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Arsenic and other trace elements in thermal

springs and in cold waters from drinking water
wells on the Bolivian Altiplano
ARTICLE in JOURNAL OF SOUTH AMERICAN EARTH SCIENCES MARCH 2015
Impact Factor: 1.36 DOI: 10.1016/j.jsames.2015.02.006

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Journal of South American Earth Sciences 60 (2015) 10e20

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Journal of South American Earth Sciences

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

Arsenic and other trace elements in thermal springs and in cold

waters from drinking water wells on the Bolivian Altiplano
~ oz a, b, *, Prosun Bhattacharya a, *, Ondra Sracek c,
Mauricio Ormachea Mun
Oswaldo Ramos Ramos a, b, Jorge Quintanilla Aguirre b, Jochen Bundschuh a, d,
Jyoti Prakash Maity e
a

KTH-International Groundwater Arsenic Research Group, Department of Sustainable Development, Environmental Science and Engineering, KTH Royal
Institute of Technology, Teknikringen 76, SE-100 44 Stockholm, Sweden
Instituto de Investigaciones Qumicas (IIQ), Facultad de Ciencias Puras y Naturales, Universidad Mayor de San Andr
es, 303, La Paz, Bolivia
c
Department of Geology, Faculty of Science, Palack University, 17. listopadu 12, 771 46 Olomouc, Czech Republic
d
Faculty of Engineering and Surveying, University of Southern Queensland, Toowoomba, Queensland 4350, Australia
e
Department of Earth and Environmental Sciences, National Chung Cheng University, 168 University Road, Ming-Shung, Chiayi County 62102, Taiwan
b

a r t i c l e i n f o

a b s t r a c t

Article history:
Received 9 June 2014
Accepted 23 February 2015
Available online 4 March 2015

Numerous hot springs and fumaroles occur along the Andes Mountains, in the Bolivian Altiplano, where
people use thermal springs for recreational purposes as pools, baths and also for consumption as
drinking water and irrigation once it is mixed with natural surface waters; most of these thermal springs

emerge from earth surface and ow naturally into the rivers streams which drain further into the Poopo
Lake. Physicochemical characteristics of the thermal water samples showed pH from 6.3 to 8.3 with an
average of 7.0, redox potential from 106 to 204 mV with an average of 172 mV, temperatures from
40 to 75  C with an average of 56  C and high electrical conductivity ranging from 1.8 to 75 mS/cm and
averaged 13 mS/cm. Predominant major ions are Na and Cl and the principal water types are 37.5% Na
eCl type and 37.5% NaeCleHCO3 type. Arsenic concentrations ranged from 7.8 to 65.3 mg/L and arsenic
speciation indicate the predominance of As(III) species. Sediments collected from the outlets of thermal
waters show high iron content, and ferric oxides and hydroxides are assumed to be principal mineral
phases for arsenic attenuation by adsorption/co-precipitation processes. Arsenic concentrations in cold
water samples from shallow aquifers are higher than those in thermal springs (range < 5.6e233.2 mg/L),
it is likely that thermal water discharge is not the main source of high arsenic content in the shallow
aquifer as they are very immature and may only have a small component corresponding to the deep
geothermal reservoir. As people use both thermal waters and cold waters for consumption, there is a
high risk for arsenic exposure in the area.
2015 Elsevier Ltd. All rights reserved.

Keywords:
Arsenic
Bolivian Altiplano
Hydrochemistry
Lithium
Thermal springs

1. Introduction
Surface waters and groundwater aquifers are severely
impacted by mining activity in the central Bolivian Altiplano
(BA), heavy metals and arsenic (As) are principal pollutants of
water and soils in localized areas around mines (PPO, 1992,
1996a,b,c, 1997; Garca, 2006). Economically the rural area of

* Corresponding authors. KTH e International Groundwater Arsenic Research

Group, Division of Land and Water Resources Engineering, Department of Sustainable Development, Environmental Sciences and Engineering, Royal Institute of
Technology (KTH), Teknikringen 76, SE-100 44 Stockholm, Sweden. Tel.: 46
87908136; fax: 46 8208946.
E-mail addresses: ormachea@kth.se, maurormache@gmail.com (M. Ormachea
~ oz), prosun@kth.se (P. Bhattacharya).
Mun
http://dx.doi.org/10.1016/j.jsames.2015.02.006
0895-9811/ 2015 Elsevier Ltd. All rights reserved.

the BA is one of the poorest regions in the country; the climate is

arid and water scarcity together with poor quality of the limited
water resources i.e., high salinity and pollution are major concerns for obtaining safe drinking water. There are also indications
that surface- and ground-water contain elevated concentrations
of natural As (PPO, 1996b; Van Den Bergh et al., 2010; Ramos
et al., 2012; Ormachea et al., 2012, 2013), due to a lack of clean
water resources much of this water is used as drinking water
especially in rural areas. Thermal springs and fumaroles occur
extensively along the eastern fringe of the Andes (Eastern
 Lake basin in the central BA. We
Cordillera) close to the Poopo
hypothesize that discharges from such thermal springs may
result in natural high As concentrations in the environment and
in the groundwater aquifers.

