Home Physical Sciences Variation in tungsten(vi) oxide particle size for enhancing the radiation shielding ability of silicone rubber composites
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Variation in tungsten(vi) oxide particle size for enhancing the radiation shielding ability of silicone rubber composites

  • Dalal A. Aloraini , Aljawhara H. Almuqrin , M. I. Sayyed and Mohamed Elsafi EMAIL logo
Published/Copyright: December 20, 2023
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Abstract

In this work, the attenuation properties of silicon rubber (SR) composites reinforced by both micro- and nano-sized Tungsten trioxide (WO3) particles are studied. Different SR composites with different combinations of micro-WO3 and nano-WO3 have been prepared. The main composite, SR-(WO3)60m (40% SR containing 60% micro-WO3), and other compositions were prepared by replacing percentages of microparticles with nanoparticles of WO3. The linear attenuation coefficient for these composites was measured in the range of 0.06–1.333 MeV. The existence of micro and nanoparticles together may result in enhanced interactions with incoming photons, leading to greater shielding. In other words, micro-WO3 and nano-WO3 have various sizes and surface areas. At 0.06 MeV, we notice a distinguished decrease in the half value layer (HVL) from SR-W60m to SR-W60n. The sequence of reducing HVL values (SR-(WO3)60m > SR-(WO3)60n > SR-(WO3)40m20n > SR-(WO3)20m40n > SR-(WO3)30m30n) suggest that the inclusion of both micro- and nano-WO3 contributes to more efficient radiation shielding compared to the reference material. The radiation shielding efficiency (RSE) for SR-(WO3)30m30n at 0.662 MeV is 38.40%. This means that if a beam of photons with energy of 0.662 MeV interacts with SR-W40m20n sample, only 38.12% of the photons are successfully absorbed or stopped, whereas the remaining 61.88% can pass through this sample. At 1.333 MeV, the lowest RSE is observed, which means that the prepared composites have weak attenuation ability at higher energy levels.

1 Introduction

Radiation protection materials are an essential part of the bigger plan to protect people and the environment from the harmful effects of ionizing radiation. There is a greater need than ever for radiation shielding that works and can be counted on due to the spread of technologies like nuclear power, medical imaging, and industrial processes that use radioactive materials (1,2,3). Gamma rays, X-rays, and high-energy particles are all examples of these. People having medical procedures, and people in the general public are exposed to less radiation (4,5,6). The use of micro and nanoparticles of tungsten trioxide (WO3) mixed with polymers is an interesting new development in this area. WO3 is added to the rubber at the micro and nanoscales to improve its ability to block radiation (7,8).

Lead and concrete have been used as shielding materials to block ionizing radiation for a long time because they have high atomic number and density. For instance, lead is hazardous when produced, used, or thrown away and pollutes the environment. Lead and concrete are less practical and more challenging to use in some circumstances due to their weight (9,10). Polymers can be formed into various shapes, making it possible to create designs that meet particular requirements. Particularly useful in settings like hospitals where conditions are not always ideal. Polymers can be less expensive than concrete and lead, which could reduce the project’s overall cost. Polymers present an exciting and successful method to enhance radiation shielding because of their unique qualities and capacity for shaping (11,12,13,14,15,16).

Silicon rubber (SR) is a beneficial substance that can be applied in various ways due to its unique characteristics and adaptability. SR is the best material for sealing and insulating electronic components due to its excellent electrical insulation properties and ability to shield electronic components from moisture and dust (17). It is used in the medical industry to create long-lasting, allergy-free implants and devices. It is used in the automotive industry to make hoses, gaskets, and seals because SR can withstand various temperature changes and chemical contact. It creates seals for windows, doors, and appliances because it is solid and flexible. Neither air nor water can escape from these seals. It can be utilized in ionizing radiation-related industrial and medical applications by combining it with materials like micro- and nano-WO3 (18).

