10
EVALUATION OF THE NATURAL RADIOACTIVITY LEVEL OF NIGERIAN TAR SAND DEPOSITS, EASTERN DAHOMEY BASIN, SOUTHWESTERN NIGERIA by Adewale AKINMOSIN 1* , Michael A. OLADUNJOYE 2 , and Fabian ESSIEN 1 1 Department of Geosciences, University of Lagos, Lagos, Nigeria 2 Department of Geology, University of Ibadan, Ibadan, Nigeria Scientific paper DOI: 10.2298/NTRP1601079A The specific activities of natural radionuclides in twenty seven samples collected from the east- ern Dahomey basin in southwestern Nigeria were evaluated. Experimental results were ob- tained by using a 3'' × 3'' sodium iodide NaI(Tl) detector. A major trace element assessment of the samples was made by Inductively Coupled Plasma Mass Spectrometry techniques. Gamma ray radioactive standard sources, 137 Cs and 60 Co, were used to calibrate the measurement sys- tem and the International Atomic Energy Agency SOIL-375 radioactive standard source was also used to analyze and compute the specific activities of desired natural radionuclides. Three radioelements, viz. 238 U, 232 Th and 40 K, were identified in the samples with the following spe- cific activities of 238 U ranging from 9.88 ± 4.70 Bq/kg to 69.15 ± 12.37 Bq/kg with an aver- age of 26.50 ± 7.18 Bq/kg; 232 Th from 12.78 ± 5.16 Bq/kg to 36.86 ± 13.35 Bq/kg with an average of 22.77 ± 4.28 Bq/kg; 40 K ranging from 189.82 ± 79.51 Bq/kg to 518.77 ± ±.119.54 Bq/kg with an average of 297.69 ± 16.21 Bq/kg. The result was compared with the world mean values of 35, 30 and 400 Bq/kg, respectively, specified by the United Nations Sci- entific Committee on the Effects of Atomic Radiation. The mean result obtained for the radium equivalent, total absorbed dose rate, external hazard index, internal hazard index, and the an- nual effective dose equivalent, were 79.90 Bq/kg, 38.50 μSv/h, 0.22 Bq/kg, 0.29 Bq/kg, and 47.22 μSv, respectively. With respect to radiological risk to human health, the absorbed gamma dose rate in air was estimated to be in the range of 21.7 ± 0.4 to 155.7 ± 2.2 μSv/h; the outdoor annual effective dose equivalent was evaluated to vary from 26.6 ± 0.4 to 190.9 ± ±.2.7 μSv with the arithmetic mean value of 79.06 ± 33.23 μSv and compared to the world- wide effective dose of 70 μSv. Also, the values of the radium equivalent and the external hazard index for all samples in the study area were found to be lower than the accepted safety limit value of 370 Bq/kg and equally below the limit of unity, respectively. The results indicate that, at present, the radiation hazard from radionuclides in all samples analyzed is within permissible limits. Key words: tar sand, radionuclide, radiation, dose rate, absorbed rate, hazard, environment INTRODUCTION Ex ten sive seepages and oil sand exposures are known to occur along the East – West belt stretch ing over an ex panse of 120 km ´ 6 km across Lagos, Ogun, Ondo, and Edo States in south western Nige ria [1], ar eas within the east ern margin of Dahomey (Benin), a coastal sedi mentary ba sin (fig. 1). Pub lic in terest con cern ing the said resource has necessi tated a num ber of inves ti gations, such as those in volv ing the or i gin of the tar sands [2] and [3]; ge ol ogy, oil sat u ra tion, re serve es ti ma tion and tex tural char ac ter is tics [1, 4, 5]; geo chemi cal and sedimentological char ac ter is tics [6-11]; physiochemical properties in relation to production and pro cess ing [1, 12, 13], ra dio genic components of the deposits [14]. Geological studies and physicochemical prop er ties have con firmed that Nige rian tar sand is an im - por tant source of en ergy and an alterna tive source of hydro - carbon and raw mate rial for petrochem ical industries [15]. How ever, many fac tors have hampered the ex ploita tion of this re source and promi nent among these is the envi ron - men tal prob lem it may pose to the imme di ate en vi ron ment and its in hab it ants. Ra dioac tive el e ments oc cur in trace amounts in most rocks and min er als and are readily de tect - able by the gamma ra di a tion emitted during their de cay [16]. The na ture and oc currence of ra dio ac tive el e ments in crude and re sid ual oils is of in terest to min ers, refin ery oper - ators and environmentalists concerned with emissions from oil-fired power plants. The pres ent research is, there fore, A. Akinmosin, et al.: Evaluation of the Natural Radioactivity Level of Nigerian ... Nuclear Technology & Radiation Protection: Year 2016, Vol. 31, No. 1, pp. 79-88 79 * Corresponding author; e-mail: adewaleakinmosin@yahoo.com

EVALUATION OF THE NAT U RAL RA DIOAC TIV ITY LEVEL …ntrp.vin.bg.ac.rs/2016_1/Akinmosin_2016_1.pdfcific ac tiv i ties o f 238 U ran g ing fro m 9.88 ± 4.70 Bq /kg to 69.15 ± 12.37

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Page 1: EVALUATION OF THE NAT U RAL RA DIOAC TIV ITY LEVEL …ntrp.vin.bg.ac.rs/2016_1/Akinmosin_2016_1.pdfcific ac tiv i ties o f 238 U ran g ing fro m 9.88 ± 4.70 Bq /kg to 69.15 ± 12.37

EVAL U A TION OF THE NAT U RAL RA DIO AC TIV ITY LEVEL OFNI GE RIAN TAR SAND DE POS ITS, EAST ERN DA HO MEY

BA SIN, SOUTH WEST ERN NI GE RIA

by

Adewale AKINMOSIN 1*, Michael A. OLADUNJOYE 2, and Fabian ESSIEN 1

1De part ment of Geosciences, Uni ver sity of Lagos, Lagos, Ni ge ria2 De part ment of Ge ol ogy, Uni ver sity of Ibadan, Ibadan, Ni ge ria

