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1.
Although polycyclic aromatic hydrocarbons (PAHs) are common pollutants in snow, there is little quantitative data about their rates of photodegradation in this environment. To begin to address this gap, we have measured the degradation kinetics of phenanthrene, pyrene, and fluoranthene on ice, as these are the most abundant PAHs in arctic snow. Frozen aqueous solutions of individual PAHs, with and without added hydrogen peroxide (HOOH) as a source of hydroxyl radical (OH), were illuminated with simulated sunlight. For all three PAHs, direct photodecay is the main mechanism of degradation, while OH-initiated indirect photodegradation is a minor sink. Rate constants (±1 SE) for direct photodegradation extrapolated to midday, surface snow conditions at Summit, Greenland on the summer solstice are 3.8 (±0.8) × 10?5, 28 (±3) × 10?5, and 1.4 (±0.7) × 10?5 s?1 for phenanthrene, pyrene, and fluoranthene, respectively. Apparent quantum efficiencies for photodegradation with simulated sunlight were 3.8 (±0.8) × 10?3, 4.3 (±0.5) × 10?4, and 2 (±1) × 10?5, respectively. Calculated PAH lifetimes in surface snow under Summit conditions are 1–19 h during mid-summer, but increase to >100 days in the dark winter. While the short photodegradation lifetimes in the summer suggest that there should be no appreciable PAH levels in this season, past measurements at Summit sometimes show significant levels of these PAHs in summer surface snow. This discrepancy is likely due to differences in PAH location between lab samples (where the PAHs are probably in quasi-liquid layers) and real snow (where PAHs are likely primarily associated with particulate matter).  相似文献   

2.

The influences of relative humidity (RH) on the heterogeneous reaction of NO2 with soot were investigated by a coated wall flow tube reactor at ambient pressure. The initial uptake coefficient (γ initial) of NO2 showed a significant decrease with increasing RH from 7 to 70%. The γ initial on “fuel-rich” and “fuel-lean” soot at RH = 7% was (2.59 ± 0.20) × 10?5 and (5.92 ± 0.34) × 10?6, respectively, and it decreased to (5.49 ± 0.83) × 10?6 and (7.16 ± 0.73) × 10?7 at RH = 70%, respectively. Nevertheless, the HONO yields were almost independent of RH, with average values of (72 ± 3)% for the fuel-rich soot and (60 ± 2)% for the fuel-lean soot. The Langmuir-Hinshelwood mechanism was used to demonstrate the negative role of RH in the heterogeneous uptake of NO2 on soot. The species containing nitrogen formed on soot can undergo hydrolysis to produce carboxylic species or alcohols at high RH, accompanied by the release of little gas-phase HONO and NO.

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3.
Simultaneous measurements of aerosol absorption and scattering coefficients for the PM2.5 aerosols particles were done at Delhi during April 2008–March 2009 to estimate the aerosol single scattering albedo (SSA) and the Angstrom absorption exponents at the surface. The annual average SSA at 0.55 μm was found to be 0.70 ± 0.07 with only slight variations during the four seasons, summer (0.63 ± 0.06), monsoon (0.69 ± 0.07), winter (0.74 ± 0.03) and spring (0.72 ± 0.04). However, large variations in average absorption and scattering coefficients were seen during these four seasons. The average absorption coefficients during summer, monsoon, winter and spring were found to be 62.47 ± 21.27, 50.95 ± 43.61, 189.65 ± 85.94 and 90.65 ± 33.06 Mm?1 respectively. The corresponding scattering coefficients were 110.46 ± 36.15, 95.34 ± 49.46, 565.59 ± 274.59 and 236.56 ± 96.25 Mm?1. The Angstrom absorption exponent (ασ(abs)) remained close to unity throughout the year averaging at 1.02 ± 0.08, 1.02 ± 0.10, 1.04 ± 0.11, and 1.03 ± 0.05 during summer, monsoon, winter and spring seasons respectively, strongly indicating that the absorption at Delhi aerosol is mainly due to the abundance of black carbon of fossil fuel origin.  相似文献   

