Accepted Manuscript

GIS mapping-based impact assessment of groundwater contamination by arsenic

and other heavy metal contaminants in the Brahmaputra River valley: A water quality
assessment study

B.K. Nath, C. Chaliha, B. Bhuyan, E. Kalita, D.C. Baruah, A.K. Bhagabati

PII: S0959-6526(18)32420-X
DOI: 10.1016/j.jclepro.2018.08.084
Reference: JCLP 13868

To appear in: Journal of Cleaner Production

Received Date: 30 November 2017

Revised Date: 4 July 2018
Accepted Date: 8 August 2018

Please cite this article as: Nath BK, Chaliha C, Bhuyan B, Kalita E, Baruah DC, Bhagabati AK, GIS
mapping-based impact assessment of groundwater contamination by arsenic and other heavy metal
contaminants in the Brahmaputra River valley: A water quality assessment study, Journal of Cleaner
Production (2018), doi: 10.1016/j.jclepro.2018.08.084.

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 1 Title: GIS mapping-based impact assessment of groundwater contamination by arsenic and other heavy metal contaminants

2 in the Brahmaputra River valley: A water quality assessment study.

3 ACCEPTED MANUSCRIPT
B.K. Natha, C. Chalihaa, B. Bhuyanb, E. Kalitaa*, D.C. Baruahc and A.K. Bhagabatib

4 a. Department of Molecular Biology and Biotechnology, Tezpur University, Tezpur, Assam, 784028, India

5 b. Department of Geology, Gauhati University, Guwahati, Assam, 781014, India

6 c. Department of Energy, Tezpur University, Tezpur, Assam, 784028, India

7 *Corresponding author. Tel.: +91 3712 275411

8 E-mail address: ekalita@tezu.ernet.in

9 Abstract:

10 Groundwater aquifers serve as the primary source of potable water for the vast majority of the population in the Brahmaputra

11 River valley. However, these groundwater reserves form a substantial part of a rapidly weathering alluvial drainage resulting in major

12 contamination by Arsenic (As) and associated heavy metals thereby raising key concern on their safety and sustained usage. The

13 current study entails a comprehensive qualitative analysis of the potable groundwater reserves using a combination of geographical

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14 information system (GIS) and geochemical approaches to determine the severity of groundwater contamination by As and other heavy

15 metals in a total of twenty administrative districts of Assam, India. Furthermore, the groundwater solute chemistry and water quality

16 status in the 20 districts of the study area, which encompasses the Brahmaputra River valley, was also assessed to evaluate the

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17 sustainability of these potable groundwater reserves. The findings show that the groundwater aquifers present in these districts of the

18 Brahmaputra valley in Assam are severely contaminated with As with the highest concentration at ~352.56 ppb being observed in the

19 district of Nagaon. The districts of Tinsukia, Dibrugarh, Sivasagar, Dhemaji, Lakhimpur, Jorhat, Golaghat, Sonitpur, Nagaon, Morigaon,

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20 Darrang, Udalguri, Kamrup, Nalbari, and Baksa also showed the presence of elevated levels of dissolved As which on an average

21 exceeded the WHO permissible limit of 10 parts per billion as well as the Bureau of Indian Standards limit of 50 parts per billion.

22 Moreover, notable contamination by other heavy metals including lead, manganese, iron, and zinc exceeding the WHO and BIS

23 prescribed limits were prominent. Also, the groundwater was found to harbour elevated concentrations of ions such as HCO3-, Ca2+ and

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24 Mg2+ which impart severe restrictions on to the safety, aesthetics and palatability of these potable water reserves. Furthermore, the

25 dissolved As content was found to exhibit a significant correlation to the pH of the water source as well as to other elemental
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26 contaminants such as iron and manganese suggesting that the reductive dissolution of iron oxyhydroxides may serve as the underlying

27 mechanism for the As enrichment of these groundwater reserves. Additionally, the impact assessment study through the spatial

28 distribution of the groundwater quality index (GWQI) of the areas studied showed that the groundwater reserves in the majority of the

29 administrative districts are unfit for human consumption, without the intervention through requisite water treatment and/or sustainable
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30 remediation approaches. These findings indicate the need for serious introspection and reconsiderations on the part of the stakeholders

31 for the sustainable use of these groundwater resources for anthropogenic activities.

32 1. Introduction.
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33 Potable fresh-water water reserves are becoming exceedingly limiting owing to the increase in human population, climate change

34 effects and varied anthropogenic activities like agriculture, mining, earthmoving etc. (Chakraborti et al., 2017). The situation is further
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35 aggravated by the presence of contaminants and pollutants, which include several heavy metals and chemical residues from

36 agricultural/industrial discharges, in the available water resources. In the context of north-eastern India and more specifically the

37 Brahmaputra River valley, Arsenic (As) is the major pollutant of groundwater aquifers. Consequently, the major symptoms of the

38 chronic As exposure, Arsenicosis, such as neurotoxicity, mutagenic and carcinogenic anomalies, developmental defects and
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39 cardiovascular disorders, dermal lesions, peripheral neuropathies, portal fibrosis and adverse birth outcomes, are evident among the

40 people in this region (Abdul et al., 2015). Furthermore, the Northeastern Region of India has been identified as one of the twenty

41 geological provinces worldwide (Mukherjee et al., 2009) that exceed the 10 gL-1 threshold for the presence of As in groundwater
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 1 reserves, as recommended by World Health Organization (WHO). Recent studies show that the increased depletion of the

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groundwater aquifers further contributes towards the increasing concentration of the As and other heavy metals in the groundwater

3 reserves, posing serious questions on its sustainable use by the residents of the region (Macdonald et al., 2016). Therefore, the

4 periodic monitoring of these groundwater aquifers is highly imperative for the fine-tuning of the management practices of this water

5 resource, in a risk-free manner.

