Impact of Mining On The Metal Content of Dust

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Environment International 169 (2022) 107490

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Environment International
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Full length article

Impact of mining on the metal content of dust in indigenous villages of


northern Chile
Nicolás C. Zanetta-Colombo a, b, c, *, Zoë L. Fleming d, e, Eugenia M. Gayo e, f, Carlos
A. Manzano g, h, *, Marios Panagi i, Jorge Valdés j, Alexander Siegmund a, b
a
Heidelberg Center for the Environment (HCE), Heidelberg University, Heidelberg, Germany
b
Department of Geography – Research Group for Earth Observation (rgeo), Heidelberg University of Education, Heidelberg, Germany
c
Department of Geography, SAI, Heidelberg University, Heidelberg, Germany
d
Envirohealth Dynamics Lab, C+ Research Center in Technologies for Society, School of Engineering, Universidad Del Desarrollo, Santiago, Chile
e
Center for Climate and Resilience Research (CR)2, Chile
f
ANID – Millennium Science Initiative Program– Nucleo Milenio UPWELL, Chile
g
Departamento de Química, Facultad de Ciencias, Universidad de Chile, Santiago, Chile
h
School of Public Health, San Diego State University, San Diego, CA, USA
i
School of Physics and Astronomy, University of Leicester, Leicester, UK
j
Laboratorio de Sedimentología y Paleoambientes (LASPAL), Instituto de Ciencias Naturales Alexander von Humboldt, Facultad de Ciencias del Mar y de Recursos
Biológicos, Universidad de Antofagasta, Antofagasta, Chile

A R T I C L E I N F O A B S T R A C T

Handling Editor: Adrian Covaci Indigenous communities from northern Chile have historically been exposed to the impacts of massive copper
industrial activities conducted in the region. Some of the communities belonging to the Alto El Loa Indigenous
Keywords: Development Area are located less than 10 km from the “Talabre’’ tailings dam, which contains residues from
Toxic metal copper production and other metals that can be toxic to human health (e.g., As, Sb, Cd, Mo, Pb). Given the
Mining emissions
increasing demand of copper production to achieve net-zero emission scenarios and concomitant expansions of
Pollution risk
the tailings, the exposure to toxic metals is a latent risk to local communities. Despite the impact that copper
Health risk assessment
Atacama production could generate on ancestral communities from northern Chile, studies and monitoring are limited and
the results are often not made accessible for local communities. Here, we evaluate such risks by characterizing
metal concentrations in dust collected from roofs and windows of houses from the Alto El Loa area. Our results
showed that As, Sb, Cd, Cu, Mo, Ag, S, and Pb concentrations in these matrices can be connected to local copper
mining activities. Additionally, air transport models indicate that high concentrations of toxic elements (As, Sb,
and Cd) can be explained by the atmospheric transport of particles from the tailings in a NE direction up to 50 km
away. Pollution indices and Health Risk Assessment suggested a highly contaminated region with a health risk
for its inhabitants. Our analysis on a local scale seeks to make visible the case of northern Chile as a critical
territory where actions should be taken to mitigate the effects of mining in the face of this new scenario of in­
ternational demand for the raw materials necessary for the transition to a net-zero carbon global society.

1. Introduction align with many of the Sustainable Development Goals (SDGs) set by the
United Nations for 2030, such a situation could lead to new socio-
Copper has become a key metal for the technological development of environmental conflicts, particularly in developing regions of the
global modern societies. Over the next few decades, its relevance will world in which the increased extraction and production of copper and
increase, spurred on by the urgency of achieving carbon neutrality other metals could have a direct effect on some of the SDGs at a local
(Schipper et al., 2018). The demand for copper is expected to increase by scale: well-being, equality, access to clean water and sanitation, among
275–350% by 2050 (Elshkaki et al., 2016). Although this will certainly others (Zografos and Robbins, 2020).

* Corresponding authors at: Heidelberg Center for the Environment (HCE), Heidelberg University, Heidelberg, Germany (N.C. Zanetta-Colombo). Departamento de
Química, Facultad de Ciencias, Universidad de Chile, Santiago, Chile (C.A. Manzano).
E-mail addresses: [email protected] (N.C. Zanetta-Colombo), [email protected] (C.A. Manzano).

https://doi.org/10.1016/j.envint.2022.107490
Received 14 April 2022; Received in revised form 29 July 2022; Accepted 22 August 2022
Available online 24 August 2022
0160-4120/© 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
N.C. Zanetta-Colombo et al. Environment International 169 (2022) 107490

One of the most important impacts of copper mining on surrounding developmental abnormalities (Tchounwou et al., 2003; Thomas et al.,
local communities is the trace element pollution brought about by dust 2009). The impact of copper mining has been documented in the
emissions either from ore extraction, high-temperature processing, and Americas (Zapata, 2020; Moya et al., 2019), Oceania (Mudd et al.,
tailings disposal (Csavina et al., 2012). Especially, from the emission of 2020), Africa (Wilson et al., 2017), Asia (Monjezi et al., 2009; Pandey
non-essential trace elements or potentially toxic elements (PTE) even at et al., 2007), and Europe (Lilic et al., 2018; Song et al., 2017). However,
low concentrations (e.g., As, Cd, Sb, Pb, Hg, among others) (Pourret more studies are needed in rural areas of the global south, a region with
et al., 2021). PTEs represent a significant risk to ecosystems and human large copper deposits yet to be explored.
health as they are considered persistent pollutants that bioaccumulate in Chile has a long mining tradition since pre-Columbian times, with a
organisms throughout the food chain (Khan et al., 2015; Sall et al., sustained industrial development since the 16th century (Gayo et al.,
2020). Additionally, the exposure to some PTEs such as As and Pb are 2019). Today, it is the world’s largest copper producer (27% of global
associated with a wide array of chronic diseases, neurological and production in 2021) through massive operations concentrated in the
neurobehavioral disorders, increased cancer risk, as well as northern and central regions of the country (19◦ –33◦ S). The processes

Fig. 1. Regional and local settings. The map shows a) the location of the Antofagasta Region in the Chilean and South American context. b) Geomorphologic units
(numbers) are shown, as well as the location of the primary mining operations (black dots). In b) numbers allude to (1) Coastal escarpment, (2) Coastal plain, (3)
Coastal range, (4) the Atacama Desert, (5) Precordillera, (6) Loa depression, (7) Domeyko range, (8) Inter-range basins, (9) Cordillera de la Sal, (10) Salar de Atacama
basin, (11) Altiplano, (12) Active volcanoes. The dotted lines represent the approximate location of the Atacama Fault System (AFS), the Domeyko Fault System
(DFS), and the Antofagasta-Calama Lineament (ACL). c) Study area and the indigenous communities where samples were taken with the Chuquicamata (CH),
Ministro Hales (MH), Radomiro Tomic (RT), and El Abra (EA) mining operations shown. d) Wind Roses for Calama Norte (T80CN) showing the frequency of counts
by wind direction (%) and wind speed (m s− 1), separated into daylight and nighttime hours. The website http://walker.dgf.uchile.cl/Mediciones/ was run for 2011-
02-21 to 2012-12-27.

