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Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia
MPB-07685; No of Pages 13 Marine Pollution Bulletin xxx (2016) xxx–xxx
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Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia Tuti Hartati Siregar a,⁎, Nandang Priyanto a, Ajeng Kurniasari Putri a, Novalia Rachmawati a, Radestya Triwibowo a, Larissa Dsikowitzky b, Jan Schwarzbauer b a b
Research Centre for Marine and Fisheries Product Processing and Biotechnology, Ministry of Marine and Fisheries, KS Tubun Petamburan VI Slipi, Jakarta, Indonesia Institute of Geology and Geochemistry of Petroleum and Coal, RWTH Aachen University, Lochnerstr. 4-20, 52056 Aachen, Germany
a r t i c l e
i n f o
Article history: Received 30 September 2015 Received in revised form 11 April 2016 Accepted 5 May 2016 Available online xxxx Keywords: Heavy metals Seawater Marine sediment Food safety Jakarta Bay
a b s t r a c t The Jakarta Bay Ecosystem is located in the vicinity of the megacity Jakarta, the capital city of Indonesia. Surrounding rivers and canals, carrying solid and fluid waste from households and several industrial areas, flow into the bay. Therefore, the levels of selected trace hazardous elements in water, surface sediments and animal tissues were determined. Samples were collected from two different seasons. The spatial distribution pattern of trace elements in sediment and water as well as the seasonal variation of the contamination were assessed. Quality assessment of sediment using the effects range median (ERM) showed that the concentrations of Hg, Cu and Cr at some stations exceeded the recommended values. Moreover, the concentrations of several trace hazardous elements in the sediments exceeded previously reported toxicity thresholds for benthic species. © 2016 Elsevier Ltd. All rights reserved.
1. Introduction Trace elements such as Cd, Hg, Cu, Pb and As are known as harmful pollutants in marine environments. These metals enter coastal ecosystems through riverine transport of trace element loads originating from the natural weathering of rocks in the catchment areas or from anthropogenic sources, such as industrial or municipal wastewater discharges. A further source is atmospheric deposition. Trace hazardous elements that have adverse effect on human health including lead (Pb), cadmium (Cd), copper (Cu), zinc (Zn) and nickel (Ni) have been detected in water and sediment from Jakarta Bay during the last 15 years (Arifin et al., 2012; Rochyatun and Rozak, 2007; Williams et al., 2000). Because the Jakarta Bay Ecosystem is located in the vicinity of the megacity Jakarta, and surrounded by industrial zones, trace hazardous elements reach the bay from several sources such as industrial discharges, municipal wastewater discharges, surface run-off and dust precipitation (Arifin et al., 2012; Idris, 2008; Tajam and Kamal, 2013; Williams et al., 2000). In addition, agricultural activities and aquaculture practices have also influenced the pollution in the Jakarta Bay. An example of aquaculture practices in Jakarta Bay is the massive culture of green mussels (Perna viridis) since 1979 (Haryati et al., ⁎ Corresponding author. E-mail address: [email protected] (T.H. Siregar).
2013) where the production reached 1270 tons in 2013 (BPS, 2015). The mussel is the most popular and economically affordable seafood product for the coastal communities in Jakarta, and has also been marketed to the surrounding cities such as Tangerang, Bandung and Cirebon. Therefore, despite the severe pollution in this area, the Jakarta Bay provides economic and social benefit for the local fishermen. Seafood production from Jakarta Bay supplies cheap protein source for consumers in Jakarta and its surrounding. However, the consumption of seafood from this area increases the risk for local communities to be exposed to the trace hazardous elements from Jakarta Bay (Putri et al., 2012). The contamination of Jakarta Bay with trace hazardous elements was reported to be comparable to some other big cities in Indonesia, such as Semarang and Surabaya. The trend of this contamination was reported to decrease during the last 10 years due to more strict regulations (Arifin et al., 2012; BPLDH, 2014; Hosono et al., 2011; Williams et al., 2000). Unfortunately, up to today huge amounts of poorly treated wastewaters are discharged into the 13 canals/rivers which flow into the Jakarta Bay (e.g. Dsikowitzky et al., 2016). An extensive research on the dynamical distribution of hazardous metals such as Hg, Pb, Cd, Cu, Cr, Co and As in Jakarta Bay is so far missing and was therefore conducted within the present study. This research aims to draw a complete picture of the spatial distribution of trace hazardous elements in Jakarta Bay considering also the origin of the
http://dx.doi.org/10.1016/j.marpolbul.2016.05.008 0025-326X/© 2016 Elsevier Ltd. All rights reserved.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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contamination, seasonal variations and possible accumulation of the studied elements by economic important bivalve and fish species in Jakarta Bay. 2. Materials and methods 2.1. Study site Jakarta Bay is located in the North of Jakarta, the capital city of Indonesia (latitude 106°21′ to 107°03′E and longitude 5°10′ to 6°10′S). Jakarta Bay is constrained by two capes, Tanjung Pasir to the West and Tanjung Karawang to the East. There are four major rivers discharging freshwater as well as wastewater from Jakarta and its surroundings settlements into the bay, namely Sungai Cisadane in the most westward and just outside of the bay, Sungai Angke and Sungai Ciliwung in the middle of the bay and Sungai Citarum with the largest river delta at the easternmost cape. The total area of Jakarta Bay is about 514 km2, with a shoreline length of 76 km (BPLDH, 2014). The depth of Jakarta Bay is 18 m on average (BPLDH, 2014; Hosono et al., 2011; Williams et al., 2000). Besides the four major rivers, there are smaller rivers and canals discharging around 1400 m3 solid and liquid waste into the center of the bay (BPLDH, 2014). The industrial areas which are located close to the Jakarta Bay such as Cilincing North Jakarta, Pulogadung - East Jakarta, Bekasi and Bogor may also contribute to the increasing pollution of the Jakarta Bay (at stations R1, R2, R3, R6, R14, R15, see Fig. 1). According to the Statistical Bureau of DKI Jakarta (BPS, 2014) the population of Jakarta City was 10.1 million in 2014, and the total area of Jakarta City was 662.33 km2. 2.2. Sample collection A sampling network of 26 sampling stations in Jakarta Bay and of 16 estuary stations were sampled in April (wet transitional to dry season,
sampling campaign I) and November 2014 (dry transitional to wet season, sampling campaign II) (Fig. 1). Sites were positioned along transects using a Garmin 585 global positioning system (GPS) with a resolution of about 3.5 m. Sample collection was done following the method described by Hutagalung et al. (1997). Surface sediment samples were collected using a Van Veen grab. They were stored in polypropylene tubes and kept on ice until being transported to the laboratory. Water samples were recovered from 1 to 2 m depth below the water surface using a Nansen bottle. The samples were filtered using a 0.45 μm PPDF filter, filled in polypropylene bottles, acidified with 1% HNO3 for preservation and kept on ice until being transported to the laboratory. For mercury analysis, samples were stored in brown glass bottles, preserved with HNO3 and K2Cr2O7 and kept on ice until being transported to the laboratory. Mussel samples were bought from the owners of aquaculture facilities in the Jakarta Bay, while fish samples were purchased from the local fisherman who at the time of sampling caught fish in the bay. Background information about the sampled fish and mussel species are presented in Table 1. In situ measurements such as pH, salinity, temperature and turbidity were also performed. All samples were stored at 4 °C prior to analysis. 2.3. Sample preparation and analysis Before analysis, all laboratory equipment was cleaned with 2% nitric acid pro analysis (Merck, USA). Sample preparation and analysis was performed following the method provided by the instrument manual (Berghoff, Germany for microwave destruction and Agilent 7700X, USA for ICPMS analysis). Sediment samples were dried in an oven at a temperature of 105 °C for 8 h. 100 mg sample aliquots were placed in a digestion vessel. Then 8 ml of HNO3 (65%, suprapur) and 2 ml of HF (40%, pro analysis) were added. After 2 min, the vessel was closed and heated in a microwave oven (Berghof speedwave two, Germany) with the program stated in
Fig. 1. Schematic map of the study area. Water and sediment samples were taken in Jakarta Bay and at the mouths of the rivers/canals which discharge into Jakarta Bay. The sampled rivers/ canals flow through the Greater Jakarta City area. Green dots indicate the aquaculture facilities where green mussel samples (Perna viridis) were taken. The black dots indicate the locations where fish samples were bought from the local fishermen. (For interpretation of the references to color in this figure legend, the reader is referred to the web version of this article.)
