Heat And Mass Transfer in Reactor with Confined Plasma Jet in Nanopowder Production Processes A.V. Samokhin, A.G. Astashov, S.N. Polyakov, Yu.V. Tsvetkov, E.V. Troitskaya, N.V. Alekseev A.A. Baikov Institute of Metallurgy and Materials Science RAS, Moscow, Russia Abstract: A computational 3D CFD model of a plasma reactor based on the software package ANSYS / CFX is developed. The calculations show that sudden expansion of plasma flow into the reactor with water cooled wall provides necessary quenching of high temperature flow for the formation of nanoparticles by condensation from the gas phase. Flow in the reactor with confined plasma jet is characterized by the presence of stationary vortices in different temperature zones. The distribution of heat flux on the reactor wall was experimentally investigated using the partitioned reactor. The formation of a layer of copper nanoparticles was studied experimentally during recondensation of copper powder in a nitrogen plasma and a layer of tungsten nanoparticles during reduction of WO3 powder in a hydrogen-nitrogen plasma in the reactor of 20 kW in power. The distribution of local mass flux density of nanoparticles along the reactor has a maximum of joining region of high-temperature flow to the reactor wall reactor as well as the distribution of local energy flux density. Keywords: plasma jet, nanopowder, heat flux, mass flux, layer. 1. INTRODUCTION This research covers heat and mass transfer which takes place when nanopowders are synthesized in the thermal plasma jet in the reactor with a confined plasma jet. The plasma jet generated in the DC arc plasma torch flows into the cylindrical reactor with water-cooled walls, and the ratio of plasma nozzle and reactor diameters above 10 [1]. The chemical syntheses leading to generation of condensed products in the described reactor make possible to generate the target product in the form of nanopowders with the size of particles over 100 nm. Nanoparticles are generated in plasma reactors as the final products are condensed from the gas phase. As the plasma jet flows, after the channel suddenly expands, into the reactor volume, the high temperature jet quickly cools down. As the jet cools down lower than the condensation temperature, nanosized particles are formed as the result of condensation from the gas phase and continue to grow. As particles evolve from the generation point to exit from the reactor or transfer on its surface, their dispersion, phase, and chemical structures are changed after particles collide and interact with the gas phase. These processes are controlled by changing synthesis parameters - plasma jet composition, velocity and enthalpy, agent concentration, and reactor size. As nanoparticles are generated in the reactor, they inevitably deposit on the surface limiting the high-temperature gas-dispersion flux. Direct depositing of nanoparticles on the water-cooled surface prevent their sintering, but unlimited growth of the nanoparticles layer thickness depositing on the reactor surface brings about an increase in the temperature of this layer and subsequently nanoparticles degradation as the result of sintering, and possible changes in their phase and chemical composition. In order to obtain the final product of plasma synthesis in the form of nanopowder in which nanoparticles preserve the properties determined by conditions of their generation in the gas flux, any physical and chemical conversions in the deposited particle layer should be excluded or minimized. This is possible if the layer thickness does not exceed a specific value at which the temperature at the layer border does not exceed the specific threshold values of indicative physical and chemical processes– chemical and phase-related conversions of nanoparticles, and sintering of nanoparticles in this layer. 2. CFD MODELING A 3D computational model was designed to simulate transfer processes in the plasmachemical reactor to determine rate and temperature profiles in the reactor volume based on computational equation system solution including the Reynolds-averaged Navier-Stokes equations and thermal energy transfer equation. In order to close the equation system, additional equations for kinetic turbulence energy and dissipation rate (two-parameter k-ε turbulence model) were used. The properties of hightemperature gas were set in the local thermodynamic equilibrium approximation. The solution for the related hydrodynamic and heat problem was obtained with ANSYS/CFX 12.1 software system. mm in diameter and 600 mm in length for plasma fluxes of nitrogen and hydrogen and nitrogen mixture (22 vol.% Н2), for different values of thermal plasma enthalpy and flow rate, and plasma nozzle diameter. The experiments were carried out for the following range of parameter changes: plasma-forming gas flow rate: 0.5 – 2.0 m3STP/h, plasma jet enthalpy at the reactor entrance: 6.5 – 8 kWh/m3STP, plasma torch effective power: 6.6 – 12.3 kW. It was found that the heat flux density distribution along the reactor is not monotonous, and its maximum lies in the area where the high-temperature flow connects with the reactor wall (Figure 2). The heat flux density value is determined by the plasma torch effective power, and the maximal value exceeds by 2.5 – 3 times the heat flux density in the first and final reactor sections, and ranges from 25 kW/m2 to 45 kW/m2. The heat flux density distribution related to the maximum value stays virtually unchanged for all values of input heat power, gas flow rate, and initial gas enthalpy considered by experiments. Hydrogen contained in nitrogen brought about virtually no changes of measured values of heat fluxes in the reactor. After the plasma nozzle decreased from 10 mm to 6 mm, the area where the high-temperature flux Figure 1. Calculated values of the temperature distribution and flux lines in the plasma reactor. The rate profile computations suggest that the reactor flux is quite complicated and has stationary vortexes in various