22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium Numerical prediction of growth and convective transport of Si nanoparticles around an Ar thermal plasma jet with He mixture M. Shigeta and M. Tanaka Joining and Welding Research Institute, Osaka University, Osaka, Japan Abstract: Numerical simulation using the computational method, which can express fluiddynamic features of a thermal plasma flow and steep gradients of a spatial distribution of nanoparticles, is performed to predict the effects of helium mixture on not only the plasma behaviour but also the growth and convective transport of silicon nanoparticles. Keywords: Thermal plasma jet, Helium mixture, Fluid dynamic instability, Nanoparticles 1. Introduction Thermal plasmas have been expected as a powerful tool for high-speed fabrication of nanoparticles since thermal plasmas offer a high-temperature field with steep gradients at their fringes where many small nanoparticles are generated rapidly from the material vapour [1]. The fringe of a thermal plasma flow forms eddies by fluiddynamic instability and the eddies transport the growing nanoparticles by turbulent-like convection [2]. Meanwhile, helium gas mixture in an argon plasma changes the temperature and flow field [3], which consequently affects the growth and transport of nanoparticles. In other words, the mechanism of nanoparticle formation is controllable indirectly with helium gas mixture. In this study, numerical simulation using the author’s solver [2] is carried out to predict the effects of helium mixture on not only the behaviour of a thermal plasma flow but also the growth of silicon nanoparticles convectively-transported around the plasma jet. 2. Governing equations 2.1. Thermal plasma flow Thermal plasma which is generated under atmospheric pressure is described by the thermofluid approximation with several typical assumptions: (i) the whole fluid region including plasma and non-ionized gas is in a local thermodynamic equilibrium state, (ii) the plasma is optically thin, and (iii) the thermofluid field is twodimensional axisymmetric. The governing equations are given as the conservations of mass, momentum and energy: where ρ is the density of fluid, t is the time, u is the velocity vector, p is the pressure, η is the viscosity, I is the unit matrix, h is the enthalpy, λ is the thermal conductivity, C is the specific heat at constant pressure, q rad is the radiation loss, q con is the heat generation due to condensation, and Φ is the viscous dissipation. The superscript tr means transposition. The momentum exchange with nanoparticles is negligible. The thermodynamic and transport properties which have large variations with one or two orders of magnitude are taken into account and obtained as temperature-dependent data [4]. 2.2. Simultaneous growth and transport of nanoparticles The simultaneous growth and transport of nanoparticles fabricated by thermal plasma are effectively described by aerosol dynamics with the following assumptions: (i) nanoparticles are liquid spheres, (ii) nanoparticles have a monodisperse size distribution with the mean size, (iii) electric charge effects are neglected, (iv) nanoparticle temperature is identical to the fluid temperature, and (v) material vapour is treated as an ideal gas. Extending our previous model [5] treating a growth by homogeneous nucleation, heterogeneous condensation ∂ρ (1) + ∇ ⋅ (ρ u ) = 0 , ∂t ∂u 2 r + r u ⋅ ∇u = −∇p + ∇ ⋅ η (∇u ) + (∇u )tr − (∇ ⋅ u )I , (2) ∂t 3 and r O-21-4 ∂h λ + r u ⋅ ∇h = ∇ ⋅ ∇h − qrad + qcon + Φ , ∂t C (3) Fig. 1. Computational domain. 1 Fig. 2. Instantaneous temperature fields for: (a) pure Ar, (b) Ar + He(10%). and coagulation between nanoparticles, the governing equations that also express the nanoparticles’ transport by convection, diffusion and thermophoresis are written as ρ ∂ np ∂t ρ n + ρu ⋅ ∇ p ρ n = ∇ ⋅ ρD p ∇ p ρ + J − 2 2 β 0 n 11p / 6 f 1 / 6 , np − ∇ ⋅ K thh ∇ ln T ρ f f ∂f ρ + ρu ⋅ ∇ = ∇ ⋅ ρD p ∇ ∂t ρ ρ ρ + Jg c + β 0 (nv − n s )n1p/ 3 f Fig. 3. Statistical temperature profiles on z = 60 mm: (a) averages, (b) normalized standard deviations. (4) , (5) 2/3 f − ∇ ⋅ K thh ∇ ln T ρ and ρ ∂ nv ∂t ρ n + ρu ⋅ ∇ v ρ n = ∇ ⋅ ρDv ∇ v ρ − Jg c − β 0 (nv − n s )n1p/ 3 f , (6) 2/3 where n is the number density, D is the diffusion coefficient, and T is the temperature. The subscripts p, v, and s denote particle, vapour, and saturated state, respectively. The variable f is defined as f = n p g. J is the homogeneous nucleation rate and g c is the number of monomers composing a nanoparticle in a critical state. β 0 is the parameter related to collision frequency given as [5] 3vv 4π β0 = 1/ 6 6k BTvv , mv (7) where v is the volume and m is the mass. K th is the thermophoresis coefficient. The material properties of 2 Fig. 4. Instantaneous vorticity fields for: (a) pure Ar, (b) Ar + He(10%). (Line interval = 2,000 from -12,000 to 12,000 s-1) iron are obtained from the database [6]. 