Assessment and optimisation of VOC mass transfer enhancement by advanced oxidation process in a compact wet scrubber

Dimethyl disulphide (DMDS) removal was investigated in a compact scrubber (hydraulic residence time ≈20 ms), composed of a wire mesh packing structure where liquid and gas flow at co-current and high gas superficial velocity (>12 m s⁻¹). In order to regenerate the scrubbing liquid and to maintain a driving force in the scrubber, ozone and hydrogen peroxide were added to water since they allow the generation of nonselective and highly reactive species, hydroxyl radicals HO. Three ways of reagent distribution were tested. The influence of several parameters (liquid flow rate(s), ozone flow rate, pH and reagent concentrations) was investigated. The best configuration was obtained when ozone is transferred in the scrubbing liquid before introduction at the top of the scrubber simultaneously with the hydrogen peroxide solution, allowing to generate hydroxyl radical in the scrubber. With this configuration, DMDS removal could be increased from 16% with water to 34% at the same gas and liquid flow rates in the scrubber showing the potentiality of advanced oxidation process.     

The behaviour of residual contaminants at a former station site,Antarctica

In 1994, New Zealand's only mainland Antarctic base, Vanda Station, was removed from the shores of Lake Vanda, in the McMurdo Dry Valleys region of southern Victoria Land, Antarctica. Residual chemical contamination of the station site has been identified, in the form of discrete fuel spills, locally elevated Pb, Zn, Ag and Cd concentrations in soil and elevated Cu, Ni, Co and phosphate concentrations in suprapermafrost fluids in a gully formerly used for domestic washing water disposal. Pathways for contaminant transfer to Lake Vanda, potential environmental impacts and specific remediation/monitoring options are considered. While some contaminants (particularly Zn) could be selectively leached from flooded soil, during a period of rising lake level, the small area of contaminated soils exposed and low level of contamination suggests that this would not adversely affect either shallow lake water quality or the growth of cyanobacteria. Phosphate-enhanced growth of the latte may, however, be a visible consequence of the minor contamination occurring at this site.     

Ground level ozone concentrations and its association with NOx and meteorological parameters in Kathmandu valley, Nepal

This paper summarizes the results of a yearlong continuous measurements of gaseous pollutants, NO, NO₂, NO_x and O₃ in the ambient air at Kathmandu valley. Measured concentration of the pollutants in study area is a function of time. NO, NO₂ and O₃ peak occurred in succession in presence of sunlight. At the time of maximum O₃ concentration most of the NO_x are utilized. The diurnal cycle of ground level ozone concentrations, revealed mid-day peak with lower nocturnal concentrations and inverse relationship exists between O₃ and NO_x, which are evidences of photochemical O₃ formation. The observed ground level ozone during monsoon is slight lower than the pre-monsoon value. Further, lack of rainfall and higher temperature, solar radiation in the pre-monsoon have given rise to the gradual build up of ozone and it is lowest during winter. Ground level ozone concentrations measured during bandha (general strike) and weekend are 19% and 13% higher than those measured during weekdays. The most effective ozone abatement strategy for Kathmandu Valley may be control of NO_x emissions.     

Formaldehyde in rainwater at Trombay, Mumbai: a coastal site in India

Formaldehyde was measured in rainwater samples collected at a residential area of Trombay, Mumbai (a coastal site in India). A mean concentration of 2.1 μmo1/1 and a range of 0.4-11.0 μmol/l were observed. The mean formaldehyde concentration in rainwater has increased from 1.2 μmol/l in 1979 by a factor of about two at this site.     

Contribution of anthropogenic pollutants to the increase of tropospheric ozone levels in the Oporto Metropolitan Area, Portugal since the 19th century

The main purpose of this study was to evaluate the contribution of anthropogenic pollutants to the increase of tropospheric ozone levels in the Oporto Metropolitan Area (Portugal) since the 19th century. The study was based on pre-industrial and recent data series, the results being analyzed according to the atmospheric chemistry. The treatment of ozone and meteorological data was performed by classical statistics and by time-series analysis. It was concluded that in the 19th century the ozone present in the troposphere was not of photochemical origin, being possible to consider the respective concentrations as reference values. For recent data a cycle of 8h for ozone concentrations could be related to traffic. Compared to the 19th century, the current concentrations were 147% higher (252% higher in May) due to the increased photochemical production associated with the increased anthropogenic emissions.     

