Use of electrophoretic deposition in the processing of fibre reinforced ceramic and glass matrix composites: a review

Electrophoretic deposition (EPD) is a simple and cost-effective method for fabricating high-quality ‘green’ composite bodies which, after a suitable high-temperature treatment, can be densified to a composite with improved properties. In this contribution, we describe the use of EPD technique in the fabrication of fibre reinforced composites, with an emphasis on composites with glass and ceramic matrices containing metallic or ceramic fibre fabric reinforcement. EPD has been used to infiltrate preforms with tight fibre weave architectures using different nanosized ceramic particles, including silica and boehmite sols, as well as dual-component sols of mullite composition. The principles of the EPD technique are briefly explained and the different factors affecting the EPD behaviour of ceramic sols and their optimisation to obtain high infiltration of the fibre preforms are considered. In particular, the EPD fabrication of a model alumina matrix composite reinforced by Ni-coated carbon fibres is presented. The pH of the solution and the applied voltage and deposition time are shown to have a strong influence on the quality of the infiltration. Good particle packing and a high solids-loading were achieved in most cases, producing a firm ceramic deposit which adhered to the fibres. Overall, the analysis of the published data and our own results demonstrate that EPD, being simple and inexpensive, provides an attractive alternative for ceramic infiltration and coating of fibre fabrics, even if they exhibit tight fibre weave architectures. The high-quality infiltrated fibre mats are suitable prepregs for the fabrication of advanced glass and ceramic matrix composites for use in heat-resistant, structural components.     

Transparent Polycrystalline Alumina Ceramic with Sub‐Micrometre Microstructure by Means of Electrophoretic Deposition

The optical quality attainable in coarse‐grained polycrystalline alumina is severely limited by grain‐boundary scattering, which is inherent to non‐cubic materials. The optical properties of sub‐micrometre polycrystalline alumina are of growing interest triggered by the fact that a decrease in the grain sizes of the final sintered material yields an improvement in the optical quality while the scattering mechanism changes as the grain size becomes comparable with the wavelength of light. To achieve transparent alumina ceramics with a fine‐grained microstructure, however, porosity and other defects must be avoided. This necessitates the optimization of processing and sintering procedures. Electrophoretic deposition (EPD) is a colloidal process in which ceramic bodies are directly shaped from a stable suspension by application of an electric field. Electrophoretic deposition enables the formation of homogeneous, uniform green microstructures with high density, which can be sintered to transparency. It is a simple and precise technique to synthesize not only monoliths, but also composites with complex geometries [1]. Alumina green bodies were deposited from stabilized aqueous suspensions with and without doping. Green alumina compacts were evaluated based on their pore size distribution and density. Densification behaviour was characterized by dilatometric studies conducted at constant heating rate. Samples were sintered at different temperatures with subsequent post‐densification by hot isostatic pressing. Transparency was evaluated by means of spectroscopic measurements. The measured in‐line transmission of the samples at 645 nm was more than 50 % and that is 58 % of the value of sapphire. The influence of dopings on transparency was investigated. The mechanical properties of the samples were tested.     

Electrophoretic deposition from aqueous suspensions for near-shape manufacturing of advanced ceramics and glasses—applications

Due to high deposition rates and the avoidance of inflammable, often hazardous organic solvents EPD from aqueous suspensions is a fast and low-cost shaping technique for ceramics and glasses. Since the deposition rate is independent of particle size EPD has an outstanding ability for the shaping of nano-particles. In this paper the shaping of complex silica glass and zirconia components, like tubes or structured parts by means of the membrane method is shown. Three-dimensional shaped porous polymer moulds were used as ion-permeable deposition surface. To enable near-shape manufacturing, mixtures of nanosized and microsized particles were electrophoretically deposited. No size-dependent separation was observed. Due to the very high green density of these green bodies (up to 84% of the theoretical value) shrinkage could be reduced to 4.7%. Not only oxide ceramics but also silicon carbide was deposited from aqueous suspensions. Apart from bulk SiC, protective coatings with a thickness of app. 60 m were applied on top of CFC substrates by EPD. Good adhesion was observed and no cracking occurred. Furthermore, electrophoretic impregnation was used for the modification of porous green bodies. Thus silica glasses with graded density and pore size as well as functionally graded composites were prepared.     

