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1.
Abstract

This paper presents the analysis of ambient air concentrations of 10 carbonyl compounds (aldehydes and ketones) measured in the yards of 87 residences in the city of Elizabeth, NJ, throughout 1999–2001. Most of these residences were measured twice in different seasons; the sampling duration was 48 hr each time. The authors observed higher concentrations for most of the measured carbonyl compounds on warmer days, reflecting larger contributions of photochemical reactions on warmer days. The estimated contributions of photochemical production varied substantially across the measured carbonyl compounds and could be as high as 60%. Photochemical activity, however, resulted in a net loss for formaldehyde. The authors used stepwise multiple linear regression models to evaluate the impact of traffic sources and meteorological conditions on carbonyl concentrations using the data collected on colder days (with lower photochemical activities). They found that the concentrations of formal-dehyde, acetaldehyde, acrolein, propionaldehyde, crotonaldehyde, benzaldehyde, glyoxal, and methylglyoxal significantly decreased with increasing distance between a measured residence and one or more major roadways. They also found significant negative associations between concentrations for most of the measured carbonyl compounds and each of the following meteorological parameters: mixing height, wind speed, and precipitation.  相似文献   

2.
The concentrations of C1–C8 carbonyl compounds were measured at two urban sites in Hong Kong from October 1997 to September 2000. The daily total carbonyl concentrations were found to range from 2.4 to 37 μg m−3. Formaldehyde was the most abundant species, which comprised from 36 to 43% of the total detected carbonyls, followed by acetaldehyde (18–21%) and acetone (8–20%). The highest 24-hour average concentrations measured were 10 and 7.7 μg m−3 for formaldehyde and acetaldehyde, respectively. Seasonal and temporal variations in the concentrations of formaldehyde and acetaldehyde were not obvious, but lowest concentrations often occurred from June to August. The mean formaldehyde/acetaldehyde molar ratios at the two sites in summer (2.8±1.1 and 2.5±1.2) were significantly higher (p⩽0.01) than those in winter periods (1.9±0.6 and 2.0±0.6). The phenomena were explained by influences of both photochemical reactions and local meteorological conditions. Better correlations between formaldehyde and acetaldehyde, and between NOx and each of the two major carbonyls were obtained in winter periods indicating direct vehicular emissions were the principal sources. The ambient formaldehyde and acetaldehyde concentrations in the urban atmosphere of Hong Kong were within the normal ranges reported in the literature for other urban sites world-wide.  相似文献   

3.
Twenty-one carbonyl compounds were measured simultaneously at four hotel ballrooms in urban Guangzhou during the autumn, 2002. In each ballroom, measurements were carried out in business hours in the evening (20:30–24:00) on 7 consecutive days without any disturbance of the ballroom's normal operation. Nineteen out of the 21 target carbonyl compounds were identified in indoor and outdoor air. In the outdoor environment, formaldehyde was the most abundant carbonyl, followed by acetaldehyde, and there existed a strong correlation between formaldehyde and acetaldehyde. In the indoor air, however, acetaldehyde was the most abundant carbonyl, its concentrations seemed to be affected significantly by smoking. The indoor concentrations of carbonyls were found higher than their outdoor counterparts with only a few exceptions. Further studies concerning the indoor/outdoor ratios and mutual correlation of the carbonyls indicated that apart from direct emission from indoor materials and infiltration of outdoor air, other anthropogenic sources, e.g. tobacco smoke, also significantly contributed to carbonyl compounds. The possible sources of some high molecular weight carbonyls, e.g. nonanaldehyde, were also discussed briefly. Preliminary estimate of the exposures and risks due to carbonyls in the ballrooms was made, which indicated that long-term exposure in such places might cause increased chance of developing cancers.  相似文献   

