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1.
Monitoring data from the UK Automatic Urban and Rural Network are used to investigate the relationships between ambient levels of ozone (O3), nitric oxide (NO) and nitrogen dioxide (NO2) as a function of NOx, for levels ranging from those typical of UK rural sites to those observed at polluted urban kerbside sites. Particular emphasis is placed on establishing how the level of ‘oxidant’, OX (taken to be the sum of O3 and NO2) varies with the level of NOx, and therefore to gain some insight into the atmospheric sources of OX, particularly at polluted urban locations. The analyses indicate that the level of OX at a given location is made up of NOx-independent and NOx-dependent contributions. The former is effectively a regional contribution which equates to the regional background O3 level, whereas the latter is effectively a local contribution which correlates with the level of primary pollution. The local oxidant source has probable contributions from (i) direct NO2 emissions, (ii) the thermal reaction of NO with O2 at high NOx, and (iii) common-source emission of species which promote NO to NO2 conversion. The final category may include nitrous acid (HONO), which appears to be emitted directly in vehicle exhaust, and is potentially photolysed to generate HOx radicals on a short timescale throughout the year at southern UK latitudes. The analyses also show that the local oxidant source has significant site-to-site variations, and possible reasons for these variations are discussed. Relationships between OX and NOx, based on annual mean data, and fitted functions describing the relative contributions to OX made by NO2 and O3, are used to define expressions which describe the likely variation of annual mean NO2 as a function of NOx at 14 urban and suburban sites, and which can take account of possible changes in the regional background of O3.  相似文献   

2.
A time series analysis of ozone monitoring data from several locations in Switzerland from 1991 to 1999 is presented. Different methods are used to address changes in the ozone level during these years and to account for the influence of changing meteorological conditions. The results show a slight decrease of the peaks but a highly significant increase of the mean value of around 0.5–0.9 ppb yr−1. The frequency distribution has changed in the sense that very low values have become less frequent and that there is a strong increase in frequency of occurrence of half-hourly mean values between about 45 and 55 ppb. A selection procedure reveals slight tendencies towards different trends of afternoon ozone peaks in summer depending on weather and pollution situations. Ozone peaks tend to decrease on fair weather days at rural sites (but increase at urban sites) and show a small increase on cloudy and windy days. A non-linear regression model is used to estimate trends of summertime afternoon ozone peaks in the presence of meteorological variability. In the model, the long-term signal is additively split into a linear part and a part which is modulated by global radiation. The coefficients for both terms are statistically significant at many sites, with an increasing linear trend at the sites north of the Alps of around 1 ppb yr−1 and a decrease of ozone peaks under fair weather conditions relative to cloudy conditions. When additionally considering the effect of precursor concentrations in the regression models, both trends are weakened, which means that they can partly be explained by changes in local to regional emissions. However, at the sites north of the Alps remains a tendency towards a positive linear “base trend” of around 0.4 ppb yr−1. This could possibly be due to increasing background ozone concentrations.  相似文献   

3.
For a quantitative estimate of the ozone effect on vegetation reliable models for ozone uptake through the stomata are needed. Because of the analogy of ozone uptake and transpiration it is possible to utilize measurements of water loss such as sap flow for quantification of ozone uptake. This technique was applied in three beech (Fagus sylvatica) stands in Switzerland. A canopy conductance was calculated from sap flow velocity and normalized to values between 0 and 1. It represents mainly stomatal conductance as the boundary layer resistance in forests is usually small. Based on this relative conductance, stomatal functions to describe the dependence on light, temperature, vapour pressure deficit and soil moisture were derived using multivariate nonlinear regression. These functions were validated by comparison with conductance values directly estimated from sap flow. The results corroborate the current flux parameterization for beech used in the DO3SE model.  相似文献   

4.
选择石家庄市区代表性路段作为研究对象,对其交通环境空气中NOx的污染水平进行现状监测。基于Matlab软件建立拟合模型,对下一时期的NOx污染趋势进行预测。结果表明,石家庄市交通环境中NOx小时浓度介于0.047~0.237 mg/m3之间,呈早晚高,且下午明显低于上午的日变化规律;NOx日均浓度介于0.076~0.211 mg/m3之间,其浓度与车流量呈明显的正相关性。利用matlab软件建立的ARMA模型能够较好地预测道路交通环境空气中NOx的浓度变化趋势。  相似文献   

