Preparation and Characterization of Bioceramic Cordierite for Medical Applications

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Preparation and Characterization of Bioceramic Cordierite for Medical Applications

https://doi.org/10.21203/rs.3.rs-934657/v1

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The study concentration on the fabricate of bioactive behavior of pure cordierite system and investigate the structure of phase transformation and physical characteristics. cordierite powders were synthesized by chemical coprecipitation, combined Cordierite gel with water-based sol–gel which begin fundamental from magnesium oxide MgO, Alumina Al₂O₃ and silicon oxide SiO_2.Five specimens were prepared with different weight percentage of Mgo, Al₂O₃ and SiO₂powders. cylindrical shape samples were press by hydraulic press at 4 bar for 30 minutes. All specimens were sintered at 1250 ⁰C.

The microstructure examination of specimens was carried out using Field Emission Scanning Electron Microscope (FESEM), x-ray diffraction (XRD) and particle size analysis The analysis revealed cordierite phase formation at 1250 °C, and the intense peaks were identified for composites S4 and S5. The results also indicated the formation of spinel, cristobalite, corundum, protoestatite and cordierite for all the specimens.

Electronic Materials and Devices

Magnetics Materials and Devices

Bioceramic

Cordierite

spinel

phase transformation

cristobalite

corundum and protoestatite

Cordierite is one type of a ceramic material which include aluminum oxide, magnesium oxide and silicate having formula (Mg₂Al₄Si₅O₁₈). It resembles to hexagonal form of structure (cyclosilicate sheet)[1].There are Several methods for cordierite preparation [2], including crystallizing the glasses , solid state reactions, mechanical milling, , sol–gel technique, co-precipitation and combustion synthesis [3].Among these method, the simplest one is co-precipitation, it considered to be low cost and suitable for large production compared to other methods[4][5][6] ,the solid-state sintering is the most common method for synthesis and preparation of cordierite system at high temperatures. The benefit of sol–gel method is higher purity and homogeneity, final structure had finer grain size, heat treatment at low temperatures, and low cost can be considered in comparison with the solid state method for preparation of such structures[7].The advantage of Cordierite ceramics is very low coefficient of thermal expansion and high thermal shock resistance[8],high chemical stability and high mechanical strength[9].which are used in metallurgy, chemical industry , environmental protection and electronics, automobile[10],hot gas filters, membrane supports and membranes, catalysts and catalyst carriers.[11]recent research focusing on medical application of cordierite system ,especially in field of 3D scaffold for bone replacement and cell growth on bioceramic[12][13][14][15].Stoyanova studied the crystallization temperatures of spinel-like cordierite, corundum, mullite, and MgAl₂O₄,. The naturally occurring clay materials were used for the preparing of kieselguhr, and supports: bentonite,. The resulting of the composition samples varied over the following ranges: clay material, from 45 to 60%; MgO, from 10 to 20%,and Al₂O₃, from 30 to 42%;. The found that the conditions responsible for spinel formation in mullite phases and cordierite over temperature range 1050–1150°C. they discovered that the mixture was prepared by coprecipitation is more thermal stable than composites prepared by mechanical mixing [16]. Maris Rundansstudied the improvement of Cordierite phase from natural raw materials, and they observed that Cordierite with ceramic material contain can be successfully obtained when substituting around 20 wt.% of required material with dolomite and/ or 10 wt.% of illite clay. Temperature of 1200ºC is enough to obtain these ceramics. As improve by XRD analysis, the main crystalline of all specimen is that of a cordierite, with anorthite as secondary phase [17]. QingdongHou discussed the cordierite powder preparation of by solid reaction sintering, rotation evaporation , and chemical coprecipitation, the grain size and morphology of samples densify at different temperatures were conceder. Secanning electron microscope shown that the cordierite crystal structural was divided into three processes; in the range of temperatures around 1000 °C (the hexagonal flake–like grain formation) and when the temperature rise to 1200 °C (the flaky texture grain formation), so that these two sintering transition points is important. The partical size was well developed in the range of 196.5–222.7 nm. The main crystal phase was cordierite phase for the samples sintered at 1200 °C which confirm by Phase analysis and mullite phase, a little spinel phase and at 1400 °C the peak intensity of the characteristic peaks was more intense. [18]

In this paper, the cordierite was synthesized by precipitation method, using raw materials of high purity powder of Al₂O₃,MgO, and SiO₂ according to cordierite stoichiometric ratio. The impact factors such as, sintering temperature,cordierite particles size and granulation process for cordierite powders synthesis were investcated by Field Emission Scanning Electron Microscope (FESEM) and X-ray diffraction.

