22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium Transport properties of helium plasma at atmospheric pressure A. Mahfouf1, P. André1, G. Faure1 and M.-F. Elchinger2 1 Blaise Pascal University, LAEPT, Clermont Ferrand, 24 avenue des Landais, FR-63171 Aubière, France 2 Limoges University, SPCTS, CNRS, 123 avenue Albert Thomas, FR-87060 Limoges, France Abstract: Transport properties of thermal helium plasma used generally in blown plasma jet for spray process were calculated according to the Chapman-Enskog theory. The electrical conductivity, the viscosity, the thermal conductivity and combined diffusion coefficients are computed from room temperature up to 50000 K at different pressures assuming local thermodynamic equilibrium. The plasma composition is calculated using the Gibbs energy minimization method. The helium neutrals, electrons, singly and doubly ionized helium species have been taken into account in our calculations. Keywords: transport coefficients, helium plasma, viscosity, thermal conductivity, electrical conductivity 1. Introduction The knowledge of transport coefficients is an essential prerequisite for numerical simulation of thermal plasmas. Many industrials applications that use the helium plasma as spraying process [1] need accurate computation at high temperature. The estimation of transport coefficients (viscosity, thermal conductivity, electrical conductivity and diffusion coefficient) is very difficult to do experimentally at high temperature, thus the theoretical/numerical calculation is the preferred method. Two approaches solutions of the Boltzmann integro-differential equation have been proposed by Grad [2] and Chapman-Enskog [3] using the analysis of rigorous kinetic theory. The first is called Grad's moment method, the second Chapman-Enskog method. This last is the most commonly used to calculate transport coefficients. We opted for it in this paper. 2. Collision Integrals The transport of matter, momentum and energy is essentially due to the collision between particles and the existing force fields. The study of interparticular interaction is crucial to understand the phenomena of transport. In the microscopic world, the notion of collision between atoms or molecules is interpreted as an interaction between the forces associated with each of the interacting particles. Throughout this paper we suppose that the plasma is in low-density, thus we can neglect the three-body interaction and take into account only elastic collisions. 2.1. Binary collision We consider an elastic collision between two particles having masses m and M, separated by a distance r. b, r min represent the impact parameter and the distance of closest approach between the colliding particles, respectively. The angle of deflection χ is defined by the following equation: P-I-1-10 ∞ χ (b, E ) = π − 2b ∫r min dr r2 v(r ) b 2 − 2 1− E r (1) E is the total energy of the system of particles m and M. v(r) is the interaction potential between particles and is the most interesting parameter for the study of the collision problem [2]. 2.2. Interaction potential energy There are many forms of interaction potentials energy to describe the same interaction, therefore, it is hard to choose the good potential for a given interaction. However one can select it according to the nature of the interaction force (repulsive or attractive). We can show in following examples some types of interactions that can be found in thermal plasma: a. Charged ↔ Charged: This interaction is governed by the Coulomb interaction potential [4], but according to the assumption of quasi-neutrality of the plasma [5], a shielding effect must be taken into account. Consequently this binary interaction will be described by a Coulomb potential shielded at the Debye length λD [5]: V ( r ) = ±V0 with: V0 = qe λD r −r exp λD (2) 2 4πe 0 λ D A sign ( ± ) depends on the sign of the particle charge (electron-ion). The different formulas of Debye length are discussed in is discussed in [12]. b. Neutral ↔ Neutral: There are a lot of interaction potentials susceptible to describe this interaction, such as Lennard-Jones potential, Morse potential, Buckingham 1 Potential and others. We have opted for the HulbertHirschfelder potential energy curve to describe this collision because it depends only on the spectroscopic constants [4]. c. Neutral ↔ Charged: The collision between the neutral and the ion can be studied using the same interaction as neutral-neutral. d. Neutral ↔ Electron: In most cases, it is necessary to fit experimental data in order to find an adequate potential for this interaction. 