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1.
Understanding the chemical links between ozone (O3) and its two main precursors, nitrogen oxides (NOx) and volatile organic compounds (VOC), is important for designing effective photochemical smog reduction strategies. This chemical relationship will determine which precursor (NOx or VOC) emission reduction will be more effective for decreasing the ozone formation. Under certain conditions, ozone levels decrease as a result of a reduction in NOx emissions but do not respond significantly to changes in VOC emissions (NOx-sensitive condition), while under other conditions ozone concentrations decrease in response to reductions in VOCs and may even increase when NOx emissions are reduced (VOC-sensitive conditions). Indicator species can be used to assess the sensitivity of ozone to changes in the emissions of its precursors. These indicators are species or species ratios involved in ozone photochemistry which reflect the primary chemical process through which the ozone was formed. In this work we use the MM5-CAMx model system to explore the behaviour of various indicator species during two meteorological situations featuring different atmospheric conditions in a complex terrain area. The results show that indicators based on nitrogen compounds (i.e,. NOy and NOz) are suitable for defining the transition range from VOC- to NOx-sensitive chemistry, and that despite the uncertainties associated with the use of chemical indicators, the ratios O3/NOy and O3/NOz may provide a simple and useful way to summarize the response of ozone to changes in NOx and VOC emissions in Southwestern Spain.  相似文献   

2.
Abstract

To evaluate future climate change in the middle atmosphere and the chemistry–climate interaction of stratospheric ozone, we performed a long-term simulation from 1960 to 2050 with boundary conditions from the Intergovernmental Panel on Climate Change A1B greenhouse gas scenario and the World Meteorological Organization Ab halogen scenario using the chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). In addition to this standard simulation we performed five sensitivity simulations from 2000 to 2050 using the rerun files of the simulation mentioned above. For these sensitivity simulations we used the same model setup as in the standard simulation but changed the boundary conditions for carbon dioxide (CO2), methane (CH4), nitrous oxide (N2O), and ozone-depleting substances (ODS). In the first sensitivity simulation we fixed the mixing ratios of CO2, CH4, and N2O in the boundary conditions to the amounts for 2000. In each of the four other sensitivity simulations we fixed the boundary conditions of only one of CO2, CH4, N2O, or ODS to the year 2000.

In our model simulations the future evolution of greenhouse gases leads to significant cooling in the stratosphere and mesosphere. Increasing CO2 mixing ratios make the largest contributions to this radiative cooling, followed by increasing stratospheric CH4, which also forms additional H2O in the upper stratosphere and mesosphere. Increasing N2O mixing ratios makes the smallest contributions to the cooling. The simulated ozone recovery leads to warming of the middle atmosphere.

In the EMAC model the future development of ozone is influenced by several factors. 1) Cooler temperatures lead to an increase in ozone in the upper stratosphere. The strongest contribution to this ozone production is cooling due to increasing CO2 mixing ratios, followed by increasing CH4. 2) Decreasing ODS mixing ratios lead to ozone recovery, but the contribution to the total ozone increase in the upper stratosphere is only slightly higher than the contribution of the cooling by greenhouse gases. In the polar lower stratosphere a decrease in ODS is mainly responsible for ozone recovery. 3) Higher NOx and HOx mixing ratios due to increased N2O and CH4 lead to intensified ozone destruction, primarily in the middle and upper stratosphere, from additional NOx; in the mesosphere the intensified ozone destruction is caused by additional HOx. In comparison to the increase in ozone due to decreasing ODS, ozone destruction caused by increased NOx is of similar importance in some regions, especially in the middle stratosphere. 4) In the stratosphere the enhancement of the Brewer-Dobson circulation leads to a change in ozone transport. In the polar stratosphere increased downwelling leads to additional ozone in the future, especially at high northern latitudes. The dynamical impact on ozone development is higher at some altitudes in the polar stratosphere than the ozone increase due to cooler temperatures. In the tropical lower stratosphere increased residual vertical upward transport leads to a decrease in ozone.  相似文献   