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx Table 1 Scientific names, common names, habitat and feeding mode of the investigated mussel and fish species from Jakarta Bay. Common name/ Scientific name Green mussel/Perna viridis Flounder/Isettodes irumei Yellow tail fish/ Caesio erythrogaster White emperor Hairtail/Trichiurus savala Mullet/Valamugil speigteni Squid/Loligo sp Treadfin brean/ Nemipterus nematophorus Ponny fish/Lelognathus equulus Fringescale sardine/ Sardinella fimbriata
Habitat
Feeding mode
April, November 2014 April 2014
Demersal Carnivore
April, November 2014
Demersal Pelagic Pelagic Demersal
April, November 2014 April 2014 April 2014 April, November 2014
Carnivore Carnivore Carnivore Carnivore
Demersal Carnivore
November 2014
Demersal Herbivore
November 2014
Pelagic
November 2014
Carnivore
Table 2. After cooling, 0.5 ml of the sample was diluted with 9.5 ml of HNO3 (1%). Fish tissue (250 g), from 1 to 3 individual fish, depending on their weight, was blended altogether and dried in an oven at 105 °C for 8 h. Subsequently, 150 mg of the dried samples were placed in a digestion vessel. Ten milliliters of HNO3 (65%, suprapur) was added, then the vessel was closed and heated in a microwave (Berghof, Germany) with the program stated in Table 2. After cooling, 1 ml of the sample was diluted with 9 ml HNO3 (1%). The soft mussel tissue from 1 kg sample aliquots (including shells) was prepared according to the same procedure as the fish tissue. One milliliter of water sample was poured into a vessel and 9 ml of HNO3 (65%, suprapur) was added. After the vessel was closed, it was heated in a microwave (Berghof, Germany) with the program stated in Table 2. After cooling, 1 ml of sample was diluted with 9 ml of HNO3 (1%). The total concentrations of the elements Pb, Hg, Cu, Cd, As, Cr and Co in sediment samples, tissue samples and water samples were determined with an ICPMS 7700X (Agilent, USA). Operating conditions of this device are given in Table 3. Trace hazardous element concentrations were determined in surface sediment, water and animal tissue samples by performing two replicated extractions. Mean concentrations of each element are shown in Tables S1–S6 of the supplementary material. ICPMS calibration was performed using standard solutions with defined concentrations. The isotopes used for measurements and calculations were 208Pb, 202Hg, 63Cu, 111Cd, 75As, 52Cr and 59Co. A series of standard solutions (1 ppb, 5 ppb, 10 ppb, 20 ppb, 30 ppb, 40 ppb, 50 ppb and 80 ppb) was measured. A blank solution using 1% of
Table 2 Digestion program for sample preparation. Step
T (C)
P (bar)
Table 3 Operating condition of ICPMS 7700X. Forward rf power Plasma gas flow rate Carrier gas Sampler and skimmer cones Integration time Sampling period No. of replicates Tune mode
Sampling time
Pillar Filter feeder Demersal Omnivore
Time (min)
3
1550 W 15 l/min 1.05 l/min Platinum 0.1 s 0.3 s 3 He
HNO3 was prepared for each set of analysis to check the possibilities of contamination during the digestion procedure. Target element concentrations in procedural blanks were negligible. The accuracy of the analytical procedure was checked using the certified reference material (CRM) PACS-2 (NRC, Canada). Analysis was done according to the method described above for the sediment analyses in four replicates. The recovery rates of the heavy metals in the CRM are listed in Table 4. 3. Results and discussion 3.1. Concentrations and spatial distribution of trace hazardous elements in surface sediments from the Jakarta coastal area The concentration levels of the trace hazardous elements Pb, Hg, Cd, Cu, As, Cr and Co in sediment samples from Jakarta Rivers and Jakarta Bay are shown in Fig. 2. All determined concentrations are given in detail in the Supplementary Material of this article (Tables S1 and S2). A comparison of the values of the trace elements in this study to previous conditions of Jakarta Bay (Williams et al., 2000) shows that the concentrations of several metals (Cr, Cu, Pb) were three to five times higher than in 1996. However, the concentrations of other metals such as As and Co remained equal between 1996 and 2014. Previous studies at two dams of the Citarum River, a river discharging into the easternmost part of Jakarta Bay, i.e. Cirata and Saguling Dam, showed concentrations of less than 10 mg kg−1 of Hg, Cd, Cu and Pb in the year 2005 (Table 5). The average concentrations of trace hazardous elements in Jakarta Bay sediments as determined in this study are similar to those of coastal sediments taken from the vicinity of other big Asian cities (Table 5) (Censi et al., 2006; Chakraborty et al., 2014; Murtini and Rachmawati, 2007; Nakata et al., 2008; Priyanto et al., 2008; Wang et al., 2010). The spatial distribution of the studied trace hazardous elements in surface sediments of Jakarta Bay and Jakarta rivers is also shown in Fig. 2. The element concentrations in the river sediment samples were in the same range or higher than those of the bay sediments (Fig. 2). Higher concentration levels of most considered elements in the river sediments as compared to the bay sediments indicate that the major sources of these elements is riverine transport. The rivers discharge trace hazardous element loads into the bay which may originate from anthropogenic sources or from the natural weathering of volcanic rocks in the river catchments. This was assessed in detail by (Sindern
Power (%)
Digestion program for sediment samples 1 170 30 2 200 30 3 50 25
10 20 10
80 90 0
Digestion program for water samples 1 200 30 2 130 30 3 100 25
20 5 5
70 90 0
Digestion program for tissue samples 1 140 30 2 160 30 3 175 35 4 50 25
5 5 20 10
100 100 100 0
Table 4 Results of the analyses of certified reference material and standard deviation of the obtained results. Element Cr Cu As Cd Co Pb Hg
Certified value PACS-2 (mg kg−1) 90.7 ± 4.6 310 ± 12 26.2 ± 1.5 2.11 ± 0.15 11.5 ± 0.3 183 ± 8 3.04 ± 0.2
Measured value (n = 4) (mg kg−1)
Recovery rate (%)
77 ± 3.3 240 ± 8 31 ± 1.3 2.08 ± 0.15 9.9 ± 0.3 165 ± 3 2.9 ± 0.1
85 77 118 99 86 90 95
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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et al.(2016-in this issue). They showed the importance of geogenic inputs for the composition of As, Cr and in part Cu in river sediments from the Jakarta City area. Furthermore, this study indicates the presence of small-scale local Cr emissions in the northern central part of
Jakarta City. The contamination of Jakarta river sediments with Pb and to a minor extent Cu is controlled by anthropogenic sources, mainly in the central part of Jakarta City. This is in line with Williams et al. (1997, 2000) who found that geogenic sources control the abundance
Fig. 2. Trace hazardous element concentration in surface sediments sampled in April 2014 (left bars) and November 2014 (right bars). All concentrations are given in mg kg−1 dry weight.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
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Fig. 2 (continued).
of Cr (as well as Co) in Jakarta Bay sediments, while Cu and Pb mainly originate from anthropogenic sources (Williams et al., 1997, 2000). The spatial distribution of the elements which are known to have a mainly geogenic source, Co and As (Fig. 2), shows similar concentration
levels at all river/canal stations in the studied area. Only at station R1, a higher As concentration in the sediments was observed. Pb, Cu and Cr concentrations which at least partly originate from anthropogenic sources were highest at the river/canal mouths discharging into the
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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Fig. 2 (continued).
western and eastern part of Jakarta Bay. The rivers in the eastern and western parts of the study area receive the effluents from the major industrial areas in or close to Jakarta City. In Bekasi and Cikarang, in the Southeast of Jakarta, where the biggest industrial areas of Indonesia
are located, the industrial wastewaters are discharged into the Citarum River, Cikarang River and Western Tarum Channel. These rivers/canals discharge into Jakarta Bay at stations R14–R16. Another industrial area is located at the Cisadane River, which discharges into the westernmost
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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Fig. 2 (continued).
