Geoscience Frontiers 12 (2021) 101079

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Focus Paper

Arsenic contamination of groundwater: A global synopsis with focus on

the Indian Peninsula
E. Shaji a,⁎, M. Santosh b,c, K.V. Sarath a, Pranav Prakash a, V. Deepchand a, B.V. Divya a
a
Department of Geology, University of Kerala, Kariavattom Campus, Trivandrum 695 581, India
b
School of Earth Sciences and Resources, China University of Geosciences (Beijing), 29 Xueyuan Road, Beijing 100083, China
c
Department of Earth Science, University of Adelaide, Adelaide, SA 5005, Australia

a r t i c l e i n f o a b s t r a c t

Article history: More than 2.5 billion people on the globe rely on groundwater for drinking and providing high-quality drinking
Received 14 April 2020 water has become one of the major challenges of human society. Although groundwater is considered as safe,
Received in revised form 9 July 2020 high concentrations of heavy metals like arsenic (As) can pose potential human health concerns and hazards.
Accepted 25 August 2020
In this paper, we present an overview of the current scenario of arsenic contamination of groundwater in various
Available online 1 October 2020
countries across the globe with an emphasis on the Indian Peninsula. With several newly affected regions re-
Handling Editor: Sohini Ganguly ported during the last decade, a significant increase has been observed in the global scenario of arsenic contam-
ination. It is estimated that nearly 108 countries are affected by arsenic contamination in groundwater (with
Keywords: concentration beyond maximum permissible limit of 10 ppb recommended by the World Health Organization.
Arsenic contamination The highest among these are from Asia (32) and Europe (31), followed by regions like Africa (20), North
Groundwater America (11), South America (9) and Australia (4). More than 230 million people worldwide, which include
Indo-Gangetic alluvium 180 million from Asia, are at risk of arsenic poisoning. Southeast Asian countries, Bangladesh, India, Pakistan,
Orogenic belts China, Nepal, Vietnam, Burma, Thailand and Cambodia, are the most affected. In India, 20 states and 4 Union Ter-
Global tectonics
ritories have so far been affected by arsenic contamination in groundwater. An attempt to evaluate the correla-
Asia
tion between arsenic poisoning and aquifer type shows that the groundwater extracted from unconsolidated
sedimentary aquifers, particularly those which are located within the younger orogenic belts of the world, are
the worst affected. More than 90% of arsenic pollution is inferred to be geogenic. We infer that alluvial sediments
are the major source for arsenic contamination in groundwater and we postulate a strong relation with plate tec-
tonic processes, mountain building, erosion and sedimentation. Prolonged consumption of arsenic-contaminated
groundwater results in severe health issues like skin, lung, kidney and bladder cancer; coronary heart disease;
bronchiectasis; hyperkeratosis and arsenicosis. Since the major source of arsenic in groundwater is of geogenic
origin, the extend of pollution is complexly linked with aquifer geometry and aquifer properties of a region.
Therefore, remedial measures are to be designed based on the source mineral, climatological and hydrogeological
scenario of the affected region. The corrective measures available include removing arsenic from groundwater
using filters, exploring deeper or alternative aquifers, treatment of the aquifer itself, dilution method by artificial
recharge to groundwater, conjunctive use, and installation of nano-filter, among other procedures. The vast ma-
jority of people affected by arsenic contamination in the Asian countries are the poor who live in rural areas and
are not aware of the arsenic poisoning and treatment protocols. Therefore, creating awareness and providing
proper medical care to these people remain as a great challenge. Very few policy actions have been taken at in-
ternational level over the past decade to reduce arsenic contamination in drinking water, with the goal of
preventing toxic impacts on human health. We recommend that that United Nations Environment Programme
(UNEP) and WHO should take stock of the global arsenic poisoning situation and launch a global drive to create
awareness among people/medical professionals/health workers/administrators on this global concern.
© 2021 China University of Geosciences (Beijing) and Peking University. Production and hosting by Elsevier B.V. This
is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction

Groundwater is one of the most precious natural resources in our

planet. It is being exploited extensively in many parts of the world
⁎ Corresponding author. with a massive increase in extraction in the past few decades due to
E-mail address: [email protected] (E. Shaji). the availability of new and cheaper drilling and pumping technologies

https://doi.org/10.1016/j.gsf.2020.08.015
1674-9871/© 2021 China University of Geosciences (Beijing) and Peking University. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

(Barbier, 2019). Hydrogeologists refer to this drastic change in ground- et al., 2012; Hashim et al., 2019). The severely affected countries include
water utilization as ‘the silent revolution’, since it has occurred in many Bangladesh (Yang et al., 2014), India (Mukherjee et al., 2009; Bhowmick
countries in an unplanned and totally uncontrolled manner (Stone et al., et al., 2018; Chakraborti et al., 2018; Bindal and Singh, 2019; Dhillon,
2019 and references therein). The demand for good quality groundwa- 2020), China (Guo et al., 2014), Nepal (Pokhrel et al., 2009), Cambodia
ter has increased with increasing population and developmental activi- (Polya et al., 2010), Vietnam (Winkel et al., 2011; Stopelli et al., 2020),
ties across the globe. Providing safe drinking water to the world's 7.8 Myanmar (Van Geen et al., 2014), Laos (Cho et al., 2011), Indonesia
billion people is one of the greatest challenges of the century. At the be- (Winkel et al., 2008 ), the USA (Gong et al., 2014). In addition, countries
ginning of 20th century, the groundwater quality issues were minimal like Argentina, Chile, Hungary, Canada, Pakistan, Mexico, and South
and total dissolved solids and pH were the only parameters of concern. Africa are also affected (Ravenscroft et al., 2009).
However, during 21st century, there has been increased global attention However, the South and Southeast Asian Belt is considered as the
on resolving groundwater quality issues. The chemical quality of ground most arsenic polluted areas including India, Bangladesh, Nepal,
water varies significantly depending on the type of aquifers, duration of Vietnam and China (Ravenscroft et al., 2009; McArthur, 2019). The de-
rock-water interaction and the inputs from various natural and non- veloped countries, like USA and Canada, also experience widespread
natural sources. During the last decade, groundwater contamination levels of arsenic contamination in groundwater although the concentra-
from various chemical constituents is being reported from aquifers tions are characteristically lower in comparison with the Asian coun-
throughout the world and often it becomes non-potable as the constit- tries (Sorg et al., 2014)
uents exceed the limits prescribed by WHO. Geochemical processes Our synthesis of the global data reveals that 107 countries are af-
during and after aquifer recharge can either improve or cause a deteri- fected by arsenic contamination in groundwater (beyond WHO maxi-
oration of water quality (Maliva, 2020). In the recent years, pollution mum permissible limit of 10 ppb) with highest reports from Asia (32)
by arsenic (As) has become a serious issue of concern in view of its tox- and Europe (31), followed by Africa (20), North America (11), south
icity to humans (Polya et al., 2019 and references therein). Arsenic con- America (9) and Australia (4) (Fig. 1). Most of the arsenic pollution
taminants in groundwater can also affect the health of the aquifers. prone zones are located in the sedimentary basins close to the modern
This paper examines the current scenario of arsenic contamination mountain belts and deltaic areas (Fig. 1). Regions with tropical climate
of groundwater in countries across the globe with an emphasis on the are more vulnerable to arsenic contamination as this climate favours
Indian Peninsula. We review the global As contamination in groundwa- the release of As from arsenic compounds (Ranjan, 2019). The details
ter, its ill effects on humans, sources characteristics, remediation, and of the 108 affected countries are shown in the World map (Fig. 1) and
also attempt to propose some recommendations for policy makers. the list of countries are depicted in Tables 1 and 2.
In Latin America, the main sources of arsenic contamination in
2. Geochemistry of arsenic groundwater are geothermal fluids and volcanic activities (Morales-
Simfors et al., 2020). In Mexico (North America), groundwater is the
Arsenic, an element of the earth’s crust with an abundance of main source of drinking water (40%) and high As concentrations (>10
1.8 ppm by weight, combines with oxygen, chlorine and sulphur to ppb) are reported in groundwater in different parts of Mexico
form inorganic arsenic compounds. Arsenic and its compounds are (Bundschuh et al., 1997; Alarcón-Herrera et al., 2020). 1.5 million peo-
widely used in agriculture, livestock feed, medicine, electronics, metal- ple in Mexico consume water with As above 25 μg/L, and about
lurgy, chemical warfare agents etc. Arsenic is of interest in terms of en- 150,000 people are exposed to As poisoning (Alarcón-Herrera et al.,
vironmental issues and health impacts. Rock-water interactions in 2020). A new study by Alarcón-Herrera et al. (2020) explains that
aquifer systems are the major cause of release of arsenic and causes de- 8.81 million people are now exposed to high As groundwater. Similarly,
terioration in groundwater quality. Arsenic is the 12th most common el- the North American regions like Guatemala El Salvador also have high
ement in nature, and it usually appears in three allotropic forms, As content in water resources (Armienta and Segovia, 2008; Libbey
including black, yellow, and grey. If heated, it rapidly oxidizes to arsenic et al., 2015) and source is identified as volcanogenic.
trioxide (As2O3) and has a garlic odour (Fendorf et al., 2010). Arsenic is In Bolivia, South America, high concentration of As (45.9 μg/L) in
also known as ‘king of poison’ as it is a highly toxic element ranking groundwater is recently reported (Alcaine et al., 2020) and the source
number one in the 2001 priority list of hazardous substances and dis- is volcanic formations of the Neogene period. Similarly the groundwa-
ease registry defined by WHO. Since 1993, the permissible value of the ters in the southern part of the Argentinian Chaco-Pampean plain are
concentration of arsenic (As) in drinking water has been fixed as 10 characterized by the elevated presence of arsenic (Smedley and
μg/L. However, it was 50 μg/L prior to 1993. It is classified as carcinogen, Kinniburgh, 2002) and the Tertiary aeolian loess-type deposits in the
mutagens, and teratogen. IARC (International Agency for Research on Pampean plain and fluvial sediments of Tertiary and Quaternary age
Cancer) has classified As is a class1 human carcinogen. In natural may be the source (Alcaine et al., 2020).
water bodies arsenic mostly found in two states trivalent arsenic In Europe, many countries report (especially Greece, Hungary,
(As3+, Arsenite) and pentavalent arsenic (As5+) both forms are highly Romania, Croatia, Serbia, Turkey, and Spain) elevated arsenic content
toxic inorganic species (Fendorf et al., 2010). The toxicity of arsenite is in groundwater resources (Katsoyiannis et al., 2015). Similarly, the
much higher than that of arsenate. Generally, in groundwater, natural groundwater resources of the Pannonian Basin (Hungary, Romania,
occurrences of high arsenic levels were reported in aquifers - especially Croatia and Serbia) also show high values of naturally occurring arsenic
unconsolidated sediment aquifers throughout the world and have been in water (Rowland et al., 2011). A recent study by Zuzolo et al. (2020)
connected to several adverse health effects (Smedley and Kinniburgh, reports As contamination of groundwater resources from central parts
2013; Mozumder, 2019). Arsenic contamination of groundwater is esti- of Italy.
mated to be affecting 500 million people around the globe. Continuous The worst affected African countries include Botswana, Burkina Faso,
exposure to high arsenic water causes pigmentation, hyperkeratoses, Ethiopia, Ghana, Morocco, Nigeria, South Africa, Tanzania, Togo, and
ulceration, skin cancer and also affects liver, kidney, heart, and lungs Zimbabwe (Medunić et al., 2020). In all these African countries both sur-
(Sun et al., 2019 and references therein). face and groundwater resources are affected by arsenic contamination,
however, the severity varies from region to region.
3. World scenario
4. Asian scenario
The natural contamination of As in groundwater has been reported
worldwide, and the majority of these belong to South Asian and South Thirty three Asian countries are significantly affected by groundwa-
American regions (see Fig. 1; Ravenscroft et al., 2009; Bundschuh ter arsenic contamination, which include Afghanistan, Armenia,

