Ceramics International 45 (2019) 16776–16783

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Ceramics International
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Effect of temperature gradient on competitive growth behavior of Si and T

YSi2 in a Si–Y eutectic alloy prepared by Bridgeman method
Jinguang Lia, Rui Hua,∗, Jieren Yanga, Yongsheng Liub
a
State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, Xi'an, 710072, PR China
b
National Key Laboratory of Thermostructure Composites Materials, Northwestern Polytechnical University, Xi'an, 710072, PR China

A R T I C LE I N FO A B S T R A C T

Keywords: The Si–Y eutectic alloy has been prepared by Bridgeman method where the high temperature gradient (GE) can
Si–Y alloy be obtained by means of double heating combining with liquid metal cooling. The microstructures of long-
Directional solidification itudinal section and cross section at different GE have been observed. It can be seen clearly that the YSi2 phase
Temperature gradient GE presents the evolution process of thick banded shape, island shape, reticular shape and fine strip shape as GE
Interface growth temperature
increases from 90 K/cm to 200 K/cm. Based on the interface growth temperature model, it can be concluded that
Competitive growth
the interface growth temperatures of Si phase and YSi2 phase both will decrease linearly with increasing GE
while that of eutectic structure will keep a constant of 1485.6 K. Two critical temperature gradients
GEC1 = 52 K/cm and GEC2 = 111 K/cm have been calculated. Eutectic coupling growth will take the dominant
position when the actual GE is greater than GEC2. The primary Si phase will begin to form as GE is smaller than
GEC2 and will be thicker as GE is smaller than GEC1. The coupling effect of withdrawal rate and GE on the
microstructures of the Si–Y alloy also has been analyzed comprehensively.

1. Introduction primary Si phase. Furthermore, Si powder will have an adverse effect

Si–Y alloy has been considered to be a new infiltration alloy to re-
place conventional alloys such as Si–Zr, Si–Mo and Si–Mo–Ti alloys to
prepare SiCf/SiC composites [1–3]. Compared with conventional Si-
based infiltration alloys, Si–Y alloy not only has a better oxidation re-
sistance, but also has a lower melting point which can be used to avoid
the ablation of SiC fibre [4,5]. As is known to all, the unhomogeneous
composition or microstructure will lead to the different melting points
in different areas especially in large size alloy ingot [6]. In order to
achieve the goal to reduce the infiltration temperature further below
1300 °C which can effectively avoid SiC fiber decomposing into SiO and
CO [7], it is very important for Si–Y alloy to have the homogeneous full
eutectic microstructure especially in large size alloy ingot which can
increase productivity of the infiltration alloy powders. However, in
actual process of preparing Si–Y alloy, there will be a severe component
segregation even with the eutectic nominal component due to the poor
fluidity of alloy melt, meanwhile lots of primary Si phase in large size
even more than 1 mm will form in Si–Y alloy not only due to severe
component segregation, but also due to the heterogeneous temperature
fields especially in large size alloy melt. Thus, the quality of Si–Y alloy
powders crushed from the Si–Y alloy ingot will be poor because of
containing a large amount of Si powders broken from the large size
on the remelting of Si–Y alloy during infiltration process. The melting
point of Si is 1414 °C and this will cause unmelted Si phase exist during
infiltration process, which will not only make the residual Si phase to
cause unhomogeneous microstructure of the SiC/SiC composite, but
also make the fluidity of infiltration alloy melts to be more worse and
lead the infiltration efficiency to be more lower. Thus, choosing a sui-
table method to prepare the Si–Y alloy with homogeneous full eutectic
microstructure firstly before infiltration process will have practical
significance.
Unfortunately, little research has been done on the microstructure
uniformity controlling of Si–Y alloy up to now. As for alloy ingot in
large size, it is well known that segregation is a prevalent phenomenon
especially for Si–Y alloy whose fluidity is poor and the component
segregation would be more severe. The especially high degree of seg-
regation will make the system sensitive to small changes of growth
conditions, which can lead to inhomogeneities and constitutional su-
percooling in the melt near the front of crystallization, the primary Si
phase can be thus easy to form when there are some disturbances [8].
Moreover, because of the poor liquidity of Si–Y alloy melt, there will be
lots of casting defects in large size ingot and the microstructure is also
irregular at those places. Because there is a lack of reference for pre-
paring large size Si–Y alloy and also a lack of theoretical basis for

