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1.
Since rain systems show a wide variation in structure in both time and space, it is virtually impossible to model in detail the behaviour of sulphur passing through a rain system. Instead, an attempt has been made to determine the scale of the major processes going on in a frontal rain system based on the conservation equations for cloudwater, rainwater, SO2 in air, sulphate in cloud and sulphate in rainwater. When this procedure is followed it is found that cloud and rainwater amounts are determined largely as a dynamic balance between cloudwater condensation and accretion of cloud drops by rain. The removal of SO2 in rain is mainly determined by the oxidation of SO2 in cloud, enhanced by oxidation in rain. In the case when oxidation of SO2 by O3 is the primary oxidation pathway a simple formula is derived for the fractional removal efficiency, which shows which parameters are of greatest importance and has potential use in the current generation of long-range transport models. This formula shows that the removal efficiency is a strongly non-linear function of sulphur dioxide concentration. At regional average SO2 concentrations removal is efficient, but decreases rapidly at higher SO2 concentrations.  相似文献   

2.
A three-dimensional Eulerian hemispheric air pollution model, the Danish Eulerian Hemispheric Model (DEHM), is in development at the National Environmental Research Institute (NERI). The model has been used to study long-range transport of air pollution in the Northern Hemisphere. The present version of the model includes long-range transport of sulphur dioxide (SO2) and particulate sulphate (SC42−. The chemistry in the model is described by a simple linear oxidation of SO2 to SO42−, and the wet deposition of SO2 and SO4 is estimated based on the amount of precipitation, which is calculated from the contents of liquid cloud water (see Christensen, Air Pollution Modelling and its Applicatioons, Vol. X, pp. 119–127, Vol. XI, pp. 249–256, Plenum press, New York; 1995, Ph.D. thesis, National Environmental Research Institute, Denmark). The model has been used to study the air pollution in the Arctic. Results from yr simulation with an analysis of the results is presented: the model results are verified by comparisons, to measurements not only from the Arctic region but also from Europe and Canada. Some examples of episodes in the Arctic including analysis of the meteorological conditions during the episodes are presented. Finally, the model has been used to estimate the contribution from the different source regions on the northern hemisphere to the Arctic sulphur pollution.  相似文献   

3.
Fine particulate matter (PM) is relevant for human health and its components are associated with climate effects. The performance of chemistry transport models for PM, its components and precursor gases is relatively poor. The use of these models to assess the state of the atmosphere can be strengthened using data assimilation. This study focuses on simultaneous assimilation of sulphate and its precursor gas sulphur dioxide into the regional chemistry transport model LOTOS–EUROS using an ensemble Kalman filter. The process of going from a single component setup for SO2 or SO4 to an experiment in which both components are assimilated simultaneously is illustrated. In these experiments, solely emissions, or a combination of emissions and the conversion rates between SO2 and SO4 were considered uncertain. In general, the use of sequential data assimilation for the estimation of the sulphur dioxide and sulphate distribution over Europe is shown to be beneficial. However, the single component experiments gave contradicting results in direction in which the emissions are adjusted by the filter showing the limitations of such applications. The estimates of the pollutant concentrations in a multi-component assimilation have found to be more realistic. We discuss the behavior of the assimilation system for this application. The model uncertainty definition is shown to be a critical parameter. The increased complexity associated with the simultaneous assimilation of strongly related species requires a very careful specification of the experiment, which will be the main challenge in the future data assimilation applications.  相似文献   

4.
The chemical composition of pollutant species in precipitation sampled daily or weekly at 10 sites in Ireland for the five-year period, 1994–1998, is presented. Sea salts accounted for 81% of the total ionic concentration. Approximately 50% of the SO42− in precipitation was from sea-salt sources. The proportion of sea salts in precipitation decreased sharply eastwards. In contrast, the concentration of NO3 and the proportion of non-sea-salt SO42− increased eastwards reflecting the closer proximity to major emission sources. The mean (molc) ratio of SO42−:NO3 was 1.6 for all sites, indicating that SO42− was the major acid anion.The spatial correlation between SO42−, NO3 and NH4+ concentrations in precipitation was statistically significant. The regional trend in NO3 concentration was best described by linear regression against easting. SO42− concentration followed a similar pattern. However, the regression was improved by inclusion of elevation. Inclusion of northing in the regression did not significantly improve any of the relationships except for NH4+, indicating a significant increase in concentrations from northwest to southeast.The spatial distribution of deposition fluxes showed similar gradients increasing from west and southwest to east and northeast. However, the pattern of deposition shows the influence of precipitation volume in determining the overall input. Mean depositions of sulphur and nitrogen in precipitation were ≈30 ktonnes S yr−1 and 48 ktonnes N yr−1 over the five-year period, 1994–1998, for Ireland.Least-squares linear regression analysis indicated a slight decreasing trend in precipitation concentrations for SO42− (20%), NO3 (13%) and H+ (24%) and a slight increasing trend for NH4+ (15%), over the period 1991–1998.  相似文献   

