that <strong>the</strong> situation <strong>in</strong> Dan Phuong could be viewed as a k<strong>in</strong>d of <strong>in</strong>itial state of <strong>the</strong> older sediments (up to 10 ka BP) <strong>in</strong> Bangladesh and W. Bengal (Goodbred and Kuehl, 2000). In this perspective it is useful to construct a mass balance for As for <strong>the</strong> Dan Phuong field site. The flux of groundwater As <strong>in</strong>to <strong>the</strong> area can be calculated from <strong>the</strong> calculated flow <strong>in</strong>to <strong>the</strong> model doma<strong>in</strong> multiplied by observed average groundwater As concentrations. The estimated fluxes <strong>in</strong> <strong>the</strong> As mass balance are shown <strong>in</strong> Fig. 12. The average As concentrations of groundwater flow<strong>in</strong>g <strong>in</strong>to <strong>the</strong> Holocene and Pleistocene aquifers from <strong>the</strong> sou<strong>the</strong>rn boundary have been set at 4 lM (300 lg/L) and 2 lM (150 lg/L), respectively, and with <strong>the</strong> regional groundwater flow 375 kg/a As enters <strong>the</strong> model area. The water recharg<strong>in</strong>g <strong>the</strong> Holocene aquifer from <strong>the</strong> channels will ga<strong>in</strong> As ei<strong>the</strong>r by mobilization with<strong>in</strong> <strong>the</strong> aquifer or <strong>in</strong> <strong>the</strong> bottom sediments of <strong>the</strong> channel (Polizzotto et al., 2006) but <strong>the</strong>re is no net flux of As enter<strong>in</strong>g <strong>the</strong> system this way. The groundwater flow<strong>in</strong>g <strong>in</strong>to <strong>the</strong> upper layers of <strong>the</strong> Pleistocene aquifer conta<strong>in</strong>s 720 kg As, assum<strong>in</strong>g groundwater As concentrations of 4 lM, as seen <strong>in</strong> <strong>the</strong> bottom of <strong>the</strong> Holocene aquifer (Fig. 6e and f). Lower groundwater As concentrations <strong>in</strong> <strong>the</strong> Pleistocene suggests that at least some of this As is sorbed to <strong>the</strong> sediments <strong>in</strong> <strong>the</strong> Pleistocene aquifer. The mass of As leached <strong>in</strong>to <strong>the</strong> <strong>Red</strong> <strong>River</strong> with <strong>the</strong> groundwater is around 945 kg/a, with 480 kg/a com<strong>in</strong>g from <strong>the</strong> Holocene aquifer and 465 kg/a from <strong>the</strong> Pleistocene aquifer. In addition, 180 kg/a is transported with <strong>the</strong> groundwater <strong>in</strong>to <strong>the</strong> channels after <strong>the</strong> monsoon period. The total amount of As leached from <strong>the</strong> Holocene aquifer is 1100 kg/a. The average As concentration <strong>in</strong> <strong>the</strong> sediment is 7.5 lg/g (Postma et al., 2007) and <strong>the</strong> total mass of As <strong>in</strong> <strong>the</strong> 24 km 2 model area is <strong>the</strong>refore 13.3 million kg As. The amount of As leached annually <strong>the</strong>refore corresponds to 0.01% of <strong>the</strong> total As mass <strong>in</strong> <strong>the</strong> Holocene sand. There are considerable uncerta<strong>in</strong>ties <strong>in</strong> <strong>the</strong> constructed As mass balance but <strong>the</strong> ma<strong>in</strong> conclusions are quite clear. First of all, a considerable mass of As is transported annually from <strong>the</strong> aquifers to <strong>the</strong> <strong>Red</strong> <strong>River</strong>. S<strong>in</strong>ce <strong>the</strong> river F. Larsen et al. / Applied Geochemistry 23 (2008) 3099–3115 3113 water conta<strong>in</strong>s very low concentrations of dissolved As, <strong>the</strong> groundwater As is apparently precipitated toge<strong>the</strong>r with Fe-oxides and <strong>in</strong>corporated <strong>in</strong> <strong>the</strong> sediments. In <strong>the</strong> long term this constitutes an As recycl<strong>in</strong>g loop s<strong>in</strong>ce <strong>the</strong> As enriched sediment with time will be redeposited along <strong>the</strong> river and form a new aquifer. The second ma<strong>in</strong> conclusion is that <strong>the</strong> amount of As exported from <strong>the</strong> system is small compared to <strong>the</strong> pool of As present <strong>in</strong> <strong>the</strong> sediment and a timescale of thousands of years is envisaged before <strong>the</strong> Holocene sediments become depleted <strong>in</strong> As which is <strong>in</strong> agreement with <strong>the</strong> estimates of Postma et al. (2007) based on <strong>the</strong> As release rate. The present rates of organic matter decomposition and <strong>the</strong>reby of As release must decrease over time (Postma et al., 2007) as <strong>the</strong> most reactive organic C becomes consumed and <strong>the</strong>refore <strong>the</strong> time required to deplete <strong>the</strong> sediment for As is a m<strong>in</strong>imum estimate. 