J Mar Sci Technol (2013) 18:213219
DOI 10.1007/s00773-012-0201-2
ORIGINAL ARTICLE
Tributyltin in marine sediments and Philippine green mussels
(Perna viridis) in Manila Bay
Ryan U. Olivares Shigeru Tabeta
Elvira Z. Sombrito
Received: 23 February 2012 / Accepted: 28 October 2012 / Published online: 25 November 2012
JASNAOE 2012
Abstract Tributyltin (TBT) is a pollutant, mainly intro-
duced to the environment as insecticides, fungicides, bac-
tericides, wood preservatives and marine antifouling agent.
Concentrations of TBT and its degradation products were
isolated from the bivalve Perna viridis and marine sedi-
ments collected from selected coastal areas along Manila
Bay. In all samples, the extremely toxic TBT compound
was detected, calculated as Sn. In sediments, measured
concentration ranged from the limit of detection of 0.5 to
9.0 ng Sn g-1. Highest levels of TBT were observed at the
inner and northern part of the bay, adjacent to coastal areas
of varying land and water use (i.e., aquaculture, fishpond,
mangrove forests, industrial establishments, and ports).
However, the levels decrease near the bay entrance.
Accumulation in this area can also be deduced from the
movement of the prevailing wind and hydrodynamic
behavior of the bay during the time of sampling, which
transports suspended sediments from the eastern coast of
Manila to the northern coast of Bulacan. In green mussels,
the levels of TBT ranged from 2.1 to 8.9 ng Sn g-1. While
these values are relatively low, concentrations as low as
0.659 ng Sn g-1 have been reported to be toxic to mol-
luscs. The environmental levels of organotin species
determined in the samples are comparatively low by global
standards. Nevertheless, there is a need to estimate the
R. U. Olivares (&)
E. Z. Sombrito
Chemistry Research Section, Atomic Research Division,
Philippine Nuclear Research Institute, Commonwealth Avenue,
Diliman, 1105 Quezon City, Philippines
e-mail: ruolivares@pnri.dost.gov.ph
R. U. Olivares
S. Tabeta
Department of Environment Systems, Graduate School of
Frontier Sciences, The University of Tokyo,
Kashiwa 277-8583, Japan
levels of TBT in coastal waters and its associated uses, to
evaluate the effectiveness of imposed regulation prohibit-
ing the application of organotin compounds (OTs) as bio-
cides in antifouling agents on ships and aquaculture
facilities.
Keywords TBT
Organotin
Perna viridis
Marine
pollution
Sediments
1 Introduction
Tributyltin (TBT), a type of organotin (OT), has been widely
used in many industrial and agricultural applications, mainly
as insecticides, fungicides, bactericides, preservatives and
marine antifouling agent [1]. It is an aggressive biocide that
inhibits the attachment and growth of algae, barnacles,
tubeworms, mussels and other marine organisms on ships
and boat hulls, quays, buoys, fish farm nets and cages [11,
14, 32]. Consequently, health and environmental problems
associated with toxic TBT are now being addressed. It has
been implicated, even at extremely low concentrations, as
the causative agent in a number of anomalies observed in
marine animals. Various impacts of TBT in the aquatic
environment are well documented [2].
In recent years, efforts have been made for prohibiting the
application of OT antifoulants to all vessels and fish cages
by January 2003, and complete prohibition by January 2008.
In many cases, a relationship between levels of environ-
mental contamination and the intensity of shipping traffic
can be detected [36]. The Philippines, being an archipelagic
country, shares the same problem as far as marine envi-
ronment is concerned. Manila Bay, one of the important
coastal marine ecosystems and the countrys busiest com-
mercial hub, is facing the severity of this problem. In 1999,
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the Partnership in Environmental Management for the Seas
of East Asia (PEMSEA) was launched to formulate and
implement strategies and action plans to ensure the sus-
tainable management of the seas within the region. PEM-
SEA has identified Manila bay as one of the pollution hot
spots in the region, and this paved the way for the creation of
the Manila Bay Declaration, 2001. It is an innovative effort
integrating the local, national and international initiatives to
address coastal and marine issues on habitat degradation,
resource use, etc. The bay has served as a major avenue for
trade and commerce. It is considered to be the second most
productive fishing ground in the country, with competing
uses. Aquaculture activities proliferate along Bulacan,
Bataan, Cavite, and the northern Metro Manila coastlines.
The North and South Harbors in the City of Manila provide
support to the international and domestic shipping industry
[26]. Shipping ports and marine repair yards are likewise
located in major areas along the coast, with approximately
30,000 ships arriving and departing annually, transporting
goods, raw materials and passengers [3]. If indeed the call
for global prohibition has not been taken seriously, it is
expected that TBT-containing discharges from aquaculture,
shipping and repair activities can find their way to marine
organisms and sediments.
Earlier studies have shown TBT contamination in sed-
iments, seawater and bivalves in several Asian and Pacific
countries [6, 37, 38]. However, studies have not yet
reported on the level of contamination of TBT in Manila
Fig. 1 Study site
