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Introduction
A dendrite is a classic morphology of crystals during solidication, thus studying dendrite evolution is helpful to understand the essence of solidication microstructure and microsegregation. In the past decades many researchers used different methods to study dendrite evolution, such as the theoretical analysis method,14 Monte Carlo method,5 cellular automaton (CA) method,6 phase eld,7 front tracking method8 and level set method.9 Most of theoretical methods can only solve a one-dimensional problem, whereas the practical problems are always of two or three dimensions. The Monte Carlo method can predict the trend of microstructure evolution. Although the model can reect the growth kinetic of dendrite tip, it cannot correspond to real times. In the phase eld method the meshed size must be smaller than the thinnest layer of interface, which limits the calculation efciency. The front tracking method is a sharp interface approach which uses the discrete marked point to reect the interface evolution. When the microstructure grows, more and more marked points are adopted to track the interface, which increases its computational time. In addition, the front track method is difcult to deal with merging microstructures. Compared with other methods, the CA method has advantages in that it has simple rules, without limitation
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School of Material Science and Engineering, Shenyang University of Technology, Shenyang, 110023, China State Key laboratory for Fabrication and Processing of Non-ferrous Metals, General Research Institute for Non-ferrous Metals, Beijing, 100088, China *Corresponding author, email socraticliq@yahoo.com.cn.
by mesh size, and need not track the topology of the solid/liquid interface. Former researchers6,10,11 who used the CA method to simulate solidication microstructure only took account of thermal diffusion without considering solute diffusion effects. In 1997 Dilthy et al.12 presented a CA model for both thermal and solutal dendrites based on thermal and solutal diffusion controlled growth mechanism. In 1999 Nastac13 presented a model which combined thermal diffusion with solutal diffusion, and the model can simulate the columnar to equiaxed transition and show the interaction between the growing dendrites. In 2003, BeltranSanchez and Stefanescu14 modied the calculation method of the local solid/liquid interface curvature to replace the method of counting the solid fraction of the nearest neighbour cells adopted by Dilthey et al. and Nastac. 1013 In 2004, Beltran-Sanchez and Stefanescu15 introduced the front track method into the CA model that can simulate different preferential growth dendrites. All these variants of the CA method assumed that there was a sharp interface and the solid fraction in the mushy zone was obtained according to the interface position and interface velocity. However, the shape and position of dendrite morphology is unknown, which leads to the inaccurate solution of the solid fraction in the solid/liquid interface unit. In order to overcome this problem, Jacot and Rappaz combined the Thermo-Calc software with CA model to calculate the solid fraction in multicomponent alloy solidication,16 which they called the pseudofront tracking method.16 This is similar to the CA method, in which the solid fraction of the solid/ liquid interface unit is obtained by Thermo-Calc software according to the local solute concentration, temperature and curvature of the mushy zone. The
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2009 Institute of Materials, Minerals and Mining Published by Maney on behalf of the Institute Received 24 August 2008; accepted 10 November 2008 DOI 10.1179/174328109X401604
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method can simulate not only binary alloy solidication, but also multicomponent alloy solidication. The method used by Jacot presents an idea that the solid fraction of the solid/liquid interface unit can be obtained by a calculated phase diagram method. Therefore, in this paper an improved CA model is presented to calculate the solid fraction of the solid/ liquid interface unit according to calculated phase diagram, in which the exact position of the interface position is not required to be known, and the solid fraction of the interface unit can be obtained by solving a quadric equation of the solid fraction in the solid/ liquid interface unit instead of using Thermo-Calc software. The essence of the model is that if the solute concentration, temperature and the curvature of a random unit are known, then all these state parameters responding to a point in the phase diagram can be deduced. Therefore, if the state parameters of any units are known, the solid fraction can be obtained according to the phase diagram. In order to illustrate the main idea of the model, FeCSi ternary alloy is adopted in this paper.
