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  • 1
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    Development of Iron Speciation Reference Materials for Palaeoredox Analysis (2020)
    Wiley
    Details
    Publication Date: 2020-07-10
    Print ISSN: 1639-4488
    Electronic ISSN: 1751-908X
    Topics: Geosciences
    Published by Wiley
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  • 2
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    Arsenic in framboidal pyrite from recent sediments of a shallow water lagoon of the Baltic Sea (2013)
    Wiley
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    Publication Date: 2013-04-01
    Print ISSN: 0037-0746
    Electronic ISSN: 1365-3091
    Topics: Geosciences
    Published by Wiley
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  • 3
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    A revised global estimate of dissolved iron fluxes from marine sediments (2015)
    AGU (American Geophysical Union) | Wiley
    In:  Global Biogeochemical Cycles, 29 (5). pp. 691-707.
    Details
    Publication Date: 2019-09-23
    Description: Literature data on benthic dissolved iron (DFe) fluxes (µmol m−2 d−1), bottom water oxygen concentrations (O2BW, μM), and sedimentary carbon oxidation rates (COX, mmol m−2 d−1) from water depths ranging from 80 to 3700 m were assembled. The data were analyzed with a diagenetic iron model to derive an empirical function for predicting benthic DFe fluxes: inline image where γ (= 170 µmol m−2 d−1) is the maximum flux for sediments at steady state located away from river mouths. This simple function unifies previous observations that COX and O2BW are important controls on DFe fluxes. Upscaling predicts a global DFe flux from continental margin sediments of 109 ± 55 Gmol yr−1, of which 72 Gmol yr−1 is contributed by the shelf (〈200 m) and 37 Gmol yr−1 by slope sediments (200–2000 m). The predicted deep-sea flux (〉2000 m) of 41 ± 21 Gmol yr−1 is unsupported by empirical data. Previous estimates of benthic DFe fluxes derived using global iron models are far lower (approximately 10–30 Gmol yr−1). This can be attributed to (i) inadequate treatment of the role of oxygen on benthic DFe fluxes and (ii) improper consideration of continental shelf processes due to coarse spatial resolution. Globally averaged DFe concentrations in surface waters simulated with the intermediate-complexity University of Victoria Earth System Climate Model were a factor of 2 higher with the new function. We conclude that (i) the DFe flux from marginal sediments has been underestimated in the marine iron cycle and (ii) iron scavenging in the water column is more intense than currently presumed.
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  • 4
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    Fault zone controlled seafloor methane seepage in the rupture area of the 2010 Maule Earthquake, Central Chile (2016)
    AGU (American Geophysical Union) | Wiley
    In:  Geochemistry, Geophysics, Geosystems, 17 (11). pp. 4802-4813.
    Details
    Publication Date: 2020-06-29
    Description: Seafloor seepage of hydrocarbon-bearing fluids has been identified in a number of marine forearcs. However, temporal variations in seep activity and the structural and tectonic parameters that control the seepage often remain poorly constrained. Subduction-zone earthquakes for example, are often discussed to trigger seafloor seepage but causal links that go beyond theoretical considerations have not yet been fully established. This is mainly due to the inaccessibility of offshore epicentral areas, the infrequent occurrence of large earthquakes, and challenges associated with offshore monitoring of seepage over large areas and sufficient time periods. Here, we report visual, geochemical, geophysical, and modelling results and observations from the Concepción Methane Seep Area (offshore Central Chile) located in the rupture area of the 2010 Mw. 8.8 Maule earthquake. High methane concentrations in the oceanic water column and a shallow sub-bottom depth of sulfate penetration indicate active methane seepage. The stable carbon isotope signature of the methane and hydrocarbon composition of the released gas indicate a mixture of shallow-sourced biogenic gas and a deeper sourced thermogenic component. Pristine fissures and fractures observed at the seafloor together with seismically imaged large faults in the marine forearc may represent effective pathways for methane migration. Upper-plate fault activity with hydraulic fracturing and dilation is in line with increased normal Coulomb stress during large plate-boundary earthquakes, as exemplarily modelled for the 2010 earthquake. On a global perspective our results point out the possible role of recurring large subduction-zone earthquakes in driving hydrocarbon seepage from marine forearcs over long timescales.