2
E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

Fig. 1. Arsenic affected countries of the world with intensity shown by the size of the plots (see Tables 1 and 2). Note that South Asian and South American regions are the worst affected
(source: Ali et al., 2019a and references therein and web sources (www.who.int/news-room/fact-sheets/detail/arsenic; www.sos-arsenic.net/)).

Table 1 southeast Dhaka was the worst affected. Several studies confirm that
List of countries affected by As contamination in groundwater the shallow aquifers of Bangladesh are badly affected by the high levels
Continent Number of countries affected of As contamination (Yang et al., 2014; Edmunds et al., 2015). The As
concentration in groundwater ranges from < 0.5 to > 4600 μg/L
North America Canada, Costarica, Cuba, Dominica, Salvador, Guatemala,
Honduras, Jamaica, Mexico, Nicaragua and USA (11) (Whaley-Martin et al., 2017 and references therein). Huq et al. (2020)
South America Argentina, Bolivia, Brazil, Chile, Colombia, Ecuador, Paraguay, reports that out of 64 districts, 61 districts contain As exceeding the
Peru and Uruguay (9) limit of WHO (10 μg/ L) standards for potable water and it affected
Asia Afghanistan, Armenia, Azerbaijan, Kyrgyzstan, Bangladesh, more than 85 million people. Shallow groundwater of sedimentary la-
Cambodia, China, Georgia, India, Indonesia, Iran, Japan, Jordan,
Laos, Kazakhstan, Korea, Malaysia, Mongolia, Myanmar, Nepal,
custrine aquifers normally contains high As concentrations whereas
Pakistan, Philippines, Russia, Saudi Arabia, Sri Lanka, Tajikistan, deeper aquifers (> 300 m) is considered safe (Huq et al., 2020). In
Thailand, Turkey, Turkmenistan, Uzbekistan and Vietnam (31) Bangladesh, the As contamination creates several social issues and eco-
Europe Albania, Austria, Belgium, Croatia, Czech Republic, nomic problems (Rahman et al., 2018a, 2018b). The manifestation of the
Bosnia-Herzegovina, Denmark, Estonia, Finland, France,
arsenicosis is more intense among the poor, which is directly linked
Germany, Greece, hungry, Iceland, Ireland, Italy, Latvia,
Lithuania, Macedonia, Netherlands, Norway, Poland, Portugal, with the poverty circumstances (Rahman et al., 2018a).
Romania, Serbia, Slovakia, Spain, Sweden, Switzerland, Ukraine
and United Kingdom (31)
Africa Algeria, Botswana, Burkina Faso, Cameron, Egypt, Ethiopia, 4.2. Cambodia
Ghana, Kenya, Libya, Malawi, Morocco, Namibia, Niger, Nigeria,
South Africa, Tanzania, Togo, Uganda, Zambia, and Zimbabwe In South and South East Asia, from Pakistan at the western periph-
(20) ery, to Cambodia and southern China at the eastern, groundwater
Australia and Australia, Guam, New Zealand, Papua New Guinea (4)
Oceania
used for domestic purposes is contaminated with arsenic (Richards
et al., 2019). Arsenic contamination in Cambodian groundwater has a
similar natural source as in Bangladesh and appears to descend from
the Mekong River from natural processes in the Himalayan Mountains
(Natasha et al., 2019). Agusa (2002) found that groundwater wells in
Azerbaijan, Bangladesh, Cambodia, China, Georgia, India, Indonesia, Kandal province in Cambodia contained an average of 178 μg/L of arse-
Iran, Iraq, Japan, Jordan, Kazakhstan, Kyrgyzstan, Laos, Malaysia, nic. In Cambodia, arsenic was also found in shallow tube wells in the
Mongolia, Myanmar, Nepal, Pakistan, Philippines, Russia, Saudi Arabia, low-lying Mekong delta at Prey Veng province. It is estimated that
Sri Lanka, Thailand, Turkey, Turkmenistan, Uzbekistan, Vietnam, there are over 2.4 million people live in the As contaminated zone of
Tajikistan, and Korea (Fig. 1, Table 1). The most affected countries are Cambodia (Murphy et al., 2018).
China, Bangladesh, India, and Pakistan. This is followed by Vietnam.
The problems related to arsenic pollution in selected countries are sum-
marized below. 4.3. China

China is one of the most affected countries facing health issues be-
4.1. Bangladesh cause of arsenic contamination in groundwater (Zhang et al., 2020). Al-
though arsenic is present in several geographical regions in mainland
The arsenic poisoning in groundwater was first reported by the De- China, Northern China has been identified as a high-risk area. It has
partment of Public Health Engineering from the district of Chapai been estimated that 19.6 million people are at risk of being exposed to
Nawabganj in 1993 (Huq et al., 2020 and references therein). arsenic-contaminated groundwater (Rodríguez-Lado et al., 2013).
Chakraborti et al. (2016) reported that the degree of the problem in China faces groundwater quality issues from both industrial effluents
the country was very critical and revealed that the centre part of the and natural sources. The arsenic poisoning is noticed among people,

3
 Table 2
Country wise details of As-contaminated groundwater across the globe with details of population exposed and probable sources.

Country Location and maximum concentration Population Environmental condition References

(μg/L) exposed

Africa
Burkina Mogtedo, Ouahigouy, Ganzourgou, Yatenga, Balé, 560,000 Sulphide minerals from volcanic rocks and schists. Gold mineralization in Bretzler et al., 2017
Faso Soum etc. (1630) Birimian volcano-sedimentary rocks.
Cameroon Ekondo Titi (2000) 4000 Mbotake, 2006; Ravenscroft et al., 2009
Ghana Wassa West, Obuasi, Accra, Bolgatanga, Brong-Ahafo Data not available Bowell, 1994; Smedley et al., 1996; Buamah et al., 2008
(4500)
Nigeria Warri-Port Harcourt, Ogun State, Kaduna (750) Data not available Alluvial sediments, strongly reducing, slightly acidic Oke et al., 2008; Edet et al., 2004; Gbadebo, 2004
Asia
E. Shaji, M. Santosh, K.V. Sarath et al.

