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1.
Measurements of surface O3, CO, NOx and light NMHCs were made during December 2004 at Hissar, a semi-urban site in the state of Haryana in north-west region of the Indo-Gangetic Plain (IGP). The night-time O3 values were higher when levels of CO, NO and NO2 were lower but almost zero values were observed during the episodes of elevated mixing ratios of CO (above 2000 ppbv) and NOx (above 50 ppbv). Slopes derived from linear fits of O3 versus CO and O3 versus NOx scatter plots were also negative. However, elevated levels of O3 were observed when CO and NOx were in the range of 200–300 ppbv and 20–30 ppbv, respectively. Slope of CO-NOx of about 33 ppbv/ppbv is much larger than that observed in the US and Europe indicating significant impact of incomplete combustion processes emitting higher CO and lesser NOx. Correlations and ratios of these trace gases including NMHCs show dominance of recently emitted pollutants mostly from biomass burning at this site.  相似文献   

2.
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   

3.
Continuous in-situ measurements of surface ozone (O3), carbon monoxide (CO) and oxides of nitrogen (NOx) were conducted at Udaipur city in India during April 2010 to March 2011. We have analyzed the data to investigate both diurnal and seasonal variations in the mixing ratios of trace gases. The diurnal distribution of O3 showed highest values in the afternoon hours and lower values from evening till early morning. The mixing ratios of CO and NOx showed a sharp peak in the morning hours but lowest in the afternoon hours. The daily mean data of O3, CO and NOx varied in the ranges of 5–51 ppbv, 145–795 ppbv and 3–25 ppbv, respectively. The mixing ratios of O3 were highest of 28 ppbv and lowest 19 ppbv during the pre-monsoon and monsoon seasons, respectively. While the mixing ratios of both CO and NOx showed highest and lowest values during the winter and monsoon seasons, respectively. The diurnal pattern of O3 is mainly controlled by the variations in photochemistry and planetary boundary layer (PBL) depth. On the other hand, the seasonality of O3, CO and NOx were governed by the long-range transport associated mainly with the summer and winter monsoon circulations over the Indian subcontinent. The back trajectory data indicate that the seasonal variations in trace gases were caused mainly by the shift in long-range transport pattern. In monsoon season, flow of marine air and negligible presence of biomass burning in India resulted in lowest O3, CO and NOx values. The mixing ratios of CO and NOx show tight correlations during winter and pre-monsoon seasons, while poor correlation in the monsoon season. The emission ratio of ?CO/?NOx showed large seasonal variability but values were lower than those measured over the Indo Gangetic Plains (IGP). The mixing ratios of CO and NOx decreased with the increase in wind speed, while O3 tended to increase with the wind speed. Effects of other meteorological parameters in the distributions of trace gases were also noticed.  相似文献   

4.
We have studied long-term changes in tropospheric NO2 over South India using ground-based observations, and GOME and OMI satellite data. We have found that unlike urban regions, the region between Eastern and Western Ghat mountain ranges experiences statistically significant decreasing trend. There are few ground-based observatories to verify satellite based trends for rural regions. However, using a past study and recent measurements we show a statistically significant decrease in NOX and O3 mixing ratio over a rural location (Gadanki; 13.48° N, 79.18° E) in South India. In the ground-based records of surface NOX, the concentration during 2010–11 is found to be lower by 0.9 ppbv which is nearly 60 % of the values observed during 1994–95. Small but statistically significant decrease in noon-time peak ozone concentration is also observed. Noon-time peak ozone concentration has decreased from 34?±?13 ppbv during 1993–96 to 30?±?15 ppbv during 2010–11. NOX mixing ratios are very low over Gadanki. In spite of low NOX values (0.5 to 2 ppbv during 2010–11), ozone mixing ratios are not significantly low compared to many cities with high NOX. The monthly mean ozone mixing ratio varies from 9 ppbv to 37 ppbv with high values during Spring and low values during late Summer. Using a box-model, we show that presence of VOCs is also very important in addition to NOX in determining ozone levels in rural environment and to explain its seasonal cycle.  相似文献   

