Marine Pollution Bulletin xxx (xxxx) xxx–xxx

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Marine Pollution Bulletin

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Tracing the sources of lead (Pb) in Brunei Bay, Borneo by using integrated
spectrometry ICP-MS and chemometric techniques
Ghazali Adianaa,⁎, Hafizan Juahira,⁎, Bidai Josephb, Noor Azhar Mohamed Shazilib
a
East Coast Environmental Research Institute (ESERI), Universiti Sultan Zainal Abidin (UniSZA), Gong Badak Campus, 21300 Kuala Nerus, Terengganu, Malaysia
b
Institute of Oceanography and Environment, Universiti Malaysia Terengganu, 21030 Kuala Nerus, Terengganu, Malaysia

A R T I C L E I N F O A B S T R A C T

Keywords: The present study aims to define the possible sources that contribute to the level of Pb into the Brunei Bay,
Stable Pb isotopic ratios Borneo. The cluster analysis has classified the bay into the northern part with heavy and agriculture-related
Anthropogenic Pb industries; the southern area with a moderate rural human settlement as well as the southwestern area with a
Brunei Bay more pristine environment and a low level of human settlement. The score plot of spatial discriminant analysis
Cluster analysis
verified a significant influence of the river system toward the estuary, whereas the temporal discriminant
Discriminant analysis
analysis has discriminated the seasonal changes. In comparison to elsewhere, the stable Pb isotopic ratios in
Southeast South China Sea
Brunei Bay showed a fingerprint similar to coal-related sources and of aerosol input. Briefly, even though Pb in
the Brunei Bay ecosystem proved to be at a low level, the stable Pb isotopic ratios showed that human and
industrial activities are slowly contributing Pb into the bay ecosystem.

1. Introduction
Pb is a well-known mineral since Pb minerals processing was re-
corded in the history of mankind for the past 6000 years (Cheng and
Hu, 2010). Before the 20th century started, the usage of leaded gasoline
in the daily activities was globally immense due to the high usage of
tetraethyl lead (TEL), an anti-knocking in the automobile fuels
(Geraldes et al., 2006; Walraven et al., 2014). However, it was phased
out in the early of 1990s and 2000s in USA and Europe, respectively
(Noble et al., 2015) due to the level of Pb in soil and air which led to
acute Pb poisoning (Kovarik, 2005). The excessive level of lead in the
environment was accidentally found in the early 1950s by a geoche-
mist, Clair Cameron Patterson during his research in identifying the
earth's age in rocks by using Pb isotope ratios (Tilton, 1998). In 1969, a
Polish toxicologist and medical doctor, Miroslaw Jan Stasik discovered
the acute poisoning of TEL, namely, mental disorder, liver, heart muscle
and kidney damage (Stasik et al., 1969).
It is well-noted that the abundance of Pb stable isotopes depends on
the age and amount of parent element present in the rock and mineral.
However, the composition of natural stable Pb isotopes can change due
to the anthropogenic activities mainly by the related mining industries
and the usage of Pb ores. According to Kamenov and Gulson (2014), the
anthropogenic Pb ores differ from the natural Pb due to the different
sources of Pb ores. Galena is the main Pb ore mineral, the end product
during the Pb ore deposition. During the process, Pb is separated from U
and Th. The parent isotopes continually decay and produce more Pb
isotopes whereas galena is frozen once the ore is produced (Bird et al.,
2010). For example, 206Pb/207Pb ratio value for galena from Broken
Hill, Australia (Townsend and Seen, 2012), Mississippi Valley, United
States (Hurst et al., 1996) and Brazillian ore (Geraldes et al., 2006) are
1.041, 1.31, and 1.092–1.151, respectively. Each Pb ore owns a unique
isotopic signature and preserves their isotopic composition during the
environmental processes unless they are mixed up with the secondary
Pb sources. The isotopic composition depends on the results of mixing.
The stable Pb isotopes consist of four isotopes, namely,204Pb (the
most stable Pb isotope which is also known as a primordial Pb and
represents 1% out of total Pb). 206Pb (24%), 207Pb (23%) and 208Pb
(52%) are radiogenic isotopes and the daughter products of 238U, 235U
and 232Th, respectively (Komárek et al., 2008) through the nuclides
decaying process. Naturally, the occurrence and variation of stable Pb
isotopes in existence depend on the earth crust's mineral composition
and the rock age (Zaborska, 2014).
The isotopic fingerprint is an analysis based on the ratios of stable
isotopes of an element in order to identify the origin of the element. The
use of stable Pb isotope signatures (207Pb/206Pb, 208Pb/206Pb,
208
Pb/204Pb, 206Pb/204Pb, 204Pb/206Pb, 206Pb/207Pb) as geochemical
tracers in environmental studies is widely practiced based on the si-
milarities and differences in the isotope ratios (Choi et al., 2007; Bird
et al., 2010; Cheng and Hu, 2010; Ferrat et al., 2012; Izquierdo et al.,
2012; Kim et al., 2013; Kamenov and Gulson, 2014). The distribution of

