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1.
The relationships are considered between monthly and quarterly means of the fine particle sulfur (S) concentrations and wind flow direction, period of day and season of the year. The measurements used are those obtained at selected urban and at rural monitoring stations in the St Louis area during the Regional Air Pollution Study in 1975, 1976 and 1977. Higher mean fine particle S concentrations are observed with wind flows from the E compared to the W and from the NE and SE quadrants compared to the NW quadrant. Substantially higher fine particle S concentrations are obtained with wind flows from the E compared to the W even when conditions are selected so that the values of temperature, solar radiation intensity and wind speed are within the same restricted ranges. A consistent increase in the fine particle S concentrations occurs through the late morning and afternoon with decrease in the evening and especially in the early morning during spring and summer months with wind flows from the E.The contributions are estimated for local scale and regional scale processes to the observed fine particle S concentrations. Local scale processes include those involving atmospheric formation and primary emissions each contribute 0.6−1.0 and 0.6 μg m−3 of the fine particle S. Regional scale processes account for the greater part of the observed concentrations especially when the wind flows are from the SE or SW. Regional scale episodes involving passage of warm high pressure systems to the E of St Louis with accumulation of precursors made especially significant contributions to formation of fine particle S.The atmospheric gas phase and liquid phase chemical reactions contributing to the formation of fine particle S are discussed. Emphasis is placed on the effects of chemistry on the seasonal variations in concentrations of fine particle S.  相似文献   

2.
The relationships have been examined between the presence or absence of cumulus clouds and 3rd quarter fine particle sulfur concentrations in St Louis. An association between the presence of cumulus clouds with SO2 conversions in droplets and incrementally higher fine particle sulfur concentrations can be demonstrated. However, diurnal patterns of fine particle sulfur concentrations in the presence of cumulus clouds are not consistent with local contributions from sulfate formation in cumulus clouds. Morning fog often occurs on the same days on which cumulus clouds form later. Reactions of SO2 in fog droplets appear to make a contribution, but do not account for the major part of the increments in fine particle sulfur concentrations associated with cumulus clouds. The variations in fine particle sulfur concentrations observed can be explained if a substantial part of the sulfate formed in cumulus is transported upwards from the planetary boundary layer into the lower free troposphere. Subsequent multiday regional scale horizontal transport with concurrent gradual vertical transport of sulfate down to the surface would be consistent with the observed results.  相似文献   

3.
Airborne fine particle mass concentrations in Southern California have declined in recent years. Trends in sulfate and elemental carbon (EC) particle concentrations over the period 1982-1993 are consistent with this overall improvement in air quality and help to confirm some of the reasons for the changes that are seen. Fine particle sulfate concentrations have declined as a strict sulfur oxides (SOx) emission control program adopted in 1978 was implemented over time. Fine particle elemental (black) carbon concentrations have declined over a period when newer diesel engines and improved diesel fuels have been introduced into the vehicle fleet. Organic aerosol concentrations have not declined as rapidly as the EC particle concentrations, despite the fact that catalyst-equipped cars having lower particle emission rates were introduced into the vehicle fleet alongside the diesel engine improvements mentioned above. This situation is consistent with the growth in population and vehicle miles traveled in the air basin over time. Fine particle ammonium nitrate in the Los Angeles area atmosphere contributes more than half of the fine aerosol mass concentration on the highest concentration days of the year, emphasizing both the need for accurate aerosol nitrate measurements and the likely importance of deliberate control of aerosol nitrate as a part of any serious further fine particle control program for the Los Angeles area.  相似文献   

4.
During June, July and August 1981, General Motors Research Laboratories operated a comprehensive air-quality monitoring site in Detroit. Parameters monitored included the criteria pollutants, meteorological variables and the organic carbon, elemental carbon and sulfate content of the fine and coarse fractions of inhalable particulates (diameter ⩽ 15 μm). In addition, air parcel trajectories were used to compute the length of time air parcels spent in various upwind emission-source areas before arriving in Detroit. The data were analyzed using varimax-rotated principal component analysis. The results show that midwestern sources upwind of southeastern (SE) Michigan are responsible for most of the observed sulfate, which accounted for about 50% of the fine particle fraction. Significant amounts of ozone, particulate organic carbon and sulfur dioxide are also transported in from upwind sources. Local emissions dominate the concentrations of coarse particulate mass, elemental carbon, carbon monoxide and non-methane hydrocarbons. Important local sources exist for nitrogen oxides, sulfur dioxide and particulate organic carbon.  相似文献   

