Materials Science and Engineering C 11 Ž2000.

9–12
www.elsevier.comrlocatermsec

Biomimetic structure design — a possible approach to change the

brittleness of ceramics in nature q
Chang-an Wang ) , Yong Huang, Qingfeng Zan, Hai Guo, Shengyou Cai
The State Key Laboratory of New Ceramics and Fine Processing, Department of Materials Science and Engineering, Tsinghua UniÕersity,
Beijing 100084, People’s Republic of China
Accepted 17 September 1999

Abstract

Based on the analysis on structure of natural biomaterials, two kinds of ceramic composites with high toughness have been designed
and prepared: one is fibrous monolithic Si 3 N4rBN composite imitating bamboos or trees in structure, the other is laminated Si 3 N4rBN
composite imitating nacre in structure. Plastic forming methods, including extrusion and roll compaction, respectively, followed by
hot-pressed sintering are used to prepare these two materials with particular structures. Both of the two composites have high values of
fracture toughness and work of fracture: fracture toughness are 24 MPa m1r2 and 28 MPa m1r2 , respectively, for fibrous monolithic and
laminated Si 3 N4rBN composites, and works of fracture are both more than 4000 Jrm2. The load-displacement curves reveal that these
two materials with biomimetic structure exhibit non-brittle feature when applied load to fracture. Through analysis on fractographs of the
materials, it is revealed that high toughness comes from the synergistic toughening among multi-level toughening mechanisms in different
scales: weak interfaces, whiskers and elongated grains toughening in ceramic matrix cells. q 2000 Published by Elsevier Science S.A.

Keywords: Biomimetic structure; Fibrous monolithic; Laminated; Si 3 N4 rBN composites

1. Introduction what we seek for ceramic materials with high toughness

through composition control. For example, trees and bam-
A major problem in the service of ceramics as structural boos are typical long, fiber-reinforced composites. Their
materials is their brittleness. Even though many attempts fibers have different sizes and arranged modes in structure
have been used to increase their toughness, including so that they can display the optimal behaviors under
incorporation of fibers, whiskers or particles reinforce- tensile, bending, compressing stress and other applied load.
ments, and ZrO 2 phase transformation reinforcing, etc., up Another typical biomaterial is nacre, the structure of which
to date the brittleness of ceramics has not been overcome is laminated with brick wall structure. It consists of more
in nature. It seems that it is impossible for conventional than 99 vol.% inorganic phase, aragonite wafers, and less
ways to solve this problem. than 1 vol.% organic phase, mortar of proteins. This
On the other hand, in the research on the structure of particular configuration imparts over one order of magni-
natural biomaterials, such as bamboos, trees and nacres, it tude higher bending strength and toughness than those of
has been found that these natural biomaterials have very aragonite single crystals. The work of fracture of nacre is
reasonable structures which gives them many excellent 3000 times higher than that of pure aragonite w1x. So, the
properties, such as good carrying capacity, good tough- complicated and reasonable structure of natural biomateri-
ness, self-healing, and so on. Furthermore, these biomateri- als can give us an important insight into making better
als have very fine and special structures rather than com- structure materials through biomimetic design.
plicated compositions, which are distinctly different from Coblenz w2x in 1988 put forward a fibrous monolithic
structure imitating the structure of trees or bamboos. In the
q structure, fibrous polycrystalline cells are arranged paral-
This research work was supported by the National Science Founda-
tion of China Žgrant No. 59632090..
lel, and separated and combined by very thin interfacial
)
Corresponding author. Tel.: q86-1062785488; fax: q86-1062771160. phase. Baskaran et al. w3x in 1993 firstly prepared SiCrC
E-mail address: [email protected] ŽC. Wang.. fibrous monolithic structure ceramics according to the

0928-4931r00r$ - see front matter q 2000 Published by Elsevier Science S.A.

PII: S 0 9 2 8 - 4 9 3 1 Ž 0 0 . 0 0 1 3 3 - 8
10 C. Wang et al.r Materials Science and Engineering C 11 (2000) 9–12

above design mode. Clegg et al. w4x in 1990 reported a Table 2

pioneer work of preparing a laminated SiC composite Mechanical properties of laminated Si 3 N4 rBN composites
separated by graphite layers, so that very high toughness Average Average sf ŽMPa. K IC ŽMPa m1r 2 .
and flaw tolerance were obtained: 15 MPa m1r2 of fracture thickness of thickness of
green layers matrix layer after
toughness and 4625 Jrm2 of work of fracture. In recent Žmm. sintering Žmm.
years, much attention has been paid to biomimetic struc-
0.2 0.087 709.51"89.61 28.90"4.14
ture ceramics and many good results and opinions have 0.4 0.13 740.64"78.94 28.40"4.49
been obtained w5–7x. 0.8 0.36 518.93"112.94 18.75"4.41
In the present paper, according to the structures of trees 1.6 0.61 704.09"127.19 9.55"1.49
or bamboos and nacres, we designed and prepared two 3.2 1.31 572.50"73.02 11.67"3.53
kinds of ceramic composites with high toughness, fibrous
monolithic and laminated composites, and a lot of active
results were achieved.
A-2000 Shimadzu universal materials testing machine with
a crosshead speed of 0.05 mmrmin. The microstructure of
2. Experimental procedure specimens was observed with SEM.

