Estimating overall persistence and long-range transport potential of persistent organic pollutants: a comparison of seven multimedia mass balance models and atmospheric transport models

Two different approaches to modeling the environmental fate of organic chemicals have been developed in recent years. The first approach is applied in multimedia box models, calculating average concentrations in homogeneous boxes which represent the different environmental media, based on intermedia partitioning, transport, and degradation processes. In the second approach, used in atmospheric transport models, the spatially and temporally variable atmospheric dynamics form the basis for calculating the environmental distribution of chemicals, from which also exchange processes to other environmental media are modeled. The main goal of the present study was to investigate if the multimedia mass balance models CliMoChem, SimpleBox, EVn-BETR, G-CIEMS, OECD Tool and the atmospheric transport models MSCE-POP and ADEPT predict the same rankings of the overall persistence (P(ov)) and long-range transport potential (LRTP) of POPs, and to explain differences and similarities between the rankings by the mass distributions and inter-compartment mass flows. The study was performed for a group of 14 reference chemicals. For P(ov), the models yield consistent results, owing to the large influence of phase partitioning parameters and degradation rate constants, which are used similarly by all models. Concerning LRTP, there are larger differences between the models than for P(ov), due to different LRTP calculation methods and spatial model resolutions. Between atmospheric transport models and multimedia fate models, no large differences in mass distributions and inter-compartment flows can be recognized. Deviations in mass flows are mainly caused by the geometrical design of the models.     

Urban Air Quality Assessment Model: UAQAM

The Urban Air Quality Assessment Model (UAQAM) calculates urban concentrations caused by city emissions themselves, the so-called city background concentration. Three versions of the model for describing the dispersion were studied: Box, Gifford Hanna (GH) and a combined form of these two (Box–GH model). Regional background emissions contributing to the urban background concentration were accounted for by using measurements and calculations from a dispersion model on the continental scale. The results of the three UAQAM versions for a number of European cities were compared to measurements of SO₂ and NO _X . The Box–GH model shows better results when compared to the Box model and slightly better results in comparison to the GH model. The Box–GH model has been taken as a starting point for the assessment of urban air quality with UAQAM.     

Advanced mathematical programming modeling to assess the benefits from international CO2 abatement cooperation

The aim of this paper is to propose a method for coupling national energy models, to identify the dividends of international cooperation in atmospheric pollution abatement and efficient energy use. It indicates, also, how to solve the resulting large‐scale multinational model. It simulates finally a cooperation of four European countries for curbing their carbon dioxide (CO₂) emissions.     

Modeling the Effects of Air Quality Policy Changes on Water Quality in Urban Areas

This paper describes the development and application of an integrated modeling framework composed of an urban air chemistry model, an urban runoff model, and a water-quality model. The models were linked to simulate the fate and transport of air emissions of nitrogen compounds in the air, urban watershed, surface water runoff, and in a coastal receiving-water body. The model linkage is demonstrated by evaluating the potential water quality implications of reducing NO _x emissions by 32%, volatile organic compound emissions by 51%, and ammonia emissions by 30%, representing changes from 1987 levels to proposed 2000 target levels in Los Angeles, California, USA. Simulations of the Los Angeles dry season during the summer of 1987 (June 1 to August 31) indicated that by reducing emissions from 1987 to proposed year 2000 levels, the dry deposition nitrogen loads to Santa Monica Bay and the Ballona Creek watershed were reduced 21.4% and 15.0%, respectively. Water quality modeling results indicated that dry season atmospheric load reductions to the Ballona Creek Estuary did not reduce chlorophyll-a levels or significantly raise nighttime dissolved oxygen levels because the magnitude of the reductions was negligible compared to non-atmospheric inputs of nitrogen compounds. Simulations of the time period from November 18, 1987 to December 4, 1987 during the Los Angeles wet season indicated that air emissions reductions produced an 18.6% reduction in the dry deposition nitrogen load to Santa Monica Bay, a 15.5% reduction in the dry deposition nitrogen load to the Ballona Creek watershed, a 16.8% reduction in the wet deposition nitrogen load to the Ballona Creek watershed, and a 16.1% reduction in the stormwater discharge load from the Ballona Creek watershed. Although the wet season load reductions are significant, modeling results of the ultimate effect on the Ballona Creek Estuary water quality were inconclusive.     