Heavy metal oxides like WO3 must be used in radiation shielding, especially when combined with polymers. Polymers can only block some radiation in the environment because they are not very dense. It is possible to increase the overall density of polymers by incorporating dense substances like WO3, improving their ability to block radiation. WO3 effectively reflects ionizing radiation like gamma rays and X-rays because of its high atomic number and density (19). The capacity of polymers to absorb and scatter radiation increases when WO3 particles are added. Shielding solutions can be created that are lightweight, portable, efficient, and adaptable enough to handle the demands of numerous applications by combining these two factors. WO3 functions as a radiation shield because it offers sufficient protection and is simple to use. It fixes the polymer density issue and provides an environmentally friendly substitute for heavy metals (20).

Nanotechnology is a big part of modern scientific and technological progress (21), especially when using WO3 nanoparticles. These structures are between 1 and 100 nm in size. They have features that make them different from their bulk counterparts and give them several advantages in various fields. SR can block radiation with the help of WO3 nanoparticles. This is done by carefully controlling the size and location of the particles inside the material. Nanoparticles have more surface area per unit volume, which makes them more reactive and effective. Nanotechnology has made it possible to change the way things work so they can be used for many different things (22). The structure stays together better, and the particles are spread more evenly when a changed nanoparticle works well with polymers. Flexible, lightweight protective material solutions are easy to make and have many medical and industrial uses (23).

In previous related works (24,25), the authors discussed the effect of adding microparticles or WO3 nanoparticles to liquid silicone rubber, while in this work, the effect of the two sizes combined within the composite in different proportions is studied. In this work, different new SR composition has been prepared and the radiation shielding characteristics have been determined experimentally using high-pure germanium (HPGe) detector and different radioactive point sources (Cs-137, Co-60, and Am-241). The idea of the work is to study the attenuation coefficients of some SR composites containing micro and nanoparticles together in the same mixture with different ratios and the effect of these percentages on the shielding efficiency.

2 Materials and method

The materials used in this work are liquid silicon rubber (LSR) with its hardener and different sizes (micro and nano) of WO3. The LSR is a two-component system, where long polysiloxane chains are reinforced with specially treated silica. Component A contains a platinum catalyst and Component B contains methylhydrogensiloxane as a cross-linker and an alcohol inhibitor. The hardener for silicone rubber materials comprising a silane compound comprises a 2-hydroxy-propionic acid alkyl ester radical. Mix 100 parts by weight of SR with corresponding 5 parts by weight of hardener. The LSR was purchased from Al-Nasser Company in Alexandria, Egypt, with a density of 1.25 g·cm−3 and a melting point of 250°C. The WO3 microparticles were purchased from the Egyptian Chemical Company, and their purity rate was 99.3%, and their average particle size was 50  μ m , while the WO3 nanoparticles were purchased from the Nano Gate Company in Egypt. They were prepared chemically to obtain a purity percentage of 99.7%, and their average particle size was 25 nm. The characteristics of LSR and micro- and nano-WO3 was provided by Al Ghamdi et al. (25) and other related research works (26,27). The size and structure of both micro and nanoparticles of WO3 are resolved by scanning electron microscope (SEM) and transmission electron microscope (TEM) characteristics, respectively, as shown in Figure 1, where the average size of micro-WO3 was 30 ± 10  μ m , while the average size of nanoparticles was 40 ± 10  nm . The preparation of SR composite has been done according to the percentages reported in Table 1, where the composites have been mixed manually till they become homogenous and left for some time (around 24 hours) to become a flexible material, after that it can be measured. The SR-(WO3)60m was used as reference material to show the impact of nano and micro percentages together in the composite as well as the composite SR-W60m was prepared as reported previously (25).

Figure 1 
               SEM and TEM images of micro- and nano-WO3, respectively.
Figure 1

SEM and TEM images of micro- and nano-WO3, respectively.

