γ-ray shielding features and crystallization of TiO2 borotellurite glasses

γ-ray shielding features and crystallization of TiO2 borotellurite glasses

Journal of Non-Crystalline Solids 526 (2019) 119720 Contents lists available at ScienceDirect Journal of Non-Crystalline Solids journal homepage: ww...

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Journal of Non-Crystalline Solids 526 (2019) 119720

Contents lists available at ScienceDirect

Journal of Non-Crystalline Solids journal homepage: www.elsevier.com/locate/jnoncrysol

γ-ray shielding features and crystallization of TiO2 borotellurite glasses a,⁎

b

a

Y.S. Rammah , A.A. Ali , F.I. El-Agawany a b

T

Physics Department, Faculty of Science, Menoufia University, Shebin El Koom 32511, Egypt Glass Research Department, National Research Centre, Dokki, Cairo, 12622, Egypt

ARTICLE INFO

ABSTRACT

Keywords: Glasses Crystallization γ-ray (µ/ρ) (HVL) (MFP)

Glasses of composition (60B2O3 –10 Na2O – 20TeO2 – (10-x) CaO) + xTiO2 where x ranged from 0.5 to 3 mol% have been prepared and coded as BTNCT0.0 (x = 0), BTNCT0.5 (x = 0.5), BTNCT 1.0 (x = 1.0), BTNCT2.0 (x = 2.0), and BTNCT3.0 (x = 3.0). Glass transition temperature (Tg) and crystallization temperature (Tc) have been determined for the prepared samples. The addition of small concentration of TiO2 leads to change both of Tg and Tc. The glassy temperature of this glass is about 435 °C and the crystallization temperature at about 505 °C. Heat treatment has done for the glasses to obtain the crystalline phase. This action studied by both XRD, SEM, TEM, and EDAX pictures. Results proved that the glass phase performs as interconnecting amorphous zones between the crystals and the size of crystal grains is changed from 1 μm to 20 μm. The capability of using the investigated glasses as radiation shielding glasses has been evaluated. The mass attenuation coefficient (µ/ρ) has been calculated by using WinXcom software program in the range of 0.01–15 MeV photon energy. The related shielding parameters such as linear attenuation coefficient (µ), half value layer (HVL) and mean free path (MFP) were evaluated and compared with those of commercial γ-ray shielding concrete. Results reveal that the HVL values for all investigated glasses increased except for BTNCT1.0 sample. Thus, BTNCT1.0 glass sample has the lowest HVL compared to other samples.

1. Introduction Recently, glass materials have more attention from several researchers, where these glasses can be used in different applications such as optical fibers, sensors, lasers, solar cells, optoelectronic and memory switching devices [1–3]. Additive of heavy transition metal oxides, such as TeO2 to glass composition leads to increase the refractive index and nonlinear optical properties of the produced glasses [4,5]. Especially, glasses produced by adding TeO2 to other glass formers like B2O3 have been at the focus of many research investigations. TeO2 based glasses are characteristic by their interesting applications in several optical devices [6,7]. Gamma rays are considered one of the most energetic ionizing radiation, therefore it has the ability to penetrate the specimens and considered to be dangerous for human health and also human heredity [8,9]. Evaluating and understanding the radiation interaction parameters is very important to construct and develop new radiation shielding materials. It is well known that materials with high atomic number elements and high density are suitable for radiation shielding materials. The mass attenuation coefficient, linear attenuation coefficient, half value layer, mean free path, effective atomic number, and effective electron density are the common radiation interaction ⁎

quantities used by the radiation shielding materials investigators [10–13]. Concretes and polymers are considered as traditional radiation shielding materials [14–18]. These materials have many disadvantages like not transparent to the visible light and this limited the utilization of these materials in some applications. Therefore, glasses which are transparent to the light can be used to design shields for X/γ rays and neutrons. In the last few years many glasses were prepared in order to be suitable for radiation shielding materials [19–22]. The aim of the work is to investigate the structural, thermal and radiation shielding properties of glass system of composition (60B2O3–10 Na2O–20TeO2–(10-x) CaO) + xTiO2 where x ranged from 0 to 3 mol%. The differential thermal analysis (DTA), glassy temperature, and crystallization temperature of the glasses have been measured. SEM, TEM, XRD, and EDAX for the crystalline glass have been performed. The possibility of using the investigated glasses as radiation shielding glasses has been evaluated. This aim achieved by calculating the mass attenuation coefficient (µ/ρ) by using WinXcom software program in the range of 0.01–15 MeV photon energy. The related shielding parameters such as linear attenuation coefficient, half value layer, and mean free path have been evaluated. The obtained results compared with those of ordinary concrete sample. The findings show that the current glasses under study are future candidates for γ-ray

