c00.52es and manufacturing ELSEVIER Composites: Part A 32(2001)997-1006 Use of electrophoretic deposition in the processing of fibre reinforced ceramic and glass matrix composites: a review A R. Boccaccini,, C. Kaya, K.K. Chawla Fachgebiet Werkstottechnik, Technische Universitat ILmenau, PF 100565, D-98684 ILmenau, germany Interdisciplinary Research Centre(IRC) for High Performance Applications School of Metallurgy and Materials, The University of Birmingham, Edgbaston, Birmingham B15 2TT, UK Department of Materials and Mechanical Engineering, University of Alabama at Birmingham, Birmingham, AL 35294 USA Abstract 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 infuence n 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 expensive, 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 compo- sites for use in heat-resistant, structural components. C 2001 Elsevier Science Ltd. All rights reserved Keywords: A Ceramic-matrix composites(CMCs); E. Prepreg: Electrophoretic deposition 1. Introduction ceramic fabrics, including SiC-based (e.g. Nicalor Nippon Carbon Co., Japan), alumina and aluminosilicate The development of fibre reinforced ceramic and glass woven fibre mats [2-5]. Metallic fabrics are commercially atrix composites is a promising means of achieving light- available also [6] and are made from a variety of metals weight, structural materials combining high-temperature including stainless steel and special alloys(e.g. Hastelloy strength with improved fracture toughness, damage toler- X). These fabrics provide interesting reinforcing elements ance and thermal shock resistance [1]. Considerable for the fabrication of ductile phase reinforced brittle matrix research e ffort is being expended in the optimisation of composites, including glass matrix composites ceramic composite systems, with particular emphasi Ceramic and glass composites incorporating 2D or 3D being placed on the establishment of reliable and cost- fibre reinforcements are particularly prone to exhibiting effective fabrication procedures. In this context, while the uncontrolled microstructures and residual porosity. This is initial efforts were in the fabrication of unidirectional because it is extremely difficult to achieve complete infiltra- composites, they are increasingly shifting towards the tion of the matrix material into the fibre tows(where the more isotropic composite materials reinforced by two- intra-tow openings may be down to the order of s100 nm) dimensional (2D)and three-dimensional (3D) fibre architec- Traditional processing routes for 2D or 3D fibre reinforced tures. The majority of the research undertaken so far on the ceramic matrix composites have disadvantages. In particu 2D reinforcement of ceramics has been conducted using lar, simple slurry infiltration is unable to penetrate tight fibre weaves, while chemical vapour infiltration (CVI is an Corresponding author. Present address: Department of Materials, expensive technology due to the numerous re- infiltration Imperial College, London SW7 2BP, UK steps required and the high-cost equipment involved [4] E-mail address: a boccaccini@ic ac uk(.R. Boccaccini) Electrophoretic deposition(EPD)has been developed in 1359-835X/01/S.see front matter O 2001 Elsevier Science Ltd. All rights reserved. PI:S1359-835X(00)00168-8
!""# $% & '% ( ) *()+ , -'' . / 0 % & 0 % 1 2& 1 1 3 4 ' 0 & 0 2 % - 1 1 -5 63!# /- ! "!#$% & &'( ) * ( & ( + ( ( !#$ '( !#$ ( ( ( , ( (& ( - !#$ '( . !#$ ( + ( !#$ ( /& - 0 ( .( '( 1 2 & ( 3 ( ( ( !#$ ( - &'( ( & ( & (( 4556 ! 7 8 4%7& 9 ":%; ! # ; ! - & (( & ( ( ( & 2 $% & ( - ? ( 2 4$ ( ( ( 7& " / / @ % ( ( $ ( ( (( ( - ( ( & " & 655 % - ( 4$ >$ + (& ( ( ( "D+% ( ( ( & '( & '( 4 "4556% FFG9655B 6>AF&H>ACI56IJ & 4556 ! 7 8 #++ 76>AF&H>AC"55%556BH&H II ( # $ : + 8 7KG 4# 2 && 8 L(2 " %
A.R. Boccaccini et al. Composites: Part A 32(2001)997-1006 preforms has been studied theoretically and experimentally Sol particles In the present work, a complete literature review focusing on the particular use of EPd to infiltrate ceramic and metallic fibre preforms with the ultimate goal of fabricating composite materials is presented. Typical EPD experimen- tal procedures and the results achieved are described in detail, taking as example a model alumina matrix composite reinforced by Ni-coated carbon fibres Literature review fbre ureter Table 1 presents an overview of the published work deal- ing with the application of the EPD technique for the fabri Fig. 1 Schematic diagram of the epd cell for obtaining cation of fibre reinforced ceramic and glass matrix conductive fibre mats. The fibre mat the positive ele the composites. Other types of ceramic composite systems. particles in the suspension are negatively charged (e.g. silica such as whisker reinforced composites [16, 17], laminated