Ecological Indicators 48 (2015) 282–291

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Ecological Indicators
journal homepage: www.elsevier.com/locate/ecolind

Heavy metal pollution in surface water and sediment: A preliminary

assessment of an urban river in a developing country
Md Saiful Islam a,b,∗ , Md Kawser Ahmed c , Mohammad Raknuzzaman b,d ,
Md Habibullah -Al- Mamun b,d , Muhammad Kamrul Islam e
a
Department of Soil Science, Patuakhali Science and Technology University, Dumki, Patuakhali 8602, Bangladesh
b
Graduate School of Environment and Information Sciences, Yokohama National University, 79-7 Tokiwadai, Hodogaya-ku, Yokohama, Japan
c
Department of Oceanography, University of Dhaka, Dhaka 1000, Bangladesh
d
Department of Fisheries, University of Dhaka, Dhaka 1000, Bangladesh
e
Department of Horticulture, Gyeongsang National University, Jinju, South Korea

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

Article history: The concentration and chemical fractionation of globally alarming six heavy metals (Cr, Ni, Cu, As, Cd and
Received 28 April 2014 Pb) were measured in surface water and sediment of an urban river in Bangladesh. The decreasing trend
Received in revised form 11 August 2014 of metals were observed in water as Cr > Cu > As > Ni > Pb > Cd and in sediment as Cr > Ni > Cu > Pb > As > Cd.
Accepted 14 August 2014
The level of studied metals exceeded the safe limits of drinking water, indicated that water from this river
is not safe for drinking and/or cooking purposes. However, the investigated metals showed low mobility
Keywords:
except for Cd and Pb which could pose a severe threat to the aquatic environment. Contamination factor
Heavy metal
(CF) and geoaccumulation index (Igeo ) demonstrated that most of the sediment samples were moderately
River
Water
to heavily contaminated by Cr, As, Cd and Pb. The pollution load index (PLI) values were above one (>1)
Sediment indicates progressive deterioration of the sediment quality. The extent of pollution by heavy metals in the
Chemical fractionation river Korotoa implies that the condition is much frightening to the biota and inhabitants in the vicinity
of the river as well.
© 2014 Elsevier Ltd. All rights reserved.

1. Introduction The behavior of metals in the natural water is a function of the

In recent years, metal contamination in the aquatic environment
has attracted global attention owing to its environmental toxicity,
abundance and persistence (Sin et al., 2001; Armitage et al., 2007;
Yuan et al., 2011). Large quantities of hazardous chemicals espe-
cially heavy metals have been released into rivers worldwide due
to global rapid population growth and intensive domestic activ-
ities, as well as expanding industrial and agricultural production
(Srebotnjak et al., 2012; Su et al., 2013; Islam et al., 2014). Rivers in
urban areas have also been associated with water quality problems
because of the practice of discharging of untreated domestic and
industrial waste into the water bodies which leads to the increase
in the level of metals in river water (Khadse et al., 2008; Venugopal
et al., 2009).
∗ Corresponding author at: Department of Soil Science, Patuakhali Science and
Technology University, Dumki, Patuakhali 8602, Bangladesh.
Tel.: +880 818043822325, +880 1776062623.
E-mail addresses: msaifulpstu@yahoo.com, islam-md.saiful-nj@ynu.jp
(M.S. Islam).
substrate sediment composition, the suspended sediment compo-
sition, and the water chemistry (Mohiuddin et al., 2012). During
transport, heavy metals may undergo numerous changes in their
speciation due to dissolution, precipitation, sorption, and com-
plexation phenomena (Dassenakis et al., 1998; Akcay et al., 2003;
Abdel-Ghani and Elchaghaby, 2007), which affect their behavior
and bioavailability (Nicolau et al., 2006; Nouri et al., 2011). Sedi-
ment is an integral and dynamic part of the river basin, with the
variety of habitats and environments. However, information on
total metal concentrations is not sufficient for the assessment of
environmental impact of sediment contamination which lead to
the particular interest of chemical fractionation of sediment (Jain,
2004; Nwuche and Ugoji, 2010). The overall behavior of heavy
metals in the aquatic environment is strongly influenced by the
association of metals with various geochemical phases in sediments
(Morillo et al., 2004). Geochemical speciation and distribution of
metals in the defined chemical fraction also been used in predicting
the potential contamination, mobility and bioavailability (Kabala
and Singh, 2001; Pueyo et al., 2003; Caeiro et al., 2005). Thus, it is
important to assess the concentrations and distribution of heavy
metals in the riverine ecosystem.

