Preparation study for the low thermal expansion spodumene/mullite composites

In this work, spodumene/mullite ceramics with low thermal expansion were successfully prepared from spodumene, quartz, talc, and clay. The effects of spodumene content and sintering temperature on the mechanical properties of spodumene/mullite ceramics were investigated. The formed phases were then detected by X-ray diffraction analysis and the microstructures of the sintered bodies were determined by scanning electron microscopy. The interaction effects of the spodumene content and sintering temperature on the apparent porosity and bulk density were studied by response surface methodology. The results demonstrate that an appropriate sintering temperature and spodumene content can promote densification, improve the mechanical properties, and reduce the coefficient of thermal expansion (CTE) of spodumene/mullite ceramics. At the spodumene content of 40 wt.%, the sintering temperature of 1270°C, and the holding time of 90 min, the bending strength was 60.45 MPa, the CTE was 1.73 × 10^–6/°C (α_{[25–650°C]} < 2 × 10^–6/°C), the bulk density was 2.28 g cm^-3, and the apparent porosity was 0.43%. Therefore, this study was of guiding significance for reducing the production cost of spodumene low thermal expansion ceramics and improving product quality.     

Additive manufacturing of electrofused mullite slurry by digital light processing

Mullite, one of the main refractory materials, has several applications that may demand tiny structures with complex geometries, and digital light processing (DLP) can produce such parts with outstanding dimensional precision and surface quality. In this work, electrofused mullite powder was used as a raw material for additive manufacturing by DLP. Photosensitive mullite suspensions were developed and their rheological behavior, stability, and thermal decomposition were investigated. Mullite parts were printed from suspensions with different ceramic loadings, debound, and sintered at different temperatures (from 1500 to 1650 °C). Density and strength increased with an increase in both solid loading and sintering temperature. Printed parts from slurry with 50 vol% of solid loading sintered at 1650 °C reached a relative density of 97.7 ± 0.3 % and flexural strength of 95.2 ± 5.0 MPa.     

Development of cordierite/mullite composites using industrial wastes

Ceramics containing cordierite and mullite as their principal phases are promising for many applications, due to properties such as a low coefficient of thermal expansion, high durability, low dielectric constant, resistance to thermal shock, and refractoriness. The objective of this study was to produce ceramic composites suitable for use as refractory materials. The raw materials were subjected to chemical characterization and the formulations to physical, chemical, and mineralogical characterization. The specimens were formed by pressing, dried at 110°C, and sintered from 1150°C to 1300°C for 2 hours. The following properties were then determined: linear shrinkage, water absorption, apparent porosity, and flexural modulus of rupture. The phases formed, crystal morphology, and coefficient of thermal expansion were evaluated. The cordierite and mullite phases were observed in all formulations at 1250°C and 1300°C. The results obtained from the formulations with a higher content of fine kaolin residue suggest that these formulations have the potential to be used for the manufacture of refractory materials such as furnace rollers and supports.     

On the physico-mechanical,electrical and dielectric properties of mullite-glass composites

Mullite-glass composites were obtained by solid-state reactive sintering of kaolinite clay and kaolin waste mixtures with waste additions up to 100 wt%. The structural and microstructural analysis of starting powders and sintered samples were evaluated by X-ray diffractometry (XRD) and field-emission scanning electron microscopy (FESEM). The mechanical properties were evaluated by measuring the flexural strength of sintered bodies. Electrical properties of the composites were assessed by impedance spectroscopy (at 30 °C and from 400 to 700 °C) in air. A viscous flux mechanism resulting from the glassy phase filled up the open porosity and increased the mechanical strength. Electrical conductivity, dielectric constant and dielectric loss were strongly dependent on the microstructural features, namely glassy phase and porosity. The activation energies (0.89–0.99 eV) for electrical conduction were lower than typical literature values of mullite-based materials. The results indicated that the herein synthesized mullite-glass composites with up to 53.6 wt% mullite are promising low-cost materials for electronics-related applications.     