Corresponding author. E-mail address: [email protected] (Y.S. Rammah).

https://doi.org/10.1016/j.jnoncrysol.2019.119720 Received 29 August 2019; Received in revised form 21 September 2019; Accepted 25 September 2019 0022-3093/ © 2019 Elsevier B.V. All rights reserved.

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Table 1 Density and chemical composition with Wt. fraction of elements in samples in the system (60B2O3–20TeO2–10 Na2O- (10-x) CaO) + xTiO2: 0 ≤ x ≤ 3 mol%) glasses. Density ± 0.0001 (g/cm3) [21]

Sample code

BTNCT BTNCT BTNCT BTNCT BTNCT

0.0 0.5 1.0 2.0 3.0

2.9121 2.9201 2.9985 2.8702 2.8134

Weight fraction wt%

Wt. fraction of elements in each sample

B2O3

TeO2

Na2O

CaO

TiO2

B

O

Na

Ca

Ti

Te

60 60 60 60 60

20 20 20 20 20

10 10 10 10 10

10 9.5 9.0 8.0 7.0

0.0 0.5 1.0 2.0 3.0

0.186343 0.186343 0.186343 0.186343 0.186343

0.508102 0.508678 0.509254 0.510407 0.511560

0.074186 0.074186 0.074186 0.074186 0.074186

0.071469 0.067896 0.064322 0.057175 0.050028

0.000000 0.002997 0.005994 0.011988 0.017982

0.159900 0.159900 0.159900 0.159900 0.159900

shielding materials. 2. Experimental and theoretical concepts

reflects the shielding capability of the samples and can be defined as thickness of glasses needed to reduce the incident photon intensity by 50% of its initial value [26–30].

2.1. Experimental

HVL =

Five glass samples of TeO2 based glasses with chemical formula (60B2O3–10 Na2O–20TeO2–(10-x) CaO) + xTiO2 where x ranged from 0 to 3 mol%) taken from our earlier work [23] to investigate their crystallization and γ-ray shielding properties. The studied glasses are coded as BTNCT0.0 (x = 0), BTNCT0.5 (x = 0.5), BTNCT1.0 (x = 1.0), BTNCT2.0 (x = 2.0), and BTNCT3.0 (x = 3.0). Density and chemical composition with weight fraction of elements in the samples are collected in Table 1. Thermal behaviors (differential thermal analysis DTA) of the finely powdered quenched samples were examined using SEATRAM Instrumentation Regulation, Labsys TM TG-DSC16 (Setaram, Caluire, France) under inert gas. The powder was heated in Pt-holder with another Pt-holder containing Al2O3 as a reference material. The results obtained used as a guide for determining the required heattreatment temperatures needed to induce crystallization in the samples. The X-ray diffraction (XRD) measurements were carried out using a diffractometer type Philips, PW-1390 adopting Ni-filter and Cu-target. The patterns of X-ray diffraction were recorded in a 2θ ranging from 10° to 70° The JCPDS- International Center for Diffraction Data Cards used as reference data for determining the data obtained in this study. Measurements of the microstructure have been carried out using Scanning Electron Microscope (SEM) of type (JEOL- 840A). The samples were coated with surface layer of gold for perfect morphological studies.

Mean free path (MFP) is another parameter that describes the gamma photons interaction with the glass system and reflects the shielding effectiveness of any material. It is the inverse parameter to the µ and expressed in cm.

