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Departamento de Qumica Analtica, Universidad de Extremadura, Avda. de Elvas, s/n, E-06006 Badajoz, Spain
Departamento de Fsica Aplicada, Avda. de la Universidad s/n, E-10071 Cceres, Spain
Centro de Tecnologas Ambientales, Universidad Tcnica Federico Santa Mara, Av. de Espaa, 1680 Valparaso, Chile
H I G H L I G H T S
a r t i c l e
i n f o
Article history:
Received 7 December 2014
Received in revised form 27 March 2015
Accepted 4 May 2015
Available online 14 May 2015
Editor: D. Barcelo
Keywords:
Soil
Metal
Ecological risk assessment
Industrial pollution
Pollution indexes
a b s t r a c t
The present work investigates soil pollution by elemental contaminants and compares ecological risk indexes related to industrial activities for the case study of Puchuncav-Ventanas: a relevant industrial zone located in central Chile. Selected elements (As, Pb, Cd, Ni, Hg, V, Mn, Zn, Sr, Sb, Cr, Co, Cu, K, and Ba) were analyzed during a
long-term period (yearly sampling campaigns during 20072011), at 5 sampling stations representing different
degrees of impact. PCA and cluster analysis allowed identifying a copper smelter and a coal-red power plant
complex as major pollution sources. Geoaccumulation index (Igeo), enrichment factor (EF), contamination factor
(Cf), contamination degree (Cdeg), and integrated pollution index (IPI) are critically discussed for quantitative
ecological risk assessment. Igeo, EF and Cf indexes are producing comparable environmental information, showing
moderate to high pollution risks in the area that demands further monitoring and adoption of prevention and remediation measures.
Capsule: Long term assessment of elemental pollution around an industrial area. New insight on ecological risk
indexes for trace element pollution in soils, by critical comparison among them.
2015 Elsevier B.V. All rights reserved.
1. Introduction
Among the most signicant soil pollutants, trace elements are relevant due to both acute and long-time toxic effects in the soils and related environmental media (Yaylah-Abanuz, 2011), since soil pollutants
can enter the human body by ingestion, dermal contact, and inhalation,
aside from the food chain pathway starting from plant uptake (MezaMontenegro et al., 2012). The potential ecological risk associated to
soil contamination is a very controversial issue in recent years (MezaMontenegro et al., 2012), so ecological risk assessment aims to provide
Corresponding author.
E-mail address: epinilla@unex.es (E. Pinilla-Gil).
http://dx.doi.org/10.1016/j.scitotenv.2015.05.010
0048-9697/ 2015 Elsevier B.V. All rights reserved.
336
sources, there is a wide set of less impacting industrial factories operating in the area, which are briey described as follows. Puerto Ventanas is
a provider of dock and port facilities. Cementos Meln is a producer of
national construction materials which has three activity areas: cement,
concrete aggregate, and mortars. Catamutn Import, sell coal, and
steam division, which manages industrial systems from steam coal
combustion. Panimex Qumica S.A. produces plastic and fumaric acid.
Gasmar is a company dedicated to marketing of liqueed gas. Minera
Montecarmelo is a plant for treating industrial wastes. Oxiquim is a
maritime terminal. Cordex is a big factory for production of asphalt
and is a fuel terminal also.
Studies about environmental impact of industrial activities on the elemental soil levels in the Puchuncav-Ventanas area are scarce.
