A new metric space incorporating radon-222 for generation of back trajectory clusters in atmospheric pollution studies

A novel metric space for the clustering of back trajectories to be used in fine particle aerosol data analysis was proposed and evaluated. The metric is based on spatial and non-spatial variables incorporating great-circle distance, altitude and radon-222.Its performance was examined using the intra-cluster variation of measured and fingerprint apportioned aerosol mass as the quantitative criterion. The new metric was demonstrated to perform better than those based on great-circle distance, or a great-circle distance and altitude alone. The same criterion was applied to investigate the clustering performance as a function of the length of its back trajectories. The optimum back trajectory length was found to be dependent on the pollution source being considered.Performance tests, as well as the application of the new metric space to re-analysis of previously published results, were based on a three year long dataset comprising co-located aerosol fine particles (PM_2.5) collection and hourly measurements of radon-222 concentration.The new metric space can easily be redefined to include other trace species.     

Cape Point GAW Station 222Rn detector: factors affecting sensitivity and accuracy

Specific factors of a baseline ²²²Rn detector installed at Cape Point, South Africa, were studied with the aim of improving its performance. Direct sunlight caused air turbulence within the instrument, resulting in 13.6% variability of the calibration factor. Shading the instrument eliminated this effect. A residual temperature dependence of the calibration factor was reduced to negligible levels with an improved photomultiplier tube. A superior detector head permits field servicing of the instrument, and has reduced one component of the instrumental background by a factor of 2. The other component probably constitutes thoron emissions from the stainless steel walls. The detection limit of the instrument could be reduced from its current 33 to 20 mBq m⁻³ if the thoron were to be eliminated.     

Survey-based inventory for atmospheric emissions from residential combustion in Vietnam

Environmental Science and Pollution Research - Local questionnaire surveys were conducted to collect representative activity data for calculation of annual emissions from residential combustion in...     

Portuguese inventory of dioxins and furans atmospheric emissions

This article presents the results of the most recent estimation of polychlorinated dibenzo-p-dioxins (PCDD) and dibenzofurans (PCDF) atmospheric emissions in Portugal, which has covered the period 2004–2009 and includes 27 emission sources types. The results are compared with previous emissions inventories published for Portugal. The main objective of this work is to provide relevant information about the amounts of the compounds that are released into the atmosphere in Portugal, and identify their major sources and trends.     

Steps towards a European dioxin emission inventory

The results of a project aiming at collection and evaluation of information regarding the industrial and non-industrial emission sources for dioxins and furans (PCDD/PCDF) in 17 European Countries (EU 15, CH, N) are presented. An overview about national documents covering dioxin emission inventories for the period 1990-1995 is given. Some data on emissions associated with residual materials, waste and waste water are presented additionally. Based on the air emission data contained in these documents the most important emission sources were determined which are assumed to cover about 90% of the overall emissions. For the selected sources and for all 17 countries new estimates of the atmospheric PCDD/PCDF emissions were derived from average emission factors and statistical activity rates for the year 1994. As a result, on the European scale the largest annual PCDD/PCDF emission is assessed to be released from municipal waste incineration, quite closely followed by emissions from iron ore sintering. Considerable releases of dioxins and furans--based, however, on highly uncertain data--are further assessed for domestic burning, accidental fires and (former) use of contaminated wood preservatives (pentachlorophenol). A lower but still significant emission is further assigned to the sector of non-ferrous metal production; particular processes used in this branch proved to generate very high PCDD/PCDF flue gas concentrations.     

222Rn concentrations,natural flow rate and the radiation exposure levels in the Nerja Cave

²²²Rn concentrations in the air in Nerja Cave (Spain) have been measured over 4 yr and at four sampling points. Concentrations average 168 Bq m^-3 in the spring–summer when the temperature lapse rate provides a stable cave atmosphere. In the autumn–winter, the radon levels decrease to 48 Bq m^-3. ²²²Rn flux has also been measured for soils in the cave, with an average value of 34 × 10^-3 Bq m^-2 s^-1. The average natural flow rate in the spring–summer is about 0.70 m³ s^-1 and the autumn–winter is approximately 3.6 m³ s^-1 determined over 1992–1995. The radiation exposure levels for workers and tourists represent only a low percentage of the exposure guides for the general population.     

