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Feasibility Study Part – II

Theoretical Calculations of Fission 99Mo Production by


the Irradiation of LEU Metallic Uranium Foil at Tajoura
Research Reactor

Bsebsu, F. M.1,Elwaer S.2


Renewable Energies and Water Desalination Research Center
P.O. Box 30878 Tajoura (Tripoli), Libya

Abstract
The Renewable Energies and Water Desalination Research
Center (REWDRC), Libya, will implement the technology for 99Mo
isotope production using LEU foil target (This target is made of a
LEU metallic uranium foil inserted between two concentric
aluminium cylinders), to obtain new revenue streams for the
Tajoura nuclear research reactor and desiring to serve the Libyan
hospitals by providing the medical radioisotopes.
This paper will present the preliminary results for the
neutronic and activity calculations of 99Mo, taking into account
different irradiation and decay times.

1. Introduction
The Tajoura reactor is a pool type reactor, moderated and cooled by
light water located at the Renewable Energies and Water Desalinization
Research Center (REWDRC). The reactor is
designated to carry out experiments in field of
nuclear physics and nuclear engineering, 2VCV
4VCR
2VCR 1VCR 1VCV
3VCR
neutron activation analysis, solid state physics 6 5 4 1
4VCV 3 2 3VCV
and isotope production. The reactor was put 1

into operation at a power level of 10 MW in 6VCR 2 5VCR

September 1983. [1] 8VCR


3
7VCR
4

The reactor is completely converted to Low 10VCR 5 9VCR

Enriched Uranium (LEU, 19.7% of 235U) fuel of 6VCV


8VCV
6 5VCV
7VCV
14VCR 11VCR
type IRT-4M at the end of 2006; the new fuel is 10VCV 13VCR 12VCR 9VCV
16VCR 15VCR
an alloy (matrix) of aluminum and uranium- 18VCR 17VCR

dioxide (UO2–Al) with aluminum cladding. The 19VCR

moderation and core cooling are provided


through forced convection of de-mineralized
water. [2] Figure 1.
The compact core loading of Tajoura reactor Tajoura Reactor Core Horizontal
core consists of 16 IRT-4M fuel assemblies type Cross Section.
(10 (6TFA) + 6 (8TFA)) with LEU 19.7% 235U
enrichment.

1
Dr. Bsebsu, Farag Muftah, Reactor Department, Calculation Unit, Head of, Bsebsu@yahoo.com
2
Dr. Elwaer, Sami, Radiochemistry Department, Head of, samiwer@yahoo.com
The Tajoura reactor has 44 vertical irradiation channels (6 in the 8TFA fuel
assemblies, 9 in removable Beryllium reflector units, 19 VCR in the stationary
reflector blocks, and 10 VCV in reactor core Al vessel). Figure 1 shows the
Tajoura core horizontal cross section. The study of this analysis includes the
neutronic and activity analysis of 99Mo, where Figure 2 shows the LEU target
configuration, dimensions, and specifications [3]

Figure 2. LEU Target Horizontal, Vertical Cross Sections, and Dimensions.

2. Neutronic and Activity Calculations


The neutronic calculations were performed for the present core
configuration of Tajoura reactor using
neutronics computer package [4] codes, Table 1
Energy five-group structure used in
neutronic programs used routinely in the
the diffusion theory calculations
fuel management of this reactor. Broad Fine
Energy
Different cell models were needed to Grou Group
Interval [eV]
ps s
0.821 E+06 – 1.000
1 1– 5
E+07
6– 5.530 E+03 – 0.821
2
15 E+06
16 – 2.100 – 5.530
3
generate appropriate cross sections for the various reactor regions in an
energy five-group structure. The WIMS-D4 code was used to generate the
multi-group nuclear constants library for different regions as a function of
burn-up, the main transport calculation was performed in 69 energy groups,
condensing to 7 groups for the diffusion theory calculations as shown in Table
1.

In order to calculate the cross sections for fuel assembly, a complete


fuel assembly and a homogeneous extra zone was used. The extra region
includes the aluminum in the fuel elements beyond the width of the meat,
the aluminum side fuel elements, the water beyond the width of the meat
and the water channels surrounding the fuel element. In a diffusion
calculation, a fuel element will be represented by three zones, the central
zone is a homogenization of the meat, cladding and the cooling and the
lateral zones are identical to each other and are formed by a homogenous
mixture of aluminum and water. The nuclear constants for beryllium
elements, aluminum elements, blanking 225

elements, absorber tail plates and the water 200


as a reflector have been obtained using
175
different macro-cell models.
The fission product activities were 150

calculated using ORIGEN-S code from the 125

Activity, Ci
SCALE-4.4a system [5], considering an 100

irradiation at constant thermal neutron flux, 75

1.0×1014 n cm-2 s-1, and an irradiation time of 50

3 days for a target containing 8 gm of 25


uranium 19.75% enriched. The 99Mo activity in 0
curie as a function of time is shown in Figure 0 1 2 3 4 5 6 7 8 9 10 11 12
Time, days
3.