5.
The results of chemical analyses of monthly atmospheric precipitation samples from 12 stations within Czechoslovakia are presented. The sampling at the station with the longest record (Hrádek u Pacova, 80 km SE from Prague) covers 9 years. There is no clear regional pattern within the sampled territory, but a spring maximum was observed for most components. For SO4−2 and acidity a downward trend was indicated. Statistical analyses show that the important sources of mineralization of precipitation water are (in order of importance): coal combustion; sea spray; terrigenous dust; car exhaust; cement production; “European background” sulphur.  相似文献   

6.
Production, transport and deposition of sulphate and black carbon (BC) are simulated separating aerosol modes by production mechanisms, thus facilitating calculation of aerosol physical properties. The scheme uses explicit sulphur chemistry with prescribed oxidants and aerosol transformation based on Brownian coagulation rates, and is implemented in a 3-D, hemispheric-scale transport model with off-line meteorology from ECMWF. The components are DMS, SO2, sulphate and BC. Simulations are made for the year 1988. Predicted results for sulphate agree well with the measurements, except for considerable underestimations in the Arctic. In Europe SO2 is slightly overestimated and sulphate is slightly underestimated in cold seasons, whilst trends are less clear in North America. Compared to many other models, we estimate a smaller effective oxidation rate for SO2 due to reduced rates in cold clouds; a shorter turnover time for sulphate (3.7 d) due to a probably too large below-cloud scavenging ratio; and slightly smaller sulphate column burdens. Our BC results are similar to Liousse et al.’s (1996, J. Geophys. Res. 101, 19.411–19.432) except in USA, whilst the concentrations in remote areas and the turnover time (3.7 d) are considerably smaller than Cooke and Wilson’s (1996, J. Geophys. Res. 101, 190.395–19.409). Agreements with available measurements are quite close to large anthropogenic emissions (including USA), but they are considerably underestimated in Arctic winter. Transition from hydrophobic to hydrophilic BC due to coagulation is swift (6% h-1). Sensitivity tests emphasize that sub-cloud scavenging coefficients rely on careful assumptions about size distributions, and that more research is needed on sulphate production in ice-clouds. Emphasis should also be put on production of sulphate and hydrophilic BC boundary-layer clouds; inclusion of hydrophobic accumulation mode BC and sub-grid transition to hydrophilic BC in emitting grid squares.  相似文献   

7.
Precipitation samples over the Arabian Sea collected during Arabian Sea Monsoon Experiment (ARMEX) in 2002–2003 were examined for major water soluble components and acidity of aerosols during the period of winter and summer monsoon seasons. The pH of rain water was alkaline during summer monsoon and acidic during winter monsoon. Summer monsoon precipitation showed dominance of sea-salt components (∼90%) and significant amounts of non-sea salt (nss) Ca2+ and SO42−. Winter monsoon precipitation samples showed higher concentration of NO3 and NH4+ compared to that of summer monsoon, indicating more influence of anthropogenic sources. The rain water data is interpreted in terms of long-range transport and background pollution. In summer monsoon, air masses passing over the north African and Gulf continents which may be carrying nss components are advected towards the observational location. Also, prevailing strong southwesterly winds at surface level produced sea-salt aerosols which led to high sea-salt contribution in precipitation. While in winter monsoon, it was observed that, air masses coming from Asian region towards observational location carry more pollutants like NO3and nss SO42− that acidify the precipitation.  相似文献   

