The coagulation of combined sewer overflow (CSO) was investigated by jar-testing with two commercial coagulants, a ferric chloride solution (CLARFER) and a polyaluminium chloride (WAC HB). CSO samples were collected as a function of time during various wet-weather events from the inlet of Boudonville retention basin, Nancy, France. Jar-tests showed that an efficient turbidity removal can be achieved with both coagulants, though lower optimum dosages and higher re-stabilization concentrations were obtained with the aluminum-based coagulant. Optimum turbidity removal also yielded effective heavy metal elimination. However, the evolution with coagulant dosage of Cu, Zn, Pb, Cr, soluble and suspended solids contents followed various patterns. The removal behaviors can be explained by a selective aggregation of heavy metal carriers present in CSO and a specific interaction between hydrolyzed coagulant species and soluble metals. Stoichiometric relationships were established between optimal coagulant concentration, range of optimal dosing, and CSO conductivity, thus providing useful guidelines to adjust the coagulant demand during the course of CSO events.
The nature of coagulant species formed in the system ferric chloride/municipal sewage was explored with Transmission Electron Microscopy coupled with Energy Dispersive X-ray Spectroscopy (TEM-EDXS) and Fe K-edge X-ray Absorption spectroscopy. Jar-test data combined with chemical analysis of supernatant (dissolved organic carbon, iron, and phosphorus) and Fourier-Transform-Infrared spectroscopy (FTIR) of freeze-dried sediment, provided a detailed description of sewage clarification. The results showed that the nature of coagulant species evolves with Fe concentration. Up to the optimum turbidity removal, mainly iron dimers linked with one phosphate anion are detected. At higher dosages, polymers of hydrolyzed Fe appear even though PO(4) still participates in the formation of coagulant species. TEM observation of freeze-dried sediments corroborates such an evolution of Fe speciation. EDXS analyses reveal that minute amounts of sulfur, silicon, aluminum, and calcium, are associated with the coagulant species. Even though the coagulant species change with Fe concentration, the destabilization mechanism, inferred from electrophoretic mobility of aggregates and the evolution of floc size under cyclic changes of stirring conditions, is equivalent with a charge neutralization of sewage colloids in the whole range of coagulant concentration.
The nature of trace element carriers contained in sewage and combined sewer overflow (CSO) was investigated by TEM-EDX-Electron diffraction and SEM-EDX. During dry weather, chalcophile elements were found to accumulate in sewer sediments as early diagenetic sulfide phases. The sulfurization of some metal alloys was also evidenced. Other heavy metal carriers detected in sewage include metal alloys, some iron oxihydroxide phases and neoformed phosphate minerals such as anapaite. During rain events, the detailed characterization of individual mineral species allowed to differentiate the contributions from various specific sources. Metal plating particles, barite from automobile brake, or rare earth oxides from catalytic exhaust pipes, originate from road runoff, whereas PbSn alloys and lead carbonates are attributed to zinc-works from roofs and paint from building siding. Soil contribution can be traced by the presence of clay minerals, iron oxihydroxides, zircons and rare earth phosphates. However, the most abundant heavy metal carriers in CSO samples were the sulfide particles eroded from sewer sediments. The evolution of relative abundances of trace element carriers during a single storm event, suggests that the pollution due to the "first flush" effect principally results from the sewer stock of sulfides and previously deposited metal alloys, rather than from urban surface runoff.
Submerged sediment cores were collected upstream of a dam in the Orne River, northeastern France. This dam was built in the context of steelmaking to constitute a water reservoir for blast furnace cooling and wet cleaning of furnace smokes. The dam also enhanced sediment deposition in the upstream zone. This study was performed to unravel the contamination status of sediments and to evidence possible contribution sources. The sediment layers were analyzed for water content, grain size, chemical composition, crystalline phases at a bulk scale and poorly crystalline and amorphous phases at a sub-micrometer scale. Visual aspect, texture, color, and chemical and mineralogical analyses showed that the settled sediments were mainly composed of fine black matter, certainly comprising steelmaking by-products. Those materials were highly enriched with Fe, Zn, Pb and other trace metals, except for a relatively thin layer of surficial sediments that had settled more recently. Bulk mineralogy revealed crystalline iron minerals, such as magnetite, goethite, wuestite and pyrite, in the deep layers of the sediment cores. Furthermore, microscopic investigations evidenced the presence of ferrospheres, goethite nanoparticles and newly formed Fe-aluminosilicates; all originating from the former steelmaking facilities. The variation of iron mineralogy, combined with specific chemical profiles and other sediment features, demonstrate the different contributions that constitute the sediment deposit. Furthermore, chemical and mineralogical features of goethite and Fe-aluminosilicates could be used as a fingerprint for such contaminated sediments.
