International Conference ECED 2013 – Eastern and Central European Decommissioning

June 18 - 20, 2013, Trnava, Slovakia

RADIONUCLIDE INVENTORY CALCULATIONS FOR

DECOMMISSIONING PURPOSES
Amine Bouhaddane, Gabriel Farkas, Vladimír Slugeň
Slovak University of Technology in Bratislava
Faculty of Electrical Engineering and Information Technology
Institute of Nuclear and Physical Engineering
amine.bouhaddane@stuba.com

Abstract: The paper briefly describes the issue of radionuclide inventory determination in
decommissioned nuclear power plants with emphasis on VVER-440 reactor type. According to induced
activity calculation, it will be possible to optimize the time frame and choose the appropriate
dismantling procedure during the disposal of reactor internal and external components in the
decommissioning of a nuclear power plant. Prerequisite for this calculation is the collection of reactor
operation data. In this paper, abilities of MCNP5 and MCNPX codes in this field are presented.

1. INTRODUCTION

In the decommissioning phase of a nuclear power plant, the vast majority of activity is
contained in the spent nuclear fuel. However, second largest radioactivity included in reactor
components (dummy elements, reactor shaft, baffle, reactor pressure vessel etc.) cannot be
neglected. After reactor operation and fuel removal, two categories of radionuclides are the
main contributors to the radioactive inventory: the activation products bound in the reactor
structural materials designated as induced activity and radionuclides from materials
contamination, which are activated corrosion and erosion products entrained by coolant,
dispersed fuel particles and fission products escaping through fuel leakage and settling on
the cover primary circuit components. In standard cases (no accident during operation) the
principal component of radioactive inventory is, in terms of reactor decommissioning, the
activation of its structural materials.

2. RADIOACTIVE PARAMETERS INFLUENCING THE RADIONUCLIDE INVENTORY

Activation is the process of creation of artificial radioactivity of structural materials by

neutron irradiation during reactor operation. This radioactivity is also referred to as the
induced activity. Activation products are localized and bound in the material contained in the
reactor core and its surroundings irradiated by neutrons. Neutron activated materials are
therefore structural materials inside the reactor pressure vessel, but also in the areas of the
reactor thermal and biological shield consisting of reinforced concrete [1] as well as in the
spent fuel pool and in the interim spent fuel storage baskets.
For all reactor types, the radionuclide composition of activated and contaminated materials
may vary within a very wide range. The variation is influenced by numerous factors, among
which the most important are: the integrated neutron flux, the duration of the operation and
the time elapsed after reactor shutdown. Apart from these important factors, the
radionuclide inventory remaining with-in nuclear power plants after permanent shutdown will
also be affected by the following parameters:
a) Reactor type, design, power level and shutdown period;
b) Composition of structural materials, including trace elements;
c) Operational parameters, e.g. chemistry of the heat transfer medium, and
maintenance;
d) Unplanned events [1].

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 International Conference ECED 2013 – Eastern and Central European Decommissioning
June 18 - 20, 2013, Trnava, Slovakia

3. NEUTRON INDUCED ACTIVITY CALCULATION FOR VVER-440

Calculation of activation of the reactor structural materials usually consists of neutron flux
and consequently induced activity calculation. The results thus obtained are verified by dose
rate measurements and by activation analysis of samples of the reactor structural materials.
The primary input data for computational determination of the reactor induced activity are:
the reactor operating history (duration of campaigns and shutdowns, fuel assembly loading
patterns), geometric and material configuration and chemical composition of the construction
materials. In my calculations, I use the MCNP5 and MCNPX neutron transport codes. To
create a model it is necessary to seek the geometry and dimensions in the reactor technical
documentation. The reactor operating history is part of the archived nuclear power plant´s
documentation (evaluation of reactor core operating characteristics for each unit and
campaign). Entering the chemical composition of materials is most complicated by the fuel
and moderator. It is necessary to consider the enrichment of used fuel elements, burnout
level (and related radionuclide composition of the fuel), the power levels, but especially the
calculation sensitivity to the distribution of previously mentioned parameters by fuel pin, rod
or whether it is possible to use mean distribution value. According to the operational
characteristics, the concentration of boric acid in moderator is determined and based on the
temperature and pressure, the corresponding coolant density value is assigned.

3.1 MCNP model

Based on the technical documentation from NPP in Jaslovské Bohunice Unit 1&2, it was
possible to create a simplified model of the VVER-440/V-230 reactor, which can be used for
further calculations. The model consists of the active zone and the reactor internal
components. It is a one sixth model which utilizes symmetrical geometry of this reactor type.
This model contains: the fuel assemblies with flat enrichment, control rods, dummy elements
and reactor internal structural parts (core support barrel, reactor shaft, reactor pressure
vessel). Thus, the main structural elements were preserved.

Figure 1. Horizontal section of the VVER-440/V-230 active zone model: 1 – RPV, 2 – austenitic and
reinforcing RPV weld pad, 3 –coolant, 4 – reactor shaft, 5 – core support barrel, 6 – dummy element,
7 – fuel assembly, 8 – control rod, 9 – 6th group control rod.

