Monitoring of air pollution by polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans of pine needles in Korea

The atmospheric contamination levels of polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) were evaluated from the analysis of pine needles in South Korea. Pine needles were collected from 30 sampling points at five main cities in South Korea (Busan, Daegu, Gwangju, Changwon and Jeju island). The highest concentrations of PCDDs/DFs (2.19–26.88 pg I-TEQ/g of dry weight) were measured at Busan, where is the city of the highest population density and traffic volume among five cities. The lowest concentration was detected at Jeju with 0.62 pg I-TEQ/g dry weight, suggesting Jeju could be an environmental background area in Korea. The dominant homologues of PCDDs/DFs in pine needles were the lower chlorine-substituted compounds such as tetra CDDs and CDFs, and the distribution ratios of PCDDs/DFs decreased with increase of the number of chlorine substituents. Homologue profiles of pine needle samples were similar to PCDDs/DFs profiles of the vapor phase in the ambient air, and thus the pine needles absorbed the vapor phase of PCDDs/DFs from air. Results suggested that pine needles could be used as an indicator of the atmospheric contamination for PCDDs/DFs in Korea.     

Kinetics and mechanism of nitrite oxidation by hypochlorous acid in the aqueous phase

The rate coefficient for the reaction of nitrite with hypochlorite and hypochlorous acid has been studied using spectrophotometric measurements. The reaction rate has been determined in a wide range of H(+) concentration (5< or =-log[H(+)]< or =11). The kinetics were carried out as a function of NO(2)(-), H(+) and total hypochlorite ([HOCl](total)=[HOCl]+[ClO(-)]+[ClNO(2)]) concentrations. The observed overall rate law is described by: -d[HClO](T)dt=[a[NO(2)(-)](2)+b[NO(2)(-)]][H(+)](2)c+d[H(+)]+e[NO(2)(-)][H(+)](2)[HOCl](total)At T=298 K and in Na(2)SO(4) at an ionic strength (I=1.00 M), we obtained using a nonlinear fitting procedure: a=(1.83+/-0.36)x10(7) s(-1), b=(1.14+/-0.23)x10(5) Ms(-1), c=(1.12+/-0.17)x10(-13) M, d=(1.43+/-0.29)x10(-6) M(2) and e=(1.41+/-0.28)x10(3) M where the errors represent 2sigma. According to the overall rate law, a/b=k(1)/k(3), b/e=k(3), c=K(w), d/c=K(a), d=K(a)K(w) and e=K(1)K(a). In Na(2)SO(4) at an ionic strength (I=1.00 M), the values of K(1) and K(a) are (1.1+/-0.1)x10(-4) and 1.28x10(7) M(-1), respectively. A mechanism is proposed for the NO(2)(-) oxidation which involves the reversible initial step: NO(2)(-)+HOCl left harpoon over right harpoon ClNO(2)+OH(-) (K(1)), while ClNO(2) undergoes the two parallel reactions: attack by NO(2)(-) (k(1)) and hydrolysis (k(3)). ClNO(2) and N(2)O(4) are proposed as important intermediates as they control the mechanism. The rate coefficients k(1) and k(3) have been determined at different ionic strengths in NaCl and Na(2)SO(4). The influence of the ionic strength and ionic environment has been studied in this work.     

A new environmental chamber for evaluation of gas-phase chemical mechanisms and secondary aerosol formation

