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BY 4.0 license Open Access Published by De Gruyter Open Access April 23, 2022

Mechanical property evaluation of tellurite–germanate glasses and comparison of their radiation-shielding characteristics using EPICS2017 to other glass systems

  • Aljawhara H. Almuqrin , M. I. Sayyed EMAIL logo , J. F. M. Jecong , Nimitha S. Prabhu , Y. Raviprakash and Sudha D. Kamath
From the journal Open Chemistry

Abstract

In this study, four tellurite–germanate glasses containing zinc, lithium, and bismuth with varied Bi2O3 and TeO2 amounts were investigated. The mechanical qualities of sample glasses were investigated and associated with their structural properties. Furthermore, the radiation-shielding capabilities of N1–N4 glasses were evaluated at 0.662 MeV using EPICS2017. The radiation-shielding characteristics were compared with the radiation-shielding parameters published in the literature for various glass systems. When TeO2 was replaced with Bi2O3, Young’s and bulk moduli of the material decreased. The L values of glasses were higher than their S values (14–13 GPa), indicating that they can tolerate longitudinal stress better than shear stress and can be bent rather than elongated readily. The MACs calculated were comparable to those obtained using WinXcom. The tenth-value layer (TVL) of all of the sample glasses was higher than that of the bismuth aluminosilicate glasses. All of the borate glass systems containing bismuth, sodium, and antimony had lower TVLs than N1–N3 glasses. The half-value layer was more in the N4 glass with the greatest Bi2O3 content than those in 50 and 60 mol% PbO-containing strontium borate glasses.

1 Introduction

Radiation leakage is considered a serious issue that has a negative impact on human health and the environment. Since radioactive sources are being used in a wide range of human activities, effective protection against ionizing radiation is a must for a safe life. Hence, nuclear engineers are searching for better radiation barriers. Lead, a dense material, was traditionally employed in most radiation-shielding applications to protect medical personnel, the environment, and radiation workers. However, recent research studies have revealed that using lead as a shielding material raises some issues. Moreover, lead poisoning can occur when a person is exposed to extremely high quantities of lead in a short period of time [1,2,3,4,5]. To eliminate such concerns, materials including alloys, ceramics, glasses, nanomaterials, and others have been used to create low-cost, effective shields that are also environmentally friendly [6,7,8,9,10,11].

Glasses are excellent radiation shields due to their unique properties. Transparency to visible light, ease of preparation, and the ability to modify the composition during the fabrication process are some of their features [12,13,14,15]. Different glass systems have become a fundamental feature of modern architecture and a crucial part of medical devices; therefore, understanding their usage is important. Most importantly, glasses can protect us from the ionizing radiation found in space, oil, nuclear reactors, medical and dental facilities, universities, and research laboratories. However, the debate over which types of glasses are superior for radiation protection has been increasingly intense in recent years [16,17,18]. Lately, many computational and experimental works have been performed to develop an ultimate protection medium out of a variety of glass systems doped with various modifiers such as alkaline, alkali, oxides, and so on [10,11,12,16,18,19]. Researchers discovered that adding Bi2O3 to glasses improves their density [20,21] and refractive index [21]. Glass formers (B2O3, P2O5, and SiO2) are also significant glass constituents. Adding glass formers is fundamental to form ionic–covalent bonds with the oxygen atoms that constitute the structure of the glass.

Photon interaction data are required for the theoretical evaluation of a material’s radiation-shielding properties. Using EPICS2017, the most recent data library, the radiation-shielding properties of numerous materials were examined [22,23,24,25]. Even though the results were mostly comparable to those evaluated using old data libraries, namely, NIST-XCOM and EPDL97, the shielding properties measured near the K-edge absorption energies for materials containing elements with atomic numbers greater than 10 show the most significant difference between the results. Due to this, EPICS2017 is currently the most widely used data library for analyzing the radiation-shielding capabilities of any glass system [26,27,28,29].

This study looked at the mechanical properties of four tellurite–germanate glasses containing zinc, lithium, and bismuth. The radiation-shielding capabilities of these sample glasses at 0.662 MeV were also evaluated using EPICS2017. The half-value layer (HVL) and tenth-value layer (TVL) of sample glasses were also compared to the HVL and TVL of various glass systems published in the literature.