Cellular mullite materials processed by direct foaming and protein casting

In this paper, cellular mullite bodies were developed by thermal direct-consolidation of foamed aqueous mullite-bovine serum albumin (BSA) and mullite-BSA-methylcellulose suspensions, burning out (650 °C, 2 h) and sintering (1600 °C, 2 h). Some modifications to the shaping route conventionally used in protein casting were incorporated in the proposed processing to obtain bodies with controlled and homogeneous microstructures. The materials were characterized by porosity measurements, analysis of phases by XRD, and microstructural analysis by SEM and Hg-porosimetry. Characteristic parameters of cell size distributions, percentage of open and closed cells, window size and interstitial pore size distributions, and microstructural features of the mullite matrix were determined. Moreover, basic 2D cell size parameters and global 3D stereological parameters were analysed. The obtained results showed that mullite bodies with hierarchical porosity and different microstructural features were developed from the design and control of processing routes, which use BSA as a foaming and binder/consolidator agent.     

Electrospun mullite nanofibers derived from diphasic mullite sol

Fine‐grained mullite nanofibers derived from the diphasic mullite sol were successfully fabricated by electrospinning and subsequent pyrolysis at 1500°C. Polymethylsiloxane and aluminum tri‐sec‐butoxide were selected as the silicon and aluminum source to synthesize the diphasic sol. Results show that the weight loss of mullite precursor fibers in our work was about 60 wt.%, which is similar with that of fibers fabricated using the monophasic sol. This low weight loss was mainly attributed to the high ceramic yield of polymethylsiloxane and low introduced polyvinylpyrrolidone content, which ensures the integrity of fiber morphology during the sintering process. Mullite fibers with 216 nm average diameter were fabricated after sintered at 1500°C and the corresponding grain size was only ~100 nm, much smaller than that in mullite fibers derived from monophasic sols. Therefore, it can be predicated that mullite fibers in this work should possess a higher mechanical strength than those derived from monophasic sols when the sintering temperature was higher than 1400°C and therefore was an ideal starting materials for the fabrication of mullite nanofibrous ceramics used as the high‐temperature thermal insulation materials.     

Thermo-mechanical and high-temperature dielectric properties of cordierite-mullite-alumina ceramics

Heterogeneous ceramics made of cordierite (55–56 wt%), mullite (22–33 wt%) and alumina (23–11 wt%) were prepared by sintering non-standard raw materials containing corundum, talc, α-quartz, K-feldspar, kaolinite and mullite with small amounts of calcite, cristobalite and glass phases. The green specimens prepared by PVA assisted dry-pressing were sintered within the temperature range of 950–1500 °C for different dwelling times (2–8 h). The effects of sintering schedule on crystalline phase assemblage and thermomechanical properties were investigated. The sintered ceramics exhibited low coefficients of thermal expansion (CTE) (3.2–4.2×10⁻⁶ °C⁻¹), high flexural strength (90−120 MPa and high Young modulus (100 GPa). The specimens sintered at 1250 °C exhibited the best thermal shock resistance (∆T~350 °C). The thermal expansion coefficients and thermal shock resistance were studied using Schapery model, the modelling results implying the occurrence of non-negligible mechanical interactions between the phases in bulk. The dielectric properties characterized from room to high temperature (RT– HT, up to 600 °C) revealed: (i) noticeable effects of sintering schedule on dielectric constant (5–10) and dielectric loss factor (~0.02–0.04); (ii) stable dielectric properties until the failure of the electrode material. The thermomechanical properties coupled with desirable dielectric properties make the materials suitable for high density integrated circuitry or high temperature low-dielectric materials engineering.     

Phase Evolution,Microstructure, and Mechanical Properties of Alumina–Mullite–Zirconia Composites Prepared by Iranian Andalusite

This paper investigates the effects of Iranian andalusite and short milling times on alumina–mullite–zirconia composites. Andalusite powder was added at 0, 2.5, 5, and 10 wt% to an alumina–zircon mixture and the raw materials were milled for 1 or 3 h. The sintering of samples was carried out at the temperatures of 1550°C, 1600°C, and 1650°C for 3 h. Microstructural changes, phase composition, physical properties, and mechanical strength of the sintered composites were characterized by scanning electron microscopy, X‐ray diffraction, density, and strength measurement tests. Results show that andalusite promoted the decomposition of zircon and accelerated the reaction sintering of alumina–zircon, which leads to the formation of much more mullite phase and improvements to the composites’ thermal shock resistance up to about 50%.     