http://dx.doi.org/10.1016/j.ecolind.2014.08.016
1470-160X/© 2014 Elsevier Ltd. All rights reserved.
 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291
In Bangladesh, everyday a huge amount of untreated industrial
wastes is being discharged into open water bodies and its adja-
cent lands. Besides, a considerable amount of heavy metal enriched
suspended solids is coming down from neighboring country like
India through the Teesta and the Brahmaputra Rivers. Bogra dis-
trict, known as the northern capital of Bangladesh is situated on
the bank of the river Korotoa which is connected to the river Teesta
and Brahmaputra. The study river recently has been raised atten-
tion to public concern due to its extreme pollution. To date, no
scientific research regarding heavy metal issues in the study area
has been conducted so far. Therefore, the objectives of this study
are – to assess the pollution status of the river Korotoa by esti-
mating the levels of heavy metals in water and sediment, and to
observe the metal enrichment in relation to chemical speciation in
sediments.
2. Materials and methods
2.1. Description of the study area
This study focused on an important urban river located at the
northern part in Bangladesh. The study river is originated from
the Himalayas, the mother of numerous rivers. Originating from
northern frontier of Bhutan, the Korotoa enters Bangladesh terri-
tory through Darjeeling and Jalpaiguri districts of West Bengal in
India, and forms for some distance the boundary between Dina-
jpur and Rangpur districts, Bangladesh. For the present study, the
river was selected that flows through the Bogra district urbanized
area. The area of Bogra district about 71.56 km2 , total population
of this district is about 350,397. The study area is located at the
northern part of Bangladesh and situated between 24◦ 84 91.82 N
and 89◦ 37 29.57 E. Thousands of villages, towns and commer-
cial places like Shibganj, Mohasthangarh, Bogra and Sherpur have
been built on both sides of the Korotoa along its 200-km path.
Mohasthangarh, the capital of ancient Pundranagar, is still there
beside the Korotoa as a witness of history in Bangladesh. Agricul-
ture, aquaculture and fishing are the primary activities of the people
living besides this river. This river receives domestic raw sewage,
household waste, and industrial waste from surrounding habita-
tion. During the last decades, natural and human activities have
caused a complete deterioration of the river ecosystems.
2.2. Sample collection and preparation
A total of 80 samples (water and sediment) were collected
during February–September, 2013 (winter and summer season).
Samples were collected from ten different stations (S1–S10) from
upstream to downstream of the river (Fig. 1). Unfiltered water sam-
ples were collected from the center of the river for total metal anal-
yses. The samples were then transferred into acid cleaned 100 mL
polypropylene bottles. One mL of ultrapure nitric acid was added in
each polypropylene bottle to achieve a pH of ∼1 (Cenci and Martin,
2004). At each point, composite sediment samples were collected
using standard protocol (US EPA, 2001). The river bed sediment
samples were taken at a depth of 0 to 5 cm using a portable Ekman
grab sampler. Three composite samples of mass approximately
200 g were collected at each station. The upper 2 cm of each sam-
ple was taken from the center of the catcher with an acid-washed
plastic spatula to avoid any contamination from the metallic parts
of the sampler. For considering the preindustrial sample, sediment
was taken by means of a percussion hammer corer (50–80 cm in
length) for metal analysis (Schottler and Engstrom, 2006). Sediment
sampling was performed as prescribed in the Methods Manual for
the characterization of sediments (Environment Canada and MENV,
1992). Lead-210 dating by alpha spectrometry method was used to
283
determine the age and sediment accumulation rates. Composite
sediment samples were collected into polyethylene air tight bags
in the field and transported to the central laboratory of Patuakhali
Science and Technology University, Bangladesh, for pre-treatment.
The samples were dried in oven at 45 ◦ C for 48 h to gain con-
stant weight. The dried samples were then ground using mortar
and pestle and sieved through 106 ␮m aperture. The lower particle
size fraction was homogenized by grinding in an agate mortar and
stored in labeled glass bottles until chemical analyses were carried
out.
2.3. Sample digestion and metal extraction
All chemicals were analytical grade reagents and Milli-Q (Elix
UV5 and MilliQ, Millipore, USA) water was used for solution
preparation. The Teflon vessel and polypropylene containers were
cleaned, soaked in 5% HNO3 for more than 24 h, then rinsed with
Milli-Q water and dried. For metal analysis, 20 mL water sam-
ple and 0.5 g of sediment sample was treated with 5 mL 69%
HNO3 acid and 2 mL 30% H2 O2 in a closed Teflon vessel and was
digested in a Microwave Digestion System. The digested solution
was then filtered by using syringe filter (DISMIC® – 25HP PTFE, pore
size = 0.45 ␮m) Toyo Roshi Kaisha, Ltd., Japan and stored in 50 mL
polypropylene tubes (Nalgene, New York). Afterwards, the vessels
were cleaned by Milli-Q water and dried with air.
For chemical partitioning of metals, sediment samples were
analyzed using Tessier sequential chemical extraction proce-
dure (Tessier et al., 1979). The sequential extraction procedure
was divided into five operationally defined chemical fractions:
(F1) the exchangeable fraction: readily soluble and exchange-
able; (F2) the carbonate bound and specifically adsorbed fraction:
carbonate-bound, specifically adsorbed and weak organic and inor-
ganic complexes; (F3) the Fe-Mn oxides fraction: bound to iron
and manganese oxides (Fe-Mn oxides); (F4) the organic/sulphide
fraction: bound to stable organic and/or sulphide (organic) com-
plexes; and (F5) the residual fraction: held in primary and
secondary minerals within their crystal structure. The detailed
geochemical fractionation procedure of sediment is presented in
Table 1.
2.4. Instrumental analysis and quality assurance
For heavy metals, samples were analyzed by using inductively
coupled plasma mass spectrometry (ICP-MS). ICP-MS operating
conditions and parameters for metal analysis in samples are
presented in Table S1. Multi-element Standard XSTC-13 (Spex
CertiPrep® , USA) solutions was used to prepare calibration curve.
The calibration curves with R2 > 0.999 were accepted for concen-
tration calculation. Multielement solution (Agilent Technologies,
USA) 1.0 ␮g/L was used as tuning solution covering a wide range
of masses of elements. All test batches were evaluated using
an internal quality approach and validated if they satisfied the
defined internal quality controls (IQCs). For each experiment, a
run included blank, certified reference materials (CRM) and sam-
ples were analyzed in duplicate to eliminate any batch-specific
error. Before starting the analysis sequence, relative standard
deviation (RSD, <5%) was checked by using tuning solution pur-
chased from the Agilent Technologies. Quality control of laboratory
methods involved the analysis of the following reference mate-
rials: NMIJ CRM 7303 – Lake Sediment. The measured mean and
standard deviation of elemental values for reference materials
reported in Table S2. Comparison is made with the certified values,
which in both cases confirmed that the sample preparation and
instrumentation conditions provided good levels of accuracy and
precision.
284 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291

