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Arabian Journal of Geosciences

ISSN 1866-7511

Arab J Geosci
DOI 10.1007/s12517-012-0734-z
Heavy metal distribution in surface
sediments of the Tirumalairajan river
estuary and the surrounding coastal area,
east coast of India
S.Venkatramanan, T.Ramkumar,
I.Anithamary & S.Vasudevan
1 3
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ORIGINAL PAPER
Heavy metal distribution in surface sediments
of the Tirumalairajan river estuary and the surrounding
coastal area, east coast of India
S. Venkatramanan & T. Ramkumar & I. Anithamary &
S. Vasudevan
Received: 6 October 2011 / Accepted: 31 October 2012
#Saudi Society for Geosciences 2012
Abstract Surface sediments collected at the Tirumalairajan
river estuary and their surrounding coastal areas were
analyzed for the bulk metal concentration. The sedi-
ments were collected from post- and premonsoon sea-
sons. Dominances of heavy metals are in the following
order: Fe > Mn > Zn > Pb > Cu in both seasons from
estuary and coastal area. The results reveal that Fe, Mn,
Cu, Pb, and Zn demonstrated an increased pattern from
the estuary when compared to the coastal area. The
heavy metal pattern of the sediments of the Tirumalair-
ajan river estuary and its surrounding coastal area of-
fered strong evidence that the coastal area was a major
source of heavy metals to the estuarine region. For
various metals, the contamination factor and geoaccu-
mulation index (I
geo
) have been calculated to assess the
degree of pollution in sediments. The contamination
factor and geoaccumulation index show that Zn, Pb,
and Cu unpolluted to moderately pollute the sediments
in estuarine part. This study shows the major sources of
metal contamination in catchment and anthropogenic ones,
such as agriculture runoff, discharge of industrial wastewater,
and municipal sewage through the estuary and adjoining
coastal area.
Keywords Heavy metals
.
Geoaccumulation index
.
Contamination factor
.
Tirumalairajan estuary
.
East coast of
India
Introduction
Estuarine and coastal areas are complex and dynamic aquat-
ic environment (Morris et al. 1995). Physical, chemical, and
biological interactions between freshwater and saltwater
systems can have profound influences on the transport and
fate of heavy metals. The distribution of heavy metals
through complex processes of material exchange within
these aquatic environments can also be affected by anthro-
pogenic inputs. Often, such an influence is more apparent in
an estuarine and surrounding coastal area than in an open
ocean due to intense human activities. The transport of
heavy metals from rivers to estuaries and then to the open
ocean is dependent on the partitioning of heavy metals
between dissolved and particulate phases and other environ-
mental conditions. Both estuaries and coastal areas are sub-
ject to the varying influences of riverine and atmospheric
inputs, coastal and seafloor erosion, and biological activi-
ties. Nevertheless, physical and chemical transport and bio-
geochemical interactions within these areas may be the key
factors controlling land-derived natural and pollutant chem-
icals into the coastal areas. Heavy metals may be recycled
via chemical and biological processes, within the sedimen-
tary compartment and back to the water column (Salomons
and Forstner 1984; Tessier and Campbell 1987). With the
rapid industrialization and economic development in coastal
region, heavy metals are continuing to be introduced to
estuarine and coastal environment around the world (Romano
et al. 2004; Santos et al. 2005; Fenga et al. 2010). Various
studies have demonstrated that sediments from coastal areas
are greatly contaminated by heavy metals; therefore, the eval-
uation of metal distribution in surface sediments is useful to
assess pollution in the marine environment (Bellucci et al.
2002; Pekey 2006; Buccolieri et al. 2006; Jayaprakash et al.
2007; Muthuraj and Jayaprakash 2008; Anithamary et al.