Table 5 Concentrations of trace hazardous elements (mg kg−1) in sediment samples from Jakarta Bay in comparison to other Asian coastal areas. Location
Pb
Hg
Cd
Cu
As
Cr
Co
References
Jakarta Bay, Indonesia Saguling Dam, Indonesia Cirata Dam, Indonesia Other Asian countries Thailand Gulf, Thailand Jinzhou Bay, China Yatsushiro Bay, Japan Minamata Bay, Japan Kranji, Singapore Tekong, Singapore
bLOD-357 0.1–0.2 0.01–0.03
bLOD-9 0.1–0.3 0–1
bLOD-13 0.03–0.2 0.02–1
bLOD-515 1–11 0.5–7
bLOD-69 – –
bLOD-951 – –
bLOD-36 – –
This study Murtini and Rachmawati (2007) Priyanto et al. (2008)
– 41–460 18–56 10–19 24–24 24–37
– – 0.02–3.4 0.4–3.4 – –
– 1.5–64 –
8–364 26–400 3.2–64 3.7–25 15–21 6.3–8.7
– – –
27–1104 – –
17–716 – –
Censi et al. (2006) Wang et al. (2010) Nakata et al. (2008)
– –
– –
– –
Chakraborty et al. (2014)
0.15–0.22 0.05–0.07
eastern Jakarta Bay (Fig. 2). This could be due to re-suspension of surface sediments and transport of suspended particles with the water masses circulating within the Jakarta bay in a counter clockwise pattern (van der Wulp et al., 2016-in this issue).
part of Jakarta Bay (station R1). In Jakarta City, the stations R4 and R5 are influenced by the Ciliwung river system, which brings industrial wastewaters from Bogor. The spatial distributions of all determined trace hazardous elements in Jakarta Bay sediments (Fig. 2) did not show clear seaward concentration gradients as previously reported from an investigation on sediment cores from the bay conducted by Williams et al. (2000). The higher concentrations of the elements Pb, Cu, Cd and Cr at the easternmost and westernmost river stations were not reflected by higher concentrations of the respective elements in the sediments from the western and
3.2. Concentrations and spatial distribution of trace hazardous elements in water samples from the Jakarta coastal area The concentrations of trace hazardous elements in Jakarta Bay water and Jakarta river water were far lower than in the
Table 6 Concentration of trace hazardous elements (μg l−1) in water samples from Jakarta Bay in comparison to data from previous studies in the Greater Jakarta area. Location
Pb
Hg
Cd
Cu
As
Cr
Co
References
Jakarta Bay, Indonesia Jakarta Bay, Indonesia Saguling Dam, Indonesia Cirata Dam, Indonesia Maximum concentration (in μg L−1)
bLOD-492 bLOD-3.62 0.04–4 bLOD-1 50
bLOD-95
bLOD-9 bLOD-0.16 0.9–22 1–20 10
bLOD-805 bLOD-404 2–127 0.1–63 50
bLOD-31
1–9521 bLOD-4.0 – –
bLOD-52
This study Williams et al. (2000) Murtini and Rachmawati (2007) Priyanto et al. (2008) MenLH (2004)
0.05–6 0.1–63 3
– –
– –
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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sediments at the same stations. At some stations, water concentrations were below the limit of detection. The determined concentration ranges of Pb, Hg, Cd, Cu, As, Cr and Co in water samples from the study area are shown in Fig. 3. All values are documented in detail in Tables S3 and S4 of the Supplementary Material of this
article. Table 6 shows a comparison of the trace hazardous element concentration ranges in water determined in this study as compared to previous studies from the working area, where the concentration of Pb, Hg, Cu and Cr in this study were higher while Cd was lower.
Fig. 3. Trace hazardous element concentrations in water samples taken in April 2014 (left bars) and November 2014 (right bars). All concentrations are given in μg l−1.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
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Fig. 3 (continued).
Regarding the spatial distribution of the river contamination with trace hazardous elements, similar concentration levels of Co, As, Cu and Hg at all river/channel stations in the study area can be observed (Fig. 3). This is in line with the spatial distribution of Co, As and Hg in the river sediments (Section 3.1). However, Cu concentrations at the
river sediments were higher in the rivers/canals discharging into the western part of the bay (Fig. 2), but this pattern was not mirrored by the contamination of the aqueous phase. Pb and Cd were only detectable in river water samples from the western part of the study area and Cr concentration was very high at station R1 in the west. This
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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Fig. 3 (continued).
pattern may reflect the industrial inputs in the western part of the study area (Section 3.1), but the results are not as clear as for the sediment samples. Chromium might partly originate from small-scale tanning industries which occur widespread in Jakarta and its surrounding cities.
Chromium is used for several industrial purposes such as chrom plating, leather tanning and wood treatment. According to the Agency for Environmental Control, Jakarta, there are numerous leather tanneries in Jakarta (BPLDH, 2014).
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
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Fig. 3 (continued).
The spatial distribution of trace hazardous elements in water samples from the bay did not show a clear trend in regard to Cu, Cr, Pb, As, Cd and Co (Fig. 3). In contrast, the Hg concentrations in water samples from the western part of the bay were higher than in the central and eastern part of the bay. Noteworthy, the Hg concentrations in the seawater samples were higher than in the river water samples (Fig. 3). Rofiq and Takanobu (2011) assessed the history of mercury pollution in Java Island and observed that the mercury contamination of surface waters mainly originated from land-based sources, such as industrial wastewaters and gold-mining activities (Rofiq and Takanobu, 2011). However, our data from the Jakarta Bay area show higher Hg concentrations in seawater than in river water, thus do not confirm these findings. In addition, the Hg concentrations in Jakarta river sediments and water samples did not show elevated concentrations in the rivers receiving industrial wastewaters (see Section 3.1). The higher Hg concentrations in seawater could be correlated with a mercury input source in the near shore region. Such sources could be the use of Hg contaminated municipal incinerator ash as substitute for sand in artificial reefs (MacDonald, 1994) or waste-dumping from shipping vessels. The concentrations of Hg and Pb at some stations from the first and second sampling campaign exceeded the maximum concentrations of these elements in water as regulated by the Indonesian government (MenLH, 2004). Furthermore, the concentration of Cu at all stations during the second sampling campaign exceeded the maximum level allowed in water. Maximum concentrations of Hg, Cd, Cu, Pb and Zn in marine water established by the Indonesian government are 3, 10, 50, 50 and 100 μg l−1, respectively (MenLH, 2004). 3.3. Seasonal variation of trace hazardous element concentrations in water and sediment samples from the Jakarta coastal area The concentrations of all determined trace hazardous elements were higher in the sediments sampled in November 2014 (second sampling campaign) as compared to the samples taken in April 2014 (first
sampling campaign) (Fig. 2). The first sampling campaign took place after the wet season, marked with several weeks with heavy rainfall. The second sampling in November was conducted at the beginning of the wet season, after several weeks with less rainfall. We conclude that the strongly enhanced run-off in the river catchment areas during the wet season is accompanied by a dilution of the contaminated river sediments which are transported into Jakarta Bay. The order of elements concentration in the Bay for the first sampling campaign was Cd b Hg b Co b Cr b Pb b Cu b As. This order was slightly different in the rivers, which was Cd b Hg b Co b As b Pb b Cu b Cr. The order was changed in the second sampling campaign, which in the bay was Hg b Cd b Co b As b Cu b Cr b Pb. In the river for the second sampling campaign the order was Hg b Cd b As b Co b Cu b Pb b Cr. The behaviour of heavy metals in the Jakarta Bay can be divided into two groups, varies between the two weather conditions and constant regardless of the weather condition. The concentrations of Pb were higher in November while those of As were higher in April. Other elements such as Hg, Cd, Co, Cu and Cr were constant throughout the seasons. This finding is in accordance with the previously reported seasonal effects on concentration of several elements in sediments of the Cirata and Saguling Dam (Murtini & Rachmawati, 2007; Priyanto et al., 2008). Concentration of Cu in Jakarta Bay sediments were the highest among all metals. In November 2014, concentrations of most trace hazardous elements in water were higher than in April 2014 (Fig. 3). Concentration of Cu showed a large contrast at all sampling stations. In the first sampling campaign, its concentration was below the limit of detection. However, in the second sampling campaign the concentration was far above 200 μg l−1. A similar observation was made concerning the concentrations of Cr and Pb. The higher element concentrations in river water in November 2014 can be explained by the dry weather conditions prior to the sampling date and the low river-runoff, leading to the increase of concentrations in the river water.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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Table 7 Comparison of trace hazardous element concentrations in the sediment samples (mg kg−1 dry weight) with sediment quality guidelines (SQGs). SQGs are effect range median (ERM) in mg kg−1 dry weight from Long et al. (1995) for marine and estuarine sediments, the contaminant concentration at or above which adverse effects on benthic species frequently occur. Element
ERM (mg kg−1)
Concentrations April 2014 (mg kg−1)
Number of samples above threshold
Concentrations November 2014 (mg kg−1)
Number of samples above threshold
Pb Hg Cd Cu As Cr Co
218 0.71 9.6 270 70 370 –
bLOD-70 bLOD-9 bLOD-1 bLOD-515 bLOD-69 bLOD-951 bLOD-26
n.a. 3 n.a. 1 n.a. 1 –
37–199 bLOD-2 bLOD-13 bLOD-287 bLOD-34 bLOD-769 bLOD-36
n.a. 7 6 1 n.a. 1 –
3.4. Environmental risk assessment To assess the quality of sediments, concentration of elements in the sediment was compared to the effects range median (ERM) developed by Long et al. (1995). The ERM value indicates the incidence of adverse effects on benthic species. As can be seen in Table 7, some element concentrations i.e. Hg, Cu and Cr exceeded the ERM. One station exceeded the ERM of Cu and Cr, while 13 and 25 stations exceeded the ERM of Hg in both seasons, respectively. Concentration of Cr at one station was also higher than the ERM. Adverse effects on benthic invertebrate communities are likely at all stations, where the ERM threshold was exceeded. To assess the bioaccumulation of the investigated trace hazardous elements in marine biota, green mussels and several fish species caught from Jakarta Bay were also analysed. The detailed data on the element concentration in the marine biota were enclosed in the supplementary materials (Tables S5 and S6). Accumulation of metals in the animal tissue from Jakarta Bay was similar during both sampling campaigns. Copper exhibited the highest concentration level followed by As, Cr and Pb in both, the first and the second sampling campaign. Hg, Cd and Co concentrations were below the limit of detection. The concentrations of all elements were below the tolerable limit regulated by the National Agency for Food and Drug Control, Indonesia. The agency sets the maximum allowable limit of As and Cd in bivalves and fish at 1 mg kg−1; Hg in fish and bivalves at 0.5 mg kg− 1 and 1 mg kg−1, respectively; Pb in fish and bivalves at 0.3 mg kg−1 and 1.5 mg kg−1, respectively and Cu in fish and fish products at 20 mg kg−1 (DJPOM, 1989). However, the pattern of accumulation in the animal tissue samples was similar to that in sediment and water samples. Concentration of Cu and Cr were high as compared to the other elements, which was in line with the concentrations in sediment and water. This finding is in agreement with the previous study in Jakarta Bay that postulated that most of the molluscs caught from Jakarta Bay have a low heavy metal concentration (Putri et al., 2012; Takarina and Adiwibowo, 2010). However, in polychaetes, concentration of heavy metals such as Cu, Cr, Pb and Zn during 2010 exceeded the threshold (Takarina and Adiwibowo, 2010). This condition might be related to the duration of exposure. The longer the biota live in polluted water, the higher the accumulation of heavy metals. Bivalves that have been analysed in this study were between 4 and 6 months old.
