Identification of possible source markers in marine dissolved organic matter using ultrahigh resolution mass spectrometry

Kujawinski, Elizabeth B.; Longnecker, Krista; Blough, Neil V.; Vecchio, Rossana Del; Finlay, Liam; Kitner, Joshua B.; Giovannoni, Stephen J.

doi:10.1016/j.gca.2009.04.033

Cited by 226 publications

(196 citation statements)

References 72 publications

(83 reference statements)

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“…Uniform depth distributions of DOC have also been reported for the Southern Ocean (Wedborg et al, 1998;Wiebinga and de Baar, 1998;Ogawa et al, 1999) and are consistent with our constantly low wa H/C and high I DEG values. The uniform wa H/C ratios are unusual for ocean depth profiles (Kujawinski et al, 2009;Flerus et al, 2012;Hertkorn et al, 2013) but have been also reported by Koch et al (2005) for the southwestern Weddell Sea. Low H/C ratios and high I DEG values in the deep East Atlantic Ocean compared to the surface waters have been interpreted as a signature of reworked and degraded organic matter (Flerus et al, 2012).…”

Section: Ft-icr Ms Age Model Validationsupporting

confidence: 71%

“…Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) has opened a new analytical window to identify molecular formulae of thousands of marine compounds which are not accessible using standard analytical techniques (e.g., Koch et al, 2005Koch et al, , 2008Hertkorn et al, 2006;Kujawinski et al, 2009;D'Andrilli et al, 2010). Currently, much effort is undertaken to overcome the analytical restrictions of this technique (Kido Soule et al, 2010;Sleighter et al, 2010Sleighter et al, , 2012Tfaily et al, 2011) and to refine the data evaluation algorithms (Kujawinski and Behn, 2006;Koch et al, 2007;Flerus et al, 2011;Tziotis et al, 2011).…”

Section: Introductionmentioning

confidence: 99%

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Molecular transformation and degradation of refractory dissolved organic matter in the Atlantic and Southern Ocean

Lechtenfeld

Kattner

Flerus

et al. 2014

Geochimica et Cosmochimica Acta

276

259

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More than 90% of the global ocean dissolved organic carbon (DOC) is refractory, has an average age of 4000-6000 years and a lifespan from months to millennia. The fraction of dissolved organic matter (DOM) that is resistant to degradation is a long-term buffer in the global carbon cycle but its chemical composition, structure, and biochemical formation and degradation mechanisms are still unresolved. We have compiled the most comprehensive molecular dataset of 197 Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analyses from solid-phase extracted marine DOM covering two major oceans, the Atlantic sector of the Southern Ocean and the East Atlantic Ocean (ranging from 50°N to 70°S). Molecular trends and radiocarbon dating of 34 DOM samples (comprising D 14 C values from À229& to À495&) were combined to model an integrated degradation rate for bulk DOC resulting in a predicted age of >24 ka for the most persistent DOM fraction. First order kinetic degradation rates for 1557 mass peaks indicate that numerous DOM molecules cycle on timescales much longer than the turnover of the bulk DOC pool (estimated residence times of up to~100 ka) and the range of validity of radiocarbon dating. Changes in elemental composition were determined by assigning molecular formulae to the detected mass peaks. The combination of residence times with molecular information enabled modelling of the average elemental composition of the slowest degrading fraction of the DOM pool. In our dataset, a group of 361 molecular formulae represented the most stable composition in the oceanic environment ("island of stability"). These most persistent compounds encompass only a narrow range of the molecular elemental ratios H/C (average of 1.17 ± 0.13), and O/C (average of 0.52 ± 0.10) and molecular masses (360 ± 28 and 497 ± 51 Da). In the Weddell Sea DOC concentrations in the surface waters were low (46.3 ± 3.3 lM) while the organic radiocarbon was significantly more depleted than that of the East Atlantic, representing average surface water DOM ages of 4920 ± 180 a. These results are in accordance with a highly degraded DOM in the Weddell Sea surface water as also shown by the molecular degradation index I DEG obtained from FT-ICR MS data. Further, we identified 339 molecular formulae which probably contribute to an increased DOC concentration in the Southern Ocean and potentially reflect an accumulation or enhanced sequestration of refractory DOC in the Weddell Sea. These results will contribute to a better understanding of the persistent nature of marine DOM and its role as an oceanic carbon buffer in a changing climate.

