Acid leachable trace metals in sediment cores from Sunderban mangrove wetland, India: an approach...

Acid leachable trace metals in sediment cores from SunderbanMangrove Wetland, India: an approach towards regularmonitoring

M. P. Jonathan • S. K. Sarkar • P. D. Roy •

Md. A. Alam • M. Chatterjee • B. D. Bhattacharya •

A. Bhattacharya • K. K. Satpathy

Accepted: 26 September 2009 / Published online: 14 October 2009

� Springer Science+Business Media, LLC 2009

Abstract The paper presents the first document to iden-

tify the enrichment pattern of acid leachable trace metals

(ALTMs) such as Fe, Mn, Cr, Cu, Ni, Pb, Cd, Co, Mo, Ag,

As and Ba and their relationship with sediment quality

parameters (pH, organic carbon, carbonates and texture) in

core sediments (\63 lm particle size) from Indian Sun-

derban mangrove wetland, formed at the estuarine phase of

the river Hugli (Ganges). Textural analysis reveals an

overall predominance of mud. The results indicate that the

change in pH values causes coagulation and precipitation

of ALTMs. Fe and Mn have fairly close distribution pat-

terns of enrichment in surface layers which might be

ascribed to early diagnetic processes. The most prominent

feature of ALTMs is the enrichment of Fe, Mn, Cr, Cu, Ni,

Pb, and Ba in the surface–subsurface layers in the sediment

cores, which is mainly attributed to the intense industrial

and agricultural activities as well as drainage of untreated

domestic sewage to this coastal region. The ALTMs also

indicate their association with organic carbon and Fe–Mn

oxyhydroxides. The enrichment is well—supported by the

correlation, grouping and clustering of ALTMs in statisti-

cal analyses. Anthropogenic Factor values indicated

ALTMs enrichment for all trace metals due to intense

anthropogenic activities. Overall higher values of ALTMs

in sediments in comparison to other Indian coastal regions

indicate that they are mainly due to the uncontrolled

anthropogenic activities in this mangrove estuarine com-

plex. Statistical analyses suggest that five ALTMs (Cu, Pb,

As, Mo, Ba) are attached to the organic particles and the

clustering of elements separately also indicates that they

are from external source. The result of the present study

suggests the need for a regular monitoring program which

will help to improve the quality of this potential wetland.

Keywords Acid leachable � Trace metals �Core sediments � Enrichment � Sunderban wetland

Introduction

Trace metals have a great ecological significance due to

their toxicity and tendency to accumulate in both sediment

and biota. These elements are not biodegradable and

undergo a global ecological cycle. Sediments are the

important component of ecosystem in which toxic com-

pounds accumulate through complex physical and chemi-

cal adsorption mechanisms depending on the properties of

the adsorbed compounds and the nature of the sediment

matrix (Ankley et al. 1992; Leivouri 1998; Maher and

Aislabie 1992). Sediment analysis plays an important role

in the assessment of metal contamination in aquatic envi-

ronment (Borovec 1996; El-Nemr 2003; El-Nemr et al.

M. P. Jonathan

Centro Interdisciplinario de Investigaciones y Estudios sobre

Medio Ambiente y Desarrollo (CIIEMAD), Instituto Politecnico

Nacional (IPN), Calle 30 de Junio de 1520, Barrio la Laguna

Ticoman, 07340 Del. Gustavo A. Madero, Mexico, D.F., Mexico

S. K. Sarkar (&) � Md. A. Alam � M. Chatterjee �B. D. Bhattacharya � A. Bhattacharya

Department of Marine Science, University of Calcutta,

35 Ballygunge Circular Road, Calcutta 700 019, India

e-mail: [email protected]; [email protected]

P. D. Roy

Departamento de Geoquımica, Instituto de Geologıa,

Universidad Nacional Autonoma de Mexico, Ciudad

Universitaria, 04510 Mexico, D.F., Mexico

K. K. Satpathy

Indira Gandhi Centre for Atomic Research, Environmental and

Industrial Safety Section, Kalpakkam 603102, Tamil Nadu, India

123

Ecotoxicology (2010) 19:405–418

DOI 10.1007/s10646-009-0426-y

2006; Wardas et al. 1996). The trace metals transported

from human activities are often associated with organic

matter, absorbed on Fe–Mn hydrous oxides, or precipitated

as hydroxides, sulphides and carbonates (Forstner 1983).

The importance of leaching studies has gained signifi-

cant attention in recent decade due to the assessment of

metals present in different fractions in the sediment. The

leaching of metals provides an accurate data base of the

bioavailable metals in any aquatic environment which are

often readily available to organisms affecting them

directly. This bioavailable fraction is thus defined as the

amount of metal that can be exchanged with biological

organisms and be incorporated into their structure (Vang-

ronveld and Cunnihgham 1998). Reporting the actual metal

concentrations within the leached fraction alone seems a

more logical way to eliminate the need for mathematical

corrections or physical separations of the final output. This

fraction depends on the association of the elements with

particles, the binding strength and the water properties such

as pH, and the redox potential, salinity, dissolved metal

species which are in touch with the solid phase (Filgueiras

2004).

Previous studies on the pollution status of Sunderban

wetland along with the adjacent Hugli estuary have

revealed an elevated concentrations of total trace metals

(Cu and Zn) and metalloid (As) in surface and core sedi-

ments exceeding the Effects-Range Low ER-L) values

implying occasional or frequent biological effects (Sarkar

et al. 2004; Chatterjee et al. 2007, 2009a, b). Hence it is

deemed necessity to identify the enrichment pattern of

ALTMs (or labile metals) in the sediments to ascertain the

lability and mobility of these metals and their relationship

with sediment quality parameters. To the best of our

knowledge, this is the first report on the detailed account of

ALTMs in core sediments in Sunderban wetland.

