Ultrahigh resolution mass spectrometric differentiation of dissolved organic matter isolated by coupled reverse osmosis-electrodialysis from various major oceanic water masses

Chen, Hongmei; Stubbins, Aron; Perdue, Edward M.; Green, Nelson W.; Helms, John R.; Mopper, Kenneth; Hatcher, Patrick G.

doi:10.1016/j.marchem.2014.06.002

Cited by 59 publications

(76 citation statements)

References 49 publications

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“…The molecular signatures of whole water tree-DOM as revealed by negative mode electrospray ionization FT-ICR MS (Figure 2) share many features of whole water and extracted DOM from other aquatic environments (Mopper et al, 2007;Singer et al, 2012;Chen et al, 2014;Dittmar and Stubbins, 2014;Cawley et al, 2016). Shared features include a high diversity of elemental formulas distributed broadly in van Krevelen space (Figures 6A-C) and spanning a range of molecular classes ( Table 2).…”

Section: Molecular Signatures Of Tree-dommentioning

confidence: 96%

Molecular and Optical Properties of Tree-Derived Dissolved Organic Matter in Throughfall and Stemflow from Live Oaks and Eastern Red Cedar

et al. 2017

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Studies of dissolved organic matter (DOM) transport through terrestrial aquatic systems usually start at the stream. However, the interception of rainwater by vegetation marks the beginning of the terrestrial hydrological cycle making trees the headwaters of aquatic carbon cycling. Rainwater interacts with trees picking up tree-DOM, which is then exported from the tree in stemflow and throughfall. Stemflow denotes water flowing down the tree trunk, while throughfall is the water that drips through the leaves of the canopy. We report the concentrations, optical properties (light absorbance) and molecular signatures (ultrahigh resolution mass spectrometry) of tree-DOM in throughfall and stemflow from two tree species (live oak and eastern red cedar) with varying epiphyte cover on Skidaway Island, Savannah, Georgia, USA. Both stemflow and throughfall were enriched in DOM compared to rainwater, indicating trees were a significant source of DOM. The optical and molecular properties of tree-DOM were broadly consistent with those of DOM in other aquatic ecosystems. Stemflow was enriched in highly colored DOM compared to throughfall. Elemental formulas identified clustered the samples into three groups: oak stemflow, oak throughfall and cedar. The molecular properties of each cluster are consistent with an autochthonous aromatic-rich source associated with the trees, their epiphytes and the microhabitats they support. Elemental formulas enriched in oak stemflow were more diverse, enriched in aromatic formulas, and of higher molecular mass than for other tree-DOM classes, suggesting greater contributions from fresh and partially modified plant-derived organics. Oak throughfall was enriched in lower molecular weight, aliphatic and sugar formulas, suggesting greater contributions from foliar surfaces. While the optical properties and the majority of the elemental formulas within tree-DOM were consistent with vascular plant-derived organics, condensed aromatic formulas were also identified. As condensed aromatics are generally interpreted Stubbins et al.Optical and Molecular Signatures of Tree-DOM as deriving from partially combusted organics, some of the tree-DOM may have derived from the atmospheric deposition of thermogenic and other windblown organics. These initial findings should prove useful as future studies seek to track tree-DOM across the aquatic gradient from canopy roof, through soils and into fluvial networks.

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Section: Molecular Signatures Of Tree-dommentioning

confidence: 96%

Molecular and Optical Properties of Tree-Derived Dissolved Organic Matter in Throughfall and Stemflow from Live Oaks and Eastern Red Cedar

et al. 2017

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“…The extreme mass accuracy and precision of FT-ICR MS allows the exact elemental composition of ions to be calculated-a major breakthrough for the characterization of DOM and its molecular messages (Dittmar and Stubbins, 2013;Mopper et al, 2007). In each photochemical study employing FT-ICR MS, aromatic carbon or high double bond equivalent molecules constituted the most photolabile DOM fractions (Chen et al, 2014;Gonsior et al, 2009;Kujawinski et al, 2004;Stubbins et al, 2010). The average molecular weight of DOM also decreases during irradiations.…”