3.
During the BERLIOZ field phase on 20 July 1998 a 40 km wide ozone-plume 30 to 70 km north of Berlin in the lee of the city was detected. The ozone mixing ratio inside the plume was app. 15 ppb higher than outside, mainly caused by high ozone precursor emissions in Berlin, resulting in a net chemical ozone production of 6.5 ppb h–1, which overcompensates ozone advection of –3.6 ppb h–1 andturbulent diffusion of –1.1 ppb h–1. That means, although moreozone leaves the control volume far in the lee of Berlin than enters it at the leeside cityborder and although turbulent diffusion causes a loss of ozone in the leeside control volume the chemical production inside the volume leads to a net ozone increase. Using a semi-Lagrangian mass budget method to estimate the net ozone production, 5.0 ppb h–1 are calculated for theplume. This means a fraction of about 20% of ozone in the plume is producedby local emissions, therefore called `home made' by the Berlin emissions. For the same area KAMM/DRAIS simulations using an observation based initialisation, results in a net production rate between 4.0 and 6.5 ppbh–1, while the threefold nested EURAD model gives 6.0 ppbh–1. The process analysis indicates in many cases goodagreement (10% or better) between measurements and simulations not only in the ozone concentrations but also with respect to the physical and chemical processes governing the total change. Remaining differences are caused by different resolution in time and space of the models and measurements as well as by errors in the emission calculation.The upwind-downwind differences in PAN concentrations are partly similar to those of ozone, because in the BERLIOZ case they are governed mainly by photochemical production. While in the stable boundary layer at night and windward of Berlin 0.1 to 0.3 ppb are detected, in the centre of the plume at noon concentrations between 0.75 ppb and 1.0 ppb are measured. The O3/PAN ratio is about 80 to 120 and thus due to the relatively lowPAN concentrations significantly higher than found in previous studies. The low PAN formation on 20 July, was mainly restricted by the moderate nonmethane hydrocarbon levels, whereas high PAN concentrations of 3.0 ppb on 21 July, are caused by local production in the boundary layer and by large scale advection aloft.  相似文献   

4.
The objective of this study is to present differences in the variability of observed and ozone-mixing ratios simulated by a three-dimensional atmospheric chemical model using two chemical mechanisms. In this study the Comprehensive Air Quality Model with Extensions is used to make ozone simulations with the Carbon Bond mechanism, versions 4 and 5. The Paso del Norte region is used as a test-bed for these simulations. The shared variance between the simulations and measurements is typical for air quality models ranging from 0.51 to 0.86 for both mechanisms. The smallest mean normalized gross error is about 31 % with CB4 but the normalized bias is over 30 % as well. Boundary conditions, emissions and other factors affect the levels of ozone of the simulated mixing ratios and therefore error and bias but these factors have a much less affect on the simulated ozone variability. The differences in the ozone variability of the measurements and the simulations are very large and different for the two chemical mechanisms. There are many more instances of low ozone mixing ratios in the measurements than in the simulated ozone. One possible explanation is that these differences are due to problems associated with comparing point measurements with grid averages. A more disturbing possibility is that the bias could be due to the procedures used in the development and testing of air quality modeling systems. Air quality mechanisms are evaluated against environmental chamber data where the chemistry occurs at high concentrations and this may lead to a systematic positive bias in ozone simulations.  相似文献   

5.
A comparison of the atmospheric chemistry mechanisms EMEP (Co-operative Programme for Monitoring and Evaluation of the Long-Range Transmission of Air Pollutants in Europe), RADM2 (Regional Acid Deposition Model, version 2) and RACM (Regional Atmospheric Chemistry Mechanism) has been conducted. Each mechanism was used to simulate the PLUME case of Kuhn et al. (1998) and to simulate an additional 150 and 81 scenarios with and without emissions, respectively. These simulations covered scenarios that ranged from relatively clean, through rural and polluted urban conditions. Ozone isopleths and scatter plots were generated from the simulations. The mechanisms were compared primarily on the basis of calculated ozone and ozone precursor concentrations. For the gas-phase ozone precursors the differences between the mechanisms were rather small under clean conditions and more significant under polluted conditions. The differences were especially significant for the concentrations of NO2 and organic peroxy radicals. In general the EMEP mechanism yielded the most ozone and the RADM2 mechanism yielded the least. Furthermore the results suggest that a broad range simulation conditions should be used to compare mechanisms and not just a few selected scenarios.  相似文献   