S. Venkatramanan (*)
:
T. Ramkumar
:
I. Anithamary
:
S. Vasudevan
Department of Earth Sciences, Annamalai University,
Chidambaram, Tamil Nadu, India
e-mail: venkatramanansenapathi@gmail.com
T. Ramkumar
e-mail: tratrj@gmail.com
Arab J Geosci
DOI 10.1007/s12517-012-0734-z
Author's personal copy
2012). The accumulation of metal contaminants in sediments
can pose serious environmental problems to the surrounding
areas. Heavy metal contamination in sediment could affect the
water quality and bioaccumulation of metals in aquatic organ-
isms, resulting in potential long-term implications on human
health and ecosystem. It is therefore important to understand
the mechanisms of accumulation and geochemical distribu-
tion of heavy metals in sediments in order to develop pollution
control strategies and approaches to water quality manage-
ment in a coastal area. Human activities have greatly altered
the geochemical cycle of heavy metals, resulting in wide-
spread environmental contamination (Nriagu and Pacyna
1988). Heavy metal contamination in a marine coastal envi-
ronment is related to sources of pollution in the adjacent
estuaries and rivers. Metals are mainly transported to the
marine environment by rivers through estuaries. In most
circumstances, the major contribution of anthropogenic
metals in a marine coastal area is of terrestrial origin, i.e.,
from mining, industrial, and urban development's and other
human practices near rivers and estuaries (Morton and
Blackmore 2001; Delgado et al. 2010; Angelidis et al.
2011). Grain size of sediment is one of the major control-
ling factors for the distribution of heavy metals in the
coastal area (Venkatramanan et al. 2011).
The present study aims to assess the heavy metal con-
tamination of the Tirumalairajan river estuary and its sur-
rounding coastal area. The objectives of this research are:
(1) to examine heavy metal concentrations in the sediments
in the Tirumalairajan river estuary and its surrounding coast-
al area, (2) to investigate the relationship of heavy metal
contamination between the Tirumalairajan river estuary and
its surrounding coastal area using various contamination
factors, and (3) to evaluate the geochemical cycling process
of heavy metals in sediments between the Tirumalairajan
river estuary and its surrounding coastal area (e.g., physical
and chemical transportation processes of heavy metals in
estuarine and coastal areas).
Description of the study area
The present study focuses on the Tirumalairajan river estu-
ary and surrounding coastal area. It is an important tributary
of Cauvery River, and it originates in the Eastern Ghats and
flow through the state of Tamil Nadu to join the Bay of
Bengal. The study area (Fig. 1) forms part of east coast of
India. It falls between the latitude N 1052 to 1053 and
longitude E 7948 to 7951 and forms part of survey of
Fig. 1 Location map of the study area
Arab J Geosci
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India Toposheet No. 58M/13 and 16 on 1:50,000 scale. The
Arasalar, Vellar, Adappar, Vettar, and Vedaranyam canals
are distributed to the main rivers flowing in this area and
debauch into the Bay of Bengal. The study area is sur-
rounded by Tanjore District in the west, Cuddalore District
in the north, Palk Strait in the south, and Bay of Bengal in
the east. The climate of the area is generally hot, semidry,
and tropical. March to June are the hottest months and
December to February are the cooler months of the year.
The major portion of the annual rainfall is received during
the northeast monsoon recorded during October to Decem-
ber. Based on the northeast monsoon, the climatic condition
of the region is divided into monsoon (October to Decem-
ber), postmonsoon (January to March), summer (April to
June), and premonsoon (July to September) seasons. The
recorded average annual rainfall was 863 mm.
The geology of the study area is shown in Fig. 2. This
area mainly comprises quaternary sediments, which in-
crease towards the south of Coleroon River. These sedi-
ments have been delineated as an alluvial plain deposit of
the Cauvery River and its distributaries, narrow fluvio-
marine deltaic plain deposits, and marine coastal plain
deposits (east coast formation). The fluvial deposits com-
prise flood plain, flood basin, point bar, channel bar, and
palaeo-channels with admixtures of sand, silt, and clay.
The deltaic plain includes palaeo-tidal flats with clays and
sands and sand ridges or gray brown sand. The marine
coastal plains include beach, tidal flats, salt marsh, man-
grove swamps, and deposits of sand and clay. The Creta-
ceous formations of the coastal track of the Cauvery basin
consist of faunal-rich marine sedimentary rocks, namely
limestones, sandstones, clays, sandy beds, etc. The mouth
Source Geological Survey of India (GSI)
Legend
Fluvial (Qf), Fluvio Marine (Qfm),
Aeolian (Qa) and Marine (Qm)
Quternary sediment of sand, silt
and clay. Ceramic, brick & tile clays
River
Fig. 2 Geology map of the
study area
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of the river comprises alluvium deposits, which are composed
of clays and silts.
