Applied Geochemistry 108 (2019) 104382

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Applied Geochemistry
journal homepage: www.elsevier.com/locate/apgeochem

Assessment of potential contamination of Paramo soil and downstream T

water supplies in a coal-mining region of Colombia
María Daniela González-Martíneza, Carme Huguetb,∗, Jillian Pearseb, Neil McIntyrec,
Luis Alejandro Camachod
a
Los Andes University, Bogotá, 111711, Colombia
b
Geosciences Department, Los Andes University, Bogotá, 111711, Colombia
c
Sustainable Minerals Institute, The University of Queensland, Brisbane, 4072, Australia
d
Department of Civil and Environmental Engineering, Los Andes University, Bogotá, 111711, Colombia

A R T I C LE I N FO A B S T R A C T

Keywords: Colombia's water supply catchments are under increasing pressure from urban development, industry, mining
Coal mining and agriculture and associated emissions. In particular, the impacts of coal mining on water quality are com-
Environmental impact monly questioned; however, the answers are complicated in regions with multiple types of land use and dis-
Soils charge. Investigation of the degree and reasons for water quality degradation in such regions has been limited.
Paramo
Furthermore, the impacts on soils and the Paramo ecosystems, and their relationship to water quality, are
Water quality
commonly disregarded. Here we present a review of the environmental impacts in the Lenguazaque catchment in
the department of Cundinamarca. Surface water, sediments and soil measurements taken on a transect from
Paramo to the valley were analyzed along with coal mine outlet, urban discharge and agricultural data.
Observed alterations of baseline water quality include a significant decrease in dissolved oxygen concentration
and an increase of electrical conductivity, turbidity, color and total solids concentration. High heavy metals were
also measured, in both water and soil samples. The metal accumulation capacity of soils is effective and reduces
concentrations measured in water. Nonpoint sources include runoff and airborne particles released from coke
production, both difficult to quantify and characterize. Point sources such as agricultural, mining and urban
wastewater discharges are commonly found in the area and their composition has been previously documented.
This study indicates that in order to reduce contamination, illegal and small-scale mining in the area should be
controlled and that further treatment of mine and urban discharges is needed. It also demonstrated the key role
that soils play in the mitigation of metal pollution in rivers emphasizing that those should be included in
Colombian environmental quality legislation.

1. Introduction
Mining makes a significant contribution to local and national
economies in Colombia, holding 1% of global coal reserves (Ministry of
Mines and Energy, 2012). However, the national capacity to assess and
manage the water resource impacts of mining is currently limited due to
a lack of baseline data and suitable hydrological models (McIntyre
et al., 2018). Since the 1950s, coal mining and coking processes have
been practiced in several municipalities of Boyacá and Cundinamarca.
The materials that are extracted in these areas are used both for internal
consumption and for export, and represent an important source of in-
come in the region. Cundinamarca has the largest number of mining
titles in the country and produces 3% of the national coal (Habib,
2017). These titles cover both underground and open-pit mining and
are mainly characterized by being small-scale and low tech (Ardila and
Rodríguez, 1999). The municipalities that produce the largest amount
of coal in Cundinamarca are Cucunubá, Guachetá, Sutatausa and Len-
guazaque (Ministry of Mines and Energy, 2012). A significant portion of
coal extraction is carried out by companies that follow the environ-
mental procedures established by Colombian regulatory agencies
(Ministry of Mines and Energy, 2012). However, 44% of mining sites
operate without an environmental license, mostly artisanal, small scale
or illegal mines (Ministry of Mines and Energy, 2012). Most of these are
small and transient; therefore, they are not mapped and/or monitored
by governmental agencies. Many mining areas are in catchments that
include protected Paramo areas and regionally important hydrological

∗
Corresponding author.
E-mail address: m.huguet@uniandes.edu.co (C. Huguet).

