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1.
In this study, air pollutants, including ozone (O3), nitrogen oxides (NOx = NO + NO2), carbon monoxides (CO), sulfur dioxide (SO2), and volatile organic compounds (VOCs) measured in the Yangtze River Delta (YRD) region during several air flights between September/30 and October/11 are analyzed. This measurement provides horizontal and vertical distributions of air pollutants in the YRD region. The analysis of the result shows that the measured O3 concentrations range from 20 to 60 ppbv. These values are generally below the US national standard (84 ppbv), suggesting that at the present, the O3 pollutions are modest in this region. The NOx concentrations have strong spatial and temporal variations, ranging from 3 to 40 ppbv. The SO2 concentrations also have large spatial and temporal variations, ranging from 1 to 35 ppbv. The high concentrations of CO are measured with small variations, ranging from 3 to 7 ppmv. The concentrations of VOCs are relatively low, with the total VOC concentrations of less than 6 ppbv. The relative small VOC concentrations and the relative large NOx concentrations suggest that the O3 chemical formation is under a strong VOC-limited regime in the YRD region. The measured O3 and NOx concentrations are strongly anti-correlated, indicating that enhancement in NOx concentrations leads to decrease in O3 concentrations. Moreover, the O3 concentrations are more sensitive to NOx concentrations in the rural region than in the city region. The ratios of Δ[O3]/Δ[NOx] are ?2.3 and ?0.25 in the rural and in the city region, respectively. In addition, the measured NOx and SO2 concentrations are strongly correlated, highlighting that the NOx and SO2 are probably originated from same emission sources. Because SO2 emissions are significantly originated from coal burnings, the strong correlation between SO2 and NOx concentrations suggests that the NOx emission sources are mostly from coal burned sources. As a result, the future automobile increases could lead to rapid enhancements in O3 concentrations in the YRD region.  相似文献   

2.
An aircraft study of air quality in the Hong Kong region during the fall of 1994 has allowed for an estimation of the daytime source strengths for CO and NOy from the Hong Kong metropolitan center. Emission rate estimates for the Hong Kong urban plume for NOy and CO were 5.4×10e(25) molecules s-1 and 1.8×10e(26) molecules s-1 as determined for the case study of 18 October. All emission rate estimates have uncertainties of a factor of 2. On one occasion a distinct plume emanating from Shenzhen in the People’s Republic of China was encountered. While plume delimitation was insufficient for source strength calculations, transect integrals did allow for a CO/NOy ratio of about 16 to be determined. The CO/NOy ratio for the Hong Kong urban plume was about 3.3. The difference in these ratios indicates differences in the overall combustion processes and efficiencies taking place within Hong Kong and the PRC.  相似文献   

3.
Airborne measurements were performed in the plume of the Cumberland Power Plant during August 1998 using a highly sensitive SO2 instrument. The measurements confirmed previous suggestions that NOy species are removed from the plume at a faster rate than SO2. The differential removal rate (the difference between loss rate of NOy and that of SO2) was estimated to be 0.06 h−1. This value implies that the NOy loss rate is in the range of 0.09–0.14 h−1. The application of a mathematical argument, based on the convolution integral, enabled improved synchronization of the data from the SO2 and NOy instruments. Examination of the synchronized data revealed that the concentration ratio of SO2 and NOy varies across the plume. Near the source it is higher at the wings of the plume, while in the core of the plume it is similar to the ratio at the release point. Two possible explanations of the observations are discussed: conversion to non-measurable NOy species, and in-plume loss of NOy (as HNO3) via dry deposition.  相似文献   

