 Journal of Environmental Protection, 2011, 2, 418-423 doi: 10.4236/jep.2011.24047 Published Online June 2011 (http://www.SciRP.org/journal/jep) Copyright © 2011 SciRes. JEP Natural Radionuclide Concentrations and Radiological Impact Assessment of River Sediments of the Coastal Areas of Nigeria Olatunde Michael Oni1, Idowu Peter Farai2, Ayodeji Oladiran Awodugba1 1Department of Pure and Applied Physics, Ladoke Akintola University of Technology, Ogbomoso, Nigeria; 2Department of Physics, University of Ibadan, Ibadan, Nigeria. Email: omoni@lautech.edu.ng, olatundeoni@yahoo.com Received November 13th, 2010; revised February 8th, 2011; accepted March 16th, 2011. ABSTRACT This work was carried out to measure the radioactivity level in the coastal areas of Nigeria by gamma counting of river sediment samples and assess the radiological impact associated with the use of the river sediments as building material. The method of gamma spectrometry with a 7.6 cm by 7.6 cm NaI (Tl) detector was employed in determining 40K, 238U and 232Th levels in 95 and 38 sediment samples respectively collected from representative sites in the oil producing and non oil producing coastal areas of Nigeria. Results of the samples assayed showed that the radioactivity concentrations of 40K, 226Ra and 228Ra in the sediment samples of oil producing areas range from 95.4 to 160.0; 7.6 to 31.0 and 9.5 to 41.6 Bqkg–1, respectively. The respective means were calculated as 122.39 ± 47.49; 18.93 ± 12.53 and 29.31 ± 18.67 Bqkg–1. In the sediment samples from the non oil producing areas, the respective mean values are 88.48 ± 8.22, 14.87 ± 3.51 and (16.37 ± 3.87) Bqkg–1. Statistical analysis of the results showed that there is no significant difference be- tween the radionuclide concentration of the sediment samples from different rivers in the oil producing and non oil producing coastal areas, except for 40K. The values of the natural radionuclide concentrations however translate to the determination of the radiological impact assessment values. The values of the radiological assessment indices obtained were observed to be lower than limits internationally reported and recommended for building materials. It could there- fore be reported that the operations of the oil companies in the coastline, involving use of radioactive materials have not contributed adversely to the radioactivity level of the river sediments and that the use of river sediments as building material in the coastal areas of Nigeria poses no radiological risk. Keywords: Radiological Risk Indices, River Sediments In Coastal Area, Gamma Spectrometery 1. Introduction Ionising radiations in any environment is traceable to either natural or artificial sources. The artificial sources are largely due to medical and industrial activities. In the coastal areas of Nigeria, the dominating industry is the oil production and exploration. Apart from medical ex- posure, the petroleum industry is the largest importer and consumer of radioactive materials. The uses of radioac- tive sources in the industry cover both upstream and downstream operations such as well-logging, automated ionizing radiation gauge, radiography and application of radiotracers in oil well management, reservoir studies and leak detection in pipelines. Despite conscious efforts and measures to ensure safety, there is a possibility, based on accident, mishandling of equipment, improper discharge, loss and theft, that ra- dioactive materials of natural and artificial sources may pollute the terrestrial and the aquatic environment of the coastal areas which are mainly networks of rivers and creeks. Following different pathways such as erosion run-off and rainfall, large amount of these radioactive materials end up in the aquatic environment. Due to gravitational settling and other depositional phenomena, the highest proportion of the radioactive materials is mainly found in the sed iment compartment of the aqu atic ecosystem. The exposure of man to gamma radiation from these radionuclides in the aqu atic environment is not limited to the internal exposure due to ingestion through the con- sumption of contaminated aquatic foods. The use of river sediments as a constituent of building materials for floor-