Table 1

Composites’ compositions, codes, and densities

Codes Composition percentage wt% Density (g·cm−3)
SR WO3
Micro-WO3 Nano-WO3
SR-(WO3)60m 40 60 ̶ 2.365 ± 0.007
SR-(WO3)40m20n 40 40 20 2.374 ± 0.009
SR-(WO3)30m30n 40 30 30 2.380 ± 0.011
SR-(WO3)20m40n 40 20 40 2.375 ± 0.009
SR-(WO3)60n 40 ̶ 60 2.371 ± 0.006

The ingredients were mixed according to Table 1 to obtain a homogeneous composite and pour it into cylindrical molds with a thickness of 2 cm. The compositions have been measured experimentally to calculate the attenuation parameters using narrow beam technique consisting of HPGe detector, radioactive point sources, and lead collimator (28,29,30,31,32,33). The sources emit four lines, which are used in the measurements, from 0.060 MeV (emitted from Am-241) to 1.333 MeV (emitted from Co-60). The geometry of experimental technique is shown in Figure 2, where the linear attenuation coefficient (LAC) has been calculated according to Beer–Lambert attenuation law, where the mechanism of the measurements and equations of LAC and other attenuation factors such as half value layer (HVL) and tenth value layer (TVL) are mentioned in previous studies (34,35,36,37,38).

(1) LAC = 1 t ln C 0 C

(2) HVL = Ln ( 2 ) LAC

(3) TVL = 1 LAC

(4) RSE , ( % ) = 1 C C 0 × 100

where RSE is the radiation shielding efficiency, C and C 0 are the count rate in the presence and absence of SR composition according to the emitted photons which are detected by the HPGe detector and t represents the thickness of the composite.

Figure 2 
               The experimental setup for attenuation coefficient measurements.
Figure 2

The experimental setup for attenuation coefficient measurements.

3 Results and discussion

The experimental part in this work involved preparing different SR composites with different combinations of micro-WO3 and nano-WO3. The LAC for these composites was measured in the range of 0.06–1.333 MeV. Analyzing the radiation attenuation factors in the examined energy range for these composites gives insights into their gamma ray shielding performance. The LAC denotes how well a composite attenuates photons, with higher values indicating superior shielding ability. In Figure 3, we plotted the LAC for the prepared composites with WO3. Among the micro-WO3-containing composites (SR-(WO3)60m, SR-(WO3)40m20n, SR-(WO3)30m30n, SR-(WO3)20m40n, and SR-(WO3)60n), SR-(WO3)30m30n shows the highest LAC, followed by SR-(WO3)20m40n and SR-(WO3)40m20n. The high LAC value found for SR-(WO3)30m30n composite can be ascribed to the synergistic impact of combining both micro-WO3 and WO3 nanoparticles. This combination improves the overall gamma ray shielding features of the prepared SR samples. The existence of micro and nanoparticles may result in enhanced interactions with incoming photons, leading to greater shielding. In other words, micro-WO3 and nano-WO3 have various sizes and surface areas. The existence of nano-WO3 provides a larger surface area compared to micro-WO3, allowing more interactions with incoming photons, while if we add micro and nanoparticles together, this increases the surface area better, which increases the possibility of better interactions. On the other hand, SR-(WO3)30m30n, which contains micro- and nano-WO3, exhibits a comparatively high LAC, suggesting that micro- and nano-WO3 together have a favorable impact on radiation attenuation.

Figure 3 
               The variation in LAC values of prepared composites at different experimental energies: (a) at 0.060 MeV, (b) at 0.662 MeV, (c) 1.173 MeV, and (d) 1.333 MeV.
Figure 3

The variation in LAC values of prepared composites at different experimental energies: (a) at 0.060 MeV, (b) at 0.662 MeV, (c) 1.173 MeV, and (d) 1.333 MeV.

The smallest LAC value reported for SR-W60m may be ascribed to its composition consisting of micro-WO3. At 0.06 MeV, the interactions between the photons and micro-WO3 might lead to a comparatively lower attenuation ability compared to SR composites with nano-WO3 or a combination of micro- and nano-WO3.

