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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Molecular composition and isotope mapping of natural gas in the British Columbia Natural Gas Atlas

Evans, Curtis 31 January 2019 (has links)
This thesis provides a geochemical interpretation of natural gas resources in north eastern British Columbia (NEBC), Canada. The work is part of the three-year project, British Columbia Natural Gas Atlas (BC-NGA) to collect samples and compile data on molecular (C1 to C5) and stable isotope ratio (δ13C and δ2H) compositions of natural gases in NEBC. The primary objective of the BC-NGA project is to produce a comprehensive, public, web database with maps of the gas geochemical data from a variety of gas tests including mudgas collected during drilling, downhole flow tests, production gas, and gas collected from surface emissions. The area of study in NEBC is a large portion of the Western Canadian Sedimentary Basin (WCSB) with Paleozoic, Mesozoic, and Cenozoic strata of thousands of meters thickness. Within this stratigraphic package there are numerous depositional hiatus and regional aquitards complicating the generation of regional maps and profiles. This M.Sc. thesis utilizes the geochemical gas parameters to characterize the range of gases in the BC-NGA database. The thesis found that the petroleum sources and active generation processes are not uniform in the NEBC. In some cases, the original gas signatures have been overprinted by localized processes in specific strata. The results of this new data plus compilation of existing data in the BC-NGA dataset indicate that many classical interpretive diagrams, e.g., Bernard Diagram (C1/[C2+C3] vs. δ13C1) and CD Diagram (δ13C1 vs. δ2H-C1), confirm the microbial/ thermogenic nature of the gases, but lack the resolution for detailed stratigraphic interpretation of gas sources and migration. A particularly interesting finding is that δ13Ckerogen (-33 ‰) estimated from δ13C1 observed for most strata in NEBC is 13C depleted compared with conventional kerogens and the data supports new calibration of the methane isotopes. This δ13Ckerogen value is an unlikely value and therefore the offset observed compared with conventional natural gases requires a different explanation, including commingling of 13C depleted methane from microbial sources. Enhanced characterization is obtained by combinations of the gas parameter ratios: δ13C1, δ13C2, δ13C3, C2/C3, C2/iC4, (e.g., ‘Berner-Faber Diagram’, ‘Prinzhofer Diagram’, ‘Lorant Diagram’). In addition, a new plot of δ13C2-δ13C1 versus iC4/nC4 ratio was developed in this thesis. / Graduate
2

Photochemistry of aromatic hydrocarbons: implications for ozone and secondary organic aerosol formation

Suh, Inseon 16 August 2006 (has links)
Aromatic hydrocarbons constitute an important fraction (~20%) of total volatile organic compounds (VOCs) in the urban atmosphere. A better understanding of the aromatic oxidation and its association in urban and regional ozone and organic aerosol formation is essential to assess the urban air pollution. This dissertation consists of two parts: (1) theoretical investigation of the toluene oxidation initiated by OH radical using quantum chemical and kinetic calculations to understand the mechanism of O3 and SOA precursors and (2) experimental investigation of atmospheric new particle formation from aromatic acids. Density functional theory (DFT) and ab initio multiconfigurational calculations have been performed to investigate the OH-toluene reaction. The branching ratios of OH addition to ortho, para, meta, and ipso positions are predicted to be 0.52, 0.34, 0.11, and 0.03, respectively, significantly different from a recent theoretical study of the same reaction system. Aromatic peroxy radicals arising from initial OH and subsequent O2 additions to the toluene ring are shown to cyclize to form bicyclic radicals rather than undergoing reaction with NO under atmospheric conditions.Isomerization of bicyclic radicals to more stable epoxide radicals possesses significantly higher barriers and hence has slower rates than O2 addition to form bicyclic peroxy radicals. At each OH attachment site, only one isomeric pathway via the bicyclic peroxy radical is accessible to lead to ring cleavage. Decomposition of the bicyclic alkoxy radicals leads primarily to formation of glyoxal and methyl glyoxal along with other dicarbonyl compounds. Atmospheric aerosols often contain a considerable fraction of organic matter, but the role of organic compounds in new nanometer-sized particle formation is highly uncertain. Laboratory experiments show that nucleation of sulfuric acid is considerably enhanced in the presence of aromatic acids. Theoretical calculations identify the formation of an unusually stable aromatic acid-sulfuric acid complex, which likely leads to a reduced nucleation barrier. The results imply that the interaction between organic and sulfuric acids promotes efficient formation of organic and sulfate aerosols in the polluted atmosphere because of emissions from burning of fossil fuels, which strongly impact human health and global climate.

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