Compressive strength and magnetic properties of calcium silicate-zirconia-iron (III) oxide composite cements Hendrie Johann Muhamad Ridzwan, Roslinda Shamsudin, Hamisah Ismail, Mohd Reusmaazran Yusof, Muhammad Azmi Abdul Hamid, and Rozidawati Binti Awang
Citation: AIP Conference Proceedings 1940, 020006 (2018); doi: 10.1063/1.5027921 View online: https://doi.org/10.1063/1.5027921 View Table of Contents: http://aip.scitation.org/toc/apc/1940/1 Published by the American Institute of Physics
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Compressive Strength and Magnetic Properties of Calcium Silicate-Zirconia-Iron (III) Oxide Composite Cements Hendrie Johann Muhamad Ridzwan1, 3, a), Roslinda Shamsudin1, b), Hamisah Ismail1, c), Mohd Reusmaazran Yusof 1, 2, d), Muhammad Azmi Abdul Hamid1, e), and Rozidawati Binti Awang1, f) 1
School of Applied Physics, Faculty of Science & Technology, Universiti Kebangsaan Malaysia, 43600 Bangi, Selangor, Malaysia 2 Materials Technology Group (MTEG), Industrial Technology Division (BTI), Malaysian Nuclear Agency, Bangi, 43000 Kajang, Selangor, Malaysia 3 Faculty of Applied Sciences, Universiti Teknologi MARA Pahang, 26400 Jengka, Pahang, Malaysia a) Corresponding author: [email protected] [email protected]
, c)[email protected]
, d)[email protected]
, e)[email protected]
, f) [email protected]
Abstract. In this study, ZrO2 microparticles and γ-Fe2O3 nanoparticles have been added into calcium silicate based cements. The purpose of this experiment was to investigate the compressive strength and magnetic properties of the prepared composite cement. Calcium silicate (CAS) powder was prepared by hydrothermal method. SiO 2 and CaO obtained from rice husk ash and limestone respectively were autoclaved at 135 °C for 8 h and sintered at 950°C to obtain CAS powder. SiO2:CaO ratio was set at 45:55. CAS/ZrO2 sample were prepared with varying ZrO2 microparticles concentrations by 0-40 wt. %. Compressive strength value of CAS/ZrO2 cements range from 1.44 to 2.44 MPa. CAS/ZrO2/γ-Fe2O3 sample with 40 wt. % ZrO2 were prepared with varying γ-Fe2O3 nanoparticles concentrations (1-5 wt. %). The additions of γ-Fe2O3 nanoparticles showed up to twofold increase in the compressive strength of the cement. XRay diffraction (XRD) results confirm the formation of mixed phases in the produced composite cements. Vibrating sample magnetometer (VSM) analysis revealed that the ferromagnetic behaviour has been observed in CAS/ZrO2/γFe2O3 composite cements. Keywords: Calcium silicate, Hydrothermal, Compressive strength, Magnetic properties
INTRODUCTION In recent years, many bioactive types of cement based on calcium silicate (CAS) have been studied for use in bone tissue repair and dental applications. A number of CAS composite was also have been developed in order to enhance the mechanical properties of the cement. ZrO2 containing ceramics is one of the most studied materials because of its high mechanical strength properties . The inclusion of ZrO2 in the bioceramics notably increases the compressive strength while maintaining the bioactivity of the ceramics [2-3]. Meanwhile, the incorporation of magnetic material into bioactive ceramic has been developed for use in the hyperthermia treatment of cancer [4-5]. In magnetic induction hyperthermia, heat generated by alternating magnetic field on magnetic material heat the cancer infected parts of the body . If the heat treatment and the application time are carefully controlled, the cancerous cells could be destroyed without damaging the healthy cells . This method is said to be potentially suitable for treating deep-seated cancer. The oxide of iron, such as Fe2O3 is widely
The 2017 UKM FST Postgraduate Colloquium AIP Conf. Proc. 1940, 020006-1–020006-6; https://doi.org/10.1063/1.5027921 Published by AIP Publishing. 978-0-7354-1632-1/$30.00
used in magnetic application as it exhibits the magnetic properties. Apart from displaying ferromagnetic behaviour, maghemite γ-Fe2O3 is also well known as biocompatible biomaterials [8-10]. In this study, ZrO2 and γ-Fe2O3 added CAS based composites cement was prepared. In this experiment CAS was synthesized by hydrothermal method using rice husk ash (RHA) derived SiO2 and limestone derived CaO as precursors. Currently, research has not yet been carried out and received less attention by other reseachers on compressive strength and magnetic properties of magnetic material containing CAS in cementation form.
