PAHs contamination 

in groundwater from
a part of metropolitan city, India: a study
based on sampling over a 10-year period

K. Brindha & L. Elango

Environmental Earth Sciences

ISSN 1866-6280

Environ Earth Sci

DOI 10.1007/s12665-013-2914-x

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 Author's personal copy
Environ Earth Sci
DOI 10.1007/s12665-013-2914-x
ORIGINAL ARTICLE
PAHs contamination in groundwater from a part of metropolitan
city, India: a study based on sampling over a 10-year period
K. Brindha • L. Elango
Received: 9 June 2013 / Accepted: 31 October 2013
Ó Springer-Verlag Berlin Heidelberg 2013
Abstract Presence of polycyclic aromatic hydrocarbons
(PAHs) in the soil and water is of serious environmental
concern as they are carcinogenic in nature. The present
study was carried out with an aim to identify the presence
of PAHs in groundwater of Chennai, Tamil Nadu, India.
This is an industrialised area where petrochemical storage
tanks are located. Groundwater sampling was carried out in
the years 2001, 2011 and 2012 to understand the variation
in PAHs content in this area. Concentration of major ions,
pH and EC were measured during the year 2001. Of the 24
groundwater samples collected in the year 2001, most of
them were alkaline and 62.5 % were not permissible for
drinking based on pH and EC, respectively. Influence of
seawater was the major reason for the Na–Cl dominant
nature of groundwater. TPH and PAHs analysis of
groundwater carried out in 2001 and 2011, and physical
examination of groundwater in 2012 indicate the increased
level of contamination in the eastern part of the study area.
The contamination in the eastern part persists because of
the fact that groundwater is flowing towards the east and
also due to the presence of petrochemical storage tanks
near the coast. Thus this area is affected by PAHs pollution
which has endured over the past 50 years. An underground
storage tank that was functioning in this area was closed
about 50 years ago and leakage of PAHs from this tank
was reported in the year 1993. However, the present study
indicates the decrease in the area of zone of pollution,
possibly due to natural flushing of groundwater zone.
K. Brindha
L. Elango (&)
Department of Geology, Anna University,
Chennai 600 025, India
e-mail: elango34@hotmail.com; elango@annauniv.edu
Keywords Oil pollution
TPH
Poly aromatic
hydrocarbons
Coastal area
Smell of oil

