Composites Part A 29A (1998) 595-601 8 1998 Elsevier Science Limited

ELSEVIER

PII: S1359-835X(97)00121-8

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Control of composition gradient in a metalceramic functionally graded material manufactured by the centrifugal method

Yoshimi Watanabea,*, Noboru Yamanakab and Yasuyoshi FukuiC

aDepattment of Functional Machinery and Mechanics, Shinsho University, 3-15-l Tokida, Ueda 386-8567, Japan bDepartment of Mechanical Engineering, Miyakonojo National College of Technology, 473- 1 Yoshino-cho, Miyakonojo 885-8567, Japan Department of Mechanical Engineering, Kagoshima University, l-21-40 Korimoto, Kagoshima 830-0065, Japan (Received 17 December 7336; revised 7 October 7337; accepted 4 November 19971

The motion of ceramic particles in a molten metal of a viscous liquid under a centrifugal force is numerically modeled to study the formation process of composition gradients. The simulated results are in good agreement with those of experiments that used a plaster-corundum model functionally graded material (FGM). It is found

that greater gradients are obtained in cases of thinner thickness, greater applied centrifugal forces and smaller mesh size particles. In addition, the processing of mixed mesh size particles is examined. We conclude that the use of a mixture of particle sizes is particularly useful to control the composition of metal-ceramic FGMs manufactured by the centrifugal method. 0 1998 Elsevier Science Limited. All rights reserved.
(Keywords: E. casting; C. computational modelling; centrifugal method: functionally graded material; viscous liquid)

INTRODUCTION Functionally graded materials (FGMs) are a new class of materials in which the composition and/or the microstructure varied in one specific direction -3. FGMs are of practical interest because of the wide gradation of physical and/or chemical properties that are possible. A number of FGM manufacturing methods have been proposed, including the centrifugal method previously proposed by the authors4- O. In this method, a thick-walled tube or ring is produced from a mixture of a molten metal and solid ceramics particles. The composition gradient is formed mainly from the difference in the centrifugal force produced by the difference in density between the molten metal and particles. Although the centrifugal method has the advantage of possible application to mass production, accurately controlling and understanding the distribution of particles remains a difficulty. In this study, an attempt was made to establish a procedure for controlling the composition gradient precisely. Various processing parameters, such as crucible furnace temperature, mold heating furnace temperature and velocity of mold rotation will significantly influence the composition gradient in the FGM. However, the determina* Author to whom correspondence should be addressed.

tion of temperature distribution and the solidification time during the centrifugal method by experimental techniques are very difficult, as the mold rotates at a very high speed during solidification. Moreover, estimation of the solidification time and temperature distribution during solidification through heat- and mass-transfer analysis under realistic conditions during the centrifugal method is a complex problem . Therefore, for simplicity, we will disregard the temperature distribution, and will regard the molten metal as a viscous liquid that obeys Stokes law. Then, we will be s concerned with the motion of ceramic particles in a viscous liquid under a centrifugal force. The formation process of the graded distributions of particles under a centrifugal force during FGM manufacturing can be simulated, taking size effects such as particle size or ring size into consideration. With the above in mind, the graded distributions of solid spherical particles were analyzed theoretically and visualized with the aid of computer graphics. The process of the graded composition formation under a centrifugal force can be simulated considering the movement of each spherical particle that is suspended in the viscous liquid. Mixtures consisting of plaster and corundum particles were chosen as experimental models and rings having various graded compositions were manufactured by the centrifugal method. The results of the experiment were compared

595

Gradient control in metal-ceramic

graded material: Y. Watanabe et al. opposite direction. The balance between these two forces can be expressed as
2 3

with the simulations, and the validity of the method for controlling the composition gradient was discussed.

m,$=lp,-_p,l$r ANALYTICAL AND EXPERIMENTAL PROCEDURE

Gg-3ngD,$

(2)

