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Characteristics of gas–phase nitric acid and ammonium–nitrate– sulfate aerosol, and their gas–phase precursors in a suburban area in Cairo, Egypt
2013
Hassan, Salwa K. | El–Abssawy, Ahmed A. | Khoder, Mamdouh I.
Simultaneous measurements of gaseous SO2, NO2, HNO3, NH3 and particulate SO42–, NO3– and NH4+ were carried out in a suburban area in Cairo during summer 2009 and winter 2009–2010. PTFE membrane filters were used to collect particulate SO42–, NH4+ and NO3–, followed by the impregnated filter to collect HNO3. Colorimetric methods were used for determination of NO2, SO2, NH3, SO42–, NH4+ NO3–, and HNO3 levels. The mean concentrations of NO2, SO2 and NH3 were 75.0, 40.1 and 29.1 µg/m3 in winter and 54.1, 25.1 and 44.9 µg/m3 in summer, respectively. The daytime/nighttime concentration ratios were 1.3 and 1.2 for NO2, 1.3 and 1.2 for SO2 and 0.6, and 0.8 for NH3 during the winter and summer, respectively. The mean values of NH4+, SO42–, NO3–, HNO3 and total NO3– were 4.4, 19.0, 3.4, 1.1 and 4.5 µg/m3 in winter and 7.5, 28.0, 4.2, 3.1 and 7.3 µg/m3 in summer, respectively. The levels of NH4+, SO42–, NO3– and HNO3 were relatively higher in daytime than in nighttime. Sulfur conversion (Fs) and nitrogen conversion ratios (Fn) in summer were about 1.78 and 2.15 times higher than in winter, respectively. Fs and Fn were higher in daytime than in nighttime. Significant positive correlation was found between Fs and relative humidity. The positive correlation between Fn and relative humidity was insignificant. The correlation between the concentration of NH4+ and NO3– indicates that NO3– may be found in fine mode (NH4NO3) in winter and it may be present predominantly as a coarse mode, such as Ca(NO3)2, Mg(NO3)2 and NaNO3 in summer. The concentration of SO42– was significantly correlated with NH4+ concentration, suggesting neutralization by NH3 and indicating that the forms of (NH4)2SO4 and/or NH4HSO4 exist in the aerosol. The NH4+/SO42– molar ratio indicates that SO42– in aerosol may be present as (NH4)2SO4, (NH4)2SO4.CaSO4.2H2O and CaSO4.
Show more [+] Less [-]Spatial attribution of sulfate and dust aerosol sources in an urban area using receptor modeling coupled with Lagrangian trajectories
2013
Chalbot, Marie–Cecile | Lianou, Maria | Vei, Ino–Christina | Kotronarou, Anastasia | Kavouras, Ilias G.
PM10 and PM2.5 (particles with diameter less than 10 μm and 2.5 μm, respectively) aerosol samples were collected from 2002 to 2004 in Athens, Greece and analyzed for elements ranging from Na to Pb using X–ray fluorescence. Positive matrix factorization (PMF) was applied to identify and quantify the types of PM10 and PM2.5 sources. The agreement between calculated and measured particle mass concentrations was very good for both aerosol fractions. Mineral soil, road dust and sea salt particles were the most significant types of coarse particles (PM10–2.5) while their contributions to PM2.5 fraction were minimal. Secondary sulfate, diesel particles from shipping and other oil combustion activities and primary traffic exhausts were determined as the most important types of PM2.5 sources. The analysis of normalized average air mass residence times showed weak seasonal patterns on the pathways of air masses prior to their arrival in Athens. Using trajectory regression analysis, the four adjacent regions (less than 500 km) accounted for the largest fraction of fine sulfate and diesel particles. On the contrary, shipping emissions and neutralization by sea salt may explain the high contributions of the regions covering the Mediterranean Sea and Dardanelle straights. The four adjacent regions and central Europe accounted for most of road and mineral dust particles. The transport from northern Africa over Mediterranean Sea also appeared to influence the mineral dust particles.