Phosphate fertilizers represent a major source of trace metal contaminants in agricultural soils. To predict the inputs and the fate of trace metals in soils of the eastern Mediterranean region, a speciation study was conducted using a total of 44 phosphate fertilizers commercialized in the area. The contents in major anions and potentially toxic metals (Zn, Pb, Cd, and Cu) were determined using atomic absorption spectrometry (AAS) and X‐ray fluorescence spectrometry (XRF). The nature of mineral phases in the fertilizer was characterized using X‐ray diffraction and Fourier transform infrared spectrometry. The results show that sulfates are the main Cd‐bearing phases when present in the P‐fertilizer. The contents in Zn and Pb were linearly related, whereas the levels of Sb, Ag, Pd, Nb, Mo, and P2O5 were strongly correlated to each other. The annual average inputs of Zn, Cu, Pb, and Cd were calculated to be 922, 124, 26, and 6 g/ha per year, respectively. Even though such inputs comply with the maximal metals concentrations authorized in temperate countries, an accumulation of those metals in the typical arid and alkaline soils of the eastern Mediterranean countries is expected.
Two divalent cation-based coagulants, magnesium chloride and manganese chloride, were used to treat synthetic textile wastewaters containing the azo-dye pigment Levafix Brilliant Blue EBRA. The jar-tests were performed in the presence or absence of auxiliary dyeing chemicals. They proved that (i) both divalent cation-based coagulants were effective in the treatment of those alkaline effluents, (ii) better performances in terms of color removal, residual turbidity, and settled volume, were achieved with manganese chloride, and (iii) the presence of dyeing auxiliaries significantly increases the required coagulant demand for treating the textile effluent. The dye removal mechanisms were investigated by combining observations of freeze-dried sediments with transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy and selected area electron diffraction, Fourier transform infrared spectroscopy, adsorption experiments, and aggregates size measurements with a laser sizer under cyclic shear conditions. The results show that brucite (Mg(OH)(2)) particles are formed when applying MgCl(2) to the textile wastewaters, whereas a mixture of feitknechite (β-MnOOH) and hausmannite (Mn(3)O(4)) is obtained when using MnCl(2). More poorly crystallized particles are formed in presence of auxiliary dyeing chemicals. The adsorption experiments suggested that the azo-dye pigment adsorbs onto the surface of precipitating phases, whereas the aggregation dynamics indicated that a charge-neutralization mechanism underlies the formation of aggregates. The dye removal is then consistent with a precipitation/adsorption mechanism.
This study delineates the physical, chemical, and biological effects resulting from anthropogenic and endogenic activities in a sensitive dammed reservoir situated in a semi-arid region. The reservoir is characterized by two major flow regimes: a wet fill hydrologic regime and a dry spill one. A seasonal sampling campaign was carried out over a period of 2 years (2011-2013) where water samples were collected across the water column and from piezometers just outside the perimeter of the reservoir. Similarly, sediments were collected from the corresponding areas beneath the water column. The water samples were analyzed for environmental isotopic ratios, elemental composition, and physical, biological and chemical parameters, whereas the sediment and algal samples were subjected to physical, mineralogical, spectroscopic, and microscopic analyses. This investigation indicated that the dam had resulted in the alteration of the biogeochemical cycle of nutrients as well as the degradation of the sediment and water quality. The hydrological and biogeochemical processes were found to induce vertical downward transport of chemicals towards the fine grained calcareous sediments during the fill mode, whereas the sediments acted as a source of a chemical flux upward through the water column and downward towards the groundwater during the spill mode. The geomorphological characteristics of the reservoir enhanced the strong hydrological connectivity between the surface water and the groundwater where the reservoir responded quickly to natural and anthropogenic changes in the upper watershed. The water and sediments in the sensitive spill mode were of poor quality and should receive more attention due to the potential hazard for the associated hydro-project and the sustainability of the agricultural soil in the long term. Thus, a safe water and sediment management plan should be implemented in order to improve the dam functionality and to safeguard the precious water resources.
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