Journal of Environmental Radioactivity 101 (2010) 51–54

Contents lists available at ScienceDirect

Journal of Environmental Radioactivity

journal homepage: www.elsevier.com/locate/jenvrad

Radiological hazards of TENORM in the wasted petroleum pipes

M. Abo-Elmagd a, *, H.A. Soliman a, Kh.A. Salman b, N.M. El-Masry a
a
National Institute For Standard, Department of Ionizing Radiation and Radioactive Material Metrology, P. O. Box 136 Giza Code No. 12211, Egypt
b
Radiation Protection Department, Nuclear Research Center, Atomic Energy Authority, P. Code 13759, Cairo, Egypt

a r t i c l e i n f o a b s t r a c t

Article history: Disposal petroleum pipes containing sludge and scale as a technically enhanced natural occurring
Received 2 April 2009 radioactive material (TENORM) leads to internal and external radiation hazards and then a significant
Received in revised form radiation dose to the workers. In order to contribute to a future waste management policy related to the
6 August 2009
presence of TENORM in the disposal sites of wasted petroleum pipes, scale and sludge as TENORM wastes
Accepted 27 August 2009
Available online 25 September 2009
are collected form these disposal pipes for radiometric analysis. These pipes are imported from onshore
oilfields at south Sinai governorate, Egypt. The highest mean 226Ra and 228Ra concentrations of 519 and
50 kBq/kg respectively, were measured in scale samples. Sludge lies within the normal range of radium
Keywords:
TENORM wastes concentration. The average absorbed dose caused by the exposure to the wasted pipes equal to 4.09 mGy
Sludge and scale h1 from sludge and 262 mGy h1 from scale. This is much higher than the acceptable level of 0.059 mGy h
1
Radiological hazards . Due to radon inhalation, important radon related parameters are calculated which advantage in
Radon exhalation internal dose calculation. Fairly good correlation between real radium content and radon exhalation rate
for sludge samples is obtained. The hazards from sludge come from its high emanation power for radon
which equal to 3.83%. The obtained results demonstrate the need of screening oil residues for their
radionuclide content in order to decide about their final disposal.
Ó 2009 Elsevier Ltd. All rights reserved.

1. Introduction
Naturally occurring radioactive materials (NORM) generally
contain radionuclides found in nature, i.e., thorium, uranium, and
their progeny. When NORM becomes concentrated in radionuclides
due to human activity, one can speak about technologically
enhanced naturally occurring radioactive materials (TENORM). The
TENORM waste is produced from several industrial sectors such as
uranium and metal mining, phosphate ore processing, and petro-
leum industry (Egidi and Hull, 1999). The petroleum waste (scale or
sludge) have been produced by two mechanisms: either incorpo-
ration or precipitation onto the production equipment such as:
pipelines, storage tank, pumps., etc. (El Afifi and Awwad, 2005).
The precipitated TENORM wastes around walls of the petroleum
pipes reduce their efficiency and then disposed and replaced
periodically by new ones (El Afifi et al., 2009; Somlai et al., 2008).
In the last decade, attention was focused on the environmental
and health impact from the release of TENORM wastes. Knowledge
of radioactive content and basic radiological parameters in the
* Corresponding author. Tel./fax: þ20237416936.
E-mail address: abo_elmgd@hotmail.com (M. Abo-Elmagd).
disposed wasted pipes is very important for the purposes of nuclear
waste management projects such as:
 Setting up the treatment methods of TENORM wastes.
 Promote the development and/or the update of databases on
hazardous substances/wastes in Egypt.
 Propagate full understanding of the nuclear waste status to
develop an appropriate action plan for their management.
The disposal pipes from onshore oilfields at the eastern bank of
Suez gulf, south Sinai governorate, Egypt are segregated in an iso-
lated disposal site designated for this purpose. Accumulation of
large amounts of TENORM wastes with a significant activity may
cause health risks to the workers in this site through exposure,
inhalation of radon (222Rn) decayed and/or ingestion of waste dust.
The present work is aimed to contribute to a future hazards
waste management policy related to the presence of TENORM in
the area containing the disposal petroleum pipes. For this reason,
scale, sludge and sand samples from the wasted pipes and
surrounding area are collected for radiometric analysis. The anal-
ysis included the determination of activity concentration of natural
gamma-emitting radionuclides and calculating the radium equiv-
alent, absorbed and effective dose rates to decide whether they are