Show more [+] Less [-]Acid Mine Drainage Treatment Assisted by Lignite-Derived Humic Substances : Metal Removal and Speciation Modelling
2013
Olds, William E. | Tsang, Daniel C. W. | Weber, Paul
Acid mine drainage (AMD) generated by some coal mines in New Zealand is currently treated by the addition of alkaline reagents which neutralize acidity, triggering the precipitation of dissolved metals as insoluble hydroxides. Some trace metals (Ni, Zn, Cu, Cd, and Pb) are discharged into receiving water bodies due to incomplete hydroxide precipitation at circum-neutral pH. This study investigated the incorporation of lignite-derived humic substances (HS) for metal complexation and removal during AMD treatment by Ca(OH)₂ and CaCO₃ neutralization. For Ca(OH)₂ neutralization, addition of HS (regardless of dosing sequence) enhanced the removal of Zn, Cu, and Cd, probably due to the incorporation of metal–humate complex into settling flocs (via aggregation, co-precipitation, and adsorption) that were subsequently removed by sedimentation. However, additional removal of Ni and Pb was statistically indeterminate, which was ascribed to the low complexation affinity of Ni and high removal of Pb by adsorption onto Fe/Al hydroxides. Conversely, for CaCO₃ neutralization, addition of HS only marginally enhanced Cd removal, with the removal of metals probably dominated by adsorption onto the abundant undissolved calcite. Equilibrium speciation modelling showed that about 25% and 38% of the remaining Cu and Pb in the treated AMD were complexed with HS, while only 5% of remaining Cd and less than 1 wt% of remaining Ni and Zn were organically complexed. In the AMD-receiving water bodies, about 20 mg l⁻¹ of HS would be required for complete complexation (>95%) of Cu and Pb and 50 mg l⁻¹ for Cd, whereas Zn and Ni complexation would not occur at natural stream HS concentrations.
Show more [+] Less [-]Wet precipitation chemistry at a high-altitude site (3,326 m a.s.l.) in the southeastern Tibetan Plateau
2013
Liu, Bin | Kang, Shichang | Sun, Jimin | Zhang, Yulan | Xu, Ri | Wang, Yongjie | Liu, Yongwen | Cong, Zhiyuan
This paper presents the results of wet precipitation chemistry from September 2009 to August 2010 at a high-altitude forest site in the southeastern Tibetan Plateau (TP). The alkaline wet precipitation, with pH ranging from 6.25 to 9.27, was attributed to the neutralization of dust in the atmosphere. Wet deposition levels of major ions and trace elements were generally comparable with other alpine and remote sites around the world. However, the apparently greater contents/fluxes of trace elements (V, Co, Ni, Cu, Zn, and Cd), compared to those in central and southern TP and pristine sites of the world, reflected potential anthropogenic disturbances. The almost equal mole concentrations and perfect linear relationships of Na⁺and Cl⁻suggested significant sea-salts sources, and was confirmed by calculating diverse sources. Crust mineral dust was responsible for a minor fraction of the chemical components (less than 15 %) except Al and Fe, while most species (without Na⁺, Cl⁻, Mg²⁺, Al, and Fe) arose mainly from anthropogenic activities. High values of as-K⁺(anthropogenic sources potassium), as-SO₄²⁻, and as-NO₃⁻observed in winter and spring demonstrated the great effects of biomass burning and fossil fuel combustion in these seasons, which coincided with haze layer outburst in South Asia. Atmospheric circulation exerted significant influences on the chemical components in wet deposition. Marine air masses mainly originating from the Bay of Bengal provided a large number of sea salts to the chemical composition, while trace elements during summer monsoon seasons were greatly affected by industrial emissions from South Asia. The flux of wet deposition was 1.12 kg N ha⁻¹ year⁻¹for NH₄⁺–N and 0.29 kg N ha⁻¹ year⁻¹for NO₃⁻–N. The total atmospheric deposition of N was estimated to be 6.41 kg N ha⁻¹ year⁻¹, implying potential impacts on the alpine ecosystem in this region.
