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Naturally occurring radioactive materials (NORM) wastes in oil fields are a

radiological problem, but they are useful tools

Conference Paper · October 2008

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Ibrahim Sudki Othman Mohammad Said Al-Masri

Atomic Energy Commission of Syria Atomic Energy Commission of Syria
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 Naturally occurring radioactive materials (NORM) wastes in oilfields
are a radiological problem, but they are useful tools

Ibrahim Othman* , Mohammad Said Al-Masri

Atomic Energy Commission, Damascus, P. O. Box 6091, Syria

Abstract: Produced water, scales and sludges associated with the production of oil and gas contains enhanced
concentrations of radium isotopes. Uncontrolled disposal of these wastes could lead to environmental pollution
and thus to radiation exposure of members of the public. In the present work, radium isotopes in scales
accumulated in oilfield equipment, and produced water have been used for dating the deposited scales, studying
between wells interactions and water flooding processes in addition to dating contaminated soils in the Syrian
oilfields.
The 228Ra/226Ra activity ratio in scales can be considered a fingerprint of the Th/U mass ratio in the geological
formation of the reservoir. The 228Ra/226Ra activity ratio variations were found to reflect the variability of the
Th/U mass ratio of the geological formation, suggesting two different source rock types found in the Syrian
oilfields. The calculated mean Th/U mass ratio for these two possible types of source rock were 2.4 and 5.78. In
addition, the 228Ra/226Ra mean activity ratio was also used to estimate the age of some deposited scales in
tubulars; the results were compared with the 224Ra/228Ra activity ratio dating method. Moreover, 228Ra/226Ra,
224
Ra/228Ra and 210Pb/226Ra activities ratios in contaminated soils due to disposal of production water were used
to date contaminated sites at the oilfields; the results have been found to be in agreement with the actual disposal
date. The methods can be used by the regulatory body to assess any uncontrolled disposal of such waste.

Key words: Naturally Occurring Radioactive Materials (NORM), Radium-226, Waste, Oil Industry

1. Introduction

Naturally Occurring Radionuclides (NOR’s) originating from the 232Th and 238U series can be
concentrated and accumulated in tubing and surface equipment in the form of scales and sludge during
the production of oil and gas [1, 2, 3, 4, 5, 6, 7, 8]. Scales may cause problems in the operations of
installations by plugging perforations, clogging tubular and valves, thereby restricting flow. Scales and
sludge are usually removed from the production systems and stored or disposed off as low-level
radioactive wastes. Other wastes containing NORM considered in the oil and gas production are
production water, scrap production equipment, and contaminated soil. These radioactive wastes
require treatment or disposal in appropriate methods. Uncontrolled disposal of any type of these waste
could lead to environmental pollution and thus eventually to radiation exposure of members of the
public; most operating oil companies in Syria have disposed off their wastes into unlined pits and
lagoons.

Syrian oil fields are situated approximately 700 km to the Northeast of Damascus city. Oil and gas
with production water are routed to various central-processing facilities (CPF) for separation and
processing. Detailed site gamma survey and soil characterization was first performed to assess the
volume and type of waste materials at all NORM contaminated sites. Gamma survey of the affected
areas in all fields was carried out using portable radiation monitors. Radiation contour maps were then
established for each site and different zones being defined. In addition, selective core sampling in the
hot spots and average contamination zones were defined and the volume of contaminated soil to be
removed to the disposal site was determined by the exemption criteria applied. Radon measurements
in air, soil and water and radioactivity in groundwater were also conducted. The remediation plan
based on the results of the preliminarily gamma radiation survey and estimated volume of the
contaminated soil has been prepared. The risk to public, workers and the environment associated with
all available options of NORM waste disposal have been evaluated [1, 7].

Naturally occurring radionuclides have been widely used as tracers for several environmental studies

*
Ibrahim Othman, E-mail address: iothman@aec.org.sy; atomic@aec.org.sy

1
[9, 10, 11, 12, 13]. The applications include the determination of sedimentation rates in oceans and
lakes, pollution history, dating of geological deposits, soil erosion studies in addition to its
applications in the oil and gas industry. The present study describes our attempts to use naturally
occurring radioactive materials in NORM wastes in oil and gas as tracers for several applications,
namely, interwell reactions, water flooding, scale age determination and pollution history of
contaminated sites at the oilfields.

