Science of the Total Environment 780 (2021) 146274

Contents lists available at ScienceDirect

Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Review

Seven potential sources of arsenic pollution in Latin America and their

environmental and health impacts
Jochen Bundschuh a,⁎, Jerusa Schneider b,q, Mohammad Ayaz Alam c, Nabeel Khan Niazi d, Indika Herath a,
Faruque Parvez e, Barbara Tomaszewska f, Luiz Roberto Guimaraes Guilherme g, Jyoti Prakash Maity h,
Dina L. López i, Alicia Fernández Cirelli j, Alejo Pérez-Carrera k, Nury Morales-Simfors a,l,
Maria Teresa Alarcón-Herrera m, Paulo Baisch n, Dinesh Mohan a,o, Abhijit Mukherjee p
a
UNESCO Chair on Groundwater Arsenic within the 2030 Agenda for Sustainable Development, University of Southern Queensland, West Street, Toowoomba 4350, Queensland, Australia
b
Department of Geology and Natural Resources, Institute of Geosciences, University of Campinas, 13083-855 Campinas, SP, Brazil
c
Departamento de Geología, Facultad de Ingeniería, Universidad de Atacama, Avenida Copayapu 485, Copiapó, Región de Atacama, Chile
d
Institute of Soil and Environmental Sciences, University of Agriculture Faisalabad, Faisalabad 38040, Pakistan
e
Department of Environmental Health Sciences, Columbia University, 60 Haven Ave, B-1, New York, NY 10032, USA
f
AGH University of Science and Technology, Mickiewicza 30 Av., 30-059 Kraków, Poland
g
Federal University of Lavras, Department of Soil Science, 37200 900 Lavras, Minas Gerais, Brazil
h
Department of Earth and Environmental Sciences, National Chung Cheng University, 168 University Road, Min-Hsiung, Chiayi County 62102, Taiwan
i
Department of Geological Sciences, Ohio University, 316 Clippinger Laboratories, Athens, OH, USA
j
University of Buenos Aires, Faculty of Veterinary Sciences, Instituto de Investigaciones en Producción Animal (UBA-CONICET), Centro de Estudios, Transdiciplinarios del Agua (UBA), Av. Chorroarín
280, CABA C1427CWO, Argentina
k
University of Buenos Aires, Faculty of Veterinary Sciences, Centro de Estudios Transdiciplinarios del Agua (UBA), Instituto de Investigaciones en Producción Animal (UBA-CONICET), Cátedra de
Química Orgánica de Biomoléculas, Av. Chorroarín 280, CABA C1427CWO, Argentina
l
RISE Research Institutes of Sweden, Division ICT-RISE SICS East, Linköping SE-581.83, Sweden
m
Departamento de Ingeniería Sustentable, Centro de Investigación en Materiales Avanzados SC Unidad Durango, C. CIMAV # 110, Ejido Arroyo Seco, Durango, Dgo., Mexico
n
Laboratório de Oceanografia Geológica, Instituto de Oceanografia, Universidade Federal do Rio Grande (FURG), Campus Carreiros, CP 474, CEP 96203-900 Rio Grande, RS, Brazil
o
School of Environmental Sciences, Jawaharlal Nehru University, New Delhi 110067, India
p
Department of Geology and Geophysics, Indian Institute of Technology (IIT), Kharagpur, West Bengal 721302, India
q
Faculty of Agricultural Sciences, Federal University of Grande Dourados, João Rosa Góes St., 1761, Dourados, Mato Grosso do Sul, 79804-970, Brazil

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Arsenic (As) mobilization from geogenic

and anthropic sources to near-surface
environments
• Different pathways of As human expo-
sure and their health impacts with
Latin American examples
• Natural dissemination of As in sur-
rounding environments through
leaching of As bearing rocks
• Acceleration of natural dissemination of
As through mining of metallic and en-
ergy resources
• (Hydro)(bio)geochemical processes
during As exposure through drinking
water and food chain
• Health issues associated with As uptake
following intake through indigestion
and inhalation

⁎ Corresponding author.
E-mail address: jochenbundschuh@yahoo.com (J. Bundschuh).

https://doi.org/10.1016/j.scitotenv.2021.146274
0048-9697/© 2021 Elsevier B.V. All rights reserved.
J. Bundschuh, J. Schneider, M.A. Alam et al. Science of the Total Environment 780 (2021) 146274

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

Article history:
Received 19 November 2020
Received in revised form 25 February 2021
Accepted 28 February 2021
Available online 8 March 2021
Editor: Xinbin Feng
Keywords:
Arsenic sources and human exposure
Mining
Hydrocarbon and coal exploitation
Volcanism and geothermalism
Geophagy
Environmental and health impacts
This review presents a holistic overview of the occurrence, mobilization, and pathways of arsenic (As) from pre-
dominantly geogenic sources into different near-surface environmental compartments, together with the re-
spective reported or potential impacts on human health in Latin America. The main sources and pathways of
As pollution in this region include: (i) volcanism and geothermalism: (a) volcanic rocks, fluids (e.g., gases) and
ash, including large-scale transport of the latter through different mechanisms, (b) geothermal fluids and their
exploitation; (ii) natural lixiviation and accelerated mobilization from (mostly sulfidic) metal ore deposits by
mining and related activities; (iii) coal deposits and their exploitation; (iv) hydrocarbon reservoirs and co-
produced water during exploitation; (v) solute and sediment transport through rivers to the sea; (vi) atmo-
spheric As (dust and aerosol); and (vii) As exposure through geophagy and involuntary ingestion. The two
most important and well-recognized sources and mechanisms for As release into the Latin American population's
environments are: (i) volcanism and geothermalism, and (ii) strongly accelerated As release from geogenic
sources by mining and related activities. Several new analyses from As-endemic areas of Latin America empha-
size that As-related mortality and morbidity continue to rise even after decadal efforts towards lowering As ex-
posure. Several public health regulatory institutions have classified As and its compounds as carcinogenic
chemicals, as As uptake can affect several organ systems, viz. dermal, gastrointestinal, peptic, neurological, respi-
ratory, reproductive, following exposure. Accordingly, ingesting large amounts of As can damage the stomach,
kidneys, liver, heart, and nervous system; and, in severe cases, may cause death. Moreover, breathing air with
high As levels can cause lung damage, shortness of breath, chest pain, and cough. Further, As compounds,
being corrosive, can also cause skin lesions or damage eyes, and long-term exposure to As can lead to cancer de-
velopment in several organs.
© 2021 Elsevier B.V. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. An overview of As in the environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1. Arsenic distribution in the natural environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.2. Arsenic in groundwater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.3. Arsenic in the food chain . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.4. Arsenic speciation and its toxicity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
2.5. Arsenic exposure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.6. Arsenic related health issues . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.7. Arsenic related environmental regulations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3. Known and potential sources of As pollution in Latin America . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.1. Volcanism and geothermalism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.1.1. Arsenic related to volcanism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.1.2. Large-scale transport of As containing highly soluble volcanic ash . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.1.3. Arsenic in geothermal fluids . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.1.4. Effects on ground and surface waters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.2. Metal ore deposits and accelerated exposure related to mining . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.3. Geogenic As exposure related to coal exploitation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
3.4. Arsenic in co-produced water from hydrocarbon exploration and production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
3.5. Rivers with natural and anthropogenic As-rich waters and sediments discharging into the sea . . . . . . . . . . . . . . . . . . . . . . 17
3.6. Atmospheric As (dust and aerosol) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
3.7. Arsenic exposure through geophagy and involuntary ingestion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
4. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
Declaration of competing interest. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20

1. Introduction
Human exposure to arsenic (As) at toxic levels has been reported in
many Latin American countries, particularly during the last two decades
(Bundschuh et al., 2012a, 2020). However, in most cases, only limited
data on the sources and occurrence of As are available, making a correct
assessment of the scale and magnitude of this problem difficult. At pres-
ent, As contamination is reported in all 20 Latin American countries,
where As is predominantly released naturally (e.g., through weathering
and dissolution of rocks/minerals, geothermal fluids mixing with
groundwater in near-surface environments, and volcanic activities). An-
thropogenic activities, viz. mining, coal, hydrocarbon, and geothermal
exploitation, agricultural activities further accelerate this; or As release
is purely from anthropogenic sources, viz. industrial and urban wastes,
fertilizers, and pesticides. Arsenic released from both natural and an-
thropogenic source(s) can contaminate (i) ground- and surface water,
thus adversely affect drinking water and also crop production through
contaminated irrigated water, (ii) soil, (iii) biota, and (iv) air; resulting
in severe consequences on human health, especially through drinking
water intake and food chains.
The problem of human exposure of As in Latin America not only re-
mains a significant health issue that some of the authors of this work
reviewed almost a decade ago (Bundschuh et al., 2012a; McClintock
et al., 2012), but there is an urgent necessity to address this issue, as rec-
ognized in the present work. Since the publication of the reviews men-
tioned earlier, numerous scientific studies from Latin America have

2
J. Bundschuh, J. Schneider, M.A. Alam et al.
documented increased risk of cancer, cardio-respiratory diseases, repro-
ductive outcome, and cognitive effects in adults and children (e.g., Khan
et al., 2020, and references therein). In particular, several new analyses
from As-endemic Antofagasta in Chile have documented that mortality
and morbidity continue to rise even after several decades of efforts to-
wards lowering exposure (Khan et al., 2020). The importance of the
timing (age of the person) of As exposure, which can cause severe
health issues with significantly higher risk among those exposed to As
early in life, was highlighted by Steinmaus et al. (2014), based on the
studies in the same area. Moreover, another analysis from the same
area reported a ten-fold increase in the risk of As-associated lung dis-
eases among women exposed to high levels of As in the uterus (Roh
et al., 2018). Some other studies carried out in the same area found
that early-life exposure, even at a relatively low dose, increases the
risk of As-induced mortality from pulmonary tuberculosis, respiratory
problems, and reduced lung function in adults and children (Dauphine
et al., 2011; Recio-Vega et al., 2015; Steinmaus et al., 2016; Nardone
et al., 2017). Also, lifetime and cross-sectional analyses from Chile and
Mexico revealed high-risk potential associated with type 2 diabetes
(T2D) hypertension (Del Razo et al., 2011; Hall et al., 2017; Castriota
et al., 2018). Several workers have described the effects of As; viz.
lung, bladder, kidney, and laryngeal cancer, particularly in those pa-
tients exposed to As since their birth in the same area (Smith et al.,
2000a, 2012, 2018; Ferreccio et al., 2013a; Roh et al., 2018). The mortal-
ity studies conducted in the same area observed a consistent association
with As intake for bladder, laryngeal, and liver cancer among young
adults born in Antofagasta, Chile (Smith et al., 2000a, 2011, 2012).
Moreover, Laine et al. (2015) associated adverse birth outcomes, includ-
ing shorter gestational age, low birth weight, and smaller newborns, in
Mexico with early-life exposure to As.
Some studies during the last decade from Latin America have identi-
fied several factors that can substantially increase the risk of mortality
and morbidity from As induced chronic lung and renal diseases, repro-
ductive outcomes, and various types of cancer and other diseases
(Smith et al., 2000a, 2011, 2012; Laine et al., 2015, 2017). Also reported
were medical conditions like As methylation, metabolomics, genetic
polymorphism, obesity, through drinking water, food chain, and to-
bacco smoking (Del Razo et al., 2011; Drobná et al., 2013; Ferreccio
et al., 2013b; Martin et al., 2015; Rager et al., 2015; Laine et al., 2017;
Castriota et al., 2018). These findings suggest that interventions
targeting early-life As exposure and controlling lifestyle factors could
significantly reduce long-term mortality and morbidity. Khan et al.
(2020) have reviewed the effects of early-life As exposure on human
health, biomarkers, and genetic susceptibility in Latin American
countries.
This work presents a short general overview on the occurrence and
mobility of geogenic As in different environments and its impacts on
human health (Section 2), followed by the mode of occurrence and na-
ture of As in each of the identified geoenvironments have been analyzed
individually in detail (Section 3). The analysis comprises As origin,
release, and exposure related to (i) volcanism and geothermalism, (ii)
mineralized zones, (iii) coal deposits, (iv) hydrocarbon reservoirs,
(v) solute and sediment transport by rivers, (vi) atmospheric As (dust
and aerosol), and (vii) geophagy and involuntary ingestion. For each
of these sources and pathways, an overview of the associated
geoenvironments and their importance has been provided to address
the Latin American As problem, especially in the severely affected re-
gions, based on the limited available data. Moreover, the present work
emphasizes the mode of occurrence and mobilization of As from
sources, its environmental impacts, and propagation within the
food chain, following its intake through drinking water and food. It
also includes As uptake through geophagy and involuntary ingestion
and related health effects. However, such a transdisciplinary suite of
information is not available for all the contaminated areas in
Latin America either due to the absence or incompleteness of the
studies.
3
Science of the Total Environment 780 (2021) 146274
Moreover, there are areas with geoenvironment(s) identified as
prone to As contamination in other parts of the word; however, no re-
spective data is currently available from Latin America. In such cases,
this review highlights the existence of such As-associated
geoenvironments in Latin America (and their essential characteristics)
with the aid of existing data from related geoenvironments outside
Latin America while discussing the potential sources of As toxicity. Fi-
nally, this review underscores the importance of further steps towards
an integrated and sustainable approach for resolving the Latin
American As problem. For the contention of As exposure to Latin
American population, Tomaszewska et al (2020) have proposed the
use of low-enthalpy geothermal energy sources and waste heat from
geothermal power plants in membrane distillation (MD) processes
(the only heat-powered membrane technology) to obtain potable
water and/or water for crop irrigation. They considered MD as a solution
for obtaining water of good quality with a high retention of toxic solutes
such as As in groundwater. They further recommeded that in addition to
supplying heat, geothermal water undergone through MD process can
be used as drinking water.
In Latin America, different typical geogenic As sources and pathways
have been identified, which include natural geological biotrophic fac-
tors; viz. volcanism (e.g., As-rich ash and gas emissions), geochemical
anomalies (e.g., mineralized zones with As containing ores), fluid mi-
gration, and gas emission, especially in fault zones (e.g., ascending
deep As-rich geothermal fluids), and (hydro)(bio)geochemical pro-
cesses (e.g., groundwater contamination through leaching of As-
contaminated aquifer matrix). These sources and pathways directly
contribute to As release into near-surface environments, contaminating
water, soil, dust/aerosol, and living organisms and flora, resulting in det-
rimental effects on human health through drinking water, food inges-
tion, inhalation, or even skin contact. Besides, there are anthropogenic
sources, viz. As containing pesticides or fertilizers that contaminate
soils, roxarsone (an As compound used as an additive in chicken feed;
Fu et al., 2016). Typical cases with different areal extents and signifi-
cances are cataloged in Table 1. The respective pathways showing
how geogenic As is mobilized by natural and anthropogenic processes,
viz. mining or hydrocarbon exploitation, are presented in Fig. 2. In this
review, examples with the most holistic information available for the
typical As sources and pathways in Latin America have been given and
discussed.
2. An overview of As in the environment
Since the last decades of the 20th century, As has been the focus of
public attention due to the epidemic-like health problems through
groundwater consumption contaminated by millions of people. For ex-
ample, Bangladesh and the Indian state of West Bengal, which Smith
et al. (2000b, 2000c) described as the largest mass poisoning case in
history.
2.1. Arsenic distribution in the natural environment
Arsenic is ubiquitous, found in the atmosphere, soils, rocks, water,
and organisms, and is the twentieth most abundant element in the
earth's crust and the fifteenth in seawater (Herath et al., 2016). The
total estimated mass of As in the earth's crust is 4.01 × 1016 kg, with
an average of 6 mg kg−1 (Taylor and McLennan, 1985; Matschullat,
2000). The estimated natural release of As from the lithosphere by exha-
lations and terrestrial volcanic eruptions is 1.715 × 107 kg year −1,
added to 4.87 × 106 kg year−1 from the submarine volcanism
(Matschullat, 2000).
Arsenic can occur naturally in all the environmental compartments
(EFSA, 2009), with its existence in >245 minerals (Cox, 1995). Only a
small part of As found in nature is in its elemental form, while inorganic
As is generally found combined with other elements such as oxygen,
sulfur, and chlorine (O'Day, 2006; ATSDR, 2007a). The iron, silver,
J. Bundschuh, J. Schneider, M.A. Alam et al. Science of the Total Environment 780 (2021) 146274

Table 1
A catalogue of Arsenic (As) concentration in surface water, groundwater (μg L−1), and sediments (mg kg−1) in different geoenvironments in Latin America.