A new state-of-the-art indoor environmental chamber facility for the study of atmospheric processes leading to the formation of ozone and secondary organic aerosol (SOA) has been constructed and characterized. The chamber is designed for atmospheric chemical mechanism evaluation at low reactant concentrations under well-controlled environmental conditions. It consists of two collapsible 90 m³ FEP Teflon film reactors on pressure-controlled moveable frameworks inside a temperature-controlled enclosure flushed with purified air. Solar radiation is simulated with either a 200 kW Argon arc lamp or multiple blacklamps. Results of initial characterization experiments, all carried out at 300–305 K under dry conditions, concerning NO_x and formaldehyde offgasing, radical sources, particle loss rates, and background PM formation are described. Results of initial single organic–NO_x and simplified ambient surrogate–NO_x experiments to demonstrate the utility of the facility for mechanism evaluation under low NO_x conditions are summarized and compared with the predictions of the SAPRC-99 chemical mechanism. Overall, the results of the initial characterization and evaluation indicate that this new environmental chamber can provide high quality mechanism evaluation data for experiments with NO_x levels as low as 2 ppb, though the results indicate some problems with the gas-phase mechanism that need further study. Initial evaluation experiments for SOA formation, also carried out under dry conditions, indicate that the chamber can provide high quality secondary aerosol formation data at relatively low hydrocarbon concentrations.     

Temporal and spatial relationships in fine particle strong acidity, sulphate, PM1O, and PM2.5 across multiple canadian locations

The Canadian Acid Aerosol Measurement Program (CAAMP) was established in 1992 to gain a better understanding of the atmospheric behaviour of fine particle strong acidity (“acid aerosols”) and to facilitate an assessment of the potential health risks associated with acid aerosols and particles in general. During 1992. 1993 and 1994, annular denuder and filter measurements were taken at four sites in Ontario, two in Quebec, three in the Atlantic Provinces and one in the greater Vancouver area. Mean fine particle sulphate concentrations (SO₄²⁻) were highest in southern Ontario (annual average ranged from 40–70 nmol m⁻³), lowest at a site in the Vancouver area (average = 16 nmol m⁻³) and second lowest in rural Nova Scotia. However, mean fine particle strong acid concentrations (H⁺) were geographically different. The highest mean concentrations were at the east coast sites (annual average of up to 30 nmol m⁻³). Acidities were lower in areas where the fine particle acidity experienced greater neutralization from reaction with ammonia. This included the major urban centres (i.e. Toronto and Montréal) and areas with greater amounts of agricultural activity, as in rural southern Ontario. On average, ambient concentrations of fine and coarse particle mass were larger in the urban areas and also in areas where SO₄²⁻ levels were higher. All the particle components were episodic. However, compared to SO₄²⁻ and fine particles (PM_2.5 or PM_2.1, depending upon inlet design), episodes of H⁺ tended to be less frequent and of shorter duration, particularly in Ontario. Saint John, New Brunswick, had the highest mean annual H⁺ concentration, which was 30 nmol m⁻³. H⁺ episodes (24 h concentration > 100 nmol m⁻³) were also the most frequent at this location. The high levels in Saint John were partially due to local sulphur dioxide sources and heterogeneous chemistry occurring in fog, which, on average, led to a 50% enhancement in sulphate, relative to upwind conditions.There was a substantial amount of intersite correlation in the day to day variations in H⁺, SO₄²⁻ , PM_2.5 and PM₁₀ (fine + coarse particles) concentrations, which is due to the influence of synoptic-scale meteorology and the relatively long atmospheric lifetime of fine particles. Sulphate was the most regionally homogenous species. Pearson correlation coefficients comparing SO₄²⁻ between sites ranged from 0.6 to 0.9, depending on site separation and lag time. In many cases, particle episodes were observed to move across the entire eastern portion of Canada with about a two-day lag between the SO₄²⁻ levels in southern Ontario and in southern Nova Scotia.     

Experimental verification for real-time environmental emergency response system: WSPEEDI by European tracer experiment

Japan Atomic Energy Research Institute has developed an emergency response system WSPEEDI to forecast long-range atmospheric dispersions of radionuclides discharged into the atmosphere. The latest version of WSPEEDI consists of an atmospheric dynamic model MM5 for calculating meteorological fields and a particle random-walk model for atmospheric dispersion. The performance of WSPEEDI was evaluated by data obtained from a field tracer experiment over Europe (ETEX) in this paper. The model validation was done with respect to the following points: (1) the dependence of model accuracy on the temporal and spatial resolutions of the meteorological fields and (2) the superiority of an atmospheric dynamic model over a mass-consistent wind model. Regarding (1), it was shown that the calculation accuracy of the new version with high temporal resolution was improved, especially at the edge of the plume. Moreover, although the increase in horizontal spatial resolution of the old version had no substantial effect on the model performance, increase in horizontal resolution of the new version contributed to the significant improvement of the calculation accuracy. These results showed that the dynamically calculated meteorological field with the spatial resolution of the meso-β–γ scale greatly improved calculation accuracy.     