Royapuram
Chennai
India
Introduction
Environmental pollution of groundwater had been caused
in the past due to lack of sufficient knowledge or negli-
gence. This condition was soon realised and developed
countries have already taken scientific and technological
measures to remediate this problem and enforced stringent
laws. But developing countries still need to address this
issue more seriously so as to avoid a situation where
remediation becomes impossible. With rapid industriali-
sation, the challenges to humankind in tackling new kinds
of pollutants have also increased. Polycyclic aromatic
hydrocarbons (PAHs) are one of the pollutants in the
environment that are of great concern, as they are known to
be carcinogenic and mutagenic. They have been listed as
priority pollutants by the United States Environmental
Protection Agency (EPA test method, 1982).
There are various sources that lead to release of PAHs to
the environment such as industrial pollution, vehicular
emission, etc. which are given in Fig. 1. Their presence in
water, soil, sediments and plants has been studied widely
(Cao et al. 2013; Hahladakis et al. 2013; Okedeyi et al.
2013; Yun et al. 2013; Galitskaya and Pozdnyakova 2012;
Han et al. 2012; Wang et al. 2012; Ene et al. 2012; Ribeiro
et al. 2012). Maliszewska-Kordybach et al. (2009) identi-
fied PAHs in agricultural soils due to the contribution from
anthropogenic sources. Soils in Ghana polluted by PAHs
due to incomplete combustion of petroleum products,
especially from atmospheric fallout from automobile
exhausts was identified by Tay and Biney (2012).
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Agricultural soils having PAHs derived probably from
biomass and fossil fuel combustion (Agarwal et al. 2009)
and urban soil also containing PAHs from vehicular emis-
sion (Agarwal 2009) have been reported in Delhi, India. The
contamination of soils with PAHs by approximately 2.6
times more than the background value in the international
airport area of New Delhi, India, due to jet turbine exhaust
was reported by Ray et al. (2008). A study carried out by the
Central Pollution Control Board (CPCB) of India in some of
the major cities indicates the absence of PAHs in ground-
water (CPCB 2007). Li et al. (2010) observed PAHs in
water, sediments, soil and plants in Aojiang river, China,
which was due to the possible contribution from leather
industries. Industrial wastewater and municipal road runoff
contributed to PAHs in surface waters, sediments and soils
of Hangzhou, China (Chen et al. 2004). PAHs in streams
that receive wastewater from industries were analysed by Qi
et al. (2012). PAHs in drinking water constitute an impor-
tant environmental problem which was addressed in Zhe-
jiang province, China, by Zhu et al. (2008) and the sources
were petroleum products. PAHs and benzene, toluene,
ethylbenzene and xylenes (BTEX) were identified in
groundwater samples around gasoline stations in Rio de
Janerio, Brazil (do Rego and Netto 2007). The carcinogenic
and non-carcinogenic risks due to PAHs in drinking water
were assessed by Li et al. (2012).
Chennai, located in the southern part of India is the
fourth largest city in India. The metropolitan area covers
1,167 km2 with a population of 7.4 million people as per
2010 census. This rapid urbanisation of the city and its
suburban areas has resulted in a phenomenal increase in the
exploitation of groundwater resources. The city has a wide
range of industries and factories that include tanneries,
petrochemical refineries, automobile manufacturing units,
etc. Petroleum hydrocarbon (PHC) in the coastal sediments
of Chennai has been reported by Venkatachalapathy et al.
(2010a, b, 2011). But there is little information on the PAHs
pollution in groundwater of the industrial areas of this major
Fig. 1 Sources of PAHs in the environment
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Environ Earth Sci
city. This study was carried out in Royapuram area where
petroleum product storing tanks are located. In the year
1914, during World War I, a German light cruiser Emden
opened fire on the oil tanks located in this area which cre-
ated huge destruction of these tanks (Srivathsan 2012).
Later, underground storage tank was used to store oil and it
was closed about 50 years ago, i.e. around 1963 (Clement
1993). With years to come, this area was sold to the people
and eventually got converted into residential plots (Clement
1993). Amutha et al. (2009) identified Perna viridis as a
biomarker for PHC from coastal water samples collected
from Royapuram area. Pollution due to iron in soil of this
area has been reported by a leading newspaper in the city
(Geeta 2003). The concentration of PAHs in groundwater of
this area was not reported and there are no other previous
scientific studies on PAHs contamination in groundwater
from this area apart from a preliminary study by Clement