Fig. 1. Map of the study area of Korotoa River of Bogra district urban area, Bangladesh.

Table 1
Geochemical fractionation procedure of heavy metals in sediment of the present study.

Fraction Procedure

Fraction 1 (exchangeable)
Fraction 2 (bound to carbonates)
Fraction 3 (reducible)
Fraction 4 (oxidizable)
Fraction 5 (residual)
Sample extracted at room temperature for 1 h with 7.5 mL of 0.05 M ammonium acetate with continuous agitation.
Residue from fraction 1 extracted with 10.0 mL of 0.17 M acetic acid (pH, 7.0) for 5 h with continuous agitation.
Residue from fraction 2 extracted with 20.0 mL of hydroxyl ammonium chloride in 25% (v/v) acetic acid (pH, 5.0), at 96 ± 3 ◦ C
with occasional agitation for 5 h.
Residue from fraction 3 extracted with 5.0 mL of 0.02 M nitric acid and 5.0 mL of 3% hydrogen peroxide at 85 ± 2 ◦ C for 2 h with
occasional agitation. Followed by the addition of 6.0 mL of hydrogen peroxide as above for 3 h. After cooling, 5.0 mL of 3.2 M
ammonium acetate in 20% (v/v) nitric acid with continuous agitation for 30 min.
Residue from 4 extracted with a hydrofluoric/nitric acid (1:1, v/v) mixture and digest under pressure and temperature in
closed vessel.

After each extraction, samples were centrifuged, liquid-fraction-decanted and 3× 10.0 mL of Milli-Q water was added to the residue (sample-centrifuged and water-removed)
before proceeding with the next extraction.

2.5. Analytical methods for chemical parameters 2.6. Metal assessment in sediment

The pH of sediments was measured in 1:2.5 sediment to water
ratio. The suspension was allowed to stand overnight prior to pH
determination. The pH was measured using a pH meter with the
calibration of pH 4, pH 7 and pH 9 standards. For EC determination,
5.0 g of sediment was taken in 50 mL polypropylene tubes. Then,
30 mL of distilled water was added to the tube. The lid was closed
properly and was shaken for 5 min. After that, EC was measured
using an EC meter (Horiba D-52). Percent N and C of sediment was
measured using elemental analyzer (model type: vario EL III, Elen-
emtar, Germany). For N and C determination, sediment samples
were weighed in tin or silver vessels and loaded in the integrated
carousel. In a fully automatic process, the transfer of the sample
through the ball valve into the combustion tube was performed.
Each sample was individually flushed with carrier gas to remove
atmospheric nitrogen, resulting in a zero blank sampling process.
The catalytic combustion was carried out at a permanent tempera-
ture of up to 1200 ◦ C. The element concentration from the detector
signal, and the sample weight on the basis of stored calibration
curves were measured.
In the interpretation of geochemical data, choice of background
values plays an important role. Several researchers have used the
average shale values or the average crustal abundance data as refer-
ence baselines (Loska and Danuta, 2003; Olivares-Rieumont et al.,
2005; Singh et al., 2005). The degree of contamination from heavy
metals could be assessed by determining the contamination fac-
tor (CF), pollution load index (PLI), geoaccumulation index (Igeo )
and enrichment factor (EF). In the present study, pollutant indi-
cators were calculated based on the values of heavy metals from
pre-industrial sediment of the study area.
2.6.1. Pollution load index (PLI) and contamination factor (CF)
To assess the sediment quality, an integrated approach of pollu-
tion load index of the six metals is calculated according to Suresh
et al. (2011). The PLI is defined as the nth root of the multiplications
of the contamination factor of metals (CF).
PLI = (CF1 × CF2 × CF3 × . . . × CFn )1/n (1)
 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291 285

