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International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
Innovative neutron shielding materials composed of natural
rubber-styrene butadiene rubber blends, boron oxide and
iron(III) oxide
C Jumpee and D Wongsawaeng1
Department of Nuclear Engineering, Faculty of Engineering, Chulalongkorn
University, Bangkok, Thailand, 10330
E-mail: doonyapong.w@[Link]
Abstract. Optimized flexible and lightweight neutron shielding materials were
designed using the Monte Carlo N-Particle (MCNP) code. Thicknesses of 10 mm and
100 mm were tested for neutron shielding performances. Simulation results indicated
that the 10 mm shielding material of natural rubber (NR) and styrene butadiene rubber
(SBR) blend (1:1) with 60 part per hundred rubber (phr) boron oxide (B2O3) and 100
mm shielding material with four alternating layers of NR with 100 phr iron (III) oxide
(Fe2O3) and of NR and SBR blend (1:1) with 10 phr B2O3 were most suitable for
thermal neutron shielding and all-energy neutron shielding, respectively. Experimental
results verified the shielding efficiency of these optimal designs and ease of
fabrication.
1. Introduction
Neutron radiation is widely utilized in medical, agricultural and industrial applications. As neutrons
have no electrical charge, they can pass through an electron cloud to interact directly with the atomic
nucleus and transfer most of their energy to the nucleus with a mass close to that of a neutron. As the
human body has a high water content, there is a high density of hydrogen atoms present. The mass of
the hydrogen nucleus is close to that of the neutron. Therefore, exposure to free neutrons can be
hazardous, since the interaction of neutrons with molecules in the body can cause disruption to
molecules and atoms as well as cause reactions which give rise to other forms of radiation such as
protons with high Linear Energy Transfer (LET) [1], [2]. Neutron shielding requires materials with an
atomic mass close to that of the neutron. For example, hydrogen-rich materials are often used to shield
against neutrons, since ordinary hydrogen both scatters and slows down neutrons, after which neutrons
may be absorbed by an isotope exhibiting high affinity for adsorbing slow neutrons such as boron.
There have been several studies of polymeric composition containing materials with high neutron
cross section to determine their thermal neutron shielding properties. Materials made of polyethylene
or epoxy resin mixed with boron compound are widely used as neutron shielding materials, but they
usually exhibit sizable weight and volume, which results in low-flexibility performances [3], [4].
1
To whom any correspondence should be addressed.
Content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence. Any further distribution
of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.
Published under licence by IOP Publishing Ltd 1
International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
Flexible polymers such as natural rubber (NR) have been used as a matrix for neutron shielding
materials, but they only shield against thermal neutrons [5], [6].
There is considerable natural rubber cultivation in many areas of Thailand. This rubber is a
hydrocarbon polymer containing a large number of hydrogen atoms and can be easily fabricated into
flexible materials. In addition, borate minerals such as boracite, or boron compounds, are found in the
northeast of Thailand. Thus, not only is the production of neutron shielding materials comprising
natural rubber/ SBR blends and a borate material useful for neutron-related work, but it also utilizes
domestic resources.
The most effective neutron shielding material can be obtained by appropriately mixing high
hydrogen-content materials, heavy elements and thermal neutron absorbers. High hydrogen-content
materials can undergo elastic scattering with fast and intermediate-energy neutrons. Heavy elements
can undergo inelastic scattering with fast neutrons and can attenuate the secondary gamma ray
emission. Finally, neutron absorbers function to greatly reduce the number of thermal neutrons.
In this experimental work, rubbers, which are low-cost hydrocarbon polymers that can easily be
fabricated into many different products and shapes, were selected as the substrate of the composite
together with a very low-cost and often disregarded neutron absorbing material, B2O3. Fe2O3
(commonly known as rust), a very low-cost and usually disregarded material, was also utilized as the
heavy element in the composite.
The method of calculation for neutron shielding can be found in references [7], [8]. This research
incorporated inelastic scattering and shielding of secondary gamma ray emissions into the simulation.
The compositions of neutron shielding materials were optimized by Monte Carlo simulations using the
MCNP5 code to examine the neutron flux encompassing the entire range of interaction energy and
accounting for secondary gamma ray emissions.
Neutron attenuation experiments were carried out to verify neutron and secondary gamma ray
shielding performances of the designed neutron shielding materials using a simulated neutron source
(energy 1x10-8 – 100 MeV) and an Am-Be neutron source.