MFP =

TVL =

=

Wi i

(4)

ln(10) µ

Fig. 1 shows the DTA curve for glass of composition (60B2O3–10Na2O–20TeO2–8CaO) + 2TiO2. As shown in the figure the glassy temperature of this glass is about 435 °C and the crystallization temperature at about 505 °C. The studied glasses are heated at 505 °C for 2 h then raise temperature to 525 °C for another two hours to have a crystallized glass samples. Results reveal that the addition of TiO2 in small concentrations leads to change the Tg and Tc for studied glasses. The scanning electron microscopy (SEM) pictures for crystallized

(1)

µ i

(5)

3.1. Crystallization of TiO2 glasses

I and Io represent to the intensity of the un-attenuated and attenuated photon beam, x is the absorber thickness, and µ is the linear attenuation coefficient which defined as the probability of photon interaction per unit length and expressed in cm−1. The mass attenuation coefficient of the glass sample is derived from µ values divided by the glass density and expressed in cm2/g. In the field of radiation protection, the most important parameter is the mass attenuation coefficient (µ/ρ). The (µ/ρ) is used to describe the γ-ray penetration and interaction with the materials and can be calculated theoretically through the mixture rule given as [25]:

µ

1 µ

3. Results and discussion

The attenuation process of gamma rays by materials has been described by Beer–Lambert's law [24]: µx

(3)

where (μ) is the linear attenuation coefficient of the studied samples. The half value layer (HVL) and the Mean free path (MFP) are two parameters which can signify the shielding competence of the alloy samples against γ-ray (lower HVL and MFP, higher shielding competence and vice versa). The HVL and MFP for the studied alloys can be calculated through Eqs. (3) and (4). In a similar way to HVL, another parameter also used to describe the shielding capability of the glasses called tenth value layer (TVL) also calculated. It is defined as the glass thickness needed to reduce the intensity of incident radiation to one tenth of its initial value. It can be calculated using the equation;

2.2. Theoretical concepts

I =e Io

ln 2 µ

(2)

where (µ/ρ)i is the mass attenuation coefficient of the ith constituent element and wi is the weight fraction of the ith constituent element in the alloy sample. Another an attractive parameter, half value layer (HVL) in cm which

Fig. 1. DTA curve for glass containing 2 mol% TiO2. 2

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Y.S. Rammah, et al.

Fig. 2. SEM for crysalline glass containing 2 mol% TiO2.

sample containing x = 2 mol% TiO2 are shown in Fig. 2. The SEM pictures indicate that the glass phase performs as interconnecting amorphous zones between the crystals. It is noted that the glass phase does not contain voids and cracks. The SEM picture indicated that the size of crystal grains is changed from 1 μm to 20 μm. X-ray diffraction pattern (XRD) for 60B2O3 –10Na2O–20TeO2–8CaO–2TiO2 glass ceramics is shown in Fig. 3. As shown in Fig. 3 no characteristics peaks are observed in the pattern which may attributed to the concentration of crystalline phase may be less than 10% and this crystalline phase cannot be detected by X-ray diffraction. This observation confirms that the investigated glasses are in amorphous nature. This result is in a good agreement with the result of EDAX as shown in Fig. 4. Accordingly, we can suggest that the crystalline glasses containing 2 mol% of TiO2 contain a nano-crystals with amorphous zone. This result is confirmed by Transmission electron microscopy (TEM) measurements as in Fig. 5. The TEM studies (Fig. 5) reveals a nano-crystalline grain cluster. The nano crystalline grain cluster size changed from 2.5 nm to 35.3 nm [31]. Around the crystals, a free amorphous phase zone is recognized, which is characterized in the SEM picture.

