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

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Introduction well as to environmental concerns. 27,28 For instance; environmental chemists must monitor the effects of various pollutants on human health and the eco-system. As understood from the above, the rapidly expanding interest in characterization of complex mixtures and their derivatives is driven by several objectives. The identification and structural characterization of compounds, monitoring the degradation processes of complex mixtures, evaluation of mixture reactivity related to properties and the quantification of target molecules are the general aims for research projects in this field. To achieve the above goals, researchers abandoned traditional analytical methods of complex mixtures to meet revolutionized methods implemented by mass spectrometry (MS). 29 Studies have shown that the direct analysis of complex mixtures is one area of mass spectrometry that has benefited from the evolution of the technology within mass spectrometry. 7 Modern mass spectrometry, with its unsurpassed resolution allows, however, the simultaneous analysis of tens of thousands of compounds in a single experiment, which in chromatography are manifested as an unresolved complex hump. Yet the application of novel measurement strategies allowed studying such complex mixtures in food, biological system and environmental samples. With high resolution MS studies and new data sorting strategies like Kendrick plots, knowledge about the actual content of unknown complex mixture becomes more accessible. 30 Although with complex mixtures a detailed and complete characterization is still perhaps impossible, examinations of parts of these various mixtures have recently become popular studies performed mainly due to the aforementioned reasons. 13 3
Introduction 1.2 Presence and Fate of Hydrocarbons in Contaminated Sites Petroleum samples involve many hydrocarbon mixtures like paraffins, cyclic paraffins, condensed aromatics and various heteroatom hydrocarbons (mostly O, S and N heterocycles). 31 The classification of hydrocarbons is shown below. Original petroleum contains molecules of a wide boiling point range from highly volatile C4 hydrocarbons to non-volatile asphaltenes. Generally petroleum mixtures are common site contaminants and weathered petroleum residuals may stay bound to soils or sediments for years. 32 In part due to their complexity, little is known about detailed chemical composition and consequently their potential for health or environmental impacts. Petroleum mixtures consist primarily of relatively unreactive complex hydrocarbons covering a wide boiling point range. In many mixtures, hydrocarbons range from volatile, short-chained organic compounds to heavy, long-chained, branched compounds. The exact composition of petroleum products varies depending upon the source, the modifiers or chemical processing. In addition to that the chemical composition of the product can be further affected by weathering and/or biological modification upon release to the environment. 33 On the other hand, the disposal of toxic industrial wastes through landfill, incineration or other procedures is a controversial subject, as toxic chemicals or their decomposition products may contaminate ground and drinking water or escape into the atmosphere during the production, conservation and treatment of the wastes. The lack of adequate regulation and official treatment and disposal plants in many countries has led to the illegal collection, transportation and dumping of wastes that, after the introduction of legislation designed to control the problem, must be recovered, identified and properly disposed of. On the other hand the analysis of the complex mixtures of industrial solvents that, being in liquid form and often stored in metallic drums which are subject to corrosion, may contaminate the landfill sites and could be leached by running water, or escape into the atmosphere as a result of their appreciable vapor pressures. Soil contamination has been a growing concern because it can be a source of groundwater (drinking water) contamination. In addition to that contaminated soils 4
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: Introduction Analytical chemistry h
Page 23 and 24: Introduction aliphatic hydrocarbons
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
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Results and Discussion procedure ba
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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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