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Synthesis, Properties and Applications of Cordierite Ceramics, Part 2


A. Chowdhury, S. Maitra, H.S. Das, A. Sen, G.K. Samanta, P. Datta

Anirban Chowdhury is a post-graduate research student working in the area of sol gel ferroelectrics for his PhD at the Institute for Materials Research, University of Leeds, UK. He earned his BTech in Ceramics from the College of Ceramic Technology, University of Calcutta and MTech in Materials Science from IIT Kanpur. He received the prestigious ORS award and a Tetley & Lupton Scholarship for 20052008.

of the finished seal and/or to lower the thermal contraction coefficient of the composite. The MgOAl2O3SiO2 system is a very popular one for glass-ceramics where cordierite is the dominant phase along with clinoenstatite (MgO-SiO2). These materials are characterized by higher temperature stability under load than lithium aluminosilicates together with good thermal and mechanical shock resistance. Their low permittivity and high resistivity lead to a broad range of applications, e.g. microwave component materials, radomes, etc. A very recent application for cordierite is in making thick films.

Abstract

Interceram 56 (2007) [2]

As an engineering material, cordierite has many applications in different fields exploiting its unique electrical, mechanical and thermal properties. The synthetic aspect of cordierite is of constant interest to researchers. Elucidation of its structure and establishing the properties of its structure has always been considered a fascinating subject by researchers. In the present paper these different aspects of cordierite are briefly reviewed. Keywords: Cordierite, processing, properties, applications

5.1 Applications in kilns and furnaces


Cordierite is extensively used as a material for kiln furniture in whiteware industries due to its excellent thermal shock resistance. Mohr [44] worked on the development of cordierite kiln furniture, focusing on parameters such as the effect of grog addition (low expansion grog, like fused silica, can be used in special cases; generally, grogs with thermal expansion larger than cordierite are preferred), the effects of time and temperature, and the development of slag resistance (good grades of kyanite and kaolin, calcined to 15801600 C provide excellent grogs for commercial cordierites).

ial pressing.Yu et al. [46] studied the influence of different silica fume contents on the structure and properties of mullite-cordierite composites. The cordierite content increases while mullite decreases with increasing silica fume contents. The optimum formulation is as follows: cordierite - 66.3 %, mullite - 33.7 % and bulk density - 2.69 g/cm3. Hipedinger et al. [47] developed a cold-setting refractory material using the magnesia-phosphate reaction.A cement paste based on alumina, silica fume, magnesia and orthophosphoric acid was designed to form cordierite-mullite during heating. This cement paste set at room temperature and MgHPO43H2O (newberyite) phase was observed.

5.3 Other composites of cordierite


Taruta et al. [48] fabricated a machinable cordierite-mica composite by low temperature sintering. 40 mass-% mica-composition glass powder was mixed with conventional magnesia, alumina and silica powders (raw materials of cordierite) and then compacted and fired in a sealed Pt container. Mica crystallized at about 730 C, cordierite was suddenly formed at 10501100 C, and densification was achieved at 10001100 C. The formation and sintering of cordierite were promoted by a small amount of fluorine gas or fluorides (AlF3) which evaporated from the glass at >800 C, and HF gas was formed by reaction of the fluorine with the water evaporated from the glass. Machinability was achieved by the interlocking microstructure of mica developed in the composite. Shi et al. [49] prepared cordierite-ceria composite ceramics with oxygen storage capacity. Oxygen storage capacity (OSC) is an important parameter in three-way catalysts (TWC) for the purification of exhausts from automotive gasoline engines. The authors prepared the composite using the sol-gel method so as to append the OSC to the support to which the catalyst is applied. CeO2 particles are uniformly and separately distributed in the cordierite matrix, their number and granularity being dependent on the amount of Ce4+ addition. The cordierite and 10 mass-% CeO2 possess an apparent OSC, ap-