In Figure 4, we calculated the ratios of LAC values for SR-(WO3)40m20n, SR-(WO3)30m30n, SR-(WO3)20m40n, and SR-(WO3)60n to the LAC value of SR-(WO3)60m. The evaluations of the ratios of LAC give useful information on the comparative radiation shielding performances of several SR composites. By normalizing the LAC values to the reference composite (i.e., SR-(WO3)60m), the ratios give a direct comparison of how the remaining composites perform with regard to radiation protection efficacy. This parameter helps distinguish which compositions display weaker or stronger radiation shielding in comparison with a standard material, helping in the estimation and optimization of SR composition for improved radiation protection utilizations. In the selected energy range, there appears to be a harmonious tendency in the ratios of LAC values for SR-(WO3)40m20n, SR-(WO3)30m30n, SR-(WO3)20m40n, and SR-(WO3)60n compared to the reference composite (i.e. SR-(WO3)60m). The ratios consistently varied between 1.095 to 1.263, suggesting that these composites in general exhibit moderately larger LAC values in comparison with SR-(WO3)60m. From Figure 4, the ratios higher than one imply that all the prepared composites have higher LAC than the reference composite (SR-(WO3)60m). This means that the four composites with nano-WO3 or combination of micro- and nano-WO3 are more efficient in shieling the photons compared to the reference sample. Also, Figure 4 shows that the composites with both micro- and nano-WO3 (SR-(WO3)40m20n, SR-(WO3)30m30n, and SR-(WO3)20m40n) have slightly higher ratios in comparison with the composite with only nano-WO3 (SR-(WO3)60n). This affirms that the addition of both particle sizes can participate to enhance radiation shielding.

Figure 4 
               The ratio factor between SR-(WO3)60m and other prepared SR composites.
Figure 4

The ratio factor between SR-(WO3)60m and other prepared SR composites.

We determined the HVL for the prepared composites and illustrated the findings in Figure 5. Analyzing the HVL data gives perspectives into the radiation shielding abilities of the prepared composites at varying energy ranges. Higher HVL values imply weaker radiation attenuation effectiveness, as a bigger thickness is required to shield the intensity of the photons by half. Comparing the HVL values for different compositions allows us to estimate which composite provides stronger or weaker shielding. At 0.06 MeV, we notice a distinguished decrease in the HVL from SR-(WO3)60m to SR-(WO3)60n. The sequence of reducing HVL values (SR-(WO3)60m > SR-(WO3)60n > SR-(WO3)40m20n > SR-(WO3)20m40n > SR-(WO3)60n) suggest that the inclusion of both micro- and nano-WO3 contributes to more efficient radiation shielding compared to the reference material, which is similar to the result obtained in the previous figure. At 0.06 MeV, a high numerical difference is found between the values of HVL for SR-(WO3)60m and SR-(WO3)60n. This numerical comparison confirms that SR-(WO3)60n, which consists of nano-WO3, has better radiation attenuation compared to SR-W60m. The lesser HVL value for SR-(WO3)60n implies that a smaller thickness is required to attain the same level of radiation shielding as SR-(WO3)60m, displaying the benefit of utilizing nano-WO3. At higher energies, the difference in HVL between SR-(WO3)60m and SR-(WO3)60n is more pronounced, which again show the better attenuation performance of the composite with nano-WO3 compared to the sample with solely micro-WO3.

Figure 5 
               The HVL of SR composite as a function of photon energy.
Figure 5

The HVL of SR composite as a function of photon energy.

We calculated the TVL for the composites and compared the HVL and TVL for SR-(WO3)60n and SR-(WO3)40m20n at 0.06 MeV (Figure 6). We note that the HVL is smaller than the TVL and this is correct for both composites given in Figure 6. For example, the HVL for SR-W60m is 0.15 cm, while its TVL is 0.51 cm. The HVL is lesser than the TVL since the HVL represents a quicker lessening in the intensity of the photons. When a beam of photons moves via a composite with a thickness equivalent to the HVL, its intensity decreases to 50%. But for the TVL, the intensity of the photons is decreased to only one-tenth of its initial level after moving through a thicker layer.

Figure 6 
               The TVL of SR composite as a function of photon energy.
Figure 6

The TVL of SR composite as a function of photon energy.

This link reflects the exponential nature of photons attenuation via a medium. This means that the intensity drops quickly when the thickness of the medium increases. Hence, the HVL is naturally leaser than the TVL.

