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1.
Field measurements of NO and NO2 emissions from soils have been performed in Finthen near Mainz (F.R.G.) and in Utrera near Seville (Spain). The applied method employed a flow box coupled with a chemiluminescent NO x detector allowing the determination of minimum flux rates of 2 g N m-2 h-1 for NO and 3 g m-2 h-1 for NO2.The NO and NO2 flux rates were found to be strongly dependent on soil surface temperatures and showed strong daily variations with maximum values during the early afternoon and minimum values during the early morning. Between the daily variation patterns of NO and NO2, there was a time lag of about 2 h which seem to be due to the different physico-chemical properties of NO and NO2. The apparent activation energy of NO emission calculated from the Arrhenius equation ranged between 44 and 103 kJ per mole. The NO and NO2 emission rates were positively correlated with soil moisture in the upper soil layer.The measurements carried out in August in Finthen clearly indicate the establishment of NO and NO2 equilibrium mixing ratios which appeared to be on the order of 20 ppbv for NO and 10 ppbv for NO2. The soil acted as a net sink for ambient air NO and NO2 mixing ratios higher than the equilibrium values and a net source for NO and NO2 mixing ratios lower than the equilibrium values. This behaviour as well as the observation of equilibrium mixing ratios clearly indicate that NO and NO2 are formed and destroyed concurrently in the soil.Average flux rates measured on bare unfertilized soils were about 10 g N m-2 h-1 for NO2 and 8 g N m-2 h-1 for NO. The NO and NO2 flux rates were significantly reduced on plant covered soil plots. In some cases, the flux rates of both gases became negative indicating that the vegetation may act as a sink for atmospheric NO and NO2.Application of mineral fertilizers increased the NO and NO2 emission rates. Highest emission rates were observed for urea followed by NH4Cl, NH4NO3 and NaNO3. The fertilizer loss rates ranged from 0.1% for NaNO3 to 5.4% for urea. Vegetation cover substantially reduced the fertilizer loss rate.The total NO x emission from soil is estimated to be 11 Tg N yr-1. This figure is an upper limit and includes the emission of 7 Tg N yr-1 from natural unfertilized soils, 2 Tg N yr-1 from fertilized soils as well as 2 Tg N yr-1 from animal excreta. Despite its speculative character, this estimation indicates that NO x emission by soil is important for tropospheric chemistry especially in remote areas where the NO x production by other sources is comparatively small.  相似文献   

2.
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   

3.
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   

4.
Continuous measurements of surface ozone (O3), NOx (NO + NO2) and meteorological parameters have been made in Kannur (11.9?°N, 75.4?°E, 5?m asl), India from November 2009 to October 2010. It was observed that O3 and NOx showed distinct diurnal and seasonal variabilities at this site. The annual average diurnal profile of O3 showed a peak of (30.3?±?10.4) ppbv in the late afternoon and a minimum of (3.2?±?0.7) ppbv in the early morning. The maximum value of O3 mixing ratio was observed in winter (44?±?3.1) ppbv and minimum during monsoon (18.46?±?3.5) ppbv. The rate of production of O3 was found to be higher in December (10.1?ppbv/h) and lower in July (1.8?ppbv/h) during the time interval 0800?C1000?h. A correlation coefficient of 0.52 for the relationship between O3 and [NO2]/[NO] reveals the role of NO2 photolysis that generates O3 at this site. The correlation between O3 and meteorological parameters indicate the influence of seasonal changes on O3 production. Investigations were further extended to explore the week day weekend variations in O3 mixing ratio at an urban site reveals the enhancement of O3. The variations of O3 mixing ratio with seasonal air mass flows were elucidated with the aid of backward air trajectories. This study also indicates how vapor phase organic species present in the ambient air at this location may influence the complex chemistry involving (VOCs) that enhances the production of O3 at this location.  相似文献   

