Fachgebiet Geochemie und Hydrogeologie
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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, Simultaneous speciation analysis of As, Sb and Se redox couples by SF-ICP-MS coupled to HPLCA new method was developed for the simultaneous speciation analysis of inorganic arsenic (III, V), antimony (III, V) and selenium (IV, VI) in fluid samples by double-focusing sector field-inductively coupled plasma-mass spectrometry (SF-ICP-MS) coupled with high performance liquid chromatography (HPLC). A Hamilton PRX-X100 anion exchange column with EDTA (pH of 4.7) and 3% methanol as mobile phase was used for separation of the six species. The flow rate was set at 1.5 mL min−1. The overall analysis time was shortened down to within 11 minutes for all six desired species after a solvent gradient (linear ramp from 5 mM to 30 mM) was introduced in. The detection limits for As(III), As(V), Sb(III), Sb(V), Se(VI) and Se(IV) were 0.02 μg L−1, 0.06 μg L−1, 0.2 μg L−1, 0.02 μg L−1, 0.2 μg L−1 and 0.4 μg L−1 respectively, which were obtained from 11 replicate measurements of blank. The stability of retention time and linearity of calibration curve were also evaluated. Relative standard deviations (RSD) of ≤9% for retention times (at least 20 replicate measurements) and correlation coefficients (R2) of ≥0.9998 for calibration curves (at least 6 replicate experiments) were obtained. Finally, the proposed method was applied to the analysis of one synthetic sample, two hot spring samples and two certified reference materials. The results showed a good spike recovery, indicating that basically no mass loss occurred during chromatographic separation. For two certified reference materials, the detected results were in good agreement with the certified values.Wissenschaftlicher ArtikelBand:6Heft:1466 121 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Understanding arsenic behavior in carbonate aquifers: Implications for aquifer storage and recovery (ASR)Geochemical reactive transport modeling was coupled to bench-scale leaching experiments to investigate and verify the mobilization of geogenic arsenic (As) under a range of redox conditions from an arsenic-rich pyrite bearing limestone aquifer. Modeling and experimental observations showed similar results and confirmed the following: (1) native groundwater and aquifer matrix, including pyrite, were in chemical equilibrium, thus preventing the release of As due to pyrite dissolution under ambient conditions; (2) mixing of oxygen- and nitrate-rich surface water with oxygen-depleted native groundwater changed the redox conditions and promoted the dissolution of pyrite, and (3) the behavior of As along a flow path was controlled by a complex series of interconnected reactions. This included the oxidative dissolution of pyrite and simultaneous sorption of As onto neo-formed hydrous ferric oxides (HFO), followed by the reductive dissolution of HFO and secondary release of adsorbed As under reducing conditions. Arsenic contamination of drinking water in these systems is thus controlled by the re-equilibration of the system to more reducing conditions rather than a purely oxidative process.Wissenschaftlicher ArtikelBand:5261 44 - 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 111 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Boron isotope variations in geothermal systems on Java, IndonesiaThis paper presents δ11B data for hot springs, hot acid crater lakes, geothermal brines and a steam vent from Java, Indonesia. The processes that produce a large range of the δ11B values were investigated, including the possible input of seawater as well as the contrast δ11B compositions of acid sulfate and acid chloride crater lakes. The δ11B values of hot springs ranged from − 2.4 to + 28.7‰ and acid crater lakes ranged from + 0.6 to + 34.9‰. The δ11B and Cl/B values in waters from the Parangtritis and Krakal geothermal systems confirmed seawater input. The δ11B values of acid sulfate crater lakes ranged from + 5.5 to + 34.9‰ and were higher than the δ11B of + 0.6‰ of the acid chloride crater lake. The heavier δ11B in the acid sulfate crater lakes was caused by a combination of vapor phase addition and further enrichment due to evaporation and B adsorption onto clay minerals. In contrast, the light δ11B of the acid chloride crater lake was a result of acid water-rocks interaction. The correlations of δ11B composition with δ18O and δ2H indicated that the B isotope corresponded to their groundwater mixing sources, but not for J21 (Segaran) and J48 (Cikundul) that underwent 11B isotope enrichment by B adsorption into minerals.Wissenschaftlicher ArtikelBand:31175 111 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Competitive Adsorption of As(III) and As(V) by Ferrihydrite: Equilibrium, Kinetics, and Surface ComplexationThe competitive/simultaneous adsorption of arsenite (As(III)) and arsenate (As(V)) onto ferrihydrite is one of main processes controlling the distribution of arsenic under oxidizing conditions in the natural environment. Adsorption reactions of As(III) and As(V) with ferrihydrite were investigated by employing a combination of batch adsorption experiments and Fourier transform infrared (FTIR) spectroscopy measurements in single and binary systems, i.e., both As species were present at the same time. Isotherm studies showed that the adsorption of As(III) in the binary system