Materials and method

Study area

The Indian Sunderban (21�310600 to 22�1201400N and

88�1102800 to 89�0505300E), formed at the estuarine phase of

the Hugli river of an area of *9,600 km2, is a mangrove

wetland belonging to the low-lying coastal zone. This is

one of the most dynamic, complex and vulnerable biocli-

matic zone in a typical, tropical geographical location in

the northeastern part of the Bay of Bengal. It is a tide-

dominated estuarine wetland set on the lower deltaic plains

of Ganges–Brahmaputra Rivers. The wetland is charac-

terized by a complex network of tidal creeks, which sur-

round hundreds of tidal islands exposed to different

elevations at high and low semi-diurnal tides.

This coastal environment suffers from environmental

degradation due to rapid human settlement, tourism and

port activities, and operation of excessive number of

mechanized boats, deforestation and increasing agricultural

and aquaculture practices. The ongoing degradation is also

related to huge siltation, flooding, storm runoff, atmo-

spheric deposition and other stresses resulting changes in

water quality, depletion of fishery resources, choking of

river mouth and inlets, and overall loss of biodiversity as

evident in recent years (Sarkar and Bhattacharya 2003,

2007). A significant ecological change is pronounced in

this area due to huge discharges of untreated or semi-

treated domestic and municipal wastes as well as effluents

from multifarious industries (as shown in Fig. 1) carried by

the rivers as well as contaminated mud disposal from

harbor dredging (Sarkar et al. 2007)

Six sampling sites were selected covering both eastern

and western flank of Sunderban namely, Lot 8 (S1), Gan-

gasagar (S2), Jharkhali (S3), Gosaba (S4), Canning (S5) and

Dhamakhali (S6). The topographical and physico-chemical

characteristics of all the six sites have already been

reported in previous publications (Chatterjee et al. 2009a, b;

Sarkar et al. 2007). The sampling stations belong to dis-

tinctive geographic, geomorphic and sedimentological

settings with variations of energy domains characterized by

wave-tide climate. The variations of physical processes

such as suspension-resuspension, lateral and vertical

transport by biological activities (bioturbation), floccula-

tion and deflocculation of mud clasts result in a spatial

variation of the substratum behavior both in local and

regional scales. The sites have diverse human interferences

with a variable degree of exposure to heavy metal and trace

organic contamination. Moreover, the sites can be differ-

entiated in terms of river discharge, erosion, flocculation

and atmospheric deposition. The Gangasagar site is located

at the southwestern edge of Sagar Island and faces the

eastern margin of the funnel-mouthed Hugli (Ganges

River) estuary. The site experiences high turbidity

throughout the year, mainly due to its location in the

confluence of Hugli River and Bay of Bengal (Fig. 1). The

Lot 8 site is located on the upstream side of Gangasagar.

The rest of the four stations occur more towards the eastern

part of the Sunderban wetland, by the sides of the distrib-

utory channel and the tidal river systems, infested with

mangrove vegetation.

Sample collection

Core samples were collected from the six selected sites

with the help of a steel corer (40 cm in length and 5 cm in

diameter) which is gently pushed into the sediments and

retrieved back in sealed position. They were transported in

frozen conditions (-4�C) to the laboratory. The core length

406 M. P. Jonathan et al.

123

varied between stations (maximum depth of 40 cm) due to

variations in the nature of substratum. The water on top

was decanted and the samples were sub-sampled at 4 cm

interval with the help of PVC spatula. A thin film of sed-

iment next to the core was left to avoid contamination. The

samples were oven dried (40�C) and were disaggregated

using an agate mortar and pestle, sieved through 63 lm

sieve, which was stored in pre-cleaned inert polypropylene

bags for chemical analysis. All glass wares used in col-

lection and laboratory were pre-cleaned to minimize

external contamination. The sediment samples were char-

acterized for particle size, pH and organic carbon and

carbonate and the detailed experimental procedures are

presented elsewhere (Chatterjee et al. 2007). Unfortunately

sediment dating was not done since the samples were

collected from meso-macrotidal environment, which does

not suit the dating techniques and the loss of the uppermost

cores (Binelli et al. 2007).

Analytical methods

The acid leachable fraction extracts almost the whole

degree of elements as it is absorbed by sediments depicting

the contamination of an area (Agemian and Chau 1976;

Taliadouri 1995; Janakiraman et al. 2007). The extraction

of acid leachable metals was done by weighing 5 g of dry

sediment sample in a 100 ml plastic bottle in which 75 ml

of 0.5 N HCl was added and after mechanically shaking for

16 h it was filtered with Whatman ‘A’ filter paper. The

final filtered solution was analyzed for acid leachable Fe,

Mn, Cr, Cu, Ni, Pb, Cd, Mo, Ag, As and Ba in ICP-MS.

High purity standards (NIST, USA) were used and standard

Fig. 1 Study area map with

sample locations in Sunderban

mangroves, East coast of India

Acid leachable trace metals in sediment cores 407

123

solutions were prepared. The accuracy of the analysis was

determined by standard addition method and the recovery

of elements was 75–97%. A standard reference material

MAG1 was used to ensure the quality control and accuracy

of the analysis (Table 1). The samples were analyzed thrice

and the average of the analysis is presented in this study.

Statistical procedures

In order to establish the geochemical processes and

enrichment of metals (Bridgeman 1992), correlation coef-

ficient matrix and R-mode factor analysis with varimax

rotation were applied to the core samples to know the

processes in six different hydrodynamic conditions (SPSS

1995). For generating the dendrogram, data were stan-

dardized using the formula : X-l/r (where X is the vari-

able, l is the mean and r is the standard deviation).

Significant differences among sampling sites were checked

by main effects analysis of variance (ANOVA) usingP16PAHs as variables and stations and depth profiles as

different factors. The data set was analysed with principal

component analysis (PCA) which is often used as an

explorative tool to extract components needed to explain

variance of observed data. All statistical analyses were

carried out by the software package STATISTICA 6.0.

