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Radiation Protection Dosimetry (2019), pp. 1–13 doi:10.1093/rpd/ncz043
ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING
PETROLEUM RAW MATERIALS AND THEIR WASTE
Nabil M. Hassan1,
*, N. A. Mansou1
, S. Salama2
and M. S. Seoud3
1
Department of Physics, Faculty of Science, Zagazig University, PO Box 44519, Zagazig, Egypt
2
Radiation Protection and Civil Defense, Nuclear Research Center, Egyptian Atomic Energy Authority
(EAEA), PO Box 13759, Cairo, Egypt
3
Calibration and Radiation Dosimetry Division, Radiation Protection Department, Ministry of Health,
Kuwait
*Corresponding author: nmmh1976@Zu.edu.eg
Received 18 October 2018; revised 27 February 2019; editorial decision 28 February 2019;
accepted 9 March 2019
Activity concentrations of 238
U, 232
Th and 40
K in raw and waste petroleum materials (Egypt and Kuwait) were measured
using gamma ray spectrometer. The average values of 226
Ra, 232
Th and 40
K were 21.1 ± 3.2, 7.6 ± 1.3 and 88.4 ± 8.2 Bq
kg−1
for Egyptian samples while for Kuwaiti samples, they were 25.2 ± 3.4, 6.1 ± 2.2 and 67.8 ± 6.4 Bq kg−1
, respectively.
All samples had activity less than the exemption level recommended by the International Atomic Energy Agency. Moreover,
radiological indices of radium equivalent, external, internal, alpha and gamma indices and radiation dose as well were calcu-
lated and their values were lower than the recommended regulatory limits. Thus, radiation exposure to petroleum materials
did not present a significant radiological hazard.
INTRODUCTION
Petroleum and gas, petroleum production are an
important global industry as it is the main source of
energy, but also is an important economic income
for several countries including Kuwait and Egypt.
Lately, a great deal of care has been advanced
regarding the possible effect on human health from
the ionizing radiation given off from the radio-
nuclide concentrations of 226
Ra, 232
Th and 40
K of
Naturally Occurring Radioactive Materials (NORM)
which are upheld in the petroleum and gas petroleum
products and their wastes. Particularly crude oil,
scale, sludge, contaminated water and sand(1, 2)
. The
presence of natural radionuclides of 226
Ra, 232
Th and
40
K (NORM) in petroleum products and their wastes
has been reported by several researchers(1–5)
. The
NORM amount produced depends on various para-
meters. Unambiguously, it depends on the geological
structure of the rocks of the reservoir which have
various quantities of natural radionuclides of 226
Ra,
232
Th and 40
K. The NORM amount can be also
enhanced as an effect of some industrial operations
which in such case it is known as Technologically
Enhanced NORM(6, 7)
.
The presence of natural radionuclides of NORM in
oil and gas, petroleum products and wastes can induce
external and internal radiation exposure due to gam-
ma rays, beta particles and alpha particles emitted
from 238
U, 232
Th and their radioactive daughters as
well as from 40
K. Consequently, petroleum and gas,
petroleum products and their wastes that might
sustain a high level of NORM could have the poten-
tial to be carcinogenic materials(8, 9)
. For the sake of
the safety for the workers in the petroleum industry,
the concentration of natural radionuclides of 226
Ra
(226
Ra is a radioactive daughter of 238
U), 232
Th and
40
K should be regularly measured in all types of pet-
roleum products and their wastes(10)
.
The NORM associated with the processing of
crude oil and natural gas operations is produced in
the form of scale, sludge and produced water(11)
.
Typically, the scale is formed due to the precipitation
of barium, strontium sulfates and calcium carbonate
along the inner surface of tubes and equipment. On
the other hand, the sludge formed from carbonates
and silicates is a mixture of oil, sediment and erosion
products. It is also both scale and sludge could accu-
mulate at the bottom of storage tanks, tubing and
other equipment that takes varying amounts of
226
Ra, 232
Th and 40
K. While the amount of forming
or produced water is depressed during the removal
process of the oil and gas from an underground res-
ervoir of the well, however, by time, the pressure of
well is decreased that allow the injected amount of
brine into the well to increase the force per unit area.
As a result of this pressure balancing process, the
formed water, scale and sludge would increase(12–15)
.
The present work aimed to assess the activity con-
centrations of radioactive elements of 226
Ra, 232
Th
and 40
K in the petroleum products and their wastes
of scale, sludge, water and sand around the oil
wells located in Egypt and Kuwait. The radionuclide
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concentrations in Egyptian petroleum products and
their wastes were compared with their value in
Kuwaiti petroleum products and their wastes and
with the worldwide recommended limits as well.
Moreover, the radiological hazard indices of radium
equivalent activity (Raeq), external (Hex) and internal
hazard indices (Hin), alpha and gamma indices and
annual effective dose were calculated and compared
with the worldwide safety values recommended by
the United Nations Scientific Committee on the
Effects of Atomic Radiation (UNSCEAR) and
International Atomic Energy Agency (IAEA).
MATERIALS AND METHODS
Sample Preparation
The released amount of ionizing radiation from oil
products and their wastes is a very important issue
for radiation protection point of view since it varied
from the oil well to others, depending on the rocks
of the reservoir that have various quantities of nat-
ural radionuclides of 226
Ra (238
U), 232
Th and 40
K.
Several researchers highlight the varied level of
NORM (226
Ra (238
U), 232
Th and 40
K) in oil pro-
ducts and their wastes maintained high-level natural
radionuclides. For example, Abo-Elmagd et al.(9)
,
reported that oil products and their waste from the
South Sinai governorate, Egypt maintained a high
level of NORM, Mansour et al.(13)
, reported that oil
products and their wastes of the Eastern Desert of
Egypt maintained also a high level of natural radio-
nuclides. Also, Hassan et al.(16)
, reported that a high
level of emanated radon from oil products and their
wastes of the Eastern Desert of Egypt. Therefore, it
is very important to evaluate the level NORM in oil
products and wastes in all oil wells.
In the present work, eight samples of different types
of oil, one sample of water, three samples of sludge,
one sample of scale and four samples of sand were
collected from the oil wells of Greater Burgan, South
Fuwars and Ratqa located in Kuwait, as shown in
Table 1 and Figure 1. On the other hand, four samples
of different types of oil, one sample of water, five sam-
ples of sludge, one sample of liquid gas and one sam-
ple of sand were collected from the three main oil
provinces in Egypt (Western Desert, Nile Delta and
Gulf of Suez (Ras Gharib)), as shown in Table 2 and
Figure 2. The regions that the samples were collected
from the regions where oil production is actively con-
ducted by the government of Egypt and Kuwait. The
wells mentioned in the current study are used as a
baseline to investigate the radiation levels of all
regions. The work is a continuous work for the previ-
ously published papers for other regions(9, 13, 16)
.
The solid samples were crushed into a fine powder
and then were sieved through a 1-mm mesh size to
remove the larger grain size to be more homogenous.
These solid samples, then were dried in an oven at
110°C for 24 h to ensure complete dryness from
moisture. After moisture removal, the samples were
cooled down to room temperature in a desiccator.
The prepared samples were packed into airtight plas-
tic containers, (6-cm diameter and 8-cm height)
made from polyethylene. The liquid samples were
packed into the same geometry plastic containers.
Table 1. Specific activity concentrations of 226
Ra, 232
Th and 40
K in the Kuwaiti petroleum products and wastes materials.
Sample type Location Code Activity concentrations (Bq kg−1
)
226
Ra 232
Th 40
K
Heavy eocene oil Greater Burgan (KO1) ND ND 13.6 ± 1.1
Heavy crude oil Greater Burgan (KO2) 6.8 ± 3.2 4.8 ± 1.3 81.2 ± 10.2
Heavy crude oil South Fuwars (KO3) 17.0 ± 6.4 ND 126 ± 12
Crude oil South Fuwars (kO4) ND ND 56.6 ± 16.7
Crude oil Greater Burgan (KO5) 7.1 ± 4.3 10.5 ± 5.1 89.9 ± 10.2
Crude oil Ratqa (KO6) 16.3 ± 0.5 2.2 ± 0.6 84.9 ± 1.8
Oil Ratqa (KO7) 5.8 ± 1.3 4.1 ± 2.2 49.8 ± 5.5
Plankton oil Greater Burgan (KP1) 126 ± 3 ND 81.6 ± 6.9
Plankton oil Greater Burgan (KP2) 2.8 ± 0.1 ND 59.6 ± 1.0
Water Ratqa (KWO1) 3.9 ± 2.6 ND 54.2 ± 4.6
Sludge Greater Burgan (KSL1) 94.2 ± 5.3 27.7 ± 0.6 ND
Sludge Ratqa (KSL2) 42.4 ± 11.8 6.0 ± 2.5 81.8 ± 6.8
Sludge Ratqa (KSL3) 13.1 ± 1.7 1.5 ± 1.2 54.8 ± 5.8
Sand South Fuwars (KS1) 55.3 ± 8.9 3.9 ± 3.5 183 ± 14
Sand Greater Burgan (KS2) 3.8 ± 2.1 3.2 ± 2.5 43.4 ± 4.6
Sand Ratqa (KS3) 3.0 ± 1.8 ND 49.5 ± 4.4
Sand Ratqa (KS4) 28.8 ± 2.4 5.4 ± 0.5 69.9 ± 6.2
Average 25.2 ± 3.4 6.1 ± 2.2 67.8 ± 6.4
ND is a non-detectable value.
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All containers were carefully sealed with adhesive to
prevent any possibility of escaping of radon (222
Rn)
or thoron (220
Rn)(6, 17)
and stored for 1 month in
order to achieve radioactive secular equilibrium
between 226
Ra and 222
Rn. Simultaneously, an empty
same geometry container was sealed and left in the
same period to be applied for future background
measurement.
Measurement of Radionuclide Concentrations
The natural radionuclide concentrations of 226
Ra,
232
Th and 40
K in the samples of this study were mea-
sured using an High Purity Germanium detector of
vertical closed-end coaxial manufactured by
Canberra. This detector has an accurately measured
efficiency and an energy resolution of 2.1 keV at
Figure 1. The location map of oil fields in Kuwait.
Table 2. Specific activity concentrations of 226
Ra, 232
Th and 40
K in the Egyptian Petroleum products and wastes materials
ND is a non-detectable value.
