Large-scale Uranium Contamination of Groundwater Resources in India

Transcription

1 Supporting Information Large-scale Uranium Contamination of Groundwater Resources in India Rachel M. Coyte, Ratan C. Jain^, Sudhir K. Srivastava #, Kailash C. Sharma, Abedalrazq Khalil $, Lin Ma, Avner Vengosh * Nicholas ^Gujarat School of the Environment, Duke University, Durham, rth Carolina 27708, United States Water Resources Development Corporation Ltd, Gandhinagar, Gujarat , India. # Central Ground Water Board, Ministry of Water Resources, River Development, and Ganga Rejuvenation, Bhujal Bhawan, Faridabad, , India Ground Water Department, Government of Rajasthan, Jaipur , India $ Water Global Practice, World Bank Group Singapore Office, Singapore Department of Geological Sciences, University of Texas at El Paso, El Paso, Texas 79968, United States * vengosh@duke.edu. Phone: Fax: Contents Page Table S1: Compiled studies of the occurrence of uranium in groundwater resources in India S2 Table S2: Chemistry data for wells measured in Rajasthan and Gujarat alluvial aquifers S8 Table S3: Uranium Isotope of groundwater investigated in this study S22 Table S4: Statistical analysis of differences in U concentration populations for different lithological pairs S24 Table S5: Spearman correlations for nitrate versus uranium sorted by aquifer S25 Table S6: Spearman correlations for bicarbonate versus uranium sorted by aquifer S25 Table S7: Modeling of the uranium speciation using PHREEQC software S26 Figure S1: Box plot of nitrate concentrations of groundwater from different aquifers in Rajasthan and Gujarat S27 Figure S2: Uranium versus nitrate concentrations of groundwater sorted by aquifer lithology S28 Figure S3: Uranium and 238 U/ 234 U activity ratio variations with depth of groundwater from Gujarat alluvial aquifers S29 References S30 S1

2 Table S1: Compiled Studies of the occurrence of uranium in groundwater resources in India State District Dominant Aquifer # wells Maximum U concentration (µg/l) Minimum concentration (µg/l) Mean U concentration (µg/l) Median concentration (µg/l) tes Jammu and Jammu Alluvium, Siwalik Kashmir 1 Jammu and Kathua Alluvium, Siwalik, slate, Kashmir 2 granitoids Jammu and Udhampur Alluvium, Siwalik abstract Kashmir 3 only Himachal Hamirpur Alluvium, sandstone, tertiary Pradesh 2 Siwalik group Himachal Kangra Siwalik, sandstone, Precambrian Pradesh 2 silicates (weathered and fractures), alluvium Punjab 4 Amristar Alluvium Punjab 5 Amristar Alluvium Punjab 6 Bathinda Alluvium Punjab 7 Bathinda Alluvium < Punjab 8 Bathinda Alluvium Punjab 9 Bathinda Alluvium Punjab 10 Bathinda Alluvium abstract only Punjab 11 Bathinda Alluvium Punjab 5 Bathinda Alluvium Punjab 12 Bathinda Alluvium Punjab 13 Bathinda Alluvium Punjab 14 Bathinda Alluvium S2

3 Punjab 15 Bathinda and Mansa Alluvium Punjab 16 Bathinda and Mansa Alluvium Punjab 17 Bathinda and Mansa Alluvium Punjab 8 Mansa Alluvium Punjab 8 Mansa Alluvium Punjab 18 Mansa Alluvium abstract only Punjab 5 Mansa Alluvium Punjab 12 Mansa Alluvium Punjab 14 Mansa Alluvium Punjab 19 Faridkot Alluvium Punjab 8 Faridkot Alluvium Punjab 5 Faridkot Alluvium Punjab 12 Faridkot Alluvium Punjab 14 Faridkot Alluvium Punjab 20 Fatehgarh Alluvium Punjab 21 Fazilka Alluvium Punjab 12 Ferozepur Alluvium Punjab 9 Hoshiarpur Alluvium Punjab 22,23 Hoshiarpur Alluvium Punjab 15 Hoshiarpur Alluvium Punjab 5 Hoshiarpur Alluvium Punjab 22,23 Jalandhar Alluvium Punjab 22,23 Kapurthala Alluvium Punjab 22,23 Kapurthala Alluvium S3

4 Punjab 24 Malwa region Alluvium Punjab 19 Muktsar Alluvium Punjab 8 Muktsar Alluvium Punjab 6 Muktsar Alluvium Punjab 25 Rupnagar Alluvium Punjab 20 S.A.S Nagar Alluvium Punjab 26 Sangrur Alluvium Punjab 22,23 Shaheed Bhagat Singh Nagar Alluvium Punjab 9 Shahid Bhagat Singh Nagar Alluvium Punjab 5 Tarn-taran Alluvium Haryana 27 Bhiwani Alluvium Haryana 28 Fatehabad Allvuium Haryana 29 Fatehabad Alluvium Haryana 27 Fatehabad Alluvium Haryana 29 Fatehabad Alluvium abstract only Haryana 30 Hisar Alluvium Haryana 29 Hisar Alluvium Haryana 27 Hisar Alluvium Haryana 31 Mahendragarh Alluvium, soil is calcareous with lime nodules Haryana 32 Panipat Alluvium abstract only Haryana 27 Sirsa Alluvium Haryana 33 Sirsa Alluvium abstract S4

