Catalytic Upgrading of Low Cost Carbon Resources Under Methane Environment

Wang, Aiguo

Catalytic Upgrading of Low Cost Carbon Resources Under Methane Environment

dc.contributor.advisor	Song, Hua
dc.contributor.advisor	Mahinpey, Nader
dc.contributor.author	Wang, Aiguo
dc.contributor.committeemember	Du, Ke
dc.contributor.committeemember	Kuhn, John N.
dc.contributor.committeemember	Lu, Qingye
dc.contributor.committeemember	Cheng, Yugeng
dc.date	2018-11
dc.date.accessioned	2018-09-20T13:47:53Z
dc.date.available	2018-09-20T13:47:53Z
dc.date.issued	2018-09-12
dc.description.abstract	The heavy reliance on fossil fuels raises concerns about economic stability and environmental impact, making it desirable to find a renewable energy source that is cost competitive with traditional fuels. Catalytic conversion of low cost carbon resources such as biomass into biofuels and valuable chemicals has the potential of alleviating the dependence on fossil fuels. However, due to high oxygen content of biomass, the upgraded products are highly oxygenated and disadvantageous. The presence of oxygenated compounds, such as alcohols, carboxylic acids, phenolics, and furans, results in the products with low energy density, poor quality as well as incompatibility infrastructure. Hydrodeoxygenation is an efficient method to improve the quality of biomass-derived products by oxygen elimination. However, it requires high operating pressure and substantial consumption of expensive and unavailable hydrogen, which makes this process unpractical and economically unfeasible in a large scale. Methane, as the main component in natural gas that is an abundant natural resource present in Canada, is an ideal alternative to hydrogen for the valorization of bio-derived products. Methane (CH4) with the highest H/Ceff ratio could benefit the formation of hydrocarbon products with higher energy density and reduce the coke formation. The activation of methane can provide hydrogen atoms for the deoxygenation of oxygenated chemical compounds, and methyl moieties to form the aromatic hydrocarbons, thus improve the quality and yield of liquid products. Due to the complexity of biomass, several model compounds including ethanol, acetic acid, phenol, furfural, cellulose and lignin representing different functional groups, are selected to investigate the technical feasibility of catalytic co-conversion of bio-based compounds and methane to valuable aromatic hydrocarbons. Mechanistic investigations such as liquid and solid-state 1H, 2H and 13C NMR combined with experimental analyses evidence methane incorporation into aromatic products. Various catalyst characterizations including XRD, TEM, DRIFT, NH3-TPD, XPS, and XAS, are employed to reveal the relationship between the physicochemical properties of the catalyst and its excellent performance. The mechanistic understanding provides valuable insights into the catalytic chemistry of biomass valorization with methane, and the rational design of catalysts for cost-efficient utilizations of biomass and natural gas resources.	en_US
dc.identifier.citation	Wang, A. (2018). Catalytic Upgrading of Low Cost Carbon Resources Under Methane Environment (Doctoral thesis, University of Calgary, Calgary, Canada). Retrieved from https://prism.ucalgary.ca. doi:10.11575/PRISM/32945	en_US
dc.identifier.doi	http://dx.doi.org/10.11575/PRISM/32945
dc.identifier.uri	http://hdl.handle.net/1880/107782
dc.language.iso	eng
dc.publisher.faculty	Graduate Studies
dc.publisher.faculty	Schulich School of Engineering
dc.publisher.institution	University of Calgary	en
dc.publisher.place	Calgary	en
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	zeolite
dc.subject	Catalysis
dc.subject	Methane
dc.subject	Biomass
dc.subject	Aromatics
dc.subject	Model compounds
dc.subject.classification	Energy	en_US
dc.subject.classification	Engineering--Chemical	en_US
dc.subject.classification	Engineering--Environmental	en_US
dc.subject.classification	Materials Science	en_US
dc.subject.classification	Engineering--Petroleum	en_US
dc.title	Catalytic Upgrading of Low Cost Carbon Resources Under Methane Environment
dc.type	doctoral thesis
thesis.degree.discipline	Chemical and Petroleum Engineering
thesis.degree.grantor	University of Calgary
thesis.degree.name	Doctor of Philosophy (PhD)
ucalgary.item.requestcopy	true