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Permanent link (DOI): https://doi.org/10.7939/R30D7N

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Mesophase Formation in Heavy Oil Open Access

Descriptions

Other title
Subject/Keyword
Hot-stage microscopy
Heavy oil
Mesophase
Type of item
Thesis
Degree grantor
University of Alberta
Author or creator
Bagheri, Seyed Reza
Supervisor and department
Gray, Murray (Chemical and Materials Engineering)
McCaffrey, William (Chemical and Materials Engineering)
Examining committee member and department
Koch, Bob (Mechanical Engineering)
Shaw, John (Chemical and Materials Engineering)
Miura, Kouichi (Chemical Engineering)
McCaffrey, William (Chemical and Materials Engineering)
Gray, Murray (Chemical and Materials Engineering)
Department
Department of Chemical and Materials Engineering
Specialization

Date accepted
2012-05-11T15:36:22Z
Graduation date
2012-11
Degree
Doctor of Philosophy
Degree level
Doctoral
Abstract
Coke formation is a major problem in the petroleum industry because of its effect on liquid yield, catalyst deactivation, and fouling of reactor internals and downstream vessels. Carbonaceous mesophase is a liquid crystalline phase which forms during cracking of heavy oil, as a subset of coke. A novel hot-stage reactor was designed and built to allow the in situ observation of mesophase formation at operating conditions of industrial reactors. The reactor was equipped with a magnetic stirrer to allow the addition of catalyst particles. The effect of cooling and depressurization on the formation and growth of carbonaceous mesophase in petroleum vacuum residue was studied using this reactor. The results showed that cooling below the cracking temperature at constant pressure can stop the formation and growth of mesophase by stopping chemical reactions. On the other hand, depressurization to atmospheric pressure, while maintaining reaction temperature, can promote the formation and growth of mesophase. The effect of stirring on mesophase formation was also investigated. Stirring can result in a bimodal distribution of size of mesophase domains in which very large mesophase regions coexist with a large number of small mesophase domains. Catalyst gives a delay in the onset of mesophase formation by its chemical activity, and a decrease in the amount of bulk mesophase regions by suppressing the coalescence of smaller mesophase domains as a physical effect. The results showed catalyst is less effective at higher catalyst concentrations due to the agglomeration of its particles. Mesophase formation was studied by a depolarized light scattering technique. A mechanism for mesophase formation in pitches has been suggested based on the evaluation of the previous models for mesophase formation with the scattering results. The results suggest that mesophase formation is a not a phase separation or nucleation process, but the homogeneous self-assembly of planer aromatic molecules into clusters and finally spherical submicron domains that coalesce to form the final micron-scale mesophase spheres. The role of asphaltenes in mesophase formation suggests that asphaltenes are a more aggregated phase in comparison to maltenes at high temperatures.
Language
English
DOI
doi:10.7939/R30D7N
Rights
Permission is hereby granted to the University of Alberta Libraries to reproduce single copies of this thesis and to lend or sell such copies for private, scholarly or scientific research purposes only. Where the thesis is converted to, or otherwise made available in digital form, the University of Alberta will advise potential users of the thesis of these terms. The author reserves all other publication and other rights in association with the copyright in the thesis and, except as herein before provided, neither the thesis nor any substantial portion thereof may be printed or otherwise reproduced in any material form whatsoever without the author's prior written permission.
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