Geoenvironment Location Sample Range Mean References

Geogenic As sources and natural release

(Section 3.1)
(i) Volcanism and Geothermal systems Argentina: Pampa GW* 0.003–1.33 Smedley et al., 2002; O'Reilly et al., 2010
(Sections 3.1.1 and 3.1.3) Puna plateau, Argentinean GW* 6.17 Peralta Arnold et al., 2017
Andes
Chile GW* 2 Chong et al., 2010; Cortecci et al., 2005; Hauser,
1997; Sánchez-Yañez et al., 2017
Aguascalientes city (México) GW* 0.05 Trejo-Vázquez and Bonilla-Petriciolet, 2002
(ii) Large-scale transport of As containing Argentina: Chaco-Pampean
highly soluble volcanic ash affecting ground plain (Fig. 3)
and surface water (Sections 3.1.2 and 3.1.4) (i) Salí and Burruyacú basins; GW 6–250 61.5 (i) Nicolli et al., 2004, 2009a
(ii) Río Dulce cone; GW 2–13,494 411 (ii) Claesson and Fagerberg, 2003; Bejarano
Sifuentes and Nordberg, 2003; Mellano and
Ramirez, 2004; Bundschuh et al., 2004; Lindback
and Sjolin, 2006
(iii) Southeatern part of GW 103–3810 390 (iii) Nicolli et al., 1985
Córdoba province;
(iv) Central notrthern part of GW 0.015–780 97.8 (iv) Nicolli et al., 2009b
the Santa Fe province;
(v) Northern part of the La GW 4–5280 372 (v) Smedley et al., 2002
Pampa province
Technically enhanced geogenic Brazil: The Iron Quadrangle GW <5 to 2980 450 Borba et al., 2004; Gonçalves et al., 2007;
Arsenic Matschullat et al., 2000; Deschamps and
Metal ore deposits and accelerated exposure Matschullat, 2007; Bundschuh et al., 2012a, 2012b
related to mining (Section 3.2) Brazil: The Iron Quadrangle SW 3–349 nr Matschullat et al., 2000; Deschamps et al., 2002;
Borba et al., 2003; Mello et al., 2006; de Mello
et al., 2007; Deschamps and Matschullat, 2007;
Bundschuh et al., 2012a, 2012b
Brazil: The Ribeira Valley SW 1–9 nr Takamori and Figueiredo, 2002; Figueiredo et al.,
2010
Brazil: Paracatu SD 150 to >1000 de Rezende, 2009; Mello et al., 2006; Ono et al.,
2011, 2012; de Andrade et al., 2012; Bidone et al.,
2014; Egler et al., 2014; de Mello et al., 2014;
Sabadini-Santos et al., 2014; Guilherme et al.,
2014; Rezende et al., 2015; Bidone et al., 2018
Brazil: The Santana District SW ND to >50 nr Figueiredo et al., 2010
Brazil: The Santana District SD 696–1600 nr Lima, 2003
Chile: Illapata SW 48.7–1252 nr Yañez et al., 2005
Peru: 5 districts
(i) Achaya (Ramis river) SW 7.1–31.5 16.9 George et al., 2014
(ii) La Oroya (La Oroya) 2.2–13.3 7.7
(iii) Lima (Rimac river; 14.6–42.5
Fig. 4)
(iv) Puno (Collacachi) nr 21.7
(v) Taraco (Ramis) 1.4–13.6 5.8
Peru: 7 districts
(i) Achaya GW nr 4.6 George et al., 2014
(ii) Ananea nr 0.1
(iii) Caracoto 31.9–113.1 67.0
(iv) Juliaca 1.6–154.8 51.7
(v) Plateria nr 0.1
(vi) San Antón 45.6–59.4 52.5
(vii) Taraco 9.6–63.0 29.6
Colombia: 3 districts SD ND to >40 nr Arias Espana et al., 2018
Tolima, Caldas and Nariño
Mexico: Zimapán GW 0.06–0.42 0.31 Sracek et al., 2010
Guatemala: Chimaltenango GW 0.44–49 47.5 Lotter et al., 2014
Geogenic As exposure related to coal Southern Brazil: Figueira SD 253–2176 3.4 Campaner and Luiz-Silva, 2009; Campaner et al.,
exploitation (Section 3.3) region, northern part of the 2014
state of Paraná
Southern Brazil: Figueira SW <0.0006–0.0018 nr Campaner et al., 2014
region, northern part of the
state of Paraná
As in co-produced water from hydrocarbon SE Mexico Produced Up to 2000 nr Birkle et al., 2010
exploration and production (E&P) Water
(Section 3.4) Brazilian offshore platforms Produced 5–12 nr Gabardo et al., 2011
Water
Rivers with naturally and anthropogenic As-rich Paraíba do Sul river basin SPM nr 6 Viana, 2013
water and sediments discharging into the sea Paraíba do Sul river basin SD ND to >270 nr Mirlean et al., 2014
(Section 3.5) Paracatu river SW nr 31 Rezende et al., 2015; Bidone et al., 2014; Bidone
et al., 2018
Nicaragua: 7 Communities
(i) El Mojón GW 0.4–2.6 1.6 Barragne-Bigot, 2004
(ii) Cerro Mina de Água 0.6–12.5 3.0
(iii) El Charco and Santa 3.2–95.0 19.7

