Development of a Novel Mass Spectrometric ... - Jacobs University

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Introduction can reduce the usability of land for development. Nowadays the major significant source of contamination to land and marine environment remains to be oil spills. Due to increased petroleum production and transportation activities, our world has witnessed a lot of accidental oil spills in the recent years. 34 For example the Gulf of Mexico was stricken by a British Petroleum oil spill which endangered the whole wild life in that area. Rehabilitation of the area was launched instantly. As a result to such accidents, the biodegradation of oil and its derived products have been the focus of many studies. Nevertheless an important concern remains due to the toxicity of these oil constituents. Despite hydrocarbons have low solubility in water; they can accumulate in the fatty tissues of organisms. The long term toxicity of n-hexane in humans is well known. Alkanes with more than 11 carbons are not toxic most organisms due to their low solubility in water and low chemical reactivity. However, aromatic hydrocarbons are problematic because of their aqueous solubility and enhanced bioavailability. 35 Hereby studies have tried to answer questions related to composition and persistence of potential complex pollutants. In equal footing, studies have investigated the bioremediation process of petroleum components in polluted areas. 36 While some types of hydrocarbons are readily biodegraded in marine environment; others like multi-ring aromatics are difficult to be biodegraded. These compounds resist microbial degradation partly due to their structure. 37 The environmental impact of the unknown oil should be assessed by the determination of individual petroleum hydrocarbons in a complex mixture of compounds. However such mixtures are difficult to separate by most analytical techniques. Chromatography does not resolve (and thus identify) a substantial proportion of complex hydrocarbon mixtures. These components are often referred to as the unresolved complex mixture (UCM), or 'hump', (term UCM was introduced by Gough and Rowland), which is especially pronounced for biodegraded petroleum. 16 It is known that microorganisms metabolize various classes of petroleum compounds which results in the reduction of dominant saturated aliphatic hydrocarbons. UCM is believed to compose of branched and cyclic 5
Introduction aliphatic hydrocarbons and aromatic hydrocarbons (see Figure 1-1), which usually show the greatest resistance to biodegradation. 38,39 These compounds give rise to UCM referred to as a hump by Gough and Rowland in 1990. UCM is used as an indicator of petrogenic environmental input due to its persistence after accidental or chronic oil spills. Historically, UCM has been considered non-toxic but more recent studies suggest otherwise. 23 The chemical analysis of crude oils and related samples are necessary for tracking compositional changes of products affected by biodegradation or weathering 25 such as in oil spills or in complex mixtures undergoing biological treatments like solid waste. Characterization of UCM has been an important competition among researchers who applied different strategies to guess the composition beyond the GC hump. Concerned with the toxic behavior of the above reported hydrocarbon forms, other researchers have been looking for improved methods of quantification. Therefore, development of informative analytical methods that unambiguously reveal the quantity and identify hydrocarbons found in different complex mixtures are highly required. Overall environmental awareness demand the investigation of the presence and concentration of primary contaminant classes such as polyaromatic hydrocarbons (PAH), amines or polychlorinated biphenyls (PCBs) in water, soils or sands. Regulatory bodies like Environmental Protection Agency (EPA, USA) are always interested in assessing and minimizing the impact of chemical waste and in detecting specific toxicants accidently released into the environment. 40 Classification of Hydrocarbons, HCs: •Straight branched aliphatic, cycloaliphatic (Decane to Tetracontane) •Polycyclic Aromatic Hydrocarbons, PAHs ( Naphthalene, Pyrene) And the collection extends to others in terms of degradability, solubility and volatility: 6
Page 1 and 2: Development of a Novel Mass Spectro
Page 3 and 4: Declaration of Authorship I ,Nadim
Page 5 and 6: This work has been carried out unde
Page 7 and 8: Contents Contents Declaration of Au
Page 9 and 10: List of Figures List of Figures Fig
Page 11 and 12: List of Figures Figure 3-39 MS 2 fr
Page 13 and 14: List of Tables List of Tables Table
Page 15 and 16: Abbreviations Abbreviations APCI AP
Page 17 and 18: Abbreviations UV VGOs VOCs VRs ultr
Page 19 and 20: Introduction Analytical chemistry h
Page 21: Introduction 1.2 Presence and Fate
Page 25 and 26: Introduction Figure 1-1 Examples of
Page 27 and 28: Introduction Figure 1-2 Range of io
Page 29 and 30: Introduction fractions. 42 Another
Page 31 and 32: Introduction 1.3.5 APLI Other crude
Page 33 and 34: Introduction products). Other molec
Page 35 and 36: Introduction Other studies performe
Page 37 and 38: Introduction APLI-FT ICR-MS Crude o
Page 39 and 40: Introduction spectrometry in as muc
Page 41 and 42: Introduction catalytic processing t
Page 43 and 44: Introduction Figure 1-6 Kendrick ma
Page 45 and 46: Introduction including determinatio
Page 47 and 48: Introduction 1.5 Scope and Signific
Page 49 and 50: Experimental e) Other model mixture
Page 51 and 52: Experimental 2.2.2 Preparation of O
Page 53 and 54: Experimental 2.4 Graphical Presenta
Page 55 and 56: Results and Discussion experiment.
Page 57 and 58: Results and Discussion Intens. [%]
Page 59 and 60: Results and Discussion common featu
Page 61 and 62: Results and Discussion 3.2 APCI-TOF
Page 63 and 64: Results and Discussion These compou
Page 67 and 68: Results and Discussion Ions were pr
Page 71 and 72: Results and Discussion procedure ba
Page 73 and 74:
Results and Discussion Intens. [%]
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Results and Discussion to produce m
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Results and Discussion 519.5863 519
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Results and Discussion Higher mass
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Results and Discussion isolated fro
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Results and Discussion 3.4.5 Tandem
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Results and Discussion injected int
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Results and Discussion 3.4.8 Quanti
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Results and Discussion Int. x 10000
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Results and Discussion Table 3.6 Qu
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Results and Discussion assessment o
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Results and Discussion hydrocarbons
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Results and Discussion of n-alkanes
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Results and Discussion flow (in I2)
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Results and Discussion Other intere
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Results and Discussion Figure 3-80
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Results and Discussion KMD 2.4 2.2
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Results and Discussion KMD 1.1 1 Le
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Results and Discussion 3.6.4 Asphal
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Conclusions In conclusion we could
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References References 1. Fay, R. M.
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References 23. Colavecchia, M. V.,
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References 47. Dzidic, I., Petersen
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References Hydroconversion Processe
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References 91. Golovlev, V. V., All
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Appendix Light shredder waste Meas.
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419.4592 C 30 H 59 419.4611 4.6 421
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Liqui Moly car motor oil Meas. m/z
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345.3511 C 25 H 45 345.3516 1.5 349
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