Journal of Environmental Protection, 2011, 2, 840-847
doi:10.4236/jep.2011.26095 Published Online August 2011 (http://www.SciRP.org/journal/jep)
Distribution of Antimony in a Tropical Estuary
Dominated by Mangroves
Sanjay K. Mandal, Natasha Majumder, Chumki Chowdhury, Raghab Ray, Manab K. Dutta,
Tapan K. Jana
Department of Marine Science, Calcutta University, Kolkata, India.
Received May 10th, 2011; revised June 18th, 2011; accepted July 22nd, 2011.
ABSTRACT
Seasonal variation of antimony was studied in order to characterize its distribution in estuarine water, pore water,
sediment, and digenetic behavior in the Sundarbans mangrove ecosystem. The mean concentration of dissolved inor-
ganic Sb ranged between 230.8 and 303.1 ng·L–1 over the period of study with a minimum during the post-monsoon
closely associated with spring diatom bloom. Molecular diffusion flux of Sb was found greater than its value advected
and deposited on sediment-water interface and th ere was significant remob ilization of Sb in the Sundarbans man grove
ecosystem.
Keywords: Antimony (III & V), Molecular Diffusion Flux, Phytoplankton Bloom, Mangrove
1. Introduction
Antimony is ubiquitously present in the environment as a
result of natural (rock weathering and soil runoff) and
anthropogenic (fossil fuel combustion, mining and
smelting activity and the application of super phosphate
fertilizers to agricultural soil) activities [1-4]. Current
world production of antimony is about 140,000 tons per
year [5] and is used for several purposes such as semi-
conductor, diods, lead batteries, antifriction alloys, type
metals, flame retardants etc. The rare element antimony
has an estimated abundance of 0.2 ± 0.3 mg·kg–1 [6] in
the earth crust and background concentrations in soils of
<0.3 ± 8.4 mg·kg–1 [7], but it tends to concentrate in the
surface soils [8]. Important anthropogenic sources of
antimony in soil are vehicle emissions [9,10] and emis-
sions of smelters [6]. Due to its versatile uses and release
from this source, there is increasing concern relating to
its occurrence more than admissible drinking water limit
of 6 μg·L–1 in the aquatic system [11]. The biogeo-
chemical process in the ocean and estuaries are complex
due to the occurrence of Sb compounds in Sb (V) & Sb
(III) oxidation state. The process responsible for their
variation are 1) interconversion between Sb (V) & (III)
oxidation state under oxic and anoxic condition 2) indis-
crepency in the adsorption/desorption kinetics between
Sb (III) & (V) 3) biological activity such as phytoplank-
ton production, biovolatilisation by fungus [12-17].
These processes controlling the transformation and trans-
port of antimony have been identified as research priori-
ties in an ecosystem [2]. Highly productive Sundarbans
mangrove ecosystem (4.71 - 6.54 Mg C·ha–1·year–1) with
4.85 Mg C·ha–1·year–1 of litter production [18] and sea-
sonal shift of phytoplankton production with diatom
bloom during post monsoon period [19] could affect the
antimony reactivity and cycling in the Sundarbans man-
grove ecosystem situated along coastal boundary of
Ganga-Brahmaputra delta. Elevated concentrations of Sb
in an ecosystem could be related to anthropogenic sources
and associated with high As concentration [2]. Arsenic
found in the Ganga-Brahmaputra delta [20] is redistrib-
uted by biogeochemical processes in the Sundarbans
mangrove ecosystem [21].
The present study was intended to identify the bio-
geochemical processes affecting Sb distribution and to
explain its ultimate source from the Sundarban mangrove
ecosystem.
2. Materials and Methods
Study area: The study site is located in the Indian
Sundarban at 21˚32', 22˚40'N and 88˚05', 89˚E (Figure
1). This natural mangrove forest is a part of the estuarine
system of the River Ganges on the northeast coast of Bay
of Bengal. It covers a total area of 9630 km2, and 4264
km2 is comprised of intertidal zone. This area is covered

Distribution of Antimony in a Tropical Estuary Dominated by Mangroves841
Figure 1. Map showing the station location.
with thick mangroves, which are subdivided into a forest
sub-ecosystem and 1781 km2 is an aquatic sub-ecosystem.