The distribution of the chlorinated solvents dichloromethane,perchloroethylene, and trichloroethylene in the global atmosphere

Dichloromethane, perchloroethylene, and trichloroethylene are commercially important chlorinated solvents whose health and environmental impacts are under scrutiny in the industrial world. Their distributions in the global atmosphere have been computed based on data from the Reactive Chlorine Emissions Inventory (RCEI) project using the Global Balance Environment (GLOBE) model, a 3-D radiative-dynamical-chemical model. Their atmospheric lifetimes, scaled to an observed methyl chloroform lifetime of 4.8 years, are 158 days, 105 days, and 4.3 days, respectively. They have strong interhemispheric gradients, with maximum zonal mean surface concentrations in the winter mid-latitude northern hemisphere of approximately 40 ppt, 9 ppt, and 2.5 ppt, respectively. Their spatial distributions show significant seasonal variability, and are sensitive to vertical mixing by cumulus convection and horizontal mixing by synoptic-scale turbulence. While the model interhemispheric exchange time (1.0 years) and computed atmospheric lifetimes are very sensitive to sub-grid scale diffusion, interhemispheric gradients of the chlorinated solvents are not. The simulated results suggest a greater importance for oceanic emissions of perchloroethylene and trichloroethylene than has previously been assumed.     

Atmospheric particulate matter and air quality in the Mediterranean: a review

This article synthesises the results obtained in several projects on atmospheric aerosol (particulate matter – PM) pollution developed during the last years in the Western Mediterranean. It focuses on particulate matter sources and the strategies for suitable monitoring in ambient air. The article has been structured in several sections that give response to the main questions that prompted these studies. After analysing the main PM features in the Mediterranean, a brief review of the main factors differentiating the particulate matter composition with respect to Central Europe is presented. Finally, the suitability of the different metrics or parameters for monitoring ambient air PM levels in different types of environments is discussed. Selected article from the 6th European Meeting on Environmental Chemistry, University of Belgrade, Serbia and Montenegro organized by Prof. Dr. Branimir Jovancicevic (www.research.plymouth.ac.uk/ace).     

大气污染预测预报研究

以排放到大气环境中的烟尘为例，进行大气污染预测预报，并利用保证率的概念表示预测的结果，为大气污染的预测预报工作提供了一种基本方法。     

大气环境中OH自由基测定

采用自旋捕集技术和电子自旋共振法结合测定大气环境中ＯＨ自由基，首先用自旋捕集剂将ＯＨ自由基捕集，生成比较稳定的自然旋加合物，，然后带回实验室处理测定，该法为开展大气光化学研究提供了一种采样方便，利于实测的方法，据３个采样点的实测结果表明，相对误差约为３５％，比文献所示结果略大。     

氨气敏电极法测定大气中氨

以Ｈ２ＳＯ４（０．０５ｍｏｌ／Ｌ）和ＮＨ３（１．００ｍｇ／Ｌ）的混合溶液作吸收液，采用气敏电极测定大气中氨，发挥了离子选择电极所具有的快速、灵敏及测定范围宽等优点，保证了大气中低浓度氨测定的准确性和可靠性。实验表明，该方法检测限为０．０１４～０．０１８ｍｇ／ｍ＾２，精密度约为１４．３％（相对标准偏差），回收率在９７％～１０２％之间，经６个月实验室验证的结果，无论是精密度的变异系数或回收率的置信系数