Ginocchio (2000) analyzed the effect of copper smelter on grassland
in terms of physicochemical soil characteristics, plant species diversity
and abundance, founding a signicant impact of industrial activities
on plant species regeneration capabilities. De Gregori et al. (2002) carried out the redox speciation of selenium present at ultratrace levels
in rainwater collected at the area. The same group (De Gregori et al.,
2003) conducted a work aimed to the monitoring of copper, arsenic
and antimony levels in agricultural soils impacted and non-impacted
by mining activities, from three regions in Chile including the
Puchuncav-Ventanas industrial area. The high concentrations measured in impacted soils from Puchuncav-Ventanas (300 mg kg1 Cu,
34.5 mg kg1 As and 5.3 mg kg1 Sb) clearly showed the impact produced in this zone by the industrial and mining activities developed in
their proximities. Ginocchio et al. (2004) reported Cu, Zn, Pb and Cd
concentrations (among other parameters) in different soil layers around
the area. The levels found in the 05 cm layer were 361.6 mg kg1 for
Cu, 157.8 mg kg 1 for Zn, 79.9 mg kg 1 for Pb and 0.8 mg kg 1 for
Cd. Copper mobility in soil around the copper smelter was investigated
by Neaman et al. (2009). The same author reported results about the
effectiveness of lime and compost of in situ immobilization of trace elements in soil by using earthworms as bioindicators of toxicity (Neaman
et al., 2009). These previous works in the area focused on a limited numbers of trace elements analyzed after single sampling campaigns. A
more detailed evaluation of trace elements in soils, focused on the
study of their distribution in particle size fractions has been recently
published by Parra et al. (2014). In the present work, we describe the results of a systematic, long-term investigation about ecological risk from
multi-element soil pollution at the Puchuncav-Ventanas area, comprising spatial and temporal variability, source assignment and ecological
risk index calculations.
2. Materials and methods
2.1. Sampling area and soil characteristics
The Puchuncav-Ventanas industrial area is located in a district
(Fig. 1) belonging to the V Region of Chile, Valparaiso Province. The
area is located in the Chilean mainland coast (34 45 S, 71 29 W),
58 km North from Valparaso (Regional Capital Region V), 45 km
North from Via del Mar and 160 km North-West from Santiago de
Chile. It comprises an area of 301 km2, with a population of 13,000.
The main communication ways are the F-30E Road, Highway 5 North
(via Catapilco), and Nogales-Puchuncav way. Specic locations for soil
sampling were selected in the area as depicted in Fig. 1. La Greda (LG)
sampling point (32 44 57 S, 71 28 30 W) is located 1.69 km NE
from the main emission sources in the area, whereas Los Maitenes
(LM) sampling point (32 45 41 S, 71 27 18 W) is located 2.39 km
E. These two locations are expected to be the most impacted points.
Puchuncav village (PU) sampling point (32 43 17 S, 71 24 43
W) is located 8 km NE from the industrial area and Valle Alegre (VA)
sampling sites (32 48 30 S, 71 26 10 W) is 6.72 km SE around the
Certied values
(mg/kg)
Measured concentration
(mg/kg)
Mean recovery
(%)
As*
Cd
Pb*
V
Mn*
Co
Cu*
Zn*
Sr
Ti*
Sb
Ba
0.154 0.010
12.3 0.3
0.552 0.003
82 9
0.214 0.006
5.99 0.14
0.342 0.005
0.418 0.015
255 7
0.311 0.007
52.5 1.6
792 36
0.166 0.039
12.4 3.0
0.563 0.160
78 9
0.229 0.033
6.52 1.52
0.370 0.101
0.492 0.087
221 3
0.353 0.003
44.0 0.4
736 86
90
84
80
103
99
90
86
105
88
114
84
91
337
were obtained from PerkinElmer (Waltham, MA, USA). Working solutions were prepared by dilution with ultrapure water
(resistivity N 12 M) obtained from an Ultramatic system (Wasserlab,
Spain).
Dilute standards and real samples were adjusted to desired pH with
sub-boiled HNO3 (69%) obtained from a quartz sub-boiling system
(Krner, Rosenheim, Germany). 1 g L1 Y(III) and In(III) standards
(Parneac, Spain) were used as internal standards. HClO4 (70%)
Suprapur from Merck and HF (48%) Panreac Hiperpur were used for
sample digestion and pH adjustment. Standard Reference Material
2710a Montana I Soil from the U.S. National Institute of Standards
and Technology (NIST) was used for accuracy testing.
Table 2
Element concentrations in the soil collected at the sampling stations within the Puchuncav-Ventanas industrial area. La Greda (LG), Los Maitenes (LM), Puchuncav village (PU), Valle
Alegre (VA) and reference station at Maitencillo (MA). All results are in mg/kg. n is the number of samples.