2.3. Collision cross-section In the case of the elastic collision, one can define the total collision cross-section Q(E) as: ∞ Q ( E ) = 2π ∫ (1 − χoσ( χ ) ).bdb 0 π (3) χ γ ∞ ∫e −( γ ) 2 (γ ) 2 s +3 Q ( E ) dγ (7) 0 = E/kT and Q(E) is seen in the previous section. , are the orders of approximation, k is the Boltzmann constant and µ the reduced mass of the colliding particles. 3.2. Viscosity The viscosity η ( kg.m s ) is the transport coefficient related to gradient in velocity expressed as follows: 1 1 (4) is defined in Eq.(1). <Ω ( 2, 2 ) (T ) > (8) J = −α∇ϕ (5) where J the flux vector is appropriate to quantity ϕ , and α is a proportionality constant known as the transport coefficient. The negative sign applies because the quantity is transported from regions of high concentration to regions of low concentration. 3.1. Coefficient of self-diffusion In the case of gradient in concentration, the transport coefficient is called the diffusion coefficient D (m.2s-1). Chapman-Enskog have formulated all transport coefficients, Eq.(6), Eq.(8) and Eq.(9), in term of collision integrals [2], [3], Eq.(7), the coefficient of self-diffusion of pure gas was formulated in a first approximation as follows: T3 D (T ) = 2.628 × 10 −7 M The flux correspondent is the viscous stress tensor [1]. 3.3 Thermal conductivity In the case of gradient in temperature, the quantity ϕ transported is the energy which is related to heat flux vector Eq.(5) through the thermal conductivity κ ( J .m −1 .s −1 .K −1 ) 3. Transport Coefficients of Pure Gases Gradient in concentration, velocity and temperature, causes a net transport or a net displacement of mass, momentum, and energy, respectively [5]. We can formulate mathematically this notion of transport as general form of a flux: 1 2 1 (6) (1,1) (T ) > < pΩ where M, p and T are the molecular weight of the particle, the pressure in atmosphere and temperature in Kelvin, 2 with kT 2πµ is the differential scattering cross-section: b db σ (χ , E) = σin( χ ) dχ and Ω ,s (T ) = 2 η (T ) = 2.6693 × 10 −6 (MT )2 0 σ (χ , E) (1,1) −1 −1 = 2π ∫ (1 − χoσ( χ ) ).σ ( χ , E ) σin( χ ) dχ with o respectively. < Ω ( A ) > is the reduced diffusion collision integral and is was formulated by Hirschfelder [2] as: expressed as: 1 1 T 2 (9) κ (T ) = 8.3227 × 10 ( 2, 2 ) (T ) > M <Ω −5 We remark that all transport coefficients Eq.(6), Eq.(8) and Eq.(9) are expressed in function of so called collision integrals see the Eq.(7), and the integral collision is function of collision cross section see the Eq.(3) which is itself function of angle of deflection see the Eq.(1). In summary, to compute the coefficients returns to evaluate efficiently three integrals which are included one into the other one. We have developed a numerical program which compute the three integrals in same time using the Clenshaw-Curtis quadrature [6] and we have successfully eliminated the singularities [7] that occur in collision cross section. Our program has been used to calculate the transport coefficients of the helium gas for temperature below 10000 K, the results in Table 1 are compared with those of literature [8] and they are in good agreement. Only helium neutrals have been taken into account up to this temperature (10000 K). 4. Plasma Equilibrium Compositions At high temperature (T > 10000 K) we have to take account all interactions which may occur between neutrals (He), ions (He+, He++) and electrons (e-). To determine the proportion of each species in the helium plasma at each temperature we have computed the equilibrium compositions of dissociated and ionized helium for different pressures using the Gibbs energy P-I-1-10 Table 1. Variation of transport coefficients of helium gas with temperature. T (K) 300 500 1000 2000 4000 5000 7000 10000 η κ (10-3.W.m-1.K-1) 154.904 221.117 363.106 606.99 1036.420 1237.182 1626.459 2188.097 (10-6.Pa.s) 19.885 28.276 46.613 77.922 133.049 158.822 208.795 280.895 show the temperature dependence of the electrical conductivity of helium plasma in Fig. 2. D (10-4.m2.s-1) 1.705 4.101 13.661 46.349 160.755 241.290 447.861 865.839 minimisation method [9]. Fig. 1 presents the variations of the helium plasma compositions as a function of temperature for different pressures. Fig. 2. Evolution of electrical conductivity of partially helium plasma with temperature for different pressures. The electrical conductivity depends only on transport of electrons and our results are in good agreement with those in ref [11] at one atmosphere. 