Sci en tific pa perDOI: 10.2298/NTRP1601079A

The spe cific ac tiv i ties of nat u ral radionuclides in twenty seven sam ples col lected from the east -ern Da ho mey ba sin in south west ern Ni ge ria were eval u ated. Ex per i men tal re sults were ob -tained by us ing a 3'' ́ 3'' so dium io dide NaI(Tl) de tec tor. A ma jor trace el e ment as sess ment ofthe sam ples was made by In duc tively Cou pled Plasma Mass Spec trom e try tech niques. Gammaray ra dio ac tive stan dard sources, 137Cs and 60Co, were used to cal i brate the mea sure ment sys -tem and the In ter na tional Atomic En ergy Agency SOIL-375 ra dio ac tive stan dard source wasalso used to an a lyze and com pute the spe cific ac tiv i ties of de sired nat u ral radionuclides. Threeradio ele ments, viz. 238U, 232Th and 40K, were iden ti fied in the sam ples with the fol low ing spe -cific ac tiv i ties of 238U rang ing from 9.88 ± 4.70 Bq/kg to 69.15 ± 12.37 Bq/kg with an av er -age of 26.50 ± 7.18 Bq/kg; 232Th from 12.78 ± 5.16 Bq/kg to 36.86 ± 13.35 Bq/kg with an av er age of 22.77 ± 4.28 Bq/kg; 40K rang ing from 189.82 ± 79.51 Bq/kg to 518.77 ±±.119.54 Bq/kg with an av er age of 297.69 ± 16.21 Bq/kg. The re sult was com pared with theworld mean val ues of 35, 30 and 400 Bq/kg, re spec tively, spec i fied by the United Na tions Sci -en tific Com mit tee on the Ef fects of Atomic Ra di a tion. The mean re sult ob tained for the ra dium equiv a lent, to tal ab sorbed dose rate, ex ter nal haz ard in dex, in ter nal haz ard in dex, and the an -nual ef fec tive dose equiv a lent, were 79.90 Bq/kg, 38.50 mSv/h, 0.22 Bq/kg, 0.29 Bq/kg, and47.22 mSv, re spec tively. With re spect to ra dio log i cal risk to hu man health, the ab sorbed gamma dose rate in air was es ti mated to be in the range of 21.7 ± 0.4 to 155.7 ± 2.2 mSv/h;the out door an nual ef fec tive dose equiv a lent was eval u ated to vary from 26.6 ± 0.4 to 190.9 ±±.2.7 mSv with the arith me tic mean value of 79.06 ± 33.23 mSv and com pared to the world -wide ef fec tive dose of 70 mSv. Also, the val ues of the ra dium equiv a lent and the ex ter nal haz ardin dex for all sam ples in the study area were found to be lower than the ac cepted safety limitvalue of 370 Bq/kg and equally be low the limit of unity, re spec tively. The re sults in di cate that, at pres ent, the ra di a tion haz ard from radionuclides in all sam ples an a lyzed is within per mis si blelim its.

Key words: tar sand, radionuclide, ra di a tion, dose rate, ab sorbed rate, haz ard, en vi ron ment

INTRODUCTION

Ex ten sive seepages and oil sand ex po sures areknown to oc cur along the East – West belt stretch ing over an ex panse of 120 km ́ 6 km across Lagos, Ogun, Ondo, andEdo States in south west ern Ni ge ria [1], ar eas within theeast ern mar gin of Da ho mey (Benin), a coastal sed i men taryba sin (fig. 1). Pub lic in ter est con cern ing the said re sourcehas ne ces si tated a num ber of in ves ti ga tions, such as thosein volv ing the or i gin of the tar sands [2] and [3]; ge ol ogy, oilsat u ra tion, re serve es ti ma tion and tex tural char ac ter is tics[1, 4, 5]; geo chem i cal and sedimentological char ac ter is tics[6-11]; physiochemical prop er ties in re la tion to pro duc tion

and pro cess ing [1, 12, 13], ra dio genic com po nents of thede pos its [14]. Geo log i cal stud ies and physicochemicalprop er ties have con firmed that Ni ge rian tar sand is an im -por tant source of en ergy and an al ter na tive source of hy dro -car bon and raw ma te rial for pet ro chem i cal in dus tries [15].How ever, many fac tors have ham pered the ex ploi ta tion ofthis re source and prom i nent among these is the en vi ron -men tal prob lem it may pose to the im me di ate en vi ron mentand its in hab it ants. Ra dio ac tive el e ments oc cur in traceamounts in most rocks and min er als and are readily de tect -able by the gamma ra di a tion emit ted dur ing their de cay[16]. The na ture and oc cur rence of ra dio ac tive el e ments incrude and re sid ual oils is of in ter est to min ers, re fin ery op er -a tors and en vi ron men tal ists con cerned with emis sions fromoil-fired power plants. The pres ent re search is, there fore,

A. Akinmosin, et al.: Eval u a tion of the Nat u ral Ra dio ac tiv ity Level of Ni ge rian ...Nu clear Tech nol ogy & Ra di a tion Pro tec tion: Year 2016, Vol. 31, No. 1, pp. 79-88 79

* Cor re spond ing au thor; e-mail: adewaleakinmosin@ya hoo.com

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aimed at gen er at ing a base line data on the nat u ral ra dio ac -tiv ity level of the tar sand de pos its in the east ern Da ho meyba sin.