4.
As part of an international research project, aerosol samples were collected by several filter-based devices on Nuclepore polycarbonate membrane, Teflon membrane and quartz fibre filters over separate daylight periods and nights, and on-line aerosol measurements were performed by TEOM and aethalometer within an urban canyon (kerbside) and at a near-city background site in Budapest, Hungary from 23 April–5 May 2002. Aerosol masses in PM2.0, PM10–2.0, PM2.5, PM10 size fractions and of TSP were determined gravimetrically; atmospheric concentrations of organic (OC) and elemental carbon (EC) for PM2.5 (or PM2.0), PM10 fractions and for TSP were measured by thermal–optical transmission method. Repeatability of the mass determination by Nuclepore filters seems to be 5–6%. Collections on Teflon filters yielded smaller mass on average by 8(±12)% than that for the Nuclepore filters. Quartz filters overestimated the PM10 mass in comparison with the Nuclepore filters due primarily to sampling artefacts on average by 10(±16)% at the kerbside. Tandem filter set-ups were utilised for correcting the sampling artefacts for OC by subtraction method. At the kerbside, the aerosol mass was made up on average of 35(±4)% of organic matter (OM) in the PM10 fraction, while the contribution of OM to the PM2.5 mass was 43(±9)%. At the background, OM also accounted for 43(±13)% of the PM2.0 mass. On average, EC made up 14(±6)%, 7(±2)% and 4.5(±1.1)% of the mass in the PM2.5, PM10 fractions and TSP, respectively, at the kerbside; while its contribution was only 2.1(±0.5)% in the PM2.0 fraction in the near-city background. Temporal variability for PM mass, OC and EC concentrations was related to road traffic, local meteorology and long-range transport of air masses. It was concluded that a direct coupling between the atmospheric concentration levels and vehicle circulation can be identified within the urban canyon, nevertheless, the local meteorology in particular and long-range transport of air masses have much more influence on the air quality than changes in the source intensity of road traffic. Concentration ratios of OC/EC were evaluated, and the amount of secondary organic aerosol (SOA) was estimated by using EC as tracer for the primary OC emissions. Mean contribution and standard deviation of the SOA to the OM in the PM2.5 size fraction at the kerbside over daylight periods and nights were of 37(±18) and 46(±16)%, respectively.  相似文献   

5.
Lahore, Pakistan is an emerging megacity that is heavily polluted with high levels of particle air pollution. In this study, respirable particulate matter (PM2.5 and PM10) were collected every sixth day in Lahore from 12 January 2007 to 19 January 2008. Ambient aerosol was characterized using well-established chemical methods for mass, organic carbon (OC), elemental carbon (EC), ionic species (sulfate, nitrate, chloride, ammonium, sodium, calcium, and potassium), and organic species. The annual average concentration (±one standard deviation) of PM2.5 was 194 ± 94 μg m?3 and PM10 was 336 ± 135 μg m?3. Coarse aerosol (PM10?2.5) was dominated by crustal sources like dust (74 ± 16%, annual average ± one standard deviation), whereas fine particles were dominated by carbonaceous aerosol (organic matter and elemental carbon, 61 ± 17%). Organic tracer species were used to identify sources of PM2.5 OC and chemical mass balance (CMB) modeling was used to estimate relative source contributions. On an annual basis, non-catalyzed motor vehicles accounted for more than half of primary OC (53 ± 19%). Lesser sources included biomass burning (10 ± 5%) and the combined source of diesel engines and residual fuel oil combustion (6 ± 2%). Secondary organic aerosol (SOA) was an important contributor to ambient OC, particularly during the winter when secondary processing of aerosol species during fog episodes was expected. Coal combustion alone contributed a small percentage of organic aerosol (1.9 ± 0.3%), but showed strong linear correlation with unidentified sources of OC that contributed more significantly (27 ± 16%). Brick kilns, where coal and other low quality fuels are burned together, are suggested as the most probable origins of unapportioned OC. The chemical profiling of emissions from brick kilns and other sources unique to Lahore would contribute to a better understanding of OC sources in this megacity.  相似文献   

