A G RSENIC EOCHEMISTRY IN THE W B , ALLUVIAL AQUIFERS OF EST ENGAL I NDIA Implications for targeting safe aquifers for sustainable drinking water supply Ashis Biswas September 2013 TRITA-LWR PHD 1071 ISSN 1650-8602 ISRN KTH/LWR/PHD 1071-SE ISBN 978-91-7501-849-2 Ashis Biswas TRITA LWR PhD 1071 Cover illustration: Top left: Household hand pumped tubewell; Top right: Low-cost hand suction drilling technique used for household tubewell installation; Bottom left: Typical sediments recovered during drilling (Photograph: Ashis Biswas©, 2011); Bottom right: Piezometer nest at Chakudanga, Chakdaha (Photograph: Prosun Bhattacharya©, 2010) ©Ashis Biswas 2013 PhD Thesis KTH-International Groundwater Arsenic Research Group Division of Land and Water Resources Engineering Department of Sustainable Development, Environmental Sciences and Engineering KTH Royal Institute of Technology SE-100 44 STOCKHOLM, Sweden Reference to this publication should be written as: Biswas, A. (2013) Arsenic Geochemistry in the alluvial aquifers of West Bengal, India: Implications for targeting safe aquifers for sustainable drinking water supply. PhD Thesis, TRITA LWR PhD 1071, 71 p. ii Arsenic geochemistry in the alluvial aquifers of West Bengal, India Dedicated to my Family… iii Ashis Biswas TRITA LWR PhD 1071 iv Arsenic geochemistry in the alluvial aquifers of West Bengal, India FOREWORD The presence of naturally occurring arsenic in groundwater has been designated as “The largest mass poisoning in human history”. While arsenic is an old poison familiar since ages to us, its presence in groundwater in concentrations causing chronic poisoning came as a surprise. In the Bengal basin the problem is especially serious as in the past decades the rural water supply has been more or less completely switched to groundwater with excessive arsenic. Remedial actions have been tested in the form of filters, water harvesting etc but have not been accepted due to cost or social reasons. This thesis is focused on the fact that excess arsenic is not ubiquitous in the shallow groundwater, accessible with local, affordable drilling technology. In the late 1990s the mechanism for arsenic mobilization into the groundwater was explained by redox reactions resulting in reduction of ferric oxyhydroxides releasing the adsorbed arsenic. This thesis shows that while this may be a major process there are several contributing processes that are needed to produce the toxic groundwater. The thesis has elucidated new findings regarding the sedimentary history and water pathways important for the redox chemistry and the arsenic mobilization. The thesis has demonstrated that the processes are site specific. Thus, the thesis gives new insights into the processes mobilizing arsenic into the groundwater. Additionally it presents also a number of means to identify arsenic low groundwater within the depth of 50 m, easily accessible with the cheap local drilling technology. This identification covers a range from simple ones such as observing the color of the precipitates found on well platforms to deeper insights into the sedimentology and reactions regarding redox and surface chemistry of the sediments, all which can prioritize an urgently needed remedy of the current situation. Prof. Em. Gunnar Jacks Stockholm, KTH, September 2013 v Ashis Biswas TRITA LWR PhD 1071 vi Arsenic geochemistry in the alluvial aquifers of West Bengal, India ACKNOWLEDGEMENTS First of all, I would like to express my sincere gratitude to my main supervisor Prof. Prosun Bhattacharya at the Division of Land and Water Resources Engineering (LWR) for hosting me as the doctoral student at KTH Royal Institute of Technology (KTH). Without his support, encouragement and guidance it was not possible to complete my doctoral study at KTH. I have heart-full appreciation for my co-supervisor