(4)
where k1,p and k2,p are the solute partition coefcients of the different solute components, which are assumed as a constant in this article, C1,l and C2,l are the liquid solute concentration in the solid/liquid interface unit, C1,s and C2,s are the solid solute concentration in the solid/liquid interface unit, superscript 1 and 2 stand for the different solute components. According to the phase diagram, if kinetic undercooling is ignored, the relationship between the solute concentration, curvature and temperature in the solid/ liquid interface unit is given by
T ~Teq zm1 (C1,l {C1,0 )zm2 (C2,l {C2,0 ){
CK f(h,Q)
(5)
where T* is the temperature of the solid/liquid interface unit, Teq is the equilibrium temperature, m1 and m2 are the liquidus slope of components 1 and 2, which are assumed as a constant, C1,0 and C2,0 are the initial solute concentration of components 1 and 2 respectively, c is the GibbsThomson coefcient, K is the curvature of the solid/liquid interface, C1,l and C2,l are the interface solute concentration of components 1 and 2 respectively, f(h, Q) is the anisotropic function of the solid/liquid interface, h is the normal direction of the solid/liquid interface and Q is the preferential growth direction. f(h, Q) can be calculated according to Ref. 14. The curvature of the solid/liquid interface can be deduced from the formula of curvature denition14,17 K~ z (1zz2 )3=2 (6)
where z9 and z0 are the rst and second derivatives of the solid fraction respectively, and which are given z~ d y d fs =d x (fs )x ~ ~ d x d fs =d y (fs )y d y d fs =d x ~ d x d fs =d y (fs )2 (fs )yy z(fs )2 (fs )xx {2(fs )x (fs )y (fs )xy x y (fs )3 y z (1zz2 )3=2 2(fs )x (fs )y (fs )xy {(fs )2 (fs )yy {(fs )2 (fs )xx x y h i3=2 (fs )2 z(fs )2 x y (9) (8) (7)
z~ ~
K~
where fs is the solid fraction of the solid/liquid interface zone, Lh is the latent heat released per volume. Solute diffusion governing equation LCi,I (3) ~+:(Di,Ii +Ci,I ) Lt where D is the solute diffusing coefcient, the subscript I stands for the liquid or solid phase, the subscript i stands for the different solute components. When the solid/liquid interface advances, the solute will be redistributed in the solid/liquid interface unit, which can be expressed as
the subscript of x and y are the deviation of the solid fraction in x and y axis directions. Equation (1) can be divided into two parts: in the rst part, the latent heat is neglected and only the heat diffusion is considered, which can be expressed as equation (10); in the second part the heat diffusion is neglected and the latent heat is considered only, which can be expressed as equation (11)
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a t50?002 s; b t50?008 s; c t50?012 s; d t50?016 s 1 Carbon concentration eld at different solidication times
(10) (11)
where T9 is the temperature in the solid/liquid interface unit that considered the latent heat released, T is the temperature calculated by heat diffusing equation without considering the latent heat released, dfs is the increment of the solid fraction in the solid/liquid interface unit, dfs ~fsnz1 {fsn . Therefore, equation (11) can be rewritten as following T~Tz Lh nz1 (f {fsn ) Cp s (12)
average solute concentration is equal to the sum of the solid fraction multiplying the solid solute concentration, and the liquid fraction multiplying the liquid solute concentration. Therefore the average solute concentration is given as 8 fs ~0 > Ci,l < nz1 nz1 Ci ~ Ci,s fs zCi,l (1{fs ) 0vfs v1 (13) > : fs ~1 Ci,s where C is the averaging solute concentration at the (nz1)th step, the subscript l and s are corresponded to the liquid and solid phases respectively. As the solid and the liquid within these units are approximated to be of uniform composition, the liquid solute concentration in the solid/liquid interface unit can be deduced as follows Cli ~ Ci Ci ~ 1{fsnz1 zki,p :fsnz1 1{(1{ki,p ):fsnz1 (14)
where the superscript nz1 and n stand for the (nz1)th and the nth steps respectively. For these interface units there are three kinds of solute concentration for each solute component the liquid solute concentration, the solid solute concentration and the averaged solute concentration respectively. In the solid phase, the average solute concentration is equal to the solid solute concentration, and the liquid solute concentration is equal to zero; in the liquid phase the average solute concentration is equal to the liquid solute concentration, and the solid solute concentration is equal to zero; in the solid/liquid interface unit, the
Combined the Eq. (5) and Eq. (11), the following relationship can be got: T~T ~Tz L nz1 (f {fsn ) Cp s (15)
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a t50?002 s; b t50?008 s; c t50?012 s; d t50?016 s 2 Silicon solute concentration eld at different solidication times
Tz
Lh nz1 (f {fsn )~ Cp s
(18)