2. Material and methods

2. 1. Area of study
The study was carried out in two main operating oil companies field in Syria (DER EZZOR
PETROLEUM COMPANT, DEZPC and AL-FURAT PETROLEUM COMPANY, AFPC)
(Figure 1). The study was focused on the three main oil fields, namely Al Jafra, Al Qahar, and Attala
in DEZPC and four fields in AFPC, namely, Tanak, Omar, Al-Tayyem and El-Ward. Most of these
fields penetrate the two sandy layers known as Rutbah and Mulussa, which have good reservoir
quality and high productivity; these layers are known to be fractured carbonate layers. DEZPC
production started in 1991 while AFPC oilfields are in operation since 1986. As for the small and
marginal fields, the two companies applied the experience of jet water pumping in wells, in addition
to gas lift. Treated (from Euphrates River) and produced water are injected in all fields through
injecting wells. Oil and gas with production water are routed to central-processing facilities (CPF)
for separation and processing.

Figure 1. Syrian Oilfields Location

2
2. 2. Sample collection and preparation
Soil samples were collected using a stainless steel core sampler with a 7-cm diameter from the
contaminated sites in DEZPC & AFPC fields. Only the top 0 – 5 cm layers of surface soil were
considered as surface samples; more than 3000 surface soil samples being collected. In addition, more
than 150 scales samples were collected from different equipment before decontamination at the
NORM Decontamination Facility located at Omar field (AFPC). All soil and scale samples were dried
in the oven for 48 hours at 105 C. The samples were then grinned and about 40 g of each sample was
filled in a special counting container and stored for two weeks for counting. In addition, approximately
5 liters of production water samples were collected from wellheads for laboratory analysis. The
samples were typically a mixture of oil and water so the mixture was allowed to separate and cool

2. 3. Determination of radium isotopes

Radioactivity analysis for determination of radium isotopes in soil, scale and production water samples
was carried out by gamma spectrometry. For soil samples (40 gram) and about 20 g of each scale
sample were filled in a special counting container and stored for one month for counting allowing
establishment of secular equilibrium between 226Ra, 228Ra and 224Ra and their decay products. 226Ra,
228
Ra and 224Ra activities were then determined by measuring their gamma emitting daughters, 214Pb
(351.9 keV), 214Bi (609 keV), 212Pb (238 keV), 212Bi (727.3 keV) and 228Ac (911.1 keV) by gamma
spectrometry using high resolution (2 keV at 1.33 MeV), high relative efficiency (80%) and low
background HpGe detectors. For water samples, one liter of each water sample was subsequently
sealed in standard air-tight plastic container and stored for one month prior to counting for 24 hours
using HpGe detector (Relative Efficiency 26.5%). Efficiency calibration was performed using
reference samples (RGU, RGTH and RGK) provided by the International Atomic Energy Agency,
IAEA. Quality control procedures were applied using in-house control samples and reference samples
provided by the IAEA and Environmental Laboratory Measurement, EML, (Department of Energy,
USA).

2. 4. Determination of 210Pb
The dried soil samples were measured by gamma spectrometer (HpGe Planar model, Canberra, the
relative efficiency is 10%). All samples were prepared as cylindrical shape (r = 2.5 cm, and h varied
from 0.95 to 1.1 cm) pressed using a pressure of 40 ton cm-2. The calibration source was prepared
using the same procedure. The 210Pb is measured directly through its gamma line 46.5 keV with an
intensity of 4.0%.

3. Results and Discussions

3. 1. The use of 228Ra/226Ra activity ratio in produced water for interwell reactions and water
flooding process

Variations of radium isotopes concentrations in produced water of one specific producing oil well are
related to the volume and type of the injected water for waterflooding process [6]. Injection fresh
water or treated produced water containing low concentrations of radium isotopes will dilute the
produced water radioactivity content. The data obtained for 226Ra, 228Ra and the 228Ra/226Ra activity
ratio in produced water have been statistically evaluated using the so-called Explanatory Data
Analysis method (one example of which is the Box Plot used herein) (Figures 2, 3 and 4). Large
variations of 226Ra and 228Ra activity concentrations were found in both Al Jafra and Attala (DEZPC)
produced water. This was due to the fact that the water injection process was not uniformly applied
during the study period, with consequent variability in the associated dilution factors for the Ra
isotopes in the produced water. Of particular note is that fresh water from the River Euphrates and
treated produced water from Al Jafra producing wells are mixed together and injected in one of the
injection wells. A different trend has been observed for Qahar produced water where small variations
of 226Ra activity concentrations were found in comparison with 228Ra activity concentrations. Even
though no water injection process was practiced in the Qahar field during the study, this trend may be
due to variations in water/oil ratio where the highest value (75%) was found to be in Qahar field.
However, the median values for 226Ra activity concentration in produced water collected from Attala

3
and Al Jafra field were close, which indicates that the producing wells in both fields are
interconnected; all wells in both fields are within 3 km radius. Similar relationship was also observed
for the 228Ra/226Ra activity ratio. The average values of the 228Ra/226Ra activity ratio were found to be
0.79, 0.86 and 1.91 for Al Jafra, Attala and Qahar oilfields, respectively. This may suggest that there is
no interwell reactions between Al Jafra (and Attala) and Qahar oil producing wells; Qahar oil wells are
located about 66 km from Al Jafra field.