GE OL OGY AND STRA TIG RA PHYOF THE DA HO MEY BASIN

The Benin (Da ho mey) ba sin is a part of the sys -tem of the West Af ri can pericratonic (mar gin sag) ba -sin [17, 18] de vel oped dur ing the com mence ment ofrift ing, as so ci ated with the open ing of the Gulf ofGuinea in the Late Ju ras sic to the Early Cre ta ceous[19, 20]. The crustal sep a ra tion, typ i cally pre ceded bycrustal thin ning, was ac com pa nied by an ex tended pe -riod of ther mally in duced ba sin sub si dence throughthe Mid dle – Up per Cre ta ceous to Ter tiary times, asthe South Amer i can and the Af ri can plates en tered adrift phase to ac com mo date the emerg ing At lan ticOcean [21, 22]. The Ghana Ridge, pre sum ably an off -

set ex ten sion of the Romanche Frac ture Zone, con -fines the ba sin in the west while the Benin Hinge Line,a base ment es carp ment which sep a rates the OkitipupaStruc ture from the Niger Delta ba sin, con fines it in theeast. The Benin Hinge Line sup pos edly de fines thecon ti nen tal ex ten sion of the Chain Frac ture Zone. Theon shore part of the ba sin cov ers a broad arc-shapedpro file of about 600 km2 in ex tent. The on shore sec tion of the ba sin at tains a max i mum width along its N-Saxis of around 130 km in the prox im ity of the bor derbe tween Ni ge ria and the Re pub lic of Benin. The ba sinnar rows to about 50 km on the east ern side where it as -sumes a con vex up wards out line with con com i tantthin ning of sed i ments. Along the north east ern fringeof the ba sin, where it rims the Okitipupa Ridge, tar(oil) sands and bi tu men seepages oc cur [23].

The lithostratigraphic units of the Cre ta ceous toTer tiary sed i men tary suc ces sion of the east ern mar ginof the Da ho mey ba sin, as clas si fied by the Min is try ofSolid Min er als [24], are sum ma rized in tab. 1.

A. Akinmosin, et al.: Eval u a tion of the Nat u ral Ra dio ac tiv ity Level of Ni ge rian ...80 Nu clear Tech nol ogy & Ra di a tion Pro tec tion: Year 2016, Vol. 31, No. 1, pp. 79-88

Fig ure 1. Gen er al ized geo log i cal map of the east ern Da ho mey ba sin show ing the area ex tent of tar sand de pos its(Mod i fied af ter [1])

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SITE DE SCRIP TION

The study ar eas are lo cated within Ogun andOndo States, ap prox i mately within lat i tudes N 06 38'54.6" and N 06 46' 47.7 and lon gi tudes E 003 58' 21.4"and E 004 58' 28.57". They are lo cated in the east ernpart of the Da ho mey ba sin around the Okitipupa ridge,

South-West Ni ge ria. Their to pog ra phies range from rel -a tively low to high re liefs. Imeri-Ijebu, J4, Loda, andIgorisa lo ca tions are of low re lief, while Orisunmibare,Gbegude, and Idobilayo are ar eas with a high re lief sys -tem (8 m-54 m).

The out crop points are gen er ally sloped and lo -cated within farm lands or thick veg e tated ar eas (fig. 2).

A. Akinmosin, et al.: Eval u a tion of the Nat u ral Ra dio ac tiv ity Level of Ni ge rian ...Nu clear Tech nol ogy & Ra di a tion Pro tec tion: Year 2016, Vol. 31, No. 1, pp. 79-88 81

Ta ble 1. The strati graphic col umn of the da ho mey ba sin, [24]

Formation Age Thickness (feet) Comments

Benin formationCoastal plains sands

Tertiary

Pleistocene – Oligocene 0-1600 Coastal – plain clastics

Oshosun – ilaro –Ameki formations Eocene 200-1000

Fluvial and marine sandsand clays

Ewekoro formation Palaeocene 400-1000 Marine shale, limestone

Araromi formationAbeokuta formation

Cretaceous

Maastrichtian 500-1000Coastal sand, shale, marineshale

Afowo formationTuronian SstAlbian Sst

Campanian – Aptian 0-800Marine sandstone, shale,limestone

Ise formation Barremian 0-6000+Continental and lacustrineriftbasin fill

Crystalline basement(undifferentiated) Cambrian – Precambrian

Metamorphic and igneouscomplex

Fig ure 2. Lo ca tion map of the study areas

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METH OD OL OGY

Sam ple col lec tion

The sam ples were col lected at ten dif fer ent lo ca -tions across the tar sand belt (from east ern to west ernparts). De tailed in for ma tion, as ob tained from eachsam pling lo ca tion, is in di cated in tab. 2.

Lab o ra tory work

Gamma-ray spec tro met ric anal y sis was car riedout on twenty six sam ples at the Cen tre for En ergy andRe search De vel op ment, Obafemi Awolowo Uni ver -sity, Ile-Ife, Ni ge ria. The sam ples were trans ferredfrom bags into clean air tight con tain ers and sealed fortwenty eight days so as to at tain sec u lar equi lib riumand, also, to pre vent the es cape of Ra-226. More over,an empty clean con tainer was weighed and then sealedfor a min i mum of twenty eight days to serve as theback ground count. Var i ous de tec tors have been usedto mea sure the ra di a tion en ergy de pos ited in the me -dium. The choice of the de tec tor for low-count ingmea sure ments is a func tion of many fac tors, but en -ergy res o lu tion and count ing ef fi ciency are the mostim por tant ones to be con sid ered. The two types of de -tec tors used in this study are: in or ganic scin til la tioncoun ter so dium io dide (NaI) ac ti vated with thalium

(Tl), the other one be ing a high-pu rity ger ma nium de -tec tor (HPGe). Af ter a min i mum of twenty eight (28)days for the sealed sam ples to at tain sec u lar equi lib -rium, the beach sam ple was placed in a HPGe de tec toren closed in a lead shield and counted for ten hours(3600 s). An iden ti cal but empty con tainer was sealedfor the same twenty eight days and also counted for tenhours. A stan dard soil sam ple that con tains cer ti fiedra dio ac tiv ity con cen tra tion due to 238U, 232Th, and 40Kby weight was counted for ten hours, as well. The highres o lu tion of the HPGe de tec tor made the iden ti fi ca -tion of a wide spec trum of g-ray en ergy in the sam plespos si ble and the photopeaks ob served with reg u lar ityin the sam ples were iden ti fied. The area un der eachpeak of the spec tra pro duced was ana lysed us ing aspec tra anal y sis pro gram, SAMPO-90, whichmatched g-en er gies at var i ous en ergy lev els to a li brary of pos si ble ra dio iso topes. The back ground peakheight area was sub tracted from the stan dard peak area in or der to get the net-peak area val ues for both thestan dard and the samplings, re spec tively.

