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Aquatic Geochemistry
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  Hybrid Journal Hybrid journal (It can contain Open Access articles)
ISSN (Print) 1573-1421 - ISSN (Online) 1380-6165
Published by Springer-Verlag Homepage  [2467 journals]
  • Aggregation and Dispersion Behaviours of Riverine Trace Metals (Fe, Al, V,
           Mn, Ni, and Zn) and Organic Matter in Freshwater and Estuarine Conditions:
           A case study in Shira and Midori Rivers, Kumamoto, Japan

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      Abstract: Abstract The aggregation and dispersion of metals and organic matter are an important morphological alteration process for their transportation and bioavailability in coastal areas. However, variable mixing behaviours can be observed for some substances (e.g. Mn and Cu) due to the variable interaction systems in natural systems. In this study, riverine freshwater in the Shira and Midori rivers, Kumamoto, Japan, was mixed with artificial seawater to investigate the aggregation and dispersion behaviours of trace metals (i.e. Fe, Al, Mn, Zn, Cu, V, and Ni) and organic matter. In particular, their interactions were examined with differentiating the fast and slow transformations and considering the effects of suspended substances. Comparisons of sequential processes, including seawater mixing, decantation, centrifugation, and multiple filtrations, illustrated the aggregation and dispersion characteristics of the metals and organic matter as follows. A strong aggregating nature was evident for Fe in estuarine systems. In addition, the slow aggregation of Fe was accelerated by river-borne suspended substances. Small Fe (oxy)hydroxide particles were the major forms of dissolved Fe in both freshwater and estuarine systems and were partly associated with the other metals. In contrast, Zn and Ni were characterised by strong dispersion properties, although it can resorb onto suspended substances in estuarine systems. Synchronous behaviours with Zn and Ni were observed for V, Cu, and organic matter in the Midori River. The adsorption of Mn onto suspended substances was evident in the freshwater systems instead of the estuarine systems. Meanwhile, the behaviour of Mn is known to be dependent on its abundance in suspended forms, its redox state, and the influence of Fe. V and Cu, which are non-conservative in nature, were affected by other metals such as Fe, Zn, and Ni. Al, whose behaviour is largely dependent on the target estuary, which was also affected by other metals. Slow aggregation of organic matter was induced by suspended substances which were produced by fast transformation. In addition, evident interactions between suspended and dissolved substances were observed with the behaviours of Fe, Zn, Ni, and organic matter, indicating that the deposition and dispersion at the early stage of estuarine mixing can influence the subsequent slow transformation in real environments.
      PubDate: 2022-11-27
       
  • Microbial Acid Sulfate Weathering of Basaltic Rocks: Implication for
           Enzymatic Reactions

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      Abstract: Abstract Two basaltic rocks were reacted in acid sulfate and non-acid sulfate solutions with an initial pH value of 2 in the presence and absence of A. ferrooxidans to determine if basalt dissolution can support the metabolically active growth of A. ferrooxidans. Similar elemental release rates (RSi, RCa, RMg) calculated for both biotic and abiotic experiments suggest rather a negligible microbial impact on the dissolution of basaltic rocks within the acid sulfate solution. Nevertheless, in contrast with the abiotic experiments, measurements of remarkably high concentration of Fe(III)aq in microbial experiments confirmed the bacterial metabolism. Moreover, detected cell division and increasing total cell numbers with the extent of the experiments provide further evidence for the growth of metabolically active A. ferrooxidans during the dissolution of the rocks. Formation of jarosite ((K, Na, H3O)Fe3(SO4)2(OH)6) only in the biotic experiments is attributed to the microbially catalyzed Fe(II)aq oxidation. Overall, our results showed that acidic solutions that reacted with basaltic rocks can sustain the growth of Fe(II)aq oxidizing bacteria. Furthermore, identification of jarosite only in the biotic experiments emphasizes the enzymatic Fe(II) oxidation as the key step for its formation during basalt weathering at acid conditions, highlighting its biosignature potential on Earth and Earth-like planets (e.g., Mars).
      PubDate: 2022-09-29
       
  • Spatiotemporal Variations of Riverine CO2 Partial Pressure and its Effect
           on CO2 Flux at the Water–Air Interface in a Small Karst River