Modelling the contribution of different sources of sulphur to atmospheric deposition in the United Kingdom

In order to understand relationships between sources and receptors of atmospheric deposition, computer models must be used. This paper describes a Lagrangian acid deposition model that represents emissions of trace species across Northern Europe. The chemistry of sulphur dioxide, dimethyl sulphide and hydrogen sulphide is represented and the model tested against estimates of UK wet and dry deposition. Mean UK wet and dry deposition for the period 1992–1994 was 206 and 145 ktonne S yr^-1, respectively. The model predicted wet and dry deposition of 222 and 166 ktonne S yr^-1, in good agreement with measurements. The model has been used to examine the sources of deposited S to the UK. For a base year of 1992, 86% of the UK's SO₂ emissions are exported. The S deposition attributable from mainland European sources was 36% of the UK total S deposition, in good agreement with other UK models but this differs substantially from the calculations of the EMEP model. Natural sources of S deposition from planktonic emissions of dimethyl sulphide, biological emissions of hydrogen sulphide and non-eruptive volcanic emissions of sulphur dioxide contributed approximately 1% of the modelled UK S deposition, of which 95% originated from dimethyl sulphide. The explicit chemical scheme for dimethyl sulphide incorporated into the model showed that 24% of the resultant deposited S was methane sulphonic acid. Boundary conditions of the model were tested and it was found that initialisation of sulphur dioxide and sulphate concentrations to representative ambient conditions had a very small effect. The modelled contribution of UK and European sources to UK S deposition was approximately 40 and 60%, respectively, showing the dramatic change arising from projected UK SO₂ emissions in 2010. This revised version was published online in July 2006 with corrections to the Cover Date.     

Modeling of NO x Emissions from Oil Refinery Furnaces

The current paper investigates the possibility of establishing an empirically based model for predicting the emission rate of nitrogen oxides (NO _x ) from oil refinery furnaces, in order to continually track emissions with respect to environmental licence limits. Model input data were collected by direct stack monitoring using an electrochemical cell NO _x analyser, as well as a range of telemetry sensors to obtain refinery process parameters. Principal Component Analysis (PCA), in conjunction with Partial Least Squares (PLS) regression was then used to build a series of models able to predict NO _x emissions from the furnaces. The models produced were proven to be robust, with a relatively high accuracy, and are able to predict NO _x levels over the range of operating conditions which were sampled. It was found that due to structural/operational variations a separate model is usually required for each furnace. The models can be integrated with the refinery operating system to predict NO _x emission rates on a continuous basis. Two models representing structurally different furnaces are considered in this paper. This revised version was published online in July 2006 with corrections to the Cover Date.     

常州市工业大气污染物排放特征研究

通过调查企业生产情况,采用现场实测、模型、排放因子等方法,获得了常州市工业大气污染物的排放量,从行业、排放口高度、空间、时间及重点源所占比例等方面,分析了常州市工业大气污染物的分布特征。结果显示:常州市工业PM、PM_(10)、PM_(2.5)、SO_2、NO_x、CO、NH_3、VOCs排放量分别为3.089、1.348、0.695、5.380、7.077、14.459、0.030、0.848万t;钢铁、水泥、热电、金属制品、化工是常州市大气污染物产生的主要行业;高架源、中架源、低架源排放比例依次增加;11.5%的企业占据了全市排放量的86%以上;SO2等污染物各月排放量基本稳定,PM2.5等上半年排放量波动较大;市区企业的集中排放在不利气象条件下易造成大气污染。     

Estimation of Emissions of γ-Hexachlorcyclohexane from the Great Lakes–St. Lawrence Ecosystem Using a Coupled Efficient Kalman Filter–Atmospheric Transport–Soil Model