5.
The photolysis of nitrogen dioxide and formaldehyde are two of the most influential reactions in the formation of photochemical air pollution, and their rates are computed using actinic flux determined from a radiative transfer model. In this study, we compare predicted and measured nitrogen dioxide photolysis rate coefficients (jNO2). We used the Tropospheric Ultraviolet-Visible (TUV) radiation transfer model to predict jNO2 values corresponding to measurements performed in Riverside, California as part of the 1997 Southern California Ozone Study (SCOS’97). Spectrally resolved irradiance measured at the same site allowed us to determine atmospheric optical properties, such as aerosol optical depth and total ozone column, that are needed as inputs for the radiative transfer model. Matching measurements of aerosol optical depth, ozone column, and jNO2 were obtained for 14 days during SCOS’97. By using collocated measurements of the light extinction caused by aerosols and ozone over the full height of the atmosphere as model input, it was possible to predict sudden changes in jNO2 resulting from atmospheric variability. While the diurnal profile of the rate coefficient was readily reproduced, jNO2 model predicted values were found to be consistently higher than measured values. The bias between measured and predicted values was 17–36%, depending on the assumed single scattering albedo. By statistical analysis, we restricted the most likely values of the single scattering albedo to a range that produced bias on the order of 20–25%. It is likely that measurement error is responsible for a significant part of the bias. The aerosol single scattering albedo was found to be a major source of uncertainty in radiative transfer model predictions. Our best estimate indicates its average value at UV-wavelengths for the period of interest is between 0.77 and 0.85.  相似文献   

6.
The ambient air quality monitoring data of 2006 and 2007 from a recently established Pearl River Delta (PRD) regional air quality monitoring network are analyzed to investigate the characteristics of ground-level ozone in the region. Four sites covering urban, suburban, rural and coastal areas are selected as representatives for detailed analysis in this paper. The results show that there are distinct seasonal and diurnal cycles in ground-level ozone across the PRD region. Low ozone concentrations are generally observed in summer, while high O3 levels are typically found in autumn. The O3 diurnal variations in the urban areas are larger than those at the rural sites. The O3 concentrations showed no statistically significant difference between weekend and weekdays in contrast to the findings in many other urban areas in the world. The average ozone concentrations are lower in urban areas compared to the sites outside urban centers. Back trajectories are used to show the major air-mass transport patterns and to examine the changes in ozone from the respective upwind sites to a site in the center of the PRD (Wanqingsha). The results show higher average ozone concentrations at the upwind sites in the continental and coastal air masses, but higher 1 h-max O3 concentrations (by 8–16 ppbv) at the center PRD site under each of air-mass category, suggesting that the ozone pollution in the PRD region exhibits both regional and super-regional characteristics.  相似文献   

7.
Possible effects of climate change on air quality are studied for two urban sites in the UK, London and Glasgow. Hourly meteorological data were obtained from climate simulations for two periods representing the current climate and a plausible late 21st century climate. Of the meteorological quantities relevant to air quality, significant changes were found in temperature, specific humidity, wind speed, wind direction, cloud cover, solar radiation, surface sensible heat flux and precipitation. Using these data, dispersion estimates were made for a variety of single sources and some significant changes in environmental impact were found in the future climate. In addition, estimates for future background concentrations of NOx, NO2, ozone and PM10 upwind of London and Glasgow were made using the meteorological data in a statistical model. These showed falls in NOx and increases in ozone for London, while a fall in NO2 was the largest percentage change for Glasgow. Other changes were small. With these background estimates, annual-average concentrations of NOx, NO2, ozone and PM10 were estimated within the two urban areas. For London, results averaged over a number of sites showed a fall in NOx and a rise in ozone, but only small changes in NO2 and PM10. For Glasgow, the changes in all four chemical species were small. Large-scale background ozone values from a global chemical transport model are also presented. These show a decrease in background ozone due to climate change. To assess the net impact of both large scale and local processes will require models which treat all relevant scales.  相似文献   

