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Atmospheric Environment (v.39, #5)

Editorial board (pp. i).

List for forthcoming papers (pp. i-ii).

Endocrine disrupting chemical emissions from combustion sources: diesel particulate emissions and domestic waste open burn emissions by Sukh Sidhu; Brian Gullett; Richard Striebich; Joy Klosterman; Jesse Contreras; Michael DeVito (pp. 801-811).

Emissions of endocrine disrupting chemicals (EDCs) from combustion sources are poorly characterized due to the large number of compounds present in the emissions, the complexity of the analytical separations required, and the uncertainty regarding identification of chemicals with endocrine effects. In this work, multidimensional gas chromatographic-mass spectrometry (MDGC-MS) was used to characterize emissions from both controlled (diesel engine) and uncontrolled (open burning of domestic waste) combustion sources. The results of this study suggest that, by using MDGC-MS, one can resolve a much greater percentage of the chromatogram and identify about 84% of these resolved compounds. This increase in resolution helped to identify and quantify various classes of polycyclic aromatic hydrocarbons (PAHs) in the combustion emissions that had not been identified previously. Significant emissions (when compared to industrial sources) of known EDCs, dioctyl phthalate (over ∼2,500,000kgyear⁻¹) and bisphenol A (over ∼75,000kgyear⁻¹) were estimated from uncontrolled domestic waste burning. Emissions of several suspected EDCs (oxygenated PAHs) were observed in both diesel soot and the uncontrolled domestic waste burn samples. The emission rates of known and suspected EDCs estimated in this study suggest that combustion emissions need to be characterized for EDCs to further assess its importance as a source of EDC exposure.

Keywords: Bisphenol A; Diesel emissions; Open barrel burning; Oxygenate PAHs; Multidimensional GC-MS

Emission inventory of eight elements, Fe, Al, K, Mg, Mn, Na, Ca and Ti, in dust source region of East Asia by Jie Xuan (pp. 813-821).

Based on calculation of the emission rate of the atmospheric mineral dust and the data of elemental contents in surface soils, this paper calculates the emission inventory of eight main elements of the atmospheric dust, Fe, Al, K, Mg, Mn, Na, Ca and Ti, in the dust source region of East Asia. As the dust sources in both Northern China and the Southern Mongolia are of three types and, in each of the six source type areas, surface soils are relatively uniform in soil types and soil texture, a simple method to calculate the emission of an element in one source type area is proposed by multiplying the total emission of the dust PM₁₀ and PM₅₀ in the source type area with the mean percentage content of the element in surface soils of the area. Comparison of our calculation of the total Fe emission in the source region of East Asia with the total Fe deposition to the North Pacific Ocean, measured and calculated by previous authors, shows very good agreement. This general method can also be used for the emission calculation of any other element.

Keywords: Atmospheric dust; Dust emission; Element emission; Dust sources; East Asia

Atmospheric bulk deposition of soluble phosphorus in Ashiu Experimental Forest, Central Japan: source apportionment and sample contamination problem by S. Tsukuda; M. Sugiyama; Y. Harita; K. Nishimura (pp. 823-836).

Atmospheric bulk depositions of soluble reactive phosphorus (SRP), soluble unreactive phosphorus (SUP), soluble total phosphorus (STP), Na, SO₄, V and Mo were monitored for 3 years in Ashiu Experimental Forest in Central Japan. Relations among P, SO₄, V and Mo data were analyzed to determine if any part of P deposition is derived from fossil fuel combustion. Contamination by local particles was evaluated and its influence on atmospheric P input estimates was discussed. The mean bulk depositions of SRP, SUP, STP, Na, SO₄, V and Mo were 175, 76, 251, 156000, 40100, 10.3, and 1.52μmolm⁻²year⁻¹, respectively. Bulk depositions of Na, nss-SO₄, V and Mo were within the range of published data, while P deposition represented the lowest value found in literature. The low P deposition likely reflected the applied methodology to reduce sample contamination, i.e. (1) placement of samplers off the ground surface, (2) installation of multiple samplers, (3) rejection of samples with visible contamination, and (4) choosing the lowest values as the least contaminated. P and Na showed single peak during winter and spring, while nss-SO₄, V and Mo showed two peaks during winter and during summer. Nss-SO₄ and Mo data suggested that 59–89% of deposited STP was derived from fossil fuel combustion. Elemental composition of fossil fuels and airmass backward trajectories suggested that a large part of anthropogenic P originates from coal combustion in China. It was speculated that the rest (11–41%) of STP deposition might be predominantly attributed to contamination of local biogenic material. The result suggests that even after precautionary methodologies were employed, the data might still be affected by contamination. It should be remembered that one must take considerable care when interpreting P deposition data to evaluate atmospheric P input to terrestrial ecosystems.