Elements
As
Pb
Cd
Ni
Hg
V
Mn
Zn
Sr
Sb
Cr
Co
Cu
K
Ba
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
Maxmin
Mean
LG (n = 26)
LM (n = 26)
VA (n = 21)
PU (n = 25)
MA (n = 21)
93.2622.8
50.84
165.8424.56
84.8
2.830.52
1.34
92.623.62
20.02
3.810.0001
0.77
147.929.77
86.36
721.48181.44
408.13
540.1641.3
232.26
446.31171.33
273.52
9.831.08
4.84
35.2513.23
24.32
11.342.53
7.45
2872.75452.77
1403.19
12769.351603.85
2499.11
464.9357.14
301.88
110.569.56
56.98
210.2716.8
89.06
2.840.45
1.3
85.122.43
16.76
1.380.0001
0.31
160.9443.31
115.43
721.5392.62
497.65
309.6980
157.04
312.22132.86
218.98
15.990.48
6.49
36.7217.61
26.83
11.065.76
7.96
1786.77237.19
771.29
14667.994381.55
9647.39
463.83216.78
339.91
15.168.59
11.64
35.4611.12
19.84
0.560.14
0.24
18.270.04
10.19
0.490.0001
0.08
185.5576.28
135.72
1178.97573.97
772.47
170.3144.73
90.94
216.67119.21
164.53
2.140.54
1.32
36.1418.03
27.2
20.587.78
12.28
173.8250.56
93.35
14109.013754.94
9725.81
429.06280.5
343.36
49.488.7
27.51
94.096.41
45.57
1.460.05
0.55
79.421.54
14.17
1.340.0001
0.2
127.4150.06
97.47
1014.12325.6
569.19
161.9333.28
100.43
218.86142.27
175.97
7.280.39
3.33
50.7616.25
33.38
14.47.04
9.08
629.9140.37
284.07
10814.643512.23
7473.35
464.46218.37
302.09
36.096.63
15.63
85.0316.85
18.93
0.330.17
0.25
13.780.04
10.22
0.050.0001
0.01
170.5794
137.91
864.91576.77
711.06
254.663.11
123.2
301.43222.92
242.25
1.840.68
1.32
42.228.5
34.72
11.268.61
9.58
51.7432.22
42.34
11392.723768.36
8277.52
355.56223.65
266.5
338
Table 3
Trace element concentration (mg/kg) in soil samples from Punchuncav-Ventanas area compared with other case studies of polluted areas around the world, and reference soil quality
standard guidelines.
Copper smelting areas
38.12
62.00qq
0.89
15.56
0.36
107.48
551.04
148.39
210.81
4.14
27.91
9.03
669.37
8539.64
320.91
4.1
29
63
12
76
3.1
15.3
34.4
56.8
1501
12.77
33.79
0.64
26.14
0.01
53.14
384.43
39.95
32.4
21.06
26.7
6.29
89.8
89.2
70.5
59.5
600
22
50
130
360
87
91
2000
Australia (Australian
Department of
Environment and
Conservation, 2010)
Netherlands (Ministry
of Housing, Spatial
Planning and the
Environment, 2000)
20
1500
3
60
50
200
100
300
55
530
12
210
10
720
15
380
240
190
625
Geoaccumulation index (Igeo): It allows the estimation of contamination comparing preindustrial and recent metal concentrations in soils. It was originally proposed by Mller (1969) for
sediments and then modied by Loska et al. (2004) for soil pollution
estimation. It has been widely applied to several trace metal
studies in Europe (Yaylah-Abanuz, 2011).This index is expressed in
Eq. (1):
Igeo log2 Cn =1:5 Bn
where Cn is the measured concentration of element n in the soil sample, and Bn is the geochemical background value of element n in the
upper Earth's crust (Wedepohl, 1995). The constant value 1.5 is included to consider the natural uctuation of the concentration of a
given substance.
Igeo values are categorized in seven groups as follows: practically uncontaminated (Igeo 0); uncontaminated to moderately contaminated (0 b Igeo b 1); moderately contaminated (1 b Igeo b 2);
moderately to heavily contaminated (2 b Igeo b 3); heavily contaminated (3 b Igeo b 4); heavily to extremely contaminated (4 b Igeo b 5)
and extremely contaminated (Igeo N 5).
Enrichment factor (EF): This method is based on the standardization
of an element concentration tested against a reference element
(Yaylah-Abanuz, 2011). Fe, Sc, Ti, Al, Ca, or Mn is generally used as
reference elements for calculation of EF (Quevauviller, 1989). Mn
was selected as a reference element in this study.
