Non-thermal Plasma Assisted Catalytic Upgrading of Low-cost Hydrocarbons

Meng, Shijun

Non-thermal Plasma Assisted Catalytic Upgrading of Low-cost Hydrocarbons

dc.contributor.advisor	Song, Hua
dc.contributor.author	Meng, Shijun
dc.contributor.committeemember	Hu, Jinguang
dc.contributor.committeemember	Mahinpey, Nader
dc.contributor.committeemember	Du, Ke
dc.contributor.committeemember	Zheng, Ying
dc.date	2023-06
dc.date.accessioned	2023-05-09T16:07:32Z
dc.date.available	2023-05-09T16:07:32Z
dc.date.issued	2023-05-03
dc.description.abstract	The catalytic upgrading of low-cost hydrocarbons under mild conditions (< 100 ℃ and atmospheric pressure) is explored with the assistance of non-thermal plasma. This novel technology can effectively convert methane at near ambient temperature and atmospheric pressure. A methane conversion higher than 40% can be achieved over the SBA-15 catalyst. Unlike the conventional thermos-catalytic process, activated methane can directly convert into the liquid product without the participation of any other co-reactants, with the liquid product primarily composed of gasoline range iso-paraffins. Over the optimized catalyst, the production of undesired coke and by-products are well-controlled. The effect of dielectric constant, porous structure, and acidity of the packed catalyst on catalytic performance is also studied. Additionally, as a promising H-donor, activated methane can participate in a series of hydrotreating reactions, such as catalytic reforming of naphtha and hydrodesulfurization of crude oil. Upon plasma activation, the co-fed methane can effectively accelerate hydrogenation and isomerization reactions for iso-paraffin production over an optimized Ga-based ZSM-5 catalyst. A systematic model compound study is conducted to gain a better understanding of the reaction mechanism. This novel process also successfully achieves the partial desulfurization of fed coker naphtha by close to 60%, which triggered another model compound study of non-thermal plasma assisted catalytic desulfurization study and thiophene is selected as the model compound. Sn-Ga/SBA-15 exhibits the best performance regarding thiophene conversion and H2S emission, even in a 12-hour prolonged run. It is also proved that the reaction atmosphere can greatly affect the composition of gas and solid products. An in-situ O2-plasma oxidation method is proposed and evaluated for NTP reactor regeneration, which can effectively remove the solid deposits from the quartz tube and spent catalyst. The knowledge obtained from this thesis indicates the feasibility of non-thermal plasma assisted light hydrocarbon catalytic upgrading and the synergistic effect between catalysis and plasma activation, which provides a novel process for the current petrochemical infrastructure.
dc.identifier.citation	Meng, S. (2023). Non-thermal plasma assisted catalytic upgrading of low-cost hydrocarbons (Doctoral thesis, University of Calgary, Calgary, Canada). Retrieved from https://prism.ucalgary.ca.
dc.identifier.uri	http://hdl.handle.net/1880/116192
dc.identifier.uri	https://dx.doi.org/10.11575/PRISM/dspace/41037
dc.language.iso	en
dc.publisher.faculty	Graduate Studies
dc.publisher.institution	University of Calgary
dc.rights	University of Calgary graduate students retain copyright ownership and moral rights for their thesis. You may use this material in any way that is permitted by the Copyright Act or through licensing that has been assigned to the document. For uses that are not allowable under copyright legislation or licensing, you are required to seek permission.
dc.subject	Non-thermal plasma
dc.subject	Catalysis
dc.subject	Methane activation
dc.subject	refinery
dc.subject	Natural gas
dc.subject.classification	Engineering--Chemical
dc.subject.classification	Engineering--Petroleum
dc.subject.classification	Energy
dc.subject.classification	Materials Science
dc.title	Non-thermal Plasma Assisted Catalytic Upgrading of Low-cost Hydrocarbons
dc.type	doctoral thesis
thesis.degree.discipline	Engineering – Chemical & Petroleum
thesis.degree.grantor	University of Calgary
thesis.degree.name	Doctor of Philosophy (PhD)
ucalgary.thesis.accesssetbystudent	I do not require a thesis withhold – my thesis will have open access and can be viewed and downloaded publicly as soon as possible.