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1.
Summary The air quality modelling system (HIRES-AIRCHEM) of The University of New South Wales is tested with regard to forecast distributions of sulfur dioxide (SO2), nitrogen dioxide (NO2) and ozone (O3) over the Sydney basin and surrounding area. This is achieved by assimilating the emissions inventory of the New South Wales State Environment Protection Authority. This inventory contains both road and non-road sources. The HIRES-AIRCHEM system was run over the greater Sydney metropolitan area for a four day period in February 1998. During this period O3 readings, in particular, exceeded the EPAs threshold maximum of 80ppb. The model forecasts of the NO2-, SO2- and O3-distributions verify well with the EPAs monitored readings. Diurnal concentrations are greatest in the late afternoon, as expected, when photochemical processes are most active. Furthermore, the forecast spatial distribution of NO2 and SO2 shows maximum values radiating out along major roads from the Sydney CBD and other population centres. This is consistent with NO2 and SO2 being major pollutants associated with vehicular traffic. These promising results have significant implications for possible future use of the system as a tool for routinely assessing air quality.  相似文献   

2.
In 1997 and 1998 several field campaigns for monitoring non-methane volatile organic compounds (NMVOCs) and nitrogen oxides (NOx) were carried out in a road traffic tunnel and in the city center of Wuppertal, Germany. C2–C10 aliphatic and aromatic hydrocarbons were monitored using a compact GC instrument. DOAS White and long path systems were used to measure aromatic hydrocarbons and oxygenated aromatic compounds. A formaldehyde monitor was used to measure formaldehyde. Chemiluminescence NO analysers with NO2 converter were used for measuring NO and NO2. The high mixing ratios of the NMVOCs observed in the road traffic tunnel, especially 2.9 ppbv phenol, 1.5ppbv para-cresol and 4.4 ppbv benzaldehyde, in comparison with themeasured background concentration clearly indicate that these compounds were directly emitted from road traffic. Para-Cresol was for the first timeselectively detected as primary pollutant from traffic. From the measured data a NMVOC profile of the tunnel air and the city air, normalised to benzene (ppbC/ppbC), was derived. For most compounds the observed city air NMVOC profile is almost identical with that obtained in the traffic tunnel. Since benzene originates mainly from road traffic emission, the comparison of the normalised emission ratios indicate that the road traffic emissions in Wuppertal have still the largest impact on the city air composition, which is in contrast to the German emission inventory. In both NMVOC profiles, aromatic compounds have remarkably large contributions of more than 40 ppbC%. In addtion, total NMVOC/NOx ratios from 0.6 up to 3.0ppbC/ppb in the traffic tunnel air and 3.4± 0.5 in the city air of Wuppertal were obtained. From the observed para-cresol/toluene and ortho-cresol/toluene ratios in the city air, evidence was found thatalso during daytime NO3 radical reactions play an important role in urban air.  相似文献   

3.
Dimethylsulfide (DMS), sulfur dioxide (SO2), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO4 2–), sodium (Na+), ammonium (NH4 +), and nitrate (NO3 –) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO2 concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m–3 (STP). The nonsea-salt sulfate (ns-SO4 2–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO2 and nss-SO4 2– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na+ and NO3 –, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions.  相似文献   

4.
Emissions of nitric oxide and other odd nitrogen oxides (NO x ) from a flooded rice field were studied after urea had been broadcast into the floodwater.The NO x flux from the fertilized area was very low (0.2×10-9 g N m-2 s-1) for the first few days after application of urea and was high (0.95×10-9 g N m-2 s-1) in the subsequent period when significant nitrite and nitrate were present in the floodwater. At night, little if any NO x was exhaled but ambient NO2 was absorbed by the floodwater. An uptake velocity for NO2 of 3×10-4 m s-1 was measured during one night. Maximum NO x losses were observed near 1300 h when temperature and solar ultraviolet light were maximum.While the amounts of nitrogen oxides emitted are of little agronomic importance (2×10-3 per cent of the fertilizer nitrogen was lost as NO x during the 10-day study period), they may well be of significance as a source for some gas reactions in the atmosphere and for the global nitrogen cycle.Of the fertilizer nitrogen applied (as urea) approximately 30% was lost to the atmosphere by NH3 volatilization, 15% by denitrification, presumably as N2, and the remainder, less minor losses of NO and N2O, remained in the plant/soil/water system.Now at Forestry Department, Australian National University, G.P.O. Box 4, ACT 2601, Australia.  相似文献   

