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International Conference on Advances in Nuclear Science and Engineering in Conjunction with LKSTN 2007 (23-26)

Neutronic aspect of Subcritical Assemby for Mo-99


Production (SAMOP) Reactor
Topan Setiadipura* , Elfrida Saragi
Computational Division PPIN-BATAN, Serpong, Indonesia2Affiliation, City, Country
*E-mail:tsdipura@batan.go.id

Abstract
NEUTRONIC ASPECT OF SUBCRITICAL ASSEMBLY FOR Mo-99 PRODUCTION (SAMOP)
REACTOR. Design of a subcritical assembly for Mo-99 production (SAMOP) is in progress at National Nuclear
Energy Agency. The main purpose of the project is to b able to produce Mo-99, which is a parent of Tc-99m an
important nuclide for nuclear medicine application. The major source of Mo-99 is from fission of U-235. The
conventional technique is by forming the uranium into targets and irradiated by neutrons from research or test
reactors, then the irradiated targets are dissolved and the Mo-99 is extracted from the solution. Another
technique to produce Mo-99 from U-235 is by using homogeneous reactor fueled with uranyl nitrate. This
method introduced by Ball in 1992 and some advantages compared with the conventional method. On the
SAMOP design, the low enriched uranyl nitrate is placed in the stainless steel container and irradiated by
neutron generator. In this paper, the neutronic aspect of the design will be reported. Including the criticality
analysis to secure the subcriticality of the design and the neutron flux distribution analysis, also the effect of the
graphite reflector. The neutronic analysis was using the general monte carlo code, MCNP.

Keywords: Mo-99, uranyl nitrate, subcritical, neutronic, monte carlo

product, 99Mo, is extracted from the solutions. In


1. Introduction
1992, Ball [2] introduced a method of "targetless"
99
Mo is used as a parent isotope of the production of fission product Mo-99 using an
widely used medical radiotracer 99mTc. It is estimated aqueous homogeneous reactor fueled with uranyl
that 99mTc is used in over 85%of all nuclear medicine nitrate. The design anticipated that the uranium salt
clinical studies in the world. The strong demand for could be made with low enriched uraniurn [3,4].
99mTc has stimulated a search for reliable supplies
of 99Mo [1].
Basically, there are two process or reaction
to produce 99mTc, fission from U-235 or capture
reaction of 98Mo as shown in the picture 1. The
fission yield of 99Mo is about 6.1%. The fission-
produced 99Mo has a high specific activity (~104 Ci
99
Mo /g Mo) which makes it the most important
source of 99Mo in the world. The fission technique,
however, requires considerable capital investment
and produces large quantities of radioactive waste.
The cross section of the 98Mo (n,γ) 99Mo reaction is
small (σth ~ 0.14 barns) and only a small portion of
the 98Mo is converted to 99Mo. The resulting specific
activity (~Ci 99Mo /g Mo) is much lower than that of Figure 1. Two different reaction to produce
the fission-produced 99Mo. Advanced generator 99
Tc from 99Mo.
technologies are required to produce high quality
99mTc generators from the capture-produced 99Mo. Subcritical Assembly for Mo-99 Production
For the fissioning process, the conventional (SAMOP) is designed at the PTAPB-BATAN based
way is to form the U-235 into a target which then on the Ball’s method. The core of the SAMOP is the
irradiated by neutrons from research or test reactor. Uranyl Nitrate solution in the SS-304 tank which
These irradiated targets are dissolved and the fission irradiated by the neutrons from a D-T neutron

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International Conference on Advances in Nuclear Science and Engineering in Conjunction with LKSTN 2007 (23-26)

generator. Geometrical data of the SAMOP design is Energy


given in the table below θ, degree Intensity
(MeV)
Table 1. Samop Geometrical Data 0 1,059 14.962
Parameter Value 10 1,048 14.948
Core tank (Inner tank) 20 1,046 14.906
Diameter 15.35cm 30 1,043 14.839
Height 35cm 40 1,038 14.748
Uranyl Nitrate Solution Height 30.7cm 50 1,031 14.637
SS-304 thick 0.3cm 60 1,024 14.509
Coolant Tank (Outer tank) 70 1,017 14.368
Diameter 80cm 80 1,008 14.220
Height 190cm 90 1,000 14.069
Distance Inner Tank – Reflector 1cm 100 0,992 13.919
Distance Inner Tank – Outer tank 40cm 110 0,984 13.776
based 120 0,976 13.642
130 0,969 13.523
140 0,964 13.421
150 0,959 13.339
2. Methodology
160 0,956 13.278
The neutronic calculation is done using
MCNP [6], a general purpose monte carlo code. To 170 0,954 13.241
do the calculation on the MCNP we modeled the 180 0,953 13.229
neutron source term from the neutron generator, the
geometry and material of the SAMOP reactor. The Uranyl Nitrate used in this calculation is enriched to
geometrical model of the SAMOP reactor on the 20%, and the Uranium concentration is 300 g/L. The
Visual Editor of MCNP is shown in the picture material composition of Uranyl Nitrate is given in the
below: table below