5.
In scintillometry Monin–Obukhov similarity theory (MOST) is used to calculate the surface sensible heat flux from the structure parameter of temperature (CT2){(C_{T^2})} . In order to prevent saturation a scintillometer can be installed at an elevated level. However, in that case the observation level might be located outside the atmospheric surface layer (ASL) and thus the validity of MOST questioned. Therefore, we examine two concepts to determine the turbulent surface sensible heat flux from the structure parameter at elevated levels with data obtained at 60-m height on the Cabauw tower (the Netherlands). In the first concept (MOSTs) CT2{C_{T^2}} is still scaled with the surface flux, whereas in the second (MOSTl) CT2{C_{T^2}} is scaled with the local sensible heat flux. The CT2{C_{T^2}} obtained from both concepts is compared with direct observations of CT2{C_{T^2}} using a sonic anemometer/thermometer. In the afternoon (when the measurement height is located within the ASL) both concepts give results that are comparable to the directly observed values of CT2{C_{T^2}} . In the morning (data outside the ASL), our data do not unequivocally support either of the two concepts. First, the peak in CT2{C_{T^2}} that occurs when the measurement height is located in the entrainment zone disqualifies the use of MOST. Second, during the morning transition, local scaling shows the correct pattern (zero flux and a minimum in CT2{C_{T^2}}) but underestimates CT2{C_{T^2}} by a factor of ten. Third, from the best linear fit a we found that the slope of MOSTl gave better results, whereas the offset is closer to zero for MOSTs. Further, the correlation between the direct observations and MOST-scaled results is low and similar for the two concepts. In the end, we conclude that MOST is not applicable for the morning hours when the observation level is above the ASL.  相似文献   

6.
The photodissociation coefficient, J NO2 of NO2 in the atmosphere was calculated at 235 and 298 K using the measured temperature dependences of the absorption cross-sections and quantum yields. These calculations gave a ratio J NO2(298 K)/J NO2(235 K)=1.155±0.010 which is only weakly dependent on altitude, surface albedo and solar zenith angle.  相似文献   

7.
Barnes  I.  Bastian  V.  Becker  K. H.  Fink  E. H.  Nelsen  W. 《Journal of Atmospheric Chemistry》1986,4(4):445-466
The reactions of OH radicals with SO2, H2S, thiophenol, and a series of aliphatic thiols (1–5 C-atoms) have been investigated in 201 and 381 reaction chambers at 1 atm total pressure and 300 K using a competitive kinetic technique. Initially, OH radicals were produced by photolysis of CH3ONO/NO mixtures in air. Applying this OH source rate constants for OH with SO2, H2S, and thiophenol in synthetic air were determined to be (1.1±0.2)×10-12, (5.5±0.8)×10-12 and (1.1±0.2)×10-11 cm3 s-1, respectively. However, when this method was applied to the aliphatic thiols the rate constants obtained were found to be dependent on the partial pressures of O2 and NO. These effects have been attributed to the built-up of a radical species, not yet identified, which leads to uncontrolled chain reactions in the system. Using the photolysis of H2O2 at wavelengths greater than 260 nm as the OH source in 1 atm N2, rate constants for the 1–5 aliphatic thiols in the range 2.9 to 5.6×10-11 cm3 s-1 were obtained. The rate constants obtained in the present study are compared with recent literature values.  相似文献   

8.
Atmospheric hydroxyl (OH), hydroperoxy (HO2), total peroxy (HO2 and organic peroxy radicals, RO2) mixing ratios and OH reactivity (first order OH loss rate) were measured at a rural site in central Pennsylvania during May and June 2002. OH and HO2 mixing ratios were measured with laser induced fluorescence (LIF); HO2 + RO2 mixing ratios were measured with chemical ionization mass spectrometry (CIMS). The daytime maximum mixing ratios were up to 0.6 parts per trillion by volume (pptv) for OH, 30 pptv for HO2, and 45 pptv for HO2 + RO2. A parameterized RACM (Regional Atmospheric Chemistry Mechanism) box model was used to predict steady state OH, HO2 and HO2 + RO2 concentrations by constraining the model to the measured OH reactivity and previously measured volatile organic compound (VOC) distributions. The averaged model calculations are generally in good agreement with the observations. For OH, the model matched the observations for day and night, with an average observed-to-modeled ratio of 0.80. In previous studies such as PROPHET98, nighttime NO was near 0 pptv and observed nighttime OH was significantly larger than modeled OH. In this study, nighttime observed and modeled OH agree to within measurement and model uncertainties because the main source of the nighttime OH was the reaction HO2 + NO → OH + NO2, with the NO being continually emitted from the surrounding fertilized corn field. The observed-to-modeled ratio for HO2 is 1.0 on average, although daytime HO2 is underpredicted by a factor of 1.2 and nighttime HO2 is over-predicted by a factor of ∼2. The average measured and modeled HO2 + RO2 agree well during daytime, but the modeled value is about twice the measured value during nighttime. While measured HO2 + RO2 values agree with modeled values for NO mixing ratios less than a few parts per billion by volume (ppbv), it increases substantially above the expected value for NO greater than a few ppbv. This observation of the higher-than-expected HO2 + RO2 with the CIMS technique confirms the observed increase of HO2 above expected values at higher NO mixing ratios in HO2 measurements with the LIF technique. The maximum instantaneous O3 production rate calculated from HO2 and RO2 reactions with NO was as high as 10–15 ppb h−1 at midday; the total daily O3 production varied from 13 to 113 ppbv d−1 and was 48 ppbv d−1 on average during this campaign.  相似文献   

