Spherical diffusion flames have several unique characteristics that make them attractive from experimental and theoretical perspectives. They can be modeled with one spatial dimension, which frees computational resources for detailed chemistry, transport, and radiative loss models. This dissertation is a numerical study of two classes of spherical diffusion flames: hydrogen micro-diffusion flames, emphasizing kinetic extinction, and ethylene diffusion flames, emphasizing sooting limits. The flames were modeled using a one-dimensional, time-accurate diffusion flame code with detailed chemistry and transport. Radiative losses from products were modeled using a detailed absorption/emission statistical narrow band model and the discrete ordinates method. During this work the code has been enhanced by the implementation of a soot formation/oxidation model using the method of moments.

Hydrogen micro-diffusion flames were studied experimentally and numerically. The experiments involved gas jets of hydrogen. At their quenching limits, these flames had heat release rates of 0.46 and 0.25 W in air and in oxygen, respectively. These are the weakest flames ever observed. The modeling results confirmed the quenching limits and revealed high rates of reactant leakage near the limits. The effects of the burner size and mass flow rate were predicted to have a significant impact on the flame chemistry and species distribution profiles, favoring kinetic extinction.

Spherical ethylene diffusion flames at their sooting limits were also examined. Seventeen normal and inverse spherical flames were considered. Initially sooty, these flames were experimentally observed to reach their sooting limits 2 s after ignition. Structure of the flames at 2 s was considered, with an emphasis on the relationships among local temperature, carbon to oxygen atom ratio (C/O), and scalar dissipation rate. A critical C/O ratio was identified, along with two different sooting limit regimes. Diffusion flames with local scalar dissipation rates below 2 s^-1 were found to have temperatures near 1410 K at the location of the critical C/O ratio, whereas flames with greater local scalar dissipation rate exhibited increased temperatures.

The present work sheds light on important combustion phenomenon related to flame extinction and soot formation. Applications to energy efficiency, pollutant reduction, and fire safety are expected.