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J Mar Sci Technol (2013) 18:213219
Bay sediments, although Tanabe et al. [36] mentioned the
level of TBT in green mussels in selected coastal areas of
the Philippines.
From the perspective of sustainable marine and coastal
management, and in line with the efforts to address marine
pollution in the coastal areas, the potential impact of this
problemparticularly the adverse implications on public
health and safetyshould be recognized and properly doc-
umented. It is essential to conduct continuous monitoring,
and to estimate the levels of TBT in coastal waters and its
associated uses, to evaluate the effectiveness of the imposed
regulation in prohibiting the application of OT compounds.
This report provides initial data on bay-wide distribution
of OT compounds in marine sediments and a second
attempt to document the level in mussels 10 years after the
first documented study of Tanabe et al. [36]. Moreover, the
data presented here will serve as a baseline data for
the levels of TBT in Manila Bay, by which future studies in
the bay can be assessed.
2 Description of the study site
Manila Bay is a semi-enclosed estuary that is connected to
the South China Sea via a 16.7 km wide entrance (Fig. 1).
The Regional Program for (PEMSEA) has identified
Manila Bay, being one of the pollution hot spots in the
region, for the development and implementation of a
J Mar Sci Technol (2013) 18:213219
Fig. 2 Sampling stations for sediments and mussels
strategic environmental management plan. Manila Bay
receives drainage from approximately 17,000 km2 of
watershed, consisting of 26 catchments areas [10] with
main contributories such as the Pasig, Pampanga and
Bulacan Rivers [30]. Seasonal and annual variations in
discharges are pronounced, with the largest input occurring
from June to October (wet season) and the lowest from
November to March (dry season). The mean depth of the
bay is 25 m and the volume is 31 km3. The typical reten-
tion time for freshwater in the bay is between two weeks
and one month, depending on the season [27, 40].
The pilot study for the Integrated Environmental Moni-
toring Program for Manila Bay (IEMP-MB) Team collected
the samples (mussel and sediment) during the pilot study
cruise on board RPS Corregidor. Nine (9) grab sediment
samples were collected from the pilot study stations from
February 10 to February 11, 2005. Mussels were collected
from four (4) aquaculture locations (Orion, Limay, Bacoor
Bay and Paranaque) on January 20 and January 25, 2005.
Details of the sample locations for sediments and mussels is
shown in Fig. 2.
3 Methodology
3.1 Sample preparation
The sediment grab samples were subsampled in the labo-
ratory for the determination of OT compounds. Twenty
215
(20) grams of the sediment samples were dried to constant
weight in a freeze dryer. Meanwhile, mussels soft parts
were shucked from the shell and weighed. Pooled mussel
meat was homogenized using a Waring Laboratory Blen-
der. Homogenates were freeze-dried using a Telstar Lio-
alfa-6 freeze dryer. Dried samples were pulverized, and
portions of these were packed in glass vials and sent for
analysis. Analyses of the samples for TBT were conducted
at the Marine Environmental Laboratory of the Interna-
tional Atomic Energy Agency in Monaco.
3.2 Analysis
Tributyltin and its degradation products were determined
based on the methods used by de Mora et al. [8]. The OT
compounds were determined by capillary gas chromatog-
raphy with a flame photometric detector at k = 610 nm.
The detector and splitless injector were maintained at
250 C. Separations were carried out under a helium flow
rate of 1.3 mL min-1. The temperature programme was
60 C for 2 min, 60270 C at 6 C min-1, and 270 C for
20 min. Under such conditions, the following OT species
were resolved: monobutyltin (MBT), dibutyltin (DBT),
TBT, diphenyltin (DPhT) and triphenyltin (TPhT). A
quality control system based on three internal standards
was adopted [5]. Tripropyltin was used to indicate the
derivatization reaction efficiency, and all the chromato-
graphic peak areas were normalized to that of tripropyltin.
Tetraoctyltin was used to check the overall solvent
extraction efficiency. Both internal standards were spiked just
prior to leaching. Tetrabutyltin, spiked in all samples prior to
injection, was used as a GC-internal standard to quantify the
recoveries of both internal standards. Appropriate blanks were
analyzed with each batch of samples and, in addition, refer-
ence materials were determined simultaneously. The detec-
tion limit for OT analyses, based on a typical instrumental
signal-to-noise ratio of 3:1, varies somewhat between sam-
ples. These variations are real and dependent on the sample
weight, the final volume of the extract, and the recovery
efficiency of the internal standard, because the response
factor for each compound is normalized to the response of
the internal standard. The detection limits (ng Sn g-1 dry
weight) for OT species (MBT, DBT, and TBT) in sediments
were 2.3, 0.4, and 0.5, respectively. In mussels, the detection
limits were 3.9, 1.8, and 1.2, respectively.
4 Results and discussion
4.1 Concentration of TBT in sediments
The data obtained from the analysis of TBT in Manila Bay
sediment samples is presented in Table 1.
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Table 1 OT concentrations (ng Sn g-1 dry weight) in sediment