In order to synthesis ceramics cordierite samples, three white powders include magnesium oxide from (Parchem Fine & Specialty Chemicals, USA) with purity 99%, aluminum oxide from (Riedel-de Haën, Germany) and silicon dioxide from (Daejung Chemicals) were used, five different groups were prepared according to calculated chemical composition and molecular wieght fraction for each group of (xMgo, xAl2O3, xSiO2) respectively as shown in table 1. Firstly ,100 g of raw material for each system was utilized to synthesis cordierite, dissolved with 100ml of distilled water and mixed for 3 hours with 120 RPM, secondly, the mixture was stirred at 80 r/m for 2h to obtain a well-mixed sol. Thirdly, the filter papers utilized to dry mixture then finally incubated with 100C^o for 1hr. the dried samples exposed to hydraulic press with 4 bar for 30 minute , after that it was calcined and sintering temperature was 1250C⁰ for 2h and heating rate was 42 C^o/ min.

ternary equilibrium diagram (Figure 2) Represent the three compositions in the SiO₂-Al₂O₃-MgO system, the concentration of oxides was determining without loss on content and ignition of the MgO. The compositions of S1, S2and S3, were found in the region sapphirine which is small area in vicinity of 6 invariant points of cordierite [19]. The compositions S4 & S5 were located in cordierite region. The differences observation was related to raw materials which starting with and S4& S5 formulation with talc which gives the nearest composition of cordierite stoichiometric point, mainly to MgO and SiO₂ concentration. One of the major problems of e cordierite is its small area of existence due to the vicinity of 6 invariant points

XRD measurements are performed at an angle of 10-80^o with scanning speed of 5°/min using an LabX XRD-6000 X-ray Diffractometer from Shimadzu with CuKα radiation (1.5406A^O) operated at 30 mA and 40 keV. The X- Ray data was plotted using the origin Pro software and the peaks were matched with JCPDS software to get the phases present. The corrected Debye-Scherrer formula was used calculated grain size (Dhkl) of the identified crystalline phase:

λ = wavelength of CuKα1 (1.54056 Å). However, the cordierite nanocrystalline size was determined as shown in Table 1.2 and it was in the range of 30–80 nm.

Table2: XRD spectral data for different samples

samples	2-Theta	d(nm)	I%	FWHM	G.S(nm)
S1	17.902	0.4957	6.3	0.159	65
	52.319	0.1742	50.5	0.162	69
	57.332	0.1607	98.5	0.195	54
S2	25.827	0.3448	85.6	0.218	42
	36.922	0.2435	89.3	0.326	27
	44.906	0.2018	62.9	0.299	30
S3	28.04	0.3175	86.6	0.17	59
	32.74	0.2731	18.4	0.195	49
	66.471	0.1404	86.4	0.153	81
S4	43.275	0.2089	17.4	0.177	58
	47.633	0.1905	5.9	0.191	53
	66.461	0.1406	67.6	0.161	75
S5	19.13	0.4635	5.5	0.167	60
	35.272	0.2545	19.2	0.153	72
	57.643	0.1598	100	0.163	70

The table 2 shows a summary of the results of the process for the X-ray diffraction examination, which include all parameters values ( were obtained for all the systems prepared by the chemical precipitation method that were clarified in the paragraph of the practical part.

The results in the table showed values at three peaks in the first system (S1)(1,1,1), which are at with grain size (G.S) 65nm,69nm and 54 nm respectively . This is shown in Figure 3, where this figure appeared at a temperature of 1250°C several systems added to the cordierite system, namely spinel, corundum and cristobalite , these systems result from an internal interaction of the three reactants (Mgo, Al₂O₃ ,SiO₂) at temperatures below 1250°C, with regarding second system S2 (1,2,1) , it can be noted that system include cordierite with appearing sub system ( spinel, cristobalite, corundum) .

As the ratio of silica to alumina change because of the reaction of alumina and silica present in thechemical composition. The cordierite peaks cordierite began to show only at temperature of 1200 °C, and then intensified when the temperature reach 1250 °C. The cordierite phase was observed in the five compositions, at 1250 °C. Askin et al. [20] reported similar results.