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

High As concentrations have been widely reported in

geothermal reservoirs at the Los Azufres and Los Humeros sites
along the Trans-Mexican Volcanic Belt (TMVB) (Birkle et al., 2010).
At Los Azufres site, As concentration in geothermal waters reaches
49.6 mg/L, but highest concentrations up to 73.6 mg/L are reported
from Los Humeros site. Discharge of geothermal waters at Los
Azufres and their leakage from evaporation ponds contaminates
surface drainage where concentrations of As up to 8 mg/l were
found (Birkle and Merkel, 2000). In Yellowstone National Park As
concentrations in geothermal springs exceed 1 mg/L (Ball et al.,
1998) and over 100,000 kg of geothermal As is estimated to leave
the western boundary of the Park each year (Nimick et al., 1998). In
Chile, the concentration of As at the geothermal eld El Tatio reaches 27 mg/L and concentration of about 1.4 mg/L were detected
downstream in the Rio Loa fed by the discharge of geothermal
water (Romero et al., 2003). Following the discharge of geothermal
waters, As is attenuated by several processes including dilution and
adsorption onto stream sediments enriched in ferric oxyhydroxides
(Webster and Nordstrom, 2003). However, in arid environments
geothermal As can be concentrated by evaporation and thus, its
concentration frequently increases in spite of on-going attenuation
processes (Banks et al., 2004; Welch et al., 2000).
In Bolivia, no comprehensive studies have been carried out so far
on the hydrochemistry of thermal springs that occur in a large scale
mainly along the Andes Mountains. A general description of the
locations and major ions in some thermal springs of Oruro Department was made by Huaranca Olivera and Neumann-Redlin (2000)
and Taquichiri (2005). Another study deals with water remediation
in which among other water samples, two thermal springs were
characterized for water quality (Klartell and Sandholm, 2009). In a
very recent investigation, Morteani et al. (2014), assessed the potential of some thermal waters of the BA to form ores.
The purpose of this study is to make a geochemical assessment
and determine the hydrochemical characteristics of thermal
springs and its relationship with the distribution of As and other
trace elements in the central BA. The principal objectives of the
study were (a) to determine basic hydrogeochemical characteristics
of thermal springs, and (b) to determine the importance of thermal
springs as potential sources for high As concentration in groundwater in the area. Selected cold water samples collected from
shallow wells from our concurrent studies (Ramos et al., 2012),
were included in this paper to dene local meteoric composition,
for comparison with water samples from hot springs collected for
this study and to understand the possible geochemical evolution of
hot springs by the mixing with cold groundwater.
2. The study area
2.1. Location, physiography and climate
The study area is located in the central BA, a plateau whose
topographic elevation ranges from 3600 to 3900 m above sea level
(PPO-3, 1996a, b, c). The endorheic system TDPS (Titicaca, Desa, and Salares subsystems) (Fig. 1), comprises a large
guadero, Poopo
area of 143900 km2 at a high altitude in the BA plateau (Revollo,
 Lake basin is a part of the TDPS system and is
2001). The Poopo
located in the central BA at an altitude of 3686 m above mean sea
level. The lake has a maximum length of 90 km and a maximum
 Lake has an area that varies from
width of 53 km. The Poopo
2650 km2 to 4200 km2 on a seasonal basis (Quintanilla, 1994).
 Lake basin is characterized by a cold semi-arid climate
Poopo
with annual average temperature of 7  C with a signicant daily
variation (Huaranca Olivera and Neumann-Redlin, 2000). The mean
annual rainfall for a period of 40 years is 372 mm (Risacher and
Fritz, 2000), most precipitation falls as rain during the December