Recycling of aluminum dross and silica fume wastes for production of mullite-containing ceramics: Powder preparation,sinterability and properties

The improper disposal of industrial wastes causes environmental pollution so their recycling for fabrication of new products became an interesting research issue. In this work, sintered mullite-containing ceramics were prepared from aluminum dross and silica fume (up to 40 wt%) waste materials after sintering up to 1500 °C. Before sintering, the starting waste materials were converted into nano powders by mechanical milling alloying method up to 15 h. The obtained waste nano powders were investigated using different techniques as X-ray diffraction (XRD), transmission electron microscope (TEM) and scanning electron microscope (SEM). On the other hand, phase identification by XRD, physical properties determination (bulk density and apparent porosity), microstructure by SEM, mechanical and electrical properties of sintered bodies were investigated. The results revealed that mullite phase was formed in higher amounts with increasing both sintering temperature (1500 °C) and silica fume content. At 1300 °C, amorphous mullite was formed in addition to the alumina phase. It is also noted that the apparent porosity and bulk density were reduced with increasing silica content. However, they exhibited opposite trend when the temperature increased from 1300 into 1500 °C. Moreover, with increasing the mullite content, the microhardness, compressive strength, Younges modulus and electrical conductivity were decreased and reached 10.2 GPa, 216.9 MPa, 119.7 GPa and 4.9 × 10 ^?12 S/m, respectively, for the sample that contained higher amount of mullite, while the fracture toughness was improved and reached to 3.44 MPa m^0.5.     

High-toughness mullite ceramics fabricated by hot-press sintering of pyrophyllite and AlOOH at low temperatures

High-toughness mullite ceramics were fabricated through hot-press sintering (HPS) of pyrophyllite and AlOOH, which were wet-milled and well mixed using a planetary ball mill. The impacts of sintering temperatures and contents of AlOOH on mullite phase formation, densification, microstructure and mechanical properties in ceramic materials were investigated through XRD, SEM and mechanical properties determination. The results indicated that high-toughness mullite ceramics could be successfully prepared by HPS at temperatures higher than 1200°C for 120 min. Increasing the sintering temperature from 1000 to 1300°C significantly enhanced the flexural strength and fracture toughness of samples. The highest flexural strength of 297.97±25.32 MPa and fracture toughness of 4.64±0.11 MPa⋅m^1/2 were obtained for samples sintered at 1300°C. Further increase of temperature to 1400°C resulted in slight decrease of flexural strength and fracture toughness. Compared with the mullite ceramics prepared only using pyrophyllite as raw material, incorporation of AlOOH into raw material significantly increased the mechanical properties of final mullite ceramics. And stoichiometric AlOOH and pyrophyllite as starting material gave the best performance in fracture toughness. The high-toughness of mullite ceramics were ascribed to the high mullite phase content, fine mullite whiskers and in situ formed, intertwined three-dimensional network structure obtained through HPS at a low temperature of 1300°C.     

Aluminosilicate fiber/mullite matrix composites with favorable high-temperature properties

Oxide-based ceramic matrix composites with a highly porous mullite matrix and Nextel™ 720 alumino silicate fibers have been fabricated by infiltrating filaments with a mullite precursor slurry, and by subsequent one-dimensional (1D) and two-dimensional (2D)-winding up the fiber bundles on mandrels. The green bodies were pressureless sintered in air at 1300°C. These composites which require no fiber/matrix interface are characterized by favorable damage tolerance and bending strengths of 160 MPa at room temperature and up to temperatures of 1200°C. These properties make it an excellent low-cost choice for combustion chamber liners, diffusor rings and other thermal protection systems for high temperature applications in oxidizing environment.     

Preparation and performance study of cordierite/mullite composite ceramics for solar thermal energy storage

The employment of solar energy in recent years has reached a remarkable edge. It has become even more popular as the cost of fossil fuel continues to rise. Energy storage system improves an adjustability and marketability of solar thermal and allowing it to produce electricity in demand. This study attempted to prepare cordierite/mullite composite ceramics used as solar thermal storage material from calcined bauxite, talcum, soda feldspar, potassium feldspar, quartz, and mullite. The thermal physical performances were evaluated and characterized by XRD, SEM, EPMA, and EDS. It was found that the optimum sintering temperature was 1280°C for preparing, and the corresponding water adsorption was 11.25%, apparent porosity was 23.59%, bulk density was 2.10 mg·cm^?3, bending strength was 88.52 MPa. The residual bending strength of specimen sintered at 1280°C after thermal shock of 30 times decreased to be 57 MPa that was 36% lower than that before. The thermal conductivity of samples sintered at 1280°C was tested to be 2.20 W·(m·K)^?1 (26°C), and after wrapped a PCM (phase change materials) of K₂SO₄, the thermal storage density was 933 kJ·kg^?1 with the temperature difference (ΔT) ranged in 0‐800°C. The prepared cordierite/mullite composite ceramic was proved to be a promising material for solar thermal energy storage.     

