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  • PANGAEA  (283)
  • Frontiers  (10)
  • Wiley  (9)
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  • 1
    Publication Date: 2018-02-28
    Description: Geochemical data (CH4, SO42−, I−, Cl−, particulate organic carbon (POC), δ13C-CH4, and δ13C-CO2) are presented from the upper 30 m of marine sediment on a tectonic submarine accretionary wedge offshore southwest Taiwan. The sampling stations covered three ridges (Tai-Nan, Yung-An, and Good Weather), each characterized by bottom simulating reflectors, acoustic turbidity, and different types of faulting and anticlines. Sulfate and iodide concentrations varied little from seawater-like values in the upper 1–3 m of sediment at all stations; a feature that is consistent with irrigation of seawater by gas bubbles rising through the soft surface sediments. Below this depth, sulfate was rapidly consumed within 5–10 m by anaerobic oxidation of methane (AOM) at the sulfate-methane transition. Carbon isotopic data imply a mainly biogenic methane source. A numerical transport-reaction model was used to identify the supply pathways of methane and estimate depth-integrated turnover rates at the three ridges. Methane gas ascending from deep layers, facilitated by thrusts and faults, was by far the dominant term in the methane budget at all sites. Differences in the proximity of the sampling sites to the faults and anticlines mainly accounted for the variability in gas fluxes and depth-integrated AOM rates. By comparison, methane produced in situ by POC degradation within the modeled sediment column was unimportant. This study demonstrates that the geochemical trends in the continental margins offshore SW Taiwan are closely related to the different geological settings.
    Type: Article , PeerReviewed
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  • 2
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    AGU (American Geophysical Union) | Wiley
    In:  Global Biogeochemical Cycles, 29 . pp. 812-829.
    Publication Date: 2017-12-19
    Description: An empirical function is derived for predicting the rate-depth profile of particulate organic carbon (POC) degradation in surface marine sediments including the bioturbated layer. The rate takes the form of a power law analogous to the Middelburg function. The functional parameters were optimized by simulating measured benthic O2 and NO3− fluxes at 185 stations worldwide using a diagenetic model. The novelty of this work rests with the finding that the vertically-resolved POC degradation rate in the bioturbated zone can be determined using a simple function where the POC rain rate is the governing variable. Although imperfect, the model is able to fit 71 % of paired O2 and NO3− fluxes to within 50% of measured values. It further provides realistic geochemical concentration-depth profiles, NO3− penetration depths and apparent first-order POC mineralization rate constants. The model performs less well on the continental shelf due to the high heterogeneity there. When applied to globally resolved maps of rain rate, the model predicts a global denitrification rate of 182 ± 88 Tg yr−1 of N and a POC burial rate of 107 ± 52 Tg yr−1 of C with a mean carbon burial efficiency of 6.1%. These results are in very good agreement with published values. Our proposed function is conceptually simple, requires less parameterization than multi-G type models and is suitable for non-steady state applications. It provides a basis for more accurately simulating benthic nutrient fluxes and carbonate dissolution rates in Earth system models.
    Type: Article , PeerReviewed
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  • 3
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    AGU (American Geophysical Union) | Wiley
    In:  Global Biogeochemical Cycles, 29 (5). pp. 691-707.
    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.
    Type: Article , PeerReviewed
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  • 4
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    AGU (American Geophysical Union) | Wiley
    In:  Geochemistry, Geophysics, Geosystems, 18 (5). pp. 1959-1985.
    Publication Date: 2020-02-06
    Description: Our study presents a basin-scale 3D modeling solution, quantifying and exploring gas hydrate accumulations in the marine environment around the Green Canyon (GC955) area, Gulf of Mexico. It is the first modeling study that considers the full complexity of gas hydrate formation in a natural geological system. Overall, it comprises a comprehensive basin re-construction, accounting for depositional and transient thermal history of the basin, source rock maturation, petroleum components generation, expulsion and migration, salt tectonics and associated multi-stage fault development. The resulting 3D gas hydrate distribution in the Green Canyon area is consistent with independent borehole observations. An important mechanism identified in this study and leading to high gas hydrate saturation (〉 80 vol. %) at the base of the gas hydrate stability zone (GHSZ), is the recycling of gas hydrate and free gas enhanced by high Neogene sedimentation rates in the region. Our model predicts the rapid development of secondary intra-salt mini-basins situated on top of the allochthonous salt deposits which leads to significant sediment subsidence and an ensuing dislocation of the lower GHSZ boundary. Consequently, large amounts of gas hydrates located in the deepest parts of the basin dissociate and the released free methane gas migrates upwards to recharge the GHSZ. In total, we have predicted the gas hydrate budget for the Green Canyon area that amounts to ∼3,256 Mt of gas hydrate which is equivalent to ∼340 Mt of carbon (∼7 x 1011 m3 of CH4 at STP conditions), and consists mostly of biogenic hydrates.