Results and discussion

Sediment geochemistry

Textural parameters like sand and mud (silt ? clay) as well

as distribution patterns of pH, organic carbon and carbon-

ate of six sediment cores are presented in Tables 2 and 3

respectively.

Regarding textural composition, the four stations (S1–

S4) show variable admixture of sand, silt and clay with an

overall size range from sandy to clayey very fine. This

wide array of textural differences may be attributed to

vigorous estuarine mixing, suspension-resuspension and

flocculation-deflocculation processes. On the other hand,

the absolute dominance of sand (constituting [90% in

sediments) in the core sediments of Gangasagar (S2) may

be referred to its relatively high energy intertidal beach

settings which is influenced by waves and long-shore

currents that prevents deposition of fine-grained mud par-

ticles. The textural variations seem to have influenced the

trace metal accumulation in the core sediments (as shown

in Fig. 2a–k) involving certain complex physicochemical

processes. Interestingly, maximum concentrations of five

Table 1 Comparison of MAG1 certified values for total trace metals

Elements Present study MAG1

Fe2O3 (%) 6.68 6.80

MnO (%) 0.094 0.098

Cr (mg kg-1) 99.01 97

Cu (mg kg-1) 28.94 30

Ni (mg kg-1) 51.86 53

Pb (mg kg-1) 23.01 24

Cd (mg kg-1) 0.18 0.20

Mo NA –

Ag (mg kg-1) 0.074 0.08

As (mg kg-1) 8.09 9.2

Ba (mg kg-1) 472.56 479

Table 2 Down core variations of sediment texture in five short core samples from Sunderban mangrove region, India

Parameters Sand (%) Mud (silt ? clay) (%) Sediment texture

aSample nos.

Depth (cm)

S1 S2 S3 S4 S5 S6 S1 S2 S3 S4 S5 S6 S1 S2 S3 S4 S5 S6

0–4 4.24 32.24 5.16 41.16 99.43 45.16 95.76 67.76 94.84 58.84 0.56 54.84 SC CL FS FL S FL

4–8 2.60 63.56 1.84 45.88 95.13 32.24 97.40 36.44 98.16 54.12 4.87 67.76 FS SL SC SCL S CL

8–12 2.56 0.84 1.96 4.80 91.87 63.56 97.44 99.16 98.04 95.20 8.13 36.44 C SC SC C S SL

12–16 1.40 1.60 25.92 0.36 93.51 0.84 98.60 98.40 74.08 99.64 6.49 99.16 SC SC C SC S SC

16–20 9.84 1.44 26.56 0.44 94.10 19.80 90.16 98.56 73.44 99.56 5.90 80.32 FS SC C C S SLCL

20–24 4.80 2.48 20.88 0.60 93.98 4.24 95.20 97.52 79.08 99.40 6.02 95.76 C SC C CS S SC

24–28 8.64 2.36 1.16 1.20 – 2.60 91.36 97.64 99.04 98.80 – 97.40 SC SLCL SC SC – FS

28–32 5.96 2.44 1.88 7.36 – – 94.04 97.56 98.12 92.64 – – SC SC C CS – –

32–36 45.16 3.12 54.40 – – – 54.84 96.88 45.60 – – – FL CS S – – –

36–40 – – 37.70 – – – – – 62.30 – – – – – L – – –

a Site names: S1—Lot8; S2—Gangasagar; S3—Jharkhali; S4—Gosaba; S5—Canning; S6—Dhamakhali

Sediment textures: Sand S; Loam L; Sandy Loam SL; Coarse Loam CL; Fine Loam FL; Sandy Clay Loam SCL; Coarse Silt CS; Silty Clay Loam

SLCL; Fine Silt FS; Silty Clay SC; Clay C; Fine clay FC


123

Table 3 Down core variations of pH, organic carbon and carbonates in five short core samples from Sunderban mangrove region, India

Parameters pH Organic carbon (%) Calcium carbonate (%)

aSample nos. Depth (cm) S1 S2 S3 S4 S5 S6 S1 S2 S3 S4 S5 S6 S1 S2 S3 S4 S5 S6

0–4 8.7 8.1 8.1 8.2 8.5 8.2 0.66 0.79 1.60 0.90 0.61 0.80 5.6 5.2 1.6 2.4 2.0 1.6

4–8 8.9 8.1 8.0 8.1 8.3 8.2 0.33 0.69 1.40 0.73 0.59 0.76 5.6 5.2 2.0 6.8 6.0 1.2

8–12 8.7 8.2 8.2 8.2 8.4 8.1 0.62 0.81 1.10 0.71 0.57 0.78 6.4 5.2 6.0 2.8 2.4 2.0

12–16 8.7 8.1 8.2 8.3 8.5 8.1 0.24 0.74 1.20 0.73 0.53 0.74 4.8 7.2 3.2 1.2 2.4 2.0

16–20 8.8 8.0 8.1 8.3 8.5 8.2 0.29 0.79 1.30 0.73 0.53 0.67 4.8 5.2 3.2 2.4 4.0 1.6

20–24 8.6 8.2 7.4 8.3 8.4 8.4 0.66 0.83 2.60 0.84 0.53 0.74 6.4 6.8 0.8 3.2 3.6 1.6

24–28 8.5 8.1 6.8 8.3 – 8.3 0.18 1.09 3.07 0.82 – 6.8 5.6 2.4 3.2 – 0.4

28–32 8.6 8.4 6.5 8.2 – – 0.35 1.06 3.21 0.82 – – 4.8 5.2 2.0 2.8 – –

32–36 8.3 8.2 6.4 – – – 0.18 1.21 3.25 – – – 7.2 6.8 4.8 – – –

36–40 – – 6.6 – – – – – 3.52 – – – – – 4.4 – – –

a Site names: S1—Lot8; S2—Gangasagar; S3—Jharkhali; S4—Gosaba; S5—Canning; S6—Dhamakhali

Fig. 2 a–f Down core distribution of ALTMs (Fe, Mn, Cr, Cu, Ni, Pb) in Sunderban mangrove sediments (values expressed in mg kg-1).

g–k Down core distribution of ALTMs (Cd, Mo, Ag, As, Ba) in Sunderban mangrove sediments (values expressed in mg kg-1)


123

ALTMs (Cu, Ni, Pb, As and Ba) were recorded at Jharkhali

(S3) at 32–36 cm depth where the sediments are sandy in

nature but associated with higher values of organic carbon

(3.25%) and carbonate (4.8%) contents.