4
J. Bundschuh, J. Schneider, M.A. Alam et al.
Table 1 (continued)
Geoenvironment Location
Rosa del Peñón
(iv) La Cruz de la India
(v) Las Pilas
(vi) Kinuma
Brazil: Cast áreas, viz. Rio de
Janeiro, Bahia and Espirito
Santo states
Peru: Western Amazonia
Atmospheric As (dust and aerosol) (Section 3.6) Brazil: Patos Lagoon estuary
Brazil: Paracatu
Geophagy and involuntary ingestion Tanzania[a]
(Section 3.7)
SW: Surface water (μg.L−1).
GW: Groundwater (μg L−1).
GW*: Groundwater (mg L−1).
SD: Sediments (mg kg−1).
SPM: Suspended particulate material (mg kg−1).
RW: Rainwater (μg L−1).
ASPM: Atmospheric suspended particulate matter (ng m−3).
nr: not reported.
ND: No detected.
[a] Referential data, in the absence of similar research in Latin America.
⁎ Oral Minimal Risk Levels (MRLs) in mg kg−1/day for chronic exposure to chemical element as established by ATSDR (2007a) [0.0003 mg kg−1/day].
lead, copper, nickel, antimony, and cobalt deposits contain As bearing
minerals abundantly (WHO, 2001). Arsenopyrite (FeAsS) is the most
common As-bearing mineral, followed by pigment gold (As2S3), realgar
(As4S4), and loellingite (FeAs2) (WHO, 2001). The presence of As in vol-
atile forms is generally neglected due to its low occurrence in the
environment.
2.2. Arsenic in groundwater
In general, the predominance of As in the dissolved fraction occurs in
reducing environments (Fendorf et al., 2010), which justifies the pres-
ence of As in groundwater, where reducing conditions prevail; while
the opposite is the case for surface water, with the absence of As in ox-
idizing conditions. Surface water resources, such as lakes and rivers, are
less contaminated by As compared to groundwater, the high As values
of which (>50 μg L−1) can often be a result of the mixing of As-rich geo-
thermal waters and the presence of As bearing minerals, such as arseno-
pyrite (Borba et al., 2004) in the aquifer rocks. On the other hand, As
concentration is low in rivers draining sedimentary terrains, as sedi-
mentary rocks generally contain low As levels (Barats et al., 2014).
2.3. Arsenic in the food chain
Contamination through food largely depends on the levels of As in
water and soil to which these foods are exposed (Huq et al., 2006;
Komárek et al., 2007; EFSA, 2009). Animals consumed by a population
may have an exposure to As through ingestion of contaminated water
and food, followed by bioaccumulation of this element in their tissues
(Dionísio et al., 2011).
Concerning animals used for human consumption, the effect of
chronic contamination by As through food intake is still not entirely
clear in chickens (Ghosh et al., 2012). The organs usually have a more
significant amount of contaminant than the muscles, especially the
skin and the liver (Ghosh et al., 2012; Islam et al., 2013; Caldas et al.,
2016; Hu et al., 2017). Organoarsenic stimulants, used in poultry
farms due to their antibiotic functions, aid in developing and enhancing
meat color (Fu et al., 2016). Despite their low toxicity, these stimulants
can be metabolized in inorganic As, creating a risk of human exposure
(Dionisio et al., 2011; Nachman et al., 2013).
The aquatic environment favors the accumulation of As mainly in
algae and invertebrates (exoskeleton). Detritivorous fishes are more ex-
posed to As, given their eating habits, with As accumulated mostly in
Science of the Total Environment 780 (2021) 146274
Sample Range Mean References
1.3–90.2 16.6
0.5–8.6 2.7
1.7–106.7 33.1
SD 2.55–232.3 59.1 Mirlean et al., 2011, 2012, 2013, 2016; Cagnin
et al., 2017
GW >0.5–715 10 de Meyer et al., 2017
RW NDto 35.6 9.13 Mirlean and Roisenberg, 2006
ASPM <0.64 to 18.8 5.7 de Mello et al., 2014
Pregnant 0.0002–0.045 0.0003⁎ Quansah et al., 2015
women
their liver (EFSA, 2009). Arsenic sources of the oceans are diffuse and
contribute As in inorganic, viz. arsenates [As(V)] and arsenites [As
(III)], as well as organic forms, viz. monomethylarsonic (MMA) and
dimethylarsinic (DMA) acids (Sakuma, 2004; see Section 2.4 for further
details on As speciation and its toxicity). Marine fish and other seafood
play a prominent role in the accumulation of As, although it is mainly in
the form of arsenobetaine as an organic form of low toxicity (EFSA,
2009).
2.4. Arsenic speciation and its toxicity
Another critical consideration is As speciation (Fig. 1) since not all its
species are equally toxic. In fact, As toxicity depends on its speciation in
the following order: [As(III)] > [As(V)] > organoarsenicals (Fergusson,
1990). Moreover, its toxicity varies widely with its oxidation state. Arse-
nic commonly exists in both inorganic and organic forms (Fig. 1), as tri-
valent [As(III)] and pentavalent [As(V)] arsenicals. However, [As(III)]
species, including methylated compounds (monomethylarsonic
(MMA) and dimethylarsinic (DMA) acids), are more toxic than [As
(V)] species. The latter is because methylated [As(III)] compounds are
more reactive towards tissue biomolecules than their [As(V)] counter-
parts (Kalman et al., 2014). In this process ([iAs(V)] → [iAs(III)] →
[MMA(V)] → [MMA(III)] → [DMA(V)]; more details in Fig. 1), inorganic
pentavalent As [iAs(V)] first reduces to the more toxic inorganic triva-
lent As [iAs(III)]. It then methylates and oxidizes to [As(V)] bearing
monomethylarsonic [MMA(V)] acid simultaneously (Challenger, 1945;
Bhumbla and Keefer, 1994; Akter et al., 2005; Rehman and
Naranmandura, 2012). The latter then reduces to trivalent As [As(III)]
bearing monomethylarsonous [(MMA(III)] acid. During oxidative meth-
ylation, it is transformed into dimethylarsinic [(DMA(V)] acid, which
then reduces to dimethylarsinous [(DMA(III)] acid (Khairul et al.,
2017). Once released to the atmosphere by microorganisms, these spe-
cies oxidize in non-volatile species and deposit again in the lithosphere
(ATSDR, 2007a). According to WHO (1981, 2001), inorganic species are
generally more toxic than organic ones. Moreover, arsenite [As(III)] is
60 times more toxic than arsenate [As(V)], which is 70 times more
toxic than methylated (MMA and DMA) species. While methylated spe-
cies are moderately toxic, arsenobetaine (AsB) and arsenocholine (AsC)
are nontoxic (Kumaresan and Riyazuddin, 2001). Therefore, for an accu-
rate environmental and human health risk assessment, identification
and quantification of the As species is essential, especially the more
toxic ones, rather than merely reporting total As concentrations, as
5
J. Bundschuh, J. Schneider, M.A. Alam et al.
Fig. 1. Redox potential (Eh)–pH diagram for arsenic speciation in the aqueous system [As-O2-H2O] at 25 °C and 1 bar (adapted from Smedley and Kinniburgh, 2002). (b) Transformation of
arsenic species (adapted from Bhumbla and Keefer, 1994; Akter et al., 2005) (c) Chemical structures of some toxicologically relevant arsenic species mentioned on the Section 2.2.
has been the norm for several decades. Understanding As behavior is
crucial for developing tools for strengthening remediation measures to
mitigate As and other contamination of soils, sediments, and water.
2.5. Arsenic exposure
According to the U.S. Environmental Protection Agency (US EPA,
1992, 2002, 2019), the term ‘exposure’ can be defined qualitatively as
the contact made between the agent (chemical, physical or biological)
and the outer boundary of an organism. The quantification of exposure
is the amount or concentration of the agent in its transport or carrier
medium (viz. soil, water, or air) at the organism's exchange boundaries
(i.e., point of contact), available for uptake and intake by an organism.
The term ‘intake’ describes an agent's entry into an organism (e.g., via
ingestion or inhalation) without passing an absorption barrier (IPCS,
2004; EUGRIS, 2007; US EPA, 2011). On the other hand, the term ‘up-
take’ describes the agent's absorption into an organism's circulatory sys-
tem (e.g., absorption of an agent through human skin into the blood;
IPCS, 2004; EUGRIS, 2007; US EPA, 2011). The term ‘dose,’ defined as
the amount of a substance available for interactions with metabolic pro-
cesses or biologically significant receptors after crossing the outer
boundary of an organism, in term of mass (of an agent) per body weight
per period of time, quantifies both intake and uptake (US EPA, 1992,
2002, 2019).
Arsenic sources can be local or dispersed in air and water, thus
transported over long distances as suspended particles, aerosols, or in
its gaseous form (Nriagu et al., 2007). Apart from these natural activi-
ties, As can originate from anthropogenic activities as well. The particles
produced by the foundries of Pb, Au, Pt, Cu, Zn, and Co represent an es-
sential source of As in solid, aqueous, and gaseous forms, later being
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Science of the Total Environment 780 (2021) 146274
particularly important (Krishnaraj, 2015). Other exposure sources in-
clude burning fossil fuels, agricultural products such as insecticides, her-
bicides, wood preservatives, glass, enamels, paints, fabrics, and leather
manufacturing (Gontijo and Bittencourt, 2005). Volcanic activities,
weathering of sulfurized gold rocks, hydrothermal mineral deposits,
natural fires, and marine spray are the primary natural sources of As
emissions to the environment (Nriagu et al., 2007).
2.6. Arsenic related health issues
The presence of As in the environment does not always lead to expo-
sure, and it is exposure to As, not merely its presence, that causes ad-
verse health effects, i.e., when one comes into contact with it. The
adverse health effects of As exposure depends on several factors; viz.
amount of exposure (dose), way of exposure (contact, inhalation, inges-
tion, etc.), duration of exposure, chemical form (As species), together
with co-exposure to other toxic elements (s) (ATSDR, 2007b). Please
see Section 2.5 for more details on the terms like exposure, intake, up-
take, and dose used in this section and elsewhere in this review.
Arsenic uptake can affect several organ systems, viz. dermal (skin),
gastrointestinal (digestion), peptic (liver), neurological (nervous sys-
tem), respiratory (from the nose to the lungs), and reproductive (fertil-
ity, pregnancy, and childbirth) following exposure (e.g., Abernathy
et al., 2003; ATSDR, 2007a, 2007b, 2016, 2017; Chung et al., 2014). Ac-
cordingly, ingesting large amounts of As can damage the stomach, kid-
neys, liver, heart, and nervous system, and in severe cases, may cause
death (ATSDR, 2007a, 2007b, 2016). Moreover, breathing air with high
As levels can cause lung damage, shortness of breath, chest pain, and
cough, leading to death in severe cases (ATSDR, 2007a, 2007b, 2016,
2017). Further, As compounds, being corrosive, can also cause skin
J. Bundschuh, J. Schneider, M.A. Alam et al.
Fig. 2. Geogenic and antropogenic sources of arsenic, its mobilization into different environments and pathways to humans.
lesions or damage eyes, and long term As exposure can cause adverse
effects and changes to the skin and blood circulation (ATSDR, 2007a,
2007b, 2016, 2017). The International Agency for Research on Cancer
(IARC, 1973, 1980, 1987, 2004, 2012), US EPA (1984, 1988, 1992,
1997, 2002, 2011, 2019), National Toxicology Program (NTP, 2016) of
the U.S. Department of Health and Human Services have classified As
and its compounds as cancer-causing (carcinogenic) chemicals. Accord-
ingly, long term As exposure may cause lung, skin, and bladder cancers,
while short-term As exposure is likely to be associated at the most with
only a minimal risk of cancer. In some regional studies on women and
children in different parts of the world, including Latin America, viz.
Bangladesh (e.g. Ahmad et al., 2001; Hopenhayn et al., 2003; Ahamed
et al., 2006; von Ehrenstein et al., 2006; Rahman et al., 2007; Cherry
et al., 2008; Bloom et al., 2014; Kile et al., 2015; Rahman et al., 2017,
2018), West Bengal state of India (e.g. Chakraborti et al., 2004;
Mukherjee et al., 2005; von Ehrenstein et al., 2006), China (e.g. Myers
et al., 2010; Xu et al., 2011; Liang et al., 2020; Liu et al., 2018; Song
et al., 2019), Taiwan (e.g. Yang et al., 2003; Chou et al., 2012),
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Science of the Total Environment 780 (2021) 146274
Argentina (e.g. Concha et al., 1998) and Chile (e.g. Hopenhayn-Rich
et al., 2000; Hopenhayn et al., 2003; Smith et al., 2000a, 2011,
2012; Vormittag et al., 2018; Khan et al., 2020), Tenerife Island,
Spain (e.g. Vall et al., 2012), Mexico (e.g. Laine et al., 2015), USA
(e.g. Shi et al., 2015; Claus Henn et al., 2016; Gilbert-Diamond
et al., 2016; Almberg et al., 2017), where very high levels of As are
found in drinking water, effects such as a low birth weight and
death of the unborn child or young infant have been observed rela-
tively frequently, as evident in the reviews based on global data by
various workers (e.g. Bloom et al., 2014 and Quansah et al., 2015).
Similarly, in some experimental studies on animals, adverse effects
on reproduction (e.g., fertility and pregnancy issues affecting
mothers, intrauterine growth and congenital abnormalities affecting
the fetus, or fertility issues in men) were observed following expo-
sure to high As levels (e.g., Danielsson et al., 1984; Vreeburg et al.,
1988; Biswas et al., 1994; Pant et al., 2001, 2004; Uckun et al.,
2002; Sarkar et al., 2003; Chinoy et al., 2004; Hardy et al., 2005;
Jana et al., 2006; Chang et al., 2007).
J. Bundschuh, J. Schneider, M.A. Alam et al.
2.7. Arsenic related environmental regulations
The reviews of the permissible legal limit of As in potable water of
many countries consider the updated scientific knowledge about the
toxic effects of As due to ingestion of As-contaminated water (Ahmad
et al., 2018; Ersbøll et al., 2018; Ahmad and Bhattacharya, 2019). The
World Health Organization (WHO, 1993) reference value for As in
drinking water was reduced from 50 to 10 μg L−1 based on its carcino-
genic potential, following the detection of the permissible limit at lower
concentrations due to analytical advancement of the detection tech-
niques. The US EPA (2000) suggested a limit of 5 μg L−1 in drinking
water to ensure a better safety margin, which did not get accepted be-
cause of its financial implications (Smith et al., 2002). In Brazil,
CONAMA (2005, 2008), which regulates surface and groundwater qual-
ity respectively, established the maximum permissible As concentration
in drinking water to be 10 μg L−1. In Mexico, the corresponding limit for
As is 25 μg L−1 (Mexico, 2017), although there is a proposal to reduce it
to 10 μg L−1 (Osuna-Martínez et al., 2021). Some countries still maintain
the previous 50 μg L−1 limit, viz. Bangladesh, India (Rahman et al.,
2015). Although India has reduced the acceptable limit to 10 μg L−1, it
still maintains the earlier permissible limit of 50 μg L−1 in the absence
of an alternate water source (BIS, 2012; UNICEF, 2018).
3. Known and potential sources of As pollution in Latin America
3.1. Volcanism and geothermalism
Latin American active volcanoes and geothermal systems have been
the focus of numerous geochemical investigations. However, despite As
being a known contaminant in these environments, there are only a few
studies on its origin, mobility, speciation, and environmental and
human health (e.g., Morales et al., 2015; Morales-Simfors et al., 2020).
3.1.1. Arsenic related to volcanism
In Latin America, many densely populated areas are located in the