Materials and experiment The model material used for a metal-ceramic FGM was a mixture of plaster and corundum particles. The mixtures were cast into thick-walled rings using a steel mold of a horizontal centrifugal caster. Extensive descriptions of the centrifugal method and the model FGM have been presented elsewhere4*8- 0. Plaster was used as an alternative to molten metal and the selected particle sizes were #60 mesh (from 235 to 265 pm) and #320 mesh (from 46 to 54 pm). The average volume fraction of corundum was kept to 15 ~01% in this study. For experimental convenience it was assumed that the viscosity of plaster before solidification was constant in the case of a constant solidification period and 12 min was selected for the solidification period of the mixtures. However, the viscosity of the plaster depended on the volume of mixed water. Thus, the relation between the solidification period of mixtures and the volume of mixed water was measured by means of the Vicat apparatus prior to the experiment. The usage of the constant solidification period of mixtures as a parameter of viscosity could guarantee a constant viscosity of plaster throughout the experiments. The manufactured rings had an outer diameter of 90 mm, a length of 30 mm and thicknesses of 10, 15 and 20 mm. Three levels of centrifugal force were applied, and are characterized by G numbers of 2.1, 12.4, and 80.0. Here, the G number is the ratio of the centrifugal force to gravity and is given by the following equation: G = 2DoN2 (1)

where dxldt, d2xfdt2, m, p, g, D, and 7 are velocity, acceleration, mass, density, gravitational acceleration, particle diameter and the viscosity of the molten metal, respectively. The subscript indices and denote ceramic and metal, c m respectively. The first term of eqn (2) represents the buoyant force and the second results from the viscous drag. The moving direction of the particles due to the centrifugal force is determined by the relative values of densities: if pc > pm, particles move toward the outer periphery of the ring, and vice versa. The terms ,oc, pm, 7 and D, in eqn (2) are assumed to be time independent, and eqn (2) can be solved under the initial condition of dxldt = 0 at t = 0. The solution is $= c-$~ [l -exp( - &)I (3)

In the case of Al-Sic FGM, the terminal velocity state is reached at a very early period of the centrifugal casting. Therefore the term of exp( - 9@8Dzp,) in eqn (3) becomes much smaller than one and then vanishes. Thus, eqn (3) can be approximated by

dx -_= bc- ,dGgD:

dt

1817

(4)

It is obvious from eqn (4) that the velocity of the particles is proportional to the difference in density between particle and molten metal, to G number and to the square of the particle diameter, and it is inversely proportional to the viscosity of the molten metal. Computer simulation It is known that the viscosity of the melt increases according to the increase in number of particles in the suspension. Various equations have been proposed to predict the variation of the viscosity in the case of a relatively large volume fraction of particles13. Most useful is the Brinkmann equation14, which gives the viscosity 1 as
770

where Do is the diameter of the cast ring (m) and N is the velocity of mold rotation (s-l). As a result, FGM rings having different graded compositions were obtained from the combination of particle size, thickness and G number. Each ring was sectioned and the distribution of the corundum particles was measured along the thickness direction on a radial plane of the ring by a photographic method. The thickness direction was divided into ten regions of equal width and the number of particles in each region was counted. Since the average volume fraction of particles was known to be 15 vol%, the variation of volume fraction was calculated from the ratio of the particle numbers for each region to the sum. Fundamental equations During manufacture of thick-walled tubes or rings of metal-ceramic FGMs, the system of ceramic particles in molten metal behaves as a suspension of hard particles in a viscous liquid. Two significant forces act on each particle: the radial centrifugal force, and a viscous drag force in the

17=

l--

Vmax

>

2.5

(5)

where q. is the viscosity of the molten metal without particles, V is the particle volume fraction and V,, is the maximum packing fraction. The V,,,, varies depending on the packing condition and the theoretical value is in the range of 0.52 for the simple cubic packing to 0.74 for the close packing of spherical particles. When we manufactured the Al-Sic FGM, the maximum volume fraction of SIC particle is determined to be around 43 ~01%~. This means that a packing of the simple cubic may be optimum and V,, = 0.52 is chosen as the maximum packing fraction of the plaster-corundum system by taking account of the result of the Al-SIC system.

