Formation of sulfur and nitrogen cross-linked macromolecules under aqueous conditions

Amrani, Alon; Turner, John; Ma, Qisheng; Tang, Yongchun; Hatcher, Patrick G.

doi:10.1016/j.gca.2007.06.051

Cited by 41 publications

(33 citation statements)

References 56 publications

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“…The detailed mechanism of sulfur incorporation in reduced sediments is unknown, but the most discussed possible mechanism for the sulfur incorporation is the Michael addition that would result in thiols (Krein and Aizenshtat, 1994;Movassagh and Shaygan, 2006;Amrani et al, 2007). As thiols were not detected here, it is likely that the thiols which are reactive nucleophiles themselves (Movassagh and Shaygan, 2006;Nair et al, 2014) incur a second Michael addition intraor intermolecularly to form thioethers.…”

Section: Potential Reaction Pathways Of Sulfur Incorporationmentioning

confidence: 86%

“…This experimental procedure was chosen because sulfide and S are present in sulfidic seawater and together form polysulfides (Adam et al, 1998). Polysulfides are the most nucleophilic species of reduced sulfur and likely the most important sulfur species for diagenetic sulfur incorporation into organic matter (Krein and Aizenshtat, 1994;Amrani et al, 2007). Long-term (4 weeks) sulfurization experiments were complemented by a very short (1-h) incubation.…”

Section: Sulfurization Experimentsmentioning

confidence: 99%

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Experimental Evidence for Abiotic Sulfurization of Marine Dissolved Organic Matter

et al. 2017

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Dissolved organic sulfur (DOS) is the largest pool of organic sulfur in the oceans, and as such it is an important component of the global sulfur cycle. DOS in the ocean is resistant against microbial degradation and turns over on a millennium time scale. However, sources and mechanisms behind its stability are largely unknown. Here, we hypothesize that in sulfate-reducing sediments sulfur is abiotically incorporated into dissolved organic matter (DOM) and released to the ocean. We exposed natural seawater and the filtrate of a plankton culture to sulfidic conditions. Already after 1-h at 20 • C, DOS concentrations had increased 4-fold in these experiments, and 14-fold after 4 weeks at 50 • C, indicating that organic matter does not need long residence times in natural sulfidic environments to be affected by sulfurization. Molecular analysis via ultrahigh-resolution mass spectrometry showed that sulfur was covalently and unselectively bound to DOM. Experimentally produced and natural DOS from sediments were highly similar on a molecular and structural level. By combining our data with published benthic DOC fluxes we estimate that 30-200 Tg DOS are annually transported from anaerobic and sulfate reducing sediments to the oceans. Uncertainties in this first speculative assessment are large. However, this first attempt illustrates that benthic DOS flux is potentially one order of magnitude larger than that via rivers indicating that this could balance the estimated global net removal of refractory DOS.

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Section: Potential Reaction Pathways Of Sulfur Incorporationmentioning

confidence: 86%

Section: Sulfurization Experimentsmentioning

confidence: 99%

Experimental Evidence for Abiotic Sulfurization of Marine Dissolved Organic Matter

et al. 2017

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“…Because macromolecules are non-volatile, their S 0 would contribute to both RSS T and RSS NV . Mechanisms to explain uptake include formation of organic polysulfides (R-S n À ) or polysulfanes (R-S n -R 0 ) (Vairavamurthy et al, 1997a;Amrani and Aizenshtat, 2004;Amrani et al, 2007). Alternatively, S 8 might be simply physically encapsulated by surfactant macromolecules.…”

Section: Analytes Contributing To Rss Measurementsmentioning

confidence: 99%

“…Similarly, sulfide and inorganic polysulfides are aggressive nucleophiles that facilitate important organic reactions, like the destruction of anthropogenic halocarbons (Barbash and Reinhard, 1989;Miller et al, 1998;Lippa and Roberts, 2002;Wu and Jans, 2006). They are involved in sulfidation and cross-linking reactions that produce biorefractory organic carbon in aquatic and sedimentary environments (Vairavamurthy et al, 1997a;Adam et al, 2000;Ciglenečki et al, 2000;Filley et al, 2002;Amrani and Aizenshtat, 2004;Amrani et al, 2007). In anoxic waters, they control redox processes by buffering Eh (Boulègue and Michard, 1979) and by stabilizing specific products in sometimes unexpected oxidation states (Helz et al, 2002;Vorlicek et al, 2004;Helz and Tossell, 2008).…”

Section: Introductionmentioning

confidence: 99%

Reduced sulfur species in a stratified seawater lake (Rogoznica Lake, Croatia); seasonal variations and argument for organic carriers of reactive sulfur

Bura-Nakić

Helz

Ciglenečki

et al. 2009

Geochimica et Cosmochimica Acta

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“…Sulfur-oxidizing bacteria can produce and store sulfur intra-or extra-cellularly (Van Gemerden and Mas 1995). Inorganic polysulfides readily react with organic and inorganic compounds abundant in sediments (Luther 1991;Amrani et al 2007).…”

Section: Introductionmentioning

confidence: 99%

Improved cyanolysis protocol for detection of zero‐valent sulfur in natural aquatic systems

Kamyshny

2009

Limnology & Ocean Methods

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We propose a novel protocol for detection of reactive zero-valent sulfur (ZVS) in natural aquatic samples including seawater. Reaction with hot potassium cyanide at slightly acidic conditions recovers ZVS from colloidal fraction of particulate elemental sulfur, polysulfides (S n 2-), and their protonated forms. Preconcentration by partial evaporation of the sample and separation of thiocyanate anions by high-performance liquid chromatography on the C30 reverse phase column modified with poly(ethylene glycol) followed by spectrophotometric detection at 220 nm wavelength allows us to detect reactive ZVS with detection limit of 3 nmol L -1 for fresh water samples and 6 nmol L -1 for seawater samples. Storage at 4°C for 6 weeks does not change the concentration of thiocyanate in the sample by more than 10%.

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Formation of sulfur and nitrogen cross-linked macromolecules under aqueous conditions

Cited by 41 publications

References 56 publications

Experimental Evidence for Abiotic Sulfurization of Marine Dissolved Organic Matter

Experimental Evidence for Abiotic Sulfurization of Marine Dissolved Organic Matter

Reduced sulfur species in a stratified seawater lake (Rogoznica Lake, Croatia); seasonal variations and argument for organic carriers of reactive sulfur

Improved cyanolysis protocol for detection of zero‐valent sulfur in natural aquatic systems

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