∗
Corresponding author. State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, Xi'an, 710072, Shaanxi Province, PR China.
E-mail address: rhu@nwpu.edu.cn (R. Hu).

https://doi.org/10.1016/j.ceramint.2019.05.213
Received 11 April 2019; Received in revised form 9 May 2019; Accepted 20 May 2019
Available online 21 May 2019
0272-8842/ © 2019 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
J. Li, et al. Ceramics International 45 (2019) 16776–16783

microstructure regulation with Si–Y alloy, the production efficiency of

Si–Y alloy in large size would be reduced. Therefore, it is of great sig-
nificance to study the solidification characteristics of Si–Y infiltration
alloys and realize the homogenization regulation of microstructures.
Directional solidification is an effective method to control the soli-
dification microstructure of alloys and study the solidification me-
chanism. In directional solidification experiments both withdrawal rate
V and GE may be controlled independently, so that one may study the
dependence of solidification microstructure on either GE (at constant V)
or V (at constant GE) [9]. In our previous study, the effect of withdrawal
rate V on microstructure evolution have been investigated and the
competitive growth among the Si phase, the YSi2 phase and the eutectic
structure with a low temperature gradient (GE) of 47 K/cm in direc-
tional solidification have been discussed [10]. Although the withdrawal
rate has an important influence on the evolution of solidification mi-
crostructure, the influence of GE cannot be ignored due to really poor Fig. 1. Schematic of the Bridgman furnace with double heating design.
fluidity of Si–Y eutectic system which may cause hypereutectic or hy-
poeutectic components to be present in the local area especially in large prepared.
size ingot. According to eutectic growth interface stability criterion GE/ Using standard metallographic techniques, the specimens for ana-
V ≥ K where the K can be regarded as a constant related to the com- lysis were prepared. They were etched with a Keller solution which was
position [11], a higher GE will make it possible to obtain fully eutectic composed of 2.5 ml HNO3 + 1.5 ml HCl +1 ml HF + 95 ml distilled
structure even if the components do deviate which have been confirmed water and soaked at room temperature for 3 min for the longitudinal
in NiAl–Cr (Mo) system [12,13]. The research on Al–Si eutectic system sections and 2 min for the cross sections. The FEI Nova field emission
by W. R. Huang also have shown that the component undercooling will scanning electron microscopy (FESEM) equipped with the energy dis-
increase gradually as the GE decreased. When the GE reached a certain persive spectroscopy (EDS) was used to characterize the microstructure
critical value, it will cause the transformation from regular interface to and solute's segregation. X-ray diffraction was used to characterize
irregular interface, which will also be accompanied by the appearance phases in specimens with a scan rate of 2°/min.
of primary phase. The macroscopic morphology of Al–Si eutectic un-
derwent the transformation of cellular dendrite shape, columnar den-
3. Results and discussion
drite shape and oblong equiaxed crystal shape as GE decreased [14].
The research on Pb–Sn eutectic system and Si–TaSi2 eutectic system
3.1. Acquisition and controlling of high GE
also suggested that a higher GE can increase the critical withdrawal rate
and be beneficial to improve microstructure uniformity meanwhile
In directional solidification, maintaining a high GE can reduce the
reduce eutectic spacing [9,15].
component segregation degree caused by increasing withdrawal rate
However, few literature about the effect of GE on microstructure
[16]. The double heating combined with liquid metal cooling has been
homogenization of Si–Y alloy could be found up to now. To provide an
regarded as an effective method to obtain a higher GE.
effective theoretical support for the preparation of large size Si–Y in-
Under the condition of double heating, the relationship among the
filtration alloy, in this paper, the microstructure evolution of Si–Y alloy
temperature gradient GE, the withdrawal rate V, the radius r of cy-
at different GE has been investigated by directional solidification
lindrical sample and the heat transfer coefficient h can be expressed as
method and the competitive growth mechanism of each phase has been
[17,18].
investigated systematically by using interface growth temperature
model. The results in this paper will allow us to prepare the large size GE = [2hαT − T0/ rV − ρLf V ]/ KL (1)
Si–Y infiltration alloy ingot with homogeneous microstructure where
the production efficiency can be improved significantly. where Lf is the crystallization latent heat, ρ is the density of melt, T0 is
the temperature of cooling medium. It can be concluded that adopting
2. Experimental procedure Ga-In-Sn liquid alloy with high heat transfer coefficient (hGa-In-
Sn = 14122 > hwater = 2041), reducing sample size r（r = 3.5 mm in