6.
Simultaneous daily measurements of water-soluble organic nitrogen (WSON), ammonium and nitrate were made between July and November 2008 at a rural location in south-east Scotland, using a ‘Cofer’ nebulizing sampler for the gas phase and collection on an open-face PTFE membrane for the particle phase. Average concentrations of NH3 were 82 ± 17 nmol N m?3 (error is s.d. of triplicate samples), while oxidised N concentrations in the gas phase (from trapping NO2 and HNO3) were smaller, at 2.6 ± 2.2 nmol N m?3, and gas-phase WSON concentrations were 18 ± 11 nmol N m?3. The estimated collection efficiency of the nebulizing samplers for the gas phase was 88 (±8) % for NH3, 37 (±16) % for NO2 and 57 (±7) % for WSON; reported average concentrations have not been corrected for sampling efficiency. Concentrations in the particle phase were smaller, except for nitrate, at 21 ± 9, 10 ± 6 and 8 ± 9 nmol N m?3, respectively. The absence of correlation in either phase between WSON and either (NH3 + NH4+) or NO3? concentrations suggests atmospheric WSON has diverse sources. During wet days, concentrations of gas and particle-phase inorganic N were lower than on dry days, whereas the converse was true for WSON. These data represent the first reports of simultaneous measurements of gas and particle phase water-soluble nitrogen compounds in rural air on a daily basis, and show that WSON occurs in both phases, contributing 20–25% of the total water-soluble nitrogen in air, in good agreement with earlier data on the contribution of WSON to total dissolved N in rainfall in the UK.  相似文献   

7.
The wetlands play an important role in global carbon and nitrogen storage, and they are also natural sources of greenhouse gases such as methane (CH4) and nitrous oxide (N2O). Land-use change is an important factor affecting the exchange of greenhouse gases between wetlands and the atmosphere. However, few studies have investigated the effect of land-use change on CH4 and N2O emissions from freshwater marsh in China. Therefore, a field study was carried out over a year to investigate the seasonal changes of the emissions of CH4 and N2O at three sites (Deyeuxia angustifolia marsh, dryland and rice field) in the Sanjiang Plain of Northeast China. Marsh was the source of CH4 showing a distinct temporal variation. Maximum fluxes occurred in June and the highest value was 20.69 ± 2.57 mg CH4 m?2 h?1. The seasonal change of N2O fluxes from marsh was not obvious, consisted of a series of emission pulses. The marsh acted as a N2O sink during winter, while became a N2O source in the growing season. The results showed that gas exchange between soil/snow and the atmosphere in the winter season contributed greatly to the annual budgets. The winter season CH4 flux was about 3.24% of the annual flux and the winter uptake of N2O accounted for 13.70% of the growing-season emission. Conversion marsh to dryland resulted in a shift from a strong CH4 source to a weak sink (from 199.12 ± 39.04 to ?1.37 ± 0.68 kg CH4 ha?1 yr?1), while increased N2O emissions somewhat (from 4.07 ± 1.72 to 4.90 ± 1.52 kg N2O ha?1 yr?1). Conversion marsh to rice field significantly decreased CH4 emission from 199.12 ± 39.04 to 94.82 ± 9.86 kg CH4 ha?1 yr?1 and N2O emission from 4.07 ± 1.72 to 2.09 ± 0.79 kg N2O ha?1 yr?1.  相似文献   

8.

