NUMERICAL SIMULATION OF ACOUSTIC AGGLOMERATION OF DUST PARTICLES IN HIGH TEMPERATURE EXHAUST GAS Sergey V. Komarov and Masahiro Hirasawa Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan Phone +81-22-217-5177, email : komarov@tagen.tohoku.ac.jp A numerical simulation is made on the agglomeration of dust particles (Zn, size 0.2 to 32 m) which are exposed to a powerful standing sound wave of a certain frequency (35 to 1000 Hz). The particles are carried by a high temperature carrier gas (Ar, 100 to 900ºC) inside a vertical sonoprocessing chamber (I.D. 0.11 m, height 1.7 m) from the bottom to the top. A computer code, in which the particles agglomeration due to standing sound wave motion is modeled, is developed and implemented in the commercially available CFD software PHOENICS. The prediction the agglomeration rate is made for various particle sizes, sound frequencies and sound pressures. The computational results are compared with the experimental results obtained under the same conditions. Both the computational and experimental results show that the agglomeration rate becomes larger as the sound pressure increases. The finer are the particles in the exhaust gas, the higher must be the frequency of sound in order to remove the particles from the gas. Introduction Many metallurgical processes are accompanied by formation of large amount of dust in exhaust gas. Because the dust consists of very fine particles, treatment of such a dust-loaded gas has required costly and technically complicated equipment. At present, increasingly stringent regulation of air pollutant emission calls for further investigation in improving the efficiency of exhaust gas purification methods. The present study deals with a method of cleaning exhaust gas based on application of powerful sound waves. The method has received the name “acoustic agglomeration”. The acoustic agglomeration of dust particles has been long recognized as a method of the dust removal from exhaust gas (1,2). The first investigations on application of power sound waves to high temperature metallurgical processes were undertaken in the former Soviet Union. The obtained results revealed that sound wave is an attractive tool for the control of dust content in exhaust gas carried off from metallurgical units (3,4). However, the efficiency of acoustic agglomeration under high temperature is strongly dependent on such parameters as sound frequency, intensity, temperature, and, physical properties of the gas and dust particles. The effects of these parameters have been poorly understood yet. Several mathematical models of the acoustic agglomeration are available today, but a number of disadvantages inherent to these models prevent us to apply the models to the metallurgical processes. The followings are the main disadvantages: (1) the models consider particles to be stationary relative to the sound source: (2) the models ignore the mutual motion among the particles: (3) the models ignore temperature variations within the gas phase. The goal of the present study is to develop a mathematical model that is applicable to the prediction of the rate of agglomeration among various size of particles which are exposed to sound waves of various frequencies and intensities under conditions of variable temperature inside the sonoprocessing chamber. A part of the computed results 12 - are to be verified experimentally. Theory Particle entrainment coefficient For a better understanding of the model content, the acoustic agglomeration mechanism is briefly reviewed here. One of the main origins of acoustic agglomeration is a relative motion of two particles of different size affected by sound wave. Mednikov (5) showed that when a particle of diameter dp is exposed to a sound wave of frequency f, amplitude of the particle oscillation, Ap is differ from that of sound wave, A. The ratio of Ap to A is called “entrainment coefficient”. If the particle is small enough to obey Stokes’ law (Re < 0.1), the entrainment coefficient, can be given by the following equations. Ap p d p2 1 (1) (2) A 18 g 1 2 2 Here, (=2f) is the angular frequency, is the particle relaxation time (Eq.2) which is a function of the particle density p, diameter dp and the gas dynamic viscosity g. Figure 1 presents as a function of frequency for three particle diameters and two temperatures corresponding to those at the lower (800 ºC) and upper (20 ºC) parts of the experimental apparatus used in the present study. The three particle sizes represent a typical set of small (dp = 1 m), middle (dp = 0 10 1 8 m) and large (dp = 22 m) particles observed in the experiments. Oscillation amplitude of the smaller particle is -1 practically not different from that of sound 10 2 wave even at higher frequencies. On the other hand, drastically decreases as dp (m) T frequency increases for middle and larger -2 3 1 10 1 0 particles. Since real dust is always a mixture 20 C 2 8 0 of particles of various sizes, sound wave of a 800 C 3 22 certain frequency should force smaller -3 10 particles in oscillation, while larger particles 1 2 3 10 10 10 can remain stationary. This promotes a f (Hz) collision between the particles and their Fig.1 Frequency dependence of agglomeration. This effect is often called entrainment coefficient “orthokinetic mechanism”. In the present mathematical model, the particle agglomeration was assumed to proceed only due to