1. Introduction

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Advances in Materials Physics and Chemistry

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10.4236/ampc.2020.1012024

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Chemical Durability, Structure Properties and Bioactivity of Glasses 48P2O5-30CaO-(22−x)Na2O-xTiO2(With 0 < x ≤ 3; mol%)

Yassine

Er-Rouissi

¹Sara

Aqdim

²Abdeslam

El Bouari

²Fouzia

Hmimid

³Said

Aqdim

⁴^*

Department of Biology, Faculty of Science, Laboratory Health & Environment, Hassan II University Ain Chock, Casablanca, Morocco

Faculty of Sciences Ben-M’sik, Laboratory Physical-Chemistry of Applied Materials, Hassan II University, Casablanca, Morocco

Department of Chemistry, Faculty of Science, Mineral Chemistry Laboratory, Hassan II University Ain Chock, Casablanca, Morocco

Faculty of Sciences, Laboratory of Materials Engineering for Environment and Valorization, Hassan II University Ain Chock, Casablanca, Morocco

24122020

101230531810, October 202021, December 2020 24, December 2020

2014

This work is licensed under the Creative Commons Attribution International License (CC BY). http://creativecommons.org/licenses/by/4.0/

Phosphate glasses of composition 48P ₂O ₅-30CaO-(22 −x)Na ₂O-xTiO ₂ (with 0 < x ≤ 3, mol%) were prepared by direct melting at 1080 °C ± 20 °C. The chemical durability of these glasses shows an improvement when the Ti O ₂ content varies from 0 to 2 mol%. The measurements of differential thermal analysis and density, both, indicate the increase of the glass transition temperature and the density. The increase of Tg leads to an improvement of glass rigidity. X-ray diffraction analysis of the glasses annealed at 650 °C for 48 h, indicates the appearance of a mixture of metaphosphate and pyrophosphate phases when the Ti O ₂ content varies from 0 to 2 mol%, the last become majority when the Ti O ₂ content rich 2 mol%. Nevertheless, when the Ti O ₂ content exceeds 2 mol%, the analysis, both, by infrared spectroscopy and X-ray diffraction, reveals a radical change of structure with the formation of majorities isolated orthophosphate groups. SEM micrographs illustrated that the number of crystallites increased in the glass network when the Ti O ₂ content increased at the expense of the Na ₂O content. An increase in the TiO ₂ content beyond 2 mol% led to the formation of a larger number of crystallites of different sizes, dominated by small crystallite sizes assigned to majority isolated short orthophosphate groups. This phenomenon led to a decrease in chemical durability and seems to be the main cause promoting the bioactivity of glasses. The results of the bioactivity, after a test in an SBF physiological solution within 15 days, shows, both, the formation of hydroxyapatite and tricalcium phosphate layers, in addition to the layer Ca ₂P ₂O ₇, known by its bioactivity, in some samples. The results obtained on the glasses studied make them potential candidates for an application in tissue engineering.

Chemical Durability Phosphate Glasses Titan Oxide Bioactivity SBF

1. Introduction

Several studies have been carried out on phosphate-based glasses as promising materials for various applications in all fields. The properties of phosphate glasses such as low melting point, high thermal expansion coefficient, sealing materials and bioactivity, including the concept of the biomaterials degradation, make them potential candidates for many technological applications [1] - [11]. The bioactivity of phosphate glasses and in particular the property of being completely dissolved in aqueous medium; this degradation concept can be controlled by modifying the intermediate oxides so that the latter are in congruence with the chemical durability and can be used for glasses rich in phosphate and calcium applied as biomaterials [11] - [17]. Calcium phosphate glasses and glass ceramics in the orthophosphate region (CaO/P₂O₅ = 0.5 - 2) [18] were obtained by using of other oxides such as Na₂O, Al₂O₃, Fe₂O₃, ZnO, MgO, TiO₂, which can easily depolymerize P₂O₅ oxide from long ultraphosphate (O/P = 2.5) chains to isolated short orthophosphate chains (O/P = 4). Our goal is to develop bioactive glasses, focusing particularly on the effect of the substitution of TiO₂ to calcium phosphate oxide glasses for use in the medical field. The study of composition glasses 48P₂O₅-30CaO-(22−x)Na₂O-xTiO₂ (with 0 < x ≤ 3; mol%) as a function of the TiO₂ content has shown a rigidity of the glass network in congruence with its biodegradability. The increase in the TiO₂ content (with 0 < x ≤ 2; mol%) in the glass network entrained an increase of the chemical durability, and Tg, followed by an important change from metaphosphate (Q²) to pyrophosphate structural units (Q¹). When the TiO₂ content beyond 2 mol%, the chemical durability undergo a slow decrease and the structure evolve toward majority isolated short orthophosphate units (Q⁰), confirmed by IR spectrum and X-Ray diffraction, SEM micrographs illustrated that the number of crystallites increased in the glass network when the TiO₂ content increased at the expense of the Na₂O content. This indicates that we are near the border between the glass and the crystal [15] [19] [20]. The chemical reactivity of these materials was evaluated after immersion in the simulated body fluid (SBF) at 37˚C for 15 days. The analysis results seem important for the beginning of the glasses bioactivity.

