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Shock-tube study of the decomposition of tetramethylsilane using gas chromatography and high-repetition-rate time-of-flight mass spectrometry.
Physical Chemistry Chemical Physics : PCCP 2018 April 26
The decomposition of tetramethylsilane was studied in shock-tube experiments in a temperature range of 1270-1580 K and pressures ranging from 1.5 to 2.3 bar behind reflected shock waves combining gas chromatography/mass spectrometry (GC/MS) and high-repetition-rate time-of-flight mass spectrometry (HRR-TOF-MS). The main observed products were methane (CH4), ethylene (C2H4), ethane (C2H6), and acetylene (C2H2). In addition, the formation of a solid deposit was observed, which was identified to consist of silicon- and carbon-containing nanoparticles. A kinetics sub-mechanism with 13 silicon species and 20 silicon-containing reactions was developed. It was combined with the USC_MechII mechanism for hydrocarbons, which was able to simulate the experimental observations. The main decomposition channel of TMS is the Si-C bond scission forming methyl (CH3) and trimethylsilyl radicals (Si(CH3)3). The rate constant for TMS decomposition is represented by the Arrhenius expression ktotal[TMS → products] = 5.9 × 1012 exp(-267 kJ mol-1/RT) s-1.
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