Assessment of 222Rn emanation from ore body and backfill tailings in low-grade underground uranium mine

This paper presents a comparative study of ²²²Rn emanation from the ore and backfill tailings in an underground uranium mine located at Jaduguda, India. The effects of surface area, porosity, ²²⁶Ra and moisture contents on ²²²Rn emanation rate were examined. The study revealed that the bulk porosity of backfill tailings is more than two orders of magnitude than that of the ore. The geometric mean radon emanation rates from the ore body and backfill tailings were found to be 10.01?×?10^?3 and 1.03 Bq m^?2 s^?1, respectively. Significant positive linear correlations between ²²²Rn emanation rate and the ²²⁶Ra content of ore and tailings were observed. For normalised ²²⁶Ra content, the ²²²Rn emanation rate from tailings was found to be 283 times higher than the ore due to higher bulk porosity and surface area. The relative radon emanation from the tailings with moisture fraction of 0.14 was found to be 2.4 times higher than the oven-dried tailings. The study suggested that the mill tailings used as a backfill material significantly contributes to radon emanation as compared to the ore body itself and the ²²⁶Ra content and bulk porosity are the dominant factors for radon emanation into the mine atmosphere.     

Global atmospheric emission inventory of polycyclic aromatic hydrocarbons (PAHs) for 2004

The global atmospheric emissions of the 16 polycyclic aromatic hydrocarbons (PAHs) listed as the US EPA priority pollutants were estimated using reported emission activity and emission factor data for the reference year 2004. A database for emission factors was compiled, and their geometric means and frequency distributions applied for emission calculation and uncertainty analysis, respectively. The results for 37 countries were compared with other PAH emission inventories. It was estimated that the total global atmospheric emission of these 16 PAHs in 2004 was 520 giga grams per year (Gg y^?1) with biofuel (56.7%), wildfire (17.0%) and consumer product usage (6.9%) as the major sources, and China (114 Gg y^?1), India (90 Gg y^?1) and United States (32 Gg y^?1) were the top three countries with the highest PAH emissions. The PAH sources in the individual countries varied remarkably. For example, biofuel burning was the dominant PAH source in India, wildfire emissions were the dominant PAH source in Brazil, while consumer products were the major PAH emission source in the United States. In China, in addition to biomass combustion, coke ovens were a significant source of PAHs. Globally, benzo(a)pyrene accounted for 0.05% to 2.08% of the total PAH emission, with developing countries accounting for the higher percentages. The PAH emission density varied dramatically from 0.0013 kg km^?2 y in the Falkland Islands to 360 kg km^?2 y in Singapore with a global mean value of 3.98 kg km^?2 y. The atmospheric emission of PAHs was positively correlated to the country's gross domestic product and negatively correlated with average income. Finally, a linear bivariate regression model was developed to explain the global PAH emission data.     

The European dioxin air emission inventory project--final results

Main results of the second stage of the so-called "European Dioxin Emission Inventory" are presented. They cover emission testing data gained from various facilities in the EU (among these the first emission measurements reported from Portugal and Greece) and some central European countries. Further, updated dioxin emission estimates for the most important emission sources in the 17 western European countries and an evaluation of the emission time trend from 1985 to 2005 are presented. The major conclusions are, that at present, iron ore sintering is likely to be the most important emission source type followed by the former "No. 1", municipal waste incineration; measurement data from a considerable number of installations are still missing, in particular from the metal industries in Spain and Italy; there still exist an unknown number of health care waste incinerators with flue gas PCDD/F concentrations above 100 ng I-TEQ/m3 which must be considered as important local sources; in general, considerable emission reduction has been achieved with respect to the industrial emission sources, whereas emissions from non-industrial sources hardly decreased; hence, in the near future the emissions from non-industrial sources are likely to exceed those from industrial installations; the goal of 90% emission reduction set in the 5th EU Action Programme will be achieved for some source types only.     

A photochemical reactor for studies of atmospheric chemistry

A photochemical reactor for studies of atmospheric kinetics and spectroscopy has been built at the Copenhagen Center for Atmospheric Research. The reactor consists of a vacuum FTIR spectrometer coupled to a 100 L quartz cylinder by multipass optics mounted on electropolished stainless steel end flanges, surrounded by UV-A, UV-C and broadband sun lamps in a temperature-controlled housing. The combination of a quartz vessel and UV-C lamps allows higher concentrations of O(¹D) and OH than can be generated by similar chambers. The reactor is able to produce radical concentrations of ca. 8 × 10¹¹ cm^?3 for OH, 3 × 10⁶ cm^?3 for O(¹D), 3.3 × 10¹⁰ cm^?3 for O(³P) and 1.6 × 10¹² cm^?3 for Cl. The reactor can be operated at pressures from 10^?3 to 10³ mbar and temperatures from 240 to 330 K. As a test of the system we have studied the reaction CHCl₃ + Cl using the relative rate technique and find k_CHCl3+Cl/k_CH4+Cl = 1.03 ± 0.11, in good agreement with the accepted value.     