Prof. Debashis Chatterjee at the Department of Chemistry (DC), University of Kalyani (KU). I am grateful to him for motivating me to pursue doctoral study and ensuring all- time access to his laboratory, logistic supports during field campaigns and the time for academic discussions. I am also thankful for giving me the opportunity to work as a research fellow in the collaborative project between DC-KU and Institute of Mineralogy and Geochemistry (IMG), Karlsruhe Institute of Technology (KIT), dealing with the investigation of role of microbiogeochemical processes in arsenic mobilization in the aquifers of Bengal Basin, prior to my joining as a doctoral student at KTH. This project has substantial contribution in my PhD study at KTH. I am grateful to Prof. Gunnar Jacks at LWR, KTH, who also ensured unlimited access to him for any scientific discussion and was always ready to help me in the laboratory work. I have also enjoyed those non-scientific discussions with him, which have enriched me as human beings. I feel really fortunate having him in my advisory committee. I am equally thankful to Dr. Zsolt Berner (IMG, KIT), Dr. Bibhash Nath (School of Geosciences, The University of Sydney), Dr. Abhijit Mukherjee (Department of Geology and Geophysics, Indian Institute of Technology-Kharagpur) and Prof. Jon Petter Gustafsson (LWR, KTH) for their guidance at different stages of my research. I am also thankful to Prof. Berit Balfors at LWR, KTH for her revision of my thesis and afterward very fruitful discussion. I would like to warmly acknowledge the supports of all of my co-authors in the papers. I am very much thankful to my friend Dr. Harald Neidhardt at IMG, KIT, currently at EAWAG, who was always ready to extend his support throughout my research. We have so many great memories during field work at Chakdaha together with Dr. Dominik Freikowski (Institute of Biology for Engineers and Biotechnology of Waste Water Treatment, KIT). I am also thankful to all of my colleagues and friends both at KU and KTH for ensuring a nice and homely working environment and keeping me always mentally fresh. Especially, I would like to thank Amit K. Kundu at DC, KU for taking care of sampling, when I was at KTH. I would like to acknowledge the analytical support from DC, KU; IMG, KIT; Department of Geological Sciences (IGV), Stockholm University (SU) and Department of Solid State Chemistry, Institute of Chemical Technology in Prague (Dr. Barbora Doušová). I am also thankful to Bertil Nilsson and Ann Fylkner at LWR, KTH. Without such analytical supports it was not possible to finish my study on time. I am especially grateful to Prof. Carl-Magnus Mörth at IGV, SU for discussing about different aspect of possible analysis over there and ensuring such supports, which has substantially developed the outputs of my research. I would like to thank Heike Siegmund (IGV, SU), who has always analyzed my samples with top priority. I would also like to acknowledge the support of Luminescence Laboratory (Prof. Helena Alexanderson) and vii Ashis Biswas TRITA LWR PhD 1071 Radiocarbon Dating Laboratory of the Department of Geology, Lund University for the dating of aquifer sediments from my study area. I am thankful to Dr. Saugata Datta at Kansas State University for giving me the opportunity to work at National Synchrotron Light Source (NSLS) at Brookhaven National Laboratory (BNL) with his research group and it is a lifetime experience for me. I am thankful to P. K. Das (Bapi), N. Bhabani (Probhu), R. Das (Bapi) and S. Karmakar (Bablu) and his drilling team, who were always ready to work at the field even at very short notice. I would also like to acknowledge local villagers in my study area, especially Mr. Atul Chandra Mandal and Mr. Sadhan Ghosh for ensuring the unlimited access to their courtyards for piezometers installation and