! C1 {C1,0 z Teq zm1 1{(1{k1,p ):fsnz1 ! C2 (16) m2 {C2,0 {CKf(h,Q) 1{(1{k2,p ):fsnz1 1{fsnz1 (1{k1,p ) 1{fsnz1 (1{k2,p ) is multiplied in both sides of equation (16), and then the following equation can be obtained 8 L n > T{Teq { Ch fs zm1 C1,0 zm2 C2,0 zCK f(h,Q){ p > > > > m C {m C > 1 1 > 2 2 2 > 3 > > L > Teq {Tz Ch fsn {m1 C1,0 {m2 C2,0 { > > p > 7 nz1 > 6 > z6 7:f > > 4 CK f(h,Q)zm1 C1 (1{k2,p )z 5 s > < m2 C2 (1{k1,p ) (17) > 2 3 > L > > T{Teq { Ch fsn zm1 C1,0 z > p > 6 > 7 > 6 > z m2 C2,0 zCK f(h,Q):(1{k1,p ):(1{k2,p )z 7:(f nz1 )2 > 4 > 5 s > > L > > (2{k1,p {k2,p ): Ch > p > > > : L z Cp :(1{k1,p ):(1{k2,p ):(fsnz1 )3 ~0 Equation (17) can be simplied as follows
where A, B, C and D are coefcients and constant, which can be expressed as 8 L > A~ Ch :(1{k1,p ):(1{k1,p ) > p > > > > B~T{Teq { Lh f n zm1 C1,0 zm2 C2,0 z > > Cp s > > > CK f(h,Q):(1{k ):(1{k )z > > 1,p 2,p > > > (2{k {k ): Lh < 1,p 2,p Cp (19) > C~Teq {Tz Lh f n {m1 C1,0 {m2 C2,0 { > > Cp s > > > > CK f(h,Q)zm1 C1 (1{k2,p )zm2 C2 (1{k1,p ) > > > > L > > D~T{Teq { Ch fsn zm1 C1,0 zm2 C2,0 z > p > > : CK f(h,Q){m1 C1 {m2 C2 where C1,0 is the initial liquid carbon concentration, and C1,050?6%; C2,0 is the initial liquid silicon concentration, and C2,050?15%. Equation (18) is a classic cubic equation, which has three roots at most. In this paper, the Newton iteration method is adopted to solve equation (18), which can be expressed as fs ~fs {y=y (20)
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a t50?002 s; b t50?008 s; c t50?012 s; d t50?019 s 3 Carbon concentration of dendrite with 45u preferential growth direction corresponding to horizontal direction
the rst order difference for fsnz1 , and y~ 3:A:(fsnz1 )2 z2:B:(fsnz1 )zC. Therefore, equation (18) has three roots at most, and the reasonable root should be satised with the relationship fsnz1 {fsn 0:2 in each time step, that is to say, in each time step, the solid fraction increment is not more than 0?2. The boundary condition and the initial conditions are given as following 8 > LT=Lt~h(T{Tsur ) < (21) T(x,y,t~0)~T0 > : C(x,y,t~0)~C0 where h is the interface heat transferring coefcient on the boundary, Tsur is the surrounding temperature, which is assumed as a constant and Tsur525uC and T0 is initial liquid temperature. In this model, the interface velocity cannot be deduced from the solid fraction because the interface shape and position is unknown. Therefore, the advancing velocity of the solid/liquid interface can be given as ! LCi,s LCi,l V ~ Di,s {Di,l (22) = Ci (1{ki,p ) Ln s Ln l The time step is an important factor affecting the calculating efciency, which can be calculated according
(23)
where Min is a function of selecting the minimum value 2 a2 a2 a2 a2 a among D1,l , D1,s , D2,l , D2,s , a and Vmax , dt is time step, Vmax a is the maximum velocity in the all solid/liquid interface unit, which can be obtained from equation (22), a is the size of the meshed grid, 1/5 means that the advancing interface cannot move over 1/5 of the meshed grid in each time step. The CA rules of nucleation and capturing are adopted as Refs. 13 and 14, and the solute diffusing equation can be solved according to Ref. 14. The calculation steps are given as follows: (i) setting the initial and boundary conditions according to equation (21) (ii) calculating the time step according to equation (23) (iii) calculating the temperature field without considering the latent heat releasing according to equation (10) (iv) calculating the solid fraction according to equation (18) (v) Bringing the new solid fraction of the solid/ liquid interface unit into equations (9), (11),
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a t50?002 s; b t50?008 s; c t50?012 s; d t50?019 s 4 Silicon concentration of dendrite with 45u preferential growth direction corresponding to horizontal direction
(14) and (22) to get the curvature, temperature solute concentration and velocity of the solid/ liquid interface unit (vi) calculating the solute concentration according to equation (3) that takes the change of the solute concentration in the solid/liquid interface unit into account (vii) restoring the variable data for each unit, such as temperature, solute concentration, curvature and solid fraction (viii) repeating the above steps until reaching the appointed calculating number. In this paper an Fe6C0?15Si ternary alloy was adopted, and the parameters used are listed in Table 1. The size of meshed grid is 161 mm, and the whole simulated zone is 0?2560?25 mm. The silicon solute diffusion coefcient in the solid and liquid phase is assumed to be the same as carbon, and the liquid slope and solute partition coefcient are selected by calculating phase software. In order to simplify the model, rst a solid seed is put into the centre of the simulated zone with a uniform temperature, whose preferred growth direction adopts 0 and 45u, respectively. Then, a stochastic nucleation model is adopted to simulate the solidication microstructure and solute microsegregation in the same solidication conditions.