(60B2O3–20TeO2–10 Na2O- (10-x) CaO) + xTiO2: 0 ≤ x ≤ 3 mol%). The (µ/ρ) values for all glasses (BTNCT0.0–BTNCT3.0) have been calculated with help of WinXcom software program in the range of 0.01–15 MeV photon energy [32]. Fig. 6 introduces a plot of (µ/ρ) for proposed glasses with respect to photon energy in the range 0.01–15 MeV. It is obvious that the (µ/ρ) values based on two parameters which are most effective; fraction weight of elements and photon energy. One found that the values of (µ/ρ) for all glasses exhibit an exponential decrease from 0.01 MeV till reaching to a distinguishable peak at 0.03181 MeV. The appearance of this peak can be attributed to the K-edge of Tellurium (Te) element found in the glass samples [33]. But generally, the variation of (µ/ρ) values of all samples with photon energy is approximately the same. Indeed, the (µ/ρ) values of all glasses are high at low energy photon and then decreased quickly. This decreasing may be reflected to the predominance of photoelectric effect as this effect depends on the photon energy 1/E3.5 and the atomic number of the absorber (glass samples) as Z4, where the studied glass system contains heavy element tellurium (Te=52) added by a constant fraction equal 0.159900 in all samples [33]. In the intermediate range of photon energies, the slight decrease attributed to the Compton effect. Finally, at high energy photon i.e., greater than 3 MeV, (µ/ρ) values exhibit a slow increase. This trend may be attributed to the pair production phenomenon which reported by many researches [25–28,34–36]. As an example, for the comparison between the investigated glasses, the µ/ρ at photon energies of 0.356 MeV (133Ba),

3.2. Shielding features Table 1 shows the density, chemical composition and weight fraction of each element in the investigated glass system 3

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Fig. 3. XRD pattern of glass ceramics contaninig 2 mol% TiO2.

Fig. 4. EDAX for crystallized glass containing 2 mol% TiO2.

0.511 MeV (22Na), 0.662 MeV (137Cs), 1.173 MeV (60Co), and 1.330 MeV (60Co) for all glasses were calculated and listed in Table 2. Analyzing these data shows that the shielding capability of the investigated glasses arranged in the order (BTNCT0.0 > BTNCT 0.5 > BTNCT1.0 > BTNCT2.0 > BTNCT3.0), but the change is too small as TeO2 is constant in all samples and slight increase found in TiO2 content while CaO content has a slight decrease. The linear attenuation coefficient (µ) values with respect to photon energy are calculated by Eq. (2) and displayed in Fig. 7, as mentioned before, the (µ) based mainly on the sample density. Comparing the density of the studied glasses, one found that BTNCT1.0 glass sample has the highest value (2.9985 g/cm3), thus this sample has high µ compared to the other samples as shown in the inset in Fig. 7. Generally, the trend of Fig. 7 can be similarly explained as what is mentioned before in Fig. 6. HVL has been calculated for all investigated glasses (BTNCT0.0 – BTNCT3.0) using Eq. (3), compared with that of ordinary concrete in 0.01–15 MeV photon energy, and displayed in Fig. 8. Having a look on Fig. 8, one found that there is a constant trend in HVL values in 0.01–0.1 MeV photon energy and all HVL values are small (0.0213 cm

Fig. 5. TEM crysalline glass containing 2 mol%TiO2.

and 0.022 cm for BTNCT0.0 and BTNCT3.0, respectively at 0.015 MeV). This result reflects the capability of using such these glasses as a good γray shield at low photon energy [34–36]. At Ephoton > 0.1 MeV, HVL increased and the change in the values is noticeable. For example, (HVL)BTNCT0.0 = 1.57 cm, (HVL)BTNCT0.5 = 1.58 cm, (HVL)BTNCT1.0 = 1.53 cm, (HVL)BTNCT2.0 = 1.6 cm, (HVL)BTNCT3.0 = 1.63 cm at 4

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Fig. 6. MAC values of BTNCT0.0–BTNCT3.0 glasses compared with ordinary concrete in 0.01–15 MeV photon energy.

Fig. 8. HVL values of BTNCT0.0–BTNCT3.0 glasses compared with ordinary concrete.

Table 2 Mass attenuation coefficients (µ/ρ) of system (60B2O3–20TeO2–10 Na2O-(10-x) CaO) + xTiO2: 0 ≤ x ≤ 3 mol%) glasses. Energy (MeV)

Mass attenuation coefficient (µ/ρ)×10−2 (cm2/g) ± 0.01 BTNCT 0.0

BTNCT 0.5

BTNCT 1.0

BTNCT 2.0

BTNCT 3.0

0.356 0.511 0.662 1.173 1.330

10.19 8.486 7.492 5.646 5.294

10.18 8.484 7.410 5.645 5.293

10.18 8.482 7.488 5.644 5.291

10.18 8.478 7.484 5.641 5.289

10.17 8.474 7.481 5.638 5.286

Fig. 9. MFP values of BTNCT0.0–BTNCT3.0 glasses compared with Ordinary concrete.