An optical investigation of transient layers in magnetic garnet films grown by liquid phase epitaxy

The growth of garnet films using Liquid Phase Epitaxy has led not only to materials with improved performance for bubble domain memories but to materials which exhibit improved microwave properties as well. We have investigated the optical properties of such films and found that there exist transient layers at the substrate/film interface and at the film/air interface. Our results and conclusions regarding the substrate/film interface do not agree with those of Davies et al⁽¹⁾. The discovery of a post growth lead rich layer has not been previously reported to our knowledge and has important implications for both bubble domain and optical applications of garnet films.     

Macroscopic strain in facetted regions of garnet crystals

Morphological studies of Czochralski-grown gadolinium gallium garnet single crystals have revealed facetting characteristics identical to those observed in yttrium aluminium garnet. Accurate lattice parameter measurements made at various points within single crystals of these materials have been used to determine the strains associated with such facets. A possible explanation for the origin of the strain is proposed and the effect of facet imperfections upon the use of garnets in optical and magnetic thin film devices is discussed.     

Novel Techniques for Manufacturing Woven Fiber Reinforced Ceramic Matrix Composites. I. Perform Fabrication

Further research and development of the processing science and technology for ceramic matrix composites (CMCs) is essential for the full industrial exploitation of these materials. This paper describes and discusses a novel, cost-effective processing technique for manufacturing CMCs containing 2-dimensional woven fiber reinforcements. The technique relies on the colloidal processing of ceramic sol precursors and the use of electrophoretic deposition (EPD) to impregnate these sols into woven fiber preforms. The fabrication routes for a woven SiC fiber reinforced mullite matrix and a woven alumina fiber reinforced alumina matrix composite have been investigated. The parameters necessary for the formation of dense green body compacts using EPD are described for the two composite systems. Micro structural examination of these compacts highlights the importance of the infiltration and drying stages to the fabrication of crack-free composite bodies. The laboratory-scale results achieved to date indicate that the processing approach investigated offers great potential for the manufacture of high-quality CMC products for high temperature structural applications.     

电泳沉积技术制备铁电陶瓷薄膜的研究进展

综述了电泳沉积技术在制备铁电陶瓷薄膜方面的最新研究进展,讨论了陶瓷特性、电压、分散剂、热处理时间等因素对电泳沉积铁电薄膜性能的影响.最后展望了电泳沉积技术制备铁电陶瓷薄膜的进一步发展.     

Electrophoretic deposition applied to ceramic dental crowns and bridges

Electrophoretic deposition (EPD) was used as shaping technique for ceramic dental crowns and dental three-unit and four-unit bridges in the high loaded molar region. Because of esthetical aspects and their biocompatibility ceramics are the material of choice for dental applications. Allergic reactions or toxic tissue damages can be prevented largely by application of ceramic dental products. Zirconia in its tetragonal yttria stabilized polycrystal form (TZP) and alumina toughened zirconia (ATZ) offer highest strength combined with highest toughness. In this publication, the influence of the kind and the amount of dispersing agent on the rheological properties of the ceramic suspensions was investigated. For EPD plaster stumps which had been prepared for the dental crowns and bridges by the dental technician were coated with silver and were directly used as deposition electrodes. For optimisation of the removing step of the deposited crown or bridge cap from the plaster stumps organic temporary binders and organic intermediate layers were investigated. The dental parts were sintered either to full density or to porous ceramics for a subsequent glass infiltration step.     

3D Printing of Ceramics with Controllable Green-Body Configuration Assisted by the Polyvinyl Alcohol-Based Physical Gels

Additive manufacturing of ceramics has received intense attention. In particular, 3D-printed ceramics with customized shapes are highly desirable in the chemical industry, aerospace, and biomedical engineering. Nevertheless, developing a simple and cost-effective process that shapes dense ceramics to complex geometries remains challenging because of the high hardness and low ductility of ceramic materials. Extrusion-based printing, such as direct ink writing (DIW), often requires supporting materials that pose additional difficulties during printing. Herein, a simple approach is developed to produce stretchable ceramic green bodies of zirconia and alumina for DIW. The ink is composed of polyvinyl alcohol (PVA) and an aqueous suspension of ceramic powders. Besides the colloidal network formed by the ceramic particles, PVA plays an important role in tuning the printability of the aqueous ink. Through a freeze-thaw process, PVA crystallizes to form physical networks. This strategy provides highly stretchable hydrogel green bodies that can be reprogrammed to complex geometries difficult for common DIW printing. The subsequent drying, debinding, and sintering processes produce ceramics with dense structures and fine mechanical properties. In short, this work demonstrates an efficient method for the DIW of ceramic parts that can be reprogrammed to complex geometries.     

