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1.
Non-methane organic carbon (NMOC) measurements made in Atlanta, Georgia from 1999–2007 are used with nitrogen oxide (NOx or NOy) and ozone (O3) data to investigate relationships between O3 precursors and peak 8-hour O3 concentrations in the city. Data from a WNW-to-ENE transect of sites illustrate that the mean urban peak 8-hour O3 excess constitutes about 20% of the peak 8-hour O3 measured at the area-wide maximum O3 site when air-mass movement is from the northwest quadrant; local influence is potentially greater on days with more stagnation or recirculation. The peak 8-hour O3 concentrations in Atlanta increase as (1) surface temperature (T), ambient NMOC and NOy concentrations, and previous-day peak O3 concentrations increase, and as (2) relative humidity, surface wind speeds, and ratios of NMOC-to-NOy decrease. An observation-based statistical model is introduced to relate area-wide peak 8-hour O3 concentrations to ambient NMOC and NOy concentrations, while accounting for the non-linear dependences of peak 8-hour O3 concentrations on meteorological factors. On the majority of days when the area-wide peak 8-hour O3 exceeds 75 ppbv, meteorologically-adjusted peak 8-hour O3 concentrations increase as ambient NMOC concentrations increase (NMOC sensitive) and ambient NOy concentrations decrease. This result contrasts with regional conditions in which O3 formation appears to be NOx-sensitive in character. The results offer observationally-based information of relevance to O3 management strategies in the Atlanta area, potentially contributing to “weight-of-evidence” assessments.  相似文献   

2.
Ozone dose-crop loss conversion functions for alfalfa (Medicago sativa, L. var. Moapa 69) yield reduction and defoliation were developed using standardized field plots within an ambient O3 gradient in the South Coast Air Basin. Seasonal yields and defoliation values were tested with O3 dose, average daily maximum temperature, average daily minimum temperature, and average daily relative humidity in regression analyses to determine significant functional relationships. Only the ambient O3 dose variable was found to have a significant effect on alfalfa yield or defoliation (yield, r = –0.827, t-slope = 3.900**; defoliation, r = –0.890, t-slope = 5.190**). The ozone dose-crop loss conversion functions were calculated by converting the dose-response functions to dose-percent reduction functions.  相似文献   

3.
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   

4.
A study was designed to examine responses of loblolly pine (Pinus taeda) to chronic exposure to ozone (O3) in the field. Seedlings of four full-sib families of loblolly pine were planted in a field near Raleigh, NC, and exposed daily (May 27 to October 24, 1985) in open-top chambers to O3 ranging from 0.5 to 1.96 times the O3 concentration in non-filtered (NF) air. One-fourth of the plants in each plot were removed during each of two harvests (August and October) to measure effects of O3 on plant growth. Plants of each family exhibited foliar symptoms characteristic of O3 injury after five months of exposure to any greater-than-ambient O3 concentration, and one family exhibited symptoms after five months of exposure to NF air. Ozone dose-plant response relationships were quantified by regression for stem height, stem diameter, biomass, and other plant morphological and yield characteristics. All relationships were linear for three families, but one family exhibited no significant growth response relationship of O3 dose. Dose-response equations suggest a maximum growth suppression of 10 percent for NF air compared to charcoal-filtered air (i.e., 0.5 × NF) in the first season of exposure.  相似文献   

5.
In a 50- to 70-year-old mixed stand of Norway spruce (Picea abies (L.) Karst.) and European beech (Fagus sylvatica L.) in Germany, tree cohorts have been exposed to double ambient ozone (2×O3) from 2000 through 2007 and can be compared with trees in the same stand under the ambient ozone regime (1×O3). Annual diameter growth, allocation pattern, stem form, and stem volume were quantified at the individual tree and stand level. Ozone fumigation induced a shift in the resource allocation into height growth at the expense of diameter growth. This change in allometry leads to rather cone-shaped stem forms and reduced stem stability in the case of spruce, and even neiloidal stem shapes in the case of beech. Neglect of such ozone-induced changes in stem shape may lead to a flawed estimation of volume growth. On the stand level, 2×O3 caused, on average, a decrease of 10.2 m3 ha−1 yr−1 in European beech.  相似文献   