The irradiation time has a large impact Figure 3. Mo activity for 8 grams of
99

on specific activity. All the molybdenum 19.75% enriched uranium, an irradiation


time of 3 days and Φth = 1.0×1014 n cm-2
isotopes from 95Mo to 100Mo are produced from s-1
fission and they continue to build up, making
the 99Mo Ci content per gram of molybdenum material decrease with
increased irradiation time. A determination of the specific activity of the 99Mo
must consider the fission products which are stable isotopes of molybdenum
(97Mo, 98Mo and 100Mo). Table 2.
Activity of 99
Mo and Specific
The results of the ORIGEN-S [5] Activity of 99Mo, Asp, Ci per mg of
calculations during the irradiation period are Mo (97Mo, 98Mo, 99Mo and 100Mo) for
presented in the Table 2 and Figure 4, where Different Irradiation Times
Asp is the specific activity of 99Mo in Ci per t i, 99
Mo, Asp [Ci/mg
[h] [Ci] Mo]
mg of Mo. At end-of-irradiation (72 hrs), the 12 34.20 215,26
activity of 99Mo is 203 Ci, that is 25.38 Ci 16 45.21 211.16
99 24 67.23 208,50
Mo per gram of 19.75% enriched uranium
99 32 89.90 203.89
irradiated, the Mo yield after 10 hrs of 36 101.29 205,58
decay in pool is 183 Ci the specific activity of 40 112.81 202.67
99
Mo is 103.00 Ci per milligram of 48 134.84 200.65
60 175.08 200.65
molybdenum (97Mo, 98Mo, 99Mo and 100Mo), 72 203.12 199.25
the total activity of the actinides is 450 Ci/g U and the total activity of the
fission products is 3904 Ci/g U.
At the end of the irradiation, the LEU foil target will be allowed to decay
in the reactor pool for a period of 6 hours minimum. Prior to reactor start up,
the irradiated target will be removed from the reactor pool and transported to
the hot cell for disassembly. Allowing the target to decay in the reactor pool
for 6 hours will reduce the end-of-irradiation total fission product activity in
85.37%. [6]

3. Conclusions
The neutronic calculations were performed supposing that the target
would be introduced in the cell 6-1 position of the reactor grid in the
removable beryllium reflector, the present maximum neutron flux position of
Tajoura reactor. In this case, the mean neutron thermal flux is 1.0×10 14 n cm-2
s-1 and the power generated in the target is 7.6 KW.
The fission product activities have been calculated using ORIGEN-S
code from the SCALE-4.4a system, considering an irradiation at constant
thermal neutron flux, 1.0×1014 n cm-2 s-1, for Table 3.
Activity of 99Mo and Total Activity of Fission
a target containing 8 gm of uranium 19.75% Products, ATfp, in Ci/g U after 72 hours of
Irradiation and Different Decay Times
enriched, taking into account different td, 99
Mo, ATfp [Ci/mg
irradiation and decay times. [h] [Ci] Mo]
0 203.12 3904.00
The irradiation time has a large impact 1 201.72 1852.87
on specific activity. All the molybdenum 2 200.46 1060.70
isotopes from 95Mo to 100Mo are produced 3 199.24 753.93
4 198.04 635.14
from fission and they continue to build up,
99 5 196.86 589.13
making the Mo Ci content per gram of 6 195.71 571.32
molybdenum material decrease with 7 194.59 564.42
increased irradiation time. A determination 8 193.49 561.75
99 9 192.42 560.71
of the specific activity of the Mo must 10 191.36 560.31
consider the fission products which are 15 186.44 560.06
stable isotopes of molybdenum (97Mo, 98Mo 20 182.02 560.06
100
and Mo).

Acknowledgment
The authors wish to express their thanks to Dr. Faisel Abotweirat (Head
of Reactor Department) for supporting this work and
Dr Charlie Allen (Missouri University Research Reactor 216

(MURR), Columbia Research Reactor, and University of 214

Missouri) for his helping during the Origen results for 212

8 g LEU foil 210


Specific Activity of Mo

208

4. References 206 Asp(t)=197.97+28.24e


-td/23.22

204

1. KNOW-HOW DOCUMENTATIONS: "Tajoura 202

Nuclear Research Design", Building 1, Design 200

Features of the Control Rod Arrangement in the 198


10 20 30 40 50 60 70 80 90100110120130140150
Decay Time (td), [hrs]

Figure 4. 99
Mo Specific activity
as a function of Decay Time.
Reactor Ensuring Replacement with the Fuel Charge Pattern in the Core,
622-1-KH-151 (9), 1979.

2. Bsebsu, F. M.:”IRT- 4M Fuel Assembly Design and Calculation


Parameters”, Technical Report, REWRDC: R-CU2-01-2005, Tajoura (Tripoli)
Libya, 2005.01.31

3. Charlie Allen, Technical Drawing of LEU Target Assembly, Email massage,


2007.

4. Eduardo A. Villarino, MTR_PC V3.0, Neutronic, Thermal Hydraulic


and Shielding Calculations on PC, INVAP SE, Argentina, 2001.

5. Charlie Allen, ORIGEN Code Results for 8 g LEU foil, Email massage, 2007.

6. Jorge Medel, Fission Mo-99 Production by the Irradiation of a LEU Metallic


Uranium Foil at RECH-1 Reactor, Chilean Nuclear Energy Commission,
Santiago, Chile, January, 2007

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