8.
Factor analysis comparisons between the MAP3S network and Minnesota precipitation chemistry data show marked differences. An assessment of ambient aerosol and precipitation chemistry data obtained at several Colorado and Minnesota sites suggests that natural source inputs may contribute to the sulfate observed in ambient aerosol and at least partly, explain the marked differences of Minnesota and Colorado precipitation chemistry data from that of MAP3S (eastern U.S.). However, a recently proposed mechanism, SO2 to SO4 conversion on the surface of dust particles, may be more important than natural sources in explaining western and midwestern precipitation chemistry data. It is concluded that these predominantly non-acidic SO4 sources may explain the poor association between the H+ and SO4 in many western and some midwestern precipitation chemistry data sets.  相似文献   

9.
To identify the characteristics of air pollutants and factors attributing to the formation of haze in Wuhan, this study analyzed the hourly observations of air pollutants (PM2.5, PM10, NO2, SO2, O3, and CO) from March 1, 2013, to February 28, 2014, and used hybrid receptor models for a case study. The results showed that the annual average concentrations for PM2.5, PM10, NO2, SO2, O3, and CO during the whole period were 89.6 μg m?3, 134.9 μg m?3, 54.9 μg m?3, 32.4 μg m?3, 62.3 μg m?3, and 1.1 mg m?3, respectively. The monthly variations revealed that the peak values of PM2.5, PM10, NO2, SO2, and CO occurred in December because of increased local emissions and severe weather conditions, while the lowest values occurred in July mainly due to larger precipitation. The maximum O3 concentrations occurred in warm seasons from May to August, which may be partly due to the high temperature and solar radiation. Diurnal analysis showed that hourly PM2.5, PM10, NO2, and CO concentrations had two ascending stages accompanying by the two traffic peaks. However, the O3 concentration variations were different with the highest concentration in the afternoon. A case study utilizing hybrid receptor models showed the significant impact of regional transport on the haze formation in Wuhan and revealed that the mainly potential polluted sources were located in the north and south of Wuhan, such as Baoding and Handan in Hebei province, and Changsha in Hunan province. Implications: Wuhan city requires a 5% reduction of the annual mean of PM2.5 concentration by the end of 2017. In order to accomplish this goal, Wuhan has adopted some measures to improve its air quality. This work has determined the main pollution sources that affect the formation of haze in Wuhan by transport. We showed that apart from the local emissions, north and south of Wuhan were the potential sources contributing to the high PM2.5 concentrations in Wuhan, such as Baoding and Handan in Hebei province, Zhumadian and Jiaozuo in Henan province, and Changsha and Zhuzhou in Hunan province.  相似文献   

10.
A statistical Lagrangian atmospheric transport model was used to generate annual maps of deposition of sulphur and oxidised and reduced nitrogen for the UK at a 5×5 km2 resolution. The model was run using emissions for the year 2002. The model was compared with measurements of gas concentrations (SO2, NOx, HNO3 and NH3) and of wet deposition and aerosol concentrations of SO42−, NO3 and NH4+ from national monitoring networks. Good correlation was obtained, demonstrating that the model is capable of accurately estimating the mass balance and spatial distribution of sulphur and nitrogen compounds in the atmosphere. A future emissions scenario for the year 2020 was used to test the influence of shipping emissions on sulphur deposition in the UK. The results show that, if shipping emissions are assumed to increase at a rate of 2.5% per year, their relative contribution to sulphur deposition is expected to increase from 9% to 28% between 2002 and 2020. The model was compared to both a European scale and a global scale chemical transport model and found to give broad agreement with the magnitude and location of sulphur deposition associated with shipping emissions. Enforcement of the MARPOL convention to reduce the sulphur content in marine fuel to 1% was estimated to result in a 6% reduction in total sulphur deposition to the UK for the year 2020. The percentage area of sensitive habitats with exceedance of critical loads for acidity in the UK was predicted to decrease by 1% with the implementation of the MARPOL convention.  相似文献   