6 Studies conducted till date indicate the presence of As, beyond threshold limits, in most of the northeastern states of India

7 viz. Arunachal Pradesh, Nagaland, Manipur, Tripura and Assam (Saurav et al., 2015; Borah et al., 2016; Chandrasekhar et al.,

8 2016). With the advent of Geographical Information Systems (GIS) technologies, the mapping of heavy metal contaminated

9 groundwater zones have facilitated a better understanding of the geochemical origin of such contaminants in groundwater sources

10 (Ganapuram et al., 2009, Asadi et al., 2007). In this context, very limited studies have been carried towards the development of

11 geospatial maps that report the distribution of these contaminants along the Brahmaputra River valley, which can also illustrate the role

12 of varied geogenic and anthropogenic factors contributing to their augmentation in the potable groundwater aquifers of these areas

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13 (Saurav et al., 2015; Das et al., 2015, Haloi and Sharma, 2011). The current study is therefore aimed towards the assessment of the

14 groundwater levels of As, as well as other heavy metal contaminants like Lead (Pb), Iron (Fe), Copper (Cu), Zinc (Zn) and Manganese

15 (Mn) in the Brahmaputra River valley of Assam, comprising of twenty independent administrative districts, in order to gain a

16 comprehensive insight on the groundwater quality and its suitability for potable use. Moreover, attempts were also made to evaluate

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17 possible interrelationships between the key water quality parameters such as groundwater source depth, source pH and the

18 concentration of heavy metals with As contamination. Additionally, the major groundwater solute chemistry in the study area was also

19 investigated by the estimation of commonly prevalent ions and dissolved solids in order to propose the possible mechanism controlling

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20 the mobility of As in the groundwater in these areas. Furthermore, a comprehensive Groundwater Quality Index was developed for the

21 area under study and collated with the GIS map data to offer a simple yet informative overall insight into the quality status of the

22 groundwater in the Brahmaputra River valley.

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23 2. Background information on the Study Area:

24 The state of Assam has been reasonably well studied for the distribution and contamination of As in the existing water systems, for as
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25 many as twenty-one districts. Earlier studies conducted in this region indicate the presence of significantly high As concertation in the

26 groundwater systems of the Brahmaputra River valley (Tamuli et al., 2017; Kumar et al., 2017; Choudhury et al.,2017; Borah et al.,

27 2016; Sailo and Mahanta, 2016; Mahanta et al., 2015). However, most of these studies have been conducted in non-overlapping

28 areas within Assam and the only comprehensive report on As contamination, based on the survey of ~17 districts, is by Verma et al.,
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29 2016. The present study area (Fig. 1) covers the entire Brahmaputra River valley, lying between 26014’11” to 27031’59” North latitude

30 and 90015’12” to 94035’44” East longitude, with a total geographical area of 44514 km2. It comprises of twenty (20) independent

31 administrative districts (2017) of Assam ranging from Dhubri located in the south-west of the Brahmaputra valley to Tinsukia in the
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32 upper north-east and encompasses the Northwestern (NW) and northern (N) provenances along the eastern Himalayas. The major

33 factors contributing to the enhancement of As in groundwater sources in the region are believed to be the result of geochemical

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processes of rock formation and associated hydrogeological parameters that stand to influence the groundwater reserves along the

35 Brahmaputra riverine system. In this context, the chemical composition of surface water that recharges the groundwater aquifers, the

36 geochemical interactions between aquifer water and the alluvial matrices, residence time and the presence of reactive organic matter

37 have been reported to strongly influence As enrichment of groundwater reserves in the region (Mukherjee et al., 2009; Mukherjee et
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38 al., 2012; Verma et al., 2016). Additionally, the denudation rate of the Brahmaputra river basin, considered one of the highest globally,

39 and the erosion of the East-West Himalayan range caused by the Tsangpo–Siang–Brahmaputra drainage system are the other major

40 contributors of As enrichment of groundwater reserves in this region (Verma et al., 2016; Galy and France-Lanord, 2001; Sarin et al.,

41 1989).
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 1 The Brahmaputra River valley is surrounded by the Eastern Himalayan belt on the North and the East, while the southern and

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south sides are bounded the Naga-thrust belt and the Shillong Plateau respectively (Verma et al., 2016). The river Brahmaputra,

3 originates in the north of the Himalayas at an elevation of approximately 5200 m at Mt. Kailash, as a profound glacier mass. It then

4 flows through Tibet, along with the depression of the Indus–Tsangpo suture zone, and further through the Namche Barwa syntaxis, to

5 enter the Indian state of Arunachal Pradesh as the Dihang or Siang river (Verma et al., 2016; Verma et al., 2015). The Dihang

6 progresses further towards a sharp turn directed south-west to enter into the alluvial floodplains of Assam. At this juncture, it is known

7 as the Brahmaputra River, where it follows a braided riverine course. The area under study being geographically close to the fertile

8 floodplains of the Brahmaputra, shelters the majority of the agrarian communities in the state, housing an estimated population of

9 ~24607308 individuals (Table 1). The area receives a substantially high annual rainfall of 2387 mm (Table 1) and the geomorphology is

10 dominated by flat alluvial plains, comprising both younger and older alluvium. The area also features low altitude structural hills in the

11 areas bordering Meghalaya, Arunachal Pradesh and Bhutan.

