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Geochemical Evidences for the Sources of the Cr(VI) Contamination

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Geochemical Evidences for the Sources of the Cr(VI) Contamination European Water 41: 23-34, 2013. © 2013 E.W. Publications Geochemical evidences for the sources of the Cr(VI) contamination in groundwater in central Euboea and Assopos-Thiva basins, Greece: Natural versus anthropogenic origin I. Megremi, Ch. Vasilatos, A. Atsarou, Ch. Theodoratou, M. Economou-Eliopoulos and I. Mitsis Faculty of Geology and Geoenvironment, University of Athens e-mail: [email protected] Abstract: Analytical data of the water chemistry in central Euboea and the Assopos-Thiva basins, Greece, has revealed high concentrations of Cr(total) and Cr(VI) exceeding, sometimes, the Greek and the EU drinking water maximum acceptable level (50g/L). The case of groundwater contamination in central Euboea related mainly to natural processes (rocks and ores) was compared with that of the neighboring area of Assopos and Thiva basins (areas of Avlida, Thiva, Oropos, Avlona) characterized by widespread industrial activity. The concentrations of Cr(VI) detected in several groundwater samples, ranged from < 2 (below detection limit) to 360μg/L in central Euboea and from < 2 to 185μg/L in Assopos-Thiva basins, Eastern Sterea Hellas, Greece. The ratio of Cr(VI) to Cr(total) ranging from 0,8 to 1 and the excellent correlation (r2= 0.98, p=0.000) between Cr(VI) and Cr(total), indicated that hexavalent chromium is the predominant form of dissolved chromium in groundwater of all areas studied, with a pH near to neutral. The concentrations of other elements in the majority of the analyzed water samples in all areas were below the permissible limits for drinking water. Water samples from Assopos-Thiva basins were characterized by lower Si contents compared to those from central Euboea. Based on Na, Ca, Mg, Si and Cr(VI) content of the water samples, several discrimination diagrams have been proposed for the identification of their origin. According to their Na, Ca, Mg, Si and Cr contents, the water samples from central Euboea could be distinguished to a) those influenced by the sea water, having high Na and B concentrations, b) those with lower Na, an average of Cr(total) equal to 25μg/L and Mg/Si ratio approximately to 2.3 and c) those with very high Cr(total) values, up to 360 μg/L. The hydrochemical differences of the water samples from Euboea, have been attributed to natural processes for the (a) and (b) cases, whilst in the case (c) the chromium contamination in groundwater was probably associated with human activities. In the extended area of Assopos-Thiva basins (areas of Avlida, Thiva, Schimatari, Oropos, Avlona) the groundwater samples on the basis of their concentration in Cr(total) were classified into three groups: Group A with Cr(total) concentrations lower than 2μg/L, Group B with Cr(total) concentrations ranging from 2 to 50μg/L and Group C with Cr(total) concentrations higher than 50μg/L. The plots of Cr versus Mg/Ca, Mg/Na versus Ca/Na, B versus Si/(Si+Na) and Mg/Si versus Ca/Si ratios revealed a significant degree of salinization and a wide variation in the Cr content. The spatial association of wells with Cr < 2μg/L and those with high Cr concentrations in the whole region of the Assopos-Thiva basins and central Euboea may be related with the depth of the aquifers. The highest values of Cr(VI), recorded in shallow (alluvial) aquifers, were probably due to the circulation of water in an oxidizing environment, that has been affected by anthropogenic activities. Keywords: chromium speciation, toxic metals, groundwater contamination, hydrogeochemistry 1. INTRODUCTION The higher mobility and toxicity of Cr(VI) compared to Cr(III) for biological systems has been extensively documented, due to its strong oxidizing potential (Kotas and Stasicka, 2000, Bielicka et. al., 2005, Wise S. and Wise J., 2012). The speciation and the transport of chromium within the terrestrial and water systems are governed by pH and redox conditions. Three subsystems had been distinguished, considering chromium transport in natural waters: river, lake and ocean water (Bielicka et. al., 2005). In the neutral and alkaline pH conditions the Cr(III) in water has low solubility and readily precipitates as Cr(OH)3(s) or mixed Cr-Fe hydroxides colloids in pH values greater than 4 (Schlautman and Ihnsup, 2001). The Cr(III) ions have a tendency to bind with the suspended solids and thus are detectable in the sediment (Kotas and Stasicka, 2000). Trivalent chromium is the most stable oxidation state of chromium. In the pH range of natural water (6.5 to 2- - 2- 8.5), Cr(VI) exists as chromate CrO4 , bichromate HCrO4 and dichromate Cr2O7 ions. These ions 24 I. Megremi et al. form several Cr(VI) compounds, which are relatively soluble and thus mobile in the environment. The Cr(VI) in groundwater can be reduced to Cr(III) in low pH, under reducing conditions In contrast, Cr(III), is an essential nutrient required for normal glucose and lipid metabolism in