4.
Ambient levels of carbonyl compounds and their possible sources, vehicular exhaust and cooking exhaust, were studied at seven places in Guangzhou, including five districts (a residential area, an industrial area, a botanical garden, a downtown area and a semi-rural area), a bus station and a restaurant during the period of June–September 2003. Nineteen carbonyl compounds were identified in the ambient air, of which acetone was the most abundant carbonyl, followed by formaldehyde and acetaldehyde. Only little changes were found in carbonyl concentration levels in the five different districts because of their dispersion and mixture in the atmosphere in summer. The lower correlations between the carbonyls’ concentrations might result from the mixture of carbonyls derived from different sources, including strong photochemical reactions at noon in summer. Formaldehyde and acetaldehyde were the main carbonyls in bus station, while straight-chain carbonyls were comparatively abundant in cooking exhaust. Besides vehicular exhaust, cooking might be another major source of carbonyl compounds in Guangzhou City, especially for high molecular weight carbonyls.  相似文献   

5.
In order to study the daily, weekly, and seasonal patterns and possible origins of air concentrations of volatile organic compounds (VOCs), measurements were taken on a minute-by-minute basis with a PTR-MS in the vicinity of a highway in a semi-urban site near Barcelona. Four periods of the year were chosen and samples were taken under different meteorological conditions and at different phenological stages of the surrounding vegetation. None of the measured VOCs concentrations exceeded air-quality guidelines. The results showed that diurnal, weekly, and seasonal fluctuations in measured VOC concentrations depended on variations in the strength of sources, as well as on photochemical activity and meteorological conditions. There was a decrease in concentrations in most VOCs when mixing depth, photochemical destruction, and wind speed increased at midday. On the other hand, high values of some VOCs occurred at night when the strength of their sinks and the mixing layer decreased. Interestingly, in June, night emissions and concentration peaks of methanol and acetone occurred in periods with dew formation and no wind. VOCs related to anthropogenic emissions presented a weekly pattern of variation with a clear distinction being found between working days and the weekend. The seasonal variation showed higher levels in December for all VOCs, except for isoprene. The thinning of the mixing layer leading to greater concentrations of volatiles and lower wind speeds in winter could account for those higher VOC levels. Benzene and toluene originated mainly from anthropogenic emissions. The sources of acetaldehyde, methanol, and acetone appeared to be mainly biogenic and these compounds were the most abundant of all the measured VOCs. Isoprene concentration patterns suggest a predominantly anthropogenic origin in December and March and a mainly biogenic origin in June and October. All these data provide useful information on the dynamics of VOCs in an area where ozone levels in summer exceed quite often the standard protection thresholds for O3.  相似文献   

6.
Salthammer T  Mentese S 《Chemosphere》2008,73(8):1351-1356
The level of carbonyl compounds in indoor air is crucial due to possible health effects and the high prevalence of their potential sources. Therefore, selecting a convenient and rapid analytical technique for the reliable detection of carbonyl compound concentrations is important. The acetyl acetone (acac) method is a widely used standard procedure for detecting gaseous formaldehyde. For measuring formaldehyde along with other carbonyl compounds, the DNPH-method is commonly applied. The recommended procedure for measuring volatile organic compounds (VOCs) is sampling on Tenax TA, followed by thermal desorption and GC/MS analysis. In this study, different analytical techniques for the quantification of formaldehyde, pentanal, and hexanal are critically compared. It was found that the acac- and DNPH-method are in very good agreement for formaldehyde. In contrast, the DNPH-method significantly underestimates indoor air concentrations of the higher aldehydes in comparison to sampling on Tenax TA, although both methods are strongly correlated. The reported results are part of the EURIMA-WKI study on levels of indoor air pollutants resulting from construction, building materials and interior decoration.  相似文献   