2 Materials and methods

2.1 Glass samples

The glass samples and compositions in this work are based on the research of Sayyed et al. [30]. They synthesized a series of tellurite–germanate glasses containing zinc, lithium, and bismuth, coded as N1, N2, N3, and N4, using the melt-quench method. The compositions of these Bi2O3–Li2O–ZnO–GeO2–TeO2 glasses are presented in Table 1. With Bi2O3 replacing TeO2, the glass density (ρ) increased from 5.1560 to 5.6405 g/cm3. The X-ray diffraction pattern indicated that these glasses were non-crystalline. The structural units in the network were validated using attenuated total reflectance Fourier transform infrared spectroscopy, and the optical bandgap and Urbach energy were determined using optical absorption spectroscopy [30].

Table 1.

The physical and mechanical properties of the Bi2O3–Li2O–ZnO–GeO2–TeO2 glasses

Glass Composition (mol%) [30] ρ (g/cm3) [30] PD Elastic constants (GPa) ϑ
Bi2O3 Li2O ZnO GeO2 TeO2 E K S L H
N1 0 10 10 10 70 5.1560 0.61 37 27 14 46 2.16 0.27
N2 5 10 10 10 65 5.3175 0.58 35 24 14 42 2.18 0.26
N3 10 10 10 10 60 5.4790 0.56 33 22 13 40 2.19 0.25
N4 15 10 10 10 55 5.6405 0.54 32 20 13 38 2.20 0.24

2.2 Mechanical properties

Sayyed et al. had only evaluated the sample glasses’ structural, optical, and radiation-shielding properties [30]. The sample glasses were explored further in this study by analyzing their mechanical properties and correlating them to their structural properties. The Makishima–Mackenzie theory [31] was considered for the determination of mechanical properties. The packing density (PD) of the glasses was calculated by the ratio of and V i x i V, where V i is the packing factor of each chemical in the glass and x i is its mole fraction. The parameter V i of each chemical in the composition was obtained by Makishima–Mackenzie theory which considers the ionic radii of the constituent elements in the chemicals. The dissociation energy per unit volume (G t) of the glasses was determined from the dissociation energy per unit volume for each constituent oxide using the density, molecular weight, and molar heat of formation of the oxide [31], the values of which were taken from ref. [32]. Using G t and PD, the elastic moduli, which are Young’s modulus (E), bulk modulus (K), shear modulus (S), longitudinal modulus (L), Poisson’s ratio ( ϑ ) , and microhardness (H), were calculated as follows [31]:

(1) E   =   2 G t PD ,

(2) K   =   1.2 PD   E ,

(3) S = 3 E K 9 K E ,

(4) L = K + 4 3 S ,

(5) ϑ = E 2 S 1 ,

(6) H = ( 1 2 ϑ ) E 6 ( 1 + ϑ ) .

2.3 Radiation-shielding parameters

In a multi-element system, the photon cross section (σ, in barns atom−1) is defined as a weighted sum of the cross sections of the constituent elements, as shown in equation (7), where f i is the atom fraction of the ith element.

(7) σ = f i σ i .

Equation (8) defines the total atomic cross section as the sum of partial cross sections where σ PE, σ coh, σ incoh, σ PP-N, and σ PP-E are the photoelectric, coherent, incoherent, pair production in the nuclear field, and pair production in the electron field (or triplet production) cross sections, respectively.

(8) σ T = σ PE + σ coh + σ incoh + σ PP-N + σ PP-E .

A related number termed the mass attenuation coefficient (MAC) (μ/ρ, in cm2/g) is proportional to the cross section. Equation (9) describes their relationship, where N A is Avogadro’s number, A i is the atomic mass of the ith element, ρ is the density of the material, and μ is the linear attenuation coefficient (in cm−1). Equation (10) describes the HVL, which is the length of the material that reduces the beam intensity by half. The TVL specified in equation (11) is the material length that reduces the beam intensity by one-tenth.

(9) μ ρ = σ T N A f i σ i ,

(10) HVL = ln 2 μ ,

(11) TVL = ln 10 μ .

The radiation-shielding properties of N1–N4 glasses were re-evaluated using EPICS2017 at 0.662 MeV, as previously determined by Sayyed et al. [30] using WinXcom software. Furthermore, the HVL and TVL of sample glasses were compared to the HVL and TVL of numerous glass systems published in the literature.

