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1.
A three dimensional chemical transport model (PMCAMx) is applied to the Mexico City Metropolitan Area (MCMA) in order to simulate the chemical composition and mass of the major PM1 (fine) and PM1–10 (coarse) inorganic components and determine the effect of mineral dust on their formation. The aerosol thermodynamic model ISORROPIA-II is used to explicitly simulate the effect of Ca, Mg, and K from dust on semi-volatile partitioning and water uptake. The hybrid approach is applied to simulate the inorganic components, assuming that the smallest particles are in thermodynamic equilibrium, while describing the mass transfer to and from the larger ones. The official MCMA 2004 emissions inventory with improved dust and NaCl emissions is used. The comparison between the model predictions and measurements during a week of April of 2003 at Centro Nacional de Investigacion y Capacitacion Ambiental (CENICA) “Supersite” shows that the model reproduces reasonably well the fine mode composition and its diurnal variation. Sulfate predicted levels are relatively uniform in the area (approximately 3 μg m?3), while ammonium nitrate peaks in Mexico City (approximately 7 μg m?3) and its concentration rapidly decreases due to dilution and evaporation away from the urban area. In areas of high dust concentrations, the associated alkalinity is predicted to increase the concentration of nitrate, chloride and ammonium in the coarse mode by up to 2 μg m?3 (a factor of 10), 0.4 μg m?3, and 0.6 μg m?3 (75%), respectively. The predicted ammonium nitrate levels inside Mexico City for this period are sensitive to the physical state (solid versus liquid) of the particles during periods with RH less than 50%.  相似文献   

2.
Field data for coarse particulate matter ([PM] PM10) and fine particulate matter (PM2.5) were collected at selected sites in Southeast Kansas from March 1999 to October 2000, using portable MiniVol particulate samplers. The purpose was to assess the influence on air quality of four industrial facilities that burn hazardous waste in the area located in the communities of Chanute, Independence, Fredonia, and Coffeyville. Both spatial and temporal variation were observed in the data. Variation because of sampling site was found to be statistically significant for PM10 but not for PM2.5. PM10 concentrations were typically slightly higher at sites located within the four study communities than at background sites. Sampling sites were located north and south of the four targeted sources to provide upwind and downwind monitoring pairs. No statistically significant differences were found between upwind and downwind samples for either PM10 or PM2.5, indicating that the targeted sources did not contribute significantly to PM concentrations. Wind direction can frequently contribute to temporal variation in air pollutant concentrations and was investigated in this study. Sampling days were divided into four classifications: predominantly south winds, predominantly north winds, calm/variable winds, and winds from other directions. The effect of wind direction was found to be statistically significant for both PM10 and PM2.5. For both size ranges, PM concentrations were typically highest on days with predominantly south winds; days with calm/variable winds generally produced higher concentrations than did those with predominantly north winds or those with winds from "other" directions. The significant effect of wind direction suggests that regional sources may exert a large influence on PM concentrations in the area.  相似文献   

3.
An indoor size-dependent particulate matter (PM) transport approach is developed to investigate coarse PM (PM10), fine PM (PM2.5), and very fine PM (PM1) removal behaviors in a ventilated partitioned indoor environment. The approach adopts the Eulerian large eddy simulation of turbulent flow and the Lagrangian particle trajectory tracking to solve the continuous airflow phase and the discrete particle phase, respectively. Model verification, including sensitivity tests of grid resolution and particle numbers, is conducted by comparison with the full-size experiments conducted previously. Good agreement with the measured mass concentrations is found. Numerical scenario simulations of the effect of ventilation patterns on PM removal are performed by using three common ventilation patterns (piston displacement, mixing, and cross-flow displacement ventilation) with a measured indoor PM10 profile in the Taipei metropolis as the initial condition. The temporal variations of suspended PM10, PM2.5, and PM1 mass concentrations and particle removal mechanisms are discussed. The simulated results show that for all the of the three ventilation patterns, PM2.5 and PM1 are much more difficult to remove than PM10. From the purpose of health protection for indoor occupants, it is not enough to only use the PM10 level as the indoor PM index. Indoor PM2.5 and PM1 levels should be also considered. Cross-flow displacement ventilation is more effective to remove all PM10, PM2.5, and PM1 than the other ventilation patterns. Displacement ventilation would result in more escaped particles and less deposited particles than mixing ventilation.  相似文献   