https://doi.org/10.1016/j.apgeochem.2019.104382
Received 14 December 2018; Received in revised form 7 July 2019; Accepted 8 July 2019
Available online 12 July 2019
0883-2927/ © 2019 Elsevier Ltd. All rights reserved.
M.D. González-Martínez, et al.
features.
Contaminants generated by coal mining may reach water sources
through a variety of paths such as lixiviation of soils as particulate
material and the atmosphere as particles and gases (Segura, 2007).
Mine outlets can potentially contaminate water sources through the
introduction of substances added as part of the coal processing and the
exposure of geologically sourced minerals that may alter the original
physical and chemical properties of rivers (Aduvire, 2006).
Contaminant sources can be classified as point or nonpoint and both
types are present in the study area. Point source pollution is limited to a
single identifiable source from which pollutants are discharged. Mine
outlets have been cited as one of the most important sources of water
contamination in Colombia (García et al., 2001). They often have high
suspended solid concentrations and, depending on the coal composi-
tion, also low pH and metals that can be harmful to biological activity
(Aduvire, 2006). A study carried out in six municipalities in Boyacá
reported elevated concentrations of lead, iron, mercury and aluminum
in rivers near coal mining sites when compared to water quality stan-
dards established by Colombian regulation in resolution 2115 of 2007
(Agudelo et al., 2016). High lead concentrations in soils were reported
near coal mining areas in Boyacá when compared with nearby zones
where this activity is not present (Agudelo et al., 2016). In Cundina-
marca department, samples taken by the regional corporation CAR
(Corporación Autónoma Regional de Cundinamarca) have shown that
outlets from coal mines contain high concentrations of total suspended
solids, dissolved solids, oils, sulfates and nitrates, all of which affect
water quality (Tiwary, 2001). Besides the mining activity, point sources
from dumping of untreated urban waste or those related to agricultural
activity cannot be disregarded as they can also have a great impact on
water quality. Nonpoint sources of contamination in the area include
particles released from coke production and runoff from areas where
mining, agriculture and cattle ranching are developed (Viman, Oroian,
& Fleș;eriu, 2010). Water from rainfall containing contaminant particles
eventually saturates the underlying rock and percolates to aquifers, a
water source that could also be potentially affected.
Soils are ecosystems containing a collection of minerals, organic
matter, gases, water and organisms that provide environmental services
and a source of products used by communities (Tatarko, 2009). Soil
management and health affect land productivity, stability and en-
vironmental sustainability (Baxter and Williamson, 2001). While metal
concentrations in soils are not regulated by Colombian laws, their
monitoring is crucial as they are a key component of ecosystems.
Contaminants that infiltrate into soil from point and nonpoint sources
can accumulate and subsequently be liberated and transported to rivers
(Llambí et al., 2012). High concentrations of heavy metals such as zinc
can also interrupt the activity of microorganisms and earthworms, thus
slowing and affecting processes such as the breakdown of organic
matter in soils (Wuana and Okieimen, 2011). Metals also represent a
hazard to population and environments as they can be directly ingested
from the soil or indirectly through food and water (Wuana and
Okieimen, 2011). In extreme cases or over time, processes such as
raindrop impact, tillage and compaction can lead to the breakdown of
soil structure (Baxter and Williamson, 2001). The exposed soil profiles
are vulnerable to wind erosion, water erosion and mass movement
(Baxter and Williamson, 2001), which result in mobilization of metals
to rivers and lagoons. Heavy metals in soils are problematic because
they bioaccumulate, are potentially toxic and do not undergo microbial
or chemical degradation, thus persisting in the environment long after
their introduction (Masters and Ela, 2008). Heavy metals are initially
adsorbed through fast reactions once they enter soil profiles, followed
by slow adsorption and redistribution into different chemical forms
(Wuana and Okieimen, 2011).
Many mining regions in Colombia contain Paramos, which play an
important role in regulating water quality due mainly to their soil type.
Paramos are high mountain ecosystems and are one of the main sources
of fresh water and a complex habitat for endemic plant and animal
2
Applied Geochemistry 108 (2019) 104382
species (Colombian Environment and Sustainable Development
Ministry, 2018). Soils in Paramo have the capacity to accumulate high
volumes of water, help regulate the water cycle and provide freshwater
to cities and municipalities in the region (Instituto Geográfico Agustín
Codazzi, 2010). Soils are dark and permeable with high content of so-
dium and potassium and are mostly covered by abundant vegetation
and moss with high absorption capacity (Ospina, 2003). Paramo soils in
South America are the result of the weathering of exposed rock from the
last glaciations (Pleistocene) when Paramo regions were covered in ice
(Hofstede et al., 2014). Some soils are also formed by younger volcanic
ash, but in all cases, Paramo soils are young, since formation is slow due
to low temperatures (Hofstede et al., 2014). Paramo soils are proficient
in filtering and storing because of their high porosity and saturated
hydraulic conductivity, and high retention of water in partially satu-
rated conditions (Buytaert et al., 2005; Díaz-Granados et al., 2005).
Soils, especially in this ecosystem, can act as filters retaining particles
and contaminants in their less superficial horizons thanks to their tex-
ture. Land use changes in paramo areas may alter the soil's original
properties by causing soil compaction, decrease of moisture retention
and altered chemical properties (Estupiñán et al., 2009). While
common soils can have an average composition of 50% minerals and
organic matter, 25% air and 25% water, Paramo soils are composed of
70% water, 20% minerals and organic matter and 10% air, thus almost
90% of their volume can be porous (Llambí et al., 2012). Paramo soils
are typically acid with pH ranging between 3.9 and 5.4 (Guhl, 1982).
Here we show integrated results of water, river sediments and soil
quality in the agricultural and coal mining municipality of
Lenguazaque, in the department of Cundinamarca (Fig. 1). This is the
first study to examine potential contamination in the area. Health ha-
zards have been identified in other regions associated with both mining
and agricultural activities (Ardila and Rodríguez, 1999). However,
there is a lack of published studies assessing levels of soil and water
contamination in Colombian regions used dually for mining and agri-
culture, particularly in the context of risks to Paramos.
The aim of this paper is to discern the type and extent of con-
tamination and to indicate the likely sources responsible land use ac-
tivities. Specifically, the paper aims to identify the relative importance
of contributions to contamination from coal mining, agriculture and
wastewater discharges. The paper also aims to assess the contamination
levels with respect to existing Colombian water quality regulations to
identify possible impacts on public health and the environment. Finally,
the paper examines the role of Paramo soils in regulating water quality.
2. Materials and methods
2.1. Study area
The study was carried out in the area surrounding the municipality
of Lenguazaque and the Lenguazaque River located in the department
of Cundinamarca, Colombia. The municipality is located inside the
hydrographic basin of the Ubaté – Suárez Rivers in the northeast area of
Cundinamarca (Fig. 1A). The main rivers located in the study area are
the Ubaté, Lenguazaque, Suta and Tibita (Fig. 1B), while important
lagoons in the area include Cucunubá, Suesca and Fúquene. The Fú-
quene lagoon is the biggest among these and marks the end of the
Lenguazaque River. Lenguazaque has the second highest coal produc-
tion of all municipalities in the coal mining region (Ministry of Mines
and Energy, 2012).
The municipality of Lenguazaque includes the Rabanal Paramo
(Fig. 1B). The Paramo has a total area of 17,800 ha, shared by the
municipalities of Villapinzón and Guachetá in Cundinamarca, and the
municipalities of Ventaquemada, Samacá and Ráquira in Boyacá
(Instituto de Investigación de Recursos Biológicos Alexander Van
Humboldt, 2014). The Rabanal Paramo is located between 2,690 and
3,500 m. a.s.l. Average annual temperature in this Paramo ranges be-
tween 8 °C and 10 °C, and annual average precipitation varies from
M.D. González-Martínez, et al. Applied Geochemistry 108 (2019) 104382