12 The Brahmaputra alluvial floodplains in the state of Assam is primarily bounded by two different orogenic belts viz. the

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13 Himalayan orogenic belt including the trans-Himalayan range in the north and the north-east direction and Indo–Burmese ranges in the

14 south and the south-east. Numerous tributaries of the Brahmaputra, often carrying sediments from various rock types, join the main

15 river area from different directions to deposit the eroded sediments into the Brahmaputra basin. In the Indus–Tsangpo Suture zone, the

16 flow of these primary river channels and the associated tributaries result in the erosion of plutonic and volcanic rocks of Trans-

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17 Himalayan batholith as well as the Paleozoic-Eocene sedimentary rocks (Goodbred et al., 2014). As the riverine flow is further directed

18 towards the eastern syntaxis, the river channels traverse the highly metamorphosed Transhimalayan Plutonic Belt comprising of meta-

19 volcanic rocks, granite, granodiorite, diorite, tonalite, and leucogranite (Singh and France-Lanord, 2002). The Brahmaputra also

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20 receives numerous tributaries from the North Himalayan slopes such as the Subansiri, the Jia-Bhoreli, the Puthimari, the Manas and

21 the Tipkai which result in the drainage of metamorphic rocks, igneous rocks and sedimentary rock sequences. Also, other tributaries

22 flowing through the Higher Himalayas, the Lesser Himalayas and the Sub-Himalayas (Siwaliks) encroach high- grade schists and

23 gneisses rocks, medium to high-grade metamorphic rocks and rocks of the Carboniferous-Permian strata predominated by quartzite,

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24 phyllite, slate, sandstone, shale, arenite, coal beds, and conglomerates before draining into the primary river channel (Verma et al.,

25 2016). These deposits primarily function as aquifers in the study area and contribute towards the enrichment of various metals in the
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26 groundwater reserves depending upon the source geochemistry.

27 The As enrichment of groundwater reserves in the Brahmaputra Valley has been often attributed as a consequential artifact

28 of interactions between various bio-geochemical processes. However, the information on sustained assessment of As enrichment along

29 this highly populous region is rather limiting. Further, studies that explore the possible interactions/correlation of As with respect to the
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30 other major elemental contaminants like Iron (Fe), Lead (Pb), Copper (Cd), Manganese (Mn) and Zinc (Zn) across the Brahmaputra

31 River valley are very few in number (Mahanta et al., 2015; Kakati, 2012; Chakrabarty et al., 2011; Buragohain et al., 2010).

32 Moreover, groundwater aquifers serve as the primary source for drinking water for the majority of the resident population across the
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33 entire Brahmaputra River valley. However, very limited research has been undertaken on the groundwater quality assessment in the

34 entire region and studies that offer an overall insight into the sustainability of groundwater reserves for domestic and/or agricultural use
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35 are thereby very few in number (Haloi and Sharma 2012; Kakati and Sharma, 2007).
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2 Fig. 1. Location map of the study area generated using ArcGIS software.
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 1 Table 1. Geographical area, resident population and average annual rainfall for the area under study

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2 (http://cgwb.gov.in/District_Profile/Assam_districtprofile.html)

Geographical area Population Average annual rainfall

District
(Km2) (2011 census) (mm)

Tinsukia 3790.0 1316948 2323

Dibrugarh 3381.0 1327748 2819
Sivasagar 2668.0 1150253 2400
Dhemaji 3237.0 688077 3435
Lakhimpur 2277.0 1040644 3268
Jorhat 2851.0 1091295 1867
Golaghat 3502.0 1058674 2119
Sonitpur 5280.6 1925975 2173
Nagaon 4110.3 2826006 1541
Morigaon 1551.0 957853 1770

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Darrang 1630.0 764300 2127
Udalguri 1673.9 832769 2000
Kamrup 4111.0 2777621 2127
Nalbari 2257.0 1148824 1904

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Baksa 2007.5 953773 2972
Barpeta 2677.0 169319 2051
Bongaigaon 1725.3 732639 3219
Goalpara 1842.0 1008959 2169

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Kokrajhar 3165.4 886999 3100
Dhubri 1664.1 1948632 2363

3 3. Materials and Methods:

4 3.1. Sampling and analyses protocols.

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5 Groundwater samples were collected from a total of twenty administrative districts located in the area under study. The sampling sites

6 were selected in a manner to represent the different geological formations, depth as well as incorporate anthropogenic input from
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7 agricultural areas located in the vicinity. Deep tube wells accounting for a depth of more than ~60 ft. were primarily selected as the

8 desired source for the groundwater samples. However, a few locations accounting for depth in the range below 60 ft. were also taken

9 into consideration to ascertain a possible correlation between water depth and the concentration of As present. The sampling was
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10 carried out in accordance to methods well documented in the literature (Kumar et al., 2017, Verma et al., 2016, Chetia et al., 2011).