6.
Abstract

Ground-level ozone is a secondary pollutant that has recently gained notoriety for its detrimental effects on human and vegetation health. In this paper, a systematic approach is applied to develop artificial neural network (ANN) models for ground-level ozone (O3) prediction in Edmonton, Alberta, Canada, using ambient monitoring data for input. The intent of these models is to provide regulatory agencies with a tool for addressing data gaps in ambient monitoring information and predicting O3 events. The models are used to determine the meteorological conditions and precursors that most affect O3 concentrations. O3 time-series effects and the efficacy of the systematic approach are also assessed. The developed models showed good predictive success, with coefficient of multiple determination values ranging from 0.75 to 0.94 for forecasts up to 2 hr in advance. The inputs most important for O3 prediction were temperature and concentrations of nitric oxide, total hydrocarbons, sulfur dioxide, and nitrogen dioxide.  相似文献   

7.
A basin-wide air quality trend analysis for the South Coast Air Basin of California is conducted for hydrocarbons (HC), NOx, O3 and CO using multi-station composite daily maximum-hour average ambient concentrations for the third quarter (July, August and September) from 1968 to 1985. Emissions and air quality trends are compared for the period 1968-1984. Ambient HC and NOX trends are somewhat different from estimated emission trends of HC and NOx, while a definite, downward trend of ambient CO is consistent with vehicular emission control measures. Basin-wide ambient HC, NOx and O3 appear to show downward trends for the period 1970-1985, but because of high fluctuations it is difficult to delineate trends for shorter periods. The meteorology (850 mb temperature)-adjusted O3 shows a more consistent downward trend than does unadjusted O3. Polynomial and multiplicative regression models for basin-wide empirical O3-HC-NOx relationships Indicate that the O3 variation is explained largely by the meteorological variable (850 mb temperature) although model estimations are improved by adding HC and NOx concentration terms.  相似文献   

8.
Abstract

Emission trading is a market‐based approach designed to improve the efficiency and economic viability of emission control programs; emission trading has typically been confined to trades among single pollutants. Interpollutant trading (IPT), as described in this work, allows for trades among emissions of different compounds that affect the same air quality end point, in this work, ambient ozone (O3) concentrations. Because emissions of different compounds impact air quality end points differently, weighting factors or trading ratios (tons of emissions of nitrogen oxides (NOx) equivalent to a ton of emissions of volatile organic compounds [VOCs]) must be developed to allow for IPT. In this work, IPT indices based on reductions in O3 concentrations and based on reductions in population exposures to O3 were developed and evaluated using a three‐dimensional gridded photochemical model for Austin, TX, a city currently on the cusp of nonattainment with the National Ambient Air Quality Standards for O3 concentrations averaged over 8 hr. Emissions of VOC and NOx from area and mobile sources in Austin are larger than emissions from point sources. The analysis indicated that mobile and area sources exhibited similar impacts. Trading ratios based on maximum O3 concentration or population exposure were similar. In contrast, the trading ratios did exhibit significant (more than a factor of two) day‐to‐day variability. Analysis of the air quality modeling indicated that the daily variability in trading ratios could be attributed to daily variations in both emissions and meteorology.  相似文献   

9.
A meta-analysis was conducted to quantitatively assess the effects of ethylenediurea (EDU) on ozone (O3) injury, growth, physiology and productivity of plants grown in ambient air conditions. Results indicated that EDU significantly reduced O3-caused visible injury by 76%, and increased photosynthetic rate by 8%, above-ground biomass by 7% and crop yield by 15% in comparison with non-EDU treated plants, suggesting that ozone reduces growth and yield under current ambient conditions. EDU significantly ameliorated the biomass and yield of crops and grasses, but had no significant effect on tree growth with an exception of stem diameter. EDU applied as a soil drench at a concentration of 200-400 mg/L has the highest positive effect on crops grown in the field. Long-term research on full-grown tree species is needed. In conclusion, EDU is a powerful tool for assessing effects of ambient [O3] on vegetation.  相似文献   

