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Distribution of
137Cs Radionuclide in Industrial Wastes Effluent of Gresik, East Java, Indonesia
Muslim1, H. Suseno2 and F. Rafsani1
1Department of Marine Science, Diponegoro University Semarang, 50275 – Indonesia
2Radioactive Waste Technology Center – National Nuclear EnergyAgency, Kawasan Puspiptek Serpong Tangerang– Indonesia
A R T I C L E I N F O A B S T R A C T AIJ use only:
Received date:
Revised date Accepted date Keywords:
137Cs
industrial wastes distribution Gresik
The distribution of anthropogenic radionuclides 137Cs was measured from industrial waste effluent of Gresik to Gresik Sea in east Java, Indonesia. The activity of 37Csdetected at all stationswas much lower than in northeast Japan both before and after NPPFukushima accident.This indicated that in Gresik industrials waste did not consist of 137Cs. The lowest activity 137Cs occurred at the station nearest to the industrial waste effluent that contained some particle ions that were able to scavenge137Cs and then precipate this radionuclide.
Furthermore,the greatest 137Cs occured at the station that has high current speedsthatstirred up sediment to release 137Csin seawater as a secondary source.
The lowest salinity did not effect on the activity of 137Cs even though the lowest salinity and activity 137Cs occured at the same station.
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1. Introduction
Indonesia is one of the countries in the world that does not use nuclear energy, but some artificial radionucline have been detected in some locations both in the sea water, sediment and marine organisms in Indonesian waters[1]. Transport of artificial radionuclides to Indonesiafrom the resourcesradionuclides can cause surface infusion of these isotopesinto the sea, including atmospheric transport and subsequently transported to off-shore and deeper regions [2]bycurrent and horizontal mixing [3, 4, 5], or by wind-driven circulation of the surface waters [6] and global currents such as Mindanao Current, The Great Ocean Conveyor Belt and Indonesian Through Floware the important currents that transport huge amounts of seawater from the Pacific Ocean to the IndianOcean [7].
137Cs is a soluble element in seawater sourced from anthropogenic activities [8],and has been recognised as nuclear global fallout since the first nuclear weapons were denonated in New Mexico and Japan in 1945. This radionuclide is transported globally with water masses in the oceans [9, 10] that is then
advected and diffused to the worlds ocean [11].
Chernobyl and Fukushima accidents in 26 April 1986 and 11 March 2011, respectively also have produced some artificial radionuclides globally. Therefore serious attention must be given to this worldwide pollution problem as these radionuclides can be concentrated in surface soils and sediments[12]; thus, many countries need to seriously investigate the activity and distributionof 137Cs in the sea as this radionuclide has a long half life (30.2yrs) and can accumulate in soil, plant and marine organisms [13, 14, 15].
Gresik is one of cities in East Java province of Indonesia located in north Java island and connected to the Java Sea in the north part.
Many kinds of industries have produced many products such as palm oil, industrial chemicals (e.g. oxygen, nitrogen, argon, acetylene), phosphate fertilizer, detergents, ceramic, tiles, paper, wood processing, rubber, electrics, steel, cement, asbestos, fish processing, glass, shoes, paint, pestiside, textiles, wood furniture etc. All of the industrial wastes flow through to the river that flows to the Java Sea. Martien et al., [16]
and Morita et al., [17] found that 137Cs will accumulate in soil, plants and marine organisms
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and are affected by competing ions such as potassium, calcium, ammonium and other inorganic minerals such asother monovalent cations [18] . In order to understand the sources and present levels of 137Cs in the coastal waters of Gresik, the hydrology factors that will affect their distribution processes in the water column such as currents, salinity and pH were determined in seawater.
The objective of this study is to determine the distribution of 137Cs in Gresik waters, Indonesia (part of the Java Sea)and whether this distribution is affected by pollution in the area that can be correlated with hydrological factors.
2. Materials and methods 2.1. Sampling
In September 21, 2013 collection of sea water samples was carried out. The surface sea water samples were collected using 10 L plastic bucket and then collected into a big polyethylene containers(80 L) onboard ship.
Containers were rinsed at least twice with seawater collected from the location before the final samples were taken. The total volume of sea water samples at each station was 60 L.
Sampling site stations located in the northern region of the Gresik area; shown in Fig. 1, and the coordinates and total depth of the sampling stations are presented in Table 1. The cruises were part of the impact of the Fukushima radioactive releases in the Asia-Pacific Regionmonitoring program in Indonesia as a part of IAEA program. Seawater samples were taken from surface seawater and along the water profile with simultaneous current, salinity, pH and temperature profiling.
Fig. 1. Map of the sampling sites.
Table 1. Station site information
Station Coordinate Depth
Longitude Latitude (Cm)
1 112°37.792’ 07°06.473’ 80
2 112°37.725’ 07°06.190’ 68
3 112°37.534’ 07°05.930’ 341
4 112°37.874’ 07°05.868’ 127
5 112°38.038’ 07°05.76’ 143
6 112°38.289’ 07°05.984’ 123
2.2. Analysis
The activity of 137Csin sea water was
determined by usingammonium
molybdophosphate (AMP) methods”according to IAEA procedure.This method has been successfully applied to the analysis of 137Cs in small volumes of seawater [19,20]. Cesium was precipitated as a chloroplatinate, the overall chemical yield was determined gravimetrically and the samples counted on a low-background beta counter.