Fig. 1. Maps of (A) Colombia, showing the departments of Boyacá and Cundinamarca. The green dot shows the location of the case study basin. (B) Lenguazaque
catchment study area. The blue dots show sites where water and soil samples were collected on the main course of the Lenguazaque River. The red dots indicate
discharges to the river that were sampled. The squares show the two coal mine outlets sampled by Corporación Autónoma Regional de Cundinamarca (CAR) and light
blue triangles represent all sites where CAR water monitoring campaigns were carried out. The main urban areas are shown in orange and water flow of main rivers is
indicated by blue arrows. Km 0 of the sampling campaign is indicated. (For interpretation of the references to color in this figure legend, the reader is referred to the
Web version of this article.)

600 mm to 1,200 mm between measuring stations (IAvH, CAR, CORP- mineral material (Guatame and Sarmiento, 2004; Ardila and Rodríguez,
OBOYACÁ, CORPOCHIVOR, 2008). Water stored in this ecosystem 1999). Coal extracted is mainly bituminous and semi-anthracitic
through lagoons, soil percolation and mosses benefits 300,000 people in (Guatame and Sarmiento, 2004) and is used for both internal con-
the area, provides 92 local aqueducts and is an important source of sumption and export. Most of the coal extracted for local consumption
freshwater for the Garagoa, Suárez, and Moniquirá rivers as well as the is used for heat and power applications and to produce coke (fuel made
Fúquene lagoon (Pérez, 2014). The social and economic aspects of the by heating coal in absence of air; Guatame and Sarmiento, 2004).
municipalities surrounding the Rabanal Paramo rely on the water re-
serves provided by this ecosystem. Even though this Paramo has de-
2.2. Surface water and soil sampling
clared a protected natural reserve in 1992 (Alfaro, 2009), both legal
and illegal coal mines can be found in the area.
In-situ water quality parameters were measured from eight sites in
The precipitation regime in the Lenguazaque River basin is bimodal
the study area, and water samples collected at six of these sites were
with two peak levels of rainfall occurring during March–May and
transported to a laboratory for further analysis. River sediments were
October–November (Unión Temporal Audicon – Ambiotec, 2006). An-
collected at three of these sites and transported for analysis. Soil sam-
nual average precipitation in the basin is 870 mm (Unión Temporal
ples were collected from six further sites, each near a water quality site.
Audicon – Ambiotec, 2006). Considering the hydrologic characteristics
Water quality sites sampled during the first sampling campaign (March
of the area and the extension of flood plains in the basin, deposition of
2017) are W1, W2, W3 and W4 (Table 1), and in the second campaign,
contaminants to soils during peak rainfall periods is likely to be sig-
Wt1, Wt2, Wt3 and Wt4 (Table 1; Fig. 1B). Soil quality sites from the
nificant.
first campaign are referred to as S1 to 4 and from the second campaign
The Lenguazaque river basin is mainly composed by Cretaceous,
(February 2019) as Ss1-4 (Table 1; Fig. 1B). River sediment samples
Tertiary and some Quaternary sedimentary rocks deposited in shallow
were only taken during the second campaign and are Sed1, Sed2 and
marine and transitional environments (Duarte and Monroy, 2012). The
Sed4 (Table 1; Fig. 1B).
coal reserves found in the area are of a thermal, metallurgical and semi-
The sites were selected to determine the variation in quality starting
antractitic type with a high content of inert and variable proportions of
at a relatively natural source (no upstream point sources) and moving