2. Experimental Section

Phosphate glasses are prepared by direct melting of the (NH₄)H₂PO₄, CaCO₃, Na₂O, TiO₂ mixture in suitable proportions. The reagents are intimately crushed then introduced into a porcelain crucible. Then, they are heated initially at 300˚C for 2 h and then at 500˚C for 1h to complete the decomposition. The reaction mixture is then heated at 900˚C. For 40 minutes and finally at 1080˚C. For 30 minutes in order to obtain a homogeneous liquid. Then it is cast in an aluminum plate previously heated to 200˚C to avoid thermal shock. Pellets 5 to 10 mm in diameter and 1 to 3 mm thick are obtained. The samples were then immersed in distilled water at 90˚C for 20 days to determine the dissolution rate evaluated from the mass loss as a function of time. Analysis by IR spectroscopy was done in a frequency range of between 400 and 1600 cm⁻¹ with a resolution of 2 cm⁻¹, using a Fourier transform spectrometer. The vitreous state was first evidenced from the shiny and transparency aspect, which was then confirmed by X-ray diffraction (XRD) patterns. Samples glasses were analyzed by X-ray diffraction after an annealing time of 48 h at 650˚C. Differential thermal analysis (DTA) was performed using a Perkin-Elmer DTA7, at a heating rate of 10˚C/min in a flowing nitrogen atmosphere (30 cm³/mn) with alumina crucibles. The Archimedes method was used to measure the density of glasses using orthophthalate as a floating medium. The microstructures of the sample glasses were characterised by scanning electron microscopy (SEM), equipped with a full system micro-analyser (EDX-EDAX). Glass powder of each sample was soaked in SBF solution at 37˚C for 21 days.

3. Results and Discussion3.1. Chemical Durability

The glass series 48P₂O₅-30CaO-(22−x)Na₂O-xTiO₂ (with 0 < x ≤ 3 mol%), was approximated by measuring the dissolution rate (DR) which was defined as the weight loss of the glass expressed in terms g∙cm⁻²∙mn⁻¹. The DR values reported in Table 1 show a dissolution decrease versus TiO₂ contents between 0.5 and 2 mole %, after their immersion in 100 ml of distilled water, heated at 90˚C for 21 consecutive days (Figure 1). However, when the TiO₂ content exceeds 2 mol%, there is a relatively significant increase in the dissolution rate. The value

Table 1 The composition and some characteristics of the quaternary glasses 48P2O5-30CaO-(22−x)Na2O-xTiO2 (with 0 < x ≤ 3; mol%)

Glass Sample	Starting Oxide mixtures mol %				[O/P] Ratio	log (D_R) (g∙cm⁻²∙min⁻¹) (±0.2)	Tg (˚C)	Tc (˚C)
Glass Sample	P₂O₅	CaO	Na₂O	TiO₂	[O/P] Ratio	log (D_R) (g∙cm⁻²∙min⁻¹) (±0.2)	(±2)
48T05	48	30	21.5	0.5	3046	−4.9	405	495
48T10	48	30	21	1	3052	−5.1	449	498
48T15	48	30	20.5	1.5	3057	−5.7	473	525
48T20	48	30	20	2	3062	−6.05	476	540
48T25	48	30	19.5	2.5	3067	−5.9	430	490
48T30	48	30	19	3	3072	−5.5	450	496

of leached pH, for different samples, after 21 days, is represented as a function of the TiO₂ content (Figure 2), it indicates that the pH of the solution varies in a range between 3 and 7 ± 0.5, values which correspond to the leached pH of a bioactive glass [18] [21] [22] [23].