Bangladesh 61 District (4730) 85 million Holocene alluvial sediments (floodplain and deltaic sediments), organic Rosenboom, 2004; Hossain, 2006; Edmunds et al., 2015
matter, reducing, high alkalinity, arsenic-rich sediments
Burma Irrawady delta (630) 3.4 million Holocene alluvial sediments strong reducing Van Geen et al., 2014
Cambodia Mekong delta, Kandal Province (1610) 2.4 million Holocene alluvial sediments strong reducing Berg et al., 2007; Kim et al., 2011; Ul Haque, 2015;
UNICEF, 2016; Richards et al., 2019
China Anhui, Beijing, Guangdng, Henan, Heilongjiang, Inner 19.6 million Holocene alluvial sediments strong reducing, abundant hydrated ferric oxides, Guo et al., 2008; He and Hering, 2009; Rodríguez-Lado
Mongolia, Jilin, Shanxi, Xinjiang etc. (2000) increased pH, iron phase in sediment aquifers et al., 2013; Chen et al., 2017
India 20 District (3880) 50 million Holocene alluvial and deltaic sediments, oxidation of arsenic rich pyrite or Chakraborti et al., 2003, 2004, 2009, 2016, 2018;
anoxic reduction of ferric iron hydroxides in the sediments to ferrous iron Mukherjee et al., 2006; Nickson et al., 2007; Bhowmick
et al., 2018
Japan Kyushu geothermal fields, Fukuoka; Kumamoto; No data Volcanic sediments, Holocene coastal sands, Quaternary alluvium aquifer Tsuda et al., 1995; Mitsunobu et al., 2013; Even et al.,
Fukui; Takatsuki Torokuetc (25,700) 2017
Nepal 25 Districts (2620) 13 million Geogenic and the dissolution of arsenic-bearing rocks, sediments and Neku and Tandukar, 2003; Pokhrel et al., 2009; Thakur
minerals; changes in reduction conditions, iron oxyhydroxides et al., 2011; Brikowski et al., 2014
Pakistan 27 Districts (2580) 13 million people out of Quaternary sediments (alluvial and deltaic origins; high percentage of fine to Fatmi et al., 2009; Brahman et al., 2013; Bibi et al., 2015;
total 40 million in 27 very fine sand and silt) Rehman et al., 2016; Rasheed et al., 2017; Ali et al.,
districts 2019a, 2019b
Russia Kamchatka (360,000) Data not available Hot springs Karpov and Naboko, 1990
Australia and Oceania

4
Vietnam Red River Delta and Mekong Delta (3050) 10 million Pleistocene and Holocene sediments; strongly reducing, high alkalinity, Stanger, 2005; Berg et al., 2007; Nguyen and Itoi, 2009
arsenic-rich sediments
Australia Victoria region, New South Wales (300,000) 1976 Pyrite sediments, hydroxides and Fe oxyhydroxides, gold mining Hinwood et al., 1999; Smith and Smith, 2004; Appleyard
et al., 2006
Guam Tumon Bay (1200) Vuki et al., 2007
New Waiotapu Valley, Rarangi, Marlborough (8500) 1939 Alluvial aquifers, reduced groundwater, geothermal water Grimmett and McIntosh, 1939; Webster and Nordstrom,
Zealand 2003
Europe
France Tinee and Vesubie valleys, Vosges and the Pyrenees, 17,000 Sedimentary basin, oxidation, ore deposits containing arsenopyrite Saoudi et al., 2012; Barats et al., 2014; Drouhot et al.,
Aquitaine basin (263) 2014
Germany Bavaria, Saxony, Wiesbaden (550) Data not available Alluvium sediments, mineralized sandstone Heinrichs and Udluft, 1999; Schwenzer et al., 2001
Italy Limbardia, Emilia Romagna and Veneto (1300) Shallow groundwater, hydrothermal, geothermal arsenic common around the Tamasi and Cini, 2004; Vivona et al., 2007
volcanic canters
Spain Madrid basin, Duero Basin (613) 50,000 Alluvial sediments, strong reducing Garcia-Sanchez et al., 2005; Gómez et al., 2006; Sanz
et al., 2007
UK Midlands, Cornwall, Liverpool, Northwest England Data not available Limestone, sandstone, estuarine alluvium, mining, alluvial or glacial aquifers Millward et al., 1997; Middleton et al., 2016
(355)
North America
Canada Nova Scotia, Saskatchewan, Ontario, British Columbia, Data not available Thermal spring, Sulphide mineralization in volcanic rocks, high pH, sorption Wyllie, 1937; Boyle et al., 1998; Kim et al., 2002; Kwong
Alberta (100,000) to ion oxides et al., 2007; Dummer et al., 2015; Bondu et al., 2017
Mexico Region Lagunera, Valle del Guadiana, valle da Zimapan 2 million Volcanic sediments oxidation of sulphide and arsenopyrite, dissolution of Wyllie, 1937; Boyle et al., 1998; Kwong et al., 2007;
(2400) scorodite Dummer et al., 2015
USA Alaska, Arizona, California, Hawaii, Idaho, Maryland Data not available Holocene and older basin-fill sediments, high pH, up-flow of geothermal Southwick et al., 1983; Stauffer and Thompson, 1984;
Massachusetts, Nevada, Oregon, Utah, Washington water; dissolution of or desorption from iron oxide; dissolution of sulphide Welch et al., 2000; Flanagan et al., 2015
etc. (24,300) minerals
South America
Argentina Chaco-Pampean Plain, Cordoba, Salta, Jujuy, La Pampa 2 million Tertiary- Quaternary volcanic deposits, post volcanic geysers and thermal Nicolli et al., 1989, 2012; Auge, 2014; Panigatti et al.,
(14,969) springs, excessive irrigation strongly affects local geochemical and 2014; Robles et al., 2016
hydrochemical conditions
Brazil Ribera Valley, Amapa State, Rio das Valihas, Minas, Data not available Sulphide-rich gold-bearing rocks that constitute the aquifers Matschullat, 2000; Figueiredo et al., 2007; Bidone et al.,
Geoscience Frontiers 12 (2021) 101079

Gerais, Rondonia State, Amazon (100,000) 2016; Ciminelli et al., 2017; Thi et al., 2019
Chile Northern and Central Chile (27,000) 500,000 Quaternary volcanogenic sediment, oxidizing, arid conditions, high salinity Borgono and Greiber, 1971; Corradini et al., 2018
E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