composites [18-20), composite coatings [21], composites with porous layers [22]and functionally graded materials recent years simple and inexpensive method for [22-24]have been fabricated by the EPD technique More- infiltration of tightly woven fibre over, the use of electrodeposition to coat ceramic fibres with preforms omplete in chnique is based on using nanoscale metals with the aim to fabricate metal matrix composites has ceramic particles in a stable non-agglomerated form(such also been investigated [25, 26]. However, research on these as in a sol or colloidal suspension) and exploiting their net areas will not be reviewed here, this paper being restricted to surface electrostatic charge characteristics while in suspen the use of epd for the fabrication of fibre reinforced sion. On application of an electric field the particles will ceramic and glass matrix composites migrate towards and deposit on an electrode. If the deposi- The feasibility of infiltrating ceramic woven fibre tion electrode is replaced by a conducting fibre preform, the preforms by EPD has been demonstrated for a variety of suspended particles will be attracted into and deposited single and mixed component ceramic sols, as summarised in within it, providing an appropriate means of effectively Table 1. Mainly graphite [22, 27-32, SiC-based infiltrating densely packed fibre bundles. A schematic [4, 7, 22, 33-40], alumina [35, 41-43]and aluminosilicate diagram of the basic Epd cell is shown in Fig. 1 (mullite)37, 44, 45] woven fibre mats have been employed The movement of ceramic sol particles in an aqueous es investigated have been silica, alumina, suspension within an electric field is governed by the field mullite, SiC, Si3 N4 and borosilicate glass. Both aqueous strength, and the pH, ionic strength and viscosity of the and non-aqueous suspensions have been used, although solution [4]. The electrophoretic mobility(EM) of the aqueous colloidal suspensions or sols are preferred due to harged particles in suspension is given by [8] environmental and cost advantages [46]. The experiments U have been invariably carried out in laboratory scale, using EM= E (1) EPD cells of small dimensions, i.e. the gap between the electrodes was between 1 and 5 cm in most studies. and where U is the velocity, E the field strength, e the dielectric the area of the fibre preforms infiltrated was smaller than constant,s the zeta potential and n the viscosity. Accord- 100 cm". When EPD is used as a ceramic forming techni ingly, a suitable suspension for EPD should have high- que, it is possible to use either constant current or constant particle surface charge, high dielectric constant of the liquid voltage conditions. An analysis of the literature showed, phase and low viscosity. Moreover, low conductivity of the however, that all investigations have been conducted by suspending medium to minimise solvent transport is using constant voltage conditions, the reason being most probably that this is the simplest mode of operation The phenomenon of electrophoresis has been known In the case of non-conductive fibres, such as aluminosis since the beginning of the last century [9] and has found ate(mullite)fibres of the type Nextel 720(3M Co., MN extended application in ceramic technology. In available USA)or alumina fibres(e.g. Almax, Mitsui Mining Co comprehensive review articles, complete descriptions of Japan), a modification of the basic EPD cell must the basics of the EPD technique and its applications in conducted. This has been called electrophoretic filtration ceramics have been presented [8, 10-12]. Moreover, the deposition(EFD) and it is a modification of a method deep electrophoretic penetration of porous substrates, used previously by Clasen [47]. Here, both electrodes are which is related to the Epd infiltration of tight fibre made from stainless steel and a filter metallic membrane is
96A= + 2 ( ( ( ( !#$ ( - !#$ & ( ( 2 ( /& - 6 ( 2 & !#$ '( & 3 ( 2 4= 7& >9E5= ( <>AE69E>= ( "(% <>GEEEA= - ( ( 7 7>/E '(( &'(( ( ( ( '(( ( ( : :/ 7% ( " :( : @ % !#$ ( ( - "!M$% ( ( <EG= 0 FFH -9(9 1 9 : )' 8 - 63 *3+ !!;< M 6 7 !#$ ( - ( " 0 F <E=%
A.R. Boccaccini et al./Composites: Part A 32(2001)997-1006 毛了 5号29855 目 了 32 直量 z了 z 喜了 E u∽e 昌喜 着百 点s3 是另豆另三是真自是 |至登登§置置
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
A.R. Boccaccini et aL./Composites: Part A 32(2001)997-1006 之 三 n∞玉9 9 卫装马> 8号=3529 5目三 三 0323
6555 -9(9 1 9 : )' 8 - 63 *3+ !!;6B8 I 7 , 6A "4A O 34 > 4 O % '(( 0 F E 4 5= 4555 & I(>6B8 I /, &( 7( B5 6 <>6= 4555 ( "(% "/ G45%I( &( : ( ; ( 655 G 4=