3.2. Density and Molar Volumes

The Archimedes principle was used to measure the density of glasses using orthophthalate as a floating medium. The density of the glasses was obtained by using the relation (1),

ρ = [ m air m air + m ortho − m ( ortho + glass ) ] ρ ortho (1)

With: m_air: the mass of the sample measured in the area.

m_ortho: Orthophthalate mass only.

m₍_ortho+glass₎: Mass of glass immersed in diethyl orthophthalate.

ρ_ortho: 1.11422 g∙cm⁻³.

The density variation of composition glasses are represented in Figure 2. The molar volume and the anionic radius of the oxygen in the glass were determined respectively from the relationships (2) and (3):

V 0 M = M / ρ N A N 0 ∗ (2)

r c a l ( O = ) = 3 V 0 M / 2 (3)

With M = molar mass, ρ = density, N_A = Avogadro number; N 0 ∗ number of oxygen atoms in the molecular formula. The value of the molar volume and the oxygen radius were calculated from the approximate hypothesis of close packing of oxygen anions O²⁻, having r(O²⁻) recapitulated for each composition in Table 2 [1] [15]. As can be seen from Figure 3, density increased with TiO₂ content at the expense of Na₂O. This seems obvious since the molar mass of titanium oxide is greater than that of sodium oxide. However, when the TiO₂ content becomes greater than 2 mol%, a decrease in the density is noted [9] [13] [14].

Table 2 Glass composition expressed in terms of quaternary system

Glass sample Code	Chemical compositions (mol%)	Glass compositions inside the ternary diagram
48T05	48P₂O₅∙30CaO∙21.5Na₂O∙0.5TiO₂	0.3173(Na₂O∙P₂O₅)∙0.0096(TiO₂∙P₂O₅)∙0.6731(CaO∙P₂O₅)
48T10	48P₂O₅∙30CaO∙21Na₂O∙1TiO₂	0.3077 (Na₂O∙P₂O₅)∙0.0192(TiO₂∙P₂O₅)∙0.6731(CaO∙P₂O₅)
48T15	48P₂O₅∙30CaO∙20.5Na₂O∙1.5TiO₂	0.2982(Na₂O∙P₂O₅)∙0.02887(TiO₂∙P₂O₅)∙0.6731(CaO∙P₂O₅)
48T20	48P₂O₅∙30CaO∙20Na₂O∙2TiO₂	0.2884(Na₂O∙P₂O₅)∙0.0385(TiO₂∙P₂O₅)∙0.6731(CaO∙P₂O₅)
48T25	48P₂O₅∙30CaO∙19.5Na₂O∙2.5TiO₂	0.2788(Na₂O∙P₂O₅)∙0.0481(TiO₂∙P₂O₅)∙0.6731(CaO∙P₂O₅)
48T30	48P₂O₅∙30CaO∙19Na₂O∙3TiO₂	0.26923(Na₂O∙P₂O₅)∙0.0576(TiO₂∙P₂O₅)∙0.6731(CaO∙P₂O₅)

3.3. Infra-Red Spectra

The infrared spectra of 48P₂O₅-30CaO-(22−x)Na₂O-xTiO₂ series glasses (with 0 < x ≤ 3) are shown in Figure 4. All the vibration bands of the treated samples are in the frequency range from 1400 to 400 cm⁻¹. Analysis of the infrared spectra obtained for all the glasses shows a wide band at around 510 cm⁻¹ attributed to the vibration mode of the skeleton δ (P-O-P) [1] [3] [9]. The vibration bands located around 754 - 784 cm⁻¹ are attributed to the vibration mode Ѵsym (P-O-P)