Letter theoretical model of optical properties of ceramic materials application to aluminium oxide

Abstract

This study, concerning the optical properties of ceramic materials, consisted of the development of a theoretical model based on the Maheu theory. The use of this model for the case of aluminium oxide required the determination of various parameters which are discussed. The theoretical results are compared with experimental data obtained by laser spectrophotometry. This work focuses on the fact that the model can be applied to other ceramic materials similar to aluminium oxide.     

Electrophoretic deposition of lead zirconate titanate (PZT) powder from ethanol suspension prepared with phosphate ester

The formation of thick PZT films via electrophoretic deposition (EPD) was studied. The colloidal suspension of a nano-sized PZT powder dispersed in ethanol was prepared using a phosphate ester (PE) as a dispersant. The amount of PE addition on the stability of the PZT suspension has been investigated by measuring the pH and conductivity of the suspension, deposition weight and the relative density of the PZT green compacts. The effect of the applied voltage on the relative green density was also determined as a function of the wt% PE. The composition and microstructure of the sintered PZT ceramics were characterized by XRD and SEM. The electrical properties of the PZT ceramics were also investigated.     

Preparation of weakly agglomerated yttrium aluminum garnet powders by burning a mixture of yttrium aluminum hydroxynitrates, urea, and acetic acid

We have optimized the composition of a mixture of aluminum yttrium hydroxynitrates, urea, and acetic acid for the self-propagating high-temperature synthesis of yttrium aluminum garnet (YAG) powder. The powder prepared in this way offers a low degree of agglomeration, and the ceramic produced from it has a low carbon content. A technique has been proposed for carbon determination in YAG ceramics through gas chromatographic analysis of the gaseous products of carbide hydrolysis after the dissolution of the ceramic in pyrophosphoric acid.     

Silica moulds built by stereolithography

In this work the production of ceramic moulds for aluminium casting using a stereolithographic apparatus is presented. Suspensions of silica powders in a photoreactive resin were used in standard STL equipment in order to build green parts. UV curable pre-ceramic suspensions have been studied using photocalorimetric and rheological characterizations. Thermogravimetry was used to analyse the behaviour of the pre-ceramic green during thermal treatment. Stereolithgraphy apparatus (SLA) was modified in order to fabricate ceramic green. Silica objects were obtained by pyrolysis of the organic binder and subsequent sintering at high temperature. A characterization of mechanical properties of the green and sintered ceramic materials was performed. Finally moulds for investment casting of aluminium were built by stereolithography and used for casting as a green as well as after sintering.     

电泳沉积制备氮化铝陶瓷的研究

采用电泳沉积法成功制备相对密度达到61.9%的均匀氮化铝素坯, 经无压烧结后可获得热导率为200W/(m·K)的氮化铝陶瓷. 研究表明, 以无水乙醇为溶剂、加入0.1wt%聚丙烯酸（PAA）做分散剂、pH值控制在9.7左右的悬浮液具有最佳分散性. 电泳沉积（EPD）成型比干压成型制备的预烧体孔容减小, 比湿法成型制得的预烧体大孔显著减少. 用扫描电子显微镜（SEM）对三种不同成型方法制得氮化铝陶瓷的显微结构进行了研究, 结果表明, EPD法所得氮化铝陶瓷的显微结构均匀, 晶粒尺寸5μm左右.     