5.
Indoor fine particles: the role of terpene emissions from consumer products   总被引:1,自引:0,他引:1  
Consumer products can emit significant quantities of terpenes, which can react with ozone (O3). Resulting byproducts include compounds with low vapor pressures that contribute to the growth of secondary organic aerosols (SOAs). The focus of this study was to evaluate the potential for SOA growth, in the presence of O3, following the use of a lime-scented liquid air freshener, a pine-scented solid air freshener, a lemon-scented general-purpose cleaner, a wood floor cleaner, and a perfume. Two chamber experiments were performed for each of these five terpene-containing agents, one at an elevated O3 concentration and-the other at a lower O3 concentration. Particle number and mass concentrations increased and O3 concentrations decreased during each experiment. Experiments with terpene-based air fresheners produced the highest increases in particle number and mass concentrations. The results of this study clearly demonstrate that homogeneous reactions between O3 and terpenes from various consumer products can lead to increases in fine particle mass concentrations when these products are used indoors. Particle increases can occur during periods of elevated outdoor O3 concentrations or indoor O3 generation, coupled with elevated terpene releases. Human exposure to fine particles can be reduced by minimizing indoor terpene concentrations or O3 concentrations.  相似文献   

6.
The Canadian Acid Aerosol Measurement Program (CAAMP) was established in 1992 to gain a better understanding of the atmospheric behaviour of fine particle strong acidity (“acid aerosols”) and to facilitate an assessment of the potential health risks associated with acid aerosols and particles in general. During 1992. 1993 and 1994, annular denuder and filter measurements were taken at four sites in Ontario, two in Quebec, three in the Atlantic Provinces and one in the greater Vancouver area. Mean fine particle sulphate concentrations (SO42−) were highest in southern Ontario (annual average ranged from 40–70 nmol m−3), lowest at a site in the Vancouver area (average = 16 nmol m−3) and second lowest in rural Nova Scotia. However, mean fine particle strong acid concentrations (H+) were geographically different. The highest mean concentrations were at the east coast sites (annual average of up to 30 nmol m−3). Acidities were lower in areas where the fine particle acidity experienced greater neutralization from reaction with ammonia. This included the major urban centres (i.e. Toronto and Montréal) and areas with greater amounts of agricultural activity, as in rural southern Ontario. On average, ambient concentrations of fine and coarse particle mass were larger in the urban areas and also in areas where SO42− levels were higher. All the particle components were episodic. However, compared to SO42− and fine particles (PM2.5 or PM2.1, depending upon inlet design), episodes of H+ tended to be less frequent and of shorter duration, particularly in Ontario. Saint John, New Brunswick, had the highest mean annual H+ concentration, which was 30 nmol m−3. H+ episodes (24 h concentration > 100 nmol m−3) were also the most frequent at this location. The high levels in Saint John were partially due to local sulphur dioxide sources and heterogeneous chemistry occurring in fog, which, on average, led to a 50% enhancement in sulphate, relative to upwind conditions.There was a substantial amount of intersite correlation in the day to day variations in H+, SO42− , PM2.5 and PM10 (fine + coarse particles) concentrations, which is due to the influence of synoptic-scale meteorology and the relatively long atmospheric lifetime of fine particles. Sulphate was the most regionally homogenous species. Pearson correlation coefficients comparing SO42− between sites ranged from 0.6 to 0.9, depending on site separation and lag time. In many cases, particle episodes were observed to move across the entire eastern portion of Canada with about a two-day lag between the SO42− levels in southern Ontario and in southern Nova Scotia.  相似文献   

