‘Applied Radiacon and tsatpes 87 (2008) 650-855, Contents lists available at ScienceDirect Applied Radiation and Isotopes journal homepage: www.elsevier.com/locate/apradiso ELSEVIER Distribution of naturally occurring radionuclides activity concentration in East Malaysian marine sediment MW. Yii*, A. Zaharudin, 1. Abdul-Kadir Malaysian Mca Agency (Nuclear Malas ang 43000 Kon. Malaysia feet Accented 30 Noverder 2008 Studies of naturally curring radioactive materials (NORM) distribution of *Ra,2°Ra and °K in Fast Malaysia were carved ut as pat of a marine coastal environmenk projec. The results of measurements will serve as baseline data and background reference level for Malaysia coastlines. Sediments fom 21 ‘coastal locations and 10 nearshore locations were collected for analyses, The samples were dried finely ‘round, sealed in a container and stored for 4 minimum of 20 days to establish secular equilibrium between “Ra and "Ra and their espective radioactive progenies. They were counted using a high- purity germaniurs (HPGe) spectrometer covering the respective progeny energy peak. For “K. the Presence of this wae measured directly va its MGDkeV energy peak. The concentration of "Ra. "Ra snd Kin samples obtained from coastal Sarawak ranged between 23 and 41 (mean 30+2)Bajkg. 27 fand 45 (mean 39:+4)qjkz and. 142 and 680 {mean 452 +58) Blk. respectively. Meanwhile, the Concentration of ##Ra, “Ka and “K for samples obzained from coastal Saba ranged between 16 30 {mean 23.£2)Ba/kg, 25 and 45 (mean 35::4)Bq/kz and 402 and 842 (mean 5773.75)Balk, respectively. For the Sarawak near shore stations, the concentration of "Re, ¥Ra and “K ranged becween II and 36 (meen 224:2)Bajkg, 21 and 65 (mean 38:5)3qjke and 149 and 517 (mean 308 +41) Balk. respectively. Meanwhile. the concentration of **Ra, Ra and “* for samples obtained {som Sabah ranged between 9 and 31 (mean 142) Baik, 10 and 46 (mean 21-3) Bag and 180 and 580 (mean 269 +36) Balke respectively The clclaed external hazatd values of between O17 and 033 (less than unity) showed that there is litle sk of external hazard to the workers handling the Keywords: Marine sediment sediments 1. Introduction Radioactivity monitoring in the marine environment is normally based on analyses of specific nuclides in seawater, suspended particulate matters and sediments, The naturally existing radio- nuclides in the uranium-238 sevies and thorium-222 series and ppotassium-40 are present everywhere inthe Earth's crust. Radium- 225 (#*Ra, uranium series progeny), radium-228 (#*Ra, thorium Series progeny) and potassium-40 (*K) are of most concern due to theirs high solubility and mobility, The knowledge of the concentrations and distributions of these radionuclides are of interest since it provides useful information in the monitoring of environmental contamination by natural radioactivity. Koide etal. (1973) specified that the activity concentration of ‘the progenies from the natural decay series in the marine environment may not necessarily be in equilibrium with their parents. TWo main sources of matine radioactivity result ftom the TT earspondng author: Te: 6038825 010: fox 6058928297 969-s043/5-se ont matter © 2009 Fsevie Ln. Al rights reserved, 44102016) apradse.200811019, 4 2008 Elsevier Ld, Al rights reserved, ‘weathering and, mineral recycling of the terrestrial rocks ‘Thorium-232 Th), uranium-235 5) and uranium-238 (2*U) are three major radionuclide precursors in the decay series, Which produce other radionuclides such as radium, radon, actinium, protactinium, lead and polonium. These progenies frst appear atthe lithosphere level and enter the marine environment through several pathways such as erosion, river transport, fallout, rainwater and others (Stralberg etal. 2003). In coastal areas and on the continental shelf, tis reasonable to assume that the sediments have a range of concentration of natural radionuclides similar to that of terrestrial rocks and the radioactive equilibrium is maintained. The distributions of terrestrial activity concentrations for "Ra, *Ra and *K for areas of Peninsular Malaysia have been widely reported elsewhere (UNSCEAR, 2000; Malaysian Nuclear Agency, 2006; Omar et al, 1990; Redzuwan et al, 1997; Muhamad-Samuci et al, 2005). However, in Malaysia no such study has been reported for natural ‘media from the marine environment and for present interest the authors are not aware of any published data for the East Malaysia region (ie. for Sarawak and Sabah). Hence. the objective of this study is to determine the activity concentration levels of “Ra,MW Vie Applied Radiation and rep 6 (2008) 30-035 on 226Ra and “°K in the marine sediments surrounding East Malaysia and to establish these levels for use as baseline data 2, Experimental 21. Sampling preparation and measurement A total of 21 coastal (<15Nmi) and 10 near shore (10-120 'Nmi) stations as shown in Fig, 1, were identified as the study sites Stations were selected based on water depth, availability of sediment ang to cover the entire coastlines of the country (East Malaysia). For each coastal station, it was further divided into three sub-stations with an interval of about 1Nmi from each other, All the coastal stations were selected whereby they are located close to the river estuary in order to check the input ofthe natural radioactivity ftom terrestrial sources at the same time. However, during actual sampling, no sediment could be collected at a coastal sub-station, SR 14 B ‘The coastal sediments were collected using a PONAK grab sampler, Near shore sediments were collected using gravity box corer and sliced into 2em sections before analysis. Basically, all the coastal samples appeared to be fine mud. However, some of, the cores showed thorough vertical mixing of fine and sandy mud. ‘Two to three replicated sannples were collected from each station, Each replicated sample was dred, finely ground and mixed before a portion was put into a 350ml plastic container and weighed. ‘These containers were sealed wich thick PVC tape and stored fora Period in excess of 30 days to establish secular equilibrium between Ra and "Ra and their respective radioactive progenies. All samples were counted for at least 50,000s using high- purity germanium (HPGe) spectrometer and corrected to the date of sampling. The 2*Ra and "Ra were measuted through the photo peaks of their progenies; “Pb (295 22 and 351.93 keV) and Epi (60931 keV) for 2°Ra and 2Ac (91120keV) for “Ra, Meanwhile, “°K content was measured directly via its 1460keV energy peak. 22. Counting system ‘The HPGe gamma spectrometry was calibrated as reported earlier by Yi et al. (2007), whilst the radioactivity concentrations in the environmental samples were calculated xising equation 33 reported by Yang et al. (2005), The minimum detectable activity SOUTH CHINA SEA son eH MALAYSIA. sae” sce sug "~~" BORNEO (INDONESIA) yee ue ae ene Fig 1. Map shewing sampling lectins (ntpa) for both Ra and **Ra was quantified at 5 Ba/kg per dry weighs, whilst K was quantified at 10 Bajkg,after considering the size and the counting time of the sample. 3, Results and discussion ‘The concentration of Ra, Ra and “°K in the marine sediment at the coastal and near shore stations of Sarawak and Sabah are shown in Figs. 2-5 and summarized in Table 1, The activity concentrations of all samples were found to be greater than the MDA. Surrounding physical conditions at sampling locations are summarized in Tables 2 and 3, The activity concentrations of radionuclides in most of the cores are quite ‘uniform suggesting that there is thorough vertical mixing of sediment throughout the core, The mean values of 2"Ra and 22*Ra are much lower than the Peninsular Malaysian normal soils of 74 Bq/kg "Ra and 98 Balkg 2hRa as reported by Omar etal. (1980). Also, the Ra in Sarawak and Sabah are lower than normal soil in Malaysia, at 38-94 (mean 657) Bqjkg. as reported in the UNSCEAR (2000) as well as by Muhamad-Samudi et al, (2006), which reported 7#°Ra found in Dengkil soil ranged from 20.07 to 976.65 Ba/kg. Furthermore, the level of #*Ra in East Malaysia was also much lower compared to the coastal marine sediment found in the East Coast of Peninsular Malaysia, ranging between 45,23 and 121.49 Ba/kg (Zal U'yun et al, 2005), However, the mean values of ?#*Ra and *#*Ra in this study are comparable to the Sarawak and Sabah normal soils of, 2SBafkg ?