3
M.D. González-Martínez, et al. Applied Geochemistry 108 (2019) 104382

Table 1 solids that were dried at 103–108 °C, total dissolved solids dried at
Samples taken for the present study. Sample code, type and coordinates are 180 °C, and total suspended solids dried at 103–105 °C. Two methods
detailed. were used for determination of metal concentration in water, APHA's
Sample code Type Coordinates metals by plasma emission spectroscopy (method 3120 B) (APHA,
2012) and EPA’S microwave assisted digestion of aqueous samples and
W1 Water 5°22′44″N, 73°38′51″W extracts (method 3015A) (U.S. EPA, 2007).
W2 Water 5°19′43″N, 73°41′51″W
W3 Water 5°19′37″N, 73°41′54″W
W4 Water 5°19′28″N, 73°45′50″W 2.4. Analysis of soil sample and sediment composition
Wt1 Water 5°23′01″N, 73°38′47″W
Wt2 Water 5°19′45″N, 73°42′06″W At the soil sites, around 300 g of soil from the clearly developed
Wt3 Water 5°19′59″N, 73°44′55″W
horizons were collected in sealable bags and taken back for analysis.
Wt4 Water 5°19′28,5″N, 73°46′02″W
Sed1 Sediment 5°23′01″N, 73°38′47″W
From the eight measuring sites (S1–S4, Ss1-Ss4) a total of 18 soil
Sed2 Sediment 5°23′01″N, 73°38′47″W samples were analyzed. Only horizons B and C were sampled at S1 and
Sed4 Sediment 5°19′28,5″N, 73°46′02″W S3; horizon B was sampled at S2; horizons A and B were identified at
S1 Soil 5°22′44″N, 73°38′51″W Ss2 and Ss4; and all horizons A, B and C were sampled at S4, Ss1 and
S2 Soil 5°19′43″N, 73°41′51″W
Ss2 (Fig. 1B). Elemental composition for each of the 18 samples was
S3 Soil 5°19′37″N, 73°41′54″W
S4 Soil 5°19′28″N, 73°45′50″W determined using a handheld XRF (X-ray fluorescence) analyzer spec-
Ss1 Soil 5°23′01″N, 73°38′47″W trometer. Samples were prepared by grinding them into small particles
Ss2 Soil 5°19′45″N, 73°42′06″W using a mortar to homogenize the size of all soil components. The
Ss3 Soil 5°19′59″N, 73°44′55″W
ground sample was placed in a bag, further homogenized and then sub-
Ss4 Soil 5°19′28,5″N, 73°46′02″W
sampled from different points within the container to reduce sampling
error. Approximately 3 g of each sample was put in sampling containers
downstream through municipal wastewater and coal mine outlets. W1 and covered with XRF sample Chemplex thin-film sample support using
was selected on the Mojica stream, which receives water supply directly an exposure time of 90 s. Beforehand, a calibration was done with a
from the Rabanal Paramo and represents pristine water conditions in blank sample containing no soil to ensure that the equipment had no
the area. Similarly, Wt1 was collected from a small stream in the sample contamination. Elemental concentrations for this calibration
Rabanal Paramo. W2, Wt2, Wt3 and W4 are located on the main course were null, ensuring the correct calibration of the equipment. To account
of the Lenguazaque River. Samples from W3 were taken from for XRF analytical error, three measurements of each sample were done
Lenguzaque's wastewater discharge on the Lenguazaque River. This site and a mean value was calculated for each element. The standard de-
includes river water with a range of pollution sources including do- viations were always below the third decimal and hence were not
mestic, coal mines and agricultural runoff. Wt4 was collected from plotted.
another unnamed stream that flows to the Lenguazaque River. The objective of the analysis of soils and sediments in this study was
All soil samples were collected no more than 5 m away from the to identify the presence and amount of metals that may originate from
water collection sites. Locations were revisited and superficial soil human activities. For this purpose, elemental concentrations naturally
profiles near the river were identified. Although all profiles were present in the parent material should be considered. Those base con-
mainly exposed, a shovel was used to remove additional surface ma- centrations are present in horizon C of all exposed profiles. Horizon C
terial and vegetation. Soils were divided into horizons according to concentrations were therefore subtracted from the horizon A and B
differences in color using the Münsell's color chart (Münsell Color concentrations to obtain normalized values. Normalized values can also
(Firm), 1994) and texture following Thien's guide (Thien, 1979). be compared with those of river water and mine outlet samples.
Weathering caused by runoff and heavy rainfall in the area meant that
some superficial horizons were not present at some sites. Collection of 3. Results
soil from horizon B was prioritized since accumulation of contaminants
occurs mainly in this soil horizon (Balasubramanian, 2017). 3.1. Water quality
When possible, sediments from the river were collected. This was
done using a plastic shovel and storing the sediments in sealed plastic 3.1.1. Physicochemical parameters
bags. Apparent color ranged from 40 to 60 Pt/Co. The lowest value was
In addition to the two campaigns conducted within this project, measured at W1 and W2 while the highest was found at W4 (Fig. 2A).
eight water quality monitoring campaigns at six sites on the river were The lowest electrical conductivity was measured at W1 (19 μS/cm)
carried out between 2013 and 2016 by Corporación Autónoma while the peak value was registered at W2 (165 μS/cm; Fig. 2B).
Regional de Cundinamarca (CAR). These sites are labelled as CAR 1–6 A further increase in electrical conductivity is also observed in the
(Fig. 1B). Additionally, in 2016, CAR monitored outlets of two coal CAR data going downstream, from 66.86 μS/cm at CAR1 to 180 μS/cm
mines (M1 and M2 in Fig. 1B). at CAR6 (Fig. 2B; CAR, 2017). In the Lenguazaque River dissolved
oxygen ranges from 4.28 to 7.2 mg/L. The minimum was found at Wt3
and the maximum at W1. This decline is almost linear over the sampled
2.3. Water quality analysis length of river (Fig. 2C). Values that do not follow this trend occur near
downstream of discharges to the river. Decreasing values are also ob-
At each site (W1–W4, Wt1-Wt4) in situ water quality parameters served downstream when considering the CAR data, which changes
were measured using a Hydrolab Quanta multi-probe meter. These from 6.5 mg/L at CAR1 to 2.05 mg/L at CAR6 (Fig. 2C; CAR, 2017). A
parameters included pH, dissolved oxygen, conductivity and tempera- progressive decrease of dissolved oxygen levels from 2013 to 2016 is
ture. Analysis of the samples at sites W1–W4, Wt1 and Wt3 was done also observed (CAR, 2017). The most acidic water was registered at W1
following APHA (American Water Works Association) standard (pH 4.9), turning more neutral at the furthest measuring point on the
methods for each parameter (Rice et al., 2012). This included a visual course of the river at Wt4 (pH 6.84; Fig. 2D). Values of pH reported by
comparison for apparent color (method 2120B) and the nephelometric CAR for the coal mine outlets M1 and M2 are 3.3 and 7.11 respectively.
method for turbidity (method 2130B) (APHA, 2012). Determination of
solids concentration was carried out following standard methods 3.1.2. Presence and concentration of solids
2540 B through F (APHA, 2012), which include settleable solids, total Turbidity increases almost linearly going from 6.31 NTU at W1 to