11

to March, precipitation is higher closer to the mountains in the east,

the dry season is from May to September (Huaranca Olivera and
Neumann-Redlin, 2000). Extreme weather situations are frequent
with both droughts and oods, as a result of the natural variation in
precipitation further upstream in the basin (Garcia, 2006). Erosion
of the top soil due to overgrazing and deforestation is a severe
problem in the BA (Van Damme, 2002).
2.2. Geology and hydrogeology
 Lake basin is located between the Eastern and the
The Poopo
Western Cordillera of Los Andes, both of different geological
evolutionary history (YPFB-GEOBOL, 1996). The Eastern Cordillera
is composed of Paleozoic and Mezozoic rocks, which were deposited on the Precambrian basement and deformed by multiple
orogenic cycles from Paleozoic to Cenozoic. Principal rocks are
Ordovician limestones, quartzites, slates and schists with low angle
faults. The Western Cordillera is composed of volcanic material
accumulated in late Tertiary and early Quaternary. Principal rocks
are basalts, dacites, rhyodacites, and andesitic lavas (Fig. 1).
 Lake sub-systems are conThe Titicaca Lake and the Poopo
nected by the Desaguadero River, and the Lacajahuira River con Lake and the Coipasa Salt Flat. The area of the
nects the Poopo
 Lake watershed is 24,013 km2 and the basin comprises 22
Poopo
 and Uru
ephemeral river sub-basins (Calizaya, 2009). The Poopo
Uru Lakes are shallow ones with maximum depths of 3.5 and 0.8 m,
respectively (Pillco and Bengtsson, 2006).
Most recharge in the study area occurs during the summer
period between December and February (Garreaud and Aceituno,
2000). The western limestone and sandstone formations are signicant recharge zones due to their high permeabilities (Van
Damme, 2002) and constitute potentially productive aquifers. The
eastern mountain chain plays a critical role in the local hydrology
because high local precipitation is a source of recharge for
groundwater in the plain. The general ow pattern in the plain is
 . The ow is slow due to low hypointing towards the Lake Poopo
draulic gradient and low permeability of the sediments; the predominant lacustrine and alluvial sediments typically have high
fractions of silt and clay reducing water ow.
In Bolivia, three main areas with geothermal manifestations
have been identied: Western Cordillera, the Altiplano border of
the Eastern Cordillera and the Eastern Cordillera (Huaranca Olivera
and Neumann-Redlin, 2000). The present study is focused on the
 Lake basin due to the extensive
Eastern Cordillera within the Poopo
occurrence of thermal springs in this area (Fig. 1).
Structurally, the Altiplano corresponds to a graben-type continental basin which resulted from the displacement and uplift of the
Paleozoic block of the Eastern Cordillera (Huaranca Olivera and
Neumann-Redlin, 2000). The occurrence of springs near the
border of Eastern Cordillera and the Altiplano correspond to the
face of a very deep fault line. Product of a normal heat ow at
depths of 2000e3000 m, these hot waters take advantage of this
fracture zone to rise up to the surface. The origin of the thermal
waters in the Eastern Cordillera is related to the rather complex
structural factor of the Andes. The Andes have been subjected to
several compressive stresses and also affected by phases of plutonic
magmatism, on the one hand and a second Late Miocene subvolcanic to extrusive magmatism on the other. Thermal manifestations are mainly found in folded Paleozoic strata, linked to local
faults and fractures. There is no evidence of a direct relationship of
geothermal waters to igneous bodies at the surface; although such
relationship is inferred to exist at depths such in the form of
magmatic chambers or heat-emitting nuclei (Huaranca Olivera and
Neumann-Redlin, 2000). Large deposition of black or reddish sediments suggests the ongoing precipitation of sulphides and

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

12

Fig. 1. The BA and the TDPS endorheic system (inset map upper right). Map of the study area, main geologic formations, major villages and sampling sites.

hydroxides from the thermal water of the springs (Lehrberg and

Morteani, 1989).
3. Material and methods
3.1. Sampling and measurement of in situ eld parameters
At each sampling site, the geographical locations and elevation
were recorded using a hand-held global positions system (GPS)
GARMIN 12 and plotted in a map (Table 1 and Fig. 1). Before

sampling, temperature, oxidation reduction potential (ORP), pH

and electrical conductivity (EC) were measured in the eld using a
portable HACH sensION1 instrument equipped with a combination
electrode, ORP was measured using Ag/AgCl electrode and corrected with respect to standard hydrogen electrode. After cooling
(approx. 5e10 min) to a 35  C, alkalinity (reported as HCO-3) was
measured on the site by titrating with 0.01 N HCl.
Water samples were collected from 16 hot springs for the
analysis of major cations, trace elements, anions and As speciation,
following standard protocol for water sampling (Bhattacharya et al.,

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

3.3. Data analysis

Table 1
Geographical locations of hot springs sites.
#

1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16

Location

Soracachi
Obrajes
Capachos
Machacamarca

Poopo
Cabrera
~a
Pazn
Urmiri 1
Urmiri 3
Urmiri 4
~ as
Malliri de Pen
Phutina
Aguas Calientes
Challapata
Castilluma
Vichajlope

13

Coordinates
Latitude

Longitude

17 470 00.0000 S

17 490 35.2100 S
17 530 29.3800 S
18 100 11.5000 S
18 220 47.9400 S
18 220 57.1400 S
18 350 27.3400 S
18 340 30.5200 S
18 340 21.6000 S
18 340 25.8300 S
18 440 45.7200 S
18 500 06.9900 S
18 520 60.0000 S
18 550 54.4800 S
19 080 33.3600 S
19 160 15.4500 S

67 010 06.4700 W

66 590 26.9700 W
67 020 39.2800 W
66 590 49.9000 W
66 570 34.3700 W
66 560 39.5900 W
66 550 30.7500 W
66 520 09.1600 W
66 520 04.8400 W
66 520 11.1700 W
66 430 13.0200 W
66 390 59.3800 W
66 320 17.0000 W
66 460 51.8900 W
66 390 59.3800 W
66 420 57.4200 W

Elevation
(masl)
3799
3804
3739
3763
3785
3795
3734
3796
3804
3798
3823
3811
3739
3737
3897
3841