⁎
Corresponding authors.
E-mail addresses: adiana.ghazali@gmail.com (G. Adiana), hafizanjuahir@unisza.edu.my (H. Juahir).

http://dx.doi.org/10.1016/j.marpolbul.2017.08.055
Received 22 February 2017; Received in revised form 23 August 2017; Accepted 26 August 2017
0025-326X/ © 2017 Elsevier Ltd. All rights reserved.

Please cite this article as: Ghazali, A., Marine Pollution Bulletin (2017), http://dx.doi.org/10.1016/j.marpolbul.2017.08.055
G. Adiana et al.
Pb isotopes and the fingerprint method for the metals in environment
archives help to quantify the anthropogenic metal pollution for a given
site and assist in the identification of the sources as well as the path-
ways of contaminants by differentiating the geogenic and anthro-
pogenic elements. The concentrations of primordial Pb, U and Th, the
half-lives of the parent isotopes and concentrations of Pb, U and Th in
the original magmatic mixture are the factors which affect the differ-
ences in the isotopic signatures (Komárek et al., 2008). Besides that, the
Pb isotopic composition is not significantly affected by the physical-
chemical fractionation processes.
The Pb isotopic ratio interpretations are commonly presented in a
simple linear trends diagram that compares the isotopic ratios
(Kylander et al., 2010; Walraven et al., 2014). Apart from that bar
graph, a box plot of Pb isotopic ratio range was also widely applied to
display the comparison of the same Pb isotopic ratio at various places
(Bollhöfer and Rosman, 2000; Geraldes et al., 2006). The similar value
or the range of Pb isotopic ratio at different places indicates the similar
Pb sources. Besides that, if Pb isotopic ratio value showed a similar
value with galena from elsewhere, it may indicate that the Pb finger-
print sources are from that particular galena (Geraldes et al., 2006;
Bazzano et al., 2014).
The SCOPUS online database (www.scopus.com) has listed five ar-
ticles found in Brunei Bay area from 1968 to 2012. These articles were
discussed on the deposited sediment into the Champion Delta
(Lambiase and Cullen, 2013), the distribution of dugong (Rajamani and
Marsh, 2010), the concern on the oil spills (Rahmat and Yusof, 2005;
Wing, 2005) and the proboscis monkey (Yeager, 1995). Meanwhile, a
local researcher from Universiti Malaysia Sabah, Saleh et al. (2007)
emphasized the need for environmental regulation enforcement to
protect and conserve the unique diversity of Brunei Bay. Bengayawan
(2007) wrote an article in the Brunei Times on the call for a serious
attention towards the health of Brunei Bay ecosystem due to the
dumping of sewage effluent, domestic sewage, urban waste run-off and
the vigorous mangrove cutting activities. The main purpose of the
present study was constructed to identify the source of Pb in the Brunei
Bay ecosystem. This study will able to classify the area that is being
dominated by the anthropogenic and natural Pb using the chemometric
analysis.
2. Material and methods
2.1. Sample collection and analysis
Water and surface sediment samples were collected at 18 stations in
the coastal area (coastal station) during May 2013, October 2013, and
April 2014. In the meantime, both samples were collected at the coastal
station and additional 31 stations during June 2013 and January 2014
which covered the middle bay (transect station) and Labuan Island
(Labuan station) as presented in Fig. 1.
All the apparatus, sampling equipment and sample bottles were
previously cleaned using a cleaning agent, Decon 90 and soaked in
diluted nitric acid (10%) for one week. All cleaned and soaked materials
were thoroughly rinsed with deionized water to remove trace metals on
the apparatus surface. Later, these materials were then dried under a
Class-100 laminar flow hood and kept in clean polyethylene plastic
bags. Chelex-100 resin and polytetrafluoroethylene (PTFE) membranes
were soaked in 10% nitric acid for three days prior to remove trace
metals on the surface of resin and membranes. Water samples were
collected using an acid washed Teflon Mercos sampler. To avoid con-
tamination of metals such as lead and zinc from the boat, water sam-
pling activity was done at the front of the boat. Sampling bottles were
flushed completely with water sample before filling the bottle with
water sample. Sample bottles were wrapped in plastic bags and stored