Behaviour of cordierite materials under mechanical and thermal biaxial stress

Abstract

A commercial cordierite powder (< 0.17 wt-% impurities) was selected for a study of material behaviour under mechanical and thermal stresses. Disks were slip cast, sintered for 2 h at 1450°C, and indented (Vickers, 44.1 N) at the centre of the surface to be subjected to mechanical and thermal shock tests. The sintered bodies (84 wt-% cordierite, 10 wt-% mullite, 6 wt-% glass) reached 95% of theoretical density. The microstructure consisted of homogeneous, mainly equiaxed grains (mean size ≈0.5 μm) and a few elongated grains (aspect ratio ≈1.9). A glass phase was identified at triple points, and intergranular pores (< 10 μm) and a few isolated larger pores (up to 40 μm) were observed. The fracture strength σ_F was measured by biaxial flexure, employing a ball on discontinuous ring configuration with displacement con1 trol (0.05 mm min ^-1). In each thermal shock test, the indented specimen was heated to a selected temperature and the disk centre was then suddenly cooled using a high velocity air jet at room temperature. The initial temperature was increased by increments of 10°C until crack propagation was detected and the value of the thermal shock resistance Δ T_C was evaluated. The values obtained were compared with cordierite disks without indents and with alumina materials. The fracture features of the specimens broken in both mechanical and thermal shock tests (crack patterns and fracture surfaces) were characterised, taking into account the developed microstructures (grains, phases, pores) and the fracture origin at the controlled size defect introduced by indentation.     

Recycling and Utilization of some Waste Clays for Production of Sintered Ceramic Bodies

The recycling of industrial waste clays for production of an interesting ceramic product is the main goal of the present research work. Ceramic bodies were prepared using Feeders or Cyclons waste clays, sand and feldspar. 0.0, 15, 20, and 25 wt.% of sand were added at the expanse of kaolin (75-50 wt.%). Constant mass percent (25 wt.%) of feldspar was added for all ceramic compositions. The designed batches were sintered at 1200–1400 °C. Physical properties were determined by water displacement method. Phase composition and microstructure were investigated by x-ray diffraction and scanning electron microscope, respectively. The compressive strength was also determined. The results indicated that the ceramic bodies prepared from Cyclons’ waste clay exhibited higher physical and mechanical properties than that prepared from Feeders’ clay after sintering at 1400 °C. The addition of sand enhances the porosity, water absorption, bulk density and mechanical strength after sintering at 1400 °C due to the formation of mullite network and glassy phases.

     

The Effect of La2O3 Addition on Sol–Gel Derived Mullitization

Monophasic gel with stoichiometric 3Al₂O₃·2SiO₂ composition and gels with 0.99, 1.96, and 2.91 mol% La₂O₃ added were sol–gel derived. The crystallization path, structure evolution, microstructure, and morphology of calcined premullite powders and sintered ceramic bodies have been investigated as a function of La₂O₃ content and sintering temperature. In addition to mullite, spinel phase at about 980°C, and α‐alumina at above 1000°C were determined; however, neither La₂O₃ nor La‐related compounds had crystallized. The La₂O₃ predominately incorporated into the glassy phase, enhanced with La₂O₃ level, which affected both mullite structure and composition, as confirmed by electron microscopy, Rietveld structure refinement, determination of unit cell parameters, electron microscopy, and achieved density of the sintered bodies. Increased thermal treatment changes the alumina/silica ratio in mullite (towards 3:2 below 1200°C, and toward 2:1 above), and decreases the mullite/amorphous ratio. Sintered dense ceramic bodies revealed a positive densification effect and increased sinterability as a result of the lanthanum‐induced increase in glassy phase.     

Preparation and Performance Study of Mullite/Al2O3 Composite Ceramics for Solar Thermal Transmission Pipeline