0265-931X/$ – see front matter Ó 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jenvrad.2009.08.016
52 M. Abo-Elmagd et al. / Journal of Environmental Radioactivity 101 (2010) 51–54

acceptable according to the exception levels established by IAEA
(1994). Also, the important radon related parameters are measured.
2. Experimental work
2.1. Samples preparation
The TENORM samples were catalogued and dried at 110  C in an
oven for complete removal of moisture. For radioactivity
measurements, the samples were sealed in radon-impermeable
airtight plastic cans. The containers were identical to those con-
taining standard samples in the calibration experiment of HPGe
detector. The samples were stored for more than 30 days to achieve
secular equilibrium between 226Ra and 222Rn.
Samples weights of 100 g were placed in a glass container of
3.75  104 m3 volume and 4.5  103 m2 base area. The emanated
radon gas from the samples was measured by a Lucas cell to
determine the radon related parameters.
where ARa, ATh, and AK are the specific activities (Bq kg1) of 226Ra,
232
Th and 40K, respectively. This formula is based on the estimation
that 1 Bq kg1 of 226Ra, 0.7 Bq kg1 of 232Th and 13 Bq kg1 of 40K
produce the same g-ray dose rates (Tufail et al., 2006).
The contribution of terrestrial gamma radiation to absorbed
doses in air can be calculated using the following formula
(UNSCEAR, 2000).
DðnGy=hÞ ¼ 0:462  ARa þ 0:604  ATh þ 0:0417  AK (2)
where D (nGy/h) is the absorbed dose rate at 1 m from samples.
The external dose rates due to gamma rays of 226Ra, and 232Th,
40
K in TENORM were converted to annual effective dose by using
the following relation (UNSCEAR, 2000).
EðmSv=yÞ ¼ DðnGy=hÞ  8760ðh=yÞ  O  CðmSv=nGyÞ (3)
where E is the annual effective dose (in mSv), O is the occupancy
factor, and C is the absorbed-to-effective dose conversion factor (0.7
 106 mSv per nGy).