Figure 2. Box plot for 226Ra concentration in produced water from the three oil fields. The box plot
shows the median value and the 25% and 75% percentiles. The short horizontal lines label the 10%
and 90% percentile, while the asterisks represent outlying values.
140

120

100

80
Ra (Bq l )
-1

60
226

40

20

Jafra Attala Qhar

Figure 3. Box plot for 228Ra concentration in produced water from the three oil fields

80

60
Ra (Bq l )
-1

40
228

20

0
Jafra Attala Qahar

4
Figure 4. Box plot for 228Ra/226Ra activity ratio in produced water from the three oil fields

3.0

2.5

2.0
Ra/ Ra
226

1.5
228

1.0

0.5

Jafra Attala Qahar

The relation between 226Ra and 228Ra activity concentrations in produced water collected from the Al
Jafra field was examined where the linear correlation coefficient (R2) of 0.52 was calculated; all data
from Al Jafra produced water were used for 226Ra vs 228Ra plot. The correlation coefficient was
decreased to 0.33 when all data of the three oilfields were plotted. In addition, the relation was also
studied using only the data for produced water samples collected at the same time from Al Jafra field
and more linear relationship was observed; a correlation coefficient of 0.73 was found. This also
suggests that the studied wells in Al Jafra are interconnected. Moreover, the 228Ra/226Ra activity ratio
of a specific producing well is not greatly variable with time if fresh water is used for injection, but the
ratio could be altered when treated produced water from different reservoir having different activity
ratio is used. Therefore, the 228Ra/226Ra activity ratio variation with time in Al Jafra oilfield was found
to be negligible. This due to the fact that only fresh water form (Euphrates River) and treated produced
water from Al Jafra oil wells were used for waterflooding during the study. The mean 228Ra/226Ra
activity ratio of the injected water was determined and found to be 0.75, which is close to the mean
value (0.79) obtained for Al Jafra produced water (Table 1).

Table 1. Range of radioactivity levels in produced water from the three oil fields and the Th/U mass
ratio of the geological formation of the reservoir
226 228 224
Ra Ra Ra
Field Bql-1 Bql-1 Bql-1 (228Ra/226Ra) 0 Th/U
(mean value±1σ) (mean value±1σ) (mean value±1σ)
13.8-111.2 12.4-67.4 0.2-3.7
Al-Jafra (40) 0.79±0.21 2.4
(51.9±23.4) (37.5±12.6) (1.1±0.7)
9.9-58 8.8-50.5 0.6-1.5
Attala (6) 0.86±0.04 2.6
(41.0±15.1) (35.0±13.0) (0.93±0.3)
13.9-20.9 20.7-57.5 0.4-2.3
Qahar (12) 1.91±0.67 5.78
(18.7±2.2) (26.1±14.0) (1±0.7)
(n): number of samples

5
3. 2. Age determinations of deposited scales

Radium isotopes and some of their decay products have been used to date young barites deposits on
the sea floor and radioactive barites at contaminated sites within oilfields production sites [14]. The
average age of oil field equipment (< 40 years) can be estimated by comparing the present
measurement activity ratio of (228Ra/226Ra) to that of the initial activity ratio (228Ra/226Ra) 0 [14],
provided that the radium isotopes incorporated into an insoluble radium mineral approximates a
chemically closed system since the time of its formation. In present studies, the ratio is determined
from the direct radioactivity measurement of the scale samples, while the initial activity ratio of
(228Ra/226/Ra) 0 is estimated by measuring the radium isotopes in modern produced water.
Alternatively, the latter can be considered to be in the range of 0.5-2, corresponding to a
thorium/uranium mass ratio of 1.5-6 [14]. For relatively newly formed scale (less than 10 years old),
as in the present situation, the measured activity ratio of 224Ra/228Ra can be used to estimate the
average scale age of the oil-field equipment. This can be conducted by applying the ingrowth decay
ratio of 224Ra and 228Ra where the present activity of 224Ra in scales is only from the decay of 228Ra,
with half-life of 5.75 years, via 228Th (half-life 1.9 years); thorium is not present in freshly produced
scales. Taking into consideration the above assumptions, the average age of scales in the oil-field
equipment can be estimated by applying the following equation:

T (years) = - ln [ 1- (224Ra/228Ra)/1.49] 4.098 (1)

The factors, 1.49 and 4.098, are derived from fitting data of the 224Ra and 228Ra activity ratio. Some
results are presented in Figure 5. The 25% and 75% probability percentiles have been used to compare
the average ages. The calculated ages were compared with the related equipment maintenance data
sheet.