9.
郭凤霞  陈聪 《大气科学》2012,36(4):713-721
为了解闪电对对流层上部NOx的贡献,本文利用美国全球水资源和气候中心（GHRC）提供的1995年4月~2005年12月的闪电卫星格点资料及高层大气研究卫星 (UARS) 上的卤素掩星试验装置 (HALOE) 1991年10 月~2005 年11月的观测资料,分析了中国地区闪电与对流层上部NOx体积混合比的时空分布特征及两者的相关性.结果表明:中国地区闪电和对流层上部的NOx在季节分布、年际分布和空间分布上保持很好的一致性,闪电是对流层上部NOx的重要来源;NO极值高度在350 hPa左右,云闪直接产生的NO是极值产生的主要原因,NO2的极值高度在250 hPa左右,因为闪电产生的NO在传输过程中会被氧化成NO2并通过雷暴的垂直输送作用抬升到更高高度;强对流活动有利于NOx的传输,而人类活动产生的NOx一般较难输送到对流层上部,因此闪电多发区的NOx极值较大,所在的高度也较高.  相似文献   

10.
A multi-layer deposited ice film was prepared through water vapor deposition on a Ni plate in a vacuum chamber at 90 K, and was used as it was or after annealing at 140 K. NO2 was adsorbed as N2O4 approximately 90 K on the ice film prepared as above, and irradiated by 193 nm excimer laser light. The time-of-flight (TOF) spectra of the desorbed species, i.e., NO2, NO, O2 and O, were measured by a quadrupole mass spectrometer. The photochemical process obeyed an one-photon process. The relative yields of the products and their TOF spectra were dependent on the preparation condition of the ice film and also varied with the continuation of the laser irradiation. From the ice film annealed at 140 K, NO2, NO and O2 were desorbed with an approximate ratio of 1:1:0.01. From the non-annealed film, the relative yield of NO2 was much smaller than that of NO. The TOF spectrum of NO from the non-annealed ice film consisted of distinctly different two components corresponding to the 1700 and 100 K translational temperature, respectively. The fast component was lost when additional ice was deposited on the adsorbed N2O4. NO was supposed to be a predissociation product from the electronically excited NO2 prepared through the photodissociation of N2O4.  相似文献   

11.
The chemical reactivity of NO and NO2 is so rapid that their fluxes and concentrations can be considerably modified from that expected for conserved variables in the atmospheric surface layer, even as low as a meter above the surface. Fitzjarrald and Lenschow (1983) have calculated flux and mean concentration profiles for NO, NO2 and O3 in the surface layer using numerical techniques. However, their solutions do not approach the photostationary state at large heights. Here we solve a simpler set of equations analytically (i.e. we assume a constant O3 concentration and neutral hydrodynamic stability), and are able to show how the flux profiles behave at large heights assuming that the concentrations approach their photostationary values. We find, for example, that at large heights the ratio of the flux of NO to that of NO2 is equal to the ratio of their concentrations. These results are relevant to estimating surface fluxes of NO and NO2, and are most applicable to nonurban environments where NO and NO2 concentrations are usually much less than O3 concentration.The National Center for Atmospheric Research is sponsored by the National Science Foundation.  相似文献   