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N.C. Zanetta-Colombo et al. Environment International 169 (2022) 107490

involved in metal mining (i.e., excavation, crushing, grinding, separa­ The region has a hyper arid climate with two sources of humidity.
tion, smelting, refining, and tailings management) are a large anthro­ During the austral summer (December – February), northeastern
pogenic source of PTEs on a national scale, representing 98% of all (monsoonal) air flows from the Amazon, leading to allowing rain and
emissions in the country (Zhu et al., 2020), which have increased with snow (Houston and Hartley, 2003). Extreme events associated with La
the recent expansion of production and exports (Cerda et al., 2019; Niña usually generate floods in the area. During austral winter (June –
Eichler et al., 2015, 2017; Gayo et al., 2019; Schwanck et al., 2016; August), south westerly airflows bring frontal precipitation from extra­
Vleeschouwer et al., 2014). tropical cyclones, where extreme events tend to be associated with El
The study of the potential impacts of PTE emissions in Chile has Niño (Houston, 2006).
focused on urban areas (Madrid et al., 2022; Muñoz et al., 2019; Tapia Precipitation, although scarce, increases with altitude, with an
et al., 2018), while rural areas have been poorly addressed. This has average annual precipitation of 4.2 mm in Calama and 63.3 mm in
created an important gap of information in mining regions, in which Caspana (see their locations in Fig. 1c) with significant contributions of
socio-environmental conflicts have emerged (Manzano et al., 2021; summer rains in the upper part of the basin (Houston, 2006).
Romero-Toledo, 2019; Tapia et al., 2018; Zang et al., 2018). There is a strong diurnal variability in wind speed and direction.
Located between the hyperarid Atacama Desert and the Andean Northerly down-valley wind direction occurs during the night, while
mountains (Fig. 1), Alto El Loa is the leading mining center in the westerly upslope flows are characteristic during the daytime (Muñoz
country and one of the most important in Latin America. Here, the et al., 2018; González-Rojas et al., 2021) (Fig. 1).
Chuquicamata mine (once considered the largest open-pit mine in the The Loa River, the longest in Chile 440 km, originates in this area (at
world) has developed its industrial activity since the beginning of the 3950 m a.s.l.) and extends westward to the Pacific Ocean, creating an
20th century, and other large industrial facilities such as Radomiro important green corridor that crosses the hyper-arid core of the Atacama
Tomic, El Abra, Collahuasi, and Ministro Hales have been operating Desert. The Loa River flow has progressively decreased over the past
since the 1990s. Moreover, the country’s largest tailing dam (Talabre, decades because of the intensive exploitation of the aquifers adjacent to
~60 km2) is also located in this area. it by mining activities, affecting the indigenous communities and the
Alto El Loa is an Indigenous Development Area (IDA), a protection native flora and fauna (Herrera et al., 2021). The Loa River receives
figure that the Chilean government implemented in 1995 in order to surface and groundwater contributions from the Salado River in its
protect the quality of life of its native people (Vergara et al., 2006), and upper course, near Chiu Chiu. The Salado River (Fig. 1c), which in turn
it is the most illustrative example of the socio-environmental tensions is a tributary of the El Tatio geothermal field, has been studied for its
between indigenous communities (Atacameño, Quechua, and Aymaras) high concentrations of As, which has led it to be considered the primary
and mining companies (Carrasco, 2015) which has been fuelled by the source of this toxic metal in the Loa basin (Romero et al., 2003).
expansion of mining operations in response to the prevailing neo­ Geological background and geomorphological units: In northern
liberalist (extractivism) economic model of Chile (Smart, 2017). Despite Chile, the occurrence of the porphyry Cu and porphyry-related mineral
the demands of communities for more clarity about the consequences of deposit and their spatial distribution is strongly associated with the
mining operations on human and environmental health, no public eastward-migrating tectonic-magmatic activities, controlled by the
environmental monitoring has been implemented so far, and much of Atacama and Domeyko fault system (Zhu and Lu, 2016). In the Anto­
the information derives from a few sparse studies (De Gregori et al., fagasta Region, the Coastal Cordillera, a Carboniferous – Early Triassic
2003; González-Rojas et al., 2021). magmatic arc, contains numerous copper deposits from the Upper
This study aims to evaluate the potential impacts of the local mining Jurassic, such as Mantos Blancos (Ramírez et al., 2006). Tracking the
industry on the IDA territory by analysing concentrations and spatio- displacement of tectonic activity, a Paleocene-early Eocene belt of
temporal patterns in the distribution of PTEs. We provide the first porphyry copper deposits is situated within the Central Depression,
insight into local levels of environmental contamination (i.e., pollution where the Spence deposit stands out as part of the Antofagasta – Calama
levels and enrichment factors) as well as potential exposure to PTEs via Lineament (Palacios et al., 2007). Slightly further east, a late Eocene-
ingestion. We focused on settled dust as this environmental matrix offers early Oligocene belt is hosted by rocks of the Precordillera, which
the means to assess the population’s exposure to potentially toxic ele­ occur along the Domeyko Fault Zone (DFZ) (Fig. 1b). During the
ments in outdoor (Moya et al., 2019; Rout et al., 2013; Tapia et al., 2018; structural and geomorphological evolution of the Precordillera, some
Taylor et al., 2014) and in indoor environments (Gohain and Deka, deposits have been exhumed and exposed at the surface (Cameron et al.,
2020; Shi and Wang, 2021; Yang et al., 2015). More importantly, in 2008), such as the Chuquicamata porphyry Cu (Mo-Ag) deposit.
areas where official environmental monitoring is limited or absent, this Controlled by the initial intrusions (~36–33 Ma) through mineralization
inexpensive approach allows an assessment of pollution sources, their to post-mineral brecciation and offset by the West fault system (Ossan­
intensity and potential impacts. Additionally, since the impact of mining don et al., 2001), Chuquicamata has been exploited since pre-colonial
operations does not solely rely on the quantity and toxicity of emissions times (Fuller, 2004) and is the world’s greatest copper orebody. The
(Csavina et al., 2012), but also on dispersion processes, we evaluated the Calama basin, located between 2000 and 3500 m a.s.l. (22◦ − 23◦ S), is a
potential for atmospheric transport of air pollution which can be mid-elevation sedimentary plateau covering approximately 2000 km2.
indicative of the quantity and type of settled dust in the IDA. Most of the indigenous villages of Alto El Loa are situated within this
basin, usually within or close to the deep river canyons that form natural
2. Materials and methods oases and shelters from the persistent winds.
Mining and Talabre tailings: The Talabre tailings have their origin
2.1. Sampling area in the Chuquicamata porphyry copper deposits (Smuda et al., 2014). The
primary minerals extracted are sulfides (including pyrite (FeS2), bornite
The Antofagasta Region, in the North of Chile, has a total population (Cu5FeS4), chalcopyrite (CuFeS2), and digenite (CuAsS4)) among others.
of 607,504 inhabitants (INE, 2018). This region has undergone signifi­ After crushing and milling, the ore is treated chemically to separate the
cant transformations in recent decades, mainly because of the expansion ore from secondary elements and impurities. 80% of the water used in
of large-scale mining operations, which has affected other traditional the process is obtained from the Loa River and 20% from the water
agricultural practices, increasing rural-to-urban migration (Calderón- recovered from the tailing after the flotation process. With an average
Seguel et al., 2021). The largest urban center in the region is the city of tailing deposition of about 200,000 t/day, the total volume of the
Calama, which has a population of 165,731, approximately 98% of Talabre impoundment is approx. 600,000 m3 and in 2009 covered a
which are located in urban centers, while less than 2% are located in total surface area of 52 km2 (Smuda et al., 2014). Once the sedimenta­
rural areas (INE, 2018). tion reaches 3 m in the tailing, the discharge point is shifted to another