proximity of active volcanic areas with high As concentrations;
e.g., Momotombo (0.79 mg L−1, Nicaragua), Santa Ana (0.020 mg L−1,
El Salvador), Popocatépetl (1.2 mg L−1, Mexico), and Ubinas (0.17 mg
L−1, Peru) volcanoes and Copahue crater lake (0.87 mg L−1,
Argentina). Thus a significant Latin American population is coexposed
to volcanic and health hazards (Bundschuh et al., 2020, and references
therein). The risk of natural exposure to As and other geogenic contam-
inants (e.g., B, Zn, Mo, Sn, Sb, Tl, Pb) following future eruptions are sig-
nificant with increasing migration to large cities (e.g., Mexico City,
Guatemala City, San Salvador, San Jose, Quito) located close to the volca-
noes. Due to the anomalous concentrations of As and other geogenic
contaminants, natural waters and water supplies are significantly im-
pacted negatively, with increasing turbidity levels (with volcanic ash
suspended in water), acidity, and presence of toxic elements (Stewart
et al., 2006). On the other hand, groundwater is affected by As trans-
ferred by mixing of As-rich geothermal/magmatic fluids to shallower
aquifers (Morales-Simfors et al., 2020). For example, in the aquifers re-
lated to San Salvador and San Miguel volcanoes in El Salvador, most of
the wells contain high As (0.040 mg L−1 in San Salvador and 0.022 mg
L−1 in San Miguel) concentrations. Of these two active volcanoes, the
former is within the city limits of San Salvador, which has a metropoli-
tan population of 2.4 million (UN, 2019), while the latter is only 11 km
away from San Miguel city. It is worth mentioning that the wells tapping
these aquifers supply water for drinking purpose (Morales-Simfors
et al., 2020). On the other hand, the source of As contamination of
Callazas and Salado rivers in the Tacna region of Peru is the Yucamane
volcano, which affects the communities living near this volcano
(McClintock et al., 2012). Moreover, As concentrations in the Yucamane
geothermal discharges range from 0.34 to 11.1 mg L−1 (F. Arlington
Apaza, personal communication, 2019), suggesting that people using
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Science of the Total Environment 780 (2021) 146274
this contaminated thermal water are vulnerable to As pollution, which
further increases the risk of severe health issues in the area.
Volcanic activity can also affect areas hundreds or thousands of kilo-
meters away due to airborne dispersion of gases and ash. or even at a
hemispheric to global scale due to climate impacts (Hansell et al.,
2006). For example, the deposition of volcanic ash due to the volcanism
in the Andean arc may be one of the possible sources of high As concen-
trations in many regions of the Chaco-Pampean plain of Argentina
(Smedley et al., 2002; Nicolli et al., 2012; Bundschuh et al., 2012a). Ac-
cording to Smedley et al. (2002), deeper groundwater and shallow aqui-
fers showed high As concentration of around <0.010 - > 5 mg L−1 and
<0.004–5.280 mg L−1, respectively. In this region, As often occurs to-
gether with F, V, and Mo in groundwater (Bundschuh et al., 2012a; J.
Bundschuh et al., 2017). This highly contaminated water is used as
drinking water and for irrigation purposes in the region (see
Section 3.1.4, in this work). For example, El Chichón volcano's crater
lake caused the most devastating volcanic eruption in the 20th century
in Mexico (López et al., 2012), leading to a significant impact on global
climate (Robock, 2000). Rouwet et al. (2009) reported As concentration
between 0.0008 and 0.060 mg L−1 in thermal and cold spring waters at
El Chichón for the period 2006–2007. All thermal springs discharge into
the Magdalena River that drains towards the Gulf of Mexico.
Arsenic concentrations in volcanic materials have been poorly mon-
itored and studied despite being a well-known toxic and carcinogenic
metalloid (Roy and Saha, 2002; Bundschuh et al., 2012a, 2012b; J.
Bundschuh et al., 2017; M. Bundschuh et al., 2017) and a conspicuous
component of volcanic gases. It is found in various chemical species
throughout the environment and can be readily transformed and mobi-
lized by microbes, changes in geochemical conditions, and other envi-
ronmental processes (Bundschuh and Maity, 2015; J. Bundschuh et al.,
2017; M. Bundschuh et al., 2017). understand the behavior of As and
its compounds is essential for assessing their environmental and health
impacts. This task can be accomplished by investigating the (hydro)geo-
chemical variation of As and other mobile contaminants during the
magmatic and hydrothermal processes.
3.1.2. Large-scale transport of As containing highly soluble volcanic ash
The young and ongoing volcanic activity marks the Andean Cordil-
lera and the mountain ranges of Central America and Mexico, gives
rise to different geogenic As sources and pathways for As. Arsenic pres-
ent in volcanic ash is primarily concentrated in the rhyolitic volcanic
glass. This glass is easily soluble in water (e.g., surface and groundwater)
due to its amorphous character. The As bearing volcanic glass in volcanic
ash may get deposited locally or is transported by rivers (fluvial) or
wind (eolic) into the forelands, away from the mountains, where it
mixes with other sediments (long term process) that subsequently con-
stitute aquifer matrices together. A significant portion of the emitted ash
is directly transported in the atmosphere to the foreland (short-term,
within a few days after the volcanic eruption). Thus It can significantly
impact surface water bodies, soils, etc. Besides, the volcanic rocks in
the mountain ranges can be the source of As, when eroded and
transported into the forelands, affecting these environments. Conse-
quently, the Andes and the volcanic regions of Central America and
Mexico are permanent As sources. However, varying climatic and
(hydro)geochemical conditions and other parameters impact the re-
lease, mobility, and accumulation of As in the foreland aquifers;
e.g., dry (arid to semiarid) and hot climate favors it.
These processes were studied intensively in Argentina, especially in
the Chaco-Pampean Plain (see the Example: Chaco-Pampean Plain).
However, despite an analogous As source and geological setting existent
in the Peruvian Andes, such association was not reported until a recent
study documented As in the foreland groundwater (de Meyer et al.,
2017). These authors carried out the first integrated survey on the oc-
currence and distribution of geogenic contaminants (including As) in
groundwater resources of western Amazonia in Peru. These authors re-
port the existence of quite a few studies on the chemical quality of
J. Bundschuh, J. Schneider, M.A. Alam et al.
groundwater. On the other hand, there has been a significant increase in
groundwater wells providing drinking water in this area during recent
decades. Most of the wells evaluated by de Meyer et al. (2017) have
As (up to 700 μg L−1), aluminum (up to 3.3 mg L−1), and manganese
(up to 4 mg L−1) at levels harmful to human health. High concentrations
of toxic elements highlight the urgent need to assess groundwater qual-
ity throughout western Amazonia and further north along the Andes in
its foreland.
Arsenic composition of volcanic ashes collected after eruptions of the
volcanos Hudson in 1991, Chaitén in 2008, and Puyehue in 2011 (all in
Chile) were analyzed to determine As speciation and to get information
about the mechanisms of As release to the aquatic systems (Bia et al.,
2015). The bulk chemical and mineralogical composition was determined
using different techniques (ICP/OES, XRD, and SEM/EDS). The near-
surface (2–10 nm) analysis of the ash samples using X-ray photoelectron
spectrometry (XPS) was used to determine its composition and solid
speciation of As and Fe. Leaching experiments at variable pH were also
carried out to understand the kinetics of As release. The results showed
that As is in the form of As(III)-S and As(V)-O bonding species at the
ash surface, with As(V)-O species related to adsorbed arsenate ion or Fe
arsenate salts precipitating as a thin layer on the surface. However, the
main As carrier was the Al-silicate glass present in the ash (94%), and As
on the surface was more mobile, i.e., quickly releasing to the water.
Example: Chaco-Pampean Plain (Argentina, Bolivia, Paraguay)
The most well-known area affected by contamination, which is also
the largest of its kind, is the Chaco-Pampean Plain covering over one
million square kilometers. It stretches over large parts of Argentina
and extends into Bolivia and Paraguay (Fig. 3). However, practically no
data is available from these last two countries.
A. Arsenic origin and mobilization
With coverage of about 1 million square kilometers, the Chaco-
Pampean Plain is the world's largest known region with groundwater
As concentrations at toxic levels (>10 μg L−1; WHO, 2010). It covers
all or parts of La Pampa, Buenos Aires, Mendoza, San Luis, San Juan La
Rioja, Santa Fe, Cordoba, Tucumán, Santiago del Estero, Chaco, Salta,
and Formosa provinces (Fig. 3). However, the level of As exposure in
each of the affected areas is different. Some localities have the water
supply through a distribution network that does not have a removal
plant for As; thus, the supplied water generally contains As. The occur-
rence of As and its adverse health effects, such as skin lesions, were first
reported more than a century ago from Córdoba province (Belville;
Goyenechea, 1917; Ayerza, 1917a, 1917b). Ever since research has con-
tinued; however, it took until the 1990s to get momentum (e.g., Nicolli
et al., 1989, 2001a, 2001b, 2004, 2009a, 2009b; Smedley and
Kinniburgh, 2002; Smedley et al., 2005; Bhattacharya et al., 2006;
Farías et al., 2003; Bundschuh et al., 2004; Litter et al., 2019). This mo-
mentum led to some significant studies in the region; viz. hydro(geo)
chemistry of groundwater, hydrogeology (e.g., groundwater flow pat-
tern and local recharge), geochemistry, and mineralogy/sedimentology
of aquifer sediments and their interconnections (e.g., As sources, mobi-
lization/immobilization, transport). In the following analysis, the most
complete data sets available from 5 regions of the Chaco Pampean
Plain have been used to discuss the geochemical setting and the corre-
lation of As concentration to other elements. The studied parts of the
Chaco-Pampean Plain are: (i) northwestern areas: Salí and Burruyacú
basins (separated in shallow, artesian and deep aquifers); (ii) central
areas: Río Dulce cone; (iii) eastern area of Córdoba province; (iv) east-
ern areas: northern part of the Santa Fe province; (v) southern areas:
northern part of the La Pampa province. The main As species
found in moderately reducing to oxidizing groundwater environments
is [As(V)] the concentration of which positively correlates with those
of V (r = 0.66, 0.58, 0.57, 0.86, 0.85), Mo (r = 0.64, 0.62, −0.02, 0.76,
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Science of the Total Environment 780 (2021) 146274
0.26), U (r = U: 0.60, 0.22, 0.42, 0.30, 0.32), B (r = 0.54, 0.75, 0.78,
0.28, 0.27) and F (r = 0.38, 0.87, na, 0.83, 0.70; na: not available; p <
0.05). This correlation is because of the same source of these elements,
i.e., volcanic ash transported by wind or rivers from the Andes to the
Chaco Pampean Plain, where it is found as layers or is dispersed in the
aquifer sediments (5–25%). These deposits, under favorable geochemi-
cal conditions, can be easily dissolved by groundwater because the vol-
canic ash of the sediments is over 90% amorphous (rhyolitic glass with
5–8 mg kg−1 of As; Nicolli et al., 1989, 2012; Smedley et al., 2002,
2005; Bundschuh et al., 2004, 2012a, Bhattacharya et al., 2006; Litter
et al., 2019) and therefore highly soluble. During the transport, it
might precipitate or get adsorbed again (e.g., on Fe and Al (oxy)hydrox-
ides) if geochemical conditions change and favor these processes. For
example, Ca-HCO3 type near-neutral pH groundwater represents the
areas with low As concentrations in groundwater; whereas, Na-HCO3
type high pH (>8) represents the areas with high As concentrations in
groundwater, as under such conditions As can be remobilized or dis-
solved. These geochemical conditions, changing in time and space, ex-
plain the variation in As concentrations even at very short distances
(even within few meters, explaining the wide range of As concentra-
tions and pH and Eh values). In the five regions of the Chaco-Pampean
plain, there is a patchy distribution of As concentration, wherein the
patches correspond to the so-called “hot spots” of As that are very typ-
ical of this plain (Bundschuh et al., 2004, 2012a; Bhattacharya et al.,
2006; Raychowdhury et al. (2014). These changing geochemical condi-
tions have been attributed to ion exchange as the principal chemical
process. Additionally, competing ions for adsorption sites and evapora-
tive As increase must be considered. Ion exchange is favored in areas
with higher groundwater residence time, facilitating longer contact be-
tween groundwater and aquifer sediments, where Na from the sedi-
ment is interchanged with Ca2+ and Mg2+ from the aqueous phase,
resulting in the NaHCO3 groundwater type and pH increase. This in-
crease in pH favors As desorption from (Fe, Mn) (oxy)hydroxides)
found in the areas with high groundwater As concentrations (Nicolli
et al., 1989, 2010, 2012; Smedley et al., 2002, 2005; Bundschuh et al.,
2004, 2012a; Bhattacharya et al., 2006; Raychowdhury et al., 2014).
This is supported by the positive correlation of As with pH (r = 0.18,
0.12, 0.33, 0.51, 0.47), Na (r = 0.55, 0.16, −0.01, −0.12, 0.01) and the
negative correlation factors of As with Ca (r = 0.16, −0.15, −0.25,
−0.29, −0.21) and Mg (r = 0.10, −0.15, −0.23, −0.25, −0.19) (p <
0.05) for these five areas. However, relatively low correlation coeffi-
cients (r) suggest that ion exchange is not the only process.
B. Arsenic transfer into the human food chain
In the Chaco-Pampean plain, human exposure to As is primarily at-
tributed to ingestion of As-contaminated groundwater (Pérez Carrera
and Fernández-Cirelli, 2014; Pérez-Carrera et al., 2010, 2016a, 2016b),
which is either directly used for drinking or food preparation
(Bundschuh et al., 2012b). Despite this being the most likely source
and mechanism of As exposure, few studies are reporting other As
sources affecting human health; viz., As contaminated food products,
e.g., vegetables, meat and milk products, cereals, eggs, poultry, seafood,
etc. (Branco Corguinha et al., 2015; Pérez-Carrera et al., 2010, 2016a,
2016b). The Panel on Contaminants in the Food Chain of European
Food Safety Authority (CONTAM Panel, EFSA; https://www.efsa.
europa.eu/en/panels/contam) identified a benchmark dose of lower
confidence limit (BMDL10) ranging between 0.3 and 8 μg kg−1 bw
(bodyweight) per day for different types of cancer (EFSA, 2009). This
benchmarking does not consider very low (<0.3 μg kg−1 bw) As expo-
sure limit through dietary intake. Arsenic in food originates from differ-
ent environmental matrices, such as potable and irrigation water and
soil (Branco Corguinha et al., 2015; Otero et al., 2016; Ciminelli et al.,
2017). To evaluate As transfer to the human food chain, several authors
use indexes such as biotransfer factor (BTF; Stevens, 1991; Dowdy et al.,
1996; Pérez Carrera and Fernández Cirelli, 2005; Monagali et al., 2018).
J. Bundschuh, J. Schneider, M.A. Alam et al. Science of the Total Environment 780 (2021) 146274