 Natural Radionuclide Concentrations and Radiological Impact Assessment of River Sediments 419 of the Coastal Areas of Nigeria ing, plastering and in moulding bricks in the coastal areas of Nigeria has the probability of increasing the external exposure level to man if such sediments have high con- centratio n of radionu clides. In other parts of the world, research activities have been done in recent time on the contribution to radiation ex- posure from building materials [1-4]. Reports on related work on building materials are few and scanty in Nigeria . Among the reported few are [5] and [6]. In 2009, the radiological safety assessment of surface-water dam sedi- ments in the south west ern Nigeria was performe d by [ 7]. In the building, it has been pointed ou t that the highest concentrations of radionuclides are found in mineral- based materials such as stone, sand, bricks, cement and sediments [8].Though these radionuclides are known to be widely distributed in the environment, their concen- trations have been found and reported [9] to depend on the geological setting of a particular environment, and such they vary from place to place. The objective of this work however is to determine th e radioactivity level of naturally occurring 40K, 238U and 232Th in river sediments across the oil producing coastal areas of Nigeria. The measured radioactivity concentra- tion would thereafter translate to the calculation of the impact indices in order to assess the radiological implica- tion of the use of sediments as a constituent of building materials in the area, which for over four decades have been witnessing the use of v arious types and strengths of radionuclide by the oil companies [10] being accused of polluting the environment of the coastal area in various ways and degrees. 2. Materials and Methods Sediment samples were collected at different points along twenty major rivers in the oil producing coastal area while seven locations were samples for the non oil pro- ducing area. The spacing of the points, which vary be- tween 100 and 500 metres was determined largely by accessibility. Conscious efforts were made to sample around operational sites of the oil companies at lo cations not exceeding 1 km from the operational sites. In all, a total of 133 sediment samples were collected. The map of the areas of sample collection with oil facilities pre- sent is shown in Figure 1. At each sampling location, divers were provided with grab samplers to collect the river sedim ents which consi st Figure 1. Map of study area showing locations where samples were collected. Copyright © 2011 SciRes. JEP
 Natural Radionuclide Concentrations and Radiological Impact Assessment of River Sediments 420 of the Coastal Areas of Nigeria of particulate organic and inorganic matter. After drain- ing off water, each sample was bagged and labeled. The samples were oven dried at a temperature of 105˚C be- fore pulverization [11] and [12]. The dried samples were then packed 200 g by mass in labeled cylindrical plastic containers of uniform base diameter of 5.0 cm which could sit on the 7.6 cm by 7.6 cm NaI (Tl) detector. The plastic containers were tightly covered, sealed and left for 28 days prior to counting, for attainment of secu- lar equilibrium between 238U and 232Th and their respec- tive progenies [11,13,14]. The radionuclide concentration in the sediment sam- ples was measured with a well calibrated [7] low level gamma counting spectrometer consisting of a 7.6 cm by 7.6 cm NaI (Tl) detector (Model 802 series) manufac- tured by Canberra Inc. The detector was coupled to a Canberra series 10 plus multi-channel analyzer (MCA) through a preamplifier base. The photopeak regions of 40K (1.46 MeV); 214Bi (1.76 MeV) and 208Tl (2.165) re- spectively were used for the analysis 40K, 238U and 232Th in the samples. A region of interest was created around the 0.662 MeV to detect and measure any trace of 137Cs as an index of artificial radionuclides. All samples were counted at a constant geometry and for a constant time of 10 hours. 3. Radiological Indicators Following the measurement of the radionuclide concen- trations in the samples, the radium equivalent activity (Raeq), external hazard index (Hex) and internal hazard index (Hin) were used as radiological indicators to esti- mate the radiological implications of the use of the sedi- ment samples as building materials. Assuming secular equilibrium between 40K, 232Th and 238U and their proge- nies, Raeq, the most frequently used indicators for the assessment of the gamma-ray radiation hazard to humans from environmental samples is defined [15] as 10 10 130 7 eqKTh Ra RaCC C (1) where CK, CTh and CRa are th e respective activity con cen- trations of 40K, 232Th and 226Ra, measured in Bqkg–1 of the dry weight. The external hazard index, Hex, commonly used to evaluate the indoor radiation dose rate due to external exposure to gamma radiation from natural radionuclides in building materials can be calculated from the expres- sion of [16] presented as 1 4810259 370 Th Ra K ex CC C H (2) where CK, CTh and CRa are the activities concentrations of 40K, 232Th and 226Ra (in Bq/kg) respectively. This expres- sion indicates that the value of this index must be less than unity in order to keep the radiation hazard to be insignificant. Thus, the maximum values of Hex equal to unity correspond to the upper limit of Raeq being 370 Bq/kg. Considering the