6. Conclusions 1. The flood pla<strong>in</strong> aquifers at Dan Phuong show dur<strong>in</strong>g <strong>the</strong> dry season (October to May/June) a regional groundwater flow directed towards <strong>the</strong> <strong>Red</strong> <strong>River</strong>, with horizontal particle velocities up to 37 m/a. In this period, <strong>the</strong> water stage of <strong>the</strong> <strong>Red</strong> <strong>River</strong> distributaries is typically above <strong>the</strong> groundwater table and recharge of <strong>the</strong> shallow aquifer occurs by leakage through <strong>the</strong> low permeable bottom sediments. 2. Dur<strong>in</strong>g <strong>the</strong> monsoon, <strong>the</strong> water stages <strong>in</strong> <strong>the</strong> <strong>Red</strong> <strong>River</strong> and its distributaries <strong>in</strong>creases up to 6–8 m. This <strong>in</strong>crease is stall<strong>in</strong>g <strong>the</strong> regional groundwater flow <strong>in</strong> <strong>the</strong> adjacent aquifer and <strong>the</strong> result is a pattern of rapid fluctuations <strong>in</strong> groundwater table elevations and flow direction. Dur<strong>in</strong>g this phase, <strong>the</strong> groundwater tables <strong>in</strong>creases up to 4 m with<strong>in</strong> 2–3 months. Rapid fluctuations <strong>in</strong> <strong>the</strong> stages of <strong>the</strong> river and channels are generat<strong>in</strong>g a succession of ga<strong>in</strong><strong>in</strong>g and los<strong>in</strong>g phases at <strong>the</strong> <strong>in</strong>terface with <strong>the</strong> aquifer. Fig. 12. A mass balance of As <strong>in</strong> <strong>the</strong> Holocene aquifer. <strong>Groundwater</strong> flows are simulated values from <strong>the</strong> numerical model<strong>in</strong>g and groundwater As concentrations are average observed concentrations <strong>in</strong> <strong>the</strong> Holocene and Pleistocene aquifers.
3114 F. Larsen et al. / Applied Geochemistry 23 (2008) 3099–3115 3. Numerical model<strong>in</strong>g of <strong>the</strong> groundwater flow shows that recharge of <strong>the</strong> Holocene aquifer by surface water from <strong>Red</strong> <strong>River</strong> distributaries and from ra<strong>in</strong>water through a conf<strong>in</strong><strong>in</strong>g clay-rich layer are of <strong>the</strong> same order, be<strong>in</strong>g approximately 1.5 million m 3 /a <strong>in</strong> <strong>the</strong> modeled area. An average areal recharge rate from percolation of 60–100 mm/a through <strong>the</strong> conf<strong>in</strong><strong>in</strong>g clay was obta<strong>in</strong>ed from <strong>the</strong> transient groundwater flow model, while a total recharge rate of 195 mm/a below conf<strong>in</strong><strong>in</strong>g clay layers was estimated from 3 H/ 3 He dat<strong>in</strong>g of <strong>the</strong> water. 4. At places where <strong>the</strong> conf<strong>in</strong><strong>in</strong>g, clay-rich layer is less than 2–3 m thick, water conta<strong>in</strong><strong>in</strong>g electron acceptors (O2, NO3and SO 2 4 ) is transported <strong>in</strong>to <strong>the</strong> aquifer through fractures, or sandy outcrops, and <strong>in</strong>fluences <strong>the</strong> redox conditions <strong>in</strong> <strong>the</strong> underly<strong>in</strong>g aquifer. The spatial variation <strong>in</strong> <strong>the</strong> As content of <strong>the</strong> groundwater becomes, accord<strong>in</strong>gly, a function of <strong>the</strong> hydrogeological sett<strong>in</strong>g. 5. Arsenic is mobilized <strong>in</strong> <strong>the</strong> Holocene aquifer at a rate of about 14 lg/L/a, possibly with retardation <strong>in</strong> <strong>the</strong> Pleistocene aquifer. An As mass balance for <strong>the</strong> field site shows that around 1100 kg of As is <strong>in</strong> <strong>the</strong>se years annually leached from <strong>the</strong> Holocene sand and discharged <strong>in</strong>to <strong>the</strong> <strong>Red</strong> <strong>River</strong>, correspond<strong>in</strong>g to 0.01% of <strong>the</strong> total pool of As present <strong>in</strong> <strong>the</strong> Holocene sand. 6. Variations <strong>in</strong> stable isotope composition of precipitation, surface water and groundwater have proved to be a useful tool <strong>in</strong> trac<strong>in</strong>g surface–groundwater <strong>in</strong>teractions <strong>in</strong> <strong>the</strong> shallow Holocene aquifer. This is ma<strong>in</strong>ly due to <strong>the</strong> amount effect <strong>in</strong> <strong>the</strong> precipitation which <strong>in</strong> parts of Sou<strong>the</strong>ast Asia offers a dist<strong>in</strong>ct seasonal isotopic signature, which can be traced <strong>in</strong> <strong>the</strong> hydrological cycle. In <strong>the</strong> studied site, groundwater from <strong>the</strong> Pleistocene aquifer is more depleted than water from <strong>the</strong> Holocene aquifer, probably reflect<strong>in</strong>g a component of recharge water from <strong>the</strong> surround<strong>in</strong>g mounta<strong>in</strong>s of <strong>the</strong> <strong>Red</strong> <strong>River</strong> flood pla<strong>in</strong>. Acknowledgements This work is part of research capacity build<strong>in</strong>g project f<strong>in</strong>anced by <strong>the</strong> Danish aid organization DANIDA. Fur<strong>the</strong>r project <strong>in</strong>formation can be viewed at http://www.vietas.env.dtu.dk. Prof. Klaus Froehlich is thanked for a good discussion on <strong>the</strong> use of stable isotope <strong>in</strong> recharge studies. We also thank Kristian Anker Rasmussen (GEUS) and Torben Dol<strong>in</strong> (DTU) for <strong>the</strong> draw<strong>in</strong>g work. Alexander van Geen and David Polya are acknowledged for constructive comments and <strong>in</strong>puts <strong>in</strong> <strong>the</strong> review process. An anonymous reviewer is also thanked for positive comments and ideas. References Araguás-Araguás, L., Froenlich, K., Rozanski, K., 1998. Stable isotope composition of precipitation over sou<strong>the</strong>ast Asia. J. Geophys. Res. 103 (28), 721–728. 742. Barlow, P.M., Moench, A.F., 1998. Analytical solutions and computer programs for hydraulic <strong>in</strong>teraction of stream-aquifer systems. U.S. Geol. Surv. Open-File Rep., 98–415A. Berg, M., Tran, H.C., Nguyen, T.C., Pham, H.V., Schertenleib, R., Giger, W., 2001. Arsenic contam<strong>in</strong>ation of groundwater and dr<strong>in</strong>k<strong>in</strong>g water <strong>in</strong> <strong>Vietnam</strong>: a human health threat. Environ. Sci. Technol. 35, 2621– 2626. Berg, M., Pham, T.K.T., Stengel, C., Bruschman, J., Pham, H.V., Nguyen, V.D., Giger, W., Stüben, D., 2008. Hydrogeological and sedimentary controls lead<strong>in</strong>g to <strong>arsenic</strong> contam<strong>in</strong>ation of groundwater <strong>in</strong> <strong>the</strong> Hanoi area, <strong>Vietnam</strong>: The impact of iron–<strong>arsenic</strong> ratios, peat, river bank deposits, and excessive groundwater abstraction. Chem. Geol. 249, 91–112. Brunke, M., Gonser, T., 1997. Special Review: The ecological significance of exchange processes between river and groundwater. Freshwater Biol. 37, 1–33. Chambon, J., 2007. 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Groundwater arsenic in the Red Rive
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Søren Jessen Groundwater arsenic i
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organic matter may prevent As mobil
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Resumé Naturligt frigivet arsen (A
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efterfølgende forsøgt at opstille
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Preface This PhD thesis deals with
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Table of contents 1 INTRODUCTION: T
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The PhD research presented in this
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A more complex and intimate relatio
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in large part by changes in the eus
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5 The mitigation potential of bank
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Noteworthy is, that the ratio of Fe
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