(1993) reporting BTEX compounds in groundwater. Even
now, there are many oil storage tanks functioning to store
oil that is brought in ships and transferred to these tanks at
the Chennai harbour (Fig. 2). A detailed investigation is
essential to monitor the status of groundwater pollution with
respect to PAHs to take suitable measures in this area.
Hence, this study was carried out with an objective to
identify the extent of PAHs contamination in groundwater
of Royapuram area, Chennai, India.
Study area
Royapuram is located in the northern part of the Chennai
city, Tamil Nadu, India (Fig. 2). This area is bounded by
the Bay of Bengal in the east. Summer prevails from April
to June with temperature ranging between 38 °C and
42 °C. Winter prevails from November to January with
temperature between 18 °C and 34 °C. The annual rainfall
is about 1,200 mm which is mainly (60 %) due to the
northeast monsoon occurring during October to December.
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Environ Earth Sci
Fig. 2 Location of the study
area and monitoring wells
The other 40 % of the rainfall is contributed by the
southwest monsoon occurring during July to September.
Topographically this area gently slopes towards the east.
This area is highly populated and hence it is much modified
by human activities. Many small and big industries are
located in this area. There are many oil storage tanks
functioning in this area.
This area is a gently sloping coastal plain consisting of
sand, clay and shale of marine origin. In some places, sand
and silt are present up to 15 m followed by thin layer of
silty clay. Beneath the silty clay, silty sand with a thickness
ranging from 4 to 12 m is present. Highly weathered rock
is present at about 40 m below ground surface with a
thickness ranging from 1 to 4 m followed by moderately
weathered rock. Groundwater occurs under unconfined
conditions in this unconsolidated formation. Transmissivity
varies between 6 and 872 m2/d and the storativity between
2.9 9 10-4 and 4.5 9 10-3 (CGWB 2008). Hydraulic
conductivity in the formation is expected to vary between
10 and 60 m/day. Generally groundwater occurs at a
shallow depth of less than 10 m. The groundwater flow is
towards the sea. Rainfall is the principal source of
recharge. The wells in this area generally yield up to 7lps
(CGWB 2008).
Materials and methods
Followed by a field survey and based on the measurement
of electrical conductivity (EC in lS/cm), groundwater
samples were collected from 24 bore wells located in this
area during February 2001 (Fig. 2). The EC and pH were
measured in the field using Eutech portable digital meters.
The pH meter was calibrated before use by 4.01, 7 and
10.01 buffer solution. The EC meter was calibrated using
84 and 1,413 lS/cm conductivity solution. Groundwater
samples for major ion analysis were collected in HDPE
bottles of 500 ml capacity. For the PAHs analysis,
groundwater samples were collected in glass bottles of 2 l
capacity. The bottles were labelled properly and brought to
the laboratory for analysis. Calcium and magnesium were
determined with 0.05 N EDTA solution titrimetrically.
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Sodium and potassium were measured using flame pho-
tometer. Carbonate and bicarbonate were estimated by
titration with 0.01 N H2SO4. Chloride was determined by
titrating against AgNO3 and sulphate was determined using
spectrophotometer. All the procedures followed for the
analysis of groundwater samples are as per APHA (1998).
To ascertain the accuracy of the analytical experiments, the
ion balance error was calculated and was found to be
within ±5 %. Total dissolved solids (TDS) was calculated
using the measured EC values by the relationship, TDS
(mg/l) = EC (lS/cm) 9 0.64 (Lloyd and Heathcote 1985).
Total Hardness (TH) was calculated by TH (mg/
l) = 2.497 Ca (mg/l) ? 4.115 Mg (mg/l) (Sawyer and
McCarty 1967). The total petroleum hydrocarbon (TPH)
was determined in 14 samples by synchronous scanning
fluorescence spectroscopy.
In January 2011, 5 groundwater samples were collected
from the same area (Fig. 2) and analysed only for PAHs
concentration following protocol EPA 3510C/8100. The
situation was further analysed by a field visit during August
2012. Nearly 22 houses having bore wells for pumping
groundwater for their daily activities were investigated for
the physical characteristics such as colour and odour.
Results and discussion
The pH of groundwater varied from 7 to 9.6 with a mean of
8.4 during the year 2001. Thus most of the groundwater
samples are alkaline in nature. The EC of groundwater
gives a general idea on the overall groundwater quality in
an area as it depends on the concentration of the total ions
and temperature of the groundwater. The EC in this area
varied from 480 lS/cm to 9,700 lS/cm. Based on the EC,
