Organization of long range transport of air pollution monitoring in Europe

In the 1950s a network of stations for observation of the chemical composition of air and precipitation was established in Europe. Analyzing these data, Oden (1968) was able to show that a central area in Europe with highly acid precipitation was expanding from year to year. This was further substantiated by Granat (1972), and the explanation is the increasing use of fossil fuels in Europe. In 1969, the problem was examined by OECD, and on the initiative of the Scandinavian countries, a joint research program to study the long range transport of air pollutants was started in 1972. The program will be completed with a final report in 1976. In this program, atmospheric dispersion models are used to describe emission, dispersion and deposition of SO₂ and sulphate with particular emphasis on the acidification of the precipitation. An emission field has been constructed for Europe, and data from the European weather forecasting system are used for the dispersion calculations. Calculated concentrations and deposition are compared with data from about 70 ground stations and measurements from aircraft. Results show that the main cause for acidification of precipitation is the increasing use of fossil fuels. Large amounts of H₂SO₄ can be transported over distances up to a few thousand kilometers. In southern Scandinavia where the soil is highly acid (podsol), this has caused severe damage to life in rivers and lakes, and it is feared that in the future, there will be serious damage to forestry. In the Alps, where the soil has a high carbonate content, such effects are not expected. The long range transport of air pollutants has also been shown to increase the corrosion of materials. Work is now in progress to establish a more permanent system for the monitoring of air pollutants in Europe. The first plans for such a system were presented at the meeting in Oslo in December 1974, where countries from both Eastern and Western Europe participated. The work is supported by the Economic Commission for Europe, UN, in cooperation with other international organizations such as the World Meteorological Organization and the GEMS program of the United Nations Environment Programme. In this connection, studies have also been taken up in several countries concerning the effects of the long range transport of air pollutants. In the future monitoring system, a coordination of these efforts is envisaged.     

森林植被截留对大气污染物湿沉降的影响

试验研究了裸地、马尾松林、香樟林的大气降水、穿透雨和树干径流以及地表径流的污染物离子浓度。结果表明:大气降水的污染物质离子浓度大小依次为SO42->NO3->Cl->F-;马尾松、香樟林群落的穿透雨、树干径流的污染物质含量显著高于大气降水,说明它们对降水中污染离子的富集作用很强,马尾松林的穿透雨和树干径流的污染物离子的总量高于香樟林。各林型大气污染物降水的SO42-离子含量都较高,两种林型的地表径流污染物质含量显著高于大气降水,但污染物浓度比树干径流有显著降低,说明土壤表面和枯枝落叶对降水中污染物的吸附能力很强。     

Acidic Precipitation and Large-Scale Transport of Air Pollutants Observed in Korea

Acid rain at a rural site in Chongwon (KHN), central Korea has been under observation since 1990. To substantiate the 10-year observations, rain samples from six other sites were also collected and analyzed. Results show that acid rain occurred frequently at all sites. At KHN, seasonal and annual variability of pH values had a 10-year VWM value of 4.67 and an arithmetic mean value of 5.09. In general, a high value of pH occurred during springtime when the occurrence of yellow sand (dust) was prevalent in East Asia; during summer, heavy rain usually contained neutral pH values. During other seasons, the degree of acidic precipitation usually coincided with certain air flows. Most frequently, air flows and cyclones coming from south and central China often resulted in precipitation with low pH values observed in Korea. Using daily satellite observations from 1996, we have also been monitoring the long-range and large-scale transport of air pollutants (LSTAP) over East Asia. Many samples of LSTAP were obtained when they were crossing the Yellow Sea and moving over the Korean Peninsula and to SW Japan. The width of the Yellow Sea is ca. 350～700 km and air pollutants take 1～2 days to cross it. Cases of acid rain in Korea clearly correlate wth the LSTAP from source regions in China.     

The Effect of Changes in European Anthropogenic Emissions on the Concentrations of Sulphur and Nitrogen Components in Air and Precipitation in Lithuania