the orthokinetic mechanism. Agglomeration kernel The core of the proposed mathematical model is the agglomeration kernel. An expression for the agglomeration kernel is based on the behavior of two groups of particles of different size located in sound wave. Firstly, suppose that the particles of one group are enough big for the effect of sound motion to be neglected (= 0) while the particles of the other group are enough small for their inertial motion to be neglected (= 1). In this case, all small particles, contained within a volume Va, should be collided with the big particles during one acoustic oscillation cycle. Here, Va is often referred to as “agglomeration volume”. As shown in Fig.2, the agglomeration volume is a cylinder, 22 - the radius of which is the sum of radiuses of the big and small particles (R1 and R2), and the height of which is equal to twice the amplitude, A, of the displacement of the small particle. However, in the practical cases of particle agglomeration, both the big and small particles are vibrated, i.e. 0< < 1. In this case, the collision probability is expressed as Va multiplied by 1 - 2 . The agglomeration kernel, 12, is hence given by the following equation (3), where f is the sound wave frequency. 12 2 ( R1 R2 ) 2 Af 1 2 (3) Considering the angular frequency = 2f, and also considering the amplitude of acoustic velocity in sound wave that is given by the product of A and , one can obtain another expression for the agglomeration kernel as following. 12 ( R1 R2 ) 2 U a 1 2 (4) The physical meaning of the agglomeration kernel is the frequency of collision between two particles of different sizes when the volume concentrations of the particles of the both sizes are unity. Mathematical formulation The motion of the dust containing gas within the vertically arranged sonoprocessing chamber was simulated as a non-isothermal two-phase turbulent flow. For simplification of computational procedure, the simulation was carried out in two steps. At first, the gas phase flow was simulated on the assumption that the volume fraction of particles in the gas phase was small enough so that any influence of particle presence on the gas flow and gas properties was ignored. Then, mass transfer equations of particles were solved on the assumption that the vertical component of particle velocity, Wp, was smaller than that of gas velocity by the particle terminal velocity, WT, while the velocities of gas and particles in the horizontal direction are the same. In the case of small Reynolds number (Re < 0.1), WT of a spherical particle can be determined from Eq.5. p d p2 g WT (5) 18 The following assumptions were also made: (1) all particles are spherical; (2) physical properties of gas are dependent of temperature; (3) particles are involved in the eddy motion inside the sonoprocessing chamber in the same way as the fluid particles of the gas; (4) two particles agglomerate at every collision; (5) once a particle contact to the surface of the wall or bottom of the sonoprocessing chamber, it is removed from the gas phase regardless with the temperature at the surface. The fluid equations were formulated on the basis of the standard k- model for a non-isothermal gas flow in axially symmetrical coordinates. The k- model includes the following governing equations: gas-phase mass conservation equation, gas-phase momentum equations in the r and z direction, conservation equations for the turbulent kinetic energy and its dissipation, and gas-phase energy equation. The details of the model can be found in textbooks on hydrodynamics (6). Based on the polydispersivity of dust system, the ensemble of the particle system was 32 - assumed to consist of M groups of particles of different sizes. The mass transfer equation of the particles in k-th group can be written as the following. Ck (VCk ) (WCk WT Ck ) 1 Ck Ck Deff r Deff S (6) t r z r z z k r r Equation (6) represents time and spatial variations of particle number density, Ck, of k-th group due to convection, diffusion and acoustic agglomeration (Sk). The particle effective diffusion coefficient, Deff, is defined as Deff t (7) Sct where t is the turbulent viscosity of gas, and Sct is the turbulent Schmidt number which is assumed to be unity in the present study. The source/sink term Sk represents the rate of change in the particle number density of the k-th group. Following T.L.Hoffmann(7), Sk can be given as M dCk 1 k Sk ij Ci C j Ck ik Ci (8) dt 2 i jk i 1 Here, the first term on the right side represents the “birth” of particles in k-th group due to acoustically driven collisions between particles whose size is smaller then that of particles of k-th group. The second term accounts for the “death” of particles in k-th group due to agglomeration. In the case of polydispersed system, the general agglomeration kernel, ij, is represented by the following equation for the collisions between the particles of i-th group and those of j-th group. ij ( Ri R j ) 2 U a i j ( 9) In the present study, the acoustic agglomeration is considered under the condition of standing sound wave. In the case of standing wave, the amplitude of acoustic velocity, Ua, is a function of distance, z, from the sound source and the wave number k (=/c), and is represented by U a U a ,0 cos( kz) (10) Here c is the sonic velocity, and Ua,0 is the acoustic velocity amplitude at z = 0. The commercial CFD code PHOENICS was used for the present numerical simulation. Incorporating the equations (1), (2), (5) to (10) into the code allowed predictions of the agglomeration rate for various particle sizes, sound frequencies and sound pressures. Experimental The computational domain, boundary and initial conditions were set according to the experimental conditions. Figure 3 shows main parts of the experimental setup. Since the system was axially symmetric, only the right half of the setup is presented in the figure. The working space of the experimental apparatus was comprised of three graphite tubes of 108 mm in I.D.