5.
Ammonia (NH3) is the most abundant alkaline gas in the atmosphere and plays a key role in atmospheric chemistry. Reliable and high-time-resolution data for gaseous ammonia are necessary to understand the sources and sinks of ammonia gas in ambient air. In the present study, a sensitive and continuous instrument for measuring gaseous ammonia was developed. Ammonia gas in ambient air was collected in an aqueous solution using a counter-current flow tube (CCFT) sampler. Then, ammonium formed in the aqueous solution was detected by the indophenol method. Based on a CCFT length of 50 cm and air flow rate of 1 L/min, the collection efficiency exceeded 98.5 % at an ammonia mixing ratio of up to 120 ppbv. The detection limit of this method was 0.062 ppbv. Interferences from several gases were investigated, and the results showed that the present method was not affected by NOx, O3, SO2, HONO, methylamine, formaldehyde, hydrogen sulfide or a mixture of these gases. The most important result was that only gaseous ammonia was detected in the present method without any interference from the particulate ammonium in ambient air. Comparisons with data based on the dry denuder method indicated that the present method showed good agreement with the denuder method.  相似文献   

6.
An hourly quantification of inorganic water-soluble PM10 ions and corresponding trace gases was performed using the Monitor for AeRosols and Gases in ambient Air (MARGA) at the TROPOS research site in Melpitz, Germany. The data availability amounts to over 80% for the five-year measurement period from 2010 to 2014. Comparisons were performed for the evaluation of the MARGA, resulting in coefficients of determinations (slopes) of 0.91 (0.90) for the measurements against the SO2 gas monitor, 0.84 (0.88), 0.79 (1.39), 0.85 (1.20) for the ACSM NO3 ?, SO4 2? and NH4 + measurements, respectively, and 0.85 (0.65), 0.88 (0.68), 0.91 (0.83), 0.86 (0.82) for the filter measurements of Cl?, NO3 ?, SO4 2? and NH4 +, respectively. A HONO comparison with a batch denuder shows large scatter (R2 = 0.41). The MARGA HNO3 is underestimated compared to a batch and coated denuder with shorter inlets (slopes of 0.16 and 0.08, respectively). Less NH3 was observed in coated denuders for high ambient concentrations. Long-time measurements show clear daily and seasonal variabilities. Potential Source Contribution Function (PSCF) analysis indicates the emission area of particulate ions Cl?, NO3 ?, SO4 2?, NH4 +, K+ and gaseous SO2 to lie in eastern European countries, predominantly in wintertime. Coarse mode sea salt particles are transported from the North Sea to Melpitz. The particles at Melpitz are nearly neutralised with a mean molar ratio of 0.90 for the five-year study. A slight increase of the neutralization ratio over the last three years indicates a stronger decrease of the anthropogenically emitted NO3 ? and SO4 2? compared to NH4 +.  相似文献   

7.
Measurements of NOx,y were made at Alert, Nunavut, Canada (82.5° N, 62.3° W) during surface layer ozone depletion events. In spring 1998, depletion events were rare and occurred under variable actinic flux, ice fog, and snowfall conditions. NOy changed by less than 10% between normal, partially depleted, and nearly completely depleted ozone air masses. The observation of a diurnal variation in NOx under continuous sunlight supports a source from the snowpack but with rapid conversion to nitrogen reservoirs that are primarily deposited to the surface or airborne ice crystals. It was unclear whether NOx was reduced or enhanced in different stages of the ozone depletion chemistry because of variations in solar and ambient conditions. Because ozone was depleted from 15–20 ppbv to less than 1 ppbv in just over a day in one event it is apparent that the surface source of NOx did not grossly inhibit the removal of ozone. In another case ozone was shown to be destroyed to less than the 0.5 ppbv detection limit of the instrument. However, simple model calculations show that the rate of depletion of ozone and its final steady-state abundance depend sensitively on the strength of the surface source of NOx due to competition from ozone production involving NOx and peroxy radicals. The behavior of the NO/NO2 ratio was qualitatively consistent with enhanced BrO during the period of active ozone destruction. The model is also used to emphasize that the diurnal partitioning of BrOx during ozone depletion events is sensitive to even sub ppbv variations in O3.  相似文献   