4.
The deposition of airborne Pb particulates has been experimentally investigated in different fields. Three fields with different surface conditions were selected for which the roughness sizes have been determined under neutral atmospheric conditions. A modified low-pressure Andersen impactor was used to determine the particle-size distribution. The sampler classifies particle size in ultra-fine range down to 0.08 μm aerodynamic diameter. The flux of particulate Pb was measured on the surfaces of: alfalfa leaves, real grass and soil under stable and unstable atmospheric conditions.Data from a meteorological tower were analysed to determine the standard deviation of horizontal wind direction from which the atmospheric stability class was determined. The deposition surfaces were wet-ashed with HNO3 and analysed for Pb by atomic absorption spectrophotometry and the particulate fluxes were obtained. The particulate fluxes were also calculated from the size-distribution data and values of deposition velocity were obtained from two deposition models (Sehmel and Hodgson, 1978; El-Shobokshy and Sharaf El-Din, 1984).It is concluded that both surface roughness and atmospheric stability are the main controlling factors in particulate deposition, together with particle diameter. For unstable conditions, there was quite good agreement between measured and calculated particulate flux using both of the above theoretical models. For stable conditions, Sehmel and Hodgson's model failed to predict accurate fluxes because their model shows the independence of deposition velocity on atmospheric stability.  相似文献   

5.
Nitrogen deposition is a continuing problem in European alpine regions. We hypothesised that, despite climatic limitations, low-alpine Calluna heathland would respond to nitrogen addition with increased shoot growth and flowering and that fire and grazing would modify responses. In a five-year study, 0-50kgNha(-1)y(-1) were added, combined with burning (+/-) and clipping (+/-). Calluna vulgaris responded with increased shoot extension, but effects on flowering were variable. Burning enhanced the positive effect of nitrogen addition and negative effects of clipping. Sub-dominant shrubs generally did not respond to nitrogen. C. vulgaris shoot extension was stimulated by nitrogen addition of 10kgNha(-1)y(-1) (above background) supporting suggestions that alpine heathlands are sensitive to low levels of nitrogen deposition. Increased C. vulgaris growth could negatively impact on important lichen components of this vegetation through increased shading and competition. Climatic factors constrain productivity in this community, but do not prevent rapid responses to nitrogen deposition by some species.  相似文献   

6.
Daily counts of non-accidental deaths in Santiago, Chile, from 1988 to 1996 were regressed on six air pollutants--fine particles (PM2.5), coarse particles (PM10-2.5), CO, SO2, NO2, and O3. Controlling for seasonal and meteorological conditions was done using three different models--a generalized linear model, a generalized additive model, and a generalized additive model on previously filtered data. Single- and two-pollutant models were tested for lags of 1-5 days and the average of the previous 2-5 days. The increase in mortality associated with the mean levels of air pollution varied from 4 to 11%, depending on the pollutants and the way season of the year was considered. The results were not sensitive to the modeling approaches, but different effects for warmer and colder months were found. Fine particles were more important than coarse particles in the whole year and in winter, but not in summer. NO2 and CO were also significantly associated with daily mortality, as was O3 in the warmer months. No consistent effect was observed for SO2. Given particle composition in Santiago, these results suggest that combustion-generated pollutants, especially from motor vehicles, may be associated with increased mortality. Temperature was closely associated with mortality. High temperatures led to deaths on the same day, while low temperatures lead to deaths from 1 to 4 days later.  相似文献   

7.
Bimonthly integrated measurements of NO2 and NH3 have been made over one year at distances up to 10 m away from the edges of roads across Scotland, using a stratified sampling scheme in terms of road traffic density and background N deposition. The rate of decrease in gas concentrations away from the edge of the roads was rapid, with concentrations falling by 90% within the first 10 m for NH3 and the first 15 m for NO2. The longer transport distance for NO2 reflects the production of secondary NO2 from reaction of emitted NO and O3. Concentrations above the background, estimated at the edge of the traffic lane, were linearly proportional to traffic density for NH3 (microg NH3 m(-3) = 1 x 10(-4) x numbers of cars per day), reflecting emissions from three-way catalysts. For NO2, where emissions depend strongly on vehicle type and fuel, traffic density was calculated in terms of 'car equivalents'; NO2 concentrations at the edge of the traffic lane were proportional to the number of car equivalents (microg NO2 m(-3) = 1 x 10(-4) x numbers of car equivalents per day). Although absolute concentrations (microg m(-3)) of NH3 were five times smaller than for NO2, the greater deposition velocity for NH3 to vegetation means that approximately equivalent amounts of dry N deposition to road side vegetation from vehicle emissions comes from NH3 and NO2. Depending on traffic density, the additional N deposition attributable to vehicle exhaust gases is between 1 and 15 kg N ha(-1) y(-1) at the edge of the vehicle lane, falling to 0.2-10 kg N ha(-1) y(-1) at 10 m from the edge of the road.  相似文献   