2.2. Radioactivity measurement

The collected TENORM were analyzed for natural radioactivity
(226Ra, 232Th, 228Ra and 40K) by g-spectroscopy using high-resolu-
tion HPGe spectrometry system with 30% counting efficiency. The
resolution of this spectrometer was 1.85 keV at 1332 keV g-rays of
60
Co. The absolute efficiency calibration of the detector was
determined using standard samples prepared in National institute
for Standard (NIS), Egypt. Detailed information concerning the
HPGe-detectors calibration, and also the procedures followed can
be found elsewhere (Sroor et al., 2001).
After measurement and subtraction of the background, the
activity concentrations were calculated.
a) 226
Ra concentration was determined by measuring the 295.1
(19.2%) and 352 (37.1%) keV g-rays from 214Pb and the 609.3
(46.1%) and 1120.3 (15%) keV g-rays from 214Bi. The 226Ra
concentration was calculated by averaging over the measured
concentrations for 214Pb and 214Bi.
b) 232Th activity was determined from the g-peaks of 238.6
(44.6%) keV from 212Pb and 338.4 (12%), and 583.0 (30%) keV
g-rays from 208Tl.
c) 228Ra activity was determined from the g-peaks of 911.2 (29%)
from 228Ac.
d) 40K concentration was measured from its 1460 (10.7%) keV
g-line.
The counting time was about 60,000 s to obtain a g-spectrum of
good statistics.
To represent the specific activities of 226Ra, 232Th and 40K by
a single quantity, which takes into account the radiation hazards
associated with them, a common index has been introduced in
term of radium equivalent activity. It is defined as (OECD, 1979;
Beretka and Mathew, 1985).
Raeq ¼ ARa þ 1:43  ATh þ 0:077  AK
2.3. Radon related parameters
A calibrated Lucas cell coupled with an electronic apparatus
AB-5 (Pylon electronic) was connected with the sealed cup by two
plastic pipes and valves. Such a system enables the air containing
radon from the cup to be removed only to the Lucas cell and vice
versa. Each weight was sealed for a known time followed by grap
sampling for 10 min using the AB-5 pump at 0.5 l/m flow rate (Chau
et al., 2005). After waiting 4 h from the end of sampling, the radon
content in the Lucas cell was counted. Each counting consisted of 6
runs; each of them lasted 5 min, takes the average and then
calculates the net count per minute (NCPM) by subtracting the
count background. Using the following equation, the radon
concentration in the cell Rn (PCi/l) can be calculated (Pylon
Instruction, 1989):
NCPM  C
Rn ¼ (4)
3  2:22  E  Vc  A
where C, A are the correction factors for decay during the counting
time and time interval between end of sampling and the start of
counting, respectively, The digit 3 is designed for the three alpha
emitters in equilibrium, 2.22 is used to convert disintegration per
minute (DPM) to Pci, Vc is the Lucas cell volume (0.151 l) and E is the
efficiency of the Lucas cell for radon measurements (0.74 CPM/
DPM)
The radon activity Q (Pci) of the used sample weight is given by
(Pylon Instruction, 1989):
Rn  VT
Q ¼
(5)
1  elt
where, VT is the total volume (0.755 l) which is the sum of cell
volume (0.151 l), sealed cup volume (0.375 l), pump volume (0.154 l)
and total pipe and connector volumes (0.075 l). t (h) is the time
(1) elapsed from sealing the cup to the end of pumping and l (7.55 
103 h1) is the radon decay constant.

Table 1
Minimum, maximum and average activity concentration of TENORM in the wasted petroleum pipes.

Sample N Ra-226 kBq/kg Th-232 kBq/kg K-40 kBq/kg

Min. Max. Average  SD Min. Max. Average  SD Min. Max. Average  SD

SC 10 493 519 506  18 35.38 54.08 44.7  13 LLD 0.177 0.059  0.10
SL 9 5.27 8.68 6.99  1.4 1.08 2.09 1.37  0.4 LLD 0.667 0.148  0.29
SA 6 0.09 0.15 0.12  0.04 0.04 0.05 0.044  0.01 0.584 0.690 0.637  0.07

N: Number of samples, SD: Standard deviation, LLD: lower limit of detection, SC: Scale, SL: Sludge, SA: Sand.
 M. Abo-Elmagd et al. / Journal of Environmental Radioactivity 101 (2010) 51–54 53

Table 2
Minimum, maximum and average calculated value of radium equivalent, absorbed dose and annual effective dose caused by exposure to TENORM in the wasted petroleum
pipes.

Sample No. Raeq Bq kg1  103 Absorbed dose rate, D mGy h1 Annual Effective Dose, E mSv

Min. Max. Average  SD Min. Max. Average  SD Min. Max. Average  SD

SC 10 544 596 570  37 250 273 262  16 306 335 321  20
SL 9 6.9 11.7 8.97  1.9 3.2 5.3 4.09  0.9 3.9 6.5 5.02  1.1
SA 6 0.19 0.27 0.23  0.1 0.09 0.13 0.11  0.03 0.11 0.16 0.13  0.03