8.
During a 3-year study, gaseous hydrogenperoxide (H2O2) concentrations were measuredas part of the SANA project at the Melpitz FieldResearch Station and in the city of Leipzig. Typicaldaily mean H2O2 mixing ratios on sunny dayswere 0.15 to 0.25 ppbv with maximum values of 0.3 to0.5 ppbv at Melpitz, and 0.3 to 0.6 ppbv with maximumvalues of 0.4 to 1.0 ppbv in Leipzig. Over the entireperiod of the project the maximum hourly mean valueswere 2.1 ppbv and 5.3 ppbv in Melpitz and Leipzig,respectively. The data were not complete enough to show a trend.Linear regression analysis shows, that ozone(O3), temperature and solar radiation arepositively correlated with H2O2, whereasnitrogen oxides (NOx), carbon monoxide (CO) andrelative humidity are negatively correlated. Negativecorrelation between H2O2 and CO is caused byjoint occurrence of CO with NOx in exhaust gases.Negative correlation between H2O2 andrelative humidity is not necessarily in contradictionto the accelerating effect of water vapour onH2O2 formation. The strong positivecorrelation of H2O2 with the dew pointdifference however seems to better reflect theinfluence of water vapour. Multiple linear regression analysis (MLRA) of thecomponents measured, indicates the great influence of CO on the formation of H2O2 in the gasphase.  相似文献   

9.
Ambient gas phase nitrous acid (HONO) has been measured by Tunable Diode Laser Absorption Spectroscopy with sub-ppbv detection limits. An R-branch line in the 1263.4 cm–1 3 band was found tobe free of interference and suitable for ambient HONO measurements. Nitrous acid was measured during the night and early morning at an urban site in Toronto, Canada, during the summer of 1998. Average mixing ratios, integrated over 30 minutes, ranged from below the minimum detection limit of 300 pptv to 1.9 ppbv, with the highest concentrations observed during the early morning hours. During the night of 19 June 1998, the concentration of HONO increased by as much as 0.5 ppbv/hr. The usual decrease in HONO after sunrise was delayed by a few hours, possibly due to a combination of an increase in the production rate of HONO with rush hour, and attenuation of the early morning light by high NO2 within the aerosol fog/haze.  相似文献   

10.
Simultaneous ozone measurements were made at a rural site, 25 km SSW of the city of Jerusalem, and in the center of the city during a period of 28 months. The ozone data were supplemented by SO2, NO/NO x ,and meteorological measurements at both sites. Elevated ozone concentrations were recorded at the rural site, mostly during the spring months (May and June) during which the monthly averages and the monthly averages of the daily 30 min maximum levels equalled those measured in the city. During the summer months, both average and peak levels were lower at the rural site by 20 and 35 ppb. The increased ozone levels at the rural site were accompanied by a parallel increase of SO2 and NO x ,suggesting hat the excess ozone at the rural site is a result of a transformation during transport of air pollutants from coastal sources.  相似文献   

11.
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   

12.
The objectives of this study were to identify species and levels of volatile organic compounds (VOCs), and determine their oxidation capacity in the rural atmosphere of western Senegal. A field study was conducted to obtain air samples during September 14 and September 15, 2006 for analyses of VOCs. Methanol, acetone, and acetaldehyde were the most abundant detected chemical species and their maximum mixing ratios reached 6 parts per billion on a volume basis (ppbv). Local emission sources such as firewood and charcoal burning strongly influenced VOC concentrations. The VOC concentrations exhibited little temporal variations due to the low reactivity with hydroxyl radicals, with reactivity values ranging from 0.001 to 2.6 s−1. The conditions in this rural site were rather clean. Low ambient NO x levels limited ozone production. Nitrogen oxide (NO x ) levels reached values less than 2 ppbv and maximum VOC/NO x ratios reached 60 ppbvC/ppbv, with an overall average of 2.4 ± 4.5 ppbvC/ppbv. This indicates that the rural western Senegal region is NO x limited in terms of oxidant formation potential. Therefore, during the study period photochemical ozone production became limited due to low ambient NO x levels. The estimated ozone formation reactivity for VOCs was low and ranged between −5.5 mol of ozone/mol of benzaldehyde to 0.6 mol/mol of anthropogenic dienes.  相似文献   