This work aimed to determine the seasonal variations of polycyclic aromatic hydrocarbons (PAHs) in airborne PM10 at two background sites (Masná—MS, Líšeň—LN) in Brno over a 5-year period (2009–2013). Samples were collected on quartz filters using a low-volume sampler by continual filtration. Concentrations of PAHs in collected PM10 samples were determined using a gas chromatography with a mass spectrometer as a detector. A different number of PAHs were determined to be at each site, i.e., 11 PAHs at the MS site and six PAHs at the LN site, and similarities between them were identified using non-parametric analysis of variance. Potential sources were identified using principal component analysis (PCA) and PAHs diagnostic ratios. The work also focused on health risk assessment. This was estimated using toxic equivalent factors to calculate individual lifetime cancer risk, which quantifies risk of exposure to PAHs for specific age groups. The average 11-PAH concentrations in M|S site annually ranged from 19.28 ± 19.02 ng m−3 (2011) to 40.37 ± 21.35 ng m−3 (2013). With regard to the LN site, the average six-PAH concentrations annually ranged from 3.64 ± 3.87 ng m−3 (2009) and 5.27 ± 6.19 ng m−3 (2012). PCA and diagnostic ratios indicate the main sources to be traffic emissions and coal combustion. Health risk assessment showed carcinogenic risk under limit value in all cases.

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9.
Measurements carried out in Paris Magenta railway station in April–May 2006 underlined a repeatable diurnal cycle of aerosol concentrations and optical properties. The average daytime PM10 and PM2.5 concentrations in such a confined space were approximately 5–30 times higher than those measured in Paris streets. Particles are mainly constituted of dust, with high concentrations of iron and other metals, but are also composed of black and organic carbon. Aerosol levels are linked to the rate at which rain and people pass through the station. Concentrations are also influenced by ambient air from the nearby streets through tunnel ventilation. During daytime approximately 70% of aerosol mass concentrations are governed by coarse absorbing particles with a low Angström exponent (~0.8) and a low single-scattering albedo (~0.7). The corresponding aerosol density is about 2 g cm?3 and their complex refractive index at 355 nm is close to 1.56–0.035 i. The high absorption properties are linked to the significant proportion of iron oxides together with black carbon in braking systems. During the night, particles are mostly submicronic, thus presenting a greater Angström exponent (~2). The aerosol density is lower (1.8 g cm?3) and their complex refractive index presents a lower imaginary part (1.58–0.013 i), associated to a stronger single-scattering albedo (~0.85–0.90), mostly influenced by the ambient air. For the first time we have assessed the emission (deposition) rates in an underground station for PM10, PM2.5 and black carbon concentrations to be 3314 ± 781(?1164 ± 160), 1186 ± 358(?401 ± 66) and 167 ± 46(?25 ± 9) μg m?2 h?1, respectively.  相似文献   

10.
Continuous measurements of aerosol size distributions (3 nm–2 μm) were carried out over a 26 month period (1 April 2001–31 May 2003; 650 days with valid data) in urban East St. Louis, IL, as a part of the US Environmental Protection Agency's Supersite program. This paper analyzes data for the 155 days on which “regional nucleation events” were observed during this study. Such events were observed during every month of the study except January 2003. We observed some differences, however, between events in the summer (defined here as April–September) and winter (December–February). Regional nucleation events were observed more frequently in summer months (36±13% of days) than in winter (8±7%), and nucleated particles grew faster in the summer (6.7±4.8 nm h−1) than in winter (1.8±1.9 nm h−1). The daily maximum in the number concentration of nanoparticles formed by nucleation (4.8±3.5×104 cm−3) was highly variable and showed no clear seasonal dependence. Particle formation increased particle concentrations by an average factor of 3.1±2.8. Maximum daily rates of 3 nm particle production (17±20 cm−3 s−1) were also highly variable and without a clear seasonal dependence. During these events, particle formation rates were typically near their maxima at 08:00–09:00 a.m., but particle production sometimes persisted at diminishing rates until late in the afternoon (15:00–16:00 p.m.).  相似文献   