In Figure 7, we plotted the mean free path (MFP) for the prepared composites. Clearly, at 0.06 MeV, the SR-(WO3)30m30n sample has the least MFP, followed by SR-(WO3)20m40n. This order suggests that, at this energy level, the inclusion of nano-WO3 in these two composites leads to a bit shorter distance photons can move compared to the other materials. SR-(WO3)60n, with a higher proportion of nano-WO3, also possesses a slightly reduced MFP in comparison with SR-(WO3)60m. With the increase in the energy of the photons, a similar pattern persists. The results at 0.662 MeV demonstrated that the addition of nano-WO3 leads to a reduction in the MFP, since the four composites with noano-WO3 have lower MFP than SR-(WO3)60m. The energy has a notable impact on the MFP of these composites, since the MFP for the current composites is in the order of 0.18–0.22 cm at 0.060 MeV, 4.22–4.95 cm at 0.662 MeV, and 7.04–7.71 cm at 1.333 MeV. If we compare the MFP for SR-(WO3)60m at 0.060 and 1.333 MeV, we found a very big difference between the MFP of this glass at these two energies. Specifically, the MFP at 0.060 MeV measures 0.22 cm, while at 1.333 MeV, it reaches 7.71 cm. This comparison between the MFP for SR-(WO3)60m at 0.060 and 1.333 MeV shows a substantial raise in MFP as the energy of the radiation increases. This high difference showcases the varying interaction processes between the incoming photons and the composites at different energy ranges. At 0.060 MeV, the comparatively small MFP value implies that the photons with energy of 0.06 MeV can move an average distance of about 0.22 cm within the SR-(WO3)60m sample before being attenuated. This suggests a quicker interaction between photons and the SR-W60m sample, leading to a faster reduction in intensity. Contrastly, at 1.333 MeV, the high MFP value of 7.71 cm indicates that photons with high energy can penetrate deeper into the SR-(WO3)60m, interacting over a longer distance before being shielded. The high MFP signifies a higher chance for the photons to move through the medium, leading to a slower decrease in the intensity over a greater distance.

Figure 7 
               The MFP of SR composite as a function of photon energy.
Figure 7

The MFP of SR composite as a function of photon energy.

We evaluated the RSE for the prepared composites with a thickness of 2 cm and the findings are shown in Figure 8. Apparently, the higher RSE (corresponds to smaller transmission of photons) occurs at 0.06 MeV. It is about 100% for all composites, indicating that these prepared SR with WO3 can stop all the incoming radiation with low energy (particularly with energy of 0.06 MeV). As the energy reached 0.662 MeV, we found a significant decrease in the RSE. This reduction in RSE implies a substantial influx of radiation with energy of 0.662 MeV that can penetrate the prepared SR with different WO3 contents. For instance, the RSE for SR-(WO3)40m20n at 0.662 MeV is 38.12%. This means that if a beam of photons with energy of 0.662 MEV interacts with SR-(WO3)40m20n sample, only 38.12% of the photons are successfully absorbed or stopped, whereas the remaining 61.88% can pass through this sample. At 1.333 MeV, the lowest RSE is observed, which means that the prepared composites have weak attenuation ability at higher energy levels.

Figure 8 
               The RSE of SR composite as a function of photon energy.
Figure 8

The RSE of SR composite as a function of photon energy.

In Table 2, we compared the MFP of SR-(WO3)40m20n, SR-(WO3)30m30n, and SR-(WO3)20m40n with five other samples (SR-BT40 and SR-BT50 (41) as well as S-2, S-3, and S-4 (42), which are different SR TeO2 composites as follows: SR-BT40 is composite with 50% per weight SR, 10% B2O3 and 40%; SR-BT50 is composite with 40% SR, 10% B2O3 and 50%; S-2 refers to 60% SR and 40% WO3-NPs; S-3 represents a mixing of 60% SR and 40% BaO-NPs; and S-4 represents a mixing of 60% SR, 20% BaO-NPs, and 20% WO3-NPs. At 0.06 MeV, among the given composites, SR-BT50 has the highest LAC (6.49 cm−1), implying its efficiency in shielding the photons. This is followed by S-3 (5.83 cm−1) and SR-W30m30n (5.72 cm−1), which illustrate good shielding performance. Moreover, S-2 (2.52 cm−1) has the smallest LAC value, implying relatively weaker radiation shielding. S-4 (4.24 cm−1) and SR-(WO3)40m20n (5.59 cm−1) lie within the mid-range in terms of protection efficiency. SR-(WO3)40m20n (5.59 cm−1) lies between the lower and higher LAC values of the given composites, positioning it as a moderately efficient shield. At 0.662 MeV, we found that SR-W30m30n has the highest LAC (0.242 cm−1), denoting its good performance in terms of radiation shielding at 0.662 MeV. This confirms that SR-(WO3)40m20n is especially well-suited for applications necessitating robust radiation protection. SR-(WO3)40m20n has a close LAC with SR-(WO3)30m30n, demonstrating its good ability to shield the radiation. Also, SR-W20m40n shows an LAC value of 0.239 cm−1, indicating its good attenuation features. The comparison at other energies is clear in Table 2.