Comparison of modelled and measured ozone concentrations and meteorology for a site in south-west Sweden: implications for ozone uptake calculations

Measurements of ground-level ozone concentrations and meteorology (temperature, vapour pressure deficit (VPD), solar radiation) at the monitoring site Ostad (south-west Sweden) were compared to data from the corresponding grid in the EMEP photo-oxidant model for 1997, 1999 and 2000. The influence of synoptic weather on the agreement between model and measurements was studied. Implications of differences between modelled and observed inputs for ozone flux calculations for wheat and potato were investigated. The EMEP model output of ozone, temperature and VPD correlated well with measurements during daytime. Deviations were larger during the night, especially in calm conditions, attributed to local climatological conditions at the monitoring site deviating from average conditions of the grid. These differences did not lead to significant differences in calculated ozone uptake, which was reproduced remarkably well. The uptake calculations were sensitive to errors in the ozone and temperature input data, especially when including a flux threshold.     

Characterisation of local and external contributions of atmospheric particulate matter at a background coastal site

This study applies a methodology for discriminating local and external contributions of atmospheric particulate matter (PM) at a rural background station in the North-western coast of Spain. The main inputs at the nearest scale have come from soil dust, marine aerosol and road traffic. At a larger scale, the highest contributions have come from fossil-fuel combustion sources, giving rise to relatively high ammonium sulphate background levels, mainly in summer. External contributions from long-range transport processes of African dust and nitrate have been detected. Morocco and Western Sahara have been identified as the main potential source regions of African dust, with a higher content of Al and Ti than other crustal components. Geographical areas from central and Eastern Europe have been identified as potential sources of particulate nitrate. The discrimination of the PM contribution from natural and anthropogenic sources at different geographical scales is a necessary information for establishing PM reduction strategies in specific areas.     

Chemical composition of aerosol size fractions at a coastal site in southwestern Italy: seasonal variability and transport influence

The present study focuses on the elemental characterization of fine and coarse particles collected at a coastal site of southwestern Italy, in a suburban area of the Calabria region. A chemical tracer analysis was carried out to identify the major emission sources influencing on the atmospheric aerosol levels. Size-resolved particulate samples were collected during three 2-week seasonal sampling campaigns: autumn (19 October to 2 November 2003), winter (19 January to 2 February 2004) and spring (26 April to 10 May 2004). Ambient concentrations of selected elements (Fe, Mn, Mg, Ca, V, Cu, Cr, Ni, Zn, Pb, and Cd) associated to fine and coarse size fractions were determined using atomic absorption spectrometry (AAS). The enrichment factor method was applied, suggesting a prevailing anthropogenic component for all the detected elements, with Fe, Mg, Mn, and Ca as exceptions. Trajectory sector analysis was used in order to discriminate the influence of different air mass origins and paths. Long-range transport from both the continental Europe and the Saharan region proved to be the main influencing factors. African dust outbreaks, whose occurrence frequency was greater during the autumn and spring seasonal monitoring periods, gave rise to a total of eight exceedances of the European Commission (EC) PM10 daily limit value as well as an increase in values of the crustal-derived elements (Fe, Mg, and Ca). Long-range transport from the heavily industrialized area of Central/Eastern Europe contributed to the high levels of Zn, Cd, and Pb that were recorded during the winter sampling campaign. Seasonal trend and comparison with measurements previously performed across the Mediterranean basin were also presented and discussed.     

Seasonal variation of polycyclic aromatic hydrocarbons (PAHs) emissions in China

A regression model based on the provincial energy consumption data was developed to calculate the monthly proportions of residential energy consumption compared to the total year volume. This model was also validated by comparing with some survey and statistical data. With this model, a PAHs emission inventory with seasonal variation was developed. The seasonal variations of different sources in different regions of China and the spatial distribution of the major sources in different seasons were also achieved. The PAHs emissions were larger in the winter than in the summer, with a difference of about 1.3-folds between the months with the largest and the smallest emissions. Residential solid fuel combustion dominated the pattern of seasonal variation with the winter-time emissions as much as 1.6 times as that in the summer, while the emissions from wild fires and open fire straw burning was mainly concentrated during the spring and summer.     

