Cordierite Ceramic Through Glass and Ceramic Routes from Kaolin and Talc

160 Egypt. J. Chem. Vol. 64, No. 4 pp. 1751 - 1758 (2021)

Egyptian Journal of Chemistry http://ejchem.journals.ekb.eg/

Cordierite Ceramic Through Glass and Ceramic Routes From Kaolin And Talc

Ahmed M. Yahyaa*, Baher A. El-Kaliobya , Abdel Monem M. Soltana, Sayed H. Kenawyb , Esmat M. A. Hamzawyc

a Geology Department, Faculty of Science, Ain Shams University, Cairo 11566, Egypt b Refractories, Ceramics and Building Materials Department, National Research Centre (NRC), Giza, Egypt c Glass Research Department, National Research Centre (NRC), Giza, Egypt

Abstract

Based on kaolin and talc, cordierite was prepared through melt quench and ceramic process of two compositions. The sintering process of ceramics between 1000 and 1300 °C shows mainly the manifestation of cordierite with little ratios of spinel, enstatite, mullite and cristobalite. However, the sintering of their corresponding glasses between 1100 °C and 1200 °C shows the crystallization of cordierite as the main phase with little cristobalite and spinel. In microstructure, the sintering of the ceramic samples revealed nano size rounded- or rod- crystals either free or in clusters in glassy matrix. Whereas, sintering of the corresponding glasses showed clear euhedral to subhedral tetragonal to hexagonal crystals in submicron scale that spread in the residual glassy matrix. The density of the sintered ceramic samples was in the range of 1.96 and 2.43 g/cm3 corresponding to porosity of 29.34 and 5.46 % respectively. While the density of the sintered glasses was 1.90 and 2.35 gm/cm3, corresponding to porosity of 36.20 and 3.30 % respectively. The sintered glass samples presented low and negative coefficient of thermal expansion (CTE) of 36.1 and -36.1 × 10-. °C-1 (in the range ~ 24 -500 and 700 °C). The microhardness values were between 468 and 577 Kg/mm2. As a result, the prepared cordierite ceramic may be possibly used as refractoriness in electric heater supports, such as electric stove or heater cooling plate and ceramic heater base.

Keywords: Ceramic, glass-ceramic; cordierite; CTE; hardness 1. Introduction are going to use powder method by solid-state and Materials based on magnesium aluminum silicate melt quench routs. However, the raw materials usually

(MAS) system have many industrial applications. contain a quantity of Fe2O3, CaO, TiO2, … etc. As it is Some minerals such as cordierite, mullite, osumilite, well known that these oxides enhance the nucleation spinel and proto pyroxene were detected within such in ceramic and glass industry, which in turn have ternary diagram MgO-Al2O3-SiO2 [1-2]. Cordierite influence on the crystallization process [11 – 16].

(Mg2Al4Si5O18) and osumilite [(K,Na)(Fe,Mg)2 Impurities based on cordierite ceramic batch, such as

(Al,Fe)3(Si,Al)12O30] glass-ceramic and ceramic have TiO2, Fe2O3, CaO, K2O and Na2O have influence on low thermal expansion coefficient, high mechanical , the developed phases and their properties [15]. It is chemical stability and low dielectric constant [3]. well known that kaolin-talc system was usually used Their properties make it a promising candidate for in the preparation of cordierite ceramics [7]. Cordierite many industrial applications, such as floor tiles, containing glass-ceramic in nanoscale microstructure substrate material for solar cell, electric heater have very low thermal expansion coefficient prepared supports (such as electric stove, ceramic heater base, from kaolin- magnesite containing impurities of TiO2 and electric heater cooling plate) [4]. and Fe2O3 [6, 16]. Likewise, presence of Na2O and

There are different methods for the synthesis of K2O would lower the refractoriness of the cordierite aluminosilicate phases in the MgO-Al2O3-SiO2 system ceramics and enhance their thermal expansion [13]. such as melt quench, ceramic, sol-gel or wet and In the present research, cordierite ceramics and composite routes [5-10]. Among these methods, we glass-ceramics were fabricated using talc, kaolin,