7.
An indoor air quality model was used to predict dynamic particle mass concentrations based on homogeneous chemical mechanisms and partitioning of semi-volatile products to particles. The ozone–limonene reaction mechanism was combined with gas-phase chemistry of common atmospheric organic and inorganic compounds and incorporated into the indoor air quality model. Experiments were conducted in an environmental chamber to investigate secondary particle formation resulting from ozone/limonene reactions. Experimental results indicate that significant fine particle growth occurs due to the interaction of ozone and limonene and subsequent intermediate by-products. Secondary particle mass concentrations were estimated from the measured particle size distribution. Predicted particle mass concentrations were in good agreement with experimental results—generally within ∼25% at steady-state conditions. Both experimental and predicted results suggest that air exchange rate plays a significant role in determining secondary fine particle levels in indoor environments. Secondary particle mass concentrations are predicted to increase substantially with lower air exchange rates, an interesting result given a continuing trend toward more energy efficient buildings. Lower air exchange rates also shifted the particle size distribution toward larger particle diameters. Secondary particle mass concentrations are also predicted to increase with higher outdoor ozone concentrations, higher outdoor particle concentrations, higher indoor limonene emission rates, and lower indoor temperatures.  相似文献   

8.
Fang GC  Chang CN  Wu YS  Wang V  Fu PP  Yang DG  Chen SC  Chu CC 《Chemosphere》2000,41(5):639-644
Daily average concentrations of fine and coarse particulates, and TSP samples have been measured simultaneously at daytime and night-time periods by using Universal and PS-1 sampler in a suburban area of central Taiwan from June to August 1998. The samples were analyzed by atomic absorption spectrometry to determine the fine and coarse particulate concentrations of metallic elements (Ca, Fe, Mn, Pb, Cu, Zn and Cr). The concentration of PM2.5 and TSP showed a decreased trend for the daytime period. The fine particle concentrations were about two times as that of coarse particulate concentrations. The averaged fine particulate concentrations at daytime are higher than at night-time. Ca and Fe were mostly in the coarse particulate mode. The correlation coefficients were 0.63 and 0.69 for elements Ca and Fe in the coarse particle mode for day and night periods. Pb showed a similar distribution ratio with Mn for the fine to coarse particle ratios at both day and night period. Pb and Mn are highly correlated for the day (R = 0.78) and night period (R = 0.61) at particle size <2.5 microm. Cu and Zn were mainly in fine particles at both day and night period. Fe and Ca consist of the major parts of all the elements. Elemental Mn is the lowest among the rest of the heavy metals.  相似文献   

9.
Dicarboxylic acid concentration trends and sampling artifacts   总被引:1,自引:0,他引:1  
Dicarboxylic acids associated with airborne particulate matter were measured during a summer period in Philadelphia that included multiple air pollution episodes. Samples were collected for two 10 h periods each day using a high-volume sampler with two quartz fiber filters in series, and analyzed by gas chromatography mass spectrometry (GCMS) with diazomethane derivatization. Among the dicarboxylic acids investigated, phthalic acid and adipic acid exhibited the greatest diurnal variations and the strongest linear relationship with maximum daily ozone concentration. Dicarboxylic acids and ozone concentration exhibited a poor linear relationship with organic to elemental carbon ratio. All species investigated were affected by significant sampling artifact errors at low concentrations, but sampling errors were negligible at high concentrations observed during ozone episodes.  相似文献   

10.
Continuous measurements of particle size distributions of 3-407 nm were collected from August 2002 to July 2004 at the Fresno Supersite to understand their number concentrations, size distributions, and formation processes. Measurements for fine particulate matter (PM2.5) mass, sulfate (SO4(2-)), nitrate (NO3-), black carbon (BC), particle-bound polycyclic aromatic hydrocarbons (PAHs), nitrogen oxides (NOx), carbon monoxide (CO), ozone (O3), and meteorological data (wind speed, wind direction, temperature [T], relative humidity [RH], and solar radiation) were used to determine the causes of nanoparticle (3-10 nm) and ultrafine (10-100 nm) particle events. These events were found to be divided into four types: (1) 3- to 10-nm morning nucleation; (2) 10- to 30-nm morning traffic; (3) 10- to 30-nm afternoon photochemical; and (4) 50- to 84-nm evening home heating, including residential wood combustion. Intense examples of the first type (>10(4) number [#]/cm3) were observed on 29 days, nearly always during the summer. The second type of event was observed on more than 73 days and occurred throughout the year. The third type was observed on 36 days, from spring through summer. The fourth type was found on 109 days, all of them during the winter. Although sulfur dioxide (SO2) emissions in Central California are low, the small residual amounts in gasoline and diesel fuel are apparently sufficient to initiate nucleation events. These were measured in the morning, soon after the shallow surface inversion coupled with layers aloft where nucleation probably was initiated. PM2.5 concentrations were poorly correlated with nanoparticle number.  相似文献   