4
M.D. González-Martínez, et al.
Fig. 2. Physicochemical parameters measured in water samples. (A) Apparent
color in Platinum–Cobalt Scale; (B) Electrical conductivity; (C) Dissolved
oxygen concentration; (D) pH. Blue dots are measurements from the main
course of the Lenguazaque River (W1, W2, Wt2, Wt3, W4), red dots are from
Wt1, W3 and Wt4 (Fig. 1B). Light blue triangles are CAR measurements (CAR1-
CAR6; CAR, 2017, Fig. 1B). The horizontal axis is distance downstream of the
Mojica stream source (Fig. 1B). (For interpretation of the references to color in
this figure legend, the reader is referred to the Web version of this article.)
13.6 NTU at W4 (Fig. 3A). The maximum value was measured at W3
(17.8 NTU) which corresponds to the Lenguazaque urban discharge.
The peak dissolved solid concentration is at W2 (76 mg/L). Values at
W2, W3 and W4 are rather similar relative to the minimum at W1
(20 mg/L; Fig. 3B). Settleable solids show a similar tendency with a
minimum value at W1 (0.1 mg/L) and maximum at W2 (0.3 mg/L;
Fig. 3C).
Suspended solid concentrations in the Lenguazaque river have a
similar tendency to those of turbidity. Values increase from W1 (10 mg/
L) to W4 (14 mg/L) and a peak is observed at W3 (18 mg/L; Fig. 3D).
The reported concentration for M2 (7 mg/L) is below all measurements
from the Lenguazaque river (CAR, 2017). For total solids, the minimum
value is registered at W1 (42 mg/L) while the maximum is found at W3
(110 mg/L; Fig. 3E). This parameter also increases downstream from
86.5 mg/L at CAR2 to 171 mg/L at CAR6 (Fig. 3E; CAR, 2017). Mon-
itoring campaigns from 2013 to 2016 indicated that total solids con-
centration has also increased over time (CAR, 2017).
3.2. Metal presence in surface water and soils
3.2.1. Iron and manganese
The iron concentration in the river exhibits a minimum at W1
(0.52 mg/L) and reaches a maximum at Wt3 (12.6 mg/L; Fig. 4A). Ex-
cept for Wt3, all samples collected from the Lenguazaque River have
lower iron concentrations than those reported at mine outlet M2 by
CAR (2 mg/L; CAR, 2017).
The highest iron concentration in river sediments was measured at
Sed2 (3.26 ppm; Fig. 4B) which is in the middle course of the river
5
Applied Geochemistry 108 (2019) 104382
Fig. 3. Solid parameters measured in water samples. (A) Turbidity measured in
NTU (Nephelometric Turbidity Units); (B) Dissolved solid concentration (mg/
L); (C) Settleable solid concentration (mg/L); (D) Suspended solid concentration
(mg/L); (E) Total solid concentration (mg/L). Blue dots are measurements from
the main course of the Lenguazaque River and red dots are from tributaries.
Light blue triangles are CAR measurements (CAR1CAR6; CAR, 2017, Fig. 1B).
The horizontal axis is distance downstream of the Mojica stream source
(Fig. 1B). (For interpretation of the references to color in this figure legend, the
reader is referred to the Web version of this article.)
segment studied. The minimum was obtained from Sed4 (2.08 ppm;
Fig. 4B). Soils at S4 (Fig. 1B) were naturally high in iron with con-
centrations ranging from 1.01 ppm in horizon B (Fig. 4D) to 10 ppm in
horizon C (Fig. 4E). Soils collected at other sites have lower Fe values.
The peak iron concentration for most of the samples was found in
horizon B, while the minimum was most commonly measured in hor-
izon A.
Manganese in water samples is minimum at W1 (0.03 mg/L) and
maximum at Wt3 (0.244 mg/L; Fig. 4F). All samples are below the peak
value reported by CAR at M2 (0.25 mg/L; CAR, 2017). Manganese
concentration in sediments increases with distance from the source,
with the minimum reported at Sed1 (0.019 ppm) and the peak at Sed4
(0.06 ppm; Fig. 4G). At the soil sites, horizons A and B are below the
detection limit at S4. Soils at Ss2 were high in manganese concentration
ranging from 0.015 ppm at horizon C (Fig. 4J) to 0.03 ppm at horizon A
(Fig. 4H).
3.2.2. Heavy metals: lead and zinc
Lead concentrations in the Lenguazaque river ranged from
0.012 mg/L at W1 to 0.011 mg/L at W4 (Fig. 5A). Both samples col-
lected from the second campaign (Wt1, Wt3) had concentrations below
the detection limit. CAR measurements indicated a Pb concentration of
0.01 mg/L at M2 (CAR, 2017).
When considering river sediments, lead is more concentrated in
M.D. González-Martínez, et al. Applied Geochemistry 108 (2019) 104382

Fig. 4. Iron (A–E) and manganese (F–J) concentrations measured in river water samples (mg/L), in river sediments (ppm) and in soil samples (ppm). Blue bars show
concentrations measured in sediments, green for horizon A, yellow for horizon B and orange for horizon C. Samples with concentrations below detection level are
indicated as < DL. Blue dots are measurements from the main course of the Lenguazaque River and red dots are from tributaries. (For interpretation of the
references to color in this figure legend, the reader is referred to the Web version of this article.)