5.
Surface ozone, NO, NO2, and NO x were measured at a coastal site (Shihua) and a nearby inland site (Zhujing) in suburban Shanghai for the whole year of 2009. More days with ozone pollution in a longer time range were observed at the coastal site than the inland site. The diurnal variations of NO x concentrations were obviously higher at Zhujing station, while those of ozone concentrations were higher at Shihua station, indicating their different air pollution conditions. Coastal wind has significant influence on the levels and characteristics of the air pollutants. The ozone concentrations during maritime winds (MW) were much higher than those during continental winds (CW) at each of the site, while the NO and NO2 concentrations were both opposite. The ozone concentrations at Shihua station were much higher than those at Zhujing station, while the NO and NO2 concentrations were both opposite. The ozone concentrations at both of the two sites showed a distinct “weekend effects” and “weekdays effects” patterns during CW and MW, respectively. Correlation analysis of the pollutants showed that, the compounds during MW were more age than those during CW, and the compounds at Shihua were more age than those at Zhujing. The air pollutions at both of the two sites are mainly associated with the pollutants emitted in this region instead of long range transport.  相似文献   

6.
The paper presents monitoring results and environmental pollution assessment for the Gdask-Sopot-Gdynia Tricity (Poland), based onanalysis of precipitation. Precipitation samples were collected over a period of 12 months (January–December 1998) at ten locations in the Tricity. The following selected ions were determined in the samples:SO4 2–, F–, Cl–, NO3 –,PO4 3–, NH4 +, Na+,Mg2+, Ca2+, K+. The results were subjected to full statistical evaluation. Values of the parameters determined were correlated with each other. An attempt was made to explain co-occurrences of certain ions and the significance of their mutual effects. Pollutant concentrations and loads in precipitation were also correlated with data on wind direction and temperature in the region.Deposition of pollutants was very high in spring due to the prevailing air circulation patterns and low temperatures. Analysis of the correlations between co-occurring ions confirmed the significant impact of the location (sea coast) on the composition of rain water. Ionic ratios in rainwater were similar to those observed for sea salt samples. In addition, heavy traffic was most probably responsible for high concentrations of various forms of nitrogen and sulphates in the vicinity of major highways.  相似文献   

7.
We present a 16-month record of ozone (O3), carbon monoxide (CO), total reactive nitrogen (NOy), sulphur dioxide (SO2), methane (CH4), C2 – C8 non-methane hydrocarbons (NMHCs), C1 – C2 halocarbons, and dimethyl sulfide (DMS) measured at a southern China coastal site. The study aimed to establish/update seasonal profiles of chemically active trace gases and pollution tracers in subtropical Asia and to characterize the composition of the `background' atmosphere over the South China Sea (SCS) and of pollution outflow from the industrialized Pearl River Delta (PRD) region and southern China. Most of the measured trace gases of anthropogenic origin exhibited a winter maximum and a summer minimum, while O3 showed a maximum in autumn which is in contrast to the seasonal behavior of O3 in rural eastern China and in many mid-latitude remote locations in the western Pacific. The data were segregated into two groups representing the SCS background air and the outflow of regional continental pollution (PRD plus southern China), based on CO mixing ratios and meteorological conditions. NMHCs and halocarbon data were further analyzed to examine the relationships between their variability and atmospheric lifetime and to elucidate the extent of atmospheric processing in the sampled air parcels. The trace gas variability (S) versus lifetime (τ) relationship, defined by the power law, Slnx = Aτ− b, (where X is the trace gas mixing ratio) gives a fit parameter A of 1.39 and exponent b of 0.42 for SCS air, and A of 2.86 and b of 0.31 for the regional continental air masses. An examination of ln[n-butane]/ln[ethane] versus ln[propane]/ln[ethane] indicates that their relative abundance was dominated by mixing as opposed to photochemistry in both SCS and regional outflow air masses. The very low ratios of ethyne/CO, propane/ethane and toluene/benzene suggest that the SCS air mass has undergone intense atmospheric processing since these gases were released into the atmosphere. Compared to the results from other polluted rural sites and from urban areas, the large values of these species in the outflow of PRD/southern China suggest source(s) emitting higher levels of ethyne, benzene, and toluene, relative to light alkanes. These chemical characteristics could be unique indicators of anthropogenic emissions from southern China.  相似文献   