A.R. Boccaccini et al./Composites: Part A 32(2001)997-1006 diphasic (or mixed) sols(e.g. silica-alumina dual sols of mullite composition), the process becomes more compl cated than with the single species (e.g. single silica or alumina sols). This is because it is necessary to control the mobility and zeta potential of both species in order for both of them to migrate to the same electrode and co-deposit without segregation under EPD conditions. In particular, for the fabrication of mullite matrices, it is necessary to main tain the initial silica-alumina proportion in the deposit material to warrant stoichiometric mullite composition Several authors have shown ways to engineer the surface sPTo84、eeU charge of the particles by the addition of surfactants [44]or to control short range particle-particle interactions and M micrograph of EPD-infiltrated Nicalon'fibre mat using a rheological characteristics of the colloidal suspensions by f mullite Details of the EPD technique used are careful variation of the particle size, solids-loading and pH iginal work [38). A high level of matrix infiltration is seen. It [48, 49]. In the case of diphasic(mixed sols of mullite nown that the deposited material fairly kept the original mulli composition, the pH is chosen so t sitely charged, i.e. the alumina and silica particles are posi tively and negatively charged, respectively. Thus, placed between the deposition electrode and the non heterocoagulated particle clusters are formed, which move onducting fibre preform [35, 41, 42]. On applying a rela- as single, composite particles [38, 43]. An example of a ively high voltage (e.g. 60V for alumina sol [35]), the Nicalon fibre mat infiltrated by a mixed sol of mullite alumina particles migrate and deposit on to the membrane composition using EPD is shown in Fig. 2 [38]. A high from one direction only, through the fibre preform, until a level of matrix infiltration is seen. It was shown in this sufficient matrix thickness which envelopes the preform is work that the deposited material fairly kept the original achieved. The high voltage causes hydrogen evolution at the mullite stoichiometric composition anode but the gas is prevented from becoming part of the One of the most critical processing steps that compact by the presence of the filter membrane. In this way optimised, as emphasised by most authors, is the drying of alumina-alumina [35] and mullite-mullite [45] woven fibre the infiltrated fibre preforms. This is because extensive reinforced ceramic matrix composites could be fabricated. microcracking of the gelled ceramic matrix can occur on An analysis of the published work shows that the quality drying, as usually occurs in sol-gel processing. Cracking of the infiltration also depended strongly on the architecture frequently develops due to the differential shrinkage of the of the fibre preform employed but, in general, EPD was able gel network generating tensile stresses at the surface, which to infiltrate even the very tight woven fibre mats used. The may lead to the catastrophic growth of microscopic flaw parameters of the EPD infiltration []. However, thin films(<1-2 um)can be dried without applied and deposition time, were optimised in the different cracking because the tensile stresses developed when they studies to obtain a high solids-loading in the intra-tow shrink are insufficient to cause the growth of cracks [50] regions and firm, adherent, ceramic deposits. When using Thus, a careful control of the thickness of the matrix mate rials deposited by EPD is required, as highlighted in the literature [4, 35]. Fig. 3 shows the different cracking devel- opment upon drying in two Nicalon fibre mats which have been EPD-infiltrated with mullite composition sol [34]. Th sample with thicker deposit exhibits extensive microcrack- ing, while the optimisation of deposit thickness leads to a minimisation of microcracking The analysis of the literature reveals that when the ePd and drying conditions were optimised, the infiltrated fibre fabrics were of sufficient quality (high infiltration, no macroporosity and minimal microcrack development)to be used as preforms for the fabrication of ceramic or glass 25 mm matrix composites The EPD process has also been successfully applied to infiltrate metallic fibre fabrics. Boehmite. silica and titania Fig. 3. Macrograph showing the development of microcracking in SiC Nicalon fibre mats EPD- infiltrated with mullite composition mixed sol nanoparticles have been used as precursors for the ceramic pon drying. Extensive microcracking is developed in thick deposits(left) matrices [22,,, 52]. In borosilicate and soda-lime glass This is minimised by depositing thin films of 1-2 um thickness(right)[341 matrix composites, EPD infiltration of the metallic fibre
& ( <>AE6E4= 3 & " B5 D ( <>A=% ( ( ( ( 2 - ( ( ( + (9( <>A= (9( HE>= / ( ( !#$ M 4 <>H= + 2 2 ( 3 ( ( - ( 2 ( (( ( 9 2 '( ( 2 2 ( . A= M > 2 & ( / !#$& ( <>E= - 2 2& 2 2 - ( !#$ ( '( " 2 % ( - !#$ (( ( ( 6A6A4= + & !#$ -9(9 1 9 : )' 8 - 63 *3+ !!;H= + 2 ( <>H= M > : 2 7 / !#$& ( ( ! 2 2 "% - 694 2 " % <>E=