6.
We have studied long-term changes in tropospheric NO2 over South India using ground-based observations, and GOME and OMI satellite data. We have found that unlike urban regions, the region between Eastern and Western Ghat mountain ranges experiences statistically significant decreasing trend. There are few ground-based observatories to verify satellite based trends for rural regions. However, using a past study and recent measurements we show a statistically significant decrease in NOX and O3 mixing ratio over a rural location (Gadanki; 13.48° N, 79.18° E) in South India. In the ground-based records of surface NOX, the concentration during 2010–11 is found to be lower by 0.9 ppbv which is nearly 60 % of the values observed during 1994–95. Small but statistically significant decrease in noon-time peak ozone concentration is also observed. Noon-time peak ozone concentration has decreased from 34?±?13 ppbv during 1993–96 to 30?±?15 ppbv during 2010–11. NOX mixing ratios are very low over Gadanki. In spite of low NOX values (0.5 to 2 ppbv during 2010–11), ozone mixing ratios are not significantly low compared to many cities with high NOX. The monthly mean ozone mixing ratio varies from 9 ppbv to 37 ppbv with high values during Spring and low values during late Summer. Using a box-model, we show that presence of VOCs is also very important in addition to NOX in determining ozone levels in rural environment and to explain its seasonal cycle.  相似文献   

7.
The relationship between the emission of ozone precursors and the chemical production of tropospheric ozone(O3) in the Pearl River Delta Region(PRD) was studied using numerical simulation.The aim of this study was to examine the volatile organic compound(VOC)-or nitrogen oxide(NOx =NO+NO2)limited conditions at present and when surface temperature is increasing due to global warming,thus to make recommendations for future ozone abatement policies for the PRD region.The model used for this application is the U.S.Environmental Protection Agency’s(EPA’s) third-generation air-quality modeling system;it consists of the mesoscale meteorological model MM5 and the chemical transport model named Community Multi-scale Air Quality(CMAQ).A series of sensitivity tests were conducted to assess the influence of VOC and NOx variations on ozone production.Tropical cyclone was shown to be one of the important synoptic weather patterns leading to ozone pollution.The simulations were based on a tropicalcyclone-related episode that occurred during 14-16 September 2004.The results show that,in the future,the control strategy for emissions should be tightened.To reduce the current level of ozone to meet the Hong Kong Environmental Protection Department(EPD) air-quality objective(hourly average of 120 ppb),emphasis should be put on restricting the increase of NOx emissions.Furthermore,for a wide range of possible changes in precursor emissions,temperature increase will increase the ozone peak in the PRD region;the areas affected by photochemical smog are growing wider,but the locations of the ozone plume are rather invariant.  相似文献   

8.
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9.
Abstract

The dependence of ozone formation on the mixing ratios of volatile organic compounds (VOCs) and nitrogen oxides (NOx) has been widely studied. In addition to the atmospheric levels of VOCs and NOx, the extent of photochemical processing of VOCs has a strong impact on ozone levels. Although methods for measuring atmospheric mixing ratios of VOCs and NOx are well established and results of those measurements are widely available, determination of the extent of photochemical processing of VOCs, known as photochemical age (PCA), is difficult. In this article a recently developed methodology for the determination of PCA for individual compounds based on the change in their stable carbon isotope composition is used to investigate the dependence between ozone and VOC or NOx mixing ratios at a rural site in Ontario, Canada, during fall and winter. The results show that under these conditions the variability in VOC mixing ratios is predominantly a result of the varying impact of local emissions and not a result of changes in the extent of atmospheric processing. This explains why the mixing ratio of ozone shows no systematic dependence on the mixing ratios of VOCs or NOx in this environment and at this time of the year.  相似文献   

10.
Presented is a detailed comparison of CH4 and δ13C–CH4 measurements with simulations of the global transport model TM3. Experimental data were obtained during campaigns along the Trans-Siberian railroad in the framework of the TROICA project. Two summer (1999 and 2001) and one spring (2003) expeditions are evaluated. Model simulations include sensitivity tests to further investigate the isotopic composition of natural gas and emissions from Siberian wetlands. Comparison of the average mixing ratio of methane and its isotopic composition (δ13C) has been performed for different geographic zones, including the European part of Russia, Western Siberia and Central Siberia. Simulations are in reasonable agreement with the measurements for the European part of Russia and confirm a high contribution of natural gas to the observed methane levels. An increase of emission from bogs shifts the simulated methane isotopic composition closer to the observations. The relative importance of the Western Siberia emissions in current inventories is underestimated in comparison with other wetland regions in the former USSR. Simulated average mixing ratios are in a good agreement with the observations in Central Siberia, while 13C(CH4) values tend to be higher than measured in all considered scenarios. These results point to a bias in the modeled source mixture over Russia, which could be repaired by shifting emissions from isotopically heavy methane sources (e.g. coal, oil or biomass burning) to light sources (e.g. wetlands, ruminants, waste treatment). Alternatively, the average isotopic signature of Siberian wetlands may be lighter than expected.  相似文献   