8.
In 1974, Junge postulated a relationship between variability of concentrations of gases in air at remote locations and their atmospheric residence time, and this Junge relationship has subsequently been observed empirically for a range of trace gases. Here, we analyze two previously-published datasets of concentrations of cyclic volatile methyl siloxanes (cVMS) in air and find Junge relationships in both. The first dataset is a time series of concentrations of decamethylcyclopentasiloxane (D5) measured between January and June, 2009 at a rural site in southern Sweden that shows a Junge relationship in the temporal variability of the measurements. The second dataset consists of measurements of hexamethylcyclotrisiloxane (D3), octamethylcyclotetrasiloxane (D4) and D5 made simultaneously at 12 sites in the Global Atmospheric Passive Sampling (GAPS) network that shows a Junge relationship in the spatial variability of the three cVMS congeners. We use the Junge relationship for the GAPS dataset to estimate atmospheric lifetimes of dodecamethylcyclohexasiloxane (D6), 8:2–fluorotelomer alcohol and trichlorinated biphenyls that are within a factor of 3 of estimates based on degradation rate constants for reaction with hydroxyl radical determined in laboratory studies.  相似文献   

9.
Over the past few years, concern has increased in Canada over the health and environmental impacts of elevated concentrations of ground-level ozone. During the summer the most populated regions of Canada frequently record ozone concentrations that exceed the one-hour average maximum acceptable air quality objective of 32 parts per billion (ppb). In 1988 the Canadian Council of Ministers of the Environment agreed to develop a federal/provincial management plan to control nitrogen oxide and volatile organic compound emissions to reduce ozone concentrations in all affected regions of the country. In addition to the proposed interim control measures, the plan recommended that studies be undertaken to acquire the information necessary to develop sound control strategies. This report represents one of those studies and provides a summary of ground-level ozone measurements for eastern Canada for the 1980 to 1991 period with an emphasis on seasonal variations, trends, and occurrences of high concentrations.

Southwestern Ontario experiences the highest maximum hourly ozone concentrations and the greatest frequency of hours greater than the 82 ppb acceptable objective. Urban sites have the highest frequencies of ozone concentration measurements in the < 10 ppb range, while rural and remote sites show peaks in frequency distribution in the 20 to 30 ppb range. Trend analysis of summertime (May to September) average daily maximum ozone concentration showed no consistent pattern for eastern Canadian sites during 1980 to 1991. Sites in Montreal showed statistically insignificant downward trends while sites in Toronto showed small but statistically significant upward trends. These ozone-increasing trends are associated with reductions in nitric oxide concentrations. At all sites there was large year-to-year variability in peak ozone levels and in the frequency of hours with ozone concentrations above the maximum acceptable objective.  相似文献   

10.
Malondialdehyde (MDA), a product of lipid peroxidation and biomarker of oxidative stress, is measured over the long term in spruce Picea abies needles under real conditions in three Czech mountain border areas. The trends presented collate the MDA content in spruce needles with ambient ozone, temperature and precipitation as casual, and defoliation as a subsequent factor for the period 1994-2006. We have found the overall decreasing trends in MDA and defoliation. The highest MDA and defoliation are recorded in the Jizerske, the lowest in the Krusne hory Mts. Out of the examined variables the MDA is predicted best by mean temperature in vegetation season, median of O3 concentrations and AOT40; these three variables account for 34% of MDA1 and 36% of MDA2 variability. Our hypothesis that higher ambient O3 exposure results in higher MDA contents in P. abies needles under real conditions has not been approved.  相似文献   