2002). Water samples included: (1) ltered (using Sartorius

0.45 mm inline lters) for major anion analyses; (2) ltered and
acidied with HNO3 (14 M) for the analyses of cations and other
trace elements including As. Arsenic speciation was performed
with Disposable Cartridges (MetalSoft Center, USA) in the eld,
following the methodology described by Meng et al. (2001). These
cartridges strongly adsorb As(V) while allowing As(III) to pass
through. All samples were kept at 4  C until laboratory analyses.
Sediments related to thermal springs were taken on the same
sites as the thermal water samples and then they were stored in a
plastic zip lock bag. A total of twelve sediment samples were taken
during the eld work; sediment sampling was feasible in almost all
hot springs sites, but in some places the access was impossible.
3.2. Analytical methods
3.2.1. Major ion and trace elements analyses in water
2
Major anions Cl, NO
3 and SO4 were analyzed at the laboratory of the Division of Land and Water Resources Engineering at
KTH using a Dionex DX-120 Ion-Chromatograph (IC). The major
cations, Na, K, Ca2, Mg2, As and trace elements were analyzed
in the ltered acidied water samples using a Varian Vista Pro
Inductively Coupled Plasma Optical Emission Spectrometry (ICPOES) at Stockholm University. The As-speciation samples gave the
As(III) concentration and subtraction from the As(Tot) in the trace
elements samples then gave the amount of As(V). For quality
control, eld blanks, reagent blanks and spiked samples were
prepared and analyzed. Accuracy was tested by analyzing a
certied reference material: NIST SRM 1643 eeTrace elements in
water. Replicate analyses were carried out to check the precision
of the results, accuracy and precision indicated variations within
the range of 8%.
3.2.2. Sediment analyses
Sediment samples were sieved to homogenize the particle size
(sieve opening 2 mm) and dried in an oven at 35  C. 0.5 g of the
dried sample were digested with HNO3 (bi-distilled acid, 96.2%)
using a 3000 Anton Paar microwave digestion system at 280  C and
a maximum pressure of 8600 KPa, after digesting, samples were
ltered through 0.45 mm lter and diluted to 50 mL with deionized
water. The solutions were analyzed for elemental composition
including As, using a Varian Vista Pro Inductively Coupled Plasma
Optical Emission Spectrophotometer (ICP-OES) at Stockholm
University.

To evaluate the water chemistry results, Aquachem software

(4.0.264 Waterloo Hydrogeologic Inc, 2003) was used to create
Piper, Box & whisker, Giggenbach and bivariate plots, to determine
water type and to calculate the ion-balance of the thermal waters.
Saturation indices and As speciation were calculated using
PHREEQC program (Parkhurst and Appelo, 1999) and MINTEQ
database (minteq.dat). Thermodynamic data for Ca-arsenate minerals and complexes (Bothe and Brown, 1999) and Mg complexes
with As (Whiting, 1992) were added to identify additional aqueous
species and saturation indices.
4. Results and discussions
4.1. Environmental parameters of thermal springs
Results of thermal springs are presented in Table 2, the pH
values ranged from 6.3 to 8.3 with an average of 7.0. Measurement
of ORP ranged from 106 to 204 mV (average: 172 mV). The
positive redox value can be the result of the mixing of thermal
waters on their way to the surface with cool dilute meteoric ground
waters. Temperatures of the springs varied considerably, ranging
from 40 to 75  C (Average: 56  C). Electrical conductivity is high and
varies widely within a range between 1860 and 75810 mS/cm.
4.2. Hydrochemistry of thermal water
4.2.1. Major elements
Water chemistry data of major ions presented in Table 2 were
plotted in a Piper diagram which shows no clear difference between the chemical compositions of the thermal waters in the BA,
the thermal waters are mostly of the NaeCl and NaeCleHCO3 type.
Here it is assumed that deeper hot waters of NaeCl type during
their ascension reach groundwater rich in bicarbonate, evolving to
waters NaeCleHCO3 types before reaching the ground surface
(Fig. 2).
Concentrations of predominant ions Na and Cl in thermal
waters are present in the ranges of 339e12866 mg/L (average:
2635 mg/L) and 177e21022 mg/L (average: 3781 mg/L), respectively (Fig. 3a). The highest salinity is present in the sample
collected near Challapata (14) (Fig. 1) which lies in the lacustrine
deposits. Na and Cl are strongly positively correlated (Fig. 4),
suggesting that thermal springs are inuenced by the dissolution of
evaporate minerals such as halite present in large amount as a
consequence of the arid climate and high rate of evaporation. Sodium and chloride occur in halite at equal molar concentrations
(Na/Cl molar 1, Na/Cl mass 0.648), in our thermal water samples, the mass ratios higher than 0.65 (Fig. 4) may indicate halite is
not the only source of sodium in hot springs and other processes
like the weathering of plagioclase minerals could inuence the
salinity (Ramos Ramos et al., 2014, Raychowdhury et al., 2014)
(Fig. 4). Compared with data from Ramos et al. (2012), concentrations of Na and Cl are much higher in thermal waters than in cold
waters (Table 2).
Another major anion in thermal waters is HCO-3, present in the
concentration range of 429e1892 mg/L with an average of 997 mg/L
(Fig. 3a). High concentration of this anion is presumably due the
weathering/dissolution of limestone present in large amounts
along the sedimentary rocks in the Eastern Cordillera. In the
Giggenbach (1988) diagram, thermal springs fall within the eld of
immature waters (Fig. 5) which may suggest the effects of a variety
of processes including re-equilibrium and strong dilution/mixing
with shallow cold waters. Mixing of full equilibrated NaeCl waters
with shallower meteoric waters can produce the bicarbonate-rich

14

Table 2
Major ion composition in thermal springs and in cold waters from shallow wells.
Location

Hot springs
1
Soracachi
2
Obrajes
3
Capachos
4
Machacam.