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  • 5
    Publication Date: 2020-02-06
    Description: Monthly time-series data (1998–2009) of bottom water oxygen, nitrate and nitrite concentrations from the outer shelf (150 m water depth) in the oxygen minimum zone offshore Peru were coupled to a layered biogeochemical sediment model to investigate benthic-pelagic coupling over multi-annual time scales. The model includes the mineralization of four reactive pools of particulate organic carbon (POC) with lifetimes of 0.13, 1.3, 20, and 1700 year that were constrained using empirical data. Total POC rain rates to the seafloor were derived from satellite based estimates of primary production. Solute fluxes and concentrations in sediment porewater showed highly dynamic behavior over the course of a typical year. Conversion of fixed N to N2 by denitrification varied from 1.1 mmol m−2 d−1 of N in winter to 1.8 mmol m−2 d−1 of N in summer with a long term mean N loss for the shelf of 1.5 mmol m−2 d−1 of N. Fixed N loss across the whole time-series agreed very well with a previously-published vertically-integrated sediment model for coupling the benthic and pelagic N cycle in regional and global models. Dissimilatory nitrate reduction to ammonium (DNRA) emerges as a major process in the benthic N cycle, producing on average 1.9 mmol m−2 d−1 of ammonium: more than twice the rate of ammonification of organic nitrogen. The model predicts sulfide emissions from the sediment of up to 1 mmol m−2 d−1 when POC rain rate exceeds 20 mmol m−2 d−1, in agreement with past observations of benthic sulfide fluxes and sulfide plume distributions in the water column. This study demonstrates that sediments on the Peruvian shelf are not static repositories that are independent of changes taking place in the water column. Our results strongly suggest the shelf sediments must exert an important feedback on biogeochemical processes in the overlying waters, and should be considered in regional model studies.
    Type: Article , PeerReviewed
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  • 6
    Publication Date: 2023-02-08
    Description: We report on the geochemistry of hydrocarbons and pore waters down to 62.5 mbsf, collected by drilling with the MARUM‐MeBo70 and by gravity coring at the Lunde pockmark in the Vestnesa Ridge. Our data document the origin and transformations of volatiles feeding gas emissions previously documented in this region. Gas hydrates are present where a fracture network beneath the pockmark focusses migration of thermogenic hydrocarbons characterized by their C1/C2+ and stable isotopic compositions (δ2H‐CH4, δ13C‐CH4). Measured geothermal gradients (~80°C km‐1) and known formation temperatures (〉70°C) suggest that those hydrocarbons are formed at depths 〉800 mbsf. A combined analytical/modeling approach, including concentration and isotopic mass balances, reveals that pockmark sediments experience diffuse migration of thermogenic hydrocarbons. However, at sites without channeled flow this appears to be limited to depths 〉 ~50 mbsf. At all sites we document a contribution of microbial methanogenesis to the overall carbon cycle that includes a component of secondary carbonate reduction (CR) – i.e. reduction of dissolved inorganic carbon (DIC) generated by anaerobic oxidation of methane (AOM) in the uppermost methanogenic zone. AOM and CR rates are spatially variable within the pockmark and are highest at high‐flux sites. These reactions are revealed by δ13C‐DIC depletions at the sulfate‐methane interface at all sites. However, δ13C‐CH4 depletions are only observed at the low methane flux sites because changes in the isotopic composition of the overall methane pool are masked at high‐flux sites. 13C‐depletions of TOC suggest that at seeps sites, methane‐derived carbon is incorporated into de novo synthesized biomass.
    Type: Article , PeerReviewed
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  • 7
    Publication Date: 2022-01-31
    Description: During R/V Meteor cruise 141/1, pore fluids of near surface sediments were investigated to find indications for hydrothermal activity in the Terceira Rift (TR), a hyper‐slow spreading center in the Central North Atlantic Ocean. To date, submarine hydrothermal fluid venting in the TR has only been reported for the D. João de Castro seamount, which presently seems to be inactive. Pore fluids sampled close to a volcanic cone at 2800 m water depth show an anomalous composition with Mg, SO4, and total alkalinity (TA) concentrations significantly higher than seawater and a nearby reference core. The most straightforward way of interpreting these deviations is the dissolution of the hydrothermally formed mineral caminite (MgSO4 0.25Mg(OH)2 0.2H2O). This interpretation is corroborated by a thorough investigation of fluid isotope systems (δ26Mg, δ30Si, δ34S, δ44/42Ca, and 87Sr/86Sr). Caminite is known from mineral assemblages with anhydrite, and forms in hydrothermal recharge zones only under specific conditions such as high fluid temperatures and in altered oceanic crust, which are conditions generally met at the TR. We hypothesize that caminite was formed during hydrothermal activity and is now dissolving during the waning state of the hydrothermal system, so that caminite mineralization is shifted out of its stability zone. Ongoing fluid circulation through the basement is transporting the geochemical signal via slow advection towards the seafloor.