Reference value 0.370 0.059 0.07

From the activity Q (after converting it to Bq), the effective
radium content RaEff (Bq kg1) areal EA (Bq m2 h1) and mass EM
(Bq kg1 h1) exhalation rates can be determined:
Q activity is higher than the exemption limit of 10 kBq kg1 that
RaEff: ¼
M proposed by the European Union for such residues (EU BSS, 1996)
Ql
EA ¼
S clear that radium equivalent for scale and sludge exceeds the
Ql
EM ¼
M sludge it reached 8.97  1.9 kBq kg1. As a comparison, the radium
where, M (kg) is the TENORM weight, S (m2) is its surface area.
The ratio between effective and real radium content is the
sample emanation power for radon which also calculated.
3. Results and discussion
3.1. Radiometric parameters
The minimum, maximum and average activity concentration of
226
Ra, 232Th and 40K in the scale, sludge and sand samples collected
from disposal wasted petroleum pipes are listed in Table 1. In scale
samples, 226Ra, 232Th activities are elevated compared to sludge and
sand samples which consistent with the work of Gazineu and Hazin
(2008). According to the standard deviation of 3.5% in 226Ra activity
measurements and 29% in 232Th, the fluctuation in the measured
232
Th is higher than it for 226Ra. Also, high fluctuation is observed in
sludge sample for both 226Ra and 232Th. The sand samples show
much lower activity but still higher than the worldwide average
concentration of soil (33 and 45 Bq kg1 for 238U and 232Th series
respectively) which indicates its contamination with radionuclide
from TENORM in the wasted petroleum pipes. 228Ra activity
concentration is ranged from 32 to 50 kBq kg1 for Scale and from 1
to 1.9 kBq kg1 for sludge. The sand samples have average 228Ra
activity concentration equal to 0.042 kBq kg1 which within the
worldwide average (UNSCEAR, 2000). 40K activity concentration is
insignificant compared with 226Ra and 232Th which ranged from
LLD (lower limit of detection) to 0.69 kBq kg1.
Enhanced 226Ra activity in TENORM over 232Th (or 228Ra) and
40
K is due to the physicochemical properties of 226Ra such as its
longer half life and its lower solubility. This properties lead to the
disequilibrium state in both 238U and 232Th series. The ratio
226
Ra/228Ra for scale samples is 13 where it is equal to 6 in sludge.
The ratio 228Ra/224Ra in scale samples is 0.7 where it is equal to
0.8 in sludge which is compatible and indicates that there is
disequilibrium in 232Th series.
For all presented scale samples, 226Ra and 228Ra concentration
(6)
where the sludge is lower than this exemption limit.
Table 2 shows some important radiometric parameters. It is
(7)
maximum permissible value (Ref. value is 370 Bq/kg). The higher
radium equivalent is about 570  37 kBq kg1 in Scale, whilst in
(8)
equivalent index found in this study is higher than that observed in
the wastes associated with oil and gas production in Gabal El Zeit
field in Suez gulf (El Afifi and Awwad, 2005).
The total absorbed dose rate due to gamma-emissions was
estimated from Eq. (2) and the obtained values are listed in Table 2.
It is recommended that the acceptable total absorbed dose rate by
the workers in areas containing gamma -radiations from 238U and
232
Th series and their respective decay progenies, as well as 40K,
must not exceed 0.059 mGy/h (UNSCEAR, 2000). It is obvious that
the calculated total absorbed dose rates for all waste samples are
highly larger than the recommended dose level that is acceptable.
The average annual effective dose as calculated from equation (3) is
equal to 0.13, 5.02 and 321 mSv for sand, sludge and scale respec-
tively. The worldwide average annual effective dose is 0.07 mSv
based on 0.2 occupancy factor and 0.7 Sv Gy1 conversion factor for
absorbed dose in air to received effective dose by adult (UNSCEAR,
2000). The detailed range and standard deviation are listed in Table 2.
3.2. Radon related parameters
Table 3 lists the radon related parameters that measured by
active technique (Lucas cell) and use equations (4)–(8) for detail
calculations. Due to the variety in the samples density and volume,
the back diffusion effect is taken into consideration (Jang et al.,
2005; Kovler, 2006). For scale samples, the effective radium content
(RaEff) found to be vary from 1436  429 to 3162  575 Bq kg1 for
coarse (within 1 mm grain size) and dust (100 mm grain size) scale
respectively. Lower the grain size higher the probability of escaping
radon from the sample and it is obvious in higher emanation power
of dust sample (0.63%) than coarse ones (0.29%). Sludge has lower
effective radium content (268  66 Bq kg1) due to its lower real
radium activity concentration but has higher radon emanation

Table 3
Basic radon related parameters in TENORM wastes from the petroleum pipes.