Sample type Location Code Activity concentrations (Bq kg−1
)
226
Ra 232
Th 40
K
Crude oil The Nile Delta (EO1) 14.9 ± 1.2 3.4 ± 1.4 77.3 ± 3.0
Crude oil The Nile Delta (EO2) 10.2 ± 1.9 ND 66.5 ± 10.0
Crude oil Suez (EO3) 13.4 ± 4.4 6.2 ± 2.8 91.8 ± 7.1
Crude oil Suez (EO4) 21.3 ± 5.4 ND 121 ± 15
Liquid gas The Nile Delta (ELG1) 10.8 ± 6.5 ND 143 ± 16
Water Suez (EWO1) 3.7 ± 1.7 ND 50.2 ± 4.5
Sludge The Nile Delta (ESL1) 7.6 ± 2.4 8.4 ± 2.6 52.2 ± 8.7
Sludge The Nile Delta (ESL2) 12.9 ± 1.4 3.1 ± 1.6 54.5 ± 5.4
Sludge The Nile Delta (ESL3) 20.6 ± 2.1 4.4 ± 1.9 51.9 ± 4.9
Sludge Suez (ESL4) 11.3 ± 5.1 14.8 ± 2.8 73.4 ± 14.1
Sludge Suez (ESL5) 123 ± 5 48.3 ± 0.8 241 ± 3
Sand The Nile Delta (ES1) 3.4 ± 1.2 3.1 ± 1.8 37.8 ± 6.7
Average 21.1 ± 3.2 7.6 ± 1.3 88.4 ± 8.2
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1.33 MeV of gamma ray line of 60
Co (located at the
Egyptian Atomic Energy Agency, Cairo, Egypt). In
order to reduce the effects of background measured
by the detector, it is shielded with a cylindrical lead
(Pb) of thickness 10 cm which contains an inner con-
centric cylinder of Cu with a thickness of 8 mm. The
detector is connected to a data acquisition system,
using a personal computer, which has a Multi-
Channel-Analyzer (8192 channels). The data ana-
lysis was carried out via gamma spectroscopy pro-
gram of Genie 2000 spectral analysis software. The
HPGe detector’s peak calibration and efficiency were
carried out using standard point source package (RSS-
8) of eight radionuclides of Cs-137, Ba-133, Cd-109,
Zn-65, Co-60, Co-57, Mn-54 and Na-22 supplied by
the IAEA. For bulk measurements, the 40
K in KCl
standard bulk solution was used as a normalizing fac-
tor. The bulk source was packaged in the same con-
tainer geometric as those used for samples.
The natural radionuclide concentrations of 238
U
(226
Ra), 232
Th and 40
K in each sample were detected
over a time frame of around 24 h. Since 226
Ra and
its progenies produce ~98.5% of radiological effects
of natural uranium series, the contribution of natural
238
U and the precursors of 226
Ra were ignored.
Thus, 226
Ra was considered to be the reference of the
238
U series instead of 238
U(17, 18)
. 226
Ra specific
activity was measured from the gamma rays lines at
the energies of 351.9 keV (36.6%) and 295.2 keV
(18.5%) associated with the decay 214
Pb, and at the
energies of 609.3 keV (46.1%) and 1120 keV (15%)
associated with the decay 214
Bi, as shown in
Figure 3. On the other hand, thorium (232
Th) spe-
cific activity was estimated from the gamma rays of
energies of 911.1 keV (29%) associated with the
decay of 228
Ac, 583.1 keV (84.5%) associated with
the decay of 208
Tl and 238.6 keV (43.6%) associated
with the decay of 212
Pb as shown in Figure 3.
Finally, potassium (40
K) specific activity was esti-
mated from the gamma ray of the energy of
1460.9 keV (10.67%) associated with the decay 40
K
itself(19, 20)
. The self-attenuation and coincidence
summing effects were ignored in this study. The
activity concentrations of natural radionuclides, A,
(Bq kg−1
) are calculated from Eq (1)(19, 21)
.
ρ ε
= ( )
A
C
wt
1
i i
where C is the net count above the background, pi is the
absolute emission probability of each gamma ray (men-
tioned in brackets after gamma rays energies), w is the
net dry sample weight (kg), The samples’ weights were
ranged between 350 and 500 g, t is the measurement
time and εi is the absolute efficiency of the detector is
associated with each gamma rays energy value.
Figure 2. The location map of oil fields in Egypt.
4
N. M. HASSAN ET AL.
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RESULTS AND DISCUSSION
The goal of this work is to measure the activity con-
centrations of 226
Ra, 232
Th and 40
K in some ran-
domly selected materials of different types of oil,
scale, sludge, water and sand from oil wells located in
both Egypt and Kuwait. The results of this study
are summarized in Tables 1 and 2. The activity con-
centrations of 226
Ra, 232
Th and 40
K in petroleum
products and their wastes were varied from ND (non-
detectable value, KO4) to 123 ± 3 (KP1) Bq kg−1
with a
mean value of 25.2 ± 3.4 Bq kg−1
for 226
Ra, ND (KO1)
to 27.7 ± 0.6 (KSL1) Bq kg−1
with a mean value
of 6.1 ± 2.2 Bq kg−1
for 232
Th and ND (KSL1)
to 183.39 ± 13.73 (KS1) Bq kg−1
with a mean value
of 67.8 ± 6.4 Bq kg−1
for 40
K, in the selected samples
from Kuwait, as shown in Figures 4–6 and Tables 1.
On the other hand, the Egyptian samples were varied
from 3.4 ± 1.2 (ES1) to 123 ± 5 (ESL5) Bq kg−1
with a
mean value of 21.1 ± 3.2 Bq kg−1
for 226
Ra, ND
(EO2) to 48.3 ± 0.8 (ESL5) Bq kg−1
with a mean value
of 7.6 ± 1.3 Bq kg−1
for 232
Th and 37.8 ± 6.7
(ES1) to 241 ± 3 (ESL5) Bq kg−1
with a mean value
of 88.4 ± 8.2 Bq kg−1
for 40
K, respectively, as shown
in Figures 4–6 and Tables 2. The maximum activity
levels for all measured radionuclides in selected samples
were 126 ± 3 Bq kg−1
(KP1) of 226
Ra, 27.7 ± 0.6 (KSL1)
Bq kg−1
of 232
Th and 183 ± 14 (ESL5) Bq kg−1
of 40
K for Kuwaiti samples while for Egyptian sam-
ples, they were 123 ± 5 Bq kg−1
(ESL5) of 226
Ra,
48.3 ± 0.8 (ESL5) Bq kg−1
of 232
Th and 241 ± 3
(ESL5) Bq kg−1
of 40
K, respectively. The radionuclide
concentration of Egyptian and Kuwaiti petroleum
products and their wastes were comparable with
almost the same average values. However, specific
activities of 226
Ra, 232
Th and 40
K in sludge samples
were higher than their values in crude oil, water and
sand for Egyptian samples. Similarly, the Kuwaiti
radionuclide concentration of 226
Ra in the plankton
oil refinery of greater Burgan oil well was higher
than its value in all other samples, 232
Th in sludge of
greater Burgan oil well was higher than its value in
all other samples and 40
K in sand of south Fuwars
was higher than its value in all other samples. The
obtained results indicate that the specific activity
concentrations in all selected material from Egypt
and Kuwait were comparable or less than the
global median specific activity concentrations in
soil of 35, 30 and 400 Bq kg−1
for 226
Ra, 232
Th and
40
K, respectively, reported by UNSCEAR(21, 22)
.
Moreover, the radionuclide concentrations in the
studied materials were much lower than the exemp-
tion level for NORM of 1 Bq g−1
for uranium and
thorium and 10 Bq g−1
for 40
K recommended by the
IAEA basic safety standards(23, 24)
. Thus, there is no
radiological risk for worker or public dealing with
those materials so that the radiation exposure from
the selected material can be ignored. The values of
natural radionuclides in the present study were
compared with their values in the same material
previously described in the literature, as pictured in
Table 3.
In order to compute the radiation hazards asso-
ciated with materials maintained various levels of
226
Ra, 232
Th and 40
K in a single quantity, the radium
equivalent activity (Raeq) has been introduced by
UNSCEAR(21, 22, 34)
, Eq. 2.
= + + ( )
Ra A A A
1.43 0.077 2
eq Ra Th K
where, ARa, ATh and AK are activity concentrations
of 226
Ra, 232
Th and 40
K, respectively, in Bq kg−1
.
The radium equivalent index was calculated based
Figure 3. Typical gamma ray spectrum of natural radionuclides of Egyptian (ESL5) and Kuwait (KSL1) sludge waste
materials.
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on the assumption that 370 Bq kg−1
of 226
Ra,
259 Bq kg−1
of 232
Th and 4810 Bq kg−1
of 40
K produce
the same equivalent dose of gamma ray. For the
sake of safety, Raeq activity concentration of material
should be <370 Bq kg−1
to keep gamma ray dose below
1.5 mSv y−1(35–37)
. Radium equivalent concentration
in Egyptian petroleum products and wastes was ranged
from 7.5 ± 2.0 Bq kg−1
(EWO1) to 210 ± 7 Bq kg−1
(ESL5) with a mean value 38.8 ± 5.8 Bq kg−1
while for
Kuwaiti samples, it was ranged from 1.7 ± 1.0 Bq kg−1
(KO1) to 134 ± 6 Bq kg−1
(KSL1) with a mean value
of 34.4 ± 5.6 Bq kg−1
, as shown in Figure 7, and
Tables 4 and 5. The Radium equivalent of all investi-
gated petroleum products and wastes was less than the
recommended limit of 370 Bq kg−1
which implies that
these materials have no radiological hazards and can be
safely used in various industries.
Radiation hazard mainly comes from external
gamma rays emitted from natural radionuclides
of 226
Ra, 232
Th and 40
K. The external hazard of gamma
0
20
40
60
80
100
120
EO1 EO2 EO3 EO4 __ __ __ __ __ ELG1 EWO1 ESL1 ESL2 ESL3 ESL4 ESL5 ES1 __ __ __
KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4
Activity
Conc.
Bq/Kg
Sample Code
Ra-226 Activity
Egypt Kuwait
Figure 4. Specific activity concentrations of Ra-226 in Egyptian and Kuwaiti samples.
0
5
10
15
20
25
30
EO1 EO2 EO3 EO4 __ __ __
__ __ EWO1
EWG1 ESL2
ESL1 ESL3 ESL4 ESL5 ES1 __
__ __
KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4
Activity
Conc.
Bq/Kg
Sample Code
Th-232 Activity
Egypt Kuwait
Figure 5. Specific activity concentrations of Th-232 in Egyptian and Kuwaiti samples.