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The viscosity of plaster v. is kept constant in the present study and eqn (4) can be rewritten using eqn (5):

(6)
where

and

f(V)=

II/

2.5

l--

Vmax

>

For ease of computer calculation, a concept of relative time, At = Cdr. is introduced as an interval of calculation and eqn (6) is arranged as

where AX is the distance moved in unit time At for each particle. It is possible to evaluate the actual time dt if the value of the relative time is determined. The value of At = 7 X lo6 m- s- is used here because the calculated distribution pattern is unchanged even in the case of shorter At. It corresponds to dt = 0.5 s in the case of Al-Sic FGM manufactured under G = 100 where the material constants are pC = 3.15 Mg m-3, pm = 2.37 Mg rne3, and q. = 2.9 mPas. It is also possible to evaluate the viscosity of plaster q. from the comparisons between experiment and analysis if the analytical method is proper. A final consideration for the simulation is the fact that the particle diameters have a distribution range even at a fixed mesh size. This means the D, values are variable and AX given by eqn (7) will depend on the distribution shape range. We address this in our simulation by dividing the distribution range into three groups of a minimum, average and maximum particle sizes. A quarter is the minimum of 235 pm particles, another quarter is the maximum of

265 brn particles and the rest is the average of 250 pm particles in the case of #60 mesh particle. The particles of each group are initially arranged on equally divided lattice points considering the volume fraction of particles, because the results were very similar to those obtained using a more difficult Monte Carlo method. Needless to say, the centrifugal force changes as the position on the ring changes. However, in this study, since the movement in unit time of At was calculated for each particle, the computer calculation becomes troublesome while using the above condition. Therefore, for ease of computer calculation, the variation in centrifugal force was not taken into account in the simulation. In addition, since the products by the centrifugal method are rings or tubes, it is necessary to use a cylindrical coordinate space when calculating the volume fraction of the reinforcing particles. Fortunately, the error due to the substitution of a 1-D Cartesian space for a cylindrical coordinate space has the tendency to cancel the error due to assuming a constant centrifugal force. Therefore, we will assume the 1-D Cartesian space.

RESULTS

AND DISCUSSION

Particle distributions in experiment Model FGM rings are manufactured by the centrifugal method using mixtures of plaster and corundum. Typical radial planes of sectioned rings having 15 mm thickness of applied G = 2.1, 12.4 and 80.0 are shown in Figures 1 and 2 for #60 and #320 mesh particles, respectively. The standard experimental conditions are 15 ~01% of corundum and 12 min solidification period. The left and right edges of the pictures in Figures I and 2 correspond to the inner and the outer peripheries of the rings, respectively. It is found that rings manufactured by larger G value clearly show the darker contrast owing to the segregation of the corundum, which is black.

Figure 1 Micrographs of sectioned ring radial planes of 15 mm thickness containing 12.4 and 80.0. respectively

#60 mesh corundum.

The applied G number of (a). (b) and (c) are 2. I.

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Figure 2

Micrographs of sectioned ring radial planes of 15 mm thickness containing 12.4 and 80.0, respectively

#320 mesh corundum.

The applied G number of (a), (b) and (c) are 2.1,

30

(c)

G=80.0

0.0

0.2

0.4

0.6

0.8

1.0

0.0

0.2

0.4

0.6

0.8

1.0

Normalized

Thickness

Normalized

Thickness

Figure 3 The variations of corundum volume fraction measured from Figure I containing #60 mesh corundum. The applied G number of (a), (b) and (c) are 2.1, 12.4 and 80.0, respectively

Figure 4 The variations of corundum volume fraction measured from Fi,spre 2 containing #320 mesh corundum. The applied G number of (a), (b) and (c) are 2.1, 12.4 and 80.0, respectively

Particle distributions Figures 3 and 4 show the histograms of corundum volume fraction measured from Figures 1 and 2, respectively. The ring thickness is normalized, where 0.0 and 1.0 correspond to the inner and outer peripheries, respectively. It is found that the gradient of particle volume fraction increases with increase of the G number. Moreover, smaller gradients are obtained in the case of smaller particles as compared in Figures 3 and 4. For the evaluation of the thickness effect on graded composition, 10 and 20 mm thickness rings using #60 particles are manufactured under the same condition of Figure 3(b); applied G = 12.4. The histograms of corundum distributions are shown in Figure 5(a) and (b) for 10 and 20 mm thickness, respectively. From the comparisons among Figure 3(b), Figure 5(a) and 5(b), it is found that thinner ring gives the greater gradation.

