Distribution of acids and nitrogen-containing compounds in biodegraded oils of the Liaohe Basin by negative ion ESI FT-ICR MS

Liao, Yuhong; Shi, Quan; Hsu, Chang Samuel; Pan, Yinhua; Zhang, Yahe

doi:10.1016/j.orggeochem.2012.03.006

Cited by 109 publications

(111 citation statements)

References 70 publications

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“…Although we found, based on a principal component analysis (PCA, data not shown), that nitrogen and sulfur containing molecular formulas contributed only a little to the sample heterogeneity, their occurrence might be a good indicator for microbial alteration in future studies. The increase of the heteroatom contribution by microbial activity (as determined with FT-ICR MS) was also observed in other experiments and environments (Schmidt et al, 2009;Liao et al, 2012;Rossel et al, 2013).…”

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

confidence: 79%

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 Osupporting

confidence: 79%

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

et al. 2014

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“…The Es3 and Es1 members studied are reservoired in turbiditic sandstones and conglomerate and sandstones, respectively (Huang et al, 2004a,b). These samples are similar to those described in Huang et al (2003Huang et al ( , 2004a and Liao et al (2009Liao et al ( , 2012, which have experienced a natural sequence of biodegradation with Es3 oils in the range of 2-4 and Es1 oils in the range of 5-8 on the Peters and Moldowan biodegradation scale (abbreviated as PM level in the following text; Peters and Moldowan, 1993). For simplicity, tar sand bitumens are coded according to their biodegradation levels on the PM scale, e.g., tar sand bitumen of PM level 2 is coded as LH-2.…”

Section: Sample Descriptionsupporting

confidence: 70%

“…The results by Liao et al (2012) suggested that these oxygen-containing polar constituents bonded to asphaltene structure were gradually enriched in subunits with cyclic or aromatic structures, while n-fatty acids were progressively consumed during biodegradation, similar to the consumption of organic acids in maltenes. Additionally, ESI FT-ICR MS analyses of biodegraded oils (Kim et al, 2005;Liao et al, 2012;Pan et al, 2013) showed that the cyclic oxygen-containing polar compounds, generally including naphthenic acids, aromatic acids and phenols, are considered to have higher bio-resistance than n-fatty acids/n-alcohols.…”

Section: Discussionmentioning

confidence: 90%

“…This indicates that the cyclic oxygen-containing polar constituents bonded to the asphaltene structure by hydrogen and ester bonds, which usually have higher molecular weight, become gradually richer. This was shown by Liao et al (2012), who used ESI FT-ICR MS to study the oxygen-containing polar constituents bonded to asphaltene structures by hydrogen bonds (and also some may by ester bonds) at various biodegradation levels.…”

Section: Discussionmentioning

confidence: 99%

“…In a study by Liao et al (2009), asphaltenes at various degrees of biodegradation were subjected to elemental and isotope analysis using pyrolysis gas chromatography mass spectrometry (Py-GC-MS) and the results revealed that the molecular composition and structure of asphaltenes may be altered during biodegradation. In our recent work (Liao et al, 2012;Pan et al, 2013), the polar compounds in biodegraded tar sand bitumens from both the Liaohe Basin and Athabasca were studied using negative-ion electrospray (ESI) Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), and the results showed that the acidic compounds in asphaltene fractions are dominated by fatty and naphthenic acids and display significant changes with increasing biodegradation. It is generally accepted that the asphaltene fraction contains alkyl groups attached to the asphaltene core through covalent bonding such as ether and ester bonds, in addition to a small portion of free polar components attached through hydrogen bonds (Peng et al, 1997;Strausz et al, 1999a).…”

Section: Introductionmentioning

confidence: 99%

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Effect of biodegradation on the molecular composition and structure of asphaltenes: Clues from quantitative Py–GC and THM–GC

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The investigation of the bitumen from ancient Greek amphora using FT ICR MS, H/D exchange and novel spectrum reduction approach.

et al. 2016

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Recently Russian archeologists have discovered on Taman peninsula an ancient (V B.C.) Greek amphora full of dense bitumen. This is the oldest amphora in the world that contains bitumen. We report the investigation of this bitumen using ultrahigh resolution Fourier transform mass spectrometry. Also we used recently developed in-ESI source Hydrogen/Deuterium exchange approach for the structural characterization of the individual molecules and estimation of the biodegradation of the bitumen. The increase of number of the labile hydrogens compared to the non-degraded oil can serve as an additional evidence of the degradation of bitumen via oxidation. For the facilitation of the spectrum processing we have developed the special iterative spectrum reduction approach. It was observed that molecules that have only oxygen heteroatoms possess two -OH groups what is unusual for the petroleum. Based on this we suggested that the bitumen degraded during its being in amphora for 2500 years. Copyright © 2016 John Wiley & Sons, Ltd.

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Distribution of acids and nitrogen-containing compounds in biodegraded oils of the Liaohe Basin by negative ion ESI FT-ICR MS

Cited by 109 publications

References 70 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?

Effect of biodegradation on the molecular composition and structure of asphaltenes: Clues from quantitative Py–GC and THM–GC

The investigation of the bitumen from ancient Greek amphora using FT ICR MS, H/D exchange and novel spectrum reduction approach.

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