The distance from the study area to the region, which
spans from the first point in south 24 Pgs and the last
point in north Malda is approximately 150 - 580 km. The
Hooghly estuary, a tributary of the river Ganges, is the
main artery of the Sundarban mangrove ecosystem.
Farakka dam located at ~286 km upstream from the
mouth of the river regulates fresh water flow through the
estuary. The Ganges drains much of the southern slopes
of the Himalaya and delivers an enormous supply of
sediment to the Bengal fan. Suspended particulate matter
(SPM) exhibited seasonality with highest level during
monsoon (282.2 mg·L–1) periods and lowest levels during
the pre-monsoon period (12.0 mg·L–1). It decreases ex-
ponentially with respect to salinity (S): SPM = 109 e–0.0718
× S (r2 = 0.5). The annual load of sediment from the es-
tuary to the northeast coast of Bay of Bengal was esti-
mated to be 65.19 × 106 t and monsoonal runoff could
account for 88% of the total transport [22]. Fresh water
discharge of the Hooghly River varies between 2952 and
11,897 m3·s–1 during the southwest monsoon and be-
tween 900 and 1500 m3·s–1 in the non-monsoonal months.
The salt front rarely penetrates beyond Diamond Harbor,
which is 80 km from the mouth of the Hooghly estuary.
Several discrete islands and low-lying intertidal zones are
covered with thick mangrove and are inundated during
spring tide. Heights of natural mangrove plants genera,

Distribution of Antimony in a Tropical Estuary Dominated by Mangroves 842
such as Avicennia, Acanthus, Aegiceras, Bruguiera, and
Ceriops >10 m are rare. The climate of the area is domi-
nated by the southwest monsoon (June-September),
northeast monsoon or post-monsoon (October-January),
and pre-monsoon (February-May).
2.1. Experiments Design
Measurements were performed every month from Janu-
ary to December in 2007 at two sites: one located at Lo-
thian Island in the confluence of Saptamukhi River and
Bay of Bengal, and the other located at Sajnekhali, which
is 117 km from Lothian Island. Samples were also col-
lected at three stations, Beguakhali, Kachuberia, and
Diamond Harbor, which covered the breadth of the salin-
ity gradient zone. Different sites of the littoral zone cov-
ered with mangrove were selected for monthly sampling
of pore water [23], sediment during low tidal expose, and
tidal water during the low and high tidal phase. A corer
made of stainless steel (5.5 cm i.d.) was used to extrude
sediment, and sectioned at three depth intervals (0 - 2, 2 -
4, and 4 - 6 cm). Surface water samples were collected
using Niskin bottles at 3 h intervals from a boat. Tidal
and pore water samples were filtered (0.45 m millipore
filters, previously dried and weighed) under nitrogen
atmosphere. These filter samples were stabilized by the
addition of H2SO4 to yield a 0.1% v:v in acid-washed PP
bottles, and stored in an ice box for antimony speciation
analysis. Filtered tidal and pore water samples collected
in PP bottles were also stored in the cold and dark with-
out the addition of acid or HgCl2 for analyses of salinity,
sulfate and sulphide. Ground water collected from the
tube well of ~150 m deep was preserved in an ice box
after acidification for Sb analysis. Tidal and pore water
samples were also collected and preserved with HgCl2
for pH determination [24]. Phytoplankton was collected
from surface water in the day time during high tide by
using bolting silk 20 µm plankton net. For quantitative
estimation, 1L samples were preserved with Lugol’s so-
lution and buffered formaldehyde. After 24hrs of sedi-
mentation, the supernatant was reduced to a minimum
volume by filtration (0.45 µm). Settled and filtered mate-
rials were combined and used for phytoplankton enu-
meration, identification and biovolume with the help of a
Sedgwick rafter counting chamber [25].