4.
A field experiment was conducted in August 1998 to investigate the concentrations of isoprene and isoprene reaction products in the surface and mixed layers of the atmosphere in Central Texas. Measured near ground-level concentrations of isoprene ranged from 0.3 (lower limit of detection – LLD) to 10.2 ppbv in rural regions and from 0.3 to 6.0 ppbv in the Austin urban area. Rural ambient formaldehyde levels ranged from 0.4 ppbv (LLD) to 20.0 ppbv for 160 rural samples collected, while the observed range was smaller at Austin (0.4–3.4 ppbv) for a smaller set of samples (37 urban samples collected). Methacrolein levels did not vary as widely, with rural measurements from 0.1 ppbv (LLD) to 3.7 ppbv and urban concentrations varying between 0.2 and 5.7 ppbv. Isoprene flux measurements, calculated using a simple box model and measured mixed-layer isoprene concentrations, were in reasonable agreement with emission estimates based on local ground cover data. Ozone formation attributable to biogenic hydrocarbon oxidation was also calculated. The calculations indicated that if the ozone formation occurred at low VOC/NOx ratios, up to 20 ppbv of ozone formed could be attributable to biogenic photooxidation. In contrast, if the biogenic hydrocarbon reaction products were formed under low NOx conditions, ozone production attributable to biogenics oxidation would be as low as 1 ppbv. This variability in ozone formation potentials implies that biogenic emissions in rural areas will not lead to peak ozone levels in the absence of transport of NOx from urban centers or large rural NOx sources.  相似文献   

5.
The CALINE4 roadway dispersion model has been applied to concentrations of NOx and NO2 measured near Gandy Boulevard in Tampa, FL (USA) during May 2002. A NOx emission factor of 0.86 gr mi−1 was estimated by treating NO+NO2 (NOx) as a conserved species and minimizing the differences between measured and calculated NOx concentrations. This emission factor was then used to calculate NO2 concentrations using the NO/NO2 transformation reactions built into CALINE4. A comparison of measured and calculated NO2 concentrations indicates that for ambient O3 concentrations less than 40 ppb the model under-predicts the chemical transformation of NO. The enhanced transformation of NO may be due to reactions of NO with oxidants such as peroxy radicals that are present either in the atmosphere or in vehicle exhaust.  相似文献   

6.
Real-world emissions of a traffic fleet on a transit route in Austria were determined in the Tauerntunnel experiment in October 1997. The total number of vehicles and the average speed was nearly the same on both measuring days (465 vehicles 30 min−1 and 76 km h−1 on the workday, 477 and 78 km h−1 on Sunday). The average workday fleet contained 17.6% heavy-duty vehicles (HDV) and the average Sunday fleet 2.8% HDV resulting in up to four times higher emission rates per vehicle per km on the workday than on Sunday for most of the regulated components (CO2, CO, NOx, SO2, and particulate matter-PM10). Emission rates of NMVOC accounted for 200 mg vehicle−1 km−1 on both days. The relative contributions of light-duty vehicles (LDV) and HDV to the total emissions indicated that aldehydes, BTEX (benzene, toluene, ethylbenzene, xylenes), and alkanes are mainly produced by LDV, while HDV dominated emissions of CO, NOx, SO2, and PM10. Emissions of NOx caused by HDV were 16,100 mg vehicle−1 km−1 (as NO2). Produced by LDV they were much lower at 360 mg vehicle−1 km−1. Comparing the emission rates to the results that were obtained by the 1988 experiment at the same place significant changes in the emission levels of hydrocarbons and CO, which accounted 1997 to only 10% of the levels in 1988, were noticed. However, the decrease of PM has been modest leading to values of 80 and 60% of the levels in 1988 on the workday and on Sunday, respectively. Emission rates of NOx determined on the workday in 1997 were 3130 mg vehicle−1 km−1 and even higher than in 1988 (2630 mg vehicle−1 km−1), presumable due to the increase of the HD-traffic.  相似文献   

7.
In a companion paper by Hu et al. [2007. A kinetic mechanism for predicting secondary organic aerosol formation from toluene oxidation in the presence of NOx and natural sunlight. Atmospheric Environment, doi:10.1016/j.atmosenv.2007.04.025], a kinetic mechanism was developed from data generated in the University of North Carolina's (UNC) 270 m3 dual outdoor aerosol smog chamber, to predict secondary organic aerosol (SOA) formation from toluene oxidation in the atmosphere. In this paper, experimental data sets from European Photoreactor (EUPHORE), smog chambers at the California Institute of Technology (Caltech), and the UNC 300 m3 dual-outdoor gas phase chamber were used to evaluate the toluene mechanism. The model simulates SOA formation for the ‘low-NOx’ and ‘mid-NOx’ experiments from EUPHORE chambers reasonably well, but over-predicts SOA mass concentrations for the ‘high-NOx’ run. The model well simulates the SOA mass concentrations observed from the Caltech chambers. Experiments with the three key toluene products, 1,4-butenedial, 4-oxo-2-pentenal and o-cresol in the presence of oxides of nitrogen (NOx) are also simulated by the developed mechanism. The model well predicts the NOx time–concentration profiles and the decay of these two carbonyls, but underestimates ozone (O3) formation for 4-oxo-2-pentenal. It well simulates SOA formation from 1,4-butenedial but overestimates (possibly due to experimental problems) the measured aerosol mass concentrations from 4-oxo-2-pentenal. The model underestimates SOA production from o-cresol, mostly due to its under-prediction of o-cresol decay. The effects of varying temperature, relative humidity, glyoxal uptake, organic nitrate yields, and background seed aerosol concentrations, were also investigated.  相似文献   

