Physicochemical evolution of nascent soot particles in a laminar premixed flame: from nucleation to early growth

In this work, particle inception and early growth stages were investigated in an ethylene/air premixed flame by the evolution of the particle size and structure with flame residence time. Particle size distribution was measured by a scanning mobility particle seizer and chemical-physical investigation was carried out by Raman microspectroscopy, UV-visible light absorption and cyclic voltammetry. From early inception of particles, just downstream the flame front, to the formation of primary soot particles, in the post-oxidation flame zone, particles participate in a series of chemical and physical reactions that strongly modify their nanostructure and physicochemical properties, resulting in different optical and electronic characteristics. The results presented in this study show that the evolution from a mono-modal to a bi-modal size distribution is associated to a particle graphitization process consisting of a slight increase of the in plane average size of the polyaromatic units within the particles, La, and on the formation of stacks of polyaromatic planes. These outcomes suggest that in our flame conditions particle coagulation/coalescence has a major role in the initial soot formation, affecting both physical and chemical particle properties.