Ce dopant segregation in Y3Al5O12 optical ceramics

Ce³⁺-doped YAG garnet optical ceramic have been sintered at the Shanghai Institute of Ceramics in China to characterize dopant distribution in optical ceramics by combining optical spectroscopy and two spatially resolved techniques as imaging confocal microscopy and transmission electron microscopy. A strong Ce³⁺ segregation and spatial variations of content between grains and grain boundaries has been confirmed by quantitative data obtained by TEM microscopy. This observation is another evidence of the inhomogeneous Ce³⁺ distribution across grain and grain boundaries in optical ceramics comparable to that of Nd³⁺ ions in YAG ceramics. These results correlate well with low segregation coefficients of Nd³⁺ and Ce³⁺ observed in the garnet crystals grown from the melt and/or flux.     

拟薄水铝石凝胶制备牙科托槽用ZTA陶瓷的研究

利用拟薄水铝石的凝胶作用,以浓HNO_3为引发剂,将Al_2O_3(1μm)粉末和含3%Y_2O_3的ZrO_2(200nm)粉末均匀填充在拟薄水铝石的溶胶双电层内,在一定温度和时间下胶凝固化并干燥成坯。将生坯通过不同的温度烧结后,制备出ZTA陶瓷正畸托槽材料。主要研究拟薄水铝石的胶体行为、不同固含量下生坯的性能以及ZrO_2对陶瓷晶粒结构和力学性能的影响。结果表明,经拟薄水铝石凝胶制备的陶瓷生坯具有一定抗弯强度(达4 MPa),可用于力学加工。在该制备方法中,ZrO_2可更好地发挥增韧作用,增加陶瓷烧结后致密度,提高陶瓷托槽材料的抗弯强度。     

Glass-ceramic interactions and thick-film metallization of aluminium nitride

A frit-bonded thick-film metallization for aluminium nitride (AIN) ceramic substrates has been developed. The glass system is thermodynamically stable with respect to AIN at the temperatures employed during thick-film processing. The model glass, a lithium borate, has comparable physical properties to that of the standard lead borosilicate glasses used in fritbonded films designed for oxide ceramics. The wetting properties of the glass on AIN, in both air and nitrogen atmospheres, have been determined by use of a hot-stage microscope. The low-temperature oxidation of the AIN surface was found to be a significant factor in the glass spreading rate. The glass was formulated into a palladium-silver thick-film metallization and the performance of this material on three types of AIN substrate was determined. Examination of the film morphology and the fracture surfaces was carried out using scanning electron microscopy.     

Purity and morphology of aluminium films

A continuous wire feed source of aluminium of 99.999% purity in conjunction with a composite ceramic boat has been used to deposit aluminium films of high purity in vacuum. The impurity content was analysed by proton-induced X-ray analysis with a Van de Graaff accelerator, supplemented by X-ray fluorescence, optical emission and Auger electron spectroscopy. The low impurity content achieved ( 50 atomic ppm) is attributed to the small quantity of molten aluminium maintained in the boat at one time.

The morphology of the Al films was studied by reflection electron diffraction, X-ray diffraction and scanning electron microscopy. Thick Al films grew with {111} and {311} texture orientations. The grain size variation with thickness generally followed the known variation with the deposition rate.     

Fabrication of lead-free piezoelectric (Bi<Subscript>0.5</Subscript>Na<Subscript>0.5</Subscript>)TiO<Subscript>3</Subscript>–BaTiO<Subscript>3</Subscript> ceramics using electrophoretic deposition

Electrophoretic deposition (EPD) process has certain advantages such as it can be applied for a mass production and also can be combined with magnetic crystal alignment technique. In this work, we prepared lead-free 85(Bi_0.5Na_0.5)TiO₃–15BaTiO₃ (85BNT–15BT) piezoelectric ceramics by conventional uniaxial pressing and EPD process. Various conditions were optimized such as suspension media, applied electrical field, and deposition time in order to yield dense green ceramics of 85BNT–15BT composition using EPD process. 85BNT–15BT ceramics prepared using EPD process revealed the Curie temperature of about 250 °C, coercive field of about 30 kV/cm, and piezoelectric constant (d ₃₃) of 75 pC/N. The EPD-processed samples exhibited structural and electrical properties similar to that of the conventionally processed one suggesting the successful fabrication of 85BNT–15BT piezoelectric ceramics by EPD method without composition deviation. This study lays a foundation on the fabrication of Bi-based lead-free piezoelectric ceramics by an alternative route other than the conventionally practiced solid-state reaction method maintaining the similar chemical composition, moreover, leaving a large space to explore more in the future.