Before sea water was precpitated by AMP, 60L of sea water was acidified with 4M HCl (to pH about 1). 20mg of Cs carrier was added and then the sample stirred for 1-2 hours by bubbling air or N2 gas. We then mixed 13g AMP with seawater to make aslurry and stirred the solution for at least 30 mins to absorb Cs onto the AMP. The AMP settled in the container overnight. The supernatant was siphoned off and discarded.The AMP was collected in a smaller beaker and allowed to settle. This solution was centrifuged for 10 mins and the supernatant discarded. The AMP was then dissolved in 10N NaOH and centrifuged to remove undissolved solids.We then boiled solution to eliminate ammonia,checked vapour with wet pH paper until NH3 emission ceased;diluted sample with 500 mL distilled water and brought the pH to 1.5–2 when the solution turned yellow. The 137Csactivity was determined by its photon/gamma emission at 661keV energy and also the 134Cs emissions at 605 and 796keV. The detector was calibrated by counting a standard solution of 137Cs, using the same counting geometry.
3. Result and discussion
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3.1. 137Cs activity
The 137Cs activity in Gresik seawaterswas detected and persistent even though the Gresik site is very far-off from the source of the Fukushimaincident.This radionuclide activity could also reflect past nuclear bomb testfallout andthe nuclear power plan accident of Chernobylbecause 137Cs is a long-lived radionuclide (T1/2 30.2 y.).
The level of activity of 137Cs fluctuated at each station sampled witha range of activity from 0.078 to 0.319 mBq/L (Table 2) that is much lower compared with activity in northeast Japan both before and after the NPP Fukushima accident in April-December 2009 and May 2012, respectively. Concentrations reported have been 2-3 mBq/L and 2.5-4 mBq/L, respectively [2]. These results indicated that the137Cs was not present in the waste industrials effluent of Gresik. The lowest activity occured at station 3 that had the deepest depth. It low activity may due to the soil particles (suspended sediments)at station 3 that contained some ions such as potassium, calcium, ammonium and other inorganic ionsthat scavenged137Cs and precipated the radionuclide to the bottom sediments, thus the concentration of 137Cs in sediment that have received deposition of radionuclides will increase [21]. However, Aoyama et al., [19], Evangeliou et al., [22] and Nakanishi et al [23] found that the activity of
137Cs in deep water and coastal water in Japan decreased with depth or was concentrated in surface sediments. The activity of 137Cs in the surface seawater wasmuch higher than in the sub-surface layers.
Table 2. Water quality, current speed and 137Cs activity at Gresik.
The highest activity 137Cs radionuclide occured at station 5 (0.319 mBq/L) caused by the resuspension of bottom sedimentscaused by high curren speeds (0.191m/s) that produce elevated 137Cs activity from these sediment as a secoundary source.
Dissoloved oxygen, temperature, pH and salinity did not show any effect on the distribution of 137Cs even though the lowest salinity (27‰) and the lowest 137Cs activity (0.078 mBq/L) occured at station 3. In this case, the lowest 137Cs activity was not caused by salinity, but it was most likely caused by proximityto the estuary and was nearest stationtothe industrial waste effluent of Gresik that contained ions can could scavenge 137Cs.
Zalewska and Lipska [24] found that the decreasing of activity 137Cs occured at stations closest to river-estuaries and in low salinity water, because the 137Cs was diluted by fresh water, and because the behavior of the radionuclide in the water column is affected by physical processes such as advection, mixing and diffusion [25].
4. Conclusion
The activity of 137Cs in Gresik seawater was detected even though the concentrasion was very low when compared with activities in the Japan Sea, both before and after NPP Fukushima accident. The results indicate that the source of 137Cs in Gresik did not come from industrial wastes effluent, but could originate from global fallout. Industrial waste particles could accumulate 137Cs from the seawater and precipate in bottom sediment, thus explaining why the activity of disolved 137Csat thislocation was low. 137Cs in sediment could be released to seawater when current speedsare high and thus become a secondary source of 137Cs.
Acknowledgements
We would to thank Esa Fajar dan Patar Widyantofor their help in seawater collections.
We also wish to thank members of Radioactive Waste Technology Center – National Nuclear Energy Agency for facilitating the data analysis.
References
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Stati on
Dep th Curre
nt speed
m/s
DO Te
mp p
H Salin
ity (‰)
Activi ty
Cm mg
/L °C (mBq/
L)
1 80
0.006 5.9 31.
4 7.
93 29
0.241
2 68 0.031 3.3
29.
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3 341 0.134 4.8
30.
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54 27 0.078
4 127 0.105 5.9
29.
5 7.
54 30 0.126
5 143 0.191 4.8
30.
3 7.
49 31 0.319
6 123 0.102 4.7
30.
9 7.
53 30 0.248
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