8.
Year-long measurements of NOx and ozone performed during the NOXAR project are compared to results from the ECHAM4.L39(DLR)/CHEM (E39/C) and GISS coupled chemistry–climate models. The measurements were taken on flights between Europe and the eastern United States and between Europe and the Far East in the latitude range 40–65°N. Our comparison concentrates on the upper troposphere and reveals strong longitudinal variations in seasonal mean NOx of more than 200 pptv, which both models are able to reproduce qualitatively. Vertical profiles show maximum NOx values 2–3 km below the tropopause (“E-shape”) with a strong seasonal cycle. E39/C simulates a maximum located at the tropopause and with a reasonable seasonal cycle. The GISS model reproduces the seasonal cycle but not the profile's shape due to its coarser vertical resolution. A comparison of NOx frequency distributions reveals that both models are capable of reproducing the observed variability, except that E39/C shows no very high NOx mixing ratios.Both models show that lightning and surface NOx emissions contribute the most to the seasonal cycle of NOx at tropopause altitudes. The impact of lightning in the upper troposphere does not vary strongly with altitude, whereas the impact of surface emissions decreases with altitude. Among all sources, lightning contributes the most to the variability of NOx in the upper troposphere in northern mid-latitudes during summer.  相似文献   

9.
10.
The influence of NOx (NO+NO2) concentrations on the product distribution of the OH-initiated oxidation of DMS has been studied at room temperature using total NOx concentrations varying from 0 to ∼1800 ppbv (30–600 ppbv NO2 and 140–1760 ppbv NO). Clear trends in the formation yields of the products SO2, COS, MSA, MTF (methyl thiolformate), MSPN (methanesulphonyl peroxynitrate), DMSO and DMSO2 have been observed with variation in NOx. The presence of low levels of NO reduces the yields of both MTF and COS to zero. The formation yields of MSA and DMSO2 increase with increasing NOx concentration, whereas the yields of DMSO and SO2 decrease. The following approximate changes in the yield, not corrected for possible loss processes, have been measured for variation of NOx between 0 and ∼1800 ppbv: DMSO decreases from 20 to 3%S; DMSO2 increases from 3 to 15%S, SO2 decreases from 70 to 30%S and MSA increases from 4 to 17%S. Under the experiments conditions NOx levels of several tens of ppbv are required before a perceptible change is observed in the MSA yield. If applicable to the atmosphere such a situation is only likely to be observed near coastal areas affected by pollution. MSPN (CH3SO2O2NO2) is observed as an oxidation product in the presence of NO2 even at low levels (e.g. 60 ppbv). Its possible role as a NOx reservoir in the troposphere is considered.  相似文献   