human body, as it enhances the effect of insulin. Chromium enters the human body through inhalation, ingestion and dermal absorption. The general population is exposed to chromium through ingestion from food and water, while occupational exposure occurs predominantly through inhalation and dermal contact. Although Cr(VI) is a known carcinogen through inhalation, the WHO, EU and US agencies have not yet classified it in terms of ingestion (WHO, 2003). Due to the toxicity of hexavalent chromium, the California Office of Environmental Health Hazard Assessment (ΟΕΗΗΑ) developed a Public Health Goal (PHG) for hexavalent chromium of 0,02 μg/L in drinking water (OEHHA, 2011). In all other U.S. states the Federal drinking water standard for total chromium is 100μg/L(WHO, 2003). However, that situation may change as a result of recent research showing elevated levels of Cr(VI) in the drinking water supplies of 31 different cities across the United States. The U.S. Environmental Protection Agency had planned to establish federal limits for Cr(VI) in drinking water in 2012, following the completion of its own risk assessment (OEHHA, 2011). Italy has regulated a maximum permissible level of Cr(VI) in drinking water at 5 μg/L (Fantoni et. al., 2002, Stepek, 2002). Most countries, including in the European Union, have currently regulated the limit of 50μg/L for total chromium in drinking water (EC, 1998) which assumes a mixture of hexavalant chromium and trivalent chromium. Greece has adopted the above limit [EC, 1998 Council Directive (98/83/EC)]. Hexavalent chromium and its compounds can originate in the aqueous environment from both anthropogenic (industry wastes and emissions, combustion processes e.t.c.) and natural sources (weathering of chromium bearing minerals). Numerous studies of naturally occurring aqueous Cr(VI) at concentrations up to 73μg/L have been reported in ground and surface waters from New Caledonia, California, Italy and Mexico, associated mainly with serpentine soils and ultramafic rocks (Ball and Izbicki, 2004, Oze et al., 2007, Izbicki et al., 2008, Wise S. and Wise J., 2012). Given that chromium is a major trace element in both serpentinized ultramafic ophiolitic rocks and Ni-laterites and extended massive serpentinized ultramafic ophiolitic formations and large Ni- laterite deposits are located in the central part of Greece (Lokris and Euboea), (Katsikatsos et. al., 1986, Valeton et al., 1987, Eliopoulos and Economou-Eliopoulos, 2000), where previous analytical data had shown significant (several tens of μg/L) Cr(total) concentrations (Megremi 2010), the area of central Euboea had been selected as a case of chromium bearing natural water related to natural processes. This study is a compilation of geochemical data on the Cr species from central Euboea (Megremi et al., 2012), and neighbouring Assopos-Thiva basins (Atsarou and Economou-Eliopoulos, 2012, Theodoratou and Economou-Eliopoulos, 2012) presented at the International Conference Protection and Restoration of the Environment, held in Thessaloniki (July 2012) and additional data, in an attempt to create relationships between Cr with other elements determined in natural waters and define the sources of the Cr(VI) contamination (natural processes versus human activities). 2. HYDRO-GEOLOGICAL SETTING In the central Euboea (Figure 1, sampling area 1), the sampled springs have being issued from the upper Cretaceous limestones and are located near to the contact with the underlying upper Jurassic-lower Cretaceous ophiolitic complex. The ophiolitic complex is consisted by serpentinites, diabases and peridotites. The main aquifer of the wells is hosted into the same ophiolitic complex and it is assumed as a fissured rock aquifer. Alluvial deposits comprise the aquifer of many shallow wells used for agricultural activities. The wells have a depth between 4-180m (Megremi, 2010). In the extended area of Assopos -Thiva basins (Figure 1, sampling area 2), the wells are sited on a thick Neogene formation (up to over 600 m thick), consisted by intercalations of marles, sands, clays and limestones. The aquifer is porous and is consisted of several sub-aquifers, as the clay European Water 41 (2013) 25 intercalations are impermeable by the water. The wells have a depth between 200-220m and those which are used for the agriculture in that area, have a depth between 15-300m. At the southeast of this basin there are the Mavrosouvala wells (at the edge of the sampling area 1, towards Malakasa town, see Figure 1). Those are sited in middle Triassic to middle Lias, limestone formation (up to over 500 m thick) which is the north extension of the thick Parnis Mountain limestone formation (Vasilatos et al, 2010). 3. MATERIALS AND METHODS A total of 41 groundwater samples were collected from the extended area of the municipality of Messapia and N. Artaki (areas of N.Artaki – Kastella – Psachna – Makrymalli – Kondodespoti) in central Euboea and 21 groundwater samples from the neighboring area of Assopos-Thiva basins (areas of Oropos and Avlona) (Figure 1).
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