11.
Meteorological analyses of acidic deposition data were undertaken to quantify the effect of Sudbury emissions on precipitation quality and air quality in Ontario during the period 1980–1983 with particular emphasis on the Sudbury smelter shutdown period (July 1982–March 1983). The techniques used included air parcel trajectories and detailed meteorological analysis.Results indicate that the contribution of the Sudbury smelters to sulphate wet deposition in central and southern Ontario was small—less than 12 % of the wet deposition at the study sites. The smelter contribution to sulphur dry deposition was greater—possibly as high as 47 % of the total at Kapuskasing, and up to about 20–30% of the total in central Ontario, with a smaller contribution (less than 5 %) to the southwest and west of Sudbury. These percentages apply to the smelter emission rate in the early 1980s, i.e. about 0.9 million metric tons of SO2 per year.  相似文献   

12.
Sulphate size distributions were measured at the coastal station of Mumbai (formerly Bombay) through 1998, during the Indian ocean experiment (INDOEX) first field phase (FFP), to fill current gaps in size-resolved aerosol chemical composition data. The paper examines meteorological, seasonal and source-contribution effects on sulphate aerosol and discusses potential effects of sulphate on regional climate. Sulphate size-distributions were largely trimodal with a condensation mode (mass median aerodynamic diameter or MMAD 0.6 μm), a droplet mode (MMAD 1.9–2.4 μm) and a coarse mode (MMAD 5 μm). Condensation mode sulphate mass-fractions were highest in winter, consistent with the high meteorological potential for gas-to-particle conversion along with low relative humidity (RH). The droplet mode concentrations and MMADs were larger in the pre-monsoon and winter than in monsoon, implying sulphate predominance in larger sized particles within this mode. In these seasons the high RH, and consequently greater aerosol water in the droplet mode, would favour aerosol-phase partitioning and reactions of SO2. Coarse mode sulphate concentrations were lowest in the monsoon, when continental contribution to sulphate was low and washout was efficient. In winter and pre-monsoon, coarse mode sulphate concentrations were somewhat higher, likely from SO2 gas-to-particle conversion. Low daytime sulphate concentrations with a large coarse fraction, along with largely onshore winds, indicated marine aerosol predominance. High nighttime sulphate concentrations and a coincident large fine fraction indicated contributions from anthropogenic/industrial sources or from gas-to-particle conversion. Monthly mean sulphate concentrations increased with increasing SO2 concentrations, RH and easterly wind direction, indicating the importance of gas-to-particle conversion and industrial sources located to the east. Atmospheric chemistry effects on sulphate size distributions in Mumbai, indicated by this data, must be further examined.  相似文献   

13.
Air and precipitation measurements at five sites were undertaken from 2001 to 2003 in four different provinces in China, as part of the acid rain monitoring program IMPACTS. The sites were located in Tie Shan Ping (TSP) in Chongqing, Cai Jia Tang (CJT) in Hunan, Lei Gong Shan (LGS) and Liu Chong Guan (LCG) in Guizhou and Li Xi He (LXH) in Guangdong. The site characteristics are quite varied with TSP and LCG located relatively near big cites while the three others are situated in more regionally representative areas. The distances to urban centres are reflected in the air pollution concentrations, with annual average concentrations of SO2 ranging from 0.5 to above 40 μg S m−3. The main components in the airborne particles are (NH4)2SO4 and CaSO4. Reduced nitrogen has a considerably higher concentration level than oxidised nitrogen, reflecting the high ammonia emissions from agriculture. The gas/particle ratio for the nitrogen compounds is about 1:1 at all the three intensive measurement sites, while for sulphur it varies from 2.5 to 0.5 depending on the distance to the emission sources. As in air, the predominant ions in precipitation are sulphate, calcium and ammonium. The volume weighted annual concentration of sulphate ranges from about 70 μeq l−1 at the most rural site (LGS) to about 200 μeq l−1 at TSP and LCG. The calcium concentration ranges from 25 to 250 μeq l−1, while the total nitrogen concentration is between 30 and 150 μeq l−1; ammonium is generally twice as high as nitrate. China's acid rain research has traditionally been focused on urban sites, but these measurements show a significant influence of long range transported air pollutants to rural areas in China. The concentration levels are significantly higher than seen in most other parts of the world.  相似文献   