11.
Vehicle particle emissions are studied extensively because of their health effects, contribution to ambient PM levels and possible impact on climate. The aim of this work was to obtain a better understanding of secondary particle formation and growth in a diluting vehicle exhaust plume using 3-d information of simulations together with measurements. Detailed coupled computational fluid dynamics (CFD) and aerosol dynamics simulations have been conducted for H2SO4–H2O and soot particles based on measurements within a vehicle exhaust plume under real conditions on public roads.Turbulent diffusion of soot and nucleation particles is responsible for the measured decrease of number concentrations within the diesel car exhaust plume and decreases coagulation rates. Particle size distribution measurements at 0.45 and 0.9 m distance to the tailpipe indicate a consistent soot mode (particle diameter Dp∼50 nm) at variable operating conditions. Soot mode number concentrations reached up to 1013 m−3 depending on operating conditions and mixing.For nucleation particles the simulations showed a strong sensitivity to the spatial dilution pattern, related cooling and exhaust H2SO4(g). The highest simulated nucleation rates were about 0.05–0.1 m from the axis of the plume. The simulated particle number concentration pattern is in approximate accordance with measured concentrations, along the jet centreline and 0.45 and 0.9 m from the tailpipe. Although the test car was run with ultralow sulphur fuel, high nucleation particle (Dp⩽15 nm) concentrations (>1013 m−3) were measured under driving conditions of strong acceleration or the combination of high vehicle speed (>140 km h−1) and high engine rotational speed (>3800 revolutions per minute (rpm)).Strong mixing and cooling caused rapid nucleation immediately behind the tailpipe, so that the highest particle number concentrations were recorded at a distance, x=0.45 m behind the tailpipe. The simulated growth of H2SO4–H2O nucleation particles was unrealistically low compared with measurements. The possible role of low and semi-volatile organic components on the growth processes is discussed. Simulations for simplified H2SO4–H2O–octane–gasoil aerosol resulted in sufficient growth of nucleation particles.  相似文献   

12.
Comparisons were made between the predictions of six photochemical air quality simulation models (PAQSMs) and three indicators of ozone response to emission reductions: the ratios of O3/NOz and O3/NOy and the extent of reaction. The values of the two indicator ratios and the extent of reaction were computed from the model-predicted mixing ratios of ozone and oxidized nitrogen species and were compared to the changes in peak 1 and 8 h ozone mixing ratios predicted by the PAQSMs. The ozone changes were determined from the ozone levels predicted for base-case emission levels and for reduced emissions of volatile organic compounds (VOCs) and oxides of nitrogen (NOx). For all simulations, the model-predicted responses of peak 1 and 8 h ozone mixing ratios to VOC or NOx emission reductions were correlated with the base-case extent of reaction and ratios of O3/NOz and O3/NOy. Peak ozone values increased following NOx control in 95% (median over all simulations) of the high-ozone (>80 ppbv hourly mixing ratio in the base-case) grid cells having mean afternoon O3/NOz ratios less than 5 : 1, O3/NOy less than 4 : 1, or extent less than 0.6. Peak ozone levels decreased in response to NOx reductions in 95% (median over all simulations) of the grid cells having peak hourly ozone mixing ratios greater than 80 ppbv and where mean afternoon O3/NOz exceeded 10 : 1, O3/NOy was greater than 8 : 1, or extent exceeded 0.8. Ozone responses varied in grid cells where O3/NOz was between 5 : 1 and 10 : 1, O3/NOy was between 4 : 1 and 8 : 1, or extent was between 0.6 and 0.8. The responses in such grid cells were affected by ozone responses in upwind grid cells and by the changes in ozone levels along the upwind boundaries of the modeling domains.  相似文献   

13.
Sub-regional and sector level distribution of SO2 and NOx emissions inventories for India have been estimated for all the 466 Indian districts using base data for years 1990 and 1995. Although, national level emissions provide general guidelines for assessing mitigation alternatives, but significant regional and sectoral variability exist in Indian emissions. Districts reasonably capture this variability to a fine grid as 80% of these districts are smaller than 1°×1° resolution with 60% being smaller than even 1/2°×1/2°. Moreover, districts in India have well-established administrative and institutional mechanisms that would be useful for implementing and monitoring measures. District level emission estimates thus offer a finer regional scale inventory covering the combined interests of the scientific community and policy makers. The inventory assessment methodology adopted is similar to that prescribed by the Intergovernmental Panel on Climate Change (IPCC) for greenhouse gas (GHG) emissions. The sectoral decomposition at district level includes emissions from fossil fuel combustion, non-energy emissions from industrial activities and agriculture. Total SO2 and NOx emissions from India were 3542 and 2636 Gg, respectively (1990) and 4638 and 3462 Gg (1995) growing at annual rate of around 5.5%. The sectoral composition of SO2 emissions indicates a predominance of electric power generation sector (46%). Power and transport sector emissions equally dominate NOx emissions contributing nearly 30% each. However, majority of power plants are situated in predominantly rural districts while the latter are concentrated in large urban centers. Mitigation efforts for transport sector NOx emissions would therefore be higher. The district level analysis indicates diverse spatial distribution with the top 5% emitting districts contributing 46.5 and 33.3% of total national SO2 and NOx emissions, respectively. This skewed emission pattern, with a few districts, sectors and point sources emitting significant SO2 and NOx, offers mitigation flexibility to policy makers for cost-effective mitigation.  相似文献   