分光光度法测定降水中微量过氧化氢

研究了一种测定降水中微量过氧化氢的方法。在0.4～1.5mol／L磷酸介质中，过氧化氢与钒（V）及2－（3，5-二溴-2-吡啶偶氮）－5-二乙氨基苯酚（3,5-diBr-PADAP）反应形成一种组成比为1：1：1的蓝色三元配合物，其最大吸收波长为598nm，表现摩尔吸光系数为5.6×104L·mol-1·cm-1。过氧化氮量在2×10-7～1．3×10－5mol／L时服从比耳定律。方法简便，选择性较高，用于降水中微量过氧化氢的直接测定，结果令人满意。     

Ten years of atmospheric methane observations at a high elevation site in Western China

In this paper, the continuous (1994–2001) and discrete air sample (1991–2001) measurements of atmospheric CH₄ from the Waliguan Baseline Observatory located in western China (36°17′N, 100°54′E, 3816 m asl) are presented and characterized. The CH₄ time series show large episodic events on the order of 100 ppb throughout the year. During spring, a diurnal cycle with average amplitude of 7 ppb and a morning maximum and late afternoon minimum is observed. In winter, a diurnal cycle with average amplitude of 14 ppb is observed with an afternoon maximum and morning minimum. Unlike most terrestrial observational sites, no obvious diurnal patterns are present during the summer or autumn. A background data selection procedure was developed based on local horizontal and vertical winds. A selected hourly data set representative of “baseline” conditions was derived with approximately 50% of the valid hourly data. The range of CH₄ mixing ratios, annual means, annual increases and mean annual cycle at Waliguan during the 1992–2001 were derived from discrete and continuous data representative of “baseline” conditions and compared to air samples collected at other Northern Hemisphere sites. The range of CH₄ monthly means of 1746–1822 ppb, average annual means of 1786.7±10.8 ppb and mean annual increase of 4.5±4.2 ppb yr⁻¹ at Waliguan were inline with measurements from sites located between 30° and 60°N. There were variations observed in the CH₄ annual increase patterns at Waliguan that were slightly different from the global pattern. The mean CH₄ annual cycle at Waliguan shows an unusual pattern of two gentle peaks in summer and February along with two small valleys in early winter and spring and a mean peak-to-peak amplitude of 11 ppb, much smaller than amplitudes observed at most other mid- and high-northern latitude sites. The Waliguan CH₄ data are strongly influenced by continental Asian CH₄ emissions and provide key information for global atmospheric CH₄ models.     

Chemical composition and seasonal variation of acid deposition in Guangzhou, South China: comparison with precipitation in other major Chinese cities

With the aim of understanding the origin of acid rains in South China, we analyzed rainwaters collected from Guangzhou, China, between March 2005 and February 2006. The pH of rainwater collected during the monitoring period varied from 4.22 to 5.87; acid rain represented about 94% of total precipitation during this period. The rainwater was characterized by high concentrations of SO₄²⁻, NO₃⁻, Ca²⁺, and NH₄⁺. SO₄²⁻ and NO₃⁻, the main precursors of acid rain, were related to the combustion of coal and fertilizer use/traffic emissions, respectively. Ca²⁺ and NH₄⁺ act as neutralizers of acid, accounting for the decoupling between high SO₄²⁻ concentrations and relatively high pH in the Guangzhou precipitation. The acid rain in Guangzhou is most pronounced during spring and summer. A comparison with acid precipitation in other Chinese cities reveals a decreasing neutralization capacity from north to south, probably related to the role and origin of alkaline bases in precipitation.     