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N.C. Zanetta-Colombo et al. Environment International 169 (2022) 107490

basin and subsequently, water-saturation decreases due to drainage and and markers of traffic emissions were not measured. The detection limits
evaporation, forming unsaturated vadose zones, exposing dry sediments for each element are included in the results in Table 1.
that could be lifted by winds.
2.3. Statistical methods
2.2. Sample collection, processing, and analysis
Descriptive statistics (i.e., mean, standard deviation, skew, kurtosis),
A social participative sampling methodology was used, allowing and the coefficient of variation (CV), were used to categorize and
local people to accompany the process and, after having a brief training describe the distribution of elements in the study area. Similar ap­
by the researchers, participate in the sampling process. It has been proaches have been used in other urban environments worldwide (Hou
proposed that simple local engagement, including active collaborations et al., 2019; Doyi et al., 2019; Fan et al., 2022). The CV was calculated to
and codesign of strategies, can alleviate what has been called the envi­ compare the variability of the metal concentration from the total settled
ronmental belief paradox (the disparity between the level of concern dust. According to previous studies, the CV was categorized into four
and engagement of affected communities in environmental justice is­ classes: CV ≤ 20% was regarded as low variability, 21% < CV > 50%
sues) (Dietz and Whitley, 2018; Pearson et al., 2018). Allowing the indicated moderate variability, 51% < CV ≤ 100% as regarded as high
community to be part of the scientific process can help us develop shared variability, and CV > 100% was considered very high variability.
perspectives on the problem they are facing, and promote pro- The Spearman correlation coefficients were calculated to determine
environmental behaviour. correlations among elements, while principal component analysis (PCA)
The sampling points were selected based on community relevance (e. was conducted to explore further connections.
g., schools and community centers) and were often suggested by locals.
Outdoor dust was collected between January 5 and January 8, 2021. 2.4. Potential transport of dust particles
Twenty-nine samples were collected from the roofs and windowsills
(from now on referred to as “windows”) in seven indigenous villages of
Potential for dust resuspension at Talabre: The tailings discharge
Alto El Loa: Lasana (La, n = 5), Chiu Chiu (Ch, n = 6), Conchi Viejo (Cv,
at Talabre consists of 45.1 wt% solids and 54.9 wt% water (Smuda et al.,
n = 4), Taira (Ta, n = 4), Cupo (Cu, n = 2), Caspana (Ca, n = 4), and
2014). High levels of solar radiation and limited surface humidity favor
Toconce (To = 4) located within a radius of 60 km from Talabre and
high evaporation, which decreases the water content of the tailings,
Chuquicamata (Fig. 1). A synthetic bristle brush, washed with distilled
leaving dry material available on the surface that can be subjected to
water after each sampling, was used to sweep accumulated dust into a
atmospheric transport. The Normalized Difference Water Index (NDWI)
polypropylene container. Similar methods have been previously used to
was calculated for the Talabre tailing dam for 127 days between 2018
report trace metals concentrations in deposited dust in roofs near in­
and 2020, using the threshold (>0.015) for wet tailing proposed by (Hao
dustrial areas in South Korea (Lee et al., 2020), China (Yu et al., 2017),
et al., 2019). NDWI was calculated by Google Earth Engine and Landsat
and Peru (Chui Betancur et al., 2016); and in roads near urban centers
7, using the following formula:
(Trujillo-González et al., 2016; Amato et al., 2009). Each sample was
composed of at least three subsamples of the same type and sector to G − NIR
NDWI = (1)
increase representativeness. In addition, surface soil samples of 2 cm G + NIR
depth (collation of 6 samples collected with stainless steel spoons from a
1 m2 area) were collected in the dust sampling sites to obtain a vertical where NIR is the spectral reflectance in the Near Infra-red Band (Band
gradient (roof – windows – soil). For reasons of force majeure, no soil 8), and G is the spectral reflectance in the Green Band (Band 3).
samples were collected in the village of Chiu Chiu. The geographical Dispersion modelling: The Numerical Atmospheric Modelling
positions of sampling sites were measured by a portable GPS (Garmin Environment (NAME) model, created by the UK Met Office (Jones et al.,
Etrex 30 model). The geographical coordinates of all sampling sites can 2007) was used to plot air mass footprints that show the dispersion of the
be found in the supplemental information (Table S1). air that passes over the surface of the mine and its transport for the next
Sample processing was carried out in the Faculty of Engineering at 9 h. NAME uses meteorological fields from the Unified Model (Brown
the Universidad del Desarrollo (UDD) in Santiago, Chile. Samples were et al., 2012), to track the pathways of hypothetical inert tracers. The
dried in an oven (1 hr. at 100 ◦ C) and sieved to the < 75 µm fraction with fields used in this study had a resolution of 0.23◦ longitude by 0.16◦
a stainless steel mesh standard testing sieve (ASTM E-11/2009) to latitude with 59 vertical levels up to an approximate height of 30 km. 3-
separate the coarser particles and components that could interfere with hourly footprints were modelled for the whole of 2020 for 9 h forwards
further analysis. The sieve was washed with demineralized water after (since already after this time many air masses have already crossed the
sieving each sample to avoid cross-contamination. Particles below border to Bolivia) from Talabre on a 0.05◦ × 0.05◦ resolution, focussing
75 µm in diameter are conventionally considered “dust”, and this frac­ on the layer from 0 to 100 m above the surface, thus taking into account
tion has been widely used for health risk assessment in populations when substances or emissions could be picked up from a surface and
exposed to potential contaminants, mainly through ingestion routes when they could reappear on the surface further afield. The models were
(Zhao et al., 2016; Fan et al., 2022; Malakootian et al., 2021). Addi­ carried out in an objective way, taking into account a long-lived tracer
tionally, some studies indicate that this fraction can contain relatively (with CO as the tracer) and estimating the potential extent of transport
high metal concentrations (Kolakkandi, et al., 2020; Förstner and Sal­ of any air mass. The run was done without knowledge of chemical
omons, 1980; Horowitz et al., 1990). composition and without any knowledge of suspension or deposition of
A subset (0.2 g) of the < 75 µm fraction was digested in 20 ml of a particulate matter, making it an objective view on the potential extent of
multi-acid (5 ml HNO3, 2.5 ml HCIO4, 10 ml HF, 5 ml HCl/ 20% HCl) influence of winds from one area to another. The units were based on a
and analysed using Inductively Coupled Plasma Optical Emission release of a known quantity of air masses (hypothetical particles) in
Spectrometry (ICP-OES, PerkinElmer Avio® 500) with spectral correc­ grams (g) during an integrated time-period (s) and the results are dis­
tions using an ion-exchange chromatography (IEC) model. Blank and played per grid box, which has a volume component.
standard reference materials (OREAS 153b and OREAS 602, Melbourne,
Australia) were used for quality assurance and quality control 2.5. Risk assessment
(Table S2). Elemental analyses were made at the certified laboratory:
SGS Minerals S.A. in Santiago, Chile. The analysis focused on the Enrichment factors and Geoaccumulation index: The enrichment
determination of elements potentially coming from mining activities in factor (EF) and the index of geoaccumulation (Igeo) were applied to
rural areas of northern Chile, and thus, other abundant crustal elements assess metal concentrations and distribution in the settled dust of the