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a t50?002 s; b t50?006 s; c t50?01 s; d t50?012 s 5 Carbon concentration at different solidication times
centre of the dendrite. This is caused by the low silicon solute diffusion coefcient. When the solidication time is 0?012 s, the dendrite grows continuously, and the silicon solute concentration at the tip of primary dendrite arm approaches 0?14%. When the solidication time is 0?016 s, the second dendrite arms grow and the silicon solute concentration at the edge of the primary dendrite arms is nearly 0?14%. Comparing Fig. 2 with Fig. 1, it can be seen that at the same solidication time the dendrite morphology is also same, but the silicon
Table 1 Parameters used in model
solute concentration distribution along the primary dendrite arms is much more uneven in Fig. 2 than carbon solute concentration distribution along primary dendrite arms in Fig. 1. Figure 3 indicates the carbon concentration distribution. When the solidication time is 0?002 s (Fig. 3a), carbon concentration in the solid seed is about 0?4%. When the solidication time is 0?008 s (Fig. 3b), the solid seed begins to grow and its preferential growth direction is 45u from the horizontal direction.
Density, kg m23 Heat diffusion coefficient, m2 s21 Carbon solute diffusion coefficient in liquid phase, m2 s21 Carbon solute diffusion coefficient in solid phase, m2 s21 Carbon solute partition coefficient at equilibrium condition Silicon solute diffusion coefficient in liquid phase, m2 s21 Silicon solute diffusion coefficient in solid phase, m2 s21 Silicon solute partition coefficient at equilibrium condition Latent heat, kJ kg21 Specific heat, J kg21 K21 Liquidus slope in equilibrium condition of FeC phase diagram, K/% Liquidus slope in equilibrium condition of FeSi phase diagram, K/% GibbsThomson coefficient, m K21 Melting temperature, uC Initial temperature, uC Boundary heat transfer heat coefficient, W m22 K21 *Parameters adopted from Ref. 13.
7300* 6.1E-6 2E-9* 5E-10* 0.34* 2E-9 5E-10 0.59 270* 800* 280* 217.1 1.9E-7* 1490* 1480* 1000
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a t50?002 s; b t50?006 s; c t5 0?010 s; d t50?012 s 6 Silicon concentration at different solidication times
Furthermore, the carbon concentration in the dendrite arms also increases to about 0?5%, which can be seen in Fig. 3b. When the solidication time is 0?012 s (Fig. 3c), the dendrite grows continuously and the second dendrite arms appear along the primary dendrite arms. When the solidication time is 0?019 s (Fig. 3d), the dendrite grows continuously, and the carbon concentration in the local zone approaches 0?55%. In addition, Fig. 3 shows clearly that there are more secondary dendrite arms forming along the primary dendrite arms than in Fig. 1, which leads to the solute accumulated zone forming among the dendrite arms. Figure 4 indicates the silicon concentration distribution at different solidication times. When solidication time is 0?002 s, as shown in Fig. 4a, the solid seed grows, and the silicon concentration in the solid seed is about 0?11%. When solidication time is 0?08 s (Fig. 4b), the solid seed turns into a dendrite, in which the preferential growth direction is 45u, and the silicon concentration of the dendrite increases to 0?125%. As the solidication time reaches 0?012 s (Fig. 4c), the second dendrite arms appear along the primary dendrite arms, and the silicon concentration in the primary dendrite arm is near to 0?14% and the silicon concentration among the secondary dendrite arms is more than 0?185%. At the solidication time of 0?019 s (Fig. 4d), the silicon concentration in the primary dendrite arms and the