A Si-18at. %Y alloy master ingot was prepared which was melted
three times in order to ensure a homogeneous composition by vacuum
arc melting using 99.999% polysilicon powder and 99.9% Y powder.
Then the alloy ingot was cut into cubes by electric spark cutting ma-
chine and was filled in a 7 mm × 110 mm thin-walled alundum tube.
The directional solidification experiment was carried out in the
Bridgman furnace with a high purity argon atmosphere. In order to
obtain a higher GE, double heating method was adopted in this paper,
as shown in Fig. 1. At the location near the Ga-In-Sn liquid metal
cooling bath, an additional high purity graphite heating element,
Heater 2, was added. In addition, two thermocouples were placed ad-
jacent to the solid-liquid interface in order to obtain the GE. One was
next to the liquid phase and the other was next to the solid phase. Both
two thermocouples were attached to the outer wall of the thin-walled
alundum tube, so as to measure the temperature in each region more
accurately. The molten alloy was pulled down into the cooling bath
with four different GE of 90 K/cm, 120 K/cm, 160 K/cm and 200 K/cm
respectively at a constant withdrawal rate 1.5 mm/min. The cylindrical
bars of Si–Y eutectic alloy with 7 mm diameter and 80 mm length were
this paper）and appropriately increasing the temperature T of direc-
tional solidification all will be conducive to obtain a high GE.
Through adjusting the heating power, the temperature of solid
phase TS, the temperature of liquid phase TL have been measured by
two thermocouples respectively and the GE can be calculated as shown
in Fig. 2. The results have shown that the GE can reach 90 K/cm, 120 K/
cm, 160 K/cm and 200 K/cm respectively when the liquid phase tem-
peratures are 1703 K, 1768 K, 1850K, 1943K.
3.2. Directionally solidified microstructures
The Si–Y eutectic alloy has been prepared by Bridgeman method
with GE of 90 K/cm, 120 K/cm, 160 K/cm and 200 K/cm respectively.
The microstructure morphology has been observed by SEM. It can be
seen the directional solidified microstructure has been more regular and
more orderly than that of master alloy, as shown in Fig. 3(a)–b.
The phase and composition have been detected by XRD and EDS
respectively. According to the XRD detection results, there are only Si
phase and YSi2 phase in Si–Y eutectic alloy. Combining with EDS

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Fig. 2. The relation curve of the GE with the directional solidification heating
power P.

composition detection results, it can be determined that the black area Fig. 4. Microstructures of longitudinal sections at different GE: (a) 90 K/cm, (b)
is Si phase and white area is YSi2 phase, as shown in Fig. 3(c)–d. The 120 K/cm, (c) 160 K/cm and (d) 200 K/cm.
interface between Si phase and YSi2 phase is curved and irregular just
like Al2O3/Y3Al5O12/ZrO2 composites fabricated by directional solidi-
shape distributed along the thick primary Si phase to island shape and
fication which belongs to faceted system [19]. The actual composition
finally to fine, long strip shape in Si–Y eutectic alloy with a constant GE
of alloy measured by EDS is Si-18.02 at. %Y which is close to the
of 47 K/cm but different withdrawal rates [10].
nominal composition Si-18 at. %Y. Hence, the effect of element vola-
When the GE is 90 K/cm, a large number of primary Si phases exist
tilization on alloy composition during directional solidification could be
in the microstructure whose average diameter is 50 μm approximately,
negligible.
as shown in Fig. 4(a). The growth direction of primary Si phases is
The microstructure of directional solidification Si–Y alloy samples
highly parallel to the opposite direction of withdrawal in directional
has been observed by SEM, and obvious differences in microstructure
solidification. At the boundary of primary Si phase, Y element is en-
morphology can be found. The microstructure in longitudinal section is
riched due to the poor fluidity of alloy melt, which can result in the
shown in Fig. 4. It can be seen clearly that the YSi2 phase presents the
formation of thick banded YSi2 phase where the study by F. W. Dynys
evolution process of thick banded shape, island shape, reticular shape
also confirmed the existence of thick blocky YSi2 phase [20]. More than
and strip shape successively as GE increases from 90 K/cm to 200 K/cm,
10 μm away from the primary Si phase, there is a large amount of
which is consistent with the evolution process of YSi2 phase from blocks

