Molecular characterization of dissolved organic matter (DOM) along a river to ocean transect of the lower Chesapeake Bay by ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry

Sleighter, Rachel L.; Hatcher, Patrick G.

doi:10.1016/j.marchem.2008.04.008

Cited by 395 publications

(385 citation statements)

References 75 publications

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“…Most molecular formulae with positive correlations to the first canonical axes of salinity (Figures 5c and d) and DNA ( Figure 6a) were relatively saturated (H/C ratio of 41), which is typical for marine DOM (Koch et al, 2005;Sleighter and Hatcher, 2008;Kujawinski et al, 2009;Medeiros et al, 2015). Some combustionderived condensed aromatic compounds ('black carbon', very low H/C and O/C ratios) also partially correlated with the canonical axis of DNA.…”

Section: Identifying the Key Factors-dom Moleculesmentioning

confidence: 91%

Deciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine system

et al. 2016

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Dissolved organic matter (DOM) is the main substrate and energy source for heterotrophic bacterioplankton. To understand the interactions between DOM and the bacterial community (BC), it is important to identify the key factors on both sides in detail, chemically distinct moieties in DOM and the various bacterial taxa. Next-generation sequencing facilitates the classification of millions of reads of environmental DNA and RNA amplicons and ultrahigh-resolution mass spectrometry yields up to 10 000 DOM molecular formulae in a marine water sample. Linking this detailed biological and chemical information is a crucial first step toward a mechanistic understanding of the role of microorganisms in the marine carbon cycle. In this study, we interpreted the complex microbiological and molecular information via a novel combination of multivariate statistics. We were able to reveal distinct relationships between the key factors of organic matter cycling along a latitudinal transect across the North Sea. Total BC and DOM composition were mainly driven by mixing of distinct water masses and presumably retain their respective terrigenous imprint on similar timescales on their way through the North Sea. The active microbial community, however, was rather influenced by local events and correlated with specific DOM molecular formulae indicative of compounds that are easily degradable. These trends were most pronounced on the highest resolved level, that is, operationally defined 'species', reflecting the functional diversity of microorganisms at high taxonomic resolution.

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Section: Identifying the Key Factors-dom Moleculesmentioning

confidence: 91%

Deciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine system

et al. 2016

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“…Likewise, the coupling of electrospray ionization (ESI) to high-field Fourier-transform ion cyclotron resonance (FT-ICR) MS has provided unprecedented resolution of the molecular components of natural organic matter (NOM) as well as molecular details of biogeochemical processes (Kujawinski et al 2002;Kim et al 2003aKim et al , 2003bKim et al , 2004Kim et al , 2006Kramer et al 2004;Kujawinski et al 2004;Koch et al 2005;Dittmar and Koch 2006;Grannas et al 2006;Hertkorn et al 2006; Kujawinski and Behn 2006;Mopper et al 2007;Reemtsma et al 2008;Sleighter and Hatcher 2008).…”

Section: Introductionmentioning

confidence: 99%

“…SPE is also an effective means of removing inorganic ions, which can give rise to matrix effects and ion suppression. However, all SPE resins are inherently selective because retention is based on intermolecular forces, as was recently demonstrated by a study of Dismal Swamp water (Sleighter and Hatcher 2008) analyzed directly by ESI without preconcentration. It was clear that water-soluble tannins and amides/amines are excluded by SPE.…”

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confidence: 99%

Electrospray and photoionization mass spectrometry for the characterization of organic matter in natural waters: a qualitative assessment

Hockaday

Purcell

Marshall

et al. 2009

Limnology & Ocean Methods

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Fourier‐transform ion cyclotron resonance mass spectrometry (MS) has demonstrated potential to revolutionize the fields of limnology and chemical oceanography by identifying the individual molecular components of organic matter in natural waters. The use of MS for this purpose is made possible by the electrospray technique which successfully ionizes polar, nonvolatile organic molecules. Another recently developed ion source, atmospheric pressure photoionization (APPI), extends MS capabilities to less polar molecules. This article presents early results on the application of APPI MS to natural organic matter. We compare APPI MS and electrospray MS data for dissolved organic matter from Lake Drummond (Virginia, USA). Collectively, electrospray and APPI MS identify more than 6000 molecular species to which we assign unique molecular formulas. Fewer than 1000 molecular species are common to both electrospray and APPI mass spectra, indicating that the techniques are highly complementary in the types of molecules they ionize. Access to a broad range of molecules provided by combining APPI and electrospray has prompted a qualitative analysis. The goal is to assess the extent to which molecular MS data correspond with elemental (CHNOS) and structural characteristics determined by combustion elemental analyses and 13C nuclear magnetic resonance (NMR). Because the data obtained by these different methods are not directly comparable, we propose a novel data analysis procedure that facilitates their comparison. The bulk elemental composition calculated from electrospray MS data are in close agreement (± 15%) with values determined by combustion elemental analysis. APPI and electrospray MS detect protein contributions in agreement with 13C NMR (6 wt %) but underestimate carbohydrates relative to 13C NMR. Nevertheless, MS results agree with NMR on the relative proportions of noncarbohydrate compounds in the organic matter: lignins > lipids > peptides. Finally, we use a molecular mixing model to simulate a 13C NMR spectrum from the MS datasets. The correspondence of the simulated and measured 13C NMR signals (74%) suggests that, collectively, the molecular species identified by APPI and electrospray MS comprise a large portion of the organic matter in Lake Drummond. These results add credibility to electrospray and APPI MS in limnology and oceanography applications, but further characterization of ion source behavior is fundamental to the accurate interpretation of MS data.

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“…The PC3, PC4, PC6 are protein-like (Tyrosine-like, peak B) at 280/305-310, peak N (associated with phytoplankton productivity), and peak T. Fluorescent technology benefits to discover these fluorophores , as defined by Stedmon (2007). These kinds of fluorophores mainly are the small particle organisms, and their molecule weight is smaller than 1.0 KDa (Sleighter and Hatcher, 2008;Helms et al, 2008). The PC5 is the fluorophore of photochemical production for high molecule weight (mainly ranging from 1.0 to 3.0 KDa) terrestrially humic-like.…”

Section: Parallel Factor Analysismentioning

confidence: 99%

Study of influencing factors to chromophoric dissolved organic matter absorption properties from fluorescence features in Taihu lake in autumn

Huang

Sun

et al. 2013

J Limnol

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In order to identify the components of chromophoric dissolved organic matter (CDOM) 19.93, 18.82, 16.88, 16.39, 12.26, and 15.72%, respectively is tryptophan-like, which is the product of phytoplankton and aquatic debris rather than the wastewater treatment drainaged from city. In this study, six fluorophores with multiple excitation-emission matrices (EEMs) peaks (A, B, C, N, M, T) were identified according to the parallel factor analysis (PARAFAC). The average contribution of each component to the CDOM is

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Molecular characterization of dissolved organic matter (DOM) along a river to ocean transect of the lower Chesapeake Bay by ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry

Cited by 395 publications

References 75 publications

Deciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine system

Deciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine system

Electrospray and photoionization mass spectrometry for the characterization of organic matter in natural waters: a qualitative assessment

Study of influencing factors to chromophoric dissolved organic matter absorption properties from fluorescence features in Taihu lake in autumn

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