who live in arid regions of the Northern provinces, probably because of Kohistan, mafic and ultramafic rocks are the main source of arsenic in
scarcity of clean water for cooking and drinking from sources other than groundwater.
groundwater (Zhang et al., 2020). Arsenicosis was first reported in
Kuitun region, located in the Xinjiang Uygur Autonomous Region of 4.5. Sri Lanka
China in 1980.
In the Taiwan region, a good correlation was established between Although arsenic-contaminated groundwater is not reported partic-
total arsenic and iron contents in groundwater samples and the marine ularly in the metamorphic aquifers of Sri Lanka, elevated levels were
sequences. The presence of clay layer within the aquifer may increase As found in sedimentary formations in certain parts (Mannar, Mulativu,
contamination in groundwater (Liu and Wu, 2019). In Taiwan, concen- Puttalam, and Jaffna) of the island (Chandrajith et al., 2020). In all
tration of arsenic in groundwater ranges from 10 to 1800 μg/L (Chen these regions, groundwater is extracted from unconfined aquifers of
et al., 1995). Chronic arsenic problems were observed among a popula- the Holocene sand dunes that are underlain by Miocene limestones.
tion of 40,421 in 37 villages in the country (World Bank, 2005; Liu and
Wu, 2019). Rainfall significantly affects the arsenic concentration in 4.6. Thailand
the northern area. Black shale or pyrite material occurring in underlying
geological strata are identified as the source of arsenic. Over-pumping In Thailand, arsenic in groundwater originates mostly from tin min-
groundwater introduces dissolved oxygen that oxidizes the immobile ing activities (Kim et al., 2011). Thailand is one of several countries in
sulphide minerals, releases As by reductive dissolution of As-rich iron Southeast Asia, having problems with tin residue (Tiankao and
oxyhydroxides, and increases the mobile As in water (Liu et al., 2010; Chotpantarat, 2018, and references therein). The waste piles, resulting
Maliva, 2020 and references therein). from tin mining, contain high As (as arsenopyrite). The case studies
The Chinese National Survey Program, conducted by the Chinese from Ron Phibun sub-district, Nakhon Si Thammarat, a province in the
Ministry of Health between 2001 and 2005, tested groundwater sam- southern part of Thailand (Williams et al., 1996; Smedley and
ples from around 445,000 wells in 20,517 villages of 292 counties for ar- Kinniburgh, 2002) recognized health problems. Approximately 1000
senic contamination (Rodríguez-Lado et al., 2013 and references people have been diagnosed with As-related skin disorders, particularly
therein). In almost 5% of wells, arsenic levels were higher than the for- in and close to the Ron Phibun town (Fordyce et al., 1995; Williams
mer Chinese standard of 50 ppb, and about 10,000 individuals were et al., 1996; Choprapawon and Rodcline, 1997). The affected area lies
found to be affected by arsenicosis. within the Southeast Asian Tin Belt (Schwartz, 1995). Arsenic concen-
The Inner Mongolia is reported as another endemic area of severe trations are found at up to 5000 μg/L in shallow groundwater from the
arsenicosis in China. This area is mainly in the southern part of Moun- Quaternary alluvial sediment that has been extensively dredged during
tain Yinshan, and the region connecting the plain north of Yellow tin-mining operations (Tiankao and Chotpantarat, 2018).
River and the alluvial plain of Heihe River, where the groundwater is
rich in natural arsenic. More than 600,000 people in 5 cities and 678 vil- 4.7. Vietnam
lages are identified as potential victims, and >3000 people were diag-
nosed with arsenicosis (Sun, 2004). Nguyen et al. (2020a, b) reported that the people living in Nui Phao,
Thai Nguyen in the northern Vietnam region have high risk of As poi-
4.4. Pakistan soning from groundwater and vegetables. The study reveals that 75%
of the groundwater samples had As exceeding the permissible limit of
Rabbani et al. (2017) and Ali et al. (2019a) reported that 13 million 10 μg/L by World Health Organization (WHO, 1999, 2004). The arsenic
people across 27 districts of Pakistan are prone to As contamination in contamination of Vietnam was first reported in 2001 along the Red
their drinking water and people residing along the Indus River are fac- River alluvial tract (Bozack et al., 2019 and references therein). In
ing higher threats. Total 9% of water resources in Pakistan were ob- Vietnam, a high concentration of pollutants such as As, Fe, and Mn
served to carry elevated levels of arsenic above the allowable limit. were identified in groundwater pumped from tube wells which tap
Around 25%–36% population of two provinces in Pakistan, namely the Pleistocene aquifer (Smedley and Kinniburgh, 2002). The Red
Sindh and Punjab, are exposed to drinking water As contamination River delta is the primary source of As contamination and more than
over 10 ppb (Zubair et al., 2018 and references therein). About 11 dis- ten million people are at risk of adverse health effects (Bozack et al.,
tricts of Punjab and Sindh provinces in Pakistan were found with As 2019). The sediments in the Mekong River delta are rich in organic com-
contamination in groundwater beyond the national defined permissible pounds that create an anoxic condition and that leads to the reduction
level (Ali et al., 2019b). The study by Ali et al. (2019a, 2019b) reports of dissolved iron oxides, which in turn causes the release of arsenic
that about 656 villages and 6,173,680 people are at the risk of exposure (Le Luu, 2019). This is confirmed by another study that biological reduc-
to As in their water supply. In Sindh province, Tharparkar and Hydera- tion of iron metal plays a vital role on the release of arsenic from Holo-
bad along Indus River and in the Punjab province, Lahore and Kausar cene sediments (Stopelli et al., 2020). In Vietnam, total arsenic
are well-known hotspot sites of natural geogenic As contamination concentration of 1–185 μg/L (average 39 μg/L) and 1–3050 μg/L (159
in groundwater (Ali et al., 2019a). The most important aquifer of μg/L) were found in groundwater in the Mekong River delta and Red
Pakistan is situated in Indus plain, and this area is characterized by River delta, respectively (Berg et al., 2007).
Quaternary sedimentary deposits, mainly composed of alluvial and Over all more than 230 million people worldwide, which include
deltaic origin, and the sediment thickness ranges from few meters to 180 million from Asia, are at risk of arsenic poisoning (See Table 2).
several hundred meters in different parts. The aquifer which taps sedi-
mentary deposit in this area has high arsenic contamination (Smedley, 5. The scenario in Peninsular India
2008; Ali et al., 2019b). In general, the sources are identified as both
anthropogenic and natural (Smedley, 2008; Farooq et al., 2016). Coal Groundwater plays a vital role in India to meet the water demands of
mining activities and geothermal sources contribute in Jhelum and various sectors, such as domestic, industrial and irrigational needs (Saha
Chakwal Punjab provinces (Iqbal, 2001). In Tharparkar of Sindh prov- and Ray, 2019; Suhag, 2019). The alluvial tracts of Ganga and Brahma-
ince, arid environment and complex geology promote reductive disso- putra rivers are the wealthiest groundwater province in the country.
lution of As minerals leading to contamination (100–2580 μg/L) in Most of the extraction occurs along the Indo-Gangetic basin in Northern
groundwater (Brahman et al., 2013). In Tharimirwah, Kotdigi, Sobo and Northwestern India, which has resulted in significant drawdown
Dero, and Kingri, alluvial deposit of Indus river is the primary source and water table decline in many locations (Rodell et al., 2009;
of As contamination (Rabbani et al., 2017). In the northern region of MacDonald et al., 2016). In India, it is reported that a population over

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

50 million is currently at risk from groundwater arsenic contamination. Jharkhand, Arunachal Pradesh, Assam, Manipur, Meghalaya, Mizoram, Na-
Several workers carried out extensive work on arsenic contamination in galand, Sikkim, Tripura, Punjab, Himachal Pradesh, Chhattisgarh and
groundwaters in India, especially in Ganga basin (Chakraborti et al., Andhra Pradesh (World Bank, 2005; Mukherjee et al., 2006; Chakraborti
2018 and references therein). The Ganga River basin covers nearly et al., 2018). However, our synthesis reveals that in India, 20 states
26% of India’s landmass and is home to a population of over 500 million (West Bengal, Jharkhand, Bihar, Uttar Pradesh, Assam, Gujarat, Haryana,
(Chakraborti et al., 2018). The Ganga River basin is one of the most fer- Madhya Pradesh, Panjab, Arunachal Pradesh, , Karnataka, Tamil Nadu,
tile and densely populated areas in the world (Khan et al., 2016). Pres- Himachal Pradesh, Telangana, Andhra Pradesh, Orrisa, Nagaland, Tripura,
ently, the Ganga is one of the world’s most polluted rivers, containing Manipur, Chhattisgarh) and 4 Union territories (Delhi, Daman and Diu,
a number of toxins including chromium, arsenic, cadmium, lead, copper Puducherry, Jammu and Kashmir) are affected now (Fig. 2).
and mercury, as well as pesticides and pathogenic microbes nearly 3000 In India, high arsenic groundwater occurs in two categories: (1) allu-
times higher than the safe limit prescribed by the World Health Organi- vial terrane and (2) hard rock terrane. Alluvial aquifers are the main
zation (WHO, 2011; Tandon and Sinha, 2018). source (90%) of arsenic in India. Hard rock aquifers accounts only 10%,
High arsenic (>10 ppb) groundwater has been reported in shallow which includes states like Karnataka and Chattisgarh (Fig. 3). In Karna-
aquifers from 10 states in India (CGWB, 2018), however, the deeper aqui- taka, arsenic is reported in association with sulfide mineralization, espe-
fers of India (>100 m) are free from arsenic. Arsenic contamination in cially arsenopyrite. It is mainly restricted to the gold mineralized areas
groundwater was first reported from the Chandigarh region of north covering parts of Raichur and Yadgir districts. In Chattisgarh, it has
India (Datta and Kaul, 1976), and the second case was reported in the been reported from the acid volcanic associated with Kotri lineament.
lower Gangetic plain of West Bengal (Garat et al., 1984). This was followed In the following sections, we present the state-wise details of As con-
by reports from several states including West Bengal, Bihar, Uttar Pradesh, tamination in groundwater.

Fig. 2. Arsenic affected states and Union Territories in India. 20 states and 4 Union territories are affected (source: www.mapsofindia.com; Chakraborti et al., 2018 and references therein;
CGWB, 2018).

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

Fig. 3. Arsenic affected areas superimposed on the general geology of India. Alluvial aquifers are the main source (90%) of arsenic in India and hard rock aquifer accounts only 10% (modified
map of Aquifer systems of India; CGWB, 2017, 2018).