BTNCT1.0 glass sample exhibits small MFP values, which reflects the higher probability of photon interaction with this sample. It is worse mentioning that the investigated glasses is much better than ordinary concrete [37] in gamma photon shielding applications as µ/ρ and µ values of all glasses are higher than that of ordinary concrete. Also, HVL and MFP of all investigated glasses is much smaller than that of ordinary concrete. This is shown in Figs. 6–9. Additionally, values of tenth value layer (TVL) for all studied glasses (not presented in this text), but the variation of TVL with the density of samples at different photon energy is displayed in Fig. 10. It is clearly seen that the TVL values increased with increasing the photon energy and decreased with increasing the density of the investigated glasses. The BTNCT1.0 glass sample is the dense material (density = 2.9985 g/ cm3) [23]. This means that it contains higher number of atoms when compared with lower dense materials, so, it characterized by the lowest TVL values which ensured that it has the best shielding properties between all investigated glasses in this work. At the end, our goal in this section is to spot the talk on the main three probabilities of gamma interaction with the investigated glasses at energy

Fig. 7. LAC values of BTNCT0.0–BTNCT3.0 glasses compared with ordinary concrete in 0.01–15 MeV photon energy.

0.2 MeV. It is clearly seen from this example that HVL values for all investigated glasses increased except for BTNCT1.0 sample. Thus, BTNCT1.0 glass sample has the lowest HVL compared to other glasses and ordinary concrete sample as shown in the inset in Fig. 8. The MFP behavior for all investigated glasses with respect to photon energy in (0.01–15) MeV range is calculated using Eq. (4) and displayed in Fig. 9. Fig. 9 shows that MFP exhibits the same trend as in HVL. Low values of mean free path at low photon energy < 0.1 MeV are present, then a gradual increase with the increase in photon energy also present. 5

Journal of Non-Crystalline Solids 526 (2019) 119720

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Fig. 10. Variation of TVL with density of glasses at different photon energy. Table 3 Photoelectric interaction of system (60B2O3–20TeO2–10 Na2O- (10-x) CaO) + xTiO2: 0 ≤ x ≤ 3 mol%) glasses. Energy (MeV)

0.356 0.511 0.662 1.173 1.330

Fig. 12. Variation of Compton scattering with TiO2 content at different photon energy.

Photoelectric interaction (×10−3 cm2/g) ± 0.001 BTNCT 0.0

BTNCT 0.5

BTNCT 1.0

BTNCT 2.0

BTNCT 3.0

7.202 2.815 1.505 0.4429 0.3519

7.203 2.815 1.505 0.4430 0.3519

7.204 2.816 1.505 0.4430 0.3520

7.205 2.816 1.505 0.4431 0.3520

7.206 2.817 1.506 0.4432 0.3521

Table 5 Pair production (P.P) interaction of system (60B2O3–20TeO2–10 Na2O-(10-x) CaO) + xTiO2: 0 ≤ x ≤ 3 wt%) glasses. Energy (MeV)

1.173 1.330

Pair production interaction (×10−5cm2/g) ± 0.001 BTNCT 0.0

BTNCT 0.5

BTNCT 1.0

BTNCT 2.0

BTNCT 3.0

1.695 9.127

1.694 9.124

1.693 9.122

1.692 9.116

1.961 9.110

Fig. 11. Variation of photoelectric effect with TiO2 content at different photon energy. Table 4 Compton interaction of system (60B2O3–20TeO2–10 CaO) + xTiO2: 0 ≤ x ≤ 3 mol%) glasses. Energy (MeV)

0.356 0.511 0.662 1.173 1.330

Na2O-

(10-x)