5 Haryana 32 Sonipat Alluvium abstract only Multiple 25 Upper Siwaliks Siwalik Uttar Bulandshahr Alluvium bdl abstract Pradesh 34 only Rajasthan 35 Bikaner Alluvium, sandstone, limestone only Rajasthan 33 Churu Alluvium, schist, phyllite, sandstone abstract only Rajasthan 36 Hanmangarh Alluvium, sandstone 50 abstract only Rajasthan 35 Jhunjhunu Alluvium, quartzites, phyllite/schist, gneiss, limestone, granite, pegmatites, amphibolites Rajasthan 35 Jodhpur Alluvium, sandstone, limestone, rhyolite, granite, schist, phyllite Rajasthan 35 Nagaur Alluvium, sandstone, limestone, granite, schist, phyllite Rajasthan 37 rthern Rajasthan Alluvium, weathered and fractured metamorphic, sandstone Rajasthan 36 Sikar Alluvium, quartzite, schist, phyllite, gneiss, amphibolite Rajasthan 36 Sri Ganganagar Alluvium, sandstone, limestone, evaporate sequence Maharashtra 38 Nagpur Archean (weathered and fractured granite, gneiss) and Deccan trap Chhattisgarh 39 Durg Mostly shale, limestone, some BCG, gneiss and sandstone abstract only abstract only abstract only S5

6 Jharkhand 40 East Singhbhum Weathered and fractured granite gneiss and metasediments Jharkhand 41 East Singhbhum Weathered and fractured granite gneiss and metasediments Jharkhand 42 East Singhbhum Weathered and fractured granite gneiss and metasediments Jharkhand 43 East Singhbhum Weathered and fractured granite gneiss and metasediments Jharkhand 44 East Singhbhum Weathered and fractured granite gneiss and metasediments Jharkhand 45 East Singhbhum Weathered and fractured granite gneiss and metasediments Jharkhand 40 Western Singhbhum Granite-gneiss, Quartzite and older Alluvium < abstract only < <1 West Bengal 46 Murshidabad Alluvium < West Bengal 47 Murshidabad Alluvium bdl 3.20 West Bengal 46 Nadia Alluvium < West Bengal 48 Nadia Alluvium West Bengal 49 rth 24 Parganas district Alluvium < West Bengal 46 rth 24 Parganas district Alluvium < West Bengal 50 Purulia Weathered and fractured granite gneiss and metasediments West Bengal 46 South 24 Parganas Alluvium < Odisha 51 Ganjam Weathered & Fractured < S6

7 Crystalline Rocks Andhra Pradesh 52 Guntur 1. Granite/ Gneiss schistose basement (fracture and weathering) 2. Slates, phyllites, quartzites (joints, bedding planes, soil zones) 3. Limestone, quartzites (bedding planes, joints, fissures) Andhra Guntur Neoproterozoic Quartz Arenite, Pradesh 53 known to have uranium mineralization Andhra YSR Kadapa district Shale, limestone, dolomite Pradesh 54 (CGWB)(Sandy, clayey sedimentary sequence) Telangana 55 Nalgonda Granite gneiss, minor metamorphic (weathered) Telangana 56 Nalgonda Shallow granitic Telangana 57 Nalgonda Archean crystalline rocks (weathering and fracture) Telangana 58 Nalgonda Weathered/ fractured granite/ gneiss Telangana 59 Nalgonda Weathered/fractured/ jointed Granite, under phreatic and semi-confined to confined conditions (CGWB) abstract only Karnataka 60 Bangalore Granite gneiss Karnataka 61 Bangalore Granite gneiss Karnataka 62 Chamarajanagar Jointed and fractured gneisses and charnockites Karnataka 63 Kolar Weathered and fractured Granite Gneisses and schists Telangana 64 Hyderabad Granite, gneiss, phreatic conditions in weathered zone abstract only S7

8 and under semi-confined to confined conditions in the fractured zones Tamil Nadu 65 Madurai Weathered and fractured crystalline rock Tamil Nadu 66 Madurai Weathered and fractured crystalline rock Tamil Nadu 67 Madurai Weathered and fractured crystalline rock Tamil Nadu 68 Nagapattinam Deep lower miocene to recent quaternary Tamil Nadu 69 Tirunelveli Alluvium and weathered/ fractured granite/ gneiss/ charnockite bdl (.2ppb) < Table S2: Chemistry for Wells Measured in Rajasthan and Gujarat Alluvial Aquifers Sample Aquifer Depth (m) State Well Type Drinking Specific Conductivity (μs/cm) ph HCO 3 - Jai 133 Alluvium Rajasthan Tube well Yes bdl bdl Jai 135 Alluvium Rajasthan Tube well Yes bdl bdl Ab Alluvium Rajasthan Tube well Yes bdl bdl sample 26R Alluvium Rajasthan Tube well Yes bdl Crowne 2 Alluvium Rajasthan Tube well Yes t recorded t recorded 658 bdl bdl Dausa Alluvium Rajasthan Handpump Yes bdl bdl Dausa Alluvium Rajasthan Handpump Yes bdl Dausa Alluvium Rajasthan Handpump Yes bdl bdl Dausa Alluvium Rajasthan Handpump bdl bdl Dausa Alluvium Rajasthan Tube well Yes bdl bdl (mg/l) Fe (mg/l) Mn (mg/l) U (μg/l) NO 3 - (mg/l) S8