in simulation

Initially, calculation is performed under the condition of 15 ~01% of #60 mesh particles for 15 mm thickness ring where particles are positioned on equally divided lattice points. Typical results of the migration distance of each particle for the relative times 5At, 20A.t and 40At are shown in Figure 6. The left and right ends of the figures correspond to the inner and outer peripheries of the ring, respectively. The particles move left to right towards the outer periphery with the relative time spent. Figure 7 shows the histograms of volume fraction in each region of Figure 6 for the quantitative comparisons. As shown in Figure 7, the gradient of particle volume fraction increases with the relative time. It should be noted here that the G number is inversely proportional to the actual time from eqn (4) and the solidification period is taken as

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constant. This means longer relative time is obtained in the case of greater applied G value and vice versa. Thus, the results of computer simulation, relating to the G number, do not contradict the experimental results. Next, we pay attention to the effect of particle sizes on the formation of graded composition. The particle distribution for #120 (from 106 pm to 125 pm) and #320 mesh particles are shown in Figure 8. The mean volume fraction of particles, the ring thickness, and the relative time are 15vol%, 15 mm, and 40At. respectively, which are the same conditions as in Figure 7(c). Thus, comparisons are made using the results of Figure 7(c) of #60 mesh particle, Figure 8(a) of #120 mesh particle and Figure 8(b) of #320 mesh

particle. The migration distance is greater in the case of larger particles and the graded distribution decreases as the particle size decreases, which shows good agreement with the experiment. Finally, simulation is done to confirm the effect of the ring thickness on the graded distribution. The conditions of mesh size. the mean volume fraction and the relative time are #60. 15 ~01% and 40At. respectively, which are also same conditions as in Figure 7(c). The results of ring thickness 10 and 20 mm are shown in Figure 9. Therefore, comparisons are made using the results of Figure 9(Lz) of 10 mm thickness, Figure 7(c) of 1.5 mm thickness and Figure 9(b) of 20 mm thickness. In this series. the gradation of particle distribution decreases as the ring thickness

40 30 % 20 ._ ; O E?i 3 2 10 0
(b) Ring Thickness; 20mm

30I20 10/ 0, 30/

1
-

(b) 20 At

30 20 10 0 0.0 0.2 0.4 0.6 0.8

8 9

20

1.0

Normalized

Thickness

ti a 10 3 e 0 u 40 E 7 9 30 20

Figure 5 The effect of ring thickness on the variations of corundum volume fraction measured using #60 mesh corundum and applied G = 12.4 for the comparison with Figure 3(b). The ring thickness of (a) and (b) are 10 and 20 mm, respectively

10 0 0.0 0.2 0.4 0.6 0.8 1.1) Normalized Thickness

Figure 7 The variations of corundum volume fractton measured from Figure 6 applying 15 ~01% of #60 mesh particles and 15 mm thickness. The relative times of (a). (b) and tc) are SAr. 20At and 4OAr. respectively, where Ar = 7 X IO6 mm SC

I0.2 Figure 6 Simulation of particle movement under the condition of 15 ~01% of ##60 mesh particles in the case of a 15 mm thickness ring. The relative times of (a), (b) and (c) are 5Ar, 20Ar and 40At. respectively. whereAt= X lOm- s-l

0.0

0.2

0.4

0.6

0.8

1.0

Normalized Figure 8 The effect of fraction simulated under 40Ar for the comparison are #I20 and #320 mesh

Thickness

nominal particle size on the variations of volume the condition of 15 ~01%. 15mm thickness and with Figure 7(c). The particle sizes of (a) and (b) particles, respectively

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increases, which also agrees with experiment. In this way, the agreement between the results obtained by computer simulation and those obtained by experiment is excellent. Some further explanation is required for the difference between experimental and simulation results near the outer surface of the ring. Although the simulation results always show a higher rate of accumulation near the outer surface of the ring than at other positions, the experimental results do not always show the same high accumulation. This difference may come from the so-called wall effect in rheology, but an alternative possibility comes from the shape of particles. Although the shape of particles is assumed to be spherical in this study, the Sic particles in the Al-Sic FGM and the corundum particles in the plastercorundum FGM are more granularly shaped than spherical. A number of studies have shown that any deviation in shape from spherical means an increase in viscosity for the same volume fraction15. The assumption of spherical particles also leads to a higher rate of accumulation near the outer surface of the ring. It must be emphasized here that despite the difference at the very outer position of the ring, the results discussed here are otherwise in good agreement with the experiments. Our assumption of constant temperature distribution and centrifugal force did not adversely affect predictions of graded distribution of particles. Therefore, it is concluded that the present simulation is a useful tool to obtain the information about the graded composition of FGMs produced by the centrifugal method.