11.
A method of analyzing spatial flow and precipitation patterns associated with long-range transport is presented. This technique uses hourly precipitation data and model-calculated mixed layer trajectories to determine these patterns upwind of a receptor site. Precipitation is determined at hourly points along trajectories in a statistical sense using estimates of error in long-range trajectory calculations. This technique is used in seasonal analyses of fine particle concentrations at a remote northern Great Plains sampling site during summer 1980. The analyses show that there are distinctly different flow and precipitation patterns during high and low fine particle concentration periods. Highest fine sulfur particle concentrations occurred when flow was from the south with a higher frequency of precipitation. Highest fine soil particle concentrations occurred when precipitation frequencies were lower.  相似文献   

12.
The impact of various atmospheric transport directions on ambient fine particle (PM2.5) concentrations at several sites in southeastern Canada was estimated (for May-September) using back-trajectory analysis. Three-day back trajectories (four per day) were paired with 6-hr average PM2.5 mass concentrations measured using tapered element oscillating microbalances (TEOM). PM2.5 concentrations at rural locations in the region were affected by nonlocal sources originating in both Canada and the United States. Comparison of sites revealed that, on average, the local contribution to total PM2.5 in the greater Toronto area (GTA) is approximately 30-35%. At each location, average PM2.5 concentrations under south/southwesterly flow conditions were 2-4 times higher than under the corresponding northerly flow conditions. The chemical composition of both urban and rural PM2.5 was determined during two separate 2-week spring/summer measurement campaigns. Components identified included SO4(2-) NO3-, NH4+, black carbon and organic carbon (OC), and trace elements. Higher particle mass at the urban Toronto site was composed of a higher proportion of all components. However, black carbon, NO3-, NaCl, and trace elements were found to be the most enriched over the rural/regional background levels.  相似文献   

13.
The Big Bend Regional Aerosol and Visibility Observational (BRAVO) field study was conducted from July to October 1999 and was followed by several years of modeling and data analyses to examine the causes of haze at Big Bend National Park TX (BBNP). During BRAVO, daily speciated fine (diameter <2.5 microm) particulate concentrations were measured at 37 sites throughout Texas. At the primary receptor site, K-Bar Ranch, there were many additional measurements including a "high-sensitivity" version of the 24-hr fine particulate elemental data. The spatial, temporal, and interspecies patterns in these data are examined here to qualitatively investigate source regions and source types influencing the fine particulate concentrations in Texas with an emphasis on sources of sulfates, the largest contributor to fine mass and light extinction. Peak values of particulate sulfur (S) varied spatially and seasonally. Maximum S was in Northeast Texas during the summer, whereas peak S at BBNP was in the fall. Sulfate acidity at BBNP also varied by month. Sources of Se were evident in Northeast Texas and from the Carbón I and II plants. High S episodes at BBNP during BRAVO had several different trace element characteristics. Carbon concentrations at BBNP during BRAVO were probably mostly urban-related, with arrival from the Houston area likely. The Houston artificial tracer released during the second half of BRAVO was highly correlated with some carbon fractions. There was evidence of the influence of African dust at sites throughout Texas during the summer. Patterns in several trace elements were also examined. Vanadium was associated with air masses from Mexico. Lead concentrations in southern Texas have dropped dramatically over the past several years.  相似文献   

14.
In this paper, the concept of scale analysis is applied to evaluate ozone predictions from two regional-scale air quality models. To this end, seasonal time series of observations and predictions from the RAMS3b/UAM-V and MM5/MAQSIP (SMRAQ) modeling systems for ozone were spectrally decomposed into fluctuations operating on the intra-day, diurnal, synoptic and longer-term time scales. Traditional model evaluation statistics are also presented to illustrate how the scale analysis approach can help improve our understanding of the models’ performance. The results indicate that UAM-V underestimates the total variance (energy) of the ozone time series when compared with observations, but shows a higher mean value than the observations. On the other hand, MAQSIP is able to better reproduce the average energy and mean concentration of the observations. However, both modeling systems do not capture the amount of variability present on the intra-day time scale primarily due to the grid resolution used in the models. For both modeling systems, the correlations between the predictions and observations are insignificant for the intra-day component, high for the diurnal component because of the inherent diurnal cycle but low for the amplitude of the diurnal component, and highest for the synoptic and baseline components. This better model performance on longer time scales suggests that current regional-scale models are most skillful in characterizing average patterns over extended periods, rather than in predicting concentrations at specific locations, during 1–2 day episodic events. In addition, we discuss the implications of these results to using the model-predicted daily maximum ozone concentrations in the regulatory framework in light of the uncertainties introduced by the models’ poor performance on the intra-day and diurnal time scales.  相似文献   