3
2

Atlantic Ocean

Fig. 3. The Chaco Pappean Plain of Argenina with selected principal areas affected by arsenic in groundwater: 1: Burruyacú basin (eastern plain of Tucumán Province); 2: Salí River basin
(eastern plain of Tucumán Province); 3: Río Dulce cone; 4: southeastern part of Córdoba province; 5: central-northern part of the Santa Fe province; and 6: northern part of the La Pampa
province. The digital elevation model is courtesy of NASA/JPL-Caltech (http://photojournal.jpl.nasa.gov).

C. Arsenic contamination in food production
(i) Dairy products
The primary livestock in Latin America is cattle, with Argentina
(practically exclusively the Chaco Pampean Plain) being the second-
largest dairy producer in the region (after Brazil and before Mexico;
FAO, 2020). Therefore, the BTF of As to dairy products has been studied
in some Argentine areas to estimate the risk of As exposure through the
environmental matrix. However, despite the importance of possible As
presence, studies on BTF remain scarce.
Pérez Carrera and Fernández Cirelli (2005, 2007) and Pérez-Carrera
et al. (2010, 2016b) evaluated As content in muscle, liver, kidney, and
milk in cattle from the southeastern part of Córdoba province
(Argentina). A very low BTF value (from 1.5 × 10−5 to 4.3 × 10−4 day
L−1) was calculated for milk, assuming drinking water as the only
source of As biotransfer for bovine milk (Pérez Carrera and Fernández
Cirelli, 2005). These values were similar to the estimated values of BTF
found in Comarca Lagunera (Mexico), ranging from 3.2 × 10−5 to 6.7
× 10−4 day L−1 (Rosas et al., 1999). When As content in forage was
taken into account, together with As water content, to estimate BTF,
there were no significant changes in the estimates (Pérez Carrera and