12.
Continuous measurements of ozone and its precursors including NO, NO2, and CO at an urban site (32°03′N, 118°44′E) in Nanjing, China during the period from January 2000 to February 2003 are presented. The effects of local meteorological conditions and distant transports associated with seasonal changed Asian monsoons on the temporal variations of O3 and its precursors are studied by statistical, backward trajectory, and episode analyses. The diurnal variation in O3 shows high concentrations during daytime and low concentrations during late night and early morning, while the precursors show high concentrations during night and early morning and low concentrations during daytime. The diurnal variations in air pollutants are closely related to those in local meteorological conditions. Both temperature and wind speed have significant positive correlations with O3 and significant negative correlations with the precursors. Relative humidity has a significant negative correlation with O3 and significant positive correlations with the precursors. The seasonal variation in O3 shows low concentrations in late autumn and winter and high concentrations in late spring and early summer, while the precursors show high concentrations in late autumn and winter and low concentrations in summer. Local mobile and stationary sources make a great contribution to the precursors, but distant transports also play a very important role in the seasonal variations of the air pollutants. The distant transport associated with the southeastern maritime monsoon contributes substantially to the O3 because the originally clean maritime air mass is polluted when passing over the highly industrialized and urbanized areas in the Yangtze River Delta. The high frequency of this type of air mass in summer causes the fact that a common seasonal characteristic of surface O3 in East Asia, summer minimum, is not observed at this site. The distant transports associated with the northern continental monsoons that dominate in autumn and winter are related to the high concentrations of the precursors in these two seasons. This study can contribute to a better understanding of the O3 pollution in vast inland of China affected by meteorological conditions and the rapid urbanization and industrialization.  相似文献   

13.
A stainless steel soil corer which was filled with homogenized soil was used to measure the flux (J) of NO between soil and atmosphere and the vertical profile of the NO mixing ratios (m) in the soil atmosphere, both as function of the NO mixing ratio (mm a ) in the atmosphere of the headspace. The NO emission flux decreased linearly with increasing NO mixing ratio and turned into a deposition flux after passage of the compensation point (m c) at about 400 ppbv NO. Almost the same compensation point was obtained when the turnover of NO was measured in flask-incubated soil samples as function of the NO mixing ratio. The flux (J) of NO at the soil-atmosphere interface was calculated from the production rate (P) of NO and the NO uptake rate constant (k) that were measured in these flask-incubated soil samples using the diffusion model of Galbally and Johansson (1989). The calculated fluxes agreed within <15% with those actually measured. The vertical profiles of NO were fitted to an exponential function and analyzed by Fick's first law of diffusion. The shape of the profiles indicated a net production of NO in the upper 10 cm soil layer when the atmospheric NO mixing ratio was below the compensation point and in a net consumption of NO when the atmospheric NO mixing ratio was above the compensation point. In soil layers below 10 cm depth, the turnover of NO resulted in compensation of production and consumption rates. Measurement of the actual diffusion coefficient using SF6 showed that gas transport in the soil core was not only due to molecular diffusion but in addition due to a bidirectional gas flow. The experimentally determined diffusion coefficient was smaller than that computed from soil porosities, but resulted together with the additional transport term in NO fluxes that were close (< ±15%) to those measured. This is the first comprehensive study of NO concentration profiles and turnover rates in soil providing a theoretical basis for modelling NO fluxes at the soil-atmosphere interface.  相似文献   

14.
Precipitation samples were collected by filtrating bulk sampler in Kitakyushu City, Japan, from January 1988 to December 1990. Volume weighted annual mean of pH was 4.93, but the pH distribution indicated that most probable value lay in the range pH 6.0–6.4. Volume weighted annual mean concentrations of major ionic components were as follows; SO 4 2– : 84.2, NO 3 – : 28.1, Cl–: 86.3, NH 4 + : 45.5, Ca2+: 63.3, Mg2+: 27.0, K+: 3.4, Na+: 69.0 µ eq l–1. The highest concentrations of these ionic components were observed in winter and the lowest occurred in the rainy season. The ratio of ex-SO 4 2– /NO 3 – exhibited the lowest ratio in summer, and the highest ratio in winter. Good correlations were obtained between Cl– and Na+, ex-SO 4 2+ and ex-Ca2+, NO 3 – and ex-Ca2+, and NH 4 + and ex-SO 4 2– , respectively. However, no correlation between Cl– and Na+ with Ca2+ was observed. The relationship of H+ with (ex-SO 4 2– + NO 3 – ) - (ex-Ca2+ + NH 4 + ) indicated positive correlation.  相似文献   