5
Poopo
6
Cabrera
~a
7
Pazn
8
Urmiri 1
9
Urmiri 3
10
Urmiri 4
11
Malliri
12
Phutina
13
Aguas C.
14
Challapata
15
Castilluma
16
Vichajlope
Cold watersa
17
Quillacas
18
Condo K
19
Caraynacha
20
Llapallapani
21
Challapata
22
Huancane
~a
23
Pazn
24
Cayumalliri
25
Paria
26
Soracachi
27
Cayhuasi

EC (mS/cm)

pH

Eh (mV)

T ( C)

HCO-3 (mg/L)

Cl (mg/L)

SO2
4 (mg/L)

NO-3 (mg/L)

Ca2 (mg/L)

Mg2 (mg/L)

Na (mg/L)

K (mg/L)

E. N. (%)

Water type

2750
2070
3900
30400
19140
17490
10500
6410
6830
5560
3760
22100
1860
75810
4270
5430

8.29
7.49
7.68
7.09
7.24
7.21
6.57
6.59
6.99
7.25
6.33
6.61
6.52
6.82
6.45
6.66

106
153
141
174
166
168
204
203
180
165
196
180
185
168
189
177

75
65
45
40
68
67
58
60
50
55
45
40
58
40
70
65

1892
1038
1141
1033
429
604
684
752
805
671
832
1181
846
1637
1222
1879

204
177
874
9730
5649
5187
2889
1637
1733
1452
808
6939
297
21022
879
1015

40
60
8
106
357
186
63
36
34
39
69
44
18
746
29
68

0.9
0.5
4.4
<0.1
3.8
<0.1
<0.1
<0.1
<0.1
<0.1
2.2
55
6.9
1.4
4.0
2.9

10.4
9.7
26.4
172
77.3
94.1
98.6
79.0
77.0
72.6
42.5
138
46.1
200
46.8
46.7

3.6
2.4
7.4
65.1
38.7
29.3
13.7
12.5
13.2
10.9
20.9
37.7
21.1
196
12.2
11.9

698
546
856
6365
3905
3557
2050
1213
1292
1065
767
4671
339
12866
858
1109

20.8
15.3
24.6
277
166
178
118
86.1
92.3
83.3
17.5
134
14.2
328
68.9
56.9

6.9
5.0
3.1
0.8
2.7
2.0
2.3
0.7
0.6
1.7
0.2
0.0
7.6
3.1
1.6
5.1

NaeHCO3
NaeHCO3eCl
NaeCleHCO3
NaeCl
NaeCl
NaeCl
NaeCl
NaeCleHCO3
NaeCleHCO3
NaeCleHCO3
NaeCleHCO3
NaeCl
NaeHCO3eCl
NaeCl
NaeCleHCO3
NaeHCO3eCl

1200
570
400
210
650
870
1270
640
2120
912
640

7.90
7.55
7.48
6.97
6.84
7.13
7.19
6.70
7.41
7.33
6.70

141
165
168
195
197
185
180
212
173
165
167

12
10
13
14
16
14
13
13
12
15
13

79.1
48.7
30.5
40.1
35.7
46.7
282.6
72.1
242.8
145.4
72.1

1.3
1.3
2.2
3.5
41.9
2.6
1.3
22.9
1.8
7.1
22.9

36.2
43.1
42.9
11.5
55.3
70.1
114.3
64.5
72.5
55.1
64.5

6.7
7.4
6.2
4.3
15.3
13.8
20.5
15.1
58.6
62.3
15.1

16.6
8.9
13.9
6.2
6.5
7.2
23.6
3.0
42.1
6.1
3.0

2.3
3.9
9.6
3.0
10.0
13.0
14.3
1.1
0.7
1.0
4.1

NaeCleHCO3
NaeCaeHCO3
CaeNaeHCO3
NaeCaeSO4eHCO3
CaeNaeMgeHCO3eCl
NaeCaeHCO3eCl
NaeCaeSO4eHCO3
CaeNaeHCO3eSO4
NaeMgeHCO3eCleSO4
MgeCaeNaeHCO3eSO4
MgeNaeCaeHCO3eSO4

234.3
227
172.1
43.9
135.5
292.9
300.2
205.0
717.6
427.1
205.0

<; Below detection level.

a
Selected cold waters from our concurrent studies (Ramos et al., 2012).

189.7
30.4
20.9
7.1
47.0
78.8
72.1
33.9
198.2
19.7
33.9

175.0
51.0
44.4
14.6
44.3
130.5
211.5
35.0
291.5
56.8
35.0

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

15

Fig. 2. Piper diagram showing water types of thermal springs. Arrows in the plot indicate the possible pathway of geochemical evolution by mixing with cold waters.

waters as it occurs in most of the thermal springs around the BA

(Fig. 2). Applying the K/Mg geothermometer on the thermal waters
(Giggenbach, 1988), the estimated equilibrium temperature of the
geothermal reservoir reach 109  C (average); this result is in full
agreement with the studies by Morteani et al. (2014), although lack
of a full chemical equilibrium in the thermal reservoir may cause
the chemical geothermometer to provide uncertain results; hence

the calculated temperature of the reservoir should be used with

caution.
Concentrations of K, Ca2 and Mg2 in thermal waters are
generally low compared to Na. Typical K concentration ranges
from 14.2 to 328 mg/L with an average of 105 mg/L (Fig. 3a). Ca2
and Mg2 are present in the range of 9.7e200 mg/L (average:
77 mg/L) and 2.4e196 mg/L (average: 31 mg/L), respectively

Fig. 3. Box and Whisker plot for the distribution of: (a) major ions and (b) trace elements in thermal waters.