______*Corresponding author e-mail: [email protected] Receive Date: 16 December 2020, Revise Date: 02 January 2021, Accept Date: 06 January 2021 DOI: 10.21608/ejchem.2021.53853.3115 ©2021 National Information and Documentation Center (NIDOC)

1752 A.M. Yahya et.al. ______commercial alumina. Sintering behavior, phase The chemical composition of the batches is in Table 2. compositions, microstructure, physical, mechanical Powder of glass and ceramic were pressed into disc and thermal properties were studied. Furthermore, green bodies using polyvinyl alcohol [PVA, (solution some properties of ceramics and glass ceramics are 7 %)] as binder under uniaxial pressure (15 bar) using. given to see the potential application of them. The green samples were dried at 180 ᴼC to evaporate 2. Experimental the PVA solution then sintered in a Nabertherm- The starting materials are mainly talc (South electrical furnace for 2 hours between 1000 – 1300 ᴼC Eastern desert, Egypt) and kaolin (Southern Sinai, with heating rate 5 ᴼC/minute. Masbh salama, Egypt), in addition to commercial alumina. Table 1 demonstrates the chemical analyses For characterization of the sintered samples, X-ray of raw materials. Talc and kaolin were subjected to diffraction (XRD, BRUKER, D8 ADVANCED CuO grinding and pulverizing through ball mill to develop target, Germany) was used for the identification of the powder (grain size < 63 um). The batch composition developed crystalline phases. The scanning electron was based on cordierite Mg2Al4Si5O18 talc was microscopy accoupled with energy-dispersive x-ray represented as source of MgO, kaolin and commercial microanalysis (SEM/EDAX, model FEJ Quanta 250 alumina are sources of Al2O3 and both talc and kaolin Fei, Holland) was used to study the microstructure and are the source of SiO2. Through melt quenching chemical analysis. process, the admixed batches were melted in a Physical properties comprising linear shrinkage platinum crucible at 1400 ᴼC in an electric gloubar (Ls-% in volume); bulk density (Db-g/cm3); apparent furnace for two hours. Molten glasses were quenched porosity (Pa-%) and water absorption (Wa-%) were in distilled water. The glass frit samples were ground measured through Archimedes method. The sintered in a planetary mill for 5 minutes (650 rpm for 1 samples at 1200 ᴼC were tested by a heating minute). For preparation of ceramic batch, green dilatometer (NETZSCH DIL 402 PC, Germany) up to powder was mixed and milled in an agate ball mill 700 ᴼC. grinder (650 rpm for 1 minute) then dried overnight.

Table 1. Chemical analysis of the starting raw materials

Raw Material SiO2 TiO2 Al2O3 Fe2O3 MgO CaO Na2O K2O P2O5 LOI Talc1 47.94 0.38 6.64 8.62 21.84 7.47 0.22 0.05 0.09 6.16 Talc2 49.01 0.05 5.90 9.16 24.56 5.61 0.17 0.01 0.01 4.81 Kaolin 44.56 1.98 37.34 1.12 0.39 0.09 0.10 0.02 008 14.10 Table 2. Chemical composition of the C5 and C6 batches.

Raw Material SiO2 TiO2 Al2O3 Fe2O3 MgO CaO T.A. P2O5 Mg/Si C5 48.75 1.12 26.21 5.63 13.17 4.48 0.21 0.09 0.27 C6 49.45 1.05 26.93 5.49 13.38 3.05 0.15 0.01 0.27

3. Results and Discussion 1000 °C / 2h and 1300 °C / 2h, protoenstatite (MgSiO3, COD # 96-154-8551 and mullite (Al2.25O4.871Si0.75, 3.1. Characterization of sintered glass and ceramic COD card # 96-900-1568) were developed too. The early sintering of ceramic CS5 and CS6 samples at The developed crystalline phases after sintering 1000 °C / 2h and 1100 °C temperatures led to the process, between 1000 and 1300 °C, of glasses (GC5 crystallization of mullite with cristobalite, and GC6) and ceramics (CS5 and CS6) are identified protoenstatite and spinel. Increasing the temperature in Figure 1 and 2. Cordierite (Al4Mg2Si5O18, COD up to 1200 °C/2h endorsed the crystallization of card # 96-900-6272) is the main crystalline phase in cordierite as the main phase with little protoenstatite, both samples, however, spinel (Al1.99Mg0.998O4, COD spinel and cristobalite. At 1300 °C/2h, cordierite was card # 96-900-2072) and cristobalite (SiO2, COD card crystallized with spinel in both CS5 and CS6 ceramic # 96-900-8231) were crystallized in the sintered GC5 samples (Fig 2). Lately, Valášková et. al., prepared and GC6 glasses at 1100 °C / 2h and 1200 °C /2h. In ceramic containing cordierite/indialite, enstatite and both CS5 and CS6 ceramic samples sintered between non-crystalline phases from kaolin, quartz, and ______Egypt. J. Chem. 64, No. 4 (2021)