An efficient linear Kalman filter has been combined with a coupled atmospheric transport and soil–air exchange model to determine organochlorine pesticides emissions on the regional scale. In this study, results of -HCH emissions from the Great Lakes–St. Lawrence ecosystem, estimated from the coupled model, are presented and discussed. A source receptor technique is used to identify a priori the locations of emission sources of -HCH, the emissions are then updated through a Kalman filtering procedure which minimizes the weighted difference between the predicted mixing ratios from the coupled model and the measured concentrations over the Great Lakes–St. Lawrence river region. Two experiments using the inverse algorithm are carried out. In the first experiment, the coupled atmospheric transport and soil–air exchange model is implemented to predict -HCH air and soil concentrations. Emissions are then updated every 12 days using the updated soil concentrations and emission factors. However, the updated emissions are not input into the coupled atmospheric transport and soil–air exchange model. On the other hand, in the second experiment the updated emissions are fed back to the coupled model, so that the model is reinitialized in each 12 days. The results from the inverse technique for the year 1995 have been compared with grided -HCH emission inventory in Canada, generated by emission factors. It is shown that the estimated emissions of -HCH are consistent with the measured emissions. It is found that the St. Lawrence valley has larger emissions of -HCH than the Great Lakes region, indicating an opposite distribution to the emission usage inventory, but in agreement with the measured -HCH concentration.     

成都双流国际机场大气污染物排放清单与时空分布特征

基于成都双流国际机场活动水平数据,采用排放因子法和计算模型等,编制了机场大气污染物排放清单,并完成了时空分配和不确定性分析,建立了高分辨率网格化排放清单。结果表明,成都双流国际机场标准起飞着陆(LTO)循环数为2.4×10~5次/a,CO、VOCs、NO_x、PM_(10)、PM_(2.5)、SO_2排放量分别为1.2×10~3、1.3×10~2、2.1×10~3、2.8×10、2.7×10、2.5×10~2t/a,且主要由飞机发动机排放;活动水平数据仅包括LTO循环数和地面保障设备两部分;污染物排放分布和跑道类型相关性较高;排放清单活动水平数据可靠性较高,而排放因子存在一定的不确定性。     

Measures of flow variability for great lakes tributaries

Design of monitoring programs for load estimation is often hampered by the lack of existing chemical data from which to determine patterns of flux variance, which determine the sampling program requirements when loads are to be calculated using flux-dependent models like the Beale Ratio Estimator. In contrast, detailed flow data are generally available for the important tributaries. For pollutants from non-point sources there is often a correlation between flow and pollutant flux. Thus, measures of flow variability might be calibrated to flux variability for well-known watersheds, after which flow variability could be used as a proxy for flux variability to estimate sampling needs for tributaries for which adequate chemical observations are lacking.Three types of measures of flow variability were explored: ratio measures, which are of the form q _x/q_y, where q _xis the flow corresponding to the percentile x, and y=100–x; spread measures, of the form (q _x–q_y)/q_m, where q _mis the median flow; and the coefficient of variation of the logs of flows. In the latter, flows are log transformed because flow distributions are often approximately log-normal. Three ratio measures were evaluated, based on the percentiles (10,90), (20,80), and (25,75). The analogous spread measures were also evaluated; the spread measure based on percentiles (25,75) is derived from the commonly used fourth spread of non-parametric statistics. The ratio measures and the spread measures are scale independent, and thus are measures only of the shape of the distribution. The coefficient of variation is also scale independent, but in log space.Values of these measures of flow variability for 120 Great Lakes tributaries are highly intercorrelated, although the relationship is often non-linear. The coefficient of variation of the log of the flows is also well correlated with the coefficient of variation of fluxes of suspended solids, total phosphorus, and chloride, for a smaller set of rivers where the existence of abundant chemical data allows comparison.Tributaries with abnormal distributions often show up as outliers when one measure of flow variability is plotted against another. Several examples are discussed.     