5 Applications of cordierite ceramics


Cordierite is widely used in various fields of ceramics. Its traditional applications are as follows: Refractory products saggars, kiln furniture (widely popular in whiteware industries), gas burners, etc. Electro-ceramics resistors, fusibles, flame guards, etc. Tablewares Flameproof application developments in fast-firing techniques which allow wide temperature variations during the cooling cycle have renewed interest in this type of body. Cordierite is common as a refractory filler. Refractory fillers are frequently blended with powdered solder glass to increase the strength

5.2 Cordierite-mullite composites


A major field of application for cordierite lies in the production of composites and fibre strengthening. Different attempts have been made to develop cordierite-mullite composites with good thermal shock resistance as well as high mechanical strength.Camerucci et al.[45] prepared cordierite and cordierite-mullite ceramics by the slip casting method. The rheological behaviour of the slip became Newtonian when the solid content was reduced to 60 mass-% and a plasticizer was added. This led to higher green densities (~63 %) of the body. Different firing cycles were tested to improve the sintered density, which ultimately reached values between 96.5 and 97.5 % of the theoretical density. In all cases,both the green and the sintered densities were significantly higher than those obtained by ax-

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propriate porosity, flexural strength and thermal expansion coefficient. It will be helpful to enhance the OSC of the catalytic converters and so improve the purification effects for the exhausts. Ma et al. [50] fabricated AlN-cordierite composites using different AlN contents and investigated the effect of AlN content on the mechanical, thermal and dielectric properties of these materials. It was observed that there exists an optimum AlN content for the mechanical and thermal properties while the dielectric property decreases with an increase in AlN content. Kaya et al. [51] fabricated stainless steel (316L) fibre-reinforced cordierite-matrix composites of tubular shape using electrophoretic deposition and pressureless sintering. The sintered composites, which had an internal and external deposit thickness of ~1 mm, were free of surface cracks when a deposition time of 2.5 min was used.Metal-fibre-reinforced cordierite composites such as those developed here may constitute a promising alternative for manufacturing damage-tolerant tubular components for applications at temperatures up to ~900 C.Shyu and Wang [52] studied the relationship of the amount and viscosity of glass with the sintered densities of cordierite-borosilicate glass composites. The dielectric constant of these composites was in the range of 4.95.7 at 1 MHz. Sonje et al. [53] incorporated cordierite as a low coefficient of thermal expansion (CTE) ceramic particulate filler into different epoxy resins to produce an isotropic low CTE polymeric composite material for electronic circuit board applications. The dependence of the CTE values on the properties of the epoxy resins, the nature of interfacial bonding and the dispersion of the fillers in the resin matrix were also studied. positions. Ferraris et al. [55] synthesized cordierite-mullite coating to be applied on SiCf/SiC composites. The composites were coated by a simple and low cost slurry technique and heat treated at 1180 C for 1 h in order to obtain a uniform, pore-free and crystalline coating through the glass-ceramic method. The melting point of the crystalline phases formed in the coating during the coating process (cordierite, 2MgO-2Al2O3-5SiO2 and mullite, 3Al2O3-2SiO2 rate of 3 : 1 mass-%) was measured at about 1430 C. Perham et al. [56] also worked in a somewhat similar direction as they developed a method for the joining of SiC substrates using a cordierite glass-ceramic which, being amorphous, melts the SiC substrates to form a strong bond when rapidly fired. Doping with a fluoride ion flux can lower the peak processing temperature without significantly altering the crystallizing path.High strength can be achieved through this process (F >500 MPa). crystallization of the thick film was determined to be ~83 kcal/mol (~350 kJ/mol). In the case of the 3 mass-% PbO sample fired in a nitrogen atmosphere at 950 C for 30 min, the remaining glass was estimated using the parallel mixing rule, to have a dielectric constant of 15.3 at 1 MHz. The estimated coefficient of thermal expansion of the remaining glass for the 3 mass-% PbO sample was 19 106 / K.

