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1.
Simultaneous chloroform (CHCl3) emission and ozone (O3) deposition are regularly observed under nocturnal inversions during the summer months from and to the peat bogs in the vicinity of the Mace Head Atmospheric Research Station, Connemara, Co Galway, Ireland. Emissions were estimated using the nocturnal box model applied to routine atmospheric observations collected over a 14-year period from 1995 to 2008. Strict criteria were applied in the selection of events of low wind speed, under a stable night-time inversion layer in baseline air conditions, with no transport from Europe. The mean peatland CHCl3 flux was 2.91 μg m?2 h?1 with highly variable fluxes ranging from 0.44 to 12.94 μg m?2 h?1. These fluxes are generally larger than those reported previously for similar biomes and if representative would make a significant contribution to the global estimated source of CHCl3. Fluxes were not strongly correlated with either atmospheric temperature or the level of precipitation. Over the 14-year period there appears to have been a small increase in overall CHCl3 emissions, although we stress that the nocturnal box model has a number of limitations and assumptions which should be taken into account.  相似文献   

2.
Methane emissions from the peat bogs in Connemara, Ireland have been inferred from the trace gas observations at the Mace Head Atmospheric Research Station using the nocturnal box method. A total of 237 local events, during April to September, over a 12-year period have been studied. Simultaneous emissions of methane, carbon dioxide and chloroform are routinely observed under nocturnal inversions with low wind speeds from the peat bogs proximal to Mace Head. Night-time deposition of ozone and hydrogen occurs concurrently with these emissions. Using the temporally correlated methane and ozone data we estimate methane emissions from each event. Simultaneous methane and chloroform emissions, together with ozone and hydrogen deposition have been characterised, leading to the estimation of methane emission rates for each event. The mean methane emission flux was found to be 400 ± 90 ng m?2 s?1. A strong seasonal cycle was found in the methane emission fluxes but there was little evidence of a long-term trend in the emissions from the peat bogs in the vicinity of the Mace Head station.  相似文献   

3.
Continuous measurements of black carbon aerosol (BCA) at the Mace Head Atmospheric Research Station on the Atlantic Ocean coast of Ireland show the occurrence of dramatically elevated concentrations when regionally polluted air masses are advected to the station. These occurrences correlate well with similar elevations in carbon monoxide and a wide range of other trace gases monitored near-simultaneously with the BCA. Using daily sector allocation and a sophisticated Lagrangian dispersion model, two independent estimates of the European emission source strength of BCA that are required to explain the Mace Head observations have been made. The best estimates of the UK and European emission source strengths of BCA are 46±14 and [(482–511)±140]×103 tonnes yr−1, respectively, and these estimates compare favourably with published inventories, at least to within ±25%, though they are considerably smaller than the emissions employed in some early global climate model studies.  相似文献   

4.
The mixing ratios of HCFC-141b (1,1-dichlorofluoroethane) and HCFC-142b (1-chloro-1,1-difluoroethane) have been rising steadily in baseline air at Mace Head, Ireland over the 10-year period from 1994 to 2004. These HCFCs are widely used replacements for the chlorofluorocarbons phased out under the Montreal Protocol and its subsequent amendments. Analysis of the HCFC content of regionally-polluted air arriving at Mace Head from the European continent shows that European emissions reached a peak during 2000–2001 and have declined subsequently, following the phase-out in their usage. European emissions of HCFC-141b have been further constrained by observations at the High-Alpine Jungfraujoch site. The reductions are consistent with the phase-out of HCFC production and use from the year 2001 onwards mandated by European regulations designed to exceed the requirements of the Montreal Protocol.  相似文献   