CORDIERITE CERAMIC THROUGH GLASS AND CERAMIC ROUTES FROM KAOLIN AND TALC 1753 ______muscovite were sintered with vermiculite can imagine the results of sintering between 1000 and 2+ (Mg,Fe ,Al)3 (Al,SiO)4O10(OH)2.4(H2O) [17]. We 1300 °C temperatures as follow:

Equation (1): o Al2O3(SiO2)2(H2O)2 + Mg₃ Si₄ O₁₀(OH)₂ ~1400 C/2h Brown glass Kaolinite Talc Amorphous silica ~ 1100 ᴼC/2h Equation (2): Glass → Cristobalite – Cordierite –Spinel ~ 1200 ᴼC/2h Equation (3): Glass → Cordierite – Cristobalite – Spinel Equation (4): ~ 1000−1100 ᴼC/2h Al2O3(SiO2)2(H2O)2 + Mg₃ Si₄ O₁₀(OH)₂ → MgSiO3 + Al2.25O4.871Si0.75 + SiO2 Kaolinite Talc Enstatite Mullite amorphous silica Equation (5): ~ 1100−1200 ᴼC/2h SiO2 → SiO2 Amorphous silica Cristobalite Equation (6): ~ 1200−1300 ᴼC/2h 3(MgO.SiO2) + 3Al2O3.2SiO2 → 2MgO.2Al2O3.5SiO2 + MgO.Al2O3 Enstatite Mullite Cordierite Mg-Al spinel Equation (7): ~1300 ᴼC/2h 3(MgO.SiO2) + MgO.Al2O3 + 2SiO2 → 2MgO.2Al2O3.5SiO2 Enstatite Spinel Cristobalite Cordierite

Fig 1. X-ray diffraction patterns of GC5 and GC6 samples Fig 2. X-ray diffraction patterns of CS5 and CS6 samples sintered at 1100 °C /2h and 1200 °C/2h. sintered within 1000 °C /2h and 1300 °C/2h range.

The microstructure of GC5, GC6, CS5 and CS6 glassy matrix (Fig. 3). The sintered ceramic CS5 and samples sintered at 1200 °C/2h were scanned by SEM CS6 samples showed scattered pores (~ 3 and ~ 5 % (Fig. 3, 4). Scattered pores were spread in both GC5 respectively) in matrix of fused residual glass (Fig. 4). and GC6 samples which was bigger in GC6 (~ 10 %) The cordierite with spinel and cristobalite in CS5 than in GC5 (~ 5 %) (Fig. 3). The microstructure of sample was modified into rod-like particles whose GC5 showed rounded to subrounded cluster of nano- width between 100 and 200 nanometer. However, in size particles (50-100 nanometer) which are clear the CS6 sintered sample the microstructure shows through spread pores whereas in case of GC6 ceramic clear cordierite crystals of hexagon marking spread in euhedral crystals of both cordierite (hexagonal) and glassy matrix (Fig. 4). cristobalite (cubic) in sub-micron size in residual ______Egypt. J. Chem. 64. No. 4 (2021)

1754 A.M. Yahya et.al. ______However, cordierite nanocomposite was prepared from kaolin, talc and alumina with vermiculite and zirconium [18]. Also, nano-cordierite particles were prepared from sintered kaolin, talc and vermiculite

doped with CeO2 [19]. In general, sintering of GC5 and CS5 samples gave nano size rounded- or rod- crystals either free or in clusters in glassy matrix. In contract, sintering of GC6 and CS6 samples gave clear euhedral to subhedral tetragonal to hexagonal crystals in submicron scale. The EDX microanalysis of some clear crystals and Fig 3. SEM micrographs of GC5 and GC6 samples sintered at 1200 grain are given in Table 3. Figure 5 shows the results of the microanalysis compared to the developed phases.