in an ice-chest loaded with ice to minimize the biological activity that
may happen.
The water sample was filtered using 0.45 μm PTFE membranes for
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Marine Pollution Bulletin xxx (xxxx) xxx–xxx
dissolved and particulate Pb whereas surface sediment sample was
sampled using Ponar grab and kept in double layer zip-lock plastic bags.
Dissolved sample was preserved with concentrated nitric acid in the
acid-washed polyethylene (PE) bottle whereas the particulate samples
retained on the filtered PTFE membrane was kept individually in a PE
container. Both samples were then sealed in PE bag individually. All
samples were then kept at low-temperature prior transportation to the
laboratory. The physical parameters were measured in-situ during the
sampling trip by using well-inspected ADCP SonTek 0.5 kHz,
Multiparameter YSI 6600, CTD Seabird and portable HANA pH/ORP
meter HI 8424.
Dissolved samples were pre-concentrated using Chelex-100 resin
under Class-100 clean laminar flow hood whereas particulate and sur-
face sediment samples were digested using a mixture of Suprapur acids
in the Teflon bomb under oven heating (Bowles et al., 2006; William,
2008; Adiana et al., 2014; Adiana et al., 2016). It is generally believed
that the measurement of Pb stable isotopes should be carried out using
thermal ionization mass spectrometry (TIMS) or Multiple Collector In-
ductively Coupled Plasma Mass Spectrometry (MC-ICP-MS). In the
present study, the stable Pb isotopes in the collected samples were
analyzed using Quadrupole Inductively Coupled Plasma Mass Spectro-
metry (Q-ICP-MS) due to the laboratory constraint. According to Ettler
et al. (2004) and Marguí et al. (2006), a proper analysis of stable Pb
isotopes using Q-ICP-MS can be carried out with the instrumental bias
correction and validation using SRM 981, Common Lead Isotopic
Standard. The method used in the present study was adopted from
Townsend et al. (1998). The mass bias discrimination in collected
samples was corrected using the external standard, i.e. SRM 981 in
order to identify the ‘true’ values of stable Pb isotopes. In order to
correct isotope fractionations in Pb isotopes, SRM 981 standard (50 ppb
and 100 ppb) was measured before and after the sample measurement.
Up to 4 min of rinsing time was performed between each sample. This
normalization method was performed on all samples measured for Pb
isotopic composition as determined by ICP-MS (Townsend and Snape,
2002). The measurements were performed in 1200 sweeps scan mea-
surement. The recovery results are recorded in Table 1.
2.2. Data analysis
Cluster analysis was carried out using PRIMER ver.6 (Singh et al.,
2005) in order to define the similarity of stable Pb isotopes ratio be-
tween the sampling locations. The raw dataset was treated as en-
vironmental data type with sampling location as the variable. The da-
taset was transform using Log (X + 1) and the cluster analysis between
the variables was carried out using resemblance measure of Euclidean
distance (Chabukdhara and Nema, 2012).
To investigate the discrimination within the data set, discriminant
analysis (DA) was applied on the raw data set of the 18 coastal stations
which represent the most complete collected data set within all sam-
pling periods. The sampling stations were grouped into three major
areas, namely, river, estuary, and coastal based on the sampling loca-
tion. To facilitate the spatial dissimilarity using DA, the raw data set
was divided into sampling areas as the dependent variables and the
ratios of stable Pb isotope are represented as the independent variables.
On the other hand, the raw data sets for temporal variations, few groups
of seasons were treated as dependent variables while the stable Pb
isotope ratios stand for independent variables. In this study, DA was
utilized to the raw data set using XLSTAT 2014.5.03 (Retnam et al.,
2013). The temporal (seasons) and spatial (stations) variations in stable
Pb isotope ratios were calculated using standard, forward stepwise, and
backward stepwise modes where all variables are reviewed and eval-
uated to be included in the model (Juahir et al., 2009; Juahir et al.,
2011).
G. Adiana et al. Marine Pollution Bulletin xxx (xxxx) xxx–xxx