The changes that have occurred to the system S3 (1,1,2) can be observed where S3 include high ratio in comparable with AL₂O₃ and Mgo , from figure 3, we notice the decline of the cordierite curve and the emergence of other systems (S3, S5) clearly as a result of side reactions between the materials.

The system S4 ( 2,1,2), the result show that spinel curves was dominant in addition to cordierite system and this is attributed to the reaction of AL₂O₃ and Mgo at temperature under 1250°C and formation of spinel .finally, the system S5 is a fixed system in which the cordierite system is achieved in a stable and clear way, in addition to other systems, and this means that at a temperature of 1250°C, cordierite can form at a ratio (2,2,5) and this is agreement with other author's results [17,18]

The densification temperature plays important role in the cristobalite and spinel phase transformation into cordierite phase. As the temperatures of sintering range 1200–1300 °C, cordierite phasewill be dominant phase, butcristobalite and spinel are undetectable.[21]

The peaks Mullite phase will start to disappear at 1200 °C, according to [22]When thetemperature reach 1250 °C the mullite phase may be react with (MgO) magnesium oxide in the talc to create cordierite phase. The average diameter of the particles less 100 nm, which is similar to previous studied reported that it is possible to obtained cordieritephase fromtalc and pure kaolin, [23]. For the system S5 which will the particles have diameter smaller than 100nm this may contributed to form cordierite phase, the kineticsreaction of solid state is effected by surface area. It was also found different sizes of the particle in the mixture of different components, it will be favor of wider distribution of the particles, lead to high area of the contact which is significant parameter in formation and diffusion new phase.

The diameter of the about all particles of composite S5 are a smaller than 2 μm, which may related to the cordierite formation, since kinetics of the solid state reaction is infected by surface area. The waste mixture also was found that containing particle with different sizes favored distribution of a wider particle size, will increasing the contact area, which is a important factor in the formation and diffusion of cordierite phase. The largest mean particle size of Composition S5 70 nm.

Figure 3 X-ray diffraction shows, the XRD patterns of the compositions after sintering at 1250 °C.The most detected phases were spinel, magnesia, cristobalite and corundum peaks as shown in Figure3. The result of reaction between silica, alumina and magnesia at 1250 °C, in the system (MgO·Al₂O₃·SiO₂) resulted in dominant phase emergence of cordierite, which is the aim of this study.

Greater intensity peaks of composition S4 was observed from the Analysis of the peaks of cordierite for the system S3 and S4, this due to the smaller grain size, which making them more reactive. furthermore, at this temperature there was a small increase in cristobalite peaks

at 1200 °C,Cordierite started to formthe intense peaks showed increasingly at 1250 °C. for Composition S5 figure 3 which was similar to composition S4,

the mechanism can beexplaining this, always more probable of solid state has been considered reaction between binary compounds, and then among three compounds. For this reason, the formation of the cordierite (2MgO·5SiO₂2Al₂O₃) will start from the two compounds reaction, or a binary compound and an oxide reaction.

The presence of impurities in the raw materials which been used, can cause the formation of glassy phase, but considering the effectis not significant so that it will be not considered.

Scanning electron microscope examination

The structure was examined with Field-Emission scanning electron microscopy of MIRA3 TESCAN, the figure 4 represent the morphology of system S1 where the particles agglomerate slightly and most of them are spherical with a small number of reunion at lower sintering

The shapes and magnifications show the coherence and complete interaction between the materials and that the value of the diametersD1= 76.27 nm, D2= 42.63nm, D3=73.51 nm, and the figure 5 represent the percentages of the substances involved in the reaction, and it can be observed that there is a consistency and accuracy in the preparation process that was interpreted by EDXtest.

The figure 6 shows an electron microscope image of the S2 system. Through the image, it is shown that the average particle size is between 44-59 nanometers, and the shape of the precipitated particles is close to the cuboid. It is noted in the image that there is great homogeneity in the reactants and high fusion at degrees of 1250°C.The results of EDX in figure 7 show that there is a great convergence of the stoichiometric ratio of practical work with the results of EDX according to the system (1,2,1) (MgAl₄SiO₉₎ and this explains the accuracy of the results of using the preparation method. For system S1 and S2 the high content of alumina has not high impact on cord rite formation because the reaction with other constituent need slightly higher than this temperature.

regarding system S3 (MgAl₂Si₂O₈), the figures 8 was clarified that the average particle size is between 31 to 123 nanometers. It is also shown that the particle size is semi-cubic and semi-rectangular. As for the EDX test, the results in figure 9 showed a degree of accuracy between the theoretical side and the results of the EDX test, and this proves the success of the appropriate preparation process.