The resultant distributions of particles are shown in Figure 10, where Figure 10(a) is the experiment of G = 12.4 and Figure 10(b) is the simulation of 40At. The volume fractions of #60 and #320 mesh particles are 11.25 and 3.75 vol%, respectively, and the ring thickness is 15 mm. In Figure 10, both distribution profiles are almost the same and smoother compared with those in Figure 3(b), Figure 4(b), Figure 7(c) and Figure 8(b). As mentioned previously, the migration distance per unit time of #320 mesh particles (smaller particles) is shorter than that of #60 mesh particles (larger particles). The particle-free region in Figure 10 is consequently shorter in comparison with that in Figure 3(b) or Figure 7(c). This means that the gradation in composition can be controlled not only by changing the G number or the mean volume fraction of particles but also by applying particles of different mesh size simultaneously.

3 p

QJ 40 30

Cb) Rii

Thickness; 20mm

Control of composition

gradient
0.0 0.2 0.4 0.6 0.8 1.0

The composition gradient formed by the centrifugal method can be affected by the difference in density between particles and a molten metal, the applied G number, the particle size, the viscosity of the melt, the mean volume fraction of particles, the thickness of the manufactured ring and the solidification time. It is obvious that both density and viscosity are the materials constants and both the volume fraction and thickness are the constants of the products. Moreover, applied G number and solidification time show a mutual relation and the effect has already been mentioned. One of the easily changeable and hopeful parameters for the control of the graded composition is the particle size judging from eqn (6) and the simulated results. Therefore, the composition gradient may be controlled precisely by using particles of different mesh size simultaneously. This idea was examined by both experimental and computer simulation of model materials containing both #60 and #320 mesh particles*.

Normalized

Thickness

Figure 9 The effect of ring thickness on the variations of volume fraction simulated under the condition of 15 ~01% of #60 mesh particles and 40At for the comparison with Figure 7(c). The ring thickness of (a) and(b) are 10 and 20 mm, respectively

*The effect of mix of different particle sizes on suspension viscosity has been studied by Farris16. When the particle size ratio is 5:l (in this study, larger particle size (#60) and smaller particle size (#320) are 250 pm and 50 pm, respectively), the suspension viscosity is strongly affected by the friction of smaller particles at a total particles volume of more than 50%. However, the effect is small at a total particle volume of less than 30%. Since this is true in all but one of our cases, we can safely estimate the viscosity in binary particle size systems by eqn (5), which applies for single particle size systems.

0.0

0.2

0.4

0.6

0.8

1.0

Normalized

Thickness

Figure 10 The effect of mix of different mesh particles on the variations of volume fraction under the condition of 11.25 ~01% of #60 mesh particles and 3.75 ~01% of #320 mesh particles and 15 mm thickness. (a) Experiment of the applied G = 12.4. (b) The simulation of 40At

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SUMMARY In the present study, the movement of solid particles in viscous liquid was examined to establish a method of controlling composition in functionally graded materials (FGMs) manufactured by the centrifugal method. The graded distributions of spherical ceramic particles were analyzed by a computer simulation. The graded distribution in FGMs manufactured by the centrifugal method will be significantly influenced by many processing parameters. which include the difference in density between particles and molten metal, the applied G number, the particle size, the viscosity of the molten metal, the mean volume fraction of particles, the ring thickness and the solidification time. The results of computer simulation did not contradict the experiment using the mixture of plaster and corundum. Moreover, it is shown that the composition gradation can be controlled more precisely using the mixed particles of different mesh size simultaneously. The computer simulation is useful to predict the graded composition of the products manufactured by the centrifugal method.

work described in this study was performed by Mr Y. Takeda, graduate school student of Kagoshima University.

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2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13.

ACKNOWLEDGEMENTS The authors would like to express their thanks to Prof. K. Kume of Kagoshima University for his helpful guidance and advice in using a Vicat apparatus. Part of the experimental
14. 15. 16.

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