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      Abstract: Abstract In the global carbon cycle, rivers are the main transport channel for terrestrial carbon sources into the ocean, and their CO2 fluxes at the water–air interface affect the carbon budget. As an important component of the carbon cycle in the terrestrial ecosystem, karst regions exhibit carbon source and sink effects due to their special environmental conditions. To elaborate the spatial and temporal distribution of CO2 fluxes at the water–air interface of karst rivers and the influencing factors, systematic monitoring of small karst rivers in southwest China was conducted between November and December 2019 and between June and July 2020, respectively. The results show that: (1) the water chemistry of Chiwuxi River belonged to the HCO3–Ca–Mg type, and Ca2+ and HCO3− temporally showed a larger concentration in the dry season than in the wet season. (2) CO2 partial pressure (pCO2) and CO2 fluxes showed a seasonal characteristic of higher values in the wet season than in the dry season. pCO2 ranged from 323.59 to 1380.38 μatm and CO2 fluxes ranged from −24.31 to 353.74 mmol (m2 d)−1. During the wet season, the Chiwuxi River showed a carbon source effect. During the dry season, the photosynthesis of aquatic plants reduced CO2 outgassing. (3) Isotopic compositions of dissolved inorganic carbon (δ13CDIC) showed a higher value in the dry season than in the wet season. The dissolved inorganic carbon mainly originated from soil CO2 and carbonate weathering. To improve the understanding of riverine carbon cycling, it is necessary to study CO2 fluxes at the water–air interface of small rivers in the karst region. Thus, this will help to reduce the uncertainty of CO2 fluxes in global rivers.
      PubDate: 2022-09-13
      DOI: 10.1007/s10498-022-09406-9
       
  • Influence of Diverse Urban Pressures on Water Characteristics in a Small
           Eastern Mediterranean Watershed

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      Abstract: Abstract This work focuses on the characterization of a typical coastal karst watershed by addressing its physico-chemical parameters. The concentrations of the main ions clearly indicate the dominance of Ca2+ and HCO3− with a carbonate weathering rate equivalent to 230t/Km2/year; that is a typical weathering of karst watersheds. The spatio-temporal variability of dissolved organic matter (DOM) is also assessed in the watershed. Many samples were collected under different hydrological conditions from three representative sites. The evolution of OM composition along an urbanization gradient from upstream to downstream Kadisha watershed reveals the very strong impact of urban discharges on the receiving waters. Substantial differences in DOC results are highlighted in relation to the urban or natural origin of the DOM. Upstream OM flux is quantified and compared to downstream OM flux showing that, during the low flow period, the downstream flux is 29 times higher than the upstream. Also, a large fraction of non-humic substances, including hydrophilic organic matter HPI, is detected in the downstream section impacted by urban discharges. The higher values of SUVA noticed for DOM at upstream compared to downstream, reflects the low aromaticity and non-humic character of DOM in downstream. These outcomes show the impact of the Tripoli urban discharges on the quality and quantity of OM in the receiving waters downstream of the Kadisha catchment. This is typical at low water period when the dilution factor of urban discharges in the receiving waters is the least.
      PubDate: 2022-06-17
      DOI: 10.1007/s10498-022-09405-w
       
  • Fluid–Rock Interactions in Geothermal Reservoirs, Germany: Thermal
           Autoclave Experiments Using Sandstones and Natural Hydrothermal Brines

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      Abstract: Abstract As renewable energy, geothermal can contribute substantially to the energy transition. To generate electricity or to harvest heat, high-saline fluids are tapped by wells of a few kilometres and extracted from hydrothermal reservoirs. After the heat exchanger units have been passed by, these fluids are reinjected into the reservoir. Due to the pressure and temperature differences between the subsurface and the surface, as well as the cooling of the fluids in the power plant, unwanted chemical reactions can occur within the reservoir, in the borehole, and within the power plant itself. This can reduce the permeability of the reservoir as well as the output of the geothermal power plant. This study aims to simulate real subsurface reactions using batch and leaching experiments with sandstone or sandstone powder as solid phase, and deionised water or natural brine as liquid phase. It is demonstrated that fluid composition changes after only a few days. In particular, calcite, aragonite, clay minerals, and zinc phases precipitate from the natural brine. In contrast, in particular minerals containing potassium, arsenic, barium, and silica are dissolved. Due to the experimental set-up, these mineral reactions mainly took place on the surface of the samples, which is why no substantial changes in petrophysical properties could be observed. However, it is assumed that the observed reactions on the reservoir scale have a relevant influence on parameters such as permeability.
      PubDate: 2022-05-31
      DOI: 10.1007/s10498-022-09404-x
       