1002 A.R. Boccaccini et al. Composites: Part A 32(2001)997-1006 3. A case in point: Ni-coated carb alumina matrix composite 3.1. Description of the EPD experimental procedure The feasibility of fabricating Ni-coated carbon fibre rein- forced alumina matrix composites via a single-infiltration EPD process is considered here, as a typical example of the application of EPD technique in the fabrication of ceramic A commercially available boehmite (Y-AlOOH) sol (Remet corp, USA, Remal A20) having 40 nm average ek U particle size was used as alumina source. The sol contains 20 wt% solids-loading and the boehmite particles are in the lath shape. The as-received boehmite sol was seeded with EM micrograph of a metallic fibre mat which has been fully nanosize(13 nm)8-alumina powder(Aluminium Oxide C ltrated by silica sol using EPD. The working voltage was 4 V and Degussa AG, Germany) containing 0.5 wt% a-alumina deposition time 2 min [52]- (BDH Chemicals, UK). The seeding powder was first dispersed in distilled water, then the dispersion was added to the boehmite sol while this was stirred magnetically preforms was conducted by using silica nanoparticles in Finally, the seeded boehmite sol was ball-mixed for 12 h colloidal suspensions [53, 54]. In these composites, the using high purity TzP balls in a plastic container. EPD porous silica deposit was used to provide adequate Ni-coated carbon fibres(Inco spp, Incofiber, 12K50 matrix/fibre interfacial bonding and to avoid possible UK) were used as reinforcement. These fibres were in the reactions between the silicate glass matrices and the form of continuous tows of Ni-coated single carbon fibres, metallic fibres with 12,000 tows coated to 50% by weight with nickel. The Using EPD, the infiltrated metallic fabrics were suffi- nickel coating provided excellent conductivity which is iently infiltrated with matrix material so as to be used as essential for EPD, as well as ease of fibre handling and preforms for the fabrication of metal fibre reinforced cera- adequate wettability. The tows were unidirectional aligned mic or glass matrix composites. An example of a metallic in a grooved perspex frame. EPD experiments were carried fibre mat, fully infiltrated by silica sol using EPD, is shown out under vacuum. Ni-coated carbon fibres held in the frame in Fig 4[52]. The working voltage was 4 V and deposition were used as the deposition electrode(cathode). Two stain- time 2 min less steel plates on either side of the cathode served as the It must be pointed out that the reinforcement of ceramic positive(anode) electrodes. After the fibre preform was matrices by continuous ductile elements has not been as placed in the sol, the system was vacuum degassed to much investigated as their ceramic-ceramic counterparts, remove any entrapped air, and then the cell electrodes despite the advantages they may offer. These include were connected to a 0-60v dc power supply. EPD was performed subsequently under constant voltage conditions due to the intrinsic ductility of metallic fibres and the possi- (5, 10, 15 and 20 V)using varying deposition times( from 50 bility of exploiting their plastic deformation for composite to 500 s). An electrode separation distance of 15 mm was toughness enhancement [55] used in all the experiments. Under the applied electric field, Overall, it appears that EPD is a very versatile and cost- very fine bo effective technique to infiltrate complex fibre architectures, surface charge, as determined from the EM data, migrated paving the way for the development of ceramic and glass towards the negative electrode, i. e. the Ni-coated carbon matrix composites with 2D and 3D reinforcement. More- fibre tows The particles infiltrated the fibre tows and depos over, due to the high matrix homogeneity and high relative ited until a sufficient matrix thickness, which enveloped the density achieved in the green bodies by EPD, several e tows, was achieved. The fibre preform acting authors showed that the required subsequent densification electrode was connected to a balance linked to a computer [32,35, 40,42,44,51,52, 53], avoiding, therefore, e tering The apparatus is able to record the weight gain per milli- second during the deposition process, i.e. in real time. The intensive traditional hot-pressing route. Specific experimen- dimensions of the cathode (25 X 25 mm") were half the al information about the EPd fabrication of Ni-coated anode's dimensions (50 X 50 mm]) in order to eliminate carbon fibre reinforced alumina matrix composites, a system the ' edge effect which may give an inhomogeneous being developed currently by the authors, is given below. thickness from the centre to the edges of the cathode. The The objective is to describe the processing steps and to show EPD-prepared green body specimens containing about 25 optimisation of the EPD arameters 30 vol% fibre loading were dried under humidity controlled