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N.C. Zanetta-Colombo et al. Environment International 169 (2022) 107490

Table 1
Descriptive statistics and basic testing for metals in total settled dust. The Coefficient of Variability that displays the variability in the measurements between sites is
graded by (*) with *** showing the highest variability, then ** and then *. Those without * showed little variation, suggesting there was little anthropogenic influence.
Metal Al Fe S Ti Cu Zn As V Pb Mo Cr Ni Co Sb Cd Ag
Unit % % % % % mg mg mg mg mg mg mg mg mg mg mg
kg− 1 kg− 1 kg− 1 kg− 1 kg− 1 kg− 1 kg− 1 kg− 1 kg− 1 kg− 1 kg− 1

ns total 29 29 29 29 29 29 29 29 29 29 29 29 29 25 15 26
DL 0.01 0.01 0.01 0.01 0.01 1 1 1 1 2 1 1 1 2 1 0.5
ns BDL – – – – – – – – – – – – – 4 14 3
mean 7.3 4.1 0.6 0.5 0.2 2352.1 197.8 131.4 101.9 79 42 16.2 14.4 12.1 2.6 2.4
sd 0.6 0.6 0.4 0.1 0.2 3324.7 137.9 18.1 63.2 80 17.8 2.2 5.3 9.7 1.6 2.1
median 7.5 4 0.5 0.5 0.2 547 147 130 88 65 36 16 13 9 2 1.7
min 6.2 3.1 0.2 0.3 n.d. 159 67 104 25 5 25 13 10 2 1 0.5
max 8.4 5.7 1.6 0.7 0.7 12,498 564 204 221 338 119 23 39 38 6 8.9
range 2.2 2.6 1.4 0.4 0.7 12,339 497 100 196 333 94 10 29 36 5 8.4
skew − 0.3 0.9 1.5 1.1 0.8 1.5 1.4 2.1 0.5 1.5 2.8 1.1 3.4 1.3 0.8 1.5
kurtosis − 0.8 0.9 1.1 2.1 − 0.6 1.2 0.9 6.5 − 1.2 2 9.4 1.2 12.6 0.8 − 0.9 1.7
CV (%) 8 14 65** 18 78** 141*** 70** 14 62 101*** 42* 13 37* 80** 63** 89**

villages of Alto El Loa, relative to the regional background levels, EPA, 2009)); EF is the exposure frequency of 365 days year− 1 (assuming
following equations (2) and (3). children spending all the time in their villages); ED is the exposure
( M) duration (6 years for children is assumed in this study), equivalent to the
EF = ( M)
X sample
(2) average lifetime (Huang et al., 2008); BW is the average body weight in
X background kg (18.6 kg average for the range 3 to < 6 years) (US EPA, 2009); and AT
is the averaging time estimated as the ED * 365 days. This is a well-
Igeo=
Cn
(3) known method that has provided important information on the poten­
1.5*Bn tial health risk associated with contaminated areas worldwide (Kurt-
Karakus, 2012; Hou et al., 2019; Doyi et al., 2019; Fan et al., 2022). It
where M is the concentration of the metal being analysed and X is the was calculated for children, who are likely to ingest more through their
concentration of the reference element; and where Cn is the measured playing habits and who are more susceptible to the effects of pollution as
concentration of metal, Bn is the geochemical background, and a factor their organism is still growing and developing.
of 1.5 is used to include the possible variation of background values due Potential non-carcinogenic risk related to specific PTE were then
to lithogenic effects (Müller, 1979). assessed using Hazard Quotient (HQ) according to the Eq. (5).
An element with low variability of occurrence is used as a reference
for the EF. Typically, Al, Fe, Mn, or Rb are used as reference elements, HQ =
ADD
(5)
which should not have a direct anthropogenic source. Since Mn and Rb RfD
were not measured in this study, and Al is a major component of the
roofs sampled (55% Al: 43.4% Zn: 1.6% Si), we used Fe as the reference where RfD (mg/kg/day) indicates the oral reference dose of PTE as
element (Fe showed the second lowest variability in the study area, CV: suggested by US EPA (3 × 10− 4 for As, 1 × 10− 3 for Cd, 4 × 10− 4 for Sb,
14%). If the EF ranges from 0.5 to 1.5, natural weathering processes or 4 × 10− 2 for Cu, 5 × 10− 3 for Mo, 5 × 10− 3 for Ag). The US EPA has not
crustal materials might be influencing this concentration. However, if established an RfD for Pb, but was derived from published studies
the values exceed 1.5, there is a possibility that the trace metal (1.4 × 10− 3) (Cao et al., 2015). If the HQ is greater than 1, there may be
contamination occurred because of anthropogenic activities. Pollution concern for potential adverse non-cancer health effects. The greater the
levels of EF were classified as: deficiency to minimal enrichment value of HQ, the greater the level of concern (Huang et al., 2008).
(EF < 2), moderate enrichment (2 < EF < 5), significant enrichment Considering that the exposure to more than two pollutants can result in
(5 < EF < 20), very high enrichment (20 < EF < 40), and extremely high an additive effect, the Hazard Index (HI), the sum of individual HQ, was
enrichment (EF > 40) (Barbieri, 2016). calculated (Eq. (6)) to assess the overall potential of non-carcinogenic
The Igeo index was evaluated following the scale proposed by Müller effects posed by more than one PTE. If HI < 1 then no significant risk
(1981): unpolluted (Igeo < 0), unpolluted to moderately polluted occurs, but when HI > 1 chronic risk is more likely to occur.
(0 < Igeo < 1), moderately polluted (1 < Igeo < 2), moderately to strongly ∑n
HI = HQ (6)
polluted (2 < Igeo < 3), strongly polluted (3 < Igeo < 4), very strongly i=i