5.1. Assam Quaternary alluvium holding multi aquifer system, although As in

groundwater is not reported from the hard rock aquifers of Bihar
In Assam, arsenic in groundwater was first reported in 2004. Con- (Kumari et al., 2019).
centrations of As and other elements are higher at shallow depths, as re-
ported for other regions of the Brahmaputra floodplain (Verma et al., 5.3. Chhattisgarh
2015; Kumar et al., 2016a, 2016b; Das et al., 2017, 2018; Patel et al.,
2019). In Chhattisgarh, high concentration of As in groundwater was re-
ported in the village of Kaudikasa in Rajnandgaon district (Shukla
5.2. Bihar et al., 2010) and the high arsenic groundwater (up to 250 μg/L) wells
are located in the granitic terrain with pegmatitic intrusions. Arsenic re-
In Bihar, elevated levels of arsenic in groundwater was first reported lated skin cancer and keratosis were also identified from the area. High
in 2002, from two villages of Bhojpur district located in the middle arsenic is also reported from tube-wells of Ambagarh-Chowki block
Ganga plain (CGWB, 2018). The total population at risk is around (Acharyya et al., 2005), and is restricted to the N–S trending Dongargarh
9 million (Thakur and Gupta, 2019). Most of the arsenic-contaminated rift zone. The affected areas are underlain by acid volcanics, and gran-
districts tap groundwater from alluvial aquifer of the Ganga river ites. In the Chhattisgarh state, arsenic groundwater contamination is
basin in Bihar. Geological formations in the affected areas are considered to be due to natural deposition of arsenic-rich pyrite, and

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

its mobilization is due to microbial respiration of organic carbon 5.9. Tamil Nadu
(Ahmed et al., 2004).
Sridharan and Nathan (2018) reported arsenic contamination in
groundwater of Puducherry region. The Puducherry region is a sedi-
5.4. Haryana mentary terrain composed of marine sediments, alluvium, laterites,
thin seams of peat and lignite whose age ranges from Cretaceous to Re-
Arsenic concentration exceeding limit has been reported in ground- cent. Over-pumping of groundwater, the rapid growth of industries, ur-
water in different parts of Haryana (Bhattacharya, 2017) Sediment con- banizations, increase in population lead to ground water contamination.
taining arsenic-rich minerals which were dissolved under reducing
conditions released As into the groundwater. The study of CGWB 5.10. Uttar Pradesh
showed arsenic concentration in groundwater to be more than 50 ppb
from different districts covered by alluvial aquifers (CGWB, 2018). The Arsenic-contamination of groundwater was first reported in the
source of arsenic is geogenic and is occurring in alluvial sediments. Ballia district. The arsenic-affected villagers used to drink water gener-
The districts exposed to groundwater arsenic-contamination are ally from hand-pumps which tap groundwater from shallow aquifers
drained by Yamuna river and its tributaries which originate from the of depth about 20–30 m. Twenty districts have been reported to have el-
Himalaya ranges (Bhattacharya, 2017). evated arsenic in groundwater in scattered pockets. All the arsenic-
affected districts in Uttar Pradesh and 12 districts in Bihar are aligned
along the linear tract along the course of the river Ganga.
5.5. Jharkhand
Shah (2015) summarised the status of arsenic contamination in
groundwater resources of the north-eastern states of India. Arsenic in
Groundwater with arsenic contamination above 50 ppb was first re-
groundwater has been reported in the states of Assam, Arunachal
ported during 2004 from the Sahebganj district of Jharkhand located be-
Pradesh, Manipur, Nagaland and Tripura and the Brahmaputra Valley,
tween the Middle and Lower Ganga Plains by CGWB. Later high arsenic
Barak Valley and Manipur Valley are the most affected areas. Arsenic
groundwater (up to 133 μg/L) was reported from Sahibganj district
contaminated shallow tube-wells are located in the Holocene aquifer.
along the river Ganga in Jharkhand (Alam et al., 2016 and references
The sources of arsenic are geogenic and the process of release of arsenic
therein). Arsenic-contamination has been reported from the area close
in groundwater is reductive dissolution of iron hydroxides.
to the Ganga River and it is in those areas where the Ganga River has
shifted course during the recent past. More than two hundred thousand
5.11. West Bengal
people were affected by arsenic toxicity. Tirkey et al. (2016) studied the
arsenic and other heavy metals in the groundwater samples of Ranchi
Arsenic contamination in ground water in West Bengal was first de-
city, Jharkhand.
tected in 1978, and around 16.66 million people (according to 2001 cen-
sus) in 8 districts in West Bengal are at risk (Das, 2019). Das et al. (1996)
and Chowdhury et al. (1999) reported that, in West Bengal, areas af-
5.6. Karnataka
fected by arsenic contamination in groundwater are located in the
upper delta plain, and are mostly reported from the abandoned
In Karnataka, elevated As in groundwater is reported from hard rock
meander belt. The source of the arsenic is geological. Bore-hole sample
aquifers and is reported mostly from the areas of gold mining and asso-
analyses show high arsenic concentrations only in soil layers rich in
ciated activities, greenstone belts of Yadgir district and southern region
iron-pyrites (Das, 2019). It has been reported that more than 50 million
of Gulbarga district (Chakraborti et al., 2013 and references therein).
people living along the Ganga–Brahmaputra basins are affected by the
The occurrence of arsenic is related to arsenopyrite present in the host
high levels of arsenic in drinking water. High arsenic groundwater has
rock. Examples are the Hutti Gold mining area in Lingasugur taluk of
been observed mainly in the districts of North 24 Parganas, Burdwan,
Raichur district and abandoned gold mining areas in Shorapur taluk of
Howrah, Hooghly, Kolkata, and Nadia (Singh, 2006). The highest con-
present Yadgir district. After extraction of the gold, the chemical waste
centration of arsenic in groundwater was reported from Burdwan re-
was dumped on the ground surface in the adjoining areas of the mine.
gion, followed by Kolkata (Sen and Sarkar, 2019).
These dumped materials having arsenopyrite leached out arsenic dur-
Here we present a new map to show relation between As contami-
ing rainy season and joined the groundwater regime. Groundwater of
nated areas of India and regional geology (Fig. 3). This map shows a
Ingaldhal and surrounding villages of Chitradurga district also shows el-
good correlation between aquifer types and As contamination. The
evated levels of arsenic (Hebbar and Janardhan, 2016).
map shows that 90% of the affected areas belong to alluvial deposits of
different ages. The hard rock aquifers of different ages spread across
5.7. Manipur the country account only 10%. There are only limited reports from
Decan traps and the regions with crystalline basement in the shield
Arsenic has been detected in ground water in the valley districts of areas and 90% of the hard rock aquifers (including Cuddapah and Gond-
Manipur namely, Kakching, Imphal East, Imphal West, and Bishnupur. wana) are relatively safe zones (Fig. 3).
These districts are located along the river courses which originate
from the eastern Himalayas. 6. Sources of arsenic contamination

The main sources of arsenic contamination can be classified as natu-

5.8. Punjab ral and anthropogenic, and are evaluated below.

CGWB (Central Ground Water Board) reports the presence of Arse- 6.1. Natural sources
nic in groundwater from Panjab during 2004 (CGWB, 2018). Arsenic
concentration exceeding value of 10 ppb was found at 12 locations in There are several natural sources, as well as anthropogenic actions
districts of Amritsar, Gurdaspur, Hoshiarpur, Kapurthala and Ropar. All that may introduce arsenic into groundwater and drinking water. The
these arsenic-exposed districts are located along the river courses of major natural sources include geologic formations (e.g., sedimentary
the Ravi and Beas, which have also routes originating from the deposits/rocks, volcanic rocks and soils), geothermal activity, coal and
Himalayas. volcanic activities. Geothermal water can be a source of inorganic

