Photochemical Production of Sulfate and Methanesulfonic Acid from Dissolved Organic Sulfur

Ossola, Rachele; Tolu, Julie; Clerc, Baptiste; Erickson, Paul R.; Winkel, Lenny H. E.; McNeill, Kristopher

doi:10.1021/acs.est.9b04721

Cited by 37 publications

(62 citation statements)

References 56 publications

(126 reference statements)

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“…For example, one study demonstrated substantial photo‐oxidation of organic sulfur within DOM (Gomez‐Saez et al ., 2017). Another study showed that organic sulfur within terrigenous DOM is readily mineralized to sulfate by sunlight (Ossola et al ., 2019).…”

Section: Resultsmentioning

confidence: 99%

Experimental metatranscriptomics reveals the costs and benefits of dissolved organic matter photo‐alteration for freshwater microbes

Nalven

Ward

Payet

et al. 2020

Environmental Microbiology

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Summary Microbes and sunlight convert terrigenous dissolved organic matter (DOM) in surface waters to greenhouse gases. Prior studies show contrasting results about how biological and photochemical processes interact to contribute to the degradation of DOM. In this study, DOM leached from the organic layer of tundra soil was exposed to natural sunlight or kept in the dark, incubated in the dark with the natural microbial community, and analysed for gene expression and DOM chemical composition. Microbial gene expression (metatranscriptomics) in light and dark treatments diverged substantially after 4 h. Gene expression suggested that sunlight exposure of DOM initially stimulated microbial growth by (i) replacing the function of enzymes that degrade higher molecular weight DOM such as enzymes for aromatic carbon degradation, oxygenation, and decarboxylation, and (ii) releasing low molecular weight compounds and inorganic nutrients from DOM. However, growth stimulation following sunlight exposure of DOM came at a cost. Sunlight depleted the pool of aromatic compounds that supported microbial growth in the dark treatment, ultimately causing slower growth in the light treatment over 5 days. These first measurements of microbial metatranscriptomic responses to photo‐alteration of DOM provide a mechanistic explanation for how sunlight exposure of terrigenous DOM alters microbial processing and respiration of DOM.

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Section: Resultsmentioning

confidence: 99%

Experimental metatranscriptomics reveals the costs and benefits of dissolved organic matter photo‐alteration for freshwater microbes

Nalven

Ward

Payet

et al. 2020

Environmental Microbiology

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“…Stock solutions of 500 mg L –1 DOM in ultrapure water were produced from the International Humic Substances Society’s (IHSS) “Upper Mississippi River NOM” (UMRNOM, cat no: 1R110N; IHSS, St. Paul, USA) and the “Pony lake fulvic acid” (PLFA, cat no: 1R109F; IHSS, St. Paul, USA) and stored in amber glass vials after the pH was set to ca . 10 with sodium hydroxide solution (NaOH, 32%, Merck, Darmstadt, Germany). The NOM stock solutions were then sonicated for 2 × 10 min in an ultrasonic bath (SONOREX Super 10 P, Berlin, Germany), followed by a readjustment of the pH value to the target pH, using a diluted nitric acid solution (10%; 1.7 M) (HNO 3 , Roth, HNO 3 Suprapur 69%).…”

Section: Methodsmentioning

confidence: 99%

“…10 with sodium hydroxide solution (NaOH, 32%, Merck, Darmstadt, Germany). The NOM stock solutions were then sonicated for 2 × 10 min in an ultrasonic bath (SONOREX Super 10 P, Berlin, Germany), followed by a readjustment of the pH value to the target pH, using a diluted nitric acid solution (10%; 1.7 M) (HNO 3 , Roth, HNO 3 Suprapur 69%). The NOM stock solutions were stored at 4 °C and used within 1 week.…”

Section: Methodsmentioning

confidence: 99%

Reaction of DMS and HOBr as a Sink for Marine DMS and an Inhibitor of Bromoform Formation

Müller

Gunten

Bouchet

et al. 2021

Environ. Sci. Technol.