16

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

(Fig. 3a). Main sources of Ca2 and Mg2 are the weathering and/or
dissolution of limestone and dolomite present in large amounts in
the sedimentary geological formations of the study area. PHREEQC
calculated saturation indices (mean values) reveal that water of
most thermal springs are in equilibrium with carbonate minerals,
such as aragonite [CaCO3], calcite [CaCO3] and dolomite
[CaMg(CO3)2]; this suggests that the water chemistry is mainly
controlled by the precipitation/dissolution of carbonate minerals
(Fig. 6).
The thermal waters are low in NO-3; the maximum value of
55 mg/L (Fig. 3a) suggests an anthropogenic contamination of the
sample collected in Phutina (12) (Fig. 1); however, values are
generally low and many samples showed concentrations below the
detection level with an average concentration of 5 mg/L (Table 2).
For SO2
4 , concentrations are relatively high, ranging from 8 to
746 mg/L and average of 119 mg/L (Fig. 3a). The elevated SO2
4
concentrations in hot springs may be derived either from mixing
with shallow groundwater and from the dissolution of gypsum or
oxidative leaching of sulphides.

Fig. 4. Plot of Na/Cl mass ratio versus concentration of Cl. Bivariate plot NaeCl shows
strong correlation (inset upper left).

4.2.2. Trace element composition

Thirteen of the sixteen sampled hot springs used for consumption have As levels higher than the WHO guideline value of
10 mg/L. Concentration of As(Tot) ranged from 7.8 to 65.3 mg/L
(Fig. 3b). Samples for As speciation were separated in the eld using
disposable cartridges and analyzed in the laboratory, arsenite
concentrations ranged from below detection level (5.2 mg/L) to
59.7 mg/L (65%) while arsenate ranged from below detection level

Fig. 5. NaeKeMg triangular diagram (Giggenbach, 1988) showing samples of this study.

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

17

Fig. 6. SI for selected minerals in thermal waters.

(5.2 mg/L) to 47.7 mg/L (35%). As(III) is predominant in eight samples,

three samples have arsenate as predominant species and ve
samples have similar concentrations of As(III) and As(V) (Table 3).
The relatively low SO2
4 concentrations in comparison to those of
HCO-3 and Cl (Fig. 3a) suggest that As(III) is likely the dominant
oxidation state for As in deep geothermal waters. When geothermal
water mixes with water of shallow aquifers, signicant amounts of
As will remain in solution, either as As(V) or As(III). Arsenic species

distribution depends on residence time of the groundwater in the

 pez et al., 2012). In
aquifer and on the kinetics of As(III) oxidation (Lo
general, As concentrations in thermal waters show no correlation
with other parameters (r < 0.2), although there is a trend to link
high As concentrations with NaeCl water type (r 0.59). The
highest concentrations of As are found in mature NaeCl waters that
have been in contact with the rocks for a long period of time,
suggesting that the increase in As concentration is due to a longer

Table 3
Arsenic and trace elements in thermal springs and in cold waters from shallow wells.
#

Location

Hot springs
1
Soracachi
2
Obrajes
3
Capachos
4
Machacam.

5
Poopo
6
Cabrera
~a
7
Pazn
8
Urmiri 1
9
Urmiri 3
10
Urmiri 4
11
Malliri
12
Phutina
13
Aguas C.
14
Challapata
15
Castilluma
16
Vichajlope
Cold watersa
17
Quillacas
18
Condo K
19
Caraynacha
20
Llapallapani
21
Challapata
22
Huancane
~a
23
Pazn
24
Cayumalliri
25
Paria
26
Soracachi
27
Cayhuasi

As(Tot) mg/L
10.7
16.5
32.4
65.3
29.1
20.9
18.3
14.8
8.6
14.4
59.7
32.4
9.7
18.8
7.8
11.6
233.3
229.4
54.8
41.1
17.3
19.6
185.7
<5.6
24.3
6.7
<5.6

As(III) mg/L

As(V) mg/L

10.7
<5.2
9.0
17.6
29.1
14.8
18.3
14.8
8.6
14.4
59.7
17.4
<5.2
11.3
<5.2
11.6

<5.2
16.5
23.3
47.7
<5.2
6.1
<5.2
<5.2
<5.2
<5.2
<5.2
15.0
9.7
7.5
7.8
<5.2

e
e
e
e
e
e
e
e
e
e
e

e
e
e
e
e
e
e
e
e
e
e

Al mg/L
28.6
9.3
9.2
11.9
12.0
22.5
13.6
13.9
30.8
23.6
12.6
11.1
10.7
14.8
16.8
17.0
17.4
16.5
295
16.3
14.5
16.9
19.2
16.3
25.9
14.6
13.9