Seasonal and spatial variations of enhanced gamma ray dose rates derived from 222Rn progeny during precipitation in Japan

Enhanced gamma (Δγ) ray dose rates due to ²²²Rn progeny wet deposited on the ground surface measured at six monitoring sites in Japan were statistically analyzed to investigate their temporal and spatial variations. Variations of Δγ ray dose rates indicated significant regional differences between the sites on the Sea of Japan coast and those located inland and on the Pacific coast in Japan. At the sites located on the Sea of Japan coast, significant seasonal variation was evident, with higher dose rates in autumn and winter, and lower dose rates in summer. In contrast, however, no significant seasonal variation was observed at the inland and Pacific coast sites in Japan. The variation of Δγ ray dose rates was characterized by three major factors: climatologically changed air masses arriving in Japan, variation of ²²²Rn and its progeny concentrations in the air column, and the regional characteristics of precipitation. It is evident that the contribution from local ²²²Rn to Δγ ray dose rates was smaller than those from continental ²²²Rn. Meso-scale atmospheric disturbance, however, was suggested as an important process for extremely high Δγ ray dose rates, possibly by the accumulation of additional local ²²²Rn with stronger convergence. It is therefore possible that the variation of Δγ ray dose rates reflects the chemical climatology of ²²²Rn and its progeny.     

Cluster analysis applied to atmospheric aerosol samples from the Norwegian Arctic

Cluster analysis is shown to be a useful technique for the identification and characterization of atmospheric aerosol particles. A general procedure for combining the cluster analysis results from a large number of samples is described and shown to be successful for comparing such samples. Two similarity measures, one not previously described, are evaluated for use in cluster analysis.The new analysis procedure was applied to the examination of 11 coarse-fraction and 19 fine-fraction aerosol samples collected during September and October, 1984 at Ny Alesund, Spitzbergen, Norway, ~ 1400 km north of the Arctic Circle. The aerosol at this site consists primarily of Si-, Cl- and S-rich particles, the relative abundance of each varying from sample to sample. Considerable differences in composition were observed between simultaneously collected coarse- and fine-fractions.     

Temporal variations of atmospheric aerosol in four European urban areas

Purpose

The concentrations of PM₁₀ mass, PM_2.5 mass and particle number were continuously measured for 18 months in urban background locations across Europe to determine the spatial and temporal variability of particulate matter.

Methods

Daily PM₁₀ and PM_2.5 samples were continuously collected from October 2002 to April 2004 in background areas in Helsinki, Athens, Amsterdam and Birmingham. Particle mass was determined using analytical microbalances with precision of 1 ??g. Pre- and post-reflectance measurements were taken using smoke-stain reflectometers. One-minute measurements of particle number were obtained using condensation particle counters.

Results

The 18-month mean PM₁₀ and PM_2.5 mass concentrations ranged from 15.4 ??g/m³ in Helsinki to 56.7 ??g/m³ in Athens and from 9.0 ??g/m³ in Helsinki to 25.0 ??g/m³ in Athens, respectively. Particle number concentrations ranged from 10,091 part/cm³ in Helsinki to 24,180 part/cm³ in Athens with highest levels being measured in winter. Fine particles accounted for more than 60% of PM₁₀ with the exception of Athens where PM_2.5 comprised 43% of PM₁₀. Higher PM mass and number concentrations were measured in winter as compared to summer in all urban areas at a significance level p?Conclusions Significant quantitative and qualitative differences for particle mass across the four urban areas in Europe were observed. These were due to strong local and regional characteristics of particulate pollution sources which contribute to the heterogeneity of health responses. In addition, these findings also bear on the ability of different countries to comply with existing directives and the effectiveness of mitigation policies.     

乌昌石区域的非金属矿物制品业大气污染物排放清单研究

建立了乌昌石区域非金属矿物制品业CO、NO_x、SO_2、PM_(2.5)和PM_(10) 5种大气污染物的排放清单,并进行了时空分布特征分析,初步探究了估算的不确定性。结果显示,乌昌石区域非金属矿物制品业CO、NO_x、SO_2、PM_(2.5)和PM_(10)总排放量分别为3.71×10~4、2.76×10~4、3.10×10~4、3.04×10~4、1.29×10~5 t。熟石膏行业是CO的主要排放源;水泥(干法)行业是NO_x、SO_2、PM_(2.5)和PM_(10)的主要排放源。乌鲁木齐市是CO、NO_x和SO_2排放量的最大贡献源;石河子市是PM_(2.5)和PM_(10)排放量的最大贡献源。乌昌石区域5月至9月是一年中污染物排放的高峰期,11:00至20:00是一天中污染物排放的高峰期。空间上,乌昌石区域的污染物排放主要分布在乌鲁木齐市中部、西南部以及石河子市。     

