Long-Range Transport of Sulfur from Northeast Asia to Chengshantu, Shandong Peninsula: Measurement and Simulation

Observations of air pollutants were conducted at Chengshantu in January 1996 to clarify the extent of trans-boundary pollution from the Asian continent. A nested air quality prediction modeling system (NAQPMS), which included parameters on emission, transport, diffusion, deposition and transformation of sulfur oxides, was performed to compile sulfur concentrations over the observation site. The model calculation reproduced the observed variations of sulfur oxides and sulfate well, although the model calculations could not reproduce the extensively low sulfate concentrations. Using nesting improves the ability of the modeling system to capture peak episodes seen in the observations. Calculation of the origins of deposited sulfur in each country with the NAQPMS shows that the long-range transport of sulfur is very serious. For Japan, 49% of sulfur deposition was from other countries during the campaign period.     

Simulation of Dry Deposition Rates of Acidic Pollutants—An Assessment of Deposition Pathways in Hiroshima, Japan

A eulerian grid photochemical transport and dispersion model was used to simulate the dry deposition rates of nitrogen (as HNO₃) and sulfur (as SO₂) in Hiroshima, west Japan. Seasonal patterns of predicted dry deposition fluxes reveal that HNO₃ is most prevalent at more remote locations while SO₂ is deposited near to and slightly downwind from the major emission sources. The predicted dry deposition rates of HNO₃ and SO₂ were compared to the values measured at Mt. Gokurakuji (located in Hatsukaichi) and in Hiroshima City. The simulation results show that the model under-predicted (about 44% and 80%, respectively) both nitrogen and sulfur deposition rates at Mt. Gokurakuji and in Hiroshima City, indicating that the acid deposition in Hiroshima prefecture is possibly affected by long-range transboundary transport of acidic pollutants. Comparison of wet to dry deposition ratios (4.5 and 8.7 for nitrogen and 4.6 and 7.0 for sulfur) from the two observation sites above indicates that wet deposition maybe the most important acid deposition pathway in Hiroshima, Japan.     

Evaluating the Contribution of Long-Range Transport of Heavy Metals from the Asian Continent to Their Concentrations in Sediment Cores from Lake Shinji,Western Japan

The historical trend of heavy metal pollution recorded in sediment cores from Lake Shinji, western Japan, was investigated to evaluate the contribution of increasing long-range transport of heavy metals from the Asian continent in recent years. The concentrations of Cd, Co, Cr, Cu, Ni, Pb, Sb, and Zn and lead isotope ratios were determined for sediment cores collected at two sites in the lake. Among the metals, Cd, Sb, and Zn showed markedly high concentrations since the 1970s. Moreover, a high Pb concentration and less radiogenic lead isotope ratios have been observed since the 1980s in the core from a site close to the mouth of a major river. Air masses from the Asian continent, including China, Russia, and South Korea, have less radiogenic lead isotope ratios than those from Japan. This suggests that the recent increase in Pb concentration in the sediment core is primarily due to the long-range transport of heavy metals from the Asian continent, followed by their deposition in the catchment area of the river. The concentration ratios of Pb/Cd, Pb/Sb, and Pb/Zn of the sediment around 2000 were calculated on the basis of the metal concentrations in excess of those before 1940. They were then compared with the volume-weighted annual average concentration ratios of Pb/Cd, Pb/Sb, and Pb/Zn of rain samples collected on the shore of the lake for 1999–2001. The result showed that the ratios of the former to the latter are 1.0 for Cd, 0.69 for Sb, and 0.31 for Zn. Thus, it is likely that the long-range transport of Cd and Sb from the Asian continent also contributes significantly to the recent increase in the concentrations of these metals in the sediment core from Lake Shinji. For Zn, however, the contribution from the Asian continent was evaluated to be small, suggesting the importance of local sources such as effluent discharges.     