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Recently, we suggested that hypobromous acid (HOBr) is a sink for the marine volatile organic sulfur compound dimethyl sulfide (DMS). However, HOBr is also known to react with reactive moieties of dissolved organic matter (DOM) such as phenolic compounds to form bromoform (CHBr3) and other brominated compounds. The reaction between HOBr and DMS may thus compete with the reaction between HOBr and DOM. To study this potential competition, kinetic batch and diffusion-reactor experiments with DMS, HOBr, and DOM were performed. Based on the reaction kinetics, we modeled concentrations of DMS, HOBr, and CHBr3 during typical algal bloom fluxes of DMS and HOBr (10–13 to 10–9 M s–1). For an intermediate to high HOBr flux (≥10–11 M s–1) and a DMS flux ≤10–11 M s–1, the model shows that the DMS degradation by HOBr was higher than for photochemical oxidation, biological consumption, and sea–air gas exchange combined. For HOBr fluxes ≤10–11 M s–1 and a DMS flux of 10–11 M s–1, our model shows that CHBr3 decreases by 86% compared to a lower DMS flux of 10–12 M s–1. Therefore, the reaction between HOBr and DMS likely not only presents a sink for DMS but also may lead to suppressed CHBr3 formation.

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“…Aquatic photochemistry is an interdisciplinary field that examines how sunlight-driven reactions impact the fate and composition of diverse materials in surface waters, including major and minor elements (e.g., C, − N, , O, , S, P, Fe, , and Mn), inorganic and organic pollutants (e.g., heavy metals, , crude oil, − pharmaceuticals and personal care products, , pesticides, and plastics , ), and biomolecules (e.g., lipids, , amino acids, , and pigments). Accurate assessment of photochemical processes requires information about the reaction kinetics, which depend on the light available at different wavelengths throughout the water column and the photochemical reaction efficiency, or apparent quantum yield (AQY; mol product per mol light absorbed), at those wavelengths.…”

Section: Introductionmentioning

confidence: 99%

Rapid and Reproducible Characterization of the Wavelength Dependence of Aquatic Photochemical Reactions Using Light-Emitting Diodes

Ward

Bowen

Freeman

et al. 2021

Environ. Sci. Technol. Lett.

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Arguably, the largest knowledge gap in the aquatic photochemistry discipline is the wavelength dependence of sunlight-driven reaction rates in surface waters. Here, we introduce a new light-emitting diode (LED)-based approach to directly quantify the wavelength dependence of aquatic photochemical reaction rates. The LEDs generate narrowbanded, spatially uniform light at five wavelengths (275, 309, 348, 369, and 406 nm), with irradiances that are stable and easily adjusted to desired levels. Strong agreement was observed between irradiance measurements in each LED reactor using chemical actinometry and spectroradiometry. Apparent quantum yield (AQY) spectra of photochemical oxygen consumption by Suwannee River organic matter were determined four times across a sixmonth period. The shape and magnitude of the AQY spectra were highly reproducible, as indicated by strong exponential fits (R 2 ≥ 0.98) and low variability in oxidation rates across the four trials (coefficient of variation = ∼10%). This LED-based approach is cost effective, high throughput, and portable, allowing a broader community to study the wavelength dependence of aquatic photochemical processes in more detail than was previously possible. We anticipate that this approach will substantially advance our understanding of the wavelength dependence of photochemical reactions in surface waters and improve the accuracy of kinetic models.

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Photochemical Production of Sulfate and Methanesulfonic Acid from Dissolved Organic Sulfur

Cited by 37 publications

References 56 publications

Experimental metatranscriptomics reveals the costs and benefits of dissolved organic matter photo‐alteration for freshwater microbes

Experimental metatranscriptomics reveals the costs and benefits of dissolved organic matter photo‐alteration for freshwater microbes

Reaction of DMS and HOBr as a Sink for Marine DMS and an Inhibitor of Bromoform Formation

Rapid and Reproducible Characterization of the Wavelength Dependence of Aquatic Photochemical Reactions Using Light-Emitting Diodes

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