10.
The results of long-term investigations of Scots pine (Pinus sylvestris L.) growth and condition in the impact zone of one of the biggest air pollution sources in Lithuania--mineral fertilizers plant "Achema" are presented. The main attention is laid to the recovery of damaged stands since annual emissions to air were reduced essentially. The investigations indicated, that the recovery of tree increment was mostly caused by distinct reduction of emissions of nitrogen and sulphur oxides and dust of mineral fertilizers. Despite reduced pollution, crown defoliation of investigated stands has continued to increase for a certain period. After the crown recovery of damaged stands has started, the recovery of most damaged survived trees was most intensive and convergence of defoliated to a different extend stands and trees is characteristic feature of this period. No defoliation threshold has been determined beyond of which recovery of trees would be impossible. Recovery of more than a quarter of damaged trees was registered even in the case of 90% of defoliation. Recovery of dominant trees occurs to be faster of that for suppressed trees within the same level of defoliation. The impact of stand density on the crown recovery rate is negative, the higher density (more intensive competition), the slower recovery of damaged trees. The dependence of growth rate on defoliation was found to be of logistic character: while crown defoliation consists up to 25-30%, tree increment losses are rather inconsiderable, further increase of defoliation leads to the essentially higher increment losses, however having achieved 65-70% defoliation, further increase of defoliation does not result such intensive decrease of radial increment.  相似文献   

11.
Abstract

Analyses of ozone (O3) measurements in conjunction with photochemical modeling were used to assess the feasibility of attaining the federal 8-hr O3 standard in the eastern United States. Various combinations of volatile organic compound (VOC) and oxides of nitrogen (NOx) emission reductions were effective in lowering modeled peak 1-hr O3 concentrations. VOC emissions reductions alone had only a modest impact on modeled peak 8-hr O3 concentrations. Anthropogenic NOx emissions reductions of 46–86% of 1996 base case values were needed to reach the level of the 8-hr standard in some areas. As NOx emissions are reduced, O3 production efficiency increases, which accounts for the less than proportional response of calculated 8-hr O3 levels. Such increases in O3 production efficiency also were noted in previous modeling work for central California. O3 production in some urban core areas, such as New York City and Chicago, IL, was found to be VOC-limited. In these areas, moderate NOx emissions reductions may be accompanied by increases in peak 8-hr O3 levels. The findings help to explain differences in historical trends in 1- and 8-hr O3 levels and have serious implications for the feasibility of attaining the 8-hr O3 standard in several areas of the eastern United States.  相似文献   

12.
Numerous papers analyze ground-level ozone (O3) trends since the 1980s, but few have linked O3 trends with observed changes in nitrogen oxide (NOx) and volatile organic compound (VOC) emissions and ambient concentrations. This analysis of emissions and ambient measurements examines this linkage across the United States on multiple spatial scales from continental to urban. O3 concentrations follow the general decreases in both NOx and VOC emissions and ambient concentrations of precursors (nitrogen dioxide, NO2; nonmethane organic compounds, NMOCs). Annual fourth-highest daily peak 8-hr average ozone and annual average or 98th percentile daily maximum hourly NO2 concentrations show a statistically significant (p < 0.05) linear fit whose slope is less than 1:1 and intercept is in the 30 to >50 ppbv range. This empirical relationship is consistent with current understanding of O3 photochemistry. The linear O3–NO2 relationships found from our multispatial scale analysis can be used to extrapolate the rate of change of O3 with projected NOx emission reductions, which suggests that future declines in annual fourth-highest daily average 8-hr maximum O3 concentrations are unlikely to reach 65 ppbv or lower everywhere in the next decade. Measurements do not indicate increased annual reduction rates in (high) O3 concentrations beyond the multidecadal precursor proportionality, since aggressive measures for NOx and VOC reduction are in place and have not produced an accelerated O3 reduction rate beyond that prior to the mid-2000s. Empirically estimated changes in O3 with emissions suggest that O3 is less sensitive to precursor reductions than is found by the CAMx (v. 6.1) photochemical model. Options for increasing the rate of O3 change are limited by photochemical factors, including the increase in NOx sensitivity with time (NMOC/NOx ratio increase), increase in O3 production efficiency at lower NOx concentrations (higher O3/NOy ratio), and the presence of natural NOx and NMOC precursors and background O3.