Table 3. Material composition of the Uranyl


Nitrate

Atomic Density
Nuclide
(atom/barn cm)
U-234 1.2977E-06
U-235 1.5374E-04
U-238 6.0591E-04
N 1.5219E-03
Figure 2. Geometrial model of the SAMOP H 5.5457E-02
reactor, from the side of the reactor (left) and O 3.3816E-02
from the top of the reactor. (right).
KCODE card is used to calculate the effective
Energy and intensity of the source neutron multiplication factor, k-eff, of the SAMOP core. And
as a function of the angle is modeled using several the F4 tally is used to calculate the flux distribution
probability distribution. The intensity distribution is of the SAMOP core. Using the F4 tally, the average
modeled using Source Information (SI) card for the neutron flux is estimated by summing the neutrons
cosines of the angle where the intensity is known and track length in the cells. The track length estimator is
the Source Probability (SP) card for the related generally quite reliable to because there are
intensity. Dependent Source (DS) cards is used for frequently many tracks in the cell (compared to the
the energy distribution because the energy is depends number of the collisions), leading to many
on the direction distribution. The intensity contribution to this tally[6]. To calculate the flux of
(normalized for the value of angle 90o degree) and different area of the core, F4 tally is applied to a
energy of the neutron source is given in the table small spherical cells with different position that
below [5] represented the area of the core. To simplified the
Table 2. Neutron source characteristic tallying, the height of the cells position is divided
into three level, and in each level there are nine cells
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International Conference on Advances in Nuclear Science and Engineering in Conjunction with LKSTN 2007 (23-26)

represented the center and the pheripery of the core at Effect of diferent Graphit Reflector Width

that level. The detail cells configuration and 0.99


numbering is shown in the figure below, 0.98

0.97

0.96

0.95

k-eff
0.94

0.93

0.92

0.91

0.9

0.89
0 5 10 15 20 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40
tebal reflektor (cm)

Figure 5. Effect of Diferent Graphite Reflector


Thicknes

From the calculation, the k-eff of the core without the


reflector is 0.92319 which is to low for the
Figure 3. Cell configuration for detail flux application. This k-eff can be increased by additional
calculation. (radial) reflector. The calculation shows that the
increase of the k-eff is more significant by using
The above figure picturing the cells of the berrylium reflector than using graphite reflector. The
upper level, with the center of the cell height is results also shows that using any reflector material,
27.55cm (from the base of the core tank), cells 17-25 there is a limitation of the k-eff, it can be higher even
for the middle level, and cells 26-34 for the lower the reflector thickness is increase.
level with the height of the cell’s center is 15.35 and The flux distribution inside the SAMOP
3.15 respectively. core for different reflector width is given in the figure

Flux Distribution
3. Results and Discussion
0.05
The k-eff that represented the criticality
condition of the SAMOP reactor is calculated for 0.045

different width of the reflector. In this calculation we 0.04

calculate for two reflector material berrylium and 0.035


N o rm a liz e d F lu x

graphit, each with different width starting from zero 0.03 sam_f3
to 40cm. 0.025 sam_f4
0.02 sam_g6
Effect of diferent Be Reflector Width
0.015
1.04
0.01
1.02
0.005
1
0
8
10
12
14
16
18
20
22
24
26
28
30
32
34

0.98

0.96 Cell Number


k-eff

below
0.94

0.92
Figure 6. Flux distribution of the SAMOP core
0.9
for different reflector width.
0.88

0.86 The above figure picturing the distribution for


0 5 10 15 20 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40
tebal reflektor reflector thickness 10cm, 5 cm and without reflector.
As the reflector getting thicker the flux is getting
Figure 4. Effect of Diferent Be Reflector Thicknes higher as expected. The results shows that the higher
flux is in the center of the core. The average flux in
the core for different reflector thickness are given in
the table below
25
International Conference on Advances in Nuclear Science and Engineering in Conjunction with LKSTN 2007 (23-26)

BATAN Yogyakarta for the opportunity to involve


Table 4. Flux average of the SAMOP core in the project.
for different reflector thickness
Reflector thickness Average flux (n/cm2-s)
0 (non reflector) 4.21e+9 References
5cm 6.85e+9
10cm 9.27e+9 1. S.C.Mo (1993), Production of 99Mo Using
16cm 1.16e+10 LEU and Molybdenum Targets, RERTR
Meeting 1993.
2. Ball,R.M.(1992), Testimony Before the
4. Conclusion Congressional Committee on U.S. Resources
The neutronic aspect of the SAMOP on the Production of Mo-99 with Aqueous
reactor design is already done including the Homogeneous Reactors, Mike Synar,
criticality of the core and the neutron flux Chairman.
distribution on the core. Regarding the criticality, it 3. Ball, R.M. (1994), Use of LEU in the Aqueous
is confirmed that the core is subcritic and the level Homogeneuos Medical Isotope Production
of the subcriticality, the k-eff, can be increase close Reacto, RERTR Meeting, Williamsburg,
to critical at least by using thicker reflector. And it Virginia 1994.
is investigated that the Be reflector is much more 4. Ball,R.M.(1995), The Mo-99 Solution, Nuclear
effective to increase the k-eff of the core. The Engineering International.
average flux in the core is about 1.16E+10 for the 5. Slamet Santoso (2007), Neutron Yield and
graphite reflector thickness 16cm where the k-eff Energy Calculation of thr Neutron Generator
value is between 0.97 – 0.98. for SAMOP, not published.
6. X-5 Monte Carlo Team (2003), “MCNP-A
General Monte Carlo N-Particle Transport
Code, Version 5 “ Vol.1, LA-UR-03-1987
Acknowledgment
The Authors would like to aknowledge
Prof. Sarip and the SAMOP Team at the PTAPB-

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