Table 2

Comparison of present work with other published works

Codes LAC HVL MFP
0.060 MeV 0.662 MeV 1.333 MeV 0.060 MeV 0.662 MeV 1.333 MeV 0.060 MeV 0.662 MeV 1.333 MeV
SR-BT40 5.0424 0.1637 0.1141 0.1375 4.2348 6.0733 0.1983 6.1095 8.7619
SR-BT50 6.4890 0.1703 0.1220 0.1068 4.0713 5.6825 0.1541 5.8737 8.1981
S-2 2.5163 0.1589 0.1034 0.2755 4.3631 6.7039 0.3974 6.2947 9.6717
S-3 5.8280 0.1425 0.0970 0.1189 4.8641 7.1467 0.1716 7.0174 10.3105
S-4 4.2366 0.1504 0.1001 0.1636 4.6081 6.9279 0.2360 6.6481 9.9948
SR-(WO3)40m20n 5.5877 0.2400 0.1431 0.1240 2.8881 4.8437 0.1790 4.1667 6.9880
SR-(WO3)30m30n 5.7245 0.2423 0.1443 0.1211 2.8610 4.8020 0.1747 4.1275 6.9278
SR-(WO3)20m40n 5.5935 0.2399 0.1430 0.1239 2.8893 4.8481 0.1788 4.1684 6.9944

4 Conclusion

In this research, the variation in the size of WO3 particles inside SR and its effect on the efficiency of the material as a shield for ionizing radiation was studied. The LAC for these composites was measured in the range of 0.06–1.333 MeV. The existence of micro and nanoparticles together may result in enhanced interactions with incoming photons, leading to greater shielding. In other words, micro-WO3 and nano-WO3 have various sizes and surface areas. At 0.060 MeV, we notice a distinguished decrease in the HVL from SR-(WO3)60m to SR-(WO3)60n. The sequence of reducing HVL values ((SR-(WO3)60m > SR-(WO3)60n > SR-(WO3)40m20n > SR-(WO3)20m40n > SR-(WO3)30m30n)) suggest that the inclusion of both micro and nano-WO3 contributes to more efficient radiation shielding compared to the reference material. The RSE for SR-(WO3)30m30n at 0.662 MeV is 38.40%. This means that if a beam of photons with energy of 0.662 MEV interacts with SR-(WO3)30m30n sample, only 38.40% of the photons are successfully absorbed or stopped, whereas the remaining 61.18% can pass through this sample. At 1.333 MeV, the lowest RSE is observed, which means that the prepared composites have weak attenuation ability at higher energy levels. The current composites were compared with other flexible composites and good and effective results were obtained.

Acknowledgements

The authors express their gratitude to Princess Nourah bint Abdulrahman University researchers supporting Project number (PNURSP2023R57), Princess Nourah bint Abdulrahman University, Riyadh, Saudi Arabia.

  1. Funding information: The authors express their gratitude to Princess Nourah bint Abdulrahman University researchers supporting Project number (PNURSP2023R57), Princess Nourah bint Abdulrahman University, Riyadh, Saudi Arabia.

  2. Conflict of interest: There is no conflict of interest.

  3. Ethics approval: Not applicable.

  4. Consent to participate: Not applicable.

  5. Consent for publication: Not applicable.

  6. Data availability statement: All data generated or analyzed during this study are included in this published article.

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Received: 2023-09-02
Revised: 2023-10-17
Accepted: 2023-11-15
Published Online: 2023-12-20

© 2023 the author(s), published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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