8.
Measurements of ground level ozone (O3), nitrogen dioxide (NO2) and meteorological parameters (air temperature, relative humidity and wind speed and direction) has been made for 3 years from March 2007 to February 2010 at Nagercoil (8.2°N, 77.5°E, 23 m above sea level), an equatorial rural coastal site of southern India. The monthly average of daytime maximum of O3 concentrations ranged from 28 to 50 parts per billion (ppb) with an annual average of 19.8 ppb. Similarly, monthly average of NO2 concentration ranged from 3.4 ppb to 7.7 ppb with an annual average of 5.3 ppb. The monthly variation of meteorological parameters shows the little changes being a coastal site. The estimated summer crops yield losses by 1.1–15.6 % from present O3 concentration level associated with AOT40 index 3.1–5 ppm h.  相似文献   

9.
The daily variations in the atmospheric pollutants like suspended particulate matter (SPM), respirable suspended particulate matter (RSPM), sulphur dioxide (SO2) and nitrogen dioxide (NO2) depend on both local meteorological processes and various natural as well as anthropogenic sources and sinks. It was shown in an earlier work (Goswami and Baruah in Mon Wea Rev 136(9):3597?C3607, 2008) that the daily variations in SPM over a location could be simulated quite well by considering daily meteorological fields from NCEP Reanalysis in combination with a model for natural and anthropogenic sources over Delhi. In the present work, we extend the scope of the model to include three other pollutants: RSPM, SO2 and NO2. While the basic conservation equations and the meteorological fields are common to all the three (and SPM) pollutants, the sources and sinks for each is modeled in a species-specific manner to obtain maximum skill. As we do not consider active chemistry, the present model provides the minimal dynamics of pollution over an urban location in terms of annual load; the model error is about 10% on the average, with no significant bias for any of the species.  相似文献   

10.
Aircraft observations of oxides of nitrogen (NO y ), measured with a ferrous sulfate converter, over the sea surrounding the Japanese islands (30–43° N, 131–141° E) were carried out in the winter of 1983 and 1984 at altitudes mostly between 3 and 8 km. NO y defined here is the sum of NO, NO2, and other unstable oxides of nitrogen that are converted to NO by ferrous sulfate. The main observations were:
  1. Over the Pacific Ocean between the latitudes of 30–35° N, the observed NO y mixing ratio between 3 and 8 km was a fairly constant 200 pptv. The NO mixing ratio increased with altitude from 15 pptv at 3 km to 35 pptv at 7 km.
  2. Over the Sea of Japan, tropospheric NO y mesured between 1 and 6 km started increasing with latitude North of 35° N and reached about 1000 pptv at 40° N.
  3. NO y was measured in an air mass transported from the stratosphere near a tropopause fold region. When the ozone mixing ratio was between 80 and 140 ppbv, the NO y mixing ratio was about 200 pptv.
  相似文献   