4. Conclusion and suggestion The trace hazardous element contamination in Jakarta Bay differed between the considered metals, and for some elements also differed between pre monsoon and post monsoon. The concentrations of most elements were lower after the wet season and higher at the end of the dry season. The order of element concentrations in tissue samples of economic important bivalve and fish species from Jakarta Bay reflected the element concentrations found in water and sediment samples from the bay. Elements such as Cu, Cr and Hg exceeded the effects range median (ERM) at some stations. At these stations, adverse effects
on benthic communities can be expected. Because the Jakarta Bay is heavily polluted due to the riverine transport of enormous amounts of solid and liquid wastes coming from the megacity Jakarta and its industrial zones, the cities` waste management has to be improved. Although the clean river program has been set up to improve public awareness, this program has not fully succeeded yet. Large parts of the city lack adequate sewage treatment and adequate rubbish collection services. Up to today, huge amounts of untreated or partially treated wastewaters are still discharged into the 13 rivers/canals which flow into Jakarta Bay. Further comprehensive information regarding the pollution of Jakarta Bay is urgently requested as a basis for the development of new environmental regulations and to implement a suitable monitoring system in the bay. Acknowledgments We gratefully acknowledge the assistance of Ms. Sri Iswani during laboratory work at the Research Centre for Marine and Fisheries Product Processing and Biotechnology, Ministry of Marine Affairs and Fisheries, Jakarta. Appendix A. Supplementary data Supplementary data to this article can be found online at http://dx. doi.org/10.1016/j.marpolbul.2016.05.008. References Arifin, Z., Puspitasari, R., Miyazaki, N., 2012. Heavy metals contamination in Indonesian coastal marine ecosystem: a historical perspective. Coast. Mar. Sci. 35 (1), 227–233. BPLDH, 2014. Status Lingkungan Hidup Daerah Provinsi Daerah Khusus Ibukota Jakarta Tahun 2013 (The Environmental Status of the Province DKI Jakarta in 2013). BPLDH Jakarta, Jakarta (Retrieved from http://bpldh.jakarta.go.id). BPS, 2014. Statistik Daerah Provinsi DKI Jakarta (District Statistic of DKI Jakarta Province). Statistic Bureau of DKI Jakarta Province (Retrieved from http://jakarta.bps.go.id). BPS, 2015. Cilincing Dalam Angka 2015 (Cilincing in figures 2015) (31750.1509) BPS Kota Administrasi Jakarta Utara, Jakarta (Retrieved from www.jakutkota.bps.go.id). Censi, P., Spoto, S.E., Saiano, F., Sprovieri, M., Mazzola, S., Nardone, G., ... Ottonello, D., 2006. Heavy metals in coastal water systems. A case study from the northwestern Gulf of Thailand. Chemosphere 64 (7), 1167–1176. http://dx.doi.org/10.1016/j. chemosphere.2005.11.008. Chakraborty, S., Bhattacharya, T., Singh, G., Maity, J.P., 2014. Benthic macroalgae as biological indicators of heavy metal pollution in the marine environments: a biomonitoring approach for pollution assessment. Ecotoxicol. Environ. Saf. 100 (0), 61–68. http://dx. doi.org/10.1016/j.ecoenv.2013.12.003. DJPOM, 1989. Batas Maksimum Logam Dalam Makanan (The Maximum of Metals Residue in Food). (Nomor: 03725/B/Sk/vii/89). DJPOM, Jakarta. Dsikowitzky, L., Ferse, S., Schwarzbauer, J., Vogt, T.S., Irianto, H.E., 2016. Editorial - Impact of megacities on tropical coastal ecosystems - the case of Jakarta, Indonesia. In: Dsikowitzky, L., Schwarzbauer, J. (Eds.), Impacts of megacities on tropical coastal ecosystems – The case of Jakarta, Indonesia. Special Issue, Mar. Pollut. Bull. http:// dx.doi.org/10.1016/j.marpolbul.2015.11.060. Haryati, S., Sanim, B., Riani, E., Ardianto, L.a., Sutrisno, D., 2013. Valuasi ekonomi dampak pencemaran dan analisis kebijakan pengendalian pencemaran di Teluk Jakarta (Valuation Economic of Water Pollution Impacts and Pollution Control Policy in Jakarta Bay. Globe 15 (2), 185–190. Hosono, T., Su, C.-C., Delinom, R., Umezawa, Y., Toyota, T., Kaneko, S., Taniguchi, M., 2011. Decline in heavy metal contamination in marine sediments in Jakarta Bay, Indonesia due to increasing environmental regulations. Estuar. Coast. Shelf Sci. 92 (2), 297–306. http://dx.doi.org/10.1016/j.ecss.2011.01.010.
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T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx Hutagalung, H.P., Setiapermana, D.a., Riyono, S.H., 1997. Metode Analisis Air Laut, Sedimen Dan Biota. LIPI, Jakarta. Idris, A.M., 2008. Combining multivariate analysis and geochemical approaches for assessing heavy metal level in sediments from Sudanese harbors along the Red Sea coast. Microchem. J. 90 (2), 159–163. http://dx.doi.org/10.1016/j.microc.2008.05.004. Long, E., Macdonald, D., Smith, S., Calder, F., 1995. Incidence of adverse biological effects within ranges of chemical concentrations in marine and estuarine sediments. Environ. Manag. 19 (1), 81–97. http://dx.doi.org/10.1007/bf02472006. MacDonald, J.M., 1994. Artificial reef debate: habitat enhancement or waste disposal? Ocean Dev. Int. Law 25 (1), 87–118. MenLH, 2004. KepmenLH No. 51. p. 2004. Murtini, J.T., Rachmawati, N., 2007. Heavy metals content of fish, water and sediment in Saguling Dam, West Java. [research article]. J. Mar. Fish. Postharvest Biotechnol. 2 (2), 153–159. Nakata, H., Shimada, H., Yoshimoto, M., Narumi, R., Akimoto, K., Yamashita, T., ... Takikawa, K., 2008. Concentrations and distribution of mercury and other heavy metals in surface sediments of the Yatsushiro Sea including Minamata Bay, Japan. Bull. Environ. Contam. Toxicol. 80 (1), 78–84. http://dx.doi.org/10.1007/s00128007-9320-6. Priyanto, N., Dwiyitno, Ariyani, F., 2008. Heavy metal residues (Hg, Pb, Cd and Cu) in fish, water and sediment at Cirata Reservoir, West Java. Mar. Fish. Postharvest Biotechnol. 3 (1), 69. Putri, L.S.E., Prasetyo, A.D., Arifin, Z., 2012. Green mussle (Perna viridis L.) as bioindicator of heavy metals pollution at Kamal Estuary, Jakarta Bay, Indonesia. J. Environ. Res. Dev. 6 (3), 390–396. Rochyatun, E., Rozak, A., 2007. Observation on heavy metals of sediments in Jakarta Bay. Makara Sains 11 (1), 28–36.