Fig 4. SEM micrographs of CS5 and CS6 samples sintered at 1200 °C/2h.

Fig. 5. EDX microanalysis of GC5, GC6, CS5 and CS6 sintered at 1200 °C/2h.

______Egypt. J. Chem. 64, No. 4 (2021)

CORDIERITE CERAMIC THROUGH GLASS AND CERAMIC ROUTES FROM KAOLIN AND TALC 1755 ______

Table 3. EDX microanalysis of the GC5, GC6, CS5 and CS6 samples. Chemical Nominal Nominal Nominal Nominal GC5 CS5 GC6 CS6 constituent cordierite Spinel enstatite mullite O 49.23 44.98 47.81 48.82 23.73 37.37 51.89 48.09 Mg 8.31 17.08 24.21 n.d. 6.37 8.13 7.68 8.15 Al 18.45 37.93 n.d. 38.00 14.42 10.62 13.70 15.49 Si 24.01 n.d. 27.98 13.18 33.41 26.03 19.96 21.31 Fe n.d. n.d. n.d. n.d. 8.61 11.71 4.11 3.81 Ca n.d. n.d. n.d. n.d. 13.41 5.78 2.64 n.d. Developed Cord/Crist/ Cord/Crist Cord/En/ Cord/En/Mullite phases Spinel /Spinel Crist Table 4. Density, linear shrinkage, apparent porosity, and water absorption of the GC5, GC6, CS5 and CS6 samples sintered at 1200 °C/2h. Sintering temperature GC5 GC6 °C/2h L.S. Db Pa Wa L.S. Db Pa Wa 1100 6.89 2.41 9.50 3.94 2.90 1.96 29.34 14.90 1150 7.20 2.43 5.97 2.46 3.01 1.96 27.92 14.19 1200 9.15 2.28 5.46 2.39 4.83 2.09 9.60 4.61 CS5 CS6 1000 1.70 1.90 36.20 19.50 2.10 2.00 30.80 15.40 1100 3.10 1.95 32.00 16.40 3.10 2.20 26.40 12.60 1200 5.80 2.29 4.90 2.20 5.60 2.35 3.30 1.40

Note*: L.S.: Linear shrinkage; Db: Bulk density; Pa: Apparent porosity; Wa: Water absorption [22–25]. Also, cordierite glass-ceramics have CTE of 3.2. Physical Properties of sintered glasses and 25.00 × 10-7 and 4.39 × 10-6 ᴼC-1 [22 – 25]. On the other ceramics hand, low and negative CTE of ceramic containing cordierite was obtained and the authors ascribed that Linear shrinkage (L.S.), bulk density (Db), apparent to change in the c-axis of the crystal structure of porosity (Pa) and water absorption (Wa) are the basic cordierite [26 – 27]. Earlier, cordierite associated with parameter to evaluate densification of the prepared little amount of other phases has CTE value ~ 3.38 × ceramics as shown in Table 4. In the sintered ceramic 10-6 ᴼC-1, and in case of increasing the MgO ratio [i.e. samples, the linear shrinkage and bulk density increase increase of magnesium silicate phase], CTE value ᴼ with the sintering temperature from 1000 to 1200 C developed to 2.82 × 10-6 ᴼC-1 and 2.32 × 10-6 ᴼC-1 with which may be attributed to the development of liquid sapphirine phase [28]. In the bulk cordierite ceramic, phase filling some pores in ceramic samples or partial the authors attributed the change in CTE value to the melting in sintered glasses [20]. In the later formation of multi-crystalline phases with cordierite consequence, densification continues to rise due to such as quartz and cristobalite which causes micro- crystallization of cordierite content through decreasing cracking due to the changes in the CTE of the the ratio of cristobalite and spinel, which accelerates developed crystalline phases with cordierite [29]. the diffusion of substance that contribute to the Lately, the porous sintered 2MgO∙2Al2O3∙2B2O3∙ densification. 5SiO2 glass gave low and – ve CTE [30]. In ceramics and glass-ceramics, the coefficient of In the present work, low and –ve CTE cordierite thermal expansion CTE is the factor of the crystalline containing sintered ceramic or glass may be due to phases and residual glass [19]. For crystalline samples, either the change in c-axis or the cracks either due to the value of CTE of the sintered ceramic were 6.38 and change in CTE of the developed phases or the -. ᴼ -1 ᴼ -36.1 × 10 C (in the range of 24- 500 and 700 C) developed pores [30]. In general, the CTE was higher - whereas the values were between 1.63 and -3.93 × 10 in sintered ceramic compared to those in the sintered 6 ᴼ -1 ᴼ C (in the range of 24- 500 and 700 C) in case of glasses which may be due to the presence of remnants sintered glasses (Table 5). The aforementioned work particles of minerals coexist with cordierite which may mentioned that the CTE value of crystalline cordierite have high CTE [28]. On the other hand, the low CTE -6 ᴼ -1 ceramic was 1.60 and 3.38 × 10 C [11, 13] and was in the sintered glasses containing cordierite with little -7 -6 ᴼ -1 25 × 10 and 4.39 × 10 C for the glass-ceramics cristobalite, spinel, enstatite and mullite, was ______Egypt. J. Chem. 64. No. 4 (2021)