sample Sed2 (0.002 ppm), less-so in sample Sed1 (0.001, Fig. 5B). Lead
was detected in all the soil samples except for horizon C at Ss2. Horizon
A concentrations range from 0.0013 ppm at Ss2 to 0.0037 ppm at S4
(Fig. 5C). The maximum Pb value for horizon B was in sample S4
(0.0063 ppm), while values in other samples ranged between 0.002 and
0.0027 ppm (Fig. 5D). A progressive increase of Pb concentration in
soils is registered for horizon C, from 0.002 ppm at S1 to 0.0037 ppm at
S4 (Fig. 5E).
A peak in zinc concentration in surface water is reached at Wt3
(0.037 mg/L), while the minimum is at W4 (0.009 mg/L; Fig. 5F). At
site Wt1, zinc was below the detection limit. The zinc concentration
measured by CAR at coal mine outlet M2 was 0.025 mg/L (CAR, 2017).
Similar to lead in sediments, the maximum zinc value was at Sed2
(0.015 ppm) while the minimum was at Sed1 (0.007 ppm; Fig. 5G). The
soil horizon A zinc concentration at S4 was the lowest (0.002 ppm;
Fig. 5H). The horizon B zinc concentration was below detection limit at
S4 and was maximum at S3 (0.016 ppm; Fig. 5I). For horizon C, the
minimum was found at Ss2 (0.0035 ppm), while the maximum was at
S4 (0.011 ppm; Fig. 5J).
4. Discussion
4.1. Potential sources of contamination
The main point sources of contamination identified in Lenguazaque
River are mine outlets and wastewater discharges from urban areas.
Possible nonpoint sources identified are agricultural runoff and parti-
culate material from coke production that is then deposited in water
sources through runoff and percolation. Nonpoint sources are difficult
to quantify and characterize but they could be an important contribu-
tion to the alterations of water and soil quality in this study area.
The observed decrease of dissolved oxygen in the river could ori-
ginate from both point and nonpoint sources. Raw wastewater dis-
charges, coal mine outlets and nonpoint pollution from agriculture have
an important role in the decrease of dissolved oxygen levels in the
Lenguazaque River. Since the dissolved oxygen concentration measured
at mine outlets and downstream of them are low, mine outlets in the
study, seem to alter the pristine Paramo water. However, it is likely that
other land uses are equally or more important at least to dissolved
oxygen and electrical conductivity. Organics and nutrients from urban

6
M.D. González-Martínez, et al. Applied Geochemistry 108 (2019) 104382

Fig. 5. Lead (A–E) and zinc (F–J) concentrations measured in river water samples (mg/L), river sediments (ppm), and in soil samples (ppm). Blue bars show
concentrations measured in sediments, green for horizon A, yellow for horizon B and orange for horizon C. Samples with concentrations below detection level are
indicated as < DL. Blue dots are measurements from the main course of the Lenguazaque River and red dots are from tributaries. (For interpretation of the
references to color in this figure legend, the reader is referred to the Web version of this article.)

wastewater discharges have known effect on the dissolved oxygen
(Vanegas, 2013; Mayorga, 2014). Organic carbon and nutrients from
agricultural runoff are also likely to change the oxygen concentration
(Vanegas, 2013; Mayorga, 2014). The small stream sampled at the
Paramo (Wt1) displays the lowest dissolved oxygen in contrast to the
other Paramo sample, Wt4, which is considered more representative of
pristine Paramo water. This is probably because the Wt1 sample was
taken during dry season with very low water levels. Especially since
there was no evidence of point sources and discharges in the Paramo
area.
Our results indicate that solid concentrations in the Lenguazaque
river are likely to be the result of domestic pollution and agricultural
runoff. Total solid concentrations measured in CAR5 and CAR6 are
mainly attributed to domestic pollution from the near-upstream dis-
charge from Ubaté with some input from the extensive agricultural
activities in the area. Discharges from coal mining should also be
considered since it reportedly increases turbidity and suspended and
total solids close to mining sites (Defensoría del pueblo, 2015). Increase
in solids could also be related to the deposition of particulate emissions
from coking ovens in the area, but as a nonpoint source, a clear link is
difficult to establish.
Iron and manganese concentrations in water samples can originate
from both point and nonpoint sources, specifically mine outlets and
runoff from mining and agricultural sites. The highest iron and man-
ganese concentrations were observed at Wt3 (Fig. 4A; Fig. 4F). This site
is located after the Lenguazaque wastewater discharge but presents also
multiple potential nonpoint sources. The site nearest downstream of the
discharge (W3) has a similar manganese concentration to that of Wt3,
indicating that urban wastewater or nonpoint runoff could be the
source also at this site. The concentration of Fe at W3 is substantially
lower than at Wt2 (downstream of the M1 mine outlet), indicating that
the abnormal Fe concentration is attributable to discharges and runoff
from the mining site even though measurements of these are within
regulated limits. Agriculture may also contribute to higher Fe levels