13.
Measurements of atmospheric composition have been made over a remote rainforest landscape. A box model has previously been demonstrated to model the observed daytime chemistry well. However the box model is unable to explain the nocturnal measurements of relatively high [NO] and [O3], but relatively low observed [NO2]. It is shown that a one-dimensional (1-D) column model with simple O3-NOx chemistry and a simple representation of vertical transport is able to explain the observed nocturnal concentrations and predict the likely vertical profiles of these species in the nocturnal boundary layer (NBL). Concentrations of tracers carried over from the end of the night can affect the atmospheric chemistry of the following day. To ascertain the anomaly introduced by using the box model to represent the NBL, vertically-averaged NBL concentrations at the end of the night are compared between the 1-D model and the box model. It is found that, under low to medium [NOx] conditions (NOx?<?1 ppbv), a simple parametrisation can be used to modify the box model deposition velocity of ozone, in order to achieve good agreement between the box and 1-D models for these end-of-night concentrations of NOx and O3. This parametrisation would could also be used in global climate-chemistry models with limited vertical resolution near the surface. Box-model results for the following day differ substantially if this effective nocturnal deposition velocity for ozone is implemented; for instance, there is a 9% increase in the following days peak ozone concentration. However under medium to high [NOx] conditions (NOx > 1 ppbv), the effect on the chemistry due to the vertical distribution of the species means no box model can adequately represent chemistry in the NBL without modifying reaction rate coefficients.  相似文献   

14.
Measurements of NO2, HCHO, and H2O2 were made by the highly specific method of mid infra-red absorption spectroscopy using tunable diode lasers (TDLAS) during the 1988 Polarstern expedition. The TDLAS data are compared to those obtained during the cruise using less direct methods. Southern Hemisphere NO2 levels suggest nett photochemical destruction of O3 in the boundary layer. Northern Hemisphere HCHO averaged 0.47±0.2 ppbv; the HCHO measurements are used in a simple calculation to estimate OH noontime maxima of 3–6×106 cm-3.  相似文献   

15.
A small, lightweight (1.5 kg) and fast-response ozone sensor for direct eddy flux measurements has been built. The basis for detection is the chemiluminescence of an organic dye adsorbed on dry silica gel in the reaction with ozone. The chemiluminescence is monitored with a cheap and small blue-sensitive photomultiplier. At a flow rate of 100 l min-1 the ozone sensor has a 90% response time of significantly better than 0.1 s with a detection limit lower than 50 ppt at S/N=3. There are no interferences from other atmospheric trace gases like NOx, H2O2 and PAN. Water vapour and SO2 enhance the chemiluminescence efficiency of the ozone sensor. Since their response times are 22 seconds and 30 minutes, respectively, no correlation between rapid ozone fluctuations and those of these two trace gases is noticed by the ozone sensor when operating at a frequency of 10 Hz.The ozone sensor was tested for several weeks in continuous measurements of ozone fluxes and deposition velocities over different croplands using the eddy correlation technique. Good agreement was found between ozone dry deposition velocities derived from profile measurements and by eddy correlation.  相似文献   

16.
In July 1974 an NO/O3 chemiluminescent instrument was used to obtain measurements of NO in the stratosphere during two balloon flights launched from Churchill (59°N, 95°W). On the first flight, an altitude profile was obtained in which the NO volume mixing ratio was observed to increase from 0.3 to 2.7 ppbv between 19 and 29.5 km. On the second flight, the mixing ratio was observed to increase from 0.25 to 2.7 ppbv between 19 and 29 km and to remain almost constant at about 2.7 ppbv from 29 to 34.5 km. On this flight, the sunset decay of NO was also obtained while the payload was at a constant float altitude of 34.5 km. These decay measurements are compared satisfactorily with the results obtained from a time dependent stratospheric model.  相似文献   