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 International Conference ECED 2013 – Eastern and Central European Decommissioning
June 18 - 20, 2013, Trnava, Slovakia

For this calculation, the MCNP5 code version 1.60 was employed along with continuous
energy spectra cross-section libraries ENDF/B-VII.0 and dosimetric data libraries LLLDOS.
MCNP is a general-purpose Monte Carlo radiation transport code for modeling the interaction
of radiation with matter. This code enables precise three-dimensional modeling of the active
zone and of the reactor internals. The main drawback of this calculational system is high
demand on computing resources. However, in the last few years, significant improvement in
the field of computer technology opened the door towards greater use of this method. On
the other hand, one of the main advantages is the use of the continuous-energy spectra in
neutron transport calculations, which allows achieving more precise results.
The requirements for the code of choice were: a well validated neutron physics
implementation, including access to established evaluated data files (ENDF/B –VII.0), a
possibility of isotope production via neutron capture, inelastic neutron scattering, elastic
scattering and other and more complex reaction channels, including multiple reactions.

3.2 MCNP5 calculation

In this section, the ability of MCNP5 to calculate the reaction rates was utilized. Potentially
occurring radionuclides are limited by the chemical composition of structural materials. Some
of them can be neglected due to their neutron-physical properties, e.g. low activation rate or
short half-life. Following nuclides which contribute the most to the activation of the
08Ch18N10T austenitic structural steel (structural material for fuel assemblies, control rods,
dummy elements etc.): Cr (50, 52, 53, 54), Mn (55), Fe (54, 56, 57, 58), Co (59), Ni (58, 60,
61 62, 64) and Mo (92, 94, 95, 96 ,97, 98, 100) and the most probable reactions: (n,γ),
(n,p), (n,d), (n,t) and (n,α) were monitored.
Based on the reaction rate (RR) calculation it was possible to determine the specific activity
of single radionuclides (Ai*):

Ai* = (1 − e − λτ ).RR (1)

-1
where λ[s ] is the decay constant and τ[s] is the irradiation time.
In Table 1 you can see the specific activities of selected radionuclides, which were produced
in the dummy elements during their first reactor campaign in EBO Unit 1 (after reducing the
zone and change of the loading pattern). The reactor operation data used in this task was
obtained from the document: Evaluation of the operational characteristics of the reactor core
VVER-440 Unit 1 in 13th campaign.

Table 1. Obtained MCNP5 results for the VVER-440/V-230 dummy element.

Specific induced
Radionuclide T1/2, radiation type σ [GBq/t]
activity [GBq/t]
51
Cr 27.7025 d, EC 1.29E+08 1.39E+05
55
Fe 2.73 y, EC 1.63E+07 2.63E+04
58
Co 70.86 d, EC, β+ 4.10E+06 4.05E+05
59
Fe 44.503 d, β- 2.69E+06 1.81E+04
54
Mn 312.3 d, EC, 1.73E+06 2.51E+02
60
Co 5.2714 y, β- 1.36E+06 1.94E+05
63
Ni 100.1 y, β- 2.97E+05 1.78E+02
59
Ni 7.6E04 y, EC 2.24E+03 1.34E+00
95
Nb 34.975 d, β- 9.73E+02 7.08E+01
57
Co 271.79 d, EC 6.48E+02 1.50E+01
93
Mo 4.0E03 y, EC, X 1.56E+02 9.39E-02

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 International Conference ECED 2013 – Eastern and Central European Decommissioning
June 18 - 20, 2013, Trnava, Slovakia

For better illustration, the calculated values were plotted (Figure 2). Due to relatively short
half-life, 51Cr was omitted from the chart (Figure 2). The results confirm, that the most
important radionuclides in the reactor components dismantling process are 55Fe (1st
decade), 60Co (10 - 50y) and 63Ni (during the whole process).

1,00E+08 55Fe

1,00E+07 58Co
59Fe
1,00E+06
54Mn
Ai [GBq/t]

1,00E+05
60Co
1,00E+04 63Ni

1,00E+03 59Ni
95Nb
1,00E+02
57Co
1,00E+01
93Mo
1,00E+00
0 10 20 t [y] 30 40 50
Figure 2. Specific activity of selected radionuclides in the dummy element during first 50 years after
irradiation.

