UC San Diego

The dissertation focuses on fundamental processes involved in the formation of carbon and manganese oxide nanoparticles by gas-to-particle conversion. A systematic approach through complementary experimental and modeling is implemented to study the evolution of flame formed particles and their dependence on flame conditions and growth environment.

Stretch stabilized stagnation flames are utilized to assess flame temperature and equivalence ratio effects for soot formed in higher-temperature regimes. This unique condition (Tf > 2100 K) results in a new combination of “young”, nucleation sized particles with a “mature” carbon structure. A significant transformation in carbon structure observed from the evolution in Raman spectra promises development of functional high-surface area sp2 carbon materials.

Particle nucleation and growth of manganese oxide nanoparticles is examined in a complementary experimental and modeling study of high temperature premixed stagnation flames. Manganese oxide nanoparticles having varying oxidation states are observed depending on the flame conditions. Analysis of the formation of MnO indicates that a thermodynamicbarrier limits nucleation.

Fundamental insights gained from simple laboratory flames inform particle formation in turbulent spray flames. The dissertation provides insight into flame spray synthesis (FSS), facilitating scaled, cost-effective, and versatile nanoparticle synthesis. FSS of carbon black is studied using coal tar distillate diluted in toluene as a carbon particle feedstock. Although the precursor is the same, this synthesis differs from conventional furnace black processes. Particles are formed directly in the flame rather than through downstream pyrolysis. Resulting carbon black particles are small but could potentially be tailored based on growth conditions.

A new diagnostic for determining chemical species information is introduced in collaboration with Argonne National Laboratory. Multi-probe optical emission spectroscopy is performed to analyze the axial evolution of manganese during FSS. “Optical Emission Spectroscopy Tool (OSAT)” is developed to enable data analysis, systematic feature recognition and axial species evolution. The axial evolution of Mn(I) through the flame provides fundamental insight such as the location of oxide formation.

This dissertation focusses on fundamental gas-to-particle conversion processes. Understanding the fundamental dependence of nanoparticles on the flame growth conditions is key towards engineering the size, structure, and morphology.