5.
This study aims to evaluate near surface ozone simulated with the modelling system RegCM3/CAMx against ozone measurements from the EMEP database for the recent decade 1991–2000. The RegCM3/CAMx simulations were performed on a 50 km × 50 km grid over Europe driven either by ERA-40 reanalysis (hereafter referred as ERA simulation) or the global circulation model (GCM) ECHAM5 (hereafter referred as ECHAM simulation). A set of statistical metrics is used for the model evaluation, including temporal correlation coefficient, the ratio of the standard deviations and the bias of simulated versus observed values. Overall, a good agreement is found for both ERA and ECHAM simulations at the majority of the selected EMEP stations in all metrics throughout the year based either on monthly or daily ozone values. Based on these results, it is assessed that the modelling system RegCM3/CAMx is suitable to be used for present and future regional climate-air quality simulations with emphasis on near surface ozone. The ERA simulations reproduce more accurately the observed ozone values in comparison to ECHAM simulations because the meteorology of the ERA experiment is closer to real atmospheric conditions than the GCM based experiment. On a seasonal basis, both ERA and ECHAM simulations exhibit a seasonally dependent bias, with winter and spring ozone values being generally under-estimated by the model and summer and autumn values being slightly overestimated. This seasonally dependent bias is also evident from median and peak midday ozone values. However, the highest observed midday ozone peaks in summer, with values higher than 80 ppbv, could not be captured either by ERA or ECHAM simulations. An analysis of day-time and night-time ERA and ECHAM modelled ozone values shows that CAMx performs better during the day-time.  相似文献   

6.
In order to evaluate the spatial variation of aerosol (particulate matter with aerodynamic diameter < or = 10 microm [PM10]) and ozone (03) concentrations and characterize the atmospheric conditions that lead to 03 and PM10-rich episodes in southern Italy during summer 2007, an intensive sampling campaign was simultaneously performed, from middle of July to the end of August, at three ground-based sites (marine, urban, and high-altitude monitoring stations) in Calabria region. A cluster analysis, based on the prevailing air mass backward trajectories, was performed, allowing to discriminate the contribution of different air masses origin and paths. Results showed that both PM10 and 03 levels reached similar high values when air masses originated from the industrialized continental Europe as well as under the influence of wildfire emissions. Among natural sources, dust intrusion and wildfire events seem to involve a marked impact on the recorded data. Typical fair weather of Mediterranean summer and persisting anticyclone system at synoptic scale were indeed favorable conditions to the arrival of heavily dust-loaded air masses over three periods of consecutive days and more than half of the observed PM10 daily exceedances have been attributed to Saharan dust events. During the identified dust outbreaks, a consistent increase in PM10 levels with a concurrent decrease in 03 values was also observed and discussed.  相似文献   

7.
Atmospheric concentration of sulfur dioxide (SO2) was intermittently measured at an air quality monitoring (AQM) station in the Yong-san district of Seoul, Korea, between 1987 and 2013. The SO2 level was compared with other important pollutants concurrently measured, including methane (CH4), carbon monoxide (CO), nitric oxide (NO), nitrogen dioxide (NO2), ozone (O3), and particulate matter (PM10). If split into three different periods (period 1, 1987–1988, period 2, 1999–2000, and period 3, 2004–2013), the respective mean [SO2] values (6.57 ± 4.29, 6.30 ± 2.44, and 5.29 ± 0.63 ppb) showed a slight reduction across the entire study period. The concentrations of SO2 are found to be strongly correlated with other pollutants such as CO (r = 0.614, p = 0.02), which tracked reductions in reported emissions due to tighter emissions standards enacted by the South Korean government. There was also a clear seasonal trend in the SO2 level, especially in periods 2 and 3, reflecting the combined effects of domestic heating by coal briquettes and meteorological conditions. Although only a 16% concentration reduction was achieved during the 27-year study duration, this is significant if one considers rapid urbanization, an 83.2% increase in population, and rapid industrialization that took place during that period.