Materials and methods
Sediment sampling
Ten surface sediment samples were collected in the study
area (postmonsoon and premonsoon of 2009). The sampling
locations were relatively evenly distributed in Tirumalaira-
jan river estuary and its surrounding coastal area. The sur-
face samples (to a depth of 5 cm) were taken with a grab
sampler (Van Veen). All of the sediment samples were
stored in polyethylene bags at 46 C immediately after
collection and prior to undergoing analysis in a laboratory.
For total metal analysis, the sediments were dried at 5060 C
in an oven and disaggregated in an agate mortar, before
chemical treatment.
Analyses of heavy metals
For each sample, a known quantity (1 g) of sediment was
digested with a solution of concentrated HClO
4
(2 ml) and
HF (10 ml) to near dryness. Subsequently, a second addition
of HClO
4
(1 ml) and HF (10 ml) was made, and the mixture
was evaporated to near dryness. Finally, HClO
4
alone was
added and the sample was evaporated until white fumes
appeared. The residue was dissolved in concentrated HCl
and diluted to 25 ml (Tessier et al. 1979). Heavy metal
concentrations (Fe, Mn, Zn, Pb, and Cu) were measured
using an inductively coupled plasma optical emission spec-
trometer (ICP-OES, PerkinElmer Optima 5300 DV). Below
detection limits for metal analysis were Fe0.004 g/g,
Mn0.001 g/g, Zn0.005 g/g, Pb0.042 g/g, and
Cu0.009 g/g. The accuracy of the analytical method was
analyzed by the standard reference material MAG-1 (marine
mud from the United States Geological Survey). The average
recoveriesstandard deviation found for each metal were
8215, 7814, 7324, 7122, and 7723 for Fe, Mn,
Zn, Pb, and Cu, respectively.
Results and discussion
Heavy metal distribution
The concentrations of heavy metals in the sediment at the
Tirumalairajan river estuary and its surrounding coastal area
are represented in Figs. 3a, b and 4a, b. The concentrations
of Fe, Mn, Zn, Pb, and Cu of the sediments in the Tiruma-
lairajan river estuary were significantly lower than those at
the coastal area in both seasons. The distribution patterns for
heavy metals of potentially anthropogenic origin (Zn and
Pb) in the surface sediments are broadly similar with the
highest concentrations for other elements being particularly
associated with the increasing fine fraction in the estuarine
region. The elevation of the Fe concentrations of the Tiru-
malairajan river estuary sediments was particularly evident
when compared with those at the coastal area. The mean Fe
concentration of the Tirumalairajan river estuary sediments
was four times lower than that at the coastal area. In the
Tirumalairajan river estuary, the bulk metal concentration of
Fe, Mn, Zn, Pb, and Cu in the sediment ranged from 1,806
to 2,906 g/g, 10.4 to 18.6 g/g, 28.4 to 44.3 g/g, 1.01 to
7.3 g/g, and 18.7 to 28.8 g/g, respectively, in postmon-
soon. In case of premonsoon season, the metal concentration
of Fe, Mn, Zn, Pb, and Cu in the sediment ranged from
1,804 to 2,802 g/g, 6.4 to 17.6 g/g, 28.2 to 42.4 g/g,
1.42 to 3.5 g/g, and 12 to 21.9 g/g, respectively. During
postmonsoon season, the concentration of heavy metals in
estuary indicates enrichment in stations 3, 4, and 5, whereas
in premonsoon season, the heavy metal concentration in-
creased in an upstream direction. The concentration of Fe
Fig. 3 a Distribution of metals in Tirumalairajan estuary during post-
monsoon. b Distribution of metals in Tirumalairajan estuary during
premonsoon
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and Mn within the estuarine sediments can be related to
various natural processes, and other metals were derived
from the Karaikal Harbor (Anithamary et al. 2012). Zn,
Pb, and Cu found in estuary (stations 2, 3, and 4) are due
to the high tourist boat activities in Karaikal beach and
small-scale development of industries in the area (Millward
and Moore 1982; Nath et al. 1989, Santhiya et al. 2011). The
level of heavy metal in surrounding coastal areas (stations 5
and 6) in case of postmonsoon season and the heavy metal
concentration observed at stations 3 and 4 during premon-
soon season indicate the anthropogenic activities in the
coastal areas. Moreover, it is also due to the recent devel-
opment of major industries (in the coastal areas and offshore
drilling) and minor harbor activities where heavy movement
of naval vessels takes place throughout the year for regular
surveillance in the coastal region (Hershelman et al. 1981;
Luoma and Phillips 1988; Fukushima et al. 1992; Jonathan
and Ram Mohan 2003). In addition, the high values are also
attributed to the continental input and runoff from the minor
rivers that drain in this region and the Cauvery River and its
tributaries which drain through the agricultural belt in
the rural areas of Tamil Nadu state. The above inferences are
very well supported by the high values of Zn, Pb, and Cu
which are all components of the fertilizers used in agricultural
activities (Forstner 1984; Krumgalz 1989, 1993; Krumgalz et
al. 1992).