7.
Emissions of carbonyl compounds such as formaldehyde, acetaldehyde, and acrolein are of interest to the scientific and regulatory communities due to their suspected or likely impacts on human health. The present work investigates emissions of carbonyl compounds from nine Class 8 heavy-duty diesel (HDD) tractors and also from nine diesel-powered backup generators (BUGs); the former were chosen because of their ubiquity as an emission source, and the latter because of their proximity to centers of human activity. The HDD tractors were operated on the ARB 4-Mode heavy heavy-duty diesel truck (HHDDT) driving cycle, while the BUGs were operated on the ISO 8178 Type D2 5-mode steady-state cycle and sampled using a mobile emissions laboratory (UCR MEL) equipped with a full-scale dilution tunnel. Samples were analyzed using the SAE930142 (Auto/Oil) method for 11 aldehydes, from formaldehyde to hexanaldehyde, and 2 ketones (acetone and methyl ethyl ketone). Although absolute carbonyl emissions varied widely by BUG, the relative contributions of the different carbonyls were similar (e.g., median: 56% for formaldehyde). A slight increasing trend with engine load was observed for relative formaldehyde contribution, but not for acetaldehyde contribution, for the BUGs. On-road per-mile carbonyl emission factors were a strong function of operating mode of the ARB HHDDT cycle, and found to decrease in the order Creep>Transient>Cruise. This order is qualitatively similar to emission factors for PAHs and n-alkanes determined for the same set of Class 8 diesel tractors in an earlier work. In general, relative carbonyl contributions for the HDD tractors were similar to those for BUGs (e.g., median: 54% for formaldehyde). These results indicate that while engine operating mode and application appear to exert a strong influence on the total absolute mass emission rate of the carbonyls measured, they do not appear to exert as strong an influence on the relative mass emission rates of individual carbonyls.  相似文献   

8.
Personal 48-hr exposures of 15 randomly selected participants as well as microenvironment concentrations in each participant's residence and workplace were measured for 16 carbonyl compounds during summer-fall 1997 as a part of the Air Pollution Exposure Distributions within Adult Urban Populations in Europe (EXPOLIS) study in Helsinki, Finland. When formaldehyde and acetaldehyde were excluded, geometric mean ambient air concentrations outside each participant's residence were less than 1 ppb for all target compounds. Geometric mean residential indoor concentrations of carbonyls were systematically higher than geometric mean personal exposures and indoor workplace concentrations. Additionally, residential indoor/outdoor ratios indicated substantial indoor sources for most target compounds. Carbonyls in residential indoor air correlated significantly, suggesting similar mechanisms of entry into indoor environments. Overall, this study demonstrated the important role of non-traffic-related emissions in the personal exposures of participants in Helsinki and that comprehensive apportionment of population risk to air toxics should include exposure concentrations derived from product emissions and chemical formation in indoor air.  相似文献   

9.
The natural background in the ozone concentration at rural locations in the United States and western Europe has been estimated by use of several approaches. The approaches utilized include the following: (1) historical trends in ozone concentration measurements, (2) recent ozone measurements at remote sites, (3) use of tracers of air originating in the stratosphere or upper troposphere and (4) results from applications of tropospheric photochemical models. While each of these approaches has its own limitations it appears that the natural background of ozone during the warmer months of the year is in the range of 10 to 20 ppb. Most of the ozone originating in the lower stratosphere or upper troposphere is lost by chemical or physical removal processes as well as undergoing dilution by air in the lower troposphere before reaching ground level rural locations. Lower tropospheric photochemical processes, those below 5 km, are likely to account for most of the ozone measured at rural locations during the warmer months of the year.

A key aspect to improved quantitation of the contributions from lower tropospheric photochemical processes to ozone concentrations continues to be more extensive atmospheric measurements of the distribution of reactive species of nitrogen. The emission densities of anthropogenic sources of NOx are known to be highly variable over populated areas of continents as well as between continental areas and the oceans. The emission densities of biogenic sources of NOx are small, likely to be highly variable, but poorly quantitated. These wide variations indicate the need for use of three dimensional tropospheric photochemical models over large continental regions.

Available results do indicate higher efficiencies for ozone formation at lower NOx concentrations, especially below 1 ppb.  相似文献   

10.
Several years of formaldehyde measurements at six rural European sites are compared with EMEP oxidant model calculations. The model results agree well with the measured values both with regard to average seasonal cycles as well as on an episodic day-to-day basis at all sites except for Ispra in Northern Italy. For several of the sites the agreement is better during the summer months whereas the model underestimates the concentrations in winter. The model results show that formaldehyde in summer is mainly controlled by photochemical processes such as reaction with OH, photolysis and formation through NO+peroxy radicals. Furthermore, in spite of the short chemical lifetime of formaldehyde in summer, emission pulses of volatile organic compounds (VOC) and isoprene influence formaldehyde concentrations even 48 h after the emission. These results indicate that formaldehyde is well suited for validating photochemical transport models on a long-range (European) scale. Furthermore, the reasonable agreement between model calculations and measurements for carbonyls presented here, combined with previous findings for non-methane hydrocarbons (NMHC) and evaluation of the condensed EMEP chemical mechanism against a detailed Master chemical mechanism gives encouraging support that the EMEP model describes the main ozone-forming photochemical processes in a reasonable way.  相似文献   