Implications: Since 1970, a network of air quality monitoring (AQM) stations has been operated by the Korean Ministry of Environment (KMOE) for routine nationwide monitoring of air pollutant concentrations in urban/suburban areas. To date, the information obtained from these stations has provided a platform for analyzing long-term trends of major pollutant species. In this study, we examined the long-term trends of SO2 levels and relevant environmental parameters monitored continuously in the Yong-san district of Seoul between 1987 and 2013. The data were analyzed over various time scales (i.e., monthly, seasonal, and annual intervals). The results obtained from this study will allow us to assess the effectiveness of abatement strategy and to predict future concentrations trends in association with future abatement strategies and technologies.  相似文献   


8.
9.
Concentrations of airborne lead at Springfield, Missouri, in 1975-1993 have been determined by analysis of particulate material collected on glass-fiber filters during the 19-year period. Nitric acid-soluble lead in 1100 samples collected at a total of 19 monitoring stations was determined by atomic absorption spectroscopy and by differential pulse polarography. Ambient concentrations of airborne lead were found to decrease steadily (by more than 90%) during this period in spite of increases in area population and in automobile traffic. The decrease is significantly correlated with national trends in total emissions of lead to the atmosphere and with US ambient lead levels. Airborne lead from a coal-fired power plant was small compared with that from gasoline burning.  相似文献   

10.
Using a trajectory climatology for the period 1992–2001 we have examined how seasonal changes in transport cause changes in the concentrations of tropospheric ozone (O3), gaseous elemental mercury (GEM) and non-methane hydrocarbons (NMHCs) observed at the Mt. Zeppelin station, Ny-Ålesund (78.9°N, 11.9°E). During April–June O3 depletion events were frequently observed in connection with air transport across the Arctic Basin. The O3 loss was most pronounced in air masses advected close to the surface. This result supports the idea that the O3 depletion reactions take place in the lowermost part of the atmosphere in the central Arctic Basin. A strong positive correlation between springtime O3 depletion events and the oxidation of GEM to divalent mercury was found. During air mass advection from Siberia, the Barents Sea and the Norwegian Sea the strongest correlation was observed during April–May, whereas air masses originating from the Canadian Arctic and the central Arctic areas showed the highest O3–GEM correlation in May–June. We suggest that this 1-month lag could either be due to the position of the marginal ice zone or temperature differences between the northwestern and northeastern air masses. In connection with springtime O3 depletion events low concentrations of some NMHCs, especially ethane and ethyne, were observed, indicating that both bromine (ethyne oxidant) and chlorine radicals (ethane oxidant) are present in the Arctic atmosphere during spring. In winter, negative correlations between O3 and NMHCs were found in connection with air transport from Europe and Siberia, which we interpret as O3 destruction taking place in industrially contaminated plumes.  相似文献   

11.
In order to improve our knowledge of the surface ozone in the south of the Iberian Peninsula, annual, monthly, weekly and daily ozone concentrations have been closely monitored in the Seville metropolitan area highlighting those episodes that exceed the European Ozone Directive. A three-year period (2003-2005) and eight ozone stations were used; five of them located in the city's busiest areas and the rest in adjacent zones ( approximately 25km). In addition, the wind regime was also studied in order to understand the main characteristics of the surface atmospheric dynamics. The lowest ozone concentrations 17-33microgm(-3) took place in January while the highest 57-95microgm(-3) occurred in June. The ozone concentration week-weekend differences from May to September indicate that this phenomenon does not affect the ozone stations analysed. Daily cycles show minimum values between 7:00 and 8:00 UTC and maximum at noon, exceeding 90microgm(-3) during summer months. From March to October the ozone concentrations were above the target value for the protection of human health, especially during the summer months, with values up to 30% over the limit. The information threshold has been exceeded at all ozone stations studied but with greater frequency in the stations far from the city centre. In addition, at these latter stations the alert threshold was also exceeded on six occasions. This study in the city of Seville indicates that the high ozone levels are due to local atmospheric effects, mainly since the ozone air masses may undergo recirculation processes. The ozone is transported to the city from the S-SW, having a major impact in the NE areas.  相似文献   