5.6 Cordierite filters


Cordierite has been successfully tried in a number of industrial day-to-day applica-tions. Negro et al. [59] studied the mechanical behaviour of cordierite ceramic filters for automotive emission control in a fired condition after thermal shock and thermal ageing. Park et al. [60] investigated the feasibility of porous cordierite in foam type structures such as filters for dust collection.Various shaped porous cordierites with different pore sizes and with constant porosity of 80 % were prepared by the conventional mechanical foaming method combined with gel casting using water-soluble polymers. Gas permeability of the membrane layers of 150 m was above 200 1013 m2. In the dust collection test, the removal efficiency for particulates finer than 10 m was above 99.99 %. Montanaro [61] studied the interactions of sodium sulphite, iron oxide and cerium oxide from fuel additives with a cordierite monolith filter in the operating temperature range of a diesel soot filter. He concluded that the said oxides do not react significantly with the filter, but sodium sulphite leads to a diffuse etching starting from low operating temperatures. However, the total porosity and pore size distribution were not affected by these interactions. Park et al. [62] developed a new trap to reduce the particulate matter emission from diesel engines and to control the combustion rate of the particulate matter filtered in the trap. Cordierite is a major component of the trap as it is susceptible to thermal shock.

5.5 Cordierite thick films


A more recent but highly promising application of cordierite is the synthesis of cordierite thick films. Mei et al. [57] prepared thick films of cordierite-based glass ceramics by aqueous tape casting from suspensions containing cordierite/glass mass-% of 70/30 to 30/70. The suspensions with 5060 mass-% glass showed the lowest viscosity values, while the green tape containing 30 mass-% glass showed a homogeneous microstructure at both the top and bottom surfaces. The green densities increased with the glass content. The sintered tapes (1150 C, 2 h) containing 5060 mass-% glass showed the lowest values for the dielectric constant (similar to 5.2) and dielectric loss (similar to 0.002) at 1 MHz. Cho et al. [58] developed a cordierite based thick film on an oxidized copper layer where the authors found evidence of copper diffusion as it was incorporated into the cordierite and the remaining Cu was precipitated, which ultimately lowered the densification and crystallization temperature. The authors also studied the microstructure, crystallization kinetics and properties of nonstoichiometric cordierite (2.4 MgO, 2Al2O3, 5SiO2, containing 3 mass-% P2O5 and 3 mass-% PbO) based thick film dielectrics. A stable glass ceramic thick film microstructure that was formed in a 96 % alumina substrate was observed after firing at a temperature of 915 C for 30 min in nitrogen atmosphere. The activation energy for

5.4 Cordierite coatings


Weaver et al. [54] studied the role of bulk nucleation in the formation of crystalline cordierite coatings produced by air plasma spraying. Cordierite glasses doped with 6.3, 8.3 and 10.1 mass-% TiO2 were plasma sprayed onto SiO2based refractory concrete substrates. Only the cordierite powders containing 8.3 and 10.1 mass-% TiO2 produced crystalline coatings. For compositions with less than 8 mass-% TiO2 the crystallization is believed to be controlled by surface nucleation at imperfections. Bulk nucleation-controlled crystallization was observed at compositions above 8 mass-% TiO2 and the presence of Al2TiO5 was detected in these com-

5.7 Cordierite substrates


Reznik et al. [63] utilized cordierite as substrate material and produced pyrolytic carbon deposits by the CVD technique on a planar cordierite substrate using methane as a source gas. The surface morphology was characterized by a cell structure induced by grains elongated perpendicular to the substrate surface. The material located at the interface was more amorphous compared to the graphite-like materials