11.
Mohamed MF  Kang D  Aneja VP 《Chemosphere》2002,47(8):863-882
Volatile organic compounds (VOCs) have been determined to be human risk factors in urban environments, as well as primary contributors to the formation of photochemical oxidants. Ambient air quality measurements of 54 VOCs including hydrocarbons, halogenated hydrocarbons and carbonyls were conducted in or near 13 urban locations in the United States during September 1996 to August 1997. Air samples were collected and analyzed in accordance with US Environmental Protection Agency-approved methods. The target compounds most commonly found were benzene, toluene, xylene and ethylbenzene. These aromatic compounds were highly correlated and proportionally related in a manner suggesting that the primary contributors were mobile sources in all the urban locations studied. Concentrations of total hydrocarbons ranged between 1.39 and 11.93 parts per billion, by volume (ppbv). Ambient air levels of halogenated hydrocarbons appeared to exhibit unique spatial variations, and no single factor seemed to explain trends for this group of compounds. The highest halogenated hydrocarbon concentrations ranged from 0.24 ppbv for methylene chloride to 1.22 ppbv for chloromethane. At participating urban locations for the year of data considered, levels of carbonyls were higher than the level of the other organic compound groups, suggesting that emissions from motor vehicles and photochemical reactions strongly influence ambient air concentrations of carbonyls. Of the most prevalent carbonyls, formaldehyde and acetaldehyde were the dominant compounds, ranging from 1.5-7.4 ppbv for formaldehyde, to 0.8-2.7 ppbv for acetaldehyde.  相似文献   

12.
Guo H  Lee SC  Louie PK  Ho KF 《Chemosphere》2004,57(10):1363-1372
Ambient air quality measurements of 156 species including 39 alkanes, 32 alkenes, 2 alkynes, 24 aromatic hydrocarbons, 43 halocarbons and 16 carbonyls, were carried out for 120 air samples collected at two sampling stations (CW and TW) in 2001 throughout Hong Kong. Spatial variations of volatile organic compounds (VOCs) in the atmosphere were investigated. Levels of most alkanes and alkenes at TW site were higher than that at the CW site, while the BTEX concentrations at the two sites were close. The BTEX ratios at CW and TW were 1.6:10.1:1.0:1.6 and 2.1:10.8:1.0:2.0, respectively. For major halogenated hydrocarbons, the mean concentrations of chloromethane, CFCs 12 and 22 did not show spatial variations at the two sites. However, site-specific differences were observed for trichloroethene and tetrachloroethene. Furthermore, there were no significant differences for carbonyls such as formaldehyde, acetaldehyde and acetone between the two sites. The levels of selected hydrocarbons in winter were 1-5 times that in summer. There were no common seasonal trends for carbonyls in Hong Kong. The ambient level of formaldehyde, the most abundant carbonyl, was higher in summer. However, levels of acetaldehyde, acetone and benzaldehyde in winter were 1.6-3.8 times that in summer. The levels of CFCs 11 and 12, and chloromethane in summer were higher than that in winter. Strong correlation of most hydrocarbons with propene and n-butane suggested that the primary contributors of hydrocarbons were vehicular emissions in Hong Kong. In addition, gasoline evaporation, use of solvents, leakage of liquefied petroleum gas (LPG), natural gas leakage and other industrial emissions, and even biogenic emissions affected the ambient levels of hydrocarbons. The sources of halocarbons were mainly materials used in industrial processes and as solvents. Correlation analysis suggested that photochemical reactions made significant contributions to the ambient levels of carbonyls in summer whereas in winter motor vehicle emissions would be the major sources of the carbonyls. The photochemical reactivity of selected VOCs was estimated in this study. The largest contributors to ozone formation were formaldehyde, toluene, propene, m,p-xylene, acetaldehyde, 1-butene/i-butene, isoprene and n-butane, suggesting that motor vehicles, gasoline evaporation, use of solvents, leakage of LPG, photochemical processes and biogenic emission are sources in the production of ozone. On the other hand, VOCs from vehicles and gasoline evaporation were predominant with respect to reactions with OH radical.  相似文献   