( ( ( AE= + !#$ ( ( '( I !#$ (& ( & ( ( !#$ M E $ : & ( !#$ ( '( ('( ( ( <>4>AE5E4EEA6A4A>= & & ( 7 & ( !#$ /& ( ( ( - ? !#$ 699 ' 2 =' '& - /& & ( & !#$ !#$ '( "&330% " 7 45% E5 , ( ( ( - 45 O & - & , "6> % &( "(( 3 $( 1 1 % 5A O &( "$0 % - M & 64 ( ( -P# /& "+ + 64A5 % ( - (( /& 64555 A5O 2 - 2 ( !#$ '( - ( !#$ ( ( (( /& ( " % - & " % (( 59B5 D ( !#$ ('( ( "A 65 6A 45 D% ( " A5 A55 % 6A ( ( !: /& - & ( ( 2 - 2 ( - ( & ( - "4A 4A 4 % * "A5 A5 4 % ) * ( 2 - !#$& ( 4A9 >5 O ( ( 6554 -9(9 1 9 : )' 8 - 63 *3+ !!;< M E 7!: ( ( !#$ - 2 E D 4 <A4=
A.R. Boccaccini et al./Composites: Part A 32(2001)997-1006 5 vvvv 050 -10V 20V △仓白 Fig. 5. EPD of boehmite sols on to Ni-coated carbon fibre mats. Graphs of the(a)electrophoretic deposit weight and(b)electrophoretic deposit thickness, as a atmosphere for one day and left in normal air for another lomerates within the suspension. EPD experiments day before being pressureless sintered at 1250C for 2 h were carried out under vacuum in order to eliminate under nitrogen atmosphere. the undesirable formation and entrapment of bubbles To prepare green and sintered fibre reinforced ceramic within the deposit due to the electrolysis(evolution of matrix composite(CMC) samples for cross-sectional scan gases)of the aqueous sol dispersion medium. Under ning electron microscopy (SEM), the specimens were vacuum, very fine boehmite can penetrate placed in a vacuum chamber and vacuum-impregnated deep into the inter/intra-fibre filling all the with Epofix resin. Impregnated green and sintered CMC voids, resulting in the formation samples were left to harden overnight and then cut into green(and sintered) composites slices using a diamond saw. A high resolution scanning The graphs in Fig. 5(a) and(b) show the results of electron microscope ( Field Emission Gun, FEG SEM lectrophoretic deposit weight and thickness, respec Hitachi S4000, Japan) was employed to characterise the tively, as a function of deposition time for different various microstructural features of the infiltrated and applied voltages. EPD experiments were performed for intered composite bodies, including grain shape and size, up to 500 s, as this gave a deposit thickness of about porosity distribution and location, ductile interface, deposit 660 um which was enough to produce a composite with thickness and infiltration of the matrix into the fibre arch an acceptable green density. The deposit thickness tecture in both green and sintered samples increased with increasing deposition time. When aqueous-based sols are used in EPD experiments, one 3. 2. Evaluation of EPD experiments associated problem is the electrolysis of the water. Higher voltages resulted in rapid deposit formation, The boehmite sol used was kinetically stable and well but also in the undesirable formation and entrapment dispersed, as there were no big heteroflocculated of bubbles within the deposit due to the electrolysis
( 64A5 4 ( - 9 ":% & & "7!:% (( ((& ! + : ( ( ( "M ! 1( M!1 7!: 0 7&E555 @ % ( (( ( ( , ( ( 2 & ( 6939 2 2 =' - ( 2 .( ( !#$ ( ( (( ( ( ( "( % '(( ( (( I & ( &'( " % - M A"% "% ( 2 & ( !#$ ( A55 2 ( BB5 ( ( - 2 K '((& ( !#$ 0 ( ( ( ( ( -9(9 1 9 : )' 8 - 63 *3+ !!; M A !#$ /& 1 "% "% 2 (
1004 A.R. Boccaccini et al. Composites: Part A 32(2001)997-1006 the velocity and deposition rate of the charged colloidal boehmite particles also decreased EPD parameters were optimised in order to achieve fully infiltrated Ni-coated carbon fibre reinforced alumina composites with the minimum amount of excess material being present in the outer regions of the preform. The opti mum deposition voltage and time were determined as 15 V and 400 s, respectively, for full infiltration. The full infiltra- tion resulted in an EPD deposit thickness of >650 um. Using these parameters, it was possible to produce fully infiltrated mats with only a thin(100 um) excess layer This was beneficial as the fibre mats then have a reduced propensity to form large cracks during the drying stage. This cracking is due to the differential shrinkage of the gel network which generates tensile stresses at the surface of the deposits, as mentioned above(see Fig 3) microstructures of composites produced under optimised EPD parameters. Fig. 6(a) shows an SEM micrograph of an EPD-formed green body containing 30 vol% fibre load- ing. High green densities(about 61% of theoretical density) were achieved at 15 V for 400 s. Green density was measured by dividing the mass of the sample by its geome- trically determined volume. It can also be seen in Fig. 6(b) that the Ni-coated carbon fibre preform was fully infiltrated with the boehmite sol. Even in regions