8.
A study of deposition velocities to snow was conducted during the 1982–1983 and 1983–1984 winters at the University of Michigan Biological Station in northern Michigan. Weekly measurements were made of dry deposition rates to snow and the atmospheric concentrations of the depositing species. SO2, with an average concentration of 2.2 ppb, was the dominant atmospheric sulfur containing species. NO2, with an average concentration of 1.8 ppb, was the dominant atmospheric nitrogenous species. NO3 deposition was due primarily to HNO3, which averaged 0.2 ppb. The HNO3 deposition velocity averaged 1.4cm s−1. The SO2 deposition velocity varied with temperature, averaging 0.15 cm s−1 for samples with appreciable exposure time above − 3°C, and 0.06 cm s−1 for samples which remained below an ambient temperature of −3°C. Deposition velocities of Ca2+, Mg2+ , Na+, K+ and NH+4 were 2.1, 1.5, 0.44, 0.51 and 0.10cm s−1, respectively. The mass median diameters of these species were 4.4, 2.7, 1.8, 0.9 and 0.46 μm, respectively.  相似文献   

9.
In this work, the effect of meteorological parameters and local topography on mass concentrations of fine (PM2.5) and coarse (PM2.5-10) particles and their seasonal behavior was investigated. A total of 236 pairs of samplers were collected using an Anderson Dichotomous sampler between December 2004 and October 2005. The average mass concentrations of PM2.5, PM2.5-10, and particulate matter less than 10 microm in aerodynamic diameter (PM10) were found to be 29.38, 23.85, and 53.23 microg/m3, respectively. The concentrations of PM2.5 and PM10 were found to be higher in heating seasons (December to May) than in summer. The increase of relative humidity, cloudiness, and lower temperature was found to be highly related to the increase of particulate matter (PM) episodic events. During non-rainy days, the episodic events for PM2.5 and PM10 were increased by 30 and 10.7%, respectively. This is a result of the extensive use of fuel during winter for heating purposes and also because of stagnant air masses formed because of low temperature and low wind speed over the study area.  相似文献   

10.
A three-dimensional chemical transport model (PMCAMx) was used to investigate changes in fine particle (PM2.5) concentrations in response to changes in sulfur dioxide (SO2) and ammonia (NH3) emissions during July 2001 and January 2002 in the eastern United States. A uniform 50% reduction in SO2 emissions was predicted to produce an average decrease of PM2.5 concentrations by 26% during July but only 6% during January. A 50% reduction of NH3 emissions leads to an average 4 and 9% decrease in PM2.5 in July and January, respectively. During the summer, the highest concentration of sulfate is in South Indiana (12.8 microg x m(-3)), and the 50% reduction of SO2 emissions results in a 5.7 microg x m(-3) (44%) sulfate decrease over this area. During winter, the SO2 emissions reduction results in a 1.5 microg x m(-3) (29%) decrease of the peak sulfate levels (5.2 microg x m(-3)) over Southeast Georgia. The maximum nitrate and ammonium concentrations are predicted to be over the Midwest (1.9 (-3)g x m(-3) in Ohio and 5.3 microg x m(-3) in South Indiana, respectively) in the summer whereas in the winter these concentrations are higher over the Northeast (3 microg x m(-3) of nitrate in Connecticut and 2.7 microg x m(-3) of ammonium in New York). The 50% NH3 emissions reduction is more effective for controlling nitrate, compared with SO2 reductions, producing a 1.1 microg x m(-3) nitrate decrease over Ohio in July and a 1.2 microg x m(-3) decrease over Connecticut in January. Ammonium decreases significantly when either SO2 or NH3 emissions are decreased. However, the SO2 control strategy has better results in July when ammonium decreases, up to 2 microg x m(-3) (37%), are predicted in South Indiana. The NH3 control strategy has better results in January (ammonium decreases up to 0.4 microg x m(-3) in New York). The spatial and temporal characteristics of the effectiveness of these emission control strategies during the summer and winter seasons are discussed.  相似文献   