of pyrophosphate groups (Q¹), while the bands at around 1094 cm⁻¹ and 1267 cm⁻¹ are respectively assigned to the Ѵsym (PO₂)/Ѵasy (PO₃) of pyrophosphate groups (Q¹) and vibration mode Ѵasy (PO₂) of metaphosphate groups (Q²) [2] [4] [5] [9] [12]. The band at around 1150 cm⁻¹, attributed to the stretching vibration Ѵsym (PO₂) in Q¹ - Q² units, appears when the TiO₂ content increased in the glass network [4] [9] [12], while the intensity of the band 1267 cm⁻¹ attributed to metaphosphates groups (Q²) decreased. In the other hand, the band at 880 - 917 cm⁻¹, attributed to asymmetric vibration Ѵasy (P-O-P) in the Q¹ unit, shift to high frequencies as the TiO₂ content increased in the network glass [2] [4] [5] [9] [15]. However, the characteristic vibration band of Ѵsym ( PO 4 3 − ) in the Q⁰ unit, located around 994 cm⁻¹, appeared when the TiO₂ content becomes greater than 1.5 mol%, while the band at 1094 cm⁻¹, attributed to the Ѵsym (PO₂)/Ѵasy (PO₃) vibration mode of pyrophosphate groups, becomes smaller and smaller [9] [24]. Furthermore, the structure deduced from vibrational spectroscopy is compatible with the localization analysis of the compounds (45T05, 45T10, 45T15) inside the ternary diagram given in Figure 5 and Table 3. However, when the TiO₂ content increased beyond 1.5 mole% (45T20, 45T25), we noticed the appearance, in addition to the olygophopshate groups (Q¹ - Q²), of isolated short ortho phosphate groups (Q˚) [16] [25] which indicated the approach of the border area between glass and crystal, this can be explained by several factors (high T_f of TiO₂, crystallite level in the glass bath, Ti + Ca/P ratio) [15] [20].

Table 3 Density and related molar data of the 48P2O5-30CaO-(22−x)Na2O-xTiO2 system

Glass sample code	Starting oxide mixtures mol %				ρ (g∙cm⁻³) (±0.01)	Molar mass (g∙mol⁻¹)	Molar volume (Å3) Vo_M = M/[ρ N_A No*]	Calculated oxygen radius (Å) r_cal (O²⁻)
Glass sample code	P₂O₅	CaO	Na₂O	TiO₂	ρ (g∙cm⁻³) (±0.01)	Molar mass (g∙mol⁻¹)	Molar volume (Å3) Vo_M = M/[ρ N_A No*]	Calculated oxygen radius (Å) r_cal (O²⁻)
48T05	48	30	21.5	0.5	2.57	98,719	21.81	1397
48T10	48	30	21	1	2.59	98,809	21.58	1392
48T15	48	30	20.5	1.5	2.60	98,898	21.52	1390
48T20	48	30	20	2	2.61	98,988	21.40	1388
48T25	48	30	19.5	2.5	2.59	990,775	21.55	1391
48T30	48	30	19	3	2.58	101,564	22.13	1403

3.4. X-Ray Diffraction and DTA

As expected, X-ray crystallography confirmed the vitreous nature of all the investigated glass samples studied. In fact, X-ray diffraction pattern (XRD) recordings show the absence of diffraction peaks. DSC of the glasses (Figure 6) indicates both an increase in the glass transition temperature and the crystallization temperature versus Ti₂O content. When the Ti₂O content increases from 0.5 to 2 mol%, the glass transition temperature (Tg) increases in the 405˚C - 476˚C range, whereas the crystallization temperature (Tc) increases in the 495˚C - 540˚C range (see Table 1) [24]. Beyond 2 mole %, the glass transition temperature (Tg) and the crystallisation temperature Tc undergo, respectively, a decrease from 476˚C to 430˚C and from 540˚C to 490˚C. The heat treatment of the 48T15, 48T20 and 48T25 glasses at 650, gives the XRD patterns shown in Figure 7. These spectra show a structural evolution from metaphosphate to pyrophosphate