Black Acidic Rime Ice in the Remote Island of Yakushima, a World Natural Heritage Area

In order to clarify the long-range transport of atmospheric pollutants in the East Asian regions, we have studied the components in rime ice on Yakushima Island, located in southwestern Japan near the China continent. The presence of a large number of particles has been found in the rime ice. Very small particles whose diameters are around 1 µm were identified as coal fly ash. The air mass at an altitude between 1500 m to 2000 m was probably long-range transported in association with a stable atmospheric layer in which the particles were efficiently scavenged by supercooled droplets. A back trajectory analysis also indicated the predominance of a north wind in the winter and in the other seasons as well. Such transport and deposition mechanisms may produce the greater pollutant deposition sometimes observed in mountain areas. Similar events may not be rare and could make an important contribution to the annual pollutants.     

东亚季风与城市活动影响下南京市大气沉降多元特征研究

Atmospheric deposition, a major pathway of metals entering into soils, plays an important role in soil environment, especially in urban regions where a large amount of pollutants are emitted into atmosphere through various sources. In order to understand the characteristics of atmospheric deposition in urban area and its relation with natural and anthropogenic sources, a three-year study of atmospheric deposition at three typical sites, industrial zone (IN), urban residential area (RZ) and suburban forested scenic area (FA), was carried out in Nanjing, a metropolitan city in eastern China from 2005 to 2007. The bulk deposition rate and element composition of atmospheric deposition varied spatio-temporally in the urban zones of Nanjing. The concentrations of Cu, Zn, Pb and Ca in the atmospheric deposits were strongly enriched in the whole Nanjing region; however, anthropogenic pollutants in atmospheric deposits were diluted by the input of external mineral dust transported from northwestern China. Source apportionment through principal component analysis (PCA) showed that the background atmospheric deposition at the FA site was the combination of external aerosol and local emission sources. The input of long-range transported Asian dust had an important influence on the urban background deposition, especially in spring when the continental dust from the northwestern China prevailed. Marine aerosol source was observed in summer and autumn, the seasons dominated by summer monsoon in Nanjing. In contrast, the contribution of local anthropogenic emission source was constant regardless of seasons. At the RZ and IN sites, the atmospheric deposition was more significantly affected by the nearby human activities than at the FA site. In addition, different urban activities and both the winter and summer Asian monsoons had substantial impacts on the characteristics of dust deposition in urban Nanjing.     

基于氮排放数据的中国大陆大气氮素湿沉降量估算

大气氮素湿沉降与氮的排放紧密相关,通过对已知的氮素排放数据与收集的氮素湿沉降实测数据对应分析发现,不同地区氮素的排放与湿沉降之间存在稳定的比值关系。根据这些比值关系,估算了1980—2007年中国大陆氮素湿沉降量,并运用GIS技术进行了大气氮素湿沉降强度和时空分布。结果表明,我国大陆区域氮素湿沉降呈明显的增长趋势,沉降总量由1980年的4.96Tg增长到2007年的11.80 Tg,单位面积通量分别为516 kg N.km-2.a-1和1 128 kg N.km-2.a-1。氮素湿沉降的空间分布不均,东部、东南沿海地区和中部地区沉降量较高,广大西部地区较低。化学氮肥的施用、燃料的使用和禽畜养殖规模扩大是导致氮湿沉降量增加的主要原因。     

Transport of Atmospheric Pollutants from East Asia

Air-borne measurements of air pollutants transported from northeast Asia to Japan and the Pacific Ocean were carried out three times from 1996 to 1999 over the seas between Japan and Asian Continent. Those campaigns were named PEACAMPOT II under auspices of the IGAC/APARE program. A transport pattern of a highly polluted air mass from central China was found. Such air mass was driven by the quick movement of low pressure traveling from Taiwan area to the northeast of Japan. This finding supported well the results of modeling studies for long-range transport of atmospheric pollutants from East Asia.     

Development of hybrid LRT model to estimate sulfur deposition in Japan

We have developed a hybrid long-range transport (LRT) model to estimate long-term sulfur deposition amounts in Japan. This model combines a trajectory model for the LRT with an Eulerian model for the short-range transport and deposition. The hybrid model shows the ability to predict concentrations influenced by large nearby sources, which the trajectory model we previously developed consistently underestimated. The hybrid model is designed as an engineering model, which allows for long-term estimation without the requirements of detailed data on meteorology, surface condition, and emission over the whole domain, and huge computer resources required for comprehensive Eulerian models.     