polluted (4 < Igeo < 5), and extremely polluted (5 < Igeo). This study Carcinogenic risk (CR) indicates the possibility of an individual
used the average background values for the Antofagasta Region, developing any kind of cancer due to exposure to carcinogenic hazards
composed of 17 soil samples collected in pollution-free zones (Fig. S1) (US EPA, 1989). The CR of As and Cd, both carcinogenic elements, were
by the Chilean National Center for the Environment (CENMA, 2014). calculated according to Eq. (7).
Health Risk Assessment: The health risk assessment model pro­ CR = ADDxSF (7)
posed by the United States Environmental Protection Agency (US EPA)
was applied to quantify the potential non-carcinogenic and carcinogenic where SF (mg/kg body per day)− 1 refers to the slope factor which is 1.5
risk from ingesting settled dust by children in Alto El Loa (US EPA, 1989; for As and 6.1 for Cd. If the risk is higher than the threshold value of
US EPA, 2009; US EPA, 2013). 1 × 10− 4 – 1 × 10− 6, the risk is considered as unacceptable according to
(Ci × IngR × EF × ED) USEPA, while values below 1 × 10− 6 are not considered to pose sig­
ADD = × 10− 6
(4) nificant health effects.
(BW × AT)

where ADD is the average daily intake doses (mg kg− 1 day− 1); C rep­
resents the PTE concentrations in settled dust (mg kg− 1); IngR is the
recommended central tendency of settled dust ingestion rates for chil­
dren (200 mg day− 1 for the age < 6 including soil and outdoor dust (US

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3. Results and discussion residents.

3.1. Concentrations and spatial distribution of PTEs


3.2. Correlations between PTEs in dust samples and identification of
The statistical description of the metals found in the research area is potential sources
presented in Table 1. The mean metal concentration of the total settled
dust (average of roof and windows concentration) ranked in the order Al The correlation coefficients and statistical significance between all
(7.3 %) > Fe (4.1 %) > S (0.6 %) > Ti (0.5 %) > Cu (0.2 %) > Zn pairs of elements are presented in Table S4 in the supplemental infor­
(2352.10 mg kg− 1) > As (197.76 mg kg− 1) > V (131.38 mg kg− 1) > Pb mation. Positive and significant (p ≤ 0.001) correlations were observed
(101.86 mg kg− 1) > Mo (78.97 mg kg− 1) > Cr (42.03 mg kg− 1) > Ni between Cu and Ag, Mo, and As with coefficients ranging between 0.82
(16.24 mg kg− 1) > Co (14.45 mg kg− 1) > Sb (12.08 mg kg− 1) > Cd and 0.96, suggesting a common source. Positive and significant corre­
(2.60 mg kg− 1) > Ag (2.40 mg kg− 1). Table S3 shows the metal average lation coefficients were also found between As-Cd (0.81) and As-Sb
concentrations in dust obtained from the three surfaces under study (0.92) (Fig. 2); while Fe showed strong positive and significant corre­
(roofs, windows, and soils). All soil samples (17) presented values for Sb lations with V and Al and negative correlation with As, Cd, and Sb
below the detection limit (BDL), while Cd and Mo presented 10 and 9 (Fig. 2).
samples BDL. Four principal components (factor 1, factor 2, factor 3, and factor 4)
In general, the concentration of metals in the dust collected from with eigenvalues > 1 were extracted from the PCA analysis (Table S5).
roofs was higher than for windows: 2.2 times higher for Zn, 1.8 for Mo, These four factors explained 84% of the overall variance, with 43% for
1.5 for Cu, 1.4 for Ag, As, and Sb, 1.3 for Pb, 1.1 for Cd, Cr, and Co, 1.0 factor 1, 24% for factor 2, 8% for factor 3, and 9% for factor 4. Factor 1
for Ni, Al, S, Fe, and V, and 0.9 for Ti; and for soils: three times lower has strong positive loading for Cu, As, Cd, Sb, Ag, and Mo, moderate
than roofs and two times lower than windows. The biggest differences positive loading for Pb and S (the same metals that were seen to have the
between roof and soils were found for Zn, Mo, Cu, As, and Pb, with highest CVs), and weak positive loading for Zn and Cr. Factor 2 has
concentrations 15, 6, 4, 3, and 2.9 times higher in roof samples strong positive loading for Fe, V, and Ti, moderate positive loading for
(Table S1). Half of the metals under study (Ag, As, Cu, Cd, Mo, S, Sb, and Ni and Al, and weak positive loading for Cr. Factor 3 has strong positive
Pb) showed their maximum concentrations in roofs from the villages of loading for Co and weak positive loading for Ni. Factor 4 has moderate
Lasana and Cupo (NE of the Talabre tailing dam). Pb concentrations positive loading for Zn and Al. The principal component 1 which is the
were also close to the maximum at Caspana and Conchi Viejo (to the east biggest contribution of variability is likely from anthropogenic activities
and north of Talabre, respectively). including mining and metal processing and like the CV suggests that Cu,
The Coefficient of Variability (CV) was calculated to compare the As, Cd, Sb, Ag, and Mo vary significantly between villages. Fig. 3 pre­
variability of the element concentration from the total settled dust sents a visual representation of the first two components (PC1 and PC2),
collected in all sampling sites (Table 1). Zn and Mo showed very high their elements and their contributions.
variability with CVs of 141% and 101%, respectively, while Ag, Sb, Cu, The relationship observed between As, Cd, Sb, Cu, Mo, Ag, and Pb in
As, S, Cd, and Pb showed high variability with CV values between 89% Factor 1 of Principal Component Analysis and the high and statistically
and 62%. These elements mentioned would have the highest possibility significant correlation coefficients between them suggests they may
of being influenced by specific sources in the area, such as anthropo­ have resulted from the emission of mining activities through the process
genic activities. On the other hand, the CV values of Cr and Co (moderate of extraction (Cu-Mo) and high-temperature processes and the re-
variability) and Ti, V, Fe, Ni, and Al (low variability), indicate that its suspension of the Talabre tailing material (As-Cd-Sb-Ag-Mo
contents were almost constant across Alto El Loa, suggesting low
anthropogenic contribution (Table 1). Highly skewed coefficients were
found for Co, Cr, V, Zn, Mo, Ag, S, As, Sb, Ti and Ni, indicating asym­
metrical distributions. The skewed coefficients of Fe, Cd and Cu were
considered moderately skewed, while Pb and Al, symmetrical. All metals
showed kurtosis greater than zero except for Cu, Al, Cd and Pb.
The large variation of the concentration of As, Sb, Zn, Pb Cu, and Mo
within Alto El Loa villages shows an inhomogeneity in the region.
Mining operations, and mainly the emission from the Talabre tailing
dam, might be impacting some of the villages in Alto El Loa. Maximum
concentrations were found in Lasana (~13 km from Talabre) and Cupo
(~50 km from Talabre), indicating that these villages might be the most
exposed due to meteorological factors such wind patterns that determine
the transport of pollutants over long distances (Fig. 1). However, we
suspect that high Pb concentrations in Conchi Viejo could be associated
with the large vehicle fleet from the El Abra mining site, approximately
5 km away from the village. Additionally, the elevated Pb concentra­
tions in Caspana could be due to the use of diesel-powered generators.
The vertical distribution of the concentrations
(roofs > windows > soil, 3:2:1) suggested that the dust settling on the
roof is less influenced by soil and site-specific conditions, and could be
an indicator of potential atmospheric transport. In this sense, roofs may
be a good surface for sampling since the signal from local conditions
Fig. 2. Correlation matrix showing the covariance between metals for all dust
seems to be low. The windows, on the other hand, showed concentra­
samples collected from Alto El Loa. Each cell shows the correlation between two
tions that could be influenced by both the materials transported from
variables, blue indicates a positive correlation coefficient and red indicates a
within the community (e.g., soils) and from distant sources (e.g., mining negative correlation coefficient (or an inverse correlation). The statistical sig­
operations). The concentrations of both outdoor surfaces could always nificance is represented by the size and color intensity of the cell. Fully colored
enter the indoor environment (Moya and Phillips, 2014; Ibanez et al., cells indicate high statistical significance. Note the high degree of correlation
2010; Madany et al., 1994), generating a greater risk for the health of the between As, Cd, Sb, Cu, Mo, Ag, S, Zn and Pb.

