Experimental and modelling study of the plasma vapour-phase synthesis of ultrafine aluminum nitride powders.

摘要

An experimental and theoretical study of the fundamentals of the vapour phase synthesis of ultrafine aluminum nitride (AIN) particles using thermal plasma was carried out. The study used the concept of a transferred-arc reactor which produces AlN ultrafine powders in two stages: evaporation of aluminum (Al) metal by the transferred-arc in non nitriding conditions; and the reaction between Al vapour and ammonia (NH₃) in a separate tubular reactor. A new version of this reactor concept was built in which the transferred-arc chamber and tubular reactor were vertically aligned. This reactor design allowed the study of both radial and axial mixing of ammonia with the plasma chamber off-gas. Ultrafine powders with a specific surface area (SSA) in the range of 38–270 m2/g were produced in two plasma chamber off-gas temperature levels (1800 and 2000 K), with different quenching intensities, and two different plasma gas compositions (pure Ar and Ar/H₂ mixture). The dependence of the particle size and composition on the reactor operating conditions was investigated. Depending on the plasma gas composition, two different trends were observed for the SSA as a function of quenching intensity, with the radial injection of NH₃. A two-dimensional numerical model was developed for the nucleation and growth of ultrafine particles in this system, using the method of moments. A new equation for the nucleation rate for the AlN system was developed. This equation considers the effect of reaction on the surface of clusters of the new phase. This new modelling approach could explain the trends observed experimentally. The importance of the mechanisms for the gas-to-condensed phase transition in the AlN system were examined. The sinterability of the powder produced was examined. Sintering to full density was achieved at 1550°C. Because of the high oxygen content of the powder, a second phase identified as aluminum oxynitride (ALON) was observed to form.