15.
The photochemical oxidation of SO2 in the presence of NO and C3H6 was studied in a 18.2 liter pyrex reactor. When light intensity, irradiation time and SO2 concentration were constant, SO4 2- concentration, derived from the total volume of aerosol produced, peaked when [C3H6]/[NO] was approximately 6.0. Another increase im SO4 2- formation was reached at very high ratios (>50). The experimental observations are consistent with the two SO2 oxidation mechanisms. At low [C3H6]/[NO] ratios, the processes proceed via the HO–SO2 reaction, while at high ratios the O3–C3H6 adduct is assumed to oxidize SO2 to produce SO4 2- aerosols.  相似文献   

16.
Eddy correlation measurements of NO vertical flux were made periodically from October 1983 through June 1984 at a height of eight meters above grass in northeastern Illinois, U.S.A. From 207 data points, each representing a 25 min average, 19 daytime cases and 8 nighttime cases were selected on the basis of steady, nonadvective atmospheric conditions. Each case was represented by a set of data constituting a 3 to 5 hr average. Concentrations of O3, NO, and NO y (from which NO2 was inferred) and local atmospheric and surface conditions also were measured, to provide the information necessary to assess the relative importance of surface deposition, surface emission, and air chemistry on the observed NO flux. On the basis of a linear regression analysis applied with independent variables representing physical, chemical, and biological processes, surface uptake of NO was very small for data primarily collected in the daytime during spring, and measured deposition velocities at a height of 8 m were very small, much smaller than expected for NO2. For the same time period, the surface emission rates of elemental nitrogen in NO were in the range of 1.4 to 4.2 ng m-2 s-1 for moist, unsaturated soils at temperatures near 15° C. These emissions were partially masked in the measured fluxes by rapid in-air chemical reactions involving O3 and NO2. The effects of rapid in-air chemical reactions involving O3 were to decrease the (upward) flux of NO with height. While the information collected at night was too limited to strongly support hypotheses concerning emissions and deposition, a pathway for NO production by reactions involving NO3 and related compounds was indicated. For daytime conditions, this production pathway is not evident, probably because of the relatively strong effects of photochemical reactions involving NO, NO2, and O3.Formerly with the Chemical Technology Division of Argonne National Laboratory and currently affiliated with Bio-Rad Laboratories, Digilab Division, Minneapolis, MN, U.S.A.  相似文献   

17.
The paper presents the importance of the Nocturnal Boundary Layer in driving the diurnal variability of the atmospheric CO2 mixing ratio and the carbon isotope ratio at ground level from an urban station in India. Our observations are the first of their kind from this region. The atmospheric CO2 mixing ratio and the carbon isotopic ratio were measured for both the morning (05:30–07:30 IST) and afternoon time (16:00–18:00 IST) air samples at 5 m above ground level in Bangalore city, Karnataka State (12° 58′ N, 77° 38′ E, masl = 920 m) for a 10 day period during the winter of 2008. We observed a change of ~7% the in CO2 mixing ratio between the morning and afternoon time air samples. A stable isotope analysis of CO2 from morning samples showed a depletion in the carbon isotope ratio by ~2‰ compared to the afternoon samples. Along with the ground-based measurement of air samples, data of radiosonde measurements were also obtained from the Indian Meteorological Department to identify the vertical atmospheric structure at different time in a day. We proposed the presence or absence of the NBL as a controlling factor for the observed variability in the mixing ratio as well as its isotopic composition. Here we used the Keeling model approach to find out the carbon isotope ratio for the local sources. The local sources have further been characterized as anthropogenic and biological respiration (in %) using a two-component mixing model. We also used a vertical mixing model based on the concept of the mixing of isotopically depleted (carbon isotope) “polluted air” (PA) with isotopically enriched “free atmospheric air” (FA) above. Using this modeling approach, the contribution of FA at ground level is being estimated for both the morning and afternoon time air samples.  相似文献   