10
J. Bundschuh, J. Schneider, M.A. Alam et al.
Fernández Cirelli, 2007). A more recent study in the Chaco-Pampean
Plain reported BTF values between 1.5 × 10−5 and 7.3 × 10−4 day L−1.
An inverse relationship exists between As concentration in drinking
water and BTF values. These BTF values were used to estimate As con-
tent in milk (0.5 to 8.0 μg L−1) from As levels in water (16 to 2190 μg
L−1; Pérez-Carrera et al., 2016b). In another region of the Chaco-
Pampean Plain, in Santa Fe province, As values were below 10 μg L−1
in milk, despite high As levels (>100 μg L−1 in 9 samples) in animal
drinking water (Sigrist et al., 2010). Additionally, total As (Astot) content
present in dairy products was determined. Sigrist et al. (2016) esti-
mated the inorganic As (Asin) level from Astot and the contribution
through the human dietary intake (0.9 μg kg−1 of Astot with <0.9 Asin
μg kg−1 and 28 μg kg−1 of Astot with <20 Asin μg kg−1 in cheese).
(ii) Meat products
On the other hand, beef and other bovine tissues from the Chaco-
Pampean plain are the leading products in the local and international
market. Therefore, it is essential to assure their quality and safety.
Pérez-Carrera et al. (2010) and Pérez-Carrera et al. (2016a, 2016b) ana-
lyzed As contents of ingested contaminated groundwater (geogenic
sources) in bovine tissues. In this study, As was not detected in bovine
muscle or mammary gland tissues (<50 ng g−1); but in bovine liver
and kidney, the mean As concentration was found to be 3.8 mg kg−1
and 43.8 mg kg−1 dry mass, respectively. There are no data available
for As in chicken from the Chaco Pampean plain, but studies from
other Latin American regions underscore the need to investigate this.
Naula Naula (2012) analyzed As content in chicken liver and gizzard
in Ecuador. They observed that much of the samples exceeded the
FDA limit of As concentration (0.5 mg kg−1 dry mass of As for eggs
and tissues of chickens and poultry). The mean As level was 51.76 mg
kg−1 in the liver and 50.86 mg kg−1 (dry mass) in the gizzard.
Espinoza Valdivieso and Suarez Zulueta (2015) found similar results in
the liver of chickens from Peru, where the average As concentration
was 0.858 mg kg−1 dry mass. The origin of As in chicken in the Chaco-
Pampean plain is unknown. It is unlikely due to food additives, as As
containing food additives are forbidden in Argentina (Zulma et al.,
2011).
The studies on As uptake by cattle performed in the Chaco Pampean
Plain (Pérez Carrera and Fernández Cirelli, 2007; Pérez-Carrera et al.,
2016a, 2016b) considered only the ingestion through water and did
not consider uptake by forage, although As in vegetable and crops is
the primary source of As in human diet (Saldaña-Robles et al., 2018). Ar-
senic uptake in plants and crops is proportionally associated with high
As in soils and irrigation waters (Shah et al., 2017). Several authors
have reported the presence of As in different kinds of vegetables and
crops. Alonso et al. (2014) reported high concentrations of As in agricul-
tural areas, with levels up to 5.40 mg kg−1 in vegetables and 255 μg L−1
in irrigation water. A recent study about two orchards of Santa Fe prov-
ince, As content determined in lettuce plants, were between 0.72 and
0.75 mg kg−1 dry mass, below the 1 mg kg−1 recommended by the
Argentine Food Code for solid food. In the Chaco-Pampean Plain
(Argentina), Sigrist et al. (2016) reported high As values in commercial
cereals and derivatives. Arsenic range determined in commercially sold
rice was from 87 to 316 μg kg−1 and in rice-based food from 52 to 201 μg
kg−1 and in other cereals flour between <LOQ to 73 μg kg−1. In this
study, contribution to Asin intake was calculated and reported that the
main contributors to Asin intake were rice and wheat flour and their de-
rived products.
(iii) Seafood production
The presence of trace elements in commercial fish muscle is a signif-
icant problem for food security (Volpedo et al., 2015). Avigliano et al.
(2016) found that Astot in edible muscles of Odontesthes bonariensis
(0.1 mg kg−1 wet weight) and Lycengraulis grossidens (0,9 mg kg−1
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Science of the Total Environment 780 (2021) 146274
wet weight) from Paraná River Delta (Argentina) is below the permissi-
ble limit for As (1 mg kg−1 wet weight) in fish products established by
Argentinean Food Codex (CAA, 2012). In the same species
(O. bonariensis) from Chasicó Lake in Buenos Aires province of
Argentina, a mean of 3.03 ± 0.87 mg kg−1 dry weight of Astot was
found in the liver by Puntoriero et al. (2018). Arsenic concentrations
are generally high in seafood, wherein the main arsenical species are
arsenobetaine and arsenolipids in fishes and crustaceans. However,
these As species have relatively low toxicity (Chávez-Capilla et al.,
2016). In another study from Mexico, Ibañez (2007) reported BTF values
between 1.1 × 10−3 day L−1 and 5.3 × 10−4 day L−1 from shrimps and
squids. Astot values determined in Silverside sp. muscle from Chaco-
Pampean Plain (Argentina) by Volpedo et al. (2015) were lower than
1 mg kg−1, the maximum As concentration recommended by the
Argentine Food Code for solid food (CAA, 2012). Avigliano et al.
(2015) found Astot in the silverside muscle from the Chaco-Pampean
plain, in concentrations between 0.03 and 0.76 mg kg−1 (wet weight).
These values were below those reported by Rosso et al. (2013; 0.8 and
1.23 mg kg−1 wet weight) in the same region. In comparison to these
values reported from Argentina, Spanopoulos-Zarco et al. (2015)
found As in three fish species in Mexico: T. kennedyi (0.632 μg g−1
wet weight), P. grandisquamis (0.166 μg g−1 wet weight), and
D. peruvianus (0.157 μg g−1 wet weight). In the same country, Rubio-
Franchini et al. (2016) found mean values below 0.014 μg g−1 for
Oreochromis nilotica. In Brazil, Fabiano et al. (2016) reported high values
of As in fish, and Ciminelli et al. (2017) reported that the contribution of
As from fish and meat represents 23% of the total As intake from food in
that country.
(iv) Local health impacts
There are very few studies on epidemiological and health risk
assessment compared to the significant number of sites with As-
contaminated groundwater and numerous hydrogeological, hydrogeo-
chemical, sedimentological, and environmental studies within the
Chaco-Pampean plain. This is despite groundwater As problem being
known for over a century and As-contaminated groundwater being
the only available local water source in rural or periurban regions. This
situation impacts especially the poor (e.g., large populations from the
Chaco part of the plain), who cannot afford to purchase purified bottled
water for drinking and cooking purposes, as inhabitants from more af-
fluent rural and periurban regions can (e.g., in the Pampean part of
the plain, which is much prosperous and apparently concerned about
As contamination than the Chaco part). Besides, the more affluent com-
munities can afford the installation of drinking water treatment plants.
As-related health impacts (skin lesions) due to groundwater con-
sumption were described as “Bell Ville Disease” over 100 years ago in
the locality of Bell Ville (close to Córdoba), in the central Chaco-
Pampean plain by Goyenechea (1917). Ayerza (1917a, 1917b) found
1300 out of 8534 (~15%) inhabitants of the Bell Ville community having
this disease. He also described As-related cardiovascular and cutaneous
symptoms for this disease and renamed it “Chronic Endemic Regional
Arsenicism.” A statistical approach of patients' data of Bell Ville hospital
showed that 511 patients were affected by As (1934–1944) (Trelles
et al., 1970). Studies from other sites (Buenos Aires, Córdoba, Chaco,
Santa Fe, and Salta provinces) described As-related health impacts in
339 patients registered at hospitals (Tello, 1986, 1988). As-affected per-
sons (87) from Santiago del Estero, Chaco, and Salta provinces have
been studied during the 1972–1993 period (Biagini et al., 1995).
Based on the review of 82 peer-reviewed papers, McClintock et al.
(2012) reported As exposure and related health effects in the Latin
American population, including from Chaco-Pampean plain, with 82%
of water samples exceeding WHO drinking water standard of 10 μg
L−1 (Nicolli et al., 1989). Accordingly, the people in Latin America
have been exposed to As concentrations up to >2000 μg L−1, which is
200 times higher than the WHO (2017) guideline value for drinking
J. Bundschuh, J. Schneider, M.A. Alam et al.
water. This review work showed a critical link between high levels of
chronic As exposure and adverse health effects, including different
types of cancer, reproductive problems, and 's cognitive issues in chil-
dren. Some of the reviewed studies showed that genetic polymor-
phisms could influence the susceptibility to diseases through their
modulation of As metabolism, with the involvement of As methyltrans-
ferase (AS3MT), glutathione S-transferase (GST), and genes of
one‑carbon metabolism (McClintock et al., 2012 and references
therein).
Lerda (1994) investigated long-term exposure to drinking water
containing >0.13 mg L−1 of As and its relationship to the frequency of
sister-chromatic exchanges (SCE) in the lymphocytes. He investigated
282 people exposed to As levels above 0.13 mg L−1 in drinking water
with 155 control individuals in Argentina. The population exposed to
high levels of As showed a significantly elevated response to SCE and
other health effects (e.g., hyperkeratosis, melanosis, actinic keratosis,
basal cell carcinoma; Lerda, 1994).
3.1.3. Arsenic in geothermal fluids
Geothermal fluids and surface manifestations (e.g., hot springs, fu-
maroles, geysers) contain a wide variety of dissolved constituents, in-
cluding As, the concentrations of which vary depending on the
lithology of the host rocks and tectonic setting. The study encompassing
15 countries in Latin America by Morales-Simfors et al. (2020) charac-
terized 423 sites with As originating from geothermal sources, mostly
related to present volcanic activity (0.001 < As < 73 mg L−1, mean:
36.5 mg L−1). When these As rich thermal waters mix with ground-
or surface water, they contaminate these water resources (Bundschuh
and Maity, 2015); e.g., in northern Telica municipality (Nicaragua),
where high As (0.010 to 0.325 mg L−1) concentrations have been
found in several wells used for drinking water. OPS/OMS and Nuevas
Esperanzas (2011) have attributed high As (>0.050 mg L−1 in shallow
groundwater) concentration to geothermal activities with As-rich ther-
mal waters in the region. Other examples of high As concentrations in
geothermal systems are (i) El Tatio-Geiser Field (Chile), which is the
principal natural source of As (up to 50 mg L−1; Risacher and Hauser,
2008; Risacher et al., 2011) in the Loa River, the primary surface water
resource in the hyper-arid Atacama Desert of Chile (Alsina et al., 2014;
Muñoz-Saéz et al., 2015); (ii) Los Humeros Geothermal Field
(73.60 mg L−1; González et al., 2001) in Mexico; (iii) Miravalles and
Rincón de la Vieja geothermal wells (25.4 and 10 mg L−1, respectively;
Hammarlund and Piñones, 2009) in Costa Rica; (iv) Zunil geothermal
wells (As up to 12.34 mg L−1, ZP-6 exploration well; Adams et al.,
1991) in Guatemala; and (v) Platanares wells (As 450 μg L−1; Barberi
et al., 2013) in Honduras.
Arsenic is one of the important constituents in geothermal fluids
(Ballantyne and Moore, 1988). It is highly mobile in geothermal systems
and can be removed from the solution by its uptake into sulfide min-
erals and iron hydroxides (Ballantyne and Moore, 1988; Smedley and
Kinniburgh, 2002). The gas arsine (AsH3) exists to a significant extent
in geothermal systems, and its toxicity effects are of particular concern
(Signorelli, 1997). The amount and nature of the dissolved chemical
species in the geothermal waters are highly variable, depending on
(i) the reservoir rock composition, (ii) pressure, (iii) temperature, (iv)
redox condition (pH), (v) presence of gases and (vi) microbiological ac-
tivity (Bundschuh and Maity, 2015).
According to de Moor et al. (2006), the hydrothermal system may
cause (i) modification of the composition of gases passing through the
hydrothermal system after gas separation from magma, (ii) scrubbing
of reactive gases by interaction with meteoric/hydrothermal water,
(iii) addition of volatiles through boiling off of hydrothermal liquids
and sublimation/combustion of hydrothermal minerals, and (iv)
changes to the permeability of the upper volcanic system. Among the
geothermal springs, those with NaCl-type water and high bicarbonate
have the highest As concentrations (Bundschuh and Maity, 2015;
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Science of the Total Environment 780 (2021) 146274
Morales-Simfors et al., 2020). These waters correspond to original reser-
voir waters, which were not significantly altered during its ascent.
3.1.4. Effects on ground and surface waters
The interaction of water with volcanic rocks has resulted in high As
levels (>10 μg L−1) for drinking water in several aquifers exploited for
human consumption in Latin America (Morales-Simfors et al., 2020).
For example, in El Salvador, drinking water supply wells located in the
aquifers surrounding the San Salvador and San Miguel volcanoes pres-
ent high concentrations of As. The concentration of dissolved As in the
groundwater mix depends on (i) As concentration of the geothermal
water component, (ii) pH/Eh conditions of the geothermal water, (iii)
cold water/solid aquifer matrix components, (iv) mixture ratio between
both types of waters and (iv) availability of mineral phases that may act
as suitable sorption sites for dissolved As (Bundschuh and Maity, 2015;
Morales-Simfors et al., 2020).
Peralta Arnold et al. (2017) reported high concentrations of As
(6.17 mg L−1) in NaCl-type waters from the Puna plateau in Argentin-
ean Andes. In some villages in the same region, Concha et al. (2010) re-
ported elevated levels of As in tap water (3.5–220 μg L−1) and
drinking spring water (1000 μg L−1). Smedley et al. (2002) attributed
the elevated As concentrations (3–1330 μg L−1) in the Pampa
(Argentina) to the weathering processes and volcanic activity in the
area, which have created the pH conditions (7.0–9.9) in which As can
become mobilized (O'Reilly et al., 2010). In the Central Volcanic Zone
of Chile, high As concentrations have been detected (up to 2000 μg
L−1 for 48 hot springs; Hauser, 1997; Cortecci et al., 2005; Chong
et al., 2010; Sánchez-Yañez et al., 2017), where As is mostly found in
its oxidized form [As(V)] (Fernández-Turiel et al., 2005). Smith et al.
(2006) found in northern Chile that the exposure of As in drinking
water during early childhood or in the uterus has pronounced pulmo-
nary effects, significantly increasing subsequent mortality in young
adults from both malignant and non-malignant lung disease. Ground-
water contamination by As (50 μg L−1) and F (1.5 mg L−1) has also
been reported in Aguascalientes city in Mexico, suggesting a public
health risk for the population (Trejo-Vázquez and Bonilla-Petriciolet,
2002).
Lamela et al. (2019) investigated volcanic activity's effect on princi-
pal rivers' water quality in northern Argentinean Patagonia. This study
attributes environmental pollution to active volcanism and statistically
shows the influence of volcanic activity on water quality and chemical
composition of biota. River waters in the region and the Patagonian
and Antarctic biota (samples of animals, plants, algae, and bacteria)
were analyzed for their As and other elements (P, S, Cl, K, Ca, Ti, V, Cr,
Mn, Fe, Co, Ni, Cu, Zn, Ga, Ge, Se, Br, Rb, and Sr) concentrations, by syn-
chrotron radiation X-ray fluorescence (SRXRF) spectrometry. Elevated
As concentrations (up to 950 μg L−1) were found in water samples
from Patagonian rivers. Analysis of metal and As-proteins associations
in As-accumulating organisms was done using SRXRF. Hierarchical clus-
ter analysis results showed that the biological samples' elemental con-
centrations were related to the volcanic environments. Moreover, the
results suggest that Se, Co, Cu, Br, and Cl can be proxies for As concentra-
tions in the organisms.
3.2. Metal ore deposits and accelerated exposure related to mining
Latin America is rich in mineral resources, especially in Argentina,
Chile, Bolivia, Uruguay, Peru, Brazil, Ecuador, Colombia, Panama, Costa
Rica, Nicaragua, Guatemala, and Mexico. In addition to As release by nat-
ural weathering and lixiviation processes, extraction of As-rich (mostly)
sulfide ores produces contaminated waste. This waste gets deposited as
tailing piles and can result in an accelerated release of As and other con-
taminants into the environment, resulting in contamination in different
environmental forms and compartments (groundwater, surface water,
rainwater, surface run-off, sediment, soil, dust, atmosphere; García-
Sánchez and Álvarez-Ayuso, 2003; de Mello et al., 2014; Mirlean et al.,
J. Bundschuh, J. Schneider, M.A. Alam et al. Science of the Total Environment 780 (2021) 146274

2016; J. Bundschuh et al., 2017; M. Bundschuh et al., 2017; de Meyer
et al., 2017; Cagnin et al., 2017; Hatje et al., 2017). Table 1 provides ex-
amples of mining-related environmental impacts due to As contamina-
tion. However, most mining sites and related ore processing facilities
have not been studied, especially the smaller ones. Artisan mines, many
of which are illegal or unregulated (Colombia: 66%; Güiza, 2013), make
the majority of the mines in several countries (Colombia: 72%). For
most of the studied sites, a holistic approach that includes ground- and
surface water, soil, sediments, and atmospheric studies combined with
As impact assessment on food and health is not available.
The dissolution of the minerals of the mining residues, such as arse-
nopyrite (FeAsS), is a constant contamination source (de Mello et al.,
2014; Ferreira and Leite, 2015). If As and other contaminants are re-
leased into rivers and sorbed into the sediments, the particulate and dis-
solved As can be transported over large distances, impacting the areas
along its course before reaching the ocean, where it can further impact
the marine areas along the coastline. For example, the Rímac River in
Peru is polluted in the upstream area by mining; still, its water is used
downstream for irrigation before discharging into the Pacific Ocean,
impacting the coastal environment (Segura et al., 2016; Mirlean et al.,
2016; Cagnin et al., 2017; de Meyer et al., 2017) (Table 1).
In the Brazilian territory, the studies carried out during the last two
decades have been concentrated mainly in four regions: (i) “Iron Quad-
rangle” region, Minas Gerais state, in which As is released into the envi-
ronment through activities related to gold mining (Matschullat et al.,
2000; Deschamps et al., 2002, 2003; Borba et al., 2003; Borba and
Figueiredo, 2004; Mello et al., 2006; Deschamps and Matschullat,
2007; Bundschuh et al., 2012a; Silva et al., 2018; Carvalho et al., 2018;
Paraguassú et al., 2019); (ii) Ribeira Valley region (Paraná, and São
Paulo states), which is highly contaminated due to mining, processing
and refining of “Pb-Zn-Ag” ores, in which As is naturally found in
rocks and soils (Figueiredo et al., 2003; Abreu and Figueiredo, 2004;
Akcil and Koldas, 2006; Blodau, 2006; Campaner and Luiz-Silva, 2009;
Cha et al., 2018); (iii) the Amazonia region, including the area of the
municipality of Santana, in the state of Amapá (AP), where As is associ-
ated with manganese (Mn) ores exploited during the last five decades
(Santos et al., 2003; Mandal et al., 2004; J. Bundschuh et al., 2017; M.
Bundschuh et al., 2017; de Meyer et al., 2017; da Silva Júnior et al.,
2019); and (iv) impact of coastal zone by As-laden river water
discharging into the Atlantic Ocean (Mirlean et al., 2011, 2012, 2013,
2014, 2016; Cagnin et al., 2017; de Meyer et al., 2017; Dolci et al.,
2017; Gao et al., 2018; Baeyens et al., 2019). According to Figueiredo
et al. (2010), in mining and ore processing regions, e.g., in Amapá, exac-
erbation of the natural occurrence of As by anthropogenic activities such
as extraction of base metals from natural (geogenic) sources, can be ob-
served, which leads to severe contamination of river systems and soils.
However, we must consider the existence of many other areas that are
still unknown or slightly studied, where thousands of people may be
impacted – without their knowledge – from chronic exposure to As
due to lack of awareness and protection from responsible authorities.
The following section showcases examples from Brazil in more detail.
Examples from Brazil
Among the studies carried out in Brazil, most are related to As
sources arising from mining and metal refining processes. Other As
studies in Brazil include the use of agrochemicals and substances in
the poultry industry (Rocha et al., 2015) as the origin for As contamina-
tion and human exposure (Toujague de la Rosa, 1999). A recent study
revealed that the median As content in Brazilian soils ranged from
0.14 to 41.1 mg kg−1 in reference soils and 0.28 to 58.3 mg kg−1 in ag-
ricultural soils (Menezes et al., 2020). Uddh-Söderberg et al. (2015)
highlighted that the total concentration of As in the soil is generally
not a reliable predictor of the assimilation of this element by the plants,
because the bioavailability of As depends on factors such as the hydro-
geology and geochemistry of the soil. Besides, a relatively higher pro-
portion of As accumulation in vegetables highlights the importance of
further investigation regarding the local population's risk exposure.
Some of these studies are listed in Table 2.
A. Iron Quadrangle
The most critical environmental problem of As contamination in
Brazil is reported from the Iron Quadrangle in Minas Gerais state,
known for gold production since the late seventeenth century (Borba
et al., 2003). The primary natural sources of As at the Iron Quadrangle
are the rocks containing auriferous sulfide deposits. The exploitation
of these ores contributes to the increased As content in different

Table 2
Arsenic content in samples of sediment and hair (μg kg−1), water, urine and blood (μg L−1), meat and liver of cattle and chicken (μg g−1) obtained in different studies in Brazil regions,
states or cities.

Location Sample Minimal As Average As Maximum As References

concentration concentration concentration

The Santana District, Amapá state Groundwater – – 2000 Figueiredo et al., 2007
Hair 0.063 0.2 1.94 Santos et al., 2003
Blood (contol) 1.11 1.14 1.27
Sediments – – 4000 × 103 Figueiredo et al., 2007
The Iron Quadrangle, Minas Gerais state Surface water – – 3000 Figueiredo et al., 2007
Urine – 25.70 >40 Matschullat et al., 2000
Sediments – – 345 × 103 Toujague de la Rosa, 1999
The Ribeira Valley, Paraná – São Paulo states Surface water – – 9.00 Takamori and Figueiredo, 2002
Urine 1.00 8.51 76.19 Sakuma, 2004
Paraná State Sediments – – 1600 × 103 Lima, 2003
Surface water – – 231
Blood (1° analyze) 3.26 3.37 3.48 Rocha et al., 2015
Blood (2° analyze) 3.61 3.78 3.77
Blood (3° analyze) 2.07 2.10 2.36
Rio Branco, Acre state Blood <LD 4.91 30.75 Freire et al., 2015
Beef 0.06 0.11 0.021
Bull's liver 0.07 15 0.25
Campos dos Goytacazes, Rio de Janeiro state Chicken meat 0.06 0.13 0.31 Caldas et al., 2016
Chicken liver 0.09 0.53 1.78
Beef 0.005a 0.066a 0.946a
Bull's liver 0.001a 0.009a 0.049a
Chicken meat 0.005a 0.047a 0.725a
Chicken liver 0.004a 0.046a 3.15a
a
Estimated amount of arsenic consumed in food (μg day−1 kg−1).