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

arsenic in surface water and groundwater (Welch et al., 2000). Although The main source of As in Bangladesh is largely from the Bengal Basin
concentrations of arsenic in the earth’s crust fluctuate, the average formed by the Ganga–Brahmaputra–Meghna (GBM) River system. This
levels are commonly reported to range from 1.5 to 5 mg/kg. Arsenic is sedimentary basin has been formed by deposition of large volumes of
a significant component of many mineral species in magmatic, hydro- arsenic-containing sediments that originated mainly from the
thermal, and sedimentary rocks. It is widely present in sulfide ores of Himalayas and was carried down by the mighty GBM rivers during the
metals, including copper, lead, silver, and gold. There are over 100 Pleistocene and Holocene periods. From these sediments, arsenic is
arsenic-containing minerals, including arsenic pyrites (e.g., FeAsS), leaching into the groundwater aquifers located in the fan deposit
realgar (AsS), lollingite (FeAs2, Fe2As3, Fe2As5), and orpiment (As2S3) areas and Holocene alluvium.
(details of arsenic-bearing minerals with pictures are listed in Supple-
mentary Table 1). Figure 4 shows arsenic concentration range (mg/kg) 7. Arsenic speciation in groundwater
in common rocks, sediments and soils types. As seen in the table slate/
phyllite has the maximum concentration followed by peaty soils and The factors responsible for release of arsenic into the groundwater
mudstones/marine shales. Therefore, high As groundwater is expected are pH, presence of organic matter in sediments (like peat, lignite
in sedimentary aquifers. and plant debris), water table fluctuation (Hinkle and Polette, 1999;
Rodrıguez et al., 2004), water saturation of sediments, limited supply
of sulphur and microbial activities (Matisoff et al., 1982; Chapelle and
6.2. Anthropogenic sources Lovley, 1992; Lovley, 1997), groundwater flow direction, age of ground-
water and topography (Fendorf et al., 2010), and marine transgression
Anthropogenic related arsenic contamination in groundwater is re- (Trafford et al., 1996; Berg et al., 2001). The mechanisms which cause
ported in 54 countries and is largely created by human intervention, the release of arsenic into groundwater include: (1) oxidation and dis-
mining, coal and petroleum extraction. solution of As and Fe bearing minerals (Welch et al., 2000; McArthur
The source characterisation, continent wise, is given in Fig. 5, where et al., 2001; Smedley and Kinniburgh, 2002); (2) weathering and reduc-
it is clear that the major source of As on all continents is sedimentary tive dissolution of arsenic-bearing primary and secondary minerals
formations, particularly Holocene sediments. The details are also given in the presence of natural organic matter (NOM) (Berg et al., 2001);
in Table 2. In Asia, sedimentary formations contribute 45%, followed (3) combination of both oxidative and reductive dissolution of
by mining (30%), coal (10%), petroleum (10%) and volcanic rocks (5%). arsenic-bearing iron oxides and oxyhydroxides (Nickson et al., 1998;
In Europe, sedimentary formations and mining activities contribute Kinniburgh and Smedley, 2001; McArthur et al., 2001); (4) competitive
equally followed by volcanic rocks, coal and petroleum. In America, sed- exchange of As by other compatible ions such as nitrate, phosphate
imentary formations, mining activities and volcanic rocks contribute (Chowdhury et al., 1999) and bicarbonate (Nickson et al., 2000). As-
equally followed by coal and petroleum. In Africa, mining and sedimen- rich minerals are linked with the Quaternary deposits of alluvial sedi-
tary formations are the major contributors with little addition from coal, ments belonging to the Holocene age (Mukherjee et al., 2009; Shah
petroleum and volcanic rocks. In Australia all sectors contribute equally. et al., 2010). As contamination occurs due to the reductive dissolution
Anthropogenic related arsenic contamination may be categorised of As-bearing minerals (Postma et al., 2016), the As-rich sediments are
into different types such as mining-related, coal-related, or coal burn- transported by rivers originating from the Himalayas and are deposited
ing. Sulfides are frequently associated with gold ores, and are a potential into downstream basins and deltaic areas. The organic matter buried
source of arsenic. Mining and smelting of these minerals create environ- along with the sediment is utilized by microbes for metabolic activities.
mental hazards of arsenic leaking into groundwater and surface water The microbial reduction of iron (Fe) from Fe3+ to Fe2+ due to the con-
from slag pits, waste dumps, extraction basins, and mines. Mining- sumption of oxygen bound to As-bearing ferroxy hydroxides results in
related (coal mining) arsenic contamination is being affected in 74 the subsequent release of As in water (Drahota et al., 2013; Verma
countries across the world. Petroleum-related arsenic has affected 17 et al., 2016). Arsenic contamination can take place in reducing aquifer
countries in the world. environments, in oxidizing environments with high pH (Nickson et al.,
The main sources of As in the groundwater of India is alluvial sedi- 2005), and with oxidative weathering of sulfide minerals and with geo-
ments, and are mainly derived from Himalayan sediments due to ero- thermal activity. Soil texture also plays a significant role in providing the
sion. Arsenic gets mobilized through the reductive dissolution of Fe3+ appropriate environment for As release into the groundwater (Hoque
- oxyhydroxides in a reducing environment (Kumar et al., 2016a). et al., 2009).
We use published chemical data on pH, Electrical Conductivity (EC)
and As content to make scatter plots of As vs EC and As vs pH (Fig. 6a
and b). It is observed that EC does not have any correlation with As con-
tent, however, pH has definite correlation with As content, with alkaline
water favouring the release of As to the groundwater.

8. Arsenic contamination in the context of global plate tectonics

We show tectonic map of the world showing regions of high As in

groundwater in order to evaluate the correlation between As contami-
nation in the global plate tectonic context (Fig. 7). Arsenic contamina-
tion is markedly high in groundwaters of the circum-Himalayan
region, and on the foot hills of the present-day mountain belts like
Alpine-Himalayan-Tibet belt and Cordilleran-Andean belt (Fig. 7). The
groundwaters hosted in Holocene aquifers, consisting of Himalayan
sediments deposited by the great Asian rivers in deltaic environments,
generally show high As content. The Ganga-Brahmaputra river systems
are the major contributors of the Bengal fan, which is considered as one
Fig. 4. Average arsenic concentrations in rocks, sediments and soils. The main sources of As
of the largest modern deltas of the world. Guillot and Charlet (2007)
could be slate/phyllite/mudstone/marine shale/peaty soils (source: Smedley and proposed that the serpentinites enriched in arsenic and the arc-related
Kinniburgh, 2002 and web resources (www.igrac.net/publications/143)). rocks of Indus-Tsangpo suture zone could be one of the primary sources

9
E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

Fig. 5. Pie-chart showing continent-wise arsenic source characterisation. It is clear that the major source of As on all continents is sedimentary formations followed by mining (see Tables 1
and 2).

Fig. 6. (a) Scatter plot of As vs. EC (Electrical Conductivity) in different countries. The published data show that EC does not have any correlation with As. (b) Scatter plot of As vs. pH As in
different countries. The published data show that pH has correlation with As.

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

Fig. 7. Arsenic contaminated regions superimposed on the tectonic map of the world. See that arsenic affected regions are mostly confined in the sedimentary basins close to the modern
mountain belts and deltaic areas.

of arsenic. Further they argue that intense tectonic activity in frontal Hi- predefined limit of 10 mg/L by using limited As data points along with
malayan belt associated with high rainfall conditions during the Holo- independent variables, such as geology, topography, and soil properties.
cene could be the possible reason for arsenic remobilization, Rodríguez-Lado et al. (2013) used proxies such as Holocene sediments,
transportation and disposition. soil salinity, soil texture, topographic wetness index (TWI), drainage
A close look at the global distribution of As-enriched areas in Fig. 7 density, slope, distance to rivers, and gravity anomaly, out of which Ho-
reveals that the As enriched aquifers are associated with sedimentary locene sediments, soil salinity, subsoil texture, and TWI were found to
basins adjoining major orogenic belts. Many of these sedimentary ba- be most significant in predicting the occurrence of As in groundwater.
sins may be tectonically controlled and occur as foreland basins that de- A few studies used are linear regression (LR) (Zhang et al., 2013), prin-
veloped by lithospheric flexure at the time of mountain building cipal component regression (PCR) (Luo et al., 2012), Bayesian modeling
processes along convergent plate boundaries. High arsenic groundwater (Cha et al., 2016) and artificial neural network (ANN)-based regression
of these basins may thus be related to global plate tectonic framework of (Cho et al., 2011; Bonelli et al., 2017) for As prediction models. Such
major orogenic belts. The transportation of As-enriched magmatic rocks models (Cho et al., 2011; Cha et al., 2016) have shown accuracies vary-
from the depth to surficial deposits through tectonic processes such as ing between 60% and 70%.
exhumation, and subsequent release or mobilization of arsenic in Of late, machine learning models have also been used for such stud-
groundwater occurs under conducive surficial biogeochemical pro- ies. Machine learning models (e.g., random forests and neural net-
cesses. The widespread presence of As has been correlated with works) show higher prediction accuracy than LRM due to their
orogens, as in areas as diverse as the Indus–Ganges–Brahmaputra strength in modelling complex relationships between response and
basin (Himalayan orogen), the Chaco-Pampean basin (Andean orogen), predictor variables (Tesoriero et al., 2017). The machine learning algo-
Rocky mountain basin (Western Cordilleran orogen), and New England rithms develop sophisticated model subunits for capturing complex re-
and north-eastern USA (the Appalachian orogen). lationships to specify in parametric models. However, such machine
learning model studies are rare in India, even though new regions
9. Prediction of spatial distribution of arsenic contamination have been added to existing high-As risk areas, affecting millions of peo-
ple in India. A hybrid random forest model has been used by Bindal and
A few studies have used methods such as Thiessen polygon, inverse Singh (2019) to predict the regions in Uttar Pradesh (UP) at risk due to
distance weighing (IDW) (Gong et al., 2014), global polynomial interpo- As contamination. They predicted that 12% of the total population of
lation (Bhunia et al., 2016), and kriging (Gong et al., 2014; Sovann and Uttar Pradesh, which accounts for 23.48 million people are at risk in
Polya, 2014) to predict the spatial variation of contaminants in ground- UP. The predictive abilities of the other models such as univariate,
water from different aquifers of the world. Although these methods are LRM, fuzzy, adaptive fuzzy regression (AFR) and adaptive neuro fuzzy
effective, non-availability of accurate spatial data points is the hurdle to inference system (ANFIS) were compared with that of a hybrid random
produce meaningful outcomes. However, these methods do not account forest model. Bretzler et al. (2017) used multivariate logistic regression
for spatial dependency of the data to predict the occurrence of the con- method to create arsenic prediction models from the data sets collected
taminants. There is always a paucity of reliable georeferenced data; from Burkina Faso, West Africa. They have predicted that aquifers of the
thus, these models do not perform well. Therefore, predictive models Birimian formation with arsenic-bearing sulphide minerals, has the
that consider the factors responsible for contamination are used to over- highest probability of yielding groundwater arsenic concentrations >
come the limitations of the models that use interpolation for prediction. 10 μg/L and further added that more than 560,000 people are potentially
Logistic regression models (LRM) have been commonly employed to exposed to arsenic-contaminated groundwater in Burkina Faso. Winkel
predict the spatial distributions of arsenic worldwide (Dummer et al., et al. (2008) predicted the groundwater arsenic contamination in
2015). Several studies have used logistic regression (Zhang et al., Southeast Asia using logistic regression model by combining geological
2013) to assess the likelihood of As contamination greater than the and surface soil parameters from the Bengal, Red River and Mekong

