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Hydrogeochemical Comparison And Available online at www.sciencedirect.com Journal of Contaminant Hydrology 99 (2008) 31–48 www.elsevier.com/locate/jconhyd Hydrogeochemical comparison and effects of overlapping redox zones on groundwater arsenic near the Western (Bhagirathi sub-basin, India) and Eastern (Meghna sub-basin, Bangladesh) margins of the Bengal Basin ⁎ Abhijit Mukherjee a, , Mattias von Brömssen b, Bridget R. Scanlon a, Prosun Bhattacharya b, Alan E. Fryar c, Md. Aziz Hasan b, Kazi Matin Ahmed d, Debashis Chatterjee e, Gunnar Jacks b, Ondra Sracek f a Bureau of Economic Geology, Jackson School of Geosciences, University of Texas at Austin, Austin, TX 78758, USA b KTH-International Groundwater Arsenic Research Group, Department of Land and Water Resources Engineering, Royal Institute of Technology (KTH), Teknikringen 76, Stockholm, SE-10044, Sweden c Department of Earth and Environmental Sciences, University of Kentucky, 101 Slone Research Bldg, Lexington, KY 40506-0053, USA d Department of Geology, University of Dhaka, Curzon Hall Campus, Dhaka, 1000, Bangladesh e Department of Chemistry, University of Kalyani, Kalyani, West Bengal, India f Institute of Geological Sciences, Faculty of Science, Masaryk University, Kotlářská 2, 611 37 Brno, Czech Republic Received 27 June 2007; received in revised form 12 October 2007; accepted 16 October 2007 Available online 25 October 2007 Abstract Although arsenic (As) contamination of groundwater in the Bengal Basin has received wide attention over the past decade, comparative studies of hydrogeochemistry in geologically different sub-basins within the basin have been lacking. Groundwater samples were collected from sub-basins in the western margin (River Bhagirathi sub-basin, Nadia, India; 90 samples) and eastern margin (River Meghna sub-basin; Brahmanbaria, Bangladesh; 35 samples) of the Bengal Basin. Groundwater in the western site (Nadia) has mostly Ca–HCO3 water while that in the eastern site (Brahmanbaria) is much more variable consisting of at least six different facies. The two sites show differences in major and minor solute trends indicating varying pathways of hydrogeochemical evolution However, both sites have similar reducing, postoxic environments ( pe:+5to−2) with high concentrations of dissolved organic carbon, indicating dominantly metal-reducing processes and similarity in As mobilization mechanism. The trends of − + 2− various redox-sensitive solutes (e.g. As, CH4, Fe, Mn, NO3,NH4,SO4 ) indicate overlapping redox zones, leading to partial redox equilibrium conditions where As, once liberated from source minerals, would tend to remain in solution because of the complex interplay among the electron acceptors. © 2007 Elsevier B.V. All rights reserved. Keywords: Arsenic; Groundwater; Bengal Basin; Redox; Hydrogeochemistry ⁎ Corresponding author. E-mail addresses: [email protected] (A. Mukherjee), [email protected] (M. von Brömssen), [email protected] (B.R. Scanlon), [email protected] (P. Bhattacharya), [email protected] (A.E. Fryar), [email protected] (M.A. Hasan), [email protected] (K.M. Ahmed), [email protected] (D. Chatterjee), [email protected] (G. Jacks), [email protected] (O. Sracek). 0169-7722/$ - see front matter © 2007 Elsevier B.V. All rights reserved. doi:10.1016/j.jconhyd.2007.10.005 32 A. Mukherjee et al. / Journal of Contaminant Hydrology 99 (2008) 31–48 1. Introduction control on the hydrogeochemistry and therefore on the distribution of As in Bengal Basin aquifers. Geogenic, non-point source, carcinogenic arsenic (As) There has been a large number of local-scale studies is now considered as one of the most serious natural (e.g. Harvey et al., 2002; Zheng et al., 2004; von Brömssen contaminants in groundwater worldwide (Mukherjee and et al., 2007) and regional reconnaissance studies (e.g. BGS/ Bhattacharya, 2001; Bhattacharya et al., 2002a; Smedley DPHE/MML, 2001; Dowling et al., 2003) in both and Kinniburgh, 2002; Mukherjee et al., 2007). The Bengal Bangladesh and India, however, very few studies (e.g. Basin, comprising most of Bangladesh and parts of the Hasan et al., 2007; Metral et al., in review) have evaluated Indian state of West Bengal, is regarded to be the most the hydrogeochemistry and As distribution and mobiliza- acutely arsenic-affected geological province in the world. tion mechanisms simultaneously in hydrogeologically The basin, formed by the sedimentation of the rivers different parts of the basin. The present study builds upon Ganges (6th largest in the world), Brahmaputra (4th largest previous hydrogeochemical studies conducted by Bhatta- in the world), and Meghna, along with their numerous charya et al. (2006) and Hasan et al. (2007) in eastern tributaries and distributaries (hence also called GBM Bangladesh and by Mukherjee (2006) and Mukherjee and basin), is the world's largest fluvio-deltaic basin (Alam Fryar (2008) in the deep aquifers of West Bengal. The et al., 2003). More than 95% of the N120 million present work [with new data from the shallow aquifers of inhabitants (N2% of total world population) rely on the study site in West Bengal (72 new locations)] differs groundwater for drinking, and ∼70% of all irrigation in from the previous studies as it involves a comparison of the this region is groundwater-fed (Hasan et al., 2007). hydrogeochemistry (up to a depth of 300 m below ground However, the presence of elevated dissolved As in level [bgl]) between two geologically distinct, sub-basinal groundwater has endangered the lives of ∼35 million scale study sites located along the eastern margin (Meghna people in Bangladesh (Smedley and Kinniburgh, 2002)and sub-basin, Brahmanbaria in Bangladesh) and western ∼15 million people in West Bengal (Mukherjee, 2006), margin (Bhagirathi sub-basin, Nadia in West Bengal) of and has contaminated ∼25% to ∼33% (Ahmed et al., the Bengal Basin. In the course of this hydrogeochemical 2004; McArthur et al., 2004)of∼11 million tube wells comparison, we also investigate the applicability of the providing water in Bangladesh alone (Smedley, 2005). findings on chemical evolution processes and As dynamics Arsenic concentrations in groundwater of the Bengal Basin from each area (e.g. Bhattacharya et al., 2006; Mukherjee vary widely, ranging from b5 μg/L to 4100 μg/L in West and Fryar, 2008) to the other. We also investigated for Bengal (Ghosh and Mukherjee, 2002) and to 4730 μg/L in presence of common mechanisms for the liberation and Bangladesh (Rahman et al., 2006). retention of As in solution in the two sites. The observations Data from various previous studies at different locations from this study lead to the proposition of hypothesis of (mostly in Bangladesh) show that groundwater in the overlapping redox zonation and partial redox equilibrium shallow grey sediments of the basin, supposedly of (which to our knowledge have not previously been Holocene age, is most contaminated, whereas groundwater discussed for As-affected areas of Asia) as major in the deeper, yellowish or brownish, supposedly deeper controlling factors for arsenic retention and mobilization Holocene sediments is much less contaminated (e.g. von in groundwater. The generalization, description and Brömssen et al., 2007). However, in the western part of the conclusions of this study are drawn at a sub-basinal scale basin, such arsenic-free, yellowish or brownish colored and may not be valid for smaller-scale study sites because aquifer sediments have not been identified (Mukherjee, of local-scale complexities (e.g. aquifer architecture, land 2006). Similarly, several authors (e.g. Swartz et al., 2004) use, recharge patterns, surface water/groundwater interac- have noted considerable heterogeneity in groundwater As tions). Hence, evaluating local-scale variations in ground- concentrations in the Bengal Basin at scales of tens to water chemistry study sites is beyond the scope of the hundreds of meters horizontally. Nonetheless, regional- present study. scale studies have shown consistent spatial patterns in major and trace solute chemistry (including As) for aquifers 2. Summary of present knowledge on arsenic source at these scales (e.g. JICA, 2002; Dowling et al., 2003; and mobilization in Bengal Basin Mukherjee and Fryar, 2008), with the possibility of differences existing between sub-basins with dissimilar Although the general nature of the processes controlling geologic and geomorphic evolutionary histories (e.g. the fate of As in Recent alluvial aquifers has been Mukherjee, 2006; Hasan et al., (2007)). Hence, it is hypothesized, no consensus has been reached as to the apparent that basin geology, hydrogeology, scale of exact reactions controlling As mobilization and retention in heterogeneity, and depositional facies have substantial solution. Similarly, the primary source sediments of As in A. Mukherjee et al. / Journal of Contaminant Hydrology 99 (2008) 31–48 33 these aquifers are not known with certainty. In the Bengal of the basin (Imam and Shaw, 1985) and 16–22 km of Basin, solid-phase As in sediment varies with sediment size Tertiary to Quaternary alluvial sediments in the active and is not particularly high (Swartz et al., 2004), ranging delta area in the eastern part of the basin (Alam et al., from1to30mg/kg(Bhattacharya et al., 2001; McArthur 2003). et al., 2001; Harvey et al., 2002; Ahmed et al., 2004). The Physiographically, the Bengal Basin can be divided As has been found associated with Fe-hydroxide (mineral into two major units, the Pleistocene uplands and phases in the aquitard clays (e.g. Chakraborti et al., 2001;
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