2. Materials and Methods
2.1. Material selection and MCNP simulation
The main raw materials were selected from simple elements or compound materials, taking into
consideration cost, radiation shielding performances and physical and thermal properties. The main
compositions of the selected neutron shielding material to shield against the entire range of neutron
energy and secondary gamma ray emission are listed in Table 1. They consisted of natural rubber
(NR), styrene butadiene rubber (SBR-1502 from BST elastomer Co., Ltd. Thailand) and neutron
absorber/scattering agent [boron oxide (B2O3), iron(III) oxide (Fe2O3) and lead dioxide (PbO2)]. 40 phr
of each agent was used for each sample because preliminary fabrication indicated that at 40 phr,
rubber still exhibited desirable properties. The lead or iron content is desirable for inelastic neutron
scattering to effectively bring the neutron energy down to lower-energy regions. In addition, lead and
iron are used for attenuation of gamma radiation. Neutrons in the lower-energy regions can be
moderated by hydrogen and other light elements by elastic scattering. In the thermal energy region,
boron (as B2O3) is used for neutron absorption. Because the interaction between a thermal neutron and
boron-10 produces a secondary gamma ray from the following interaction:
Thermal neutron + B-10 He-4 + Li-7* (478 keV gamma ray),
without the gamma ray attenuating material (Pb or Fe), this neutron shielding material would itself
become a significant source of gamma radiation.
For each sample in table 1, the input card of the MCNP5 transport code was appropriately prepared
for testing and comparison of shielding properties of different materials. A simplified model was
employed: a single radiation source, an isotropic emission of simulated neutron source with energy
1x10-8 – 100 MeV, was located at the center of a sphere filled with the shielding material as shown in
2
International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
figure. 1. The spherical shielding material was considered for shielding the neutron dose equivalent
rate [(rem/hr)/source strength] and the secondary gamma dose equivalent rate [(rem/hr)/source
strength]. The spherical model of radius 10 mm or 100 mm was chosen for neutron shielding in the
thermal region or in the entire-energy range, respectively, to ensure that all neutron particles interacted
with the shielding material at least one time before leaving the system. For each shielding material, the
dose equivalent rate per source strength was estimated on the outer surface of the sphere.
Table 1. Main compositions of considered neutron shielding materials
(40 phr each of B2O3, PbO2 and Fe2O3)
Element content (part per hundred rubber; phr)
Sample
No. of Density
No.
Material composition
layers (g/cm3)
H C B-10 B-11 O Fe Pb
0 0 No material (air) 0.00120 Air *
1 1 NR+SBR 0.987 10.378 89.622 - - - - -
2 1 NR+SBR+B2O3 1.210 10.378 89.622 2.460 9.963 27.577 - -
3 1 NR+SBR+PbO2 1.343 10.378 89.622 - - 5.351 - 34.649
4 1 NR+SBR+Fe2O3 1.301 10.378 89.622 - - 12.023 - 13.988
5 1 NR+SBR+B2O3+PbO2 1.273 10.378 89.622 1.230 4.982 16.464 - 17.325
6 1 NR+SBR+B2O3+Fe2O3 1.254 10.378 89.622 - - 19.800 - 27.977
Multi-layer samples
Layer 1 Layer 2 Layer 3 Layer 4 Layer 5
7 4 Sample 2 Sample 3 Sample 2 Sample 3 -
8 4 Sample 2 Sample 4 Sample 2 Sample 4 -
9 4 Sample 3 Sample 2 Sample 3 Sample 2 -
10 4 Sample 4 Sample2 Sample4 Sample 2 -
11 5 Sample 2 Sample 3 Sample 2 Sample 3 Sample 2
12 5 Sample 2 Sample 4 Sample 4 Sample 4 Sample 2
13 5 Sample 3 Sample 2 Sample 3 Sample 2 Sample 3
*[8] Air’s composition (weight fraction) ; Carbon : Nitrogen : Oxygen : Argon
0.000124 : 0.755268 : 0.231781 : 0.012827
3
International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
Figure 1. Schematic representation of the Monte Carlo model
Table 2. Ingredients for fabrication of most appropriate rubber compounds
Samples
Ingredient (phr) 10
1 2 4
Layer 1 Layer 2 Layer 3 Layer 4
NR 50 50 100 100 50 100 50
SBR-1502 50 50 0 0 50 0 50
ZnO 5 5 5 5 5 5 5
Steric acid 2 2 2 2 2 2 2
Wingstay-L 1 1 1 1 1 1 1
B2O3 0 60 0 0 10 0 10
Fe2O3 0 0 5 100 0 100 0
MBTS a 1.2 1.2 1.2 1.2 1.2 1.2 1.2
TMTD b
1 1 1 1 1 1 1
c
DPG 0.5 0.5 0.5 0.5 0.5 0.5 0.5
Sulfur 2.5 2.5 2.5 2.5 2.5 2.5 2.5
Compression molded
8 30 4 4 15 4 15
time (min.)