11.
The HO2 uptake to aerosol particles is potentially significant sink for the HO2 radical in the marine atmosphere. To assess the heterogeneous loss of HO2 on marine aerosol particles, we have investigated the uptake coefficients (γ) of HO2 for submicron aerosol particles of KCl, synthetic sea salt, and natural seawater under ambient conditions (760 Torr and 296 ± 2 K) using an aerosol flow tube (AFT) coupled with a chemical conversion/laser-induced fluorescence (CC/LIF) technique. γ values determined for dry and wet aerosols of KCl were 0.02 ± 0.01 and 0.07 ± 0.03 at 66% and 75% RH, respectively, while γ values for those doped with CuSO4 was 0.55 ± 0.19 at 75% RH. γ values determined for synthetic sea-salt particles were 0.07 ± 0.03, 0.12 ± 0.04 and 0.13 ± 0.04 at 35%, 50%, 75% RH, respectively, while γ values for natural seawater particles were 0.10 ± 0.03, 0.11 ± 0.02 and 0.10 ± 0.03 at 35%, 50%, 75% RH, respectively. We recommend a HO2 uptake coefficient in marine areas of 0.1 for modeling and estimated the contribution of heterogeneous loss of HO2 by sea-salt aerosol particles in marine areas using a box model. Our box-model simulations suggested that daytime maximum HO2 concentrations decreased to 87–94% of the values without heterogeneous loss.  相似文献   

12.
We measured mercury speciation in coastal rainwater samples from Monterey Bay, California in 2007–2008 to investigate the source of monomethylmercury (MMHg) in rainwater and determine the relative importance of wet atmospheric deposition of MMHg to coastal waters compared to other sources on the central Pacific coast. Total mercury (HgT) ranged from 10 to 88 pM, with a sample mean ± standard deviation of 33 ± 22 pM (volume-weighted average 29 pM). MMHg concentrations ranged from 0.12 to 2.3 pM with a sample mean of 0.7 ± 0.5 pM (volume-weighted average 0.68 pM). Reactive mercury (HgR) concentrations ranged from 0.87 to 47 pM, sample mean 7.8 ± 8.3 pM (volume-weighted average 6.1 pM). Acetate concentration in rainwater, measured in a subset of samples, ranged from 0.34 to 3.1 μM, and averaged 1.6 ± 0.9 μM (volume-weighted average 1.3 μM). Dimethylmercury (DMHg) concentrations were below the limit of detection in air (<0.01 ng m?3) and rainwater (<0.05 pM). Despite previous suggestions that DMHg in upwelled ocean waters is a potential source of MMHg in coastal rainwater, MMHg in rain was not related to coastal upwelling seasons or surface water DMHg concentrations. Instead, a multiple linear regression analysis demonstrated that MMHg concentrations were positively and significantly correlated (p = 0.002, adjusted R2 = 0.88) with those of acetate and HgR. These data appear to support previous suggestions that the aqueous phase methylation of Hg(II) by acetate may be the source of MMHg in rainwater, but imply that acetate concentrations in rainwater play a more important role relative to HgR than previously hypothesized. However, the calculated chemical speciation of Hg(II) in rainwater and the minimal predicted complexation of Hg(II) by acetate suggest that the aqueous phase methylation of Hg(II) by acetate is unlikely to account for the MMHg found in precipitation, or that the mechanism of this reaction in the atmosphere differs from that previously reported (Gardfeldt et al., 2003).  相似文献   

13.

This study investigated organic matter (OM) and nutrient removal efficiency of mixed algal species from slaughterhouse wastewater (SWW) by using photo-bioreactor. For this purpose, different dilution multiples of 10, 4, and 2 were applied to the SWW, and pure wastewater was finally used for algal cultivation. OM and nutrient removal performance in an algal photo-bioreactor were severely affected by the dilution ratio. After 7 days of cultivation, the highest removal percentages of total organic carbon (TOC), total nitrogen (TN), and total phosphorus (TP) were 89.6, 70.2, and 96.2 %, respectively. Furthermore, the changes in eukaryotic algae and cyanobacterial species in the algal photo-bioreactors were investigated using polymerase chain reaction (PCR) and denaturing gradient gel electrophoresis (DGGE) techniques. The results indicated that cyanobacterial species were more efficient than eukaryotic species in removing nutrients from the SWW. This study suggests that mixed algal photo-bioreactors could be used efficiently in the treatment of SWW.