3 Results and discussion

3.1 Mechanical properties

The density (ρ) values of the N1–N4 coded glasses of the Bi2O3–Li2O–ZnO–GeO2–TeO2 system obtained by Sayyed et al. [30] are given in Table 1. The replacement of TeO2 with Bi2O3 resulted in a gradual increment in the density, which could be attributed to the substitution of the lighter atoms (Te) with heavier atoms (Bi). Figure 1(a) displays the trend in the molar volume (V) of the N1–N4 glasses, wherein the values derived by Sayyed et al. [30] demonstrated that the addition of Bi2O3 would increase the brittleness of this glass system due to volume expansion. The molar volume gradually increased from 22.75 to 28.95 cm3/mol when the Bi2O3 content was increased from 0 to 15 mol%. The increasing values of V suggested that the structure is becoming more open [33]. The calculation of the PD is another way to test this [33]. The trend in the PD of the N1–N4 glasses is shown in Figure 1(b), and the corresponding values are presented in Table 1. The PD of the glass system decreased from 0.61 to 0.54 with the addition of the Bi2O3 content, indicating that the glass structure is becoming more open. This could be due to the addition of Bi2O3 causing the formation of non-bridging oxygens (NBOs). Sayyed et al. [30] attributed the increase in the refractive index of this glass system upon Bi2O3 addition to the NBOs. Therefore, the increase in the molar volume and the decrease in the PD together confirm the role of Bi3+ ions as network modifiers via NBO production [20]. This supports the “open structure” concept, which is defined as the network voids’ inability to accommodate network-modifying ions without causing the glass matrix to expand [20].

Figure 1 
                  Trend in the (a) molar volume, (b) PD, and (c) elastic moduli of the N1–N4 glasses.
Figure 1

Trend in the (a) molar volume, (b) PD, and (c) elastic moduli of the N1–N4 glasses.

The mechanical properties of the glasses are given in Table 1. The trend in the elastic moduli (E, K, S, and L) of the N1–N4 glasses is shown in Figure 1(c). Young’s modulus, which is defined as the ratio of stress and strain, is a measure of the stiffness of material. The values of E slightly reduced from 37 to 32 GPa with Bi2O3 E addition from 0 to 15 mol%, implying that the matrix stiffness is decreasing. The bulk modulus also decreased from 27 to 20 GPa with successive Bi2O3 addition. The values of L of the glasses (46–38 GPa) were greater than their corresponding S values (14–13 GPa), indicating that the glasses can withstand longitudinal stress better than shear stress and can be bent easily rather than elongated. ϑ , the ratio of the transverse and longitudinal strains when tensile force is exerted, ranged from 0.27 to 0.24.

3.2 Radiation-shielding properties

Figure 2 shows the MACs of the four sample glasses at 0.662 MeV evaluated using the EPICS2017 data library. The calculated MACs are comparable to those MACs obtained using WinXcom software. It can be seen from the figure that as more TeO2 oxide is replaced with Bi2O3 oxide, the MAC increases. N4 has the highest MAC among the glass samples because it contains the most Bi2O3 oxide. This is to be expected since Bi2O3 (16.80 barns atom−1) has a far larger cross section than TeO2 (6.62 barns atom−1). It is worth noting that, as demonstrated in equation (9), the MAC is proportional to the cross section.

Figure 2 
                  MAC of the N1–N4 glasses at 0.662 MeV evaluated using EPICS2017.
Figure 2

MAC of the N1–N4 glasses at 0.662 MeV evaluated using EPICS2017.

As mentioned earlier, TVL is the shield thickness at which the intensity of the gamma-photons declines by one-tenth [34], while the HVL is the shield thickness of the material needed to decrease the intensity of the gamma-rays by half [35,36]. Hence, a material with a lower TVL and HVL is a better shield, as a smaller thickness is sufficient to attenuate the radiation by the required factor.

The TVLs of N1–N4 glasses were compared to those of other glass systems with comparable properties [35,36,37,38,39,40]. The comparison of TVLs of the N1–N4 glasses to those of the bismuth aluminosilicate glasses examined by Singh et al. [37] at 0.662 MeV is shown in Figure 3. The TVL of the N1 glass was 5.99 cm, whereas the TVL of the N4 glass was 4.67 cm. From N1 to N4, the TVLs of the sample glasses decreased. This indicates that among the samples analyzed, the N4 glass is the best shield. All of the sample glasses had higher TVLs than the bismuth aluminosilicate glasses. This could be due to the fact that the density of the N1–N4 glasses varied between 5.1560 and 5.6405 g/cm3, but the density of the compared glass system was between 5.412 and 5.768 g/cm3.

Figure 3 
                  TVL comparison of the N1–N4 glasses with bismuth aluminosilicate glasses [37].
Figure 3

TVL comparison of the N1–N4 glasses with bismuth aluminosilicate glasses [37].

As shown in Figure 4, the TVLs of the sample glasses were compared with those of the lithium-containing lead borate glasses examined by Kumar [38]. The TVLs of all of the sample glasses were higher than that of the PbO–Li2O–B2O3 glass system under consideration.

Figure 4 
                  TVL comparison of the N1–N4 glasses with lead lithium borate glasses [38].
Figure 4

TVL comparison of the N1–N4 glasses with lead lithium borate glasses [38].