13.
Ozone concentration data measured in 1977–1979 and 1981–1983 at rural sites in north-west England have been analysed in relation to elevated concentrations. Overall, concentrations exceed 60 ppb on 11.2% of days, 80 ppb on 4.2% of days and reach levels in excess of 100 ppb on 1.5% of days monitored. It is concluded that photochemical pollution is the most frequent cause of elevated concentrations, and that both long-range (continental) and middle-distance (U.K. urban) sources contribute. On a smaller percentage of days, elevated ozone levels arise from enhanced intrusions of stratospheric air associated with vigorous frontal activity. The meteorological situations associated with tropospheric photochemical ozone formation are summer anticyclonic conditions, in common with other observations in the U.K. and other parts of the world.  相似文献   

14.
Abstract

Personal 48-hr exposures of 15 randomly selected participants as well as microenvironment concentrations in each participant’s residence and workplace were measured for 16 carbonyl compounds during summer–fall 1997 as a part of the Air Pollution Exposure Distributions within Adult Urban Populations in Europe (EXPOLIS) study in Helsinki, Finland. When formaldehyde and acetaldehyde were excluded, geometric mean ambient air concentrations outside each participant’s residence were less than 1 ppb for all target compounds. Geometric mean residential indoor concentrations of carbonyls were systematically higher than geometric mean personal exposures and indoor workplace concentrations. Additionally, residential indoor/outdoor ratios indicated substantial indoor sources for most target compounds. Carbonyls in residential indoor air correlated significantly, suggesting similar mechanisms of entry into indoor environments. Overall, this study demonstrated the important role of non-traffic-related emissions in the personal exposures of participants in Helsinki and that comprehensive apportionment of population risk to air toxics should include exposure concentrations derived from product emissions and chemical formation in indoor air.  相似文献   

15.
Abstract

Ozone and several polar volatile organic compounds (VOCs) including organic acids and carbonyls (aldehydes and ketones) were measured over an approximately 24 hour period in four residences during the winter of 1993 and in nine residences during the summer of 1993. All residences were in the greater Boston, Massachusetts area. The relation of the polar VOCs to the ozone concentration was examined. Indoor carbonyl concentrations were similar between the summer and winter, with the total mean winter concentration being 31.7 ppb and the total mean summer concentration being 36.6 ppb. However, the average air exchange rate was 0.9 hr?1 during the winter and 2.6 hr?1 during the summer. Therefore, the estimated carbonyl emission rates were significantly higher during the summer. Indoor organic acid concentrations were about twice as high during the summer as during the winter. For formic acid, the indoor winter mean was 9.8 ppb, and the summer indoor mean was 17.8 ppb. For acetic acid, the indoor winter mean was 15.5 ppb, and the summer indoor mean was 28.7 ppb. The concentrations of the polar VOCs were found to be significantly correlated with one another. Also, the emission rates of the polar VOCs were found to be correlated with both the environmental variables such as temperature and relative humidity and the ozone removal rate; however, it was difficult to apportion the relative effects of the environmental variables and the ozone removal.  相似文献   

16.
Carbonyl compounds in the urban environment of Athens,Greece   总被引:6,自引:0,他引:6  
The concentration levels of 15 selected carbonyl compounds in 62 samples were determined at two sites in Athens basin from June to December 2000. Formaldehyde was the most abundant species (0.05-39 microg m(-3)), which comprised from 22% to 37% of the total measured compounds, followed by acetaldehyde (4.32-49 microg m(-3)), acetone/acrolein (0.64-198 microg m(-3)) and butanal (0.79-140 microg m(-3)). The mean formaldehyde/acetaldehyde and acetaldehyde/propanal molar ratios were calculated. No significant seasonal differences were observed for all the carbonyls. Photochemical production was found to weigh upon atmospheric levels for 83-93% in summer days, dropping below 33% in the winter. The importance of formaldehyde and acetaldehyde as a source of hydroxyl radicals in Athens was also assessed.  相似文献   