MATERIALS AND METHODS Rice husk as the raw material for silica (SiO2) was collected from the rice mill in Penang. Limestone (CaCO3) was acquired from Imerys Minerals Malaysia Sdn Bhd. ZrO2 microparticles (~5μm) and γ-Fe2O3 nanopowder (~50nm) were purchased from Sigma Aldrich. As previously reported with a slight modification, the calcium silicate (CAS) powder was synthesized by hydrothermal method using autoclave [11-12]. In brief, rice husk was heat treated at 950 °C for 1 h to produce silica (SiO2). Calcium carbonate (CaCO3) was calcined at 1100 °C for 5 h to obtain calcium oxide (CaO). The weight percentage of SiO2 and CaO obtained were 89.5 wt. % and 91.97 wt. % respectively. SiO2 and CaO powder with the ratio of 45:55 were mixed with an adequate amount of distilled water. The mixture was magnetic stirred for 10 min before it was autoclaved for 8 h at 135 °C. Then, the resulting solution was oven dried at 90 °C for 24 h. After that, they were calcined at 950 °C for 5 h to produce CAS powder. The composite cement samples were prepared by mixing each powder (refer Table 1) in an agate mortar before adding buffer solution and mix with spatula. The buffer solution with the liquid-to-powder (L/P) ratios of 0.5 mL/g was used for preparing all cement samples as listed in Table 1. After mixing, a cylindrically shaped specimen samples with dimensions of 6 mm (diameter) x 12 mm (height) were formed using Teflon molds were allowed to set. The specimens were incubated at 36.5 °C and 100% relative humidity for 1 day. Compressive strength testing was measured using Universal Testing Machine (Instron 8874), at a loading rate of 1 mm min-1 until failure or 50% maximum deformation. At least, 5 specimens were tested for each sample. Calcined raw material were characterized using X–ray fluorescence (XRF). Phase analysis of the hydrothermal method prepared CAS and CAS/ZrO2/γ-Fe2O3 composite cement was carried out using X-Ray diffraction (XRD). Magnetic measurements were carried out at room temperature using the vibrating sample magnetometer (VSM) with a maximum magnetic field of 20000 G. TABLE 1. Nominal compositions of the prepared calcium silicate based composite cement.
Sample CSZr CSZr10 CSZr20 CSZr30 CSZr40 CSZrFe1 CSZrFe2 CSZrFe3 CSZrFe4 CSZrFe5
Weight percentage (wt%) Calcium silicate ZrO2 100 0 90 10 80 20 70 30 60 40 59 40 58 40 57 40 56 40 55 40
γ-Fe2O3 0 0 0 0 0 1 2 3 4 5
RESULTS AND DISCUSSION The XRF results in Table 2. shows the chemical composition of the prepared rice husk ash derived SiO2 and limestone derived CaO. 89.5 wt% of SiO2 was obtained by firing rice husk ash at 950 °C for 1 h. Meanwhile, 91.97 wt% of CaO was obtained from CaCO3 calcined at 1100 °C for 5 h. Rice husk ash and calcined CaCO3 were used as starting materials for preparing the CAS powder via hydrothermal method.
TABLE 2. XRF analysis of the raw materials.
