Experimental characterization of the chemical composition and structure of molecular soot precursors and soot particles in a laminar diffusion flame by coupling ToF-SIMS and Raman spectroscopy
Résumé
The transformation process in sooting flames leading to the formation of nanoparticles in the condensed phase from molecular precursors in the gas phase (soot nucleation) is not yet fully understood [1]. Information on the physical chemical properties of the nascent particles is difficult to access
experimentally but also essential for the validation of the hypotheses on soot nucleation currently being examined by the scientific community. In this work, we characterize the molecular precursors and the soot particles formed in a laminar diffusion methane flame by combining several in situ and ex situ diagnostics (fluorescence, incandescence, secondary ion mass spectrometry and Raman spectroscopy) with the goal of inferring the chemical composition and the structure of the nascent particles. The presented work highlights that several of the investigated physical chemical properties suddenly change within a narrow flame region that acquires the character of a discontinuity point correlated to the soot nucleation process. Notably, the obtained data shows evidences of the transition from flat to curved molecular structures, and the progressive apparition of finite size, sandwiched graphene like layers. Furthermore, the fraction of atomic hydrogen features a local maximum immediately upstream the detection of nascent soot particles consistent with the increasing in flame rate of C-C covalent bonds formation postulated by the major hypotheses explaining the nucleation of soot particles.
References
[1] J.W. Martin, M. Salamanca, M. Kraft, Soot inception: Carbonaceous nanoparticle formation in flames, Progress in Energy and Combustion Science. 88 (2022) 100956.
https://doi.org/10.1016/j.pecs.2021.100956.