14.
NOx emissions from a medium speed diesel engine on board a servicing passenger ferry have been indirectly measured using a predictive emission monitoring system (PEMS) over a 1-yr period. Conventional NOx measurements were carried out with a continuous emission monitoring system (CEMS) at the start of the study to provide historical data for the empirical PEMS function. On three other occasions during the year the CEMS was also used to verify the PEMS and follow any changes in emission signature of the engine. The PEMS consisted of monitoring exhaust O2 concentrations (in situ electrochemical probe), engine load, combustion air temperature and humidity, and barometric pressure. Practical experiences with the PEMS equipment were positive and measurement data were transferred to a land-based office by using a modem data communication system. The initial PEMS function (PEMS1) gave systematic differences of 1.1–6.9% of the calibration domain (0–1725 ppm) and a relative accuracy of 6.7% when compared with CEMS for whole journeys and varying load situations. Further improvements on the performance could be obtained by updating this function. The calculated yearly emission for a total engine running time of 4618 h was 316 t NOx±38 t and the average NOx emission corrected for ambient conditions 14.3 g kWhcorr−1. The exhaust profile of the engine in terms of NOx, CO and CO2 emissions as determined by CEMS was similar for most of the year. Towards the end of the study period, a significantly lower NOx emission was detected which was probably caused by replacement of fuel injector nozzles. The study suggests that PEMS can be a viable option for continuous, long-term NOx measurements on board ships.  相似文献   

15.
Annual mean limits for NO2 concentrations have been set in the European Union, which will be most challenging to meet in large urban conurbations. In this paper, we discuss techniques that have been developed to predict current and future NO2 concentrations in London, utilising ambient data. Hourly average NOx (NO+NO2) and NO2 concentrations are used to calculate NOx frequency distributions. By defining relationships between the annual mean NOx and NO2 at different sites, it is possible to investigate different NOx reduction strategies. The application of the frequency distribution approach to monitoring sites in London shows that given the likely change in emissions by 2005, it is unlikely that much of central and inner London will meet the objective. The approaches used suggest that meeting the objective in central London will be the most challenging for policy makers requiring NOx concentrations as low as 30 ppb, compared with values closer to 36–40 ppb for outer London. Predictions for 2005 indicate that concentrations of NO2 up to 6 ppb in excess of the objective are likely in central London.  相似文献   

16.
Ozone was measured in six- and NOx in five sampling periods in 1996–97, mostly during summer, at a 1070 m altitude site in northern Peloponnese. Mean values in each sampling period ranged from 43–48 ppb exceeding the European Union 24 h plant protection standard. The background ozone concentration of 43 ppb derived from the correlation of ozone with NOx also exceeded the EU plant protection standard. Ozone exhibited maxima in the afternoon and minima during the night; in certain 24–48 h periods, however, the ozone concentrations remained practically constant; in these short periods air mass back trajectories indicated air masses which originated in north Africa. NOx concentrations had maximum of 24 h around noon. Their mean concentrations ranged from 0.5–0.7 ppb, smaller than respective concentrations in north-central Europe.  相似文献   

17.
The evolution of photochemical smog in a plant plume was investigated with the aid of an instrumented helicopter. Air samples were taken in the plume of the Cumberland Power Plant, located in central Tennessee, during the afternoon of 16 July 1995 as part of the Southern Oxidants Study – Nashville Middle Tennessee Ozone Study. Twelve cross-wind air sampling traverses were made at six distance groups from 35 to 116 km from the source. During the sampling period the winds were from the west–northwest and the plume drifted towards the city of Nashville TN. Ten of the traverses were made upwind of the city, where the power plant plume was isolated, and two traverses downwind of the city when the plumes were possibly mixed. The results revealed that even six hours after the release, excess ozone production was limited to the edges of the plume. Only when the plume was sufficiently dispersed, but still upwind of Nashville, was excess ozone (up to 109 ppbv, 50–60 ppbv above background levels) produced in the center of the plume. The concentrations image of the plume and a Lagrangian particle model suggests that portions of the power plant plume mixed with the urban plume. The mixed urban power plant plume began to regenerate O3 that peaked at 120 ppbv at a short distance (15–25 km) downwind of Nashville. Ozone productivity (the ratio of excess O3 to NOy and NOz) in the isolated plume was significantly lower compared with that found in the city plume. The production of nitrate, a chain termination product, was significantly higher in the power plant plume compared to the mixed plume, indicating shorter chain length of the photochemical smog chain reaction mechanism.  相似文献   