Fig. 1. Sampling stations.

Table 1 showed a pollution level of moderately polluted to polluted (Adiana

Analytical quality control data for stable lead isotopic ratios. et al., 2016).
A resemblance image of cluster analysis of the stable Pb isotope
Isotopes ratio SRM 981 certified value SRM 981 measured Recovery (%)
value
ratios in Brunei Bay using the data set of stable Pb isotopic ratio for
dissolved, particulate and surface sediment samples in shown in Fig. 3.
207
Pb/206Pb 0.91464 ± 0.00033 0.98772 ± 0.00061 107.99 In general, the lowest Euclidean distance value, i.e. 0.015 has
208
Pb/206Pb 2.1681 ± 0.0008 2.13226 ± 0.00073 98.35 classed the sampling stations into 10 different areas (Fig. 4a) based on
their exclusive signature. The area was labeled as follows:
3. Results and discussion
i. SCS: indicated the effect of South China Sea towards the sampling
stations.
Fig. 2 shows the range of stable Pb isotopic ratios in surface sedi-
ii. River: shows a unique signature of the river system, namely,
ment and in dissolved and particulate phase during all sampling per-
Menumbok River at station B14, Weston River at station B4, and
iods. The ratio of 208Pb/207Pb in dissolved, particulate and surface se-
Lawas River at station B8.
diment ranged from 2.385–2.494, 2.431–2.509 and 2.441–2.499,
iii. LMB: found to be affected by the transportation and boat traffic
respectively while 208Pb/206Pb ratio ranged 2.074–2.119, 2.055–2.18
activities as it is the main route connecting Labuan Island to
and 2.081–2.128 in dissolved, particulate and surface sediment con-
Menumbok and Brunei.
secutively. The ratio of 206Pb/207Pb found in dissolved, particulate and
iv. Northern: the anchoring area for ships and tankers which are
surface sediment was in the range 1.140–1.207, 1.138–1.219 and
protected by the Labuan Island.
1.14–1.21, respectively. Besides that, the range of 207Pb/206Pb in dis-
v. Weston: an area which received input from Weston River is flushed
solved, particulate and surface sediment was 0.8311–0.861,
out.
0.811–0.865 and 0.831–0.868 respectively.
vi. Lawas: an area which received input from Lawas River is flushed
In general, between May 2013 and April 2014, the concentration of
out.
Pb in Brunei Bay was in the range of 0.09–3.25 μg/L, 0.08–2.60 μg/g,
vii. Middle: the middle region of Brunei Bay and received mixed input
and 9.72–37.4 μg/g in dissolved phase, particulate phase and surface
from other areas.
sediment, respectively. The concentrations of Pb in collected samples
viii. Southern: a shallow mudflat area which is fully occupied with
are generally below and comparable to those reported elsewhere
fishing activities.
(Table 2). Based on the comparison with Malaysia Marine Water
ix. B7: received input from Sipitang paper mill.
Quality Standard (INWQS), the range of dissolved Pb in Brunei Bay
x. B15: an area connected to Sungai Raya which is linked to Labu
waters was classified as background level which meets the marine
Forest Reserve and Selirong Recreational Park, Brunei.
protected areas requirements. Similarly, the range of particulate Pb in
Brunei Bay waters was grouped as non-anthropogenic Pb as the con-
The Euclidean distance of 0.044 (Fig. 4b) merged the area labeled
centration range falls within a 95% confidence level of the normal-
LMB, SCS, Northern, Middle, Weston, River, and B7 into one large area.
ization plots with none enrichment factors (Adiana, 2016). However,
This area is identified as the industrialization-related areas, namely, the
the enrichment factor (EF) of Pb in the surface sediment of Brunei Bay
boat traffic, ships and tankers anchoring area, petroleum-related ac-
showed a minor (EF = 1.23) and moderate enrichment (EF = 3.62)
tivities, tourism, paper mill, logging, palm oil plantation and dense
during May 2013 and July 2013 respectively. Additionally, the geoac-
local settlement. Other than that, the Euclidean distance of 0.044 has
cumulation index (Igeo) during May 2013 (Igeo = 0.88) signified Pb in
classed other areas as Lawas (an area with a larger scale of human
the surface sediment of Brunei Bay was classified as non-polluted to
settlement that mainly engage in fishing activities using small boats);
moderately polluted level whereas in July 2013 (Igeo = 2.19), Pb

