Bühring, Solveig
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Bühring, Solveig
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Bühring, Solveig
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Bühring, Solveig I.
Bühring, Solveig Irena
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Item-typ:Veröffentlichung, Arsenic and sulfur nanoparticle synthesis mimicking environmental conditions of submarine shallow-water hydrothermal vents(2022-01); ; ; Arsenic and sulfur mineralization is a natural phenomenon occurring in hydrothermal systems where parameters like temperature and organic matter (OM) can influence the mobilization of the toxic metalloid in marine environments. In the present study we analyze the influence of temperature and OM (particularly sulfur-containing additives) on As and S precipitation based on the recent discovery of As-rich nanoparticles in the hydrothermal system near the coast of the Greek island Milos. To this end, we experimentally recreate the formation of amorphous colloidal particles rich in As and S via acidification (pH 3-4) of aqueous precursors at various temperatures. At higher temperatures, we observe the formation of monodisperse particles within the first 24 h of the experiment, generating colloidal particles with diameters close to 160 nm. The S:As ratio and particle size of the synthetized particles closely correlates with values for AsxSy particles detected in the hydrothermal system off Milos. Furthermore, organic sulfur containing additives (cysteine and glutathione, GSH) are a key factor in the process of nucleation and growth of amorphous colloidal AsxSy particles and, together with the temperature gradient present in shallow hydrothermal vents, dictate the stabilization of As-bearing nanomaterials in the environment. Based on these findings, we present a simple model that summarizes our new insights into the formation and mobility of colloidal As in aquatic ecosystems. In this context, amorphous AsxSy particles can present harmful effects to micro- and macro-biota not foreseen in bulk As material.Buch136 105 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Amorphous arsenic sulfide nanoparticles in a shallow water hydrothermal system(Elsevier Science, 2019-04-23); ; ; ; Hydrothermal fluids can contain trace elements such as arsenic (As), which are toxic to surrounding biota. In these kind of fluids, the bioavailability and biotransformation of As have been investigated but so far the ratio of total soluble As (<200 nm) versus the amount of As contained in a nanoparticulate phase has not been reported. Here, for the first time, the presence of As in the nanoparticulate fraction (between 200 and 20 nm) is described for arsenic-rich hydrothermal fluids in a marine shallow-water hydrothermal system. Samples of diffusively venting hydrothermal fluids, pore-water and seawater were collected in the hydrothermal system located in Paleochori Bay, Milos Island (Greece), and the fraction between 200 and 20 nm (As200-20) was studied. Up to 38% of the soluble arsenic was present within the As200-20 fraction in pore fluids, 10 to 20% in hydrothermal fluids and 5% in seawater. Identification and characterization of particles in hydrothermal fluid, pore-water and seawater was performed by scanning electron microscopy coupled to energy dispersive X-ray spectroscopy (SEM-EDX), transmission electron microscopy (TEM) with selected area electron diffraction (SAED) and dynamic light scattering (DLS). The particles are of spherical morphology with a polydisperse size distribution (PDI: 0.37) and diameters close to 100 nm. EDX studies confirmed a chemical composition rich in As and S. The SAED pattern revealed absence of a crystal phase indicating the presence of an amorphous arsenic sulfide material. These results bring into discussion the role of the nanoparticulate fraction for As dispersion, bioavailability, and potentially harmful effects in marine coastal ecosystems.Wissenschaftlicher ArtikelBand:211100 156 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Molecular evidence for abiotic sulfurization of dissolved organic matter in marine shallow hydrothermal systems(Elsevier Science, 2016-10-01); ; ; ; Shallow submarine hydrothermal systems are extreme environments with strong redox gradients at the interface of hot, reduced fluids and cold, oxygenated seawater. Hydrothermal fluids are often depleted in sulfate when compared to surrounding seawater and can contain high concentrations of hydrogen sulfide (H2S). It is well known that sulfur in its various oxidation states plays an important role in processing and transformation of organic matter. However, the formation and the reactivity of dissolved organic sulfur (DOS) in the water column at hydrothermal systems are so far not well understood. We investigated DOS dynamics and its relation to the physicochemical environment by studying the molecular composition of dissolved organic matter (DOM) in three contrasting shallow hydrothermal systems off Milos (Eastern Mediterranean), Dominica (Caribbean Sea) and Iceland (North Atlantic). We used ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) to characterize the DOM on a molecular level. The molecular information was complemented with general geochemical data, quantitative dissolved organic carbon (DOC) and DOS analyses as well as isotopic measurements (δ2H, δ18O and F14C). In contrast to the predominantly meteoric fluids from Dominica and Iceland, hydrothermal fluids from Milos were mainly fed by recirculating seawater. The hydrothermal fluids from Milos were enriched in H2S and DOS, as indicated by high DOS/DOC ratios and by the fact that >90% of all assigned DOM formulas that were exclusively present in the fluids contained sulfur. In all three systems, DOS from hydrothermal fluids had on average lower O/C ratios (0.26–0.34) than surrounding surface seawater DOS (0.45–0.52), suggesting shallow hydrothermal systems as a source of reduced DOS, which will likely get oxidized upon contact with oxygenated seawater. Evaluation of hypothetical sulfurization reactions suggests DOM reduction and sulfurization during seawater recirculation in Milos seafloor. The four most effective potential sulfurization reactions were those exchanging an O atom by one S atom in the formula or the equivalent + H2S reaction, correspondingly exchanging H2O, H2 and/or O2 by a H2S molecule. Our study reveals novel insights into DOS dynamics in marine hydrothermal environments and provides a conceptual framework for molecular-scale mechanisms in organic sulfur geochemistry.Wissenschaftlicher ArtikelBand:190105 107