14.
The Indo-Gangetic plain (IGP) has received extensive attention of the global scientific community due to higher levels of trace gases and aerosols over this region. Satellite retrievals and model simulations show that, in particular, the eastern part IGP is highly polluted. Despite this attention, in situ measurements of trace gases are very limited over this region. This paper presents measurements of SO2, CO, CH4, and C2–C5 NMHCs during March 2012–February 2013 over Kolkata, a megacity in the eastern IGP, with a focus on processes impacting their levels. The mean SO2 and C2H6 concentrations during winter and post-monsoon periods were eight and three times higher compared to pre-monsoon and monsoon. Early morning enhancements in SO2 and several NMHCs during winter connote boundary layer effects. Daytime elevations in SO2 during pre-monsoon and monsoon suggest impacts of photo-oxidation. Inter-species correlations and trajectory analysis evince transport of SO2 from regional combustion sources (e.g., coal burning in power plants, industries) along the east of the Indo-Gangetic plain impacting SO2 levels at the site. However, C2H2 to CO ratio over Kolkata, which are comparable to other urban regions in India, show impacts of local biofuel combustions. Further, high levels of C3H8 and C4H10 evince the dominance of LPG/petrochemicals over the study location. The suite of trace gases measured during this study helps to decipher between impacts of local emissions and influence of transport on their levels.  相似文献   

15.
The trends in and relationships between ambient air concentrations of sulfur dioxide and sulfate aerosols at 48 urban sites and 27 nonurban sites throughout the U.S. between 1963 and 1972 have been analyzed. The substantial decreases in ambient SO2 concentrations measured at urban sites in the eastern and midwestern U.S. are consistent with the corresponding reductions in local SO2 emissions, but these decreases have been accompanied by only modest decreases in ambient sulfate concentrations. Large differences in the amounts of SO2 emitted within individual air quality control regions are associated with much smaller differences in the corresponding ambient sulfate concentrations. Substantial changes in the patterns of SO2 emissions between air quality regions result in essentially no differences between ambient sulfate concentrations in those air quality regions. Comparisons of several air quality regions in the eastern and western U.S. with similar SO2 emission levels and patterns of emissions clearly demonstrates the higher ambient sulfate concentration levels in eastern air quality control regions. Relationships between SO2, sulfates, and vanadium concentrations at eastern nonurban U.S. sites cannot be explained by local emission sources. These various observed results can be best explained by long distance sulfur oxide transport with chemical conversion of SO2 to sulfates occurring over ranges of hundreds of kilometers. This conclusion has been suggested earlier and the present analysis strongly supports previous discussions. An impact of long range transport of sulfates is to emphasize the need for Consistent strategies for reduction of sulfur oxides throughout large geographical regions. Additions of large capacities involving elevated sources in mid-continental or western regions could result in significant increases in sulfate concentrations well downwind of such sources. Some of the types of research activities required to quantitate crucial experimental parameters are discussed.  相似文献   

16.
A model has been constructed of the dynamics and microphysics of a hill cap cloud. This has been used to investigate the aqueous phase oxidation of SO2 in the cloud droplets and the subsequent turbulent deposition of chemical species onto the hill surface. It is suggested that the dominant oxidant is H2O2 in these clouds and that therefore the process is likely to be oxidant limited. The amount of sulphate produced is comparable to that found in cloud condensation nuclei typically found over the U.K. and elsewhere away from strong local sources of sulphate aerosol. Ammonia concentrations are very important as they alter the cloud water pH and hence the solubility of SO2.Turbulent or ‘occult’ deposition is very sensitive to wind speed, the stability profile of the atmosphere and to the surface roughness. In a supercritical flow regime the occult deposition is a maximum just on the lee of the hill.  相似文献   

17.
Due to the dynamic nature of the atmosphere, substantial amounts of gaseous and particulate pollutants are transported to the areas distant from their sources. In order to determine the regional concentration levels of atmospheric pollutants in Lithuania, concentrations of gaseous O3, SO2, NO2 and other pollutants have been measured at the Preila background station (55°20′ N and 21°00′ E, 5 m a.s.l.) since 1981. The long-term concentration data set enabled us to get temporal trends, both on a seasonal and longer time scale, to identify source areas of pollutants and to relate them to the emission data. Based on the data obtained, the different tendencies in the pollutant concentration changes were revealed. Positive trends for ozone (of 2.9% per year during 1983–2000) and a distinct negative trend for both sulphur dioxide (of 3.8% per year during 1981–2000) and nitrogen dioxide (of 3.8% per year during 1983–2000) were found. The air mass back-trajectory analysis was used to assess the source region of air pollutants transported to Lithuania. The pollutant concentration levels were compared with their emission changes in Europe and Lithuania. The general trends in SO2 as well as in NO2 concentrations observed are consistent with changes in SO2 and NO2 emissions in Europe and Lithuania.  相似文献   