  • Geochemical Proxies and Mineralogical Fingerprints of Sedimentary
           Processes in a Closed Shallow Lake Basin Since 1850

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      Abstract: Lake systems are essential for the environment, the biosphere, and humans but are highly impacted by anthropogenic activities accentuated by climate change. Understanding how lake ecosystems change due to human impacts and natural forces is crucial to managing their current state and possible future restoration. The high sensitivity of shallow closed lakes to natural and anthropogenic forcing makes these lacustrine ecosystems highly prone to variations in precipitation and sedimentation processes. These variation processes, occurring in the water column, produce geochemical markers or proxies recorded in lake sedimentary archives. This study investigated specific proxies on high-resolution sedimentary archives (2–3 years resolution) of the Trasimeno lake (Central Italy). The Trasimeno lake underwent three different hydrological phases during the twentieth century due to several fluctuations induced mainly by human activities and climate change. The Trasimeno lake, a large and shallow basin located in the Mediterranean area, is a good case study to assess the effects of intense anthropogenic activity related to agriculture, tourism, industry, and climate changes during the Anthropocene. The aim is to identify the main characteristics of the main sedimentary events in the lake during the last 150 years, determining the concentrations of major and trace elements, the amount of organic matter, and the mineralogical composition of the sediments. This type of work demonstrates that studying sediment archives at high resolution is a viable method for reconstructing the lake’s history through the evolution/trends of the geochemical proxies stored in the sediment records. This effort makes it possible to assess past anthropogenic impact and, under the objectives of the European Green Deal (zero-pollution ambition for a toxic-free environment), to monitor, prevent, and remedy pollution related to soil and water compartments. Graphical abstract
      PubDate: 2022-02-13
      DOI: 10.1007/s10498-022-09403-y
       
  • A Late Holocene Record of Variations in the Chemical Weathering Intensity
           and Pedogenesis in a Lake Catchment from Southern India

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      Abstract: Abstract We investigated the detrital influx, chemical weathering intensity, provenance and pedogenesis over the past 2,500 years in the catchment of Pookot Lake, southern India. The down-core variations of metal/Al ratios (Na/Al, K/Al, Mg/Al, Ca/Al, Fe/Al, Mn/Al, Zn/Al, Ba/Al) of the Pookot sediments indicate changes in the rainfall-induced terrigenous inflow to the lake. In contrast, fluctuations in the chemical index of alteration (CIA) and Rb/Sr values denote the variability in the strength of chemical weathering in the watershed of the lake. The results show that the detrital influx, and hence rainfall, remained steady except during 1500–600 cal. years B.P. (high) and 600–300 cal. year B.P. (low) in the Pookot lake catchment. However, the periods of high/low chemical weathering intensity in the catchment do not correspond to periods of high/low detrital influx to the lake basin. The similar shale-normalized rare earth elemental curves point to a uniform provenance. The past pedogenic activity is indicated by pedogenic χlf and pedogenic χfd derived from citrate-bicarbonate-dithionite (CBD) extraction. The data indicate that the fine-grained magnetite/maghemite formed during the pedogenesis mainly contributes to the magnetic signal of sediments. The degree of pedogenesis was strong during 2500–2000 cal. years B.P. and moderate throughout 1500–600 cal. years B.P. The pedogenic intensity became stronger again during ~ 600 cal. years B.P., which weakened between 600 and 300 cal. years B.P. and remained steady thereafter. The present study indicates that detrital influx proxies like metal/Al ratios are more suitable for reconstructing past climate in tropical climate rather than chemical weathering indices.
      PubDate: 2022-01-11
      DOI: 10.1007/s10498-021-09402-5
       