where CFmetals is the ratio between the content of each metal
to the background values (background value from the pre-
industrial samples of the study area in Bangladesh) in sediment,
CFmetals = Cmetal /Cbackground . Therefore, PLI value of zero indicates
perfection, a value of one indicates the presence of only baseline
level of pollutants and values above one would indicate progres-
sive deterioration of the site and estuarine quality (Tomilson et al.,
1980). The PLI gave an assessment of the overall toxicity status of
the sample and also it is a result of the contribution of the six metals.
The ratio of the measured concentration to natural abundance of a
given metal had been proposed as the index contamination factor
(CF) being classified into four grades for monitoring the pollution
of one single metal over a period of time (Turekian and Wedepohl,
1961; Loska et al., 1997): low degree (CF < 1), moderate degree
(1 ≤ CF < 3), considerable degree (3 ≤ CF < 6), and very high degree
(CF ≥ 6). Thus the CF values can monitor the enrichment of one
given metal in sediments over a period of time.
2.6.2. Geoaccumulation index (Igeo )
The degree of contamination from the trace metals could be
assessed by determining the geoaccumulation index (Igeo ). The
index of geoaccumulation (Igeo ) has been widely applied to the
assessment of soil and sediment contamination (Santos Bermejo
et al., 2003). In order to characterize the level of pollution in the sed-
iment, geoaccumulation index (Igeo ) values were calculated using
the equation,
 C 
n
Igeo = Log2
1.5Bn
where Cn is the measured concentration of metal n in the sedi-
ment and Bn is the geochemical background value of element n in
the background sample (Rudnick and Gao, 2003; Yu et al., 2011;
Rahman and Ishiga, 2012; Islam et al., 2014). The factor 1.5 is
introduced to minimize the possible variations in the background
values which may be attributed to lithogenic effects. Geoaccumu-
lation index (Igeo ) values were interpreted as: Igeo ≤ 0 – practically
uncontaminated; 0 ≤ Igeo ≤ 1 – uncontaminated to moderately con-
taminated; 1 ≤ Igeo ≤ 2 – moderately contaminated; 2 ≤ Igeo ≤ 3 –
moderately to heavily contaminated; 3 ≤ Igeo ≤ 4 – heavily contam-
inated; 4 ≤ Igeo ≤ 5 – heavily to extremely contaminated; and 5 < Igeo
– extremely contaminated.
2.6.3. Enrichment factor (EF)
Enrichment factor (EF) is considered as an effective tool to
evaluate the magnitude of contaminants in the environment
(Franco-Uria et al., 2009). The EF for each element was calculated
to evaluate anthropogenic influences on heavy metals in sediments
using the following formula (Selvaraj et al., 2004):
(CM /CAl )sample
EF = (3)
(CM /CAl )background
where (CM /CAl )sample is the ratio of concentration of heavy metal
(CM ) to that of aluminum (CAl ) in the sediment sample, and
(CM /CAl )UCC is the same reference ratio in the background sample.
Generally, an EF value of about 1 suggests that a given metal may
be entirely from crustal materials or natural weathering processes
(Zhang and Liu, 2002). Samples having enrichment factor >1.5 was
considered indicative of human influence and (arbitrarily) an EF
of 1.5–3, 3–5, 5–10 and >10 is considered the evidence of minor,
moderate, severe, and very severe modification (Birch and Olmos,
2008).
2.6.4. Statistical analysis
The data were statistically analyzed using the statistical
package, SPSS 16.0 (SPSS, USA). The means and standard deviations
of the metal concentrations in water and sediments were calcu-
lated. The median, 5th and 95th percentile values were also calcu-
lated. Other calculations were performed by Microsoft Excel 2010.
3. Results and discussion
3.1. Metal concentration in water
(2)
The results of heavy metal concentrations in surface waters
of the river Korotoa are shown in Table 2 revealed a significant
variation (p < 0.05) among the sites. The average concentra-
tion of studied metals in water followed a decreasing order of
Cr > Cu > As > Ni > Pb > Cd. The mean concentration of Cr in water
was observed 83 and 73 ␮g/L during winter and summer sea-
son, respectively which was much higher than the WHO standard
level for drinking water (5 ␮g/L). The average concentration of Cu
was observed 73 and 161 ␮g/L during winter and summer season,
respectively. Interestingly the highest value of Cu was observed
at S8 site (119 ␮g/L in winter) which might be attributed to the
domestic sewage and runoff from extensively farmed areas (Koukal
et al., 2004; Wu et al., 2008; Islam et al., 2014). Arsenic forms a
variety of inorganic and organic compounds of different toxicity
reflecting the physicochemical properties of arsenic at different
valencies. The average concentration of As was higher in win-
ter (46 ␮g/L) than that in summer (37 ␮g/L) which exceeded the
WHO standard (10 ␮g/L). In river water, considerable amount of

Table 2
Heavy metal concentration (␮g/L) in water sample of Korotoa River of the present study and maximum permitted concentration in water (␮g/L).