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Section: Ft-icr Ms Age Model Validationsupporting

confidence: 71%

Section: Introductionmentioning

confidence: 99%

Molecular transformation and degradation of refractory dissolved organic matter in the Atlantic and Southern Ocean

Lechtenfeld

Kattner

Flerus

et al. 2014

Geochimica et Cosmochimica Acta

276

259

View full text Add to dashboard Cite

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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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“…Three studies have looked specifically at interactions between DOM and SAR11, the most abundant marine bacterioplankton clade, and demonstrate the potential for identifying DOM source markers (Kujawinski et al 2009), trophic strategies (Malmstrom et al 2005), and environmental adaptations (Gómez-Pereira et al 2012) of specific heterotrophic bacterioplankton taxa. The degradation of a few specific organic compounds have been tracked in-situ using molecular techniques, revealing succession patterns within individual heterotrophic functional groups and highlighting the extreme complexity of microbe-DOM interactions in nature (Lau et al 2007, Watanabe et al 2012.…”

Section: An Interdisciplinary Approachmentioning

confidence: 99%

“…Dissolved organic matter recovered by solid phase extraction (SPE) from spent culture media (hereafter referred to as phytoplankton DOM, or DOM P ) was analyzed by high performance liquid chromatography-electrospray ionization mass spectrometry (HPLC-ESI-MS). Similar untargeted metabolomics approaches have been successfully employed to study many aspects of microbial interactions with DOM (Kujawinski et al 2009, Barofsky et al 2010), but none have yet examined the relationship between DOM composition and the taxonomy of the source organisms. We obtained and analyzed a complex data set comprised of hundreds to thousands of metabolites from each organism tested to compare features produced by different phytoplankton strains.…”

Section: Introductionmentioning

confidence: 99%

Microbial production and consumption of marine dissolved organic matter

Becker¹

2013

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Marine phytoplankton are the principal producers of oceanic dissolved organic matter (DOM), the organic substrate responsible for secondary production by heterotrophic microbes in the sea. Despite the importance of DOM in marine food webs, details regarding how marine microbes cycle DOM are limited, and few definitive connections have been made between specific producers and consumers. Consumption is thought to depend on the source of the DOM as well as the identity of the consumer; however, it remains unclear how phytoplankton diversity and DOM composition are related, and the metabolic pathways involved in the turnover of DOM by different microbial taxa are largely unknown. The motivation for this thesis is to examine the role of microbial diversity in determining the composition, lability, and physiological consumption of marine DOM. The chemical composition of DOM produced by marine phytoplankton was investigated at the molecular level using mass spectrometry. Results demonstrate that individual phytoplankton strains release a unique suite of organic compounds. Connections between DOM composition and the phylogenetic identity of the producing organism were identified on multiple levels, revealing a direct relationship between phytoplankton diversity and DOM composition. Phytoplankton-derived DOM was also employed in growth assays with oligotrophic bacterioplankton strains to examine effects on heterotrophic growth dynamics. Reproducible responses ranged from suppressed to enhanced growth rates and cell yields, and depended both on the identity of the heterotroph and the source of the DOM. Novel relationships between specific bacterioplankton types and DOM from known biological sources were found, and targets for additional studies on reactive DOM components were identified. The physiology of DOM consumption by a marine Oceanospirillales strain was studied using a combined transcriptomic and untargeted metabolomic approach. The transcriptional response of this bacterium to Prochlorococcus-derived DOM revealed an increase in anabolic processes related to metabolism of carboxylic acids and glucosides, increased gene expression related to proteorhodopsin-based phototrophy, and decreased gene expression related to motility. Putative identification of compounds present in Prochlorococcus-derived DOM supported these responses. Collectively, these findings highlight the potential for linking detailed chemical analyses of labile DOM from a known biological source with bacterioplankton diversity and physiology. My parents and my brother, Bob, Ellen, & Brian, who taught me young to pursue whatever it is that makes me happy. You've not only stood by my side, but also kept me from falling on many occasions.And finally…the menagerie. For love. For perspective. Misty, Will, Pac, & Lexi -I wouldn't trade a single crazy day. 6All things are one thing and that one thing is all things -plankton, a shimmering phosphorescence on the sea and the spinning planets and an expanding universe, all bound together by the elastic string ...

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Identification of possible source markers in marine dissolved organic matter using ultrahigh resolution mass spectrometry

Cited by 226 publications

References 72 publications

Molecular transformation and degradation of refractory dissolved organic matter in the Atlantic and Southern Ocean

Molecular transformation and degradation of refractory dissolved organic matter in the Atlantic and Southern Ocean

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

Microbial production and consumption of marine dissolved organic matter

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