Concentration and deposition of acidifying air pollutants over Sweden: Estimates for 1991 based on the match model and observations

The MATCH (Mesoscale Atmospheric Transport and CHemistry) model has been developed as a tool for air pollution assessment studies on different geographical scales. MATCH is an Eulerian atmospheric dispersion model, including physical and chemical processes governing sources, atmospheric transport and sinks of oxidized sulfur and oxidized and reduced nitrogen. Using a combination of air and precipitation chemistry measurements and the MATCH model, the national and long-range transport contributions to air pollution and deposition can be quantified in the model region. The calculations for the year 1991 show that the Swedish import was about 4.5 times larger than the export for sulfur and about six times larger for reduced nitrogen, while the Swedish import of oxidized nitrogen only exceeded the export by 10%. Using the MATCH system we estimate the long-range transport in an independent way compared to EMEP. Comparison between the EMEP and MATCH calculations for 1991 show that the total deposition of oxidized nitrogen over Sweden is similar, while the EMEP-values for total deposition of oxidized sulfur and reduced nitrogen are 25% respectively 40% smaller than what is obtained from MATCH.     

Estimation of S and NOx-N deposition budgets for the United States and Canada

Extensive wet deposition monitoring data, along with much sparser dry deposition monitoring data and isolated field characterizations of droplet deposition, are used to produce an annual deposition budget for S and NO_x-N for each contiguous U.S. state and Canadian province. The contribution to wet deposition from natural sources is estimated, and wet deposition is adjusted accordingly, to focus the analysis on deposition associated with anthropogenic emissions. The budgets, which are appropriate for 1985–1987, include adjustments for increased local wet and dry deposition near point sources and urban areas, which are generally avoided in selecting monitoring sites. When aggregated over the United States and Canada, estimated wet, dry, and droplet deposition account for about 30, 29, and 4% of anthropogenic S emissions, respectively, implying that 37% is exported. For NO_x-N, estimated wet, dry, and droplet deposition account for 30, 43, and 4% of anthropogenic emissions, with 23% exported. Results are in general agreement with a variety of other observational analyses and regional modeling simulations, particularly for eastern North America, and are consistent with estimates of net horizontal mass fluxes of S and NO_x-N across the Atlantic coast of North America.     

Modeling of first plume encounters with precipitation

A regional air pollutant transport model was used to simulate the fate of S emissions in the northeast United States. Hourly calculations were analyzed to describe trajectory characteristics and mass balances as pollutant trajectories first encounter precipitation during transport away from emission sources. Model results include air concentrations of SO₂ and sulfate, dry deposition values, and sulfate concentrations scavenged by precipitation, along with trajectory statistics. Results of sensitivity tests are compared to base case simulations which consider all precipitation events as a means of suggesting priorities for future regional transport model development.     

Deposition around a coal-fired power station during a wintertime precipitation event

The contribution to local wet deposition of emissions from a coal-fired power station at Inkoo on the south coast of Finland has been investigated during a wintertime precipitation event. Making use of intensive radiosonde and weather radar observations of meteorological factors, concentrations of sulphur in deposition due to plume washout were predicted by a short-range deposition model. The model used the scavenging coefficient to parametrize the wet removal of pollutants, and it took into account the wind drift of falling precipitation particles within the plume. The model predictions were then compared with the chemical analysis results from snowfall samples collected within 10 km of the power station during the experiment.The experiment was performed ahead of a deeply-occluded front during a period with strong advection of long-range transported pollutants. No reliable sign of the influence of the power station on the sulphate deposition could be identified. On the other hand, the deviations of acidity from the mean pH-value of 4.1 were concentrated in one sector near the expected area of deposited plume pollutants. If local emissions were responsible for these deviations, the explanation may lie in a slightly incorrectly estimated plume direction or the effects of alkaline fly ash. Nevertheless, definite conclusions cannot be drawn, because only a few collectors happened to be sited in the modelled sector of plume washout and none in its maximum area.     