11 The containers used for the storage of collected groundwater samples were rinsed three times with the water to be sampled prior to

12 collection to reduce the chances of Type I errors in analysis. The water was pumped out for about 5-10 minutes to reduce the

13 interference of oxygen and to remove the stagnant/residual water present. The pH of the collected samples was measured
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14 instantaneously in the field using an Oakton pHTestr10 portable pH meter from Eutech Instruments. Subsequently, the collected

15 samples were acidified with hydrochloric acid (HCl) and nitric acid (HNO3) in a ratio of 3:1 ml for every 100 ml of the water sample. The
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16 acidified samples were then adequately cataloged, given appropriate identification tags and stored at ~40C, away from sunlight to

17 prevent photo-oxidation till they were analyzed. Further, the geographical coordinates of the sample sites were acquired with the help of

18 a handheld GPS and were utilized for the GIS-based geospatial modeling of the groundwater sample collection sites.
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19 The total As content of the collected groundwater samples was analyzed using an Agilent MP-4200 atomic emission

20 spectrophotometer after proper calibration with standards (Tanabe et al., 2016). The instrument was subsequently calibrated for every

21 fifty measurements to rule out calibration errors. The estimated As concentrations of the samples were tabulated and the standard error

22 in each measurement was accounted for. Earlier studies conducted by various researchers indicate the presence of heavy metal
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 1 contaminants including Iron (Fe) along with other heavy metals viz. Lead (Pb), Copper (Cu), Manganese (Mn) and Zinc (Zn),) in the

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area under study (Chakrabarty et al., 2011). Therefore, the collected groundwater samples were also assessed for the presence of

3 these elemental impurities to enable the identification of the locations harbouring high values of the respective contaminant in

4 accordance to the permissible limits exercised by World Health Organization (WHO) & Bureau of Indian Standards (BIS).

5 3.2. Development of spatial distribution maps and correlation analysis.

6 To measure the spatial variability of the groundwater dataset, the observed values were subjected to spatial interpolation using the

7 Inverse Distance Weighting (IDW) approach built within the ArcGIS 10.3.1 desktop application. The resultant output was used for the

8 illustration of the magnitude and the distribution of various contaminants across the Brahmaputra River valley in the form of geospatial

9 distribution maps using the ArcGIS 10.3.1 mapping suite. Also, correlations between the concentration of As in the groundwater

10 samples and other elemental contaminants was assessed by establishing the coefficient of determination using the IBM SPSS 21

11 statistical package. Similar studies were also carried out to establish a possible correlation between the concentration of As in the

12 groundwater samples and geographical parameters viz. source depth and the pH of the groundwater source.

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13 3.3. Estimation of commonly prevalent ions and total dissolved solids in the collected groundwater samples.

14 Commonly prevalent cations viz. Na+, K+ and Ca2+ were also analyzed using the Agilent MP-4200 atomic emission spectrophotometer

15 while anions such as Cl-, SO42-, CO3- and HCO3- were analyzed using methods reported earlier (Singh et al., 2012; A.P.H.A. 1998).

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16 The total dissolved solids in the groundwater samples were analyzed in accordance with Method 160.1, USEPA. The total anion

17 concentration, total cation concentration and the percentage of total dissolved solids present in the collected groundwater samples

18 were further utilized for the generation of Piper diagram using the RockWorks 16.0 hydrogeological suite to offer a representative

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19 analysis of the groundwater solute chemistry for the districts under study.

20 3.4. Groundwater quality analysis

21 In order to conform to national and international quality standards, the groundwater quality of the study area was assessed by using the

22 Groundwater Quality Index (GWQI) (Vasanthavigar et al. 2010). The model equation used for the determination of GWQI is described

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23 below:

w C
GWQI =  SI = 
W x q =     x  x 100
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∑  w S

24 where qi is the groundwater quality rating point, Ci is the concentration of each parameter assessed and Si is the WHO standard for the

25 given parameter. The water quality status of the groundwater samples was subsequently determined on the basis of their GWQI values

26 as follows:
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27 Table 2. Classification of Groundwater quality on the basis of GWQI values (Vasanthavigar et al. 2010)

GWQI range Groundwater quality

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0 – 50 Excellent
50 – 100 Good
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100 – 200 Poor

> 200 Very poor

28 The indexed groundwater quality data was further subjected to spatial interpolation via an Inverse distance weighting (IDW) matrix built

29 within the ArcGIS 10.3.1 desktop application and used for the generation of a spatial distribution map of the Brahmaputra River valley in
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30 order to reflect upon the status of the groundwater quality encompassing the twenty independent districts under study.

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 1 4. Results and discussions.

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4.1. Distribution of Arsenic and heavy metals.

3 A total of two hundred (200) groundwater samples were collected from the study area and were stringently analyzed for the presence of

4 As and other heavy metals. The distribution of groundwater contaminants in any area is primarily controlled by geochemical

5 heterogeneity. Consequently, spatial interpolation techniques such as Inverse distance weighting (IDW) method, Kriging method etc.

6 are often used for the estimation of pollutants at unknown sampling sites to provide a comprehensive representation of their geogenic

7 distribution (Islam et al., 2017; Bhattacharya et al., 2011). Hence, the data from the analysis of the contaminant levels were geo-

8 referenced and spatially interpolated using an IDW approach for the generation of GIS-aided spatial maps to represent the source and

9 distribution of each of the contaminants. The majority of the administrative districts such as Tinsukia, Dibrugarh, Sivasagar, Dhemaji,

10 Lakhimpur, Jorhat, Golaghat, Sonitpur, Nagaon, Morigaon, Darrang, Udalguri, Kamrup, Nalbari, and Baksa (Fig. 2a, S3a) were found to

11 harbour dissolved As beyond the WHO/BIS guideline values. A total of one hundred and twenty-six (126) groundwater samples were

12 observed to contain dissolved As beyond the WHO permissible limit of 0.01 mgL-1 (10 ppb) while one hundred and nine (109) samples