RE SULTS AND DIS CUS SION

Ra dio ac tiv ity con tents

Nat u ral radionuclide con cen tra tions mea suredin the sam ples col lected at all lo ca tions are as pre -sented in tab. 3.

A. Akinmosin, et al.: Eval u a tion of the Nat u ral Ra dio ac tiv ity Level of Ni ge rian ...82 Nu clear Tech nol ogy & Ra di a tion Pro tec tion: Year 2016, Vol. 31, No. 1, pp. 79-88

Ta ble 2. Lo ca tion of sam pling points

Sam ple no Depth [m] Name of the town Brief ge ol ogy ofsam pling point

Lo ca tion

Lat i tude Lon gi tude

IM1-1 2.0

Imeri-1

Shale

06°46'47.7'' 003°58'21.7''IM1-2 2.5 Shale

IM1-3 3.0 Shale

IM2-1 0.5

Imeri-2

Tar sand

06°46'46.2'' 003°58'21.4''IM2-2 1.0 Tar sand

IM2-3 1.5 Tar sand

J4 1 0.5Junc tion-4 (J4)

Tar sand06°40'43.6'' 004°18'39.4''

J4 2 1.0 Tar sand

OR1 0.5Orisumbare

Tar sand 06°42'23.0'' 004°21'32.7''

OR2 1.0 Tar sand 06°40'59.4'' 004°21'58.4''

GB1 0.5

Gbegude

Tar sand

06°40'04.5'' 004°25'14.9''

GB2 1.0 Tar sand

GB3 1.5 Tar sand

GB4 2.0 Tar sand

GB5 2.5 Tar sand

ID1 0.5

Idobilayo

Tar sand

06°38'54.6'' 004°33'39.7''ID2 1.0 Shale

ID3 1.5 Shale

IJ1 0.5 Ijuoke Oja Lig nite 06°35'07.5'' 004°38'52.5''

LT1 0.5 Looto Ka olin 06°34'49.7'' 004°40'41.9''

LD1 0.5

Loda

Tar sand

06°39'03.7'' 004°53'08.6''LD2 1.0 Tar sand

LD3 1.5 Tar sand

LD4 2.0 Tar sand

IG1 0.5Igorisa

Bi tu men06°39'08.7'' 004°58'28.6''

IG2 1.0 Bi tu men

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Imeri

At this site, six sam ples were col lected at two dif -fer ent lo ca tions. The mean ac tiv ity con cen tra tions for the var i ous radionuclides were 197.89 ± 65.33 Bq/kg, 9.88 ±±.4.70 Bq/kg, and 13.19 ± 6.13 Bq/kg for 40K, 238Uand 232Th, re spec tively. The re sults in di cate that 40K hasthe high est ac tiv ity in all sam ples from Imeri, with the high est value of 238U be ing 69.15 ± 12.37 Bq/kg. TheImeri- 1(IM1-1) has the high est value of 40K (419.86 ±

± 98.37 Bq/kg). 232Th re corded the low est av er ageradionuclide value of 21.18 ± 8.32 Bq/kg (fig. 3).

J4

The radionuclides iden ti fied at J4 with the high -est ac tiv ity con cen tra tion be long to the de cay se ries of40K, with an av er age spe cific ac tiv ity con cen tra tion of354.33 ± 115.75 51 Bq/kg which shows an in creasewith depth. 238U and 232Th dis played a con sid er ablylower value, as shown in fig. 3.

Orisumbare

232Th and 238U have the least con tri bu tion to theto tal ac tiv ity of the sam ples col lected at Orisumbare,with con cen tra tion rang ing from 17.45 ± 7.86 to 15.59 ± 4.79 and 14.41 ± 5.36 to17.64 ± 6.41 Bq/kg, re spec -tively. The K-40 radionuclide has the high est ac tiv itywith a value of 213.30 ± 73.51 Bq/kg and 321.24 ± ±.76.8251 Bq/kg (fig. 3). The ra dio ac tive nuclides insam ples col lected at this lo ca tion dis played a rel a tive

A. Akinmosin, et al.: Eval u a tion of the Nat u ral Ra dio ac tiv ity Level of Ni ge rian ...Nu clear Tech nol ogy & Ra di a tion Pro tec tion: Year 2016, Vol. 31, No. 1, pp. 79-88 83

Ta ble 3. Re sults of ra dio ac tiv ity con cen tra tions of 40K, 238U, and 232Th se ries in the sam ples

Sam ple Name of the town 40K 238U(226Ra) 232Th(228Ra)Dose rate [mSvh–1] for g

Be fore lab.anal y sis

Af ter lab.anal y sis

IM1-1

Imeri-1

419.86 ± 98.37 69.15 ± 12.37 25.55 ± 9.03 0.12 0.12

IM1-2 319.68 ± 106.98 16.57 ± 6.21 17.59 ± 8.73 0.12 0.13

IM1-3 197.89 ± 65.33 18.61 ± 5.31 14.74 ± 5.89 0.10 0.11

IM2-1

Imeri-2

275.78 ± 42.28 48.68 ± 13.16 30.07 ± 12.78 0.12 0.14

IM2-2 207.30 ± 39.33 9.88 ± 4.70 13.19 ± 6.13 0.14 0.13

IM2-3 298.96 ± 53.34 23.28 ± 9.60 25.92 ± 7.35 0.17 0.16

J4-1Junc tion-4 (J4)

