Detailed compositional comparison of acidic NSO compounds in biodegraded reservoir and surface crude oils by negative ion electrospray Fourier transform ion cyclotron resonance mass spectrometry

Hughey, Christine A.; Galasso, Samantha A.; Zumberge, John E.

doi:10.1016/j.fuel.2006.08.029

Cited by 130 publications

(101 citation statements)

References 35 publications

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“…The technique is suitable for identifying molecular formula fingerprints of different sources (e.g. Hughey et al, 2007;Gonsior et al, 2011;Schmidt et al, 2011) and transformation processes (Rodgers et al, 2000;Kujawinski et al, 2004) of organic matter. Based on FT-ICR MS analyses, it has been previously hypothesized that the molecular composition of all refractory organic matter is similar and independent of its ultimate source (Koch et al, 2005;Rossel et al, 2013).…”

Section: B P Koch Et Al: Microbial Formation Of Marine Dissolved Omentioning

confidence: 99%

Molecular insights into the microbial formation of marine dissolved organic matter: recalcitrant or labile?

et al. 2014

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Abstract. The degradation of marine dissolved organic matter (DOM) is an important control variable in the global carbon cycle. For our understanding of the kinetics of organic matter cycling in the ocean, it is crucial to achieve a mechanistic and molecular understanding of its transformation processes. A long-term microbial experiment was performed to follow the production of non-labile DOM by marine bacteria. Two different glucose concentrations and dissolved algal exudates were used as substrates. We monitored the bacterial abundance, concentrations of dissolved and particulate organic carbon (DOC, POC), nutrients, amino acids and transparent exopolymer particles (TEP) for 2 years. The molecular characterization of extracted DOM was performed by ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) after 70 days and after ∼ 2 years of incubation. Although glucose quickly degraded, a non-labile DOC background (5-9 % of the initial DOC) was generated in the glucose incubations. Only 20 % of the organic carbon from the algal exudate degraded within the 2 years of incubation. The degradation rates for the nonlabile DOC background in the different treatments varied between 1 and 11 µmol DOC L −1 year −1 . Transparent exopolymer particles, which are released by microorganisms, were produced during glucose degradation but decreased back to half of the maximum concentration within less than 3 weeks (degradation rate: 25 µg xanthan gum equivalents L −1 d −1 ) and were below detection in all treatments after 2 years. Additional glucose was added after 2 years to test whether labile substrate can promote the degradation of background DOC (co-metabolism; priming effect). A priming effect was not observed but the glucose addition led to a slight increase of background DOC. The molecular analysis demonstrated that DOM generated during glucose degradation differed appreciably from DOM transformed during the degradation of the algal exudates. Our results led to several conclusions: (i) based on our experimental setup, higher substrate concentration resulted in a higher concentration of nonlabile DOC; (ii) TEP, generated by bacteria, degrade rapidly, thus limiting their potential contribution to carbon sequestration; (iii) the molecular signatures of DOM derived from algal exudates and glucose after 70 days of incubation differed strongly from refractory DOM. After 2 years, however, the molecular patterns of DOM in glucose incubations were more similar to deep ocean DOM whereas the degraded exudate was still different.

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Section: B P Koch Et Al: Microbial Formation Of Marine Dissolved Omentioning

confidence: 99%

Molecular insights into the microbial formation of marine dissolved organic matter: recalcitrant or labile?

et al. 2014

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“…1 They are problematic in refining processes because they lead to catalyst deactivation and cause fuel instability during transportation or storage. 13 Nitrogen compounds tend to exist in the higher boiling fractions and residues. 4 Among the refinery product streams, vacuum gas oil (VGO) is known to contain a considerable percentage of the total nitrogen compounds, which is only preceded by vacuum residue (VR).…”

Section: Introductionmentioning

confidence: 99%

Characterization of Basic Nitrogen-Containing Compounds in the Products of Lube Base Oil Processing by Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Li¹,

Zhu²,

Wu³

2014

Bulletin of the Korean Chemical Society

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The distribution of basic nitrogen-containing compounds in three vacuum gas oils (VGOs) with different boiling ranges and their dewaxed oils from the lube base oil refining unit of a refinery were characterized by positive-ion electrospray ionization (ESI) Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS). It turned out that the composition of basic nitrogen compounds in the samples varied significantly in DBE and carbon number, and the dominant basic N-containing compounds in these oil samples were N 1 class species. N 1 O 1 , N 1 O 2 , and N 2 class species with much lower relative abundance were also identified. The composition of basic nitrogen compounds in VGOs and dewaxed VGOs were correlated with increased boiling point and varied in DBE and carbon numbers. The comparison of the analytical results between VGOs and dewaxed VGOs indicated that more basic N-containing compounds in VGO with low carbon number and small molecular weight tend to be removed by solvent refining in lube base oil processing.