*Ra and 32 Bajkg ”*Ra and 18 Bajkg ”*Ra and 24Bqj kg Ra, respectively (Malaysian Nuclear Agency, 2007) This can be explained by the geological formation of Peninsular Malaysia and East Malaysia. Peninsular Malaysia is-mainly covered by the western belt that contains high-rich thorium and luranium granite rocks, while East Malaysia such as Sarawak is underlain by younger tertiary sedimentary rocks especially the region northeast of the Batang Lupar River. Sabah is more Sarawak Coastal [azz] 2 a0 Imz20ee] G5 sox 43 $£ 400 $8 200 goo 'SR'SR'SR'SR SR/SRSR SR'SR'SR'SR 06 07 08 09 10 11 12 13 14 15 16 ‘Station ‘Sabah Coastal ez2aFa| z22Ro| E1000 sox 3 _ oo EB soo BE a0 5 200 g ‘88/88 S68 SB S68 S6 SSB SB SB 06 07 08 09 10 11 12 13 14 15 Station ig. 3. Fa, Ha and Kacy tthe coastal statins of Sabahsno1 sro2 ‘Specific Activity (Bq/kg) ‘Specific Activity (Bq/kg) om 0 oe om 8 ° 0 Ta hake 10 |—*— 220Ra) 10 |—2— 228Ra oA = 2 ow Mon i i = 0 = 8 40 2 40 % 0 Fo ra sro snot ‘Specific Activity (Bq/kg) ‘Specific Activity (Ba/kg) om a aD om 0” ° ° ae 728 1 nara] 10 + 22ers Wo oA =” ~* g g = 3 rao é i 5 40 8 0 50 so 60 bad sros ‘Profi in Core Sediment, specne seety (8a) spect Act (Ba) oe oy oa a0 0 oF Tara] © saan] 30} Moa 7” =” g mn 50 gt 3 an 8 0 2 aot 50 soy 6 00 snare ane a | geologically complex as it consists large bodies of granite ‘granodiorte, tonalite, ulramafic and mafic rocks intrusion into the metamorphic rocks as well asthe deposition of sandstone and rmudstone with minor amounts of limestone and coal in a chain of circular to sub-circular shallow basins (MyMalaysia, 2008), The radionuclides are believed to migrate from terrestrial sources into water through weathering (Ahmad-Taufek et al, 2004) and human activities, then to the river and finally ending in the estuary and sea, On the other hand, the values of K in East Malaysia, generally, are comparable to the values found in the Peninsular Malaysian ‘normal soil that ranged between 170 and 430 (mean 310) Ba/ks. (UNSCEAR, 2000), Muhamad-Samd etal. (2006) also reported the level of #°K in Dengkil soil ranged between 18174 and 4452.42 Balk, However, the “K found inthe Sabah coastal is much ‘more higher than others. This could be attributed to the usage of potassium fertilizers in plantations. Ths large increase in the use of potassium fertilizers is due to the continued expansion ofMW Ye Applied Radiation and eps 6 (2008) 30-035 on seo sBoz specie Actwty (Sat) Specie Acty (29s) eee on ae an 0 of ° Z| 78a » |+—220%—] 10 —+—22are wor gX = Moa g g 20 E00 2 40 2 40 0 0 0 6 soos saot Specie Actity (Bak Specie Actily (2d) om 0 8 6 om ° ° Taha ia 0 -—2zake| 10 — MOA oA 7” -7 5 g _% = 0 2 40 2 40 so v0 0 0 3805 « 1 Profle in Core Sediment ‘Specific Activity (Ba/kg) ‘Specific Activity (Bq/kg) oF a 0 0 0 200 400 «600 800 226Ra ‘ 0 22070} 4 0 OA : eR 5 g a” Zz 0 0 B so so oo 60 [es eee oe Fig 5. Ra, Ra ane acy a he ea shor statons af Saba oil-palm cultivation, which requires significant amounts of this rhuttient (FAO, 2008). This is possible because due to the geographical landscape of Sabah, most of the plantation areas are closer to the sea when compared to Sarawak Therefore, the run-off of °k from the fertilizers can easily been injected into the Higher concentrations of radionuclides in some coastal loca tions may also be attributed to geological areas consisting of granites and. gneisses which contain higher concentration of ‘uranium series, thorium series and potassium. This assumption was supported by Rami et al. (2000), who also reported that higher concentration of uranium, thorium and potassium in sol in Johor were found in areas which are covered by granites and ‘metamorphic rocks, “The phenomenon of changing in radionuclides distribution is believed to be caused by several factors such as chemical and physical properties, precipitation, movement and transportation of the radionuclides. This statement is supported by the IAEA's report (1990) saying that the inconsistency in the radium istriution ate caused by the Te-suspension, transportation and re-sedimentation of sediments when moving from higher ground ‘or during flooding. In addition, the distributions of radium are alsoaffected by two other main processes, that the sedimentation of the suspended solid and re-suspension of the bottom sea sediments, in which both processes depend on the conditions such as current flow and choppiness of the river or sea Azevedo et al, 1984). Overall. the levels of Ra, #*Ra and “°K in sediments found in this study were quite close and comparable to the activity of the table MUM 4 Ape oso an ope 6 (2008) 630-025 “U. 2Th and “°K reported by Nguyen and Nguyen (2003) in Vietnam marine environment that ranged at 2788-5480, 30.86-59,61 and 477.4-1254 Balke, respectively, Our finding also comparable to the activity of the “?