Station MBT DBT TBT DPhT TPhT Total OT [MBT]/[OT] [TBT]/[DBT]

1 37 7.4 9.0 \0.8 \0.5 53.4 0.69 1.22

2 32 3.8 3.0 \0.8 \0.5 38.8 0.82 0.79
3 49 1.6 0.9 \0.8 \0.5 51.5 0.95 0.56
4 38 17 2.1 \0.8 \0.5 57.1 0.67 0.12
5 10 0.7 0.8 \0.8 \0.5 11.5 0.87 1.14
6 5.5 0.8 0.8 \0.8 \0.5 7.1 0.77 1.00
7 3.1 0.9 0.5 \0.8 \0.5 4.5 0.69 0.56
8 5.8 2.6 1.7 \0.8 \0.5 10.1 0.57 0.65
9 4.1 3.5 2.2 \0.8 \0.5 9.8 0.42 0.63
D.L. 2.3 0.4 0.5 0.8 0.5
MBT monobutyltin, DBT dibutyltin, TBT Tributyltin, DPhT diphenyltin, TPhT triphenyltin, OT organotin. D.L. detection limits

The TBT concentrations in sediments were highest in

station 1 (near Bulacan) at 9.0 ng Sn g-1. Higher values
were also measured in stations near the ports of Pampanga,
Bataan and Manila. These stations receive drainage from
major contributory rivers and watershed areas. The ports of
Manila provide support to the international and domestic
shipping industries. Heavy shipping activities and traffic
can be seen as the reason for the increased TBT level in
this area. While there is still a need to ascertain pollution
sources of OTs, various studies documenting the presence
of significant TBT contamination in harbors, marinas,
shipyard hull and boating activities cannot be underesti-
mated [25, 37, 38]. In selected Asian developing countries,
relatively higher OT contamination in sediments were
consequential from high boating activities and coastal
aquaculture areas [15, 36], implying the usage of TBT as a
biocide in antifouling paints used on boat hulls and marine
aquaculture facilities.
Stations 5, 6 and 7 have the lowest levels of TBT, which
are almost in the range of the detection value (0.5 to
0.7 ng Sn g-1). These stations do not indicate a significant
source of TBT, since they are located facing the bay
entrance and it is assumed that there is a significant inflow Fig. 3 Spatial distribution of TBT in sediments
and outflow of tidal movement, as summarized in the
United Nations Environment Program (UNEP) Report [39].
Figure 3 shows the spatial distribution of TBT in Manila The transport of pollutants from the eastern coast to the
Bay sediments. Higher levels of TBT concentrate mostly northern coast is a possible reason for the elevated level of
on the inner portion of the bay. Contaminants and chemical TBT in station 1. Nevertheless, the values obtained in
pollutants released into the coastal system, before they Manila Bay sediments are still lower in comparison with
eventually sink into the bottom sediments, travel through other areas, especially in countries where TBT use is not
water column and attach to suspended particles. Simula- regulated, e.g. Malaysia and Vietnam. Table 3 shows the
tions of current by a hydrodynamic model introducing comparative compilation of TBT contamination in marine
southeasterly winds (the wind prevailing from February to sediments from selected coastal areas.
May), conducted by De las Alas [7] and Olivares et al. [24], The ratio [MBT]/total OT has been used to determine if
produce a counter clockwise circulation pattern in the there were fresh or recent discharges of TBT in the marine
mid-part of the bay, and current variability, especially in system [18]. The ratio from 0.03 to 0.1 would indicate fresh
shallow areas, is highly influenced by the prevailing winds. inputs of TBT, and below this range can be a cause for