Ba mg/L

Fe mg/L

Li mg/L

Mn mg/L

Rb mg/L

Si mg/L

Sr mg/L

Zn mg/L

446
264
2588
734
140
290
472
644
807
558
176
1567
788
179
589
341

221
2.0
39
46
414
108
826
471
524
304
778
128
129
144
213
14

6288
5497
6959
<1.8
<1.8
<1.8
<1.8
<1.8
<1.8
9526
2270
<1.8
1797
15439
9666
11561

35
21
52
132
153
232
315
152
144
142
67
151
38
292
167
80

167
150
228
5713
2703
3404
3126
2207
2408
1920
185
2689
413
6092
1696
1320

12966
13570
10125
9513
9700
11025
11730
10127
10164
9721
9156
9664
9739
8336
12225
11235

650
989
1828
4492
1791
2294
2205
1845
2042
1617
703
3571
648
4209
1199
1319

4.0
<1.1
21.4
8.9
5.5
3.5
5.7
16.2
4.5
17.0
16.9
13.1
29.3
17.6
58.8
126

16
12
278
17
9.8
16
32
16
23
8.8
13

1713
230.4
63.4
52.3
48.1
152.1
915.2
41.9
2476
98.7
48.5

1.3
1.3
288
2.8
1.2
7.3
85.6
1.8
73.5
0.6
0.7

e
e
e
e
e
e
e
e
e
e
e

17011
19241
17966
20187
15403
15975
11676
13097
14633
8732
9479

337
427
290
103
322
432
837
346
1229
338
434

21.5
15.2
35.4
6.9
37.2
25.6
11.8
53.1
16.6
35.8
18.0

38.2
34.7
87.3
25.6
51.8
75.3
51.1
45.0
145
37.0
87.6

<; Below detection level.

a
Selected cold waters from our concurrent studies (Ramos et al., 2012), e; not determined.

H3AsO4

0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0.8
1.0
0.2
1.9
1.5
0.2
0.5
1.0
1.9
0
0.4
0
0
0
0
0
0
0
0
0
0.5
0.2
0
0.2
0.3
0.6
0
0.6
0
0.1
0
0
0
0
0
0
0
0
0
0.2
0.3
0
0.2
0.4
0.4
0
0.4
0
0.1
0
0
0
0
0
0
0
0
1.8
8.8
2.7
2.7
7.8
3.6
7.6
1.5
8.8
0
2.3

MgHAsO4
CaHAsO4

0
0
0
0
0
0
0
0
2
3.0
3.5
3.4
7.2
4.6
5.6
1.9
7.2
0
1.9
0
0
0
0
0
0
0
0
21.9
19.9
25.8
60.3
48.0
46.8
43.6
87.0
60.3
0
22.1

Total

0
0
0
0
0
0
0
0
29.2
39.9
46.3
72.1
73.0
100
100
100
100
0
35

0
0
0
0
0
0
0
0
2.6
6.5
13.6
3.7
8.1
44.0
41.6
8.5
44.0
0
8

Eh (mV)
calculated
AsO3
4
CaAsO-4
MgH2AsO
4
MgAsO-4
CaH2AsO
4
H2AsO-4

0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0.3
0.9
0.9
1.3
1.7
3.5
5.6
48.8
3.6
0.6
0.3
1.8
0.5
0
0
0
48.8
0
3.9

0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0

H3AsO3
Total

100
100
100
100
100
100
100
100
70.8
60.1
53.7
27.9
27.0
0
0
0
100
0
65

Sample ID

Malliri
~a
Pazn
Urmiri 1
Vicahjlope
Urmiri 3
Urmiri 4

Poopo
Soracachi
Cabrera
Challapata
Phutina
Capachos
Machacam.
Castilluma
Aguas C.
Obrajes
Max
Min
Mean

99.7
99.1
99.1
98.7
98.3
96.5
94.4
59.2
67.2
59.5
53.4
26.0
26.5
0
0
0
99.7
0
61.1

As(V) (%)

HAsO2
4
HAsO2
3

AsO3
3

residence time and interactions of the water with the wall-rocks

pez et al., 2012). Results of
(Webster and Nordstrom, 2003; Lo
aqueous speciation calculated for thermal waters by PHREEQC
indicate arsenite as the predominant species with H3AsO03 (61.1%)
and H2AsO-3 (3.9%). Arsenate occurs mostly (22.1%) as HASO2
4 and
8.0% as H2AsO-4, but is also present as MgHAsO4 (2.3%), CaHAsO4