Abouhaswa et al. studied a borate glass system containing bismuth, sodium, and antimony [39]. The TVLs of the sample glasses compared to that of the one they studied are shown in Figure 5. The TVLs of the N1–N3 glasses were greater than those of all B2O3–Bi2O3–Na2O2–Sb2O3 glasses, but the TVL of the N4 glass with the highest bismuth mol% (4.67 cm) was comparable to that of the 45B2O3–20Bi2O3–20Na2O2–15Sb2O3 (4.61 cm) glass.

Figure 5 
                  TVL comparison of the N1–N4 glasses with antimony sodium boro-bismuth glasses [39].
Figure 5

TVL comparison of the N1–N4 glasses with antimony sodium boro-bismuth glasses [39].

The TVL of a bismuth sodium borate glass system developed by Cheewasukhanont et al. [36] was compared to those of the sample glasses, as shown in Figure 6. The following trend was observed: the TVL of the N1 glass (5.99 cm) was lower than that of the 15Bi2O3–20Na2O–65B2O3 glass (6.53 cm), the TVL of the N2 glass (5.44 cm) was lower than that of the 20Bi2O3–20Na2O–60B2O3 glass (5.59 cm), the TVL of the N3 glass (5.01 cm) was lower than that of the 25Bi2O3–20Na2O–55B2O3 glass (5.21 cm), and the TVL of the N4 glass (4.67 cm) was lower than that of the 30Bi2O3–20Na2O–50B2O3 glass (4.82 cm). The TVL of N4 glass (with 15 mol% Bi2O3) was substantially lower than that of a Na2O–B2O3 glass containing 15 mol% Bi2O3. This indicates that incorporating not just Bi2O3 but also Li2O, ZnO, GeO2, and TeO2 into the glass has helped enhance the attenuation power.

Figure 6 
                  TVL comparison of the N1–N4 glasses with bismuth sodium borate glasses [36].
Figure 6

TVL comparison of the N1–N4 glasses with bismuth sodium borate glasses [36].

The TVLs of N1–N4 glasses were compared with those of the lead strontium borate glasses investigated by Kaundal et al. [35], as seen in Figure 7. The N2 glass had a TVL of 5.44 cm, which was comparable to those of the 10SrO–30PbO–60B2O3 (5.50 cm) and 20SrO–30PbO–50B2O3 (5.42 cm) glasses. Although the TVL of the N4 glass (4.67 cm) was higher than those of 50 and 60 mol% PbO-containing strontium borate glasses (4.60 and 4.25 cm, respectively), the TVL of this PbO-free glass was lower than those of 10, 20, and 30 mol% PbO-containing strontium borate glasses.

Figure 7 
                  Comparison of the TVL of the N1–N4 glasses with lead strontium borate glasses [35].
Figure 7

Comparison of the TVL of the N1–N4 glasses with lead strontium borate glasses [35].

As shown in Figure 8, the TVLs of the N1–N4 glasses are compared with that of the PbO–WO3–Na2O–MgO–B2O3 glass system investigated by Almuqrin et al. [40]. The comparison revealed that the N4 glass with the lowest TVL in this work had a value of 4.67 cm, which was even lower than the PbO-containing glasses such as 30PbO–10WO3–10Na2O–10MgO–40B2O3 (5.55 cm) and 35PbO–10WO3–10Na2O–10MgO–35B2O3 (5.12 cm).

Figure 8 
                  Comparison of the TVL of the N1–N4 glasses with PbO–WO3–Na2O–MgO–B2O3 glasses [40].
Figure 8

Comparison of the TVL of the N1–N4 glasses with PbO–WO3–Na2O–MgO–B2O3 glasses [40].

Figure 9 shows the computed HVLs of the N1–N4 glasses. The highest HVL was 1.80 cm for the N1 glass, while the lowest was 1.40 cm for the N4 glass. The HVL showed a decreasing trend from N1 to N4. This suggests that among the examined samples, the N4 glass is the best shield.

Figure 9 
                  Comparison of the HVL of the N1–N4 glasses with lead strontium borate glasses [35].
Figure 9

Comparison of the HVL of the N1–N4 glasses with lead strontium borate glasses [35].