2.2. Analytical Methods
Sulfate, sulfide, iron were analyzed by spectrophotomet-
ric method [26,27]. Relative error of accuracy was
<±10%. Air-dried sediment samples were used for grain
size analysis following the pipette method [28]. Freeze
dried sediment sample was used for the measurement of
organic carbon by the Walky-Black wet combination
method [29]. Known quantity (0.5 g) of dried sediments
was extracted by 0.1 N KOH solution with constant
shaking for 24hrs and centrifuged and fluorescence spec-
tra were recorded by using Perkin Elmer LS-50 lumines-
cence spectrophotometer for the measurement of humic
(HA) and fulvic (FA) acid [30]. An acid mixture (HF,
HNO3, HCl) for freeze dried sediment, suspended par-
ticulate matter samples were used for digestion in Teflon
reactors to perform total antimony analysis using the
Varian Hydride System-Vapor Generator (Serial No.
EL0405-314) coupled to the Spectr AA 55B true Double
Beam Atomic Absorption Spectrometer, following meth-
ods described elsewhere [31,32]. Measurement of dis-
solved Sb (III) was performed by hydride generation at
pH 6 using the buffer of tris-HCl (1.9M) and 1 MHCl/1%
w/v potassium iodide followed by NaBH4 treatment for
total antimony [33]. The analytical methods for antimony
were verified before analyses of each sample batch
against standard samples procured from MERCK K GaA,
Germany. Relative accuracy and the coefficient of varia-
tion were 96.2% and 9.2%, respectively, for antimony.
2.3. Flux Estimate
To evaluate whether the diagenic processes could lead to
significant post depositional redistribution of Sb, we es-
timated vertical diffusive flux. The net flux of dissolved
species across the sediment-water interface (F, ng·m–2·d–1)
is due to molecular diffusion in pore water (–ΦD dC/dZ),
and advective transport of the species in pore water
(ΦUC) and on sediment particles (ΦUsCs). Considering
the constant ratio (K) of the distribution of chemical spe-
cies in pore (C) and solid matter(Cs), and equal advec-
tion velocities of sediment particles (Us) and pore water
(U), the net flux is calculated from the equation: F =
–ΦD dC/dZ + Φ U(K + 1)C [34]. For elevated concentra-
tion in pore water (dC/dZ > 0), the –ve value of F indi-
cates that the net flux of antimony is directed up- ward
(from sediment to water). Bulk sediment diffusion coef-
ficient (D) was calculated from the molecular diffusion
(D0) for Sb in sea water using the equation D = Φ2D0 and
porosity (Φ) 0.65. The concentration gradient was calcu-
lated from the Sb concentration in the overly- ing water
and pore water collected from the sediment sampling
interval (0 - 30 cm).
3. Results
The seasonal maximum and minimum temperatures of
the atmosphere were 30.7 ± 1.5 and 21.5 ± 4.6˚C in June
and December, respectively. Total rainfall was recorded
as 1737 and 590 mm during the SW and NE monsoon,
respectively. Secchi disc transparency varied between 7
and 99 cm, and mean photic zone light energy was found
to be 23.48 ± 4.5 k lux. The mean antimony concentra-
tions varied in the tidal water from 230.8 to 303.1 ng·L–1,

Distribution of Antimony in a Tropical Estuary Dominated by Mangroves 843
in pore water from 375.5 to 590.9 ng·L–1, in ground water
from 250.0 to 327.5 ng·L–1, in sediment from 0.2188 to
0.5834 µg·g–1, in suspended particulate mater from 0.08
to 0.19 μg·g–1. Investigation of diurnal variations in man-
grove water of antimony (Total) concentrations demon-
strated an increase between low and high tide from 175.0
ng·L–1 to 425.0 ng·L–1 in October, from 128.0 ng·L–1 to
327.9 ng·L–1 in January and from 232.0 ng·L–1 to 464.0
ng·L–1 in March. Antimony concentrations in tidal water
demonstrated strong seasonal variations (Figure 2, Table
1), with a maximum of 303.1 ± 91.1 ng·L–1 during the
pre-monsoon and a minimum of 230.8 ± 102.0 ng·L–1
during the post-monsoon and intermediate of 279.8 ±
192.1 ng·L–1 during the monsoon. Antimony concentra-
tion was found to decrease in the study area after onset of
the monsoon. Sb was found to be associated with particle
(0.85 - 0.19 μg·g–1), and was about 1.8 folds greater in
the pore water than in the tidal water. Variation of Sb in
the salinity gradient zone of the estuary is given in Fig-
ure 3, which showed increased antimony concentrations
with increasing salinity. Phytoplankton population
showed seasonality (Table 1), with the highest levels
during post-monsoon periods (1.8 × 104 cells·L–1) and
lowest levels during the monsoon period (0.8 × 104
cells·L–1). Biswas et al. 2010 [35] observed that the
number of definable Bacillariophyceae species exceeded
Dinophyceae taxa, and highest number of bloom-form-
ing species was found during post-monsoon period.