3. Computational conditions and method Figure 1 shows a schematic illustration of the present computational domain. A plasma jet of pure argon or argon with 10% helium is ejected at 1.5 slm from the nozzle with the radius of 4.0 mm. The temperature at the nozzle exit is approximately 10,000 K. Silicon vapour is supplied at 0.1 g/min with the plasma jet. The computational domain is treated as a 2D axisymmetric coordinate system. The governing equations are simultaneously solved using a computational method that the author has developed [2] to express fluid-dynamic features of a thermal plasma flow and to capture steep O-21-4 Fig. 5. Instantaneous nanoparticle distributions for: (a) pure Ar, (b) Ar + He(10%). Fig. 6. Instantaneous mean diameter distributions for: (a) pure Ar, (b) Ar + He(10%). (Regions for n p < 1017 m-3 are cut off.) gradients of a spatial distribution of nanoparticles. 4. Results and discussion Figure 2 shows the instantaneous temperature fields at the same moment. Regardless of helium mixture, the high temperature fluid rolls up and the surrounding cold fluid is entrained at the plasma’s fringe due to fluid-dynamic instability, which agrees with the result observed in the experiment [7]. Because of this convective mixing, the plasma temperature decreases drastically. The Ar+He plasma jet shows relatively lower temperature than the Ar plasma jet in the downstream regions. In addition, the temperature distribution of Ar+He plasma jet looks more diffusive. These are attributable to larger heat capacity and larger thermal conductivity of helium than argon. Figure 3 shows the radial temperature profiles on z = 60 mm. In the vicinity of the jet axis (r < 7 mm), the Ar+He plasma has lower temperature averaged with data for 102 ms, whereas the standard deviation normalized by the local average temperature does not show much difference between the two cases. The both plasmas exhibit large standard deviations ranging from 0.5 to 0.7 in 7 mm < r < 24 mm. On the other hand, the Ar+He plasma shows a large standard deviation in r > 24 mm, which means that the region experiences much larger fluctuation of temperature when helium is mixed with an argon plasma jet. Figure 4 shows the instantaneous vorticity fields corresponding to Fig. 2. The both plasma jets exhibit complex structures which consist of multi-scale eddies with not only positive but also negative vorticities. Figures 5 and 6 respectively show the instantaneous distributions of the nanoparticle number density and the mean diameter, corresponding to the same moment as Fig. 2. Regardless of helium mixture, a large number of small silicon nanoparticles are found at the interface between the high-temperature plasma and cold gas because the silicon vapour transported with the plasma flow diffuses O-21-4 Fig. 7. Time-averaged nanoparticle profiles on z = 60 mm: (a) number densities, (b) mean diameters. through the interface. The generated small nanoparticles grow up by condensation and coagulation, being transported by the convective flow and their own diffusion simultaneously. Therefore, the nanoparticles farther from the jet axis tend to has larger sizes and smaller number densities. Figure 7 shows the time-averaged radial profiles of the number densities and the mean diameters on z = 60 mm. The both plasmas have the largest numbers of nanoparticles around r = 9 mm. Meanwhile, the nanoparticles farther from the jet axis tend to have larger sizes, except for the pure Ar plasma in r > 24 mm. This region showing the large difference between the pure Ar and Ar+He plasmas corresponds to the region with the 3 large difference of the standard deviations of temperatures as shown in Fig. 3. 5. Summary Numerical simulation was performed using the computational method which can express fluid-dynamic features of a thermal plasma flow and steep gradients of a spatial distribution of nanoparticles. The effects of helium mixture on not only the behaviour of a thermal plasma jet but also the growth of silicon nanoparticles convectivelytransported around the plasma were predicted numerically. 6. Acknowledgments This work was supported by Cyberscience center of Tohoku University for enhancement of the computational efficiency. 7. References [1] M. Shigeta, A.B. Murphy, J. Phys. D: Appl. Phys., 44, 174025 (2011). [2] M. Shigeta, Abst. IUMRS-ICA2014, D2-O28-003 (2014). [3] T. Sato, M. Shigeta, D. Kato, H. Nishiyama, Int. J. Thermal Sci., 40, 273 (2001). [4] M.I. Boulos, P. Fauchais, E. Pfender, Thermal plasmas Fundamentals and Applications, 1, Plenum Press, (1994). [5] V.A. Nemchinsky, M. Shigeta, Model. Sim. Mater. Sci. Eng., 20, 045017 (2012). [6] Japan Institute of Metals, Metal Data Book, Maruzen, (1993). [7] E. Pfender, J. Fincke, R. Spores, Plasma Chemistry and Plasma Processing, 11, 529 (1991). 4 O-21-4
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