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14.
In China, vegetable croplands are characterized by intensive fertilization and cultivation, which produce significant nitrogenous gases to the atmosphere. In this study, nitric oxides (NOX) and nitrous oxide (N2O) emissions from the croplands cultivated with three typical vegetables had been measured in Yangtze River Delta of China from September 2 to December 16, 2006. The NO fluxes varied in the ranges of 1.6–182.4, 1.4–2901 and 0.5–487 ng Nm?2 s?1 with averages of 33.8 ± 44.2, 360 ± 590 and 76 ± 112 (mean ± SD) ngNm?2 s?1 for cabbage, garlic, and radish fields (n = 88), respectively. N2O fluxes from the three vegetable fields were found to occur in pulses and significantly promoted by tillage with average values of 5.8, 8.8, and 4.3 ng Nm?2 h?1 for cabbage, garlic, and radish crops, respectively. Influence of vegetables canopy on the NO emission was investigated and quantified. It was found that on cloudy days the canopy can only shield NO emission from croplands soil while on sunny days it cannot only prevent NO emission but also assimilate NO through the open leaves stomas. Multiple linear regression analysis indicated that soil temperature was the most important factor in controlling NO emission, followed by fertilizer amount and gravimetric soil water content. About 1.2%, 11.56% and 2.56% of applied fertilizers N were emitted as NO–N and N2O–N from the cabbage, garlic and radish plots, respectively.  相似文献   

15.
Carbonaceous soil amendments are applied to contaminated soils and sediments to strongly sorb hydrophobic organic contaminants (HOCs) and reduce their freely dissolved concentrations. This limits biouptake and toxicity, but also biodegradation. To investigate whether HOCs sorbed to such amendments can be degraded at all, the desorption and biodegradation of low concentrations of 14C-labelled phenanthrene (?5 μg L?1) freshly sorbed to suspensions of the pure soil amendments activated carbon (AC), biochar (charcoal) and compost were compared. Firstly, the maximum abiotic desorption of phenanthrene from soil amendment suspensions in water, minimal salts medium (MSM) or tryptic soy broth (TSB) into a dominating silicone sink were measured. Highest fractions remained sorbed to AC (84 ± 2.3%, 87 ± 4.1%, and 53 ± 1.2% for water, MSM and TSB, respectively), followed by charcoal (35 ± 2.2%, 32 ± 1.7%, and 12 ± 0.3%, respectively) and compost (1.3 ± 0.21%, similar for all media). Secondly, the mineralization of phenanthrene sorbed to AC, charcoal and compost by Sphingomonas sp. 10-1 (DSM 12247) was determined. In contrast to the amounts desorbed, phenanthrene mineralization was similar for all the soil amendments at about 56 ± 11% of the initially applied radioactivity. Furthermore, HPLC analyses showed only minor amounts (<5%) of residual phenanthrene remaining in the suspensions, indicating almost complete biodegradation. Fitting the data to a coupled desorption and biodegradation model revealed that desorption did not limit biodegradation for any of the amendments, and that degradation could proceed due to the high numbers of bacteria and/or the production of biosurfactants or biofilms. Therefore, reduced desorption of phenanthrene from AC or charcoal did not inhibit its biodegradation, which implies that under the experimental conditions these amendments can reduce freely dissolved concentration without hindering biodegradation. In contrast, phenanthrene sorbed to compost was fully desorbed and biodegraded.  相似文献   

16.