Show more [+] Less [-]Neutralization/prevention of acid rock drainage using mixtures of alkaline by-products and sulfidic mine wastes
2013
Alakangas, Lena | Andersson, Elin | Mueller, Seth
Backfilling of open pit with sulfidic waste rock followed by inundation is a common method for reducing sulfide oxidation after mine closure. This approach can be complemented by mixing the waste rock with alkaline materials from pulp and steel mills to increase the system's neutralization potential. Leachates from 1 m(3) tanks containing sulfide-rich (ca.30 wt %) waste rock formed under dry and water saturated conditions under laboratory conditions were characterized and compared to those formed from mixtures. The waste rock leachate produced an acidic leachate (pH < 2) with high concentrations of As (65 mg/L), Cu (6 mg/L), and Zn (150 mg/L) after 258 days. The leachate from water-saturated waste rock had lower concentrations of As and Cu (<2 μg/L), Pb and Zn (20 μg/L and 5 mg/L), respectively, and its pH was around 6. Crushed (<6 mm) waste rock mixed with different fractions (1-5 wt %) of green liquid dregs, fly ash, mesa lime, and argon oxygen decarburization (AOD) slag was leached on a small scale for 65 day, and showed near-neutral pH values, except for mixtures of waste rock with AOD slag and fly ash (5 % w/w) which were more basic (pH > 9). The decrease of elemental concentration in the leachate was most pronounced for Pb and Zn, while Al and S were relatively high. Overall, the results obtained were promising and suggest that alkaline by-products could be useful additives for minimizing ARD formation.
Show more [+] Less [-]Mineralogical study and leaching behavior of a stabilized harbor sediment with hydraulic binder
2013
Chatain, Vincent | Benzaazoua, Mostafa | Loustau Cazalet, Marie | Bouzahzah, Hassan | Delolme, Cécile | Gautier, Mathieu | Blanc, Denise | de Brauer, Christine
The environmental assessment of potential effects of contaminated harbor sediments stabilized with hydraulic binders and the determination of remediation endpoints require the determination of pollutants leaching potentials. Moreover, little information about the speciation and mobility of inorganic contaminants in these specific solid matrices is available in the literature. The objective of this paper is to investigate the relationship between mineralogy and leachability of contaminants (copper, lead, and zinc) present in a French harbor sediment stabilized with quicklime and Portland cement. Batch equilibrium leaching tests at various pH, chemical analysis of leachates, and mineralogical studies (X-ray diffraction, scanning electron microscopy–energy dispersive spectroscopy, and diffuse reflectance infrared Fourier transform) have been combined in the present investigation. The acid neutralization capacity of the stabilized matrix studied is first controlled by the dissolution of portlandite (pH ~12), followed by the dissolution of C–S–H (pH ~11) and the dissolution of ettringite (pH ~10). Finally, a very high buffering capacity of this stabilized sediment is observed for pH values around 6. This equilibrium is mainly controlled by the dissolution of iron sulfides and carbonate minerals. Consequently, the mobilization of inorganic contaminants as a function of pH remains very low (<0.1 wt%) for pH values above 6 and significantly increases for pH below these values. This research confirms the importance of a combined methodology for the intrinsic characterization of potential mobilization of contaminants in a stabilized sediment and for a better understanding of geochemical processes that affect contaminant fate, transformation, and transport in the subsurface environment.