where the Ni-coated fibres were nearly touching each other, full impregnation was achieved by the nanosize boehmite powders in a very short time, i. e. 400 s, leading to high-quality green bodies. fibre reinforced alumina matrix composite containing 30 vol% fibre load. The effectiveness of the EPD providing full deposition ing. The fibre preform was infiltrated using an applied voltage of 15 V for between two fibres with a separation of 400-500 nm is 400 s Both(a) high and(b) low magnification micrographs show that the Ni-coated carbon fibre preform was fully infiltrated with the boehmite sol clearly visible in Fig. 6(b). It must be noted that these Even regions where the Ni-coated fibres were nearly touching each other green samples were not polished in order to avoid damaging ve been fully impregnated by the nanosize boehmite particles, leading to the ductile Ni interface. Thus, some cutting effects are high-quality green bodies. visible on the carbon fibres and the matrix. which resulted from the contact with the diamond saw during the very of the aqueous sol dispersion medium, while low slow-speed cutting operation voltages reduced the electrolysis, but they al o neede The subsequent composite preparation involved pres higher deposition times. Thus, a compromise had to be sureless sintering of the green bodies at 1250C for 2 h found and voltage and deposition time were optimised. under N2 atmosphere. a fully infiltrated and dense Voltages higher than 20V were not used. The thickness sintered microstructure is shown in Fig. 7. Sintered of selected electrophoretic deposits, measured from the densities of about 91% of theoretical density were fibre surface, is plotted against the deposition time for measured by using the Archimedes technique. This result different voltages in Fig. 5(b). The formation of the confirms that the electrophoretic processing approach is deposit was very rapid in the first 150 s and then very convenient in terms of obtaining dense samples at increased steadily relatively low sintering temperatures and avoiding the In situ (real time) deposit weight measurements cost-intensive hot-pressing procedure, which has been provided very reliable data to determine accurately the the common practice for the fabrication of fibre rein- deposition rate. The rate of deposition was very high at forced ceramic matrix composites so far he beginning (up to 150 s), and then it started to decrease with increasing deposition time. The decrease in deposition rate was attributed to the increase in the 4 Conclusions resistance of the deposit, as the current diminishes due to the increase in deposit thickness and the removal of A literature review on the application of the EPD tech charged boehmite particles from the sol. As a result of nique in the fabrication of fibre reinforced ceramic and glass the decrease in the potential drop across the suspension, matrix composites was carried out. Since the first studies
'(( ( ( ( -( ( D 45 D ( - 2 ( ( M A"% - 6A5 + ( " % ( ( - "( 6A5 % - ( ( ( 2 ( ( !#$ ( /& ( ( ( ( - & ( 6A D E55 ( - ( & ( !#$ 2 BA5 ( ( "655 % - ( 2 ( - 2 ( 2 2 ( " M >% - 7!: ( M B (( ( ( !#$ M B"% 7!: !#$& >5 O & 0 "( B6O % 6A D E55 1 ( & ( + M B"% /& ( ! /& ( ( , E55 &'( - !#$ ( E559A55 M B"% + ( ( / -( ( ( ( & ( - ('( & ( 64A5 4 ( /4 ( (( M G 7 ( F6O ( ( '( - ( ( & & ( & ( !#$ & '( ( 7 ( 655E -9(9 1 9 : )' 8 - 63 *3+ !!;5 O & - ( 6A D E55 "% "% /& ( ! /& ( ( , &'(
A.R. Boccaccini et al./Composites: Part A 32(2001)997-1006 ooQ e dage Fig. 7. SEM micrograph of EPD-infiltrated Ni-coated carbon fibre reinforced alumina matrix composite containing 30 vol% fibre loading after sintering at 1250"C for 2 h in nitrogen atmosphere. The micrograph shows the full deposition of the boehmite matrix into the fibre preform and a dense composite microstructure after sintering. published at the beginning of the 1990s, a variety of fibre/ [21 Liaw PK. Fiber reinforced CMCs: processing, mechanical behaviour matrix composite systems have been fabricated by EPD and modelling JOM 1995: 47(7): 38-44 Carbon, SiC (Nicalon), alumina(Almax )and aluminosis- [3] Davidson DL. Ceramic matrix composites fatigue and fracture JOM 1995:4707):46-52. licate(mullite(Nextel )woven fibre preforms have been (4) liston TI, Ponton CB, Marquis PM. Butler EG. The manufacture of used, mainly with silica, alumina, mullite, borosilicate glass woven fibre ceramic matrix ites using electrophoretic deposi and SiC matrices. Overall, the analysis of the published data tion. In: Duran P, Fernandez JF, editors. Third Euroceramics vol. I demonstrates that EPD, being simple and inexpensive, Madrid, Spain. Faenza Editrice Iberica, 1993. p. 419-24 provides an attractive alternative for ceramic infiltration 5] Ko FK. Preform fibre architecture for ceramic-matrix composites. and coating of fibre fabrics, even if they exhibit tight fibre Am Ceram Soc Bull 1989: 68: 401-14 6] Chawla KK. Fibrous materials. Cambridge: Cambridge University weave architectures. The high-quality infiltrated fibre mats Press. 