  • Upwelling of Deep-seated Fluid in the Sikhote-Alin Region, Far East of the
           Eurasian Plate

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      Abstract: Abstract Spring waters with high-pCO2 content are widely distributed in the Sikhote-Alin region in Russia. Mukhen spa is one such spring located in the northern Sikhote-Alin region. This spa has two types of upwelling spring waters and exhibits distinct chemical signatures. One of the springs originates from a shallow aquifer and features hydrogen and oxygen isotopic ratios of meteoric water with a high 3He/4He ratio, whereas the other originates from a deeper aquifer and features a distinctly negative δ18O with a lower 3He/4He ratio. To understand this apparent discrepancy and the water circulation dynamics beneath Mukhen springs, we utilized all published data concerning the major solute elements and isotopic ratios of Mukhen spring waters and compared them with the He isotopic compositions on several springs in the far eastern region, which are newly analyzed in this study. The results show that the shallow aquifer comprises meteoric water that interacts with the crust enhanced by the gas component welling up from deep underground, while the fluid in deep aquifer fingerprinted the hydration reaction of silicate and involves a mantle component possibly delivered by a deep-seated fluid and/or gas upwelling along the tectonic fault through the western margin of the Sikhote-Alin region.
      PubDate: 2021-12-01
      DOI: 10.1007/s10498-021-09398-y
       
  • Temporal and Spatial Variabilities of Chemical and Physical Parameters on
           the Heron Island Coral Reef Platform

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      Abstract: Abstract Globally, coral reefs are threatened by ocean warming and acidification. The degree to which acidification will impact reefs is dependent on the local hydrodynamics, benthic community composition, and biogeochemical processes, all of which vary on different temporal and spatial scales. Characterizing the natural spatiotemporal variability of seawater carbonate chemistry across different reefs is critical for elucidating future impacts on coral reefs. To date, most studies have focused on select habitats, whereas fewer studies have focused on reef scale variability. Here, we investigate the temporal and spatial seawater physicochemical variability across the entire Heron Island coral reef platform, Great Barrier Reef, Australia, for a limited duration of six days. Autonomous sensor measurements at three sites across the platform were complemented by reef-wide boat surveys and discrete sampling of seawater carbonate chemistry during the morning and evening. Variability in both temporal and spatial physicochemical properties were predominantly driven by solar irradiance (and its effect on biological activity) and the semidiurnal tidal cycles but were influenced by the local geomorphology resulting in isolation of the platform during low tide and rapid flooding during rising tides. As a result, seawater from previous tidal cycles was sometimes trapped in different parts of the reef leading to unexpected biogeochemical trends in space and time. This study illustrates the differences and limitations of data obtained from high-frequency measurements in a few locations compared to low-frequency measurements at high spatial resolution and coverage, showing the need for a combined approach to develop predictive capability of seawater physicochemical properties on coral reefs.
      PubDate: 2021-12-01
      DOI: 10.1007/s10498-021-09400-7
       
  • Organic versus Inorganic Carbon Exports from Glacier and Permafrost
           Watersheds in Qinghai–Tibet Plateau

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      Abstract: Abstract In a warming climate, land-to-water carbon mobilization is increasing in glacier and permafrost area. To identify the connection between exported river carbon content and the permafrost or glacier condition in the high-altitude mountain area, we studied the dissolved organic carbon and dissolved inorganic carbon concentration in three streams of Qinghai–Tibet Plateau (QTP), which were located in the continuous permafrost, seasonal permafrost and glacial basin, respectively. It was found that the DIC and DOC concentrations were lower in the glacial rivers compared with the permafrost derived rivers; but more DOC would be exported from glacier due to the large amount of melted glacier water in the high mountainous area. DIC/DOC ratio in rivers reflected the watershed landscape types. In the permafrost area, the river recharged by seasonal permafrost had higher DIC concentration than the river in the continuous permafrost region, suggesting that increased DIC concentration could be a precursor of permafrost degradation. Research is meaningful to estimate the DOC and DIC export from high mountain area.
      PubDate: 2021-12-01
      DOI: 10.1007/s10498-021-09399-x
       