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rays can be expressed by the external hazard index
(Hex) which was determined from Eq. (3)(34)
;
= + + ( )
H
A A A
370 259 4810
3
ex
Ra Th K
where, ARa, ATh and AK are the activities of 226
Ra,
232
Th and 40
K, respectively, in Bq kg−1
. Normally,
the external hazard index of a material should be
less than unity in order to limit the external gamma
radiation dose to be <1.5 mSv y−1
. In this study, the
average calculated values of external hazard index
for Egyptian and Kuwaiti petroleum products and
wastes were of 0.11 ± 0.02 and 0.09 ± 0.02 (Tables 4
and 5). The external hazard index of all studied sam-
ples was less than the recommended limit which
implies the external radiation hazard could be
ignored.
In addition to the external hazard, another factor
should be taken into account because of radon, and
its progenies as they are hazardous to the respiratory
organs is called an internal hazard index. It is caused
by radionuclides of 226
Ra, 232
Th and 40
K in add-
itional to radon and its progenies of 218
Po, 214
Pb,
210
Pb and 210
Bi. The internal hazard index (Hin) can
be defined as(34)
;
= + + ( )
H
A A A
185 259 4810
4
in
Ra Th K
For the safe use of a material, Hin should be less
than unity in order to ignore the hazards of radon
and its products on the respiratory organs. The
average value of the internal hazard index was 0.16
± 0.03 (Table 5) for all of the Egyptian and Kuwaiti
samples, which are lower than the recommended
limit. Thus, the use of Egyptian and Kuwaiti materi-
als has insignificant radiation hazards.
Normally, the petroleum products and wastes,
maintained natural radionuclides; hence they could
be a possible source of radiation exposure for the
public and workers. Thus, regular assessment of their
radiation exposure would be beneficial for the public
and workers health and safety. Radiation exposure is
mainly due to gamma radiation emitted from those
materials. The absorbed dose rate (D) due to gamma
rays in the air at 1 m of air above the selected materi-
als which maintains a uniform distribution of nat-
ural radionuclides of 226
Ra, 232
Th and 40
K, can be
calculated from the following equation(21)
.
( ) = + +
( )
−
D nGy h A A A
0.462 0.621 0.042
5
Ra Th K
1
The absorbed dose rate was calculated for the
samples as shown in Tables 6 and 7. The radiation
absorbed dose rate was varied from 3.8 ± 1.0 nGy
h−1
(EWO1) to 96.4 ± 3.2 nGy h−1
(ESL5) with a
mean value of 18.1 ± 2.7 nGy h−1
for Egyptian pet-
roleum products and wastes. For Kuwaiti samples,
the absorbed dose varied from 0.87 ± 0.48 nGy h−1
(KO1) to 61.2 ± 1.6 nGy h−1
(KP1) with a mean
value of 16.1 ± 2.6 nGy h−1
. All the selected
Egyptian and Kuwaiti materials had an absorbed
radiation dose value lower than the recommended
value by UNSCEAR(21)
, of 59 nGy h−1
except two
0
50
100
150
200
250
EO1 EO2 EO3 __
__ __ __
__ __ EWO1
ELG1 ESL2 ESL3
ESL1 ESL4 ESL5 ES1 __
__ __
KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4
Activity
Conc.
Bq/Kg
Sample Code
K-40 Activity
Egypt Kuwait
Figure 6. Specific activity concentrations of K-40 in Egyptian and Kuwaiti samples.
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samples of KP1 (61.2 ± 1.6) nGy and KSL1 (60.5 ±
2.8) nGy from Kuwaiti samples and one sample of
ESL5 (96.4 ± 3.2) nGy from Egyptian samples, as
given in Tables 6 and 7. Thus, except for three sam-
ples of KP1, KSL1 and ESL5, all the Egyptian and
Kuwaiti samples have no pose of radiation exposure.
Furthermore, the annual effective dose (E) from
gamma rays emitted from 226
Ra, 232
Th and 40
k in
the samples was calculated from Eq. (6)(22, 34)
.
= ( × ( ) × × ( )
( )
− −
E D nGy h h y O C Sv Gy
8760 /
6
1 1
where, O is the occupancy factor and C is the
absorbed to the effective dose conversion factor of
0.7 Sv/Gy(38)
. The annual effective dose due to gam-
ma rays emitted from the radionuclides of 226
Ra,
232
Th and 40
K in the selected materials was calcu-
lated within two scenarios. The first scenario (effect-
ive and actual scenario) is that workers in fields (well
locations) and factories are exposed to petroleum
products/wastes maintained radionuclides of 226
Ra,
232
Th and 40
K, for 1753 hy−1
(outdoor occupancy
factor equals ~0.2, 1753 hy−1
= 0.2 × 8760 hy−1
),
while the other scenario is that a certain population
in houses is exposed for 7012 hy−1
(outdoor occu-
pancy factor equals ~0.8, 7012 hy−1
= 0.2 × 8760 h
y−1
). This scenario is not effective in the present
study, but it was used to show the possible highest
radiological risk.
In the first scenario (effective and actual scenario),
the annual effective dose from gamma rays emitted
by 226
Ra, 232
Th and 40
k in the samples varied from
4.6 ± 1.2 μSv y−1
(EWO1) to 118 ± 4 μSv y−1
(ESL5)
with a mean value of 22.2 ± 3.3 μSv y−1
for the
Egyptian samples. On the other side, the Kuwaiti
samples varied from 1.1 ± 0.6 μSv y−1
(KO1) to 75.0
± 2.0 μSv y−1
(KP1) with a mean value of 19.8 ± 3.1
μSv y−1
, as summarized in Tables 6 and 7 and
Figure 8. Whereas in the second scenario, the annual
effective dose ranged from 18.4 ± 4.8 μSv y−1
(EWO1) to 472.8 ± 15.6 μSv y−1
(ESL5) for the
Egyptian samples and from 4.4 ± 2.4 μSv y−1
(KO1)
to 300 ± 7.6 μSv y−1
(KP1) for the Kuwaiti samples,
as seen in Tables 6 and 7. The calculated annual
Table 3. Comparison of activity concentrations of 226
Ra, 232
Th and 40
K in petroleum products and wastes materials of
various countries.
Sample type Country Activity concentrations (Bq kg−1
) Reference
226
Ra 232
Th 40
K
Scale Brazil 18–22 19.2–21.9 417–432 (25)
Scale Saudi Arabia 1284–3613 12–27 — (12)
Scale Middle East 12–245.8 1.7–40.1 484.8–9850 (3)
Scale Egypt 9140–285 823 427–34 339 51–1031 (14)
Scale Syria 0.3–1520 0.6–868 — (1)
Scale Tunisia 59 ± 7 82 ± 12 64 ± 10 (26)
Sludge Nigeria 54.5–94.2 33.3–71.2 462.1–712.4 (2)
Sludge Egypt 5.5–1785.8 < LD–885 < LD–125.5 (11)
Sludge Brazil < LLD–413 400 < LLD–117 900 417 000–432 000 (15)
Sludge UK 1.70–8.20 0.03–0.51 — (20)
Sludge Malaysia 123–153 37–42 — (27)
Sludge Iraq 1.5 0.2 2.5 (28)
Sludge Turkey < 1–809.2 < 0.8–302.5 < 3.8–623 (29)
Sludge Egypt 18.032 13.257 1261 (30)
Sludge Albania 18–20 21–22 175–348 (31)
Oil Kuwait 1.8–2.5 1.6–1.8 16.1–27.1 (32)
Heavy oil Syria 77–135 24–42 — (1)
Crude oil Ghana < 0.12–10.14 < 0.11–12.45 < 0.15–34.39 (4)
Crude oil Saudi Arabia < LD 0.05–0.3 0.2–1.8 (5)
Crude oil Turkey < 1– < 5.6 < 1–4.8 < 1– < 11 (29)
Water Egypt 26.5–217 < LD–93 < LD–248.7 (11)
Water Iran 0.1–30 — — (33)
Oil Kuwait ND–17.0 ND–10.5 13.6–126 Present study
Oil Egypt 10.2–21.3 3.4–6.2 66.5–121 Present study
Sludge Kuwait Sludge 1.5–28 ND–54.8 Present study
Sludge Egypt Sludge 3.1–48.3 52–241 Present study
Sand Kuwait 3.8–55.3 3.2–5.4 43–183 Present study
Sand Egypt 3.4 ± 1.2 3.1 ± 1.9 37.8 ± 6.7 Present study
8
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effective dose with both scenarios was less than the
worldwide average annual effective dose of 480 μSv
y−1(22)
. As well, it is much lower than 1 mSv for
the public or 20 mSv for workers recommended by
the International Commission on Radiological
Protection (ICRP-103)(35)
.
The gamma ray radiation hazards associated with
the natural radionuclides in materials can be evalu-
ated by means of the radioactivity level index called
gamma index (Iγ). According to the European
Commission guidelines, Iγ should be <1 for a
gamma radiation dose of 1 mSv y−1(23)
. The gamma
ray index (Iγ) can be calculated from Eq. (7).(39)
= + + ( )
γ
I
C C C
300 200 3000
7
Ra Th K
The Iγ of the Egyptian samples varied from 0.03
± 0.01 for (EWO1) to 0.73 ± 0.02 for (ESL5) with
a mean value of 0.14 ± 0.02. For the Kuwaiti sam-
ples, it varied from 0.007 ± 0.004 for (KO1) to
0
20
40
60
80
100
EO1 EO2 EO3 EO4 __ __ __
__ __ EWO1
ELG1 ESL2 ESL3
ESL1 ESL4 ESL5 ES1 __ __
__
KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4
Activity
Conc.
Bq/Kg
Sample Code
Specific activities concentrations of Radium Equivalent (Raeq)
Egypt Kuwait
Figure 7. Radium equivalent activity concentrations of Egyptian and Kuwaiti samples.
Table 4. Radium equivalent, external and internal hazard indices of Kuwaiti samples.