Sulfate in precipitation as observed by the European atmospheric chemistry network

The temporal variation in sulfur concentration/deposition involves long term fluctuations which show striking similarities within certain areas but are different between areas in different positions relative to major sulfur emission areas in Europe. As an example, the deposition has been constant or decreasing during the last ten years in most of the area covered by the network, indicating that an increasing amount of the sulfur emitted in Europe is transported and deposited elsewhere, possibly in an eastward direction.The seasonal variation in deposition resembles that for amount of precipitation and shows a maximum during the summer or autumn for most areas. The concentration shows a maximum in the spring and a minimum in the autumn at most stations.The concentration field has a maximum approximately over Belgium and Holland with decreasing concentrations towards SW to NE (over W) but with comparatively high levels extending up over Finland. (Areas to the east and south are not covered by the network.)The deposition field was, based on a brief discussion of the relation between concentration and amount of precipitation, obtained as the product of these latter fields. High deposition rates are found in the south of Norway and in the middle of Britain in addition to the areas with high concentration.Sulfur and hydrogen ion are the dominating ions in precipitation followed by ammonium and nitrate except in coastal areas and in places where the soil is bare.Sources of errors in the data base are discussed and the results from a large number of additional sampling sites around and between the regular network sampling sites are most helpful in this regard. These latter measurements also permit an estimate of the uncertainty in areal concentration averages which are due to local and mesoscale variability.Finally, past and future importance of continuous measurements (as in the EACN) is discussed briefly.     

Heterogeneous response of central European streams to decreased acidic atmospheric deposition

We investigated the relations between mountain streamwater chemistry and atmospheric pollution in an arca of 1611 km2 of the Czech Republic by comparing concentrations of SO4. NO3, Cl, Ca and the pH at 432 localities at the time of high (1984-1986) and relatively low (1996-2000) acidic atmospheric deposition. Medians of Cl. SO4, and NO3 decreased by 17, 96 and 60 microeq l(-1), or by 23, 17 and 49%, respectively, during 12 +/- 2 years. The decreased Cl corresponds to decreased emission of industrial Cl (as HCl). The decreased stream SO4 was proportionally lower than the 71% decrease in S-emissions due to leaching of previously accumulated SO4 from soils and non-zero background concentrations. Decreases of NO3 up to 60% in streamwaters with pH < or = 6 was greater than the decrease of N emission in central Europe, about 35%. Extensive regional decrease of NO3 is surprising and is probably described for the first time. The difference in NO3 concentrations between the two periods was probably enhanced by (a) an increase of mineralisation of forest floor in the mid-1980s and (b) by higher uptake of N in the late-1990s. The median pH of the 432 streams did not change but the pH of the sub-population with pH < 6 in the mid-1980s recovered substantially. The pH of circum-neutral streams (pH > 6.5) decreased even as acidic atmospheric deposition decreased.     

Field studies of atmospheric particulate concentration changes during precipitation

The effect of rain on changes in the atmospheric particulate concentration was evaluated, and these measurements were compared with theoretical calculations of particle washout coefficients. Cumulative particle number distributions in two size subranges, around 0.01 and 1 μm, were measured at two different times during three separate precipitation events to establish apparent washout coefficients. Raindrop size distributions and precipitation intensity measurements were also obtained to estimate the theoretical washout coefficients.The experimental washout coefficients were between 2 × 10⁻⁵s⁻¹and 1 × 10⁻⁴s⁻¹, depending on the raindrop size distribution and precipitation intensity. These values were one to two orders of magnitude greater than theoretical estimates that considered the known single droplet collection mechanisms of inertial impaction, interception, Brownian diffusion, thermophoresis, diffusiophoresis, and electrostatic charge effects. Based on these results, it appears that these mechanisms cannot adequately explain the observed decreases in particle number density during a precipitation event.     

A European survey of atmospheric heavy metal deposition in 2000-2001

The background, administration and current status of the monitoring programme "European Survey of Atmospheric Heavy Metal Deposition" is described. All European states are invited to join the survey 2000-2001. The co-ordination and responsibility for the survey will gradually be transferred from the Nordic Council of Ministers to the International Cooperative Programme on Effects of Air Pollution on Natural Vegetation and Crops (ICP Vegetation).