7
M.D. González-Martínez, et al.
through fertilizers and increased soil erosion.
Lead and zinc concentrations measured in the river are most likely
the result of the point sources from mine outlets and nonpoint from
mining and agricultural activities as well as natural abundance in
source rocks. The sample collected at the wastewater discharge W3 has
lower lead and zinc concentrations than those measured in the river
(Fig. 5A; Fig. 5F). There is a significant increase in zinc concentrations
from W1 to W2 that may be explained by the presence of mine outlets
in the area not reported by CAR, or by nonpoint sources such as agri-
cultural activities. We also observe high metal concentrations in some
of our soil samples. The highest concentrations of heavy metals in
water, sediments and soils in Colombia are found in mining regions
(Sánchez and Corredor, 2015). Lead in water has been reported in areas
where mining is common, such as in Cundinamarca (Reyes et al., 2016)
and Córdoba (Martínez et al., 2017), supporting that this is a possible
source for the levels in this case study. Zinc concentration found at S3 is
mainly influenced by Lenguazaque's wastewater discharge, but there
may be a contribution from mine outlets in the area. Although lead and
zinc contamination has been linked with mining activity in other coal
mining case studies (Wuana and Okieimen, 2011; Reyes et al., 2016;
Martínez et al., 2017), data taken so far from the Lenguazaque is not
sufficient to support this as the only source. Nonpoint sources from
agricultural and coke production runoff (Guerrero and Pineda, 2016)
are likely to have contributed to the observed concentrations in soils.
4.2. Alterations of water quality
We observe a deterioration of surface water quality considering
physicochemical parameters and metal concentrations measured in our
samples and those registered by CAR monitoring campaigns. Water
quality decreased downstream (Fig. 2), and some of the measured
parameters do not meet Colombian standards that protect public health
and ecosystems. For instance, apparent color of samples W1–W4 does
not comply with regulated values for drinking water (15 Pt/Co;
Ministry of Environment, Housing and Land Planning, 2007). Color
changes are commonly caused by the presence of metals such as alu-
minum, copper, iron and manganese and by soil particles (Inamori and
Fujimoto, 2010). Considering the water regime of the area, metals seem
more likely to have a significant role in color and will be discussed later
in this section.
Values of pH in the river water are below acceptable drinking water
standards (pH should be between 6.5 and 9; 15 Pt/Co; Ministry of
Environment, Housing and Land Planning, 2007). The pH measured at
coal mine outlets is within the relevant limits (6–9; Ministry of
Environment and Sustainable Development, 2015) only at M2. While
acidic mine outlets will affect the pH of the river, which could explain
low values downstream of M1, this cannot be the only factor. Paramo
runoff is also acidic, due to the high organic content of the soils, pro-
viding an explanation for the low values observed in the Mojica Stream.
Since the pH increases downstream, we believe that either the value is
compensated by addition of basic materials from dissolution of base
rocks and/or though remediation practices from some of the mining
and coking plants in the area.
Dissolved oxygen is one of the most important water quality para-
meters. Effects of low concentrations include undesirable odors and
coloration that affect further uses and treatments of water (Masters and
Ela, 2008). Dissolved oxygen values decrease downstream with some
stations not meeting the standard for uses like recreation, fishing or
species conservation (Ministry of Agriculture, 1984). This alteration is
likely to be due to the dumping of untreated urban waste and agri-
cultural activities. A similar alteration in dissolved oxygen levels in Rio
Frio, also in Cundinamarca, was attributed to agricultural and in-
dustrial activities (Vanegas, 2013).
In the Lenguazaque River, turbidity, suspended and total solid
concentrations increase downstream. None of the samples meets the
turbidity regulation for drinking water (maximum 2 NTU; Ministry of
8
Applied Geochemistry 108 (2019) 104382
Environment, Housing and Land Planning, 2007). Turbidity is regulated
because it can indicate presence of hazardous chemical and microbial
contaminants (APHA, AWWA & WEF, 2012). Recognized contributors
of turbidity include urban runoff, erosion, agricultural activities, nu-
trient runoff from cropland and organic matter from sewage discharges
(Minnesota Pollution Control Agency, 2008). In Colombia, increases of
turbidity, suspended and total solids have been reported in rivers close
to coal mining activity (Defensoría del pueblo, 2015); however, the
suspended solid concentration measured by CAR at M2 is below the
standard maximum of 30 mg/L for coal mine outlets (Ministry of
Environment and Sustainable Development, 2015).
While concentrations of Fe and Mn do not meet the standard for
drinking water (0.3 mg/L; Ministry of Environment, Housing and Land
Planning, 2007), water from all sites except for Wt3 may be used for
agricultural purposes (maximum 5 mg/L; Ministry of Agriculture,
1984). While concentrations of these metals are high in the parent soil,
their remobilization is associated with low pH usually associated to
mine outlets. For example while Fe reported at M2 is just under the
maximum limit of 2 mg/L (Ministry of Environment and Sustainable
Development, 2015), the outlet presents a reddish coloration associated
with oxidized iron that is not observed in other sections of the river.
The main contaminants previously identified in rivers in
Cundinamarca are pathogens and heavy metals (Mayorga, 2014) in-
cluding mercury, lead, arsenic, zinc and cadmium (Reyes et al., 2016).
Lead and zinc are heavy metals that are toxic or poisonous at low
concentrations and can enter the environment through industrial dis-
charges and mining activities including coal mines where lead and zinc
are present in the coal or the rock affected by the process (Gautam
et al., 2015). Water from the Lenguazaque River can be used for agri-
cultural purposes with current lead and zinc concentrations (Ministry of
Agriculture, 1984); however it should not be consumed without sui-
table treatment since Pb and Zn values are above the drinking water
standard (0.01 mg/L and 0.2 mg/L; Ministry of Environment and
Sustainable Development, 2015). In Colombia, contamination with
both heavy metals has been reported in areas with coal mining (Reyes
et al., 2016; Martínez et al., 2017), soil washout (Feria et al., 2010) as
well as agricultural activities (Durán and Ciabato, 2011) exist.
Concurrence Zn and Cd in rivers may also be accounted for by
fertilizer by-products or mining (Feria et al., 2010).
4.3. The role of sediments and soils in contamination retention and
accumulation