Figure 10 shows the FESEM images of sample S4 (Mg₂Al₂Si₂O₉), the average grain size range is (34-58) nm with homogeneity of the structure,Clearly, it is not possible to distinguish between the materials, as we can observe the uniform distribution of the particles and figure 11 show EDAX result

The figure 12 shows the system S5 (Mg₂Al₄Si₅O₁₈), and we note the formation of cordierite in a homogeneous and clear manner, and the grain size ranges between 33 and 49 nanometers, as can be explained by the EDX test in figure 13, the highest peak intensity for oxygen element followed by silica, alumina and magnesia respectively and this is explaining the accuracy of chemical precipitation method for preparing cordierite system.

Microstructure analysis for the specimens systems S3, S4 and S5 as shown in Figures (8,10,12), after heat treatment with applied 42°C/min heating rate and 120 minutes holding time at 1250 ^oC as sintering temperature.

The microscopic structure of specimen S3, which was prepared by sintering at 1250°C, shows that the crystal structure was circular in shape similar to round petals, a shape which is almost similar to that observed by the source [24].

The researchers investigate the growth and nucleation of cordierite crystals processes from liquid phase and indicated there are three different shapes, presented the structure such as first solid nucleate crystals inclusions in liquid phase and radially growth as rose petals, second The crystals isolated growth from both compact crystal layers and outer surfaces third growth from the center of specimen. The configuration of the crystals of the S4 system which is sintered at 1250 °C hexagons and elongated petals presented the morphology, the appearance is similar to finding which is reported by [25].

Crystals structure of component S4 is showglassy phase with heterogeneous crystals and an elongated tube-like morphology, which is due to the composition hashigh amount of flux. Also needle structure are visible may be related to mullite phase as shown in figure 10. Hexagonal crystals structure showed in composition S5 which is similar to morphology observed by [26,27]. This component was formulated with precursor of MgO and talc, which is may be responsible of different morphology, like the nucleation and parallel surfaces growth of the hexagons structure.

pure cordierite powders effectively prepared by water-based sol–gel method and density at 1250 C °. According to the chemical co-precipitation method cordierite (2Mg. 5SiO_2,2Al₂O₃) was synthesized, it can be concluded that the raw materials chemical compositions, average particle size and sintering temperature influence the cordierite formation. The nucleation temperature of cordierite started at 1250 C °. The present work presents the results of synthesis with different percentages of MgO. Al₂O₃ and SiO_2,which give different peaks intensity of the cordierite phases the heights intensity achieved with composite S4 and S5. Several reactions involves during the entire process of cordierite synthesis, to obtained cordierite phase is always a secondary phase accompanied, which is the spinel.

Scanning electron microscope technique were used to determine the microstructure. The morphological analysis revealed the formation of cordierite in a homogeneous and clear manner, and the grain size ranges between 33 and 49 nanometers hexagonal tube-like crystals and rose-like structure has been identify.

compositions S3 and S4 were located in the region of sapphirine which is small field in the vicinity of 6 invariant points of the cordierite

The S5 composition was located in the region cordierite. The differences was observed due to the raw materials which is starting and the S5 formulation with cordierite stoichiometric point talc, mainly due to the MgO percentages and SiO₂.

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Acknowledgements

We would like to show our gratitude to the (Biomedical Engineering Department Al nahrain university, Department of Medical Physics, College of Science, The University of Karkh for Science and Department of mechanical and chemical Engineering Al nahrain university) for allowing us to use their laboratories sharing their pearls of wisdom with us during the course of this research, We are also immensely grateful to collies for their comments on an earlier version of the manuscript, although any errors are our own and should not tarnish the reputations of these esteemed persons.

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the studies have been performed in accordance with the ethical standards as laid down in the 1964 Declaration of Helsinki and its later amendments or comparable ethical standard

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Preparation and Characterization of Bioceramic Cordierite for Medical Applications

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