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alarm and may pose a threat to marine organisms. In the
case of Manila Bay, since MBT is dominantly present in
sediments, measured ratios were above the given limit, and
all sediment samples ranged from 0.42 to 0.95. Hence, we
can say that there were no recent inputs of TBT into the
bay. This level further indicates the occurrence of previous
or older OT released in the past, since the level of degra-
dation products (MBT ? DBT) is considerably higher than
the TBT values. The composition of OT derivatives in
sediments was in the order of MBT [ DBT [ TBT, sug-
gesting that the lower value of TBT is due to its degrada-
tion into lesser toxic OT compounds. Owing to their slow
degradation rates and consistent flux, these compounds are
persistent in the marine environment [21, 34]. It has been
reported that if TBT-based paint chip are present in sedi-
ment, these chips degrade more slowly than TBT absorbed
by sediment particles [33]. In freshwater, half-life esti-
mates for TBT range from around 6 weeks to 5 months [9],
but degradation is slower in sediments and have been
reported to vary from 16 weeks to 3.5 years, with the latter
now believed to be representative [16, 19]. Since TBT
compounds are less likely to degrade in sediments, the
sediments themselves may display a history of OT con-
tamination in the marine environment.
The interpretation of the ratios of degradation products
used to determine the age of TBT contamination and the
history of pollutant introduction may be improved if ver-
tical profiles of TBT in the sediments are measured in
correlation with a more intensive 210Pb measurement.
Areas suspected to be contaminated by point sources can
be sampled and dated using the 210Pb method [31].
4.2 Concentration of TBT in green mussels
Mussels have been addressed as bio-indicators for moni-
toring trace toxic substances in coastal waters, due to their
high accumulation of a wide range of chemicals and toler-
ance to a wide range of salinity [12]. In order to initially
assess the TBT contamination in the coastal waters of Asian
countries, the green mussels collected along the selected
farms in Manila bay were examined for residue levels of
these contaminants. As shown in Table 2, TBT contents in
green mussel were found above the detection limit of
1.2 g Sn g-1. Higher accumulation of TBT in mussels is
measured in samples collected at station 1 and 2, with
values of 6.6 g Sn g-1and 8.9 g Sn g-1, respectively.
Mussel farms in these stations are closer to the port and pier
of Bataan, and it is possible that TBT is released regularly
from antifouling coatings of various boating and aquacul-
ture activities. Once released from an antifouling coating,
TBT is rapidly absorbed by organic materials, such as
bacteria and algae, or can be adsorbed onto suspended
particles in the water [4]. Subsequently, it is readily
217
incorporated into the tissues of filter-feeding organisms,
where it accumulates or can be deposited in the surface
sediments. On the other hand, stations 3 and 4 are located at
the southern coast of the busy port of Manila; however,
station 3 has the lowest TBT level of 2.1 ng Sn g-1. Mus-
sels from each site were sorted, to get samples of almost the
same shell lengths and weights. Unfortunately, mussel
samples collected at station 3 have relatively shorter shell
lengths compared to other areas. This difference in size may
be a factor in the bioaccumulation of TBT; hence, the lower
TBT concentration in mussels from station 3.
The levels of TBT found in the present study are sig-
nificantly lower than those reported with known TBT pol-
lution. However, concentrations as low as 0.659 ng Sn g-1
have been reported to be toxic to molluscs [23]. MBT
values were below the detection level in all locations
sampled for mussels. Earlier findings have demonstrated the
limited ability of green mussel to metabolize TBT into DBT
and MBT [36]. Despite of the contamination levels of OT
obtained in mussels, it is not clear whether pollution sources
of these compounds can be attributed to aquaculture
activities, agricultural run-off or shipping activities. Table 3
shows the comparative compilation of TBT contamination
in mussels from selected coastal areas.
Data reported by Tanabe et al. [36] indicated levels of
contamination and associated effects of butyltins (BTs),
especially in green mussels collected along the coastal
areas of Thailand, Philippines and India, during the period
of 1994 to 1997. Mussels collected in selected coastal areas
of the Philippines contained relatively high OTs, especially
in areas with high boating activities, such as around Manila
Bay. TBT levels obtained from mussels farmed adjacent to
Rizal Park, Ermita and Malate in Manila were as high as
640 ng Sn g-1. The results obtained in this report showed
a marked decrease of TBT levels. International Maritime
Organizations call for a global treaty banning the appli-
cation of TBT-based products in 2003, and a complete
prohibition of the presence of OTs by January 2008, may
have been the reason for the decline of TBT found in the
samples. One possibility that can be deduced is the distance
from which the samples are collected; [19] demonstrated
the significant correlation between the distance from the
innermost part of the bay and accumulation levels of TBT
in mussels and oysters. Concentration gradients declined
sharply within a relatively short distance due to seawater
dilution and removal by sediments.
5 Conclusion
The spatial distribution of TBT in sediments along Manila
Bay revealed that higher values were measured at the inner
portion of the bay near the ports of Pampanga, Bataan and
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Table 2 OT concentrations (ng Sn g-1 dry weight) in mussel meats