18.
Intact soils cores were taken with a stainless steel corer from a sandy podzol and a loamy luvisol, and used to measure the flux (J) of NO between soil and atmosphere and the vertical profile of the NO mixing ratios (m) in the soil atmosphere, both as function of the NO mixing ratio (m a) in the atmosphere of the headspace. These measurements were repeated after stepwise excavation of the soil column from the top, e.g. by removing the upper 2 cm soil layer. The gaseous diffusion coefficients of NO in the soil cores were either computed from soil porosity or were determined from experiments using SF6. The NO fluxes (J) that were actually measured at the soil surface were compared to the fluxes which were calculated either from the vertical NO profiles (J c ) or from the NO production and uptake rates (J m ) determined in the excavated soil samples. In the podzol, the actually measured (J) and the calculated (J m , Jm) NO fluxes agreed within a factor of 2. In the luvisol, the measured NO fluxes (J) and those calculated from the vertical NO profiles (J c ) also agreed well, but in the upper 6 cm soil layer the NO fluxes (J m ) calculated from NO production and uptake rates were up to 7 times higher than the measured NO fluxes. This poor agreement was probably due to the inhomogeneous distribution of NO production and consumption processes and the change of diffusivities within the top layers of the luvisol. Indeed, the luvisol showed a pronounced maximum of the NO mixing ratios at about 6 cm depth, whereas the podzol column exhibited a steady and exponential decrease of the NO mixing ratios with depth. The inhomogeneities in the luvisol were confirmed by incubation of the soil cores under anoxic conditions. This treatment resulted in production of NO at several depths indicating a zonation of increased potential activities within the luvisol profile which may have biased the modelling of the NO surface flux from turnover measurements in soil samples. Inhomogeneities could be achieved even in homogenized soil by fertilization with nitrate solution.  相似文献   

19.
The mixing ratios for ozone and NOx (NO+NO2) have been measured at a rural site in the United States. From the seasonal and diurnal trends in the ozone mixing ratio over a wide range of NOx levels, we have drawn certain conclusions concerning the ozone level expected at this site in the absence of local photochemical production of ozone associated with NOx from anthropogenic sources. In the summer (June 1 to September 1), the daily photochemical production of ozone is found to increase in a linear fashion with increasing NOx mixing ratio. For NOx mixing ratios less than 1 part per billion by volume (ppbv), the daily increase is found to be (17±3) [NOx]. In contrast, the winter data (December 1 to March 1) indicate no significant increase in the afternoon ozone level, suggesting that the photochemical production of ozone during the day in winter approximately balances the chemical titration of ozone by NO and other pollutants in the air. The extrapolated intercept corresponding to [NOx]=0 taken from the summer afternoon data is 13% less than that observed from the summer morning data, suggesting a daytime removal mechanism for O3 in summer that is attributed to the effects of both chemistry and surface deposition. No significant difference is observed in the intercepts inferred from the morning and afternoon data taken during the winter.The results contained herein are used to deduce the background ozone level at the measurement site as a function of season. This background is equated with the natural ozone background during winter. However, the summer data suggest that the background ozone level at our site is elevated relative to expected natural ozone levels during the summer even at low NOx levels. Finally, the monthly daytime ozone mixing ratios are reported for 0[NOx]0.2 ppbv, 0.3 ppbv[NOx]0.7 ppbv and 1 ppbv[NOx]. These monthly ozone averages reflect the seasonal ozone dependence on the NOx level.  相似文献   

20.
Ground-based FTIR measurements have been performed in the Arctic summer in July 1993 and June 1994 at 79° N to study the zenith column densities of several trace gases in the undisturbed Arctic summer atmosphere. Zenith column densities of H2O, N2O, HNO3, NO2, NO, ClONO2, ClO, HCl, HF, COF2, OCS, SF6, HCN, CH4, C2H6, C2H2, CO, O3, CFC-12, CFC-22, and CO2 were retrieved by line-by-line calculations. The results are compared with winter and springtime observations measured at the same site, with column densities obtained in the Antarctic summer atmosphere, and with measurements at midlatitudes. For HCl the spectra give lower total zenith columns than expected, but the ratio HF/HCl agrees well with midlatitude literature data. Measurements of ClONO2 give low total columns in agreement with observations at midlatitudes. In the undisturbed atmosphere HCl was found to be in excess of ClONO2. The total columns of HNO3, N2O and the sum of NO and NO2 agree with summer observations in Antarctica. Results for the tropospheric trace gas C2H6 are higher by 250% when compared with Antarctic observations. Contrary to N2O and CH4 the seasonal cycle of C2H6 and C2H2 give much higher total columns in winter/spring compared to the summer observations. This is assigned to transport of polluted airmasses from mid-latitudes into the Arctic.  相似文献   

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