  • Oxygen Consumption of Resuspended Sediments of the Upper Elbe Estuary:
           Process Identification and Prognosis

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      Abstract: Abstract The resuspension of sediment leads to an increased release of nutrients and organic substances into the overlying water column, which can have a negative effect on the oxygen budget. Especially in the warmer months with a lower oxygen saturation and higher biological activity, the oxygen content can reach critical thresholds in estuaries like the upper Elbe estuary. Many studies have dealt with the nutrient fluxes that occur during a resuspension event. However, the sediment properties that influence the oxygen consumption potential (OCP) and the different biochemical processes have not been examined in detail. To fill this gap, we investigated the biogeochemical composition, texture, and OCP of sediments at 21 locations as well as the temporal variability within one location for a period of 2 years (monthly sampling) in the upper Elbe estuary. The OCP of sediments during a seven-day resuspension event can be described by the processes of sulphate formation, nitrification, and mineralisation. Chlorophyll, total nitrogen (Ntotal), and total organic carbon showed the highest correlations with the OCP. Based on these correlations, we developed a prognosis model to calculate the OCP for the upper Elbe estuary with a single sediment parameter (Ntotal). The model is well suited to calculate the oxygen consumption of resuspended sediments in the Hamburg port area during the relevant warmer months and shows a normalised root mean squared error of < 0.11 ± 0.13. Thus, the effect of maintenance measures such as water injection dredging and ship-induced wave on the oxygen budget of the water can be calculated.
      PubDate: 2021-11-30
      DOI: 10.1007/s10498-021-09401-6
       
  • The Abiotic Nitrite Oxidation by Ligand-Bound Manganese (III): The
           Chemical Mechanism

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      Abstract: Abstract Given their environmental abundances, it has been long hypothesized that geochemical interactions between reactive forms of manganese and nitrogen may play important roles in the cycling of these elements. Indeed, recent studies have begun shedding light on the possible role of soluble, ligand-bound Mn(III) in promoting abiotic transformations under environmentally relevant conditions. Here, using the kinetic data of Karolewski et al. (Geochim Cosmochim Acta 293:365–378, 2021), we provide the chemical mechanism for the abiotic oxidation of nitrite (NO2−) by Mn(III)-pyrophosphate, MnIIIPP, to form nitrate (NO3−). Nitrous acid (HNO2), not NO2−, is the reductant in the reaction, based on thermodynamic and kinetic considerations. As soluble Mn(III) complexes react in a one-electron transfer reaction, two one-electron transfer steps must occur. In step one, HNO2 is first oxidized to nitrogen dioxide, ·NO2, a free radical via a hydrogen atom transfer (HAT) reaction. We show that this inner sphere reaction process is the rate-limiting step in the reaction sequence. In step two, ·NO2 reacts with a second MnIIIPP complex to form the nitronium ion (NO2+), which is isoelectronic with CO2. Unlike the poor electron-accepting capability of CO2, NO2+ is an excellent electron acceptor for both OH− and H2O, so NO2+ reacts quickly with water to form the end-product NO3− (step 3 in the reaction sequence). Thus, water provides the O atom in this nitrification reaction in accordance with the O-isotope data. This work provides mechanistic perspective on a potentially important interaction between Mn and nitrogen species, thereby offering a framework in which to interpret kinetic and isotopic data and to further investigate the relevance of this reaction under environmental conditions.
      PubDate: 2021-09-01
      DOI: 10.1007/s10498-021-09396-0
       
  • Chemical weathering and carbon dioxide consumption in a small tropical
           river catchment, southwestern India

