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Calculation of photon attenuation coefficient and dose rate in concrete with the addition of SiO2 and MnFe2O4 nanoparticles using MCNPX code and comparison with experimental results

LOW ENERGY ACCELERATOR, RAY AND APPLICATIONS

Calculation of photon attenuation coefficient and dose rate in concrete with the addition of SiO2 and MnFe2O4 nanoparticles using MCNPX code and comparison with experimental results

M. Hassanzadeh
S. M. Sadat Kiai
Nuclear Science and TechniquesVol.29, No.11Article number 152Published in print 01 Nov 2018Available online 26 Sep 2018
47700

One of the most important safety features of nuclear facilities is the shielding material used to protect the operating personnel from radiation exposure. The most common materials used in radiation shielding are concretes. In this study, a Monte Carlo N-Particle eXtended (MCNPX) code is used to calculate the gamma-ray attenuation coefficients and dose rates for a new concrete material composed of MnFe2O4 nanoparticles, which is then compared with the theoretical and experimental results obtained for a SiO2 nanoparticle concrete material. According to the results, the average relative differences between the simulations and the theoretical and experimental results for the linear attenuation coefficient (μ) in the SiO2 nanoparticle materials are 6.4% and 5.5%, respectively. By increasing the SiO2 content up to 1.5% and the temperature of MnFe2O4 up to 673 K, μ is increased for all energies. In addition, the photon dose rate decreases up to 9.2% and 3.7% for MnFe2O4 and SiO2 for gamma-ray energies of 0.511 and 1.274 MeV, respectively. Therefore, it was concluded that the addition of SiO2 and MnFe2O4 nanoparticles to concrete improves its nuclear properties and could lead to it being more useful in radiation shielding.

ShieldingRadiationConcreteAttenuation coefficientPhoton doseMCNPX codeSiO2 and MnFe2O4 nanoparticles

1. Introduction

Concrete has been used in nuclear facilities for its physical strength and radiation shielding capability. It contains a mixture of low and high atomic number elements, and is therefore effective in shielding photons and neutrons. Lead is found to be another suitable option for shielding against X-rays and gamma-rays [1-3].

Nowadays, the use of nanoparticles in materials has attracted attention from researchers owing to a variety of features that have led to its use in a large number of applications [3-5]. Nanoparticles are used as a mixture to improve the mechanical and structural strengths of concrete. In general, the physical properties of nanomaterial are different from those of their bulk counterparts, and frequently display new and surprising phenomena, including the hardening of concrete [6-8]. Tao studied the microstructure and water permeability of concrete incorporated with SiO2 nanoparticles, herein referred to as Nano SiO2. He stated that the presence of nanoparticles can improve the resistance to water penetration in concrete specimens [9]. Moreover, an investigation using environmental scanning electron microscopy (ESEM) demonstrated that the concrete microstructure including Nano SiO2 led to a denser concrete microstructure and improved pore structure [7, 10].

In this study, for the first time, MnFe2O4 nanoparticles [11-12] are added to concrete to improve its nuclear properties. The linear and mass attenuation coefficients are calculated using point isotropic gamma-ray sources based on the Monte Carlo N-Particle eXtended (MCNPX) code, and the results obtained were compared with the experimental and theoretical results. In addition, the configuration and materials are simulated using the MCNPX code [13, 14]. Finally, the photon dose rate is calculated for a system of concrete and MnFe2O4 nanoparticles, herein referred to as Nano MnFe2O4 and compared to Nano SiO2 for different gamma-ray energies and weight percentages.

2. Materials and methods

2.1 Materials
2.1.1 Nano SiO2

The chemical analysis of Portland concrete and Nano SiO2 is given by Elsharkawy and Sadawy [1]. Nano concrete is formed by grinding the commercially available grade Portland concrete at a high energy [7]. Tables 1 and 2 show the concrete sample without Nano SiO2 and the concrete mixed with a weight percentage of 0.5% CaO in Nano SiO2, respectively. Table 3 shows the densities of Nano SiO2 at different weight percentages of SiO2 nanoparticles [1].