1998 are adequate prepregs for the fabrication of advanced glass [71 Illston TJ, Doleman PA, Butler EG, Marquis PM, Ponton CB, Gilbert and ceramic matrix composites for use in heat-resistant M et aL. UK Patent no. 91248161. November 1991 structural components. [8] Brown DR, Salt FW. The mechanism of electrophoretic deposition. J The parameters of the EPD infiltration process, i.e. Appl Chem1965:15:40-48 [9] Hampel CA, editor. The Encyclopedia of Electrochemistry New applied voltage and deposition time, can be optimised to York: Reinhold Publishing Corp, 1964. p. 540(Reuss, 1807 obtain a high solids-loading in the intra-tow regions and a Electrophoresis). firm, adherent ceramic deposit. This was shown in this paper [10] Sarkar P, Nicholson PS. Electrophoretic deposition(EPD): mechan- specifically for a model Ni-coated carbon fibre reinforced isms, kinetics and application to ceramics. J Am Ceram So 1996:79:1987-2002. alumina matrix composite [11] Gani MSJ. Electrophoretic deposition. a review. Ind Ceram 1994; 14(4):163-74 [12] Gutierrez CP, Mosley JR, Wallace TC Electrophoretic deposition: a Acknowledgement ersatile coating method. J Electrochem Soc 1962: 109(10): 923-7. [13] Haber S, Gal-Or L Deep electrophoretic penetration and deposition Helpful discussions with colleagues at the University of of ceramic particles inside porous substrates, I. Analytical Model. J Birmingham, UK (Dr P. Trusty, Dr C B. Ponton), and at Electrochem Soc 1992: 139(4): 1071-8 the Technical University of Ilmenau(Mr U. Schindler, [14] Haber S, Gal-Or L. Deep electrophoretic penetration and deposition Dr H.G. Kruger, Prof H. Kern) are appreciated of ceramic particles inside porous substrates, Il. Experimental Model J Electrochem Soc 1992: 139(4): 1078-8 [15] Haber S. Deep electrophoretic penetration and deposition of ceramic References particles inside impermeable porous substrates. J Colloid Interface Sci 1996;179:380-90. [16] Jean J-H. Electrophoretic deposition of Al2O3-SiC composite Mater [11 Chawla KK. Ceramic matrix composites. London: Chapman and Hall, Chem Phys1995:40285-90. [17 Zhang Z, Huang Y, Jiang Z. Electrophoretic deposition forming of
( 6FF5 I !#$ 7 "/% ( "% (& "(% "/% ( ( ( 7 3 ( !#$ ( - &'( '( ( & (( - !#$ & & - /& ( ! " 0 ( ( ( "$ # - ( $ #% - +( ": 7 $ 01 (Q # 0 % # H9EE <>= $ $8 ( ( @3: 6FFA;EG"G%EB9A4 E6F94E 9GE 9G = 0 7 1&3 8 $ ( ( + : @ ! 7 6FF4;6>F"E%65G69H F"E%65GH9H6 H59F5 97 : # 6FFA;E54HA9F5 5 O 64A5 4 - ( ((
A.R. Boccaccini et al. Composites: Part A 32(2001)997-1006 SiC-TZP composites in a nonaqueous sol media. J Am Ceram Soc 38] Boccaccini AR, MacLaren L, Lewis MH, Ponton CB. Electrophoretic 94:77(7):19469 deposition infiltration of 2-D woven SiC fibre mats with mixed sols of [18] Sarkar P, Haung X, Nicholson PS Structural ceramic microlaminates mullite composition. J Eur Ceram Soc 1997; 17: 1545-50 by electrophoretic deposition. J Am Ceram Soc 1992: 75(10): 2907-9 [39 Strecker HH, Norton KP, Katz JD, Freim JO. Microwave densifica- [19] Vandeperre L. Van der Biest O. Electrophoretic forming of silicon tion of electrophoretically infiltrated silicon carbide composite. carbide laminates with graphite interfaces. In: Galassi C, editor. J Mater Sci1997;32:6429-33 ourth Euroceramics, vol. I, Faenza, Italy. Gruppo Editoriale Faenza [40] Trusty PA, Ponton CB, Boccaccini AR. Fabrication of woven Nicalon"(NL 607) SiC fibre-yttrium disilicate CMCs using 20] Fischer R, Fischer E, De Portu G, Roncari E Preparation of ceramic electrophoretic deposition. Ceram Trans 1998: 83: 391-8 micro-laminate by electrophoresis in aqueous system. J Mater Sci Lett [411 Trusty PA, Illston T], Butler EG, Marquis PM, Ponton CB.5.A 1995:14:25-7 21] Yamashita K, Nagai M, Umegaki T Fabrication of green films of SiO2 and AlyO AlO3 woven fibre reinforced composites, Adv ngle- and multi-component ceramic composites by electrophoretic Synthesis and Processing of Cor vol. 1 deposition technique. J Mater Sci 1997: 32: 6661 Ohio: The American Ceramic Society, 1995(p. 257-62) 22] Sarkar P, Datta S, Nicholson PS. Electrophoretic deposition of 42] Trusty PA, Boccaccini AR, Butler EG, Ponton CB. The development controlled ceramic microstructures Ceram Trans 1997: 85: 231-50 of mullite matrix ceramic fiber composites using electrophoretic 23] Sarkar P, Datta S, Nicholson PS. Functionally graded ceramic/ deposition Ceram Trans 1996: 78: 63-70 ceramic and metal/ceramic composites by electrophoretic deposition. [43] Kaya C, Trusty PA, Ponton CB. Electrophoretic filtration deposition Compos Part B 1997: 28B: 49-56 (EFD) of Saffil alumina fibre-reinforced mullite multilayer 124 Sarkar P, Sagakuchi S, Yonehara E, Hamagami J, Yamashita K, ceramic matrix composites. Ceram Trans 1998: 83: 399-406 Umegaki T Electrophoretic forming of functionally-graded barium/ [44] Kooner S, Westby wS, Watson CMA, Farries PM. Processing of ontium titanate ceramics. In: Shiota I, Miyamoto MY, editors. Functionally graded materials, 1996. Amsterdam: Elsevier, 1997 Nextel"(720/mullite composition composite using electrophoretic deposition. J Eur Ceram Soc 2000: 20: 631-8 221-6. 