11.
This paper presents the development of a simple and precise analytical method for the determination of nitrogen dioxide in ambient air. In this method nitrogen dioxide is determined in the form of nitrite. The determination of nitrogen dioxide needs no reagents except for a solution of sodium hydroxide mixed with sodium arsenite (NaOH–Na2As2O3) which is used as an absorbing reagent for trapping the nitrogen dioxide from the atmosphere in the form of nitrite, i.e., a prior analysis step. The determination of submicrogram levels of nitrogen dioxide is based on the selection of a strong and sharp quantitative analytical peak at 1380 cm− 1 using diffuse reflectance infrared spectroscopy (DRS-FTIR). The limit of detection (LOD) and the limit of quantification of the method are found to be 0.008 μg g− 1 NO2− and 0.05 μg g− 1 NO2−, respectively. The precision in terms of standard deviation and relative standard deviation value at a level of 2 μg NO2− / 0.1 g KBr for n = 10 is found to be 0.036 μg NO2− and 1.8%, respectively. The relative standard deviation (n = 10) for the determination of nitrogen dioxide in ambient air was observed to be in the range 2.6–3.8%. The method proposed is time-saving and eliminates the slow and cumbersome steps of pH maintenance of the reaction mixture and color formation of the EPA recommended spectrophotometric and other methods for quantitative determination of nitrogen dioxide.  相似文献   

12.
Measurements of surface ozone (O3), nitric oxide (NO), nitrogen dioxide (NO2), oxides of nitrogen (NOx=NO+NO2) and meteorological parameters have been made at Agra (North Central India, 27°10??N, 78°05??E) in post monsoon and winter season. The diurnal variation in O3 concentration shows daytime in situ photochemical production with diurnal maximum in noon hours ranging from 51 to 54 ppb in post monsoon and from 76 to 82 ppb in winter, while minimum (16?C24 ppb) during nighttime and early morning hours. Average 8-h O3 concentration varied from 12.4 to 83.9 ppb. The relationship between meteorological parameters (solar radiation intensity, temperature, relative humidity, wind speed and wind direction) and surface O3 variability was studied using principal component analysis (PCA), multiple linear regression (MLR) and correlation analysis (CA). PCA and MLR of daily mean O3 concentrations on meteorological parameters explain up to 80 % of day to day ozone variability. Correlation with meteorology is strongly emphasized on days having strong solar radiation intensity and longer sunshine time.  相似文献   

13.
Using a filter radiometer, the meridional profile of the NO2 photolysis frequency, J(NO2), was measured between 50° N and 30° S during the cruise ANTVII/1 September/October 1988 of the research vessel Polarstern on the Atlantic Ocean. Simultaneously, global broadband irradiance and acrosol were monitored. Clean marine background air with low aerosol loads (b sp=(1–2)×10-5 m-1) was encountered at the latitudes 25° N–30° N and 18° S–27° S, respectively. Under these conditions and an almost cloudless sky J(NO2) reached 7.3×10-3 s-1 (2 sr) for a zenith angle of 30°. Between 30° N and 30° S, the latitudinal variation of the J(NO2) noontime maxima was less than ± 10%, while the mean value at noon was 7.8×10-3 s-1. For the set of all data between 50° N and 30° S, a nearly linear correlation of J(NO2) vs. global broadland irradiance was found. The slope of (8.24±0.03)×10-5 s-1/mW cm-2 agrees within 10% with observations in Jülich (51° N, 6.2° E).  相似文献   