Keywords: Anthropogenic activity; Fossil fuel combustion; Molybdenum; Pollen; Vanadium

Chemometric analysis of rainwater and throughfall at several sites in Poland by Ż. Żaneta Polkowska; Aleksander Astel; Barbara Walna; Stanisław Małek; Krystyna Mędrzycka; Tadeusz Górecki; Jerzy Siepak; Jacek Namieśnik (pp. 837-855).

Precipitation and throughfall samples were collected over a period of 4 years (1 January 1996–31 December 1999) at three different sites in Poland: one on moraine hills, one in the lowlands and one in a mountainous region. The aim of this project was to study the chemical composition of the samples, ionic correlations and fluctuations of selected variables with time in relation to geographical location, type of tree cover and climatic conditions. The samples were characterized by determining the values of pH, electrolytic conductivity and concentrations levels of SO₄²⁻, NO₃⁻, Cl⁻, Ca²⁺, K⁺, Na⁺ and Mg²⁺. Statistical analysis revealed significant differences between the results obtained for different sampling site locations and characteristics (region of Poland, open area vs. throughfall) in four cases. The results obtained for precipitation samples were similar to those for throughfall samples only for acidic anions (SO₄²⁻ and Cl⁻). For open areas, pH fluctuations were observed in 12-month cycles. Differences between the concentration levels of ions in the samples from the three sites could be explained by different amounts of precipitation at these sites. Concentrations of ions in precipitation and throughfall samples followed similar trends, the concentration levels being dependent on the kind of trees in the area, their age, and acidity of the precipitation. Significant differences were found for the concentration factors of the individual ions in throughfall between the sampling sites. Ionic correlations were examined to determine which salts contributed to the observed ion levels.

Keywords: Precipitation; Throughfall; Chemical composition; Ionic correlations; Statistical analysis

Photolysis rate coefficients calculations from broadband UV-B irradiance: model-measurement interaction by Gustavo G. Palancar; Fernandez Rafael P. Fern�ndez; Beatriz M. Toselli (pp. 857-866).

Broadband UV-B irradiance measurements (YES UVB-1) from a 4-year campaign in Córdoba City (31° 24′ S, 64° 11′ W, 454m a.s.l.) and the TUV 4.1 model were used to apply a new approach (exp-mod) to convert broadband irradiance measurements at surface under clear sky conditions to actinic flux and then to J-values. The structure of the model was used to split each measurement into its diffuse and direct component and, in turn, in wavelengths. The results for the daily variation ofJO3 shows an agreement better than 5% for solar zenith angles (SZA) up to 65° and better than 10% up to 70° compared against an 8-stream discrete ordinate method. The annual variation ofJO3 for clear sky days at solar noon shows a general agreement better than 10%. The effects of the natural variation of ozone column and the Córdoba meteorology on this agreement are analyzed. Empirical relations between experimental measurements and J-values calculated with a 2-stream δ-Eddington method are also presented.