13
J. Bundschuh, J. Schneider, M.A. Alam et al.
environmental phases, especially in mining wastes accumulated since
the last century (Borba and Figueiredo, 2004; Deschamps and
Matschullat, 2007).
Costa et al. (2015) carried out a geochemical mapping of As distribu-
tion in water and fluvial sediments, using 512 sampling points distrib-
uted over an area of 7000 km2 in the Iron Quadrangle. The values of
As concentration found in surface water varied between 57.7 and 414
μg L−1 and in fluvial sediment from 0.63 to 1961 mg kg−1.
Matschullat et al. (2000) reported a study of As levels in the urine of
children aged between 7 and 12 years in the Iron Quadrangle region.
The authors found that, of the 126 samples collected, 20% had levels
around 40 μg L−1 (mean: 25.7 μg L−1). It is worth mentioning that uri-
nary As levels used in the National Health and Nutrition Examination
Survey (NHANES; https://www.cdc.gov/nchs/nhanes/index.htm)
2011–12 conducted by Centers for Disease Control and Prevention
(CDC; https://www.cdc.gov/biomonitoring/Arsenic_Biomonitoring
Summary.html) in the USA are classified as: normal: ≤50 μg L−1, high
normal: >50 to <200 μg L−1 and high: ≥200 μg L−1. The authors attrib-
uted the exposure route to As contained in soil and dust of the region.
This was because As concentration in water was <10 μg L−1, the limit
established by CONAMA (2005, 2008) for drinking water consumption.
B. Ribeira Valley
The Ribeira Valley, a region between the states of São Paulo and
Paraná, was known for mining of Zn, Ag, and Pb ores, with significant
levels of As in the form of arsenopyrite. The activity of mining and refin-
ing of metals occurred in the region known as Upper Ribeira Valley. In-
tense metal mining and refining activity took place in the valley until
1996 when the lead mining company Plumbum closed its operations.
The company left behind substantial environmental liabilities of waste
management that led to various environmental contamination sources,
especially lead and arsenic, typically originating from the extraction,
processing, and mineral refining activities. Arsenic found in the Middle
Valley presents a NE-trending As anomaly in the soils (Piririca belt;
Figueiredo et al., 2007) with the occurrence of several base metal-
bearing gold deposits. In both the valleys, As in rocks, soils, surface
water, and stream sediments have been investigated by various re-
searchers. In the Upper Valley, many years of mining activity without
environmental consideration (and control by competent authorities)
have polluted river sediments (220 μg g−1) and soils (up to 80 mg
kg−1), with relatively low concentrations of As and other contaminants
in the surface water (As levels varied from 1 to 9 μ L−1); viz. Betari River,
which, in turn, flows into the Ribeira River, near Iporanga.
Sakuma (2004) reported that urine samples analyzed among the
monitored communities were lower in the Upper Ribeira Valley region
(mean of 8.45 μg L−1 in adults, n = 86) compared to the Middle Valley
(mean values of 11.35 μg L−1, n = 51). Although these values cannot be
considered high, a difference was observed concerning the control
group, whose mean in adults was 3.87 μg L−1 (n = 83).
Toujague de la Rosa (1999) reported the values of 345 mg kg−1 of As
in stream sediments (<63 μm) from the Ribeira Valley. However, mon-
itoring the Ribeira River and tributaries in the Middle Vale region de-
tected concentrations of As that varied between 1 and 9 μg L−1
(Takamori and Figueiredo, 2002).
C. Amazon region
Manganese mining in Amapá has been going on for >50 years in the
Serra do Navio deposit (Figueiredo et al., 2007). However, the As-
contaminated area is 350 km away from the exploitation area along
the Amazon River banks. In this area, As-rich ore was processed and
mining wastes containing up to 0.17% As were exposed to open air, con-
taminating air and water. The As concentration was >2000 μg L−1 in
wells, and varied from 5 to 231 μg L−1 in surface water (with various
As values <50 and 10 μg L−1) and >1600 and 696 mg kg−1 in river
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sediments and suspended matter, respectively. A recent study high-
lights the need to complement the information about the background
levels of As in soils from the Amazon region using representative soils
that reflects the natural concentrations of each sub-region to provide
guideline values for better use of soil and water resources in the area
(da Silva Júnior et al., 2019).
D. Other occurrences of As in Brazil
(i) Paraná
In the state of Paraná, Rocha et al. (2015) carried out blood analysis
to evaluate the exposure to As in 54 vineyard farmers and 108 unex-
posed individuals. Blood samples were collected two times during the
summer and once in winter. The decrease of heat and rainfall reduces
pests' proliferation in winter; thus, the plants become relatively resis-
tant. Therefore, in this period, smaller amounts of pesticides are used
in comparison to summer. The content of As present in blood serum cor-
related positively with the amount of pesticide used at specific times of
the year, with higher contents in summer (3.4 and 3.8 μg L−1) compared
to winter (2.1 μg L−1) (Rocha et al., 2015). Compared with urine, blood
is a much less sensitive biomarker of exposure to As via drinking water
(NRC, 1999), so these reported values are quite significant for causing
adverse health effects, as corresponding As level in water intake could
be about 30 times (see the examples in NRC, 1999).
(ii) Rio Branco (Acre)
In Rio Branco, in the state of Acre, Freire et al. (2015) determined the
level of exposure to As in blood donors (n = 1183) (Table 2). They
found As in almost all donors (99.5%), with higher levels in males (aver-
age 4.93 μg L−1, geometric mean 4.25 μg L−1, maximum value 30.751 μg
L−1 compared to average 4.84 μg L−1, geometric mean 4.01 μg L−1, max-
imum value 26.28 μg L−1 in women). This study showed a more signif-
icant influence of occupational factors on the As concentration in the
study area residents (Freire et al., 2015).
(iii) Campos dos Goytacazes (Rio de Janeiro)
In Campos dos Goytacazes (Rio de Janeiro), Caldas et al. (2016) car-
ried out a study to estimate the risk of exposure of the population to As
by consumption of meat and liver of cattle and chicken due to As bear-
ing feed and mineral supplements and the probability of cancer occur-
rence. Arsenic (0.11 to 0.54 μg g−1) was found in 58% of the samples
(n = 250, Table 2). A study by the EFSA (2014) showed that this food
group has the highest inorganic As (12.3 μg Kg−1). The maximum limits
of Brazilian legislation are 0.5 mg kg−1 (muscle and eggs) and 1 mg
kg−1 (offal and fish) (ANVISA, 2013). Specifically, concerning chicken,
the type of animal most consumed by Brazilians (OECD, 2016), the
highest concentration values (0.11 to 0.54 μg g−1) are generally found
in the kidneys and liver, as they are organs of filtration and metabolism
(Ghosh et al., 2012; Caldas et al., 2016). Since As is bioaccumulative,
chickens raised in environments with exposure to high concentrations
of this element will reflect these high concentrations in their tissues.
Studies carried out in countries with known As contamination in
water, such as Bangladesh and Pakistan, show As concentration values
well above what Brazilian legislation allows for chicken cuts (EFSA,
2009; Ghosh et al., 2012). Ogbomida et al. (2018) noted a positive cor-
relation (p ≤ 0.001) between the concentration of As in soil and chicken
livers; however, they did not observe a correlation with the muscle.
(iv) Doce River
A study conducted by Cagnin et al. (2017) during November 2015 at
the Doce River site reported the collapse of the s dam into the river. Mil-
lions of liters of tailings were dumped into the river and hit the main-
land shelf of Brazil, causing the largest environmental disaster of the
country (Segura et al., 2016). These studies concluded that since the
J. Bundschuh, J. Schneider, M.A. Alam et al.
seventeenth century, gold and iron mining activities in the Doce River
watershed led to As contamination on the adjacent continental shelf,
where sediment exhibited As levels well above Brazilian legislation
level 2 (i.e., 70 mg kg−1; CONAMA, 2012; Cagnin et al., 2017).
(v) Coastal areas
In the Sepetiba Bay, Rio de Janeiro, Magalhães et al. (2001) found
high concentrations of As in sediment samples close to a Zn metallurgi-
cal industry due to the use of As trioxide in the Zn purification. Similarly,
phosphate fertilizer production in Rio Grande do Sul, more precisely in
the Patos Lagoon Estuary, increased As concentration in the lagoon sed-
iments. The As release to the atmosphere caused this contamination
since the phosphorous rocks contain 86 mg kg−1 As on average
(Mirlean and Roisenberg, 2006). In a residential area, adjacent to a pes-
ticide factory, in the city of Paulínia (state of São Paulo), 52% of the ana-
lyzed population (n = 181) had a blood concentration of 139 μg L−1,
which is much higher than the reference level of 4 μg L−1, found in an
occupationally unexposed population (Guerreiro and Vassilieff, 2003;
Guilherme et al., 2005). This dose was comparable to that observed in
people undergoing treatment with As-based medications (ATSDR,
2007a).
(vi) Paracatu (NW Minas Gerais)
In the city of Paracatu (northwestern Minas Gerais), which has
Brazil's largest gold mine and the world's largest open-pit at present,
with the ore containing mainly sulfide minerals, including arsenopyrite,
with natural occurrence of high levels of As (1510 to 2930 mg kg−1; de
Andrade et al., 2008). Several studies have reported high contamination
levels of As caused by historic mining of Au in soils, water, and sediment
in this region (Table 2; Mello et al., 2006; Ono et al., 2011, 2012; de
Andrade et al., 2012; Bidone et al., 2014; Egler et al., 2014; de Mello
et al., 2014; Sabadini-Santos et al., 2014; Guilherme et al., 2014;
Rezende et al., 2015). However, the risk associated with exposure to
As in Paracatu (0.4352 μg kg−1 day−1 for adults and 0.3536 μg kg−1
day−1 for children) can be considered low, compared to the BMDL0.5
of 3 μg kg−1 day−1 (JECFA, 2011, 2017; De Capitani et al., 2014; Ng
et al., 2014). The results of the studies carried by Ono et al. (2012) and
Guilherme et al. (2014), who showed the presence of high concentra-
tions of As (up to 2666 mg kg−1) and very low As bioaccessibility
(<4.2%) in tailings in the gold mining area in Paracatu, corroborate
this. Arsenic was predominantly present as [As(V)] and associated
with poorly crystalline Fe arsenate, which explains the low bioaccessibi-
lity of As and highlights the importance of Fe oxides in immobilizing As
in the environment (Freitas et al., 2015).
Rezende et al. (2015) evaluated As mobility in the Paracatu River
sediments. They observed that arsenite correlated positively with Mn
and Fe oxides, suggesting that As dissolution may be associated with
Mn oxide dissolution. They observed a reduction in As concentration
from 110 to 31 μg L−1 in the dissolved fraction of the river water col-
umn, e.g., as Fe increased in the sediment (3 to 9%), suggesting greater
retention of As by Fe oxides in the sediments. Besides, the preservation
and maintenance of river banks, revegetation, and sewage treatment
before discharging into rivers are some alternatives that favor a higher
dissolved oxygen concentration >5 mg L−1, which would lead to a de-
crease in the total concentration of As in the water through oxidation
of [As(III)] to the less mobile [As(V)] (Rezende et al., 2015).
According to García-Sánchez and Álvarez-Ayuso (2003), soils and
sediments around mining areas generally present high levels of As due
to high degree of contamination by mining products and processing ac-
tivities, such as mechanical dispersion of solids of primary minerals of
As and secondary minerals formed by weathering of wastes and tailings.
According to some studies carried out in Paracatu, Minas Gerais
(Santana Filho, 2005; Chapadeiro et al., 2006; de Mello et al., 2014),
the enrichment of As in the analyzed soils and sediments in this study,
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is probably related to the biogeochemical cycling process as well as sed-
iment deposition processes due to water erosion, discharge of ground-
water, and atmospheric dispersion of As-rich particulate matter from
the mining area. These processes influence the concentration of As at
each point in the function of its distance from the source. A recent
study by Aguilar et al. (2020) showed the high applicability potential
of As-resistant bacteria of Bacillus cereus and Lysinibacillus
boronitolerans species in the treatment of As contaminated soil and
aquifers.
de Mello et al. (2014) studied As contents in the atmospheric partic-
ulate material in Paracatu, where As content at several collection points
around the Morro do Ouro mineralization area varied spatially and sea-
sonally. The origin of the dust, direction, and velocity of the dominant
wind (northeast), and the seasonal distribution of precipitation control
this variation.
(vii) Food chain
In São Paulo, a study determined the content of As in octopus spe-
cies, assuming that it may be a potential source of toxic elements due
to its trophic position in the food chain and the ability to accumulate el-
ements up to 10 times more than in the environment.
Lemos et al. (2014) reported As content in the range of 0.184 to
35.38 mg kg−1 in octopuses collected along the coastline of Santos,
Guarujá, Praia Grande, and São Vicente. The study reported these octo-
puses unsuitable for consumption, as As content in most samples
exceeded the permissible legislative value of 1 mg kg−1 (Brazil, 1998).
Morgano et al. (2010) evaluated As content in bee pollen in the
states of Minas Gerais, São Paulo, and Espirito Santo, spread over a sur-
face area of 7 km2, as many authors have proposed that bee products, as
well as bees, are bioindicators of chemical pollution due to their forag-
ing activity (e.g., Conti and Botré, 2001). They found As in 60% of the
samples, with the mean values of 0.46 (state of Sao Paulo), 0.36 (state
of Minas Gerais), and 0.29 (state of Espírito Santo) mg kg−1 and with
30% of the samples having As values above the maximum tolerable
limit established for food. The pollen from Espirito Santo had the lowest
concentration of As, which was explained by the sample location in a
rural area, unlike Minas Gerais and Sao Paulo. These results confirm
the highest pollution in urban areas and show that bee pollen is sensi-
tive to environmental pollution and can be considered a bioindicator.
Batista et al. (2011, 2014) evaluated several rice varieties to estimate
the total As content and its chemical species in different Brazil regions
(states of Rio Grande do Sul, Goiás, Minas Gerais, São Paulo, and
Santa Catarina). The total concentration of As ranged from 107.9
to 427.7 μg kg−1, and the predominant forms of As were the
more toxic inorganic species (Batista et al., 2011, 2014), while to protect
consumers from excessive exposure, the Codex Alimentarius
Commission recommends that As level in rice should not exceed
0.2 mg kg−1 (200 μg kg−1; CAC, 2014).
In general, high levels As found in groundwater is of great concern;
as in many countries, this is the primary source of drinking and irriga-
tion water. In this case, the As-related problems include reducing or los-
ing agricultural productivity, impairment of crop quality, and soil
contamination. In recent years, changes in the rainfall regime have led
the more densely populated Brazil regions, such as the southeast, to ex-
perience drought. Because of this situation, well drilling has become an
alternative for water supply, highlighting the need to assess groundwa-
ter quality.
A comparison between As reported in environmental samples and
the amount allowed by legislation is a common practice to assess the
degree of As exposure to a given population. However, there is no differ-
entiation in Brazilian legislation between the chemical speciation of As
when it comes to its maximum permitted level, so the degree of expo-
sure and consequences will differ, depending on the species. For exam-
ple, inorganic species, which are more toxic, could be dangerous even at
permissible concentration level. So, the studies evaluating As
J. Bundschuh, J. Schneider, M.A. Alam et al.
contamination by only determining its total content provide limited in-
formation on its toxicity and mobility.
Another critical issue is the use of some As-containing substances in
agricultural practices without any restriction in Brazil, despite being
banned in developed countries; e.g., the herbicide methane-
monosodium arsenate (MSMA), commercially known as “Daconate
480”, used in the cultivation of coffee, cotton, sugar cane, and citrus
crops. Another example is the treatment of eucalyptus wood with a pre-
servative based on chromated copper arsenate (CCA) (Appel et al.,
2006; Nobre and Nobre, 2011; Araujo et al., 2012).
In recent years, there are increased studies on determining As in
food, used as a tool to assess the degree of exposure to a population.
For analyzing As contamination and exposure, it is essential to consider
different issues, such as the limit for the effects of intoxication to mani-
fest themselves, i.e., dosage and duration of exposure. Also, the relation-
ship between toxic manifestations and population characteristics and
the attenuating role of a balanced diet must be assessed.
The data regarding As distribution and the determination of As ex-
posure in Brazil highlights the lack of specific clinical studies on the
human body. Chronic exposure to As may be occurring in areas not
yet recognized as highly contaminated. In this sense, there is an immi-
nent need for monitoring public health conditions associated with As
contamination and intoxication. For planning and execution of monitor-
ing activities, due consideration should be given to the regions' geo-
chemical context to develop strategies to exacerbate the concentration
of As in organisms due to anthropogenic sources.
3.3. Geogenic As exposure related to coal exploitation
Coal is known for containing As, but its contents vary widely due to
the geologic variations in the world's different coal basins. The coal
Clarke value for As (average world concentration of As in coal) is 9.0
± 0.8 and 7.4 ± 1.4 mg kg−1 for bituminous coals and lignites
(Yudovich and Ketris, 2005). However, respective concentrations are
higher (50 ± 5 and 49 ± 8 mg kg−1) for their coal ash. These values
show that As is a strongly coalphile element with an affinity similar to
Ge and S.
Coals with high As content also have high pyrite and other sulfide
mineral contents, dominate by inorganic As, while those with low As con-
tent have dominant organic As (Yudovich and Ketris, 2005). Inorganic
and organic As can exist in coal chemically bound in a crystal form and
as readily leachable sorbed species. With increasing rank, coal has a lesser
sorbed fraction of As content, with a minimum in coking coals.
Arsenic can accumulate in coals in two ways due to terrigenous or
volcanic processes. In terrigenous processes, As accumulates in peat
bogs due to fluids draining from nearby sulfide deposits, as it occurs in
Finnish peats located near sulfide deposits (Minkkinen and
Yliruokanen, 1978). Examples of the mechanism of As accumulation in
coal due to volcanic processes are from Turkey and Japan. Japanese Ter-
tiary lignites seem influenced by volcanic hydrothermal fluids inputs,
which introduce As and other elements into the peat or lignite
(Sakanoue, 1960a, 1960b). These two processes produce four known
types of As accumulation in coal: a) Chinese type, produced by As en-
richment due to hydrothermal fluids, b) Dakota type, produced by
groundwater leaching As from As-bearing tufa (a variety of limestone
formed by carbonate minerals precipitation), c) Bulgarian type, gener-
ated when water containing As from leaching of sulfide deposit aureoles
enters peat bogs, d) Turkish type, formed when volcanic fluids input the
peat bog (Yudovich and Ketris, 2005).
The thresholds for the toxicity of As in coal are different for different
coals and combustion types (Kizilstein and Kholodkov, 1999). In Russia,
the established As threshold is 300 mg kg−1; however, that does not
have any scientific basis (Zharov et al., 1996: Kizilstein and
Kholodkov, 1999). In China, the correspnding value is 100 mg kg−1.
However, there is a lack of As data in the published literature for Latin
America's coals.
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Example - Coal exploitation in Brazil
The largest coal deposits in Brazil are in Rio Grande do Sul and Santa
Catarina states, while the smaller ones are in Paraná and São Paulo
states (Campaner et al., 2014). Brazil has 32 billion tons of coal reserves.
Of this total, the state of Rio Grande do Sul has 89.25% (28.8 billion tons),
Santa Catarina 10.41% (3.4 billion tons), Paraná 0.32% (100 million
tons), and São Paulo 0.02% (8.5 million tons) (Campaner et al., 2014).
The Brazilian coals are classified as bituminous and sub-bituminous,
presenting high pyrite (FeS2) contents, high concentrations of SO2− 4 , Fe,
metalloids, including As, and many metals (DNPM, 2009). During the
mining and beneficiation stages of coal exploitation, there is the disposal
of sterile solid wastes or coal spoil (mine material that is not economically
feasible for processing) and wastes made up of carbonaceous and other
materials with no commercial value. These wastes are also rich in iron sul-
fides that oxidize in the presence of air, water. Moreover, the bacterium
Thiobacillus ferroxidans triggers acidification of drainage water and disso-
lution of metals and metalloids. If there is not enough alkalinity in the sur-
rounding rocks, it leads to acid mine drainage (AMD). AMD contains a mix
of dissolved metal(loid) ions (As, Cd, Cu, Ni, Pb, Zn, Al, Cr, Hg, Mg, Mn, etc.)
in compositions and concentrations that depend on specific geological
conditions of a coal mining site (Akcil and Koldas, 2006).
Mining and beneficiation of coal in Santa Catarina and Rio Grande do
Sul states have led to hydrological pollution due to AMD (Campaner
et al., 2014). This pollution is due to rainwater infiltration on the tailings
generated by mining and processing activities that reaches surface
water bodies and infiltrate into groundwater, contaminating these
water resources (Freitas et al., 2017). These waters have low values of
pH (<3), high values of total iron, total sulfate, and several other toxic
elements that restrict their use as a drinking water source and destroy
aquatic flora and fauna (Blodau, 2006; Akcil and Koldas, 2006; Freitas
et al., 2017). Campaner and Luiz-Silva (2009) reported the presence of
high concentrations of As (253 to 2176 mg kg−1), Pb (118 to 340 mg
kg−1), and Zn (54.4 to 544 mg kg−1) in bituminous coal from the
Figueira region in the state of Paraná. This study showed that the AMD
generated in bituminous coal mining activities is a potential contamina-
tion source of As and metals for surface and groundwater.
There is the potential contamination of soil and subsoil in areas not
covered by sterile material and tailing deposits (fine materials left
after coal processing, which are reusable, e.g., as an adsorbent removing
acidity, Fe, Al, and Mn in acid drainage). This form of contamination
happens when surface run-off of uncontaminated regions mixes with
acid drainage waters and eventually in groundwater when the advance-
ment of a pollution plume reaches aquifers (Campos et al., 2010;
Campaner et al., 2014; Freitas et al., 2017).
As noted before, As data for coal and coal-contaminated waters is
scarce, making the assessment of potential health impacts of this con-
tamination difficult. This is despite As release from coal mining and re-
lated activities in different environments being a potential health
hazard similar in magnitude as those from the mining of metal ores
and associated activities. Iron hydroxide precipitation at such AMD
sites can reduce the contamination of As in AMD waters, wherein As
coprecipitates or is sorbed into the iron minerals.
Another potential and well-known contamination through coal
combustion in power plants (Pesch et al., 2002; Luo et al., 2004; Shah
et al., 2007; Wang et al., 2018); is little studied in the Latin American
countries (Chile, Pino et al., 2015).
3.4. Arsenic in co-produced water from hydrocarbon exploration and
production
Petroleum reservoir waters from sedimentary basins can contain As,
resulting from seawater's evaporation that concentrates As in oil reservoirs
(Birkle et al., 2010). For example, petroleum reservoir waters in SE Mexico
have concentrations of As up to 2000 μg L−1 at depths of 2900–6100 m
(Birkle et al., 2010). Interactions with carbonate host rocks only provide
J. Bundschuh, J. Schneider, M.A. Alam et al.
a small fraction of As content of oil waters. The primary mechanism for As