The pH values of core samples are mainly basic in

nature (pH from 8.1–8.9), excepting at Jharkhali station

(S3) where pH lies within the acidic range of 6.4–6.8 at a

depth of 24–40 cm. The acidic nature of the deeper sedi-

ment cores may be attributed to the oxidation of FeS2 and

FeS to Fe2SO42- through biogenic processes. Moreover,

the decomposition of mangrove litter and the hydrolysis of

tannin in mangrove plants also release various kinds of

organic acids (Liao 1990). The generally high pH values in

majority of the core samples are linked to the CO2- car-

bonate system in the area even though it is dominated by

the mangroves (e.g., Frontier and Pichod-Viale 1991). The

fluctuation in pH at Jharkhali (S3) also reflects the buffer-

ing capacity of saline and freshwater in the mangrove area

at deeper levels in core samples and, in addition, causes

coagulation, flocculation and co-precipitation of ALTMs

during estuarine mixing (Boyle et al. 1977; Boven et al.

2008).

The main reason for the high concentration of organic

carbon, carbonates and same ALTMS at S3 (Jharkhali) at

Fig. 2 continued


123

these depths of the lower stretch of the Bidya River pos-

sibly indicates a major event of flooding in the river that

appreciably inundated the mangrove region. The higher

content of sand also suggests that finer siliciclastic particles

of lower specific gravity could have been washed away

compared to the sand sized particles (Deflandre et al. 2002;

Shumilin et al. 2002).

Organic carbon (OC) values in the core samples are very

low varying from 0.18% at Lot 8 (S1) to 3.52% at Jharkhali

(S3) at a depth of 32–36 cm (Table 3) which was also

observed by previous workers from this wetland (Zuloaga

et al. 2009; Chatterjee et al. 2007). The prevalent low

values of organic carbon are mainly attributed to the

mixing processes and marine sedimentation at the sediment

water interface, where the rate of delivery, as well as the

rate of degradation by microbial-mediated processes, can

be high (e.g., Canuel and Martens 1993). These are also

probably related to the poor adsorbability of organics on

negatively charged quartz grains, which predominate in the

intertidal siliciclastic sediments of this estuarine environ-

ment (Sarkar et al. 2004). However, many fold increase

of OC in Jharkhali (S3) in deeper layers (2.60–3.52% at

20–40 cm) in comparison to other samples suggests that

sulfate reduction in the lower half is higher and input of

local rivers (from one side) is very rich in organic materials

as it runs through the agricultural and aquaculture ponds

(e.g., Ramesh 2003; Alongi et al. 2005).

Carbonates in the present study indicate a three fold

higher values (4.8–7.2%) in S1 and S2 than S3–S6 (0.4–6.0%;

Table 3). The higher values of S1 and S2 are due to the

proximity of the coastal area and also due to the re-precipi-

tation of carbonates in the reduced layers. The above infer-

ence is also very well supported by the alkaline nature of

sediments in the study area. Moderate enrichments of car-

bonates in the reduced layers are caused due to reprecipita-

tion and increase in alkalinity generated by the sulfate

reduction (Gaillard et al. 1989).

Down core profiles of ALTMs

The down core profiles of ALTMs Fe, Mn, Cr, Cu, Ni, Pb,

Cd, Mo, Ag, As and Ba is presented in Fig. 2a–k.

Fe and Mn

Fe and Mn have fairly close distribution patterns

of enrichment in surface/subsurface layers (*0–8 cm)

in sediment cores (Fe: 3,937–5,201 mg kg-1; Mn:

300–615 mg kg-1) at all the stations (excepting S2 and S5;

Fig. 2a, b) which might be due to the early diagnetic pro-

cesses as well as the strong association to the geochemical

matrix between the two elements. Klinkhammer et al.

(1982) and Santschi et al. (1990) asserted that Fe2? and

Mn2? species got precipitated in the top layers in mangrove

sediments as these elements diffuse upward. Again, the

synchronous decrease values for Fe (1,420 mg kg-1) and

Mn (87 mg kg-1) at Dhamakhali S6 in the same depth

profile (24–28 cm) is suggestive of the oxic/suboxic

interface (Santschi et al. 1990). The marginal low values of

Fe and Mn at *8–16 cm (Fe: 4,075–4,670 mg kg-1; Mn:

309–538 mg kg-1) suggest that the oxic-suboxic zone

exists almost equally in the same depth profile. However,

the concentration pattern of these metals in the lower half

of all the core samples (beyond 16 cm) does not exhibit

any major variation (Fe: 3,964–4,972 mg kg-1; Mn: 339–

537 mg kg-1) indicating that it is due to the metalliferous

sulfides that both the elements have similar behavior

(Taylor and Price 1983). This association is not unusual

and has been previously recognized by several authors

(Nohara and Yokota 1978; El-Sayed 1982; Abu-Hilal and

Badran 1990). In Gosaba (S4) and Gangasagar (S2),

increase in the concentration of Fe and Mn at 32–36 cm

and 20–24 cm depth respectively, indicates that recycling

is more intense under low oxygen conditions. High values

of Fe at S1, S4, and S6, could be mainly attributed to the

presence of floating old rusty and stranded barges in these

sites. These barges are the main sources for particulate Fe

which settle down and mix with the bottom sediments in

these regions. The precipitated Fe in the form of oxyhy-

droxides has the affinity to scavenge other metals such as

Cu, Pb, etc., as they pass through the water en route to the

sediment (Waldichuk 1985).