Understanding the spatial distribution patterns of microplastics (plastics?<?5 mm) contributes to the assessment of sources and sinks of pollution thus providing information for the management of biota safety and overall ecosystem functionality. We chose a semi-closed study area, Lake Bracciano (Italy), to assess the environmental variability of contamination, focusing on the water compartment and the exposure of biota, specifically fish, by analysing the ingestion of microplastics. The focus of this study is to evaluate the concentration of microplastics in water (surface and column) across the lake and the ingestion of microplastics by two fish species of economic interest: Atherina boyeri and Coregonus lavaretus, inhabiting demersal and pelagic habitats respectively. Results show a surface contamination of 392,000?±?417,000 items km?2 and a column one of 0.76?±?1.00 items m?3. Fragments were the most abundant in surface while fibres in the column. Microplastics were found in C. lavaretus specimens, corresponding to contamination frequency of 5% and concentration of 0.15 items/fish. The main polymer found in water was polyethylene (81%); of minor percentages, there were various other polymers, including polystyrene and acrylic, which were also found in fish. As scientific literature provides few research where water and fish are simultaneously sampled, this investigation wants to contribute filling this knowledge gap by investigating for the first time a volcanic lake.

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17.
The use of alcohol fuel has received much attention since 1980s. In Brazil, ethanol-fueled vehicles have been currently used on a large scale. This paper reports the atmospheric methanol, ethanol and isopropanol concentrations which were measured from May to December 1997, in Osaka, Japan, where alcohol fuel was not used, and from 3 to 9 February 1998, in Sao Paulo, Brazil, where ethanol fuel was used. The alcohols were determined by the alkyl nitrite formation reaction using gas chromatography (GC-ECD) analysis. The concentration of atmospheric alcohols, especially ethanol, measured in Sao Paulo were significantly higher than those in Osaka. In Osaka, the average concentrations of atmospheric methanol, ethanol, and isopropanol were 5.8±3.8, 8.2±4.6, and 7.2±5.9 ppbv, respectively. The average ambient levels of methanol, ethanol, and isopropanol measured in Sao Paulo were 34.1±9.2, 176.3.±38.1, and 44.2±13.7 ppbv, respectively. The ambient levels of aldehydes, which were expected to be high due to the use of alcohol fuel, were also measured at these sampling sites. The atmospheric formaldehyde average concentration measured in Osaka was 1.9±0.9 ppbv, and the average acetaldehyde concentration was 1.5±0.8 ppbv. The atmospheric formaldehyde and acetaldehyde average concentrations measured in Sao Paulo were 5.0±2.8 and 5.4±2.8 ppbv, respectively. The C2H5OH/CH3OH and CH3CHO/HCHO were compared between the two measurement sites and elsewhere in the world, which have already been reported in the literature. Due to the use of ethanol-fueled vehicles, these ratios, especially C2H5OH/CH3OH, are much higher in Brazil than these measured elsewhere in the world.  相似文献   

18.
Personal exposures, residential indoor, outdoor and workplace levels of nitrogen dioxide (NO2) were measured for 262 urban adult (25–55 years) participants in three EXPOLIS centres (Basel; Switzerland, Helsinki; Finland, and Prague; Czech Republic) using passive samplers for 48-h sampling periods during 1996–1997. The average residential outdoor and indoor NO2 levels were lowest in Helsinki (24±12 and 18±11 μg m−3, respectively), highest in Prague (61±20 and 43±23 μg m−3), with Basel in between (36±13 and 27±13 μg m−3). Average workplace NO2 levels, however, were highest in Basel (36±24 μg m−3), lowest in Helsinki (27±15 μg m−3), with Prague in between (30±18 μg m−3). A time-weighted microenvironmental exposure model explained 74% of the personal NO2 exposure variation in all centres and in average 88% of the exposures. Log-linear regression models, using residential outdoor measurements (fixed site monitoring) combined with residential and work characteristics (i.e. work location, using gas appliances and keeping windows open), explained 48% (37%) of the personal NO2 exposure variation. Regression models based on ambient fixed site concentrations alone explained only 11–19% of personal NO2 exposure variation. Thus, ambient fixed site monitoring alone was a poor predictor for personal NO2 exposure variation, but adding personal questionnaire information can significantly improve the predicting power.  相似文献   