11.
The seasonal and diurnal variations of ozone mixing ratios have been observed at Niwot Ridge. Colorado. The ozone mixing ratios have been correlated with the NO x (NO+NO2) mixing ratios measured concurrently at the site. The seasonal and diurnal variations in O3 can be reasonably well understood by considering photochemistry and transport. In the winter there is no apparent systematic diurnal variation in the O3 mixing ratio because there is little diurnal change of transport and a slow photochemistry. In the summer, the O3 levels at the site are suppressed at night due to the presence of a nocturnal inversion layer that isolated ozone near the surface, where it is destroyed. Ozone is observed to increase in the summer during the day. The increases in ozone correlate with increasing NO x levels, as well as with the levels of other compounds of anthropogenic origin. We interpret this correlation as in-situ or in-transit photochemical production of ozone from these precursors that are transported to our site. The levels of ozone recorded approach 100 ppbv at NO x mixing ratios of approximately 3 ppbv. Calculations made using a simple clean tropospheric chemical model are consistent with the NO x -related trend observed for the daytime ozone mixing ratio. However, the chemistry, which does not include nonmethane hydrocarbon photochemistry, underestimates the observed O3 production.  相似文献   

12.
In this work, the influence of South Asian biomass burning emissions on O3 and PM2.5 concentrations over the Tibetan Plateau (TP) is investigated by using the regional climate chemistry transport model WRF-Chem. The simulation is validated by comparing meteorological fields and pollutant concentrations against in situ observations and gridded datasets, providing a clear perspective on the spatiotemporal variations of O3 and PM2.5 concentrations across the Indian subcontinent, including the Tibetan Plateau. Further sensitivity simulations and analyses show that emissions from South Asian biomass burning mainly affect local O3 concentrations. For example, contribution ratios were up to 20% in the Indo-Gangetic Plain during the pre-monsoon season but below 1% over the TP throughout the year 2016. In contrast, South Asian biomass burning emissions contributed more than 60% of PM2.5 concentration over the TP during the pre-monsoon season via significant contribution of primary PM2.5 components (black carbon and organic carbon) in western India that were lofted to the TP by westerly winds. Therefore, it is suggested that cutting emissions from South Asian biomass burning is necessary to alleviate aerosol pollution over the TP, especially during the pre-monsoon season.  相似文献   

13.
Airborne measurements of stratospheric ozone and N2O from the SCIAMACHY (Scanning Imaging Absorption Spectrometer) Validation and Utilization Experiment (SCIA-VALUE) are presented. The campaign was conducted in September 2002 and February–March 2003. The Airborne Submillimeter Radiometer (ASUR) observed stratospheric constituents like O3 and N2O, among others, spanning a latitude from 5°S to 80°N during the survey. The tropical ozone source regions show high ozone volume mixing ratios (VMRs) of around 11 ppmv at 33 km altitude, and the altitude of the maximum VMR increases from the tropics to the Arctic. The N2O VMRs show the largest value of 325 ppbv in the lower stratosphere, indicating their tropospheric origin, and they decrease with increasing altitude and latitude due to photolysis. The sub-tropical and polar mixing barriers are well represented in the N2O measurements. The most striking seasonal difference found in the measurements is the large polar descent in February–March. The observed features are interpreted with the help of SLIMCAT and Bremen Chemical Transport Model (CTMB) simulations. The SLIMCAT simulations are in good agreement with the measured O3 and N2O values, where the differences are within 1 ppmv for O3 and 15 ppbv for N2O. However, the CTMB simulations underestimate the tropical middle stratospheric O3 (1–1.5 ppmv) and the tropical lower stratospheric N2O (15–30 ppbv) measurements. A detailed analysis with various measurements and model simulations suggests that the biases in the CTMB simulations are related to its parameterised chemistry schemes.  相似文献   