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

deltas. Further, their study revealed that Holocene deltaic and organic- and Losi, 1995). The pathway of As5+ methylation initially involves
rich sediments are the major source of high arsenic groundwater in the reduction of As5+ to As3+, with the subsequent methylation of
Southeast Asia. As3+ to dimethylarsine by coenzyme S-adenosylmethionine (Pierce
This study predicts that As can be released to groundwater if the area and Moore, 1982). Methylation is often enhanced by sulfate-reducing
is underlain by alluvial aquifers especially of Holocene age in foreland bacteria. Several fungal species also have shown ability to reduce arse-
basins with high organic content. The mechanism of mobilisation nic (United States Department of Health and Human Services, 2000).
could be reductive dissolution in humid / anoxic depositional environ- Various technologies are being developed for the removal of arsenic
ments under alkaline pH conditions. contamination from groundwater in different parts of the world.
To conclude, more As poisoning can be expected in areas underlain Electrocoagulation is considered an efficient technology to treat ar-
by Holocene aquifers consisting of Himalayan sediments, South and senic contaminated water and meet the drinking water quality stan-
East Asia (SE China, Yangtze-Kiang basin Indonesia, Malaysia, Siberia), dards (Mendoza-Chávez et al., 2020). A cement-based filter medium
West Asia and Middle East (Arabian Peninsula, Turkey and Iran), (CBFM) can also be used to remediate heavy metals from groundwater
South America (Western Amazonia, Pacific Plains) and in Europe (Dan- (Holmes et al., 2019).
ube delta, Baltic fringes). The other expected areas are (1) areas of in- Coagulation, chemical oxidation, advanced oxidation processes
tense sulphide mineralisation, (2) areas close to younger orogenic (AOPs), adsorption, ion-exchange, membrane filtration (nano-filter)
belts, and (3) areas of geothermal activity. and reverse osmosis are also common treatment technologies for the
remediation of arsenic-contained water. The salient summary of each
10. Health risk of these processes is given below.
Oxidation: Arsenite can be oxidized by oxygen, ozone, free chlorine,
It is believed that inorganic As3+ is more toxic than inorganic As5+ permanganate, hydrogen peroxide etc. Atmospheric oxygen,
and the inorganic arsenic ingested is excreted through urine (Thomas hypochloride and permanganate are commonly used for oxidation in
and Bradham, 2016, and references therein). For many years, methyla- developing countries. Air-oxidation of arsenic is very slow but
tion and excretion were viewed as a detoxification system. It is now chemicals like chlorine and permanganate can rapidly oxidize arsenite
recognised that these methylated forms are probably the more damag- to arsenate under wide range of conditions (Wegelin et al., 2000).
ing forms of As in respect of human metabolism. Long-term ingestion of Co-precipitation and adsorption processes: Water treatment with
water with high amount of As can cause a variety of cancers. The symp- coagulants such as aluminium alum, activated alumina, ferric chloride
toms and the ill-effects are region specific and to some extent individual and ferric sulfate are effective in removing arsenic from water. Ferric
specific too. It is reported that well-nourished individuals suffer less salts have been found to be more effective in removing arsenic than
damage than those of mal-nourished people. In India the first case of alum on a weight basis and effective over a wider range of pH. In both
arsenic-induced skin lesions was identified at the Department of Der- cases, pentavalent arsenic can be more effectively removed than triva-
matology, School of Tropical Medicine, Calcutta, India in 1983 (Saha, lent arsenic (Pierce and Moore, 1982).
2003). The illness that develops from chronic arsenic exposure is The Bucket Treatment Unit (BTU), designed for household need is
known as “arsenicosis”. Skin lesions such as melanosis, keratosis, and based on the principles of coagulation, co-precipitation and adsorption
leucomelanosis are the characteristic manifestations of arsenicosis. processes. It consists of two buckets, each 20 L capacity, placed one
The WHO defines arsenicosis as a “chronic condition arising from a above the other. Chemicals are mixed manually with arsenic contami-
prolonged ingestion of arsenic above safe dose for at least 6 months, nated water in one of the buckets by vigorous stirring and then floccu-
usually manifested by characteristic skin lesions of melanosis and/or lated by gentle stirring. The mixed water is then allowed to settle for
keratosis with or without involvement of internal organs. Arsenicosis 1–2 h. The water from the bucket is then allowed to flow into another
was first reported from Bangladesh in 1996, now it has become a severe bucket through a sand filter installed in the second bucket, very care-
worldwide problem (Smith et al., 2000 and references therein). The fully avoiding the inflow of settled sludge in the first bucket. Now the
consumption of arsenic contaminated groundwater results in serious second bucket practically contains treated water (Guha Mazumder,
health issues like skin, lung, kidney and bladder cancer, coronary heart 2003).
disease, bronchiectasis. hyperkeratosis, arsenicosis, hyperpigmentation Solar oxidation: It is a simple method of solar oxidation of arsenic in
of the palm and sole, hypertension, myocardial damage, liver damage, transparent bottles to reduce arsenic content of drinking water
Bowens disease, and diabetes, among other diseases (Lalwani et al., (Mukherjee et al., 2007). Ultraviolet radiation can catalyze the process
2004; Hopenhayn, 2006; Steinmaus et al., 2016; Chakraborti et al., of oxidation of arsenite in presence of other oxidants.
2018; Saha and Ray, 2019). Arsenic poisoning has also been linked to in- Large number of adsorbents have been utilized for removal of arse-
fant mortality, impaired intellect and motor dysfunction in children nic species (arsenite, As3+ and arsenate, As5+) but the arsenite, As3+ re-
(Wasserman et al., 2004; Rahman et al., 2009; Parvez et al., 2011; moval requires pre-oxidation of As3+ to As5+ using oxidizing agents,
Bhowmick et al., 2018; Saha and Ray, 2019). The details of the affected which makes the process costly and sometimes produce unhealthy
people are listed in the Table 2. by-products (Zhang et al., 2007; Siddiqui and Chaudhry, 2017). There-
An overview chart showing the various impacts of As poisoning on fore, to avoid the pre-oxidation step using costly oxidizing agents, vari-
humans health, collected from the above referred papers (Chakraborti ous solid materials with oxidative properties have been developed
et al., 2018; Saha and Ray, 2019 and references therein) is presented (Siddiqui and Chaudhry, 2017).
in Fig. 8. Graphene oxide (GO) and its composites have attracted widespread
attentions as novel adsorbents for the adsorption of various water
11. Removal of arsenic from groundwater pollutants due to their unique physicochemical characteristics
(Siddiqui et al., 2019).
Safe drinking water, nutritious food and adequate physical exercise Biological oxidation: Study of Pallier et al. (2010) reveals that some
are only the proven measures to fight chronic arsenic toxicity (Maeda, micro-organisms such as Gallionellaferruginea and Leptothrixochracea
1994). Proper watershed treatment and cost-effective conjunctive use support and accelerate biotic-oxidation of iron, which makes a
of water along with creating mass awareness are effective the ap- favourable environment for the adsorption of arsenic.
proaches to solve the arsenic crisis (Shakya and Ghosh, 2019). Inorganic Arsenic can also be removed from groundwater by nano-filtration
arsenic can undergo microbially mediated biochemical transformation, (NF) membrane configuration (Song et al., 2015).
i.e., the hydroxyl group of arsenic acid is replaced by the CH3 group, Managed aquifer recharge also helps to reduce the As content in
thus getting transferred into relatively non-toxic form (Frankenberger groundwater.