Station Site Mussel size (cm) MBT DBT TBT DPhT TPhT

1 Puting Buhangin, Orion 5.77.5 \3.9 5.6 6.6 \4.6 \1.2

2 Luz, Limay 4.17.0 \3.9 5.3 8.9 \4.6 \1.2
3 Pelayo, Bacoor 5.05.9 \3.9 4.1 2.1 \4.6 \1.2
4 Paranaque 4.98.9 \3.9 5.2 6.2 \4.6 \1.2
D.L. 3.9 1.8 1.2 4.6 1.2
MBT monobutyltin; DBT dibutyltin; TBT Tributyltin; DPhT diphenyltin, TPhT triphenyltin; D.L. detection limits

Table 3 Tributyltin (TBT)

Site TBT Concentration (ng Sn g-1 dry weight) Reference
concentrations in surface
sediments and green mussels Sediments
(ng Sn g-1 dry weight)
Manila Bay \0.59.0 This study
Gulf of Thailand 2.01246.0 [13]
Malaysia \0.7216.5 [37, 38]
Vietnam 0.8934.0 [22]
Suva Harbour, Fiji \538,000 [35]
San Diego Harbour, USA 143.0 [33]
North Chesapeake Bay 58570 [20]
Poole Harbour, UK 8.0213.0 [17]
Sado Estuary, Portugal 6.0213.0 [28]
Great Bay Estuary, USA 12.0-40.0 [29]
Green mussel
Manila Bay 2.18.9 This study
Selangor, Malaysia 14.223.5 [38]
Victoria Harbor, Hong Kong 63.7114.5 [6]
Philippines \1.0640 [36]
Thailand 3.0680 [36]
India \1.0150 [36]

Manila, where no significant tidal exchange is assumed.
However, the concentration of the degradation products of
TBT (DBT and MBT) in the sediment samples is higher
than the possible new inputs, indicating its degradation
over time. Meanwhile, this study reports that TBT con-
centrations in green mussels have generally declined in
comparison with the results obtained from a previous
study, conducted in Manila Bay in 1994 by the Asia
Pacific Mussel Watch Program [36].
The environmental levels of TBT detected in marine
sediments and green mussels collected along Manila Bay
were found to be within the range or lower than those areas
subjected for TBT testing in other countries. The regulation
of the use of TBT-based antifouling paints may have
reflected this decline. However, such decline may still be
subject to debate.
Fishing and aquaculture are two of the important sources
of livelihood in the Philippines. Since OT compounds are
retained in the sediments where they persist, regulation and
restriction will not immediately remove TBT and its deg-
radation products from the marine system. Hence, a con-
tinuous monitoring is necessary in order to ensure seafood
safety and the protection of the marine environment.
Acknowledgments The sediment and mussel sampling was done
under a collaborative effort among different agencies involved in the
Pilot Study for the Integrated Environmental Monitoring Program for
Manila Bay (IEMP), a project of the Department of Environment and
Natural Resources and Regional Program on Partnerships in Environ-
mental Management for the Seas of East Asia (PEMSEA). We
acknowledge with gratitude the Marine Environmental Laboratory of the
International Atomic Energy Agency in Monaco for the TBT analysis,
and the Philippine Nuclear Research Institute, especially Ms. Adelina
DM. Bulos, Mr. Efren J. Sta Maria, Ms. Ma. Celestina V. Honrado and
Ms. Merrian Tangonan, for the sample preparation and processing.
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