Sample code Radium equivalent (Raeq) (Bq Kg−1
) External index (Hex) Internal index (Hin)
(KO1) 1.7 ± 1.0 0.005 ± 0.003 0.006 ± 0.005
(KO2) 14.8 ± 10.9 0.040 ± 0.029 0.058 ± 0.038
(KO3) 26.7 ± 7.3 0.072 ± 0.020 0.118 ± 0.037
(kO4) 4.4 ± 1.3 0.012 ± 0.003 0.012 ± 0.003
(KO5) 29.0 ± 12.4 0.078 ± 0.034 0.098 ± 0.045
(KO6) 26.0 ± 1.4 0.070 ± 0.004 0.114 ± 0.005
(KO7) 15.5 ± 4.8 0.042 ± 0.013 0.058 ± 0.017
(KP1) 132 ± 3 0.356 ± 0.009 0.695 ± 0.017
(KP2) 8.7 ± 0.9 0.024 ± 0.002 0.031 ± 0.003
(KWO1) 8.1 ± 3.0 0.022 ± 0.008 0.032 ± 0.015
(KSL1) 134 ± 6 0.362 ± 0.017 0.616 ± 0.031
(KSL2) 57.2 ± 15.9 0.155 ± 0.043 0.269 ± 0.075
(KSL3) 19.5 ± 3.8 0.053 ± 0.010 0.088 ± 0.015
(KS1) 75.0 ± 14.9 0.203 ± 0.040 0.352 ± 0.064
(KS2) 11.8 ± 6.0 0.032 ± 0.016 0.042 ± 0.022
(KS3) 6.8 ± 2.1 0.018 ± 0.006 0.026 ± 0.010
(KS4) 41.8 ± 3.6 0.113 ± 0.010 0.191 ± 0.016
9
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Table 5. Radium equivalent, external and internal Hazard Indexes of Egyptian samples.
Sample code Radium equivalent (Raeq) (Bq Kg−1
) External index (Hex) Internal index (Hin)
(EO1) 25.8 ± 3.5 0.070 ± 0.009 0.110 ± 0.013
(EO2) 15.3 ± 2.7 0.041 ± 0.007 0.069 ± 0.012
(EO3) 29.4 ± 9.0 0.079 ± 0.024 0.116 ± 0.036
(EO4) 30.6 ± 6.6 0.083 ± 0.018 0.140 ± 0.032
(ELG1) 21.8 ± 7.7 0.059 ± 0.021 0.088 ± 0.038
(EWO1) 7.5 ± 2.0 0.020 ± 0.005 0.030 ± 0.010
(ESL1) 23.6 ± 6.8 0.064 ± 0.018 0.084 ± 0.025
(ESL2) 21.5 ± 4.1 0.058 ± 0.011 0.093 ± 0.015
(ESL3) 30.9 ± 5.3 0.084 ± 0.014 0.139 ± 0.020
(ESL4) 38.2 ± 10.2 0.103 ± 0.028 0.134 ± 0.041
(ESL5) 210 ± 7 0.568 ± 0.019 0.899 ± 0.033
(ES1) 10.7 ± 4.4 0.029 ± 0.012 0.038 ± 0.015
Table 7. Absorbed dose rate and effective dose, gamma and alpha indices of Egyptian samples.
Sample code Absorbed dose rate (nGy h−1
) Effective dose (μSv y−1
) Gamma index (Iγ) Alpha index (Iα)
Outdoor indoor
(EO1) 12.2 ± 1.6 15.0 ± 1.9 60.0 ± 7.6 0.093 ± 0.012 0.074 ± 0.006
(EO2) 7.5 ± 1.3 9.2 ± 1.6 36.8 ± 6.4 0.056 ± 0.010 0.051 ± 0.010
(EO3) 13.9 ± 4.1 17.0 ± 5.0 68.0 ± 20.0 0.106 ± 0.031 0.067 ± 0.022
(EO4) 14.9 ± 3.1 18.3 ± 3.9 73.2 ± 15.6 0.111 ± 0.023 0.106 ± 0.027
(ELG1) 11.0 ± 3.7 13.5 ± 4.5 54.0 ± 18.0 0.084 ± 0.027 0.054 ± 0.032
(EWO1) 3.8 ± 1.0 4.6 ± 1.2 18.4 ± 4.8 0.029 ± 0.007 0.018 ± 0.008
(ESL1) 10.9 ± 3.1 13.4 ± 3.8 53.6 ± 15.2 0.085 ± 0.024 0.038 ± 0.012
(ESL2) 10.1 ± 1.9 12.4 ± 2.3 49.6 ± 9.2 0.077 ± 0.014 0.065 ± 0.007
(ESL3) 14.4 ± 2.4 17.7 ± 2.9 70.8 ± 11.6 0.108 ± 0.018 0.103 ± 0.010
(ESL4) 17.5 ± 4.7 21.4 ± 5.7 85.6 ± 22.8 0.136 ± 0.036 0.056 ± 0.026
(ESL5) 96.4 ± 3.2 118.2 ± 3.9 472.8 ± 15.6 0.730 ± 0.023 0.613 ± 0.027
(ES1) 5.0 ± 2.0 6.2 ± 2.4 24.8 ± 9.6 0.039 ± 0.016 0.017 ± 0.006
Table 6. Absorbed dose rate and effective dose, gamma and alpha Indices of Kuwaiti samples.
Sample code Absorbed dose (nGy h−1
) Effective dose (μSv y−1
) Gamma index (Iγ) Alpha index (Iα)
Outdoor Indoor
(KO1) 0.9 ± 0.5 1.1 ± 0.6 4.4 ± 2.4 0.0067 ± 0.0035 0.003 ± 0.005
(KO2) 7.3 ± 4.9 9.0 ± 6.0 36.0 ± 24.0 0.056 ± 0.038 0.034 ± 0.016
(KO3) 13.1 ± 3.4 16.1 ± 4.2 64.4 ± 16.8 0.0987 ± 0.0250 0.085 ± 0.032
(kO4) 2.4 ± 0.7 2.9 ± 0.6 11.6 ± 2.4 0.019 ± 0.006 0.000 ± 0.000
(KO5) 13.6 ± 5.6 16.6 ± 6.9 66.4 ± 27.6 0.106 ± 0.043 0.036 ± 0.021
(KO6) 12.4 ± 0.6 15.2 ± 0.8 60.8 ± 3.2 0.094 ± 0.005 0.082 ± 0.002
(KO7) 7.3 ± 2.2 9.0 ± 2.7 36.0 ± 10.8 0.056 ± 0.017 0.029 ± 0.006
(KP1) 61.2 ± 1.6 75.0 ± 1.9 300.0 ± 7.6 0.446 ± 0.012 0.628 ± 0.014
(KP2) 4.4 ± 0.4 5.4 ± 0.5 21.6 ± 2.0 0.034 ± 0.003 0.014 ± 0.001
(KWO1) 4.1 ± 1.4 5.0 ± 1.7 20.0 ± 6.8 0.031 ± 0.010 0.020 ± 0.013
(KSL1) 60.5 ± 2.8 74.3 ± 3.5 297.2 ± 14.0 0.453 ± 0.021 0.471 ± 0.026
(KSL2) 26.6 ± 7.3 32.7 ± 8.9 130.8 ± 35.6 0.198 ± 0.054 0.212 ± 0.059
(KSL3) 9.3 ± 1.8 11.4 ± 2.2 45.6 ± 8.8 0.069 ± 0.014 0.065 ± 0.009
(KS1) 35.6 ± 6.8 43.6 ± 8.4 174.4 ± 33.6 0.265 ± 0.052 0.276 ± 0.044
(KS2) 5.6 ± 2.7 6.8 ± 3.3 27.2 ± 13.2 0.043 ± 0.021 0.019 ± 0.010
(KS3) 3.5 ± 1.0 4.3 ± 1.2 17.2 ± 4.8 0.026 ± 0.007 0.015 ± 0.009
(KS4) 19.5 ± 1.7 23.9 ± 2.1 95.6 ± 8.4 0.146 ± 0.013 0.144 ± 0.012
10
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0.453 ± 0.021 for (KSL1) with a mean value of
0.121 ± 0.019, as can be seen in Tables 6 and 7. All
the measured samples had a radioactivity level
index <1 so that these samples can be used without
special precautions(39)
.
Alpha radiation due to the released radon from
samples is called alpha index (Iα) which can be com-
puted from Eq. (8),(39)
. The alpha index should be
less than unity to reflect a radium concentration
value <200 Bq kg−1
(the upper recommended value)
which leads to a maximum released radon concen-
tration <200 Bq m-3
.
= ( )
∝
I
A
200
8
Ra
Alpha index of the Egyptian samples varied from
0.017 ± 0.006 (ES1) to 0.613 ± 0.027 (ESL5) with a
mean value of 0.105 ± 0.016. For Kuwaiti samples,
it varied from the ND value (KO4) to 0.628 ± 0.014
(KP1) with a mean value of 0.119 ± 0.016, as seen in
Tables 6 and 7. Accordingly, the values of Alpha
index for Egyptian and Kuwaiti petroleum products
and wastes were much lower than unity which
implies that all the study materials do not have radi-
ation hazard for a worker and the general public.
CONCLUSION
Natural radioactivity concentrations of 226
Ra, 232
Th
and 40
K, in petroleum products and wastes of crude
oil, water, sludge and contaminated sand collected
various petroleum well fields located Egypt and
Kuwait, were ranged from 3.35 ± 1.22 to 122.55 ±
5.42 Bq kg−1
for 226
Ra, ND value to 48.28 ±
0.82 Bq kg−1
for 232
Th and 37.83 ± 6.70 to 240.59 ±
3.42 Bq kg−1
for 40
K Egyptian samples and from
ND to 125.52 ± 2.82 Bq kg−1
for 226
Ra, ND to 27.65 ±
0.63 Bq kg−1
for 232
Th and ND to 183.39 ±
13.73 Bq kg−1
for 40
K, for Kuwaiti samples. The
radionuclides concentrations of Egyptian and Kuwaiti
petroleum products and wastes were less than the
recommended limits of UNSCEAR and ICRP for
earth’s crust and the recommended values of IAEA as
well. Moreover, the radiological hazard indexes, of
radium equivalent activities (Raeq), external and
internal indexes, gamma and alpha indexes and
annual effective doses of the Egyptian and Kuwaiti
petroleum products and wastes were less than
the recommended values of 370 Bq kg−1
, 1, 1 and
480 μSv y−1
. The absorbed dose of all the studied
samples was less than the recommended value of
59 nGy h−1
except only three samples of KP1,
KEL1 and ESL5. Thus, we deduce that the selected
petroleum products and wastes (except KP1, KSL1
and ESL5) have not caused significant radiological
risk on the worker or the public but might need
monitoring for long-term effective evaluation.