9 107 Haijai Alluvium Jai 118 Alluvium Jai 119 Alluvium Jai 122 Alluvium Jai 123 Alluvium Jai 125 Alluvium Jai 126 Alluvium Jai 127 Alluvium Jai 128 Alluvium Jai 130 Alluvium Jai 131 Alluvium Jai 138 Alluvium Jai-101 Alluvium Jai-104 Alluvium Jai-106 Alluvium Jai-108 Alluvium Jai-109 Alluvium Jai-111 Alluvium Jai-112 Alluvium Jai-113 Alluvium Jai-114 Alluvium Jai-115 Alluvium Rajasthan Tube well Yes t recorded t recorded 346 bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Tube well bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Tube well bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl Rajasthan Handpump Yes bdl bdl Rajasthan Tube well bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl S9

10 Jai-116 Alluvium Tonk- Alluvium 101 Tonk- Alluvium 103 Tonk- Alluvium 105 Tonk- Alluvium 106 Tonk- Alluvium 108 Tonk- Alluvium 110 Jai-01 Alluvium Jai-02 Alluvium Jai-03 Alluvium Jai-21 Alluvium Jai-22 Alluvium Jai-23 Alluvium Jai-25 Alluvium Jai-26 Alluvium Jai-27 Alluvium Jai-28 Alluvium Jai-29 Alluvium Jai-30 Alluvium Jai-31 Alluvium Jod-01 Alluvium Jod-02 Alluvium Jod-03 Alluvium Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl Rajasthan Handpump bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl Rajasthan Tube well Rajasthan Handpump Yes bdl bdl Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Handpump Yes Rajasthan Tube well Yes Rajasthan Handpump Yes Rajasthan Handpump Yes Rajasthan Tube well Rajasthan Tube well Rajasthan Tube well Yes Rajasthan Tube well Rajasthan Tube well Yes Rajasthan Tube well Rajasthan Tube well Rajasthan Tube well S10

11 Jod-04 Alluvium Jod-05 Alluvium Jod-06 Alluvium Jod-12 Alluvium Jod-26 Alluvium Jod-27 Alluvium Jod-28 Alluvium Jod-29 Alluvium Jod-30 Alluvium Raj-01 Alluvium Raj-02 Alluvium Raj-04 Alluvium Raj-06 Alluvium Raj-08 Alluvium Raj-09 Alluvium Raj-10 Alluvium Raj-11 Alluvium Raj-12 Alluvium Raj-13 Alluvium Raj-14 Alluvium Raj-15 Alluvium Raj-16 Alluvium Raj-17 Alluvium Rajasthan Tube well Rajasthan Tube well Yes Rajasthan Tube well Rajasthan Tube well Yes Rajasthan Tube well Rajasthan Tube well Rajasthan Tube well Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Handpump Yes Rajasthan Tube well Yes bdl Rajasthan Tube well Yes bdl Rajasthan Handpump Yes Rajasthan Handpump Yes Rajasthan Handpump Yes Rajasthan Handpump Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Handpump Yes Rajasthan Handpump Yes bdl Rajasthan Tube well Yes S11

12 Raj-18 Alluvium Raj-19 Alluvium Raj-20 Alluvium Raj-21 Alluvium Raj-22 Alluvium Raj-23 Alluvium Raj-24 Alluvium Raj-25 Alluvium Raj-26 Alluvium Raj-27 Alluvium Raj-28 Alluvium Raj-29 Alluvium Raj-30 Alluvium Raj-31 Alluvium Raj-32 Alluvium Raj-33 Alluvium Raj-34 Alluvium Raj-35 Alluvium Raj-36 Alluvium Raj-37 Alluvium 23 ab Alluvium 24R Alluvium 25R Alluvium Rajasthan Tube well Yes sample Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Handpump Yes Rajasthan Handpump bdl Rajasthan Handpump Yes bdl Rajasthan Tube well Yes bdl Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes bdl Rajasthan Tube well Yes bdl Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes bdl Rajasthan Tube well Yes Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl S12

13 Ajmer 101 Alluvium Ajmer Alluvium 102 Ajmer Alluvium 103 Ajmer Alluvium 104 Ajmer Alluvium 105 Ajmer Alluvium 106 Bundi Alluvium 103 Bundi Alluvium 104 Bundi Alluvium 105 Bundi Alluvium 106 Jai 142 Alluvium Jai-04 Alluvium Jai-05 Alluvium Jai-06 Alluvium Jai-07 Alluvium Jai-08 Alluvium Jai-09 Alluvium Jai-10 Alluvium Jai-11 Alluvium Jai-12 Alluvium Jai-15 Alluvium Jai-16 Alluvium Jai-17 Alluvium Rajasthan Tube well bdl bdl Rajasthan Tube well Yes bdl 2.0 Rajasthan Handpump bdl bdl Rajasthan Handpump Rajasthan Handpump Rajasthan Handpump bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump bdl bdl Rajasthan Handpump Yes bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Rajasthan Handpump Rajasthan Handpump Rajasthan Handpump Rajasthan Dug well Rajasthan Handpump Yes Rajasthan Tube well Yes Rajasthan Handpump Yes Rajasthan Handpump Yes Rajasthan Tube well Yes Rajasthan Handpump Yes Rajasthan Handpump Yes S13