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  • 5
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    Development of Iron Speciation Reference Materials for Palaeoredox Analysis (2020)
    Wiley
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    Publication Date: 2023-02-08
    Description: The development and application of geochemical techniques to identify redox conditions in modern and ancient aquatic environments has intensified over recent years. Iron (Fe) speciation has emerged as one of the most widely used procedures to distinguish different redox regimes in both the water column and sediments, and is the main technique used to identify oxic, ferruginous (anoxic, Fe(II) containing) and euxinic (anoxic, sulfidic) water column conditions. However, an international sediment reference material has never been developed. This has led to concern over the consistency of results published by the many laboratories that now utilise the technique. Here, we report an interlaboratory comparison of four Fe speciation reference materials for palaeoredox analysis, which span a range of compositions and reflect deposition under different redox conditions. We provide an update of extraction techniques used in Fe speciation and assess the effects of both test portion mass, and the use of different analytical procedures, on the quantification of different Fe fractions in sedimentary rocks. While atomic absorption spectroscopy and inductively coupled plasma‐optical emission spectrometry produced comparable Fe measurements for all extraction stages, the use of ferrozine consistently underestimated Fe in the extraction step targeting mixed ferrous–ferric minerals such as magnetite. We therefore suggest that the use of ferrozine is discontinued for this Fe pool. Finally, we report the combined data of four independent Fe speciation laboratories to characterise the Fe speciation composition of the reference materials. These reference materials are available to the community to provide an essential validation of in‐house Fe speciation measurements.
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  • 6
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    Recycling and burial of biogenic silica in an open margin oxygen minimum zone (2021)
    AGU (American Geophysical Union) | Wiley
    Details
    Publication Date: 2024-02-07
    Description: An extensive data set of biogenic silica (BSi) fluxes is presented for the Peruvian oxygen minimum zone (OMZ) at 11ºS and 12ºS. Each transect extends from the shelf to the upper slope (∼1000 m) and dissects the permanently anoxic waters between ∼200 – 500m water depth. BSi burial (2100 mmol m‐2 yr‐1) and recycling fluxes (3300 mmol m‐2 yr‐1) were highest on the shelf with mean preservation efficiencies (34±15%) that exceed the global mean of 10 – 20%. BSi preservation was highest on the inner shelf (up to 56%), decreasing to 7% and 12% under anoxic waters and below the OMZ, respectively. The data suggest that the main control on BSi preservation is the rate at which reactive BSi is transported away from undersaturated surface sediments by burial and bioturbation to the underlying saturated sediment layers where BSi dissolution is thermodynamically and/or kinetically inhibited. BSi burial across the entire Peruvian margin between 3ºS to 15ºS and down to 1000m water depth is estimated to be 0.1 – 0.2 Tmol yr‐1; equivalent to 2 – 7% of total burial on continental margins. Existing global data permit a simple relationship between BSi rain rate to the seafloor and the accumulation of unaltered BSi, giving the possibility to reconstruct rain rates and primary production from the sediment archive in addition to benthic Si turnover in global models.
    Type: Article , PeerReviewed
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  • 7
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    The Fate of Sedimentary Reactive Iron at the Land‐Ocean Interface:A Case Study from the Amazon Shelf (2022)
    AGU (American Geophysical Union) | Wiley
    Details
    Publication Date: 2024-02-07
    Description: Reactive iron (Fe) oxides in marine sediments may represent a source of bioavailable Fe to the ocean via reductive dissolution and sedimentary Fe release or can promote organic carbon preservation and long-term burial. Furthermore, enrichments of reactive Fe (sum of Fe oxides, carbonates and sulfides normalized to total Fe) in ancient sediments are utilized as a paleo-proxy for anoxic conditions. Considering the general importance of reactive Fe oxides in marine biogeochemistry, it is important to quantify their terrestrial sources and fate at the land-ocean interface. We applied sequential Fe extractions to sediments from the Amazon shelf to investigate the transformation of river-derived Fe oxides during early diagenesis. We found that ∼22 % of the Amazon River-derived Fe oxides are converted to Fe-containing clay minerals in Amazon shelf sediments. The incorporation of reactive Fe into authigenic clay minerals (commonly referred to as reverse weathering) is substantiated by the relationship between Fe oxide loss and potassium (K) uptake from sedimentary pore waters, which is in agreement with the previously reported Fe/K stoichiometry of authigenic clay minerals. Mass balance calculations suggest that widely applied sequential extractions do not separate Fe-rich authigenic clay minerals from reactive Fe oxides and carbonates. We conclude that the balance between terrestrial supply of reactive Fe and reverse weathering in continental margin sediments has to be taken into account in the interpretation of sedimentary Fe speciation data. Key Points - Reactive Fe is transferred from river-derived Fe oxides into Fe-containing silicate minerals during early diagenesis - Standard sequential extraction schemes do not separate Fe oxides and carbonates from authigenic silicate minerals in Amazon shelf sediments - Terrigenous supply of reactive Fe and reverse weathering need to be considered in the interpretation of sedimentary Fe speciation
    Type: Article , PeerReviewed
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  • 8
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    Stable Barium Isotope Fractionation in Pore Waters of Estuarine Sediments (2023)
    Wiley | AGU (American Geophysical Union)
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    Publication Date: 2024-02-07