A necessary distinction between spatial representativeness of an air quality monitoring station and the delimitation of exceedance areas

The European legislation on ambient air quality introduces the concepts of spatial representativeness of a monitoring station and spatial extent of an exceedance zone. Spatial representativeness is an essential macro-scale siting criterion which should be evaluated before the setting-up and during the life of a monitoring point. As for the exceedance area, it has to be defined each time an environmental objective is exceeded in an assessment zone. No specific approach is prescribed to delimit such areas. A probabilistic methodology is presented, based on a preliminary kriging estimation of atmospheric concentrations at each point of the domain. It is applied to NO₂ pollution on the urban scale. In the proposed approach, a point belongs to the area of representativeness of a station if its concentration differs from the station measurement by less than a given threshold. To take the estimation uncertainty into account, the standard deviation of the kriging error is used in a probabilistic framework. The choice of the criteria used to deal with overlapping areas is first tested on NO₂ annual mean concentration maps of France, built by combining surface monitoring observations and outputs from the CHIMERE chemistry transport model. At the local scale, data from passive sampling surveys and high -resolution auxiliary variables are used to provide a more precise estimation of the background pollution in different French cities. The traffic-related pollution can also be accounted for in the map by additional predictors such as distance to the road, and traffic-related NO_x emissions. Similarly, the proposed approach is implemented to identify the points, at a given statistical risk, where the NO₂ concentration is above the annual limit value.     

Grey Box and Component Models to Forecast Ozone Episodes: A Comparison Study

For the purpose of short-term forecasting of high ozone concentration episodes stochastic models have been suggested and developed in the literature. The present paper compares the quality of forecasts produced by a grey box and a component time-series model. The summer ozone patterns for three European urban areas (two continental and one mediterranean) are processed. By means of forecast performance indices according to EC and WHO guidelines, the following features of the models could be found: The grey box model is highly adaptive and produces forecasts with low error variance that increases with the time horizon of forecast. The component model is more 'stiff' that results in a higher forecast-error variance and poorer adaption in detail. The forecast horizon, however, could be enlarged with this model. The accuracy of predicting threshold exceedance is similar for both models. This can be understood from the assumption of a cyclical time development of ozone that was made for both models.     

基于火点辐射能量的2017—2021年广西秸秆露天燃烧排放时空分析

基于2017—2021年MODIS、VIIRS和Himawari-8等多套卫星的火点辐射能量(FRE)和云量反演数据,使用更高分辨率的火点替代相邻位置低分辨率火点的融合方法,利用晴空的火点分布数据对被云遮蔽的区域进行补偿,核算得到了2 km高分辨率的广西秸秆露天燃烧排放数据,并针对2017—2021年的广西秸秆露天燃烧排放量展开精细的时空分布研究。结果表明:2017—2021年广西秸秆露天燃烧的CO、NO_x、SO₂、NH₃、VOCs、PM₁₀和PM_2.5的年排放量均值分别为12.91万、0.78万、0.16万、0.17万、2.77万、2.26万、2.21万t,排放高值区域分布在广西中部及西南部。秸秆露天燃烧排放的主要时间集中在冬、春季节(10月至次年3月),时值晚稻收割期和甘蔗榨季,占全年排放量的60%以上。广西秸秆露天燃烧PM_2.5年均排放量是全广西PM_2.5人为源年排放量的8.74%,通过逐日排放贡献分析发现,秸秆露天燃烧具有短期排放量较大的特点,2017—2021年,在1—2月有34 d出现秸秆露天燃烧导致PM_2.5排放量超过人为源排放量50%的情况。     

Atmospheric transport of persistent organic pollutants (POPs) to Bjørnøya (Bear island)

A first medium term monitoring of atmospheric transport and distribution for persistent organic pollutants (POPs) in Bj?rn?ya (Bear island) air samples has been performed in the period between week 51/1999 and week 28/2003. A total of 50 single compounds consisting of polychlorinated biphenyls (33 congeners), hexachlorobenzene (HCB), hexachlorocyclohexane isomers (alpha-, beta-, gamma-HCH), alpha-endosulfan, cyclodiene pesticides (chlordanes, nonachlor-isomers, oxy-chlordane, heptachlor and chlordane) as well as dichlorodiphenyltrichloroethane (DDT) derivatives were analysed and quantified. Atmospheric transport of POPs was identified as an important contamination source for the island. PCBs, HCB and HCH isomers were the predominant POP groups, contributing with 70-90% to the overall POP burden quantified in the Bj?rn?ya air samples. The highest concentration levels for a single compound were found for HCB (25-35 pg m(-3)). However, the sum of 33 PCB congeners was found to be in the same concentration range (annual means between 15 and 30 pg m(-3)). Cyclodiene pesticides, DDT derivatives and alpha-endosulfan were identified as minor contaminants. Several atmospheric long-range transport episodes were identified and characterised. Indications for industrial emissions as well as agricultural sources were found for the respective atmospheric transport episodes. A first simple statistical correlation assessment showed that for long-range transport of pollution, the local meteorological situation is not as important as the air mass properties integrated over the time period of the transport event. The local weather situation, on the other hand, is important when investigating deposition rates and up-take/accumulation properties in the local ecosystem. Based upon chemical data interpretation, valuable information about the influence of primary and secondary sources on the air mass contamination with chlorinated insecticides (e.g., HCHs) was found and discussed. The interdisciplinary interpretation of contaminant data using statistical methods, chemical analysis, meteorological modelling and classical meteorological information for a comprehensive evaluation of atmospheric long range transport into the European Arctic (Bj?rn?ya) has proven to be a highly versatile tool not only for atmospheric scientists but also with strong potential for regulatory purposes.     