°Ra (32.5Bq/kg) and “°K (625 Bajkg) as reported by Yu eta. (1994) in South China Sea near Hong Kong. Therefore, zhese values can be used as the reference and baseline data for East Malaysia. Sediment in the marine environment mainly comes from the neatby terrestrial mainland. Therefore, calculation of the external hhazard index (Hz.) enables the estimation of the hazard from natural gamma-radiation on the mainland as well a the hazard to the workers who handled the sediments. The calculation was SED AS a = performed using the equation as reported by Yang et al. (2005). = a ‘The calculated external hazards valves (Table 1) ate found to be between 017 and 033 and ess than unity, This shows that there is coal litte rise of external hazard to the workers who handled the Soe Boll 2022 HAS 3924 1-680 462459 033 sediments and there i high possiblity that the natural amma pa Ne ae cand radiation on East Malaysia mainland is also low, This assumption was supported by the Malaysian Nuclear Agency's report (2007), Nex ore hae eos waasir sone) o2y thatthe mean concentration of "Ra and Ra in Sarawak and see a 355 MEST, Wet O27 Sabah novmal soils are 25 and 52Bqikz and 18 and 24Balke respectively rabie2 $end rk conden Sank satin actions Semping taton—~—“Samping exe ——«Sao Icaon Dehim)——Tempenwrec) Sait pe Tarde Tosetade ie rem 0a: 4270% tio 61308 165 230 256 ston pene foe cogs Ho-snaoe tas ae 2318 sto S008 tos: 33308 mn ae308 a 2s 3535 Seo Sh for staow ta S30 as ose sat Sees ‘saya toe: sion Mimace ais 3555 Stes Sy-2004 tor 4535% ho-aart ns Bn 3335 ster 2-04 oor s805% ho Save us 238 338 Stee e004 ton. 29968 tieesare bs ian der ston 2ehu-aooe toa: se Inject BS sont >i tio Bhatt tos: one ie jeave be 2095 aa sa Brean toa: tae In sa35e i 308 ae ie Phir 2004 03: Inez Bs mon 238 3 2-004 03: i338 us 3oer 2236 tis 2-004 toe In So34e ns zoos Doe as Soltvaoot lraase Ms wr bas ss ‘Sane 03: ho e190 35 Es 3a Smping ation ——“Samping dae —~Salo cation Se tT lane loneinee a S008 Wom come —smOoE ~*~ ie a8 soo Baton foc-So7N Hissar 2h ae So Zorktv2004 tor. nase assre 08 aa sar Soa Frjy-00¢ tos: 301m heme Sis aa ass shes Ita fos aan Te atavE 33 Br 3305 Shes Ie 2004 foe ecarn furan i fen an Sor Tuveaooe tosces0n aE is Joos 3as0 son a0 tos: 32908 hs 4530 43 woot 298 Stoo Sjasaooe fs: 5512 he-ovse is doo a0 So teyuinz004 fos as40n 2a 5 oi 278 sn Tetras tos: S820 hs Sua “3 283 xr Sei ‘h2008 : 44008 us wore 1455 an 1bjuyaooe tos. ‘sore is ieee 33 so 1 jupaooe tos sare 4s Bn an se tees oes: 50am 33 330 anMLW Wie Apple Rito and rape 6 (2008) 630-025 ws 4, Conclusion NORM concentrations in the marine sediments have been ‘measured in 21 coastal and 10 near shore stations (o cover the entire coastlines of East Malaysia. The concentration of #*Ra, 2¥Ra and °K in samples obtained from coastal Sarawak ranged between 23 and 41 (mean 30++2)fiqjkg, 27 and 45 (mean 39:44)Bqjkg and 142 and 680 (mean 46259) Bq/kg. respec- tively. Meanwhile, the concentration of #*Ra, *Ra and °K for samples obtained from coastal Sabah ranged between 16 and 30 (mean 23 42)Ba/kg, 23 and 45 (mean 3544)Bq/kg and 402. and 842 (mean 577+75)Bqikg, respectively. For the Sarawak near shore stations, the concentration of **Ra, **Ra and “°K ranged between 11 and 36 (mean 22:2)Bq/kg, 21 and 65 (mean 394,5)Bq/kg and 149 and S17 (mean 3094-41) Bajg. respectively Meanwhile, the concentration of *Ra, "Ra and “*K for samples obtained from Sabah ranged between 9 and 31 (mean 14:+2}Bqj kg, 10 and 48 (mean 214:3)Bqjkg and 140 and 580 (mean 269 4-36) Bq/kg, respectively. The activities of radionuclides in most ofthe cores were quite uniform suggesting that there were thorough vertical mixing of sediment throughout the core. Generally, concentrations of NORM in East Malaysian marine sediments are lower than that in the Peninsular Malaysia due to the difference in geological formation, Data reported in this paper is in agreement with those reported by other countries in the region and can be used as the reference level for Malaysia. The calculated external hazard values are between 0.17 and 0.33, (less than unity) showing litte risk of external hazard to workers handling the sediments and there is high probability that the natural gamma-radiation in East Malaysia mainland is also low. Acknowledgements ‘his research was funded by the Atomic Energy Licensing Board, Malaysia. The authors would like to thank the laboratory assistants and staffs of the Waste and Environmental Technology Division (Nuclear Malaysia) and Fishery Department of Malaysia for their help during the sampling and analysis of samples. 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