14.
 The potential of aircraft-induced ozone changes to force a substantial climate impact is investigated by means of simulations with an atmospheric general circulation model, coupled to a mixed layer ocean model. We present results from several numerical experiments that are based on ozone change patterns for 1992 aviation and on a future scenario for the year 2015. In both cases, the climate signal is statistically significant. The strength of the ozone impact is of comparable magnitude to that arising from aircraft CO2 emissions, thus meaning a non-negligible contribution to the total climate effect of aviation emissions. There are indications of a characteristic signature of the aircraft ozone related temperature response pattern, distinctly different from that associated with the increase of well-mixed greenhouse gases. Likewise, the climate sensitivity to non-uniform ozone changes including a strong concentration perturbation at the tropopause may be higher than the climate sensitivity to uniform changes of a greenhouse gas. In a hierarchy of experiments, for which the spatial structure of an aircraft-related ozone perturbation was left fixed, while the amplitude of the perturbation was artificially increased, the climate signal depends in a non-linear way on the radiative forcing. Received: 10 September 1998 / Accepted: 4 May 1999  相似文献   

15.
Emission inventories of NOx, CO, and individual volatile organic compounds (VOC), highly resolved in space and time, belong to the most important input parameters for chemistry and transport models (CTM) used for ozone prediction. Because of the decisive influence of the input quality on the outcome of CTM simulations, the quality of emission inventories has to be assessed. This paper presents an experimental evaluation of the highly resolved emission inventories for the city of Augsburg. The emissions of the city, determined in March and October 1998 using mass balance and tracer techniques, and derived from the measured receptor concentration ratios, were compared with emissions modeled from an emission inventory. The modeled CO emissions were in agreement with the measured ones within the combined experimental and model uncertainties. More detailed CO emission model simulations suggest that the tendency of calculated CO emissions being smaller than the measured ones may be due to higher traffic activity in Augsburg. Modeled NOx emissions were in agreement with the measured ones within the combined experimental and model uncertainties. Large deviations between modeled and measured values have been found for some individual NMHC compounds. The measured NMHC emission fingerprints were dominated by mobile sources. Substantial model predicted NMHC emissions from the solvent use could not be detected by measurements suggesting that they may not be correctly represented by the emission model.  相似文献   

16.
应用大气化学模式WRF-Chem(Weather Research and Forecast-Chemistry),分别选用亚洲排放源清单INTEX-B(Intercontinental Chemical Transport Experiment-Phase B)、REASv2.1(Regional Emission inventory in Asia version 2.1)以及全球排放源清单HTAP_v2(Hemispheric Transport of Air Pollution version 2),对浙江省2013年12月进行模拟,分别记为IN、RE和HT试验,研究人为源排放清单对大气污染物浓度数值模拟的影响。结果表明,3组试验合理的反映出PM2.5(空气动力学当量直径小于等于2.5μm的颗粒物,即细颗粒物)、PM10(空气动力学当量直径小于等于10μm的颗粒物,即可吸入颗粒物)和NO_2近地面浓度的时空分布特征,相关系数为0.5~0.8,85%以上的模拟值落在观测值的0.5~2倍范围内,但对SO_2近地面浓度模拟较差。IN、RE、HT试验对PM2.5和PM10的模拟偏差均成递减趋势,约为30%、16%和6%,HT试验的模拟值更加接近观测。INTEX-B清单中PM2.5的一次排放与二次气溶胶前提物SO_2均高于REAS与HTAP清单,因此会导致更多的硫酸盐生成,从而进一步增加PM2.5浓度。HTAP_v2清单中较低的NH3排放会抑制硝酸盐的生成,从而有助于降低PM2.5浓度。3个清单的基准年与模拟年的差异对SO_2浓度模拟的准确性影响更大,INTEX-B清单中SO_2排放量明显高于REASv2.1与HTAP_v2清单,尤其在浙北和沿海工业发达地区,导致IN试验模拟的SO_2在这些地区存在明显高估。3组试验模拟的NO_2浓度偏差最小且更为接近(-8%~4%),主要原因是3个清单在浙江省的NOx排放十分一致。从3组试验结果之间的差异程度来看,浙江省范围内PM2.5、PM10、SO_2和NO_2逐日浓度模拟值之间的平均差异程度分别约为14%、15%、51%和16%,最大差异程度分别为69%、78%、137%和132%。月均浓度与逐日浓度的平均差异程度基本一致,但最大差异程度明显更低。总体来看3组试验模拟的PM2.5、PM10与NO_2的差异程度明显低于SO_2。  相似文献   