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3.3. Transport patterns

The NAME dispersion model was run every 3 h (for the air passing
over the surface of Talabre between the 3-hour blocks of 00:00–03:00,
03:00–06:00, …., and 21:00–00:00 every day). Local time is UTC- 3
(except between April and August when it was UTC-4). The NAME runs
were done in UTC but the accumulated results showing diurnal cycles
PC2 (24 %)

were converted to local time. The video in the appendix (V1) collates all
these runs, to show the variability and the patterns of the extent of
Talabre’s influence during 2020. The air often passes over all the vil­
lages and other times it follows a narrower and direct route towards
Cupo, by-passing the villages in the north. The pattern also varies be­
tween seasons, with a broader, more dispersed footprint in winter (May
to November) than in the summer. Fig. 5 shows two typical footprints
found during the daytime (in January) and nighttime (in September),
displaying the typical westerly influence during the day, when the dust
from the mine could be transported to the villages and the reverse in
wind direction, when easterly nighttime winds would mean that there is
PC1 (43 %) unlikely to be a transport from the direction of the mine towards the
villages.
Fig. 3. Biplot for metal concentrations measured in dust samples collected from The four closest grid boxes (0.25◦ × 0.25◦ ) around each village were
Alto El Loa. This plot is a visual representation of the first two components (PC1 selected so that a regional analysis technique could detect for each 3
and PC2). The x-axis represents the PC1 explaining 43% of the total variance, hourly footprint what % contribution of the total geographical coverage
and the y-axis represents the PC2 explaining 24% of the total variance. The of the 9 h footprint each village received (Fleming et al., 2012). The
colors of the elements represent the element’s contribution to the respective
results from this analysis were plotted in the summary diurnal cycle for
component. Both PC1 and PC2 explain 67% of the total variance.
the whole of 2020 in Fig. 6a, showing how between 9:00 and 18:00 local
time (GMT-3) all villages received more air from over Talabre (westerly
r = 0.97–0.90). The association of these elements to mining emissions winds). The data has been normalized to show relative contributions for
and, in particular, to the inadequate management of mine tailings has each village. In Fig. 6b, the relative contribution of air passing over
been reported previously in Cerro de Pasco mining complex in Perú Talabre that each village receives has a seasonal influence, with for
(Molloy et al., 2020), Krugersdorp, South Africa (Ngole-Jeme and example Caspana having a greater contribution of air from Talabre in
Frantke, 2017), and in the Rosh Pinah area, Namibia (Kříbek et al., winter and Cupo a greater contribution in summer. Each village receives
2014). Factor 2 (Fe, V, and Ti) and Factor 3 (Co and Ni) are metals more air from Talabre during the daytime, but some villages are affected
characterized by natural emissions, such as rock weathering. Factor 4 more strongly in certain seasons.
(Zn and Al) could be influenced by the roof material “Aluzinc”, Since we are looking objectively at air mass transport in general and
commonly used in the study area, and which composition contains high not modelling the behaviour of suspended particles, further research is
percentages of Zn (43%), Al (55%), and Si (2%). needed to quantify the flux of atmospheric PM depositing in local vil­
A few studies have evaluated the influence of the El Tatio geothermal lages. Sometimes the air masses could pass over a village and deposit all
field and the drainage of its water into the Salado River - a tributary of the dust but other times the dust could remain suspended and be
the Loa basin - for its important contribution of As (Romero et al., 2003) deposited many km away from the source. Molloy et al. (2020) suggests
(Fig. 1c). Furthermore, these studies have suggested that El Tatio is the that due to the dryness of the area and the strong winds the area re­
primary source of As in Alto El Loa, while copper mining could be a ceives, dust particles could travel up to 50 km.
secondary contributor. Although the present study does not ignore the
relevance of El Tatio as a source of As in the El Loa basin, it suggests that
3.4. Pollution indexes
the mining activity, and specially the resuspension of dust enriched in
metals from the Talabre tailing dam, may have a significant impact on
The calculated geo-accumulation index (Igeo) values of toxic metals in
increasing the concentration levels of As and other metals in some of the Alto El Loa are presented in Fig. 7. The mean values of Igeo increased in
villages of Alto El Loa. Principal component analysis calculated by
the following order: Ag (0.18) < Cd (0.85) < Mo (7.96) < Pb (9.46) < As
Romero et al. (2003) of concentrations obtained from water and sedi­ (11.20) < Cu (16.72). In almost all samples under study, the Igeo values
ment samples in the Loa basin suggests that As (with a mean value of for Cu, As, Cr, Pb, and Mo far exceeded the lower limit of category 6
1400 ug/l, or 1.4 mg kg− 1) is associated with high concentrations of B (Igeo > 5) or “Extremely contaminated” with ranges between 14.58 and
and Li, the primary metals found in El Tatio. However, the concentra­ 18.69, 9.92–12.99, 7.73–10.87, and 4.79–10.87, respectively. Cd and Ag
tions of As found in the present study show a strong association with Cu, values range from “Not polluted” (Category 0) to “Moderately to heavily
Sb, and Cd (Fig. 2 and Fig. 3), metals present in high concentration in the polluted” (Category 3). The village with the highest Igeo values in the
sediments of Talabre. study area was Lasana, followed by Cupo (for As and Ag) and Conchi
While emissions from the Chuquicamata smelter, inaugurated in Viejo (for Cu and Mo). On the other hand, the lowest Igeo for As, Cu and
1952, were regulated in 1991 through the control of air emissions of Ag were found in Toconce and Caspana (the villages directly east and
particulate matter (PM), sulfur dioxide (SO2), arsenic (As), and mercury farthest away from Talabre), while Pb has the lowest Igeo in Taira, the
(Hg) (MINMINERIA, 1991), the Talabre tailings deposit does not have northernmost village.
measures to regulate emissions of dust rich in PTEs. In fact, through the The calculated Enrichment Factor (EF) values of toxic metals in Alto
NDWI analysis, it was possible to identify that, on average, >60% of the El Loa are presented in Fig. 8. The mean values of EF increased in the
total area is made up of dry surface material (or dry tailings) and would following order: Cd (1.03) > Ag (1.18) > Pb (3.85) > As (4.51) > Mo
be available for resuspension (Fig. 4). Climate factors such as low water (4.65) > Cu (12.91). Almost all samples analysed for Cu and As show
cover, low rainfall, high evaporation, and strong winds could enhance enrichment factors above background concentration (EF > 1.5), ranging
the resuspension and transport of PET from Talabre to the villages in the between 2.00 and 37.00 and 1.44 and 12.73, respectively. The mean EF
area (Csavina et al., 2014). of Lasana (28.12) reflects very high enrichment, while Cupo (18.50) and