12.
ABSTRACT

A case study was conducted to evaluate the SO2 emission reduction in a power plant in Central Mexico, as a result of the shifting of fuel oil to natural gas. Emissions of criteria pollutants, greenhouse gases, organic and inorganic toxics were estimated based on a 2010 report of hourly fuel oil consumption at the “Francisco Pérez Ríos” power plant in Tula, Mexico. For SO2, the dispersion of these emissions was assessed with the CALPUFF dispersion model. Emissions reductions of > 99% for SO2, PM and Pb, as well as reductions >50% for organic and inorganic toxics were observed when simulating the use of natural gas. Maximum annual (993 µg/m3) and monthly average SO2 concentrations were simulated during the cold-dry period (152–1063 µg/m3), and warm-dry period (239–432 µg/m3). Dispersion model results and those from Mexico City’s air quality forecasting system showed that SO2 emissions from the power plant affect the north of Mexico City in the cold-dry period. The evaluation of model estimates with 24 hr SO2 measured concentrations at Tepeji del Rio suggests that the combination of observations and dispersion models are useful in assessing the reduction of SO2 emissions due to shifting in fuels. Being SO2 a major precursor of acid rain, high transported sulfate concentrations are of concern and low pH values have been reported in the south of Mexico City, indicating that secondary SO2 products emitted in the power plant can be transported to Mexico City under specific atmospheric conditions.

Implications: Although the surroundings of a power plant located north of Mexico City receives most of the direct SO2 impact from fuel oil emissions, the plume is dispersed and advected to the Mexico City metropolitan area, where its secondary products may cause acid rain. The use of cleaner fuels may assure significant SO2 reductions in the plant emissions and consequent acid rain presence in nearby populated cities and should be compulsory in critical areas to comply with annual emission limits and health standards.  相似文献   

13.
To investigate the effects of low (0.05 micromol/mol) and relatively low (0.10 micromol/mol) concentrations of ozone on photoassimilate partitioning, rice plants grown in a water culture were fed with (13)C-labelled carbon dioxide at the reproductive stage in an assimilation chamber with constant concentration of (12)CO(2) and (13)CO(2). Rice plants were exposed to ozone 4 weeks before and 3 weeks after (13)CO(2) feeding. The dry weight of whole plants decreased with increasing ozone concentration, whereas net photosynthetic rate (apparent CO(2) uptake per unit leaf area) was unaffected, compared with the control, at the time of (13)CO(2) feeding. Dry matter distribution into leaf sheaths and culms was reduced more than that into leaf blades by ozone exposure. Although panicle dry weight per plant was reduced by ozone, the percentage of panicle dry weight to the whole plant tended to increase considerably. Exposure to ozone accelerated translocation of (13)C from source leaves to other plant parts. Partitioning of (13)C to panicles and roots was higher under ozone treatment than in the control. Respiratory losses of fixed (13)C from plants tended to decrease under treatment with ozone. The increase in photoassimilate partitioning in panicles can be considered to be an acclimation response of rice plants to complete reproductive stage under the restricted biomass production caused by ozone.  相似文献   