Sulphur (S) and nitrogen (N) components are of great concern because acidification and eutrophication still remain an important environmental issue in many regions of the world. Continuous monitoring (1981–1999) of S and N components both in air and precipitation in Lithuania (LT) has allowed us to evaluate the regional and temporal variations in relation to the pollutant emission changes. Despite of inter-site variability in concentration of pollutants within the regional scale, data showed a marked decrease in S concentrations both in air and precipitation over the Lithuania as a whole. Non-seasalt sulphate (nssSO₄ ^2?) concentrations in precipitation and air decreased from 2.06 to 0.52 mgS/l and from 3.97 to 1.07 µgS/m³, respectively. The number of acidic (pH<5) precipitation did not exceed 50 % during 1995–1999. The observed trends for S species are consistent with those for sulphur dioxide (SO₂) emission in Europe and Lithuania. Although nitrogen dioxide (NO₂) concentration in air decreased by 17 %, significant changes in nitrate (NO₃ ^?) concentrations neither in precipitation nor in air have been observed. Three-day backward air isobaric trajectories were used for the identification of the source region of air pollutants     

Impact of acid precipitation on freshwater ecosystems in Norway

Extensive studies of precipitation chemistry during the last 20 yr have clearly shown that highly polluted precipitation falls over large areas of Scandinavia, and that this pollution is increasing in severity and geographical extent. Precipitation in southern Norway, Sweden, and Finland contains large amounts of H⁺, SO⁼ ₄, and NO^? ₃ ions, along with heavy metals such as Cu, Zn, Cd, and Pb, that originate as air pollutants in the highly industrialized areas of Great Britain and central Europe and are transported over long distances to Scandinavia, where they are deposited in precipitation and dry-fallout. In Norway the acidification of fresh waters and accompanying decline and disappearance of fish populations were first reported in the 1920s, and since then in Sørlandet (southernmost Norway) the salmon have been eliminated from several rivers and hundreds of lakes have lost their fisheries. Justifiably, acid precipitation has become Norway's number-one environmental problem, and in 1972 the government launched a major research project entitled ‘Acid precipitation — effects on forest and fish’, (the SNSF-project). Studies of freshwater ecosystems conducted by the SNSF-project include intensive research at 10 gauged watersheds and lake basins in critical acid-areas of southern Norway, extensive surveys of the geographical extent and severity of the problem over all of Norway, and field and laboratory experiments on the effect of acid waters on the growth and physiology of a variety of organisms. Large areas of western, southern, and eastern Norway have been adversely affected by acid precipitation. The pH of many lakes is below 5.0, and sulfate, rather than bicarbonate, is the major anion. Lakes in these areas are particularly vulnerable to acid precipitation because their watersheds are underlain by highly resistant bedrock with low Ca and Mg contents. Apart from the well-documented decline in fish populations, relatively little is known about the effects of acid precipitation on the biology of these aquatic ecosystems. Biological surveys indicate that low pH-values inhibit the decomposition of allochthonous organic matter, decrease the species number of phyto-and zooplankton and benthic invertebrates, and promote the growth of benthic mosses. Acid precipitation is affecting larger and larger areas of Norway. The source of the pollutants is industrial Europe, and the prognosis is a continued increase in fossil-fuel consumption. The short-term effects of the increasing acidity of freshwater ecosystems involve interference at every trophic level. The long-term impact may be quite drastic indeed.     

The chemical composition of rainfall in a city of Northern Spain

A study was carried out over a period of 4 yr on precipitation in Santander, a coastal city with heavy rainfall in the north of Spain. An increase in acidity was found for the latter period studied, from April 1984 to April 1985, possibly due to a change in the meteorology of the area in this period. The correlations between the ions themselves, and with pollution from SO₂ and suspended particulate matter, as well as possible correlations with meteorological variables were analyzed using a multiple linear regression method. The influence of mid- and long-range transport of pollutants was also analyzed and found to be important when air masses come from highly industrialized zones both in Central Europe and in neighboring Spanish regions, although the contribution of the latter to total acid deposition is less owing to low frequency and the usually low volume of precipitation.     

Impacts of Air Pollutants on Vegetation in Developing Countries

The predicted increases in emissions of primary pollutants in many rapidly industrializing countries may have severe consequences for the health and productivity of forest trees and agricultural crops. This paper presents a review of air pollution impacts on vegetation in developing countries by summarising information describing the direct impacts to vegetation caused by a number of air pollutants (sulphur dioxide (SO₂), nitrogen oxides (NOx), ozone (O₃) and Suspended Particulate Matter (SPM)). This information has been collected by experts from a number of rapidly industrializing countries in Asia, Latin America and Africa and includes observations of visible injury in the field and the use of transect studies and controlled experimental investigations to ascribe damage to different pollutant concentrations. The ability to synthesise this information to define exposure-response relationships and subsequent air quality guidelines similar to those established in North America and Europe is assessed. In addition, the use of regional and global models describing pollution concentrations is discussed with reference to assessing the extent of adverse impacts and identifying regions likely to be most at risk from air pollution, both for the present day and in the future. The evidence summarised in the paper clearly shows that current pollutant concentrations experienced in many developing countries, particularly Asia, can result in severe damage to vegetation and that without appropriate control measures such damage is likely to worsen in the future as pollutant emissions increase.     