was less than that in single system, indicating that As(V) hindered As(III) adsorption. The presence of As(III) had almost no impact on As(V) adsorption at pH 5 in the binary systems. Freundlich model described the equilibrium data well (R 2 > 0.94), and the adsorption affinity onto ferrihydrite was in the following order: As(III)-single > As(III)-binary > As(V)-single > As(V)-binary. Kinetic data of As(III) and As(V) from single and binary systems were both well described by pseudo-second-order equation (R 2 > 0.98). FTIR showed that after adsorbing of either As species, a new peak occurred at 826 cm−1 due to the formation of Fe-O-As bonds, indicating that competition between As(III) and As(V) could take place on the surface sites as a result of the formation of a similar surface complexes.Wissenschaftlicher ArtikelBand:22779 65 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Determination of arsenic concentration and distribution in the Floridan Aquifer SystemHere we report on the different sampling strategies for almost seven years of sampling rocks/sediments for the determination of As within the Intermediate Aquifer System (IAS) and upper Floridan Aquifer System (FAS), a very large and productive limestone aquifer spanning from Georgia into Florida. In the FAS, As contamination has become a recurring problem during aquifer storage and recovery (ASR), particularly in central and south Florida. To investigate these phenomena, samples from solid drill cores and rock cuttings were collected from the Hawthorn Group, Suwannee Limestone, Ocala Limestone and Avon Park Formation. Samples were taken along drill cores and rock cuttings (referred to as ‘interval’ samples) or from particular drill core sections and rock cuttings (referred to as ‘targeted’ samples) likely to contain elevated concentrations of As as indicated by the presence of pyrite, hydrous ferric oxide, organic matter, clay minerals, fracture surfaces, and high permeable (moldic) zones. Arsenic was present in all of the stratigraphic units at low concentrations, close to the global average for As in limestone of 2.6 mg/kg. The highest As concentration was 69 mg/kg. In all units, however, the average bulk As concentration in the targeted samples was substantially higher than that in the interval samples. Based on direct spot measurements by electron microprobe and indirect calculations, pyrite was identified as the main source of As in the FAS. Concentrations in pyrite ranged from less than 100 mg/kg to more than 11,000 mg/kg. Because pyrite is heterogeneously distributed, both vertically and horizontally in the sampled stratigraphic units, the same was observed for the distribution of As. However, As concentrations generally decreased with depth, i.e., highest As values in the Hawthorn Group and lowest As values in the Ocala Limestone and Avon Park Formation. Compared to pyrite, other trace minerals contained much less As. The average As concentrations of the two types of sample media (solid cores and rock cuttings) were quite similar. These results indicate that if simply the average bulk rock As concentration of a geologic unit is the desired outcome of an investigation, either interval or targeted sampling of rock cuttings, seems to be sufficient. This is particularly important when time and money are a factor. This approach could work equally well for any other trace element. Structural sedimentary information, such as fractures, etc., is likely lost, however, when sampling rock cuttings. Thus, if this information is required, solid core samples need to be collected by hollow core diamond drilling.Wissenschaftlicher ArtikelBand:111Heft:3449 451 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Evaluating Complex Hydrogeological Settings in a Constructed Wetland: An Isotopic/Chemical Mass Balance ApproachThe objective of this study was to investigate the hydrogeological conditions of an artificial wetland, with four possible sources of water: (1) ground water, (2) industrial waste water, (3) seepage from a water body to the north, and (4) seepage from a water body to the south. The wetland was designed to improve the quality of municipal effluent and industrial wastewater. To evaluate and separate the impact of wetland processes from those due to dilution with water from “clean” sources (i.e., rain water or ground water), a combined isotope/chemical mass-balance approach was employed. The δD, δ18O, and Na were monitored for 18 months. Based on the data, the variation of individual proportions of each water type in the wetland and monitor wells was calculated. The isotopic composition of water in the wetland varied throughout the study period changing along the wetland flow path. The wetland contained mainly wastewater (88%–100%) during normal operations; however, hurricanes and inconsistent pumping added low conductivity water directly and triggered enhanced groundwater inflow into the wetland of up to 78%. Finally, the composition of water in monitor wells was mostly groundwater dominated; however seepage from a water body to the north was detected.Wissenschaftlicher ArtikelBand:3164 42 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Chemistry of hot springs along the Eastern Lau Spreading Center(Elsevier Science, 2011-02-15); ; ; ; The Eastern Lau Spreading Center (ELSC) is the southernmost part of the back-arc spreading axis in the Lau Basin, west of the Tonga trench and the active