sampling campaign. I will remember the hospitality of Mashima (wife of Mr. Atul Chandra Mandal) throughout my life; I have access to their house like my home. I would like to acknowledge the supports of Aira Saarelainen, Britt Chow and Jerzy Buczak to me as a PhD student at LWR, KTH. I am also grateful to my parents, parents-in-law and Mr. Mihir Khan for their love and mental support throughout my study. Lastly, it is the time to acknowledge some special one, who is at the same time friend, colleague and my wife, Dipti Halder. Without her supports and cooperation both academically and in the daily life, it was not possible to accomplish this research. Being with her, I can very easily switch off myself from the daily life concerns and concentrate into my own research. Does it seem I am selfish, indeed I am!! The list cannot be completed without acknowledging the funding authorities. At first, I would like to acknowledge the Erasmus Mundus External Cooperation Window (EMECW-Action II) for providing me the doctoral fellowship through EURINDIA Program, which enabled me to pursue PhD study at KTH. I would also like to acknowledge the German Research Foundation (DFG) and the German Federal Ministry for Economic Cooperation and Development (BMZ) (Stu 169/37-1) for providing the funding for collaborative project between DC, KU and IMG, KIT. I am also thankful to the financial support to KTH-International Groundwater Arsenic Research Group (KTH-GARG) by Swedish International Development Cooperation Agency (Sida) and Swedish Research Council (VR) through the Swedish Research Link grant (VR-Sida, dnr: 348-2006-6005) and the Strategic Environmental Research Foundation (MISTRA) (Idea Support Grant, dnr: 2005-035-137). Without these fundings the research presented in the thesis could not be accomplished. Finally, I want mention that doing PhD is a memorable journey in my life and I am extremely happy being at the end of this journey. I have learned so many things during this journey, which have enriched me in the professional field and also as human beings. The experiences that I have gained certainly would help me to complete the rest journey in my life successfully. Thank you all again!! Ashis Biswas Stockholm, September 2013 viii Arsenic geochemistry in the alluvial aquifers of West Bengal, India LIST OF APPENDED PAPERS AND MY CONTRIBUTIONS This thesis is based on the following five papers, which are reffered as corresponding Roman numerals throughout the text and are attached in the Appendix. Paper I Biswas, A., Bhattacharya, P., Mukherjee, A., Nath, B., Alexanderson, H., Kundu, A.K., Chatterjee, D., Jacks, G. Delineation of shallow hydrostratigraphy in arsenic affected region of Bengal Basin: Implication for targeting safe aquifers for drinking water supply. Submitted to Chem. Geol. I participated in designing of the project, executed the field work and laboratory analysis and performed lithological modeling, data analysis and main part of writing. Paper II Biswas, A., Nath, B., Bhattacharya, P., Halder, D., Kundu, A.K., Mandal, U., Mukherjee, A., Chatterjee, D., Mörth, C.M., Jacks, G., 2012. Hydrogeochemical contrast between brown and grey sand aquifers in shallow depth of Bengal Basin: Consequences for sustainable drinking water supply. Sci. Total Environ. 