345.93 ± 88.92 22.42 ± 8.30 25.26 ± 11.09 0.14 0.14

J4-2 362.72 ± 142.58 27.57 ± 10.90 19.34 ± 10.12 0.18 0.17

OR1Orisumbare

213.30 ± 73.51 14.41 ± 5.36 17.45 ± 7.86 0.12 0.12

OR2 321.24 ± 76.82 17.64 ± 6.41 15.59 ± 4.79 0.10 0.11

GB1

Gbegude

394.65 ± 99.12 47.37 ± 12.54 36.86 ± 13.35 0.15 0.16

GB2 240.09 ± 73.62 23.86 ± 9.62 29.76 ± 9.87 0.17 0.15

GB3 254.98 ± 81.53 21.07 ± 8.23 25.31 ± 8.59 0.16 0.14

GB4 299.77 ± 78.48 26.72 ± 8.86 31.46 ± 7.65 0.18 0.17

GB5 318.19 ± 95.42 32.34 ± 11.09 27.92 ± 11.53 0.20 0.21

ID1

Idobilayo

232.11 ± 58.47 27.83 ± 9.56 28.43 ± 9.80 0.21 0.20

ID2 189.82 ± 79.51 28.33 ± 8.93 15.52 ± 4.15 0.16 0.17

ID3 321.19 ± 77.32 27.04 ± 7.89 19.65 ± 8.54 0.12 0.13

IJ1 Ijuoke Oja 234.78 ± 61.85 28.28 ± 9.65 30.35 ± 9.69 0.15 0.14

LT1 Looto 196.86 ± 59.35 31.14 ± 11.32 12.78 ± 5.16 0.18 0.18

LD1

Loda

340.89 ± 88.91 15.94 ± 7.81 20.90 ± 9.18 0.17 0.16

LD2 282.20 ± 87.74 23.79 ± 8.62 18.06 ± 8.71 0.15 0.15

LD3 362.3 ± 106.85 37.63 ± 7.29 26.43 ± 11.19 0.31 0.28

LD4 343.52 ± 74.77 13.88 ± 6.33 17.55 ± 9.02 0.18 0.17

IG1Igorisa

518.77 ± 119.54 18.59 ± 6.27 20.42 ± 9.73 0.14 0.15

IG2 324.64 ± 78.91 20.10 ± 9.51 23.31 ± 8.95 0.16 0.15

Av er age meanvalue 26.37 ± 8.70 22.70 ± 8.817 298.92 ± 81.04 0.17 0.16

Fig ure 3. Pic to rial rep re sen ta tion of 40K, 238U, and 232Thin all sam ples

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in crease in radionuclide con cen tra tion with depth,with the ex cep tion of those of the 232Th se ries.

Gbegude

Gbegude is char ac ter ised by a range of val ues ofac tiv ity con cen tra tion, as re corded in all six sam plescol lected at this lo ca tion. For all of the six sam ples col -lected at Gbegude, the radionuclide con cen tra tion var -ies be tween 220.11 ± 79.13 and 394.65 ± 99.12 Bq/kgwith an av er age of 287.97 ± 84.55 Bq/kg for 40K;21.07 ± 8.23 and 47.37 ± 12.54 Bq/kg with an av er -age of 29.12 ± 9.92 Bq/kg for 238U; 25.31 ± 8.59 and36.86 ± 13.35 Bq/kg with an av er age of 29.45 ± 10.03Bq/kg for 232Th. 40K has the high est con cen tra tion ofthe three radionuclides pres ent (about 82 % of the to talac tiv ity).

Idobilayo

Three sam ples were col lected at Idobilayo at var i -ous depths (tab. 3). For 40K con cen tra tion, Idobilayo 3(ID3) has the high est value of 321.19 ± 77.327 Bq/kg,while the low est value of 232.11 ± 58.47 Bq/kg wasfound at Idobilayo 1 (ID1). 238U con cen tra tions have aslight value vari ance with an av er age value of 27.72 ±±.8.79 Bq/kg, as shown in fig. 3. The high est value ofTh-232 is at Idobilayo 2 (ID2) with a value of 28.43 ±±.9.80 Bq/kg. Gen er ally, the con cen tra tion of 40K wasrel a tively higher com pared to con cen tra tions of 238Uand 232Th in all of the an a lyzed sam ples.

Ijuoke oja

The 40K ac tiv ity con cen tra tion of the lig nite sam ple at this lo ca tion has an av er age value of 234.78 ± 61.85Bq/kg. 238U and 232Th had a value of 28.28 ± 9.65 Bq/kgand 30.35 ± 9.69 Bq/kg which is con sid er able for the av -er age range, com pared to the ac tiv ity con cen tra tion re -corded at other lo ca tions, as shown in fig. 3.

Looto

The pic to rial rep re sen ta tion of radionuclide con -cen tra tion val ues ob tained at Looto is shown in fig. 3.Looto is char ac ter ized by a rel a tive low value of theac tiv ity con cen tra tion with 196.86 ± 59.35 Bq/kg,31.14 ± 11.32 Bq/kg, and 12.78 ± 5.16 Bq/kg for 40K,238U and 232Th, re spec tively. The value of 40K is highcom pared to the value that was ob tained for 238U and232Th which is the gen eral trend at all other lo ca tions.

Loda

The spe cific ac tiv i ties mea sured in the var i oussam ples col lected at Loda are shown in fig. 3. The

ac tiv ity con cen tra tion of 40K ranged from 340.89 ± ±.88.91 Bq/kg to 282.20 ± 87.74 Bq/kg with an av er -age of 332.22 ± 89.57 Bq/kg; 13.88 ± 6.33 Bq/kg to37.63 ± 7.29 Bq/kg with an av er age of 22.81 ± 7.51Bq/kg for 282U; 17.55 ± 9.02 Bq/kg to 26.43 ± 11.19Bq/kg with an av er age of 20.74 ± 9.53 Bq/kg for 232Th. The larg est con tri bu tion to the over all ac tiv ity in all ofthe var i ous sam ples col lected at Loda was mainly from 40K, with the low est value of 282.20 ± 87.74 Bq/kg, the high est be ing 340.89 ± 88.91 Bq/kg com pared to theav er age ac tiv ity ranges of 22.81 ± 7.51 Bq/kg and20.74 ± 9.53 Bq/kg for 238U and 232Th, re spec tively.The spe cific ac tiv ity due to 232Th is rel a tively low in all sam ples in ves ti gated at this lo ca tion.