Show more [+] Less [-]Removal possibilities of colloidal chromium (III) oxide from water using polyacrylic acid
2013
Wiśniewska, Małgorzata | Szewczuk-Karpisz, Katarzyna
The lack of water is the most serious threat to humanity that leads to more efficient water and sewage treatment. Currently, many scientists are looking for new coagulants, flocculants and physicochemical methods allowing for sufficient removal of pollutants from water. The presence of various types of pigments, including chromium (III) oxide, poses the major problem. Even small amounts of these substances inhibit life processes in water. In this paper, the stability of Cr₂O₃ suspension in the absence and the presence of polyacrylic acid (PAA) was determined. To explain the changes in the system stability, the adsorption and electrokinetic measurements were performed. The chromium (III) oxide suspension not containing PAA is the most stable at pH = 3. Under these conditions, each positively charged solid particle is surrounded by a negatively charged diffusion layer which protects from particle collision and aggregates formation (electrostatic stabilization). In turn, the Cr₂O₃ suspension containing the PAA is most unstable also at pH = 3. In this case, the polymer causes destabilization of the colloidal suspension, which results from charge neutralization of solid particles by adsorbed PAA.
Show more [+] Less [-]Performance of a field-scale permeable reactive barrier based on organic substrate and zero-valent iron for in situ remediation of acid mine drainage
2013
Gibert, Oriol | Cortina, Jose Luis | De Pablo, Joan | Ayora, Carlos
A permeable reactive barrier (PRB) was installed in Aznalcóllar (Spain) in order to rehabilitate the Agrio aquifer groundwater severely contaminated with acid mine drainage after a serious mining accident. The filling material of the PRB consisted of a mixture of calcite, vegetal compost and, locally, Fe(0) and sewage sludge. Among the successes of the PRB are the continuous neutralisation of pH and the removal of metals from groundwater within the PRB (removals of >95 %). Among the shortcomings are the improper PRB design due to the complexity of the internal structure of the Agrio alluvial deposits (which resulted in an inefficient capture of the contaminated plume), the poor degradability of the compost used and the short residence time within the PRB (which hindered a complete sulphate reduction), the clogging of a section of the PRB and the heterogeneities of the filling material (which resulted in preferential flows within the PRB). Undoubtedly, it is only through accumulated experience at field-scale systems that the potentials and limits of the PRB technology can be determined.
Show more [+] Less [-]Geochemical and mineralogical characterization of a neutral, low-sulfide/high-carbonate tailings impoundment, Markušovce, eastern Slovakia
2013
Hiller, Edgar | Petrák, Marián | Tóth, Roman | Lalinská-Voleková, Bronislava | Jurkovič, Ľubomír | Kučerová, Gabriela | Radková, Anežka | Šottník, Peter | Vozár, Jaroslav
Tailings deposits generated from mining activities represent a potential risk for the aquatic environment through the release of potentially toxic metals and metalloids occurring in a variety of minerals present in the tailings. Physicochemical and mineralogical characteristics of tailings such as total concentrations of chemical elements, pH, ratio of acid-producing to acid-neutralizing minerals, and primary and secondary mineral phases are very important factors that control the actual release of potentially toxic metals and metalloids from the tailings to the environment. The aims of this study are the determination of geochemical and mineralogical characteristics of tailings deposited in voluminous impoundment situated near the village of Markušovce (eastern Slovakia) and identification of the processes controlling the mobility of selected toxic metals (Cu, Hg) and metalloids (As, Sb). The studied tailings have unique features in comparison with the other tailings investigated previously because of the specific mineral assemblage primarily consisting of barite, siderite, quartz, and minor sulfides. To meet the aims, samples of the tailings were collected from 3 boreholes and 15 excavated pits and subjected to bulk geochemical analyses (i.e., determination of chemical composition, pH, Eh, acid generation, and neutralization potentials) combined with detailed mineralogical characterization using optical microscopy, X-ray diffraction (XRD), electron microprobe analysis (EMPA), and micro-X-ray diffraction (μ-XRD). Additionally, the geochemical and mineralogical factors controlling the transfer of potentially