14 Jai-18 Alluvium Jai-19 Alluvium Jai-20 Alluvium Jod-07 Alluvium Jod-08 Alluvium Jod-09 Alluvium Jod-10 Alluvium Jod-11 Alluvium Jod-13 Alluvium Jod-14 Alluvium Jod-15 Alluvium Bundi 102 Kota 103 Kota 104 Kota 105 Kota 106 Kota 110 Jod-18 Jod-19 Jod-20 Jod-21 Kota 101 Kota 102 Rajasthan Tube well Yes Rajasthan Dug well Yes Rajasthan Handpump Yes Rajasthan Tube well Rajasthan Tube well Rajasthan Handpump Rajasthan Handpump Rajasthan Dug well Rajasthan Tube well Rajasthan Tube well Rajasthan Dug well Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Handpump Yes bdl Rajasthan Dug well Rajasthan Dug well Rajasthan Dug well Rajasthan Dug well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes bdl bdl S14

15 Kota Rajasthan Tube well Rajasthan Handpump Yes Rajasthan Tube well Yes bdl 1.2 Rajasthan Handpump Yes Rajasthan Tube well Rajasthan Tube well Yes Rajasthan Dug well Yes Rajasthan Handpump Yes Rajasthan Handpump Yes bdl Rajasthan Tube well Yes Rajasthan Handpump Rajasthan Tube well Rajasthan Tube well Yes bdl Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Dug well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes bdl Rajasthan Tube well Yes bdl Rajasthan Tube well Yes Rajasthan Tube well Yes bdl Rajasthan Tube well Yes Rajasthan Tube well Yes S15

16 Bundi 107 Bundi 108 Bundi 109 Bundi 110 Bundi 111 Kota 107 Kota 108 Kota 109 Bundi Crystalline Basement 101 Dausa Crystalline Basement 105 Dausa Crystalline Basement 106 Dausa Crystalline Basement 108 Dausa Crystalline Basement 109 Dausa Crystalline Basement 110 Dausa Crystalline Basement 111 Jai 120 Crystalline Basement Rajasthan Tube well Rajasthan Tube well Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Tube well Yes Rajasthan Handpump Yes bdl Rajasthan Tube well Yes bdl Rajasthan Handpump Yes bdl Rajasthan Handpump Yes bdl bdl Rajasthan Tube well Yes bdl Rajasthan Tube well Yes bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Tube well Yes bdl Rajasthan Handpump bdl bdl Rajasthan Tube well bdl bdl Rajasthan Handpump Yes bdl Rajasthan Tube well Yes bdl bdl Rajasthan Handpump bdl Rajasthan Handpump Yes bdl Rajasthan Handpump Yes bdl bdl S16

17 Jai 121 Crystalline Basement Jai-102 Crystalline Basement Jai-103 Crystalline Basement Jai-105 Crystalline Basement Jai-107 Crystalline Basement Jai-13 Crystalline Basement Jai-14 Crystalline Basement Jai-24 Crystalline Basement Raj-03 Crystalline Basement Ajmer Crystalline Basement 107 Ajmer Crystalline Basement 108 Ajmer Crystalline Basement 109 Ajmer Crystalline Basement 110 Bhil Crystalline Basement 101 Jai-110 Crystalline Basement Jai-117 Crystalline Basement Raj-07 Crystalline Basement Tonk- Crystalline Basement 102 Tonk- Crystalline Basement 104 Tonk- Crystalline Basement 107 Tonk- Crystalline Basement 109 Tonk- Crystalline Basement 111 Tonk- Crystalline Basement 112 Rajasthan Handpump Yes bdl bdl Rajasthan Tube well Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes Rajasthan Tube well Yes bdl Rajasthan Handpump Rajasthan Tube well Yes bdl Rajasthan Handpump bdl bdl Rajasthan Handpump bdl Rajasthan Tube well bdl bdl Rajasthan Handpump Yes bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump Yes 3929 OVER Rajasthan Handpump bdl bdl Rajasthan Handpump bdl bdl Rajasthan Handpump Yes bdl Rajasthan Handpump Yes bdl bdl Rajasthan Handpump bdl bdl Rajasthan Handpump Yes bdl S17

18 Tonk- Crystalline Basement Rajasthan Handpump bdl bdl Tonk- 114 Crystalline Basement Rajasthan Handpump Yes bdl Tonk- Crystalline Basement Rajasthan Handpump bdl bdl Tonk- 116 Crystalline Basement Rajasthan Tube well Yes bdl bdl Jod-22 Rhyolite Rajasthan Tube well Yes Jod-23 Rhyolite Rajasthan Tube well Yes Jod-24 Rhyolite Rajasthan Dug well Jod-25 Rhyolite Rajasthan Dug well Yes Jod-32 Rhyolite Rajasthan Dug well Yes Jod-33 Rhyolite Rajasthan Tube well Yes Rajk 01 Basalt 150 Gujarat Tube well Yes bdl bdl Rajk 05 Basalt 18 Gujarat Dug well bdl bdl Rajk 04 Basalt 90 Gujarat Handpump Yes bdl Rajk 10 Basalt 300 Gujarat Tube well Yes bdl bdl Rajk 06 Basalt 150 Gujarat Dug well bdl bdl Rajk 08 Basalt 130 Gujarat Tube well Yes bdl bdl Rajk 07 Basalt 160 Gujarat Tube well bdl bdl Rajk 03 Basalt 90 Gujarat Tube well Yes bdl Rajk 09 Basalt 120 Gujarat Tube well bdl bdl bdl 30.4 Rajk 02 Basalt 195 Gujarat Tube well Yes bdl bdl Meh 07 Layered Alluvial Aquifer 300 Gujarat Tube well bdl bdl Meh 05 Layered Alluvial Aquifer 330 Gujarat Tube well Yes bdl bdl Meh 06 Layered Alluvial Aquifer 330 Gujarat Tube well Yes bdl Meh 03 Layered Alluvial Aquifer 300 Gujarat Tube well bdl bdl Meh 02 Layered Alluvial Aquifer 270 Gujarat Tube well Meh 08 Layered Alluvial Aquifer 300 Gujarat Tube well bdl bdl Meh 04 Layered Alluvial Aquifer 270 Gujarat Tube well bdl bdl S18