Compton interaction (×10−2 cm2/g) ± 0.001 BTNCT 0.0

BTNCT 0.5

BTNCT 1.0

BTNCT 2.0

BTNCT 3.0

9.466 8.204 7.341 5.60 5.25

9.464 8.202 7.339 5.599 5.248

9.461 8.200 7.338 5.598 5.247

9.457 8.196 7.334 5.595 5.244

9.452 8.192 7.330 5.592 5.242

Fig. 13. Variation of pair production with TiO2 content at different photon energy.

range (0.356–1.330) MeV. These three processes are photoelectric effect, Compton interaction, and Pair production. The variation of photoelectric effect with respect to both TiO2 concentration and aforementioned photon energy (0.356–1.1330 MeV) is gathered in Table 3 and displayed in 6

Journal of Non-Crystalline Solids 526 (2019) 119720

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Fig. 11. The trend of this process exhibits a slight increase with increasing the TiO2 content from (0.0–3.0) mol% and decreasing the CaO content from (10.0–7.0) mol% and this is supported as Z of Ti is greater than that Ca, besides this, it shows a decrease with increasing the photon energy. It is in a good agreement with the explanation of the photoelectric effect process [34–36]. Also, Compton scattering variation with respect to both TiO2 concentration and aforementioned photon energy (0.356–1.1330 MeV) is gathered in Table 4 and displayed in Fig. 12. Obtained results reflect the dominance of this process in the intermediate range of energy and the data seems to be greater than that obtained in the photoelectric effect. Finally, Pair production process seems to be a weak interaction when compared to the other two processes and exhibit a noticeable increase with increasing the photon energy. The obtained data for this trend is gathered in Table 5 and sketched in Fig. 13.

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4. Conclusion In the present study, crystallization and gamma- ray shielding parameters of five glasses with 60B2O3–10 Na2O–20TeO2–(10-x) CaO) + xTiO2 where x ranged from 0 to 3 mol% was investigated. Results reveal that: 1 The glassy temperature of this glass is about 435 °C and the crystallization temperature at about 505 °C. 2 The SEM pictures indicate that the glass phase performs as interconnecting amorphous zones between the crystals and the size of crystal grains is changed from 1 μm to 20 μm. 3 XRD shows that no characteristics peaks are observed in the pattern which may attributed to the concentration of crystalline phase may be less than 10% and this crystalline phase cannot be detected by X- ray diffraction. This result is in a good agreement with the result of EDAX. 4 The (µ/ρ) for proposed glasses with respect to photon energy in the range 0.01–15 MeV. 5 The HVL values for all investigated glasses increased except for BTNCT1.0 sample. Thus, BTNCT1.0 glass sample has lowest HVL compared to other glasses. 6 The present glasses have lower HVL and MFP values than that of ordinary concrete at all energies. 7 The TVL values increased with increasing the photon energy and decreased with increasing the density of the investigated glasses. The results indicate that BTNCT1.0 glass is suitable candidate for γray shielding applications. Declaration of Competing Interest This manuscript has not been published, was not, and is not being submitted to any other journal. All necessary permissions for publication were secured prior to submission of the manuscript. All authors listed have made a significant contribution to the research reported and have read and approved the submitted manuscript, and furthermore, all those who made substantive contributions to this work have been included in the author list. References [1] S.L. Meena, B. Bhatia, Polarizability and optical basicity of Er3+ ions doped zinc lithium bismuth borate glasses, J. Pure Appl. Ind. Phys. 10 (2016) 175–183. [2] S. Thirumaran, K. Sathish, Spectroscopic investigations on structural characterization of borate glass specimen doped with transition metal ions, Res. J. Chem. Environ. 10 (2015) 77–82. [3] K.A. Matori, M.H.M. Zaid, H.J. Quah, S.H. Abdul Aziz, Z. Abdul Wahab, M.S.M. Ghazali, Studying the effect of ZnO on physical and elastic properties of (ZnO) x (P2O5) 1−x glasses sing nondestructive ultrasonic method, Adv. Mater. Sci. Eng. (2015) doi.org/10.1155/2015/596361. [4] N.V. Ovcharenko, T.V. Smirnova, High refractive index and magneto–optical glasses in the systems TeO2–WO3–Bi2O3 and TeO2–WO3–PbO, J. Non-Cryst. Solids

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