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Rofiq, I., Takanobu, I., 2011. Mercury pollution in Java Island: past and present. J. Ecotechnology Res. 16 (2), 51–57. Sindern, S., Tremöhlen, M., Dsikowitzky, L., Schwarzbauer, J., Siregar, T.H., Ariyani, F., Irianto, H.E., 2016. Heavy metals in river and coast sediments of the Jakarta Bay region (Indonesia) – geogenic versus anthropogenic sources. Mar. Pollut. Bull. (in this issue). Tajam, J., Kamal, M.L., 2013. Marine environmental risk assessment of Sungai Kilim, Langkawi, Malaysia: heavy metal enrichment factors in sediments as assessment indexes. Int. J. Oceanogr. 2013, 6. http://dx.doi.org/10.1155/2013/482451. Takarina, N.D., Adiwibowo, A., 2010. Content of heavy metals (Cr, Cu, Pb and Zn) in macrozoobenthos at Jakarta Bay. J. Coast. Dev. 14 (1), 75–80. van der Wulp, S., Hesse, K.J., Ladwig, N., Damar, A., 2016. Numerical Simulations of River Discharges, Nutrient Flux and Nutrient Gradients in Jakarta Bay. In: Dsikowitzky, L., Schwarzbauer, J. (Eds.), Impacts of megacities on tropical coastal ecosystems – The case of Jakarta, Indonesia. Mar. Pollut. Bull. (in this issue). Wang, S., Jia, Y., Wang, X., Wang, H., Zhao, Z., Liu, B., 2010. Fractionation of heavy metals in shallow marine sediments from Jinzhou Bay, China. [research support, non-US gov't]. J. Environ. Sci. 22 (1), 23–31. Williams, T.M., Rees, J.G., Setiapermana, D., 1997. Land-derived contaminant influx to Jakarta Bay, Indonesia. Geochemistry of Marine and Sediment, p. 95 (Keyworth, UK). Williams, T.M., Rees, J.G., Setiapermana, D., 2000. Metals and trace organic compounds in sediments and waters of Jakarta Bay and the Pulau Seribu Complex, Indonesia. Mar. Pollut. Bull. 40 (3), 277–285.
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Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia Tuti Hartati Siregar a,⁎, Nandang Priyanto a, Ajeng Kurniasari Putri a, Novalia Rachmawati a, Radestya Triwibowo a, Larissa Dsikowitzky b, Jan Schwarzbauer b a b
Research Centre for Marine and Fisheries Product Processing and Biotechnology, Ministry of Marine and Fisheries, KS Tubun Petamburan VI Slipi, Jakarta, Indonesia Institute of Geology and Geochemistry of Petroleum and Coal, RWTH Aachen University, Lochnerstr. 4-20, 52056 Aachen, Germany
a r t i c l e
i n f o
Article history: Received 30 September 2015 Received in revised form 11 April 2016 Accepted 5 May 2016 Available online xxxx Keywords: Heavy metals Seawater Marine sediment Food safety Jakarta Bay
a b s t r a c t The Jakarta Bay Ecosystem is located in the vicinity of the megacity Jakarta, the capital city of Indonesia. Surrounding rivers and canals, carrying solid and fluid waste from households and several industrial areas, flow into the bay. Therefore, the levels of selected trace hazardous elements in water, surface sediments and animal tissues were determined. Samples were collected from two different seasons. The spatial distribution pattern of trace elements in sediment and water as well as the seasonal variation of the contamination were assessed. Quality assessment of sediment using the effects range median (ERM) showed that the concentrations of Hg, Cu and Cr at some stations exceeded the recommended values. Moreover, the concentrations of several trace hazardous elements in the sediments exceeded previously reported toxicity thresholds for benthic species. © 2016 Elsevier Ltd. All rights reserved.
1. Introduction Trace elements such as Cd, Hg, Cu, Pb and As are known as harmful pollutants in marine environments. These metals enter coastal ecosystems through riverine transport of trace element loads originating from the natural weathering of rocks in the catchment areas or from anthropogenic sources, such as industrial or municipal wastewater discharges. A further source is atmospheric deposition. Trace hazardous elements that have adverse effect on human health including lead (Pb), cadmium (Cd), copper (Cu), zinc (Zn) and nickel (Ni) have been detected in water and sediment from Jakarta Bay during the last 15 years (Arifin et al., 2012; Rochyatun and Rozak, 2007; Williams et al., 2000). Because the Jakarta Bay Ecosystem is located in the vicinity of the megacity Jakarta, and surrounded by industrial zones, trace hazardous elements reach the bay from several sources such as industrial discharges, municipal wastewater discharges, surface run-off and dust precipitation (Arifin et al., 2012; Idris, 2008; Tajam and Kamal, 2013; Williams et al., 2000). In addition, agricultural activities and aquaculture practices have also influenced the pollution in the Jakarta Bay. An example of aquaculture practices in Jakarta Bay is the massive culture of green mussels (Perna viridis) since 1979 (Haryati et al., ⁎ Corresponding author. E-mail address: [email protected] (T.H. Siregar).
2013) where the production reached 1270 tons in 2013 (BPS, 2015). The mussel is the most popular and economically affordable seafood product for the coastal communities in Jakarta, and has also been marketed to the surrounding cities such as Tangerang, Bandung and Cirebon. Therefore, despite the severe pollution in this area, the Jakarta Bay provides economic and social benefit for the local fishermen. Seafood production from Jakarta Bay supplies cheap protein source for consumers in Jakarta and its surrounding. However, the consumption of seafood from this area increases the risk for local communities to be exposed to the trace hazardous elements from Jakarta Bay (Putri et al., 2012). The contamination of Jakarta Bay with trace hazardous elements was reported to be comparable to some other big cities in Indonesia, such as Semarang and Surabaya. The trend of this contamination was reported to decrease during the last 10 years due to more strict regulations (Arifin et al., 2012; BPLDH, 2014; Hosono et al., 2011; Williams et al., 2000). Unfortunately, up to today huge amounts of poorly treated wastewaters are discharged into the 13 canals/rivers which flow into the Jakarta Bay (e.g. Dsikowitzky et al., 2016). An extensive research on the dynamical distribution of hazardous metals such as Hg, Pb, Cd, Cu, Cr, Co and As in Jakarta Bay is so far missing and was therefore conducted within the present study. This research aims to draw a complete picture of the spatial distribution of trace hazardous elements in Jakarta Bay considering also the origin of the
http://dx.doi.org/10.1016/j.marpolbul.2016.05.008 0025-326X/© 2016 Elsevier Ltd. All rights reserved.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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contamination, seasonal variations and possible accumulation of the studied elements by economic important bivalve and fish species in Jakarta Bay. 2. Materials and methods 2.1. Study site Jakarta Bay is located in the North of Jakarta, the capital city of Indonesia (latitude 106°21′ to 107°03′E and longitude 5°10′ to 6°10′S). Jakarta Bay is constrained by two capes, Tanjung Pasir to the West and Tanjung Karawang to the East. There are four major rivers discharging freshwater as well as wastewater from Jakarta and its surroundings settlements into the bay, namely Sungai Cisadane in the most westward and just outside of the bay, Sungai Angke and Sungai Ciliwung in the middle of the bay and Sungai Citarum with the largest river delta at the easternmost cape. The total area of Jakarta Bay is about 514 km2, with a shoreline length of 76 km (BPLDH, 2014). The depth of Jakarta Bay is 18 m on average (BPLDH, 2014; Hosono et al., 2011; Williams et al., 2000). Besides the four major rivers, there are smaller rivers and canals discharging around 1400 m3 solid and liquid waste into the center of the bay (BPLDH, 2014). The industrial areas which are located close to the Jakarta Bay such as Cilincing North Jakarta, Pulogadung - East Jakarta, Bekasi and Bogor may also contribute to the increasing pollution of the Jakarta Bay (at stations R1, R2, R3, R6, R14, R15, see Fig. 1). According to the Statistical Bureau of DKI Jakarta (BPS, 2014) the population of Jakarta City was 10.1 million in 2014, and the total area of Jakarta City was 662.33 km2. 2.2. Sample collection A sampling network of 26 sampling stations in Jakarta Bay and of 16 estuary stations were sampled in April (wet transitional to dry season,
sampling campaign I) and November 2014 (dry transitional to wet season, sampling campaign II) (Fig. 1). Sites were positioned along transects using a Garmin 585 global positioning system (GPS) with a resolution of about 3.5 m. Sample collection was done following the method described by Hutagalung et al. (1997). Surface sediment samples were collected using a Van Veen grab. They were stored in polypropylene tubes and kept on ice until being transported to the laboratory. Water samples were recovered from 1 to 2 m depth below the water surface using a Nansen bottle. The samples were filtered using a 0.45 μm PPDF filter, filled in polypropylene bottles, acidified with 1% HNO3 for preservation and kept on ice until being transported to the laboratory. For mercury analysis, samples were stored in brown glass bottles, preserved with HNO3 and K2Cr2O7 and kept on ice until being transported to the laboratory. Mussel samples were bought from the owners of aquaculture facilities in the Jakarta Bay, while fish samples were purchased from the local fisherman who at the time of sampling caught fish in the bay. Background information about the sampled fish and mussel species are presented in Table 1. In situ measurements such as pH, salinity, temperature and turbidity were also performed. All samples were stored at 4 °C prior to analysis. 2.3. Sample preparation and analysis Before analysis, all laboratory equipment was cleaned with 2% nitric acid pro analysis (Merck, USA). Sample preparation and analysis was performed following the method provided by the instrument manual (Berghoff, Germany for microwave destruction and Agilent 7700X, USA for ICPMS analysis). Sediment samples were dried in an oven at a temperature of 105 °C for 8 h. 100 mg sample aliquots were placed in a digestion vessel. Then 8 ml of HNO3 (65%, suprapur) and 2 ml of HF (40%, pro analysis) were added. After 2 min, the vessel was closed and heated in a microwave oven (Berghof speedwave two, Germany) with the program stated in
Fig. 1. Schematic map of the study area. Water and sediment samples were taken in Jakarta Bay and at the mouths of the rivers/canals which discharge into Jakarta Bay. The sampled rivers/ canals flow through the Greater Jakarta City area. Green dots indicate the aquaculture facilities where green mussel samples (Perna viridis) were taken. The black dots indicate the locations where fish samples were bought from the local fishermen. (For interpretation of the references to color in this figure legend, the reader is referred to the web version of this article.)