Section: Dom Photolability Spectrum and Fate Of Terrestrial Dom Imentioning

confidence: 99%

Marine Photochemistry of Organic Matter

Mopper

Kieber

Stubbins

2015

Biogeochemistry of Marine Dissolved Organic Matter

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“…Spectral slope (S) and slope ratio (S R ) were calculated (Helms et al, 2013). DOC was measured as non-purgeable organic carbon using hightemperature catalytic combustion by high temperature combustion (720°C) on a Shimadzu TOC-VCPH (Shimadzu Scientific Instruments; Chen et al, 2014a). Specific UV absorbance (SUVA) was calculated by dividing decadic absorbance in units of m −1 by the DOC concentration in units of mg C L −1 (Weishaar et al, 2003).…”

Section: Uv-visible Spectroscopy and Dissolved Organic Carbon Analysismentioning

confidence: 99%

“…Initial seawater sample DOC concentrations were 39 to 88 μmol L −1 and were concentrated by RO/ED to 1076 to 4298 μmol L −1 (Table 1; Chen et al, 2014a). DOC recoveries for the RO/ED process ranged from 40 to 68% in the North Atlantic Ocean samples (3 samples average = 51%) and 83 to 86% in the Pacific Ocean samples (2 samples average = 84%; Chen et al, 2014a).…”

Section: Bulk Organic and Inorganic Properties Of Ro/ed Isolatesmentioning

confidence: 99%

“…DOC recoveries for the RO/ED process ranged from 40 to 68% in the North Atlantic Ocean samples (3 samples average = 51%) and 83 to 86% in the Pacific Ocean samples (2 samples average = 84%; Chen et al, 2014a). The lowest recovery (40%) was obtained on the first sample that was processed by a new RO/ED system (the 3000 m North Atlantic sample) and was likely due to the system not being adequately conditioned prior to use, as opposed to the DOM in this sample having anomalous extraction behavior (Chen et al, 2014a). Because its spectroscopic properties appeared to be consistent with the other samples, it was kept as part of this study.…”

Section: Bulk Organic and Inorganic Properties Of Ro/ed Isolatesmentioning

confidence: 99%

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Spectroscopic characterization of oceanic dissolved organic matter isolated by reverse osmosis coupled with electrodialysis

et al. 2015

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a b s t r a c tOceanic dissolved organic matter (DOM) is one of the largest pools of reduced carbon on Earth, yet DOM remains poorly chemically characterized. Studies to determine the chemical nature of oceanic DOM have been impeded by the lack of efficient and non-fractioning methods to recover oceanic DOM. Here, a DOM fraction (~40 to 86% recovery) was isolated using reverse osmosis/electrodialysis (RO/ED) and analyzed by solid-state 13 C nuclear magnetic resonance (NMR) spectroscopy. Samples were obtained from biogeochemically distinct environments: photobleached surface gyre, productive coastal upwelling zone, oxygen minimum, North Atlantic Deep Water, and North Pacific Deep Water. A ubiquitous 'background' refractory carbon pool was apparent throughout the ocean and dominated in the deep Pacific Ocean. Advanced NMR spectral editing revealed that condensed aromatic and quaternary anomeric carbons contribute to this deep refractory DOC pool, the quaternary anomeric carbons being a newly identified and potentially important component of bio-refractory carbohydrate-like carbon. Additionally, our results support the multi-pool (e.g. 3-pool: labile, semi-labile, and refractory) conceptual model of marine DOM biogeochemistry. Surface samples, hypothesized to be enriched in labile and semilabile DOM, were enriched in carbohydrate-like material consistent with prior studies. High carboxyl signals in the deep Pacific support the hypothesis that a major fraction of the refractory pool consists of carboxyl-rich alicyclic molecules (CRAM).

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Ultrahigh resolution mass spectrometric differentiation of dissolved organic matter isolated by coupled reverse osmosis-electrodialysis from various major oceanic water masses

Cited by 59 publications

References 49 publications

Molecular and Optical Properties of Tree-Derived Dissolved Organic Matter in Throughfall and Stemflow from Live Oaks and Eastern Red Cedar

Molecular and Optical Properties of Tree-Derived Dissolved Organic Matter in Throughfall and Stemflow from Live Oaks and Eastern Red Cedar

Marine Photochemistry of Organic Matter

Spectroscopic characterization of oceanic dissolved organic matter isolated by reverse osmosis coupled with electrodialysis

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