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__ __ EWO1
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ESL1 ESL4 ESL5 ES1 __ __
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H. and Ahmed, N. Radiometric analysis of Hazara
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13
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ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING PETROLEUM RAW MATERIALS AND THEIR WASTE

  • 1. Radiation Protection Dosimetry (2019), pp. 1–13 doi:10.1093/rpd/ncz043 ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING PETROLEUM RAW MATERIALS AND THEIR WASTE Nabil M. Hassan1, *, N. A. Mansou1 , S. Salama2 and M. S. Seoud3 1 Department of Physics, Faculty of Science, Zagazig University, PO Box 44519, Zagazig, Egypt 2 Radiation Protection and Civil Defense, Nuclear Research Center, Egyptian Atomic Energy Authority (EAEA), PO Box 13759, Cairo, Egypt 3 Calibration and Radiation Dosimetry Division, Radiation Protection Department, Ministry of Health, Kuwait *Corresponding author: nmmh1976@Zu.edu.eg Received 18 October 2018; revised 27 February 2019; editorial decision 28 February 2019; accepted 9 March 2019 Activity concentrations of 238 U, 232 Th and 40 K in raw and waste petroleum materials (Egypt and Kuwait) were measured using gamma ray spectrometer. The average values of 226 Ra, 232 Th and 40 K were 21.1 ± 3.2, 7.6 ± 1.3 and 88.4 ± 8.2 Bq kg−1 for Egyptian samples while for Kuwaiti samples, they were 25.2 ± 3.4, 6.1 ± 2.2 and 67.8 ± 6.4 Bq kg−1 , respectively. All samples had activity less than the exemption level recommended by the International Atomic Energy Agency. Moreover, radiological indices of radium equivalent, external, internal, alpha and gamma indices and radiation dose as well were calcu- lated and their values were lower than the recommended regulatory limits. Thus, radiation exposure to petroleum materials did not present a significant radiological hazard. INTRODUCTION Petroleum and gas, petroleum production are an important global industry as it is the main source of energy, but also is an important economic income for several countries including Kuwait and Egypt. Lately, a great deal of care has been advanced regarding the possible effect on human health from the ionizing radiation given off from the radio- nuclide concentrations of 226 Ra, 232 Th and 40 K of Naturally Occurring Radioactive Materials (NORM) which are upheld in the petroleum and gas petroleum products and their wastes. Particularly crude oil, scale, sludge, contaminated water and sand(1, 2) . The presence of natural radionuclides of 226 Ra, 232 Th and 40 K (NORM) in petroleum products and their wastes has been reported by several researchers(1–5) . The NORM amount produced depends on various para- meters. Unambiguously, it depends on the geological structure of the rocks of the reservoir which have various quantities of natural radionuclides of 226 Ra, 232 Th and 40 K. The NORM amount can be also enhanced as an effect of some industrial operations which in such case it is known as Technologically Enhanced NORM(6, 7) . The presence of natural radionuclides of NORM in oil and gas, petroleum products and wastes can induce external and internal radiation exposure due to gam- ma rays, beta particles and alpha particles emitted from 238 U, 232 Th and their radioactive daughters as well as from 40 K. Consequently, petroleum and gas, petroleum products and their wastes that might sustain a high level of NORM could have the poten- tial to be carcinogenic materials(8, 9) . For the sake of the safety for the workers in the petroleum industry, the concentration of natural radionuclides of 226 Ra (226 Ra is a radioactive daughter of 238 U), 232 Th and 40 K should be regularly measured in all types of pet- roleum products and their wastes(10) . The NORM associated with the processing of crude oil and natural gas operations is produced in the form of scale, sludge and produced water(11) . Typically, the scale is formed due to the precipitation of barium, strontium sulfates and calcium carbonate along the inner surface of tubes and equipment. On the other hand, the sludge formed from carbonates and silicates is a mixture of oil, sediment and erosion products. It is also both scale and sludge could accu- mulate at the bottom of storage tanks, tubing and other equipment that takes varying amounts of 226 Ra, 232 Th and 40 K. While the amount of forming or produced water is depressed during the removal process of the oil and gas from an underground res- ervoir of the well, however, by time, the pressure of well is decreased that allow the injected amount of brine into the well to increase the force per unit area. As a result of this pressure balancing process, the formed water, scale and sludge would increase(12–15) . The present work aimed to assess the activity con- centrations of radioactive elements of 226 Ra, 232 Th and 40 K in the petroleum products and their wastes of scale, sludge, water and sand around the oil wells located in Egypt and Kuwait. The radionuclide © The Author(s) 2019. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 2. concentrations in Egyptian petroleum products and their wastes were compared with their value in Kuwaiti petroleum products and their wastes and with the worldwide recommended limits as well. Moreover, the radiological hazard indices of radium equivalent activity (Raeq), external (Hex) and internal hazard indices (Hin), alpha and gamma indices and annual effective dose were calculated and compared with the worldwide safety values recommended by the United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) and International Atomic Energy Agency (IAEA). MATERIALS AND METHODS Sample Preparation The released amount of ionizing radiation from oil products and their wastes is a very important issue for radiation protection point of view since it varied from the oil well to others, depending on the rocks of the reservoir that have various quantities of nat- ural radionuclides of 226 Ra (238 U), 232 Th and 40 K. Several researchers highlight the varied level of NORM (226 Ra (238 U), 232 Th and 40 K) in oil pro- ducts and their wastes maintained high-level natural radionuclides. For example, Abo-Elmagd et al.(9) , reported that oil products and their waste from the South Sinai governorate, Egypt maintained a high level of NORM, Mansour et al.(13) , reported that oil products and their wastes of the Eastern Desert of Egypt maintained also a high level of natural radio- nuclides. Also, Hassan et al.(16) , reported that a high level of emanated radon from oil products and their wastes of the Eastern Desert of Egypt. Therefore, it is very important to evaluate the level NORM in oil products and wastes in all oil wells. In the present work, eight samples of different types of oil, one sample of water, three samples of sludge, one sample of scale and four samples of sand were collected from the oil wells of Greater Burgan, South Fuwars and Ratqa located in Kuwait, as shown in Table 1 and Figure 1. On the other hand, four samples of different types of oil, one sample of water, five sam- ples of sludge, one sample of liquid gas and one sam- ple of sand were collected from the three main oil provinces in Egypt (Western Desert, Nile Delta and Gulf of Suez (Ras Gharib)), as shown in Table 2 and Figure 2. The regions that the samples were collected from the regions where oil production is actively con- ducted by the government of Egypt and Kuwait. The wells mentioned in the current study are used as a baseline to investigate the radiation levels of all regions. The work is a continuous work for the previ- ously published papers for other regions(9, 13, 16) . The solid samples were crushed into a fine powder and then were sieved through a 1-mm mesh size to remove the larger grain size to be more homogenous. These solid samples, then were dried in an oven at 110°C for 24 h to ensure complete dryness from moisture. After moisture removal, the samples were cooled down to room temperature in a desiccator. The prepared samples were packed into airtight plas- tic containers, (6-cm diameter and 8-cm height) made from polyethylene. The liquid samples were packed into the same geometry plastic containers. Table 1. Specific activity concentrations of 226 Ra, 232 Th and 40 K in the Kuwaiti petroleum products and wastes materials. Sample type Location Code Activity concentrations (Bq kg−1 ) 226 Ra 232 Th 40 K Heavy eocene oil Greater Burgan (KO1) ND ND 13.6 ± 1.1 Heavy crude oil Greater Burgan (KO2) 6.8 ± 3.2 4.8 ± 1.3 81.2 ± 10.2 Heavy crude oil South Fuwars (KO3) 17.0 ± 6.4 ND 126 ± 12 Crude oil South Fuwars (kO4) ND ND 56.6 ± 16.7 Crude oil Greater Burgan (KO5) 7.1 ± 4.3 10.5 ± 5.1 89.9 ± 10.2 Crude oil Ratqa (KO6) 16.3 ± 0.5 2.2 ± 0.6 84.9 ± 1.8 Oil Ratqa (KO7) 5.8 ± 1.3 4.1 ± 2.2 49.8 ± 5.5 Plankton oil Greater Burgan (KP1) 126 ± 3 ND 81.6 ± 6.9 Plankton oil Greater Burgan (KP2) 2.8 ± 0.1 ND 59.6 ± 1.0 Water Ratqa (KWO1) 3.9 ± 2.6 ND 54.2 ± 4.6 Sludge Greater Burgan (KSL1) 94.2 ± 5.3 27.7 ± 0.6 ND Sludge Ratqa (KSL2) 42.4 ± 11.8 6.0 ± 2.5 81.8 ± 6.8 Sludge Ratqa (KSL3) 13.1 ± 1.7 1.5 ± 1.2 54.8 ± 5.8 Sand South Fuwars (KS1) 55.3 ± 8.9 3.9 ± 3.5 183 ± 14 Sand Greater Burgan (KS2) 3.8 ± 2.1 3.2 ± 2.5 43.4 ± 4.6 Sand Ratqa (KS3) 3.0 ± 1.8 ND 49.5 ± 4.4 Sand Ratqa (KS4) 28.8 ± 2.4 5.4 ± 0.5 69.9 ± 6.2 Average 25.2 ± 3.4 6.1 ± 2.2 67.8 ± 6.4 ND is a non-detectable value. 