18.
In situ measurements of nitric acid (HNO3), reactive nitrogen (NOy), nitric oxide (NO), and ozone (O3) made in the upper troposphere (UT) and lower stratosphere (LS) between 29° and 33°N latitudes during September 1999 are used to examine NOy partitioning and correlations between the measured species in these regions. The fast-response (1 s) HNO3 measurements are acquired with a new autonomous CIMS instrument. In the LS, HNO3 accounts for the majority of NOy, and the sum of HNO3 and NOx accounts for approximately 90% of NOy. In the UT, the sum of HNO3 and NOx varies between 40% and 100% of NOy. Both HNO3 and NOy are strongly positively correlated with O3, with larger correlation slopes in the UT than in the LS. In the UT at low values of the quantity (NOy–NOx–HNO3), it is uncorrelated with O3, while at higher values, a positive correlation with O3 is found. Of these two air mass types, those with higher (NOy–NOx–HNO3) mixing ratios are likely associated with the presence of peroxyacetyl nitrate (PAN) that is produced by NOx-hydrocarbon chemistry.  相似文献   

19.
Sensitivity of ozone (O3) concentrations in the Mexico City area to diurnal variations of surface air pollutant emissions is investigated using the WRF/Chem model. Our analysis shows that diurnal variations of nitrogen oxides (NOx = NO + NO2) and volatile organic compound (VOC) emissions play an important role in controlling the O3 concentrations in the Mexico City area. The contributions of NOx and VOC emissions to daytime O3 concentrations are very sensitive to the morning emissions of NOx and VOCs. Increase in morning NOx emissions leads to decrease in daytime O3 concentrations as well as the afternoon O3 maximum, while increase in morning VOC emissions tends to increase in O3 concentrations in late morning and early afternoon, indicating that O3 production in Mexico City is under VOC-limited regime. It is also found that the nighttime O3 is independent of VOCs, but is sensitive to NOx. The emissions of VOCs during other periods (early morning, evening, and night) have only small impacts on O3 concentrations, while the emissions of NOx have important impacts on O3 concentrations in the evening and the early morning.This study suggests that shifting emission pattern, while keeping the total emissions unchanged, has important impacts on air quality. For example, delaying the morning emission peak from 8 am to 10 am significantly reduced the morning peaks of NOx and VOCs, as well as the afternoon O3 maxima. It suggests that without reduction of total emission, the daytime O3 concentrations can be significantly reduced by changing the diurnal variations of the emissions of O3 precursors.  相似文献   

20.
This paper evaluates the relative impact on air quality of harbour emissions, with respect to other emission sources located in the same area. The impact assessment study was conducted in the city of Taranto, Italy. This area was considered as representative of a typical Mediterranean harbour region, where shipping, industries and urban activities co-exist at a short distance, producing an ideal case to study the interaction among these different sources. Chemical and meteorological field campaigns were carried out to provide data to this study. An emission inventory has been developed taking into account industrial sources, traffic, domestic heating, fugitive and harbour emissions. A 3D Lagrangian particle dispersion model (SPRAY) has then been applied to the study area using reconstructed meteorological fields calculated by the diagnostic meteorological model MINERVE. 3D short term hourly concentrations have been computed for both all and specific sources. Industrial activities are found to be the main contributor to SO2. Industry and traffic emissions are mainly responsible for NOx simulated concentrations. CO concentrations are found to be mainly related to traffic emissions, while primary PM10 simulated concentrations tend to be linked to industrial and fugitive emissions. Contributions of harbour activities to the seasonal average concentrations of SO2 and NOx are predicted to be up to 5 and 30 μg m−3, respectively to be compared to a overall peak values of 60 μg m−3 for SO2 and 70 μg m−3 for NOx. At selected urban monitoring stations, SO2 and NOx average source contributions are predicted to be both of about 9% from harbour activities, while 87% and 41% respectively of total concentrations are predicted to be of industrial origin.  相似文献   

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