Cr, Cu, Ni, Pb, Cd, Mo, Ag As and Ba

The distribution pattern of seven ALTMs (Cr, Cu, Ni, Pb,

Ag, As and Ba) exhibits variations between sites and

depths in the core samples which is ascribed to the metal

deposition in mangrove sediments through natural pro-

cesses as well as anthropogenic activities (Fig. 2c–k;

Forstner and Wittman 1983). Different tidal and geomor-

phological settings and variations in hydrodynamic

regimes between the stations are also responsible for the

spatial variations of trace metals. Peak values of Cu, Ni,

Pb, Mo Ag, As and Ba in Jharkhali (S3) (at 32–36 cm

depth) indicate scavenging of trace metals by Fe and Mn

oxyhydroxides and are deposited as metal sulphides with a

common source of (Prohic and Kniewald 1987).

A synchronous elevation of seven ALTMs (Fe, Mn, Cr,

Cu, Ni, and Pb) was observed at the station Canning (S6) in

the surface/subsurface layer (0–8 cm), which indicates the

diagenetic redistribution of elements. The enrichment of

ALTMs at this site is mainly due to its moribund condition

where transportation and deposition of finer organic-rich

sediments take place throughout the year. The coincident

peaks of majority of the ALTMs at 32–36 cm at Gosaba


123

(S4) and Jharhali (S3) and 20–24 cm at Gangasagar (S2)

suggest the contribution of post-depositional effects, such

as reduction of sulphides and formation of metalliferrous

sulphides under anoxic conditions or reprecipitation of

trace metals on Fe/Mn oxides and oxyhydroxides coatings

(Millward and Moore 1982; Nath et al. 1989). In addition,

the low organic carbon content causes the redox cycling of

the metals to occur relatively deep in the core sediments

and the efficient trapping of the ions within the sediment

results in a build-up of the oxide concentrations at the sub-

oxic/anoxic boundary (Wang and Van Cappellen 1996).

Moreover, the enhanced values of trace metals are resulted

from an increase in anthropogenic fluxes related to the

urban and industrial development in the upstream of the

Hugli river estuary.

Distribution of Cr concentrations in the sediment core

indicates higher values in top layers (0–8 cm) at all six

sites in the following trend: S1: 13.1–14.3 mg kg-1; S2:

12.1–12.8 mg kg-1; S3: 14.1–15.7 mg kg-1; S4: 17.6–

18.2 mg kg-1; S5: 11.9–12.2 mg kg-1 and S6: 18.0–

19.8 mg kg-1 (Fig. 2c). The higher values suggest that it is

present as Cr (VI), which is relatively mobile and after

release in the pore waters, they migrate downward into the

reducing zone and precipitates again as Cr (OH)2 (Shaw

et al. 1990; Fig. 2c). The industrial processing of chromites

significantly enhances the environmental mobility of Cr

and in the wastewater from the industries, Cr (III) and

hydrolyzed forms of Cr (VI) is readily absorbed by hydrous

Fe and Mn oxides (Davis et al. 1996). The above inference

of steady higher values similar to the surface layers is due

to the migration of Cr species further down into the sedi-

ment column.

Vertical profiles of Cu indicate the relatively high acid-

leachable values in the top layer in Lot 8 (S1) (31.5–

48.6 mg kg-1), Jharkhali (S3) (36.7–51.6 mg kg-1) and

Canning (S5) (48.9–69.8 mg kg-1; Fig. 2d). This is due to

the presence of humic-copper complexes and indicates the

presence of anthropogenic input under reducing conditions

(Lu and Chen 1977). The potential anthropogenic con-

tributors of Cu are the use of antifouling boat paints in

harbor and tourist areas (Marmolejo-Rodriguez et al.

2007), industrial effluent discharge and input of untreated

domestic sewage, as the element has a preferential asso-

ciation with organic matter (Hirner et al. 1990). However,

Cu concentrations also exhibited higher values in the

reduced layers at 32–36 cm in S2 (33.7 mg kg-1) and S3

(78.4 mg kg-1), which are due to its absorption and

scavenging by Fe and Mn oxides and hydroxides (Prohic

and Kniewald 1987).

Like Cu, a similar trend of enrichment of Ni was also

observed in the top layer (0–8 cm) at same three sites (S1

7.6–8.4 mg kg-1; S4 36.7–51.6 mg kg-1 and S6 11.6–

11.9 mg kg-1). This indicates that it is also due to the

presence of a mobile fraction of these metals in sediments

successively bound to humic acids in the mangrove sedi-

ments (e.g., Calace et al. 2005; Fig. 2d–f). The higher Ni

values at the surface layer are also due to the effective

trapping of Ni in aerobic conditions in the oxic-suboxic

conditions in the study area (Klinkhammer et al. 1982;

Sawlan and Murray 1983). In addition, the results suggest

that the increase of Ni at Jharkhali (S4) and Canning (S6),

mean value 9.31 mg kg-1 and 10.37 mg kg-1 respec-

tively, is specifically linked to the anoxic conditions and

the addition of these elements is also due to the scavenging

of Fe–Mn oxides.

According to US NOAA’s sediment quality guidelines it

is observed that the prevalent acid leachable concentrations

of both Cu (at S1, S4, and S6) and Ni (at S4) in the top

layers of the sediment core (0–8 cm) have exceeded the

effects range-low values (ERL values; 34 lg g-1 for Cu

and 20.9 lg g-1 for Ni) indicating ecotoxicological risk to

the organisms (e.g., benthic polychaetes, gastropods and

bivalve molluscs) living in the sediments.