Multi-scale Atmospheric Dispersion Modelling by Use of Adaptive Gridding Techniques

An accurate prediction of the transport-reaction behaviour of atmospheric chemical species is required to fully understand the impact on the environment of pollution emissions. Elevated levels of secondary pollutants such as ozone in the lower atmosphere can be harmful to the health of both plants and animals, and can cause damage to property present in the urban environment. Detailed models of pollution mechanisms must therefore be developed through comparisons with field measurements to aid the selection of effective abatement policies. Such models must satisfy accuracy requirements both in terms of the number of species represented, and the spatial resolution of species profiles. Computational expense often compels current models to sacrifice detail in one of these areas. This paper attempts to address the latter point by presenting an atmospheric transport-reaction modelling strategy based upon a finite volume discretisation of the atmospheric dispersion equation. The source terms within this equation are provided by an appropriate reduced chemical scheme modelling the major species in the boundary layer. Reaction and transport discretisations are solved efficiently via a splitting technique applied at the level of the non-linear equations. The solution grid is generated using time dependant adaptive techniques, which provide a finer grid around regions of high spatial error in order to adequately resolve species concentration profiles. The techniques discussed are applied in two dimensions employing emissions from both point and area sources. Preliminary results show that the application of adaptive gridding techniques to atmospheric dynamics modelling can provide more accurately resolved species concentration profiles, accompanied by a reduced CPU time invested in solution. Such a model will provide the basis for high resolution studies of the multiple scale interactions between spatially inhomogeneous source patterns in urban and regional environments.     

天津市北辰区大气污染物小尺度精细化源排放清单

以天津市北辰区空气站周边3 km为研究对象,基于拉网式实地调查,获得该地区2016年各类典型行业污染源详细的活动水平数据,以环境保护部发布的"清单编制技术指南"为参考,建立了2016年天津市北辰区空气站周边3 km大气污染源排放清单。结果表明:2016年天津市北辰区空气站周边3 km大气污染源的排放总量PM_(10)为431.28 t、PM_(2.5)为147.94 t、SO_2为48.67 t、CO为1 395.39 t、NO_x为469.52 t、VOCs为305.66 t;PM_(10)和PM_(2.5)的最大排放源是工地,贡献率分别为25.49%、15.16%;SO_2的最大排放源是散煤,贡献率为49.36%;CO和NO_x的最大排放源是道路机动车,贡献率分别为45.85%、53.89%;VOCs的最大排放源是制造业企业,贡献率为48.80%。天津市北辰区改善空气质量应从控煤、控尘、控车3个方面入手。     

大连市夏季近地面臭氧污染数值模拟和控制对策研究

通过区域空气质量模型CAMx对大连市2015年8月近地面臭氧(O_3)污染进行模拟,探讨了O_3及其生成前体物(NOx和VOCs)的来源,O_3生成控制区,并根据敏感性分析结果对前体物排放的控制效果进行了定量评估。结果表明:本地NOx排放对大连地区的NOx浓度贡献占90%以上,本地VOCs排放对大连地区的VOCs浓度贡献占80%以上,而本地NOx和VOCs排放对大连地区O_3浓度贡献仅占29%;大连市整体上为VOCs控制区,控制VOCs能有效降低O_3污染,还能有效削减O_3的峰值浓度;通过敏感性分析结果计算得出,削减大连本地工业源VOCs和民用源VOCs能够有效降低大连地区O_3浓度,削减10%的工业源VOCs能使市区O_3平均浓度降低2%左右,削减10%的民用源VOCs能使大连市区平均O_3浓度降低1%左右。建议NOx与VOCs削减比例为1∶2,对大连市O_3和PM2.5污染进行协同控制。     