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Fig. 4. a) Variation of water content in the Talabre


a) 03-02-2020 03-05-2020 tailing dam viewed by the normalized difference
Summer Autumn water index (NDWI). This index combines infrared
and visible bands, where dark blue represents water,
light blue presence of moisture, and light green the
absence of water. Maps were obtained from Sentinel
Hub Eo Browser Playground (see: https://apps.sentine
l-hub.com) b) Temporal variation of the wet tailing
(Threshold > 0.015) in Talabre between 2018 and
2020 viewed by the NDWI. The red dotted line in­
dicates the average wet tailings area for the study
period. During the period evaluated, the area of
Talabre was 66.5 km2. To see its size and position
relative to the study area, see Fig. 1c.

01-08-2020 09-11-2020
Winter Spring

b)

Conchi (17.14) are at the upper limit of significant enrichment. The of the background levels of metals is carried out locally. However, the
highest EFs for As in Lasana and Cupo indicate significant enrichment, metals that were highlighted to show greater prominence and accu­
while the rest of the Alto El Loa villages show moderate enrichment mulation within villages were similar to those found in the variability
(2.38 – 4.48). For both metals, the lowest EF values were found in analysis and in the principal component analysis (As, Cu, Pb, Mo, Ag and
Caspana and Toconce. Lasana and Cupo also show significant enrich­ Cd and Cr to a lesser extent).
ments for Mo, with averages of 10.93 and 6.64, respectively, while the
rest of the communities show moderate enrichment, except for Toconce, 3.5. Health risk assessment
which shows depletion to minimal enrichment. Cd and Ag are less
enriched in Alto El Loa than the beforementioned metals, with EFs The calculated hazard quotient (HQ) by ingestion of potentially toxic
ranging between 1.52 and 0.36 for Cd and between 4.21 and 0.26 for Ag. elements (PTEs) in Alto El Loa villages is illustrated in Fig. 9. The spatial
However, the highest enrichments for Cd and Ag, as well as for Cu, As, distribution of HQ in Alto El Loa presents a similar pattern in almost all
and Mo, are also found at Lasana and Cupo. Lasana and Cupo showed a elements evaluated, suggesting a higher potential non-carcinogenic risk
higher variability for both Igeo and EF between the samples, but in to children from potential dust ingestion in Lasana and Cupo. This is
general higher levels than in the other villages for most metals. Finally, consistent with the contamination levels (Igeo, Fig. 7) and enrichment
all villages in Alto El Loa showed enrichment factors > 0 for Pb, indi­ (EF, Fig. 8) presented and discussed in previous sections.
cating an anthropogenic contribution. Arsenic is the PTE with the highest potential non-carcinogenic risk in
The results obtained through the calculation of pollution indices with Alto El Loa, where all communities present a risk above the accepted
these regional average concentrations should be considered with level (HQ ≤ 1). While the average of Alto El Loa communities exceeds up
caution and only as a preliminary approximation until a complete study to 7.08 times the accepted levels, some samples in Lasana and Cupo

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a) 1 January 18:00 hrs. (day-time) b) 6 September 05:00 hrs. (night-time)

Fig. 5. An example of 3 hourly footprints of where the air from Talabre travels during a period of 9 h at surface (0–100 m levels). a) On the 1st of January (21:00
UTC) (1st January 18:00 local time) the air passed over Lasana and Cupo, avoiding the more northerly villages like Conchi Viejo and Taira. b) On the 6th of
September at 09:00 UTC (05:00 local time) one can see when easterly night-time winds blow, Talabre wouldń t affect the villages. The air frequently travels into
Bolivia within < 9 h and could deposit dust from the tailings on any of these surfaces it has passed over. The colors in the legend are logarithmic, with red showing in
the areas where the air spends most time.