enrichment is precipitation and co-precipitation of As with sulfides in
waters with high iron content. However, there is no information reported
neither on potential environmental impacts.
The water co-produced with hydrocarbon exploitation is a mix of
water trapped in underground formations with other waters used dur-
ing the exploitation process brought back to the surface and the mate-
rial extracted from the reservoir during the production activities
(Amini et al., 2012). It consists of mixing the producing well formation
water, condensation water, injection water from the secondary recov-
ery processes, and water used to desalinate the produced oil (Veil
et al., 2004; Fakhru'l-Razi et al., 2009).
Formation water, defined as the sea or freshwater entrapped mil-
lions of years ago during the deposition of sediments that later formed
porous sedimentary rocks between layers of impermeable rocks (Neff
et al., 2011), is the largest part of the volume of water co-produced in
hydrocarbon production. Gabardo et al. (2011) referred to this water
as connate water, a term applied initially by Lane (1906, 1909) to
water held in the pore spaces of sedimentary rocks at the time of depo-
sition and defined more precisely by Johnson (1915). The formation/
connate and produced waters differ from seawater in their characteris-
tics; as the former accumulate salts, ions, and other substances from the
minerals and other materials in contact due to their long residence time
(Figueredo et al., 2014).
The physical and chemical properties of produced water vary con-
siderably depending upon the geographic location, the host geological
formation, and the well's production time. The properties and volume
of produced water vary over a reservoir's lifetime (Dudásová et al.,
2009). The produced water, formed as a byproduct of petroleum and
gas production, is chemically very complex. There are three possible
ways of its management – discard, injection, and reuse. Each of these
ways requires specific treatment to meet the environmental demands,
operational or productive activity (Hong et al., 2003).
Fakhru'l-Razi et al. (2009) estimated the produced water generation
in the water-oil ratio of 3:1. In the final stages of the oil fields, the pro-
duction water can reach a volume ten times larger than the volume of
oil produced (Neff et al., 2011). According to the National Agency of
Petroleum, Natural Gas and Biofuels (Agência Nacional do Petróleo,
Gás Natural e Biocombustíveis - ANP) database, offshore production op-
erators in Brazil recorded a volume of about 110 million m3 of produced
water for a production of 137 million m3 of oil, resulting in a water-oil
ratio of 0.80:1. The difference observed between the Brazilian maritime
activity and the average attributed to the rest of the world (3:1) may be
associated with the age of the most Brazilian hydrocarbon fields and the
beginning of exploration and production activity in Brazil, more recent
than in several countries. It is essential to mention that this ratio (3:1)
is only the offshore activity data (Morais, 2013).
Disposal of water is permitted only under regulations established by
the environmental control agencies, which in turn develop several pol-
lutants (oil and grease content, H2S, etc.) in aqueous effluents. In Brazil's
case, the Conselho Nacional do Meio Ambiente (CONAMA) establishes
that the average monthly concentration of oil and grease content in
the discharge of effluents into the sea should be <29 mg L−1.
Stromgren et al. (1995) found that the formation water has particu-
larities of the host geological formation and is considered polluted by
heavy metals, inorganic compounds, and minerals. Besides, these con-
centrations can differ considerably from seawater.
The dilution on the produced water from oil and gas production plat-
forms affects metals and metalloids concentration, as observed in sev-
eral environmental monitoring studies in the areas of oil and natural
gas exploration and production (E&P) in Brazil (Lamparelli and Ortiz,
2007; Guerra and Angelis, 2009; IOGP, 2019). During the environmental
monitoring program of the Pampo and Pargo platforms in the Campos
Basin, only V (<0.002 mg L−1), Ba (1.3 mg L−1), and As (<0.2 mg L−1;
23 samples) had concentrations detectable by the employed analytical
methods (Standard Method 3120B, ICP-OES; Gabardo et al., 2011).
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The analysis of the results makes clear that even for these metals consid-
ered tracers of offshore E&P activities (Kennicutt et al., 1996), there are
no significant differences between the concentrations measured at any
of the sampling stations near the platform and the station located at
1000 m from the platform (Gabardo et al., 2011). The concentrations
measured for these metals in the area of influence of the Pampo and
Pargo platforms do not differ statistically from the averages reported
for ocean waters (Gabardo et al., 2011). In the Campos Basin region,
Vegueria et al. (2002) showed no significant differences between the
concentrations of 226Ra, 228Ra, V, Ni, and Pb measured at only 250 m
from the release of produced water from fixed platforms and the natural
concentrations found in the region's seawater.
Another aspect to be considered while analyzing the distribution of
metal concentrations in waters is the proximity and magnitude of the
continental inputs, particularly in the case of effluent releases in coastal
waters, such as those resulting from treatment plants (Duleba et al.,
2018). Environmental monitoring studies by the Aquatic Studies and
Research Foundation of the Universidad de São Paulo (Fundespa USP)
in the São Sebastião Channel in the state of São Paulo corroborate this,
as these studies did not observe any effect on seawater and sediments
due to the discharge of produced water and effluents in that channel
(Duleba et al., 2018). The threat of As and other contaminants present
in the produced waters to the health of the population living near oil
and gas exploitation sites needs further investigation and assessment.
3.5. Rivers with natural and anthropogenic As-rich waters and sediments
discharging into the sea
The Loa River in Chile is the most important water source for the II
Region of Antofagasta in northern Chile, where the climate is exception-
ally arid (Romero et al., 2003). Mining is the most important economic
activity of the region and also an important source of As. However, the
primary source of As to the Loa River is natural due to the lithology of
the area, the contribution of the El Tatio geothermal field's thermal wa-
ters, and high evaporation. The river water is highly saline (TDS up to
11 g L−1) and enriched in As (average 1400 mg L−1) and B (average
21,000 mg L−1). The thermal waters, very rich in As (up to 27,000 mg
L−1), contribute to the high levels of As in the Loa River, with As concen-
trations in sediments ranging from 26 to 2000 mg kg−1 (mean 320 mg
kg−1). Other minor As sources include smelter emissions and mining
wastes, and As-rich effluents from the water treatment plants.
Another river with high contamination of As in Northern Chile is the
Elqui River, which provides water to >200,000 people. The occurrence
of chalco- and arsenopyrite in the upper Andes and inputs from mining
and geothermal activities are the sources of As for this river (Dittmar,
2004). Following two-year monitoring of As concentrations and flows
of the river, Dittmar (2004) determined 2.0 tons of As per year mobiliz-
ing throughout the river (in addition to 600 tons of Fe, 110 tons of Mn,
130 tons of Cu, and 35 tons of Zn). In the upper river system, confluence
with pH-buffered waters and precipitation of iron hydroxide decreased
the concentration of elements like copper (decreasing from 100 to
0.2 mmol L−1). However, arsenates did not adsorb onto suspended
solids and behave conservatively.
In Peru, there are several water resources affected by high As con-
centrations (Bundschuh et al., 2012a). The majority of encountered As
is of geogenic origin due to the Andean region's geology and natural
weathering. However, mining activities also input substantial loads of
As contaminants to these aquatic systems. Arsenic is transported from
the high elevations in the Andes mountains to the semi- or desertic en-
vironment in the lower elevations, where the population is denser,
which is also the case for the Copiapó River in the III Region of Atacama
(Bundschuh et al., 2020). In 2002, high concentrations of As were re-
ported in the Locumba River basin ranging from 200 to 400 μg L−1
(Castro de Esparza, 2002). The Locumba Valley population has been
consuming drinking water with high levels of As for a long time;
J. Bundschuh, J. Schneider, M.A. Alam et al.
however, there is no documentation of the health effects in this region
(Castro de Esparza, 2002, 2003).
The Rímac River basin (Fig. 4), situated east of Lima, Peru, presents
high levels of As due to mining activities in the middle and higher eleva-
tions of the basin and natural rock weathering of volcanic rocks and sul-
fide ore deposits (Bundschuh et al., 2012a). Elongated Rímac River basin
16 km wide and 200 km long, from east to west. The Water and Sewage
Service of Lima (Servicio de Agua Potable y Alcantarillado de Lima,
SEDAPAL) and the General Division of Environmental Health (Dirección
General de Salud Ambiental, DIGESA) monitors the water quality of the
Rímac basin. The annual average As concentrations from 1997 to 2004
were <200 μg L−1 (acceptable for irrigation according to Peruvian na-
tional regulations). However, in specific years (e.g., 2000, 2001, 2002),
As concentrations exceeded 200 μg L−1. Besides, there are spatial varia-
tions in the concentration of As. For example, in 2000, the highest con-
centration was detected close to the Fortuna mining center (Centro
Minero Fortuna; Fig. 4), at a sulfide ore deposit. The reported concentra-
tion at the time was 9160 μg L−1. Méndez (2005) investigated the influ-
ence of mining activities on this river's water and sediment quality.
Analysis of water and sediment samples collected at ten sites in October
2004 revealed that at 60% of the sites As exceeds 10 μg L−1, with the
lowest values at Blanco River (≤2 μg L−1, detection limit) and the
highest at Parac Creek (31 μg L−1, Fig. 4), with a median of 13 μg L−1.
For the river sediments, As ranged from 21 to 1543 mg kg−1, with a me-
dian of 245 μg L−1; with the highest value at Parac Creek (1543 mg
kg−1), and the lowest at Blanco River (21 mg kg−1, Fig. 4).
Another river contaminated with As in Peru is the Aruri River, where
Pacococha and Millotingo mines input contaminants (Corzo and
Gamboa, 2018). This river flows in the upper area of the Parac micro-
watershed, from where communities of San José de Parac and San
Antonio (San Mateo Huanchor District, Lima) take water for irrigation
purposes, especially in low-flow periods. Tailings, containing sulfides,
release leached As, Cd, Cu, Zn, and Mn to Aruri and Rímac rivers.
Fig. 4. Transport of arsenic by Rímac River from the mining area Fortuna in the Peruvian Andes to the Pacific Ocean contaminating coastal areas. In its pathway river water is used for ir-
rigation for agricultural and other purposes (Bundschuh et al., 2012a – with permission, License number 5015720249189).
18
Science of the Total Environment 780 (2021) 146274
Another example of As-rich river water discharges to the sea is the
Dole River, already described in conjunction with As-impacts related
to metal ore mining in Brazil.
3.6. Atmospheric As (dust and aerosol)
Ng et al. (2019) presented a wide range of research topics related to
the anthropogenic health risk from As exposure pathways in Paracatu
gold mining town in Brazil. They measured 600 airborne dust samples,
including PM10 and total suspended particulates (TSP), apart from
other As measures from surface and groundwaters, surface soil dust
from different dwellings, and major food categories, including rice and
bean. They concluded that the contribution of inhaled As is ≤3% of the
total daily intake, and food is the main contributor to the daily total As
intake. Total As intake by ingestion and inhalation, together with the
combined risk concerning cancer, is similar to consuming two liters of
water containing 10 μg L−1 of As. The likelihood of cancer is related to
the high probability of an individual exposed to an element (viz. As,
expressed in mg kg−1/day) causing cancer when he/she is continuously
exposed till turning 70.
In Chile, a study by Pino et al. (2015) on the state of environmental
health focused on air and water pollution and climate change. They con-
cluded that there are three main air pollution areas of the country, con-
taminated by particulate matter, heavy metals, and sulfur dioxide in
(i) a north-central region connected with mining and thermal power;
(ii) a highly populated urban area with the capital of the country – San-
tiago; and (iii) a central-south region of the country with the largest
proportions of low-income families; however, they do not report any
As data. Major health effects of As-contaminated water on the popula-
tions documented in Antofagasta, Chile, include an alarming number
of lung and bladder cancer and heart disease cases (e.g., Vormittag
et al., 2018; Khan et al., 2020).
J. Bundschuh, J. Schneider, M.A. Alam et al.
3.7. Arsenic exposure through geophagy and involuntary ingestion
The intake of soil occurs unintended (e.g., ingestion of dust, dirt, soil,
etc.; especially by children) or intentionally, through geophagy – the
practice of eating earth or soil-like substances such as clay, chalk, or ter-
mite mounds (e.g., Laufer, 1930; Bisi-Johnson et al., 2010; Abrahams,
2013; Nieder et al., 2018). Mainly young children are vulnerable to
soil ingestion, as they have a predilection for eating non-food items
like soil (Nieder et al., 2018). Intentional ingestion (geophagy) of soil,
which is associated with some geographic regions, mainly in the tropics,
and is reported in several countries, such as South Africa, Cameroon,
Democratic Republic of Congo, Nigeria, Swaziland, Tanzania, Uganda,
Kenya, China, India, Philippines, and Thailand (Nkansah et al., 2016).
In South America, geophagy has been observed in animals and
humans (Figueiredo et al., 2010). Despite no data on As being included
in this study, the presented information indicates potential As risks in
Latin America by geophagy. This is more likely in mining areas, where
As constitutes a well-known component in metal ores, tailing deposits,
and dust, like in the Paracatu gold mining region in Brazil (Ng et al.,
2019). Through determining the prevalence of geophagy and knowl-
edge about its health effects among healthy Sub-Saharan, South
American, and Caribbean adults attending a travel medicine and inter-
national vaccination consultation in France, Decaudin et al. (2020) con-
cluded that despite a long period of residence in France (15 years on
average), geophagy was still a current practice among 10.9% of
Sub-Saharan, South American, and Caribbean healthy adults. They rec-
ommended that tailored information about geophagy-associated risks
specific to these regions should be made available.
Due to the lack of studies on geophagy in the Latin American region,
some information from countries outside this region or findings not di-
rectly related to but applicable to As are presented to indicate potential
risks and underscore the need for respective studies in Latin America.
Geophagy is commonly reported among pregnant, nursing, school chil-
dren, and people with psychiatric disorders; however, its causes and
health risks remain poorly understood (Fawcett et al., 2016; Miller
et al., 2018). A predominant theory about the practice of geophagy is
that soil consumption acts as a source of nutrients (Miao et al., 2015).
Mineral nutrients such as Ca, Cu, Fe, Mn, Mg, and Zn can be supplied di-
rectly to geophagists through soil ingestion (Nieder et al., 2018) but
may contain toxic heavy metal(loid)s including As. Therefore, mineral,
chemical, and biological components ingested from soils can be harmful
to human health (Odongo et al., 2016; Bisi-Johnson et al., 2010). In
terms of toxicity of the elements via soil ingestion, the primary concern
reported so far has been for Pb (Nieder et al., 2018).
In several studies, geophagic samples showed concentrations ex-
ceeding the established safe limits for As, Pb, Hg, Cd in sub-Saharan
Africa (Bonglaisin et al., 2011; Owumi and Oyelere, 2015; Miller et al.,
2018). Other studies reported high levels of As in geophagic samples
in Bangladesh and The Netherlands (Al-Rmalli et al., 2010; Reeuwijk
et al., 2013; Nyanza et al., 2014). In contrast, studies on geophagic
lands from other countries, particularly in Ghana and Togo, have de-
tected As at low or non-existent levels, with no significant impact on
As levels in the blood (Tayie et al., 2013; Mathee et al., 2014). Review
work on environmental exposure to As during pregnancy found a
strong association between As and adverse pregnancy outcomes
(Quansah et al., 2015). Given these serious consequences for maternal
and child health, As-rich substances should be avoided (Miller et al.,
2018).
Studies conducted in the municipality of Rio Grande in southern
Brazil evaluated the effects of contaminated soil on the health of the off-
spring of rats exposed during gestation and lactation (García et al.,
2018). Soil leachate was administered by gavage following the daily
limits set by the United States Environmental Protection Agency (US
EPA), which allows a daily intake of 10 g of soil in a single geophagy
event, considering the weight of a 70-kg human being (US EPA, 1997;
García et al., 2018). The results reveal that exposure of parents to
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Science of the Total Environment 780 (2021) 146274
environmental stressors can compromise the health of offspring. In
this regard, the populations living in areas close to industrial activities,
mining, and areas with a high prevalence of acid rain need special atten-
tion (García et al., 2018).
More research is necessary to develop tools to assess the potential
risks of human exposure to the pollutants and determine significant
borderline concentrations in soils to protect human health.
4. Conclusions
There are seven primary sources and pathways of As pollution of the
environment in the Latin America region, which adversely affects not
only drinking water, soil, and air quality but also contaminates the
food chain. They constitute a significant health risk for the people
inhabiting the areas endemic to this endemic problem. These sources
and pathways include:
1) Volcanism and geothermalism
a) Volcanic rocks and fluids: Dissolution of As from volcanic rocks
and fluids (e.g., gases) in groundwater are widely found in Latin
America, impacting the drinking water quality of the populated
areas, including major cities, near active volcanoes in several
countries; for example, in Managua in Nicaragua, San Salvador in
El Salvador, San José in Costa Rica, Bogotá in Colombia, Mexico
City, Puebla and Cuautla in Mexico and Antigua in Guatemala.
b) Volcanic ash: Natural large-scale (up to >1000 km) eolic or fluvi-
atile transport of As containing highly soluble volcanic ash from
the Andes to its forelands is well recognized in the Argentine
part of the Chaco-Pampean Plain (>1,000,000 km2) but has also
been reported in the plain's extension in Paraguay and Bolivia.
Moreover, it is a potential As source in the Western Amazonia
(Peru) and other areas affected by volcanism in other Andean
countries, viz. Chile, as well as Central America and Mexico.
c) Geothermal fluids: As-rich fluids from deep (several km) geother-
mal reservoirs can ascend naturally to near-surface environments,
adversely impacting ground- and surface water resources and soil.
A salient example of such As contamination is the El Tatio-Geyser
Field (Chile) in the Andes, which has contaminated the Loa River,
flowing through the Atacama Desert. The exploitation of geothermal
resources for electricity generation is even more sensitive to the
near-surface environments, as evident in developed geothermal
fields like Los Humeros (Mexico), Miravalles, and Rincón de la
Vieja (Costa Rica), Zunil (Guatemala), and Platanares (Honduras).
Impacts on near-surface environments can be relatively high in
the absence of adequate residual wastewaters management
(e.g., through reinjection into deep rock layers, thus avoiding it com-
ing in contact with surface and groundwater). Failure of such mea-
sures at Momotombo Geothermal Plant (Nicaragua) has led to
Lake Managua's contamination, a vital freshwater resource.
2) Metal ore deposits and related mining and processing activities
Metal ore deposits are rich in As-containing minerals
[e.g., arsenopyrite (FeAsS)]. Natural weathering and lixiviation pro-
cesses mobilize As. However, mining and related ore and metal pro-
cessing activities increase As mobilization to different environments
(water, sediment, soil, and atmosphere) anthropogenically by vari-
ous orders of magnitude. This type of As pollution is prevalent in
Argentina, Chile, Bolivia, Uruguay, Peru, Brazil, Ecuador, Colombia,
Panama, Costa Rica, Nicaragua, Guatemala, and Mexico.
3) Coal deposits and their exploitation lead to As contamination, recog-
nized near the coal deposits in Brazil; e.g., Rio Grande do Sul, Santa
Catarina Paraná, and São Paulo.
4) Hydrocarbon reservoirs – and their exploitation cause As contami-
nation, resulting from the evaporation of seawater that concentrates
J. Bundschuh, J. Schneider, M.A. Alam et al.
As in petroleum reservoirs (e.g., in SE Mexico), which is the reason
for high As content of co-produced water with hydrocarbon exploi-
tation.
5) Solute and sediment transport through rivers (e.g., from mining
areas located in the mountains) to the sea and also As-bearing
dust particles and aerosols lead to pollution of surface water
(e.g., Loa and Elqui rivers in Chile, Locumba, Rímac, and Aruri
rivers in Peru, Doce river in Brazil) and groundwater resources
(e.g., Chaco-Pampean plain in Argentina; El Mojón, Cerro Mina
de Água, El Charco and Santa Rosa del Peñón regions in
Nicaragua; Achaya, Ananea, Caracoto districts in Peru) and soil
(e.g., Paracatu gold mining in Brazil), including coastal area
(e.g., Rímac River in Peru).
6) Atmospheric As (dust and aerosol) contamination has been re-
ported from Brazil, although inhaled As was found to be 3% of
total As intake.
7) Arsenic exposure through geophagy and involuntary ingestion is
not well studied in Latin America, although observed in both an-
imals and humans.
Consequently, through different (hydro)(bio)geochemical pro-
cesses, all the aforementioned As sources and pathways contribute to
As release into the near-surface environments. In these environments,
humans get exposed to high As levels through drinking water, soil, par-
ticulate matter, crops, and food products (fish/ seafood, livestock meat,
milk, cheese, etc.). Epidemiological and health risk studies have docu-
mented that As problem influences poor populations and rural or
periurban regions with contaminated groundwater as the only available
local water source. These people cannot afford to purchase purified bot-
tled water for drinking and cooking purposes like inhabitants from
more affluent rural areas, or periurban regions usually do. The review
of As-related health impacts has identified several diseases in the
Latin American region; viz., “Bell Ville Disease” (named after the se-
verely affected locality in Argentina), cardiovascular and cutaneous
As-related symptoms, cancer affecting different organs, reproductive
problems, pregnancy issues affecting cognitive functions in children,
genetic polymorphisms, hyperkeratosis, melanosis, actinic keratosis,
basal cell carcinoma, among others. It is vital to establish the practice
of monitoring the risk of As exposure through coordinated efforts of
different institutions to make the risk analysis comprehensive and
specific for effective mitigation of As-related endemic health prob-
lems. The adoption of widespread monitoring of As in water supply
system could be an important step in this regard, with the participa-
tion of water supply companies. Severity and scale of As contamina-
tion in Latin America and different parts of the world underline the
need for new and in-depth studies in potentially affected areas and
continuous monitoring and mitigation efforts in the area known to
be endemic to As contamination.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgements
The authors would like to thank the anonymous reviewers for their
careful reading of the original manuscript and its revised versions. Their
insightful comments and suggestions helped us tremendously in im-
proving the quality of our work. Efficient editorial handling is much
appreciated.
20
Science of the Total Environment 780 (2021) 146274
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