Figure 2. Seasonal variations in Sb (total) and Sb(III) for tidal, pore and gr ound water.
Figure 3. Salinity versus dissolved antimony (total) in the salinity gradient zone of Saptamukhi and Hooghly estuary.

Distribution of Antimony in a Tropical Estuary Dominated by Mangroves 844
Table 1. Seasonal varia tion of pore water and sedime nt qual-
ity: Salinity (S, PSU), pH, Dissolved Iron (Fe, µg·L–1), Sul-
fate (SO4, µM), H2S(µg·L–1), Antimony (Sb, ng·L–1), Flux of
Sb (FSb,ng·m–2·d–1), Sediment textur e (% of Sand, Silt, Clay ),
Organic C(%), HA(g·g–1), FA(g·g–1) and Phytopankton
(Number·L–1).
Parameters Monsoon Post monsoon Pre monsoon
Pore water
S 19.3 ± 3.7 24.3 ± 2.3 27.8 ± 0.8
pH 7.82 ± 0.22 7.79 ± 0.17 7.63 ± 0.08
Fe (g·L–1) 38.42 ± 13.6 15.88 ± 13.3 29.26 ± 22.8
SO4 (M) 8.73 ± 1.87 11.56 ± 1.17 12.93 ± 1.79
H2S(µg·L–1) 105.4 ± 28.7 169.6 ± 45.0 93.6 ± 1.4
Sb(ng·L–1) 480.7 ± 93.1 375.5 ± 59.9 590.9 ± 105.9
FSb(ng·m–2·d–1) –6.91 –4.60 –11.16
Sediment
Sand(%) 5.83 ± 1.43 15.62 ± 4.11 5.84 ± 0.72
Silt(%) 87.5 ± 3.74 72.5 ± 5.11 79.76 ± 5.43
Clay(%) 6.16 ± 1.27 11.88 ± 3.45 14.49 ± 1.62
Organic C(%) 0.59 ± 0.05 0.66 ± 0.02 0.47 ± 0.06
HA(g·g–1) 454 ± 136.8 457.8 ± 138 216.3 ± 65.2
FA(g·g–1) 1298 ± 232.3 1308 ± 234.8 629.9 ± 113.1
Phytoplankton
(Number·L–1) 0.8 × 104 1.8 × 104 1.32 × 104
Considering the mean distribution factor (K) of 3.36 ±
1.72 and adsorption factor (6 K + 1), the combined flux
of antimony due to advection of pore water and deposi-
tion of solid particles was found to be less (4.84 to 7.61
ng·m–2·d–1) than that of molecular diffusion (9.44 to 18.8
ng·m–2·d–1). Therefore, the Sundarban mangrove ecosys-
tem acts as a source of antimony with dispersal rate be-
tween 4.6 and 11.16 ng·m–2·d–1.