2 N. M. HASSAN ET AL. Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 3. All containers were carefully sealed with adhesive to prevent any possibility of escaping of radon (222 Rn) or thoron (220 Rn)(6, 17) and stored for 1 month in order to achieve radioactive secular equilibrium between 226 Ra and 222 Rn. Simultaneously, an empty same geometry container was sealed and left in the same period to be applied for future background measurement. Measurement of Radionuclide Concentrations The natural radionuclide concentrations of 226 Ra, 232 Th and 40 K in the samples of this study were mea- sured using an High Purity Germanium detector of vertical closed-end coaxial manufactured by Canberra. This detector has an accurately measured efficiency and an energy resolution of 2.1 keV at Figure 1. The location map of oil fields in Kuwait. Table 2. Specific activity concentrations of 226 Ra, 232 Th and 40 K in the Egyptian Petroleum products and wastes materials ND is a non-detectable value. Sample type Location Code Activity concentrations (Bq kg−1 ) 226 Ra 232 Th 40 K Crude oil The Nile Delta (EO1) 14.9 ± 1.2 3.4 ± 1.4 77.3 ± 3.0 Crude oil The Nile Delta (EO2) 10.2 ± 1.9 ND 66.5 ± 10.0 Crude oil Suez (EO3) 13.4 ± 4.4 6.2 ± 2.8 91.8 ± 7.1 Crude oil Suez (EO4) 21.3 ± 5.4 ND 121 ± 15 Liquid gas The Nile Delta (ELG1) 10.8 ± 6.5 ND 143 ± 16 Water Suez (EWO1) 3.7 ± 1.7 ND 50.2 ± 4.5 Sludge The Nile Delta (ESL1) 7.6 ± 2.4 8.4 ± 2.6 52.2 ± 8.7 Sludge The Nile Delta (ESL2) 12.9 ± 1.4 3.1 ± 1.6 54.5 ± 5.4 Sludge The Nile Delta (ESL3) 20.6 ± 2.1 4.4 ± 1.9 51.9 ± 4.9 Sludge Suez (ESL4) 11.3 ± 5.1 14.8 ± 2.8 73.4 ± 14.1 Sludge Suez (ESL5) 123 ± 5 48.3 ± 0.8 241 ± 3 Sand The Nile Delta (ES1) 3.4 ± 1.2 3.1 ± 1.8 37.8 ± 6.7 Average 21.1 ± 3.2 7.6 ± 1.3 88.4 ± 8.2 3 ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING PETROLEUM RAW MATERIALS Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 4. 1.33 MeV of gamma ray line of 60 Co (located at the Egyptian Atomic Energy Agency, Cairo, Egypt). In order to reduce the effects of background measured by the detector, it is shielded with a cylindrical lead (Pb) of thickness 10 cm which contains an inner con- centric cylinder of Cu with a thickness of 8 mm. The detector is connected to a data acquisition system, using a personal computer, which has a Multi- Channel-Analyzer (8192 channels). The data ana- lysis was carried out via gamma spectroscopy pro- gram of Genie 2000 spectral analysis software. The HPGe detector’s peak calibration and efficiency were carried out using standard point source package (RSS- 8) of eight radionuclides of Cs-137, Ba-133, Cd-109, Zn-65, Co-60, Co-57, Mn-54 and Na-22 supplied by the IAEA. For bulk measurements, the 40 K in KCl standard bulk solution was used as a normalizing fac- tor. The bulk source was packaged in the same con- tainer geometric as those used for samples. The natural radionuclide concentrations of 238 U (226 Ra), 232 Th and 40 K in each sample were detected over a time frame of around 24 h. Since 226 Ra and its progenies produce ~98.5% of radiological effects of natural uranium series, the contribution of natural 238 U and the precursors of 226 Ra were ignored. Thus, 226 Ra was considered to be the reference of the 238 U series instead of 238 U(17, 18) . 226 Ra specific activity was measured from the gamma rays lines at the energies of 351.9 keV (36.6%) and 295.2 keV (18.5%) associated with the decay 214 Pb, and at the energies of 609.3 keV (46.1%) and 1120 keV (15%) associated with the decay 214 Bi, as shown in Figure 3. On the other hand, thorium (232 Th) spe- cific activity was estimated from the gamma rays of energies of 911.1 keV (29%) associated with the decay of 228 Ac, 583.1 keV (84.5%) associated with the decay of 208 Tl and 238.6 keV (43.6%) associated with the decay of 212 Pb as shown in Figure 3. Finally, potassium (40 K) specific activity was esti- mated from the gamma ray of the energy of 1460.9 keV (10.67%) associated with the decay 40 K itself(19, 20) . The self-attenuation and coincidence summing effects were ignored in this study. The activity concentrations of natural radionuclides, A, (Bq kg−1 ) are calculated from Eq (1)(19, 21) . ρ ε = ( ) A C wt 1 i i where C is the net count above the background, pi is the absolute emission probability of each gamma ray (men- tioned in brackets after gamma rays energies), w is the net dry sample weight (kg), The samples’ weights were ranged between 350 and 500 g, t is the measurement time and εi is the absolute efficiency of the detector is associated with each gamma rays energy value. Figure 2. The location map of oil fields in Egypt. 4 N. M. HASSAN ET AL. Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 5. RESULTS AND DISCUSSION The goal of this work is to measure the activity con- centrations of 226 Ra, 232 Th and 40 K in some ran- domly selected materials of different types of oil, scale, sludge, water and sand from oil wells located in both Egypt and Kuwait. The results of this study are summarized in Tables 1 and 2. The activity con- centrations of 226 Ra, 232 Th and 40 K in petroleum products and their wastes were varied from ND (non- detectable value, KO4) to 123 ± 3 (KP1) Bq kg−1 with a mean value of 25.2 ± 3.4 Bq kg−1 for 226 Ra, ND (KO1) to 27.7 ± 0.6 (KSL1) Bq kg−1 with a mean value of 6.1 ± 2.2 Bq kg−1 for 232 Th and ND (KSL1) to 183.39 ± 13.73 (KS1) Bq kg−1 with a mean value of 67.8 ± 6.4 Bq kg−1 for 40 K, in the selected samples from Kuwait, as shown in Figures 4–6 and Tables 1. On the other hand, the Egyptian samples were varied from 3.4 ± 1.2 (ES1) to 123 ± 5 (ESL5) Bq kg−1 with a mean value of 21.1 ± 3.2 Bq kg−1 for 226 Ra, ND (EO2) to 48.3 ± 0.8 (ESL5) Bq kg−1 with a mean value of 7.6 ± 1.3 Bq kg−1 for 232 Th and 37.8 ± 6.7 (ES1) to 241 ± 3 (ESL5) Bq kg−1 with a mean value of 88.4 ± 8.2 Bq kg−1 for 40 K, respectively, as shown in Figures 4–6 and Tables 2. The maximum activity levels for all measured radionuclides in selected samples were 126 ± 3 Bq kg−1 (KP1) of 226 Ra, 27.7 ± 0.6 (KSL1) Bq kg−1 of 232 Th and 183 ± 14 (ESL5) Bq kg−1 of 40 K for Kuwaiti samples while for Egyptian sam- ples, they were 123 ± 5 Bq kg−1 (ESL5) of 226 Ra, 48.3 ± 0.8 (ESL5) Bq kg−1 of 232 Th and 241 ± 3 (ESL5) Bq kg−1 of 40 K, respectively. The radionuclide concentration of Egyptian and Kuwaiti petroleum products and their wastes were comparable with almost the same average values. However, specific activities of 226 Ra, 232 Th and 40 K in sludge samples were higher than their values in crude oil, water and sand for Egyptian samples. Similarly, the Kuwaiti radionuclide concentration of 226 Ra in the plankton oil refinery of greater Burgan oil well was higher than its value in all other samples, 232 Th in sludge of greater Burgan oil well was higher than its value in all other samples and 40 K in sand of south Fuwars was higher than its value in all other samples. The obtained results indicate that the specific activity concentrations in all selected material from Egypt and Kuwait were comparable or less than the global median specific activity concentrations in soil of 35, 30 and 400 Bq kg−1 for 226 Ra, 232 Th and 40 K, respectively, reported by UNSCEAR(21, 22) . Moreover, the radionuclide concentrations in the studied materials were much lower than the exemp- tion level for NORM of 1 Bq g−1 for uranium and thorium and 10 Bq g−1 for 40 K recommended by the IAEA basic safety standards(23, 24) . Thus, there is no radiological risk for worker or public dealing with those materials so that the radiation exposure from the selected material can be ignored. The values of natural radionuclides in the present study were compared with their values in the same material previously described in the literature, as pictured in Table 3. In order to compute the radiation hazards asso- ciated with materials maintained various levels of 226 Ra, 232 Th and 40 K in a single quantity, the radium equivalent activity (Raeq) has been introduced by UNSCEAR(21, 22, 34) , Eq. 2. = + + ( ) Ra A A A 1.43 0.077 2 eq Ra Th K where, ARa, ATh and AK are activity concentrations of 226 Ra, 232 Th and 40 K, respectively, in Bq kg−1 . The radium equivalent index was calculated based Figure 3. Typical gamma ray spectrum of natural radionuclides of Egyptian (ESL5) and Kuwait (KSL1) sludge waste materials. 