11.
12.
Triclopyr is a widely used pesticide which is non-biodegradable and enters aquatic systems. The ozone facilitated photocatalyzed degradation and mineralization of Triclopyr using Au-loaded titania as heterogeneous catalyst is reported. The oxidative degradation activity of the hazardous pesticide was investigated at pH 7.8 under varied reaction conditions, including in presence and absence of ozone, titania alone, in presence and absence of light and with different loadings of Au on support. Photocatalysis with 2% Au/TiO2 in the presence of ozone yielded 100% degradation of Triclopyr in 2 h. The extent of degradation of pesticide and its mineralization were confirmed by GC-MS. For 10 mg/L of Triclopyr, 0.1 g/L of catalyst was found to be the optimum for mineralization. Results show that photocatalyzed ozonation with Au/TiO2 as catalyst is a very effective for its removal. No leaching of Au was observed in triplicate runs. Catalyst was fully recoverable and reusable with no loss of activity.  相似文献   

13.
Measurements of air pollutants from a background site in central London are analysed. These comprise hourly data for CO, NO, NO2, O3, SO2 and PM10 from 1996 to 2008 and particle number count from 2001 to 2008. The data are analysed in terms of long-term trends, annual, weekly and diurnal cycles, and autocorrelation and cross-correlation functions. CO, NO and NO2 show a typical traffic-associated pattern with two daily peaks and lesser concentrations at the weekend. Particle number count and PM10 show a similar cycle, but with smaller amplitude. Ozone has an annual cycle with a maximum in May, influenced by the spring maximum in background ozone, but the diurnal and weekly cycles are dominated by losses through reaction with nitric oxide. Particle number count shows a minimum corresponding with maximum air temperatures in August, whereas the CO, NO NO2 and SO2 show a minimum in June/July. There is a lower particle count to NOx ratio at the background site compared to a central London kerbside site (Marylebone Road) and a seasonal pattern in particle count to NOx and PM10 ratios consistent with loss of nanoparticles by evaporation during atmospheric transport. Sulphur dioxide peaks in the morning in summer, but at midday in winter consistent with emissions from elevated sources mixing down from aloft as the diurnal mixed layer deepens. Implications for epidemiological studies of air quality and health are discussed. Sulphur dioxide, carbon monoxide, nitric oxide and nitrogen dioxide show clear downward trends over the measurement period, PM10 declines initially before levels stabilised, and ozone concentrations increased.  相似文献   

14.
Air quality models are used to predict changes in pollutant concentrations resulting from envisioned emission control policies. Recognizing the need to assess the credibility of air quality models in a policy-relevant context, we perform a dynamic evaluation of the Community Multiscale Air Quality (CMAQ) modeling system for the “weekend ozone effect” to determine if observed changes in ozone due to weekday-to-weekend (WDWE) reductions in precursor emissions can be accurately simulated. The weekend ozone effect offers a unique opportunity for dynamic evaluation, as it is a widely documented phenomenon that has persisted since the 1970s. In many urban areas of the Unites States, higher ozone has been observed on weekends than weekdays, despite dramatically reduced emissions of ozone precursors (nitrogen oxides [NOx] and volatile organic compounds [VOCs]) on weekends. More recent measurements, however, suggest shifts in the spatial extent or reductions in WDWE ozone differences. Using 18 years (1988–2005) of observed and modeled ozone and temperature data across the northeastern United States, we re-examine the long-term trends in the weekend effect and confounding factors that may be complicating the interpretation of this trend and explore whether CMAQ can replicate the temporal features of the observed weekend effect. The amplitudes of the weekly ozone cycle have decreased during the 18-year period in our study domain, but the year-to-year variability in weekend minus weekday (WEWD) ozone amplitudes is quite large. Inter-annual variability in meteorology appears to influence WEWD differences in ozone, as well as WEWD differences in VOC and NOx emissions. Because of the large inter-annual variability, modeling strategies using a single episode lasting a few days or a few episodes in a given year may not capture the WEWD signal that exists over longer time periods. The CMAQ model showed skill in predicting the absolute values of ozone concentrations during the daytime. However, early morning NOx concentrations were underestimated and ozone levels were overestimated. Also, the modeled response of ozone to WEWD differences in emissions was somewhat less than that observed. This study reveals that model performance may be improved by (1) properly estimating mobile source NOx emissions and their temporal distributions, especially for diesel vehicles; (2) reducing the grid cell size in the lowest layer of CMAQ; and, (3) using time-dependent and more realistic boundary conditions for the CMAQ simulations.  相似文献   

