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Selective Photochemical Oxidation of Reduced Dissolved Organic Sulfur to Inorganic Sulfate.

ABSTRACT: The chemical nature and stability of reduced dissolved organic sulfur (DOS_Red) have implications on the biogeochemical cycling of trace and major elements across fresh and marine aquatic environments, but the underlying processes governing DOS_Red stability remain obscure. Here, dissolved organic matter (DOM) was isolated from a sulfidic wetland, and laboratory experiments quantified dark and photochemical oxidation of DOS_Red using atomic-level measurement of sulfur X-ray absorption near-edge structure (XANES) spectroscopy. DOS_Red was completely resistant to oxidation by molecular oxygen in the dark and underwent rapid and quantitative oxidation to inorganic sulfate (SO₄^2-) in the presence of sunlight. The rate of DOS_Red oxidation to SO₄^2- greatly exceeded that of DOM photomineralization, resulting in a 50% loss of total DOS and 78% loss of DOS_Red over 192 h of irradiance. Sulfonates (DOS_SO3) and other minor oxidized DOS functionalities were not susceptible to photochemical oxidation. The observed susceptibility of DOS_Red to photodesulfurization, which has implications on carbon, sulfur, and mercury cycling, should be comprehensively evaluated across diverse aquatic environments of differing DOM composition.

SUBMITTER: Poulin BA

PROVIDER: S-EPMC10275504 | biostudies-literature | 2023 Jun

REPOSITORIES: biostudies-literature

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Selective Photochemical Oxidation of Reduced Dissolved Organic Sulfur to Inorganic Sulfate.

Poulin Brett A BA

Environmental science & technology letters 20230503 6

The chemical nature and stability of reduced dissolved organic sulfur (DOSRed) have implications on the biogeochemical cycling of trace and major elements across fresh and marine aquatic environments, but the underlying processes governing DOSRed stability remain obscure. Here, dissolved organic matter (DOM) was isolated from a sulfidic wetland, and laboratory experiments quantified dark and photochemical oxidation of DOSRed using atomic-level measurement of sulf ...[more]

PMID: 37333940

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Project description:The hydrothermal vent gammaproteobacterium Thiomicrospira crunogena inhabits an unstable environment and must endure dramatic sweeps in habitat chemistry. This sulfur chemolithoautotroph responds to changes in dissolved inorganic carbon (DIC; = CO2 + HCO3- + CO3-2) availability with a carbon concentrating mechanism (CCM), in which whole-cell affinity for DIC, as well as the intracellular DIC concentration, increase substantially under DIC-limitation. To determine whether this CCM is regulated at the level of transcription, cells cultivated under high-DIC conditions in chemostats were resuspended in growth medium with low concentrations of DIC, and CCM development was tracked in the presence and absence of RNA polymerase inhibitor rifampicin. The induction of the CCM, as measured by silicone oil centrifugation, was hindered in the presence of rifampicin. Similar results were observed for carboxysome gene transcription and assembly, as assayed by qRT-PCR and transmission electron microscopy, respectively. Genome-wide transcription patterns, assayed via microarrays, were compared for cells grown under DIC-limitation versus ammonia limitation. In addition to carboxysome genes, two novel genes (Tcr_1019 and Tcr_1315), present in other organisms including chemolithoautotrophs, but whose function(s) have not been elucidated in any organism, were found to be upregulated under low-DIC conditions. Likewise, under ammonia limitation, in addition to the expected enhancement of ammonia transporter and PII-gene transcription, the transcription of two novel genes was measurably enhanced (Tcr_0466 and Tcr_2018). Upregulation of all four genes was verified via qRT-PCR (Tcr_1019: 4-fold; Tcr_1315: ~7-fold; Tcr_0466: >200-fold; Tcr_2018: 7-fold), suggesting novel components are part of the response to nutrient limitation by this organism. In this study Thiomicrospira crunogena cells were grown under inorganic carbon limitation and ammonia limitation (high inorganic carbon concentrations) to examine genome wide transcription responses

Dataset Information

Selective Photochemical Oxidation of Reduced Dissolved Organic Sulfur to Inorganic Sulfate.

Publications

Selective Photochemical Oxidation of Reduced Dissolved Organic Sulfur to Inorganic Sulfate.

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