Solid-phase extraction-stepwise elution (SPE-SE) procedure for isolation of dissolved organic matter prior to ESI-FT-ICR-MS analysis

Lv, Jitao; Zhang, Shuzhen; Luo, Lei; Cao, Dong

doi:10.1016/j.aca.2016.10.038

Cited by 54 publications

(37 citation statements)

References 32 publications

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“…The low detection or absence of carbohydrate compounds could be constrained by the low ionization efficiency of polysaccharides in the negative ion mode during the FT-ICR MS analysis [54]. Meanwhile, tannins have been previously reported as potential missing compounds after SPE [55,56]. Except for the two compound classes, the distributions of the rest of the compound classes were consistent with previous observations and/or inferences from the fraction's characteristics.…”

Section: Comparison Of Molecular Composition Of the Three Chemical Frsupporting

confidence: 82%

Comparing the Spectroscopic and Molecular Characteristics of Different Dissolved Organic Matter Fractions Isolated by Hydrophobic and Anionic Exchange Resins Using Fluorescence Spectroscopy and FT-ICR-MS

Derrien

Lee

Hur

2017

Water

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Despite the environmental significance of dissolved organic matter (DOM), characterizing DOM is still challenging due to its structural complexity and heterogeneity. In this study, three different chemical fractions, including hydrophobic acid (HPOA), transphilic acid (TPIA), and hydrophilic neutral and base (HPIN/B) fractions, were separated from bulk aquatic DOM samples, and their spectral features and the chemical composition at the molecular level were compared using both fluorescence excitation emission matrix-parallel factor analysis (EEM-PARAFAC) and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). The HPIN/B fraction was distinguished from the two acidic fractions (i.e., HPOA and TPIA) by the EEM-PARAFAC, while the TPIA fraction was discriminated by using the molecular parameters derived from the FT-ICR MS analyses. Statistical comparison suggests that the spectral dissimilarity among the three chemical fractions might result from the acido-basic properties of DOM samples, while the differences in molecular composition were more likely to be affected by the hydrophobicity of the DOM fractions. The non-metric multidimensional scaling map further revealed that the HPOA was the most heterogeneous among the three fractions. The number of overlapping formulas among the three chemical fractions constituted only <5% of all identified formulas, and those between two different fractions ranged from 2.0% to 24.1%, implying relatively homogeneous properties of the individual chemical fractions with respect to molecular composition. Although employing chemical fractionation achieved a lowering of the DOM heterogeneity, prevalent signatures of either acido-basic property or the hydrophobic nature of DOM on the characteristics of three chemical isolated fractions were not found for this study.

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Section: Comparison Of Molecular Composition Of the Three Chemical Frsupporting

confidence: 82%

Comparing the Spectroscopic and Molecular Characteristics of Different Dissolved Organic Matter Fractions Isolated by Hydrophobic and Anionic Exchange Resins Using Fluorescence Spectroscopy and FT-ICR-MS

Derrien

Lee

Hur

2017

Water

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“…Since DOM in water are polar compounds containing oxygen, they can be effectively ionized and characterized in negative ion mode ( 32 ). Similar to EEMs analysis, DOM molecules were only detected in the algal culture without antibiotics.…”

Section: Resultsmentioning

confidence: 99%

Epiphytic Bacteria Are Essential for the Production and Transformation of Algae-Derived Carboxyl-Rich Alicyclic Molecule (CRAM)-like DOM

et al. 2021

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Dissolved organic matter (DOM) serves as a major carbon and nutrient pool in oceans, and recalcitrant DOM are the primary sources for carbon sequestration in depths. Here, we demonstrate the critical roles of algae-associated microorganisms (mainly heterotrophic bacteria) in the transformation of recalcitrant dissolved organic matter through laboratory cultures of a model diatom, Skeletonema dohrnii .

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“…Even under these circumstances, the Orbitrap is able to reproduce observed trends in molecular composition and allows separation of ecosystem types based on their DOM fingerprints. Drawbacks in resolving power can be tackled by increasing the specificity for analytes of interest during extraction (Tfaily et al, 2015;Li et al, 2016;Lv et al, 2016;Raeke et al, 2016), ionization (Hertkorn et al, 2008;Hockaday et al, 2009), or instrumental detection (Sleno, 2012;Cao et al, 2016). Although not comprehensive, broad trends in heteroatom content were also captured by the Orbitrap (Figure 6 and Supplementary Table S1).…”

Section: Discussionmentioning

confidence: 99%

Molecular Signals of Heterogeneous Terrestrial Environments Identified in Dissolved Organic Matter: A Comparative Analysis of Orbitrap and Ion Cyclotron Resonance Mass Spectrometers

et al. 2018

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Terrestrial dissolved organic matter (DOM) interlinks large carbon reservoirs of soils, sediments, and marine environments but remains largely uncharacterized on the molecular level. Fourier transform mass spectrometry (FTMS) has proven to be a powerful technique to reveal DOM chemodiversity and potential information encrypted therein. State-of-the-art FT-ICR MS (ion cyclotron resonance) instruments are yet inaccessible for most researchers. To evaluate the performance of the most recent Orbitrap analyzer as a more accessible alternative, we compared our method to an established 15 T FT-ICR MS on a diverse suite of 17 mainly terrestrial DOM samples regarding (1) ion abundance patterns, (2) differential effects of DOM type on information loss, and (3) derived biogeochemical information. We show that the Orbitrap provides similar information as FT-ICR MS, especially for compound masses below 400 m/z, and is mainly limited by its actual resolving power rather than its sensitivity. Ecosystems that are dominated by inputs of plant-derived material, like DOM from soil, bog, lake, and rivers, showed remarkably low average mass to charge ratios, making them also suitable for Orbitrap measurements. The additional information gained from FT-ICR MS was highest in heteroatom-rich (N, S, P) samples from systems dominated by internal cycling, like DOM from groundwater and the deep sea. Here FT-ICR MS detected 37% more molecular formulae and 11% higher ion abundance. However, the overall information content, which was analyzed by multivariate statistical methods, was comparable for both data sets. Mass spectra-derived biogeochemical trends, for example, the decrease of DOM aromaticity during the passage through terrestrial environments, were retrieved by both instruments. We demonstrate the growing potential of the Orbitrap as an alternative FTMS analyzer in the context of challenging analyses of DOM complexity, origin, and fate.

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Solid-phase extraction-stepwise elution (SPE-SE) procedure for isolation of dissolved organic matter prior to ESI-FT-ICR-MS analysis

Cited by 54 publications

References 32 publications

Comparing the Spectroscopic and Molecular Characteristics of Different Dissolved Organic Matter Fractions Isolated by Hydrophobic and Anionic Exchange Resins Using Fluorescence Spectroscopy and FT-ICR-MS

Comparing the Spectroscopic and Molecular Characteristics of Different Dissolved Organic Matter Fractions Isolated by Hydrophobic and Anionic Exchange Resins Using Fluorescence Spectroscopy and FT-ICR-MS

Epiphytic Bacteria Are Essential for the Production and Transformation of Algae-Derived Carboxyl-Rich Alicyclic Molecule (CRAM)-like DOM

Molecular Signals of Heterogeneous Terrestrial Environments Identified in Dissolved Organic Matter: A Comparative Analysis of Orbitrap and Ion Cyclotron Resonance Mass Spectrometers

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