19.
In-situ measurements of atmospheric chlorofluorocarbons (CFCs) can be used to the assess their global and regional emissions and to check for compliance with phase-out schedules under Montreal protocol and its amendments. The atmospheric mixing ratios of CFC-11 (CCl3F), CFC-12 (CCl2F2) and CFC-113 (CCl2F–CClF2) have been measured by an automated in-situ GC-ECDs system at the regional Chinese Global Atmosphere Watch (GAW) station Shangdianzi (SDZ), from November 2006 to October 2009. The time series for these three principal CFCs showed large episodic events and background conditions occurred for approximately 30% (CFC-11), 52% (CFC-12) and 56% (CFC-113) of the measurements. The mean background mixing ratios for CFC-11, CFC-12 and CFC-113 were 244.8 ppt (parts per trillion, 10?12, molar) 539.6 ppt and 76.8 ppt, respectively, for 2006–2009. The enhanced CFC mixing ratios compared to AGAGE sites such as Trinidad Head (THD), US and Mace Head (MHD), Ireland suggest regional influences even during background conditions at SDZ, which is much closer to highly-populated areas. Between 2006 and 2009 background CFCs exhibited downward trends at rates of ?2.0 ppt yr?1 for CFC-11, ?2.5 ppt yr?1 for CFC-12 and ?0.7 ppt yr?1 for CFC-113. De-trended 3-year average background seasonal cycles displayed small fluctuations with peak-to-trough amplitudes of 1.0 ± 0.02 ppt (0.4%) for background CFC-11, 1.3 ± 2.1 ppt (0.3%) for CFC-12 and 0.2 ± 0.4 ppt (0.3%) for CFC-113. On the other hand, during pollution periods these CFCs showed much larger seasonal cycles of 11.2 ± 10.7 ppt (5%) for CFC-11, 7.5 ± 6.5 ppt (2%) for CFC-12 and 1.0 ± 1.2 ppt (1.2%) for CFC-113, with apparent winter minima and early summer maxima. This enhancement was attributed to prevailing wind directions from urban regions in summer and to enhanced anthropogenic sources during the warm season. In general, horizontal winds from northeast showed negative contribution to atmospheric CFCs loading, whereas South Western advection (urban sector: Beijing) had positive contributions.  相似文献   

20.
Elemental (S and N) and isotopic (δ34S and δ15N) contents in the moss Haplocladium microphyllum at urban, rural and forested sites in acid rain area of South China have been analyzed for comparisons to show whether they are different and can be effectively used to identify S and N sources of atmospheric deposition. Average moss S content at rural sites (0.29 ± 0.06%) was found to be in between those at urban (0.35 ± 0.05%) and forested (0.25 ± 0.04%) sites, which are significantly different. Average N contents of urban (2.60 ± 0.56%) and rural mosses (2.84 ± 0.77%) are not significantly different, while both are significantly different to that of forested mosses at most areas, indicating that the atmosphere over rural sites has been polluted by N as seriously as that over urban sites. Nitrogen supply, relative to S supply, was in excess of the requirement for protein synthesis, especially at rural and forested sites. Moss stable isotope signatures have been proven to be effective tools for deciphering atmospheric S and N sources at these sites. Through moss δ34S signatures, we found that atmospheric S at urban and forested sites was mainly from local coal combustion and domestic biomass burning, respectively, whereas northerly air masses contributed more S to forested sites. The relatively negative moss δ15N values (?7.5 ± 3.0, ?3.4 ± 2.1 and ?0.8 ± 2.1‰) demonstrated that the main form in the N deposition was NHx in these sites. More negative δ15N signatures in urban mosses (?7.5 ± 3.0‰) indicated the contribution of NH3 released from untreated city sewage and wastes, while relatively less negative δ15N for rural and forested mosses (3.4 ± 2.1 and ?0.8 ± 2.1‰) was largely derived from agricultural NH3.  相似文献   

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