25 Wan YZ, wang YL, Li g, Luo HL, Cheng Gx. Carbon fibre felt [45] Kaya C. Gu X, Al-Dawery I, Butler EG. Processing of woven mullite electrodeposited by copper and its composites. J Mater Sci Lett fibre-mullite ceramic matrix composites using electrophoretic 97;16:1561-3. deposition(submitted for publication). [46 Moreno R, Ferrari B Advanced ceramics via EPD of aqueous slurries. [26] Devrajan J, Singh RN. Electrochemical processing of metal matrix opposites. Ceram Trans 1993: 38: 115-25 Ceram Bull2000:79(1):44-8. [27] Kooner S, Campaniello J, Pickering S, Bullock E. Fibre reinforced (47) Clasen R. Formin ts of submicron silica particles by electro- ceramic matrix composite fabrication by electrophoretic infiltration. horetic deposition. In: Hausner H, Messing GL, Hirano S, editors. Ceram Trans 1995: 58: 155-60 Ceramic powder processing science. Cologne, Germany: Dt Kera- 28] Kawai C, Wakamatsu S Fabrication of C/SiC composites by an elec- mische Gesellschaft, 1989. P. 633-4 ntering method and the control of the properties. 48] Boccaccini AR, Trusty PA, Taplin DMR, Ponton CB Mater Sci1996:31:2165-70. processing of a mullite matrix material suitable for [29] Zhitomirsky I. Electrophoretic and electrolytic n of ceramic woven fibre preforms using electrophoretic deposition. J carbon fibres. J Eur Ceram Soc 1998: 18: 849-56 Soc1996;16:1319-27 30 Zhitomirsky I. horetic hydroxyapatite coatings and fibres. [49] Kaya C, Trusty PA, Ponton CB. Preparation of heterocoagulated Mater Lett200042:262-71 colloidal suspensions for fabrication of ceramic matrix composites by 31 Boccaccini AR, Schindler U, Krueger HG. Ceramic coatings on electrophoretic filtration deposition. Br Ceram Trans 1998: 97(2): 48-54 arbon and metallic fibres by electrophoretic deposition(submitted [50] Brinker CJ, Scherer Gw. Sol-gel science. New York: Academic or publication) Press. 1990. [32] Kaya C, Boccaccini AR, Chawla KK. Electrophoretic deposition [51] Boccaccini AR, Trusty PA. Electrophoretic deposition infiltration of rming of Ni-coated carbon fiber-reinforced borosilicate glass matrix metallic fabrics with a boehmite sol for the preparation of ductile- opposites. J Am Ceram Soc 2000: 83: 1885-8. toughened ceramic composites. J Mater Sci 1998: 33: 933-8 [33] Illston TJ, Ponton CB, Marquis PM. Butler EG. Electrophoret [52] Kaya C, Boccaccini AR, Trusty PA Processing and characterisation deposition of silica/alumina colloids for the manufacture of CMCs. of 2-D woven metal fibre-reinforced multilayer silica Ceram Engng sci proc 1994: 14: 1052-9 opposites using electrophoretic deposition and pressure filtration. [34] Boccaccini AR, Ponton CB Processing ceramic-matrix composites J Eur Ceram Soc 1999: 19: 2859-66 ing electrophoretic deposition JOM 1995: 47(7): 34. [53] Boccaccini AR, Ovenstone J, Trusty PA Fabrication of woven metal [35] Trusty PA, Boccaccini AR, Butler EG, Ponton CB Novel techniques fibre reinforced glass matrix composites. Appl Compos Mater 997:4:145-55 I Preform fabrication. Mater and Manuf Processes 1995: 10: 1215-26 [54] Trusty PA, Boccaccini AR. Alternative uses of waste glasses: fabrica- [36] Brown Pw. Electrophoretic deposition of mullite in a continuous tion of metal fibre reinforced glass matrix composites. Appl Compos fashion utilising non-aqueous polymeric sols. Ceram Engng Sci Mater1998:5:207-22 Proc1995:15. 55] Donald Iw, Metcalfe BL. The preparation, properties and applica 37 Ohkawa T, Elsner FH. Fabrication of fiber-reinforced composites. US tions of some glass-coated metal filaments prepared by the Taylor Patent no. 5468358. 21 November 1995 wire process. J Mater Sci 1996: 31: 1139-49
79-P# '(( @ 7 6FFE;GG"G%6FEB9F AF9BB 4BBB69E 69A5 = 7 2 # $ 7 / #7 M( I I # 6FFG;4HEF9AB ;>H66A94A 646BA9G5 5= P 2 + ! : 8 4555;E44B49G6 <>6= 7 ( 01 "( (% <>4= ! /& & @ 7 4555;H>6HHA9H <>>= + -@ # : '( #: ( !1 ! I( (( : ! 7 # 6FFE;6E65A49F <>E= # # 9 ( @3: 6FFA;EG"G%>E9G <>A= - ( # ( !1 # / '( (( + # : :( # 6FFA;65646A94B <>B= #K ! ( (( ( &'(( ! 7 # 6FFA6A <>G= 32 - ! M0 M & 7 # AEBH>AH 46 / 6FFA <>H= :8 + 8 :0 # ! 4&$ 7 ( @ !( 7 6FFG;6G6AEA9A5 <>F= 7 2 00 / # , @$ M @3 : & @ : 7 6FFG;>4BE4F9>> >F69H I43> 7 # 6 3 - 7 6FFA " 4AG9B4% 9G5 = - ( # # ! "!M$% 7 ( & ( ( & - 6FFH;H>>FF9E5B 69H >9E5 6F94G >F>>9H = 3 @ - ( # M : 6FFG;E6EA9AA 666>F9EF 655B -9(9 1 9 : )' 8 - 63 *3+ !!;<