The first goal of this thesis is to develop and validate a modeling tool into which fundamental combustion chemistry and aerosol dynamics theory are implemented for investigating soot formation/oxidation in multi-dimensional laminar coflow diffusion flames taking into account soot polydispersity and fractal-like aggregate structure. The second goal is to use the tool to study soot aggregate formation/oxidation in experimentally studied laminar coflow diffusion flames to advance the understanding of soot aggregate formation/oxidation mechanism. The first part of the thesis deals with the large CPU time problem when detailed models are coupled together. Using the domain decomposition method, a high performance parallel flame code is successfully developed. An advanced sectional aerosol dynamics model which can model fractal-like aggregate structure is successfully implemented into the parallel flame code. The performance of the parallel code is demonstrated through its application to the modeling of soot formation/oxidation in a laminar coflow CH4/air diffusion flame. The parallel efficiency reaches as high as 83%. The second part of the thesis numerically explores soot aggregate formation in a laminar coflow C2H4/air diffusion flame using detailed PAH-based combustion chemistry and a PAH-based soot formation/oxidation model. Compared to the measured data, flame temperature, axial velocity, C2H2 and OH concentrations, soot volume fraction, the average diameter and the number density of primary particles are reasonably well predicted. However, it is very challenging to predict effectively the average degree of particle aggregation. To do so, particle-particle and fluid-particle interactions that may cause non-unitary soot coagulation efficiency need to be considered. The original coagulation model is enhanced in this thesis to accommodate soot coagulation efficiency. Different types of soot coagulation efficiency are numerically investigated. It is found that a simple adjustment of soot coagulation efficiency from 100% to 20% provides good predictions on soot aggregate structure as well as flame properties. In the third part of the thesis, the effects of oxidation-driven soot aggregate fragmentation on aggregate structure and soot oxidation rate are studied. Three fragmentation models with different fragmentation patterns are developed and implemented into the sectional aerosol dynamics model. The implementation of oxidation-driven aggregate fragmentation significantly improves the prediction of soot aggregate structure in the soot oxidation region.

The first goal of this thesis is to develop and validate a modeling tool into which fundamental combustion chemistry and aerosol dynamics theory are implemented for investigating soot formation/oxidation in multi-dimensional laminar coflow diffusion flames taking into account soot polydispersity and fractal-like aggregate structure. The second goal is to use the tool to study soot aggregate formation/oxidation in experimentally studied laminar coflow diffusion flames to advance the understanding of soot aggregate formation/oxidation mechanism. The first part of the thesis deals with the large CPU time problem when detailed models are coupled together. Using the domain decomposition method, a high performance parallel flame code is successfully developed. An advanced sectional aerosol dynamics model which can model fractal-like aggregate structure is successfully implemented into the parallel flame code. The performance of the parallel code is demonstrated through its application to the modeling of soot formation/oxidation in a laminar coflow CH4/air diffusion flame. The parallel efficiency reaches as high as 83%. The second part of the thesis numerically explores soot aggregate formation in a laminar coflow C2H4/air diffusion flame using detailed PAH-based combustion chemistry and a PAH-based soot formation/oxidation model. Compared to the measured data, flame temperature, axial velocity, C2H2 and OH concentrations, soot volume fraction, the average diameter and the number density of primary particles are reasonably well predicted. However, it is very challenging to predict effectively the average degree of particle aggregation. To do so, particle-particle and fluid-particle interactions that may cause non-unitary soot coagulation efficiency need to be considered. The original coagulation model is enhanced in this thesis to accommodate soot coagulation efficiency. Different types of soot coagulation efficiency are numerically investigated. It is found that a simple adjustment of soot coagulation efficiency from 100% to 20% provides good predictions on soot aggregate structure as well as flame properties. In the third part of the thesis, the effects of oxidation-driven soot aggregate fragmentation on aggregate structure and soot oxidation rate are studied. Three fragmentation models with different fragmentation patterns are developed and implemented into the sectional aerosol dynamics model. The implementation of oxidation-driven aggregate fragmentation significantly improves the prediction of soot aggregate structure in the soot oxidation region.

An experimental study was performed to study soot formation and evolution in atmospheric, laminar, coflow, diffusion flames of Jet-A1, Synthetic Paraffinic Kerosene and their surrogates. Light extinction, rapid thermocouple insertion and thermophoretic sampling followed by transmission electron microscopy and atomic forced microscopy were used to obtain soot volume fraction profiles, temperature profiles and soot morphologies, respectively. Different soot evolution processes were observed on the flame centerline and on a streamline with a significantly different temperature history. Formation and agglomeration of the first soot particles are different on the two streamlines. Transparent liquid-like particles are produced in large volumes in the early regions of the flame centerline where T < 1500 K; these particles are undetectable by the extinction method with the wavelength of 632.8 nm. Most of the currently used computational soot models do not predict the liquid-like nature of nascent soot particles which has major effects on the modeling.

An experimental study was performed to study soot formation and evolution in atmospheric, laminar, coflow, diffusion flames of Jet-A1, Synthetic Paraffinic Kerosene and their surrogates. Light extinction, rapid thermocouple insertion and thermophoretic sampling followed by transmission electron microscopy and atomic forced microscopy were used to obtain soot volume fraction profiles, temperature profiles and soot morphologies, respectively. Different soot evolution processes were observed on the flame centerline and on a streamline with a significantly different temperature history. Formation and agglomeration of the first soot particles are different on the two streamlines. Transparent liquid-like particles are produced in large volumes in the early regions of the flame centerline where T < 1500 K; these particles are undetectable by the extinction method with the wavelength of 632.8 nm. Most of the currently used computational soot models do not predict the liquid-like nature of nascent soot particles which has major effects on the modeling.