Table 1
Chemical analysis of Portland concrete, Ref. [1]
Chemical composition Weight (%)
SiO2 23.7
Al2O3 5.6
Fe2O3 3.3
CaO 63.7
MgO 1.4
SO3 0.2
K2O 1.2
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Table 2
Chemical composition of Nano SiO2, Ref. [1]
Chemical composition Weight (%)
CaO 0.5
SiO2 93.3
Al2O3 3.2
Fe2O3 1.7
MgO 0.3
SO3 0.1
K2O 0.1
N2O 0.1
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Table 3
Effect of SiO2 nanoparticle weight percentage addition to concrete on density, Ref. [1]
SiO2 nanoparticle percentage addition Density (ρ) (g/cm3)
0.0 2.15
0.5 2.17
1.5 2.30
2.0 2.26
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To study the nuclear attenuation properties, the compressive strength of hardened concrete cubic samples (7×7×7 cm3) is considered. A beam from both point and disk isotropic gamma-ray sources of 137Cs, with one line of energy of 0.662 MeV, 60Co, with two lines of energy of 1.17 and 1.33 MeV, and 22Na, with two lines of energy of 0.511 and 1.274 MeV, was used in the MCNPX code. Figure 1 shows the disk gamma-ray source and cubic concrete sample simulated by the MCNPX code. Figures 2a and b show the tracks of photons obtained from this code for the point and disk gamma-ray sources, respectively.

Fig. 1.
(Colro online)The disk gamma-ray source and the cubic concrete sample simulated using the MCNPX code
pic
Fig. 2.
(Color online) The tracks of photons simulated using the MCNPX code; a: point source, b: disk source
pic
2.1.2 Nano MnFe2O4

We have added MnFe2O4 nanoparticles to concrete with a weight percentage of 2.0% CaO at different temperatures, as shown in Tables 4 and 5. MnFe2O4 is a magnetic oxide, in which oxygen has a close packing structure with the Mn2+ and Fe3+ ions. These spinel ferrites are very promising candidates for understanding and controlling the magnetic properties of nanoparticles at the atomic level [11-12].

Table 4
Composition analysis of Nano MnFe2O4 concrete
Composition Weight (%)
CaO 2.0
SiO2 23.7
Al2O3 3.2
Fe2O3 1.7
MgO 0.3
SO3 0.1
K2O 0.1
N2O 0.1
MnFe2O4 68.8
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Table 5
Densities of Nano MnFe2O4 at different temperatures
Temperature (K) Density (ρ) (g/cm3)
300 4.373
573 4.773
673 5.194
773 4.745
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2.2 Methods
2.2.1 MCNPX code

The shielding material parameters are the most important for characterizing the penetration and diffusion of gamma-rays [15]. Theoretical modeling of the photon attenuation coefficients of the materials permits more flexibility and simplicity compared to experimental studies. The linear attenuation coefficients, μ, in materials are determined by the transmission method according to Beer- Lambert’s law [1, 15-17]:

μ.X=Ln(I0I), (1)

where I0 and I are the incident and attenuation photon intensities, respectively, μ (cm−1) is the linear attenuation coefficient, and X is the thickness of the slab. The mass attenuation coefficient is defined as μm (cm2 g-1) = μ (cm−1)/ρ (g/cm3).

In this work, the μ and μm coefficients are obtained by the MCNPX code at various photon energies: 511, 662, 1170, 1274, and 1332.5 keV. The concrete material content ratios have been defined relative to a sample material in this code. Calculations were performed for one million histories per run using Intel Core i7 CPU 3.40 GHz computers. The obtained statistical errors were less than 1% for a long run time. The flux integrated over a surface tally (F2) has been used in the μ and μm calculations [3, 17-19].

One of two methods can be used for the calculation of the photon dose rate in concrete samples that are useful for converting the flounce quantities to units of dose. The choice is between using a heating number method or one or more flounces-to-dose conversion functions. Both approaches are valid for photon dose rate calculations, but the use of conversion functions is recommended for dose equivalent and effective dose calculations [14, 20].

