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Unraveling Chemical Compositional Changes of Biodegraded Crude Oil Using Novel Chromatographic and Mass Spectrometric Techniques
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| 자료유형 | 학위논문 |
|---|---|
| 서명/저자사항 | Unraveling Chemical Compositional Changes of Biodegraded Crude Oil Using Novel Chromatographic and Mass Spectrometric Techniques. |
| 개인저자 | Nowak, Jeremy A. |
| 단체저자명 | University of California, Berkeley. Chemistry. |
| 발행사항 | [S.l.]: University of California, Berkeley., 2019. |
| 발행사항 | Ann Arbor: ProQuest Dissertations & Theses, 2019. |
| 형태사항 | 98 p. |
| 기본자료 저록 | Dissertations Abstracts International 81-04B. Dissertation Abstract International |
| ISBN | 9781085777063 |
| 학위논문주기 | Thesis (Ph.D.)--University of California, Berkeley, 2019. |
| 일반주기 |
Source: Dissertations Abstracts International, Volume: 81-04, Section: B.
Advisor: Goldstein, Allen H. |
| 이용제한사항 | This item must not be sold to any third party vendors. |
| 요약 | Crude oil is an immensely complex mixture that contains thousands of distinct elemental compositions with hydrogen, carbon, oxygen, nitrogen, and sulfur atoms. The chemical fingerprint of a crude oil varies depending on its origin and degree of weathering, a phenomenon which includes biodegradation. This dissertation focuses on chemical composition of crude oil and its biodegradation with an emphasis on biosouring, an enzymatic process in which Sulfate Reducing microbial Communities (SRCs) reduce sulfate, thiosulfate, and elemental sulfur to sulfide. Biosouring in crude oil reservoirs results in hydrogen sulfide production, precipitation of metal sulfide complexes, increased industrial costs of petroleum production, and exposure issues for personnel. Potential treatment strategies for biosouring include the injection of nitrate or perchlorate anions into crude oil reservoirs. The objectives of this dissertation include development of new analytical techniques and their application to characterize the chemical composition of crude oil, and how it changes during biosouring and treatments, including substrate consumption and product formation.Chapter 1 introduces the motivations for the research and analytical methods applied, including single and multi-dimensional gas chromatography with vacuum ultraviolet ionization and time-of-flight mass spectrometry (GC-VUV-TOF and GCxGC-VUV-TOF), gas chromatography combined with variable ionization time-of-flight-mass spectrometry (GC-Select-eV-TOF-MS), and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) combined with electrospray ionization. Chapter 1 then describes the experiments done examining biotransformations under different reducing environments and with different crude oils.The ability to structurally characterize and isomerically quantify crude oil hydrocarbons relevant to refined fuels such as motor oil, diesel, and gasoline represents an extreme challenge for chromatographic and mass spectrometric techniques. In Chapter 2, GCxGC-VUV-TOF is applied using a tunable vacuum ultraviolet soft photoionization source, the Chemical Dynamics Beamline 9.0.2 of the Advanced Light Source at the Lawrence Berkeley National Laboratory, to directly characterize and isomerically sum the contributions of aromatic and aliphatic species to hydrocarbon classes of four crude oils. When the VUV beam is tuned to 10.5 짹 0.2 eV, both aromatic and aliphatic crude oil hydrocarbons are ionized to reveal the complete chemical abundance of C9-C30 hydrocarbons. When the VUV beam is tuned to 9.0 짹 0.2 eV only aromatic hydrocarbons are ionized, allowing separation of the aliphatic and aromatic fractions of the crude oil hydrocarbon chemical classes in an efficient manner while maintaining isomeric quantification. This technique provides an effective tool to determine the isomerically summed aromatic and aliphatic hydrocarbon compositions of crude oil, providing information that goes beyond typical GCxGC separations of the most dominant hydrocarbon isomers.A comprehensive analysis of changes in crude oil chemical composition during biosouring and experimental treatments is presented in Chapter 3. Analyses using GC-VUV-TOF and FT-ICR MS combined with electrospray ionization were applied in this chapter to identify hydrocarbon degradation patterns and product formations in crude oil samples from biosoured, nitrate-treated, and perchlorate-treated bioreactor column experiments. Crude oil hydrocarbons were selectively transformed based on molecular weight and compound class in the biosouring control environment. Both the nitrate and the perchlorate treatments significantly reduced sulfide production |
| 일반주제명 | Physical chemistry. Microbiology. Petroleum engineering. Biochemistry. |
| 언어 | 영어 |
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