11.
Environmental Science and Pollution Research - Delhi has been identified as one of the highly polluted cities in the world and recently associated with the highest population weighted PM2.5...  相似文献   

12.
Numerical precipitation scavenging models are used to investigate the relationship between the inflow concentrations of sulfur species to precipitation systems and the resulting sulfur wet deposition. Simulations have been made for summer and winter seasons using concentration ranges of SO2, aerosol SO42−, H2O2 and O3 appropriate for the eastern U.S. summer simulations use one-dimensional timedependent convective cloud and scavenging models; winter simulations use two-dimensional steady-state warm-frontal models. Sulfur scavenging mechanisms include nucleation scavenging of aerosol, aqueous reactions of H2O2, O3 and HCHO with S(IV), and nonreactive S(IV) scavenging. Over the wide range of conditions that have been examined, the relation between sulfur inflow and sulfur wet deposition varies from nearly linear to strongly nonlinear. The degree of nonlinearity is most affected by aerosol SO42− levels and relative levels of SO2 vs H2O2. Higher aerosol SO42− levels (as found in summer) produce a more linear relation. The greatest nonlinearity occurs when SO2 exceeds H2O2. Winter simulations show more nonlinearity than summer simulations.  相似文献   

13.
Two thermodynamic equilibrium models were applied to estimate changes in mean airborne fine particle (PM2.5) mass concentrations that could result from changes in ambient concentrations of sulfate, nitric acid, or ammonia in the southeastern United States, the midwestern United States, and central California. Pronounced regional differences were found. Southeastern sites exhibited the lowest current mean concentrations of nitrate, and the smallest predicted responses of PM2.5 nitrate and mass concentrations to reductions of nitric acid, which is the principal reaction product of the oxidation of nitrogen dioxide (NO2) and the primary gas-phase precursor of fine particulate nitrate. Weak responses of PM2.5 nitrate and mass concentrations to changes in nitric acid levels occurred even if sulfate concentrations were half of current levels. The midwestern sites showed higher levels of fine particulate nitrate, characterized by cold-season maxima, and were projected to show decreases in overall PM levels following decreases of either sulfate or nitric acid. For some midwestern sites, predicted PM2.5 nitrate concentrations increased as modeled sulfate levels declined, but sulfate reductions always reduced the predicted fine PM mass concentrations; PM2.5 nitrate concentrations became more sensitive to reductions of nitric acid as modeled sulfate concentrations were decreased. The California sites currently have the highest mean concentrations of fine PM nitrate and the lowest mean concentrations of fine PM sulfate. Both the estimated PM2.5 nitrate and fine mass concentrations decreased in response to modeled reductions of nitric acid at all California sites. The results indicate important regional differences in expected PM2.5 mass concentration responses to changes in sulfate and nitrate precursors. Analyses of ambient data, such as described here, can be a key part of weight of evidence (WOE) demonstrations for PM2.5 attainment plans. Acquisition of the data may require special sampling efforts, especially for PM2.5 precursor concentration data.  相似文献   