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13 showed As concentration beyond the Bureau of Indian Standards (BIS) maximum tolerable limit of 50 ppb (Table S1). The total As

14 content in the studied samples was found to vary from ≤ 0.5 parts per billion to ≤ 353 parts per billion and the highest concentration of

15 As at ~352.56 parts per billion was recorded from a sampling site located in the district of Nagaon (Table S1).

16 Other heavy metals analyzed for the collected groundwater samples also showed a wide range of variation. Lead (Pb) was

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17 found to vary from 0.01-0.25 parts per million (Fig. 2b) and a total of fifty-two (52) groundwater samples tested positive for

18 concentrations of dissolved Lead exceeding the WHO and BIS permissible limit of 0.01 parts per million (Table S2). Pb has no

19 beneficial effect on humans and chronic exposure to Pb over an extended period of time has severe health effects like bioaccumulation

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20 in the bone/connective tissue, often leading to pathological implications of the nervous system (Patrick, 2006). The samples from the

21 districts of Tinsukia, Dibrugarh, Golaghat, Jorhat, Nalbari and Sivasagar were found to have an average Pb concentration that was

22 beyond the BIS maximum threshold of 0.01 parts per million. (Fig. 2b, S3b). Iron (Fe) has been noted to be one of the most disturbing

23 constituents in potable water sources throughout India. The high concentration of Fe in water sources may promote the growth of

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24 pathogenic and non-pathogenic microflora often leaving a slimy coating in containers, reservoirs and irrigation ducts and pipelines

25 (Borah et al., 2010). The range of dissolved Fe in the collected groundwater samples varied from 0.02-55.63 parts per million (Fig.
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26 S1a) and was found to be well beyond the WHO and BIS permissible limit of 0.3 parts per million across the majority of the districts in

27 the study area (Table S2). Further, the samples from the districts of Baksa, Darrang, Nagaon, Lakhimpur and Sonitpur were found to

28 harbour the highest average concentrations (Fig. S1a, S3c). Copper (Cu) concentrations varied from 0.0-0.24 parts per million (Fig.

29 S1b, S3d) and were found to be well within the maximum permissible threshold of 1.5 parts per million (Table S2) as described by the
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30 Indian Standard-specifications for drinking water (BIS 2012). Zinc (Zn), even though an essential micronutrient, is known to result in

31 gastric erosion, impairment of various immune responses and decline in high-density lipoprotein cholesterol levels in serum at

32 concentrations exceeding 50 parts per million (WHO 2004). Dissolved Zn varied from 0.0-31.86 parts per million (Fig. 3a, S3e) in the
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33 collected groundwater samples and a total of sixteen (16) samples were found to contain Zn in the range exceeding the BIS maximum

34 tolerable limit of 15 parts per million (Table S2). Manganese (Mn) was found to vary from 0.0-4.54 parts per million (Fig. 3b) and a total
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35 of one hundred and fifty-two (152) groundwater samples were found to contain dissolved Mn at concentrations beyond the WHO

36 permissible limit of 0.4 parts per million (Table S2). However, toxicological effects of Mn are recognized as a health hazard only at

37 concentrations that are ≥10 times the desired value (WHO 2004). Thus the groundwater samples from the districts of Dhemaji, Nagaon,

38 Morigaon and Kokrajhar were deemed hazardous for potable use (Fig. 3b, S3f). Additionally, the majority of sources for the
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39 groundwater samples collected in the vicinity of the Brahmaputra floodplains were found to exhibit pH in the range 6.1-8.0 (Fig. S2a)

40 and have an average depth in the range 40-80 ft (Fig. S2b).

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1 Very few reports on the correlation of dissolved As with other elemental contaminants and/or source parameters such as

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depth and pH across the Brahmaputra River valley are currently available. Statistical correlation studies were thus carried out to

3 determine the

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2 Fig. 2. Spatially interpolated distribution maps (using IDW approach) showing the distribution of groundwater Arsenic (a) and Lead (b) in the Brahmaputra River valley.

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2 Fig. 3. Spatially interpolated distribution maps (using IDW approach) showing the distribution of groundwater Zinc (a) and Manganese (b) in the Brahmaputra River valley.

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1 degree of association between the observed values for As and other the heavy metals detected. The dissolved As was found to

2 show a strong correlation with Fe [R2: 0.92] and Mn [R2: 0.95] (Fig. 4 a, b) but showed very weak correlations with Pb [R2: 0.03],

3 Cu [R2: 0.02] and Zn [R2: 0.13] (Fig. S4 a, b, c). Additionally, a very weak correlation [R2: 0.06] was observed between the

4 dissolved As and the source depth for the groundwater samples studied (Fig. S4d). This may be attributed to the asymmetrical

5 distribution of As-enriched alluvium across the geogenic layers of the Brahmaputra River valley (Verma et al., 2015). Further, the

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6 correlation between dissolved As and the groundwater pH [R2: 0.72] was also found to be insignificant (Fig. S4e).

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8 Fig. 4. Statistical correlation studies for the determination of association between the concentration of Arsenic and the
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9 concentration of Iron (a) and Manganese (Mn) in the groundwater samples.