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located within the cells. Chen et al. [64] studied the potential of burying inductors in multilayer ceramic substrates by inserting a ferrite layer into a low-temperature cofired cordierite substrate. Bi2O3 was doped to lower the sintering temperature and increase the permeability of Ni-Zn-Cu ferrite. Sohn et al. [65] investigated the suitability of glass-ceramics containing cordierite as a crystal phase for application to magnetic disk substrates to achieve higher storage capacity. Parent glasses were prepared with a CeO2 addition as flux, and -cordierite was precipitated after heat treatment. The optimum properties for the magnetic memory disk substrates are as follows: Bending strength - 192 MPa, Vickers hardness - 642.1 kg/mm., CTE 39 107 / K, and surface roughness - 2.7 nm. supported on cordierite monoliths in the total oxidation of chlorinated hydrocarbons. In the case of monolith supported LaCoO3 perovskite, an irreversible catalyst deactivation was observed. Orlandi et al. [71] investigated the biocompatibility of two cordierite ceramics (DF and Cord 1014) with similar chemical composition and different porosity, as a potential support for cell growth in a continuous-flow, solid-bed reactor. They concluded that Cord 1014 could be a promising support for growing CHO (Chinese hamster ovary) cells in great numbers and producing recombinant hepatitis B surface antigens. temperature is raised from 850 to 900 C. The increase in the resistance of the LTCC resistors is attributed to the interruption of the conduction path by platelike anorthite crystals that are produced in the resistor-substrate interface during co-firing.

5.11 Electrochemical applications


Domenech-Carbo et al. [75] studied the electrochemistry of -, -, and -cobalt containing cordierites (Co2Al4Si5O18) attached to paraffinimpregnated graphite electrodes by linear scan and cyclic voltametries in HCl + NaCl and NaOH electrolytes. Cordierite-modified electrodes display a significant site-dependent catalytic effect on the electrochemical oxidation of mannitol in 0.1 (M) NaOH.

5.9 Optical applications


Park and Shin [72] prepared glass-ceramics containing cordierite and a small amount of rutile as the major crystalline phases for application as IR reflectors. Nucleation occurred at 750 C for 3 h and crystal growth at 1100 C for 5 h. This material showed over 90 % reflectance in the spectral range of 570 to 2500 nm.

5.8 Cordierite supports


Recent advances have been made in research on cordierite monolithic catalyst supports, particularly on honeycombs and ceramic foams. Carty and Lednor [66] reported that honeycombs are used as catalyst supports for the removal of gaseous or particulate emissions from combustion engines and for reducing nitrogen oxide emissions from power plants. They also noted that ceramic foams are attracting attention as catalyst supports due to their high thermal stability, high porosity and increased tortuosity with respect to honeycombs.Yamuna et al. [67] prepared honeycomb and pellet type carriers from kaolin-based cordierite composition, and their efficiency in pollution monitoring was studied in two-stroke vehicles. The conventionally prepared kaolin based cordierite system removed 78 % of the CO and 82 % of the hydrocarbons from the exhaust gases under idling conditions. Cordierite honeycombs are used as catalyst supports and must be coated with porous alumina to increase their specific surface area. Hua et al. [68] tried to prepare porous alumina with a large surface area on the internal surface of cordierite honeycombs through in-situ and dip-coating methods of loading -Al2O3 prior to its hydrolysis during the preparation of alumina sol. Seijger et al. [69] studied the in situ synthesis of binderless ferrierite coatings on 300 si cordierite honeycomb supports. The silica-to-alumina ratio of the synthesis mixture and the development of the ferrierite coating as a function of time were also investigated. Schneider et al. [70] studied the catalytic behaviour of perovskite (LaMnO3, LaCoO3, etc.)

5.12 Electromagnetic applications


Wang et al. [76] synthesized cordierite by solgel processing with the aim of using it as MLCI material. It has a low dielectric coefficient (3.5) at high frequency (1.8 GHz). The sintering temperature decreased with increasing Bi2O3 and B2O3 additions. Luo et al. [77] also synthesized a sol-gel derived cordierite ceramic that had a low dielectric constant and a low dissipation factor and could be co-fired with highly conductive metals such as Au,Ag, Pd, and Cu paste below 1000 C, suggesting that it would be a promising material for high frequency MLCIs.Wang et al. [78] developed cordierite-based ceramics by sintering at 950 C a glass selected from the MgOAl2O3SiO2 system with a small amount of B2O3 and P2O5 with the aim of using the material in high frequency chip inductors. Crystalline phases in this sintered sample are mostly -cordierite (hexagonal high cordierite) with trace amounts of -cordierite. It achieved 99 % of theoretical density, a dielectric constant of 5.5, a dielectric loss of 0.001 and a thermal expansion coefficient of 26.7 107/K. It has a uniformly dense microstructure with granular crystals.Yue et al. [79] prepared a series of novel composites of NiCuZn ferrite and cordierite crystallites by sintering the mixtures of nanosized NiCuZn ferrite particles and MgO-Al2O3SiO2 glass powder to be used for MLCIs. These composite materials have tuneable electromagnetic properties with high resonance frequencies. In another work, Yue et al. [80] fabricated ferrite-glass-cordierite nanocomposites by mixing and sintering NiCuZn ferrite nanopowder and MgO-Al2O3-SiO2 gel powder prepared by