431, 402-412. Reprinted with permission. Copyright (2012) Elsevier. I participated in designing of the project, executed the field work and major part of laboratory analysis and performed data analysis and main part of writing. Paper III Biswas, A., Neidhardt, H., Kundu, A.K., Halder, D., Chatterjee, D., Berner, Z., Jacks, G., Bhattacharya, P. Spatial, vertical and temporal variation of arsenic in the shallow aquifers of Bengal Basin: Controlling geochemical processes. Submitted to Geochim. Cosmochim. Acta. I participated in sediment sampling and piezometer installation, executed bi- weekly groundwater sampling and part of laboratory analysis and performed data analysis and main part of writing. Paper IV Biswas, A., Gustafsson, J.P., Neidhardt, H., Halder, D., Kundu, A.K., Chatterjee, D., Berner, Z., Bhattacharya, P. Role of competing ions on the mobilization of arsenic in groundwater of sedimentary aquifers: Insight from surface complexation modeling. Submitted to Water Res. I performed all the modeling, data analysis and main part of writing. Paper V Biswas, A., Nath, B., Bhattacharya, P., Halder, D., Kundu, A.K., Mandal, U., Mukherjee, A., Chatterjee, D., Jacks, G., 2012. Testing Tubewell Platform Color as a Rapid Screening Tool for Arsenic and Manganese in Drinking Water Wells. Environ. Sci. Technol. 46, 434-440. Reprinted with permission. Copyright (2012) American Chemical Society. I participated in designing of the project, executed the field work and laboratory analysis and performed data analysis and main part of writing. LIST OF PAPERS NOT APPENDED IN THE THESIS Paper VI Biswas, A., Majumder, S., Neidhardt, H., Halder, D., Bhowmick, S., Mukherjee – Goswami, A., Kundu, A.K., Saha, D., Berner, Z., Chatterjee, D., ix Ashis Biswas TRITA LWR PhD 1071 2011. Groundwater chemistry and redox processes: depth dependent arsenic release mechanism. Appl. Geochem. 2011, 26, 516-525. Paper VII Neidhardt, H., Biswas, A., Freikowski, D., Majumder, S., Chatterjee, D., Berner, Z., 2013. Reconstructing the sedimentation history of the Bengal Delta Plain by means of geochemical and stable isotopic data. Appl. Geochem. 36, 70- 82. Paper VIII Neidhardt, H., Berner, Z., Freikowski, D., Biswas, A., Winter, J., Chatterjee, D., Norra, S., 2013. Influences of groundwater extraction on the distribution of dissolved arsenic in shallow aquifers of West Bengal, India. J. Hazard. Mater. In Press, DOI: http://dx.doi.org/10.1016/j.jhazmat.2013.01.044. Paper IX Bhowmick, S., Nath, B., Halder, D., Biswas, A., Majumder, S., Mondal, P., Chakraborty, S., Nriagu, J., Bhattacharya, P., Iglwsias, M., Roman-Ross, G., Guha Mazumder, D., Bundschuh, J., Chatterjee, D., 2013. Arsenic mobilization in the aquifers of three physiographic settings of West Bengal, India: understanding geogenic and anthropogenic influences. J. Hazard. Mater. In Press, DOI: http://dx.doi.org/10.1016/j.jhazmat.2012.07.014. Paper X Halder, D., Bhowmick, S., Biswas, A., Chatterjee, D., Nriagu, J., Guha Mazumdar, D.N., Šlejkovec, Z., Jacks, G., Bhattacharya, P., 2013. Risk of arsenic exposure from drinking water and dietary components: Implications for risk management in rural Bengal. Environ. Sci. Technol. 47, 1120-1127. Paper XI Halder, D., Bhowmick, S., Biswas, A., Mandal, U., Nriagu, J., Guha Mazumdar, D.N., Chatterjee, D.; Bhattacharya, P., 2012. Consumption of brown rice: A potential pathway for arsenic exposure in rural Bengal. Environ. Sci. Technol. 46, 4142-4148. Paper XII Chatterjee, D., Halder, D., Majumder, S., Biswas, A., Nath, B., Bhattacharya, P., Bhowmick, S., Mukherjee-Goswami, A., Saha, D., Hazra, R., Maity, P.B., Chatterjee, D., Mukherjee, A., Bundschuh, J., 2010. Assessment of arsenic exposure from groundwater and rice in Bengal Delta region, West Bengal, India. Water Res. 44, 5803-5812. Paper XIII Chatterjee, D., Majumder, S., Biswas, A., Halder, D., Bhowmick, S., Chatterjee, D., Mukherjee- Goswami, A., Jana, J., Saha, D., Kundu, A.K., Sarkar, S., 2012. Arsenic in Grondwater of Young Bengal Delta Plain of India: It’s Distribution and Geochemistry. Indian Soc. Appl. Geochem. 170-185. Paper XIV Lawson, M., Ballentine, C.J., Polya, D.A., Boyce, A.J., Mondal, D., Chatterjee, D., Majumder, S., Biswas, A., 2008. The geochemical and isotopic composition of ground waters in West Bengal: tracing ground–surface water interaction and its role in arsenic release. Miner. Mag. 72, 441-444. x