Occurrence, distribution and seasonal variation of antibiotics in the Huangpu River, Shanghai, China

Water samples were collected from 19 sampling sites along the Huangpu River in June and December 2009. The occurrence, distribution and seasonal variation of 22 antibiotics, including four tetracyclines, three chloramphenicols, two macrolides, six fluoroquinolones, six sulfonamides and trimethoprim were investigated. It was found that all 19 sampling sites were contaminated by antibiotics. Four antibiotics (sulfamerazine, norfloxacin, fleroxacin and sarafloxacin) were not detected. The detection frequencies of the other 18 antibiotics were in the range of 5.3-100%. The median concentrations of the detected antibiotics ranged from quantification limits to 36.71 ng L⁻¹ (tetracycline) in June and to 313.44 ng L⁻¹ (sulfamethazine) in December. The number of detected antibiotics and the overall antibiotic concentrations were higher in December than in June due to the different river flow conditions. Different dominant antibiotics were observed for each group of antibiotics between June and December. Higher total concentrations of veterinary antibiotics such as tetracyclines were observed in suburban sampling sites than in unban sites, indicating the role of livestock and agricultural activities as an important source of antibiotic contamination.     

The chemical composition of tropospheric aerosols and their contributing sources to a continental background site in northern Zimbabwe from 1994 to 2000

Atmospheric aerosols were collected in separate coarse (2–10 μm diameter) and fine (diameter less than 2 μm) size fractions at Rukomechi Research Station (16.1°S, 29.4°E), Zimbabwe, in the central part of southern Africa, from September 1994 to January 2000. The samples were analysed for the particulate mass (PM), black carbon, and 47 elements. The overall data set and the separate wet and dry season data sets were examined with absolute principal component analysis (APCA). Natural and anthropogenic aerosol sources were identified in both seasons, but the sources and their contributions to the total PM were found to vary between seasons and between size fractions. Crustal matter, sea salt (SS), a mixed biogenic (BIO) emission/biomass burning (BB) component, and a copper component were identified for the coarse aerosols during the wet season. APCA attributed 29% of the total wet season coarse PM to the mixed BIO/BB component, and 32% to SS. The copper component is likely due to the copper smelters in the Zambian Copperbelt. The dry season coarse PM originated from crustal matter, BB, BIO, and SS sources, with the major contribution (32%) coming from BB. Four components (crustal matter, BB, non-ferrous smelters, and SS) were identified for the fine particles for both the wet and dry seasons. The BB component provided the major contribution to the total fine PM, accounting for 44% and 79% in the wet and dry seasons, respectively. The relative contributions to the total PM (both fine and coarse) for all sources were greater in the dry season than the wet season, except for SS.     

Exposure of acid aerosol for schoolchildren in metropolitan Taipei

Metropolitan Taipei, which is located in the subtropical area, is characterized by high population and automobile densities. For convenience, most primary schools are located near major roads. This study explores the exposure of acid aerosols for schoolchildren in areas in Taipei with different traffic densities. Acid aerosols were collected by using a honeycomb denuder filter pack sampling system (HDS). Experimental results indicated that the air pollutants were significantly correlated with traffic densities. The ambient air NO₂, SO₂, HNO₃, NO₃⁻, SO₄²⁻, and aerosol acidity concentrations were 31.3 ppb, 4.7 ppb, 1.3 ppb, 1.9 μg m⁻³, 18.5 μg m⁻³, and 49.5 nmol m⁻³ in high traffic density areas, and 6.1 ppb, 1.8 ppb, 0.9 ppb, 0.7 μg m⁻³, 8.8 μg m⁻³ and 14.7 nmol m⁻³ in low traffic density areas. The exposure levels of acid aerosols for schoolchildren would be higher than the measurements because the sampling height was 5 m above the ground. The SO₂ levels were low (0.13–8.03 ppb) in the metropolitan Taipei. However, the SO₄²⁻ concentrations were relatively high, and might be attributed to natural emissions of sulfur-rich geothermal sources. The seasonal variations of acid aerosol concentrations were also observed. The high levels of acidic particles in spring time may be attributed to the Asian dust storm and low height of the mixture layer. We conclude that automobile contributed not only the primary pollutants but also the secondary acid aerosols through the photochemical reaction. Schoolchildren were exposed to twice the acid aerosol concentrations in high traffic density areas compared to those in low traffic density areas. The incidence of allergic rhinitis of schoolchildren in the high traffic density areas was the highest in spring time. Accompanied by high temperature variation and high levels of air pollution in spring, the health risk of schoolchildren had been observed.     