Rice husk ash
Elements SiO2 K2O P2O MgO Al2O3 CaO others CaO MgO others
Weight percentage (wt%) 89.5 3.61 3.36 1.24 0.58 0.57 1.14 91.97 7.17 0.86
The XRD pattern of the prepared CAS shows most of the peaks are dominated by β-CaSiO3 phase as presented in Fig. 1. The formation of β-CaSiO3 crystals started with the nucleation of CaO and SiO2 in hydrothermal treatment at 135 °C for 8h . Then, based on the phase diagram of CaO-SiO2 system , by using the designated mole ratio with the calcining temperature of 950 °C were successfully produced the β-CaSiO3. However, minor peaks such as larnite and merwinite phases are also detected. The formation of merwinite (Ca3Mg(SiO4)2 phase was believed from the present of MgO in calcined CaCO3 as detected by XRF (Table 2.) which is 7.17% by weight.
FIGURE 1. XRD pattern of the CAS prepared by the hydrothermal method.
Meanwhile, Figure 2 shows the XRD pattern of the CSZrFe5 sample. ZrO2 is clearly dominating the present phases in the form of baddeleyites. β-CaSiO3 phase is also detected along with tricalcium silicate (Ca3SiO5) phase. Figure 3 illustrates the compressive strength properties of the CAS/ZrO2 cement samples. Generally, by increasing the amount of ZrO2, the compressive strength of the cement samples are also increased. CSZr40 sample has shown the highest value of compressive strength with 2.24 ± 0.12 MPa. Therefore, CSZr40 was selected to be added with different γ-Fe2O3 (1-5 wt. %) concentration in order to magnetize the cement samples. The addition of γFe2O3 was also to investigate its effect on the compressive strength of the cement samples. Figure 4 shows the compressive strength of γ-Fe2O3-added cement samples. The addition of γ-Fe2O3 increases the strength of the cement samples up to twofold with the CSZrFe2 sample exhibits the highest compressive strength of 5.49 ± 0.10 MPa.
Compressive Strength, (Mpa)
FIGURE 2. XRD pattern of the of the CSZrFe5 sample.
2.5 2 1.5 1 0.5 0
FIGURE 3. Compressive strength of ZrO2 added based composite cements
The results obtained have been supported as well by other research that the addition of nanoparticles into cement would enhance the compressive strength of the materials [14-15]. Figure 5 shows the magnetic hysteresis loops of the samples with different contents of γ-Fe2O3 at room temperature. It was found that the CAS/ZrO2/γ-Fe2O3 composite cement exhibit a ferromagnetic behaviour. The saturation magnetization of the samples consistently increased with the increase of γ-Fe2O3 content. The saturation magnetization of CSZrFe1, CSZrFe2, CSZrFe3, CSZrFe4, and CSZrFe5 samples are 0.54, 1.05, 1.58, 2.16, and 2.74 emu/g, respectively.
Compressive Strength, (Mpa)
6 5 4 3 2 1 0
CSZrFe1 CSZrFe2 CSZrFe3 CSZrFe4 CSZrFe5
FIGURE 4. Compressive strength ZrO2 and γ-Fe2O3 added CAS based composite cements.
-3 -12000-10000 -8000 -6000 -4000 -2000 0 2000 4000 6000 8000 10000 12000 Magnetic Field (G)
FIGURE 5. The magnetic hysteresis loops of ZrO2 and γ-Fe2O3 added CAS based composite cements.
CONCLUSION CAS/ZrO2/γ-Fe2O3 composite cements were successfully prepared. The compressive strength and magnetic properties were evaluated as well. The compressive strength of the CAS based cements increased as the ZrO2 content is increased in the sample. The compressive strength also increased with addition of γ-Fe2O3 nanoparticles. The addition of γ-Fe2O3 also successfully magnetized the cement sample as the sample demonstrated ferromagnetic
behaviour. These studies conclude that the addition of ZrO2 and γ-Fe2O3 in CAS based cement could be potentially used in hyperthermia treatment of cancer application with better mechanical strength. However, further studies on bioactivity and biocompatibility evaluation are necessary.
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