hazardous nature of internal exposure to 222Rn and its decay products to the lungs and other respiratory organ, and the fact that reducing the 226Ra to half of its maximum acceptable limit for external expo- sure only will make Hin, the internal hazard index less than unity. Thus Hin is usually estimated as 4810259 185 Th Ra K in CC C H (3) Furthermore, following the definition of the absorbed dose rate in indoor air D (nGyh–1) given by [17,18] and [19] from natural radionuclides inside a standard room of dimensions 4 m × 5 m × 2.8 m, and following the as- sumption [20] that the wall thickness is 20 cm and the density of the aggregates is 2.35 × 103 kgm–3, the frac- tional contribution to the absorbed dose rate in air from the activity concentrations of the three radionucl ides yields 1 .0.080 1.10.92 Th Ra DnGyhCCC (4) The absorbed dose rate in air however translates to the annual effective dose rate indoors for individuals using the values of the absorbed dose rate in indoor air, D (nGyh–1), the indoor occupancy time and the absorbed dose to the effective dose conversion factor(0.7 SvGy–1). Assuming an indoor occupancy factor of 0.8, the annual occupancy time is approximately 7000 hy–1. Hence the effective dose rate is estimated using: 11 16 ..7000 . 0.7 .10 E 1 mSvyDnGy hhy Sv Gy (5) 4. Results and Discussion The range for the activity concentration due to 40K was 95.4 to 160.0 Bqkg–1 while those for 238U and 232Th were respectively 7.6 to 31.0 and 9.5 to 41.6 Bqkg–1. These ranges, belonging to the same population has been rep- resented by a single mean. To establish this, variation in the radionuclide concentration levels among the twenty (20) sampled rivers in the oil producing area were sub- jected to statistical test using analysis of variance (ANOVA) at 95% confidence level. The result (Fcalculated = 0.90 < Ftable = 1.86, p = 0.58 at df = 19) showed that there is no significant difference between the radionu- clide concentration of the sediment samples from the different rivers in the oil producing coastal areas. Simi- Copyright © 2011 SciRes. JEP
 Natural Radionuclide Concentrations and Radiological Impact Assessment of River Sediments 421 of the Coastal Areas of Nigeria larly, for the non oil pro ducin g coastal areas, the result of the ANOVA (Fcalculated = 1.56 < Ftable = 2.99, p = 0.24 at df = 6) also revealed a non significant difference. Based on these findings, the representative means of the spe- cific activities of the natural radionuclides in river sedi- ments of the oil producing and non oil producing coastal areas grouped into different states of the country, Nigeria is presented in Table 1. The errors presen ted with the means of the radioactiv- ity concentrations of 40K, 238U and 232Th in the sediment samples are the standard deviations in the values ob- tained at different points along each river. However, since no significant difference exists among all the samples, the grouped mean of the samples from each of the two areas are determined and tested for pos- sible difference based on the area of collection using t- test at 0.05 level of significance. Results of the test pre- sented in Table 2 shows that there exits a significant difference between the means of 40K in the sediment samples from oil producing coastal areas and those from the non oil producing areas, while 238U and 232Th were observed not to be significantly different at 0.05 level of significance. This observed difference in the 40K level may be explainable from the geological composition of the sediment which have been reported to be more sedi- mentary in the Niger Delta region of the coastal areas [21]. The radium equivalent and the results of other radio- logical indices as shown in Table 3 revealed that despite sediment samples from Cross River having the maximum level of radium equivalent activity, based on the maxi- mum acceptable external dose level of 1.5 mGy, corre- sponding to radium equivalent of 370 Bqkg–1 for build- ing materials [22], the values of the mean radium equivalent activity for the sediments from the coastal areas are all below the recommended limit. Similarly, the observed results of other radiological indicators show that external hazard index, internal haz- ard index and the annual effective dose rate are all less than unity, hence they are below the recommended lim- its. The absorbed dose rate in each of the states of the coastal area of Nigeria is below the worldwide mean of 84 nGyh–1 for soil matrix as reported in [23]. Table 1. Mean concentrations of the radionuclides in the sediment samples. Mean concentrations (Bqkg–1) State No. of rivers No of sediment collected 40K 238U 232Th Oil producing Delta 8 39 132.80 ± 15.89 22.37 ± 6.9 23.04 ± 1.64 Bayelsa 5 23 122.69 ± 14.77 15.82 ± 1.91 21.01 ± 2.45 Rivers 4 18 109.37 ± 12.03 16.26 ± 2.45 21.19 ± 1.94 Cross Rivers 1 5 99.74 ± 11.86 30.09 ± 1.26 41.55 ± 1.78 Akwa Ibom 2 10 147.38 ± 12.94 10.12 ± 1.02 39.76 ± 1.86 Non oil Producing Ogun 2 10 79.65 ± 11.81 16.46 ± 1.97 16.93 ± 1.38 Lagos 5 28 97.31 ± 16.41 13.28 ± 2.54 39.76 ± 1.86 Table 2. Statistics of test of significance between radioactivity concentrations in sediments from oil producing and non oil producing coastal areas. N 40K (Bqkg–1) 238U (Bqkg–1) 232Th (Bqkg–1) Oil producing 20 122.39 ± 47.49 18.93 ± 12.53 29.31 ± 18.67 Non-oil producing 7 88.48 ± 8.22 14.87 ± 3.51 16.37 ± 3.87 tcalculated 3.28 0.93 1.66 ttable (α = 0.05, df = 25) 1.71 1.71 1.71 p value 0.001 0.180 0.054 Copyright © 2011 SciRes. JEP