(1) mounted inside an outer stainless steel shell (2), and a stainless steel adapter (3). The lower part of the shell was installed inside a resistance furnace (4) heating a graphite crucible (5) up to 9000C under an atmosphere of Ar. Sound waves were generated by a powerful loudspeaker (6) fixed at the top of the adapter. A perforated graphite disk (7) was placed between the lower and middle graphite tubes. The disk was served as a sound wave reflecting plate providing a formation of a standing wave in the 42 - space between the perforated disk and loudspeaker. The conditions of resonance standing wave were determined prior to the experiments. About 10 g of pure Zn was loaded into the crucible to produce Zn vapor. The vapor was carried by Ar gas (flow rate 2.6 Nl/min) and transported through the perforated disk to the lower part of the sonoprocessing chamber. Inside the sonoprocessing chamber, temperature decreases gradually from about 8000C at the disk to 400C at the loudspeaker. The temperature gradient caused condensation of Zn vapor into liquid drops and/or solid particles that were exposed to the sound wave during 5 minutes as they rose through the sonoprocessing chamber. The chamber was equipped with four side tubes A, B, C and D for dust sampling. The holes served also as a gas outlet. Two methods were used for taking the dust particle sample. The first one is the injection of the particle containing gas into a pure water bath (200 ml). Then, the particle size distribution in the suspension was analyzed with a laser particle sizer. The second sampling method is trapping the dust particles on a quartz plate (11 cm) inserted into the sonoprocessing chamber through one of the four side tubes A to D in Fig.3. The plate was placed horizontally at the center of the cross sectional area of the graphite tube. The particles trapped on the plate were analyzed with SEM for size and shape. Computational domain and boundary conditions The numerical simulation was conducted in a computational domain shown in Fig.3. The domain size was the same as the inner space of the sonoprocessing chamber. The domain was divided into non-uniform grids of 708 computational cells in the axial and radial directions, respectively. The cell size became smaller near the domain solid boundaries and gas outlet as shown in Fig.3 for the case where the gas leaves the sonoprocessing chamber through the outlet A. A complete list of the boundary conditions is presented in Table 1. A non-slip boundary condition is imposed for velocities V and W at the domain walls. The vertical Table 1. Boundary conditions P V Side wall N.s. 0 W 0 k 0 0 T T(z) Top wall N.s. 0 0 0 0 20C Inlet -gW02 0 W0 k0 0 800C Ck(k) Outlet 0 N.s. N.s. k 0 r 0 r T 0 r N.s. 52 - Ck C k 0 r C k 0 z F (%) N.s. denotes non-setting condition. component of gas velocity at the domain inlet, W0, was set to 0.0167 m/s according to the experimental condition. To determine the turbulent kinetic energy, k0, and its dissipation rate, 0, at the domain inlet, the initial level of turbulence was set at a level of 5%. The velocities at the domain outlet were computed from the pressure difference at the domain input and output (-gW02 and 0, respectively). Logarithmic wall functions were used in the calculation of the shear stress, turbulent kinetic energy, its dissipation, and the velocity components parallel to the domain boundaries. Temperatures at the domain walls and the inlet were those measured in preliminary experiments. Particular attention was given to the analysis of initial particle size distribution, Ck(k), at the domain inlet. According to the commonly accepted standpoint, two phenomena are responsible for the formation of dust particles from vapor under a temperature gradient. The first one is homogeneous nucleation of particles, and the second one is a condensation of vapor on the surface of the formed nuclei. Unfortunately, a lack of knowledge about the mechanism of these phenomena gives no way of describing the rates of particle nucleation and growth mathematically. In the present study, it was assumed that the formation of particles was finished before they enter into the sonoprocessing chamber and that the further changes in the particle size occur only due to their gravitational settling or acoustic agglomeration. Direct observation of the particles at the chamber inlet was impossible due to high temperature. However, some information on the initial particle size distribution could be retrieved from the following experimental findings. The size of the particles trapped at the levels A to D by the bubbling technique were found to obey to the lognormal distribution of Eq.(11). 