Modelling Some Heavy Metals Air Concentration in Europe

Metals, as well as other air toxic pollutants, can be responsible for a range of human health effects via inhalation or ingestion. European normatives regulate lead, arsenic, cadmium, mercury and nickel ambient air levels in order to prevent potential damage to human health and ecosystems; annual target levels of 500, 6, 5 and 20?ng/m³ for Pb, As, Cd and Ni are set for these pollutants in directives 2008/50/CE and 2004/107/CE. Air quality models constitute a powerful tool to understand tropospheric dynamic and to assign concentration values to areas where no measurement is available. However, not many models include heavy metals in their code, and mainly results for Pb, Cd and Hg have been published. In this paper, we present preliminary results on modelling Pb, Cd, As, Ni, Cu, Zn, Cr and Se air background concentration in Europe using the CHIMERE model, at a 0.2° resolution and the evaluation of the model performance in order to see its capability to reproduce observed levels. This evaluation was performed by comparing simulated values with observations at the EMEP monitoring sites, as only values at background sites can be captured at the 0.2° model resolution. Important uncertainties mainly related to emissions should be solved in order to obtain an improvement of model performance; more recent annual totals, information on snap activities for each metal, higher spatial resolution and a better knowledge of the temporal emission behaviour is necessary to adequately model these air pollutants. Also a better treatment of these particles considering more realistic metal size distribution, more refined deposition processes or some chemical processes regarding Se could result in better model results. A larger number of stations and a better temporal coverage of observations are also important to carry out a better statistical analysis of model performance.     

An Integrated Assessment Model for Fine Particulate Matter in Europe

Exposure to fine particles in the ambient air is recognized as a significant threat to human health. Two pathways contribute to the particle burden in the atmosphere: Fine particles originate from primary emissions, and secondary organic and inorganic particles are formed from the gas phase from the emissions of 'conventional' pollutants such as SO₂, NO_x, VOC and NH₃. Both types of particulate matter can be transported over long distances in the atmosphere. An integrated assessment model for particulate matter developed at IIASA addresses the relative importance of the different types of particulates, distinguishing primary and secondary particles and two size fractions. The model projects these emissions into the future and seeks cost-effective strategies for reducing health risks to population. The model integrates the control of primary emissions of fine particles with strategies to reduce the precursor emissions for the secondary aerosols. Preliminary results addressing the PM_2.5 fraction of both primary and secondary particulate matter indicate that in Europe the exposure to particulates will be significantly reduced as a side effect of the emission controls for conventional air pollutants (SO₂, NO_x, NH₃).     

Acidic deposition in California: Findings from a program of monitoring and effects research

California's 14-year, $25 million acidic deposition program has studied the causes and effects of acidic air pollutants. In contrast to the eastern United States where sulfur-derived (S-derived) by-products from coal combustion dominate precipitation chemistry, nitrogen-derived (N-derived) acids predominate in wet and dry deposition in California. Adverse effects on the human lung have not been observed after short-term exposures to acidity, but extended exposures to ambient acidity may pose a chronic risk. No irreversible, adverse effects on surface waters in the Sierra Nevada mountain range or to the state's forests have been found due to extant acidic inputs. The longer-term outlook for forests is less certain because the impacts observed elsewhere occurred after decades of S and N deposition, but at lower ambient ozone levels. Ozone is the major air pollutant stressor for forests, but atmospheric N has the potential to cause adverse changes in soil nutrient cycling. Impacts on man-made materials in southern California (e.g., galvanized steel) were found to be minor. While California does not have an ambient air quality standard for acidic air pollutants, emissions of precursors have declined since the 1960's due to changes in industrial practices, improvements in technology, and adoption of control measures for ozone. Lowering emissions from motor vehicles will be emphasized to prevent future increases in N deposition.     

Development of Automatic Continuous Measurement System of Chemical Constituents in the Precipitation

Nowadays, acid rain is generally noticed as a global environmental problem. While acid rain has very much to do with the air pollutants, the relation between air pollution and chemical constituents in precipitation is not understood clearly yet. It is important to measure a variation of ion concentration in precipitation in short term for understanding the formation mechanism of acid rain. Therefore, an automatic continuous measurement system of chemical constituents in precipitation was developed and put into practical use in this study. The developed system was able to collect automatically every 1mm of precipitation and analyze major ions within 20 minutes.     