15.
The biogenic species α-pinene, β-pinene, and d-limonene are among the most abundant monoterpenes emitted globally. They are also important precursors to secondary organic aerosol (SOA) formation in the atmosphere. This study involves the development of proposed oxidation mechanisms for these three species. Semi- and non-volatile oxidation products with the potential to lead to SOA formation are predicted explicitly. Simulation code that describes the gas-phase oxidation mechanisms including reactions that lead to ozone (O3) formation is coupled to an equilibrium absorptive partitioning code. The coupled model is used to simulate both gas-phase chemistry and SOA formation associated with oxidation of these three species in chamber experiments involving single as well as multiple oxidants. For the partitioning model, required molecular properties of the oxidation products are taken from the literature or estimated based on structural characteristics. The predicted O3 and SOA concentrations are typically within ±50% of measured values for most of the experiments except for the experiments with low initial hydrocarbon concentrations and the nitrate radical experiments with α-pinene. The developed model will be used to update a gas-phase chemical mechanism and a SOA formation module used in a three-dimensional air quality model.  相似文献   

16.
The local and regional distribution of pollutants is significantly influenced by weather patterns and variability along with the spatial patterns of emissions. Therefore, climatic changes which affect local meteorological conditions can alter air quality. We use the regional air quality model CHIMERE driven by meteorological fields from regional climate change simulations to investigate changes in summer ozone mixing ratios over Europe under increased greenhouse gas (GHG) forcing. Using three 30-year simulation periods, we find that daily peak ozone amounts as well as average ozone concentrations substantially increase during summer in future climate conditions. This is mostly due to higher temperatures and reduced cloudiness and precipitation over Europe and it leads to a higher number of ozone events exceeding information and warning thresholds. Our results show a pronounced regional variability, with the largest effects of climate change on ozone concentrations occurring over England, Belgium, Germany and France. The temperature-driven increase in biogenic emissions appears to enhance the ozone production and isoprene was identified as the most important chemical factor in the ozone sensitivity. We also find that summer ozone levels in future climate projections are similar to those found during the exceptionally warm and dry European summer of 2003. Our simulations suggest that in future climate conditions summer ozone might pose a much more serious threat to human health, agriculture and natural ecosystems in Europe, so that the effects of climate trends on pollutant amounts should be considered in future emission control measures.  相似文献   

17.
Ameliorative effects of ethylenediurea (N-[2-(2-oxo-1-imidazolinidyl) ethyl]-N′ phenylurea, abbreviated as EDU) against ozone stress were studied on selected growth, biochemical, physiological and yield characteristics of palak (Beta vulgaris L. var Allgreen) plants grown in field at a suburban site of Varanasi, India. Mean eight hourly ozone concentration varied from 52 to 73 ppb which was found to produce adverse impacts on plant functioning and growth characteristics. The palak plants were treated with 300 ppm EDU at 10 days after germination at 10 days interval up to the plant maturity. Lipid peroxidation in EDU treated plants declined significantly as compared to non-EDU treated ones. Significant increment in Fv/Fm ratio in EDU treated plants as compared to non-EDU treated ones was recorded. EDU treated plants showed significant increment in ascorbic acid contents and reduction in peroxidase activity as compared to non-EDU treated ones. As a result of the protection provided by EDU against ozone induced stress on biochemical and physiological characteristics of palak, the morphological parameters also responded positively. Significant increments were recorded in shoot length, number of leaves plant−1, leaf area and root and shoot biomass of EDU treated plants as compared to non-EDU treated ones. Contents of Na, K, Ca, Mg and Fe were higher in EDU treated plants as compared to non-EDU treated ones. The present investigation proves the usefulness of EDU in partially ameliorating ozone injury in ambient conditions.  相似文献   

18.