1756 A.M. Yahya et.al. ______

Table 5. The CTE and Vickers hardness values of the GC5, GC6, CS5 and CS6 samples sintered at 1200 ᴼC/2 h. dL/ Lo (×10-6) Vickers’ hardness Developed phases Temperature, [ᴼC] 24-500 ᴼC 24-700 ᴼC (Kg/mm2) CS5 -0.73 1.21 527 Cord + En + Crist + glass CS6 6.38 2.09 468 Cord+ En + Mull + glass GC5 1.63 0.93 553 Cord+ Crist + Spinel + glass GC6 -2.93 -0.88 577 Cord+ Crist + Spinel + glass associated with internal porosity where GC6 has the cluster in nano-size particles which are clear through higher porosity accompanying with negative CTE spread pores and euhedral crystals of both hexagonal value (Table 5). cordierite and tetragonal cristobalite in sub-micron The microhardness values of the present sintered size in residual glassy matrix. In the sintered ceramic ceramic and glass samples were between 468 and 577 scattered pores in matrix of fused residual glass and cordierite with spinel and cristobalite was modified as Kg/mm2 (Table 5). Although the pre-literature gave rod- like particles their width in nanometer appears high value of the cordierite hardness, in the range of through pore, however, their microstructure shows 2 513 – 963 kg/mm [28, 31], whereas in the present clear cordierite crystals with hexagon marking spread samples the low values of microhardness may be due in glassy matrix too. Density and porosity of the to the presence of cracks due to the internal pores in sintered ceramic are between 1.96 and 2.43 g/cm3 and the samples. between 29.34 and 5.46 % respectively, whereas as density and porosity of sintered glasses are between 4. Conclusion 1.90 and 2.35 g/cm3 and between 36.20 and 3.30 % Cordierite ceramic was prepared through ceramic respectively. Low and negative CTE were obtained in -6 and melt quench routes. Cordierite, spinel, mullite, the sintered glasses (between 6.38 and -36.1 × 10 -1 enstatite and cristobalite developed in both samples °C (in the range ~ 24 -500 and 700 °C). The through sintering process. The microstructure of the microhardness values for all sintered samples are 2 sintered glasses displayed rounded to subrounded between 468 and 577 Kg/mm . 6.Acknowledgment 5.Conflicts of interest The authors gratefully acknowledge to Applied The authors declare that they have no known mineralogy laboratory, Geology department, Faculty competing financial interests or personal relationships of science, Ain shams University, Egypt for the that could have appeared to influence the work support of this research work. reported in this paper.