Figure 5. Average age of scales deposited in various oilfield equipment.

3. 3. Determination of Th/U mass ratios of the geological formations

Another application of radium isotopes activity ratio is the determination of Th/U mass ratio of the
geological formation [9]. The thorium/uranium mass ratio was calculated according to the average
activity ratio found for the lognormal distribution of the initial ratio (228Ra/226Ra) 0 , as shown in Figure
6. This initial ratio was determined using the 228Ra and 226Ra present activity. Correction was made for
the average elapsed time since the time of scale formation, representing the average scale age values
determined as described in the previous section). 226Ra activity has been used without correction in
view of its long half-life (1600 year). The 228Ra/226Ra activity ratio variations were found to reflect the
variability of the Th/U mass ratio of the geological formation, suggesting two different source rock
types found in the Syrian oilfields. The calculated mean Th/U mass ratio for these two possible types

6
of source rock were 2.4 and 5.78. This ratio can be considered a fingerprint for the Th / U ratio of the
geological formation of the reservoir. This is in agreement with recent published study where two oil
bearing rocks were determined using the 14C method [15]. In addition, the same approach has been
used using contaminated soil collected from different fields. The obtained results of the studied oilfield
are represented in Figure 7, where AFPC oilfields samples were found to have Th/U mass ratio
between 2 and 3 with an abnormal value for Al-Maleh oilfield, and more than 3 for Al-Jafra oilfield. It
is obvious that the range of Th/U ratio for the all oilfields within the range 2-4, and the only exception
is the value of Al-Maleh oilfield, which is, exceeds 6. The only explanation for that, is the different
host rock formation of the reservoir of this field, that the host rock of the reservoir is enriched in
thorium and has less uranium content. The obtained results of the radium activity ratio, either for the
contaminated soil or the produced water, are confirming this observation; where the radium activity
ratio of Al-Maleh NORM contaminated soil is about 1.75 comparing with less than 0.67 for the other
oilfields.

Figure 6. Lognormal distribution of 228Ra/226Ra activity ratio in scales.

6

4
No of Samples

0
0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.6 1.8 2.0 2.2 2.4 2.6 2.8 3.0
(Ra-228/Ra-226)0 Ratio

Figure 7. Th/U mass ratio of different oilfields

Th/U Mass Ratio of different oilfields in Syria
7

5
Th/U Mass Ratio

0
Maleh

Ward

Al-Jafra05
Thayeem

Omar

Th/U

3. 4. Average age estimation of NORM contaminated soil using radium activity ratios

Adequate number of NORM contaminated soil samples (more than 30 samples) have been used from
each contaminated site to determine the activity ratios of 224Ra/228Ra, 228Ra/226Ra, and 210Pb/226Ra. A
lognormal distribution is used to calculate the mean ratio values and their standard deviations as

7
shown in Figure 8. The 224Ra/228Ra ratio was varied between 0.82 and 0.95 of the AFPC contaminated
sites (Thayeem, Omar, Ward, and Maleh); while it was 0.67 in Al-Jafra site (the main oilfield of
DEZPC). These differences will lead to different average age estimation in contaminated sites belongs
to each company. However, the 228Ra/226Ra activity ratio has similar variations as 224Ra/228Ra activity
ratio variations. The calculated ratios are confirming this assumption, with an exception for Al-Maleh
oilfield that belongs to AFPC and located far from other AFPC oilfield in the east of Syria. The
analyzed produced water samples from different wells in each field showed a range of 228Ra/226Ra
activity ratios, from 0.73 to 1.33 with one abnormal value 2.11; of Al-Maleh oilfield that belongs to
AFPC, which will be discussed in more details. These 228Ra/226Ra activity ratios of the analyzed
produced water samples are representing the initial radium activity ratio (228Ra/226Ra) 0 . The average
age estimation of contaminated sites (t) was obtained by applying the following formula:

 λ 228 t
( 228 Ra/ 226 Ra)t ( 228 Ra/ 226 Ra)0  e (2)