4. Discussion
Antimony concentrations in tidal water demonstrate
strong seasonal variations with a maximum during the
pre-monsoon and a minimum during the post-monsoon
and intermediate during the monsoon. Concentrations of
antimony in groundwater are well below the maximum
contaminant level of 6 μg·L–1 [11]. Annual mean value
for total Sb in the mangrove dominated estuaries and
coastal water is 271.2 ± 235.8 ng·L–1, being lower than
the average values (484 ± 552 ng·L–1) reported for the
world estuaries and greater than the mean oceanic value
(184 ± 45 ng·L–1) [2]. Its greater concentration in the
pore water relative to tidal water could be attributed to
the possible oxidative release of organic-bound Sb from
the sediment. Its non-coservative behavior with a source
from the mangrove ecosystem at the lower stretch of the
estuary is in conformity with the Scheldt estuary [36],
Mediterranean estuary [37] However, its conservative
behavior is not uncommon in a series of estuaries along
the east coast of the USA, and the Rhine estuary of the
Dutch Wadden Sea [38]; and mixed behavior, in other
estuaries [39,40]. Considerable decrease of Sb is associ-
ated with diatom bloom in the post-monsoon. Benson
and Coony [41] incubated diatom Thalassiosira nana
with 125SbCl3 and found protein-bound antimony, a stib-
nolipid, and a group of water soluble radioactive prod-
ucts. They suggested active uptake of Sb by diatom and
its conversion into organic form. Interconversion of Sb
(V) to Sb (III) followed by its excretion is a detoxifying
mechanism used by Chlorella valgaris [42,43]. During
the post monsoon, the higher ratio of Sb (III):Sb (V)
(0.6:1) than the pre-monsoon (0.47:1) and monsoon
(0.45:1) in the present study indicates the role of phyto-
plankton bloom in inter-converting oxidation state of Sb
in consistent to our earlier report [20] observed for arse-
nic. Takayanagi and Cossa, 1997 [15] attributed the de-
pletion of Sb and stabilization of Sb (III) in the surface of
Lake Pavin, France to the uptake by phytoplankton. Non
conservative behavior of Sb owing to biological uptake
of Sb by phytoplankton is a slow process relative to the
scavenging rate by aluminium in the estuarine water [44].
Stepwise multiple regression analysis demonstrates that
sulphate, H2S and iron comprise 60% of the variability of
total antimony in pore water.
Total Sb (ng·L–1) = 1318 - 5.38 S – 60 pH + 284 SO4 –
1.81 H2S + 0.84 Fe -723 Org-C (R2 = 84.5%, F=4.56, n =
12, p = 0.059). Out of the six factors p is found relatively
more significant for organic carbon (p = 0.059), sulphate
(p = 0.084) and iron (p = 0.064). Antimony could be
present in the soils as slightly soluble sulphide and could
remain in association with arseno pyrite [45,46]. Oxida-
tive release of antimony from both pyrite and soil organic
carbon could explain its elevated concentration in pore
water. Deng et al., [47] and Chen et al., [48] found from
the analyses of lake and pore waters that the major part
of Sb was associated with natural organic compounds (up
to 85% of total Sb) and the rest was in inorganic Sb (V)
and Sb (III) forms. Few recent experimental studies re-
ported association of Sb with aqueous humic acids and
demonstrated moderate binding of Sb (III) with humic
compounds [49,50]. However, the identity of binding
sites, stoichiometry and structure of complexes remained
uncertain. This is due to the fact that natural organic
matter (dominated by humic and fulvic acids) is present

Distribution of Antimony in a Tropical Estuary Dominated by Mangroves845
in extremely complex poly-functional structure, which
precludes assessing unambiguously sorption mechanisms
or nature of aqueous complexes and identifying chemical
sites (potentially numerous) responsible for Sb binding.
Sediment-water molecular diffusive flux of antimony
is greater than the combined flux due to advection of pore
water and deposition of solid particles over the sediment
and the Sundarban mangrove ecosystem acts as a source
for antimony with significant diagenetic remobilization.
5. Acknowledgements
We gratefully acknowledge financial assistance from the
UGC, New Delhi.
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