Hexamethyldisiloxane pyrolysis: Probing H-atom initiation by femtosecond two-photon LIF

Previous experiments have led to the hypothesis that pyrolysis of silica nanoparticle precursors carried in an inert central gas jet surrounded by a laminar flame is initiated not by thermal decomposition (the measured jet temperatures are too low for pyrolysis), but by reactions with H-atoms diffus...

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Veröffentlicht in:Proceedings of the Combustion Institute 2024, Vol.40 (1-4), p.105640, Article 105640
Hauptverfasser: Kim, Keunsoo, Hay, Matthew, Meng, Qinghui, Wooldridge, Margaret S., Kulatilaka, Waruna D., Tranter, Robert S.
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Sprache:eng
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Zusammenfassung:Previous experiments have led to the hypothesis that pyrolysis of silica nanoparticle precursors carried in an inert central gas jet surrounded by a laminar flame is initiated not by thermal decomposition (the measured jet temperatures are too low for pyrolysis), but by reactions with H-atoms diffusing from the surrounding flame into the jet. The current work tests this hypothesis using femtosecond two-photon laser-induced fluorescence (fs-TPLIF) to image H-atom concentrations in the same flame configuration as the previous experiments. Methane flames (ϕ = 0.83, 1.01 and 1.13) were generated using a multi-element diffusion (Hencken) burner equipped with a central tube through which the N2 jet was introduced. The fs-TPLIF line imaging showed significant concentrations of H-atoms in the nitrogen jets at heights above the burner (HAB) close to the methane flame front. The measurements indicate radial diffusion of the H atoms from the flame to the jet is significant. The H-atom concentrations in the jet increased with increasing stoichiometry of the methane flame. Additional experiments were performed with hexamethyldisiloxane entrained in the central jet flow. In each case, a diffusion flame producing silica nanoparticles was established at the boundaries between the central jet and the methane flames. The 2D H-atom images showed a transition from over-ventilated diffusion flames to under-ventilated diffusion flames with increasing equivalence ratio. Furthermore, the fs-TPLIF profiles show a significant production of H-atoms within the jet when the surrounding flame is lean. This knowledge contributes to a deeper understanding of the underlying mechanisms governing these synthesis flame systems and opens avenues for advancing silica nanoparticle synthesis techniques.
ISSN:1540-7489
DOI:10.1016/j.proci.2024.105640