17.
The objectives of this study were to identify species and levels of volatile organic compounds (VOCs), and determine their oxidation capacity in the rural atmosphere of western Senegal. A field study was conducted to obtain air samples during September 14 and September 15, 2006 for analyses of VOCs. Methanol, acetone, and acetaldehyde were the most abundant detected chemical species and their maximum mixing ratios reached 6 parts per billion on a volume basis (ppbv). Local emission sources such as firewood and charcoal burning strongly influenced VOC concentrations. The VOC concentrations exhibited little temporal variations due to the low reactivity with hydroxyl radicals, with reactivity values ranging from 0.001 to 2.6 s−1. The conditions in this rural site were rather clean. Low ambient NO x levels limited ozone production. Nitrogen oxide (NO x ) levels reached values less than 2 ppbv and maximum VOC/NO x ratios reached 60 ppbvC/ppbv, with an overall average of 2.4 ± 4.5 ppbvC/ppbv. This indicates that the rural western Senegal region is NO x limited in terms of oxidant formation potential. Therefore, during the study period photochemical ozone production became limited due to low ambient NO x levels. The estimated ozone formation reactivity for VOCs was low and ranged between −5.5 mol of ozone/mol of benzaldehyde to 0.6 mol/mol of anthropogenic dienes.  相似文献   

18.
Near-total depletions of ozone have been observed in the Arctic spring since the mid 1980s. The autocatalytic reaction cycles involving reactive halogens are now recognized to be of main importance for ozone depletion events in the polar boundary layer. We present sensitivity studies using the model MISTRA in the box-model mode on the influence of chemical species on these ozone depletion processes. In order to test the sensitivity of the chemistry under polar conditions, we compared base runs undergoing fluxes of either Br2, BrCl, or Cl2 to induce ozone depletions, with similar runs including a modification of the chemical conditions. The role of HCHO, H2O2, DMS, Cl2, C2H6, HONO, NO2, and RONO2 was investigated. Cases with elevated mixing ratios of HCHO, H2O2, DMS, Cl2, and HONO induced a shift in bromine speciation from Br / BrO to HOBr/HBr, while high mixing ratios of C2H6 induced a shift from HOBr/HBr to Br/BrO. The shifts from Br/BrO to HOBr/HBr accelerated the aerosol debromination, but also increased the total amount of deposited bromine at the surface (mainly via increased deposition of HOBr). For all NOy species studied (HONO, NO2, RONO2) the chemistry is characterized by an increased bromine deposition on snow reducing the amount of reactive bromine in the air. Ozone is less depleted under conditions of high mixing ratios of NOx. The production of HNO3 led to the acid displacement of HCl, and the release of chlorine out of salt aerosol (Cl2 or BrCl) increased.  相似文献   

19.
We conduct a retrospective study of ozone formation in the Lower Fraser Valley (LFV), using numerical models, observations, and emission inventories in order to understand relationships between reductions in local precursor emissions and episodic ozone concentrations. Because there appears to be little or no impact from precursor emissions upwind of the LFV during ozone episodes and because background concentrations of ozone and its precursors are generally from the North Pacific Ocean and quite low, summertime ozone formation in the LFV is mostly caused by local emissions. The observed change in behaviour of ozone formation must, therefore, arise from reductions in local precursor emissions. We exploit the observed changing precursor emission–ozone concentration relationship to perform a dynamical model evaluation. Complicating the analyses are an observed shift in the population patterns within the valley over the last 25 years and a small but documented change in the tropospheric background concentration of ozone. Ozone formation for four episodes, which capture the observed changes in ozone reduction and the different meteorological types that occur during LFV ozone events, are investigated using the Weather Research and Forecasting (WRF)-Sparse Matrix Operator Kernel Emissions (SMOKE)-Community Multiscale Air Quality (CMAQ) modelling system. In order to provide realistic simulations of past events, the SMOKE emission inventory is adjusted to account for temporal changes in the amount of emissions and locations of emission sources. Model output is compared with continuous observations, data collected from field campaigns, and previous modelling efforts. The WRF-SMOKE-CMAQ modelling framework is able to capture the changes in both the magnitude of the ozone concentrations and its spatial behaviour over the period of study. Many of the simulations show that the highest ozone concentrations occur outside the area sampled by the fixed monitoring network and within the LFV's numerous tributary valleys. Not all modelled episodes achieved the same agreement with observations and some of these discrepancies are likely related to shortcomings in the meteorological modelling. The model consistently overpredicts ozone at a number of stations within the City of Vancouver and underpredicts daytime NOx concentrations there. Both results are consistent with a deficiency in NOx emissions. The model shows a changing bias over time which also suggests uncertainties in the emission backcasting.