14.
To assess the impact of past, current and proposed air quality regulations on coarse particulate matter (CPM), the concentrations of CPM mass and its chemical constituents were examined in the Los Angeles Basin from 1986 to 2009 using PM data acquired from peer-reviewed journals and regulatory agency database. PM10 mass levels decreased by approximately half from 1988 to 2009 at the three sampling sites examined- located in downtown Los Angeles, Long Beach and Riverside. Annual CPM mass concentrations were calculated from the difference between daily PM10 and PM2.5 from 1999 to 2009. High CPM episodes driven by high wind speed/stagnant condition caused year-to-year fluctuations in the 99th/98th percentile CPM levels. The reductions of average CPM levels were lower than those of PM10 in the same period, therefore the decrease of PM10 level was mainly driven by reductions in the emission levels of PM2.5 (or fine) particles, as demonstrated by the higher annual reduction of average PM2.5 (0.92 microg/m3) compared with CPM (0.39 microg/m3) from 1999 to 2009 in downtown Los Angeles despite their comparable concentrations. This is further confirmed by the significant decrease of Ni, Cr, V and EC in the coarse fraction after 1995. On the other hand, the levels of several inorganic ions (sulfate, chloride and to a lesser extent nitrate) remained comparable. From 1995 to 2008, levels of Cu, a tracer of brake wear, either remained similar or decreased at a smaller rate compared with elements of combustion origins. This differential reduction of CPM components suggests that past and current regulations may have been more effective in reducing fugitive dust (Al, Fe and Si) and combustion emissions (Ni, Cr, V, and EC) rather than CPM from vehicular abrasion (Cu) and inorganic ions (NO3(-), SO4(2-) and Cl(-)) in urban areas. Implications: Limited information is currently available to provide the scientific basis for understanding the sources and physical and chemical variations of CPM, and their relations to air quality regulations and adverse health effects. This study investigates the historical trends of CPM mass and its chemical components in the Los Angeles Basin to advance our understanding on the impact of past and current air quality regulations on the coarse fraction of PM. The results of this study will aid policy makers to design more targeted regulations to control CPM sources to ensure substantial protection of public health from CPM exposure. Supplemental Materials: Supplemental materials are available for this article. Go to the publisher's online edition of the Journal of the Air & Waste Management Association for (1) details of the sampling sites and (2) the daily concentrations of high CPM/PM10 episodes.  相似文献   

15.
A Micro-Orifice Uniform Deposition Impactor (MOUDI) and a Nano-MOUDI were employed to determine the size-segregated mass distributions of ambient particulate matter (PM) and water-soluble ionic species for particulate constituents. In addition, gas precursors, including HCl, HONO, HNO3, SO2, and NH3 gases, were analyzed by an annular denuder system. PM size mass distribution, mass concentration, and ionic species concentration were measured during the day and at night during episode and non-episode periods in winter and summer. Average total suspended particle (TSP) concentrations during episode days in winter were as high as 153?±?33 μg/m3, and PM mass concentrations in summer were as low as one-third of that in winter. Generally, PM concentration at night was higher than that in the daytime in southern Taiwan during the sampling periods. In winter during the episode periods, the size-segregated mass distribution of PM mass concentration was mostly in the 0.32–3.2-μm range, and the PM concentration increased significantly in the range of 0.32–3.2 μm at night. Ammonium, nitrate, and sulfate were the dominant water-soluble ionic species in PM, contributing 34–48 % of TSP mass. High concentrations of ammonia (12.9–49 μg/m3) and SO2 (2.6–27 μg/m3) were observed in the gas precursors. The conversion ratio was high in the PM size range of 0.18–3.2 μm both during the day and at night in winter, and the conversion ratio of episode days was 20 % higher than that of non-episode days. The conversion factor was high for both nitrogen and sulfur species at nighttime, especially on episode days.  相似文献   

16.
The role of detrital quantity and quality in forest floor N leaching was investigated in a litter manipulation experiment at a deciduous forest under chronic N deposition. Dissolved inorganic nitrogen (DIN) comprised the bulk of nitrogen leaching from the control except a short period following autumn litterfall. The dominance of DIN was strengthened by litter exclusion, whereas the addition of glucose or fresh litter led to a small increase in dissolved organic nitrogen (DON) and either a temporary or gradual reduction in NO(3)(-) release, respectively. Changes in soluble organic C and microbial C in the forest floor implied that increased availability of C sources might have enhanced microbial immobilization of DIN, either temporarily following glucose application or over the longer term following litter addition. The results suggest that detrital quantity and quality can play a crucial role in determining the balance between DIN and DON in N-enriched forest soils.  相似文献   