Sample No. RaEff. Bq kg1 EM Bq kg1 h1 EA Bq m2 h1 a%

SC-coarse 5 1436  429 11  3 173  57 0.3  0.1
SC-dust 5 3162  575 24  4 373  136 0.6  0.1
SL 9 268  66 2.0  0.5 38  8 3.8  0.6
SA 3 4  2 0.03  0.02 0.7  0.4 4.2  3.3

a: Radon emanation coefficient.

54 M. Abo-Elmagd et al. / Journal of Environmental Radioactivity 101 (2010) 51–54
60
Sludge samples
R2 = 0.75
50
EA (Bq m-2 h-1)
40
30
20
10
4000 5000 6000 7000 8000
Ra-226 content (Bq kg-1)
Fig. 1. Correlation of radium content and areal exhalation rate for Sludge samples.
power than scale due to its different physical properties and
chemical composition, therefore elevated radium content in sludge
are important in radon attack problems because it has an emana-
tion power from 6 to 12 times higher than scale.
Sand samples have lower effective radium content but due to its
lower density than the TENORM sample, the sand has higher
emanation power (4.19%).
Average radon exhalation rates per unit mass in TENORM
samples is ranged from 2.0  0.5 Bq kg1 h1 for sludge to 24  4 Bq
kg1 h1 for dust scale.
Also, the average radon exhalation rates per unit area is ranged
from 38  8 Bq m2 h1 for sludge to 373  136 Bq m2 h1 for dust
scale. All these values are much higher than the reported values of
soil and building material which gives TENORM wastes special
interest in the field of radiological protection (Faheem and Mat-
iullah, 2008).
Due contamination of sand, it has exhalation rates larger than
the average worldwide value of 1.53  105 Bq kg1 h1 and
(0.2–0.3) Bq m2 h1 for mass and areal exhalation rates respec-
tively (UNSCEAR, 2000) for normal sand.
Correlation between real radium content and areal exhalation
rate for sludge samples is shown in Fig. 1, the relation is linear
with 0.75 correlation coefficient. By this correlation, it is simply
to estimate the exhalation rate and therefore the radon attack
from the knowledge of real radium content which is widely
measured parameters in TENORM waste from different waste
disposal areas.
4. Conclusion
Radionuclide analysis of the TENORM waste from disposal
petroleum pipes is necessary prior to treatment, disposal or
a decision to declassify it from TENORM waste. Scale and sludge can
represent a considerable waste problem. The concentrations of
radium in scale and sludge are high although they within the values
reported in other countries. Thus, the management of scale-
contaminated pipes should be carried out in accordance to the
related safety procedures in TENORM handling set by the national
regulatory authority.
Activity concentration of scales was higher than it for sludge
samples. For both scale and sludge, 226Ra activity concentration was
higher than 228Ra activity concentration, which, in turn, was much
higher than the 40K values. Activity concentrations for the majority
of scales and sludge samples were higher than the international
clearance levels. Therefore, special care must be taken when
dealing with these residues. Besides, workers should be warned to
stay the minimum possible time close to the places where radio-
nuclides accumulation exists, in order to minimize radiation
exposure. The disposal petroleum pipes contaminate the disposal
areas which may lead to a long term problem for the hazardous
waste management system.
The higher the radioactivity level in the wasted pipe, the higher
is the radiological impacts, especially when considering the
potential of operators to be exposed via internal contamination by
ingesting or inhaling the dust during waste processing. Attachment
of radon daughters to aerosol particles that are inhaled and
deposited in the human respiratory tract add internal radiation
