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Processing of Oxide Composites with Three-Dimensional
Fiber Architectures
James Y. Yang, Jared H. Weaver, and Frank W. Zokw
Materials Department, University of California, Santa Barbara, California 93106
Julia J. Mack
Teledyne Scientific Company, Thousand Oaks, California 91360
Fabrication of oxide fiber composites is accompanied by the fiber preform. Even with multiple infiltration cycles, the me-
development of drying cracks in the matrix following slurry in- chanical integrity of the resulting matrices is inferior to that of
filtration. The cracks are a result of the inherent shrinkage in monolithic ceramics. Consequently, matrix-dominated compos-
particle compacts during drying coupled with the mechanical ite properties rarely achieve their full potential.
constraints imposed on the matrix by the fibers. The effects are (iii) When slurry infiltration is used, shrinkage of the green
most pronounced in systems with three-dimensional fiber archi- matrix during drying coupled with the constraints imposed by
tectures. A mitigation strategy based on the addition of coarse the fibers invariably lead to the formation of matrix cracks
matrix particles to the fine particulates has been devised and with large opening displacements (ca. 10 mm).13–15 Once formed,
demonstrated. Among the various implementation strategies ex- these cracks are irreparable by subsequent impregnation and
plored, the most effective involves combining the two particle pyrolysis of ceramic precursor solutions. Their presence has im-
types (coarse and fine) into a single slurry and coinfiltrating the plications in hermeticity, thermal conductivity, and matrix-
slurry through sequential vibration- and vacuum-assisted pro- dominated mechanical properties. Additionally, when subjected
cesses. Regardless of the infiltration route, the SiC particles to thermal gradients, the cracks produce nonuniform tempera-
have no apparent detrimental effect on the fiber bundle proper- ture distributions which can, in turn, lead to further matrix
ties. Additionally, they increase the through-thickness thermal damage.16 Strategies for the mitigation of these cracks is the
diffusivity by 50%–100%. focus of the present article.
The nature of the cracking problem is illustrated in Fig. 1.
The figure shows a typical cross-section through an oxide CFCC
I. Introduction with Nextel 720t fibers in an 8-harness satin weave (8 HSW)
and a mullite/alumina matrix. (Processing details are summa-
C ONTINUOUS fiber ceramic composites (CFCCs) with two-di-
mensional (2D) fiber architectures are vulnerable to delam-
ination when subjected to out-of-plane thermal or mechanical
rized in a subsequent section.) Drying cracks are oriented in the
through-thickness direction, i.e., crack plane normals lying in
stress.1–7 The vulnerability is particularly acute in composites the plane of the fiber weave. Similar cracks have been observed
with porous matrices.1,2,5,7 One obvious remedy is to incorporate in virtually all oxide CFCCs with 2D architectures.13,14,17–22
fibers in the third (out-of-plane) direction. Indeed, the use of this Cracks are not formed in-plane because of the absence of
reinforcement strategy has impressive precedents in polymer– through-thickness constraint.
matrix composites reinforced by glass and carbon fibers.8–12 Drying cracks are inherently more problematic in 3D CFCCs
Implementation of this strategy for CFCCs, however, presents because of the additional constraint imposed by fibers in the
unique fabrication challenges: third principal direction. Figure 2 shows an example of a com-
(i) Weaving complex architectures with ceramic fibers is posite with a 3D orthogonal weave of Nextel 720t fibers and the
problematic because of the high stiffness of these fibers, espe- same mullite/alumina matrix. In this case, the through-thickness
cially relative to that of glass. Nevertheless, with appropriate drying cracks are somewhat longer than those in the 2D material
handling precautions and attention to architectural design, the (because of the larger intertow spaces) and exhibit larger open-
weaving problems can be overcome. Indeed, the preforms used ing displacements. In-plane drying cracks are also evident. These
in the present study (detailed below) were of exceptional quality are concentrated near the panel mid-plane but are also present
with minimal fiber damage. along fiber tow/matrix boundaries at other through-thickness
(ii) Processing of ceramic matrices usually involves some
combination of chemical vapor infiltration, particle slurry infil-
tration and precursor solution impregnation and pyrolysis (the
notable exception being melt infiltration of Si alloys into SiC
fiber-reinforced systems). Each of these routes on its own is ca-
pable of only partially filling the available void space within the
R. Hay—contributing editor
Manuscript No. 25363. Received October 15, 2008; approved February 11, 2009.
