Experimental investigation of silane combustion and particle nucleation using a rapid-compression facility

Abstract Ignition and reaction kinetics of silane/oxygen/diluent (SiH 4 /O 2 /Ar/N 2 ) mixtures have been studied using a rapid compression facility (RCF). Time-resolved pressure profiles and absolute, quantitative hydroxyl radical mole fraction ( χ OH ) time histories were obtained for a range of conditions representing different heating rates. At the moderate temperatures studied (∼630 K), ignition was observed to occur in two stages with no OH detected during the first stage. The separation of the two stages was typically >5 ms, thus the long test times provided by the RCF were critical to the studies. The second stage of reaction is identified by significant production of OH ( χ OH  = 45–82 ppm). Experimental uncertainty in χ OH was 32/−29% with a 15 ppm detectivity limit. The results were examined in the context of proposed silane combustion and particle nucleation reaction mechanisms. Existing silane combustion kinetics mechanisms capture many of the experimentally observed features of the system, yet fail to quantitatively reproduce the OH time histories in their entirety.

[1]  M. Koshi,et al.  Measurements of the absolute concentrations of hydrogen atom and hydroxyl produced in the silyl + oxygen reaction: determination of the product branching ratios , 1993 .

[2]  S. Kondo,et al.  Experimental study of spontaneous ignition limit of oxygen-lean silane mixtures , 1994 .

[3]  Bradley T. Zigler,et al.  Demonstration of a Free-Piston Rapid Compression Facility for the Study of High Temperature Combustion Phenomena , 2004 .

[4]  M. Donovan,et al.  An experimental investigation of gas-phase combustion synthesis of SiO2 nanoparticles using a multi-element diffusion flame burner , 2002 .

[5]  Sadashige Horiguchi,et al.  Premixed silaneoxygennitrogen flames , 1990 .

[6]  H. G. Semerjian,et al.  Simulation of ceramic particle formation: Comparison with in‐situ measurements , 1989 .

[7]  H. Schlegel,et al.  Ab Initio Study of the Initial Reactions in Silane Combustion: SiH3 + O2 .fwdarw. Products , 1994 .

[8]  M. Wooldridge,et al.  Computational modeling of the SiH3+O2 reaction and silane combustion , 2004 .

[9]  J. Katz,et al.  Silica particle synthesis in a counterflow diffusion flame reactor , 1989 .

[10]  M. Swihart,et al.  Numerical Modeling of Gas‐Phase Nucleation and Particle Growth during Chemical Vapor Deposition of Silicon , 2000 .

[11]  G. G. Stokes "J." , 1890, The New Yale Book of Quotations.

[12]  S. Kondo,et al.  A Numerical Study of Low Temperature Silane Combustion , 2000 .

[13]  H. O'neal,et al.  Stoichiometry and possible mechanism of SiH4O2 explosions , 1987 .

[14]  M. Zachariah,et al.  Modeling particle formation during low-pressure silane oxidation: Detailed chemical kinetics and aerosol dynamics , 2001 .