18.
ABSTRACT

Receptor-based chemical mass balance (CMB) analysis techniques are designed to apportion species that are conserved during pollutant transport using conserved source profiles. The techniques will fail if non-conservative species (or profiles) are not properly accounted for in the CMB model. The straightforward application of the CMB model developed for Project MOHAVE using regional profiles resulted in a significant under-prediction of total sulfate oxides (SOx, SO2 plus fine particulate sulfate) for many samples at Meadview, AZ. In addition, for these samples the concentration of the inert tracer emitted from the MOHAVE Power Project (MPP), ocPDCH, was also under-predicted. A second-generation model has been developed which assumes that separation of particles and SO2 can occur in the MPP plume during nighttime stable plume conditions. This second-generation CMB model accounts for all SOx present at the various receptor sites. In addition, the concentrations of ocPDCH and the presence of other inert tracers of emission from regional sources are accurately predicted. The major source of SOx at Meadview was the MPP, but the major source of sulfate at this site was the Las Vegas urban area. At Hopi Point in the Grand Canyon, the Baja California region (Imperial Valley and northwestern Mexico) was the major source of both SOx and sulfate.  相似文献   

19.
Although sulphur emissions (mainly as SO2) have been continuously decreasing over the last 20 years in most western industrialized countries, localized SO2 problems still exist in conjunction with strong local emission, meteorological, and topographical factors. In this study, the effect of supplementary installed flue gas desulphurization (FGD) units at high-capacity power plants on regional air pollution in the Carpathian Basin is investigated. The dispersion and accumulation of the SO2 air pollutant are studied with the regional three-dimensional on-line atmosphere-chemistry model REMOTE. The changes in the SO2 air pollution are investigated by parallel simulations in a case study, where the single modified parameter is the SO2 emission rate. The results show that FGD units significantly reduce the horizontal and the vertical dispersion of the emitted SO2, and its transboundary transport, too. Beside the SO2 removal efficiency, the dispersion and accumulation also depend on the seasonal weather conditions. During winter, the dispersion and accumulation are higher than in other seasons. Due to this phenomenon, higher SO2 removal efficiency is needed to guarantee similar air quality features like in the other seasons.  相似文献   

20.
A co-operative research project between the Malaysian Meteorological Service (MMS) and the Swedish Meteorological and Hydrological Institute (SMHI) focussing on the usage of an atmospheric transport and chemistry model, has just been initiated. Here, we describe the main features of the dispersion model and discuss a first set of calculations in light of available measurements of sulphuric species in Southeast Asia. According to our results, anthropogenic sulphur concentrations and depositions are particularly high near the large cities of the region, around a metal smelter in the southern Philippines, and in a region extending from northern Vietnam into southeastern China. These areas coincide with the high-emissions regions of Southeast Asia and we tentatively conclude that regional transport of acidifying species is not as far-reaching as in the mid-latitudes. From our calculations, and from supporting measurements we conclude that most of rural Southeast Asia is not yet severely affected by anthropogenic sulphur, but given the rapid rate of economical development in this region the situation may deteriorate quickly. Areas that are particularly at risk include the large cities, northern Vietnam, most of central Thailand, most of peninsular Malaysia, eastern Sumatra and parts of Java, all of which receive total-sulphur depositions in excess of 0.5 g S m−2 yr−1. Our model simulates sulphate in precipitation in accordance with measurements, but it has a tendency to overestimate atmospheric SO2. It remains to be investigated whether this is a problem in the model formulation or a result of unrepresentative sampling. An immediate continuation of this study should be performed with higher spatial resolution than the currently used 100×100 km2. Other imperfections in this model study, which should be addressed in future work, include parameterised vertical transport in deep convective clouds, the influence of natural emissions (primarily from volcanoes) on the concentration and deposition of sulphuric species, and the year-to-year variability of the driving meteorological conditions.  相似文献   

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