Radiation Physics and Chemistry 97 (2014) 346–348

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Radiation Physics and Chemistry

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

Investigation of radioactivity concentration in spent

technetium generators
Hajo Idriss a,c,d,n, Isam Salih b,d, Abdulaziz S. Alaamer a,c, M.H. Eisa c, A.K. Sam e
a
Al Imam Mohammad Ibn Saud Islamic University, Committee on Radiation and Environmental Pollution Protection, Riyadh, Saudi Arabia
b
Department of Physics, Taibah University, Al-Madinah Al-Munawarah, Saudi Arabia
c
Al Imam Mohammad Ibn Saud Islamic University, Physics Department, College of Science, P.O.Box 90950, Riyadh 11642, Saudi Arabia
d
Sudan Atomic Energy Commission, Khartoum, Sudan
e
Radiometrics Laboratory, IAEA Environment Laboratories, Department of Nuclear Sciences and Applications, International Atomic Energy Agency, Monaco

H I G H L I G H T S

Radioactivity investigation has been carried out in spent technetium generators.

The survey has resulted in the detection of 238U, 40K, 137Cs and 125Sb.

238U, 40K, 137Cs were measured in one sample while 125Sb was measured in 14 samples.

Monitoring of spent technetium is useful for final disposal of radioactive waste.

art ic l e i nf o a b s t r a c t

Article history: This study was carried out to survey and measure radioactivity concentration and estimate radiation
Received 29 August 2013 dose level at the surface of spent technetium generator columns for the safe final disposal of radioactive
Accepted 24 December 2013 waste. High resolution γ-spectrometry with the aid of handheld radiation survey meters has been used.
Available online 3 January 2014
The radioactivity measurements has shown that 238U, 40K and 137Cs were only measurable in one sample
Keywords: whereas 125Sb was found in 14 samples out of total of 20 samples with an activity concentration which
Spent technetium generator ranged from 21 to 7404 with an average value of 1095 Bq/kg. The activity concentration of 125Sb is highly
Gamma spectrometry variable indicating that the spent 99mTc generator columns are of different origin. This investigation
Radioactive waste highlighted the importance of radiation monitoring of spent technetium generators in the country in
Survey meters and 125Sb
order to protect workers, and the public from the dangers posed by radioactive waste.
& 2013 Elsevier Ltd. All rights reserved.

1. Introduction protect them from exposure to ionizing radiation. Following the

99m
Tc is the short-lived (T1/2 ¼6.02 h) daughter product of the
parent 99Mo, which is obtained either as a by-product of nuclear
fission of 235U or through neutron irradiation of stable 98Mo.
Technetium 99mTc is the most commonly used radiotracer in
contemporary diagnostic nuclear medicine (IAEA, 1989, 1999). In
Sudan, lead-shields of the spent technetium generators are refab-
ricated and used for shielding purposes in diagnostic X-ray rooms.
This source of supply has increased market demand for used
technetium generators and encouraged a considerable number of
people to be involved in lead collection from these generators
without being subjected to any regulatory control measures to
n
Corresponding author at: Al Imam Mohammad Ibn Saud Islamic University,
Committee on Radiation and Environmental Pollution Protection, Riyadh, Saudi
Arabia.
E-mail address: hjoidriss@gmail.com (H. Idriss).
establishment of the regulatory body in 1996, used technetium
generators have been collected in a waste management facility
within the framework of nationwide program to secure used
radioactive sources from all fields of peaceful applications with
the aim of building-up a broad database on source management
and inventory. Safe and efficient management of radioactive waste
is vital to many aspects of modern life—in medicine, health,
research and agriculture. A number of radiological accidents
occurred in different countries due to the lack of regulatory control
over used sources, some of which have led to serious conse-
quences, including the death of exposed persons (cite references of
specific accidents involving sealed sources such as Mexico, Brazil,
Turkey IAEA, 1996). The current study is an attempt to investigate
the possible presence of other isotopic impurities in spent tech-
netium generators, consequently to determine their concentra-
tions and propose additional safety measures that might be
needed during transport and storage of these spent technetium