Evidence of singlet oxygen and hydroxyl radical formation in aqueous goethite suspension using spin-trapping electron paramagnetic resonance (EPR)

The generation of reactive species in an aqueous goethite suspension, under room light and aeration conditions, was investigated using the electron paramagnetic resonance (EPR) technique employing spin trap agents. The trap reagents, including 5,5-dimethylpyrroline N-oxide (DMPO) and 2,2,6,6-tetramethylpiperidine (TEMP), were used for the detection of OH radicals (OH) and singlet oxygen (¹O₂), respectively. On the addition of DMPO to the goethite suspended solution, a DMPO-OH adduct was formed, which was not decreased, even in the presence of the OH scavenger, mannitol. This result implied a false positive interpretation from the DMPO-OH EPR signal. In the presence of TEMP reagent, a TEMP-O signal was detected, which was completely inhibited in the presence of the singlet oxygen scavenger, sodium azide. With both DMPO-OH and TEMP-O radicals in the presence and absence of radical scavengers, singlet oxygen was observed to be the key species formed in the room-light sensitized goethite suspension. In the goethite/H₂O₂ system; however, both OH and singlet oxygen were generated, with significant portions of DMPO-OH resulting from both OH and singlet oxygen. In fact, the DMPO-OH resulting from OH should be carefully calculated by correcting for the amount of DMPO-OH due to singlet oxygen. This study reports, for the first time, that the goethite suspensions may also act as a natural sensitizer, such as fulvic acids, to form singlet oxygen.     

PM2.5–10, PM2.5 and associated water-soluble inorganic species at a coastal urban site in the metropolitan region of Rio de Janeiro

The concentrations of PM_2.5−10, PM_2.5 and associated water-soluble inorganic species (WSIS) were determined in a coastal site of the metropolitan region of Rio de Janeiro, Southeastern Brazil, from October 1998 to September 1999 (n=50). Samples were dissolved in water and analyzed for major inorganic ions. The mean (± standard deviation; median) concentrations of PM_2.5−10 and PM_2.5 were, respectively, 26 (± 16; 21) μg m⁻³ and 17 (± 13; 14) μg m⁻³. Their mean concentrations were 1.7–1.8 times higher in dry season (May–October) than in rainy season (November–April). The WSIS comprised, respectively, 34% and 28% of the PM_2.5−10 and PM_2.5 masses. Chloride, Na⁺ and Mg²⁺ were the predominant ions in PM_2.5−10, indicating a significant influence of sea-salt aerosols. In PM_2.5, SO₄²⁻ (∼97% nss-SO₄²⁻) and NH₄⁺ were the most abundant ions and their equivalent concentration ratio (SO₄²⁻/NH₄⁺ ∼1.0) suggests that they were present as (NH₄)₂SO₄ particles. The mean concentration of (NH₄)₂SO₄ was 3.4 μg m⁻³. The mean equivalent PM_2.5 NO₃⁻ concentration was eight times smaller than those of SO₄²⁻ and NH₄⁺. The PM_2.5 NO₃⁻ concentration in dry season was three times higher than in rainy season, probably due to reaction of NaCl (sea salt) with HNO₃ as a result of higher levels of NO_y during the dry season and/or reduced volatilization of NH₄NO₃ due to lower wintertime temperature. Chloride depletion was observed in both size ranges, although more pronouncely in PM_2.5.     

Spatial distribution and seasonal variation of atmospheric bulk deposition of polycyclic aromatic hydrocarbons in Beijing-Tianjin region, North China

Bulk deposition samples were collected in remote, rural village and urban areas of Beijing-Tianjin region, North China in spring, summer, fall and winter from 2007 to 2008. The annually averaged PAHs concentration and deposition flux were 11.81 ± 4.61 μg/g and 5.2 ± 3.89 μg/m²/day respectively. PHE and FLA had the highest deposition flux, accounting for 35.3% and 20.7% of total deposition flux, respectively. More exposure risk from deposition existed in the fall for the local inhabitants. In addition, the PAHs deposition flux in rural villages (3.91 μg/m²/day) and urban areas (8.28 μg/m²/day) was 3.8 and 9.1 times higher than in background area (0.82 μg/m²/day), respectively. This spatial variation of deposition fluxes of PAHs was related to the PAHs emission sources, local population density and air concentration of PAHs, and the PAHs emission sources alone can explain 36%, 49%, 21% and 30% of the spatial variation in spring, summer, fall and winter, respectively.