Fig. 3. Analysis results for Si–YSi2 eutectic alloy: (a) microstructure of master alloy, (b) directional solidified microstructure, (c) the chemical composition, (d) the
XRD spectrum.

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eutectic structure. The orientation of eutectic structure is also obvious,

which is consistent with the growth direction of primary Si phase. The
YSi2 phase in eutectic structure presents a thick bar shape with the
longitudinal average length of 86 μm.
When the GE increases to 120 K/cm, the growth direction of the
alloy microstructure will be more obvious, as shown in Fig. 4(b). It can
be seen clearly that primary Si phase and thick banded YSi2 phase have
been largely eliminated, which is replaced by the eutectic structure
consisting of YSi2 phase and Si phase with serrated morphology. In
eutectic structure, since the Si phase still has a strong tendency to grow
laterally and thicken, the growth path of YSi2 phase will be cut off in
many areas. As a result, the connectivity between the upper YSi2 phase
and the lower YSi2 phase will be relatively weak which could make YSi2
phase present island morphology with the longitudinal average length
of 97 μm. The island shaped microstructure is similar to the cellular
structure in Al2O3/ZrO2(Y2O3) and Al2O3/YAG [21,22] eutectic system
whose formation can be explained that the GE is not high enough to
stabilize the interface instability caused by rapid withdrawal rate.
As the GE further increases to 160 K/cm, the microstructure of Si–Y
alloy will be full eutectic structure as shown in Fig. 4(c). While the
Fig. 5. Microstructures of cross sections at different GE: (a) 90 K/cm, (b) 120 K/
directivity of microstructure growth has been further strengthened, a
cm, (c) 160 K/cm and (d) 200 K/cm.
significant refinement also occurs in size. The shape of YSi2 phase has
transformed from an isolated island shape into a thin band shape where
the upper and lower part has better connectivity. The longitudinal can be explained by the fact that dynamic undercooling under high GE
average length of YSi2 phase has increased to 195 μm. However, the Si has stabilized the non-isothermal interface and leaded to the transfor-
phase in a few regions still has a prominent growth tendency to cut off mation of YSi2 phase from faceted phase to weak faceted phase or even
the longitudinal growth of YSi2 phase. As a result, the YSi2 phase in non-faceted phase [20].
these regions will remain laterally connected. Hence, a tight reticular As the GE increases from 90 K/cm to 200 K/cm, the primary Si phase
shaped structure will form. This morphology resembles the finely en- disappears while the eutectic structure is gradually refined. The long-
tangled structure in Al2O3/YAG composites in which single crystal itudinal average length of YSi2 phase increases from 86 μm to 325 μm
Al2O3 and single crystal YAG are three-dimensionally and continuously and the lateral average size decreases from 28 μm to 7 μm, as shown in
connected without grain boundaries [23]. Fig. 6.
When the GE increases to 200 K/cm, the microstructure still presents The size changing process exactly corresponds to the morphology