Keywords: Actinic flux; Radiative transfer calculations; C�rdoba City; Broadband UV-B measurements; Diffuse ratio

An examination of 7:00–9:00PM ambient air volatile organics in different seasons of Kaohsiung city, southern Taiwan by Chih-Chung Chih-Chung Chang; Usha Sree; Yu-Sung Lin; Jiunn-Guang Jiunn-Guang Lo (pp. 867-884).

This study presents annual data (2000) of non-methane hydrocarbons (NMHC) monitored at dusk hours in ambient air of Kaohsiung by near time sampling at 20 different locations (road-side and industrial) between 7 and 9PM. A 16-canister automatic introducing system was applied to inject the air sample into a sample pre-concentration trap (SPT) that cryo-focused the sample, followed by desorption from SPT by heating to 160°C, and analyzed by a GC system coupled with FID or MSD. The highest levels of non-methane hydrocarbons were detected in industrial zones and were two times greater than those in non-industrial areas in June and about 1.4–1.7 times greater during the rest of the year. Ethylene, 2-methyl butene and toluene were found to be the most abundant occurring analytes in the four seasons. Ethylene was mainly emitted from petroleum plants and to a lesser extent from vehicles. The major source of toluene is identified as emissions from mobile vehicles and partly from vaporization of organic solvents used in petroleum industries. n-Butane at the non-industrial sites is mainly emitted from liquefied petroleum gas (LPG)-fuelled vehicles. A 24h monitoring in December 1999 at non-industrial sites revealed a comparatively higher ratio of toluene/benzene and toluene/ethylene at night. The estimated reactivity's with OH and NO₃ radicals is greater in November and least in March and ozone formation potential appears greater in January and the least in March. A comparison of this data set with that obtained in 2003 from two specific sampling sites indicates a 5–10% reduction in emissions of alkenes and an increase of 7–10% of alkanes.

Keywords: Volatile organics; Ethylene; Butane; Toluene; Vehicle emissions; Ozone; Kaohsiung

Measurement of the vapor phase deposition of polychlorinated bipheyls (PCBs) using a water surface sampler by Y. Y�cel Tasdemir; Mustafa Odabasi; Thomas M. Holsen (pp. 885-897).

A water surface sampler (WSS) was employed in combination with greased knife-edge surface deposition plates (KSSs) to measure the vapor phase deposition rates of PCBs to the sampler at an urban site, Chicago, IL. This sampler employed a water circulation system that continuously removed deposited PCBs. Total (gas+particle) and particulate PCB fluxes were collected with the WSS and KSSs, respectively. Gas phase PCB fluxes were then calculated by subtracting the KSS fluxes (particulate) from the WSS fluxes (gas+particle). The calculated gas phase PCB fluxes averaged 830±910ngm⁻²d⁻¹. This flux value is, in general, higher than the fluxes determined using simultaneously measured air–water concentrations in natural waters and is in the absorption direction. This difference is primarily because the PCBs were continuously removed from the WSS water keeping the water PCB concentration near zero.Concurrently, ambient air samples were collected using a modified high volume air sampler. The gas phase PCB concentrations ranged between 1.10 and 4.46ngm⁻³ (average±SD, 2.29±1.28ngm⁻³). The gas phase fluxes were divided by the simultaneously measured gas phase ambient concentrations to determine the overall gas phase mass transfer coefficients (MTCs) for PCBs. The average gas phase overall MTCs ( K_g) for each homolog group ranged between 0.22 and 1.32cms⁻¹ (0.54±0.47cms⁻¹). The average MTC was in good agreement with those determined using similar techniques.

Keywords: PCB; Air-water exchange; MTC; Flux; Dry deposition

A case study of the radiative effects of Arctic aerosols in March 2000 by R. Treffeisen; A. Rinke; M. Fortmann; K. Dethloff; A. Herber; T. Yamanouchi (pp. 899-911).