(1.9%), MgH2AsO
4 (0.4%), CaH2AsO4 (0.1%), and MgAsO4 (0.1%)
(Table 4). Values of Eh calculated on the basis of As(III)/As(V) redox
couple were consistently lower than Eh values measured in the
eld (Table 4), this suggests a strong redox disequilibrium
frequently observed in natural waters. Compared with cold waters
from shallow aquifer, concentration of As(Tot) ranged from: <5.6 to
233.3 (Ramos et al., 2012) which is much higher than As concentrations in thermal springs (Table 2). Simultaneously, in the shallow
aquifer there is predominance of As(V) species (Ormachea et al.,
2013), suggesting that groundwater dilutes hot waters from
geothermal reservoir. Besides, the range of As concentrations in
geothermal elds is reported to be in several mg/L of total As (Birkle
et al., 2010; Birkle and Merkel, 2000; Ball et al., 1998; Romero et al.,
2003).
Total dissolved iron concentration showed wide variability in
the ranges of 2.0e825.6 mg/L (average 272.6 mg/L) (Fig. 3b). Saturation indices (mean values) calculated by PHREEQC indicates that
samples are supersaturated with respect to Fe-oxide/hydroxide
minerals (Fig. 6), goethite [a-FeOOH] probably will not precipitate
at that ambient temperature and pressure conditions but precipitation of ferrihydrite [Fe(OH)3] would play an important role in the
subsequent attenuation of As in the thermal springs discharge.
Lithium and Si are present in high concentrations, Li from below
detection level (1.8 mg/L) up to 15439 mg/L (average 4300 mg/L) and
Si from 8336 mg/L up to 13570 mg/L (average 10600 mg/L) (Fig. 3b).
Rubidium and Sr are also present in high concentrations, Rb from
150 mg/L up to 6092 mg/L (average 2151 mg/L) and Sr from 650 mg/L
up to 4492 mg/L (average 1963 mg/L) (Fig. 3b). All trace elements in
both, thermal springs and cold water from shallow aquifers
(Table 3) are assumed to occur in high concentrations due to active
volcanic and geothermal sources in the region followed by the
enrichment of the elements by evapoconcentration processes.
Other trace elements Al, Ba, Mn, and Zn are present in relatively low
concentrations and no correlations between them were found
(Fig. 3b).
4.3. Characterization of sediments

H4AsO
3
H2AsO-3
As(III) (%)
Species

Table 4
Arsenic speciation in hot springs calculated by PHREEQC.

e
e
e
e
e
e
e
e
137.1
28.4
3.6
133.3
39.1
e
e
e
3.6
137.1
62.9

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

18

Selected elements of HNO3 digestion in sediments are presented

in Table 5. A wide variability in As concentration is shown; almost
all samples have high As contents from 4 to 123.7 mg/kg (average
23.7 mg/kg). The sample collected near Machacamarca (4) (Fig. 1)
shows the highest As content, but is probably inuenced by the

Table 5
Selected elements from HNO3 digestion in the sediments.
Sample ID

Al mg/Kg

As mg/Kg

Fe mg/Kg

Zn mg/Kg

S mg/Kg

Obrajes
Machacam.
Cabrera
~a
Pazn
Urmiri 1
Urmiri 3
Urmiri 4
Phutina
Aguas C.
Challapata
Castilluma
Vichajlope

5495
1725
4959
4223
5640
8978
5701
3884
9781
3111
6625
5144

7.2
123.7
25.2
4.0
10.4
30.8
6.9
13.3
13.7
31.2
8.5
9.7

17447
8880
39653
10505
67546
39939
11784
7433
31119
73721
22004
6819

38.1
282.1
61.7
20.5
36.1
41.8
28.4
62.0
92.5
35.9
42.1
23.1

904
4098
449
1746
789
7349
1032
1195
349
8097
320
1616

~ oz et al. / Journal of South American Earth Sciences 60 (2015) 10e20

M. Ormachea Mun

mining activity which is located very near to this sampling site

(<500 m). In the other sites, As contents are well correlated with
those of Fe suggesting that As is adsorbed/co-precipitated in Fe(III)
mineral phases. Some other trace elements i. e. S, Al, Zn, have
relatively low concentrations.
5. Conclusions
Thermal springs are characterized by having high salinity (Na, Cl)
and near neutral pH; major ion composition shows Na, Cl and
HCO-3 as predominant ions. Chemically, the thermal waters are of
NaeCl and NaeCleHCO3 types which conrm the inuence of the
geological formations dominated by carbonate and evaporate rocks.
It is assumed that during ascending ow through geologic fractures
thermal waters are diluted by large amount of meteoric water and
locally by groundwater from the shallow aquifers. Our results suggest that deep NaeCl mature waters have highest As concentrations
concomitant with elevated Li and Si. Arsenic in thermal waters is
present mostly as As(III) indicating reducing conditions in the deep
geothermal waters. High As in sediments indicates that after
discharge at ground surface, As(III) is oxidized and natural attenuation of As occurs by the adsorption/co-precipitation on Fe mineral
phases. It is likely that thermal water discharge is not the main
source of high As content in the shallow aquifer waters, as they are
very immature and may only have a small component corresponding to the deep reservoir. More hydrologic investigations have to be
conducted to better explain the mechanisms and processes
responsible for high As occurrence in shallow aquifers.
Acknowledgments
The authors are thankful to KTH International Groundwater
Arsenic Research Group coordinated by PB. MO, PB, OR, JQ and JB
acknowledge the nancial support from Swedish International
Development
Cooperation
Agency
(Sida
Contribution:
wen and B. Nilsson
7500707606). We are thankful to A. Fylkner, M. Lo
at the Division of Land and Water Resources Engineering, Royal
rth at the
Institute of Technology, Stockholm and Carl-Magnus Mo
Department of Geology and Geochemistry, Stockholm University for
the laboratory analyses. We also express gratitude to E. Blanco from
Instituto de Investigaciones Qumicas, Universidad Mayor de San
s and L. Taquichiri from Gobierno Prefectural del DepartaAndre
mento de Oruro for their collaboration during the eld trip.
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