a full eutectic structure with excellent growth direction as shown in evolution process of YSi2 phase which is from thick banded shape to
Fig. 4(d). The Si phase and YSi2 phase in eutectic structure have nearly island shape, to reticular shape and finally to strip shape. This phe-
the same growth dynamics so as to present a orderly and staggered nomenon is related to the relative dynamic changes of the coupling
arrangement with fine strip morphology. The study of A. Henniche on eutectic growth and the competing growth of Si phase and YSi2 phase
GdAlO3-Al2O3 eutectic also shows the ceramic contains a dense, uni- under different GE, which will be explained in detail in the sections
form and fine microstructure, in which the binary oxide phases are below.
uniformly distributed and fine microstructure consists of two phases of
Al2O3 and GdAlO3 strongly entangled with each other [24,25], the 3.3. Interface growth temperature model in Si–Y eutectic alloy
microstructure of which is similar to Si–Y alloy. Under the condition of
high GE, all the island shaped structure has disappeared. With further Although Si–Y alloy belongs to the facet-facet phase system, a reg-
refinement, the length of YSi2 phase has increased to 325 μm. ular rod eutectic can be observed experimentally, which may indicate a
As the GE changes from 90 K/cm to 200 K/cm, the microstructure facet to non-facet transformation under high GE has occurred in this
evolution of cross sections is shown in Fig. 5. paper. This is consistent with the results of non-faceted growth of Si due
At the GE of 90 K/cm, there are obviously thick primary Si phases to high dynamic undercooling [27]. Research of J. J. Yu et al. shows
exist. The YSi2 phase with irregular shape is distributed at the boundary
of primary Si phase. And the average lateral size of YSi2 phases is
35 μm. As the GE increases to 120 K/cm, the primary Si phase dis-
appears completely. The YSi2 phase presents as the irregular strip shape
with the average size of 29 μm. The irregular strip structures are iso-
lated from each other which correspond to island shaped structures in
longitudinal section. When the GE reaches 160 K/cm, the strip shape of
YSi2 phase has changed to long elliptical shape with an average dia-
meter of only 16 μm in most areas, which is distributed in the Si matrix
in isolation, as shown in Fig. 5(c). The formation of long elliptical
shaped phase in eutectic has also been found in Si–TaSi2 system when
the GE reaches 210 K/cm with withdrawal rate of 0.6 mm/min [26]. At
a few other areas, the strip shaped YSi2 phase still remains, but the
transverse size has been shortened. This corresponds to the reticular
shaped structure in longitudinal section. At a high GE of 200 K/cm, the
shape of YSi2 phase has get closer to circle. The number of YSi2 phase
increases meanwhile the average diameter decreases to 8 μm, as shown
in Fig. 5(d). With increasing GE, the YSi2 phase in the cross section
gradually evolves from irregular shape to regular circle shape, which Fig. 6. Average sizes of YSi2 phase in longitudinal section and cross section.