Twenty-Year Road Traffic Emissions Trend in Greece

Air pollutants emissions from traffic are very closely connected to urban air quality, in a local scale, as well as to global problems like climate change, in a large scale. Road transport air pollutants emissions represent, in most cases, a critical parameter for a comprehensive and successful understanding of the mechanisms governing the air pollutants concentrations. Hence, reliable estimations and comprehension of road transport emissions are indispensable in order to set reliable strategies in the direction of air pollution abatement and management of air pollutants and greenhouse gases emissions. In this framework, in the present work, the emissions of air pollutants from road transport in Greece will be presented for the whole period 1990–2009 as it was found that a detailed, accurate and reliable emissions inventory was missing. The whole period emissions variation has clarified the impact of the change in the vehicle fleet, the engine technologies and the fuel quality. The calculated results have revealed that the age of the vehicles and the corresponding engine technology are the critical parameters determining the amount of the pollutants emitted. This was mainly observed in both passenger cars and heavy duty vehicles demonstrating the importance of a renewal programme of the old circulating vehicles in order to set an effective air pollution abatement strategy. Passenger cars were found to be responsible for the major part of most air pollutants emissions except from nitrogen oxides and particulates emissions. Heavy duty vehicles contribute more than 66% to nitrogen oxides and particulates emissions. For the whole time period, all calculated pollutants present a decreasing trend, with the exception of carbon dioxide and nitrous oxide which increase constantly, ranging from −96% for sulphur dioxide to −1% for PM10.     

Trace metals in precipitation in Sweden

Trace metals (Cd, Cu, Fe, Mn, Pb, and Zn) concentrations in atmospheric precipitation have been routinely monitored in Sweden since the autumn of 1983. Concentrations are highest in southern Sweden and decrease northward. It is postulated that the long range transport of anthropogenic pollutants from the rest of Europe is the major source of Cd, Pb, and Zn in precipitation. Evidence for this hypothesis is that enrichment factors indicate anthropogenic origin, and Swedish atmospheric emissions of Zn and Cd are 2 to 3 times smaller than deposition fluxes. Also, Cd, Pb, and Zn concentrations are correlated in both space and time and are also well correlated with exSO₄ ⁺, a substance known to be of anthropogenic origin transported long distances.     

Bridging the gap between air quality and precipitation chemistry

Data sets recently have become available providing simultaneous, regional scale observations of ambient air quality and precipitation chemistry. The data cover parts of the greater northeastern United States. With certain key assumptions, the observations of ambient SO_x and NO_x concentrations can be linked with precipitation concentrations through Junge's concept of rainout efficiency, assumed to be qualitatively equivalent to the washout ratio. A preliminary comparison between data taken from the Sulfate Regional Experiment (SURE) and the parallel precipitation studies using Junge's approach reveals certain useful consequences. Apparent dramatic differences in SO_x and NO_x scavenging are found. Ratios between sulfate in the aerosol and in precipitation compared with trace elements suggest the importance of particulate scavenging processes. Such results show promise for simplified analysis of these data as approaches to differentiating mechanisms involved in cloud-precipitation chemistry.     

Estimation and Prediction in the Spatial Linear Model

Often in environmental monitoring studies interesting ecological factors will be observed at several locations repeatedly over time. Generally these space-time data are subject to a sequential spatial data analysis. In geostatistics, spatial data describing an environmental phenomenon like the pH value in precipitation at several locations are regarded as a realisation from a stochastic process. Component models are used to interpret the spatial variation of the process. Decomposing the spatial process into single components is based on the theory of linear models. Trend surface analysis is seen to be the geostatistical method for best linear unbiased estimation (BLUE) of the trend component, whereas universal kriging is equivalent to best linear unbiased prediction (BLUP) of the realisation of the spatial process. Furthermore trend surface analysis and universal kriging are shown to agree with the estimation of fixed effects and prediction of fixed and random effects in mixed linear models. Since estimation and prediction for spatial data result in different interpolations the differences are explained also graphically by example. The example uses acid-precipitation monitoring data. The extension of these spatial methods for application to space-time problems by combination with dynamic linear models is treated in the discussion.     