15.
Currently, we have limited knowledge of the physical and chemical properties of emitted primary combustion aerosols and the changes in those properties caused by nucleation, condensation growth of volatile species, and particle coagulations under dilution and cooling in the ambient air. A dilution chamber was deployed to sample exhaust from a pilot-scale furnace burning various fuels at a nominal heat input rate of 160 kW/h(-1) and 3% excess oxygen. The formation mechanisms of particles smaller than 420 nm in electrical mobility diameter were experimentally investigated by measurement with a Scanning Mobility Particle Sizer (SMPS) as a function of aging times, dilution air ratios, combustion exhaust temperatures, and fuel types. Particle formation in the dilution process is a complex mixture of nucleation, coagulation, and condensational growth, depending on the concentrations of available condensable species and solid or liquid particles (such as soot, ash) in combustion exhausts. The measured particle size distributions in number concentrations measured show peaks of particle number concentrations for medium sulfur bituminous coal, No. 6 fuel oil, and natural gas at 40-50 nm, 70-100 nm, and 15-25 nm, respectively. For No. 6 fuel oil and coal, the particle number concentration is constant in the range of a dilution air ratio of 50, but the number decreases as the dilution air ratio decreases to 10. However, for natural gas, the particle number concentration is higher at a dilution air ratio of 10 and decreases at dilution air ratios of 20-50. At a dilution air ratio of 10, severe particle coagulation occurs in a relatively short time. Samples taken at different combustion exhaust temperatures for these fuel types show higher particle number concentrations at 645 K than at 450 K. As the aging time of particles increases, the particles increase in size and the number concentrations decrease. The largest gradient of particle number distribution occurs within the first 10 sec after dilution but shows only minor differences between 10 and 80 sec. The lifetimes of the ultrafine particles are relatively short, with a scale on the order of a few seconds. Results from this study suggest that an aging time of 10 sec and a dilution air ratio of 20 are sufficient to obtain representative primary particle emission samples from stationary combustion sources.  相似文献   

16.
Continuous measurements of particle number concentrations were performed in Rochester, NY, and Toronto, Ontario, Canada during the 2003 calendar year. Strong seasonal dependency in particle number concentration was observed at two sites. The average number concentration of ambient particles was 9670 +/- 6960 cm(-3) in Rochester, whereas in Toronto the average number of particles was 28,010 +/- 13,350 cm(-3). The particle number concentrations were higher in winter months than in summer months by a factor of 1.5 in Rochester and 1.6 in Toronto. In general, there were also distinct diurnal variations of aerosol number concentration. The highest weekdays/weekends ratio of number concentration was typically observed during the rush-hour period in winter months with a ratio of 2.1 in Rochester and 2.0 in Toronto. The correlation in the total particle number concentrations between the two urban sites was stronger in winter because of the common urban traffic patterns, but weaker in summer because of local sulfur dioxide (SO2)-related particle formation events in Rochester in the summer. Strong morning particle formation events were frequently observed during colder winter months. Good correlations between particle number and carbon monoxide (CO) as well as temperature suggested that motorvehicle emissions lead to the formation of new particles as the exhaust mixes with the cold air. Regional nucleation and growth events frequently occurred in April. Local SO2-related particle formation events most frequently occurred in August. SO2 and UV-B were highly correlated with particle concentration, suggesting a high association of photochemical processes with these local events. A high directionality in a northerly direction was observed for particle number and SO2, indicating the influence of point sources located north of Rochester.  相似文献   