Accurate modelling of the radiative forcing due to Arctic aerosols requires an adequate knowledge about the spectral, spatial and temporal variability of the aerosol. This needs contrasts with the limited measurements of Arctic aerosol characteristics. This paper presents two different approaches to incorporate Arctic aerosols in the regional climate model HIRHAM to overcome this problem. In the first method, Arctic aerosol properties are described via a mixture of different components from the global aerosol data set (GADS). The second method derives the aerosol model input parameter from an Arctic airborne measurement campaign (ASTAR) via a data transformation. Results from a one-dimensional radiative transfer model for a case study are presented for two selected days of March 2000, one with a high and another with a lower aerosol loading, which were considered to be representative for the Arctic spring aerosol loading. The calculated heating rate anomalies are sensitive to the assumed aerosol characteristics (absorption characteristics, particle radius, chemical composition, mass-mixing ratio). The performed study showed the importance of both methods for modelling solar radiative forcing due to Arctic aerosols. For the 2 days selected, calculated local solar heating rate anomalies between 0.05 and 0.3Kday⁻¹ were achieved. An application of a high-resolution regional climate model is presented to determine the regional climatic impact of Arctic aerosols during March 2000. The aerosol effect induced a substantial spatial variability at the regional scale and varies between a cooling of 2K in the Baffin Bay and Laptev Sea and a warming of 3K in the Beaufort Sea. Arctic aerosol loading changed the sea level pressure patterns over the Arctic Ocean with implications for additional feedbacks on a coupled atmosphere–ocean–sea ice model of the Arctic.

Keywords: Optical properties; Climate forcing; Regional climate model

New model for the sulfation of marble by dry deposition Sheltered marble—the indicator of air pollution by sulfur dioxide by Tran Thi Ngoc Lan; Nguyen Thi Phuong Thoa; R. Nishimura; Y. Tsujino; M. Yokoi; Y. Maeda (pp. 913-920).

This paper was concerned with evaluating the effect of dry deposition on deterioration of marble. Two types of marble were exposed to atmospheric environment with a rain shelter at four exposure sites in the south of Vietnam for 3-month, 1-year and 2-year periods from July 2001 to September 2003. X-ray diffraction (XRD) and X-ray fluorescent (XRF) methods were applied to study the products of marble deterioration. Ion chromatography was used to analyze dry depositions on marble. The main product of marble deterioration was gypsum (CaSO₄�2H₂O). The amount of sulfate ions deposited on marble was found to be proportional to SO₂ concentration in the air, relative humidity and duration of the exposure. In addition, sulfation of marble caused by SO₂ at a relative humidity lower than 70% is almost half of that at relative humidity higher than 70%. Moreover, marble consisting of calcite (CaCO₃) was more sensitive to SO₂ than marble consisting of dolomite (CaCO₃ and MgCO₃). A good relation between the amount of sulfate ions deposited on marble and SO₂ concentration in the air suggested that marble could serve as an indicator for atmospheric pollution by SO₂.

Keywords: Acidification; Passive sampler; Sulfation; Dolomite; Calcite

Emission of non-methane volatile organic compounds (VOCs) from boreal peatland microcosms—effects of ozone exposure by Riikka Rinnan; A. �smund Rinnan; Toini Holopainen; Jarmo K. Holopainen; Pertti Pasanen (pp. 921-930).

Non-methane volatile organic compounds (VOCs) emitted from boreal peatland microcosms were semiquantitatively determined using gas chromatography–mass spectrometry techniques in a growth chamber experiment. Furthermore, effects of vegetation composition and different ozone concentrations on these emissions were estimated by multivariate data analyses. The study concentrated on the less-studied VOCs, and isoprene was not analyzed. The analyses suggest that a sedge Eriophorum vaginatum is associated with emissions of the four most-emitted VOC groups (cyclic, aromatic, carbonyl and aliphatic hydrocarbon compounds) and also with VOCs emitted in smaller amounts (terpenoids and N-containing compounds). A woody dwarf shrub Andromeda polifolia was strongly associated with emissions of aromatic, carbonyl and terpenoid compounds. Results suggest that exposure to an ozone concentration of 150ppb leads to an increased emission of most VOC groups. Emission of aromatic compounds seems to increase linearly with increasing ozone concentration. These observations indicate that peatlands may be a source of a vast range of volatile compounds to the atmosphere. For more accurate assessment of the impact of elevated tropospheric ozone on the terpenoid and non-terpenoid VOC emissions from peatlands, well-replicated open-air ozone-exposure experiments should be conducted.