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx Table 1 Scientific names, common names, habitat and feeding mode of the investigated mussel and fish species from Jakarta Bay. Common name/ Scientific name Green mussel/Perna viridis Flounder/Isettodes irumei Yellow tail fish/ Caesio erythrogaster White emperor Hairtail/Trichiurus savala Mullet/Valamugil speigteni Squid/Loligo sp Treadfin brean/ Nemipterus nematophorus Ponny fish/Lelognathus equulus Fringescale sardine/ Sardinella fimbriata
Habitat
Feeding mode
April, November 2014 April 2014
Demersal Carnivore
April, November 2014
Demersal Pelagic Pelagic Demersal
April, November 2014 April 2014 April 2014 April, November 2014
Carnivore Carnivore Carnivore Carnivore
Demersal Carnivore
November 2014
Demersal Herbivore
November 2014
Pelagic
November 2014
Carnivore
Table 2. After cooling, 0.5 ml of the sample was diluted with 9.5 ml of HNO3 (1%). Fish tissue (250 g), from 1 to 3 individual fish, depending on their weight, was blended altogether and dried in an oven at 105 °C for 8 h. Subsequently, 150 mg of the dried samples were placed in a digestion vessel. Ten milliliters of HNO3 (65%, suprapur) was added, then the vessel was closed and heated in a microwave (Berghof, Germany) with the program stated in Table 2. After cooling, 1 ml of the sample was diluted with 9 ml HNO3 (1%). The soft mussel tissue from 1 kg sample aliquots (including shells) was prepared according to the same procedure as the fish tissue. One milliliter of water sample was poured into a vessel and 9 ml of HNO3 (65%, suprapur) was added. After the vessel was closed, it was heated in a microwave (Berghof, Germany) with the program stated in Table 2. After cooling, 1 ml of sample was diluted with 9 ml of HNO3 (1%). The total concentrations of the elements Pb, Hg, Cu, Cd, As, Cr and Co in sediment samples, tissue samples and water samples were determined with an ICPMS 7700X (Agilent, USA). Operating conditions of this device are given in Table 3. Trace hazardous element concentrations were determined in surface sediment, water and animal tissue samples by performing two replicated extractions. Mean concentrations of each element are shown in Tables S1–S6 of the supplementary material. ICPMS calibration was performed using standard solutions with defined concentrations. The isotopes used for measurements and calculations were 208Pb, 202Hg, 63Cu, 111Cd, 75As, 52Cr and 59Co. A series of standard solutions (1 ppb, 5 ppb, 10 ppb, 20 ppb, 30 ppb, 40 ppb, 50 ppb and 80 ppb) was measured. A blank solution using 1% of
Table 2 Digestion program for sample preparation. Step
T (C)
P (bar)
Table 3 Operating condition of ICPMS 7700X. Forward rf power Plasma gas flow rate Carrier gas Sampler and skimmer cones Integration time Sampling period No. of replicates Tune mode
Sampling time
Pillar Filter feeder Demersal Omnivore
Time (min)
3
1550 W 15 l/min 1.05 l/min Platinum 0.1 s 0.3 s 3 He
HNO3 was prepared for each set of analysis to check the possibilities of contamination during the digestion procedure. Target element concentrations in procedural blanks were negligible. The accuracy of the analytical procedure was checked using the certified reference material (CRM) PACS-2 (NRC, Canada). Analysis was done according to the method described above for the sediment analyses in four replicates. The recovery rates of the heavy metals in the CRM are listed in Table 4. 3. Results and discussion 3.1. Concentrations and spatial distribution of trace hazardous elements in surface sediments from the Jakarta coastal area The concentration levels of the trace hazardous elements Pb, Hg, Cd, Cu, As, Cr and Co in sediment samples from Jakarta Rivers and Jakarta Bay are shown in Fig. 2. All determined concentrations are given in detail in the Supplementary Material of this article (Tables S1 and S2). A comparison of the values of the trace elements in this study to previous conditions of Jakarta Bay (Williams et al., 2000) shows that the concentrations of several metals (Cr, Cu, Pb) were three to five times higher than in 1996. However, the concentrations of other metals such as As and Co remained equal between 1996 and 2014. Previous studies at two dams of the Citarum River, a river discharging into the easternmost part of Jakarta Bay, i.e. Cirata and Saguling Dam, showed concentrations of less than 10 mg kg−1 of Hg, Cd, Cu and Pb in the year 2005 (Table 5). The average concentrations of trace hazardous elements in Jakarta Bay sediments as determined in this study are similar to those of coastal sediments taken from the vicinity of other big Asian cities (Table 5) (Censi et al., 2006; Chakraborty et al., 2014; Murtini and Rachmawati, 2007; Nakata et al., 2008; Priyanto et al., 2008; Wang et al., 2010). The spatial distribution of the studied trace hazardous elements in surface sediments of Jakarta Bay and Jakarta rivers is also shown in Fig. 2. The element concentrations in the river sediment samples were in the same range or higher than those of the bay sediments (Fig. 2). Higher concentration levels of most considered elements in the river sediments as compared to the bay sediments indicate that the major sources of these elements is riverine transport. The rivers discharge trace hazardous element loads into the bay which may originate from anthropogenic sources or from the natural weathering of volcanic rocks in the river catchments. This was assessed in detail by (Sindern
Power (%)
Digestion program for sediment samples 1 170 30 2 200 30 3 50 25
10 20 10
80 90 0
Digestion program for water samples 1 200 30 2 130 30 3 100 25
20 5 5
70 90 0
Digestion program for tissue samples 1 140 30 2 160 30 3 175 35 4 50 25
5 5 20 10
100 100 100 0
Table 4 Results of the analyses of certified reference material and standard deviation of the obtained results. Element Cr Cu As Cd Co Pb Hg
Certified value PACS-2 (mg kg−1) 90.7 ± 4.6 310 ± 12 26.2 ± 1.5 2.11 ± 0.15 11.5 ± 0.3 183 ± 8 3.04 ± 0.2
Measured value (n = 4) (mg kg−1)
Recovery rate (%)
77 ± 3.3 240 ± 8 31 ± 1.3 2.08 ± 0.15 9.9 ± 0.3 165 ± 3 2.9 ± 0.1
85 77 118 99 86 90 95
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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et al.(2016-in this issue). They showed the importance of geogenic inputs for the composition of As, Cr and in part Cu in river sediments from the Jakarta City area. Furthermore, this study indicates the presence of small-scale local Cr emissions in the northern central part of
Jakarta City. The contamination of Jakarta river sediments with Pb and to a minor extent Cu is controlled by anthropogenic sources, mainly in the central part of Jakarta City. This is in line with Williams et al. (1997, 2000) who found that geogenic sources control the abundance
Fig. 2. Trace hazardous element concentration in surface sediments sampled in April 2014 (left bars) and November 2014 (right bars). All concentrations are given in mg kg−1 dry weight.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
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Fig. 2 (continued).
of Cr (as well as Co) in Jakarta Bay sediments, while Cu and Pb mainly originate from anthropogenic sources (Williams et al., 1997, 2000). The spatial distribution of the elements which are known to have a mainly geogenic source, Co and As (Fig. 2), shows similar concentration
levels at all river/canal stations in the studied area. Only at station R1, a higher As concentration in the sediments was observed. Pb, Cu and Cr concentrations which at least partly originate from anthropogenic sources were highest at the river/canal mouths discharging into the
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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Fig. 2 (continued).
western and eastern part of Jakarta Bay. The rivers in the eastern and western parts of the study area receive the effluents from the major industrial areas in or close to Jakarta City. In Bekasi and Cikarang, in the Southeast of Jakarta, where the biggest industrial areas of Indonesia
are located, the industrial wastewaters are discharged into the Citarum River, Cikarang River and Western Tarum Channel. These rivers/canals discharge into Jakarta Bay at stations R14–R16. Another industrial area is located at the Cisadane River, which discharges into the westernmost
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
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Fig. 2 (continued).