Fig. 2. Normalized concentration of trace and major elements during 2007 to 2011 sampling campaigns (refer to text for the normalization protocol used).
339
2
where Cn (sample) is the concentration of element n in the sample,
Cref (sample) is the concentration of the reference element (Mn) in
the sample, Bn (background) is the concentration of element n in
the upper Earth Crust (Wedepohl, 1995), and Bref (background) is
the concentration of the reference element in the earth crust.
Enrichment factor values are grouped in ve categories (Sutherland,
2000): Deciency to minimal enrichment (EF b 2); Moderate enrichment (2 b EF b 5); Signicant enrichment (5 b EF b 20); Very high enrichment (20 b EF b 40) and extremely high enrichment (EF N 40).
Contamination factor (Cf), contamination degree (Cdeg), and integrated pollution index (IPI): these are related indexes. Cf was proposed by Hkanson (1980), as the ratio between the concentration
of selected pollutants (PCBs, Hg, Cd, As, Cu, Cr, Zn, and Pb) in sediment samples and reference preindustrial concentration values. It
has been later adapted to the study of soil pollution by using upper
crust elemental concentrations (Wedepohl, 1995) as reference
values. In our case, PCBs were not measured and for this reason
we've replaced this parameter by Sb. Median lethal dose (LD50) of
Sb (WHO, 2003) is in the same range of PCBs (Euro Chlor, 2002),
so it can be assumed that both of them have a similar eco-toxic effect.
Hkanson (1980) divided the Cf into four categories: Low contamination (Cf b 1); Moderate contamination (1 Cf b 3); Considerable
contamination (3 Cf b 6) and very high contamination (Cf N 6).
Contamination degree (Cdeg) is dened as the sum of the individual
contamination factors in Eq. (4):
Cdeg
Cf
Factor 1
Factor 2
Factor 3
As
Pb
Cd
Ni
Hg
V
Mn
Zn
Sr
Sb
Cr
Co
Cu
K
Ba
% Var
0.946
0.974
0.953
0.061
0.478
0.049
0.465
0.816
0.190
0.934
0.185
0.212
0.903
0.098
0.131
40
0.025
0.001
0.124
0.057
0.199
0.688
0.540
0.034
0.680
0.080
0.803
0.645
0.214
0.053
0.116
22
0.008
0.051
0.085
0.143
0.201
0.427
0.457
0.141
0.012
0.038
0.058
0.568
0.053
0.833
0.852
8
Cdeg is divided into four groups as Cf (Hkanson, 1980): Low contamination (Cdeg b 8); Moderate contamination (8 Cdeg b 16); Considerable contamination (16 Cdeg b 32) and very high contamination
(Cdeg N 32).
The integrated pollution index (IPI) is dened as the average of the
contamination factors computed for each sample (Yaylah-Abanuz,
2011). IPI values are divided in four categories (Wei and Yang,
2010): Low pollution level (IPI 1); Moderate pollution level
(1 b IPI 2); High pollution level (2 b IPI 5) and extremely high
pollution level (IPI N 5).
Table 4
Matrix of loads for the principal component analysis (PCA). Signicant values are in bold.
Elements
340
Table 5
Contamination factors and contamination degrees of metals of soil samples collected within the study area (Low Concentration = LC, Moderate Concentration = MC, Considerable
Concentration = CC, Very High Concentration = VH).
LG
LM
VA
PU
MA
Value
Contamination
Value
Contamination
Value
Contamination
Value
Contamination
Value
Contamination
Cf (As)
Cf (Pb)
Cf (Cd)
Cf (Hg)
Cf (Zn)
Cf (Sb)
Cf (Cr)
Cf (Cu)
Cdeg
25.42
VH
28.49
VH
6.62
VH
13.75
VH
6.02
VH
4.99
CC
5.24
CC
1.38
MC
2.68
CC
0.87
LC
13.12
VH
12.72
VH
2.83
MC
5.39
CC
2.00
MC
14.76
VH
6.24
VH
1.60
MC
4.88
CC
2.38
MC
4.47
CC
3.02
MC
1.82
MC
1.93
MC
1.82
MC
15.62
VH
20.95
VH
5.2
CC
10.75
VH
2.88
MC
0.7
LC
0.77
LC
0.79
LC
0.95
LC
0.73
LC
98.13
VH
53.94
VH
7.82
VH
19.87
VH
3.04
CC
177.2
VH
131.36
VH
28.06
CC
60.2
VH
19.74
CC
less impacted areas of Puchuncav village (PU) and Valle Alegre (VA),
most of the concentrations of the assayed element in the soil are
under the limits established by the aforementioned international soil
quality standards. Only As and V are within the quality standard ranges.