Implications:?This analysis demonstrates empirical relations between O3 and precursors based on long term trends in U.S. locations. The results indicate that ground-level O3 concentrations have responded predictably to reductions in VOC and NOx since the 1980s. The analysis reveals linear relations between the highest O3 and NO2 concentrations. Extrapolation of the historic trends to the future with expected continued precursor reductions suggest that achieving the 2014 proposed reduction in the U.S. National Ambient Air Quality Standard to a level between 65 and 70 ppbv is unlikely within the next decade. Comparison of measurements with national results from a regulatory photochemical model, CAMx, v. 6.1, suggests that model predictions are more sensitive to emissions changes than the observations would support.  相似文献   

13.
14.
ABSTRACT

The deterministic modeling of ambient O3 concentrations is difficult because of the complexity of the atmospheric system in terms of the number of chemical species; the availability of accurate, time-resolved emissions data; and the required rate constants. However, other complex systems have been successfully approximated using artificial neural networks (ANNs). In this paper, ANNs are used to model and predict ambient O3 concentrations based on a limited number of measured hydrocarbon species, NOx compounds, temperature, and radiant energy. In order to examine the utility of these approaches, data from the Coastal Oxidant Assessment for Southeast Texas (COAST) program in Houston, TX, have been used. In this study, 53 hydrocarbon compounds, along with O3, nitrogen oxides, and meteorological data were continuously measured during summer 1993. Steady-state ANN models were developed to examine the ability of these models to predict current O3 concentrations from measured VOC and NO concentrations. To predict the future concentrations of O3, dynamic models were also explored and were used for extraction of chemical information such as reactivity estimations for the VOC species.

The steady-state model produced an approximation of O3 data and demonstrated the functional relationship between O3 and VOC-NOx concentrations. The dynamic models were able to the adequately predict the O3 concentration and behavior of VOC-NOx-O3 system a number of hourly intervals into the future. For 3 hr into the future, O3 concentration could be predicted with a root-mean squared error (RMSE) of 8.21 ppb. Extending the models further in time led to an RMSE of 11.46 ppb for 5-hr-ahead values. This prediction capability could be useful in determining when control actions are needed to maintain measured concentrations within acceptable value ranges.  相似文献   

15.
Shanghai Meteorological Administration has established a volatile organic compounds (VOCs) laboratory and an observational network for VOCs and ozone (O3) measurements in the city of Shanghai. In this study, the measured VOCs and O3 concentrations from 15 November (15-Nov) to 26 November (26-Nov) of 2005 in Shanghai show that there are strong day-to-day and diurnal variations. The measured O3 and VOCs concentrations have very different characterizations between the two periods. During 15-Nov to 21-Nov (defined as the first period), VOCs and O3 concentrations are lower than the values during 22-Nov to 28-Nov (defined as the second period). There is a strong diurnal variation of O3 during the second period with maximum concentrations of 40–80 ppbv at noontime, and minimum concentrations at nighttime. By contrast, during the first period, the diurnal variation of O3 is in an irregular pattern with maximum concentrations of only 20–30 ppbv. The VOC concentrations change rapidly from 30–50 ppbv during the first period to 80–100 ppbv during the second period. Two chemical models are applied to interpret the measurements. One model is a regional chemical/dynamical model (WRF-Chem) and another is a detailed chemical mechanism model (NCAR MM). Model analysis shows that the meteorological conditions are very different between the two periods, and are mainly responsible for the different chemical characterizations of O3 and VOCs between the two periods. During the first period, meteorological conditions are characterized by cloudy sky and high-surface winds in Shanghai, resulting in a higher nighttime planetary boundary layer (PBL) and faster transport of air pollutants. By contrast, during the second period, the meteorological conditions are characterized by clear sky and weak surface winds, resulting in a lower nighttime PBL and slower transport of air pollutants. The chemical mechanism model calculation shows that different VOC species has very different contributions to the high-ozone concentrations during the second period. Alkane (40 ppbv) and aromatic (30 ppbv) are among the highest VOC concentrations observed in Shanghai. The analysis suggests that the aromatic is a main contributor for the O3 chemical production in Shanghai, with approximately 79% of the O3 being produced by aromatic. This analysis implies that future increase in VOC (especially aromatic) emissions could lead to significant increase in O3 concentrations in Shanghai.  相似文献   