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that the planar interface for partially cooperative growth of eutectic
will be stable when [28]:
GE / V ≥ mL C0 (1 − k )/ DL (2)
where GE is the temperature gradient near the S/L interface, V is the
interface growth velocity which is 1.5 mm/min in this paper, mL is the
slope of the liquids of α phase which is 4.83 K/wt.% [29], C0 is the
initial solute concentration in the liquid which is equal to 41 wt% ac-
cording to Si–Y phase diagram [29], k is the segregation coefficient
equal to 0.84 [29], DL is the diffusion coefficient of solute in the liquid
which is 4.3×10−9 m2/s [10]. The critical GE can be calculated to be
1840 K/cm which is much more than the experimental GE. The reason
for the gap between theoretical results and experimental results may be
the neglect of the curvature undercooling (ΔTr) and kinetic under-
cooling (ΔTk) which also have an impact on the stability of planar in-
terface [15]. On the whole, it cannot reasonably explain the micro-
structure evolution behavior in Si–Y alloy by using Eqn. (2).
Based on solidification theory, it is known that the higher interface
growth temperature does the phase have, the greater undercooling will
the phase have, which can accelerate the nucleation and the interface
growth rate in the process of phase growing. Therefore, calculating and
comparing the interface growth temperature of Si phase, YSi2 phase and
eutectic structure will be conducive to reveal the competitive growth
behavior of primary phases and eutectic structure under different GE in
the directional solidification.
Therefore, the models of interface growth temperature can be used
qualitatively which has been used in Al–Si faceted system [30] and also
has been used in our previous studies on the effect of withdrawal rate
on competitive growth of Si–Y system [10].
Research by J.D. Hunt et al. [31] has shown that the interface
growth temperature of primary phase can be expressed by Eqn. (3) and
the interface growth temperature of a eutectic has been described by P.
Magnin et al. [32] as Eqn. (4).
Ti = TL − GE DL / V − [−8Гi mi C0 (1 − ki )/ DL]1/2 V 1/2, i= α,β (3)
Te = TE − (∅ + 1/ ∅)(K1 K2)1/2V 1/2 (4)
where TL is the liquidus temperature at alloy composition C0 [29], GE is
the temperature gradient, DL is diffusion coefficient in liquid which is
4.3×10−9 m2/s [10]. V is growth rate which is simplified to withdrawal
rate. Гi is Gibbs-Thomson coefficient where ГSi is 17×10−8 K m and ГYSi2
is 19.7×10−8 K m [10]; mi is slope of liquidus where mSi is 17×10−8 K m
and mYSi2 is 19.7×10−8 K m [29], ki is solute distribution coefficient
where kSi is 7.1 K/wt.% and kYSi2 is −15.2 K/wt.% [29]. TE is equili-
brium solidification temperature of eutectic, K1, K2, Ф are the constants
that have been calculated in the previous study [10] where K1 is
5.3×109 K s/m−2, K2 is 2×10−6 K m and Ф is 4.1 for this study.
By substituting each parameter [10] into Eqn. (3) and Eqn. (4), it
can be obtained that the interface growth temperature of the eutectic
structure is independent of the GE at a withdrawal rate of 1.5 mm/min,
which is a constant value TE = 1485.6 K. The relationship between the
interface growth temperature of primary phase and the GE is shown in
Eqn. (5) and Eqn. (6), the specific relationship curve is shown in Fig. 7.
TSi = 1487.3 − 1.72 × 10−4GE (5)
TYSi2 = 1486.4 − 1.72 × 10−4GE
(6)
Based on the above results, it can be concluded that the interface
growth temperatures of Si phase and YSi2 phase are negatively linearly
correlated with the GE. In addition, the interface growth temperature of
Si phase is always higher than that of YSi2 phase. Hence the Si phase
will have a higher undercooling than the YSi2 phase in directional so-
lidification, which can make it have a greater growth advantage to
grow preferentially and form the primary phase finally. This can also
explain why the primary phase is only Si phase rather than YSi2 phase.
Meanwhile two critical temperature gradients have been calculated,
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Ceramics International 45 (2019) 16776–16783
Fig. 7. Interface growth temperatures of the Si phase, YSi2 phase and eutectic
as a function of GE.
where the first GEC1 is approximately 52 K/cm when TYSi2 = TE and the
second GEC2 is approximately 111 K/cm when TSi = TE. As the re-
lationship among the actual GE, GEC1 and GEC2 changes, the micro-
structure of Si–Y eutectic alloy will alter correspondingly.
4. Discussion
Based on GEC1 and GEC2, the actual GE in directional solidification
process can be divided into three intervals, in which Si phase, YSi2
phase and eutectic structure have specific competitive growth patterns.
When GE＜GEC1, the relationship among interface growth tem-
peratures can be described as TSi＞TYSi2＞TE. The interface growth
temperature of Si phase is the highest. And it will be easy for Si to form
thick bar shaped primary phase due to the biggest growth dynamics.