In the heating number method, the code calculates the absorbed dose on the basis of the KERMA approximation, which is locally deposited [14]. The KERMA approximation dose can be represented using the following equations:

D(GySourceparticle)=CNi=1Nj=1TσT(E)H(E), (2) C=(1.602×1010GyMev/g)(1×1024cm2barn)(NaηM), (3)

where Na is Avogadro’s number (6.022×1023 mol-1), η is the number of atoms per molecule, M is the molar mass in grams, is the fluence score in particles/cm2, σT is the total atomic cross section at energy of scoring track in barns, H is the heating number in MeV per collision, T is the number of scoring source particle tracks and N is the number of source particles.

The second method is the flounce-to-dose conversion function. In this method, the absorbed dose rate is calculated by using DFn (Dose Function) and tally F4 operations. Suppose one wanted to compute the dose rate of some type of flux tally, either total or by energy group. This feature allows you to enter a point wise response function (such as flux-to-dose conversion factors) as a function of energy to modify a regular tally. Therefore, the absorbed dose rate is calculated by combining the DFn and F4 cards. Finally, the DFn card is defined as follows:

DFnIU FAC IC INT (4)

where IU, FAC, IC and INT are the controls units, normalization factor for dose, standard dose function, and energy interpolation, respectively [14, 20].

3. Simulation, experimental, and theoretical results

3.1 Calculation of attenuation coefficients
3.1.1 Calculation of attenuation coefficients in Nano SiO2

The μ value was calculated by the MCNPX code, and is shown in Fig. 3. This figure presents the effects of varying gamma-ray energy with μ at weight percentages of 0.0%, 0.5%, 1.5% and 2.0% SiO2 in Nano SiO2, and compares these to the experimental results of ref. 1. Calculations have been carried out using a beam of point isotropic gamma-ray sources of 137Cs, with one line of energy of 0.662 MeV, 60Co, with two lines of energy of 1.17 and 1.33 MeV, and 22Na, with two lines of energy of 0.511 and 1.274 MeV. This figure illustrates that the values of μ decrease with increasing gamma-ray energies and that the maximum and minimum values of are found at the energies of 0.511 and 1.33 MeV, respectively. In addition, these parameters increase with increasing weight percentage of SiO2 nanoparticles until 1.5%, after which they decrease due to decreasing density. In general, the relative error in all these calculations is less than 1.0%.

Fig. 3.
(Color online) Effect of gamma energy on the μ at different SiO2 nanoparticle percentages
pic
3.1.2 Calculation of attenuation coefficients of Nano MnFe2O4

Figure 4 shows the effect of gamma-ray energy on μ for Nano MnFe2O4 with 2.0% CaO at 300, 573, 673, and 773 K. Figure 5 presents the same effect for Nano MnFe2O4 at different temperatures, as calculated by the MCNPX code. As shown in Figs. 4 and 5, the values of μ decrease with increasing gamma-ray energies and the maximum and minimum values of μ are found at 0.511 and 1.33 MeV, respectively. In addition, this parameter can be increased by increasing the density up to 5.194 g/cm3, as seen for the Nano MnFe2O4 temperature of 673 K.

Fig. 4.
(Color online) Effect of gamma energy on μ at different temperatures for Nano MnFe2O4
pic
Fig. 5
(Color online) Effect of temperature of Nano MnFe2O4 on μ for different gamma energies
pic
3.1.3 Comparison of SiO2 and MnFe2O4 nanoparticles

Figure 6 shows the μm of the SiO2 and MnFe2O4 nanoparticles constituting 2.0 wt.% in concrete for different gamma-ray energies. According to Fig. 6 a fairly good agreement with the experimental results was observed, notably in the simulation of Nano SiO2 with a density of 2.26 g/cm3, whereas for the theoretical results, a good agreement was obtained at the density of 2.47 g/cm3. The average relative differences between the simulation results and the experimental and theoretical results are 6.4%, 5.5% and 2.1% for the densities of 2.26 g/cm3 and 2.47 g/cm3, respectively. Moreover, as seen in this figure, the μm of the MnFe2O4 nanoparticles is much higher compared to that of the SiO2 nanoparticles, which is attributed to a higher density.