14.
Santiago, Chile, is one of the most polluted cities in South America. As a response, over the past 15 yr, numerous pollution reduction programs have been implemented by the environmental authority, Comisión Nacional del Medio Ambiente. This paper assesses the effectiveness of these interventions by examining the trends of fine particulate matter (PM(2.5)) and its associated elements. Daily fine particle filter samples were collected in Santiago at a downtown location from April 1998 through March 2003. Additionally, meteorological variables were measured continuously. Annual average concentrations of PM(2.5) decreased only marginally, from 41.8 microg/m3 for the 1998-1999 period to 35.4 microg/m3 for the 2002-2003 period. PM(2.5) concentrations exceeded the annual U.S. Environmental Protection Agency standard of 15 microg/m3. Also, approximately 20% of the daily samples exceeded the old standard of 65 microg/m3, whereas approximately half of the samples exceeded the new standard of 35 microg/m3 (effective in 2006). Mean PM(2.5) levels measured during the cold season (April through September) were three times higher than those measured in the warm season (October through March). Particulate mass and elemental concentration trends were investigated using regression models, controlling for year, month, weekday, wind speed, temperature, and relative humidity. The results showed significant decreases for Pb, Br, and S concentrations and minor but still significant decreases for Ni, Al, Si, Ca, and Fe. The larger decreases were associated with specific remediation policies implemented, including the removal of lead from gasoline, the reduction of sulfur levels in diesel fuel, and the introduction of natural gas. These results suggest that the pollution reduction programs, especially the ones related to transport, have been effective in reducing various important components of PM(2.5). However, particle mass and other associated element levels remain high, and it is thus imperative to continue the efforts to improve air quality, particularly focusing on industrial sources.  相似文献   

15.
Hourly measurements of up to 26 C2–C8 hydrocarbons have been made at eight urban background sites, three urban-industrial sites, a kerbside and a rural site in the UK from 1993 onwards up until the end of December 2004. Average annual mean benzene and 1,3-butadiene concentrations at urban background locations have declined at about −20% per year and the observed declines have exactly mimicked the inferred declines in benzene and 1,3-butadiene emissions over the same period. Ninety-day rolling mean concentrations of ethylene, propylene, n- and i-butane, n- and i-pentane, isoprene and propane at urban and rural sites have also declined steadily by between −10% and −30% per year. Rolling mean concentrations of acetylene, 2- and 3-methylpentane, n-hexane, n-heptane, cis- and trans-but-2-ene, cis- and trans-pent-2-ene, toluene, ethylbenzene and o-, m- and p-xylene at a roadside location in London have all declined at between −14% and −21% per year. These declines demonstrate that motor vehicle exhaust catalysts and evaporative canisters have effectively and efficiently controlled vehicular emissions of hydrocarbons in the UK. Urban ethane concentrations arising largely from natural gas leakage have remained largely unchanged over this same period.  相似文献   

16.
Ambient samples of fine organic aerosol collected from a rural area (Moitinhos) in the vicinity of the small coastal Portuguese city of Aveiro over a period of more than one year have been solvent-extracted and quantitatively characterised by gas chromatography–mass spectrometry. Particles were also analysed with a thermal-optical technique in order to determine their elemental and organic carbon content. In addition, meteorological sensors and real-time black carbon, ozone and carbon monoxide monitors were used. Particulate matter values were higher than background levels in continental Europe. A patent seasonal variation for organic and elemental carbon concentrations was observed, presumably related to stronger local primary emissions and to limited vertical dispersion. The higher levels were most likely a result of residential wood burning, since black carbon and carbon monoxide maximised during late evening hours in wintertime. Of the bulk of elutable organics, more than a half, on average, was present as acidic fraction. Alcohols, aliphatic and polyaromatic hydrocarbons represented together, more than 30% of the elutable mass, also showing a marked seasonal pattern with a minimum in summer and a maximum in winter. The winter increase was more evident for resinic acids, phytosterols, n-alkanoic acids and polycyclic aromatic hydrocarbons.  相似文献   

17.
The Positive Matrix Factorization (PMF) receptor model and the Observation Based Model (OBM) were combined to analyze volatile organic compound (VOC) data collected at a suburban site (WQS) in the PRD region. The purposes are to estimate the VOC source apportionment and investigate the contributions of these sources and species of these sources to the O3 formation in PRD. Ten VOC sources were identified. We further applied the PMF-extracted concentrations of these 10 sources into the OBM and found "solvent usage 1", "diesel vehicular emissions" and "biomass/biofuel burning" contributed most to the O3 formation at WQS. Among these three sources, higher Relative Incremental Reactivity (RIR)-weighted values of ethene, toluene and m/p-xylene indicated that they were mainly responsible for local O3 formation in the region. Sensitivity analysis revealed that the sources of "diesel vehicular emissions", "biomass/biofuel burning" and "solvent usage 1" had low uncertainties whereas "gasoline evaporation" showed the highest uncertainty.  相似文献   