Figure 8. Lognormal distribution of 224Ra/228Ra ratio in different oilfields

Thayeem (Ra224/Ra- 228) N = 336, Mean = 0.95, StdDv = 0.11 Om ar (Ra224/Ra-228) N = 389, Mean = 0.82, StdDv = 0.12
Thayeem (Ra228/Ra- 226) N = 336, Mean = 0.67, StdDv = 0.08 Om ar (Ra228/Ra-226) N = 389, Mean = 0.48, StdDv = 0.06
280
200
260
Ra-224/Ra-228
180 240
Ra-224/Ra-228 Ra-228/Ra-226
220
160 Ra-228/Ra-226
200
140
180
120 160
No of obs
No of obs

140
100
120
80
100
60 80
60
40
40
20
20
0 0
0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.3
Ratio Ratio

Ward (Ra224/Ra228) N = 95, Mean = 0.67, StdDv = 0.16 Maleh (Ra224/Ra228) N = 30, Mean = 0.93, StdDv = 0.05
Ward (Ra228/Ra226) N = 95, Mean = 0.57, StdDv = 0.12 Maleh (Ra228/Ra226) N = 30, Mean = 1.74, StdDv = 0.15
45
30
40 28
Ra-224/Ra-228 Ra-224/Ra-228
26
Ra-228/Ra-226 Ra-228/Ra-226
35 24
22
30
20
18
No of obs

25
No of obs

16
20 14
12
15 10
8
10
6

5 4
2
0 0
0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.3 0.7 0.9 1.1 1.3 1.5 1.7 1.9 2.1

Ratio Ratio

Jafra01 (Ra224/Ra228) N = 57, Mean = 0.67, StdDv = 0.09

Jafra01 (Ra228/Ra226) N = 56, Mean = 0.31, StdDv = 0.10
30
28
26 Ra-224/Ra-228
Ra-228/Ra-226
24
22
20
18
No of obs

16
14

12
10
8
6
4
2
0
0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0

8
Figure 9 shows the calculated average age estimation in the studied contaminated sites and they are in
agreement with the technical available information of AFPC and DEZPC about discharging produced
water to the environment. The only exception was in Al-Maleh oil field (AFPC) and this is due to the
fact the calculation was carried out using only one available value of produced water. Another
deviation was in Al-Jafra field of DEZPC where the age of contamination using 224Ra/228Ra activity
method was overestimated while the 228Ra/226Ra activity method gave underestimated values. This
may be de to variations in 228Ra/226Ra and 224Ra/228Ra in produced water with time.

Figure 9. Average age estimation of different NORM contaminated soil sites

Range Plot (age detrmination.sta 16v *48c)

2002

2000

1998

1996

1994

1992

1990

1988
Av e24
Av e28
1986 Av ePb
Thay eem Maleh Al-Jaf ra05 Av e INFO
Omar Ward Al-Jaf ra01

3. 5. Average age estimation of NORM contaminated soil using lead 210 ingrowth method
The calculated activity ratio 210Pb/226Ra in contaminated soil was used to estimate the average age of
contaminated soil in each oilfield (Figure 9). It was assumed that the majority of measured 210Pb is
produced by the decay of its parent 226Ra; where the contribution of insoluble 210Pb that could be
transported from the reservoir is negligible. The supported 210Pb produced by the decay of 226Ra
present in soil is also negligible. The obtained results seem to be very reliable and in agreement with
the technical information supported by the AFPC and DEZPC about the period of produced water
discharge into the lagoons. However, the range of age estimation is expected to be wide since the
uncertainty associated with 210Pb determination in low energy spectrometry is high. Another affecting
factor is that the fraction loss of 222Rn emanated from NORM contaminated soil may reduce the
activity of the unsupported 210Pb, and hence underestimating the contamination age. On the other
hand, the probability of transporting an insoluble lead from the reservoir may increase the unsupported
210
Pb in soil and hence overestimating the contamination age.

4. Conclusion

Radium isotopes in oilfield wastes can be used for interwell reactions, water flooding process, age
determination of scales and dating contaminated areas in the oilfields. In addition, the 228Ra/226Ra
activity ratio can be considered a fingerprint of the U/Th mass ratio in the geological formation of the
reservoir. Scale dating method based on the initial 228Ra/226Ra activity ratio of produced water gave
comparable results with method based on the 224Ra/228Ra activity ratio in scales. Moreover, variation
of 226Ra and 228Ra activity concentrations could be suggested as a tool for studying the waterflooding
process and interwell reactions.

9
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