Kinetics of ultrafine coating of SiO2 nanoparticles, suspended in non-thermal CH4/C2H6 plasma

Capacitively coupled RF discharges in methane and ethane (1000-3000 Pa, 5-15 W/cm(3)) were used for the in-flight coating Of SiO2 nanopowders (NP) with an a-C:H layer [A. Kouprine, F. Gitzhofer, M. Boulos, A. Fridman, Polymer-like C:H thin film coating of nanopowders in capacitively coupled RF discharge, Plasma Chemistry and Plasma Processing 24 (2) (2004) 189-215]. In this present work a model of the chemical kinetics of this plasma processing has been developed, based on the GRI-Mech 3.0 mechanism [G.P. Smith, D.M. Golden, M. Frenklach, Gas Research Institute, Detailed chemical reaction mechanism. Available from: < http://www.me.berkeley.edu/ gri-mech/>], and calculations are performed, using the Chemkin-II code. The model includes the formation of two solid phases: an amorphous C:H coating, deposited on the suspended NP, and soot, incepted in the gas phase. Non-equilibrium plasma effects are taken into account by the rates of radical species' production, using the reference data on the "G-value". The CH3 and H species appear to have key roles in surface activation and the nanofilm growth. The results demonstrate the competitive character of the formation of the two solid phases: the C:H coating is dominant under T-gas < 1400-1600 K, depending on the conditions, and soot commencing to dominate at higher temperatures. This division corresponds to the passage from non-thermal plasma conditions, with the dominance of single-valent radicals and solid phase growth on the substrate only, to the plasma thermalisation with the formation of two-valent radicals and v. inception of the solid phase. The results are validated experimentally by the observation of soot formation as a function of the gas temperature, by the mass spectrograph data on the gas composition after plasma reforming, and by the reference data on coating growth rates and induction times for soot formation. (c) 2006 Elsevier Inc. All rights reserved.