A potential formation route for CHOS compounds in dissolved organic matter

Melendez‐Perez, Jose J.; Martínez-Mejía, Mónica J.; Barcellos, Roberto Lima; Filho, A. F. H. Fetter; Eberlin, Marcos N.

doi:10.1016/j.marchem.2018.03.006

Cited by 17 publications

(11 citation statements)

References 27 publications

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“…It also appears that there is a higher abundance of DOS formulas in anoxic (Schmidt et al, 2009) versus oxic (Rossel et al, 2016) sediment pore waters, consistent with higher production of organic sulfur compounds in anoxic relative to oxic sediments (Werne et al, 2004 and references within). Through laboratory experiments, Melendez-Perez et al (2018) proposed that the addition of sulfide species to lignin-like CHO compounds (with sediment minerals acting as catalysts) could serve as a possible pathway for the formation of polyoxygenated organic sulfur compounds (CHOS). To identify DOS formulas that are potentially formed in shallow hydrothermal systems through abiotic sulfurization reactions, Gomez-Saez et al (2016) used FTICR-MS to track nine possible sulfur addition reactions that involve addition or removal of hydrogen and/or oxygen atoms (a total of 27 potential sulfurization reactions).…”

Section: Introductionmentioning

confidence: 99%

Abiotic formation of dissolved organic sulfur in anoxic sediments of Santa Barbara Basin

Abdulla

Burdige

Komada

2020

Organic Geochemistry

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Sulfurization has been found to enhance organic matter preservation and petroleum formation in marine sediments. However, we do not yet have a comprehensive understanding of sulfurization mechanisms. In this study, we investigated several possible mechanisms of dissolved organic sulfur (DOS) formation in the top 4.5 m of anoxic sediments of Santa Barbara Basin (SBB), California Borderland. Using Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS), we identified chemical formulas of potential dissolved organic matter (DOM) precursors to these DOS compounds. We also examined how the formulas of abiotically formed DOS changed as a function of depth across a major redox gradient. Results show that abiotic nucleophilic addition reactions involving bisulfide (HS À) and polysulfide (HS x À) are the major sulfurization pathways that form DOS in anoxic pore waters of SBB sediments. We identified 2124 unique DOS formulas that could be generated from the addition of HS À and HS x À to 2203 DOM formulas, and this accounted for $70% of all DOS formulas detected in these pore waters. Examining the DOM formulas that served as reactants in the abiotic sulfurization reactions, we found that 64% contained only carbon, hydrogen, and oxygen (CHO formulas) while the remainder (34%) included nitrogen (DON formulas). Our results revealed high reactivity toward sulfurization among many of the CHO and DON formulas that have H/C and O/C elemental ratios that overlap with those of carboxylrich alicyclic molecules (CRAM). This specific class of formulas could play an important role in the formation of organic sulfur compounds in sulfidic marine ecosystems, and in the formation of sulfur-containing protokerogen in marine sediments. Our results further suggest that anoxic sediments are a source of DOS compounds to the oceans.

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Section: Introductionmentioning

confidence: 99%

Abiotic formation of dissolved organic sulfur in anoxic sediments of Santa Barbara Basin

Abdulla

Burdige

Komada

2020

Organic Geochemistry

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“…Abundant S-containing molecules in sulfur-rich environments have been reported. , However, CHOS molecules exhibited relatively lower abundances in the surface water than in the deeper water of the AMD lake (Figure ). This phenomenon can be caused by the faster photodegradation of CHOS molecules than that of CHO and CHON molecules. , This also explained the decreased molecular weight of CHOS molecules at 0.5 m. In addition, the remarkable reduction in the O/C ratio of CHOS molecules at 0.5 m suggested a potential decarboxylation process . The photochemical production of sulfate and volatile S-containing compounds from dissolved organic sulfur in AMD lakes can be considered …”

Section: Discussionmentioning

confidence: 91%

“…18,42 This also explained the decreased molecular weight of CHOS molecules at 0.5 m. In addition, the remarkable reduction in the O/C ratio of CHOS molecules at 0.5 m suggested a potential decarboxylation process. 43 The photochemical production of sulfate and volatile S-containing compounds from dissolved organic sulfur in AMD lakes can be considered. 44 4.2.…”

Section: Discussionmentioning

confidence: 99%

“…The high abundance of heteroatom-containing compounds in the bottom likely resulted from N-rich microbial metabolites and large-scale sulfurization products in anoxic bottom layer. 43,58…”

Section: Discussionmentioning

confidence: 99%

“… , Another feature of DOM quality in the bottom layer was the higher proportions of CHNO and CHOS compounds (Figures , S4 and S5). The high abundance of heteroatom-containing compounds in the bottom likely resulted from N-rich microbial metabolites and large-scale sulfurization products in anoxic bottom layer. , …”

Section: Discussionmentioning

confidence: 99%

See 2 more Smart Citations

The Stratified Distribution of Dissolved Organic Matter in an AMD Lake Revealed by Multi-sample Evaluation Procedure

She

Wang

Pan

et al. 2021

Environ. Sci. Technol.

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As a typical extreme environment, acid mine drainage (AMD) has been extensively studied for its biogeochemical cycle, but little is known about the quality of dissolved organic matter (DOM) in AMD. In this study, DOM molecules in an AMD lake were detected with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), and the change of DOM molecules in the stratified water column was analyzed with a multi-sample evaluation procedure. The results demonstrate that DOM quality is highly stratified and can be linked with severe biogeochemical gradients. In the surface layer, DOM molecules can be distinguished by low quantities and intensities, as well as potential photodegradation products. Oxygen-poor and oxygen-rich molecules alternately dominate the chemocline, which can be explained by the redox-dependent adsorption/desorption of DOM on metastable secondary minerals. A rich and abundant DOM pool with a high proportion of heteroatoms exists at the bottom which can be significantly influenced by material exchange with sediments. These findings emphasize the active role of DOM in extreme AMD environments and expand the understanding of the carbon cycle in the hydrosphere.

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Characterizing photochemical production carboxyl content of dissolved organic matters using absorbance spectroscopy combined with FT-ICR MS

Wei,

Li,

Zhang

et al. 2023

Chemosphere

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A potential formation route for CHOS compounds in dissolved organic matter

Cited by 17 publications

References 27 publications

Abiotic formation of dissolved organic sulfur in anoxic sediments of Santa Barbara Basin

Abiotic formation of dissolved organic sulfur in anoxic sediments of Santa Barbara Basin

The Stratified Distribution of Dissolved Organic Matter in an AMD Lake Revealed by Multi-sample Evaluation Procedure

Characterizing photochemical production carboxyl content of dissolved organic matters using absorbance spectroscopy combined with FT-ICR MS

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