Despite being usually disregarded, soils have been shown to be key
in the assimilation of contaminants (Galán and Romero, 2008). For
each type of soil there is an accumulation limit that can be exceeded
due to alterations of its original physical and chemical characteristics,
after which they become a potential contaminant source (Durán and
Ciabato, 2011). The role of soils is particularly relevant in Cundina-
marca and other metallurgical coal mining departments due to the
potential for airborne contaminants to be deposited and subsequently
transported into the surface water system through percolation, as well
as potential contamination of flood plains during floods.
Factors that may influence the presence and distribution of metals
include soil and groundwater chemistry as well as local transport me-
chanisms (Wuana and Okieimen, 2011). Soil characteristics such as
organic matter, pH, and cation-exchange capacity determine the accu-
mulation of metals (Martínez et al., 2017). Soils are a major sink for
heavy metals produced by anthropogenic activities (Wuana and
Okieimen, 2011), and the mobility of metals increases when water
becomes acidic since there is higher solubility and dissociation rate
(Durán and Ciabato, 2011). In acid soils, metals can rapidly reach toxic
levels and harm plants and their roots, which is concerning considering
the acidity of Paramo soils, and the fact that 85% of Colombian soils
have pH values below 5,5 (Guerrero and Pineda, 2016).
Iron concentrations found in soil layers can affect the quality of
M.D. González-Martínez, et al.
surface water such as rivers and lagoons and groundwater stored in
aquifers through percolation-dissolution. The re-movilization of Fe can
occur as a result of oxidation or decrease in water pH (World Health
Organization, 2003a,b). All Fe concentrations measured in river sedi-
ments and soil horizons are above those of the Lenguazaque River,
except for the abnormal measurement at Wt3. Accumulation occurs in
horizon B for sites S1, Ss1, S2 and S3, which is to be expected
(Balasubramanian, 2017). Iron concentrations in surface water are
higher downstream as horizon B accumulation decreases, supporting
the view that Paramo soil strongly retains metals (Soto, 2006). The
accumulation capacity depends on soil characteristics such as organic
matter content, mineral composition, pH, Eh (oxidation potential),
texture, permeability and microbial activity (Galán and Romero, 2008).
Input form acidic mine outlets could cause the dissolution and mobi-
lization of iron to the Lenguazaque River downstream. Iron con-
centration in sediments reaches a peak Sed2, which is located after the
wastewater discharge but is also in an area where airborne particles and
runoff are a potential concern.
Typically, Fe and Cu concentrations in soils are lower than Mn
concentrations because of the redox sequence (Hiscock, 2005), turning
iron into its predominant form as an oxide which has higher mobility
while Mn tends to be accumulated (World Health Organization,
2003a,b). However, Mn concentrations are low in the C horizons
measured thus holding little potential for contamination in our case.
Lead concentrations at S4 show accumulation in horizons A
(0.008 ppm) and B (0.003 ppm) after subtracting parental material
values from horizon C, consistent with preferential Pb usually occurring
in the most superficial soil horizons (World Health Organization,
2011a,b). Since Pb is associated with public health risks and it may
reach water through runoff, accumulation in those horizons is key for
keeping rivers uncontaminated. W4 had the lowest lead concentration
of all samples in the river, which is consistent with the accumulation
occurring at S4, indicating this is the only site where lead is accumu-
lated in soils. No accumulation is present in other samples, indicating
soils in the area are not effectively retaining Pb and this heavy metal is
mostly found in surface water at the study area. Accumulation of zinc
occurs at horizon B in S3, which matches the lowest concentration
measured in water at W3. Presence of this heavy metal can interrupt the
activity of microorganisms and earthworms, thus slowing the break-
down of organic matter in soils (Wuana and Okieimen, 2011).
Thus, we observe that lead and zinc accumulation in soils corre-
sponds with low concentrations measured in water, indicating the im-
portance of soil in the retention of metals and therefore the preservation
of water quality. In agreement with the soils acting as protective barrier
filtering, decomposing, neutralizing or stocking polluting substances
before reaching other mediums (hydrologic and biologic) (Galán and
Romero, 2008).
5. Conclusions
We observed that the water quality of the Lenguazaque River is
affected by point and nonpoint sources. Color, electrical conductivity,
turbidity, suspended and total solid concentration increase down-
stream. Dissolved oxygen concentration decreases with distance
downstream. Iron, manganese, lead and zinc concentrations show that
for some monitoring points water quality is deficient. Some of the
parameters measured in the area do not meet Colombian standards for
drinking water and recreational uses, limiting the use of the
Lenguazaque River water to agricultural purposes.
Coal mining is a common practice in the area that could be linked to
the degradation of quality of the Lenguazaque River and soils in the
area. Other point sources such as urban wastewater discharges and
nonpoint sources from coke production and agricultural development
could also result in the alteration of the physicochemical parameters of
both water and soils. Microorganisms that control important degrada-
tion processes in soils could also be harmed if physical and chemical
9
Applied Geochemistry 108 (2019) 104382
properties of soils are further degraded. Control of small scale and il-
legal mining in the area is necessary, with suitable treatment of mine
and other wastewater discharges being a priority.
Whenever metal accumulation occurs in soils, concentrations of that
metal in the Lenguazaque River decrease. Soils which are currently
accumulating metals could potentially become a contaminant source if
their retaining capacity is reached. Therefore, regulations for metal
concentration in soils in Colombia should be established since they
have an important role in contaminant mobility, environmental sus-
tainability, and productivity and provide multiple services to commu-
nities.
Conflict of interest statement
The authors declare that there is no conflict of interest.
Acknowledgements
This project was financed by FAPA project PR. 3.2015.2423 to CH.
Partial funding was also obtained from FAPA PR.3.2014.1641 to JP.
Thanks is given to CAR (Corporación Autónoma Regional de
Cundinamarca) for sharing their data with us. The authors would like to
thank Dr. I.F Blanco-Quintero and anonymous reviewer for helping us
improve the present manuscript.
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