14.
The yields of products have been calculated for the reactions of hydroxyl radicals and ozone with 19 of the two-through-six carbon anthropogenic alkenes. Based on their rate of reaction, mechanisms of reactions and the ambient air distribution for these alkenes their seasonal ambient air yields have been estimated.Aldehydes predominate as products irrespective of season, with smaller yields of several ketones. Other minor products include carboxylic acids, carbon monoxide, carbon dioxide, and alkenes. About a two-fold increase is estimated in the yields of hot biradicals and their products from summer to winter.One sensitivity analysis was made by recomputing yields at a different OH radical to O3 concentration than assumed most likely in the calculations discussed above. In addition, the sensitivity of product yields to an estimated range of seasonally averaged sunset-to-sunrise NO3 radical concentrations was calculated. The effects of free radical reactions are discussed, but these are believed to make a relatively minor contribution within the NO x -rich atmospheres that contain anthropogenic alkenes.The uncertainties in product yields associated with the range of NO3 radical concentrations assumed present is relatively small for aldehydes, as is the decrease in yield of the one carbon hot biradical. Larger uncertainties occur for ketones. Significant decreases in yields occur for larger hot biradicals, especially the branched-chain hot radicals in the presence of NO3 radicals.  相似文献   

15.
In this paper we quantify the CH4, CO2 and NO x emissions during routine operations at a major oil and gas production facility, Prudhoe Bay, Alaska, using the concentrations of combustion by products measured at the NOAA-CMDL observatory at Barrow, Alaska and fuel consumption data from Prudhoe Bay. During the 1989 and 1990 measurement campaigns, 10 periods (called events) were unambiguously identified where surface winds carry the Prudhoe Bay emissions to Barrow (approximately 300 km). The events ranged in duration from 8–48 h and bring ambient air masses containing substantially elevated concentrations of CH4, CO2 and NO y to Barrow. Using the slope of the observed CH4 vs CO2 concentrations during the events and the CO2 emissions based on reported fuel consumption data, we calculate annual CH4 emissions of (24+/–8)×103 metric tons from the facility. In a similar manner, the annual NO x emissions are calculated to be (12+/–4)×103 metric tons, which is in agreement with an independently determined value. The calculated CH4 emissions represent the amount released during routine operations including leakage. However this quantity would not include CH4 released during non-routine operations, such as from venting or gas flaring.  相似文献   

16.
Results from numerical investigations regarding the exchange of HNO3, NH3, and NH4NO3 between the atmosphere and the biosphere are presented. The investigations were performed with a modified inferential method which is based on the generally accepted micrometeorological ideas of the transfer of momentum, sensible heat and matter near the Earth's surface and the chemical reactions among these nitrogen compounds. This modified inferential method calculates the micrometeorological quantities (such as the friction velocity and the fluxes of sensible and latent heat), the height-invariant fluxes of the composed chemically conservative trace species with group concentrationsc 1=[HNO3]+[NH4NO3] (total nitrate),c 2=[NH3]+[NH4NO3] (total ammonia), andc 3=[HNO3]-[NH3] as well as the fluxes of the individual nitrogen compounds. The parameterization of the fluxes is based on the flux-gradient relationships in the turbulent region of the atmospheric surface layer. The modified inferential method requires only the data of wind velocity, temperature, humidity and concentrations (HNO3, NH3, and NH4NO3) measured at a reference height by stations of a monitoring network.  相似文献   

17.
Simultaneous measurements of peroxy and nitrate radicals at Schauinsland   总被引：3，自引：0，他引：3  
We present simultaneous field measurements of NO3 and peroxy radicals made at night in a forested area (Schauinsland, Black Forest, 48° N, 8° N, 1150 ASL), together with measurements of CO, O3, NO x , NO y , and hydrocarbons, as well as meteorological parameters. NO2, NO3, HO2, and (RO2) radicals are detected with matrix isolation/electron spin resonance (MIESR). NO3 and HO2 were found to be present in the range of 0–10 ppt, whilst organic peroxy radicals reached concentrations of 40 ppt. NO3, RO2, and HO2 exhibited strong variations, in contrast to the almost constant values of the longer lived trace gases. The data suggest anticorrelation between NO3 and RO2 radical concentrations at night.The measured trace gas set allows the calculation of NO3 and peroxy radical concentrations, using a chemical box model. From these simulations, it is concluded that the observed anthropogenic hydrocarbons are not sufficient to explain the observed RO2 concentrations. The chemical budget of both NO3 and RO2 radicals can be understood if emissions of monoterpenes are included. The measured HO2 can only be explained by the model, when NO concentrations at night of around 5 ppt are assumed to be present. The presence of HO2 radicals implies the presence of hydroxyl radicals at night in concentrations of up to 105 cm–3.  相似文献   