Trace inorganic species in precipitation and their potential use in source apportionment studies

Trace species in atmospheric particles have frequently been used to apportion pollutants in acid rain to their sources by comparing the relative concentrations of trace species at the source and receptor sites. Another approach is to use the trace species in precipitation directly in a source apportionment. This has rarely been done due to the paucity of data on trace species in precipitation and the unknown fractionation of the species during the scavenging process. A study was undertaken to analyze precipitation for a large number of trace species and to compare the concentrations with those in atmospheric particles. Precipitation was collected in Lenox, MA during the summer of 1984. Extreme measures were taken to avoid contamination during collection and analysis. Using five analytical methods, including the novel method of freeze-drying the precipitation followed by neutron-activation analysis, 31 species were analyzed in the rain. The trace concentrations measured in this study were lower than those found in earlier studies, where contamination was believed to be a problem. Concentrations of trace species in the precipitation were compared with those in atmospheric particles. A few species were enriched in precipitation relative to particles, including some large-particle species (Ca, Ti, Fe) and species with gaseous precursors (SO₄, NO₃, Br). Due to this enrichment, these species should be carefully considered before using them in source apportionment calculations. However, most species showed similar enrichments in precipitation and in atmospheric particles, suggesting that negligible fractionation had taken place during the scavenging process. These species could be used effectively in the future to apportion the pollutants in precipitation to their various sources.     

Metals in small Norwegian lakes: Relation to atmospheric deposition of pollutants

Water chemistry data from 165 lakes in Norway are discussed in relation to contribution from long-range transported air pollutants. Concentrations of lead and antimony in terrestrial mosses are used to express the relative contribution from long range transport to each lake. The contents of Al and Zn in lake water and of ‘excess’ SO₄ in low Ca lakes show high correlations with the relative heavy metal deposition values from moss analysis. The ‘excess’ SO₄ in low Ca lakes correlates strongly with Al and too a lesser extent with Mn and Fe. It is suggested that the lake water levels of Al and Mn, and even to some extent Fe, are significantly affected by acidic precipitation enhancing the leaching of these metals from mineral matter in soils and sediments. In the case of Zn, airborne supply to the lakes and their catchments appears to strongly affect the water content.     

Statistical models for the accumulation of PAH,chlorinated hydrocarbons and trace metals in epiphytic Hypnum cupressiforme

Concentrations of PAH (1.12-benzoperylene, 3.4-benzopyrene, fluoranthene), chlorinated hydrocarbons (α-BHC, lindane, PCB) and trace metals (Zn, Pb, Cu) in bulk precipitation, as well as PAH and trace metal concentrations in atmospheric dust samples from 14 sites in Bavaria, F.R.G. are presented for two vegetation periods (1979 and 1980). The same substances were also analyzed in epiphytic moss (Hypnum cupressiforme var. filiforme) sampled from tree trunks in October 1979 and 1980. Using mean immission values and the amount of precipitation as predictors and concentrations of pollutants in moss samples as criteria, a number of multiple regression models were computed in order to quantify the relationships between absolute air pollution data and accumulated trace substance values. Beta values of all variables help to determine whether bulk precipitation or atmospheric particulate matter has dominant influence on the uptake of trace substances by mosses. The study shows that epiphytic mosses can be used to monitor both heavy-metal, PAH and chlorinated hydrocarbons.     

Effects of varying air trajectories on spatial and temporal precipitation chemistry patterns

This study was designed to determine if judicious use of synoptic data and an operational trajectory model could identify probable source regions of anthropogenic pollutants in northeastern United States precipitation and thus relate receptor measurements to emissions data without consideration of the complex intervening meteorological and chemical processes. The storm event of April 8 to 10, 1979, was selected for intensive study. Precipitation chemistry data were obtained from event samples at six MAP3S sampling sites and from hourly samples at Brookhaven National Laboratory. Concentrations of hydrogen, sulfate, nitrate and ammonium ions were used as receptor data. Some emissions data for SO_x and NO_x were obtained from the MAP3S emissions inventory. Surface and upper air meteorological data were analyzed. Backward trajectories ending at each of the sampling sites during the precipitation period were computed with the Heffter Interactive-Terminal Transport Model using selected transport layers. Results show that concentrations of pollutant species in event precipitation samples were much higher at stations at end points of trajectories passing through the Ohio River valley than at stations with other trajectories. Likewise, concentrations at Brookhaven were much higher during the end period of a trajectory through the same region than with more northerly and more southerly tracks. The model produced back trajectories consistent with synoptic flows. Concentrations of air pollutants in precipitation were roughly proportional to the number of major pollutant sources along the trajectory. These results suggest that a larger number of studies might identify more restricted source areas or even establish a quantitative relationship between source emissions along a trajectory and concentrations in precipitation at receptor sites.