Keywords: Tropospheric ozone; Biogenic VOC; Sphagnum; Shrub; Wetland; Multivariate data analysis

Fuel-based motor vehicle emission inventory for the metropolitan area of Mexico city by I. Schifter; Diaz L. D�az; Mugica V. M�gica; Lopez-Salinas E. L�pez-Salinas (pp. 931-940).

The level and nature of air pollution varies substantially from city to city. Hence, the first requirement is the creation of an adequate knowledge base on local air quality on which to develop an air quality policy. Because the availability of data used in traditional on-road mobile source estimation methodologies is limited in Mexico, an alternative methodology was implemented to estimate motor vehicle emissions. In the year 2000, on-road gasoline powered vehicle emissions in the Metropolitan Area of Mexico City (MAMC), were characterized using fuel sales as a measure of vehicle activity, and exhaust emissions factors from remote sensing measurements. In a similar way, remote sensing data obtained by researchers of the University of Denver back in 1991 and 1994 were used to estimate a fuel-based emission inventory for those years. Average emissions factors were estimated in 113.5±13, 13.1±1.9 and 9.84±2.3gl⁻¹ for CO, hydrocarbons (HC) and nitrogen oxides (NO _x), respectively, based on remote sensing measurements of 42,800 vehicles. For year 2000 light and medium gasoline vehicles exhaust emissions contributed with 2065, 238, and 179 metric ton day-1 of CO, HC and NO _x, respectively. The inventory is 48% and 26% lower in CO and NO _x, respectively, than official inventory estimates for the year 1998 using travel-based models. Calculated CO reduction from 1991 to 1994 is approximately 46% while the atmospheric CO measurements, as indicator of mobile activity, in the same period decrease 51%. For the period 1994–2000 the reductions were 36% and 31%, respectively. The calculations indicate a continually decreasing inventory over the study period, and represents and ideal alternative for locations such as Mexican cities lacking the resources to develop an emissions model.

Keywords: Remote sensing; Fuel-based inventory; Mexico city

Differential optical absorption spectrometer measurement of NO₂, SO₂, O₃, HCHO and aromatic volatile organics in ambient air of Kaohsiung Petroleum Refinery in Taiwan by Kong Hwa Chiu; Usha Sree; Sen Hong Tseng; C.-H. Chien-Hou Wu; J.-G. Jiunn-Guang Lo (pp. 941-955).

UV-differential optical absorption spectrometer (DOAS) technique is considered as a promising technique to detect gaseous pollutants and was applied to conduct one-week continuous measurements in the Chinese Petroleum (CPC) refinery plant located in Lin Yuan industrial park of Kaohsiung, Southern Taiwan. With the combination of local meteorological information, including solar radiation, wind direction and speed, the results showed that the concentrations of aromatic compounds and formaldehyde (HCHO) were higher at night while the values of ozone, NO₂ and SO₂ were high during the day. The major source of aromatics was the aromatic extraction unit in the refinery while NO₂ and SO₂ were mainly emitted from chimneys with not very high average concentrations. Formaldehyde concentration was above 50ppbv during night. There exists an apparent correlation between the variation of ground-level ozone concentration and photochemical reactions. The results indicate that in addition to benzene and toluene, ozone is a deleterious pollutant. The commercial DOAS system provides reliable information on distribution patterns of major air pollutants depending on their concentration levels in ambient air.

Keywords: Ground-level ozone; Petroleum refinery; Taiwan; DOAS

Measurements of gaseous elemental mercury fluxes over intact tallgrass prairie monoliths during one full year by Daniel Obrist; Mae S. Gustin; John A. Arnone III; Dale W. Johnson; David E. Schorran; Paul S.J. Verburg (pp. 957-965).