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      Abstract: Abstract Studies done on small tropical west-flowing river catchments located in the Western Ghats in southwestern India have suggested very intense chemical weathering rates and associated CO2 consumption. Very less studies are reported from these catchments notwithstanding their importance as potential sinks of atmospheric CO2 at the global scale. A total of 156 samples were collected from a small river catchment in the southwestern India, the Payaswini–Chandragiri river Basin, during pre-monsoon, monsoon and post-monsoon seasons in 2016 and 2017, respectively. This river system comprises two small rivers originating at an elevation of 1350 m in the Western Ghats in peninsular India. The catchment area is dominated by biotite sillimanite gneiss. Sodium is the dominant cation, contributing ~ 50% of the total cations, whereas HCO3− contributes ~ 75% of total anions. The average anion concentration in the samples varied in the range HCO3− > Cl− > SO42− > NO3− > F−, whereas major cation concentration varied in the range Na+  > Ca2+  > Mg2+  > K+. The average silicate weathering rate (SWR) was 42 t km−2 y−1 in the year 2016 and 36 t km−2 y−1 in 2017. The average annual carbon dioxide consumption rate (CCR) due to silicate rock weathering was 9.6 × 105 mol km−2y−1 and 8.3 × 105 mol km−2 y−1 for 2016 and 2017, respectively. The CCR in the study area is higher than other large tropical river catchments like Amazon, Congo-Zaire, Orinoco, Parana and Indus because of its unique topography, hot and humid climate and intense rainfall.
      PubDate: 2021-09-01
      DOI: 10.1007/s10498-021-09394-2
       
  • Carbonate Alkalinity Enhances Triclosan Photolysis

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      Abstract: Abstract Triclosan (TCS) is an antimicrobial compound found in many household products used across the world. TCS is not completely removed in wastewater systems, resulting in trace-level concentrations present ubiquitously in surface waters. The direct photodegradation of TCS has been widely studied, with results indicating that TCS breaks down to chlorophenols and dioxins. To date, no studies have specifically investigated the effects of alkalinity on the photolysis of the acidic form of TCS. This study assessed the effect of carbonate/bicarbonate alkalinity, which is ubiquitous in natural waters, on the photolysis rate of TCS. Results indicate that bicarbonate enhances the photodegradation of TCS at pH values well below the pKa of TCS (7.9), with direct photolysis reaction kinetics that are very slow in the absence of buffers, but significant in the presence of bicarbonate (0.711 h−1 at pH 6.55). At pH values well above its pKa, both unbuffered- and buffered-mediated photolysis increased dramatically (1.92 h−1 for direct photolysis and 2.86 h−1 in buffered water) and is attributable to the increased photoreactivity of TCS by its conjugate base. Photolysis of methyl triclosan (MeTCS), a non-acidic analog of TCS, demonstrated the importance of TCS’s acidic functionality as MeTCS did not degrade at any pH. The observed influence of alkalinity on the acidic form of TCS photolysis was attributed to both a decrease in its excited state pKa, coupled with TCS deprotonation through an excited state proton transfer to a base (bicarbonate and to a lesser degree hydrogen phosphate) resulting in the more photo-labile conjugate base form of TCS.
      PubDate: 2021-09-01
      DOI: 10.1007/s10498-021-09397-z
       
  • Contribution of Hydrothermal Processes to the Enrichment of Lithium in
           Brines: Evidence from Water–Rock Interacting Experiments

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      Abstract: Abstract Over the world, the available lithium (Li) resources are reserved mainly in closed-basin brines, with high Li concentration (> 150 mg/L) and low Mg/Li ratio (< 10) being critical for Li extraction using precipitation-based methods. In order to investigate the enrichment of Li over Mg during the formation of Li brine deposits, batch water–rock interacting experiments between igneous rocks and aqueous solutions were carried out under low (25, 50 and 75 °C) and high (200, 300 and 400 °C) temperature conditions. Our results show that for the experiments using water and accomplished under 25 °C, the Mg and Li concentrations vary from 0.470 and 0.782 mg/L in the solution interacted with Li-rich granite, to 5.626 and < 0.002 mg/L in that interacted with basalt, with Mg/Li ratio being slightly higher than those of the igneous rocks. By contrast, while a NaCl or Na2SO4 solution was used, the Mg and Li concentrations can be improved by up to tens of times, and the Mg/Li ratio also increased slightly. Lastly and above all, with increase in the water–rock interacting temperature from 25 to 400 °C, the Mg and Li concentrations in all solutions vary conversely and the Mg/Li ratio decreases by orders of magnitude, leading to the formation of Li-rich brines with very low Mg/Li ratios at temperatures above 200 °C. By comparing the results from our experiment to those from Li-rich springs, rivers and closed-basin brines, we conclude that water evaporation over time is fundamental for the concentration of Li in brines, meanwhile high-temperature hydrothermal processes are key to the formation of Li brine deposits with low Mg/Li ratios.
      PubDate: 2021-09-01
      DOI: 10.1007/s10498-021-09395-1
       