17.
The concentration of the trace metals Cd, Cu, Fe, Mn, Ni, Pb, V and Zn has been measured in atmospheric precipitation events at the middle Atlantic coast (Lewes, DE) and on the western Atlantic island of Bermuda. The purpose is to assess the sources, transport, and wet deposition of trace metals to the western Atlantic during non-summer months when trace metals are likely to be transported by westerly air mass flow from N America to the open Atlantic. The concentrations, and wet deposition of trace metals are greater at the coast than on Bermuda, and the other at both sites (Fe > Zn > Pb > Cu, Mn, Ni > V > Cd) is similar. The trace metal enrichment factors for all metals but Mn, based on crustal Fe, are significantly greater than unity, and the order (Cd > Pb > Zn > Cu > Ni > V) is also the same at the coast as on Bermuda. This evidence suggests common sources from North America for trace metals in western Atlantic precipitation and important atmospheric transport of trace metals to the Atlantic Ocean. Calculations using enrichment factors from sea salt aerosol (Na based) indicate recycling of trace metals from the sea surface, while generally considered not to be important, could be a potentially significant process contributing to Mn and V enrichments in open western Atlantic precipitation.  相似文献   

18.
Atmospheric concentrations of major reactive nitrogen (Nr) species were quantified using passive samplers, denuders, and particulate samplers at Dongbeiwang and Quzhou, North China Plain (NCP) in a two-year study. Average concentrations of NH3, NO2, HNO3, pNH4+ and pNO3 were 12.0, 12.9, 0.6, 10.3, and 4.7 μg N m−3 across the two sites, showing different seasonal patterns of these Nr species. For example, the highest NH3 concentration occurred in summer while NO2 concentrations were greater in winter, both of which reflected impacts of N fertilization (summer) and coal-fueled home heating (winter). Based on measured Nr concentrations and their deposition velocities taken from the literature, annual N dry deposition was up to 55 kg N ha−1. Such high concentrations and deposition rates of Nr species in the NCP indicate very serious air pollution from anthropogenic sources and significant atmospheric N input to crops.  相似文献   

19.
重庆西部农业区大气沉降特征及其对地表的影响   总被引:1,自引:0,他引:1  
从2009年4月至2010年4月,在重庆西部农业区采集了50个大气干、湿沉降样品,分别测试干、湿沉降样品中K、Ca、Mg、N、P、S、Fe、As、Cd、Cr、Cu、Hg、Ni、Zn、Pb、B、Mo、Mn 18种元素的含量,计算各元素的年沉降通量。研究发现,重庆西部农业区各元素年沉降通量均低于重庆主城区和成都经济区。采用富集因子分析得出,S、Cd、N、Pb、P、Hg、Mo、Zn、Cr、As明显受人为活动影响,其中S、Hg、As、Pb是典型的燃煤元素,Cd、Cr、Zn主要来源于工业排放、汽车尾气等,N、P与农业施肥密切相关。相关性分析表明,大气沉降输入Hg引起土壤中Hg含量显著增加,大气沉降输入S引起地表水中SO2-4浓度显著升高。  相似文献   

20.
The role of emissions of volatile organic compounds and nitric oxide from biogenic sources is becoming increasingly important in regulatory air quality modeling as levels of anthropogenic emissions continue to decrease and stricter health-based air quality standards are being adopted. However, considerable uncertainties still exist in the current estimation methodologies for biogenic emissions. The impact of these uncertainties on ozone and fine particulate matter (PM2.5) levels for the eastern United States was studied, focusing on biogenic emissions estimates from two commonly used biogenic emission models, the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the Biogenic Emissions Inventory System (BEIS). Photochemical grid modeling simulations were performed for two scenarios: one reflecting present day conditions and the other reflecting a hypothetical future year with reductions in emissions of anthropogenic oxides of nitrogen (NOx). For ozone, the use of MEGAN emissions resulted in a higher ozone response to hypothetical anthropogenic NOx emission reductions compared with BEIS. Applying the current U.S. Environmental Protection Agency guidance on regulatory air quality modeling in conjunction with typical maximum ozone concentrations, the differences in estimated future year ozone design values (DVF) stemming from differences in biogenic emissions estimates were on the order of 4 parts per billion (ppb), corresponding to approximately 5% of the daily maximum 8-hr ozone National Ambient Air Quality Standard (NAAQS) of 75 ppb. For PM2.5, the differences were 0.1-0.25 microg/m3 in the summer total organic mass component of DVFs, corresponding to approximately 1-2% of the value of the annual PM2.5 NAAQS of 15 microg/m3. Spatial variations in the ozone and PM2.5 differences also reveal that the impacts of different biogenic emission estimates on ozone and PM2.5 levels are dependent on ambient levels of anthropogenic emissions.  相似文献   

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