and finally to orthophosphates phases. When the 48T15 sample was thermally treated at 650˚C, the amorphous phase partially disappeared and majority Ti(PO₃)₃ [JCPDS files N˚: 01-082-1178], NaCa(PO₃)₃ [JCPDS files N˚: 00-23-0669], Na₄Ca(PO₃)₆, [JCPDS files N˚: 00-025-0811] and CaP₂O₆ [JCPDS files N˚: 00-015-0204] (cyclic metaphosphate O/P = 3), with minor Ca₂P₂O₇ [JCDDS files N˚: 00-009-0346] and Na₅Ti₄(PO₄)₆ [JCPDS files N˚: 01-081-2420] phases occurred in the sample. When the TiO₂ content increased in the glass (48T20), the heat treatment at 650˚C caused the formation of NaTiP₂O₇ [JCPDS file N˚: 01-084-1137-], Ca₂P₂O₇ [JCPDS file N˚: 00-009-0346] and TiP₂O₇ [JCPDS file N˚00-052-1470] with some trace of metaphosphate and isolated short orthophosphates phases, and indicated the increase of pyrophosphate phases (O/P = 3.5). However, when the TiO₂ content exceeded 2 mol% (48T25), the heat treatment, at the same temperature, indicated the majority formation of Na₅Ti (PO₄)₃ [JCPDS file N˚: 01-081-2421] and CaTi₄(PO₄)₆ [JCPDS file N˚: 00-053-0740] phases to the detriment of the pyrophosphates and metaphosphate phases [23] [25] [26].

3.5. SEM Image Analysed

The SEM micrograph shows the existence of two phases, one crystalline and the other glassy (Figure 8). It also indicates the formation of crystalline phase agglomerates of different sizes [2] [15] [21] [24] [25]. Thus, a structural change is observed from Figure 8(a) to Figure 8(b) which presumably indicates the

formation of the predominant cyclic metaphosphate phases. However, when looking at Figure 8(c) there is a structural mixture between cyclic metaphosphates and, presumably, of short pyrophosphate chains. In Figure 8(d), there is a radical change in the structure from the pyrophosphate groups towards predominantly isolated shorter orthophosphate groups. Consequently, the increase of TiO₂ content in the glassy network leads to a progressive depolymerization of the cyclic metaphosphate groups towards pyrophosphate groups and finally to isolated short orthophosphate groups [24] [25].

3.6.In Vitro Bioactivity of Studies Glasses-Surface Analysis Using X-Ray Diffraction

The study in vitro bioactivity of the prepared glasses was carried out by analyzing X-ray diffraction spectra of the samples after immersion in the simulated body fluid (SBF) for 15 days at 37˚C. The result showed (Figure 9) that for the majority of studied glasses there is formation, both, of hydroxyapatite and tricalcium phosphate layers on the surfaces of the samples in addition to the Ca₂P₂O₇ phase known by its bioactivity [16]. When the TiO₂ content increases in the glass, the HA and tricalcium phosphate phases become more evident. The number of peaks and their intensities increase, while the peak intensity of the CaP₂O₇ phase decreases. The peaks of tricalcium phosphate appear at 22.84 and 24.10 (2q) are assigned, respectively, to (241) and (132) reflections [JCPDS file N˚00-033-0297], However the peaks of HA located at 26.40, 28 and 32.83 (2q) assign respectively to (002), (102) and (300) reflections [JCPDS file N˚01-074-0566] [27]. The peaks of Ca₂P₂O₇ phase appear at 30 and 31.92 (2q) are assigned respectively to (211) and (123) reflections [JCPDS file N˚00-033-0297].

A deep analysis of the spectra obtained seems to suggest that the tricalcium phosphate layer is more important than the hydroxyapatite phase when the TiO₂ content reaches 3 mol%.