17.
Atmospheric aerosols were measured in August 1983 on Allegheny Mountain and Laurel Hill in southwestern Pennsylvania. Ambient humidity was observed to influence the coarse to fine particle ratios as determined by dichotomous samplers. This influence is evident in the particle mass and in its component chemical species. The sampling run with the most pronounced mass shift resulted in an apparent loss of 50 % of the fine mass and 66 % of the fine particle sulfur to the coarse fraction. The magnitude of the mass shift appears to be related to the length of time that the aerosol was in a saturated environment and also to the original dry particle size. These observations have serious implications for receptor modeling with dichotomous sampler data whenever only the fine particles are considered.  相似文献   

18.
A high volume electrostatic field-sampler was developed for collection of fine particles, which easily can be recovered for subsequent sample characterisation and bioassays. The sampler was based on a commercial office air cleaner and consisted of a prefilter followed by electrostatic collection plates operating at 2.7 kV. The sampler performance was characterised for 26 nm to 5.4 μm-size particles in urban street air. The collection efficiency reached a maximum (60–70%) between 0.2 and 0.8 μm and dropped to ∼25% at 30 nm and 2.5 μm, respectively. After extraction in water, the particle loss was<2%. The extraction efficiency for dry lyophilised particulate matter was above 80%, allowing retrievement of ∼12 mg day−1 in urban street air at PM10 levels of ∼24 μg m−3. The ozone generating capacity of the corona discharge during operation was on the order of 10 ppb. A polycyclic aromatic hydrocarbons (PAH) degradation test using benzo[a]pyrene as a model showed that ∼85% was degraded after 24 h. However, similar results were observed when the corona discharge was switched off. Hence, the ozone and other corona discharge reactants do not appear to contribute considerably to PAH-degradation. The overall results show that the sampler type is a promising alternative to traditional sampling of fine particles for bulk analysis and bioassays. The main advantages are simple operation, high stability, high quantifiable particle recovery rates and low cost.  相似文献   

19.
In order to contribute to current knowledge of ozone concentrations and transport across the Central Massif, a monitoring station was installed at 1780 m on the upper Spanish plateau about 55 km from the city of Madrid. Ozone concentrations and standard meteorological variables were measured in June and July 2002. A smoothed ozone hourly cycle was obtained with mean values of 120 and 110 microgm(-3) during day-time and night-time, respectively. The highest ozone concentrations were recorded in the SE-S-SW wind sectors, proving the influence of transport from the Madrid urban plume to the upper plateau. This assumption was also supported by the satisfactory correlation between ozone peaks obtained at the monitoring site and those recorded in a representative station on the foothill located on the lower plateau during episodic situations. To assess the contribution of long-range transport, backward air mass trajectories were computed each day of measurements at 820 hPa. The lowest ozone mean was linked to Atlantic Ocean air masses, and the highest to air masses from Central Europe.  相似文献   

20.
Under the National Ambient Air Quality Standards (NAAQS), put in place as a result of the Clean Air Amendments of 1990, three regions in the state of Utah are in violation of the NAAQS for PM10 and PM2.5 (Salt Lake County, Ogden City, and Utah County). These regions are susceptible to strong inversions that can persist for days to weeks. This meteorology, coupled with the metropolitan nature of these regions, contributes to its violation of the NAAQS for PM during the winter. During January–February 2009, 1-hr averaged concentrations of PM10-2.5, PM2.5, NOx, NO2, NO, O3, CO, and NH3 were measured. Particulate-phase nitrate, nitrite, and sulfate and gas-phase HONO, HNO3, and SO2 were also measured on a 1-hr average basis. The results indicate that ammonium nitrate averages 40% of the total PM2.5 mass in the absence of inversions and up to 69% during strong inversions. Also, the formation of ammonium nitrate is nitric acid limited. Overall, the lower boundary layer in the Salt Lake Valley appears to be oxidant and volatile organic carbon (VOC) limited with respect to ozone formation. The most effective way to reduce ammonium nitrate secondary particle formation during the inversions period is to reduce NOx emissions. However, a decrease in NOx will increase ozone concentrations. A better definition of the complete ozone isopleths would better inform this decision.

Implications: Monitoring of air pollution constituents in Salt Lake City, UT, during periods in which PM2.5 concentrations exceeded the NAAQS, reveals that secondary aerosol formation for this region is NOx limited. Therefore, NOx emissions should be targeted in order to reduce secondary particle formation and PM2.5. Data also indicate that the highest concentrations of sulfur dioxide are associated with winds from the north-northwest, the location of several small refineries.  相似文献   


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