Rock ptarmigan (Lagopus muta) and willow ptarmigan (L. lagopus) are Arctic birds with a circumpolar distribution but there is limited knowledge about their status and trends across their circumpolar distribution. Here, we compiled information from 90 ptarmigan study sites from 7 Arctic countries, where almost half of the sites are still monitored. Rock ptarmigan showed an overall negative trend on Iceland and Greenland, while Svalbard and Newfoundland had positive trends, and no significant trends in Alaska. For willow ptarmigan, there was a negative trend in mid-Sweden and eastern Russia, while northern Fennoscandia, North America and Newfoundland had no significant trends. Both species displayed some periods with population cycles (short 3–6 years and long 9–12 years), but cyclicity changed through time for both species. We propose that simple, cost-efficient systematic surveys that capture the main feature of ptarmigan population dynamics can form the basis for citizen science efforts in order to fill knowledge gaps for the many regions that lack systematic ptarmigan monitoring programs.

  相似文献   

19.
《Chemosphere》2002,49(10)
The distribution coefficients (Kd) and desorption rates of 137Cs and 241Am radionuclides in bottom sediments at different locations in the Black Sea were studied under laboratory conditions. The Kd values were found to be 500 for 137Cs and 3800 for 241Am at the steady state and described exponential curves. Rapid uptake of the radionuclides occurred during the initial period and little accumulation happened after four days. The desorption rates for 137Cs in different bottom sediments were best described by a three-component exponential model. The desorption half-times of 137Cs ranged from 26 to 50 d at the slow components. However, the desorption rate of 241Am described one component for all sediment samples and desorption half-time was found to be 75 d. In general, the results showed that the 241Am radionuclide is more effectively transferred to bottom sediment and has longer turnover time than 137Cs under Black Sea conditions.  相似文献   

20.
The Houston-Galveston-Brazoria (HGB) area of Texas has a history of ozone exceedances and is currently classified under moderate nonattainment status for the 2008 8-hr ozone standard of 75 ppb. The HGB area is characterized by intense solar radiation, high temperature, and high humidity, which influence day-to-day variations in ozone concentrations. Long-term air quality trends independent of meteorological influence need to be constructed for ascertaining the effectiveness of air quality management in this area. The Kolmogorov-Zurbenko (KZ) filter technique, used to separate different scales of motion in a time series, is applied in the current study for maximum daily 8-hr (MDA8) ozone concentrations at an urban site (U.S. Environmental Protection Agency [EPA] Air Quality System [AQS] Site ID: 48-201-0024, Aldine) in the HGB area. This site, located within 10 miles of downtown Houston and the George Bush Intercontinental Airport, was selected for developing long-term meteorologically independent MDA8 ozone trends for the years 1990–2016. Results from this study indicate a consistent decrease in meteorologically independent MDA8 ozone between 2000 and 2016. This pattern could be partially attributed to a reduction in underlying nitrogen oxide (NOx) emissions, particularly lowering nitrogen dioxide (NO2) levels, and a decrease in the release of highly reactive volatile organic compounds (HRVOCs). Results also suggest solar radiation to be most strongly correlated to ozone, with temperature being the secondary meteorological control variable. Relative humidity and wind speed have tertiary influence at this site. This study observed that meteorological variability accounts for a high of 61% variability in baseline ozone (low-frequency component, sum of long-term and seasonal components), whereas 64% of the change in long-term MDA8 ozone post 2000 could be attributed to NOx emission reduction. Long-term MDA8 ozone trend component was estimated to be decreasing at a linear rate of 0.412 ± 0.007 ppb/yr for the years 2000–2016 and 0.155 ± 0.005 ppb/yr for the overall period of 1990–2016.

Implications: The effectiveness of air emission controls can be evaluated by developing long-term air quality trends independent of meteorological influences. The KZ filter technique is a well-established method to separate an air quality time series into short-term, seasonal, and long-term components. This paper applies the KZ filter technique to MDA8 ozone data between 1990 and 2016 at an urban site in the greater Houston area and estimates the variance accounted for by the primary meteorological control variables. Estimates for linear trends of MDA8 ozone are calculated and underlying causes are investigated to provide a guidance for further investigation into air quality management of the greater Houston area.  相似文献   


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