3.3 MCNPX calculation

Newer versions of MCNPX (since 2.5.0) include the activation feature (via BURN card),
utilizing the CINDER’90 burnup code, since it follows the temporal burnup of fissionable
material and the associated production of fission products. It may also be called an
activation code since it well describes the conversion of stable nuclides to radioactive
nuclides by particle bombardment.
Recently, the combination MCNPX and CINDER’90 for neutron-induced activation simulation
was used in Ref. [2]. Radiation transport Monte-Carlo simulations were used to determine
induced activation as well as dose to environment. For this purpose, an appropriate code
system had to be chosen. The requirements for the code of choice were:
• a well validated neutron physics implementation, including access to
established evaluated data files, a possibility of isotope production via neutron
capture, inelastic neutron scattering, elastic scattering and other, more
complex reaction channels, including multiple reactions.
• Moreover, the ability to calculate the neutron-induced activity by means of the
produced isotopes and time-dependence of the radioactive inventory are
relevant selection criteria for the code [2].
In following simulation, MCNPX was used to calculate the total activity of a VVER-440/V-230
dummy element. The MCNP active zone model was employed again and the calculation was
performed under the same boundary conditions as previous calculation. The latest version
(2.7.0) of the MCNPX code [3] was utilized.

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 International Conference ECED 2013 – Eastern and Central European Decommissioning
June 18 - 20, 2013, Trnava, Slovakia

Table 2. Obtained MCNPX results for the VVER-440/V-230 dummy element.

T1/2,
Radionuclide radiation A [Bq]
type
51
Cr 27.7025 d, EC 8.72E+15
55
Fe 2.73 y, EC 1.04E+15
58 70.86 d, EC,
Co 1.51E+15
β+
59
Fe 44.503 d, β- 1.78E+14
54
Mn 312.3 d, EC, β- 1.88E+14
60
Co 5.2714 y, β- 1.63E+14
63
Ni 100.1 y, β- 1.61E+13
59
Ni 7.6E04 y, EC 1.29E+11
57
Co 271.79 d, EC 1.67E+12
93
Mo 4.0E03 y 1.85E+09
Total activity of selected
1.18E+16
radionuclides
Calculated total activity 2.90E+16

The total calculated activity 2.90x1016 Bq was determined for time t0 – directly after the
irradiation. This value is in good agreement with the activity values presented in [4], where
the values of activity for most inner reactor parts were in order 1016 Bq (basket, reactor
shaft). The essential part of this activity is carried by short-lived radionuclides. The most
important radionuclides in terms of decommissioning are listed in Table 2.
The trend of the activity is presented in Figure 3. Further calculations are needed to
incorporate more operational conditions and longer irradiation time into the simulation.
However, MCNPX appears to be a good tool to perform activation calculations.

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 International Conference ECED 2013 – Eastern and Central European Decommissioning
June 18 - 20, 2013, Trnava, Slovakia

55Fe
1,00E+17
1,00E+16
58Co
1,00E+15
1,00E+14 59Fe
1,00E+13
1,00E+12 54Mn
1,00E+11
1,00E+10 60Co
A [Bq]

1,00E+09
1,00E+08 63Ni

1,00E+07
59Ni
1,00E+06
1,00E+05
57Co
1,00E+04
1,00E+03 93Mo
1,00E+02
1,00E+01 Σ activity
1,00E+00 of selected
0 10 20 30 40 50 RN
t [y]
Figure 3. Course of the total activity of selected radionuclides in the dummy element during first 50
years after irradiation.

4. CONCLUSION

Numerous VVER-440 nuclear power plants are in operation in Central and Eastern Europe
and a small number have already been shut down. In addition to reactors already shut
down, many other reactors will reach the end of their design lifetime in a few years and
become candidates for decommissioning [5]. Activated materials should be classified
according to the waste classification criteria defined by the individual Member States [1]. On
the one hand, care must be taken to prevent over-classification leading to unwarranted
waste disposal costs, while, on the other hand, underclassification may result in regulatory,
health and safety implications. Induced radioactivity at facilities with sufficiently long
operating histories will be close to the point of equilibrium for strong γ emitters such as 60Co.
Hence, radiation dose rates can easily exceed the Gy/h range. As such, direct
characterization would be difficult, at best. Therefore, indirect means of characterization or
remotely operated devices may be required.

ACKNOWLEDGEMENTS

This project has been partially supported by the Slovak Grant Agency for Science through
grants VEGA 1/0204/13.

REFERENCES

[1] IAEA, „Radiological Characterization of Shut Down Nuclear Reactors for Decommissioning
Purposes,“ Vienna, October 1998.

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 International Conference ECED 2013 – Eastern and Central European Decommissioning
June 18 - 20, 2013, Trnava, Slovakia

[2] B. BROMBERGER, „Simulation of Radiation Doses and Activation in a Fast-Neutron and Gamma-
based Air-Cargo Interrogation System,“ rev. 2nd International Workshop on Fast Neutron
Detectors and Applications - FNDA 2011, Ein Gedi, Israel, November 2011.
[3] G. MCKINNEY, „MCNPX USER´S MANUAL, Version 2.7.0. LA-CP-11-00438,“ LANL, Los Alamos,
April 15 2011.
[4] SZABOLCS, C., FEHÉR, S., „Conclusions of Activation Analyses of Two Different VVER-440 NPPs,“
rev. AER Working Group C and G meeting, Paks, 23 May 2013.
[5] IAEA, The decommissioning of WWER type nuclear power plants, Vienna, January 2000.