Igorisa

40K is the high est con trib u tor to the ac tiv ity in the area cov er ing about 93 % of the to tal ac tiv ity con cen -tra tions, while 238U and 232Th con trib ute by 3 % and4 %, re spec tively. In the spec i men, the ac tiv ity of 238Uis the low est in com par i son to that of 232Th and thiscon sis tency is re flected in the sam ples col lected at thelo ca tion (see fig. 3).

From fig. 3, it was ob vi ous that the sam ple col -lected at Igorisa 1(IG1) has the high est con cen tra tionof 40K, the high est con cen tra tion of 238U was re cordedat Imeri 1(IM1-1), while the high est con cen tra tion of232Th was ob served at Gbegude1(GB1).

Ac cord ing to Serra-2008 [25], it was as sertedthat illite is the pri mary po tas sium-bear ing min eral inoil sands. This is fol lowed by K-feld spar, while mus -co vite and bi o tite are mi nor phases. Akinmosin et al.,2011 [26] iden ti fied the pres ence of K-feld spar as oneof the com po nents of the Ni ge rian tar sand de pos its byscan ning the elec tron mi cro scope im ages of somesam ples. More over, from the petrographic study ofsome tar sand sam ples from the Ni ge rian tar sand belt,Akinmosin et al., 2005 [27] es tab lished that micas arepres ent in traces. Based on this prem ise, it is safe to ad -duce that the higher val ues of ra dio ac tive con cen tra -tion of 40K re corded in all cited lo ca tions over otherradionuclides can be said to have been sourced fromthe K-feld spar com po nent of the de posit. K-feld sparusu ally oc curs in the form of in clu sions within the tarsand de posit. Ura nium and tho rium may have been de -rived from ra dio ac tive min er als such as zir con, xeno -time, and pos si bly, thorite [28].

Ab sorbed dose rate in sam ples

Two dif fer ent re cords of the ab sorbed dose rate inthe sam ples were taken: be fore the lab o ra tory anal y sis andaf ter the anal y sis was car ried out us ing a Gamma-Scoutde tec tor. The re sults of the to tal ab sorbed dose rate in thetwenty six sam ples col lected are sum ma rized in tab. 3. Itvar ies be tween 0.1-0.21 µSv/h, av er ag ing 0.16 µSv/h be -

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fore the lab o ra tory anal y sis. Af ter the anal y sis, the valuevar ied from 0.11-0.28 µSv/h, the av er age dose rate be ing0.16 µSv/h. Sam ple LD3 col lected at Loda had the high estdose rate with the ab sorbed dose rate of 0.31µSv/h and0.28 µSv/h be fore and af ter the lab o ra tory anal y ses (figs. 4 and 9). This sam ple also re corded the high est val ues in ac -tiv ity con cen tra tion of all for the radionuclides iden ti fied at said lo ca tions.

Ra dio log i cal ef fects, in di cesand haz ard as sess ment

One of the main ob jec tives of ra dio ac tiv ity mea -sure ment in en vi ron men tal stud ies is not to sim ply de -ter mine the ac tiv ity con cen tra tions of 238U, 232Th, and40K, but also to es ti mate the ra di a tion ex po sure doseand as sess the bi o log i cal ef fects on hu mans. The as -sess ment of ra dio log i cal risk can be con sid ered in var i -ous terms. In the cur rent study, five re lated quan ti tieswere de duced. These in clude: (1) Ra dium equiv a lent ac tiv ity (Raeq), (2) Ab sorbeddose rate (D), (3) An nual ef fec tive dose equiv a lent(AEDE), (4) Ex ter nal haz ard in dex (Hex), and (5) In -ter nal haz ard in dex (Hin).

These ra dio log i cal pa ram e ters can be cal cu latedfrom the mea sured ac tiv ity con cen tra tions of the threemain pri mor dial radionuclides in the sam ples. The val -ues of these ra dio log i cal haz ard pa ram e ters, as de -duced in the cur rent work, are shown in tab. 4.

Ra dium equiv a lent ac tiv ity

The cal cu lated value of ra dium equiv a lent ac tiv -ity is shown in tab. 4. The mean Raeq ranges be tween43.25 and 135.08 Bq/kg with an av er age value of

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Fig ure 4. Pic to rial rep re sen ta tion of the ab sorbed doserates from gamma ra di a tion

Ta ble 4. Ra dium equiv a lent ac tiv ity, dose rate, an nual ef fec tive dose, ex ter nal haz ard in dex and in ter nal haz ard in dex atdif fer ent lo ca tions in the study area

Sam plesRa dio log i cal in di ces

Ra dium equiv a lentac tiv ity [Bqkg–1]

Dose rate[nGyh–1]

An nual ef fec tive dose[µSv] Ex ter nal haz ard in dex In ter nal haz ard in dex