5 ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING PETROLEUM RAW MATERIALS Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 6. on the assumption that 370 Bq kg−1 of 226 Ra, 259 Bq kg−1 of 232 Th and 4810 Bq kg−1 of 40 K produce the same equivalent dose of gamma ray. For the sake of safety, Raeq activity concentration of material should be <370 Bq kg−1 to keep gamma ray dose below 1.5 mSv y−1(35–37) . Radium equivalent concentration in Egyptian petroleum products and wastes was ranged from 7.5 ± 2.0 Bq kg−1 (EWO1) to 210 ± 7 Bq kg−1 (ESL5) with a mean value 38.8 ± 5.8 Bq kg−1 while for Kuwaiti samples, it was ranged from 1.7 ± 1.0 Bq kg−1 (KO1) to 134 ± 6 Bq kg−1 (KSL1) with a mean value of 34.4 ± 5.6 Bq kg−1 , as shown in Figure 7, and Tables 4 and 5. The Radium equivalent of all investi- gated petroleum products and wastes was less than the recommended limit of 370 Bq kg−1 which implies that these materials have no radiological hazards and can be safely used in various industries. Radiation hazard mainly comes from external gamma rays emitted from natural radionuclides of 226 Ra, 232 Th and 40 K. The external hazard of gamma 0 20 40 60 80 100 120 EO1 EO2 EO3 EO4 __ __ __ __ __ ELG1 EWO1 ESL1 ESL2 ESL3 ESL4 ESL5 ES1 __ __ __ KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4 Activity Conc. Bq/Kg Sample Code Ra-226 Activity Egypt Kuwait Figure 4. Specific activity concentrations of Ra-226 in Egyptian and Kuwaiti samples. 0 5 10 15 20 25 30 EO1 EO2 EO3 EO4 __ __ __ __ __ EWO1 EWG1 ESL2 ESL1 ESL3 ESL4 ESL5 ES1 __ __ __ KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4 Activity Conc. Bq/Kg Sample Code Th-232 Activity Egypt Kuwait Figure 5. Specific activity concentrations of Th-232 in Egyptian and Kuwaiti samples. 6 N. M. HASSAN ET AL. Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 7. rays can be expressed by the external hazard index (Hex) which was determined from Eq. (3)(34) ; = + + ( ) H A A A 370 259 4810 3 ex Ra Th K where, ARa, ATh and AK are the activities of 226 Ra, 232 Th and 40 K, respectively, in Bq kg−1 . Normally, the external hazard index of a material should be less than unity in order to limit the external gamma radiation dose to be <1.5 mSv y−1 . In this study, the average calculated values of external hazard index for Egyptian and Kuwaiti petroleum products and wastes were of 0.11 ± 0.02 and 0.09 ± 0.02 (Tables 4 and 5). The external hazard index of all studied sam- ples was less than the recommended limit which implies the external radiation hazard could be ignored. In addition to the external hazard, another factor should be taken into account because of radon, and its progenies as they are hazardous to the respiratory organs is called an internal hazard index. It is caused by radionuclides of 226 Ra, 232 Th and 40 K in add- itional to radon and its progenies of 218 Po, 214 Pb, 210 Pb and 210 Bi. The internal hazard index (Hin) can be defined as(34) ; = + + ( ) H A A A 185 259 4810 4 in Ra Th K For the safe use of a material, Hin should be less than unity in order to ignore the hazards of radon and its products on the respiratory organs. The average value of the internal hazard index was 0.16 ± 0.03 (Table 5) for all of the Egyptian and Kuwaiti samples, which are lower than the recommended limit. Thus, the use of Egyptian and Kuwaiti materi- als has insignificant radiation hazards. Normally, the petroleum products and wastes, maintained natural radionuclides; hence they could be a possible source of radiation exposure for the public and workers. Thus, regular assessment of their radiation exposure would be beneficial for the public and workers health and safety. Radiation exposure is mainly due to gamma radiation emitted from those materials. The absorbed dose rate (D) due to gamma rays in the air at 1 m of air above the selected materi- als which maintains a uniform distribution of nat- ural radionuclides of 226 Ra, 232 Th and 40 K, can be calculated from the following equation(21) . ( ) = + + ( ) − D nGy h A A A 0.462 0.621 0.042 5 Ra Th K 1 The absorbed dose rate was calculated for the samples as shown in Tables 6 and 7. The radiation absorbed dose rate was varied from 3.8 ± 1.0 nGy h−1 (EWO1) to 96.4 ± 3.2 nGy h−1 (ESL5) with a mean value of 18.1 ± 2.7 nGy h−1 for Egyptian pet- roleum products and wastes. For Kuwaiti samples, the absorbed dose varied from 0.87 ± 0.48 nGy h−1 (KO1) to 61.2 ± 1.6 nGy h−1 (KP1) with a mean value of 16.1 ± 2.6 nGy h−1 . All the selected Egyptian and Kuwaiti materials had an absorbed radiation dose value lower than the recommended value by UNSCEAR(21) , of 59 nGy h−1 except two 0 50 100 150 200 250 EO1 EO2 EO3 __ __ __ __ __ __ EWO1 ELG1 ESL2 ESL3 ESL1 ESL4 ESL5 ES1 __ __ __ KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4 Activity Conc. Bq/Kg Sample Code K-40 Activity Egypt Kuwait Figure 6. Specific activity concentrations of K-40 in Egyptian and Kuwaiti samples. 7 ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING PETROLEUM RAW MATERIALS Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 8. samples of KP1 (61.2 ± 1.6) nGy and KSL1 (60.5 ± 2.8) nGy from Kuwaiti samples and one sample of ESL5 (96.4 ± 3.2) nGy from Egyptian samples, as given in Tables 6 and 7. Thus, except for three sam- ples of KP1, KSL1 and ESL5, all the Egyptian and Kuwaiti samples have no pose of radiation exposure. Furthermore, the annual effective dose (E) from gamma rays emitted from 226 Ra, 232 Th and 40 k in the samples was calculated from Eq. (6)(22, 34) . = ( × ( ) × × ( ) ( ) − − E D nGy h h y O C Sv Gy 8760 / 6 1 1 where, O is the occupancy factor and C is the absorbed to the effective dose conversion factor of 0.7 Sv/Gy(38) . The annual effective dose due to gam- ma rays emitted from the radionuclides of 226 Ra, 232 Th and 40 K in the selected materials was calcu- lated within two scenarios. The first scenario (effect- ive and actual scenario) is that workers in fields (well locations) and factories are exposed to petroleum products/wastes maintained radionuclides of 226 Ra, 232 Th and 40 K, for 1753 hy−1 (outdoor occupancy factor equals ~0.2, 1753 hy−1 = 0.2 × 8760 hy−1 ), while the other scenario is that a certain population in houses is exposed for 7012 hy−1 (outdoor occu- pancy factor equals ~0.8, 7012 hy−1 = 0.2 × 8760 h y−1 ). This scenario is not effective in the present study, but it was used to show the possible highest radiological risk. In the first scenario (effective and actual scenario), the annual effective dose from gamma rays emitted by 226 Ra, 232 Th and 40 k in the samples varied from 4.6 ± 1.2 μSv y−1 (EWO1) to 118 ± 4 μSv y−1 (ESL5) with a mean value of 22.2 ± 3.3 μSv y−1 for the Egyptian samples. On the other side, the Kuwaiti samples varied from 1.1 ± 0.6 μSv y−1 (KO1) to 75.0 ± 2.0 μSv y−1 (KP1) with a mean value of 19.8 ± 3.1 μSv y−1 , as summarized in Tables 6 and 7 and Figure 8. Whereas in the second scenario, the annual effective dose ranged from 18.4 ± 4.8 μSv y−1 (EWO1) to 472.8 ± 15.6 μSv y−1 (ESL5) for the Egyptian samples and from 4.4 ± 2.4 μSv y−1 (KO1) to 300 ± 7.6 μSv y−1 (KP1) for the Kuwaiti samples, as seen in Tables 6 and 7. The calculated annual Table 3. Comparison of activity concentrations of 226 Ra, 232 Th and 40 K in petroleum products and wastes materials of various countries. Sample type Country Activity concentrations (Bq kg−1 ) Reference 226 Ra 232 Th 40 K Scale Brazil 18–22 19.2–21.9 417–432 (25) Scale Saudi Arabia 1284–3613 12–27 — (12) Scale Middle East 12–245.8 1.7–40.1 484.8–9850 (3) Scale Egypt 9140–285 823 427–34 339 51–1031 (14) Scale Syria 0.3–1520 0.6–868 — (1) Scale Tunisia 59 ± 7 82 ± 12 64 ± 10 (26) Sludge Nigeria 54.5–94.2 33.3–71.2 462.1–712.4 (2) Sludge Egypt 5.5–1785.8 < LD–885 < LD–125.5 (11) Sludge Brazil < LLD–413 400 < LLD–117 900 417 000–432 000 (15) Sludge UK 1.70–8.20 0.03–0.51 — (20) Sludge Malaysia 123–153 37–42 — (27) Sludge Iraq 1.5 0.2 2.5 (28) Sludge Turkey < 1–809.2 < 0.8–302.5 < 3.8–623 (29) Sludge Egypt 18.032 13.257 1261 (30) Sludge Albania 18–20 21–22 175–348 (31) Oil Kuwait 1.8–2.5 1.6–1.8 16.1–27.1 (32) Heavy oil Syria 77–135 24–42 — (1) Crude oil Ghana < 0.12–10.14 < 0.11–12.45 < 0.15–34.39 (4) Crude oil Saudi Arabia < LD 0.05–0.3 0.2–1.8 (5) Crude oil Turkey < 1– < 5.6 < 1–4.8 < 1– < 11 (29) Water Egypt 26.5–217 < LD–93 < LD–248.7 (11) Water Iran 0.1–30 — — (33) Oil Kuwait ND–17.0 ND–10.5 13.6–126 Present study Oil Egypt 10.2–21.3 3.4–6.2 66.5–121 Present study Sludge Kuwait Sludge 1.5–28 ND–54.8 Present study Sludge Egypt Sludge 3.1–48.3 52–241 Present study Sand Kuwait 3.8–55.3 3.2–5.4 43–183 Present study Sand Egypt 3.4 ± 1.2 3.1 ± 1.9 37.8 ± 6.7 Present study 8 N. M. HASSAN ET AL. Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 9. effective dose with both scenarios was less than the worldwide average annual effective dose of 480 μSv y−1(22) . As well, it is much lower than 1 mSv for the public or 20 mSv for workers recommended by the International Commission on Radiological Protection (ICRP-103)(35) . The gamma ray radiation hazards associated with the natural radionuclides in materials can be evalu- ated by means of the radioactivity level index called gamma index (Iγ). According to the European Commission guidelines, Iγ should be <1 for a gamma radiation dose of 1 mSv y−1(23) . The gamma ray index (Iγ) can be calculated from Eq. (7).(39) = + + ( ) γ I C C C 300 200 3000 7 Ra Th K The Iγ of the Egyptian samples varied from 0.03 ± 0.01 for (EWO1) to 0.73 ± 0.02 for (ESL5) with a mean value of 0.14 ± 0.02. For the Kuwaiti sam- ples, it varied from 0.007 ± 0.004 for (KO1) to 0 20 40 60 80 100 EO1 EO2 EO3 EO4 __ __ __ __ __ EWO1 ELG1 ESL2 ESL3 ESL1 ESL4 ESL5 ES1 __ __ __ KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4 Activity Conc. Bq/Kg Sample Code Specific activities concentrations of Radium Equivalent (Raeq) Egypt Kuwait Figure 7. Radium equivalent activity concentrations of Egyptian and Kuwaiti samples. Table 4. Radium equivalent, external and internal hazard indices of Kuwaiti samples. Sample code Radium equivalent (Raeq) (Bq Kg−1 ) External index (Hex) Internal index (Hin) (KO1) 1.7 ± 1.0 0.005 ± 0.003 0.006 ± 0.005 (KO2) 14.8 ± 10.9 0.040 ± 0.029 0.058 ± 0.038 (KO3) 26.7 ± 7.3 0.072 ± 0.020 0.118 ± 0.037 (kO4) 4.4 ± 1.3 0.012 ± 0.003 0.012 ± 0.003 (KO5) 29.0 ± 12.4 0.078 ± 0.034 0.098 ± 0.045 (KO6) 26.0 ± 1.4 0.070 ± 0.004 0.114 ± 0.005 (KO7) 15.5 ± 4.8 0.042 ± 0.013 0.058 ± 0.017 (KP1) 132 ± 3 0.356 ± 0.009 0.695 ± 0.017 (KP2) 8.7 ± 0.9 0.024 ± 0.002 0.031 ± 0.003 (KWO1) 8.1 ± 3.0 0.022 ± 0.008 0.032 ± 0.015 (KSL1) 134 ± 6 0.362 ± 0.017 0.616 ± 0.031 (KSL2) 57.2 ± 15.9 0.155 ± 0.043 0.269 ± 0.075 (KSL3) 19.5 ± 3.8 0.053 ± 0.010 0.088 ± 0.015 (KS1) 75.0 ± 14.9 0.203 ± 0.040 0.352 ± 0.064 (KS2) 11.8 ± 6.0 0.032 ± 0.016 0.042 ± 0.022 (KS3) 6.8 ± 2.1 0.018 ± 0.006 0.026 ± 0.010 (KS4) 41.8 ± 3.6 0.113 ± 0.010 0.191 ± 0.016 9 ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING PETROLEUM RAW MATERIALS Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 10. Table 5. Radium equivalent, external and internal Hazard Indexes of Egyptian samples. Sample code Radium equivalent (Raeq) (Bq Kg−1 ) External index (Hex) Internal index (Hin) (EO1) 25.8 ± 3.5 0.070 ± 0.009 0.110 ± 0.013 (EO2) 15.3 ± 2.7 0.041 ± 0.007 0.069 ± 0.012 (EO3) 29.4 ± 9.0 0.079 ± 0.024 0.116 ± 0.036 (EO4) 30.6 ± 6.6 0.083 ± 0.018 0.140 ± 0.032 (ELG1) 21.8 ± 7.7 0.059 ± 0.021 0.088 ± 0.038 (EWO1) 7.5 ± 2.0 0.020 ± 0.005 0.030 ± 0.010 (ESL1) 23.6 ± 6.8 0.064 ± 0.018 0.084 ± 0.025 (ESL2) 21.5 ± 4.1 0.058 ± 0.011 0.093 ± 0.015 (ESL3) 30.9 ± 5.3 0.084 ± 0.014 0.139 ± 0.020 (ESL4) 38.2 ± 10.2 0.103 ± 0.028 0.134 ± 0.041 (ESL5) 210 ± 7 0.568 ± 0.019 0.899 ± 0.033 (ES1) 10.7 ± 4.4 0.029 ± 0.012 0.038 ± 0.015 Table 7. Absorbed dose rate and effective dose, gamma and alpha indices of Egyptian samples. Sample code Absorbed dose rate (nGy h−1 ) Effective dose (μSv y−1 ) Gamma index (Iγ) Alpha index (Iα) Outdoor indoor (EO1) 12.2 ± 1.6 15.0 ± 1.9 60.0 ± 7.6 0.093 ± 0.012 0.074 ± 0.006 (EO2) 7.5 ± 1.3 9.2 ± 1.6 36.8 ± 6.4 0.056 ± 0.010 0.051 ± 0.010 (EO3) 13.9 ± 4.1 17.0 ± 5.0 68.0 ± 20.0 0.106 ± 0.031 0.067 ± 0.022 (EO4) 14.9 ± 3.1 18.3 ± 3.9 73.2 ± 15.6 0.111 ± 0.023 0.106 ± 0.027 (ELG1) 11.0 ± 3.7 13.5 ± 4.5 54.0 ± 18.0 0.084 ± 0.027 0.054 ± 0.032 (EWO1) 3.8 ± 1.0 4.6 ± 1.2 18.4 ± 4.8 0.029 ± 0.007 0.018 ± 0.008 (ESL1) 10.9 ± 3.1 13.4 ± 3.8 53.6 ± 15.2 0.085 ± 0.024 0.038 ± 0.012 (ESL2) 10.1 ± 1.9 12.4 ± 2.3 49.6 ± 9.2 0.077 ± 0.014 0.065 ± 0.007 (ESL3) 14.4 ± 2.4 17.7 ± 2.9 70.8 ± 11.6 0.108 ± 0.018 0.103 ± 0.010 (ESL4) 17.5 ± 4.7 21.4 ± 5.7 85.6 ± 22.8 0.136 ± 0.036 0.056 ± 0.026 (ESL5) 96.4 ± 3.2 118.2 ± 3.9 472.8 ± 15.6 0.730 ± 0.023 0.613 ± 0.027 (ES1) 5.0 ± 2.0 6.2 ± 2.4 24.8 ± 9.6 0.039 ± 0.016 0.017 ± 0.006 Table 6. Absorbed dose rate and effective dose, gamma and alpha Indices of Kuwaiti samples. Sample code Absorbed dose (nGy h−1 ) Effective dose (μSv y−1 ) Gamma index (Iγ) Alpha index (Iα) Outdoor Indoor (KO1) 0.9 ± 0.5 1.1 ± 0.6 4.4 ± 2.4 0.0067 ± 0.0035 0.003 ± 0.005 (KO2) 7.3 ± 4.9 9.0 ± 6.0 36.0 ± 24.0 0.056 ± 0.038 0.034 ± 0.016 (KO3) 13.1 ± 3.4 16.1 ± 4.2 64.4 ± 16.8 0.0987 ± 0.0250 0.085 ± 0.032 (kO4) 2.4 ± 0.7 2.9 ± 0.6 11.6 ± 2.4 0.019 ± 0.006 0.000 ± 0.000 (KO5) 13.6 ± 5.6 16.6 ± 6.9 66.4 ± 27.6 0.106 ± 0.043 0.036 ± 0.021 (KO6) 12.4 ± 0.6 15.2 ± 0.8 60.8 ± 3.2 0.094 ± 0.005 0.082 ± 0.002 (KO7) 7.3 ± 2.2 9.0 ± 2.7 36.0 ± 10.8 0.056 ± 0.017 0.029 ± 0.006 (KP1) 61.2 ± 1.6 75.0 ± 1.9 300.0 ± 7.6 0.446 ± 0.012 0.628 ± 0.014 (KP2) 4.4 ± 0.4 5.4 ± 0.5 21.6 ± 2.0 0.034 ± 0.003 0.014 ± 0.001 (KWO1) 4.1 ± 1.4 5.0 ± 1.7 20.0 ± 6.8 0.031 ± 0.010 0.020 ± 0.013 (KSL1) 60.5 ± 2.8 74.3 ± 3.5 297.2 ± 14.0 0.453 ± 0.021 0.471 ± 0.026 (KSL2) 26.6 ± 7.3 32.7 ± 8.9 130.8 ± 35.6 0.198 ± 0.054 0.212 ± 0.059 (KSL3) 9.3 ± 1.8 11.4 ± 2.2 45.6 ± 8.8 0.069 ± 0.014 0.065 ± 0.009 (KS1) 35.6 ± 6.8 43.6 ± 8.4 174.4 ± 33.6 0.265 ± 0.052 0.276 ± 0.044 (KS2) 5.6 ± 2.7 6.8 ± 3.3 27.2 ± 13.2 0.043 ± 0.021 0.019 ± 0.010 (KS3) 3.5 ± 1.0 4.3 ± 1.2 17.2 ± 4.8 0.026 ± 0.007 0.015 ± 0.009 (KS4) 19.5 ± 1.7 23.9 ± 2.1 95.6 ± 8.4 0.146 ± 0.013 0.144 ± 0.012 10 N. M. HASSAN ET AL. Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
  • 11. 0.453 ± 0.021 for (KSL1) with a mean value of 0.121 ± 0.019, as can be seen in Tables 6 and 7. All the measured samples had a radioactivity level index <1 so that these samples can be used without special precautions(39) . Alpha radiation due to the released radon from samples is called alpha index (Iα) which can be com- puted from Eq. (8),(39) . The alpha index should be less than unity to reflect a radium concentration value <200 Bq kg−1 (the upper recommended value) which leads to a maximum released radon concen- tration <200 Bq m-3 . = ( ) ∝ I A 200 8 Ra Alpha index of the Egyptian samples varied from 0.017 ± 0.006 (ES1) to 0.613 ± 0.027 (ESL5) with a mean value of 0.105 ± 0.016. For Kuwaiti samples, it varied from the ND value (KO4) to 0.628 ± 0.014 (KP1) with a mean value of 0.119 ± 0.016, as seen in Tables 6 and 7. Accordingly, the values of Alpha index for Egyptian and Kuwaiti petroleum products and wastes were much lower than unity which implies that all the study materials do not have radi- ation hazard for a worker and the general public. CONCLUSION Natural radioactivity concentrations of 226 Ra, 232 Th and 40 K, in petroleum products and wastes of crude oil, water, sludge and contaminated sand collected various petroleum well fields located Egypt and Kuwait, were ranged from 3.35 ± 1.22 to 122.55 ± 5.42 Bq kg−1 for 226 Ra, ND value to 48.28 ± 0.82 Bq kg−1 for 232 Th and 37.83 ± 6.70 to 240.59 ± 3.42 Bq kg−1 for 40 K Egyptian samples and from ND to 125.52 ± 2.82 Bq kg−1 for 226 Ra, ND to 27.65 ± 0.63 Bq kg−1 for 232 Th and ND to 183.39 ± 13.73 Bq kg−1 for 40 K, for Kuwaiti samples. The radionuclides concentrations of Egyptian and Kuwaiti petroleum products and wastes were less than the recommended limits of UNSCEAR and ICRP for earth’s crust and the recommended values of IAEA as well. Moreover, the radiological hazard indexes, of radium equivalent activities (Raeq), external and internal indexes, gamma and alpha indexes and annual effective doses of the Egyptian and Kuwaiti petroleum products and wastes were less than the recommended values of 370 Bq kg−1 , 1, 1 and 480 μSv y−1 . The absorbed dose of all the studied samples was less than the recommended value of 59 nGy h−1 except only three samples of KP1, KEL1 and ESL5. Thus, we deduce that the selected petroleum products and wastes (except KP1, KSL1 and ESL5) have not caused significant radiological risk on the worker or the public but might need monitoring for long-term effective evaluation. REFERENCES 1. Al-Masri, M. S. and Haddad, Kh. NORM emissions from heavy oil and natural gas-fired power plants in Syria. Environ. Radioact 104, 71–74 (2012). 0 10 20 30 40 50 60 70 80 EO1 EO2 EO4 EO3 __ __ __ __ __ EWO1 ELG1 ESL2 ESL3 ESL1 ESL4 ESL5 ES1 __ __ __ KO1 KO2 KO3 KO4 KO5 KO6 KO7 KP1 KP2 __ KWO1 KSL1 KSL2 KSL3 __ __ KS1 KS2 KS3 KS4 Effective Dose (µSv/y) Sample Code The Annual Effective Dose (Eeff) Egypt Kuwait Figure 8. Annual effective dose of gamma rays of Egyptian and Kuwaiti samples. 11 ASSESSMENT OF RADIOLOGICAL HAZARDS OF USING PETROLEUM RAW MATERIALS Downloaded from https://academic.oup.com/rpd/advance-article-abstract/doi/10.1093/rpd/ncz043/5466142 by guest on 14 June 2019
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