Table 5 Concentrations of trace hazardous elements (mg kg−1) in sediment samples from Jakarta Bay in comparison to other Asian coastal areas. Location
Pb
Hg
Cd
Cu
As
Cr
Co
References
Jakarta Bay, Indonesia Saguling Dam, Indonesia Cirata Dam, Indonesia Other Asian countries Thailand Gulf, Thailand Jinzhou Bay, China Yatsushiro Bay, Japan Minamata Bay, Japan Kranji, Singapore Tekong, Singapore
bLOD-357 0.1–0.2 0.01–0.03
bLOD-9 0.1–0.3 0–1
bLOD-13 0.03–0.2 0.02–1
bLOD-515 1–11 0.5–7
bLOD-69 – –
bLOD-951 – –
bLOD-36 – –
This study Murtini and Rachmawati (2007) Priyanto et al. (2008)
– 41–460 18–56 10–19 24–24 24–37
– – 0.02–3.4 0.4–3.4 – –
– 1.5–64 –
8–364 26–400 3.2–64 3.7–25 15–21 6.3–8.7
– – –
27–1104 – –
17–716 – –
Censi et al. (2006) Wang et al. (2010) Nakata et al. (2008)
– –
– –
– –
Chakraborty et al. (2014)
0.15–0.22 0.05–0.07
eastern Jakarta Bay (Fig. 2). This could be due to re-suspension of surface sediments and transport of suspended particles with the water masses circulating within the Jakarta bay in a counter clockwise pattern (van der Wulp et al., 2016-in this issue).
part of Jakarta Bay (station R1). In Jakarta City, the stations R4 and R5 are influenced by the Ciliwung river system, which brings industrial wastewaters from Bogor. The spatial distributions of all determined trace hazardous elements in Jakarta Bay sediments (Fig. 2) did not show clear seaward concentration gradients as previously reported from an investigation on sediment cores from the bay conducted by Williams et al. (2000). The higher concentrations of the elements Pb, Cu, Cd and Cr at the easternmost and westernmost river stations were not reflected by higher concentrations of the respective elements in the sediments from the western and
3.2. Concentrations and spatial distribution of trace hazardous elements in water samples from the Jakarta coastal area The concentrations of trace hazardous elements in Jakarta Bay water and Jakarta river water were far lower than in the
Table 6 Concentration of trace hazardous elements (μg l−1) in water samples from Jakarta Bay in comparison to data from previous studies in the Greater Jakarta area. Location
Pb
Hg
Cd
Cu
As
Cr
Co
References
Jakarta Bay, Indonesia Jakarta Bay, Indonesia Saguling Dam, Indonesia Cirata Dam, Indonesia Maximum concentration (in μg L−1)
bLOD-492 bLOD-3.62 0.04–4 bLOD-1 50
bLOD-95
bLOD-9 bLOD-0.16 0.9–22 1–20 10
bLOD-805 bLOD-404 2–127 0.1–63 50
bLOD-31
1–9521 bLOD-4.0 – –
bLOD-52
This study Williams et al. (2000) Murtini and Rachmawati (2007) Priyanto et al. (2008) MenLH (2004)
0.05–6 0.1–63 3
– –
– –
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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sediments at the same stations. At some stations, water concentrations were below the limit of detection. The determined concentration ranges of Pb, Hg, Cd, Cu, As, Cr and Co in water samples from the study area are shown in Fig. 3. All values are documented in detail in Tables S3 and S4 of the Supplementary Material of this
article. Table 6 shows a comparison of the trace hazardous element concentration ranges in water determined in this study as compared to previous studies from the working area, where the concentration of Pb, Hg, Cu and Cr in this study were higher while Cd was lower.
Fig. 3. Trace hazardous element concentrations in water samples taken in April 2014 (left bars) and November 2014 (right bars). All concentrations are given in μg l−1.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
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Fig. 3 (continued).
Regarding the spatial distribution of the river contamination with trace hazardous elements, similar concentration levels of Co, As, Cu and Hg at all river/channel stations in the study area can be observed (Fig. 3). This is in line with the spatial distribution of Co, As and Hg in the river sediments (Section 3.1). However, Cu concentrations at the
river sediments were higher in the rivers/canals discharging into the western part of the bay (Fig. 2), but this pattern was not mirrored by the contamination of the aqueous phase. Pb and Cd were only detectable in river water samples from the western part of the study area and Cr concentration was very high at station R1 in the west. This
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
Fig. 3 (continued).
pattern may reflect the industrial inputs in the western part of the study area (Section 3.1), but the results are not as clear as for the sediment samples. Chromium might partly originate from small-scale tanning industries which occur widespread in Jakarta and its surrounding cities.
Chromium is used for several industrial purposes such as chrom plating, leather tanning and wood treatment. According to the Agency for Environmental Control, Jakarta, there are numerous leather tanneries in Jakarta (BPLDH, 2014).
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
T.H. Siregar et al. / Marine Pollution Bulletin xxx (2016) xxx–xxx
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Fig. 3 (continued).
The spatial distribution of trace hazardous elements in water samples from the bay did not show a clear trend in regard to Cu, Cr, Pb, As, Cd and Co (Fig. 3). In contrast, the Hg concentrations in water samples from the western part of the bay were higher than in the central and eastern part of the bay. Noteworthy, the Hg concentrations in the seawater samples were higher than in the river water samples (Fig. 3). Rofiq and Takanobu (2011) assessed the history of mercury pollution in Java Island and observed that the mercury contamination of surface waters mainly originated from land-based sources, such as industrial wastewaters and gold-mining activities (Rofiq and Takanobu, 2011). However, our data from the Jakarta Bay area show higher Hg concentrations in seawater than in river water, thus do not confirm these findings. In addition, the Hg concentrations in Jakarta river sediments and water samples did not show elevated concentrations in the rivers receiving industrial wastewaters (see Section 3.1). The higher Hg concentrations in seawater could be correlated with a mercury input source in the near shore region. Such sources could be the use of Hg contaminated municipal incinerator ash as substitute for sand in artificial reefs (MacDonald, 1994) or waste-dumping from shipping vessels. The concentrations of Hg and Pb at some stations from the first and second sampling campaign exceeded the maximum concentrations of these elements in water as regulated by the Indonesian government (MenLH, 2004). Furthermore, the concentration of Cu at all stations during the second sampling campaign exceeded the maximum level allowed in water. Maximum concentrations of Hg, Cd, Cu, Pb and Zn in marine water established by the Indonesian government are 3, 10, 50, 50 and 100 μg l−1, respectively (MenLH, 2004). 3.3. Seasonal variation of trace hazardous element concentrations in water and sediment samples from the Jakarta coastal area The concentrations of all determined trace hazardous elements were higher in the sediments sampled in November 2014 (second sampling campaign) as compared to the samples taken in April 2014 (first
sampling campaign) (Fig. 2). The first sampling campaign took place after the wet season, marked with several weeks with heavy rainfall. The second sampling in November was conducted at the beginning of the wet season, after several weeks with less rainfall. We conclude that the strongly enhanced run-off in the river catchment areas during the wet season is accompanied by a dilution of the contaminated river sediments which are transported into Jakarta Bay. The order of elements concentration in the Bay for the first sampling campaign was Cd b Hg b Co b Cr b Pb b Cu b As. This order was slightly different in the rivers, which was Cd b Hg b Co b As b Pb b Cu b Cr. The order was changed in the second sampling campaign, which in the bay was Hg b Cd b Co b As b Cu b Cr b Pb. In the river for the second sampling campaign the order was Hg b Cd b As b Co b Cu b Pb b Cr. The behaviour of heavy metals in the Jakarta Bay can be divided into two groups, varies between the two weather conditions and constant regardless of the weather condition. The concentrations of Pb were higher in November while those of As were higher in April. Other elements such as Hg, Cd, Co, Cu and Cr were constant throughout the seasons. This finding is in accordance with the previously reported seasonal effects on concentration of several elements in sediments of the Cirata and Saguling Dam (Murtini & Rachmawati, 2007; Priyanto et al., 2008). Concentration of Cu in Jakarta Bay sediments were the highest among all metals. In November 2014, concentrations of most trace hazardous elements in water were higher than in April 2014 (Fig. 3). Concentration of Cu showed a large contrast at all sampling stations. In the first sampling campaign, its concentration was below the limit of detection. However, in the second sampling campaign the concentration was far above 200 μg l−1. A similar observation was made concerning the concentrations of Cr and Pb. The higher element concentrations in river water in November 2014 can be explained by the dry weather conditions prior to the sampling date and the low river-runoff, leading to the increase of concentrations in the river water.