When the primary Si phase is formed, Y element will be discharged to
the surrounding of Si phase. Due to the high viscosity of melt and weak
convection, there will be a tendency for Y element to concentrate at the
boundary of Si phase and to form a thick banded YSi2 phase. In the
range of low GE, the gap of interface growth temperature between Si
phase and YSi2 phase can be reduced by decreasing the withdrawal rate
so as to obtain the full eutectic structure. In our previous studies, when
the GE was 47 K/cm, as long as the withdrawal rate was reduced to
0.5 mm/min, a full eutectic structure can be obtained [10].
When GEC1＜GE＜GEC2, the relationship among interface growth
temperatures of each phase will change to TSi＞TE＞TYSi2. On the one
hand, the temperature of YSi2 phase has been already lower than that of
eutectic structure while the interface growth temperature of Si phase is
still the highest. As a result, the primary Si phase will still grow pro-
minently in most regions, meanwhile the YSi2 phase with thick banded
shape will form at the boundary of primary Si phase either. On the
other hand, the gap of interface growth temperature between the Si
phase and eutectic structure has been smaller, so the prominent growth
advantage of Si phase will be weakened. Hence, the average size of the
primary Si phase will decrease significantly, while the eutectic area will
expand and the number of eutectic structures will increase, as shown in
Fig. 8(a). This is consistent with the microstructure obtained when
GE = 90 K/cm in experiment.
When GEC2＜GE, it can be determined that TE＞TSi＞TYSi2. In this
case, the interface growth temperature of Si phase has been lower than
the coupling growth temperature of eutectic structure, so the formation
of primary Si phase will be inhibited, as shown in Fig. 8(b). However,
although the interface growth temperature of eutectic structure is the
highest, the interface growth temperature gap between eutectic struc-
ture and Si phase is still not great enough. Therefore, in actual growth
process, it will be disturbed by temperature fluctuations, component
J. Li, et al.
Fig. 8. Model of morphology at different G E: (a) GE ≪ GEC1,
GEC1＜GE＜GEC2, (c) GEC2＜GE, (d) GEC2≪ GE.
fluctuations and other disturbances, which may result in interface in-
stability and failure to form completely regular banded eutectic struc-
ture. At the same time, the interface growth temperature gap between
the Si phase and eutectic structure is larger than that between YSi2
phase and eutectic structure, especially when GE is slightly larger than
GEC2, the difference of growth advantage will be particularly obvious.
Therefore, in the process of eutectic growth, the growth dynamics of the
Si phase will be slightly higher than the YSi2, which will allow Si phase
to grow laterally and cut off YSi2 phase intermittently. This is similar to
the island shaped microstructure obtained when GE = 120 K/cm in this
paper. With the improvement of GE, there will be a larger interface
growth temperature gap between eutectic structure and Si phase, which
can cause the growth advantage of Si phase to be further weakened.
When GE increases to 160 K/cm, it has been difficult for Si phase to cut
off the growth of YSi2 phase horizontally in a large area due to the
weaker growth advantage. Only in the local area can maintain the is-
land shape because of some disturbances. Hence a reticular shaped
structure will be formed eventually, as shown in Fig. 8(c).
When GEC2≪ GE, the interface growth temperature gap between Si
phase and YSi2 phase can be negligible due to the much higher interface
growth temperature of eutectic structure. Hence it can be approxi-
mately considered that the Si phase and the YSi2 phase have the same
ability to grow both in horizontal and vertical direction. This will lead
the formation of the long strip shaped full eutectic structures composed
of strip Si and strip YSi2, as shown in Fig. 8(d). The experimental results
have shown that uniform fine strip eutectic structure with excellent
orientation can be formed when the GE reaches 200 K/cm.
By analyzing the research results in this paper and combining with
the previous research results on withdrawal rate [10], it is of great
significance to study the coupling effect of GE and withdrawal rate on
eliminating primary Si phase and controlling YSi2 phase. Based on the
interface growth temperature model, the relation curve between in-
terface growth temperature of Si/YSi2 phase and solidification condi-
tions has been made respectively as shown in Fig. 9.
It can be concluded that the first critical withdrawal rate VC1 (i.e.,
the withdrawal rate when TE = TSi) will gradually increase as GE in-
creases, as shown in Fig. 9(a). The experimental results have shown that
the first critical withdrawal rate VC1 increases from 1.51 mm/min to
Ceramics International 45 (2019) 16776–16783