IM1-1 135.08 65.01 79.73 0.37 0.56

IM1-2 64.1 31.71 38.88 0.18 0.22

IM1-3 53.54 25.81 31.66 0.15 0.2

IM2-1 110.98 52.24 64.06 0.31 0.44

IM2-2 43.25 21.24 26.05 0.12 0.15

IM2-3 81.27 38.97 47.79 0.23 0.29

J4-1 82.76 40.14 49.23 0.23 0.29

J4-2 80.62 39.65 48.63 0.22 0.3

OR1 54.29 26.16 32.08 0.15 0.19

OR2 62.42 31.06 38.09 0.17 0.22

GB1 127.71 60.72 74.47 0.35 0.48

GB2 83.22 39.08 47.93 0.23 0.29

GB3 75.11 35.73 43.82 0.21 0.26

GB4 92.69 43.94 53.88 0.26 0.33

GB5 94.54 45.17 55.39 0.26 0.35

ID1 84.73 39.78 48.78 0.23 0.31

ID2 63.81 30.43 37.33 0.18 0.25

ID3 77.62 37.85 46.42 0.22 0.29

IJ1 88.12 41.26 50.60 0.24 0.32

LT1 63.2 30.37 37.25 0.17 0.26

LD1 69.69 34.31 42.07 0.19 0.24

LD2 69.37 33.75 41.39 0.19 0.26

LD3 100.79 48.57 59.56 0.28 0.38

LD4 63.02 31.44 38.56 0.18 0.21

IG1 84.1 42.71 52.38 0.24 0.29

IG2 76.16 37.00 45.38 0.21 0.27

Range 43.25-135.08 21.24-65.01 26.05-79.73 0.12-0.37 0.15-0.56

Av er age 79.90 38.50 47.22 0.22 0.29

World mean range [29] <370 57

18-9370– <1 <1

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79.90 Bq/kg. The high est value of Raeq was ob servedin Imeri tar sand sam ples de noted IM1-1, while thelow est val ues are seen at the same lo ca tion (Imeri).This lo ca tion is char ac ter ized with the high est andlow est value of 238U radionuclide con cen tra tion,hence, the en tire value of Raeq falls be low the de sir able limit. Fig ure 5 is a graph i cal rep re sen ta tion of the ra -dium equiv a lent ac tiv ity.

To tal ab sorbed dose rate

The to tal ab sorbed dose rates cal cu lated for allsam ples col lected are shown in tab. 4. The value of theto tal mean ab sorbed dose rate at 1.0 m above theground level ranges from 21.24-65.00 mSv/h with anav er age of 38.5 mSv/h. The high est value was re corded at Imeri, which is rel a tively small when com pared with the value (1.0 mSv per year) rec om mended by the In -ter na tional Com mis sion on Ra dio log i cal Pro tec tion as the max i mum per mis si ble dose equiv a lent for mem -bers of the pub lic. This im plies that the tar sand in thestudy ar eas is safe for min ing and hu man ac tiv i ties. Fig ure 6 is a graph i cal rep re sen ta tion of the dose rate.

Ex ter nal haz ard in dex

The re sult pre sented in tab. 4 shows that themean Hex ranged be tween 0.12 and 0.3 with an av er age value of 0.22. These val ues, be ing less than 1 as rec -om mended by the In ter na tional Com mis sion on Ra -dio log i cal Pro tec tion, show that the sam ples are safefor ex po sure to hu man ac tiv i ties. Fig ure 7 is a graph i -cal rep re sen ta tion of the Hex.

In ter nal haz ard in dex

The val ues ob tained for the in ter nal haz ard in dex are as shown in tab. 4, dem on strat ing that the mean Hin

ranged from 0.15 to 0.56 with an av er age of 0.29.Thein ter nal haz ard in dex (Hin) of the study area is <1(max i mum value rec om mended by [30]). This im pliesthat the ra di a tion in the study area is be low the rec om -mended Hin, as shown in fig. 8.

An nual ef fec tive dose

As shown in fig. 9 the an nual ef fec tive dose wasfound to vary be tween 26.05 and 79.73 µSv with amean of 47.22 µSv (tab. 4). Two of the lo ca tions,(Imeri – IM1 and Gbegude – GB1), show a slightlyhigher value than the world av er age.

CON CLU SIONS

The level of nat u ral ra dio ac tiv ity in sam ples col -lected along the tar sand belt in the east ern Da ho meyba sin has been eval u ated via a 3'' ´ 3'' so dium io dideNaI(Tl) de tec tor. The re sults of the in ves ti ga tionshowed that pri mor dial radionuclides, namely 238U,

A. Akinmosin, et al.: Eval u a tion of the Nat u ral Ra dio ac tiv ity Level of Ni ge rian ...86 Nu clear Tech nol ogy & Ra di a tion Pro tec tion: Year 2016, Vol. 31, No. 1, pp. 79-88

Fig ure 5. Graph i cal rep re sen ta tion ofra dium equiv a lent ac tiv ity

Fig ure 6. Graph i cal rep re sen ta tion of theto tal ab sorbed dose rate

Fig ure 7. Graph i cal rep re sen ta tion of theexterna haz ard in dex

Fig ure 8. Graph i cal rep re sen ta tion of thein ter nal hazard in dex

Fig ure 9. Graph i cal rep re sen ta tion of thean nual ef fec tive dose

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232Th, and 40K, were pres ent in all sam ples. The mea -sured ac tiv ity con cen tra tions of 238U, 232Th, and 40K inall of the sam ples col lected var ied from 9.88 ± 4.70Bq/kg to 69.15 ± 12.37 Bq/kg, 12.78 ± 5.16 Bq/kg to36.86 ± 13.35 Bq/kg, and 189.82 ± 79.1 Bq/kg to518.77 ± 119.54 Bq/kg, with the av er age mean val uesof 26.37 ± 8.70 Bq/kg, 22.70 ± 8.817 Bq/kg, and298.92 ± 81.04 Bq/kg, re spec tively. The re sults ob -tained for ac tiv ity con cen tra tions of 238U and 232Thwere found to be lower than the up per range of theworld wide val ues of 17-60 Bq/kg, 11-64 Bq/kg iden ti -fied by UNSCEAR-2000 [31]. The ac tiv ity con cen tra -tion of 40K in the study area falls within the world widerange of val ues which are 140-850 Bq/kg, as re portedby Oladunjoye et al., – 2014 [28]. The high est con trib -u tor of 40K came from the bi tu men sam ples at Igorisa,while that of 238U was from the tar sand sam ples atImeri and Gbegude with the high est value of 232Th de -tected. The Ka olin sam ple col lected from Looto hasthe low est value of 232Th. In all sam pled lo ca tions, themean ac tiv ity con cen tra tion is of the or der 232Th < 238U< 40K. Gen er ally, the con cen tra tion of 232Th is lowerthan that of 238U and 40K, re spec tively. 40K ac tiv itydom i nates over 238U and 232Th el e men tal ac tiv i ties,pos si bly due to the rich ness of the tar de pos its inK-feld spars. The av er age value of the ab sorbed doserate of col lected sam ples is lower than the world av er -age value. On the ba sis of lower lev els of nat u ral ra dio -ac tiv ity, the study area can be con sid ered as hav ing aless nat u ral back ground ra di a tion area. Con se quently,at pres ent, it can be con cluded that the study area poses no im me di ate en vi ron men tal threat to its in hab it ants.