Please cite this article as: Siregar, T.H., et al., Spatial distribution and seasonal variation of the trace hazardous element contamination in Jakarta Bay, Indonesia, Marine Pollution Bulletin (2016), http://dx.doi.org/10.1016/j.marpolbul.2016.05.008
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Table 7 Comparison of trace hazardous element concentrations in the sediment samples (mg kg−1 dry weight) with sediment quality guidelines (SQGs). SQGs are effect range median (ERM) in mg kg−1 dry weight from Long et al. (1995) for marine and estuarine sediments, the contaminant concentration at or above which adverse effects on benthic species frequently occur. Element
ERM (mg kg−1)
Concentrations April 2014 (mg kg−1)
Number of samples above threshold
Concentrations November 2014 (mg kg−1)
Number of samples above threshold
Pb Hg Cd Cu As Cr Co
218 0.71 9.6 270 70 370 –
bLOD-70 bLOD-9 bLOD-1 bLOD-515 bLOD-69 bLOD-951 bLOD-26
n.a. 3 n.a. 1 n.a. 1 –
37–199 bLOD-2 bLOD-13 bLOD-287 bLOD-34 bLOD-769 bLOD-36
n.a. 7 6 1 n.a. 1 –
3.4. Environmental risk assessment To assess the quality of sediments, concentration of elements in the sediment was compared to the effects range median (ERM) developed by Long et al. (1995). The ERM value indicates the incidence of adverse effects on benthic species. As can be seen in Table 7, some element concentrations i.e. Hg, Cu and Cr exceeded the ERM. One station exceeded the ERM of Cu and Cr, while 13 and 25 stations exceeded the ERM of Hg in both seasons, respectively. Concentration of Cr at one station was also higher than the ERM. Adverse effects on benthic invertebrate communities are likely at all stations, where the ERM threshold was exceeded. To assess the bioaccumulation of the investigated trace hazardous elements in marine biota, green mussels and several fish species caught from Jakarta Bay were also analysed. The detailed data on the element concentration in the marine biota were enclosed in the supplementary materials (Tables S5 and S6). Accumulation of metals in the animal tissue from Jakarta Bay was similar during both sampling campaigns. Copper exhibited the highest concentration level followed by As, Cr and Pb in both, the first and the second sampling campaign. Hg, Cd and Co concentrations were below the limit of detection. The concentrations of all elements were below the tolerable limit regulated by the National Agency for Food and Drug Control, Indonesia. The agency sets the maximum allowable limit of As and Cd in bivalves and fish at 1 mg kg−1; Hg in fish and bivalves at 0.5 mg kg− 1 and 1 mg kg−1, respectively; Pb in fish and bivalves at 0.3 mg kg−1 and 1.5 mg kg−1, respectively and Cu in fish and fish products at 20 mg kg−1 (DJPOM, 1989). However, the pattern of accumulation in the animal tissue samples was similar to that in sediment and water samples. Concentration of Cu and Cr were high as compared to the other elements, which was in line with the concentrations in sediment and water. This finding is in agreement with the previous study in Jakarta Bay that postulated that most of the molluscs caught from Jakarta Bay have a low heavy metal concentration (Putri et al., 2012; Takarina and Adiwibowo, 2010). However, in polychaetes, concentration of heavy metals such as Cu, Cr, Pb and Zn during 2010 exceeded the threshold (Takarina and Adiwibowo, 2010). This condition might be related to the duration of exposure. The longer the biota live in polluted water, the higher the accumulation of heavy metals. Bivalves that have been analysed in this study were between 4 and 6 months old.
4. Conclusion and suggestion The trace hazardous element contamination in Jakarta Bay differed between the considered metals, and for some elements also differed between pre monsoon and post monsoon. The concentrations of most elements were lower after the wet season and higher at the end of the dry season. The order of element concentrations in tissue samples of economic important bivalve and fish species from Jakarta Bay reflected the element concentrations found in water and sediment samples from the bay. Elements such as Cu, Cr and Hg exceeded the effects range median (ERM) at some stations. At these stations, adverse effects
on benthic communities can be expected. Because the Jakarta Bay is heavily polluted due to the riverine transport of enormous amounts of solid and liquid wastes coming from the megacity Jakarta and its industrial zones, the cities` waste management has to be improved. Although the clean river program has been set up to improve public awareness, this program has not fully succeeded yet. Large parts of the city lack adequate sewage treatment and adequate rubbish collection services. Up to today, huge amounts of untreated or partially treated wastewaters are still discharged into the 13 rivers/canals which flow into Jakarta Bay. Further comprehensive information regarding the pollution of Jakarta Bay is urgently requested as a basis for the development of new environmental regulations and to implement a suitable monitoring system in the bay. Acknowledgments We gratefully acknowledge the assistance of Ms. Sri Iswani during laboratory work at the Research Centre for Marine and Fisheries Product Processing and Biotechnology, Ministry of Marine Affairs and Fisheries, Jakarta. Appendix A. Supplementary data Supplementary data to this article can be found online at http://dx. doi.org/10.1016/j.marpolbul.2016.05.008. References Arifin, Z., Puspitasari, R., Miyazaki, N., 2012. Heavy metals contamination in Indonesian coastal marine ecosystem: a historical perspective. Coast. Mar. Sci. 35 (1), 227–233. BPLDH, 2014. Status Lingkungan Hidup Daerah Provinsi Daerah Khusus Ibukota Jakarta Tahun 2013 (The Environmental Status of the Province DKI Jakarta in 2013). BPLDH Jakarta, Jakarta (Retrieved from http://bpldh.jakarta.go.id). BPS, 2014. Statistik Daerah Provinsi DKI Jakarta (District Statistic of DKI Jakarta Province). Statistic Bureau of DKI Jakarta Province (Retrieved from http://jakarta.bps.go.id). BPS, 2015. Cilincing Dalam Angka 2015 (Cilincing in figures 2015) (31750.1509) BPS Kota Administrasi Jakarta Utara, Jakarta (Retrieved from www.jakutkota.bps.go.id). Censi, P., Spoto, S.E., Saiano, F., Sprovieri, M., Mazzola, S., Nardone, G., ... Ottonello, D., 2006. Heavy metals in coastal water systems. A case study from the northwestern Gulf of Thailand. Chemosphere 64 (7), 1167–1176. http://dx.doi.org/10.1016/j. chemosphere.2005.11.008. Chakraborty, S., Bhattacharya, T., Singh, G., Maity, J.P., 2014. Benthic macroalgae as biological indicators of heavy metal pollution in the marine environments: a biomonitoring approach for pollution assessment. Ecotoxicol. Environ. Saf. 100 (0), 61–68. http://dx. doi.org/10.1016/j.ecoenv.2013.12.003. DJPOM, 1989. Batas Maksimum Logam Dalam Makanan (The Maximum of Metals Residue in Food). (Nomor: 03725/B/Sk/vii/89). DJPOM, Jakarta. Dsikowitzky, L., Ferse, S., Schwarzbauer, J., Vogt, T.S., Irianto, H.E., 2016. Editorial - Impact of megacities on tropical coastal ecosystems - the case of Jakarta, Indonesia. In: Dsikowitzky, L., Schwarzbauer, J. (Eds.), Impacts of megacities on tropical coastal ecosystems – The case of Jakarta, Indonesia. Special Issue, Mar. Pollut. Bull. http:// dx.doi.org/10.1016/j.marpolbul.2015.11.060. Haryati, S., Sanim, B., Riani, E., Ardianto, L.a., Sutrisno, D., 2013. Valuasi ekonomi dampak pencemaran dan analisis kebijakan pengendalian pencemaran di Teluk Jakarta (Valuation Economic of Water Pollution Impacts and Pollution Control Policy in Jakarta Bay. Globe 15 (2), 185–190. Hosono, T., Su, C.-C., Delinom, R., Umezawa, Y., Toyota, T., Kaneko, S., Taniguchi, M., 2011. Decline in heavy metal contamination in marine sediments in Jakarta Bay, Indonesia due to increasing environmental regulations. Estuar. Coast. Shelf Sci. 92 (2), 297–306. http://dx.doi.org/10.1016/j.ecss.2011.01.010.
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