  • Metal Speciation in Water of the Flooded Mine “Arsenic” (Karelia,
           Russia): Equilibrium-Kinetic Modeling with a Focus on the Influence of
           Humic Substances

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      Abstract: Abstract Equilibrium-kinetic modeling allows investigating metal behavior in the water–rock-organic matter system with time to evaluate anthropogenic effects on the environment. In the article, the interactions of stagnant mine drainage water of the flooded mine “Arsenic” with ore and gangue minerals were simulated using different organic matter incorporation approaches. If the model is closed to humic substances (no additional organic matter input), most fulvic acids are bound in the Fe fulvate complex. While under the removal of Fe fulvate from the model, the Cu fulvate becomes prevalent, the contribution of the fulvate complexes with Zn, Mg, and Ca also increases. This scenario simulates the organo-mineral complexes behavior well and allows identifying the sequence of metal binding to organic ligands as follows Fe > Cu > Zn > Mg > Ca. The second scenario imitates the constant input of organic matter to the model (open system regarding humic substances). The dissolved metal concentrations in the model solution are extremely high in comparison to the mine drainage water. This scenario demonstrates that excessive input of organic matter leads to the accumulation of the metals in a dissolved form and blocks the secondary mineral formation despite the faster dissolution of the primary minerals under a more acidic pH than in the first scenario. However, despite the differences between the model solution and the mine drainage water, this scenario is useful to address specific issues associated with changes in natural and anthropogenic conditions. Both scenarios show the importance of organic matter incorporation to the equilibrium-kinetic models.
      PubDate: 2021-06-01
      DOI: 10.1007/s10498-021-09393-3
       
  • Climate Change-Induced Changes in the Chemistry of a High-Altitude
           Mountain Lake in the Central Alps

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      Abstract: Abstract Mountains are among the most sensitive ecosystems to climate change, and one of the most evident signs of climate-related effect is the continuous net loss of ice from the cryosphere. Several studies showed that meltwater from glaciated and perennially frozen areas can profoundly affect alpine aquatic ecosystems. Here, we present the impressive temporal increase in solutes in Lake Leit, a mountain lake in the Central Alps that is impacted by an active rock glacier. During the last 30 years, concentrations of sulfate and base cations increased by factors of 4 and 3, respectively. Atmospheric deposition, the only catchment external source, could be excluded as possible cause. The inlets have sulfate and base cations concentrations that were up to double the concentrations of the lake outlet confirming the presence of catchment internal sources. The highest concentrations were measured in the springs at the bottom of the rock glacier. Ground surface temperatures of the rock glacier indicated a high probability of permafrost occurrence, while the annual mean air temperature after the mid-1980s showed continuously positive deviations from the long-term average values (period 1961–1990) with increasing values after 2010. δ34S of sulfate in the inlets and the outflow indicated that sulfate in Lake Leit mainly derived from dissolution of gypsum/anhydrite even if its presence is not confirmed by the Geologic Atlas of Switzerland. Because of these results, we postulate the presence of subsurface traces of sulfate-bearing evaporites, probably associated with Triassic metasediments. These deposits are very common in the closer surroundings. We further hypothesize that the thawing of permafrost affects the flow path of water enabling its contact with fresh highly weatherable minerals increasing the overall weathering rate and shifting the relative ionic composition in the discharge toward the ions that originate from the most soluble minerals. This study shows that increased permafrost thawing in the future can influence water quality in high-alpine settings.
      PubDate: 2021-06-01
      DOI: 10.1007/s10498-020-09388-6
       
  • Free Eu(III) Determination by Donnan Membrane Technique with
           Electrochemical Detection: Implementation and Evaluation