Along the beach, the concentration of bulk metals (Fe,
Mn, Zn, Pb, and Cu) ranged from 1,932 to 2,933 g/g, 5.6
to 20.1 g/g, 5.1 to 16.7 g/g, 0.77 to 1.65 g/g, and 1.04 to
4.1 g/g, respectively, in postmonsoon season. During pre-
monsoon season, the concentration of metals (Fe, Mn, Zn,
Pb, and Cu) ranged from 1,837 to 2,908 g/g, 7.6 to
15.7 g/g, 6.63 to 13.4 g/g, 0.69 to 1.2 g/g, and 1.81 to
3.86 g/g, respectively. It is mainly due to the natural
occurrence of these metals in sediments and rocks in the
catchment area and drainage region and they being the input
of metals to Tirumalairajan and Arasalar rivers and its
tributaries. These results illustrate that known ability of
FeMn to act as a scavenger of heavy metals from solution
through processes such as adsorption and co-precipitation.
The concentration of metals clearly infers that the manifold
irrigation and industrial activities contribute a huge amount
to the enrichment of metals like Zn, Pb, and Cu in the
estuary and beach sediments of the city in both seasons
(Table 1). Karaikal coast is also affected due to shipping
and harbor activities; agricultural runoff, industrial and ur-
ban waste discharges, dredging, etc. could contribute to the
enrichment of metals in the estuarine and coastal environ-
ment. The sediment metal concentrations found in this study
were of the same order of magnitude as metal concentrations
found by diverse authors in sediments of Indian estuaries
(Biksham and Subramanian 1988; Subramanian et al. 1988;
Ramesh et al. 1990; Ramanathan et al. 1993; Alagarsamy
2006). This indicated that the characteristic of estuarine
sediment showed higher level when compared to the coastal
track, which was reflected in the coastal sediments as similar
to the source of its origin from the riverine composition and
its abundances (Alagarsamy and Zhang 2010).
Pollution impact
Pollutant impacts a number of calculation methods that have
been put forward for quantifying the degree of metal enrich-
ment in sediments. Various authors (Salomons and Fostner
1984; Muller 1969; Hokanson 1980) have proposed pollu-
tion impact scales or ranges to convert the calculated nu-
merical results into broad descriptive bands of pollution
ranging from low to high intensity. Sediment quality guide-
lines provide values that allow for quantification of sedi-
ment contamination; further comparisons are required to
make an overall assessment of the degree of metal contam-
ination in estuarine and marine sediments. This is largely a
consequence of the presence of an unknown background
Fig. 4 a Distribution of metals in coastal region during postmonsoon.
b Distribution of metals in coastal region during premonsoon
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metal concentration in the sediment. Expressing metal con-
centrations as a contamination factor (CF) and geoaccumula-
tion index (I
geo
) relative to references, sites, or preindustrial
sediments from the study area represents an approach that can
overcome this problem. The geoaccumulation index was orig-
inally defined by Muller (1969).