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G. Adiana et al. Marine Pollution Bulletin xxx (xxxx) xxx–xxx

Fig. 2. Boxplot of Pb isotopic ratio in surface sediment, dissolved phase and particulate phase for all sampling periods, showing the range, median, and standard deviation values.

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G. Adiana et al. Marine Pollution Bulletin xxx (xxxx) xxx–xxx

Table 2
Comparison of Pb concentration reported elsewhere.

Location Sample Concentration of Pb Reference

Upper Continental Crust Earth crust 17 Wedepohl (1995)

South China Sea off Sabah, Sarawak & Brunei Darusalam Dissolved (μg/L) 4.144–311 Utoomprukporn and Snidvongs (1999)
Particulate (μg/g) < 4144
Florida Bay, USA Sediment (mg/kg) 8.4 Caccia et al. (2003)
Izmit Bay, Turkey Sediment (mg/kg) 102 Pekey (2006)
Kranji and Pulau Tekong, Singapore Dissolved (μg/L) 0.009–0.062 Cuong et al. (2008)
Particulate (μg/g) 1.10–6.08
Tianjin coastal area of Bohai Bay, China Water (μg/L) 3.63–12.65 Meng et al. (2008)
Sediment (mg/kg) 17.5–34.9
Yangtze River, China Water (mg/L) < 0.0002–0.0024 Yi et al. (2008)
Sediment (mg/kg) 34.2–44.17
Luoyuan Bay, China Seawater (μg/L) 0.35–1.70 Wang et al. (2010)
Eastern Beibu Bay, SCS Sediment (mg/kg) 7.12–49.33 Duo et al. (2013)
Guanabara Bay, Rio de Janeiro Sediment (mg/kg) Fonseca et al. (2013)
Dry season 22.5–89.6
Wet season 62.7–116.8
Quanzhou Bay, China Sediment (mg/kg) Zhao et al. (2013)
Inner Bay 12.9–191
Open Bay 18.3–217
Zhelin Bay, China Sediment (mg/kg) 50.9 Gu et al. (2014)
Yangtze Bay, China Sediment (mg/kg) 23.4 Wang et al. (2014)
Oyster Bay, Australia Sediment (mg/kg) 98 Alyazichi et al. (2015)
Daya Bay, China Sediment (mg/kg) 51.3 Gu et al. (2016)
Brunei Bay, Borneo Dissolved (μg/L) 0.09–3.25 Brunei Bay
Particulate(μg/g) 0.08–2.60 (Present study)
Sediment (mg/kg) 9.72–37.4