10 4.2. Distribution of commonly prevalent cations and anions

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11 The mobilization of As in the groundwater aquifers is controlled by several hydro-geochemical processes (Verma et al., 2016). The

12 correlation of dissolved As content of the samples to other redox-sensitive parameters such as the values of dissolved Fe, Mn,
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13 available cations and anions etc. play a crucial role in the understanding of the mechanism of As enrichment in the area under

14 study (Van Geen et al., 2004; Mukherjee and Fryar, 2008). Hence, the concentration of commonly prevalent cations viz. Ca2+,
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15 Mg2+, Na2+ and K+, and commonly prevalent anions viz. Cl-, SO42-, CO3- and HCO3- were determined for the collected groundwater

16 samples. The average concentration of Ca2+ ions was found to be ~77 mgL-1 (Table S3) whereas the average concentration of Mg2+

17 ions in the area under study was found to be ~6 mgL-1 (Table S3), well within their BIS guideline values of 200 mgL-1 and 100 mgL-
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18 . Moreover, the average concentrations of Cl- ions and SO42- ions were found to be ~12 mgL-1 and ~2 mgL-1 (Table S3) which were

also well within the BIS desirable limits of 1000 mgL-1 and 400 mgL-1. Furthermore, the concentration of total dissolved solids in the
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20 groundwater samples studied were found to vary from 56.0-263.20 mgL-1 (Table S3) and is found to be within the WHO accepted

21 limit of 1000 mgL-1 as well as the BIS permissible limit of 2000 mgL-1 for the desired palatability of drinking water.

22 4.3. Groundwater major solute chemistry and water aquifer interaction

23 The groundwater chemistry of the study area is represented in the form of a trilinear Piper diagram shown in Fig. 5. As observed,

24 the majority of the collected groundwater samples were found to cluster near high Ca2+ and trend towards the Mg2+ axis. This

25 indicates that for most of the groundwater samples, the cations are Ca2+ ions followed by Mg2+ ions. This clustering of the samples is
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1 indicative of the weathering of silicates and magnesium-rich rocks (dolomite) and also suggests the loss of Ca2+ through the

2 precipitation of calcite over dolomite that occurs during the interaction between the aquifer trapped water and rock matrices (Verma

3 et al., 2015; Verma et al., 2016). Additionally, the groundwater composition of the collected samples is dominated by HCO3- even

4 though the samples were also found to cluster between the SO42-+ Cl- axis and the Na2+ + K+ axes while trending towards the

5 former.

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7 Fig. 5. Representative water quality data for the collected groundwater samples using Piper diagram, showing the
8 association between the total cations (Ca2+, Mg2+, Na2+ and K+) , total anions (Cl-, SO42-, CO3- and HCO3-) and total dissolved
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9 solids (TDS).

10 The preliminary source of As enrichment in the groundwater originating in the north and northwestern parts of the

11 Brahmaputra valley is usually attributed to the geogenic composition of the area. Ophiolites, arc-related rocks in Indus–Tsangpo

12 suture zone (ITSZ) and volcanic, ophiolitic rocks in eastern Namche-Barwa syntaxial bend contribute towards the enrichment of As

13 in the area under the current study (Guillot and Charlet, 2007; Mukherjee et al., 2014). Also, the Ganges–Meghna–Brahmaputra

14 delta have been reported to be a part of the drainage system of the rapidly weathering Himalayas whose sulfide rocks contains up to

15 0.8% As (Phuong et al. 2012). The drainage of the main rivers that flow directly from the south Tibetan plateau through the present
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1 Himalayas causes the weathering of these rock formations resulting in the enrichment of the Himalayan paleo-foreland basin

2 (Siwaliks). Furthermore, the combinatorial effect of prominent tectonic shifts in coalition with weathering of Himalayan rocks by high

3 rainfall in the Holocene period is believed to have mobilized the As reserves stored in the Neogene Sediments (Siwalik). These As

4 deposits were subsequently transferred through Brahmaputra basin to the Bay of Bengal, also contributing to As enrichment in the

5 groundwater reserves (Verma et al., 2016).

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6 Moreover, iron, manganese and copper containing minerals like haematite, wuesite, magnetite, manganite and cuprite

7 have also been reported from sediment samples of the North and Northwestern areas bordering the Brahmaputra floodplains

8 (Verma et al., 2016). Their subsurface lithological studies also reveal a high amount of weathered iron-bearing minerals along with

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9 clay minerals such as illite, kaolinite, smectite in the aquifer sediments of the Brahmaputra floodplain which are known to serve as

10 potential sources of As in groundwater (Verma et al., 2016). The dissolved As in the collected groundwater samples shows a strong

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11 correlation with the redox-sensitive elements viz. (Mn) [R : 0.96] and Iron (Fe) [R :0.84]. However, As shows a very weak correlation

12 with SO42- [R2: 0.03] in the area under study, where the predominance of HCO3- ions is also indicative of the availability of reactive

13 organic matter (Phuong et al., 2012). These findings suggest that the reductive dissolution of iron-oxyhydroxides or arsenates

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14 adsorbed by detrital organic matter plays an essential role in the liberation of As in the groundwater aquifers of the Brahmaputra
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15 River valley. This is because of the reductive dissolution of Fe/Mn oxides/hydroxides by waterborne bacteria in the presence of

16 organic matter, which is known to be crucial in the release of As into its adjacent aquatic environment (Verma et al., 2016, Biswas

17 et al., 2011).
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18 4.4. Groundwater quality assessment and hydrological sustainability

19 The overall quality of groundwater is influenced by various factors which include the geological characteristics of the rock strata,
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20 rock-water interactions, dissolution/evaporation of aquifer trapped water, periodic weathering due to rainfall and various other hydro-
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21 geologic conditions (Islam et al. 2017). Consequently, the provision of universal criteria for the assessment of groundwater quality

22 and sustainability continues to be a major challenge. In this context, Water Quality Indices (WQIs) have been reported to be highly

23 effective in providing vital information on the suitability of groundwater for human consumption and have also served as a plausible
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24 option to adjudge the status of groundwater sustainability (Islam et al. 2017). Therefore, a Groundwater Quality Index (GWQI) was

25 generated for the collected groundwater samples based on the standard guideline values of the contaminants set by BIS (2012) as

26 well as on the implications of their chronic intake on human health (Islam et al. 2017). A total of thirteen (13) different parameters
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27 were employed (Table S4) and the groundwater samples were indexed into four independent classes (Table 2) to provide an insight
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28 into the groundwater quality status for the various districts under study.