second dendrite arms are about 0?14 and 0?125%, respectively. In addition, comparing Fig. 4 with Fig. 3, it can be seen that the morphology of dendrites is the same at the same solidication time. Figure 5 is the carbon concentration distribution at different solidication times. When the solidication time is 0?002 s, some nuclei form randomly in the under cooling liquid, as shown in Fig. 5a, and the carbon concentration in these nuclei is less than 0?45%. At a solidication time of 0?006 s (Fig. 6b), some nuclei prefer to grow parallel to the horizontal direction and others prefer to grow at 45u. When the solidication time is 0?012 s (Fig. 6d), some dendrites grow continuously until they meet one each other or reach the boundary. When the two dendrites meet, there will be a carbon enriched zone between the two primary dendrite arms, which leads to the carbon microsegregation on the grain boundary after the liquid solidies completely. Figure 6 shows silicon distribution at different solidication times, which reects the morphology evolution of solidication microstructure during solidication. At a solidication time of 0?002 s (Fig. 6a), some nuclei form randomly in the undercooled liquid, and the silicon concentration in the nuclei is about 0?11%. When the solidication time is 0?006 s (Fig. 6b), the nuclei grow, the dendritic morphology appears, and the silicon concentration in the dendrites is about 0?11%. As the
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solidication time increases, as can be seen in Fig. 6c, these dendrites grow continuously and the silicon concentration in these dendrites rises to about 0?125%. When the solidication time is 0?012 s (Fig. 6d), the dendrites grow continuously until they meet each other or they meet the boundary. From Fig. 6, it can be seen that the secondary dendrite arms are easier to grow except when the preferential growth direction is 0u.
Acknowledgements
The work was supported by Liaoning Educational Department (grant no. 05L-304), and supported by the Chinese Post Doctoral Foundation (grant no. 2008043340).
Reference
1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. B. Amar and E. A. Brener: Phys. Rev. Lett., 1993, 71, 589. E. A. Brener: Phys. Rev. Lett. 1993, 71, 3653. E. A. Brener: J. Cryst. Growth, 1996, 166, 339. G. B. McFadden, S. R. Coriell and R. F. Sekerka: J. Cryst. Growth, 2000, 208, 726. J. A. Spittle and S. G. R. Brown: Acta Met., 1989, 37, 1803. Ch. A. Gandin and M. Rappaz: Acta Met. Mater., 1993, 41, 345. A. Karma and W. J. Rappel: Phys. Rev. E, 1999, 60E, 3614. D. Juric and G. Tryggvason: J. Comput. Phys. 1996, 123, 127. Y. T. Kim, N. Goldenfeld and J. Dantzig: Phys. Rev. E, 2000, 62E, 2471. R. Sasikumar and R. Sreenivisan: Acta Mater., 1994, 42, 2381 2386. M. F. Zhu, J. M. Kim and C. P. Hong: ISIJ Int., 2001, 41, 992. U. Dilthey, V. Pavlik and T. Reichel: Proc. Conf. on Mathematical modeling of welding phenomena, (ed. H. Cerjak and H. K. D. H. Bhadesia), 85; 1997, London, The Institute of Material. L. Nastac: Acta Mater., 1999, 47, 42534262. L. Beltran-Sanchez and D. M. Stefanescu: Metall. Mater. Trans. A, 2003, 34A, 367382. L. Beltran-Sanchez and D. M. Stefanescu: Metall. Mater. Trans. A, 2004, 35A, 24712485. A. Jacot and M. Rappaz: Acta Mater., 2002, 50, 19091921. Q. Li, D. Z. Li and B. N. Qian: Int. J. Cast. Metal. Res., 2004, 17, 339. H. B. Dong and P. D. Lee: Acta Mater., 2005, 53, 659668.
Conclusions
A new model is presented to simulate dendrite evolution, solute microsegregation and solidication microstructure. The following conclusions can be drawn from the simulation results. 1. Owing to the back diffusion effect, solute concentration in the solid phase gradually increases as solidication proceeds and solute concentration at the dendrite edge is higher than at the dendrite centre. The last liquid to solidify contains the highest solute concentration. 2. Owing to the different solute partition coefcients of C and Si, as solidication proceeds, Si concentration distribution along the primary dendrite arm is more uneven than C. 3. When two dendrites meet, there is a solute enriched zone between them, which leads to the solute concentration and solidication rate decrease. 4. Side branch dendrite growth is more prevalent when the primary dendrite growth direction is not parallel to the heat diffusion direction. 5. The model can be extended for use in multicomponent alloy solidication as well as ternary alloy. This work is currently underway.
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