RÉSUMÉ?[Traduit par la rédaction] Nous menons une étude rétrospective de la formation de l'ozone dans le vallée du bas Fraser (VBF) à l'aide de modèles numériques, d'observations et d'inventaires d’émissions dans le but de comprendre les relations entre les réductions dans les émissions locales de polluants précurseurs et les concentrations épisodiques d'ozone. Parce qu'il semble n'y avoir que peu ou pas d'impact des émissions de polluants précurseurs en amont de la VBF durant les épisodes d'ozone et parce que les concentrations de fond de l'ozone et de ses précurseurs proviennent généralement du Pacifique Nord et sont très faibles, la formation d'ozone en été dans la VBF est principalement attribuable aux émissions locales. Le changement de comportement observé dans la formation d'ozone doit par conséquent résulter de réductions dans les émissions locales de précurseurs. Nous exploitons la relation changeante observée entre les émissions de précurseurs et la concentration de l'ozone pour effectuer une évaluation par modèle dynamique. Un déplacement observé dans les configurations de population à l'intérieur de la vallée au cours des 25 dernières années et un changement, petit mais documenté, dans la concentration troposphérique de fond de l'ozone viennent compliquer les analyses. Nous étudions la formation d'ozone lors de quatre épisodes qui capturent les changements observés dans la réduction d'ozone et les différents types météorologiques qui se produisent pendant les événements d'ozone dans la VBF en nous servant du système de modélisation SMOKE (Sparse Matrix Operator Kernel Emissions) – CMAQ (Community Multiscale Air Quality) du WRF (Weather Research and Forecasting). Afin de fournir des simulations réalistes des événements passés, nous avons ajusté l'inventaire d’émissions SMOKE pour tenir compte des changements au cours du temps dans la quantité d’émissions et dans la position des sources d’émissions. Nous comparons la sortie du modèle avec les observations continues, les données recueillies lors d’études sur le terrain et les efforts de modélisation précédents. Le cadre de modélisation WRF-SMOKE-CMAQ est capable de capturer les changements dans la grandeur des concentrations d'ozone ainsi que dans son comportement spatial durant la période de l’étude. Plusieurs des simulations montrent que les plus fortes concentrations d'ozone se produisent en dehors de la région échantillonnée par le réseau fixe de surveillance et à l'intérieur des nombreuses vallées affluentes de la VBF. Tous les épisodes modélisés n'ont pas exhibé le même accord avec les observations et certaines de ces divergences sont vraisemblablement dues à des lacunes dans la modélisation météorologique. Le modèle surprévoit constamment l'ozone à certaines stations dans la ville de Vancouver et sous-prévoit les concentrations de NOx le jour à cet endroit. Les deux résultats sont cohérents avec un déficit dans les émissions de NOx. Le modèle montre un biais qui change avec le temps, ce qui porte à croire à des incertitudes dans les émissions rétrospectives.  相似文献   

20.
The mixing ratios of surface O3 were measured at St. John's College, Agra, an urban and traffic influenced area for the period of 2000–2002. The monthly averaged O3 mixing ratios ranged between 8 to 40 ppb with an annual average of 21 ppb. Strong diurnal and seasonal variations in O3 mixing ratios were observed throughout the year except for monsoon season. The mixing ratios of O3 follow the surface temperature cycle and solar radiation (r = 0.72 and r = 0.65 with temperature and solar radiation, respectively). Concentrations were higher with winds associated with NE and NW direction indicating the impact of pollution sources on surface O3 concentration. Exceedance of ozone critical level was calculated using the AOT 40 index and found to be 840 ppb.h and 2430 ppb.h for summer and winter seasons, respectively. The present O3 exposures are lower than the critical level of O3 and suggest that the present level of O3 does not have any impact on reduction in crop yields.  相似文献   

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