a
Dibenzothaizyledisulphide, b Tetramethylthigramdisulphide , c Diphenyl Guanidine
2.2. Fabrication of the shielding materials
Composite materials shown in table 2, which were the most appropriate rubber compounds after
MCNP simulation of all compounds listed in table 1, were fabricated by trial and error, as it was
unpredictable which composition would result in a stable compound. All rubber mixtures were
prepared in a two-roll mill of 8ʺ x 20ʺ in diameter with the working distance of 300 mm (speed of slow
roll 18 rpm) and the gear ratio of 1:4. Powders of B2O3, PbO2 and Fe2O3 were appropriately introduced
into the blend according to the recipe of compositions given in table 2. Mixing time was about 25
minutes. After compounding, the stock was left for 24 hrs to mature. The sheets were cut into slabs
4
International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
and then compression molded by an electrically-heated hydraulic press at 160±2 ºC and 4 MPa for a
suitable duration of each sample.
The homogeneity of each shielding material sample was verified by neutron radiography at the
Thai Research Reactor TRR-1/M1, which is a TRIGA-type reactor. A neutron imaging plate (ND
2040) attached to the shielding material by an aluminium tape was exposed to the neutron beam for 4
minutes. The neutron flux and the Cd ratio at the position of the shielding material were approximately
9 x 105 n cm-2 s-1 and 100, respectively. The neutron imaging plate was processed by an image reader
(BAS 2500).
2.3. Experimental work on neutron attenuation
The neutron attenuation experiment was carried out at the Radiation Measurement Laboratory at the
Nuclear Engineering Department, Faculty of Engineering, Chulalongkorn University to assess neutron
shielding performances of the selected shielding materials shown in table 2. Shielding materials were
slab shaped with thicknesses of 10 mm and 100 mm and dimensions of 150 mm x 150 mm. These
slabs were stacked together to a height of 20 cm. The Am-Be neutron source whose strength was 3.08
x 103 n cm-2 s-1 was placed at the bottom of the polyethylene (PE) source holder with a distance of 40
mm from the neutron shielding material, as illustrated in figure 2. The neutron measurement was
performed using a NE-905 glass scintillation neutron detector connected to a counting system.
Neutron Detector
6LiGlass scintillator
Sample
here Cadmium sheet
PE source holder
Figure 2. Geometry of the neutron transmission test.
3. Results and Discussion
3.1. MCNP Simulation
Results from the MCNP transport code revealed that the 10-mm thick sample #2 (NR+SBR+B2O3)
and 100-mm thick sample #10 (4 alternating layers of NR+Fe2O3/NR+SBR+B2O3) exhibited excellent
neutron and secondary gamma ray shielding performances, as seen in figures 3 and 4. For sample #2,
because the thickness of 10 mm was smaller than the mean free path of fast neutrons in rubber, only
thermal neutrons could be absorbed by this material, which also had the highest boron content. For the
100-mm thick sample #10, fast neutrons could undergo inelastic scattering with iron and elastic
scattering with hydrogen present in the rubber to become thermal neutrons and finally be absorbed by
boron. Thus, sample #2 and sample #10 are suitable for thermal neutron shielding and all-energy
neutron shielding, respectively.
5
International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
Figure 3. Total dose rate equivalent [neutron (1x10-8 – 100 MeV) and secondary
photon] on the outer surface of 10-mm radius sphere shielding sample.
Figure 4. Total dose rate equivalent [neutron (1x10-8 100 MeV) and secondary
photon] on the outer surface of 100-mm radius sphere shielding sample.
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International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
(a)
(b)
Figure 5. Total neutron dose rate spectra for various materials for 10 mm
thickness (a) and for 100 mm thickness (b).
Figures 5(a) and 5(b) illustrate the neutron shielding efficiencies at different energy regions. For
sample #2, the best shielding efficiency occurred in the thermal energy range (1x10 -8 – 1x10-2 MeV)
because boron exhibits a high thermal neutron absorption cross-section. In the fast neutron regime
(1x10-1 – 1x102 MeV), for 100-mm thick shielding designs, although not clearly visible in Figure 5(b),
7
International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
sample #10 outperformed sample #2 because the total neutron dose rate equivalent was lower in the
entire fast neutron energy range. Moreover, for sample #10, it also performed better than the NR/SBR
rubber compound (sample #1) and NR/SBR/Fe2O3 (sample #4) in the thermal energy range due to the
presence of the boron compound.