the groundwater is classified into four types—desirable
(\750 lS/cm at 25 °C), permissible (750–1,500 lS/cm at
25 °C), not permissible (1,500–3,000 lS/cm at 25 °C) and
hazardous ([3,000 lS/cm at 25 °C) for drinking and
domestic purpose. About 33.3 % of the groundwater
samples were permissible and 41.7 % were not permissible
for drinking. Also, 20.8 % of the groundwater samples
were hazardous for domestic purpose. Considering the
dependence on groundwater by the people of this area for
their domestic needs, it is clear that the groundwater was
not suitable in 62.5 % of sampling wells for domestic use
as they exceed the permissible limit of 1,500 lS/cm of EC
according to the Bureau of Indian Standards (BIS 1983).
TDS and TH
The groundwater type and quality was also understood
based on the classification of TDS by Davis and DeWiest
(1966); Freeze and Cherry (1979) and TH by Sawyer and
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McCarty (1967). TDS varied from 307 mg/l to 6,208 mg/l
with a mean of 1,452 mg/l for the year 2001. According to
Davis and DeWiest (1966) classification, 4.2 % of the
groundwater samples were desirable for drinking
(\500 mg/l) and 33.3 % were permissible for drinking
(500–1,000 mg/l). However, 54.2 % were useful for irri-
gation (1,000–3,000 mg/l) and 8.3 % were unfit for irri-
gation ([3,000 mg/l). Since this is a residential area,
62.5 % of groundwater is considered unfit for drinking, i.e.
[1,000 mg/l. Groundwater in this area was fresh (37.5 %
\1,000 mg/l) to brackish (62.5 % between 1,000 and
100,000 mg/l) as per Freeze and Cherry (1979) classifica-
tion. TDS beyond 500 mg/l in drinking water may decrease
palatability and may cause gastrointestinal irritation (BIS
2003). TH calculated based on the calcium and magnesium
concentration in groundwater varied from 110 to 345 mg/l.
The groundwater was moderately hard in 16.7 %
(75–150 mg/l), hard in 62.5 % (150–300 mg/l) and very
hard in 20.8 % ([300 mg/l) in this area based on the
classification suggested by Sawyer and McCarty (1967).
The TH in drinking water should not exceed 300 mg/l as
per BIS (BIS 2003) as it may cause encrustation in water
supply structures and adverse effects on domestic use.
Major ions
The groundwater type in this area was identified for the
year 2001 based on the Piper Trilinear diagram (Piper,
1944) (Fig. 3). Na–Cl was the dominant groundwater type
and followed by Ca–Mg-Cl type of groundwater. As this
area is located very close to the coast, influence of seawater
is the reason for Na–Cl dominant nature of groundwater.
The minimum, maximum and mean concentration of major
ions is given in Fig. 4. The general order of dominance
of ions is Na [ Mg [ Ca [ K for cations and
Cl [ SO4 [ HCO3 for anions. The concentration of cal-
cium and magnesium varied from 16 to 50.1 and 13.3 to
53.4 mg/l, respectively, with a mean of 34 and 36 mg/l.
Calcium was within the desirable limit of 75 mg/l (BIS
2003) while 16 groundwater samples exceeded the desir-
able limit of 30 mg/l for magnesium. Sodium exceeded the
maximum desirable limit of 200 mg/l (WHO 1993) in 4
(16.7 %) groundwater samples and potassium exceeded the
limit of 12 mg/l (WHO 1993) in 19 (79.2 %) groundwater
samples. The occurrence of sodium in groundwater was in
the range of 15–526 mg/l with a mean of 151 mg/l. The
minimum, maximum and mean concentration of potassium
in groundwater was 5.6–76 mg/l with a mean of 32 mg/l.
Carbonate was absent in the groundwater of this area and
bicarbonate varied from 24 to 154 mg/l. The mean con-
centration of bicarbonate was 35 mg/l. Chloride concen-
tration varied between 49 and 857 mg/l and sulphate
between 53 and 148 mg/l. The mean concentration of
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chloride and sulphate was 339 and 73 mg/l, respectively. Table 1 Concentration of TPH
Sample no TPH (lg/l)
The concentration of chloride was above the desirable limit (lg/l) in groundwater samples
collected in the year 2001 A1 5.8
of 250 mg/l (BIS 2003) in 13 groundwater samples while
all the groundwater samples were within the desirable limit A2 12.9
of 200 mg/l with respect to sulphate. In general, the A3 1.6
groundwater quality can be classified as poor to moderate A4 BDL
in this area. A6 BDL
A7 BDL
Hydrocarbons in groundwater A8 BDL
A10 BDL
Fourteen groundwater samples collected in 2001 were A11 BDL
analysed for the total petroleum hydrocarbons (TPH) and A12 BDL
the results are given in Table 1. Out of the 14 samples A13 BDL
analysed, five samples had TPH ranging from 1.6 to A16 12.0
12.9 lg/l. These samples are from wells located close to A17 11.5
the ancient underground storage tank that was abandoned A18 BDL
around the year 1963 (Clement 1993) implying that the
leakage from this structure has resulted in the
Table 2 Concentration of PAHs (lg/l) in groundwater samples col-
lected in the year 2011
PAHs Sample number (all values in lg/l)
B1 B2 B3 B4 B5