Sites Cr Ni Cu As Cd Pb

Winter Summer Winter Summer Winter Summer Winter Summer Winter Summer Winter Summer

S1 87 71 13 9.3 47 41 21 16 1.0 1.0 11 9

S2 63 52 14 10 31 23 25 17 1.0 0.9 11 8
S3 53 41 33 27 44 42 24 19 4.0 3.0 20 15
S4 66 62 15 13 49 40 15 10 5.0 4.0 21 16
S5 43 33 43 37 40 33 25 21 10 8 33 23
S6 112 103 66 52 109 96 63 48 20 15 64 52
S7 107 103 23 18 92 80 60 46 15 10 49 40
S8 92 81 53 44 119 90 54 42 22 18 33 28
S9 77 72 63 56 93 73 78 73 15 11 50 39
S10 126 110 71 55 102 90 92 77 22 15 54 42
Average ± SD 83 ± 27 73 ± 27 39 ± 23 32 ± 19 73 ± 33 61 ± 28 46 ± 27 37 ± 24 11 ± 8 8±6 35 ± 19 27 ± 15

DWSBa 50 100 1000 50 5 50

TRVb 11 52 9 150 2 3
WHO (2004) 5 70 2000 10 3 10
a
Drinking water standard for Bangladesh proposed through ECR (Department of Environment, Government of the People’s Republic of Bangladesh, DoE, 1997).
b
TRV (toxicity reference value) for fresh water proposed by USEPA (1999).
286 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291

Table 3
Seasonal variation of the chemical properties in sediment of Korotoa River of Bogra district, Bangladesh.

Sites pH EC (Ms/m) %N %C C/N ratio

Winter Summer Winter Summer Winter Summer Winter Summer Winter Summer

S1 5.12 5.62 25.5 34.4 0.181 0.31 1.18 1.82 6.52 5.85
S2 5.91 6.12 29.8 15.4 0.177 0.19 1.79 1.51 10.11 7.86
S3 6.62 5.62 23.8 29.5 0.155 0.12 1.13 1.22 7.29 9.92
S4 6.93 6.88 42.8 25.7 0.172 0.21 1.21 1.55 7.03 7.31
S5 6.13 6.52 27.5 23.3 0.114 0.24 0.74 1.22 6.49 5.04
S6 6.17 5.68 42.5 24.3 0.216 0.21 2.01 1.51 9.31 7.37
S7 5.43 6.94 19.7 16.2 0.113 0.12 1.84 1.59 16.28 13.03
S8 6.88 7.91 26.7 20.4 0.112 0.22 0.89 1.11 7.95 5.02
S9 7.72 7.15 33.2 29.5 0.155 0.11 1.69 0.98 10.90 8.99
S10 8.31 6.97 22.9 17.8 0.252 0.18 2.45 1.32 9.72 7.46

Mean ± SD 6.52 ± 0.99 6.54 ± 0.77 29.4 ± 7.89 23.7 ± 6.30 0.165 ± 0.046 0.191 ± 0.062 1.49 ± 0.54 1.38 ± 0.26 9.16 ± 2.96 7.79 ± 2.43

Note: SD, standard deviation.

Table 4
Heavy metal concentrations (mg/kg dw) in sediment of Korotoa River of Bogra district, Bangladesh (n = 3).

Sites Cr Ni Cu As Cd Pb

Winter Summer Winter Summer Winter Summer Winter Summer Winter Summer Winter Summer

S1 86 67 57 48 49 35 5.4 2.6 0.79 0.26 50 45

S2 58 55 45 42 54 45 18 15 0.53 0.29 46 36
S3 57 55 46 37 52 37 6.9 4.8 1.1 0.72 44 36
S4 85 73 135 120 75 70 15 8 0.77 0.49 62 57
S5 93 83 99 79 89 76 17 13 1.1 0.83 49 44
S6 177 157 126 102 105 94 52 45 2.6 1.7 79 70
S7 183 147 163 129 117 104 51 47 1.9 1.4 58 45
S8 149 115 94 84 67 56 39 31 1.4 1.3 75 61
S9 115 105 112 100 92 81 27 20 1.6 1.0 81 70
S10 179 133 155 118 118 107 38 35 2.8 1.6 83 76

Average ± SD 118 ± 50 99 ± 38 103 ± 43 86 ± 34 82 ± 26 71 ± 27 27 ± 17 22 ± 16 1.5 ± 0.77 1.0 ± 0.53 63 ± 16 54 ± 15

Note: SD, standard deviation.

Table 5
Comparison of metals in sediment (mg/kg dw) with different international guidelines and other studies in the world.