19 Meh 13 Layered Alluvial Aquifer 300 Gujarat Tube well Yes bdl bdl Meh 10 Layered Alluvial Aquifer 457 Gujarat Tube well Yes bdl bdl Meh 01 Layered Alluvial Aquifer 300 Gujarat Tube well Yes bdl bdl Meh 09 Layered Alluvial Aquifer 270 Gujarat Tube well Yes bdl bdl Meh 11 Layered Alluvial Aquifer 300 Gujarat Tube well Yes bdl bdl Meh 12 Layered Alluvial Aquifer 350 Gujarat Tube well bdl bdl Pat 10 Layered Alluvial Aquifer 225 Gujarat Tube well bdl bdl Pat 14 Layered Alluvial Aquifer 260 Gujarat Tube well bdl bdl Pat 07 Layered Alluvial Aquifer 292 Gujarat Tube well Yes bdl bdl Pat 09 Layered Alluvial Aquifer 210 Gujarat Tube well bdl bdl Pat 12 Layered Alluvial Aquifer 305 Gujarat Tube well Yes bdl bdl Pat 11 Layered Alluvial Aquifer 310 Gujarat Tube well bdl bdl Pat 15 Layered Alluvial Aquifer 305 Gujarat Tube well bdl Pat 08 Layered Alluvial Aquifer 305 Gujarat Tube well Yes bdl bdl Pat 13 Layered Alluvial Aquifer 305 Gujarat Tube well Yes bdl bdl Pat 17 Layered Alluvial Aquifer 305 Gujarat Tube well bdl bdl bdl 1.3 Pat 06 Layered Alluvial Aquifer 320 Gujarat Tube well Yes bdl bdl Pat 16 Layered Alluvial Aquifer 275 Gujarat Tube well Yes bdl bdl Pat 21 Layered Alluvial Aquifer 260 Gujarat Tube well bdl bdl Pat 23 Layered Alluvial Aquifer 235 Gujarat Tube well bdl bdl bdl 1.7 Pat 25 Layered Alluvial Aquifer 200 Gujarat Tube well bdl bdl bdl 1.8 Pat 22 Layered Alluvial Aquifer 365 Gujarat Tube well bdl bdl bdl 1.4 Pat 26 Layered Alluvial Aquifer 300 Gujarat Tube well bdl bdl bdl 4.3 Pat 24 Layered Alluvial Aquifer 270 Gujarat Tube well bdl bdl 1.7 Pat 28 Layered Alluvial Aquifer 300 Gujarat Tube well Yes bdl bdl Pat 31 Layered Alluvial Aquifer 245 Gujarat Tube well Yes bdl bdl Pat 30 Layered Alluvial Aquifer 270 Gujarat Tube well Yes bdl 1.8 Pat 34 Layered Alluvial Aquifer 270 Gujarat Tube well Yes bdl 1.7 Pat 20 Layered Alluvial Aquifer 365 Gujarat Tube well Yes bdl bdl bdl 3.4 Pat 32 Layered Alluvial Aquifer 330 Gujarat Tube well Yes bdl bdl bdl 1.7 S19

20 Pat 29 Layered Alluvial Aquifer 240 Gujarat Tube well Pat 27 Layered Alluvial Aquifer 120 Gujarat Tube well bdl Gan 02 Layered Alluvial Aquifer 250 Gujarat Tube well Yes bdl bdl Ahme Layered Alluvial Aquifer 112 Gujarat Tube well bdl Ahme Layered Alluvial Aquifer 120 Gujarat Tube well Yes bdl bdl Ahme Layered Alluvial Aquifer 50 Gujarat Tube well bdl bdl Pat 03 Layered Alluvial Aquifer 210 Gujarat Tube well Yes bdl bdl Ahme Layered Alluvial Aquifer 50 Gujarat Tube well Yes bdl bdl Pat 35 Layered Alluvial Aquifer 330 Gujarat Tube well Yes bdl bdl 4.7 Pat 04 Layered Alluvial Aquifer 270 Gujarat Tube well Yes bdl bdl Gan 06 Layered Alluvial Aquifer 210 Gujarat Tube well Yes bdl bdl Gan 04 Layered Alluvial Aquifer 240 Gujarat Tube well Yes bdl bdl Gan 03 Layered Alluvial Aquifer 260 Gujarat Tube well bdl bdl Pat 37 Layered Alluvial Aquifer 182 Gujarat Tube well Ahme Layered Alluvial Aquifer 45 Gujarat Tube well Yes bdl bdl Pat 36 Layered Alluvial Aquifer 175 Gujarat Tube well Yes bdl Pat 02 Layered Alluvial Aquifer 240 Gujarat Tube well bdl Gan 07 Layered Alluvial Aquifer 230 Gujarat Tube well Yes bdl bdl Pat 01 Layered Alluvial Aquifer 270 Gujarat Tube well bdl bdl Ahme 01 Layered Alluvial Aquifer 213 Gujarat Tube well Yes bdl bdl Gan 05 Layered Alluvial Aquifer 245 Gujarat Tube well Yes Ahme Layered Alluvial Aquifer 215 Gujarat Tube well Yes bdl bdl Pat 05 Layered Alluvial Aquifer 300 Gujarat Tube well Yes bdl bdl Pat 38 Layered Alluvial Aquifer 330 Gujarat Tube well bdl Gan 01 Layered Alluvial Aquifer 269 Gujarat Tube well Yes bdl bdl bdl 0.3 Pat 19 Layered Alluvial Aquifer 295 Gujarat Tube well Yes bdl bdl bdl 3.1 Ahme 04 Layered Alluvial Aquifer 90 Gujarat Tube well Yes bdl bdl S20