Simulation of Urban-Scale Air Pollution Patterns in Luxembourg: Contributing Sources and Emission Scenarios

The aim of this study is to investigate the air pollution situation in an urban area in southwestern Luxembourg and to simulate annual NO₂ and PM₁₀ concentrations in response to changes in meteorological conditions and emissions using a Gaussian dispersion model. Simulations are carried out for the years 1998–2006. Emission scenarios related to road transport and nonindustrial combustion are performed in order to predict changes of air pollution levels. Road transport is by far the most important local emission source in the study area. Scenarios with more stringent emission standards for vehicles, less traffic, and fewer heavy-duty vehicles lead to reductions of NO_x and primary PM₁₀ emissions. As a result, the annual NO₂ concentrations are decreasing in most parts of the study area and are below the European annual limit value of 40 μg?m^?3. In contrast, a scenario with increased use of wood pellets for domestic heating shows an increase in urban PM₁₀ concentration. The year-to-year variability of meteorological conditions accounts for the same magnitude of absolute NO₂ and PM₁₀ concentration changes as the emission scenarios. The comparison with measurements located in the study area shows that the model is able to predict urban-scale annual average air pollution. The proposed application results show that the model can be appropriate for policy-driven air quality management and planning queries.     

Estimation of shipping emissions in Candarli Gulf, Turkey

Ships are significant air pollution sources as their high powered main engines often use heavy fuels. The major atmospheric components emitted are nitrogen oxides, particulate matter (PM), sulfur oxide gases, carbon oxides, and toxic air pollutants. Shipping emissions cause severe impacts on health and environment. These effects of emissions are emerged especially in territorial waters, inland seas, canals, straits, bays, and port regions. Candarli Gulf is one of the major industrial regions on the Aegean side of Turkey. The marine environment of the region is affected by emissions from ships calling to ten different ports. In this study, NO _x , SO₂, CO₂, hydrocarbons (HC), and PM emissions from 7,520 ships are estimated during the year of 2007. These emissions are classified regarding operation modes and types of ships. Annual shipping emissions are estimated as 631.2 t year^???1 for NO _x , 573.6 t year^???1 for SO₂, 33,848.9 t year^???1 for CO₂, 32.3 t year^???1 for HC, and 57.4 t year^???1 for PM.     

Emission database for global atmospheric research (Edgar)

Atmospheric chemistry and climate modellers require gridded global emissions data as input into their models. To meet this urgent need a global emissions source database called EDGAR is being developed by TNO and RIVM to estimate for 1990, on a regional and on a grid basis, annual emissions of greenhouse gases (CO₂, CH₄, N₂O, CO, NO_x, non-methane VOC, SO_x), of NH₃, and of ozone depleting compounds (halocarbons) from all known sources. The aim is to establish at due levels of spatial, temporal and source aggregation the emissions from both anthropogenic and biogenic sources: a complete set of data required to estimate the total source strength of the various gases with a 1×1 ° resolution (altitude resolution of 1 km) and a temporal resolution of a month, supplemented by diurnal variation, as agreed upon in the Global Emissions Inventory Activity (GEIA) of the International Atmospheric Chemistry Programme (IGAC). In this way EDGAR will meet the requirements of present and future developments in the field of atmospheric modelling. The data comprise demographic data, social and economic factors, land use distributions and emission factors (with due emphasis on the uncertainty). As understanding in this field is still changing, due attention is paid to flexibility regarding the disaggregation of sources, spatial and temporal resolution and species. The objective and methodology chosen for the construction of the database and the structural design of the database system are presented, as well as the type and sources of data and the approach used for data collection. As an example, the construction of the N₂O inventory is discussed.