Profiles of Pb in the surface layers (0–8 cm) show rel-

atively higher concentrations at Canning (S5) (19.6–

21.2 mg kg-1) than Jharkhali (S3) (16.5–17.3 mg kg-1)

and are attributed to the local redox conditions, which

allowed Pb to be co-precipitated with Mn during Mn-oxide

formation in the surficial sediment. The Pb encountered in

the sediment cores is derived from lead-bound paint

industries and input of effluents from the thermal power

plants situated in the upstream of the Hugli River estuary

(as shown in Fig. 1) together with autoexhaust emission,

atmospheric deposition and operation of large number of

mechanized fishing boats in these areas (Settle and Pett-

erson 1982; Nolting and Helder 1991). The low values of

Pb at 12–16 cm in Gangasagar (S2) (11.2–11.9 mg kg-1)

and Jharkhali (S3) (10.7 mg kg-1) indicate diagenetic and

resuspension processes and the moderately high peaks at

20–24 cm in Lot. 8 (S1) (16.6 mg kg-1 and 28.6 mg kg-1)

and at 32–36 cm in Gangasagar (S2) and Jharkhali (S3)

(16.4 mg kg-1 and 28.6 mg kg-1) indicate that additional

Pb has reprecipitated around the redox boundaries (Lee and

Cundy 2001); the downward flux of Pb is bound to bio-

genic particles (Lambert et al. 1991). The steady increase

of Pb beyond 8 cm in all the core samples (Max. mg kg-1

S1: 16.56; S2: 16.37; S3: 28.59; S4: 15.54; S5: 17.37; S6:

18.92) indicates that it has reprecipitated along the redox

boundaries and the downward flux is bound to the biogenic

particles (Lee and Cundy 2001).

Likewise, the levels of Cd do not vary greatly in the core

profiles of all the six stations which might be due to

homogenous input of this metal in the wetland system. The

metal is normally released from the sediment and escapes

to the water phase due to degradation of organic debris in

the oxygenated surface layers, but as reducing conditions


123

exist in these sediments, a moderately high Cd in the top

layer of Canning (S6) persists (0.22 mg kg-1 at 0–5 cm)

(Gendron et al. 1986). Presence of Cd in this estuarine

environment can be linked to both natural and non-point

anthropogenic sources. Anthropogenic sources are con-

nected to pollution and land use in the watersheds draining

into estuaries while natural sources can be linked to river

runoff from cadmium-rich soils and leaching from bedrock

(e.g., Rainbow 1995).

Concentration of Ag varies from 0.079 to 0.325 mg kg-1,

with maximum mean value of 0.22 mg kg-1 recorded at

Gosaba (S4) at 32–36 cm depth where the value of OC

values are also high (1.21%). This elevated level of Ag is

linked with sewage outfalls as Ag is usually tightly bound to

sewage sludge (Reimann and de Caritat 1998). The possible

additional inputs are from the Damodar and Haldi rivers,

both of which drain the petrochemical and metallurgical

industrial belt of the hinterland of the estuarine region with

a wide range of pollutants (De et al. 1985).

Arsenic concentration in the core sediments varied from

1.74 to 8.46 (mg kg-1), reaching the maximum value of

4.57 mg kg-1 at Jharkhali (S3), almost double the values

present at four stations (S1 S2 S4 and S5). The average

concentration of core samples (in mg kg-1) S1: 2.07, S2:

2.83, S3: 4.57, S4: 2.68, S5: 2.55 and S6: 3.00 indicates that

the major part of As comes from the eastern side of the

wetland (where S3 and S6 are located). The sources of As

stem from anthropogenic activities like intense exploitation

of ground water, application of fertilizers and insecticides

as well as burning of coal for domestic purposes. An

overall uniform pattern of As distribution in sediments

implies that atmospheric deposition plays a major role in

this area in addition to the organic debris brought in by the

industrial output (e.g., Leoni and Sartori 1996, 1997).

The geochemical character of As suggests that it is

solublized through diagnetic processes in organic rich

mangrove sediments (Goessler et al. 1997; Kubota et al.

2001; Shumilin et al. 2005). Diffusion along the concen-

tration gradients in the interstitial water and secondary

accumulation of arsenic of the seafloor via co-precipitation

with iron oxyhydroxides or with insoluble sulfide in the

reducing environment below the sediment surface cannot

be excluded (Belzile and Tessier 1990; Caetano and Vale

2002).

The concentration pattern of Mo does not indicate any

major variations (0.01–0.45 mg kg-1) (except S3) (Fig. 2h)

suggesting that the major part of Mo is from the moderately

found anoxic sediments (as seen in S3) which comes in

contact with the oxygenated water. In addition, the Mo

concentration in the mangrove sediments is due to the

humic fraction in the sediments and the ability of organic

molecules to reduce MoO42- (Calvert et al. 1985; Francois

1988). Ba concentration pattern in the core sample

indicates a variation from 11.97 to 43.95 mg kg-1

(Fig. 2k). The down core profile and the average concen-

tration (mg kg-1 S1: 19.37, S2: 13.94, S3: 27.08, S4: 15.48,

S5: 13.54, S6: 17.57) indicates that even though the organic

carbon values are low, Ba is enriched due to the biogenic

Ba which are transported in association with skeletal

materials (Dehairs et al. 1980). In addition, the occurrence

of Ba is also absorbed onto the CaCO3 phases that are in

the sediments (Dymond et al. 1992). The higher values of

Ba are also due to the exploitation activities (petroleum)

and the use of barite in these industries in the upstream of

the estuary (e.g., Sharma et al. 1999; Holmes et al. 1974).