This work was financially supported by the U.S. Air Force Research Laboratory
through a subcontract from Siemens Power Generation (award number 442490–59855,
monitored by Drs. M. Cinibulk and G. Fair at AFRL and Drs. J. Lane and G. Merrill at Fig. 1. Backscatter electron image of a composite with a mullite/
Siemens) and the Air Force Office of Scientific Research (award number F49550-05-1-0134, alumina matrix and NextelTM 720 fibers in an 8-harness satin weave.
monitored by Dr. B. L. Lee).
w
Author to whom correspondence should be addressed. e-mail: zok@engineering. Drying cracks are oriented in the through-thickness direction, perpen-
ucsb.edu dicular to the plane of the fibers.
1087
1088 Journal of the American Ceramic Society—Yang et al. Vol. 92, No. 5
locations. The latter cracks (not present in the 2D weave) are III. Implementation Via Vacuum-Assisted Infiltration
attributable to the constraint imposed by the through-thickness
The preceding concept was implemented using an established
Z-yarns.
vacuum-assisted slurry infiltration method, described else-
Two strategies for mitigating drying cracks have been pro-
where13,14,21 and summarized in the flowchart in Fig. 3 (along
posed. The first is to fill the large matrix-rich pockets between
route labeled I). The baseline method begins with preparation of
tows with high aspect ratio chopped fibers. In one implementa-
a dispersed slurry of B1 mm mullite (MU-107, Show Denko
tion, 2D cloths were coated with a paste of chopped alumina
K.K., Tokyo, Japan) and 0.2 mm alumina particulates (AKP-50,
fibers before stacking the cloths and infiltrating the matrix con-
Mitsui Mining Co., Tokyo, Japan), in a ratio of 4:1 (by volume),
stituents.13 Although somewhat successful in reducing the pro-
and with a total solids loading of 30% in deionized water. Nitric
pensity for matrix cracking, the use of pastes in this manner
acid was added to achieve a pH of 3, thereby assuring a well-
is inherently restricted to 2D laminates. This approach also re-
dispersed slurry. Agglomerates were broken down through a
duces the fiber content that can be achieved. The second is based
combination of stirring and ultrasonication for about 1 h. The
on freeze-drying. Specifically, the slurry carrier fluid is frozen
slurry was poured onto the preform, vacuum degassed, and then
immediately after infiltration into the fiber preform and re-
infiltrated via a vacuum-assisted process. Once infiltration was
moved by sublimation.23 Cracking is prevented because of the
complete (typically 3–4 h), the green composite was dried and
absence of capillary forces during carrier removal. Although
fired in air in a box furnace (1 h at 9001C). With the mullite/
some encouraging progress has been made using camphene as
alumina proportions used here, the mullite particles form a con-
the carrier fluid (selected for its high sublimation temperature), a
tiguous network that inhibits densification during subsequent
critical assessment of the viability of this route for fabrication of
oxide CFCCs has yet to be performed.
The objective of the present article is to present an alternate
strategy for mitigating shrinkage cracks in 3D CFCCs. Two as-
pects of the fabrication process feature prominently: (i) incor-
poration of coarse (410 mm) matrix particles in addition to the
smaller particulates (r1 mm); and (ii) use of vibration to facil-
itate infiltration. Secondary goals include identifying possible
fiber degradation mechanisms associated with the processing
route and probing the effects of the coarse particles on through-
thickness thermal diffusivity.
The remainder of the article is organized in the following way.
First, the rationale for combining coarse and fine particles in the
matrix is described. Then, an assessment is made of the efficacy
and the deficiencies of coinfiltration of these particles into fiber
preforms using an established vacuum-assisted route. With lim-
itations of the vacuum-assisted route exposed, an augmentation
based on vibration-assisted infiltration is devised and demon-
strated. Finally, measurements of the in-plane tensile properties
and through thickness diffusivity are presented.
Fig. 5. Effects of solids loading on particle packing in the two-dimensional (8-harness satin weave) fabric. The particles had been coinfiltrated by the
vacuum-assisted route. Drying cracks are almost completely eliminated in all cases. Subtle changes in inter- and intratow porosity are evident.