temperature zones (Fig. 1). Such vortexes are conditioned with sudden expansion of the plasma flow while enteringd into the reactor, and localized gas outlet from the reactor. The nanoparticles involved into vortex flow areas will stay longer in respective temperature zones which may considerably change their properties and in particular increase dimensions as the result of growth by coagulation 3. EXPERIMENTAL DISCUSSION RESULTS AND This research covers the heat flux density distribution on the surface of reactor sections 200 Figure 2. Heat flux density distribution to the wall along the reactor with various effective power of plasma torch and plasmaforming gas flow rate. 1 — 12.3 kW, 1.7 m3/h; 2 — 10.4 kW, 1.6 m3/h; 3 — 8.8 kW, 1.2 m3/h; 4 — 6.7 kW, 0.84 m3/h. connects with the reactor wall and consequently the heat flux maximum moved away from the reactor entrance. The experiments suggest that the reactor with confined plasma jet is characterized with considerable unevenness in distribution of the heat flux on its surface. In the area of the maximal heat flux, the processes of nanoparticles degradation forming the deposited layer are maximal. The research also covers generation of the nanosized copper particle layer as the copper powder re-condenses in the nitrogen plasma. The experiments were conducted for the following range of parameter changes: plasma-forming gas flow rate 1.3 – 1.6 m3STP/h, plasma flux enthalpy at the reactor entrance: 6.0 – 7.1 kWh/nm3, plasma torch effective power: 8 – 11 kW, copper powder flow rate 0.7 – 3 g/min. It was found that the heat flux density distribution along the reactor just as in the above-mentioned case with the flow without nanoparticles is not monotonous, and its maximum lies in the area where the hightemperature flow connects with the reactor wall. As the thickness of deposited nanoparticles layer grows, the thermal resistance of this layer increases to reduce to a certain degree the heat flux to the reactor wall. Distribution of the deposited nanoparticles flux density along the reactor just as the energy flux density distribution is not monotonous, and its Figure 3. Distribution of Cu nano-particle mass flux density to the wall along the reactor with various process durations. 1 — 5 min, 2 — 20 min. maximum lies in the area where the hightemperature flux connects with the reactor wall (Fig. 3). The longer the process is, and the greater the thickness of the deposited nano-particle layer is, the less is the mass flux of nano-particles on the wall. The mass flux density value is determined by the mass concentration of the condensed phase in the gas-nanoparticles flow, and the maximal value exceeds by 2 – 3 times the mass flux density in the first and final reactor sections. Figure 4. Distribution of Cu nano-particle specific surface along the reactor with various process duration. 1 — 20 min, 2 — 35 min, 3 — 80 min The fact that the nanoparticles mass flux density maximum lies near the point where the gasdispersed flux connects, can be explained by maximal values of turbulent pulsations in this area which bring about an increase in the turbulent transfer of particles to the reactor wall. Depending on plasma process parameters, the average size of produced copper nanoparticles ranged from 35 to 120 nm, and the local mass flux density for copper nanoparticles deposited on the reactor surface came to 3 – 8.5 g/m2 min. The average size of nanoparticles in layers depositing on various reactor sections increased as the layer thickness grew which is conditioned by an increase in the layer temperature and sintering of nanoparticles (Fig. 4). The research also covers generation of the tungsten nanoparticles layer obtained by the reduction of tungsten oxide powder WO3 in hydrogen-nitrogen plasma (22 vol.% Н2). The experiments were conducted for the following range of parameter changes: plasma-forming gas flow rate 1.5 – 1.6 m3STP/h, plasma enthalpy at the reactor entrance: 5.4 – 5.8 kWh/nm3, plasma torch effective power: 8 – 10 kW, WO3 powder flow rate 1.5 g/min. The average size of obtained tungsten nanoparticles ranged from 40 to 45 nm. It was found that the heat flux density and mass flux distribution to the wall along the reactor corresponds to that obtained during copper recondensation experiments. The local mass flux density for tungsten nanoparticles depositing on the reactor surface ranged from 2.1 to 5.1 g/m2 min. In contrast to the experiments with copper the average size of particles was unchanged in the layers depositing on various reactor sections. As the layer thickness grew, no increase in the average size of particles was noted. This is conditioned by a considerable difference in melting temperatures and consequently copper and tungsten sintering temperatures. As it was found during tungsten nanopowder heat treatment experiments, nanoparticles grow at temperatures above 600 С. With tungsten nanoparticles layer thicknesses obtained during experiments, this temperature was not reached, so there was no upsizing registered with nanoparticles. 4. CONCLUSIONS Distribution of the heat and nanoparticles mass flux density to the reactor wall is investigated in the reactor with confined plasma jet. It was found that the density distribution maximum for these fluxes along the reactor lies in the area where the high-temperature flow connects with the reactor wall. The maximal value exceeds by 2.5 – 3 times the flux densities in the first and final reactor sections. As the deposited nanoparticles layer thickness grows, the heat and mass fluxes to the reactor wall decrease. In case of nanoparticles with a relatively low melting temperature, the layer thickness and location of the deposit area has considerable effect on the average nanoparticles size. This research was conducted with support of the Russian Fundamental Research Foundation (Grants 10-03-00462-a and 11-08-00516-а). 5. REFERENCES 1. RF patent No. 2311225, 2007.
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