Is It Possible to Use 90Sr and 137Cs As Tracers for the Aeolian Dust Transport?

A noble approach for the estimation of the deposition of the Asian dust over Japan by using atmospheric anthropogenic radioactivity, ⁹⁰Sr and ¹³⁷Cs, is proposed. Those radioactivities once deposited globally onto the ground by the past nuclear test, etc. are resuspended along with the surface soil particles in the air by the storm and deposited again on the ground. The difference in ¹³⁷Cs/⁹⁰Sr activity ratios in the surface soil between dry and wet climatic conditions gives a clue to know about the source of the dust. It was found that the average activity ratio in the deposited material (average: 2.1, n=82) at MRI, Tsukuba in the 1990s is not close to that of the surface soil taken in neighborhood (median: 6.8, n=8), which had been considered as the primary source. While, it is close to that of the soil samples taken in the arid area in the Asian continent (median: 2.0, n=4), which is the one of the source regions of the aeolian dust. Thus we can reasonably assume that deposited dust in Tsukuba is brought not only from the neighboring fields, etc. but also from the arid area in the continent. Using a simple two-component model it was estimated that the Asian dust may transport about 90% of ⁹⁰Sr and 70% of ¹³⁷Cs depositions observed in Tsukuba in the 1990s. Also, Asian dust may transport about 2/3 of the dust deposited in Tsukuba.     

Energy use,emissions, and air pollution reduction strategies in Asia

In contrast to Europe and North America, air pollution in Asia is increasing rapidly, resulting in both local air quality problems and higher acidic depositions. In 1989, an east-west group of scientists initiated a multi-institutional research project on Acid Rain and Emissions Reduction in Asia, funded for the past two years by the World Bank and the Asian Development Bank. Phase I, covering 23 countries of Asia, focussed on the development of PC-based software called the Regional Air Pollution INformation and Simulation Model (RAINS-ASIA). A 94-region Regional Energy Scenario Generator was developed to create alternative energy/emission scenarios through the year 2020. A long-range atmospheric transport model was developed to calculate dispersion and deposition of sulfur, based upon emissions from area and large point sources, on a one-degree grid of Asia. The resulting impacts of acidic deposition on a variety of vegetation types were analyzed using the critical loads approach to test different emissions management strategies, including both energy conservation measures and sulfur abatement technologies.     

Forecast of Sulfur Deposition in Japan for Various Energy Supply and Emission Control Scenarios

In order to contribute to the analysis and solution of regional scale environmental problems in East Asia, we developed a tool for the comprehensive assessment of alternative policy options to improve air quality. This tool projects the future regional energy supply, calculates the emission levels of sulfur dioxide and estimates the geographical pattern of sulfur deposition resulting from emissions. Sulfur deposition in Japan through 2030 was forecasted for various energy supply and emission control scenarios using the analysis tool. Future sulfur depositions were calculated from the source-receptor matrix for 1995 and the growth rate of emission for the source subregion. In the case of the current legislation scenario, anthropogenic SO₂ emissions in East Asia would grow by 34 percent and sulfur deposition in Japan would increase by approximately 20 percent between 1995 and 2030. This increase in sulfur deposition over these 35 years is sligthly less than the contribution from volcanic emission to sulfur deposition in Japan. In the case of the hypothetical dirty scenario for China, sulfur deposition in several grids which face the Sea of Japan would double by 2030.     

Estimation of wet and dry deposition of pollutant sulfur in eastern Canada as a function of major source regions

The contributions of major anthropogenic source regions to wet and dry deposition of total S in eastern Canada are estimated for a winter month and a summer month with the ASTRAP model. Results indicate that the U.S. and Canada contribute approximately equal amounts to total S deposition in Canada; Canadian sources contribute more than one half of dry deposition and less than one half of wet deposition.     