River, location Cr Ni Cu As Cd Pb References

a
Korotoa (Bangladesh) 109 (55–183) 95 (37–163) 76 (35–118) 25 (2.6–52) 1.2 (0.26–2.8) 58 (36–83) This study
Buriganga River (Bangladesh) 178 200 28 – 3.3 70 Ahmad et al. (2010)
Padma River (Bangladesh) 97 28 25 – – 17 Datta and Subramanian (1998)
Jamuna River (Bangladesh) 110 33 28 – – 19 Datta and Subramanian (1998)
Bangshi River (Bangladesh) 98 26 31 1.93 0.61 60 Rahman et al. (2014)
River Ganges (India) 1.8–6.4 NA 0.98–4.4 NA 0.14–1.4 4.3–8.4 Gupta et al. (2009)
Gomti River (India) 8.15 15.7 5 NA 2.42 40.33 Singh et al. (2005)
Yellow River (China) 41–128 NA 30–102 14–48 NA 26–78 Liu et al. (2009)
Gediz River (Turkey) 170–220 101–129 108–152 NA NA 105–140 Akcay et al. (2003)
Okumeshi River (Nigeria) 0.87 1.21 NA NA 1.32 0.45 Raphael et al. (2011)
Shur River (Iran) NA NA 9174 NA 6.85 162 Karbassi et al. (2008)
ASV 90 68 45 13 0.3 20 Turekian and Wedepohl (1961)
TRV 26 16 16 6 0.6 31 USEPA (1999)
LEL 26 16 16 6 0.6 31 Persuad et al. (1993)
SEL 110 75 110 33 10 250 Persuad et al. (1993)

ASV, average shale value; TRV, toxicity reference value; LEL, lowest effect level; SEL, severe effect level; NA, not available.
a
Values in parentheses as range.

As comes mostly from the upland Himalayan catchments which is
connected with the study river at the northern part of Bangladesh
(Mitamura et al., 2008). The concentration of Cd (11 ␮g/L in winter
and 8 g/L in summer) greatly exceeded the drinking water standard
value (5 ␮g/L) (Table 2). The average concentration of Pb in water
was 35 and 27 ␮g/L during winter and summer season, respec-
tively, which were higher than the drinking water quality standard.
Considering the toxicity reference values (TRV) proposed by USEPA
(1999) almost all the heavy metals especially Cr, Cd and Pb greatly
exceeded the limit for safe water, indicated that water from this
river is not safe for drinking and/or cooking. The metals in water
were seasonally varied, where winter season exhibited higher than
summer. The lower levels of trace metals during summer might be
due to the dilution effect of water in river (Mohiuddin et al., 2012;
Islam et al., 2014).
3.2. Chemical properties and total metals in sediment
The chemical parameters and total metal concentration of sedi-
ments are presented in Tables 3 and 4. The average pH in sediment
was 6.5 which is near about neutral. The composition of the organic
carbon in sediment samples was varied among the sites due to its
origin in the aquatic environment. The organic carbon in sediments
ranged from 0.74 to 2.5% during winter and 0.98 to 1.8% during
summer (Table 3). A wide range of values for metal concentrations
was observed among the sampling sites. Factors such as salinity,
 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291 287

Fig. 2. Relative distribution of metal in sediments at different geochemical fractions of Korotoa River of Bogra district, Bangladesh.

geomorphological setup and land runoff might have played a
crucial role in the variation of metals. As shown in Table 4, con-
centrations of heavy metals at sites S6–S10 were much higher
than others sites because of the fact that these sites are located
at the downstream of the river and extensive discharging of urban
waste. Metals concentrations in sediment were higher in winter
than summer due to the lower water flow during winter which
could help to accumulate the heavy metals in sediment (Islam
et al., 2014). The average concentration of heavy metals in sed-
iments were in the decreasing order of Cr > Ni > Cu > Pb > As > Cd.
Chromium concentration in sediment was higher than other
metals as a consequence of direct discharging untreated wastes
from tanneries and textile industries (Facetti et al., 1998). Nickel
concentration in sediment was found as 103 and 86 mg/kg in
winter and summer, respectively whereas Cu content was 82
and 71 mg/kg in winter and summer, respectively. However, high
level of Cu for site S10 (118 and 107 mg/kg in winter and sum-
mer, respectively) indicates its higher input, which might be
originated from urban and industrial wastes (Mohiuddin et al.,
2012).
288 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291

The mean concentration of As in sediment was observed Winter Summer

27 mg/kg in winter and 22 mg/kg in summer which was higher than 8.0
the average shale value (ASV) (13 mg/kg). High As concentration 7.0
might be attributed to the anthropogenic activities such as treat- 6.0

PLI values
ment of agricultural land with fertilizers and arsenical pesticides 5.0
(Renner, 2004; Fu et al., 2014), treating of wood by using copper 4.0
arsenate (Pravin et al., 2012; Baeyens et al., 2007) and tanning in 3.0 Polluted
relation to some chemicals especially arsenic sulfide (Asaduzzaman 2.0
et al., 2002; Bhuiyan et al., 2011). Total Cd content ranged from 1.0
Unpolluted
0.77–2.8 mg/kg in winter and 0.26–1.7 mg/kg in summer. Slightly 0.0
S1 S2 S3 S4 S5 S6 S7 S8 S9 S10
higher Cd level was found in winter which might be due to the Sampling sites
variation in water capacity of the river where low water flow in
winter resulted the precipitation of the metals in sediment; thereby Fig. 3. Pollution load index (PLI) value of heavy metals in sediment of Korotoa River
increasing its concentration (Islam et al., 2014). Average concen- in Bogra district, Bangladesh.
tration of Pb was observed 63 and 54 mg/kg during winter and
summer season, about 3 times higher than ASV value (20 mg/kg)
which can be due to the effect from point and non-point sources; Winter Summer
such as leaded gasoline, municipal runoffs and atmospheric depo- 14
sition (Mukai et al., 1994; Mohiuddin et al., 2012; Shikazono et al.,