0969-806X/$ - see front matter & 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.radphyschem.2013.12.030
 H. Idriss et al. / Radiation Physics and Chemistry 97 (2014) 346–348 347

generators in waste management facility. The outcome of this Table 1

undertaking is also hoped to increase regulatory awareness and Statistical summary of 125Sb activity concentration (Bq/kg) and radiation dose level
at the surface of spent 99mTc generator columns (sample size 20).
culture to deal with spent technetium generator in Sudan.
125
Sample code Surface dose Sb activity
level (mSv/h) concentration
2. Material and methods (Bq/kg)

2.1. Samples collection and preparation 1 0.20 7403

2 0.10 21
3 0.10 43
A total of 20 spent technetium generators were collected from 4 0.12 315
nuclear medicine centers and transported to the Radioactive 5 0.18 34
Waste management Facility at SAEC premises in Soba. The gen- 6 0.10 352
7 0.12 126
erators were dismantled and the components were segregated.
8 1.10 1059
The columns of the technetium generators were separately col- 9 0.90 624
lected to avoid cross contamination, tested for possible leakage 10 1.50 2326
and placed in sealed 500 ml marinelli beakers for measurement by 11 1.10 47
gamma-spectrometry. The process was monitored by using survey 12 0.10 438
13 0.07 1080
meters and contamination monitors. 14 0.20 1372

Mean 0.42 1089

2.2. Dose measurement Std 0.50 1934
Min 0.07 21
Radiation dose measurements were performed with the aid of Max 1.5 7403
radiation survey meters Radiagem-4000 and RADOS-120. These
dose meters were previously calibrated at the Secondary Standard
Dosimetery Laboratory (SSDL) in Sudan Atomic Energy Commis-
sion. The calibration factor for Radiagem-4000 was 0.89 μSv/h and
for the RADOS-120 was 0.88 μSv/h. Background radiations were 1.67
measured in three different locations far from any artificial source. 1.47
1.27
Dose µSv/h

2.2.1. Gamma-spectrometric measurement

1.07
The gamma-spectrometric measurement of the technetium
0.87
generator columns sealed in 500 ml marinelli geometry was
carried out using HPGe with an efficiency of 25% coupled to a 0.67
ΣSILENA multichannel analyzer (system is based on the use of a 0.47
“Memory Buffer” on standard card (Model 9308/A and 9302/A)). 0.27
The card consists of 3 circuit blocks: MCA, ADC and amplifier
0.07
shielded with 15 cm lead. The resolution (FWHM) of the spectro- 1 2 3 4 5 6 7 8 9 10 11 12 13 14
metry system was 1.8 keV at 1332 keV gamma-ray line of 60Co. The Samples
system was calibrated in terms of energy, efficiency and resolution
Fig. 1. Plot of radiation dose measured at the surface of technetium generators
employing mixed radionuclide standard (Amersham Buchler
column.
B1575) in the same geometry as samples. Each sample was
counted for 15 h and the spectrum analysis was performed with
Gamma-2000 software from SILENA INTERNATIONAL. The envir-
onmental gamma background contribution was determined with
an empty marinelli container washed with distilled water. The net Table 2
238 40 137 99m
Measured activity concentration of U, K and Cs in spent Tc generator
integral counts under selected photo-peaks were determined by columns.
subtracting from the total counts under these photo-peaks the
238 40 137
integral count above the baseline over the same region obtained Sample code U K Cs
from background runs. The lower detection limit of the system
1 2.5 50 1.57
(LLD) was calculated and found to be 1.5 Bq/L on the average. The
2 o 0.2 o0.2 o0.2
activity concentration (Bq/kg) of 232Th was determined from the 3 o 0.2 o0.2 o0.2
photo-peaks of 208Tl (583 keV) and 228Ac (911 keV), and that of 4 o 0.2 o0.2 o0.2
238
U was obtained from the gamma-lines of 214Pb (352 keV) and 5 o 0.2 o0.2 o0.2
214
Bi (609 keV), whereas 40K and 137Cs and 125Sb concentrations 6 o 0.2 o0.2 o0.2
7 o 0.2 o0.2 o0.2
were measured directly using their respective photo peaks at 1460 8 o 0.2 o0.2 o0.2
and 662 and 428 keV. 9 o 0.2 o0.2 o0.2
10 o 0.2 o0.2 o0.2
11 o 0.2 o0.2 o0.2
3. Results and discussion 12 o 0.2 o0.2 o0.2
13 o 0.2 o0.2 o0.2
14 o 0.2 o0.2 o0.2
Radiation level at the surface of spent technetium generator 15 o 0.2 o0.2 o0.2
columns studied is characterized with high variation ranging from 16 o 0.2 o0.2 o0.2
0.07 to 1.5 mSv/h, with a mean of 0.42 mSv/h as depicted in (Table 1 17 o 0.2 o0.2 o0.2
and Fig. 1). Radioactivity measurements revealed that the activity of 18 o 0.2 o0.2 o0.2
238 19 o 0.2 o0.2 o0.2
U, 40K and 137Cs are below the detection limit 0.2 Bq/kg except in 20 o 0.2 o0.2 o0.2
one sample while 125Sb was measured in 14 samples (Table 2). The
348 H. Idriss et al. / Radiation Physics and Chemistry 97 (2014) 346–348