18.
This paper summarises some of the main results of a two-year experiment carried out in an Open-Top Chambers facility in Northern Italy. Seedlings of Populus nigra, Fagus sylvatica, Quercus robur and Fraxinus excelsior have been subjected to different ozone treatments (charcoal-filtered and non-filtered air) and soil moisture regimes (irrigated and non-irrigated plots). Stomatal conductance models were applied and parameterised under South Alpine environmental conditions and stomatal ozone fluxes have been calculated.The flux-based approach provided a better performance than AOT40 in predicting the onset of foliar visible injuries. Critical flux levels, related to visible leaf injury, are proposed for P. nigra and F. sylvatica (ranging between 30 and 33 mmol O3 m−2). Soil water stress delayed visible injury appearance and development by limiting ozone uptake. Data from charcoal-filtered treatments suggest the existence of an hourly flux threshold, below which may occur a complete ozone detoxification.  相似文献   

19.
Horizontal resolution of grid-based chemistry-transport models is limited to a few square kilometers which has been proved insufficient for assessing human exposure and health impact. We propose a general methodology, applicable on any kind of grid-based air-quality model, that combines subgrid scale information on emission and land-use data in order to disaggregate the grid-averaged emission flux into a set of source-specific components (subgrid-environments). Different subgrid concentrations are calculated inside each one of these environments providing a direct estimate of pollutant variability along with the ‘standard’ grid-averaged model output. The method was first validated over a controlled emissions case by comparing concentrations modeled in the subgrid-environments with concentrations modeled directly at higher model resolution and next over a real case-study, where subgrid concentrations were compared with monitor data from sites representing different types of urban environments (i.e. roads and residential blocks). It was shown that the method is capable to yield accurate estimates of small scale pollutant variability.  相似文献   

20.
Stable isotopes of NO3? (δ15N–NO3? and δ18O–NO3?) were monitored in precipitation at a central Pennsylvania site during six storm events in 2005 to determine whether information on atmospheric oxidants (e.g., O3, NO2, and NOx), and storm tracks (using the NOAA HYSPLIT model) were capable of explaining observed seasonal and within-storm isotopic variation. Results showed that δ15N–NO3? and δ18O–NO3? in precipitation varied significantly during individual storm events. Seasonally, δ15N–NO3? and δ18O–NO3? in precipitation followed a pattern of depletion during the summer months and enrichment during the winter months. NO3? precursor concentrations and atmospheric oxidants were useful for explaining the seasonal and within-storm variation of δ15N–NO3? for all six storm events as evidenced by negative relationships with NO2:NOx ratios and ozone (O3). In comparison, δ18O–NO3? was positively related to O3 in three dormant season storms, which suggested that the O3 oxidation pathway was important for producing the high δ18O–NO3? observed in wintertime precipitation. Storm track information was especially useful for describing differences in δ15N–NO3?. Cool-sector storms originating from the E/NE produced slightly negative δ15N–NO3? values characteristic of automobile emissions, whereas warm-sector storms with tracks from the SW/S/SE produced slightly positive δ15N–NO3? values characteristic of coal-fired emissions. Lightning also may have been an important source of atmospheric NO3? during two warm-sector thunderstorms. This study showed that (1) information about oxidant levels can be useful to predict the seasonal and within-storm variation of NO3? stable isotopes in precipitation, and (2) knowledge of storm tracks (warm-sector versus cool-sector) may be important for determining sources of NO3? in wet deposition.  相似文献   

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