dose to the workers. The main factors control the internal dose due
to radon inhalation are measured such as effective radium content,
mass and areal exhalation rates as well as the radon emanation
9000
power. Detail calculation of internal exposure due to radon inha-
lation by the workers is the aim of the future work.
References
Beretka, J., Mathew, P.J., 1985. Natural radioactivity of Australian building materials,
industrial wastes and by-products. Health Physics 48, 87–95.
Chau, N.D., Chrusciel, D., Prokolski, L., 2005. Factor controlling measurements of
radon mass exhalation rate. Journal of environmental radioactivity 82, 363–
369.
Egidi, P., Hull, C., 1999. NORM and TENORM: procedures, users, and proposed
regulations. In: Health Physics Society 1999, 32nd Midyear Topical Meeting
Albuquerque, New Mexico, USA, January 24–27, pp. 25–30.
El Afifi, E.M., Awwad, N.S., 2005. Characterization of the TE-NORM waste associated
with oil and natural gas production in Abu Rudeis, Egypt. Journal of Environ-
mental Radioactivity 82, 7–19.
El Afifi, E.M., Awwad, N.S., Hilal, M.A., 2009. Sequential chemical treatment of
radium species in TENORM waste sludge produced from oil and natural gas
production. Journal of Hazardous Materials 161, 907–912.
EU BSSdCouncil Directive 96/29/Euratom, 1996. Laying down the basic safety
standards for the protection of the health of workers and the general public
against the dangers arising from ionizing radiation. Official Journal of EC Series
L, No. 159.
Faheem, Munazza, Matiullah, 2008. Radon exhalation and its dependence on
moisture content from samples of soil and building materials. Radiation
Measurements 43, 1458–1462.
Gazineu, M.H.P., Hazin, C.A., 2008. Radium and potassium-40 in solid wastes from
the oil industry. Applied Radiation and Isotopes 66, 90–94.
International Atomic Energy Agency (IAEA), 1994. International Basic Safety Stan-
dards for the Protection Against Ionizing Radiation and for the Safety of Radi-
ation Sources GOV/2715/Vienna.
Jang, Mee, Kang, C.-S., Hyun Moon, J., 2005. Estimation of 222Rn release from the
phosphogypsum board used in housing panels. Journal of Environmental
Radioactivity 80, 153–160.
Kovler, Konstantin, 2006. Radon exhalation of hardening concrete: monitoring
cement hydration and prediction of radon concentration in construction site.
Journal of Environmental Radioactivity 86, 354–366.
OECD (Organization for Economic Co-operation and Development), 1979. Exposure
to Radiation from the Natural Radioactivity in Building Materials. Report by
a Group of Experts of the OECD. Nuclear Energy Agency, Paris, France.
Pylon Instruction, 1989. Instruction Manual for Using Pylon Model 110A and 300A
Lucas Cells with the Pylon AB-5. Pylon Electronic Company, Canada.
Somlai, J., Jobbágy, V., Somlai, K., Kovács, J., Németh, Cs., Kovács, T., 2008. Connec-
tion between radon emanation and some structural properties of coal-slag as
building material. Radiation Measurements 43, 72–76.
Sroor, A., El-Bahi, S.M., Ahmed, F., Abdel-Haleem, A.S., 2001. Natural radioactivity
and radon exhalation rate of soil in southern Egypt. Applied Radiation and
Isotopes 55, 873–879.
Tufail, M., Akhtar, Nasim, Waqas, M., 2006. Radioactive rock phosphate: the feed
stock of phosphate fertilizers used in Pakistan. Health Physics 90 (4), 361–370.
UNSCEAR (United Nations Scientific Committee on the Effects of Atomic Radiation),
2000. Sources and Effects of Ionizing Radiation. Scientific Committee on the
Effects of Atomic Radiation, New York: United Nations. Report to the General
Assembly, with Scientific Annexes; 2000.