16.
A field measurement campaign was conducted near a major road in southern Finland from September 15 to October 30, 1995. The concentrations of NO, NO2 and O3 were measured simultaneously at three locations, at three heights (3.5, 6 and 10 m) on both sides of the road. Traffic densities and relevant meteorological parameters were also measured on-site. We have compared measured concentration data with the predictions of the road network dispersion model CAR-FMI, used in combination with a meteorological pre-processing model MPP-FMI. In comparison with corresponding results presented previously in the literature, the agreement of measured and predicted datasets was good, as measured using various statistical parameters. For all data (N=587), the index of agreement (IA) was 0.83, 0.82 and 0.89 for the measurements of NOx, NO2 and O3, respectively. The IA is a statistical measure of the correlation of the predicted and measured time series of concentrations. However, the modelling system overpredicts NOx concentrations with a fractional bias FB=+13%, and O3 concentrations with FB=+8%, while for NO2 concentrations FB=−2%. We also analyzed the difference between model predictions and measured data in terms of meteorological parameters. Model performance clearly deteriorated as the wind direction approached a direction parallel to the road, and for the lowest wind speeds. The range of variability concerning atmospheric stability, ambient temperature and the amount of solar radiation was modest during the measurement campaign. As expected, no clear dependencies of model performance were therefore detected in terms of these parameters. The experimental dataset is available for the evaluation of other roadside dispersion models.  相似文献   

17.
Measurements of hydrogen peroxide (H2O2) and several meteorological and chemical parameters were made for 34 rain events which occurred in Miami, Florida between April, 1995 and October, 1996. The measured H2O2 concentrations ranged from 0.3 to 38.6 μM with an average concentration of 6.9 μM. A strong seasonal dependence for H2O2 concentrations was observed during this period, with highest concentrations in the summer and lower levels in the winter, which corresponds to the stronger solar radiation and higher vaporization of volatile organic compounds (VOCs) in the summer and fall, and the weaker sunlight and lower vaporization in the winter and spring. Measurements also showed a significant increase trend of H2O2 with increasing ambient rainwater temperature. Rains that were out from lower latitude were exposed to higher solar irradiation and contained relatively higher levels of H2O2 than those from the north. All these observations indicate that photochemical reactions that involved volatile organic compounds are the predominant source of H2O2 observed in rainwater. During several individual rainstorms, H2O2 concentration was found to increase as a function of time due to electrical storm activities. This finding suggests that lightning could be an important factor that determines the level of H2O2 during thunderstorms. Statistical data showed that the highest concentrations of H2O2 were observed only in rains containing low levels of nonsea-salt sulfate (NSS), nitrate and hydrogen ion. H2O2 concentrations in continental originated rains were much lower than marine originated ones, indicating that air pollutants in continental rains could significantly deplete the H2O2 concentration in atmospheric gas-phase, clouds and rainwater.  相似文献   