Contamination factor
Sediments have been widely used as environmental indi-
cators, and this ability to identify heavy metal contamina-
tion sources and monitor contaminants is also well-
recognized. Thus, the accumulation of metals in the sedi-
ments is strongly controlled by the nature of the substrate
as well as the physicochemical conditions controlling dis-
solution and precipitation. The accumulation of heavy met-
als in sediments gives rise to two types of impacts on
overlying water and both in a marine environment. The
heavy metals themselves may have a synergistic or antag-
onistic effect on the environment. The level of metal con-
tamination was expressed by the contamination factor
(Pekey et al. 2004; Savvides et al. 1995):
CF metal concentration in polluted sediment=
background value of the metal:
When CF>1 for a particular metal, it means that the
sediment is contaminated by the element, and if CF<1, then
there is no metal enrichment by natural or anthropogenic
inputs. While calculating the CF of the sediments in the
study area, we have taken the local background of the heavy
metals under consideration as reported by Ramanathan et al.
(1993) of background values. The CF was classified into
four groups based on the calculating values (Pekey et al.
2004; Hokanson 1980; Savvides et al. 1995):
<1: Low contamination factor
13: Moderate contamination factor
36: Considerable contamination factor
>6: Very high contamination factor
Zinc concentration is extremely high in the estuary; the
CF was >3 in all stations except the stations 1, 4, and 5 in
both seasons (CF<3) which indicates it to be a considerable
contamination zone in the estuarine region. It is mainly
derived from the anthropogenic source to the study area.
The most striking finding of this investigation is that this
could due to the continual resuspension of bottom sediments
occurring in the Tirumalairajan estuary, and the southern
part of the coast may serve to scavenge and concentrate
metals that are naturally present in water column as well
as those introduced by irrigation runoff and industrial dis-
charge (Jonathan et al. 2004; Jayaprakash et al. 2007). The
distribution pattern of heavy metals resembles the anthropo-
genic contribution of metals, and the role of sediment type
becomes a major factor affecting the distribution of metals
in this region.
The CF<1 was observed for Pb and Cu in all stations, which
means the sediments are low contaminated by Pb and Cu in
both seasons. Whereas along the coastal area, Zn was observed
in station 2, indicates the moderate contamination level. Low
contamination levels were observed for Pb and Cu (Table 2).
Geoaccumulation index (I
geo
)
A common approach to estimating the enrichment of metal
concentrations above background or baseline concentrations
is to calculate the geoaccumulation index (I
geo
) as proposed
by Muller (1969). The method assesses the degree of metal
pollution in terms of seven enrichment classes based on the
increasing numerical values of the index (Table 3). This
index is calculated as follows:
I
geo
log
2
Cn 1:5 Bn =
where Cn is the concentration of the element in the enriched
samples, and the Bn is the background or pristine value of
the element. Factor 1.5 is introduced to minimize the effect
of possible variations in the background values, which may
be attributed to lithologic variations in the sediments
(Stoffers et al. 1986; Muller 1969). Although, I
geo
was
Table 1 The concentration of heavy metals in the sediments of study area
Metals (g/g) Estuary Coastal region
Postmonsoon Premonsoon Postmonsoon Premonsoon
MinMax Mean MinMax Mean MinMax Mean MinMax Mean
Fe 1,8062,906 2,342 1,8042,802 2,214 1,9322,933 2,415 1,8372,908 2,350
Mn 10.418.6 15.5 6.417.6 12.8 5.620.1 14.8 7.615.7 12.2
Zn 28.444.3 35.8 28.242.4 35.6 5.116.7 10 6.6313.4 9.5
Pb 1.017.3 4.2 1.423.5 2.3 0.771.65 1.12 0.691.2 1.02
Cu 18.728.8 20.7 1221.9 17.4 1.044.1 2.5 1.813.86 2.9
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originally devised for use with the global standard shale
values as background metal levels, Rubio et al. (2000) have
shown that the use of regional background values yields
more appropriate results. In this study, I
geo
has been calcu-
lated using local background values for metal concentra-
tions as presented by Ramanathan et al. (1993). The
concentrations of Zn, Pb, and Cu were relatively low, which
indicates that sediment was in unpolluted to moderately
polluted category in both seasons (Table 4).