Tofua volcanic arc. Over its 397-km length it exhibits large and systematic changes in spreading rate, magmatic/tectonic processes, and proximity to the volcanic arc. In 2005, we collected 81 samples of vent water from six hydrothermal fields along the ELSC. The chemistry of these waters varies both within and between vent fields, in response to changes in substrate composition, temperature and pressure, pH, water/rock ratio, and input from magmatic gases and subducted sediment. Hot-spring temperatures range from 229° to 363 °C at the five northernmost fields, with a general decrease to the south that is reversed at the Mariner field. The southernmost field, Vai Lili, emitted water at up to 334 °C in 1989 but had a maximum venting temperature of only 121 °C in 2005, due to waning activity and admixture of bottom seawater into the subseafloor plumbing system. Chloride varies both within fields and from one field to another, from a low of 528 mmol/kg to a high of 656 mmol/kg, and may be enriched by phase separation and/or leaching of Cl from the rock. Concentrations of the soluble elements K, Rb, Cs, and B likewise increase southward as the volcanic substrate becomes more silica-rich, especially on the Valu Fa Ridge. Iodine and δ7Li increase southward, and δ11B decreases as B increases, apparently in response to increased input from subducted sediment as the arc is approached. Species that decrease southward as temperature falls are Si, H2S, Li, Na/Cl, Fe, Mn, and 87Sr/86Sr, whereas pH, alkalinity, Ca, and Sr increase. Oxygen isotopes indicate a higher water/rock ratio in the three systems on Valu Fa Ridge, consistent with higher porosity in more felsic volcanic rocks. Vent waters at the Mariner vent field on the Valu Fa Ridge are significantly hotter, more acid and metal-rich, less saline, and richer in dissolved gases and other volatiles, including H2S, CO2, and F, than the other vent fields, consistent with input of magmatic gases. The large variations in geologic and geophysical parameters produced by back-arc spreading along the ELSC, which exceed those along mid-ocean ridge spreading axes, produce similar large variations in the composition of vent waters, and thus provide new insights into the processes that control the chemistry of submarine hot springs.Wissenschaftlicher ArtikelBand:75Heft:479 132 - Some of the metrics are blocked by yourconsent settings
Item-typ:Veröffentlichung, Mercury in the hydrothermal fluids and gases in Paleochori Bay, Milos, Greece(Elsevier Science, 2021-06-20); ; ; Seafloor hydrothermal activity may constitute a considerable mercury (Hg) source to the oceans, but the flux from marine shallow-water hydrothermal systems (MSWHS) remains poorly constrained to date. To study the presence of Hg in MSWHS in Paleochori Bay (Milos Island, Greece), sea surface, bottom, pore fluid and hydrothermal gas samples were collected in June of 2017, October of 2018 and July of 2020, and analyzed for Cl, Br, SO4, As, Ca, Fe, K, Mg, Mn, Na, Si, Sr, H2S, unfiltered total Hg (THg), and filtered Hg (Hgdiss). Specific sites were selected for the analysis of volatile elemental Hg (Hgo), dimethylmercury (DMHg), monomethylmercury (MMHg), and Hg in the gas phase (Hggas). Concentrations of THg observed in samples collected from the sea surface were elevated compared to surface samples taken outside Paleochori Bay. The highest surface water concentrations (~10 to 15 pM) were measured in samples collected directly above shallow-water hydrothermal discharge areas. Pore fluids outside Paleochori Bay were significantly lower in THg (0.8 to 8.6 pM) than those taken inside (17.4 to 1511 pM). Porewaters collected from areas with visible gaseous or fluid emission were highly variable but generally elevated in THg concentrations (185 to 5066 pM). Concentrations within gases ranged from 0.7 to 2791 nmol/m3. The vast majority of samples with highly elevated THg (> 100 pM) had low Na/K ratios (< 15), indicative of rapidly rising fluid. Concentrations of Hg0, DMHg, and MMHg were below detection limits in all samples. Bottom substrate type (e.g., rocky vs. sediment covered) likely affected infiltration rates of oxygenated seawater below the sediment-water interface, thereby affecting Hg speciation and removal by precipitation. Flux rates from porewaters compared to those with gaseous emission were high (12.56 to 1088 mol THg/year and 0.37 to 1.85 mol THg/year). Sites with slow gaseous emission rates are hypothesized to have extended subsurface reaction times, resulting in lower Hg concentrations emitted to bottom waters. However, increasing rates of gas emission did not necessarily indicate higher Hg concentrations. The scavenging of Hg in the sediments and advective flux out of Paleochori Bay likely prevent significant accumulations of THg in the water column of Paleochori Bay. The total atmospheric flux from Paleochori Bay using average flux calculations over the entire surface area would contribute 6 mmol Hg/year to the atmosphere. We hypothesize that Hg concentrations within the pore fluids of Paleochori Bay reflect a balance between mixing and precipitation in the subsurface. A three-component mixing system of vapor, brine and seawater determines THg concentrations; however, precipitation due to sulfur cycling, changes in redox conditions and temperature, all play a crucial role in removing Hg from emitted fluids and gases.Wissenschaftlicher ArtikelBand:23366 69