7.References composites, Ceramic international, 31(3), 383- 1. Levin, E.M., Robbins, C.R., McMurdie, H.F., Phase 389 (2005). Diagrams for Ceramists. Journal of the American 6. Al-Harbi, O.A., Hamzawy, E.M., Nanosized Ceramic Society, 601 (1964). cordierite–sapphirine–spinel glass-ceramics from 2. Mao, H., Fabrichnaya, O., Selleby, M., Sundman, natural raw materials, Ceramic international, B., Thermodynamic assessment of the MgO– 40(4), 5283-5288 (2014). Al2O3–SiO2 system, Journal of Materials 7. Al-Harbi, O.A., Hamzawy, E.M., Method of Research, 20(4), 975-986 (2005). making porous mono cordiertie glass ceramic 3. Chowdhury, A., Maitra, S., Das, S., Sen, A., material and its use, U.S. Patent Application No. Samanta, G. K., Datta, P.: Synthesis, properties 15/258,021 (2018). and applications of cordierite ceramics Part 1, 8. Eskandari, M., Jahantigh, F., Malekfar, R., Interceram, 56 (1), 18 (2007). Synthesis and characterization of nanosized pure 4. Cheng, H., Ye, F., Chang, J., Wu, S., In situ α-cordierite glass-ceramic powders, Journal of the synthesis and thermal shock resistance Australian Ceramic Society, 54(2), 243-249 of a cordierite-mullite composite for solar thermal (2018). storage, International Journal of Applied Ceramic https://link.springer.com/article/10.1007/s41779- Technology, 16 (2), 772–780 (2019). 017-0147-2 5. Hamzawy, E.M., El-Kheshen, A.A., Zawrah, M.F., 9. Soltan, A.M.M., Elshimy,H., Abd EL-Raoof, F., Densification and properties of glass/cordierite Fuchs, F., Köenig, A., Yahya, A.M., AbdelFattah

