Journal
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS
Volume 234, Issue 7-9, Pages 1395-1426Publisher
WALTER DE GRUYTER GMBH
DOI: 10.1515/zpch-2020-0005
Keywords
cyclosiloxanes; gas-phase kinetics; GC/MS; HRR-TOF-MS; single-pulse shock tube
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Funding
- German Research Foundation (DFG) [FOR 2284, 262219004]
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Shock-tube experiments have been performed to investigate the thermal decomposition of octamethylcyclotetrasiloxane (D4, Si4O4C8H24) and hexamethylcyclotrisiloxane (D3, Si3O3C6H18) behind reflected shock waves by gas chromatography/mass spectrometry (GC/MS) and high-repetition-rate time-of-flight mass spectrometry (HRR-TOF-MS) in a temperature range of 1160-1600 K and a pressure range of 1.3-2.6 bar. The main observed stable products were methane (CH4), ethylene (C2H4), ethane (C2H6), acetylene (C2H2) and in the case of D4 pyrolysis, also D3 was measured as a product in high concentration. A kinetics sub-mechanism accounting for the D4 and D3 gas-phase chemistry was devised, which consists of 19 reactions and 15 Si-containing species. The D4/D3 submechanism was combined with the AramcoMech 2.0 (Li et al., Proc. Combust. Inst. 2017, 36, 403-411) to describe hydrocarbon chemistry. The unimolecular rate coefficients for D4 and D3 decomposition are represented by the Arrhenius expressions k(total/D4) (T) = 2.87 x 10(13) exp(-273.2 kJ mol(-1)/RT) s(-1) and k(total/D3)(T) = 9.19 x 10(14)( )exp(-332.0 kJ mol(-1)/RT) s(-1) respectively.
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