Southern (an area that has a lower level of human settlement and more
pristine environment, with a large area of seagrass beds) as well as B15
(the most pristine area amongst the sampling stations in Brunei Bay).
The classification matrices for both spatial and temporal variations
of stable Pb isotope ratios in Brunei Bay by using DA are shown in
Table 3 and Table 4.
In Table 3, the spatial discriminant standard mode generated
78.57% assignments correctly with 20 discriminant variables
(p < 0.05). Meanwhile, the accuracy of spatial classification using
forward stepwise and backward stepwise mode discriminant function
analysis are similar, i.e. 64.29% with one discriminant variable. The
standard mode score plot for different sampling areas (Fig. 5) showed
that the confidence circle of the river is overlapping with the estuary
and bay confidence circles. It proves the influence of Pb sources from
the river system towards the bay and estuary system. However, the
confidence circles for forward and backward stepwise mode with one
discriminant variable pointed out that the estuary area data set was
largely influenced by the river system compared to the bay system.
The temporal dissimilarity using DA was applied using standard and
backward stepwise model (Table 4). The temporal classification accu-
racy was 100% with 14 discriminant variables for standard mode,
whereas the accuracy of temporal classification for backward stepwise
mode was 55% correct with three discriminant variables. The score plot
for temporal discriminant (Fig. 6) showed that discriminant function
analysis (DFA) for January 2014 data set was plotted on the positive
value of the x-axis which represents the northeast monsoon (NE). The

Fig. 3. Resemblance diagram of the Pb iso-

topic ratio in Brunei Bay samples.

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Fig. 4. The classification of Brunei Bay area based on the cluster analysis.

Table 3 DFA of May 2013 and July 2013 data set was plotted on the negative
Classification matrix for spatial variations of stable Pb isotope ratios in Brunei Bay, value of the x-axis which represents the southwest monsoon (SW)
Borneo. period. As for the DFA of April 2014 and October 2013, the data set was
Spatial classification matrix
plotted in between both NE and SW data set which signified the mon-
soon interchange period.
Sampling region Predicted regions (%) Percentage of correct A comparison of present stable Pb isotope ratio data set in Brunei
Coastal Estuary River classification Bay with elsewhere is plotted using a bar graph in Fig. 7.
Standard mode
The Pb isotopic ratios found in dissolved, particulate and surface
Coastal 19 2 0 90.48%
Estuary 3 11 1 73.33% sediment of Brunei Bay were similar to those found elsewhere. The Pb
River 1 2 3 50.00% isotopic ratio values in Brunei Bay are in the range of values for at-
Total 23 15 4 78.57% mospheric aerosol and coal, the aerosol from boat and ship traffic, land-
Forward stepwise mode based transport and industrial activities. The similarity of aerosol Pb
Coastal 19 2 0 90.48% ratios in Brunei Bay with elsewhere is in agreement with those found by
Estuary 7 8 0 53.33% Chen et al. (2016). They carried out a research on the exchange of Pb
River 2 4 0 0.00%
Total 28 14 0 64.29%
isotope between dissolved and suspended particulate matter of Johor
estuary. The study found that the Pb isotope ratios found in the surface
Backward stepwise mode
water and corals match the Pb ratio found in the atmospheric aerosol.
Coastal 19 2 0 90.48%
Estuary 7 8 0 53.33% Therefore, it is proven that the dominant source of Pb in marine en-
River 2 4 0 0.00% vironment originates from the atmospheric aerosol. In April 1998, the
Total 28 14 0 64.29% Malaysian government took the first step of banning the sale and usage
of leaded petrol in order to protect the country's air quality (The New
Straits Times, 1998). By the year of 2000, leaded petrol was completely
Table 4
phased out in Malaysia. In spite of this, the International Energy Sta-
Classification matrix for temporal variations of stable Pb isotope ratios in Brunei Bay,
Borneo. tistics recorded the coal consumption in Malaysia increased drastically
by 1999 with a total of 1412 thousand short tons and the value kept on
Temporal classification matrix increasing to 27,153 thousand short per tons in the year 2012. There-
fore, the deposition of Pb aerosol from atmospheric has increased cor-
Sampling Predicted regions (%) Percentage of
region correct
responding to the increase of coal burning in Malaysia.
May July October January April classification Pb isotopic ratio found in Brunei Bay also shows some resemblance
2013 2013 2013 2014 2014 with coal. Although the coal consumption in Malaysia has drastically
increased, there are no coal-fires power stations spotted in the vicinity
Standard mode
May 2013 4 0 0 0 0 100.00%
of Brunei Bay. Based on Hutchison (2007), the geographic structure of
July 2013 0 4 0 0 0 100.00% Borneo Island mainly within the Brunei Bay area is composed of are-
October 0 0 4 0 0 100.00% naceous sediment type during the Upper Tertiary period. Arenaceous
2013 sediment is composed of sand and sandstones which include coal seams.
January 0 0 0 4 0 100.00%
The existence of coal seams in Borneo Island geographic composition
2014
April 2014 0 0 0 0 4 100.00% explains the coal fingerprints in Pb isotopic ratios in Brunei Bay. This
Total 4 4 4 4 4 100.00% finding is in agreement with coal source rocks of northwest Borneo
Backward stepwise mode
found by Chua et al. (1987) and Abdullah (2003). Besides the deposi-
May 2013 2 1 0 0 1 50.00% tion of coal burning into the water system, the source from coal rocks is
July 2013 1 1 2 0 0 25.00% counted to result in the trace of Pb in the Brunei Bay ecosystem.
October 0 0 3 0 1 75.00% The Pb isotopic ratios range in surface sediment was smaller and
2013
placed within the total dissolved and particulate magnitude. A corre-
January 0 0 1 3 0 75.00%
2014 lation was also displayed between the water column and surface sedi-
April 2014 1 0 0 1 2 50.00% ment of Brunei Bay. This finding is in agreement with Hart and Tilton
Total 4 2 6 4 4 55.00% (2013) as they found a strong correlation between Lake Superior