Ceramic raw powders ŽSi 3 N4 , b-SiC whiskers and sin-

tering aids. were mixed with organic binder ŽPVA., plasti- 3. Results and discussion
cizing agents Žglycerine. and lubricant Žliquid paraffin. and
then repeatedly rolled, turning into a well-distributed plas- 3.1. Mechanical properties
tic mud pie. Fibrous green bodies Žgreen fibers. were
obtained through extrusion. The mud pie was extruded Table 1 summarizes the mechanical properties of fi-
through orifices with different diameters Ž1.0, 0.7, 0.5 and brous monolithic Si 3 N4rBN ceramics. It can be found that
0.3 mm. to form green fibers. Laminated green bodies the fibrous monolithic Si 3 N4rBN ceramics have very high
Žgreen sheets. were obtained through roll compaction. The toughness compared with conventional monolithic Si 3 N4
green bodies Žfibers or sheets. were then coated by dipping ceramics. Table 2 shows the mechanical properties of
in slurry containing mainly BN. The coated green bodies laminated Si 3 N4rBN ceramics with different thickness of
were dried in air and arranged in a certain order into a matrix layer in which 20 wt.% SiC whiskers were added. It
graphite die and hot-pressed at 18008Cr1.5 hr22 MPa can be seen that the laminated Si 3 N4rBN ceramics can
pressure under flow N2 atmosphere. In addition, rod-like reach more than 28 MPa m1r2 of fracture toughness.
b-Si 3 N4 seeds Ž3 wt.%. or b-SiC whiskers Ž20 wt.%. were In Tables 1 and 2, it can be seen that the size of the
added into Si 3 N4 matrix cells for further toughening. matrix cells Žfiber or layer. obviously has an effect on the
Al 2 O 3 or Si 3 N4 was added into the BN interfacial phase properties of the composites. With the decrease in the size
for the purpose of adjusting the interfacial bonding state of matrix cell, the fracture toughness of the composites is
between Si 3 N4 matrix cells. markedly improved while the bending strength has no
Bending strength was determined by three point bend obvious change. Moreover, in literature w4,7x the bending
testing Žtest bars 4 = 3 = 36 mm3 .. The tensile surface of strength of this kind of ceramic with weak interfacial
the samples was polished with diamond paste down to 1 phase at room temperature was considerably reduced due
mm and the long edges of the tensile surface were rounded.
Fracture toughness was measured by SENB method Žtest
bars 4 = 6 = 30 mm3 ., and the width of the notch was less
than 0.25 mm. The curve of load-displacement and work
of fracture of the specimen were determined using an

Table 1
Mechanical properties of in-situ fibrous monolithic Si 3 N4 rBN compos-
ites
Average Add seeds Add whiskers
diameter of sf ŽMPa. K IC sf ŽMPa. K IC
green fiber ŽMPa m1r2 . ŽMPa m1r2 .
Žmm.
1.0 689.3"68 8.98"1.04 705.4"71 20.01"1.17
0.7 602.1"62 11.52"0.98 678.1"62 22.56"1.01
0.5 562.4"51 14.11"1.00 639.7"60 22.96"0.88
0.3 530.6"42 17.16"1.02 619.8"47 23.95"0.92 Fig. 1. Typical load-displacement curve of fibrous monolithic Si 3 N4 rBN
composites.
 C. Wang et al.r Materials Science and Engineering C 11 (2000) 9–12 11

Fig. 4. Microstructure of laminated Si 3 N4 rBN composites.

Fig. 2. Typical load-displacement curve of laminated Si 3 N4 rBN com-
posites.

inferred that the mechanical performance of ceramic mate-

rials can be substantially improved by special biomimetic
to the presence of weak separating interfacial phases. structural design.
However, in the present paper, the mechanical properties
can be improved obviously by adding whiskers or seeds 3.3. Microstructure and multileÕel toughening mechanisms
into the matrix phase.
Fig. 3 displays the microstructure of Si 3 N4rBN fibrous
3.2. CurÕe of load-displacement and work of fracture monolithic ceramics. On the two sides planes of the speci-
men fibers, which are arranged in uniaxial direction regu-
Fig. 1 and Fig. 2 are curves of load-displacement for larly, can be observed ŽFig. 3a.. At two end planes of the
fibrous monolithic Si 3 N4rBN ceramics and laminated specimen, it can be seen that the cross-section of the cells
Si 3 N4rBN ceramics, respectively. Compared with mono- are more like an hexagon, just like Coblenz’s design mode
lithic Si 3 N4 ceramics, fibrous monolithic Si 3 N4rBN ce- w2x. Fig. 4 shows a photograph of crack propagation of
ramics and laminated Si 3 N4rBN ceramics exhibit a non- laminated Si 3 N4rBN ceramics, which exhibits a laminated
brittle failure manner while the conventional monolithic structure and crack deflection. Note that the cells Žfibers or
Si 3 N4 fractures catastrophically. Furthermore, the size of layers. are not single crystals but domains of polycrys-
the matrix cell has an obvious influence on the mechanical talline Si 3 N4 . The BN interfacial phase acts as cell bound-
performance as shown in Fig. 1. According to the area ary phase to separate the cells.
covered by the curves of load-displacement, work of frac- The common characteristic of the two biomimetic com-
ture for two biomimetic materials can be calculated as posites is that the strong matrix cells and the relative weak
more than 4000 Jrm2 in general, while that of monolithic interfacial phases are arranged alternately with each other.
Si 3 N4 ceramics is only 100 Jrm2 or so. Hence, it may be There are multilevel toughening mechanisms in different

Fig. 3. Microstructure of fibrous monolithic Si 3 N4rBN composites.

12 C. Wang et al.r Materials Science and Engineering C 11 (2000) 9–12

scales in these kinds of composites: the 1st-grade toughen- toughening and elongated matrix grain toughening leads to
ing mechanism is weak interfacial layer toughening, which fairly high toughness and work of fracture of the compos-
is considered as the main reason for the very high tough- ites.
ness of the composites; the 2nd-grade toughening mecha-
nism is whisker toughening in the matrix cells; and the
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