17.
In the present paper, we have characterized the ambient ammonia over Delhi along with other trace gases (NH3, NO, NO2, SO2 and CO) and particulates (PM2.5 and PM10) measured during December 2011 to June 2012. The average mixing ratios of ambient NH3, NO, NO2, SO2 and CO were recorded as 21.2 ± 5.4, 19.5 ± 4.9, 17.4 ± 1.4, 1.7 ± 0.5 ppb and 1.6 ± 0.7 ppm, respectively, during winter, whereas the average mixing ratios of ambient NH3, NO, NO2, SO2 and CO were recorded as 20.8 ± 4.7, 21.7 ± 6.3, 16.8 ± 3.1, 2.2 ± 0.8 ppb and 1.8 ± 0.9 ppm, respectively, during summer. In the present case, non-significant seasonal and diurnal variations of NH3, NO, NO2, SO2 and CO were observed during both the seasons. The average monthly NH3/NH4 + ratios varied from 0.28 to 2.56 with an average value of 1.46 in winter. The higher NH3/NH4 + ratio (3.5) observed in summer indicates the abundance of NH3 in the atmosphere during summer. The higher fraction of particulate NH4 + observed in winter than summer attributes to the conversion of gaseous NH3 into NH4 +. The results emphasized that the traffic could be one of the significant sources of ambient NH3 at the urban site of Delhi as illustrated by positive correlations of NH3 with traffic-related pollutants (NO, NO2 and CO). Surface wind analysis and wind directions also support the roadside traffic and agricultural activities at the nearby area indicating possible major sources of ambient NH3 at the study site.  相似文献   

18.
Compact two-channel IR radiometers for solar occultation experiments have been constructed in order to measure concentration profiles of stratospheric trace gases. The instruments can be used as filter-or gas correlation-type radiometers depending on the trace gas under investigation. Within the LIMS correlative measurement program, balloon flights were performed with a payload of up to four of these two-channel radiometers. From the gas correlation-type measurements, profiles of the trace gas NO2 are inferred for the altitude region between about 20 km and the balloon float level. The data evaluation also includes a comprehensive analysis of the error sources and their effect on the accuracy of the NO2 profiles. The derived profiles are compared among themselves and are assessed against the observations of other authors by accounting for the diurnal, latitudinal and seasonal changes of NO2. As a by-product of our measurements, the mean absorption of the O2 collision-induced band at 6.4 m was determined within the range of the interference filter used and compared with calculations based on known absorption coefficients.  相似文献   

19.
Ambient particulate sulfate measurements have been intermittently performed at a rural site in Israel over a period of more than two years. Concurrent measurements of ambient pollutants (SO2, NO–NOx, and O3), as well as meteorological data, were also carried out. The daily data included four particulate sulfate samples representing four successive 6 h accumulating periods. The measured concentrations of sulfate ions ranged from a low 2 g m-3 observed during the winter season to a high of >50 g m-3 obtained during the summer. Little correlation was obtained between the sulfate concentration and either O3 or SO2, although sulfate and O3 showed a similar diurnal and annual trend. Based on the data distribution and on a photochemical model, it was concluded that a large part of the particulate sulfate observed at the eastern coast of the Mediterranean Sea must be related to long-range transport from distant sources.  相似文献   

20.
The seasonal and diurnal variations of ozone mixing ratios have been observed at Niwot Ridge. Colorado. The ozone mixing ratios have been correlated with the NO x (NO+NO2) mixing ratios measured concurrently at the site. The seasonal and diurnal variations in O3 can be reasonably well understood by considering photochemistry and transport. In the winter there is no apparent systematic diurnal variation in the O3 mixing ratio because there is little diurnal change of transport and a slow photochemistry. In the summer, the O3 levels at the site are suppressed at night due to the presence of a nocturnal inversion layer that isolated ozone near the surface, where it is destroyed. Ozone is observed to increase in the summer during the day. The increases in ozone correlate with increasing NO x levels, as well as with the levels of other compounds of anthropogenic origin. We interpret this correlation as in-situ or in-transit photochemical production of ozone from these precursors that are transported to our site. The levels of ozone recorded approach 100 ppbv at NO x mixing ratios of approximately 3 ppbv. Calculations made using a simple clean tropospheric chemical model are consistent with the NO x -related trend observed for the daytime ozone mixing ratio. However, the chemistry, which does not include nonmethane hydrocarbon photochemistry, underestimates the observed O3 production.  相似文献   

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