Conclusion
The results indicated the potential pathways of heavy metals
via the transport of sediment from the Tirumalairajan river
to the coastal area. It dissolved heavy metals associated with
fine particles which tended to be deposited at an interface
between freshwater and marine water zones due to the
processes of adsorption and coagulation of dissolved heavy
metals. The impact of anthropogenic heavy metal pollution
of Tirumalairajan estuary and coastal track sediments were
evaluated using CF and geoaccumulation index. The geo-
accumulation indexes are distinctly variable and suggest that
fine sediments in the study area range from unpolluted
to moderate pollute with respect to the analyzed metals
in both seasons. The CFs for zinc in the study area
indicated that the surface sediments are moderately con-
taminated, probably as a result of anthropogenic activities
and provide a useful means of distinguishing between the
natural and anthropogenic sources of metal entering an estuary
to the coastal zone. The FeMn metal acts as scavenger of the
other metals in the processes such as adsorption and co-
precipitation. Heavy metals associated with the sediment in
the upstream area were mainly controlled by the physical
process, while those deposited in the interface zone between
freshwater and marine water were dominated by the chemical
process. The results of the present investigation and the
actual knowledge about the metal distribution in these
sediments indicate that further researches into the origin
of these metal concentrations are certainly necessary in the
near future.
Acknowledgments The authors acknowledge the valuable sugges-
tions given by Abdullah M. Al-Amri, Editor-in-Chief, which greatly
helped in the final presentation of the paper. The authors are grateful to
anonymous referee for the constructive comments and suggestions
which led to significant improvements to the manuscript. Special
thanks are due to Dr. M.V. Prasanna, Lecturer, Department of Applied
Geology, Curtin University of Technology, Miri, Sarawak, Malaysia,
and S. Subramanian, Laboratory Manager, BEFESA, Desalination
Plant, Chennai, for fine tuning the manuscript. The authors would also
like to thank the results generated by ICP-OES, IIT Madras, Chennai,
Tamil Nadu, India.
Table 4 Geoaccumulation index for metals
Geoaccumulation index (I
geo
)
Estuary Postmonsoon Premonsoon
Zn Pb Cu Zn Pb Cu
1 0.24 0.13 0.12 0.24 0.03 0.12
2 0.26 0.16 0.13 0.26 0.06 0.12
3 0.26 0.15 0.13 0.25 0.10 0.13
4 0.24 0.00 0.13 0.25 0.09 0.12
5 0.23 0.00 0.12 0.23 0.03 0.10
Coastal region
A 0.17 0.04 0.04 0.15 0.01 0.04
B 0.19 0.00 0.03 0.18 0.01 0.02
C 0.15 0.01 0.06 0.13 0.01 0.04
D 0.11 0.01 0.04 0.15 0.03 0.06
E 0.14 0.02 0.00 0.16 0.01 0.04
F 0.14 0.02 0.04 0.14 0.01 0.06
Table 3 Description of the sediment quality (Muller 1969)
I
geo
value Class Quality of sediment
<0 0 Unpolluted
01 1 From unpolluted to moderately polluted
12 2 Moderately polluted
23 3 From moderately polluted to strongly polluted
34 4 Strongly polluted
45 5 From strongly to extremely polluted
>5 6 Extremely polluted
Table 2 Contamination factor for metals
Contamination factor (CF)
Estuary Postmonsoon Premonsoon
Zn Pb Cu Zn Pb Cu
1 2.22 0.43 0.83 2.31 0.13 0.78
2 3.17 0.61 0.99 3.03 0.17 0.83
3 3.10 0.53 0.94 2.67 0.29 0.95
4 2.22 0.08 0.91 2.74 0.24 0.73
5 2.03 0.09 0.81 2.02 0.12 0.52
Coastal region
A 0.86 0.14 0.12 0.63 0.10 0.11
B 1.19 0.09 0.09 0.96 0.07 0.08
C 0.64 0.09 0.18 0.47 0.10 0.12
D 0.36 0.10 0.12 0.66 0.06 0.16
E 0.52 0.07 0.05 0.73 0.10 0.12
F 0.58 0.06 0.10 0.53 0.10 0.17
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