The atmosphere is an important pathway by which mercury is transported and distributed to pristine ecosystems. The significance of anthropogenic versus natural mercury contributions to the atmosphere is controversial, and the importance of re-emission of deposited mercury from ecosystems is not known. Here we present a continuous year-long data set of gaseous elemental mercury exchange between intact soil–plant monoliths of tallgrass prairie and the atmosphere. Mercury fluxes were measured using large open-flow gas exchange chambers (7.3×5.5×4.5m³, L× W× D). Approximately 60μgm⁻² of elemental gaseous mercury was lost from four replicate grassland ecosystems (9m² surface area each) to the atmosphere over the course of 1yr. Deposition was an important flux in the winter and emissions were dominant in spring, summer, and fall. Solar radiation and air temperature were most strongly correlated with mercury emissions. Gaseous elemental mercury losses to the atmosphere exceeded other measured fluxes of mercury in and out of the grassland ecosystems. These results indicate that mercury emissions from uncontaminated terrestrial ecosystems to the atmosphere may be a significant source of atmospheric mercury. We hypothesize that most of the mercury being emitted is previously deposited mercury and that re-emissions of mercury from terrestrial ecosystems is an important process whereby mercury is continually cycled between the air and terrestrial ecosystems.

Keywords: Mercury; Tallgrass prairie; Flux measurements; Mesocosms; EcoCELLs

Measurements of trace gas distributions using Long-path DOAS-Tomography during the motorway campaign BAB II: experimental setup and results for NO₂ by I. Pundt; K.-U. Mettendorf; T. Laepple; V. Knab; P. Xie; Losch J. L�sch; C.v. Friedeburg; U. Platt; T. Wagner (pp. 967-975).

The Tomographic Differential Optical Absorption Spectroscopy (Tom-DOAS) technique and results from a first application are presented. This novel technique serves to measure 2–3-dimensional concentration fields of different trace gases (e.g. NO₂, SO₂, ozone) in the planetary boundary layer on a small scale (100–10000m) by the use of multiple light paths. Ways to use telescopes, lamps, retroreflector arrays and spectrometers for the simultaneous measurement of many light-paths are proposed. The results from a first Long-path Tom-DOAS experiment next to a German motorway, which was part of the BAB II campaign April/May 2001 [Edition of the Institut für Meteorologie und Klimaforschung, Forschungszentrum Karlsruhe/Universität Karlsruhe, pp. 45, 2001), are presented. From the measurements along 16 different light paths vertical profiles on both sides of the motorway as well as a two-dimensional map of the NO₂ vehicle emission plume are derived. The concentration distributions agree qualitatively with model simulations of an earlier campaign.

Keywords: DOAS; Tomography; Vehicle emission; NO; ₂

Multi-axis-DOAS measurements of NO₂ during the BAB II motorway emission campaign by C.v. Christoph v. Friedeburg; Irene Pundt; Kai-Uwe Mettendorf; Thomas Wagner; Ulrich Platt (pp. 977-985).

Slant column densities (SCD) of traffic-generated NO₂ were derived during the “BAB II�? motorway emission campaign in April/May 2001 using scattered sunlight and a CCD-based Multi-Axis- (MAX) DOAS setup with eight viewing directions being probed simultaneously. The setup allowed for the tracking of the diurnal variation of a motorway plume with 1min temporal resolution, an assessment of the vertical structure as well as the comparison with the plume outreach of Heidelberg.

Keywords: DOAS technique; Remote sensing; NO; ₂; measurements; Emission calculation; Model evaluation

Corrigendum to “Control of off-gassing rates of methyl isothiocyanate from the application of metam-sodium by chemigation and shank injection�? by D.A. Sullivan; M.T. Holdsworth; D.J. Hlinka (pp. 987-987).

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Atmospheric Environment (v.39, #5)