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      Abstract: Abstract The aim of this study was to develop an analytical method to determine free concentrations of Europium (Eu(III)) in natural waters. Europium(III) in solution was detected using cathodic stripping voltammetry after complexation with N-nitroso-N-phenylhydroxylamine (cupferron). Optimization of analytical parameters allowed us to detect nanomolar levels of Eu(III) in solution. Free Eu(III) in solution was measured using the Donnan membrane technique in which a natural solution (the “donor”, containing various ligands) is separated from a ligand-free solution (the “acceptor”) by a cation-exchange membrane. This membrane allows only non-colloidal cationic species to pass through it, and after an adequate time equilibrium is reached between both compartments. Total Eu(III) concentration can then be quantified in the acceptor solution and related to free Eu(III) in the natural sample. Due to its high valency, free Eu(III) tends to adsorb strongly to the cation-exchange membrane. In order to determine the physicochemical conditions minimizing this adsorption, we analyzed solutions of different Eu(III) and Ca(II) (as background ion) concentrations. Results showed that 100 mM of Ca(II) were necessary to make adsorption of Eu(III) onto the membrane negligible. The optimized setup was then used to quantify Eu(III) complexation in a Eu(III)-dissolved organic matter solution.
      PubDate: 2021-06-01
      DOI: 10.1007/s10498-021-09392-4
       
  • Effects of Bioirrigation and Salinity on Arsenic Distributions in
           Ferruginous Concretions from Salt Marsh Sediment Cores (Southern Brazil)

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      Abstract: Abstract Arsenic (As), iron (Fe), and manganese (Mn) contents were measured in sediment nodules and associated pore waters obtained from sediment cores collected from a salt marsh on Pólvora Island (southern Brazil). Sediment cores were obtained when brackish water dominated the estuary, at two different environments: an unvegetated mudflat colonized by crabs (Neohelice granulata), and a low intertidal stand vegetated by Spartina alterniflora. We determined the percentage of nodules in each depth interval of the cores, along with redox potential, and As, Fe, and Mn contents of the nodules. The mineralogy of the nodules was investigated, and results showed they are mainly composed by quartz, phyllosilicates, and amorphous Fe–Mn oxides/oxyhydroxides. Pore water results showed that bioturbation by local crabs supports oxygen penetration to depths of ca. 25 cm below the salt marsh surface, with lower Fe contents in pore water associated with the brackish period. However, S. alterniflora growth appears to have a greater impact on sediment geochemistry of Fe, Mn, and possibly As due to sulfate reduction and the associated decrease in pore water pH. Higher Fe concentrations were observed in the pore waters during the period of brackish water dominance, which also corresponded to the S. alterniflora growth season. The study demonstrates that differences in geochemical conditions (e.g., Fe content) that can develop in salt marsh sediments owing to different types of bioirrigation processes (i.e., bioirrigation driven by crabs versus that related to the growth of S. alterniflora) play important roles in the biogeochemical cycling of As.
      PubDate: 2021-06-01
      DOI: 10.1007/s10498-020-09387-7
       
  • Kinetics of Thiocyanate Formation by Reaction of Cyanide with
           Tetrathionate

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      Abstract: Abstract In aquatic systems a reaction between tetrathionate and cyanide results in the formation of thiocyanate. We have studied kinetics of the reactions of tetrathionate with free cyanide and two cyanide complexes, hexacyanoferrate(II) and hexacyanoferrate(III), at the environmentally relevant conditions. For the reaction between tetrathionate and free cyanide, the rate constant and the activation energy, but not the reaction order, strongly depend on pH. Our observations allow to propose the following pathways of thiocyanate formation by the reactions of free cyanide with tetrathionate: (1) tetrathionate reacts relatively slow with hydrogen cyanide at acidic and neutral conditions; and (2) tetrathionate reacts relatively fast with cyanide anion under highly alkaline conditions. Depending on environmental conditions, the half-lives of the reaction between free cyanide and tetrathionate will be in the ranges of hours to several years. Reactions of tetrathionate with hexacyanoferrate(II) and hexacyanoferrate(III) have no environmental significance as they are slower than the decomposition of tetrathionate. Strategy for improvement of analytical protocols for analysis of tetrathionate and cyanide is proposed based on the detected kinetics parameters.
      PubDate: 2021-03-01
      DOI: 10.1007/s10498-020-09385-9
       
 
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