 Natural Radionuclide Concentrations and Radiological Impact Assessment of River Sediments 422 of the Coastal Areas of Nigeria Table 3. Values of the radiological indices. State Raeq H ex(Bqkg–1) Hin(Bqkg–1) D(nGyh–1) HE(mSvy–1) Oil producing Delta 65.49 0.177 0.237 56.54 0.277 Bayelsa 55.27 0.149 0.192 47.48 0.232 Rivers 54.94 0.148 0.192 47.01 0.230 Cross Rivers 97.11 0.262 0.343 81.36 0.398 Akwa Ibom 78.25 0.211 0.238 64.83 0.317 Non oil producing Ogun 46.77 0.126 0.170 40.13 0.196 Lagos 43.35 0.117 0.153 37.39 0.183 5. Conclusions The natural radioactivity concentrations of a total of 133 samples of sediment collected from twenty-seven(27) ma- jor rivers in the coastal areas of Nigeria have been deter- mined. Statistical analysis of the results showed that there is no significant difference between the radionuclide con- centration of the sediment samples from different rivers in the oil producing and non oil producing coastal areas except for 40K. The values of these natural radionuclide concentrations however translate to the determination of the radiological impact assessment values. The values of the radiological assessment indices obtained were ob- served to be lower than limits international ly reported and recommended for building materials. It could therefore be reported that the oper ations of the oil companies in the coastline, involving use of radioactive mater ials have not contributed adversely to the radioactivity level of the river sediments and that the use of river sediments as building material in the coastal areas of Nigeria poses no radiological risk. As no artificial radionuclide is observed in the samples assayed, the results presented in this work may thus serve as yardstick for future work in this coastal area. REFERENCES [1] M. Sharaf, M. Mansy, El Sayed and E. Abbas, “Natural Radioactivity and Radon Exhalation Rate in Building Materials Used in Egypt,” Radiation Measurements, Vol. 31, No. 1-6, 1999, pp. 491-495. doi:10.1016/s1350-4487(99)00206-1 [2] A. K. Sam and N. Abbas, “Assessment of Radioactivity and the Associated Hazards in Local and Imported Ce- ment Types Used in Sudan,” Radiation Protection Do- simetry, Vol. 93, No. 3, 2001, pp. 275-277. [3] J. Al-Jundi, W. Salah, M. S. Bawa’aneh and F. Afaneh, “Exposure to Radiation from the Natural Radioactivity in Jordanian Building Materials,” Radiation Protection Do- simetry, Vol. 118, No. 1, 2005, pp. 93-96. doi:10.1093/Rpd/Nci332 [4] L. Xinwei, W. Lingqing and J. Xiaodan, “Radiometric Analysis of Chinese Commercial Granites,” Journal of Radioanalytical and Nuclear Chemistry, Vol. 267, No. 3, 2006, pp. 669-673. doi:10.1007/S10967-006-0101-1 [5] I. P. Farai and J. A. Ademola, “Radium Equivalent Activ- ity Concentrations in Concrete Building Blocks in Eight Cities in Southwestern Nigeria,” Journal Environmental Radioactivity, Vol. 79, 2005, No. 2, pp. 119-125. doi:10.1016/J.Jenvrad.2004.05.016 [6] I. P. Farai and J. E. Ejeh, “Radioactivity Concentrations in Common Brands of Cement in Nigeria,” Radioprotec- tion, Vol. 41, No. 4, 2006, pp. 455-462. doi:10.1051/Radiopro:2006020 [7] I. P. Farai and M. O. Isinkaye, “Radiological Safety As- sessment of Surface Water Dam Sediments Used as Building Materials in Southwestern Nigeria,” Journal of Radiological Protection, Vol. 29, No. 1, 2009, pp. 85-93. doi:10.1088/0952-4746/29/1/006 [8] T. Turtiainen, K.Salahel-Din, S. Klemola And A. P. Sihvonen, “Collective Effective Dose by the Population of Egypt from Building Materials,” Journal of Radio- logical Protection, Vol. 28, No. 2, 2008, pp. 223-232. doi:10.1088/0952-4746/28/2/006 [9] M. Iqba, M. Tufail and S. M. Mirza, “Measurement of Natural Radioactivity in Marble Found in Pakistan Using a Nai(Tl) Gamma-Ray Spectrometer,” Journal of Envi- ronmental Radioactivity, Vol. 51, No. 2, 2000, pp. 255-265. doi:10.1016/S0265-931x(00)00077-1 [10] S. A. Elegba, “Uses of Radioactive Sources in the Petro- leum Industry,” Proceedings of Workshop on Radiation Safety in the Nigeria Petroleum Industry, Lagos, June 23-25, 1993, pp. 20-34. [11] N. N. Alam, M. I. Chowdhury, M. Kamal, S. Ghose, N. Copyright © 2011 SciRes. JEP
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