About Cu, the mean value at the PU sampling point exceeds the reference values, showing the long distance impact of the copper smelter
in the dominant wind direction (SW), but the VA values are in the
range of Canadian and Australian standards, reecting that this location
is more isolated from wind transport from the emission sources. The
reference sampling area at Maitencillo (MA) presents similar elemental
soil concentrations with those measured in VA.
Soil concentration of the elements in the study area was then compared with previously reported values found in comparable industrial
areas around the world (Table 3), although direct comparison of the results is complicated due to the disparity of sampling conditions (sample
number and sites) and digestion protocols. In our case, copper smelting
and coal-ring are the two most impacting activities in the area. We
have not found reported results about case studies with these industrial
activities together, so we have compared our results with other studies
with separated industrial activities. E.g. Nkana smelter in Zambia (Ettler
et al., 2011) and Port Kembla smelter, NSW, in Australia (Martley et al.,
2004) are two comparable industrial areas affected by copper smelting
activities. The As mean value in the soils at our study area around
Codelco copper smelter is signicantly higher than those reported
around Nkana and Port Kembla smelters. This effect is observed for
all locations (LG, LM, PU and VA) even MA (Table 2). Higher Pb,
Zn and Cr values are also observed in the soils of our study area compared with the reference smelters, whereas Cu soil level is within reported ranges. About reference coal-red power plants, we have
selected Huainan in China (Tang et al., 2013) and Afsin-Elbistan, in
Turkey (ayr et al., 2012). As, Pb, Hg, V, Mn, Zn and Cu concentration
values at all sampling sites in our study area are higher than reported
values in the reference coal-red power plants areas, whereas Cd, Ni
and Cr values are lower, even at the most affected sampling point at
La Greda (LG).
Our results were then compared with the results of previous soil
monitoring campaigns conducted in the area. We have found similar
mean values of As and Sb soil concentrations (38.12 mg kg 1 and
341
Fig. 8. Integrated pollution index of the sampling locations within the study area. La Greda
(LG), Los Maitenes (LM), Puchuncav village (PU), Valle Alegre (VA) and Maitencillo (MA).
342
concentration results were normalized, by dividing average concentration of each element during a given year by the average concentration
during the whole period (20072011). It's difcult to extract a general
conclusion, about the overall temporal trend about elemental pollution
in the soils of the study area. Most of the environmentally signicant
elements assayed show maximum soil concentration values in 2007
(except Hg that peaks in 2009). Then the values decrease in 2008 to
peak again in 20092010, but reaching lower values than those measured in 2007. The values then decline in 2011 to the minimum values
measured during the studied period. The observed evolution of soil concentrations of elemental pollutants can be related with improved environmental technologies adopted by the industries in recent years,
resulting in less pollutant emission per production unit, combined to
natural soil cleaning processes as wind resuspension and leaching by
rain. Nevertheless, a permanent soil sampling and monitoring scheme
seems essential to follow elemental concentration variability and conrm the observed trends in the medium and long term.
assessment indexes (geoaccumulation index, enrichment factor, contamination factor, contamination degree and integrated pollution
index), has revealed signicant ecological impacts, more intense at locations close to the main pollution sources and under the inuence of
dominant winds but also noticeable at reference background locations
more than 10 km away from the industrial area. A copper renery and
a coal-red power plant complex have been identied as major pollution sources by the statistical analysis. The observed evolution of soil
concentrations of elemental pollutants in the studied period, showing
a decline from 2009 to 2011, can be related to improved environmental
technologies adopted by the industries in recent years. A critical comparison among the ecological risk assessment indexed used showed a
good correlation among them, so they give comparable environmental
information.
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.scitotenv.2015.05.010.
Acknowledgments
This work is supported by the Spanish Agency of International Cooperation for Development (AECID project A1/037813/11) the Spanish
Ministry of Science and Innovation (project CTQ2014-52309-P),
Gobierno de Extremadura and FEDER (GR15087).
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