Fig. 6.
(Color online) Comparison of SiO2 and MnFe2O4 nanoparticles in concrete on the μm at different gamma energies
pic

As listed below, there are sources of uncertainty in the results of the MCNPX code in comparison to the experimental and theoretical results:

1. Inherent error in the probabilistic method of the MCNPX code,

2. Inherent error in this code due to the libraries used, especially the inability to define the cross-section of the nanoparticles,

3. Physical models used in the MCNPX code.

3.2 Calculation of dose rate
3.2.1 Calculation of dose rate in Nano SiO2 and MnFe2O4 nanoparticles

Table 6 and figure 7 show the effect of adding 2.0 wt.% SiO2 and MnFe2O4 nanoparticles to concrete on the photon dose rate at different distances from the point source for gamma-ray energies of 0.511 and 1.274 MeV. According to Table 6, the photon dose rate decreases at the average values of about 9.2% and 3.7% for the gamma-ray energies of 0.511 and 1.274 MeV, respectively. This difference is due to the larger μ in Nano MnFe2O4 in comparison to Nano SiO2 (as seen in Fig. 6).

Table 6
Comparison of SiO2 and MnFe2O4 nanoparticles in concrete: photon dose rates at different distances from the point source
X (cm) MnFe2O4-0.511 MeV SiO2-0.511 MeV Relative difference % MnFe2O4-1.274 MeV SiO2-1.274 MeV Relative difference %
4.0 1.30E-03 1.45E-03 -11.5 1.75E-03 1.81E-03 -3.4
5.0 9.76E-04 1.07E-03 -9.6 1.32E-03 1.37E-03 -3.8
6.0 7.59E-04 8.27E-04 -9.0 1.04E-03 1.08E-03 -3.8
7.0 6.07E-04 6.60E-04 -8.7 8.40E-04 8.72E-04 -3.8
8.0 4.98E-04 5.40E-04 -8.4 6.93E-04 7.19E-04 -3.8
9.0 4.15E-04 4.50E-04 -8.4 5.81E-04 6.03E-04 -3.8
10.0 3.52E-04 3.83E-04 -8.8 4.95E-04 5.14E-04 -3.8
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Fig. 7.
(Color online) Comparison of SiO2 and MnFe2O4 nanoparticles: the photon dose rate at different distances from the point source
pic

4. Discussion and conclusion

Generally speaking, the linear mass attenuation coefficients and photon dose rate of a shielding material depends on the quantity, type, and energy of radiation. It can be shown that most interactions of high energy photons with atoms occur through the Compton Effect, the strength of which depends on the atomic number and amount of primary energy of the gamma source. An increase in photon dose rate can occur owing to Compton reactions involving the photons and the concrete atoms. In addition, photoelectric interactions occur in low energy photons, which is a major mechanism of photon interactions with atoms. Furthermore, there is a greater probability of photon interaction at energies much greater than the K- and L-edge energies. When small quantities of nanoparticles are uniformly dispersed in concrete, they act as a nucleus to strongly bind with the concrete hydrates. This leads to a boost in concrete hydration due to their high activity, which is beneficial for the strength of the concrete. Whilst these nanoparticles are bound to the hydrates, they also prevent the crystals from growing, which could lead to a decrease in concrete strength. The loading of the concrete pores with nanoparticles therefore leads to an increase in the strength. Finally, Nano SiO2 can offer to the hydration process, producing more C-S-H via the formation of Ca(OH)2. In this study, the interaction between a concrete material in a cubic sample configuration and a point isotropic beam for a range of gamma-ray sources has been considered and simulated using the MCNPX code. The μ, μm, and photon dose rates have been calculated by this code, from which the statistical errors of the obtained parameters were determined to be less than 1%. According to the obtained μ results, the average relative differences between simulations and the theoretical and experimental results for Nano MnFe2O4 and Nano SiO2 were 6.4% and 5.5%, respectively. In addition, the photon dose rate decreases up to 9.2% for Nano MnFe2O4 and 3.7% for Nano SiO2 for gamma-ray energies of 0.511 and 1.274 MeV, respectively. Finally, the obtained results are in close agreement with both the experimental and theoretical data. Therefore, it can be stated that the obtained data from this code is a strong tool not only for obtaining μ and μm but also for calculating the photon dose rate. It can also be used for future work such as gamma spectroscopy in material characterization, detector design, and especially in investigations of shielding materials for nuclear reactors and high energy therapy facilities.

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