29 The majority of the groundwater samples were found to harbour GWQI values indicative of a low water quality status in

30 the region. The GWQI values of the groundwater samples in the area under study were found to range from 40.73 to 1800. Of the

31 groundwater samples studied, three (3) samples showed excellent water quality while a total of nineteen (19) groundwater samples

32 were found to exhibit good water quality (Table S5). Further, a total of sixty-nine (69) groundwater samples were found to exhibit

33 poor water quality type while a total of one hundred and nine (109) samples groundwater showed very poor water quality type

34 (Table S5). Although there have been reports suggesting similar trends in some of the areas (Tamuli et al., 2017; Verma et al.,

35 2016; Borah et al., 2010), these studies do not provide a comprehensive groundwater quality assessment of the Brahmaputra River
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1 valley. Therefore, the GWQI values of the collected samples were further used for the generation of a geospatial distribution map

2 representing the overall groundwater quality in the region using an IDW interpolation approach (Fig. 6). The groundwater quality for

3 the majority of the

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1
2 Fig. 6. Spatially interpolated distribution maps (using IDW approach) showing the groundwater quality status in the Brahmaputra River valley.
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1 districts located in the vicinity of the Brahmaputra floodplains was found to be unfit for human consumption. Furthermore, most of

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2 the administrative districts located in the north-eastern region of the study area viz. Tinsukia, Dhemaji, Jorhat, Lakhimpur as well as

3 several other districts such as Sonitpur, Nagaon, Darrang, Udalguri and Baksa, located the south-eastern region, were found to
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4 harbour groundwater having GWQI values well below the poor quality threshold.

5 Groundwater sustainability is a manifold concept that incorporates hydrological, ecological, social, political and economic

6 factors (An et al., 2016; Llamas et al., 2006). Thus, the simultaneous optimization of all the aspects governing sustainability

7 presents a significant challenge. In this context, measures like periodic water quality assessment of the major groundwater reserves,
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8 sensitization and the dissemination of hydro-geochemical data among the decisions makers and stakeholders of affected areas are

9 to be adopted on a priority basis. In support of these measures, the adoption and demonstration of cost-effective mitigation

10 strategies/ alternatives to address the problem of groundwater contamination can help achieve hydrological sustainability in the
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11 affected areas (Pandey et al., 2011; Valentin and Spangenberg, 2000). The consistent monitoring and assessment of potable

12 groundwater reserves promotes a long-term understanding of the periodic fluctuations in groundwater quality and also acts as an

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early-warning mechanism to enable adequate response (Pandey et al., 2011; Collin and Melloul, 2003). Additionally, such studies

14 have been found to be highly indispensable when used in conjunction with mapping and modeling strategies for the stringent

15 assessment of the groundwater resources to provide a comprehensive picture of the aquifer conditions for accurate decision making

16 (Patra et al., 2018; Pandey et al., 2011). Also, the ability of local community leaders to establish a dynamic interaction between the
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17 set of working rules enforced by the regulatory bodies and the involvement of the community in the generation of sustainable

18 solutions for collective problems is highly crucial for governing hydrological sustainability (Choudhury and Mahanta, 2018).

19 The northeastern region of India comprises of some of the world’s highest rainfall areas and the Brahmaputra floodplains

20 have been reported to receive an annual rainfall of ~2400 mm (Table 1). Therefore, the provision of safe drinkable water through
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21 alternative sources such as surface water management and rainwater harvesting stands as a viable option in these areas severely

22 affected by groundwater contamination (Amos et al., 2018; Choudhury and Mahanta, 2018). Even though the supply quantity of
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23 surface water bodies in the Brahmaputra River valley has been reported to be reasonable, the ambiguity of surface water sources

24 and their unpredictable water quality status owing to contamination by vicinal industrial establishments and agricultural sectors

25 serves as a predominant hindrance to their utilization (Choudhury and Mahanta, 2018). In this regard, the stringent use of surface

26 water bodies only for human consumption, their regular maintenance for the alleviation of waterborne pathogens and the use of

27 environment friendly mitigation strategies such as pond sand filters (PSFs) offer a favorable solution to meet the demand for safe

28 drinking water (Choudhury and Mahanta, 2018; Hossein et al., 2015). Moreover, the implementation of corrugated galvanized iron

29 (CGI) sheet based sloping rooftops conducive to the capture of rainfall drainage and the use of rainwater harvesters and percolation

30 tanks may further ensure water security for resident communities in rural as well as urban areas (Choudhury and Mahanta, 2018;

31 Hossein et al., 2015). However, for areas wherein the use of groundwater reserves for potable practices is highly indispensable to

32 meet the demands of the resident population, the use of various water filtration strategies may be highly beneficial (Hossein et al.,

33 2015). In this regard, various cost-effective Arsenic Removal Filters (ARFs) viz. Sono 3-Kolshi filter, Granet Home-made filter, Chari

34 filter, Adarsha filter, Shafi filter, Bijoypur Clay/Processed Cellulose filter, SIT two-bucket filter etc. have been reported to offer

35 sustainable solution to the problem od As removal in neighboring Bangladesh (Jadhav et al., 2015; Ahmed, 2001). Owing to the
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1 similarity in geogenic and geographic parameters, these solutions can be tailored to address the problem of As contamination and

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2 poor water quality in the Brahmaputra River valley of Assam. Furthermore, the economic constraints that adhere to the large-scale

3 application of these approaches in rural areas may be overcome by the implementation of community ownership, thereby facilitating
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4 their smooth functioning and management in the provision of safe and contaminant free drinking water for human consumption.