AU THORS' CON TRI BU TIONS

The field work ex er cise and the lab o ra tory stud -ies were car ried out by all au thors. The manu scriptwrite up was car ried out by A. Akinmosin and proofread by M. A. Oladunjoye. Bulk of the fig ures wasdrawn by M. A. Oladunjoye while the ta bles and someof the plottings were done by F. Essien.

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Earth Sci ences Re search Jour nal, 15 (2011), 1, pp.19-26

[27] Akinmosin, A., Olabode, O. T., Bassey, C. E., Prov e -nance Study of Bi tu mi nous Sands in East ern Da ho -mey Ba sin, South west ern, Ni ge ria Based on HeavyMin eral and Quartz Va ri et ies, Ife Jour nal of Sci ence, 7(2005), 1, 2005, pp. 123-129

[28] Oladunjoye, M. A., Akinmosin, A., Ekugum, U. K., Dis tri bu tion of Ra dio ac tive El e ments of Some Rocksin South west ern Ni ge ria, RMZ- Ma te ri als and Geoen vi ron ment, 61 (2014), 4, pp. 231-240

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Receved on Sep tem ber 9, 2015Ac cepted on Jan u ary 7, 2016

A. Akinmosin, et al.: Eval u a tion of the Nat u ral Ra dio ac tiv ity Level of Ni ge rian ...88 Nu clear Tech nol ogy & Ra di a tion Pro tec tion: Year 2016, Vol. 31, No. 1, pp. 79-88

Adevale AKINMOSIN, Majkl A. OLADUNXOJE, Fa bijan ESJEN

PROCENA NIVOA PRIRODNE RADIOAKTIVNOSTI U NASLAGAMAKATRANA U BASENU ISTO^NOG DAHOMEJA U JUGOZAPADNOJ NIGERIJI

U ovom radu procewena je specifi~na aktivnost prirodnih radionuklida iz dvadesetsedam uzoraka sakupqenih u basenu u isto~nom Dahomeju u jugozapadnoj Nigeriji. Za dobijaweeksperimentalnih rezultata kori{}en je 3"´ 3" natrijum-jodidni (NaI(Tl))detektor, a primenomtehnike induktivno spregnute plazme i masene spektrometrije pra}eni su ̀ eqeni elementi. Kaostandardni izvori gama zra~ewa za kalibraciju sistema za merewe upotrebqeni su cezijum (137Cs)i kobalt (60Co), a SOIL-375, radioaktivni standardni izvor Me|unarodne agencije za atomskuenergiju primewen je za analizu i prora~un specifi~nih aktivnosti `eqenih prirodnihradionuklida. Tri radionuklida, 238U, 232Th i 40K, identifikovana su u uzorcima, a wihovespecifi~ne aktivnosti su: za 238U, od 9.88 ± 4.70 Bq/kg do 69.15 ± 12.37 Bq/kg, sa sredwom vredno{}uod 26.50 ± 7.18 Bq/kg, za 232Th, od 12.78 ± 5.16 Bq/kg do 36.86 ± 13.35 Bq/kg, sa sredwom vredno{}u od22.77 ± 4.28 Bq/kg, i za 40K,od 189.82 ± 79.51 Bq/kg do 518.77 ± 119.54 Bq/kg, sa sredwom vredno{}u od297.69 ± 16.21 Bq/kg. Rezultati su upore|eni sa sredwim vrednostima u svetu od 35 Bq/kg, 30 Bq/kg i400 Bq/kg, respektivno, koje su navedene od stane Nau~nog komiteta za efekte atomskog zra~eweUjediwenih Nacija. Sredwe vrednosti ekvivalenta radijuma, totalne apsorbovane ja~ine doze,indeksa spoqa{weg hazarda, indeksa unutra{weg hazarda i godi{weg efektivnog doznogekvivalenta su 79.90 Bq/kg, 38.50 mSv/h, 0.22 Bq/kg, 0.29 Bq/kg i 47.22 µSv, respektivno. Vode}ira~una o radiolo{kom riziku za qudsko zdravqe procewena je apsorbovana ja~ina gama zra~ewa uvazduhu u opsegu 21.7 ± 0.4 mSv/h do 155.7 ± 2.2 mSv/h, a za spoqa{wi godi{wi efektivni dozniekvivalent rezultati su bili u opsegu od 26.6 ± 0.4 mSv do 190.9 ± 2.7 mSv sa sredwom vredno{}u od79.06 ± 33.23 mSv, u pore|ewu sa efektivnom dozom u svetu od 70 mSv. Tako|e, vrednosti ekvivalenta radijuma i indeksa spoqa{weg hazarda svih uzoraka, ni`e su od prihva}ene grani~ne vrednostiod 370 Bq/kg i ispod vrednosti jedinice, respektivno. Rezultati pokazuju da je u ovom trenutkurizik od radionuklida na osnovu analiziranih uzoraka u dozvoqenim granicama.

Kqu~ne re~i: katran, radionuklid, zra~ewe, ja~ina doze, apsorbovana doza, rizik, `ivotna sredina