100 (s s ) 2 dF 1 Without sound exp (11) ds s 2 2 s2 80 Sampling point A Here F is the cumulative distribution of 60 particles; s = log di, where di is the particle 40 diameter; s is the arithmetic mean of log d; and s is the standard deviation of log d. 20 Second finding was that the order of 0 magnitude of the size of smallest particles leaving the chamber was roughly 1 10 d (m) estimated as 10-7 m, while the order of Fig.4 Particle size cummulative distribution magnitude of the size of biggest particles in the chamber was found to be 10-5 m. Based on these findings, the minimum and maximum diameters of particles in the initial distribution were taken as 0.1 and 32 m, respectively, in the present simulation. The standard deviation was found from best-fitting curve to the experimental distribution for the sampling point A shown in Fig.4. The lognormal particle size distribution was in good agreement with the experimental observations at s = 0.2. Results and discussion Analysis of the distributions of gas velocity and temperature over the computational domain reveals that the temperature gradient along the height of the sonoprocessing chamber gives rise to buoyancy forces that drive a vigorous convection inside the chamber. Figure 5 presents velocity vector (a) and temperature (b) fields over the 62 - computational domain. For the sake of convenience, all figures showing spatial distributions of computational variables are stretched by 5 times in the radial direction relative to the vertical direction. As seen in Fig.5 (a), there is a big circulatory loop inside the chamber with the upward flow close to the chamber axis and downward flow close to the chamber walls. In the loop, the vertical component of gas velocity is increased from its initial value at the sonoprocessing chamber inlet (0.0167 m/s) by more than ten times at a distance of about 10 cm above the inlet. This results in fast change in the particle number density during about 30 seconds after the particles start entering the chamber, and then the density remains almost unchanged as the time passes. Therefore, in the followings, the discussion is based on the results of calculation at 30 s. Figures 6 to 8 are the contour plots of particle number density calculated for three typical sizes of particles; small (1 m), middle (8 m) and large (26 m), respectively. The letters a), b) and c) under the plots correspond to different computational conditions: a) without sound application, b) and c) with sound application at SPL= 158 dB and frequencies 210 (b) and 990 (c) Hz, respectively. As seen in the figures, in the absence of sound a b application, small and middle particles fill the chamber volume completely and their number densities reach very high values. At the same time, the number density of large particles is close to 0 over the volume Fig.5 Velocity vector (a) and temperature (Fig.8(a)) because the gas velocity at the (b) fields sonoprocessing chamber inlet is not high enough for the large particles to be picked up by the upward gas flow. The sound application results in a significant decrease in number density of the small and middle particles, on the one hand, and in an increase in number density of the large particles, on the other hand. However, the effect of sound on the particle number density distribution is dependent on the frequency of the sound. For relatively higher frequency ( 990 Hz ), the decrease in the number density of the small particle is especially significant (Fig.6(c)). On the other hand, relatively lower frequency (210 Hz) is more effective in reducing the number density of middle particles as it follows from a comparison of Fig7(a), (b) and (c). The results can be explained in the terms of the frequency dependence of entrainment coefficient (Fig.1) and agglomeration kernel (Eq.9). Oscillation magnitude of small particles is practically independent of frequency. However, the middle particles are oscillated with a much smaller magnitude at f = 990 Hz as compared to that at f = 210 Hz. Since the rate of collision between particles is proportional to the difference in entrainment coefficients of the particles, the rates of collision and agglomeration between smaller and bigger particles should be enhanced as the frequency increases. This explains the difference in number density distributions of small particles between at frequencies 210 and at 990 Hz. In the case of middle particles, their number density is governed by the rates of two contrary processes. The first one is the birth of the middle particles from smaller ones. 72 - The second one is the particle death due to their agglomeration with other particles and Fig.7 Number density contour of middle particles (8 m) going to another particle group as described by Eq.