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    Polycyclic Aromatic Hydrocarbons and Soot Particle Formation in the Combustion Process

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    PhD Thesis Can Shao
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    Type
    Dissertation
    Authors
    Shao, Can cc
    Advisors
    Sarathy, Mani cc
    Committee members
    Roberts, William L. cc
    Dally, Bassam cc
    Gascon, Jorge cc
    Yuan, Xuan
    Program
    Mechanical Engineering
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2021-12
    Embargo End Date
    2022-12-05
    Permanent link to this record
    http://hdl.handle.net/10754/673921
    
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    Access Restrictions
    At the time of archiving, the student author of this dissertation opted to temporarily restrict access to it. The full text of this dissertation will become available to the public after the expiration of the embargo on 2022-12-05.
    Abstract
    The threat to the environment and human health posed by the emission of soot particles and their precursors during the combustion process has attracted widespread attention for some time. Generation of soot particles includes the precursor’s formation, particle nucleation, and the growth and oxidation of soot particles; these processes are experimentally and numerically studied in this dissertation. Fuel composition is one of the most important parameters in the study of the combustion emissions. In the first portion of this research, quantified soot precursors were detected in a jet stirred reactor and a flow reactor of several gasoline surrogates, which covered various fuel compositions and different MON numbers. A kinetic model was made to capture the polycyclic aromatic formations and help to clarify the chemistry behind them. Major reaction pathways were discussed, as well as the role of important intermediate species, such as acetylene, and resonantly stabilized radicals like allyl, propargyl, cyclopentadienyl, and benzyl in the formation of polycyclic aromatic hydrocarbons. In the second section, a Fourier-transform ion cyclotron resonance mass spectrometry was first used to probe the chemical constituents of soot particles. By examining the soot particle generated in the early stage of nucleation, some information about the nucleation process was gained. The aromatics in the infant soot particles were all peri-condensed, of a size and shape easily linked by Van der Waals forces to form aromatic dimers and bigger clusters under the specified flame conditions. Compositions in the mature soot particles indicated that soot particles grow through the carbonization process. As a hydrogen carrier, ammonia was considered a good additive for controlling soot formation. In the third portion of this work, chemical effects of ammonia on soot formation were studied. Ammonia can suppress soot formation by reducing the precursor’s formation. Chemical kinetic analysis revealed that C-N species generated in ethylene-ammonia flames removed carbon from participating in soot precursor formation, thereby reducing soot formation, however, high concentrations of toxic hydrogen cyanide may be formed, which warrants further investigation.
    Citation
    Shao, C. (2021). Polycyclic Aromatic Hydrocarbons and Soot Particle Formation in the Combustion Process. KAUST Research Repository. https://doi.org/10.25781/KAUST-I9R01
    DOI
    10.25781/KAUST-I9R01
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-I9R01
    Scopus Count
    Collections
    PhD Dissertations; Physical Science and Engineering (PSE) Division; Mechanical Engineering Program

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