1090 Journal of the American Ceramic Society—Yang et al. Vol. 92, No. 5
0.0
0 200 400 600 800 1000 1200 1400
Temperature (°C)
1.6
(b) 3D orthogonal weave
1.4
Thermal diffusivity (10–6m2/s)
1.2
1.0
With SiC
0.8
0.6
0.2
0.0
0 200 400 600 800 1000 1200 1400
Temperature (°C)
Fig. 10. (a) Coinfiltration of 23-mm-diameter SiC particles and mullite/ Fig. 12. Effects of fiber architecture and presence of coarse SiC parti-
alumina mixture by sequential vibration- and vacuum-assisted infil- cles on through-thickness thermal diffusivity of (a) 2D and (b) 3D
tration. (b, c) Higher magnification images of regions indicated in (a). composites.
1092 Journal of the American Ceramic Society—Yang et al. Vol. 92, No. 5
8
weaves using a vacuum assisted route. The same process leads to J. Brandt, K. Drechsler, and F.-J. Arendts, ‘‘Mechanical Performance of Com-
posites Based on Various Three-Dimensional Woven-Fibre Preforms,’’ Comp. Sci.
incomplete filling of the 3D preform used in the present study Technol., 56 [3] 381–6 (1996).
because of rapid particle settling coupled with shadowing by the 9
P. J. Callus, A. P. Mouritz, M. K. Bannister, and K. H. Leong, ‘‘Tensile Prop-
warp weavers. For this purpose, vibration of the slurry and pre- erties and Failure Mechanisms of 3D woven GRP composites,’’ Composites: Part
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10
S. Chou, H. C. Chen, and H. E. Chen, ‘‘Effect of Weave Structure on
ments. Sequential infiltration of slurries with coarse and fine Mechanical Fracture Behavior of Three-Dimensional Carbon Fiber Reinforced
particles is viable provided the coarse particles are large enough Epoxy Resin Composites,’’ Comp. Sci. Technol., 45 [1] 23–35 (1992).
11
to allow subsequent ingress of the fines. For the present system, B. N. Cox, M. S. Dadkhah, and W. L. Morris, ‘‘On the Tensile Failure of 3D
the critical particle size is about 25 mm. A more convenient route Woven Composites,’’ Composites: Part A, 27 [6] 447–58 (1996).
12
B. N. Cox, M. S. Dadkhah, W. L. Morris, and J. G. Flintoff, ‘‘Failure Mech-
is to combine the two particle types into a single slurry and co- anisms of 3D woven Composites in Tension, Compression, and Bending,’’ Acta
infiltrate them through sequential vibration- and vacuum- Metall. Mater., 42 [12] 3967–84 (1994).
13
assisted processes. Regardless of the infiltration route, the SiC C. G. Levi, J. Y. Yang, B. J. Dalgleish, F. W. Zok, and A. G. Evans, ‘‘Pro-
particles have no apparent detrimental effect on the fiber bundle cessing and Performance of an All-Oxide Ceramic Composite,’’ J. Am. Ceram.
Soc., 81 [8] 2077–86 (1998).
properties: an essential condition for successful composite de- 14
C. G. Levi, F. W. Zok, J. Y. Yang, M. Mattoni, and J. P. A. Lofvander,
sign. Additionally, they significantly increase the thermal diff- ‘‘Microstructural Design of Stable Porous Matrices for All-Oxide Ceramic Com-
usivity (by 50%). posites,’’ Z. Metallk., 90 [12] 1037–47 (1999).
15
Demonstrations of the proposed concept have been per- H. Fujita, G. Jefferson, R. M. McMeeking, and F. W. Zok, ‘‘Mullite-Alumina
Mixtures for Use as Porous Matrices in Oxide Fiber Composites,’’ J. Am. Ceram.
formed using SiC as the coarse particle constituent. This selec- Soc., 87 [2] 261–7 (2004).
tion was based largely on the availability of a wide range of 16
J. W. Hutchinson and T. J. Lu, ‘‘Laminate Delamination Due to Thermal
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17
the oxide constituents. But, in principle, other particle types can R. A. Simon, ‘‘Progress in Processing and Performance of Porous-
Matrix Oxide/Oxide Composites,’’ Int. J. Appl. Ceram. Technol., 2 [2] 141–9
be used to serve the same function. This option would allow for (2005).
tailoring of certain matrix properties, including the thermal ex- 18
R. A. Jurf and S. C. Butner, ‘‘Advances in Oxide–Oxide CMC,’’ J. Eng. Gas
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19
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High Temperature Mechanical Behavior of an Oxide/Oxide Composite,’’ J. Am.
Ceram. Soc., 86 [6] 981–90 (2003).
20
M. G. Holmquist and F. F. Lange, ‘‘Processing and Properties of a Porous
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