87, 1.76 and 1.82 μg m−3, respectively, it is due to the interaction between dust and secondary particles during the long-range transport of dust storms. Finally, according to the source apportionment with positive matrix factorization (PMF) method in this study, the major source profiles of PM10 at our study site were categorized as (1) marine salt, (2) secondary sulfate, (3) secondary nitrate and (4) crustal source.  相似文献   

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