18.
Gaseous nitrogen compounds (NO x , NO y , NH3, N2O) were measured at ground level in smoke plumes of prescribed savanna fires in Lamto, in the southern Ivory Coast, during the FOS/DECAFE experiment in January 1991. During the flaming phase, the linear regression between [NO x ] and [CO2] (differences in concentration between smoke plumes and atmosheric background) results volumic emission ratio [NO x ]/[CO2]=1.37×10–3 with only slight differences between heading and backing fires. Nearly 90% of the nitrogen oxides are emitted as NO. Average emission ratios of other compounds are: 1.91, 0.047, and 0.145×10–3 for NO y , NH3 and N2O, respectively. The emission ratios obtained during this field experiment are compred with corresponding values measured during former experiments with the same plant species in combustion chambers. An accurate determination of both the biomass actually burned and of the plant nitrogen content, allows an assessment of emission fluxes of N-compounds from Guinean savanna burns. Preliminary results dealing with the influence of fire on biogenic emissions from soils are also reported.  相似文献   

19.
Direct measurements of nitrogen oxides and ozone fluxes over grassland   总被引：1，自引：0，他引：1  
Using the eddy correlation method, fluxes of nitric oxide, nitrogen dioxide, ozone, water, and sensible heat were measured at a site 20 km north of Denver, Colorado over mature crested wheat grass, 0.75 m high in late June and early July. During this period the weather was fair with no synoptic disturbances. In the early morning a well-mixed diluted urban pollution plume traversed the site, by late morning aged pollution had mixed downward into the local boundary layer, and by afternoon the air came from a relatively unpolluted area of the high plains. The mean trace gas concentrations reflect this repeated pattern of local air flow. The fluxes of the trace gases were influenced both by the variation of the means and by other factors including temperature and biological activity. Ozone fluxes were found to be always negative and proportional to the mean, with an average deposition velocity for this case of about 0.006 m s-1. For the oxides of nitrogen this simple treatment was not appropriate. Both deposition and emission were observed, generally deposition predominated in the morning and emission in the afternoon with observed variations in the fluxes of NOx=NO+NO2 from –0.3 to +0.2 ppbv m s-1.The National Center for Atmospheric Research is sponsored by the National Science Foundation  相似文献   

20.
Oak pollen concentrations over the Houston-Galveston-Brazoria (HGB) area in southeastern Texas were modeled and evaluated against in-situ data. We modified the Community Multi-scale Air Quality (CMAQ) model to include oak pollen emission, dispersion, and deposition. The Oak Pollen Emission Model (OPEM) calculated gridded oak pollen emissions, which are based on a parameterized equation considering a plant-specific factor (C e ), surface characteristics, and meteorology. The simulation period was chosen to be February 21 to April 30 in the spring of 2010, when the observed monthly mean oak pollen concentrations were the highest in six years (2009-2014). The results indicated C e and meteorology played an important role in the calculation of oak pollen emissions. While C e was critical in determining the magnitude of oak pollen emissions, meteorology determined their variability. In particular, the contribution of the meteorology to the variation in oak pollen emissions increased with the oak pollen emission rate. The evaluation results using in-situ surface data revealed that the model underestimated pollen concentrations and was unable to accurately reproduce the peak pollen episodes. The model error was likely due to uncertainty in climatology-based C e used for the estimation of oak pollen emissions and inaccuracy in the wind fields from the Weather Research and Forecast (WRF) model.  相似文献   

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