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

Fig. 8. Flow chart showing various impacts of As poisoning on human health (source: Chakraborti et al., 2018; Saha and Ray, 2019 and references therein and web sources (www.sos-
arsenic.net/)).

Laterite is used as a low-cost adsorbent in a sustainable filtration sys- properly. The people exposed to As poisoning is reported to be more
tem to remove arsenic from groundwater in Vietnam (Nguyen et al., than 230 million across the globe, this may not be a correct figure,
2020a, 2020b). In India, clay rich laterite is easily available and can be hence a global survey should be initiated by USGS or WHO to collect
tested as filtration system to remove arsenic from groundwater. the real data.
All the above methods described in this review have their own ad- Effective and sustainable programmes for the management of the
vantages and disadvantages. The filtration methods can be chosen aquifers require active support of hydrogeologists, hydrologists, water
based on the severity of the problem and affordability. The significant sector organisations, planners and all stake holders at large. These com-
methods include awareness rising in the rural areas; providing nano- munities should be involved at all stages of groundwater development
filters and As-removal appliances for the household as well as the com- programmes, including initial surveys; decisions on siting of wells, sit-
munity level. ing of off-takes or establishing protection zones and monitoring and
surveillance.
12. Policy interventions We urge that WHO and other relevant agencies formulate new pol-
icy recommendations to reduce the impact of As poisoning in ground-
Safe drinking-water, as defined by the WHO (1999) guidelines, do water resources and to improve safe water use in affected areas across
not represent any significant risk to health over a lifetime of consump- the globe. The individual affected countries, especially Asian countries,
tion. The health concerns associated with chemical constituents of should launch a public awareness campaign on safe water treatment
drinking-water are more serious as these can cause adverse health ef- or arsenic treatment equipment, providing the information on the sta-
fects after prolonged periods of usage. There are a few chemical constit- tus of As contamination and seeking additional safe water sources
uents of water like As, that can lead to serious health problems. such as rainwater and treated groundwater. For the mitigation program,
In order to protect public health, a dual-role approach is essential, by WHO or UNEP has to create a separate fund for the solution of the global
defining the roles and responsibilities of service providers / authorities As contamination of groundwater. It is essential to develop comprehen-
responsible for water supply and by prudent drinking-water supply sive management plans involving adequate medical, paramedical and
quality surveillance. Organizational arrangements for the maintenance infrastructural support within the umbrella of primary health care.
and improvement of drinking water supply services should be in place The governmental agencies and NGOs need to reach out to the affected
in all quality affected areas. poor people, who still depend on the contaminated water for their do-
Surveillance of drinking-water quality can be defined as “the contin- mestic use. Erasing the threat of arsenicosis from the face of the Earth
uous and vigilant public health assessment and review of the safety and must be one of the prime mottos of policy makers. This paper recom-
acceptability of drinking water supplies” (WHO, 2011). However, this mends that a Global Policy for Arsenic Mitigation and Strategic Plan
recommended surveillance is not in force in many countries. Periodic (GPAMSP) may specifically be formulated to solve the arsenic problem
quality assessment of various aquifers of globe is also not executed in drinking water.

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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

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Appendix A. Supplementary data
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E. Shaji, M. Santosh, K.V. Sarath et al. Geoscience Frontiers 12 (2021) 101079

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Professor M. Santosh is Foreign Expert at the China Univer-
volcanic-sedimentary aquifers: a case study in central Italy. Hydrogeol. J. 15 (6),
sity of Geosciences, Beijing, China, Professor at the University
1183–1196.
of Adelaide, Australia and Emeritus Professor at the Kochi
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University, Japan. Founding Editor of Gondwana Research as
study in some spring waters of Guam, Western Pacific Ocean. Sci. Total Environ. 379
well as the founding Secretary General of the International
(2-3), 176–179.
Association for Gondwana Research Editorial Advisor of Geo-
Wasserman, G.A., Liu, X., Parvez, F., Ahsan, H., Factor-Litvak, P., van Geen, A., Slavkovich,
science Frontiers. Receipt of National Mineral Award, Out-
V., Lolacono, N.J., Cheng, Z., Hussain, I., Momotaj, H., 2004. Water arsenic exposure
standing Geologist Award, Thomson Reuters Research Front
and children’s intellectual function in Araihazar, Bangladesh. Environ. Health
Award and Global Talent award. He was recognized as Highly
Perspect. 112 (13), 1329–1333.
Cited Researcher continuously during last four years.
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K.V. Sarath is a Research Fellow in the Department of Geol-
United States: occurrence and geochemistry. Groundwater 38 (4), 589–604.
ogy, University of Kerala, India. He completed his Master’s
Whaley-Martin, K., Mailloux, B., van Geen, A., Bostick, B., Ahmed, K., Choudhury, I., Slater,
degree in Geology from Central University of Kerala and
G., 2017. Human and livestock waste as a reduced carbon source contributing to
Bachelor’s degree in Geology from the Kannur University.
the release of arsenic to shallow Bangladesh groundwater. Sci. Total Environ. 595,
His research interests include Hydrogeology, Petrology, Geo-
63–71.
chemistry and GIS/ Remote sensing.
WHO, 1999. Arsenic in Drinking Water. World Health Organization, Geneva, p. 210.
WHO, 2004. Guideline for Drinking-Water Quality, 3rd edition (Recommendations).
World Health Organization, Geneva.
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nic contamination in Southeast Asia from surface parameters. Nat. Geosci. 1 (8),
Pranav Prakash is a Research Scholar in the Department of
536–542.
Geology, University of Kerala. He completed his Master’s de-
Winkel, L.H., Trang, P.T.K., Lan, V.M., Stengel, C., Amini, M., Ha, N.T., Viet, P.H., Berg, M.,
gree in Applied Geology from Pondicherry University and
2011. Arsenic pollution of groundwater in Vietnam exacerbated by deep aquifer ex-
Bachelor’s degree in Geology from the University of Kerala.
ploitation for more than a century. Proc. Natl. Acad. Sci. 108 (4), 1246–1251.
His research interests include Hydrogeology, Sedimentology,
World Bank, 2005. Towards a More Effective Operational Response: Arsenic Contamina-
Natural resources Management and GIS/ Remote sensing.
tion of Groundwater in South and East Asian Countries, Volume 1, Policy Report.
World Bank.
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Zhang, A., Feng, H., Yang, G., Pan, X., Jiang, X., Huang, X., Dong, X., Yang, D., Xie, Y., Peng, L.,
Jun, L., 2007. Unventilated indoor coal-fired stoves in Guizhou province, China: cellu-
lar and genetic damage in villagers exposed to arsenic in food and air. Environ. Health
V. Deepchand is a Research Scholar in the Department of Ge-
Perspect. 115 (4), 653–658.
ology, University of Kerala, India. He completed his M.Phil
Zhang, M., Gao, B., Varnoosfaderani, S., Hebard, A., Yao, Y., Inyang, M., 2013. Preparation
and Master’s degree in Geology from University of Kerala
and characterization of a novel magnetic biochar for arsenic removal. Bioresour.
and Bachelor’s degree in Geology from Kannur University.
Technol. 130, 457–462.
His research interests include Petrology, Geochemistry, Hy-
Zhang, Z., Guo, H., Liu, S., Weng, H., Han, S., Gao, Z., 2020. Mechanisms of groundwater ar-
drogeology and GIS.
senic variations induced by extraction in the western Hetao Basin, Inner Mongolia,
China. J. Hydrol. 583, 124599.
Zubair, M., Martyniuk, C.J., Shaheen, A., 2018. Rising level of arsenic in water and fodder: a
growing threat to livestock and human populations in Pakistan. Toxin Rev. 37 (3),
171–181.
Zuzolo, D., Cicchella, D., Demetriades, A., Birke, M., Albanese, S., Dinelli, E., Lima, A., Valera,
P., De Vivo, B., 2020. Arsenic: geochemical distribution and age-related health risk in
Italy. Environ. Res. 182, 109076.

Dr. E. Shaji is an Associate Professor & Research guide in the B.V. Divya is a Research fellow in the Department of Geology,
Dept. of Geology, University of Kerala, India. Prior to the Uni- University of Kerala. She received her M.Phil and Master’s de-
versity service he worked as a professional hydrogeologist gree in Geology from the University of Kerala and Central
(Scientist D) in Central Ground Water Board, Ministry of Wa- University of Kerala respectively and Bachelor’s degree in
ter Resources, Govt of India. He has 23 years of professional/ Geology from Kannur University. Her research interests are
industry/teaching experience in Geosciences with focus on in the field of Hydrogeology, Natural Resources Management
groundwater and petrology. Three scholars took PhD with and GIS/ Remote sensing.
him, and guided several M.Phil. and M.Sc. students. He
bagged Young Scientist Award from Kerala State Council for
Science Technology and Environment, Govt. of Kerala. He is
an Associate Editor of Geoscience Frontiers.

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