______Egypt. J. Chem. 64, No. 4 (2021)

CORDIERITE CERAMIC THROUGH GLASS AND CERAMIC ROUTES FROM KAOLIN AND TALC 1757 ______

M.M., Serry M., Pöllmann, H., Microstructure Cordierite/CeO2 ceramic nanocomposites from and phase composition of cordierite-based co- vermiculite with fixed CeO2 nanoparticles, talc clinker, Ceramic international, 44(6), 5855-5866 and kaolin, Applied Clay Science, 179, 105-150 (2018). (2019). 10. Tabit, K., Waqif, M., Saâdi, L.: Crystallization 20. Wu, J., Lu, C., Xu, X., Zhang, Y., Wang, D., behavior and properties of cordierite synthesized Zhang, Q., Cordierite Ceramics Prepared from by sol-gel technique and hydrothermal treatment, Poor Quality Kaolin for Electric Heater Supports: Journal of the Australian Ceramic Society, 55(2), Sintering Process, Phase Transformation, 469-477(2019). Microstructure Evolution and Properties, Journal https://link.springer.com/article/10.1007/s41779- of Wuhan University of Technology-Mater. Sci. 018-0253-9 Ed., 33(3), 598-607 (2018). 11. Wu, J., Lu, C., Xu, X., Wang, D., Zhang, Y., Zhou, 21. Malekzadeh, H., Rezvani, M., Effect of CaO Y., Preparation and characterization of cordierite additive on sintering and crystallization behavior ceramic from coal series kaolin for electronic of cordierite glass–ceramic prepared by sol–gel application, Journal of the Australian Ceramic method, Journal of Sol-Gel Science and Society, 55(4), 943-952. (2019). Technology, 66(2), 199-205 (2013). 12. Wu, J., Lu, C., Xu, X., Wang, D., Sang, Y., Zhang, 22. Wang, S.M., Kuang, F.H., Yan, Q.Z., Ge, C.C., Qi, C., Influence of silica phase transformation on L.H., Crystallization and infrared radiation synthesis of cordierite ceramic, Journal of the properties of iron ion doped cordierite glass- Australian Ceramic Society, 53(2), 499-510 ceramics, Journal of Alloys and Compounds, (2017). 509(6), 2819-2823 (2011). https://link.springer.com/article/10.1007/s41779- 23. Holand, W., Beall, G.H.: Glass-Ceramic 017-0060-8 Technology. Third Edition, Willy (2001) 13. Lao, X., Xu, X., Jiang, W., Liang, J., Miao, L., Wu, 24. Kang, J., Chen, J., Chen, Z., Hou, Y., Qu, Y., Yue, Q., Influences of impurities and mineralogical Y., Crystallization, sinterability, and dielectric structure of different kaolin minerals on thermal properties of MgO–Al2O3–SiO2 glass-ceramics properties of cordierite ceramics for high- doped with TiO2, Journal of Materials Science: temperature thermal storage, Applied Clay Materials in Electronics, 31, 5697-5702 (2020). Science, 187, 105485 (2020). 25. Hamzawy, E.M., Al-Harbi, O.A., Sintered Mono- 14. Li, Y., Zhao, H., Effect of Fe2O3 addition on Cordierite Mg2Al4−xBxSi5O18 Glass-Ceramic with sintering behavior of cordierite ceramic obtained B/Al Replacement at the Nano-and Micro-Scale, by solid-state sintering method, Journal of the Silicon, 10(2), 439-444 (2018). Australian Ceramic Society, 55(2), 567-574. 26. Son, M.A., Chae, K.W., Kim, J.S., Kim, S.H., (2019). Structural origin of negative thermal expansion of 15. Naskar, M.K., Chatterjee, M., A novel process for cordierite honeycomb ceramics and crystal phase the synthesis of cordierite (Mg2Al4Si5O18) evolution with sintering temperature, Journal of powders from rice husk ash and other sources of the European Ceramic Society, 39(7), 2484-2492 silica and their comparative study, Journal of the (2019). European Ceramic Society, 24(13), 3499-3508 27. Evans, D.L., Fischer, G.R., Geiger, J.E., Martin, (2004). F.W., Thermal expansions and chemical 16. Eldera, S.S., Alharbi, O.A., Rüssel, C., Al-wafi, R., modifications of cordierite, Journal of the Hamzawy, E.M., Nano-scale cordierite glass- American Ceramic Society, 63(11‐ 12), 629-634 ceramic from natural raw materials with different (1980). fluoride additions, Silicon, 12, 1051-1057 (2020). 28. Lamara, S., Redaoui, D., Sahnoune, F., Heraiz, M., 17. Valášková, M., Klika, Z., Novosad, B., Smetana, Saheb, N., Microstructure, thermal expansion, B., Crystallization and Quantification of hardness and thermodynamic parameters of Crystalline and Non-Crystalline Phases in Kaolin- cordierite materials synthesized from Algerian Based Cordierites, Material, 2019 (12), 3104 natural clay minerals and magnesia, Boletín de la (2020). doi:10.3390/ma12193104. Sociedad Española de Cerámica y Vidrio, (2020). 18. Valášková, M., Tokarský, J., Hundáková, M., https://doi.org/10.1016/j.bsecv.2020.03.008 Zdrálková, J., Smetana, B., Role of vermiculite 29. Shyam, A., Bruno, G., Watkins, T.R., Pandey, A., and zirconium–vermiculite on the formation of Lara-Curzio, E., Parish, C. M., and Stafford, R. J., zircon–cordierite nanocomposites, Applied Clay The effect of porosity and microcracking on the Science, 75, 100–108 (2013). thermomechanical properties of cordierite, 19. Valášková, M., Hundáková, M., Smetana, B., Journal of the European Ceramic Society, 35(16), Drozdová, L., Klemm, V., Rafaja, D., 4557-4566 (2015). ______Egypt. J. Chem. 64. No. 4 (2021)

1758 A.M. Yahya et.al. ______

30. Eldera, S.S., Al-wafi, R., Al Harbi, O.A., Rüssel, 31. Ghosh, S., Pal, K.S., Mandal, A.K., Biswas, N., C., Hamzawy E.M.A.: Negative thermal Bhattacharya, M., Bandyopadhyay, P., Cordierite expansion in porous glass-ceramics based on based glass-ceramic glazed floor tiles by Mg2Al2B2Si5O18 prepared from Saudi raw microwave processing, Materials materials, Journal of Mechanical Science and Characterization, 95, 192-200 (2014). Technology, 34(11), 4597-4604 (2020):

______Egypt. J. Chem. 64, No. 4 (2021)