Naphthalene BDL BDL BDL BDL BDL

Acenaphthylene BDL BDL BDL BDL BDL
Acenaphthene 95.2 98.9 BDL 120.4 BDL
Fluorene BDL 95.5 BDL 142.3 BDL
Phenanthrene 122.3 106.8 115.6 143.2 127.6
Anthracene BDL BDL BDL 127.0 BDL
Fluoranthene 103.5 BDL 104.0 BDL BDL
Pyrene BDL BDL BDL BDL BDL
Benzo (a) anthracene BDL BDL BDL BDL BDL
Chrysene BDL BDL BDL BDL BDL
Benzo (b) fluoranthene BDL BDL BDL BDL BDL
Benzo (k) fluoranthene BDL BDL BDL BDL BDL
Benzo (a) pyrene BDL BDL BDL BDL BDL
Indeno (1,2,3 cd) pyrene BDL BDL BDL BDL BDL
Fig. 3 Groundwater type based on samples collected in the year 2001 Dibenzo (ah) anthracene BDL BDL BDL BDL BDL
Benzo (ghi) perylene BDL BDL BDL BDL BDL

contamination of groundwater with TPH. In the year 2011,

Fig. 4 Minimum, maximum and mean concentration of major ions in
groundwater in the year 2001
the quality of groundwater was analysed based on the
hydrocarbon content. Five groundwater samples were col-
lected from the same area and analysed for 16 PAHs
(Table 2). Eleven PAHs analysed were absent in the
groundwater. Acenaphthene, fluorene, anthracene and flu-
oranthene were present in three, two, one and two
groundwater samples, respectively. Phenanthrene was
present in all the five groundwater samples. According to
the drinking water quality standards, PAHs should not be
present in groundwater used for drinking purpose (BIS