2.58 mm/min as the GE increases from 90 K/cm to 200 K/cm. It in-
dicates that the higher GE may allow a faster withdrawal rate to obtain
the full eutectic structure. As for YSi2 phase, the second critical with-
drawal rate VC2 (i.e., the withdrawal rate when TE = TYSi2) will also
gradually increase from 2.47 mm/min to 4.21 mm/min as GE increases,
the value of which is nearly twice that of Si phase, as shown in Fig. 9(c).
It can be indicated the thick YSi2 phase is less likely to form than Si
phase which means the primary phase is more likely to be Si phase
rather than YSi2 phase.
In addition, the decline of interface temperature of eutectic struc-
ture will be slowed as the withdrawal rate increases. Based on this, in
the range of low GE, the gap interface growth temperature between
primary Si phase and eutectic structure will expand rapidly when the
actual withdrawal rate is greater than VC1, which will result in the
prominent growth advantage of Si phase and being easier to grow as
thick primary phase. In high GE range, when the withdrawal rate is
greater than VC1, the interface growth temperature gap between pri-
mary Si phase and eutectic structure will increase more slowly as
withdrawal rate increases. Although the primary Si phase will also be
formed, the size of the primary Si phase will decrease because the
growth dominance of Si phase has been weakened.
Furthermore, it is indicated that GEC2 (i.e., the withdrawal rate
when TE = TSi)will increase from 41 K/cm to 134 K/cm as the with-
drawal rate gradually increases from 0.5 mm/min to 2 mm/min, as
shown in Fig. 9(b) and GEC1 (i.e., the withdrawal rate when TE = TYSi2)
(b)
will increase from 32 K/cm to 63 K/cm accordingly as shown in
Fig. 9(d). At the same time, the increasing rate of GEC2 and GEC1 both
will slow down with increasing withdrawal rate where the GEC2 is al-
ways higher than GEC1 can also indicating the primary phase is more
likely to be Si phase. It has been calculated that the first critical with-
drawal rate VC1 can even reach 4.34 mm/min in the case of
GEC2 = 200 K/cm. That is to say, if the actual GE is maintained to be
greater than 200 K/cm and the actual withdrawal rate is less than
4.34 mm/min, the Si-18 at. %Y ingots with good composition uni-
formity and full eutectic structure can be obtained theoretically, which
can significantly increase the efficiency of the directional solidification
meanwhile the time cost of microstructure controlling can be saved.
5. Conclusions
In this paper, the microstructure evolution of Si–Y eutectic alloy has
been studied by Bridgeman directional solidification under different GE
combing with interface growth temperature model. The main conclu-
sions are as follows:
(1) As the GE increases from 90 K/cm to 200 K/cm, the morphology of
YSi2 phase will change from thick banded shape, to island shape, to
reticular shape and to fine strip shape. The longitudinal average
length of YSi2 phase increases from 86 μm to 325 μm, while the
lateral average size decreases from 28 μm to 7 μm.
(2) As the GE increases, the interface growth temperature of Si phase
and YSi2 phase both decrease linearly while that of eutectic mi-
crostructure is a constant value TE = 1485.6 K. The interface
growth temperature of Si phase is always higher than that of YSi2
phase, which can determine the primary phase only to be Si phase.
The formation of thick YSi2 phase is mainly caused by the enrich-
ment of Y elements at the interface of primary Si phase.
(3) By establishing interface growth temperature model, two critical
temperature gradients GEC1 = 52 K/cm and GEC2 = 111 K/cm have
been obtained. When the GE is less than GEC1, the size of the pri-
mary Si phase will significantly increase meanwhile the number of
eutectic structures will decrease. When the GE is greater than GEC1,
the size of the primary Si phase will be small and the eutectic region
will be large. When the GE is greater than GEC2, eutectic coupling
growth will take the dominant position and there is no primary Si
phase.
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J. Li, et al.
Fig. 9. Relationship between interface growth temperature of Si/YSi2 and solidification conditions: (a)(c) The relationship curves of interfacial growth temperature
and withdrawal rate under different GE, (b)(d) The relationship curves of interfacial growth temperature and GE under different withdrawal rates.
(4) The uniform eutectic microstructure could be obtained by faster
withdrawal rate under the condition of high GE. When the GE is
greater than 200 K/cm, as long as the actual withdrawal rate is less
than 4.34 mm/min, the full eutectic structure alloy with good
composition uniformity will be obtained theoretically.
Acknowledgement
The authors acknowledge the sponsor of Creative Research
Foundation of Science and Technology on Thermostructural Composite
Materials Laboratory (614291102010417).
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