The HVLs of the N1–N4 glasses were compared to those of other similar glasses [35,36]. Figure 9 compares the HVLs of N1–N4 glasses with those of lead strontium borate glasses studied by Kaundal et al. [35] at 0.662 MeV. The HVL of the N1 glass (1.80 cm) with no Bi2O3 content was lower than those of lead glasses such as 20SrO–10PbO–70B2O3, 10SrO–20PbO–70B2O3, and 20SrO–20PbO–60B2O3. The HVL of the N2 glass (1.63 cm) was comparable to those of 10SrO–30PbO–60B2O3 (1.65 cm) and 20SrO–30PbO–50B2O3 (1.63 cm) glasses. The N4 glass with the highest Bi2O3 concentration had HVL greater than those of 50 and 60 mol% PbO-containing strontium borate glasses. Yet, the HVL of this glass was lower than those of 10, 20, and 30 mol% PbO-containing strontium borate glasses, suggesting that this glass material has the potential to be a lead-free radiation shield.

Figure 10 shows the HVLs of the N1–N4 glasses at 0.662 MeV compared to those of some bismuth sodium borate glasses studied by Cheewasukhanont et al. [36]. The HVL of the N1 glass (1.80 cm) was substantially lower than that of the 15Bi2O3–20Na2O–65B2O3 glass (1.96 cm), while the HVL of the N2 glass (1.63 cm) was slightly lower than that of the 20Bi2O3–20Na2O–60B2O3 glass (1.68 cm). The HVL of the N4 glass (1.40 cm) was lower than those of 15Bi2O3–20Na2O–65B2O3, 20Bi2O3–20Na2O–60B2O3, 25Bi2O3–20Na2O–55B2O3, and 30Bi2O3–20Na2O–50B2O3 glasses but greater than those of 35Bi2O3–20Na2O–45B2O3 (1.38 cm) glasses. However, the HVL of the N4 glass (1.40 cm) containing 15 mol% Bi2O3 was much lower than that of the bismuth sodium borate glass with 15 mol% Bi2O3 (1.96 cm). This could be due to the higher density of the N4 glass (5.6405 g/cm3) compared to the 3.76 g/cm3 density of the 15Bi2O3–20Na2O–65B2O3 glass.

Figure 10 
                  Comparison of the HVL of the N1–N4 glasses with bismuth sodium borate glasses [36].
Figure 10

Comparison of the HVL of the N1–N4 glasses with bismuth sodium borate glasses [36].

4 Conclusion

We investigated the mechanical properties of tellurite–germanate glasses containing zinc, lithium, and bismuth with varied Bi2O3 and TeO2 contents. Also, the radiation shielding capabilities of these glasses were evaluated at 0.662 MeV using EPICS2017. We compared the radiation-shielding parameters of these glasses with various glass systems reported in the literature. We found that when TeO2 was replaced with Bi2O3, Young’s and bulk moduli of the material decreased. The MACs calculated via EPICS2017 for the tellurite–germanate glasses are comparable to those obtained using WinXcom. The TVLs of all of the selected glasses were higher than those of the bismuth aluminosilicate glasses. Moreover, all borate glass systems containing bismuth, sodium, and antimony had lower TVLs than the N1–N3 glasses. The HVL of the N1 glass (1.80 cm) was substantially lower than that of the 15Bi2O3–20Na2O–65B2O3 glass (1.96 cm), while the HVL of the N2 glass (1.63 cm) was slightly lower than that of the 20Bi2O3–20Na2O–60B2O3 glass (1.68 cm).

Acknowledgement

The authors express their gratitude to Princess Nourah bint Abdulrahman University Researchers Supporting Project number (PNURSP2022R2), 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 (PNURSP2022R2), Princess Nourah bint Abdulrahman University, Riyadh, Saudi Arabia.

  2. Author contributions: Conceptualization: A.H.A., M.I.S., and N.S.P.; methodology: M.I.S., J.F.M.J., and N.S.P.; software: J.F.M.J.; validation: N.S.P. and R.Y.; formal analysis: M.I.S. and R.Y.; investigation: A.H.A., M.I.S., R.Y., and S.D.K.; resources: J.F.M.J.; data curation: N.S.P. and R.Y.; writing – original draft preparation: A.H.A., M.I.S., J.F.M.J., and N.S.P.; writing – review and editing: A.H.A., S.D.K.; and N.S.P.; visualization: J.F.M.J. and M.I.S.; supervision: S.D.K.; project administration: A.H.A. and M.I.S.; funding acquisition: A.H.A. All authors have read and agreed to the published version of the manuscript.

  3. Conflict of interest: The authors declare no conflict of interest

  4. Ethical approval: The conducted research is not related to either human or animal use.

  5. Data availability statement: The data presented in this study are available on request from the corresponding author.

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Received: 2022-02-24
Revised: 2022-03-21
Accepted: 2022-03-29
Published Online: 2022-04-23

© 2022 Aljawhara H. Almuqrin et al., published by De Gruyter

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

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