21 Ahme Layered Alluvial Aquifer 140 Gujarat Tube well Yes bdl bdl Pat 18 Layered Alluvial Aquifer 365 Gujarat Tube well Yes bdl bdl bdl Crystalline Basement 90 Gujarat Tube well Yes bdl bdl Crystalline Basement 120 Gujarat Handpump Yes bdl bdl Crystalline Basement 60 Gujarat Tube well Yes Crystalline Basement 120 Gujarat Tube well Yes bdl bdl Crystalline Basement 200 Gujarat Tube well Yes bdl Crystalline Basement 60 Gujarat Tube well Yes bdl bdl Crystalline Basement 135 Gujarat Tube well Yes bdl bdl Crystalline Basement 90 Gujarat Tube well Yes Crystalline Basement 190 Gujarat Tube well Yes bdl bdl Crystalline Basement 60 Gujarat Handpump Yes Crystalline Basement 120 Gujarat Tube well Yes bdl Crystalline Basement 80 Gujarat Handpump Yes bdl Crystalline Basement 100 Gujarat Tube well Yes bdl bdl Crystalline Basement 120 Gujarat Tube well Yes bdl Crystalline Basement 70 Gujarat Tube well Yes bdl Crystalline Basement 120 Gujarat Tube well Yes bdl bdl Crystalline Basement 90 Gujarat Handpump Yes bdl bdl Crystalline Basement 80 Gujarat Tube well Yes bdl bdl Crystalline Basement 90 Gujarat Tube well Yes bdl bdl Crystalline Basement 60 Gujarat Tube well Yes bdl bdl Crystalline Basement 30 Gujarat Tube well Yes bdl bdl S21

22 16 Crystalline Basement 72 Gujarat Tube well Yes Bdl: Below detection limit. Instrument detection limits: Fe=0.07 mg/l, Mn=0.06 mg/l, U=0.001 μg/l, NO - 3 =0.01 mg/l Table S3: Uranium Isotope of groundwater investigated in this study Site U (µg/l) (234U/238U) AR +/- State District well depth (m) Aquifer Ahme Gujarat Ahmedabad 213 Layered Alluvial Ahme Gujarat Ahmedabad 50 Layered Alluvial Ahme Gujarat Ahmedabad 50 Layered Alluvial Gan Gujarat Gandhinagar 250 Layered Alluvial Meh Gujarat Mehsana 300 Layered Alluvial Pat Gujarat Patan 305 Layered Alluvial Pat Gujarat Patan 245 Layered Alluvial Rajk Gujarat Rajkot 130 Basalt Gujarat rkantha 120 Crystalline Basement Gujarat rkantha 30 Crystalline Basement Ahme Gujarat Ahmedabad 45 Layered Alluvial Gujarat rkantha 60 Crystalline Basement Gujarat rkantha 60 Crystalline Basement Ahme Gujarat Ahmedabad 90 Layered Alluvial Ahme Gujarat Ahmedabad 112 Layered Alluvial Gujarat rkantha 190 Crystalline Basement Pat Gujarat Patan 120 Layered Alluvial Ajmer Rajasthan Ajmer Unknown Crystalline Basement S22

23 Bhil Rajasthan Bhilwara Unknown Crystalline Basement Bundi Rajasthan Bundi Unknown Crystalline Basement Dausa Rajasthan Dausa Unknown Alluvium Dausa Rajasthan Dausa Unknown Crystalline Basement Dausa Rajasthan Dausa Unknown Crystalline Basement Jai Rajasthan Jaipur Unknown Alluvium Jai Rajasthan Jaipur Unknown Alluvium Jai Rajasthan Jaipur Unknown Alluvium Jai Rajasthan Jaipur Unknown Crystalline Basement Jai Rajasthan Jaipur Unknown Crystalline Basement Jai Rajasthan Jaipur Unknown Alluvium Jai Rajasthan Jaipur Unknown Alluvium Jai Rajasthan Jaipur Unknown Alluvium Jod Rajasthan Jodhpur Unknown Rhyolite Jod Rajasthan Barmer Unknown Alluvium Kota Rajasthan Kota Unknown Kota Rajasthan Kota Unknown Rajasthan Kota Unknown Tonk Rajasthan Tonk Unknown Alluvium Tonk Rajasthan Tonk Unknown Crystalline Basement Tonk Rajasthan Tonk Unknown Crystalline Basement Jai Rajasthan Jaipur Unknown Alluvium S23