5 5. Conclusion

6 Potable groundwater reserves still function as the primary water source for the inhabitants in the Brahmaputra floodplains and
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7 neighboring areas. The present study was focused on the groundwater aquifers linked to the Brahmaputra River valley and covered

8 all of the twenty administrative districts of Assam, that fall within the area encompassing the entire Brahmaputra river. Although the

9 present study collates well with the comprehensive report by Verma et al., 2016, 10 new districts (Tinsukia, Dhemaji, Lakhimpur,

10 Sonitpur, Nagaon, Uldaguri, Darrang, Baksa, Kamrup and Kamrup (Metro) are reported herein, to harbour As contaminated
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11 groundwater reserves exceeding the WHO prescribed threshold limit of 10 parts per billion. Further, the districts of Lakhimpur (243

12 ppb), Sonitpur (202 ppb), Nagaon (163 ppb), Udalguri (123 ppb), Darrang (115 ppb), Baksa (101 ppb), Dhemaji (83 ppb) and
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13 Tinsukia (78 ppb) were found to have alarmingly high levels of As in the groundwater reserves. This information is extremely

14 relevant to the populace inhabiting these districts as they need to respond appropriately to avoid the imminent threat of As poisoning

15 resulting from the use of the groundwater resources. In addition to the above, notable contamination by other heavy metals including

16 lead, manganese, iron and zinc and ions such as HCO3-, Ca2+ and Mg2+ were observed which is also likely to impact the water
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17 quality and have longstanding implications on the safety, aesthetics and potability of the groundwater acquired from these areas.

18 Further, the dissolved As content in the groundwater samples showed a significant correlation to the pH of the water source as well

19 as to other elemental contaminants such as iron and manganese suggesting that the reductive dissolution of iron oxyhydroxides
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20 might be considered as the prominent source for As enrichment in the groundwater. Also, the spatial distribution data for the

21 groundwater quality revealed that the majority of the sampling sites harboured groundwater which was unfit for human consumption.

22 Therefore, a reduced dependency on groundwater aquifers for potable usage, especially in regions highly affected by elevated
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23 levels of geogenic contaminants is indispensable. Furthermore, the effective management of the surface water, as well as the

24 exploration of alternative sources such as harvested rainwater to meet the demands for a steady supply of contaminant-free drinking

25 water is highly crucial. Additionally, the use of cost-effective remediation practices may offer a strategic advantage to combat the

26 geogenic contamination of groundwater in areas where the implementation of alternative approaches are challenging and the use of

27 ground-water reserves as the primary drinking water source cannot be avoided. To conclude, the current study may serve as a

28 template to the local stakeholders to aid in the design and execution of tailor-made, remediation and mitigation strategies that can

29 prevent the outbreak of Arsenicosis in the region. Such spatiotemporal studies on the groundwater quality assessment are

30 worthwhile practices that help monitor the mobilization of contaminants in ground-water aquifers, in the wake of climate change and

31 anthropogenic contributions to facilitate and promote the utilization of potable water reserves in a highly sustainable manner.

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1 Acknowledgement.

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2 The authors wish to acknowledge DBT, Govt. of India, for the Research Grant (Grant No. BT/258/NE/TBP/2011), UGC-SAP

3 Research Grant (TU/Fin/MBBT/116/05/11-12/64), DST-FIST-I and II (SRF/FST/LSI-320/2007 & SR/FST/LSI-692) and Tezpur
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4 University for the research facilities. Author C. Chaliha would like to acknowledge DST, Govt. of India for DST INSPIRE Junior

5 Research Fellowship.

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 ACCEPTED MANUSCRIPT

Title: GIS mapping-based impact assessment of groundwater contamination by arsenic and other heavy metal

contaminants in the Brahmaputra River valley: A water quality assessment study.

a a b a* c b
B.K. Nath , C. Chaliha , B. Bhuyan , E. Kalita , D.C. Baruah and A.K. Bhagabati

a. Department of Molecular Biology and Biotechnology, Tezpur University, Tezpur, Assam, 784028, India

b. Department of Geology, Gauhati University, Guwahati, Assam, 781014, India

PT
c. Department of Energy, Tezpur University, Tezpur, Assam, 784028, India

*Corresponding author. Tel.: +91 3712 275411

RI
E-mail address: ekalita@tezu.ernet.in

Highlights:

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• Spatially interpolated distribution maps for groundwater As, heavy metals, pH and depth developed

• 16 out of 20 districts surveyed had severe As contamination, highest being ~352 ppb

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• 10 new districts found to be affected by As contamination, in the comprehensive study

• Modelling of groundwater As showed correlation with Mn and Fe

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• Groundwater Quality Indexing shows most groundwater reserves unfit for human consumption
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