Fig. 6. a) Relative contribution of air masses that pass over Talabre arriving at each village according to time of day (showing the standard deviation over the whole
year). b) Relative contribution of air masses from Talabre on each village (shown as monthly averages).

exceeded them by up to 20 times. Although it is known that this region is communities of Lasana, Conchi Viejo, and Cupo exceeded the accepted
geologically enriched by arsenic (Romero et al. 2003), the fact that the limits for Cu. In this case, Conchi Viejo joins Lasana and Cupo (which, as
communities of Lasana and Cupo present an average risk higher than the already mentioned, could be affected by the transport of dust from
others suggests an anthropogenic influence and, concerning the trans­ Talabre) since the copper extraction site of the El Abra mining company
port models presented in previous sections, this difference could be is located within the community area (Fig. 1). Finally, the ingestion of
better explained by the transport of As-rich dust from the Talabre tail­ dust by children in the communities of Lasana, Conchi Viejo, Cupo, and
ings dam (Fig. 4). After ingestion, at least 90% of inorganic arsenic is Caspana could pose a potential non-carcinogenic risk to them by Pb,
absorbed via the gastrointestinal route and distributed through the given that their levels are above the accepted limits. As we have
blood to different organs such as the liver, kidneys, lungs, and bladder mentioned in previous sections, the influence of the passage and
(Watanabe and Hirano, 2013). Although health effects cannot be permanence of vehicles in Conchi Viejo (due to the proximity to the El
determined through this study, possible health effects associated with Abra mining company) and the use of fossil fuels for energy supply in the
arsenic ingestion include cardiovascular and peripheral vascular dis­ town of Caspana could be increasing the risk in these communities.
eases, developmental abnormalities, neurological and neurobehavioral When considering the addition of more than one toxic element
disorders, diabetes, portal fibrosis, hematological disorders, and multi­ through the Hazard Index (HI) (Fig. 9), all villages had exceeded the safe
ple cancers such as skin, lung, liver, urinary bladder, kidney, and colon threshold (HI ≤ 1), thus indicating a potential non-carcinogenic effect of
cancers (Tchounwou et al., 2003). Therefore, studies and public policy ingestion of settled dust. The values of HI indices were the highest in
measures to mitigate the potential adverse effects on children’s health in Lasana (HI between 12.97 and 25.28), followed by Cupo (HI between
Alto El Loa should be undertaken urgently. 5.02 and 24.78), Conchi (HI between 4.30 and 12.35), Chiu Chiu (HI
Although Sb, Cd, Mo, and Ag are PTEs that we have associated in this between 4.34 and 12.89), Caspana (HI between 3.39 and 8.72), Taira
study with emissions from the Talabre tailings, our results here suggest (HI between 3.61 and 7.20), and Toconce (HI between 2.85 and 9.35).
that the communities of Alto El Loa are not yet experiencing a health risk For carcinogenic risk due to As ingestion (Fig. 10), the ranking of CR
from ingestion of these elements. However, increased emissions - due to in the seven villages of Alto El Loa was Lasana (6.42x10− 03) > Cupo
projected increases in production (Elshkaki et al., 2016) - could increase (5.43x10− 03) > Chiu Chiu (2.84x10− 03) > Conchi Viejo
the risk, especially for Sb, which is close to acceptable limits in some (2.51x10− 03) > Toconce (1.93x10− 03) > Taira (1.92x10− 03) > Caspana
villages (Fig. 9). On the other hand, almost all dust samples taken in the (1.77x10− 03), with all samples in Alto El Loa exceeding the upper limit

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Fig. 7. Geoaccumulation index (Igeo) of the Indigenous Villages in IDA Alto El Loa. Roof samples are presented with black squares, while window samples are
presented with white squares. The blue dotted line indicates the upper limit of category 0: Not polluted, while the red dotted line indicates the lower limit of category
6: Extremely polluted. The villages shown in Fig. 1 are Lasana (La), Chiu Chiu (Ch) (close-by to the east), Conchi Viejo (Cv), Taire (Ta) (to the north), and Cupo (Cu),
Caspana (Ca) and Toconce (To) (to the east).

Fig. 8. Enrichment Factor (EF) of the Indigenous Villages in IDA Alto El Loa. Roof samples are presented with black squares, while window samples are presented
with white squares. The red dotted line (1.0 on the y-axis) indicates the boundary between natural contribution (<1.5) and anthropogenic effect (>1.5). The villages
shown in Fig. 1 are Lasana (La), Chiu Chiu (Ch) (close-by to the east), Conchi Viejo (Cv), Taire (Ta) (to the north), and Cupo (Cu), Caspana (Ca) and Toconce (To) (to
the east).

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Fig. 9. HQ for each metal and total HI for Ingestion in Alto El Loa. The red dotted line indicates the accepted level limit (HQ ≤ 1). Roof samples are presented with
black squares, while window samples are presented with white squares. The villages shown in Fig. 1 are Lasana (La), Chiu Chiu (Ch) (close-by to the east), Conchi
Viejo (Cv), Taire (Ta) (to the north), and Cupo (Cu), Caspana (Ca) and Toconce (To) (to the east).

Fig. 10. CR for As and Cd for Children in Alto El Loa. The blue dotted line (10− 06, lower limit) and the red dotted line (10− 04, upper limit) indicate acceptable ranges.
Roof samples are presented with black squares, while window samples are presented with white squares. The villages shown in Fig. 1 are Lasana (La), Chiu Chiu (Ch)
(close-by to the east), Conchi Viejo (Cv), Taire (Ta) (to the north), and Cupo (Cu), Caspana (Ca) and Toconce (To) (to the east).

of the accepted range (10− 04), showing a high carcinogenic risk. With 4. Conclusions
values up to 9.09 and 8.91 times above the upper limit of the accepted
range, Lasana and Cupo, respectively, have CRs 1.97 and 1.67 times Our study suggests that the variations in As, Sb, Cd, Cu, Mo, Ag, Pb,
higher than the Alto El Loa average and 3.49 and 2.95 times higher than and S concentrations in outdoor settled dust in the Alto El Loa villages
the average of the communities with the lowest CR in the study area can be explained by emissions from mining activities. The Talabre
(Caspana y Taira). On the other hand, the CR values for Cd are within the tailing dam -adjacent to Indigenous villages- can be an important source
accepted ranges (Fig. 9), with no carcinogenic risk for children in Alto El of dust containing high concentrations of potentially toxic elements and
Loa through potential Cd ingestion. the predominant winds could easily transport this to neighbouring

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villages. Our results indeed indicate that wind direction and intensity Appendix A. Supplementary material
play a pivotal role in the transport of dust particles, particularly during
the daytime, but also seasonally. Supplementary data to this article can be found online at https://doi.
The highest concentrations, as well as the highest variability in the org/10.1016/j.envint.2022.107490.
trace metals were found in the villages of Lasana and Cupo, to the
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