Date of Completion

6-21-2016

Embargo Period

6-21-2016

Major Advisor

Prof. Chih-Jen Sung

Associate Advisor

Prof. Michael Renfro

Associate Advisor

Prof. Baki Cetegen

Field of Study

Mechanical Engineering

Open Access

Open Access

Abstract

Due to the complexity of the fluid dynamics and non-linear reactions in the combustion zone, a simplified approach to study this process is required. Given these complexities, it is practically very challenging to take measurements in very high temperature and pressure zones in practical combustion systems, and if by any means those measurements can be made, it is equally challenging to analyze those measurements. Hence, in order to more comprehensively understand these processes, the problem needs to be resolved into the smaller and controllable sub-category of experiments, by creating laminar flamelets. One approach used in creating these flamelets is by establishing simplified non-premixed flames in the counterflow configuration. Alongwith all the fundamental properties of combustion, it is important to study the health hazard and environmentally detrimental emissions, such as soot and polycyclic aromatic hydrocarbons (PAHs). Such combustion studies need to be carried out using the non-intrusive in-situ optical diagnostics measurement techniques, such as the Laser Induced Incandescence (LII), Planar Laser Induced Fluorescence (PLIF) and Light Extinction (LE). These measurements for renewable biofuels aid in better understanding of the soot formation process, as well as in developing the fuel specific knowledge to bring them into commercial use. Furthermore since the most practical combustion systems operate at elevated pressures, it is also important to understand the soot formation process under elevated pressure conditions. Considering these, in the current study, the soot and PAH formation processes for butane and butanol isomers (C4 fuels) at atmospheric pressure; and for ethylene at elevated pressure have been experimentally investigated and compared in a counterflow non-premixed flame configuration.

Under the investigated conditions, butane isomers were observed to form more soot than butanol isomers, thereby showing the effect of the hydroxyl group. The effects of isomeric structural differences on sooting propensity were also observed within the butane and butanol isomers. In addition, while soot volume fraction was seen to increase with increasing fuel mole fraction, the ranking of sooting propensity for these C4 fuels remained unchanged. For the conditions studied, the sooting tendency ranking generally follows n-butane > iso-butane > tert-butanol > n-butanol > iso-butanol > sec-butanol. . The counterflow non-premixed flames were also simulated using the gas-phase chemical kinetic models, USC Mech II [1], Sarathy et al. [2] and Merchant et al. [3] available in the literature to compute the spatially-resolved profiles of soot precursors, including acetylene and propargyl.

For these C4 fuels, the PAHs of various aromatic ring size groups (2, 3, 4, and larger aromatic rings) have been characterized and compared in non-premixed combustion configuration. In particular, the formation and growth of the PAHs of different aromatic ring sizes in these counterflow flames was examined by tracking the PAH-PLIF signals at various detection wavelengths. PAH-PLIF experiments were conducted, by blending each of the branched-chain isomers with the baseline straight-chain isomer, in order to study the synergistic effects. The fuel structure effects on the PAH formation and growth processes were also analyzed by comparing the PAH growth pathways for these C4 fuels. A chemical kinetic model, POLIMI mechanism [4-7], available in the literature that includes both the fuel oxidation and the PAH chemistry was also used to simulate and compare the PAH species up to A4 rings.

Counterflow non-premixed sooting ethylene‒air flames with fuel mole fractions of 0.20‒0.40 in the pressure range of 1‒6 atm were investigated experimentally with the laser diagnostic techniques of LII, PLIF and LE. A better understating of the quantitative soot formation process has been developed for ethylene counterflow flames under elevated pressure conditions. The effect of pressure on the formation of PAHs with different aromatic ring sizes has also been determined qualitatively. With increase in pressure, the increase in soot volume fraction and PAH-PLIF signals were observed. A chemical kinetic model available in the literature, that includes both the fuel oxidation and the PAH chemistry, was also used to simulate and compare the PAH species up to A4 rings. At the incipient stage of the PAH formation, the simulated results exhibited similar behavior to the experimental observations. A chemical kinetic model, WF-PAH mechanism [8], available in the literature was also used to compute the PAHs up to four aromatic rings. This chemical kinetic model predicted enhancing PAHs formation with an increase in pressure, consistent with the experimental trend.

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