Contamination factor (CF)

2012), chemical manufacturing and steel works in urban area of
Bogra district. As a whole, concentrations of most of the metals
exceeded some well recognized standard values and in agreement
with some previous studies (Table 5).
3.3. Chemical fractionation of metals in sediment
Chemical fractionation differentiates metals of natural origin
and/or derived from anthropogenic sources. Metal fractionation is
of critical importance to their potential toxicity and mobility (Maiz
et al., 2000). The sequential extraction technique is proposed for
this purpose to provide information about the strength and ways of
metal associating with sediments (Tessier et al., 1979). The percent-
ages of metal concentrations derived from the sequential extraction
were presented in Fig. 2. The metals in exchangeable fraction are
considered to be the weakest bonded metals in sediments which
may equilibrate with the aqueous phase and thus become more eas-
ily bioavailable (Pardo et al., 1990). The more proportion of metals
in this fraction, the more mobile they are, and the higher risk they
could pose to the environment. Metals from anthropogenic sources
are predominantly found in the most labile sediment fractions,
which are vulnerable to small changes in environmental conditions
(Alves et al., 2007).
The metals associated with different fractions in
sediments followed the descending order of: Cr: resid-
ual > organic > carbonate > Fe-Mn oxides > exchangeable; Ni:
residual > organic > Fe-Mn oxides > carbonate > exchangeable; Cu:
residual > organic > exchangeable > carbonate > Fe-Mn oxides; As:
residual > Fe-Mn oxides > organic > carbonate > exchangeable; Cd:
exchangeable > carbonate > organic > Fe-Mn oxides > residual and
Pb: residual > exchangeable > carbonate > organic > Fe-Mn oxides
(Fig. 2). In general, results of the sequential extraction indicates
that the residual fraction dominated the fraction of Cr (27–40%), Ni
(23–42%), As (24–37%) and Pb (24–33%) in winter and Cr (15–43%),
Ni (28–35%), As (43–62%) and Pb (24–36%) in summer season,
respectively. This result suggested that Cr, Ni, As, and Pb had the
strongest associations to the crystalline sedimentary components
and likely to reflect the geological characteristics (Hamilton et al.,
1984).
Considering that bioavailability is related to solubility
(Xiangdong et al., 2000), the bioavailability of metal decreases
in the order of exchangeable > acid reduction > organic > residual
forms. Among the studied metals, Cd (17–53%) showed the highest
proportion in the sedimentary fraction. The metals in sediment
at the residual phase represents largely embedded in the crystal
lattice of sediment (Yuan et al., 2004).
12
10
Very high degree
8
6
Considerable degree
4
2 Moderate degree
0
Low degree
Cr Ni Cu As Cd Pb
Metals
Fig. 4. Contamination factor (CF) of heavy metals in sediment of Korotoa River of
Bogra district, Bangladesh.
3.4. Assessment of metal pollution in sediments
The calculated pollution load index (PLI) values of metals in sed-
iment are summarized in Fig. 3 which were ranged from 2.4 to
7.2 during winter and 1.6–5.7 during summer confirming that the
sediment of the studied river was heavily contaminated (PLI > 1).
However, the higher PLI values indicated that Cr, Cd and Pb are the
major contributors to the sediment pollution. The PLI can provide
some understanding to the inhabitants about the quality of the
environment. In addition, it also provides valuable information to
the decision makers on the pollution status of the area (Suresh
et al., 2012). Higher PLI values were observed in sampling sites S6
to S10, which might be due to the effects of urban activities. The
value of contamination factor (CF) for all metals showed moderate
degree of contamination (CF > 1), whereas As and Cd showed very
high degree of contamination (CF > 6) (Fig. 4). Overall, the CF for all
metals were the descending order of Cd > Pb > As > Cr > Cu > Ni. The
mean CF values of Cr, Ni, Cu, As, Cd and Pb were 4.2, 3.1, 2.4, 6.9, 12
and 4.3 during winter and 3.5, 2.6, 2.1, 5.7, 8.0 and 3.7 during sum-
mer season. Fig. 5 presents the geoaccumulation factor (Igeo) values
of the studied metals. Among the studied metals, the Igeo values
showed the decreasing order of Cd > As > Pb > Cu > Ni > Cr. Among
the sites, the range of Igeo values for Cr, Ni, and Cu were 0.44–2.1,
−0.15 to 1.7 and −0.06 to 1.2 during winter and 0.39–1.9, −0.42
to 1.3 and −0.53 to 1.1 during summer, indicating unpolluted to
moderately polluted status of the sediment whereas, the Igeo val-
ues for As (−0.11 to 3.1 and −1.2 to 3.0 during winter and summer
season, respectively) indicates unpolluted to heavily polluted sta-
tus. On the other hand, the Igeo values of Pb (1.0–1.9 during winter
and 0.72–1.8 during summer) indicate moderately contamination
of sediment. However, the highest Igeo value was obtained for Cd
 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291 289

Fig. 5. Geoaccumulation index (Igeo ) value of heavy metals in sediment of Korotoa River of Bogra district, Bangladesh.