4. Discussion

Phosphate glasses of composition 48P₂O₅-30CaO-(22−x)Na₂O-xTiO₂ (with 0 < x ≤ 3; mol%) have been investigated. The structure and the chemical durability have been studies using various techniques such IR, XRD, DSC, SEM... Both X-ray diffraction and IR spectroscopy have confirmed the structure change from metaphosphate to olygophosphates when the TiO₂ content increases from 0.5 to 2 mol% in the glass. However, beyond 2 mol% of TiO₂, the appearance of isolated orthophosphates groups is observed. The scanning electron microscope indicated a morphological changing from one cliche to another as the TiO₂ content increased from 0.5 to 2.5 mol%. This change elucidates the passage from cyclic metaphopsphate groups to olygophosphate (mixture meta and pyrophosphate) and finally to isolated short ortho phosphates groups. The variation of transition temperature versus TiO₂ content indicated an increase in Tg from 405˚C to 430˚C when the TiO₂ content increased from 0.5 to 2 mol%, elucidating an improvement in the rigidity of the glass [26] [28]. Beyond 2 mol% TiO₂, the transition temperature (Tg) decreased from 430˚C to 395˚C, indicating a slight weakness of the glass due to the radical change of structure by the formation, of isolated ortho phosphate groups, confirmed , both, by IR spectroscopy and XRD [12] [15] [20]. The increase of isolated short orthophosphate chains in the glass network, at the expense of olygophosphate chains, when the Ti₂O content exceeded 2 mol%, can be explained by the fact that we were close to the border area between crystal and glass [15] [20]. The number of crystallites of different sizes generally increased and exceeded the equilibrium that must be established between the glass bath and the crystallites; hence, we note a significant decrease in chemical durability. At the light of the results obtained, both, for chemical durability, X-ray diffraction and IR spectra analysis (D_R ≈ 10⁻⁶ g∙cm⁻²∙min⁻¹, development of isolated orthophosphate groups ( PO 4 3 − ) [20] [23], the chemical reactivity of these materials studied was evaluated after immersion in the simulated body fluid (SBF) at 37˚C for 15 days. Once in contact with the biological fluids (SBF solution), the bioactive glasses presented the particularity of generating a series of physicochemical reaction to the liquid-glass interface [17] [18] [20]. This series of reactions constitutes the mechanism of bioactivity. The XRD spectra, after test in vitro, indicate the formation of a mixture of hydroxyapatite and tricalcium layers in addition of some traces of calcium pyrophosphate phases, known for its bioactivity [25]. An in-depth analysis of the X-ray spectra obtained, after immersion in the simulated body fluid (SBF), showed that, both, the formation of tricalcium phosphate and of hydroxyapatite layers become more important when the TiO₂ content reached 3 mol%, which, further elucidates that the bioactivity of glasses is like to be greatly successful when once the glass composition is close to the border zone between glass and crystal. In addition, bioactivity appeared in all glasses studied, even those which contain traces of isolated short orthophosphate groups (x ≤ 2 mol%), this, probably, proves that these last ones are the triggers of bioactivity in the glasses.

5. Conclusion

The influence of TiO₂ on the glass forming characteristics and properties of Na₂O-TiO₂-CaO-P₂O₅ glasses has been investigated. The structure and the chemical durability have been studied using various techniques such IR, XRD, DSC, SEM. The variation of the transition temperature versus TiO₂ content indicates an increase in Tg when the TiO₂ content increases and indicates an improvement in the rigidity of the glass. SEM micrograph indicates the existence of two phases one crystalline and the other vitreous. The morphological of the phase crystalline change from one micrograph to another as the TiO₂ content increases from 0.5 to 2.5 mol% and indicates that the structure moves from cyclic metaphosphate and olygophosphate groups to orthophosphate groups. The chemical reactivity of these materials was evaluated after contacting the different glasses with a synthetic physiological fluid (SBF). The XRD spectra of these glasses, after test in vitro, indicate the formation of a mixture of hydroxyapatite and tricalcium layers with some traces of calcium pyrophosphate phases. The presence of these layers is very interested for an eventual biological application in vivo.

Acknowledgements

The authors wish to thank National Center for Scientific and Technical Research [Division of Technical Support Unit for Scientific Research (TSUSR) Rabat, Morocco] for their assistance to the realization of this work. We also thank Ms. Pr. R. ELOUATIB (Laboratory physic and chemistry of inorganic materials) for the support that has brought us.

Conflicts of Interest

The authors declare no conflicts of interest regarding the publication of this paper.

Cite this paper

Er-Rouissi, Y., Aqdim, S., Bouari, A.E., Hmimid, F. and Aqdim, S. (2020) Chemical Durability, Structure Properties and Bioactivity of Glasses 48P₂O₅-30CaO-(22−x)Na₂O-xTiO₂ (With 0 < x ≤ 3; mol%). Advances in Materials Physics and Chemistry, 10, 305-318. https://doi.org/10.4236/ampc.2020.1012024

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