5.10 Electrical and electronic applications


Cordierite electric ceramics have an important role in modern technology. They have been used in electrothermics for the production of electric heater supports. Nowadays, due to its electrical, electromechanical and thermal properties, this ceramic finds its applications in electronics for the production of microelectronic components and in the machine-building industry for the manufacture of internal combustion components.Acimovic et al. [73] prepared cordierite ceramics based on sepiolite and examined their applications in foundries, defining the technological parameters for the production of refractory coatings for sand moulds and cores, and of refractory linings for use in the lost loam process. Ting et al. [74] studied the interactions between ruthenia-based resistors and cordierite-glass substrates in low-temperature co-fired ceramics which are composed of a RuO2-based resistor and a cordierite-glass substrate that are sintered at temperatures of 850 C and 900 C. X-ray diffractometry revealed that the lead ruthenate pyrochlore (Pb2Ru2O6.5) in peak-fired thick-film resistors (TFR) disappears and the co-fired samples contain only RuO2 in the resistor film when sintered at 900 C. The overall resistance of the LTCC resistors is increased by a factor of ~3 when the

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the sol-gel process. The composites have tuneable electric and magnetic properties with resonant frequencies higher than 2 GHz. In addition to the traditional application of cordierite in kiln furniture, its use as composite material has been discussed. Among these, ceria-cordierite composites show an oxygen storage capacity (OSC), which is helpful for enhancing the efficiency of catalytic converters in automobile engines. The application of crystalline cordierite as a coating and joining material between two SiC substrates has a promising future. Cordierite material proved effective in the filtration of the automotive emissions, especially in a foam structure. The potential use of ceramic substrates in capacitor and magnetic disks for higher memory storage capacity has been discussed. Honeycomb and pellet type carriers from kaolin-based cordierite composition and their efficiency in pollution monitoring have been described for two-stroke vehicles. The conventionally prepared kaolin based cordierite system removes 78 % of CO and 82 % of hydrocarbons under idling conditions. The catalytic behaviour of perovskite (LaMnO3,LaCoO3,etc.) supported on cordierite monoliths in the total oxidation of chlorinated hydrocarbons has also been discussed in this paper. It was shown that the biocompatibility of two cordierite ceramics could be a promising support for growing CHO (Chinese hamster ovary) cells in great numbers and producing recombinant hepatitis B surface antigens. Cordierite ceramics can also be used in optical applications such as IR reflectors with glass-ceramics containing cordierite and a small amount of rutile as the main crystalline phases. Nowadays, this ceramic finds its applications in electronics for the production of microelectronic components and in the machine-building industry for the manufacture of internal combustion components.The use of cordierite materials in electrochemical applications and in electromagnetic applications in MLCIs and high frequency chip inductors has gained increased importance in recent years. salts. Some novel synthesis techniques have also been reported in this field. Different additives were observed to exert profound influences on the synthesis techniques and the property (particularly, mechanical and electrical) development of cordierite ceramics.Apart from various traditional applications, several new applications of cordierite either in the single state or in the form of composites, exploiting its different advantageous properties, have been reported. More research is required to improve upon its properties and to explore its newer applications.
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6 Summary and conclusion


Cordierite can be synthesized both by conventional techniques using solid state reaction, employing relatively cheap raw materials, and by using solution techniques using synthetic materials such as different organic and inorganic

Received: 16.03.2005

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