toxic elements from tailings to waters were also determined using short-term batch test (European norm EN 12457), sampling of drainage waters and speciation–equilibrium calculations performed with PHREEQC. The tailings mineral assemblage consists of siderite, barite, quartz, and dolomite. Sulfide minerals constitute only a minor proportion of the tailings mineral assemblage and their occurrence follows the order: chalcopyrite > pyrite > tetrahedrite > arsenopyrite. The mineralogical composition of the tailings corresponds well to the primary mineralization mined. The neutralization capacity of the tailings is high, as confirmed by the values of neutralization potential to acid generation potential ratio, ranging from 6.7 to 63.9, and neutral to slightly alkaline pH of the tailings (paste pH 7.16–8.12) and the waters (pH 7.00–8.52). This is explained by abundant occurrence of carbonate minerals in the tailings, which readily neutralize the acidity generated by sulfide oxidation. The total solid-phase concentrations of metal(loid)s decrease as Cu > Sb > Hg > As and reflect the proportions of sulfides present in the tailings. Sulfide oxidation generally extends to a depth of 2 m. μ-XRD and EMPA were used to study secondary products developed on the surface of sulfide minerals and within the tailings. The main secondary minerals identified are goethite and X-ray amorphous Fe oxyhydroxides and their occurrence decreases with increasing tailings depth. Secondary Fe phases are found as mineral coatings or individual grains and retain relatively high amounts of metal(loid)s (up to 57.6 wt% Cu, 1.60 wt% Hg, 23.8 wt% As, and 2.37 wt% Sb). Based on batch leaching tests and lysimeter results, the mobility of potentially toxic elements in the tailings is low. The limited mobility of metals and metalloids is due to their retention by Fe oxyhydroxides and low solubilities of metal(loid)-bearing sulfides. The observations are consistent with PHREEQC calculations, which predict the precipitation of Fe oxyhydroxides as the main solubility-controlling mineral phases for As, Cu, Hg, and Sb. Waters discharging from tailings impoundment are characterized by a neutral to slightly alkaline pH (7.52–7.96) and low concentrations of dissolved metal(loid)s (<5–7.0 μg/L Cu, <0.1–0.3 μg/L Hg, 5.0–16 μg/L As, and 5.0–43 μg/L Sb). Primary factors influencing aqueous chemistry at the site are mutual processes of sulfide oxidation and carbonate dissolution as well as precipitation reactions and sorption onto hydrous ferric oxides abundantly present at the discharge of the impoundment waters. The results of the study show that, presently, there are no threats of acid mine drainage formation at the site and significant contamination of natural aquatic ecosystem in the close vicinity of the tailings impoundment.
Show more [+] Less [-]Co-treatment of acid mine drainage with municipal wastewater: performance evaluation
2013
Hughes, Theresa A. | Gray, N. F.
Co-treatment of acid mine drainage (AMD) with municipal wastewater (MWW) using the activated sludge process is a novel treatment technology offering potential savings over alternative systems in materials, proprietary chemicals and energy inputs. The impacts of AMD on laboratory-scale activated sludge units (plug-flow and sequencing batch reactors) treating synthetic MWW were investigated. Synthetic AMD containing Al, Cu, Fe, Mn, Pb, Zn and SO4 at a range of concentrations and pH values was formulated to simulate three possible co-treatment processes, i.e., (1) adding raw AMD to the activated sludge aeration tank, (2) pre-treating AMD prior to adding to the aeration tank by mixing with digested sludge and (3) pre-treating AMD by mixing with screened MWW. Continuous AMD loading to the activated sludge reactors during co-treatment did not cause a significant decrease in chemical oxygen demand (COD), 5-day biochemical oxygen demand, or total organic carbon removal; average COD removal rates ranged from 87-93 %. Enhanced phosphate removal was observed in reactors loaded with Fe- and Al-rich AMD, with final effluent TP concentrations <2 mg/L. Removal rates for dissolved Al, Cu, Fe and Pb were 52-84 %, 47-61 %, 74-86 % and 100 %, respectively, in both systems. Manganese and Zn removal were strongly linked to acidity; removal from net-acidic AMD was <10 % for both metals, whereas removal from circum-neutral AMD averaged 93-95 % for Mn and 58-90 % for Zn. Pre-mixing with screened MWW was the best process option in terms of AMD neutralization and metal removal. However, significant MWW alkalinity was consumed, suggesting an alkali supplement may be necessary.
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