6
G. Adiana et al.
Fig. 5. The spatial discriminant score plot.
surface sediment and water by comparing the magnitude of Pb isotopic
ratios.
4. Conclusions
This study has used the empirical findings to trace the sources of Pb
in Brunei Bay by using the stable Pb isotopic ratio analysis. Generally,
based on INWQS guidelines, the concentrations of Pb in Brunei Bay
waters proved to be at a natural level of an aquatic ecosystem.
However, between May 2013 and July 2013 sampling period, there was
some minor enrichment of anthropogenic Pb in the surface sediment of
Brunei Bay which led to a moderate pollution level of Pb. The resem-
blance analysis with the smallest Euclidean distance (0.015) has clas-
sified the sampling stations into a few areas, namely, Lawas, Southern,
Weston, Middle, Northern, River, SCS, LMB, B7, and B15. Each class
displayed the unique signature based on their distinctive characteristics
and surrounding activities. The use of the largest Euclidean distance
(0.044) in the resemblance analysis has narrowed down the classifica-
tion into three main groups signifying the industrial-related activities,
and moderate and least human settlement areas and activities.
The forward stepwise and backward stepwise mode of spatial dis-
similarity by using DA has highlighted one discriminant variable with
64.29% assignments correctly. The confidence circles of score plot
showed that the river system has largely influenced the estuary system
Fig. 6. The temporal discriminant score plot.
7
Marine Pollution Bulletin xxx (xxxx) xxx–xxx
as compared to the bay system. Meanwhile, the temporal dissimilarity
using the backward stepwise mode has distinguished three discriminant
variables and the confidence circles of the score plot have set apart the
sampling periods into the northeast monsoon, southwest monsoon, and
the monsoon interchange period.
A comparison of Pb isotopic ratio in Brunei Bay with data from
other regions displayed the signature of aerosol input and coal use re-
lated activities. The framework strongly suggested that the major con-
tribution of anthropogenic Pb in Brunei Bay were derived from in-
dustrial activities around Brunei Bay. The land-based activities do count
in contributing a few of anthropogenic elements into the Brunei Bay
ecosystem. Furthermore, the Brunei Bay can be classified as a well-
preserved marine system but the increasing human population and in-
dustrial development may affect the Brunei Bay health in a matter of
time.
Acknowledgements
The Ministry of Education Malaysia (MOE) funded this research
through the Higher Institution Centre of Excellent (HiCoE) in a Marine
Science research grant (grant numbers: 66928). The authors would like
to thank MOE for the research grant and the Institute of Oceanography
and Environment for the assistance given during sampling and analysis.
Thank you to Universiti Malaysia Terengganu for providing the
G. Adiana et al. Marine Pollution Bulletin xxx (xxxx) xxx–xxx

206
Fig. 7. Comparison of Pb/207Pb ratio in Brunei Bay with elsewhere.

scholarship (Biasiswa Tuanku Canselor).
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