24 Table S4. Statistical analysis of differences in U concentration populations for different lithological pairs using the Wilcoxon Rank Sum Test. P-values represent the probability of erroneously rejecting the null hypothesis (i.e., the median difference between the two populations is zero). For the box plot distribution of U in groundwater from these aquifers see Figure 2. Rajasthan Alluvium (n=135) Rajasthan Crystalline Basement (n=35) Rajasthan Rhyolite (n=6) Rajasthan Mixed Consolidated (n=50) Gujarat Alluvium (n=66) Gujarat Crystalline Basement (n=22) Gujarat Basalt (n=10) Rajasthan Alluvium <0.001 <0.001 <0.001 <0.001 Rajasthan Crystalline <0.001 <0.001 <0.001 <0.001 Basement Rajasthan Rhyolite <0.001 Rajasthan Mixed Consolidated <0.001 < Gujarat Alluvium <0.001 < Gujarat Crystalline <0.001 < <0.001 Basement Gujarat Basalt <0.001 <0.001 < <0.001 S24

25 Table S5. Spearman s rank correlations for nitrate versus uranium sorted by aquifer. Correlations significant at the 0.05 level are shown in bold. Aquifer p-value ρ Rajasthan Alluvium Rajasthan Crystalline Basement Rajasthan Rhyolite < Rajasthan < Gujarat Alluvium < Gujarat Crystalline Basement Gujarat Basalt Table S6. Spearman s rank correlations for bicarbonate versus uranium sorted by aquifer. Correlations significant at the 0.05 level are shown in bold. Aquifer p-value ρ Rajasthan Alluvium < Rajasthan Crystalline Basement < Rajasthan Rhyolite < Rajasthan < Gujarat Alluvium < Gujarat Crystalline Basement Gujarat Basalt S25

26 Table S7. Modeling of uranium speciation using PHREEQC software (llnl.dat), with (MUO 2 (CO 3 ) 3 2- and M 2 UO 2 (CO 3 ) 3 0 ) formation constants added manually. Calculations assume a pe value of 4. Sample U (molality) -2 CaUO 2 (CO 3 ) 3 0 Ca 2 UO 2 (CO 3 ) 3-2 MgUO 2 (CO 3 ) 3-4 UO 2 (CO 3 ) 3-2 UO 2 (CO 3 ) 2-2 SrUO 2 (CO 3 ) 3 Jai E % 19.4% 11.4% 6.3% 1.0% 0.6% Tonk E % 42.0% 6.8% 1.7% 1.1% 0.3% Ahme E % 3.4% 12.1% 24.1% 7.5% 1.8% Pat E % 53.2% 3.3% 1.1% 1.5% 0.2% Bundi E % 19.6% 15.2% 6.5% 0.7% 0.6% Gan E % 67.3% 1.9% 0.3% 0.3% 0.1% Tonk E % 11.5% 11.9% 14.6% 1.5% 1.4% Jai E % 75.1% 1.9% 0.3% 0.3% 0.1% E % 82.9% 0.7% 0.1% 0.7% 0.0% S26

27 Figure S1. Box plot of nitrate concentrations of groundwater from different aquifers in Rajasthan and Gujarat investigated in this study. Red lines represent the WHO s guideline values for nitrate in drinking water. te the large scale of nitrate contamination and exceedance of the drinking water guideline in most of the investigated groundwater. S27

28 Figure S2. Uranium versus nitrate concentrations of groundwater investigated in this study sorted by aquifer lithology. te for the lack of direct correlations between uranium and nitrate. For statistical analysis see Table S5. S28

29 Figure S3: Uranium and 238 U/ 234 U activity ratio variations with depth of groundwater from Gujarat alluvial aquifers. te the relatively decrease of uranium concentrations (p-value=0.009, ρ=-0.319) and increase of 238 U/ 234 U activity ratios (p-value=0.003, ρ= ) with depth. S29

30 References (1) Ajay, K.; Manpreet, K.; Rohit, M.; Sumit, S.; Rosaline, M.; Singh, K. P.; Bajwa, B. S. Quantification and Assessment of Health Risk Due to Ingestion of Uranium in Groundwater of Jammu District, Jammu & Kashmir, India. J. Radioanal. Nucl. Chem. 2016, 310, (2) Singh, P.; Singh, P.; Sahoo, B. K.; Bajwa, B. S. A Study on Uranium and Radon Levels in Drinking Water Sources of a Mineralized Zone of Himachal Pradesh, India. J. Radioanal. Nucl. Chem. 2016, 309, (3) Sharma, S.; Kumar, A.; Mehra, R.; Mishra, R. Ingestion Doses and Hazard Quotients Due to Intake of Uranium in Drinking Water from Udhampur District of Jammu and Kashmir State, India. Radioprotection 2017, 52, (4) Singh, S.; Rani, A.; Mahajan, R. K.; Walia, T. P. S. Analysis of Uranium and Its Correlation with Some Physico-Chemical Properties of Drinking Water Samples from Amritsar, Punjab. J. Environ. Monit. 2003, 5, (5) Saini, K.; Singh, P.; Bajwa, B. S. Comparative Statistical Analysis of Carcinogenic and n-carcinogenic Effects of Uranium in Groundwater Samples from Different Regions of Punjab, India. Appl. Radiat. Isot. Instrum. Methods Use Agric. Ind. Med. 2016, 118, (6) Singh, K. P.; Kishore, N.; Tuli, N.; Loyal, R. S.; Kaur, M.; Taak, J. K. Uranium Contamination of Groundwater in Southwest Parts of Punjab State, India, with Special Reference to Role of Basement Granite. In Clean and Sustainable Groundwater in India; Springer Hydrogeology; Springer, Singapore, 2018; pp (7) Alrakabi, M.; Singh, G.; Bhalla, A.; Kumar, S.; Kumar, S.; Srivastava, A.; Rai, B.; Singh, N.; Shahi, J. S.; Mehta, D. Study of Uranium Contamination of Ground Water in Punjab State in India Using X-Ray Fluorescence Technique. J. Radioanal. Nucl. Chem. 2012, 294, (8) Rishi, M. S.; Keesari, T.; Sharma, D. A.; Pant, D.; Sinha, U. K. Spatial Trends in Uranium Distribution in Groundwaters of Southwest Punjab, India - A Hydrochemical Perspective. J. Radioanal. Nucl. Chem. 2017, 311, (9) Bhalla, A.; Singh, G.; Kumar, S.; Shahi, J. S.; Mehta, D. Elemental Analysis of Ground Water from Different Regions of Punjab State (India) Using EDXRF Technique and the Sources of Water Contamination Int. Conf. Environ. Comput. Sci. 2011, 19, (10) Sharma, N.; Singh, J. Human kidney and skeleton uranium burden, radiation dose and health risks from high uranium contents in drinking water of bathinda district (malwa region) of punjab state, india. Radiat. Prot. Dosimetry 2017, 176, (11) Virk, H. Measurement of Concentration of Natural Uranium in Ground Waters of Bathinda District (S. Punjab) for the Assessment of Annual Effective Dose; (12) Bajwa, B. S.; Kumar, S.; Singh, S.; Sahoo, S. K.; Tripathi, R. M. Uranium and Other Heavy Toxic Elements Distribution in the Drinking Water Samples of SW-Punjab, India. J. Radiat. Res. Appl. Sci. 2017, 10, (13) Singh, L.; Kumar, R.; Kumar, S.; Bajwa, B. S.; Singh, S. Health Risk Assessments Due to Uranium Contamination of Drinking Water in Bathinda Region, Punjab State, India. Radioprotection 2013, 48, S30