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  • 8
    Publication Date: 2022-03-09
    Description: During expedition MARIA S. MERIAN MSM57/2 to the Svalbard margin offshore Prins Karls Forland, the seafloor drill rig MARUM-MeBo70 was used to assess the landward termination of the gas hydrate system in water depths between 340 and 446 m. The study region shows abundant seafloor gas vents, clustered at a water depth of ~400 m. The sedimentary environment within the upper 100 meters below seafloor (mbsf) is dominated by ice-berg scours and glacial unconformities. Sediments cored included glacial diamictons and sheet-sands interbedded with mud. Seismic data show a bottom simulating reflector terminating ~30 km seaward in ~760 m water depth before it reaches the theoretical limit of the gas hydrate stability zone (GHSZ) at the drilling transect. We present results of the first in situ temperature measurements conducted with MeBo70 down to 28 mbsf. The data yield temperature gradients between ~38°C km-1 at the deepest site (446 m) and ~41°C km-1 at a shallower drill site (390 m). These data constrain combined with in situ pore-fluid data, sediment porosities, and thermal conductivities the dynamic evolution of the GHSZ during the past 70 years for which bottom water temperature records exist. Gas hydrate is not stable in the sediments at sites shallower than 390 m water depth at the time of acquisition (August 2016). Only at the drill site in 446 m water depth, favorable gas hydrate stability conditions are met (maximum vertical extent of ~60 mbsf); however, coring did not encounter any gas hydrates.
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  • 9
    Publication Date: 2024-02-07
    Description: Enhanced weathering of mafic and ultra-mafic minerals has been suggested as a strategy for carbon dioxide removal (CDR) and a contribution to achieve a balance between global CO2 sources and sinks (net zero emission). This study was designed to assess CDR by dissolution of ultramafic sand (UMS) in artificial seawater (ASW). Fine grained UMS with an olivine content of ~75% was reacted in ASW for up to 134 days at 1 bar and 21.5–23.9°C. A decline in total alkalinity (TA) was observed over the course of the experiments. This unexpected result indicates that TA removal via precipitation of cation-rich authigenic phases exceeded the production of TA induced by olivine dissolution. The TA decline was accompanied by a decrease in dissolved inorganic carbon and Ca concentrations presumably induced by CaCO3 precipitation. Temporal changes in dissolved Si, Ca, Mg, and TA concentrations observed during the experiments were evaluated by a numerical model to identify secondary mineral phases and quantify rates of authigenic phase formation. The modeling indicates that CaCO3, FeOOH and a range of Mg-Si-phases were precipitated during the experiments. Chemical analysis of precipitates and reacted UMS surfaces confirmed that these authigenic phases accumulated in the batch reactors. Nickel released during olivine dissolution, a potential toxic element for certain organisms, was incorporated in the secondary phases and is thus not a suitable proxy for dissolution rates as proposed by earlier studies. The overall reaction stoichiometry derived from lab experiments was applied in a box model simulating atmospheric CO2 uptake in a continental shelf setting induced by olivine addition. The model results indicate that CO2 uptake is reduced by a factor of 5 due to secondary mineral formation and the buffering capacity of seawater. In comparable natural settings, olivine addition may thus be a less efficient CDR method than previously believed.
    Type: Article , PeerReviewed
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  • 10
    Publication Date: 2024-02-07
    Description: Benthic nitrogen cycling in the Mauritanian upwelling region (NW Africa) was studied in June 2014 from the shelf to the upper slope where minimum bottom water O 2 concentrations of 25 µM were recorded. Benthic incubation chambers were deployed at 9 stations to measure fluxes of O 2 , dissolved inorganic carbon (DIC) and nutrients (NO 3 - , NO 2 - , NH 4 + , PO 4 3- , H 4 SiO 4 ) along with the N and O isotopic composition of nitrate (δ 15 N-NO 3 - and δ 18 O-NO 3 - ) and ammonium (δ 15 N-NH 4 + ). O 2 and DIC fluxes were similar to those measured during a previous campaign in 2011 whereas NH 4 + and PO 4 3- fluxes on the shelf were 2 – 3 times higher and possibly linked to a long-term decline in bottom water O 2 concentrations. The mean isotopic fractionation of NO 3 - uptake on the margin, inferred from the loss of NO 3 - inside the chambers, was 1.5 ± 0.4 ‰ for 15/14 N ( 15 ϵ app ) and 2.0 ± 0.5 ‰ for 18/16 O ( 18 ϵ app ). The mean 18 ϵ app : 15 ϵ app ratio on the shelf (〈 100 m) was 2.1 ± 0.3, and higher than the value of 1 expected for microbial NO 3 - reduction. The 15 ϵ app are similar to previously reported isotope effects for NO 3 - respiration in marine sediments but lower than determined in 2011 at a same site on the shelf. The sediments were also a source of 15 N-enriched NH 4 + (9.0 ± 0.7 ‰). A numerical model tuned to the benthic flux data and that specifically accounts for the efflux of 15 N-enriched NH 4 + from the seafloor, predicted a net benthic isotope effect of N loss ( 15 ϵ sed ) of 3.6 ‰; far above the more widely considered value of ~0‰. This result is further evidence that the assumption of a universally low or negligible benthic N isotope effect is not applicable to oxygen-deficient settings. The model further suggests that 18 ϵ app : 15 ϵ app trajectories > 1 in the benthic chambers are most likely due to aerobic ammonium oxidation and nitrite oxidation in surface sediments rather than anammox, in agreement with published observations in the water column of oxygen deficient regions.
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