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“…Although petroleum samples have been most frequently analyzed by ESI (i.e., Stanford, 2006;Hughey, 2007;Mapolelo, 2010;Wu, 2003;McKenna, 2010a;McKenna, 2010b) [1][2][3][4][5][6][7][8][9][10] APPI offers several advantages over ESI for this particular study. First, negative APPI is well-suited to our interest in the water-soluble acidic compounds within our samples that are of environmental interest.…”

Section: S1 Discussion On Choice Of Ionization Methodsmentioning

confidence: 99%

Comprehensive study of a heavy fuel oil spill : modeling and analytical approaches to understanding environmental weathering

Lemkau¹

2012

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Driven by increasingly heavy oil reserves and more efficient refining technologies, use of heavy fuel oils for power generation is rising. Unlike other refined products and crude oils, a large portion of these heavy oils is undetectable using the traditional gas chromatography-based techniques on which oil spill science has been based. In the current study, samples collected after the 2007 M/V Cosco Busan heavy fuel oil spill (San Francisco, CA) were analyzed using gas chromatography (GC)-based techniques, numerical modeling and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) to examine natural weathering of the oil over a one and a half year period. Traditional GC techniques detected variable evidence of evaporation/ dissolution, biodegradation and photodegradation. Petroleum hydrocarbon compounds smaller than ~n-C 16 were rapidly lost due to evaporation and dissolution. Significant biodegradation was not detected until one month post spill while photodegradation was only observed at one field site. To further examine the processes of evaporation and dissolution, samples were analyzed with comprehensive two-dimensional GC (GC×GC) and a physiochemical model developed to approximate quantitative apportionment of compounds lost to the atmosphere and water. Model results suggest temperature is the primary control of evaporation. Finally, to examine the prominent non-GC amenable component of the oil, samples were analyzed with FT-ICR MS. Results showed expected clustering of samples, with those samples collected sooner after the spill having the most compositional similarity to the unweathered oil. Analysis of dominant heteroatom classes within the oil showed losses of high molecular weight species and the formation of stable core structures with time. These results highlight the susceptibility to weathering of these higher molecular weight components, previously believed to be recalcitrant in the environment. Research findings indicate that environmental weathering results in removal or alteration of larger alkylated compounds as well as loss of lower molecular weight species through evaporation/dissolution, biodegradation and photodegradation, with a resultant fraction of stable compounds likely to remain in the environment years after the spill. This research demonstrates the advantages of combining multiple analytical and modeling approaches for a fuller understanding of oil spill chemistry. AcknowledgementsThere are so many people that have helped me -personally and scientifically-along this journey. First I would like to thank my advisor Chris Reddy. You have been an amazing mentor, pushing me, allowing me to grow as a scientist and never wavering in your encouragement and support. I appreciate your willingness to explore the world outside of science through your public outreach. Although you may be a scientific workaholic (a topic of debate), you have always been tolerant of those of us who are less so, and I thank you for that. I appreciate the many people and experiences you...

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Detailed compositional comparison of acidic NSO compounds in biodegraded reservoir and surface crude oils by negative ion electrospray Fourier transform ion cyclotron resonance mass spectrometry

Cited by 130 publications

References 35 publications

Molecular insights into the microbial formation of marine dissolved organic matter: recalcitrant or labile?

Molecular insights into the microbial formation of marine dissolved organic matter: recalcitrant or labile?

Characterization of Basic Nitrogen-Containing Compounds in the Products of Lube Base Oil Processing by Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Comprehensive study of a heavy fuel oil spill : modeling and analytical approaches to understanding environmental weathering

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