    Description: The development of stable barium (Ba) isotope measurements provides a novel tool to investigate the geochemical cycling of Ba in the ocean and its sediments. In sediment pore waters, gradients of dissolved Ba concentrations result from various diagenetic processes. The distribution and fractionation of Ba isotopes in the pore waters are expected to further improve our understanding of these early diagenetic control mechanisms. Here, we present pore water profiles of dissolved stable Ba isotopic signatures (δ138Bapw) from shallow water sediments covering the entire Pearl River Estuary (PRE) in Southern China. We find pronounced depth-dependent Ba isotope variations generally showing a shift from heavy to light δ138Bapw signatures from the sediment surface down to 15 cm depth. These gradients are well reproduced by a diffusion-reaction model, which generates an apparent fractionation factor (138ε) of −0.60 ± 0.10‰ pointing to preferential removal of low-mass Ba isotopes from the pore water during solution-solid phase interactions. Consequently, the combined diagenetic processes induce the highest δ138Bapw values of +0.5 to +0.7‰ in the pore waters of the topmost sediment layer. Although the detrital fraction dominates the Ba content in the PRE surface sediments, the determined gradients of pore water Ba isotopes, together with concentration variations of Ba and other redox-sensitive elements such as manganese (Mn), show that non-detrital excess Ba carriers including Mn oxides and authigenic barite clearly affect the post-depositional Ba dynamics. Stable Ba isotopes are thus a potentially powerful tracer of Ba geochemistry during early sediment diagenesis in estuarine depositional environments. Key Points We present a data set of dissolved stable Ba isotopic compositions in surface sediment pore waters of a large river estuary Pore water Ba isotope values generally decrease with increasing sediment depth, reflecting post-depositional Ba isotope fractionation A diffusion-reaction model predicts the distribution and fractionation of stable Ba isotopes in the sediment pore waters well
    Type: Article , PeerReviewed
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  • 9
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    Constraining global marine iron sources and ligand-mediated scavenging fluxes with GEOTRACES dissolved iron measurements in an ocean biogeochemical model (2021)
    AGU (American Geophysical Union) | Wiley
    Details
    Publication Date: 2024-02-07
    Description: Iron is a key micronutrient controlling phytoplankton growth in vast regions of the global ocean. Despite its importance, uncertainties remain high regarding external iron source fluxes and internal cycling on a global scale. In this study, we used a global dissolved iron dataset, including GEOTRACES measurements, to constrain source and scavenging fluxes in the marine iron component of a global ocean biogeochemical model. Our model simulations tested three key uncertainties: source inputs of atmospheric soluble iron deposition (varying from 1.4–3.4 Gmol/yr), reductive sedimentary iron release (14–117 Gmol/yr), and compared a variable ligand parameterization to a constant distribution. In each simulation, scavenging rates were tuned to reproduce the observed global mean iron inventory for consistency. The variable ligand parameterization improved the global model-data misfit the most, suggesting that heterotrophic bacteria are an important source of ligands to the ocean. Model simulations containing high source fluxes of atmospheric soluble iron deposition (3.4 Gmol/yr) and reductive sedimentary iron release (114 Gmol/yr) further improved the model most notably in the surface ocean. High scavenging rates were then required to maintain the iron inventory resulting in relatively short surface and global ocean residence times of 0.83 and 7.5 years, respectively. The model simulates a tight spatial coupling between source inputs and scavenging rates, which may be too strong due to underrepresented ligands near source inputs, contributing to large uncertainties when constraining individual fluxes with dissolved iron concentrations. Model biases remain high and are discussed to help improve global marine iron cycle models.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
    Format: other
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  • 10
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    A novel device for trace metal‐clean sampling of bottom water and suspended particles at the ocean's lower boundary: The Benthic Trace Profiler (2022)
    Wiley | ASLO (Association for the Sciences of Limnology and Oceanography)
    Details
    Publication Date: 2024-02-07
    Description: The benthic boundary layer plays a crucial role in the exchange of trace metals between surface sediments and the water column. So far it has been difficult to study dissolved–particulate interactions of trace metals in this highly reactive interface layer due to the lack of suitable sampling methods. We developed a new device, called Benthic Trace Profiler (BTP), which enables simultaneous sampling of near-bottom water and suspended particles in high depth resolution within the first 3 m above the seafloor. The device was tested successfully in the Baltic Sea. The concentrations of several trace metals (Co, Ni, Cu, Zn, and Cd) in the collected bottom waters overlapped with concentrations in water column samples above collected with conventional methods. This observation indicates that the sampling device and method is trace metal clean. The trace metals Fe and Mn showed concentration gradients within the benthic boundary layer indicating an upward diffusive flux. This observation is consistent with a diffusive benthic flux of these trace metals across the sediment–water interface, which was independently verified using pore-water profiles. Suspended particles can be used to study precipitation processes and to determine the carrier phases of trace metals. The BTP fulfilled all the intended requirements as it allowed a simultaneous, uncontaminating and oxygen-free sampling of seawater and suspended particles to gather high-resolution profiles of dissolved and particulate trace metal concentrations above the seafloor. The device closes the gap between water column and sediment sampling and helps researchers to better understand trace metal exchange processes across the ocean's lower boundary.
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