8000 dismantled based on the IAEA recommendations or stored according

to radiation protection regulations (IAEA, 1994). Activities such as
7000
the medical uses of radiation, and the management of radioactive
6000 waste is subject to rigorous standards of safety, regulated at
Activity Bq/Kg

5000 the national level. Inadequate management after use or loss of

radioactive material and radiation sources has resulted in exposure
4000
to the public and extensive contamination of equipment, buildings
3000 and land (IAEA, 1999). Radioactive sources that are not under good
2000 regulation can result in a number of undesirable and significant
consequences including human health, socio-physiological, political
1000
and economic impacts as well as harm to the environment (Idriss
0 et al., 2012). There have been many instances of accidental smelting
1 2 3 4 5 6 7 8 9 10 11 12 13 14
of industrial radioactive sources, contaminating smelters and put-
Samples
ting radioactive metals into commercial and consumer products. To
Fig. 2. Plot of activity concentration of 125
Sb in spent 99m
Tc generator columns. avoid cross contamination, these technetium generator columns
were dismantled from scraps, tested for possible leakage and
conditioned into reinforced metal drums with a cement matrix to
3 achieve greater confinement for long-term storage under strict
institutional control.

2
Dose

4. Conclusion

R² = 0.0045 Based on these results of radioactivity level in spent techne-

1
tium generators, the following conclusions can be drawn:

0
The importance of legislation making radiation monitoring of

0 1000 2000 3000 4000 5000 6000 7000 8000 spent technetium generators in the country to protect workers
125 and the public from the dangers posed by contamination
Sb activity

We need to set up a comprehensive nationwide radiation
Fig. 3. Activity concentration as a function of dose at the surface of technetium survey of spent technetium generators to bring under regula-
generators column.
tory control all the associated sources.

activity concentration values obtained for 238U, 40K and 137Cs were
2.5, 50 and 1.5 Bq/kg, respectively. Activity concentration of 125Sb is
highly variable ranging from 21 to 7403 Bq/kg with an average value
of 193471089 Bq/kg (Table 1 and Fig. 2). These radioactivity data
can be attributed to the fact that these technetium generators
consist of fission products generated during the production of
99
Mo (IAEA, 1994) (IAEA technical document, 1999). It has been
reported that traces of other radioactive isotopes obtained as fission
products of 235U co-elute with 99Mo (El-Tahawy, et al. 1994). Never-
theless, 40K is not a fission product and its presence may be a result
of contamination during handling. The activity concentration of
125
Sb is highly variable owing to the various samples origins. The
presence of these radioactive isotopes in the spent technetium
generators is concerning, and their potential radiological effects
should be investigated. Given the presence of these long lived
radioactive nuclides with relatively high activities, we suggest that
spent 99Mo generators should be treated as radioactive waste.
However, the activity concentration of radioactive nuclides observed
here is significantly higher that reported in a similar studies (El-
Tahawy et al., 1994) (IAEA, 2009). The regression analysis has shown
that no correlation was found between 125Sb activity concentration
and surface dose levels (Fig. 3). Long-term exposure to relatively
high concentrations of antimony can cause irritation of the eyes, skin
and lungs. As exposure continues more serious health effects may
occur, including lung diseases, heart problems, diarrhea, severe
vomiting and stomach ache. It is not known whether antimony
can cause cancer or reproductive failure. Spent technetium gen-
erators are usually sent back to the producer where they are
Acknowledgments
The authors are extremely grateful to the staff of the Sudan
Atomic Energy Commission, Our sincere thanks are also extended to
Sahr Algadi, Hatem Himida, Rawia, Saddig Gumma, Abas Yassin,
Afra Sam for their kind assistance in sample collection and analysis.
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