17.
The relationships between the monthly and seasonal averages of the daily 1200–1500 h O3 inflow concentrations and wind flow direction have been evaluated. The O3 measurements used are those during inflow of air parcels from upwind to rural monitoring stations outside of St. Louis, MO. The results obtained are consistent with the O3 measurements reported from other monitoring studies at rural locations both to the west and east of St. Louis. Although there is a stratospheric component to these ground level rural O3 concentrations, it is likely that most of the O3 measured during the warmer months of the year is associated with photochemical O3 formation in the planetary boundary layer and in the free troposphere. A substantial part of the increments in rural O3 concentrations which occur from west to east of St. Louis during the warmer months of the year appear best to be accounted for as a result of photochemical formation O3 precursors from anthropogenic emission sources to the east of St. Louis. Differences in the values of meteorological parameters with wind flow direction account for only a small part of the differences in O3 concentration observed.  相似文献   

18.
Measurements of carbonyl compound concentrations at different sites in the Paris area have been carried out. Interpretation of the results made use of the following data: general meteorological conditions, wind field analysis and type of primary pollutant sources. The principal phenomena observed were: a sharp formaldehyde decrease during rainfall; concentration levels of lower aldehydes in rural sites comparable to those found in the literature; an important variation in the ratio of primary aldehydes to secondary aldehydes depending on meteorological conditions; a significant increase in lower aldehyde concentrations downwind from the urban center despite vertical dispersion of the pollutants.  相似文献   

19.
This paper describes a laboratory project to assess the accuracy of emission and indoor air quality models to be used in predicting formaldehyde (HCHO) concentrations in residences due to pressed-wood products made with urea-formaldehyde bonding resins. The products tested were partlcleboard underlayment, hardwood- plywood paneling and medium-density fiberboard (mdf). The products were initially characterized in chambers by measuring their formaldehyde surface emission rates over a range of formaldehyde concentrations, air exchange rates and two combinations of temperature and relative humidity (23° C and 5 0% RH; 26°C and 60% RH). They were then installed in a two-room prototype house in three different combinations (underlayment flooring only; underlayment flooring and paneling; and underlayment flooring, paneling, and mdf). The equilibrium formaldehyde concentrations were monitored as a function of air exchange rate. Particleboard underlayment and mdf, but not paneling, behaved as the emission model predicted over a large concentration range, under both sets of temperature and relative humidity. Good agreement was also obtained between measured formaldehyde concentrations and those predicted by a mass-balance indoor air quality model.  相似文献   

20.
A study was conducted to evaluate five techniques for determining ambient formaldehyde concentrations. One technique used a spectroscopic determination, and the other four techniques used derivatization followed by fluorometric analysis or high-performance liquid chromatography with detection by u.v. absorption. Formaldehyde was generated by two techniques. In the first technique, zero air was bubbled through a solution of aqueous formaldehyde to produce gas-phase formaldehyde. Various compounds serving as possible interferences were added singly or in combination to these air mixtures. In the second technique, formaldehyde was generated as a product from controlled irradiations of hydrocarbons and nitrogen oxides in a smog chamber operated in a dynamic mode. The study was conducted as a blind intercomparison with no knowledge by the participants of the HCHO concentrations or the interferences added.The data from each of the techniques were compared against mean values in each sampling period. For formaldehyde in zero air, average deviations for each of the techniques ranged between 15 and 30%. At a formaldehyde concentration of 10 ppb, each technique showed no evidence for interferences by O3 (190 ppbv), NO2 (300 ppbv), SO2 (20 ppbv), and H2O2 (7 ppbv). The agreement for formaldehyde concentrations measured for the photochemical mixtures was similar to that of the mixtures in zero air.Ambient measurements were also performed on three evenings and for one 36-h period. Ambient formaldehyde concentrations ranged from 1 to 10 ppbv. Ambient H2O2 measurements were also performed. A strong correlation in the diurnal concentration profile for formaldehyde and H2O2 was observed over the 36-h period.  相似文献   

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