期刊
CHEMICAL ENGINEERING SCIENCE
卷 209, 期 -, 页码 -出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ces.2019.115209
关键词
Tetramethylsilane; Reaction mechanisms; Genetic algorithm; Flame-synthesized nanoparticles; Molecular-beam mass spectrometry; Quantum-chemical calculations
资金
- German Research Foundation (DFG) [FOR 2284, 262219004, WL 63/1, KA 3871/4, SCHU 1369/25]
Tetramethysilane (TMS) is a precursor for flame synthesis of silica (SiO2) nanoparticles. A chemical reaction mechanism was developed for the oxidation of TMS in a lean low-pressure (p approximate to 30 mbar) H-2/O-2/Ar flame using species mole fractions, obtained from molecular-beam mass spectrometry (MBMS) measurements in a matrix-supported flat flame doped with 600 ppm TMS. The thermodynamic data of Si-containing species were determined from quantum-chemical calculations at the G4 level of theory. The formation and subsequent consumption of Si(OH)(4), one of the main products of TMS oxidation, and the formation of Si4O10H4 clusters are hypothesized to be the primary pathway in the synthesis of silica nanoparticles. The reaction rate coefficients are either estimated via an algorithmic optimization procedure or are assumed based on analogies to similar reactions in the literature. The mechanism was further validated based on MBMS measurements with the same base flame doped with 400 and 800 ppm TMS. (C) 2019 Elsevier Ltd. All rights reserved.
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