For lowering sintering temperature of mullite/Al₂O₃ composite ceramics for solar thermal transmission pipeline, kaolin, potassium feldspar, quartz, and γ‐Al₂O₃ were used as raw materials to in situ synthesize the composite ceramics with pressureless sintering method. Densification, mechanical properties, thermal expansion coefficient, thermal shock resistance, phase composition, and microstructure were investigated. The experiment results demonstrated that the introduction of potassium feldspar and quartz decreased the lowest sintering temperatures greatly to 1300°C. The optimum sample A3 sintered at 1340°C obtained the best performances. The water absorption, apparent porosity, bulk density, bending strength, and thermal expansion coefficient of A3 were 0.04%, 0.12%, 2.71 g/cm³, 94.82 MPa, and 5.83 × 10^?6/°C, respectively. After 30 thermal shock cycles (wind cooling from 1100°C to room temperature), no cracks were observed on the surfaces of the sample, and the bending strength increased by ?7.96%. XRD analysis indicated that the main phases of samples before and after 30 thermal shock cycles were consistently mullite, corundum, and α‐cristobalite, while the content of mullite increased after thermal shock. SEM micrographs illustrated that the mullite grains growth and micro‐cracks appeared after thermal shock endowed the composite ceramics with excellent thermal shock resistance.     

Porous mullite ceramics with low thermal conductivity prepared by foaming and starch consolidation

Porous mullite ceramics were prepared from an industrial grade mullite powder by foaming and starch consolidation. The viscosities of the original suspensions and the foamed ones with solid loading of 62.5 and 67.5 wt% were measured. After the steps of forming and drying, the green bodies were sintered under different temperatures from 1,200 to 1,600 °C for 2 h. The influence of solid loading of suspension and sintering temperature on the porosity and compressive strength was evaluated. The sintered mullite ceramics, with porosity from 86 to 73 vol% and corresponding compressive strength from 1 to 22 MPa, contained a multi-modal microstructure with large spherical pores and small pores on internal walls. Thermal conductivity measurement carried out by the transient plane source technique at room temperature resulted in values as low as 0.09 W/mK. In addition, the relationship between thermal conductivity and porosity was discussed in detail.     

Insight into the corrosion failure of mullite thermal insulation materials in carbon monoxide

The service condition of mullite thermal insulation materials is complicated, the effects of carbon deposition are always considered the primary cause of damage to mullite ceramic in carbon monoxide atmosphere. In the present study, mullite thermal insulation material was subjected to a carbon monoxide atmosphere at 1100°C–1400°C. The thermodynamics stability, phase composition, and microstructure of the mullite thermal insulation material were analyzed. Furthermore, the effects of carbon monoxide corrosion on thermal shock resistance and compressive creep behavior at high temperatures were evaluated. The carbon content in the mullite-based insulation material is below 0.02% after treatment at 1100°C–1400°C. After treatment at 1400°C, most areas in the specimen comprised corundum and glass phase, and K, Na, Ca, Mg, and Fe were detected as impurities, leading to the improvement of cold crushing strength after 20 thermal shocks but a remarkable recession in high-temperature compressive creep.     

High-temperature diametral compression strength of microwave-sintered mullite

The mechanical strength of mullite materials sintered by the conventional route or by microwave was evaluated by diametral compression at room temperature and 1400 °C. Crack patterns and fracture mechanisms were analyzed and the results were discussed in terms of the final microstructures. The conventional and microwave sintered materials showed similar densification degrees and homogeneous microstructures with small equiaxial grains. Independent of the sintering route, the fracture strength did not change as the temperature increased. However, the mechanical strength of microwave sintered mullite was always higher than the conventionally sintered materials. Moreover, in both mullite materials, microcracks produced by the effects of thermal expansion and/or elastic anisotropies during sintering and/or mechanical testing were critical defects. In the early steps, microcracks occurred in transgranular mode. However, upon approaching the critical condition, their propagation was more intergranular until they coalesced and the specimen failed, generally in a triple-cleft fracture.     

Mechanical,morphological and dielectric properties of sintered mullite ceramics at two different heating rates prepared from alkaline monophasic salts

The sintering behavior of nanocrystalline orthorhombic mullite powders was investigated. The changes in microstructure, mechanical and dielectric properties with two different heating rates were explained. Microstructural characteristics depending on heating rate were explained at different sintering temperatures. Dielectric properties of prepared mullite nanocomposites were studied to examine the synthesized mullite ceramics as high permittivity materials in the microwave range. It was indicated that a sharp decrease in bulk density was observed at 1600 °C due to the exaggerated growth of mullite grains. Moreover, a maximum hardness value of 4.97 GPa was obtained at 1600 °C with slow heating rate (5 °min^?1). The DC electrical resistivity with a slow heating rate at 1300 °C was approximately three times the value of the mullite sample sintered with a fast heating rate (30 °min^?1). The minimum dielectric loss of about 0.017 at 1.5 GHz was achieved at a sintering temperature of 1500 °C with a slow heating rate.