To further determine the optimized amount of B2O3 and Fe2O3 additions, a simulation of a 10 mm
thick sample #2 with varying amounts of B2O3 added from 0 to 70 phr was performed. Results are
shown in figure 6(a). As more B2O3 was added, the total dose rate equivalent became reduced and
appeared to saturate after about 60 phr. Thus, the most appropriate B2O3 addition for sample #2 was
chosen to be 60 phr. Moreover, a simulation of a 100 mm thick sample #10 with varying amounts of
B2O3 added from 0 to 70 phr and Fe2O3 added from 0 to 100 phr was performed. The reason why the
amount of Fe2O3 added was limited to 100 phr was because during a trial fabrication test, the rubber
became very rigid at 100 phr and more, making it much less flexible. Results in figure 6(b) revealed
that the most appropriate amounts were 100 phr of Fe2O3 and 10 phr of B2O3.
Total dose equivalent rate [(rem/hr)/neutron]
2.14E-08
2.13E-08
2.12E-08
2.11E-08
2.10E-08
2.09E-08
2.08E-08
2.07E-08
2.06E-08
2.05E-08
2.04E-080
5
10
20
30
40
50
60
70
80 70
60
90 50
40
100 30
20
10
(a) (b) 5
Figure 6. Total dose rate on outer surface of sphere neutron shielding at different mass ratios of
neutron absorber contents (Part per hundred rubber; phr) for (a) 10 mm of sample#2 and (b) 100
mm of sample#10.
3.2. Fabrication of rubber compound
The optimized designs according to the MCNP simulation were fabricated by trial and error. The
successfully-fabricated shielding materials with slab geometry are shown in figures 7(a) and 8(a).
Homogeneity was one of several factors determining the suitability of the fabricated shielding
materials. In reality, for the rubber compounds of samples #2 and #10, if they were left exposed to
moisture in room condition, B2O3 would quickly react with water vapour in the atmosphere, turning
into boric acid crystals, causing a problem with homogeneity. Thus, the samples must be completely
encased in a thin layer of conventional rubber compound. Therefore, figure 7(a) represents the rubber
compound encased in the green conventional rubber. In figure 8(a), because the rubber with iron oxide
didn’t require any encasement, the red slab represented the actual rubber compound. The
corresponding neutron radiographs displayed in figures 7(b) and 8(b) exhibiting a very even color tone
indicated that the neutron absorbing/scattering materials (B2O3 or Fe2O3) can be homogenously
dispersed in the rubber compounds of NR and SBR.
8
International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
Figure 7. (a) Front view and (b) side view of 10 mm (NR+SBR+B2O3 60 PHR: sample#2)
shielding material samples trial-produced to fabricate slab shape. (c) Neutron radiograph of this
shielding material (front view).
Figure 8. (a) Side view of 100 mm (4 layers: sample#10) shielding material samples trial-
produced to fabricate slab shape. (b) Neutron radiograph of this shielding material.
3.3. Neutron transmission test
From the neutron transmission test, the 10 mm rubber compound with 60 phr of B2O3 can reduce the
neutron dose from the Am-Be source by 53.91%. The 100 mm rubber compound composed of 4
alternating layers with 100 phr Fe2O3 and 20 phr B2O3 can reduce the neutron dose by 72.56%.
4. Conclusion
Optimized flexible and lightweight neutron shielding materials were designed using the MCNP code.
The neutron shielding materials with thicknesses of 10 mm and 100 mm were examined for neutron
shielding performances. Simulation results indicate that the 10 mm shielding material of NR and SBR
blend (1:1) with 60 phr B2O3, and the 100 mm shielding material having 4 alternating layers of NR
with 100 phr Fe2O3 and of NR and SBR blend (1:1) with 10 phr B2O3 were most suitable for thermal
neutron shielding and all-energy neutron shielding, respectively. Experimental results verified the
shielding efficiency of these optimal designs and the ease of fabrication. The designed shielding
materials are highly suitable for applications in nuclear science and technology.
Acknowledgments
This work was financially supported by the Graduate School, Chulalongkorn University and The
Commission on Higher Education under Strategic Scholarships for Frontier Research Network for the
Thai Ph.D. Doctoral Degree Program.
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International Nuclear Science and Technology Conference 2014 (INST2014) IOP Publishing
Journal of Physics: Conference Series 611 (2015) 012019 doi:10.1088/1742-6596/611/1/012019
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