Statistical analyses

To evaluate the potential relationship with various ALTMs

(Fe, Mn, Cr, Cu, Ni, Pb, Cd, Mo, Ag, As, Ba), pH, textural

parameters (sand, mud), organic carbon and carbonates, a

correlation matrix analysis was worked out and presented

in Table 4. The association of pH with Fe (r2 = 0.76), Mn

(r2 = 0.74) clearly infers that they are due to the change in

the fresh/saline water interactions. Organic carbon in the

present study indicates that it exerts some control for

anthropogenic contributions (Cu: r2 = 0.67; Pb: r2 = 0.65;

As: r2 = 0.86; Mo: r2 = 0.85; Ba: r2 = 0.82) due to the

effluent discharged by various industries (e.g., Samuel and

Phillips 1988). The positive relationship of Fe and Mn with

Cr (r2 = 0.0.78, 0.70), Cd (r2 = 0.92, 0.93) and Ag

(r2 = 0.61, 0.66) indicates that they are closely associated

with Fe–Mn oxyhydroxides and also due to the change in

pH conditions in the mangrove sediments. The interme-

tallic association is as follows: Cr versus Cd (r2 = 0.93);

Cu versus Ni (r2 = 0.69), Pb (r2 = 0.86), Mo (r2 = 0.63),

As (r2 = 0.74), Ba (r2 = 0.76); Ni versus Pb (r2 = 0.76),

As (r2 = 0.59), Ba (r2 = 0.50); Pb versus Mo (r2 = 0.62),

As (r2 = 0.78), Ba (r2 = 0.83); Cd versus Ag (r2 = 0.52);

Mo versus As (r2 = 0.68), Ba (r2 = 0.79) and As versus

Ba (r2 = 0.84). The above association indicates that the

contamination is local and from multifarious industrial

sources in the region suggesting differential behavior in

different core samples at some depths which needs exten-

sive investigation through analysis of surface sediments to

identify the type of effluents during different period of

times. The inverse negative relationship of sand, mud with

the ALTMs in the present study suggest that these metals

are hosted as coatings in the sand fractions, minerals, rock

fragments and industrial wastes (Alvarez-Iglesias et al.

2000). The geochemical association of elements does vary

moderately which is associated with different factors, such

as differences in hydrodynamics, churning, erosion, bio-

turbation, periodic dredging (in river mouths) etc. This type

of association is not unusual and has been previously

reported by several authors (Abu-Hilal and Badran 1990;


123

Krauskopf 1965; Nohara and Yokota 1978; El-Sayed

1982).

The cluster diagram based on the linear pair coefficient

pair of correlation between different variables (Fig. 3) of

six different core samples forms two different clusters :

elemental association with sand and organic carbon (cluster I)

and association with mud, carbonate and pH (cluster II).

The association of Ni, Pb, Cu, Mo, Ba, As (contaminant

elements) in cluster I clearly suggests that they have a

common origin in the aquatic environment. In addition, the

association with sand also suggests that they are preferably

attached to the coarser grains and are recently deposited as

coatings. Moreover, the presence of organic carbon in this

cluster also infers that they are transported as organic

debris to the mangrove region. On the other hand, the

cluster II suggests that the combination of Fe–Mn with pH,

mud and carbonates suggest that the change in pH also

affects the association of ALTMs due to the presence of

carbonates. The close linkage distance of Cd, Cr, Ag

indicates that they are attached to the Fe–Mn hydroxides

and it is due to the higher mobility/geochemical nature in

the sediments.

Anthropogenic factor and comparison studies

Anthropogenic factor (AF) was calculated in order to know

the anthropogenic input of heavy metals in the studied core

samples using the following formula: AF = Cs/Cd, where

Cs and Cd refer to the concentrations of the elements in the

surface sediments and at the deepest part in the sediment

column (Szefer et al. 1995). In the case of AF, the enrich-

ment of the element is normalized relative to the depth in

the sediment core, when AF [1 for a particular element it

means that contamination exists; otherwise if AF B1, there

is no metal enrichment of natural anthropogenic origin

(Ruiz-Ferrnandez et al. 2001). The calculated AFs for trace

Table 4 Correlation matrix data of core samples (S1–S6) from the Sunderban mangrove region, east coast of India

pH Org.C CO3 Fe Mn Cr Cu Ni Pb Cd Mo Ag As Ba

pH 1.00

Org.C -0.94*�� 1.00

CO3 – – 1.00

Fe 0.76*�� -0.77*�� – 1.00

Mn 0.74*�� -0.77*�� – 0.81*�� 1.00

Cr 0.44*� -0.46*�� – 0.78*�� 0.70*�� 1.00

Cu -0.67*�� 0.67*�� -0.36* -0.44*� – – 1.00

Ni -0.43*� 0.34* -0.30* – – 0.36* 0.69*�� 1.00

Pb -0.67*�� 0.65*�� – -0.46*� – – 0.86*�� 0.76*�� 1.00

Cd 0.58*�� -0.62*�� – 0.92*�� 0.80*�� 0.93*�� – – – 1.00

Mo -0.77*�� 0.85*�� – -0.82*�� -0.72*�� -0.59*�� 0.63*�� – 0.62*�� -0.72*�� 1.00

Ag 0.48*�� -0.48*�� – 0.61*�� 0.66*�� 0.36* -0.18* – – 0.52*�� -0.45*� 1.00

As -0.89*�� 0.86*�� – -0.71*�� -0.63*�� -0.38*� 0.74*�� 0.59*�� 0.78*�� -0.51*�� 0.68*�� -0.40*� 1.00

Ba -0.78*�� 0.82*�� – -0.68*�� -0.56*�� -0.40*� 0.76*�� 0.50*�� 0.83*�� -0.55*�� 0.79*�� -0.38*� 0.84*�� 1.00

Sand and mud has no significance. n = 49; p \ 0.05*; 0.01�; 0.001�

Fig. 3 Results of cluster

analysis based on complete

linkage method for core samples

in Sunderban wetland


123

elements in the six core samples are as follows: S1: Mo

(13.17) [ Cu (2.66) [ Ag (1.48) [ Ba (1.30) [ Pb

(1.29) [ Ni (1.26) [ Cr (1.21) [ Cd (1.20) [ Mn (1.18) [Fe (1.13) [ As (1.09); S2: Mo (1.15) [ Fe (0.81) [ Mn