31 (14) Saini, K.; Bajwa, B. S. Uranium Distribution Study in the Drinking Water Samples of SW Punjab, India. Adv. Appl. Sci. Res. 2016, 7, (15) Saini, K.; Duggal, V.; Bajwa, B. S. Assessment of Radiation Dose Due to Intake of Uranium through Groundwater and Its Carcinogenic and n-carcinogenic Risks in Southwest and rtheast Punjab, India. Indoor Built Environ. 2017, X (16) Kumar, A.; Rout, D.; Narayanan, U.; Mishra, M.; Tripathi, R.; Singh, J.; Kumar, S.; Kushwaha, H.. Geochemical Modeling of Uranium Speciation in the Subsurface Aquatic Environment of Punjab State in India. J. Geol. Min. Res. 2011, 3, (17) Sharma, D. A.; Rishi, M. S.; Keesari, T.; Pant, D.; Singh, R.; Thakur, N.; Sinha, U. K. Distribution of Uranium in Groundwaters of Bathinda and Mansa Districts of Punjab, India: Inferences from an Isotope Hydrochemical Study. J. Radioanal. Nucl. Chem. 2017, 313, (18) Sharma, N.; Singh, J. Radiological and Chemical Risk Assessment Due to High Uranium Contents Observed in the Ground Waters of Mansa District (Malwa Region) of Punjab State, India: An Area of High Cancer Incidence. Expo. Health 2016, 8, (19) Pant, D.; Keesari, T.; Sharma, D.; Rishi, M.; Singh, G.; Jaryal, A.; Sinha, U. K.; Dash, A.; Tripathi, R. M. Study on Uranium Contamination in Groundwater of Faridkot and Muktsar Districts of Punjab Using Stable Isotopes of Water. J. Radioanal. Nucl. Chem. 2017, 313, (20) Virk, H.; Jakhu, R.; Bangotra, P. Natural Uranium Content in Ground Waters of Mohali and Fatehgarh Districts of rth Punjab (India) for the Assessment of Excess Cancer Risk. Glob. J. Hum.-Soc. Sci. B Geogr. Geo-Sci. Environ. Sci. Disaster Manag. 2016, 16, (21) Virk, H. Uranium Content Anomalies in Groundwaters of Fazilka District of Punjab (India) for the Assessment of Excess Cancer Risk. Res. Rev. J. Oncol. Hematol. 2017, 6, (22) Krishan, G.; Lapworth, D.; Someshwar Rao, M.; Kumar, C. P.; Smilovic, M.; Semwal, P. Natural (Baseline) Groundwater Quality In The Bist-Doab Catchment, Punjab, India: A Pilot Study Comparing Shallow and Deep Aquifers. Int. J. Earth Sci. Eng. 2014, 7, (23) Lapworth, D. J.; Krishan, G.; MacDonald, A. M.; Rao, M. S. Groundwater Quality in the Alluvial Aquifer System of rthwest India: New Evidence of the Extent of Anthropogenic and Geogenic Contamination. Sci. Total Environ. 2017, , (24) Tripathi, R. M.; Sahoo, S. K.; Mohapatra, S.; Lenka, P.; Dubey, J. S.; Puranik, V. D. Study of Uranium Isotopic Composition in Groundwater and Deviation from Secular Equilibrium Condition. J. Radioanal. Nucl. Chem. 2013, 295, (25) Singh, J.; Singh, H.; Singh, S.; Bajwa, B. S. Estimation of Uranium and Radon Concentration in Some Drinking Water Samples of Upper Siwaliks, India. Environ. Monit. Assess. 2009, 154, (26) Virk, H. Uranium Anomalies in Groundwater of Sangrur District of Punjab (India) for Cancer Risk Assessment. Curr. Sci. 2017, 113, S31

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