(1.6–3.9 and 0.51 to 3.2 during winter and summer season, respec-
tively) which might be due to the higher concentration in sediment
and lower level in the background sample.
Enrichment factor (EF) is a normalization technique widely used
to categorize the metal fractions that is associated with sediments.
The spatial distributions of calculated EF for each of the studied
metals were displayed in Fig. 6. Taking as a whole, the mean EF
values of all the studied metals suggested their enrichments in
surface sediments of the river Korotoa in Bangladesh. For most of
the sites EF of the studied metals were higher than 1.5 indicat-
ing strong human influence to the metal pollution in sediments
(Fig. 6). The mean EF values of Cr, Ni, Cu, As, Cd and Pb were 2.3,
1.7, 1.3, 3.5, 5.9 and 2.4, respectively. Metals in the residual fraction
are an indication of lithogenic input, while those in non-residual
fractions can mainly be explained by anthropogenic inputs (Gao
and Chen, 2012). As shown in Fig. 7, there was a strong correlation
between non-residual fraction and their corresponding EF values of
Cu, Cd and Pb (Fig. 7). This indicated that anthropogenic inputs were
probably the major contributor for the enrichment of metals in the
surface sediments of the studied river. It is presumed that high EF
values indicate an anthropogenic source of heavy metals, mainly
from activities such as industrialization, urbanization, deposition

4 8
3
EFc of Cr

EFc of As

6
2 4
1 2
0 0
S1 S2 S3 S4 S5 S6 S7 S8 S9 S10 S1 S2 S3 S4 S5 S6 S7 S8 S9 S10

3 10 Sampling sites
EFc of Cd
EFc of Ni

2
5
1

0 0
S1 S2 S3 S4 S5 S6 S7 S8 S9 S10 S1 S2 S3 S4 S5 S6 S7 S8 S9 S10

4 Sampling sites 4 Sampling sites

EFc of Cu

EFc of Pb

3 3
2 2
1 1
0 0
S1 S2 S3 S4 S5 S6 S7 S8 S9 S10 S1 S2 S3 S4 S5 S6 S7 S8 S9 S10
Sampling sites Sampling sites
Fig. 6. Enrichment factor (EF) values for heavy metals in surface sediments of sampling sites, Korotoa River. The horizontal dot lines represent EF value of 1.5.
290 M.S. Islam et al. / Ecological Indicators 48 (2015) 282–291

40 y = 7.2379x + 2.9552 80 12 20

Non-residual Cr (mg/kg)

Non-residual As (mg/kg)
y = 1.3412x - 0.3071

Residual As (mg/kg)
Residual Cr (mg/kg)
R² = 0.4265
10 R² = 0.6799
30 60 15
8
20 40 6 10
4
10 y = 11.207x + 8.818
20 y = 2.3896x - 0.8564 5
2 R² = 0.7567
R² = 0.3042
0 0 0 0
0 1 2 3 4 0 2 4 6 8
EFc of Cr EFc of As

30 y = 7.2037x + 4.783 50 0.6 0.4

Non-residual Cd (mg/kg)
Non-residual Ni (mg/kg)

Residual Cd (mg/kg)
Residual Ni (mg/kg)
R² = 0.4703 y = 0.0484x - 0.0061
25 40 0.5 R² = 0.5285 0.3
20 0.4
30
15 0.3 0.2
20
10 0.2
y = 9.612x + 13.062 10 y = 0.0207x + 0.041 0.1
5 0.1
R² = 0.4303 R² = 0.3928
0 0 0 0
0 1 2 3 0 2 4 6 8 10
EFc of Ni EFc of CD

y = 6.5845x + 5.9092 y = 1.2672x + 7.8201

25 30 15 30

Non-residual Pb (mg/kg)
Non-residual Cu (mg/kg)

R² = 0.1163

Residual Pb (mg/kg)
Residual Cu (mg/kg)
R² = 0.3228
20 25 25
20 10 20
15
15 15
10
10 5 10
y = 2.0877x + 16.73 y = 3.0549x + 8.8068
5 5 5
R² = 0.0255 R² = 0.1054
0 0 0 0
0 0.5 1 1.5 2 2.5 0 1 2 3 4
EFc of Cu EFc of Pb

Fig. 7. Relationships between the studied metals in non-residual/residual fractions and their corresponding enrichment factors (EFs). The regression lines and equations in
black color were based on the data of metals in non-residual fractions and EFs; the regression lines and equations in blue color were based on the data of metals in residual
fractions and EFs.

of industrial wastes, and others. Since, the bioavailability and tox- Appendix A. Supplementary data
icity of any metal in sediments depend upon the chemical form and
concentration of the elements (Kwon et al., 2001), it can be inferred Supplementary data associated with this article can be
that trace elements in sediment samples with the highest EF values, found, in the online version, at http://dx.doi.org/10.1016/j.ecolind.
along with higher labile fractions in sediments have a potential for 2014.08.016.
mobility and bioavailability in the aquatic ecosystems.
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