(0.78) [ Ba (0.74) [ As (0.72) [ Pb (0.71) [ Cr (0.71) [Ni (0.71) [ Ag (0.70) [ Cd (0.67) [ Cu (0.45); S3: Cu

(1.82) [ Ba (1.27) [ Cr (1.22) [ Ag (1.22) [ Pb (1.21) [Mn (1.19) [ Ni (1.11) [ Cd (1.04) [ Fe (1.03) [ As

(0.96) [ Mo (0.33); S4: Fe (0.96) [ Cr (0.87) [ Cd

(0.86) [ Ba (0.85) [ Ni (0.84) [ Mn (0.83) [ As (0.76) [Pb (0.72) [ Cu (0.70) [ Ag (0.59) [ Mo (0.45); S5: Ba

(1.35) [ Cr (1.32) [ Cd (1.28) [ Ni (1.26) [ Ag (1.24) [Pb (1.23) [ Mn (1.21) [ Fe (1.12) [ As (1.03) [ Cu

(0.94) [ Mo (0.90) and S6: Ag (1.24) [ Mn (1.16) [ Fe

(1.07) [ Cd (1.05) [ Cr (1.04) [ As (0.74) [ Pb (0.72) [Ba (0.67) [ Ni (0.64) [ Cu (0.60) [ Mo (0.36) respec-

tively. The higher values of AFs ([1) in all the core samples

indicate that the area is affected by the heavy input of

industrial effluents from the industries situated in the

upstream side of the feeding rivers in the mangrove region.

The comparison of ALTMs in the estuarine, mangrove,

and coastal regions in the east coast of India are presented

in Table 5. The results indicate approximately a three fold

increase for Fe, Cr, Cu, Ni and a two fold increase for Mn

and Pb. The elevated values indicate the typical nature of

mangrove sediments to capture trace metals. Further, the

enrichment also indicates that it is not only due to

anthropogenic activities surrounding the mangrove wetland

(such as boating, fishing, tourist activities etc.,) but also

due to discharge of untreated sewage and effluents of the

multifarious industries situated in the upper stretch of the

Hugli river (as shown in Fig. 1). In addition, tourism and

port activities, harbor dredging, operation of excessive

number of mechanized boats and increasing agricultural

and aquacultural practices also aggravate the problem.

Conclusions

The work presents first comprehensive data base of ALT-

Ms in core sediments of Sunderban mangrove wetland

highlighting the geochemical processes concerned with the

differences in distribution patterns. The results indicate that

ALTMs are trapped in the mangrove sediments due to the

change in pH conditions at various sites and the reduction

of organic carbon and carbonates in the mangrove region.

The down core profile distribution of ALTMs also suggests

that Fe, Mn enrichment is due to the diagnetic behavior of

the metal. The higher values of other ALTMs (Cr, Cu, Ni,

Pb, As and Ba) are mainly due to the uncontrolled dis-

charge of domestic and industrial effluents into the rivers

feeding the mangrove region. The association of ALTMs

with the organic particles as evidenced from statistical

analyses further endorses the above inference. Within the

acid leachable data on trace metal in core sediments, the

highest value of ‘‘the polluted mantle’’ are overall found in

the eastern flank of Sunderban wetland with high average

of trace metals. The coastal environment of West Bengal is

considerably constrained due to implementation of dredg-

ing, drilling and other chemical activities. Hence the

authors recommend regular monitoring on enrichment of

trace metals considering both biotic and abiotic compart-

ments of Sunderban for effective management of this

virgin and fragile environment.

Table 5 Comparison of acid leachable elements in sediments of present study with estuarine sediments from selected southeast coast Indian

Rivers

Method of extraction Study areas Fe Mn Cr Cu Ni Co Pb Zn Cd

Fe–Mn fraction oxide (1) 43.8 31.2 – 23.6 – – 41.1 15.8 –

HOAc (2) 255 82 4.25 – 5.91 5.04 3.06 3.60 0.15

HOAc (3) 1,673 108 5.4 NA 3.1 3.0 6.3 16.6 0.11

HOAc (4) 702 86 2.6 – 2.49 3.46 9.96 5.92 0.08

HCl (5) 11,062 514 23.53 12.16 19.88 14.33 21.27 16.73 0.72

HCl (6) 2,690 219.21 5.64 4.49 5.82 6.59 10.24 9.87 0.93

HCl (7) 1,786 55.2 16.24 7.53 7.8 NA 24.2 11.31 0.60

HCl (8) 1,673 26.7 6.79 3.77 3.77 3.03 7.2 8.88 0.39

HCl Present study 4,457 393 13.52 36.60 8.47 NA 15.37 NA 0.015

All values in lg g-1 (Except the present study is expressed in mg kg-1). All values are from surface sediments; NA not analyzed

Study areas (1) River Yamuna (Subramanian et al. 1987); (2) Gulf of Mannar (Jonathan and Ram Mohan 2003); (3) Ennore Creek core sediments

(Selvaraj et al. 2003); (4) Kalpakkam coast (Selvaraj et al. 2004);(5) Mullipallam Creek, South India (Janakiraman et al. 2007; (6) River

Tambraparani (Chandrashekharan, personal communication); (7) Pichavaram mangroves (Lakshumanan 2001); (8) Uppanar River Cuddalore

(Ayyamperumal et al. 2006)


123

Acknowledgments The research work was supported by University

Grants Commission (UGC), New Delhi, India [(Sanction No UGC/

199/UPE/07] under the scheme of ‘‘University with Potential for

Excellence’’ (Modern Biology Group). One of the authors (Md. Aftab

Alam) is greatly indebted to UGC for awarding him project fellow-

ship. M.P. Jonathan and P.D. Roy thank the support by SNI-CO-

NACyT, Mexico.

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Acid leachable trace metals in sediment cores from Sunderban mangrove wetland, India: an approach...

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