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Fig. 5 Photographs showing
thin film of oil floating on
groundwater during August
2012
Fig. 6 Demarcation of areas
based on smell and presence
of oil in groundwater during
August 2012
2003). This shows that traces of hydrocarbons are still
persistent in groundwater even after 10 years. However, in
the year 2001 TPH in groundwater was analysed whereas
in 2011 PAHs was analysed. There is no evidence that TPH
and PAHs contamination leaked into groundwater during
the same event. Figure 2 shows that samples taken in 2001
were taken in the eastern side of the ancient underground
storage tank and its surroundings, whereas samples taken in
2011 were taken close to the comparatively newer oil
storage tanks located along the flow direction. Hence,
PAHs contamination of the groundwater could also be due
to leakage of the current practices of oil storage in tanks
near the harbour.
During field investigation, representative elderly resi-
dents were chosen and were enquired about the ground-
water quality in the past. It is understood from the residents
that the groundwater quality was poor since the last five
decades, i.e. from 1960s. They have reported that oil used
to be floating on the vessels filled with groundwater. But
the situation has improved from the olden days and the
groundwater was better for household use. Possibly due to
groundwater flow and constant pumping over the years, the
groundwater quality has improved in the northwestern parts
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of the study area. This study indicates that the level of
contamination has significantly reduced over the entire
area. The groundwater that was contaminated by PAHs and
TPH due to leakage from the underground storage tank in
the western part has moved towards the east due to the
hydraulic gradient and also pumping of contaminated water
for different uses would have resulted into lowering of
concentration of PAHs in the western part of the area.
The smell and colour of groundwater and the visible thin
layer of oil on top of the water collected from the eastern
parts of the study area during the year 2012 also rely upon
the fact that the current practices of oil storage in huge
tanks may also be the reason for groundwater contamina-
tion (Fig. 5). These areas have restricted access and hence
groundwater or soil samples could not be collected from
the site where the tanks are located. The source for the
constant presence of hydrocarbons in this area may not
only be the leaks from the underground storage tank. This
may also be due to the presence of huge oil storage tanks
that are in use now. These tanks are used to store oil which
is transported by ships into and from the Chennai harbour.
The spillage during these activities has resulted in oil
pollution which is visible in this area. This has also been
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Environ Earth Sci
reported by Amutha et al. (2009). Also, PHC were recorded
in the Chennai harbour sediments by Venkatachalapathy
et al. (2010a) ranging from 10,030 to 39,790 lg/l. So these
activities may also be the source of groundwater contam-
ination in this area.
In the field investigation carried out by physical exami-
nation of groundwater for colour and smell of oil in 22 bore
wells in August 2012, it was observed that the groundwater
was colourless to pale yellow in the wells located from the
west of the study area to the east. Groundwater which was
colourless after pumping turned turbid or pale yellow after
1 min of collection. This is due to the presence of iron in the
groundwater which has been reported in many parts of
Chennai (CGWB 2008). Iron is present in groundwater due
to the weathering of iron bearing minerals/rocks and due to
the contribution from sediments. Iron normally occurs in
the sediments as Fe3?. Due to microbial activities,
groundwater contaminated with hydrocarbons results in
reducing conditions and is with poor oxygen content. Under
these conditions, iron from the aquifer materials gets
reduced to soluble Fe2?. Iron which normally exists in
water as soluble ferrous iron (Fe2?) does not impart any
colour to the water. When this water comes in contact with
oxygen in air the ferrous iron gets oxidised to ferric iron
(Fe3?) which turns the water from pale yellow to reddish
brown. This ferric iron is insoluble and precipitates as
yellow salts in the containers and storage tanks. This water
cannot be used even for laundry purposes as it may impart
the colour to the clothes as permanent stains. The smell of
oil was mild in the west of the study area to prominent in the
eastern part where the oil storage tanks are located now. In
the northern part the groundwater had no smell which may
imply that the groundwater where the underground storage
tank was located has improved due to constant pumping by
the residential houses which has removed most of the TPH
leaving traces. Observation of overhead water storage tanks
in the eastern part of the study area had oil that was floating
as a thin film in the tank and the colour of the water was
yellow (Fig. 5). The area with wells having mild smell of oil
to visible floating of oil was demarcated as shown in Fig. 6.
PAHs are a concern in environmental media such as
groundwater. Since PAHs should be completely absent in
drinking water as they are carcinogenic, it is important that
the people of this area are advised not to use the ground-
water for drinking and cooking purpose. Also alternate
source of water supply has to be provided to the residential
areas.
Conclusion
Groundwater quality was assessed in an industrialised area
in Chennai metropolitan city with an objective to
understand the distribution and sources of PAHs contami-
nation over a period of 12 years by the observations made
in the years 2001, 2011 and 2012. The major groundwater
type was Na–Cl which is mainly due to the influence of
seawater as this area is bounded by sea in the east. About
62 % of the groundwater was not suitable for drinking and
domestic purpose based on TDS in 2001. Of the 14
groundwater samples analysed, five had TPH which ranged
from 1.6 to 12.9 lg/l. The source for the presence of TPH
in groundwater was the underground storage tank which
served to store oil over five decades back. Leakage from
this tank had contaminated the groundwater. However, the
level of contamination has reduced due to natural
groundwater flow as well as pumping of groundwater for
various uses. In 2011, five PAHs namely acenaphthene,
fluorene, anthracene, fluoranthene and phenanthrene were
observed by chemical analysis in the groundwater collected
from this area. Physical examination of 22 groundwater
samples in 2012 was carried out and strong smell of oil was
observed in groundwater samples located in the eastern
part of the area while the area where the ancient under-
ground storage tank was located had mild odour. This is
due to the presence of oil storage tanks near the coast
which receive oil from the ships. The spillage during
loading and unloading or any leaks which has been left
unnoticed may also be the reason for the presence of oil
smell particularly of diesel in groundwater in the eastern
part. The western part of this area seems to have got rea-
sonably cleaned by the continuous pumping activity over
50 years by the local residents which has removed all the
oil leaving traces along with the groundwater. However, it
is necessary to address this issue to safeguard the
groundwater resource. Also, it is necessary to study the soil
and sediment samples for the presence of PAHs.
Acknowledgments The authors would like to thank the Department
of Science and Technology’s Funds for Improvement in Science and
Technology scheme (grant no. SR/FST/ESI-106/2010), University
Grants Commission’s Special Assistance Programme [grant no. UGC
DRS II F.550/10/DRS/2007(SAP-1)] and University Grants Com-
mission’s Centre with Potential for Excellence in Environmental
Science [grant no. F.No.1-9/2002 (NS/PE)] for their financial support
which helped in creating facilities to carry out this work. The second
author wishes to thank Dr. Prabhakar Clement, Department of Civil
engineering, Auburn University, Auburn, USA, who motivated him to
take up this work initially and Dr. Hannes Neugebauer, Hydrogeol-
ogist, DB Netz AG, Regionalbereich Süd, Munich, Germany, for his
suggestions. The authors also thank the two anonymous reviewers for
their constructive comments which helped in improving the
manuscript.
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