18.
Ozone Transport     
Elevated concentrations of ozone, often above the national ambient air quality standard for photochemical oxidants, have been measured in both urban and rural areas of Connecticut. One such episode took place on June 10, 1974. Ozone levels, after stabilizing at values slightly above the standard (i.e., 80 to 110 ppb; Connecticut generated ozone concentrations), rose sharply late in the afternoon reaching concentrations as high as 310 ppb (almost 4 times the standard) in Hartford. The trajectory of the air mass, which arrived in Hartford at the time of maximum O3 occurence, had its origin in the metropolitan New York area during the early morning rush hour on the episode day. This illustrates that the advective transport of O3 and O3 precursors into Connecticut from New York are probably responsible for a significant portion (approximately two-thirds) of the elevated O3 concentrations measured throughout Connecticut on days when winds are from the south-southwest direction. The fact that peak O3 levels occur late in the afternoon, several hours after maximum sunlight intensity, reinforces the conclusion that excessive O3 concentrations developed as O3 and ozone precursors were generated in the vicinity of New York City and then drifted inland into Connecticut on the afternoon sea breeze.

It appears to be unrealistic to develop a hydrocarbon control strategy for Connecticut in order to meet the photochemical oxidant ambient air quality standard when O3 and/or ozone precursors ad-vectively transported into the State cause oxidant levels to exceed the standard. The complete cessation of all anthropogenic hydrocarbon emissions in Connecticut would not necessarily assure that the standard would be attained here. The implication is that a regional (i.e., the eastern part of the United States) hydrocarbon control strategy is needed to reduce adequately ozone formation and transport so as to allow Connecticut to meet the current oxidant standard.  相似文献   

19.
The city of Santiago, Chile experiences frequent high pollution episodes and as a consequence very high ozone concentrations, which are associated with health problems including increasing daily mortality and hospital admissions for respiratory illnesses. The development of ozone abatement strategies requires the determination of the potential of each pollutant to produce ozone, taking into account known mechanisms and chemical kinetics in addition to ambient atmospheric conditions. In this study, the photochemical formation of ozone during a summer campaign carried out from March 8–20, 2005 has been investigated using an urban photochemical box model based on the Master Chemical Mechanism (MCMv3.1). The MCM box model has been constrained with 10 min averages of simultaneous measurements of HONO, HCHO, CO, NO, j(O1D), j(NO2), 31 volatile organic compounds (VOCs) and meteorological parameters. The O3–NOx–VOC sensitivities have been determined by simulating ozone formation at different VOC and NOx concentrations. Ozone sensitivity analyses showed that photochemical ozone formation is VOC-limited under average summertime conditions in Santiago. The results of the model simulations have been compared with a set of potential empirical indicator relationships including H2O2/HNO3, HCHO/NOy and O3/NOz. The ozone forming potential of each measured VOC has been determined using the MCM box model. The impacts of the above study on possible summertime ozone control strategies in Santiago are discussed.  相似文献   

20.
Passive diffusion tubes are recognised as a cost-effective sampling method for characterising the spatial variability, as well as the seasonal and annual trends, of NO2 concentrations in urban areas. In addition, NOX and O3 passive diffusion tubes have been developed and deployed in urban and rural areas. Despite their many advantages (e.g. low operational and analysis cost, small size and no need for power supply), they have certain limitations mainly related to their accuracy and precision. In particular, the absorbent solution used, the length of the exposure period, the exact location and use of protective devices, and other environmental conditions (e.g. wind, ambient temperature and relative humidity) may have a significant impact on the performance of passive diffusion tubes. The aim of this study is to evaluate the performance of co-located NO2, NOX and O3 diffusion tubes in an urban environment.A one-year passive sampling campaign was carried out in Birmingham (UK) for this purpose. NO2, NOX and O3 diffusion tubes (including triplicate sets of each) were co-located at one urban background and two roadside permanent air quality monitoring stations equipped with standard gas analysers. In addition, meteorological data, such as wind speed and direction, ambient temperature and relative humidity, were obtained during the same period of time. A thorough QA/QC procedure, including storage and laboratory blanks was followed throughout the campaign. The analysis of results showed a very good agreement of NO2 passive samplers with co-located chemiluminescence analysers, but substantial underestimations of total NOX levels by the diffusion tubes. The O3 diffusion sampler appeared to marginally overestimate the automatic UV analyser results, especially during warm weather periods.  相似文献   

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