5.2. Thermal conductivity We have considered only translational thermal conductivity of heavy species λ tr and electrons λ tr , than reactive and internal thermal conductivity have not been taken into account in the present calculation. These two coefficients were calculated by using the third approximation of the Chapman-Enskog method for the electron component Eq. (12) and the first approximation for heavy components Eq. (11): h Fig. 1. Mole fractions of different species in helium plasmas at different pressures. 5. Transport Coefficients of Multicomponent Mixture Viscosity, thermal conductivity and electrical conductivity of thermal helium plasma are computed on basis of the pre-calculated equilibrium plasma compositions. 5.1. Electrical conductivity Devoto [10] has developed analytical expressions of electrical conductivity for partially ionized gas as function of collision transport cross-section. We have calculated the electrical conductivity of helium plasma using the third approximation of Devoto method, and the expression is given by: 𝜎= 3 𝑒 2 𝑛𝑒2 2 � 2𝜋 𝑚𝑒 𝐾𝐾 � 1� 2 𝑞 11 𝑞 12 � � 12 𝑞 𝑞 22 𝑞 00 𝑞 01 𝑞 02 �𝑞 01 𝑞 11 𝑞 12 � 𝑞 02 𝑞 12 𝑞 22 (10) λtrh L11 Lv1 x = 1 L11 Lv1 L1v x1 Lvv xv xv 0 L1v Lvv 2πk T 75 λ = ne k B B e 8 me e tr e 1 2 (11) q 22 ( ) q 11 q 22 − q 12 2 (12) The element of matrix L ij can be found in ref [2] which are function of collision integrals Eq.(7) and the elements x i correspond to the mole fraction of each species (He, He+, He++ and e-). The elements qij are given in ref [9]. Fig. 3 shows the temperature dependence of the translational thermal and electron thermal conductivity in helium plasma for different pressures. where the elements of determinant qij are given in [10] and they are function of collision cross-section. We can P-I-1-10 3 Fig. 4. Evolution of Viscosity of partially helium plasma with temperature for different pressures. Fig. 3. Evolution of heavy translational thermal conductivity (top) and electron thermal conductivity (bottom) of partially helium plasma with temperature for different pressures. 5.3. Viscosity The contribution of electron to the viscosity is negligible than only heavy species contribute to the total viscosity. Chapman-Enskog method have been used in the first approximation to evaluate the viscosity: H1v x1 H vv xv x xv 0 η =− 1 H11 H1v H v1 H vv H11 H v1 (13) 7. References [1] M. Vardelle. J. Thermal Spray Technol., 10, 2 (2001) [2] J.O. Hirschfelder. Molecular theory of gases and liquids. (Wiley) (1954) [3] S. Chapman and T.G. Cowling. The Mathematical Theory of Non-uniform Gases. (Cambridge: Cambridge University Press) (1970) [4] J.C. Rainwater. J. Chem. Phys., 77, 1 (1982) [5] G.B. Benson. Massachusetts Institute of Technology. (1996) [6] L.D. Higgins and F.J. Smith. Molecular Phys., 14, 4 (1968) [7] A. Mahfouf, P. André and G. Faure. in: 9th Int. Student Conf. on Advanced Science and Technology. (Clermont-Ferrand) 27 (2014) [8] M. J. Slaman and R.A. Aziz. Int. J. Thermophys., 12, 5 (1991) [9] F. Bendjebbar and P. André. Plasma Sources Sci. Technol., 14, 8 (2012) [10] R.S. Devoto. Phys. Fluids, 10, 2105 (1967) [11] R.S. Devoto. J. Plasma Phys., 2, 1 (1968) [12] P. André, G. Faure, S. Lalléchère and A. Mahfouf. in: 17th Int. Symp. on Electro Magnetic Compatibility. (Clermont-Ferrand) 18 (2014) The element of matrix H ij can be found in ref [2] which are function of collision integrals Eq.(7). Fig. 4 shows the temperature dependence of the viscosity in helium plasma for different pressures. 6. Conclusion Viscosity, thermal conductivity, and electrical conductivity were computed successfully for the equilibrium helium plasma, and the results can be used as input data for the reliable numerical simulation of thermal plasmas. 4 P-I-1-10
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