A computed sulphur budget for the eastern Canadian provinces

Sulphur budgets for Ontario, Quebec and the Atlantic Provinces have been computed using the Long-Range Transport of Air Pollutants model (LRTAP) which has been developed within the Atmospheric Environment Service of Canada. Meteorological data from 1978 and a North American SO₂ emissions inventory for 1970–1974 form the basic model input. The S budgets for the eastern Canadian regions were computed for large-scale emission scenarios. The budget shows the trans-boundary mass transport, S deposition and S concentrations within the regions for each scenario and shows the relative contribution to the deposition in each region. For eastern Canada, the model shows an annual S transboundary input of about 2 Tg S, an emission of about 1.8 Tg S, a deposition of about 2.4 Tg S and an output of about 1.4 Tg S. For southwestern Ontario, the model shows an annual average SO₂ concentration of 25 to 30 μg m^?3 (10 ppb), an annual sulphate concentration of about 8 μg m^?3, an annual wet deposition of S of about 15 kg S ha^?1 and an annual sulphate concentration in precipitation of about 5 to 6 mg l^?1.     

A Numerical Simulation of Acid Deposition in East Asia

The goal of the present study is to do a long term simulation and to derive a source receptor-relation using a comprehensive Eulerian acid deposition model coupled with a dynamic meteorological model. The selected modeling period is from March 1 to April 30, 1996. A dynamic meteorological model named MM5 was first used to calculate meteorological fields and then STEM preprocessors were invoked to generate dry deposition velocities and eddy diffusivities. Finally, a multi-scale STEM was applied to simulate both wet and dry acid deposition phenomena. The source-receptor relations were also estimated for sulfate and nitrate species using a counter species method. The model results for SO₂ and O₃ agree very well with measurements. However the model under-predicts the NO₂ concentration due to insufficient grid resolution as well as due to inaccurate field measurement. The transport contribution for total mass and wet deposition is much larger than that of dry deposition.     

Mercury from Combustion Sources: A Review of the Chemical Species Emitted and Their Transport in the Atmosphere

Different species of mercury have different physical/chemical properties and thus behave quite differently in air pollution control equipment and in the atmosphere. In general, emissions of mercury from coal combustion sources are approximately 20–50% elemental mercury (Hg°) and 50–80% divalent mercury (Hg(II)), which may be predominantly HgCl₂. Emissions of mercury from waste incinerators are approximately 10–20% Hg° and 75–85% Hg(II). The partitioning of mercury in flue gas between the elemental and divalent forms may be dependent on the concentration of particulate carbon, HCl and other pollutants in the stack emissions. The emission of mercury from combustion facilities depends on the species in the exhaust stream and the type of air pollution control equipment used at the source. Air pollution control equipment for mercury removal at combustion facilities includes activated carbon injection, sodium sulfide infection and wet lime/limestone flue gas desulfurization. While Hg(II) is water-soluble and may be removed from the atmosphere by wet and dry deposition close to combustion sources, the combination of a high vapor pressure and low water-solubility facilitate the long-range transport of Hg° in the atmosphere. Background mercury in the atmosphere is predominantly Hg°. Elemental mercury is eventually removed from the atmosphere by dry deposition onto surfaces and by wet deposition after oxidation to water-soluble, divalent mercury.     

Study of wet and dry atmospheric deposition at two altitudes in central Switzerland

The analysis of various ions in atmospheric deposition at two altitudes (515 m and 950 m a.s.l.) in Switzerland during 1983/84 revealed that dry deposition depends more on altitude than wet deposition. During autumn and winter, when vertical air exchange is limited, dry deposition of substances from anthropogenic sources (e.g. SO₄-S) was higher at the lower site. In the course of the year, the pattern of wet deposition was independent of altitude and showed highest rates for S, N and Ca in summertime. A comparison between rates of wet, particulate and gaseous S and N deposition suggested that during the growing season wet deposition is the dominant flux. Total (wet + dry) deposition of S, N and Cl was lower than in other parts of Europe, but a substantial increase of NO₃-N deposition during the past 25 years must have occured.