(8). As it follows from the above consideration, the higher frequency should enhance the particle birth rate. On the other hand, because the entrainment coefficient of middle particle at lower frequency is larger than that at higher one, the wave of 210 Hz should result in a faster rate of the middle particle death than that at 990 Hz. This is the reason why the number density of middle particles is higher at f = 990 than that at f = 210 Hz. The same explanation is applied to the behavior of the large particles. Exposing the gas that contains particle to sound wave a) b) c) resulting a) b) c) causes the particle agglomeration, Fig.6 Number density contour ofin the large particle formation in the small particles (1 m) sonoprocessing chamber. The formation rate is especially high at the lower part of the a) b) c) sonoprocessing chamber where the number Fig.8 Number density contour of density of smaller particles is large. Because large particles (26 m) the agglomeration between small and middle particles is enhanced at higher frequencies, sonoprocessing of gas by the high frequency wave (990 Hz) should result in a formation of big particles in a larger quantity than that achieved by sonoprocessing with the low frequency wave (210 Hz). Higher frequency is beneficial for the increase in the number density of the large particle also from the 82 - p (%) viewpoint of particle death rate because of the large difference in entrainment coefficients at frequencies of 210 and 990 Hz. The rate of agglomeration of a big particle with another particles of similar size should be much smaller at f =990 than that at f = 210 Hz, which assures that the death rate of the large particle is smaller at higher frequency. Thus, the numerically predicted results of the number density of differently sized particles reveal that the acoustically driven agglomeration is responsible for a change in distribution of the particle number density in such a way that the number of small particles reduces while the number of big particles increases. These results can be verified by the experiments. Figure 9 shows distribution of particle in size for two cases: a) without sonoprocessing and b) with sonoprocessing with frequency of 990 Hz. The particle samples were taken at the point A (Fig.3) with the bubbling technique. At a quick look at, it is obvious that the sonoprocessing causes a shift of the particle size distribution toward larger sizes. Here, it is noted that we could find neither small (less than or equal to1 m) nor big (larger than or equal to16 m) particles in the samples due to the inherent limitation of the particle sampling method. In the case of bubbling technique, very fine particles are carried away from the bubbler together with carrier gas flow, while very large 20 Without sound With sound, f =992 Hz particles fall down and stick SPL = 152 dB to the bottom part of the 16 sampling tube during they fly through sampling tube. 12 It is also noted that the presence of very fine and 8 large particles in the sonoprocessing chamber 4 has been confirmed by the other sampling methods. 0 d ( m) Both the predicted and 1 10 1 10 p experimental results show a Fig.9 Particle size distribution significant reduction in the total number density of particle due to the acoustic agglomeration. Figure 10 is a plot of the relative total number density of particles, N/N0, versus sound pressure at a frequency of 210 Hz. Here, N0 denotes the total number density in the absence of sound 1.0 Experiment Simulation N/N0 0.8 f = 210 Hz 0.6 0.4 0.2 0 1 2 3 Ps (kPa) Fig.10 Dependence of total relative number density of on particles sound pressure 92 - wave. As seen in the figure, the higher the sound pressure the smaller is the total number density of particles. The mechanism of particle reduction is explained as follows. The particles agglomeration induces the increase in the average size of particle in the gas phase. This results in an increase in average particle terminal velocity (Eq.5), which leads, in turn, to an enhanced precipitation of enlarged particles onto the sonoprocessing chamber bottom and thus to the decrease in total number density of particles. However, in Fig.10, the computed results predict more steep reduction in N/N0 with sound pressure than the experimental result. This result is supposedly attributed to an overestimating of agglomeration probability originated from the first and fourth assumptions in the proposed mathematical model mentioned in the previous section. Actually, non-spherical particle formed during agglomeration must have a larger drag coefficient relative to gas flow than the spherical one. If some particles do not agglomerate but rebound each other after collision, then the efficiency of acoustic agglomeration must be smaller than the present model. In these cases, the rate of agglomeration can become smaller than the calculation in the present study. The effect of various particle shapes and a coefficient of particle rebounding should be included in an improved model. Such an improvement is to be made in the next step of our investigation. Conclusions A mathematical model of the agglomeration for differently sized particles under different conditions of sonoprocessing of high temperature particle laden exhaust gas was developed and implemented in the CFD software PHOENICS. The sound frequency and sound pressure were found to be of prime importance in controlling the distribution of particles in size and their number density in exhaust gas. Generally, acoustically driven agglomeration results in the decrease in number density of fine particles and increase in number density of large particles. According to the results of numerical simulation, the finer the particles in the exhaust, the higher must be the frequency of sound in order to proceed the agglomeration between the finer and larger particles. The total number density of particles in exhaust gas is drastically decreased as the sound pressure increases. The results of model calculation agree with experimental results qualitatively well. Reference 1. 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