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  • 1
    Publication Date: 2024-02-07
    Description: Highlights ● We developed a pH eddy covariance system to detect a sub-seafloor CO2 release. ● It detected CO2 emission to the water column at injection rates of 5.7–143 kg d − 1. ● It was also sensitive enough to quantify benthic biological CO2 production. ● Close to bubble streams, the kinetics of aqueous CO2 equilibration are important. ● This system can be used to detect, attribute, and quantify seafloor sources of CO2. We detected a controlled release of CO2 (g) with pH eddy covariance. We quantified CO2 emission using measurements of water velocity and pH in the plume of aqueous CO2 generated by the bubble streams, and using model predictions of vertical CO2 dissolution and its dispersion downstream. CO2 (g) was injected 3 m below the floor of the North Sea at rates of 5.7–143 kg d − 1. Instruments were 2.6 m from the center of the bubble streams. In the absence of injected CO2, pH eddy covariance quantified the proton flux due to naturally-occurring benthic organic matter mineralization (equivalent to a dissolved inorganic carbon flux of 7.6 ± 3.3 mmol m − 2 d − 1, s.e., n = 33). At the lowest injection rate, the proton flux due to CO2 dissolution was 20-fold greater than this. To accurately quantify emission, the kinetics of the carbonate system had to be accounted for. At the peak injection rate, 73 ± 13% (s.d.) of the injected CO2 was emitted, but when kinetics were neglected, the calculated CO2 emission was one-fifth of this. Our results demonstrate that geochemical techniques can detect and quantify very small seafloor sources of CO2 and attribute them to natural or abiotic origins.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
    Format: text
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  • 2
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Koopmans, D., Meyer, V., Schaap, A., Dewar, M., Farber, P., Long, M., Gros, J., Connelly, D., & Holtappels, M. Detection and quantification of a release of carbon dioxide gas at the seafloor using pH eddy covariance and measurements of plume advection. International Journal of Greenhouse Gas Control, 112, (2021): 103476, https://doi.org/10.1016/j.ijggc.2021.103476.
    Description: We detected a controlled release of CO2 (g) with pH eddy covariance. We quantified CO2 emission using measurements of water velocity and pH in the plume of aqueous CO2 generated by the bubble streams, and using model predictions of vertical CO2 dissolution and its dispersion downstream. CO2 (g) was injected 3 m below the floor of the North Sea at rates of 5.7–143 kg d − 1. Instruments were 2.6 m from the center of the bubble streams. In the absence of injected CO2, pH eddy covariance quantified the proton flux due to naturally-occurring benthic organic matter mineralization (equivalent to a dissolved inorganic carbon flux of 7.6 ± 3.3 mmol m − 2 d − 1, s.e., n = 33). At the lowest injection rate, the proton flux due to CO2 dissolution was 20-fold greater than this. To accurately quantify emission, the kinetics of the carbonate system had to be accounted for. At the peak injection rate, 73 ± 13% (s.d.) of the injected CO2 was emitted, but when kinetics were neglected, the calculated CO2 emission was one-fifth of this. Our results demonstrate that geochemical techniques can detect and quantify very small seafloor sources of CO2 and attribute them to natural or abiotic origins.
    Description: This project received funding from the European Union's Horizon 2020 research and innovation program under grant agreement No. 654462 (STEMM-CCS), it also received funding from the Max Planck Society and the Helmholtz Society. MHL was supported by US NSF grant # OCE-1657727.
    Keywords: CO2 vent ; Offshore CCS ; Leakage detection and quantification ; Marine sediment ; Proton flux
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
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    American Chemical Society (ACS)
    In:  EPIC3Environmental Science and Technology, American Chemical Society (ACS), ISSN: 0013-936X
    Publication Date: 2024-04-08
    Description: Marine permeable sediments are important sites for organic matter turnover in the coastal ocean. However, little is known about their role in trapping dissolved organic matter (DOM). Here, we examined DOM abundance and molecular compositions (9804 formulas identified) in subtidal permeable sediments along a near- to offshore gradient in the German North Sea. With the salinity increasing from 30.1 to 34.6 PSU, the DOM composition in bottom water shifts from relatively higher abundances of aromatic compounds to more highly unsaturated compounds. In the bulk sediment, DOM leached by ultrapure water (UPW) from the solid phase is 54 ± 20 times more abundant than DOM in porewater, with higher H/C ratios and a more terrigenous signature. With 0.5 M HCl, the amount of leached DOM (enriched in aromatic and oxygen-rich compounds) is doubled compared to UPW, mainly due to the dissolution of poorly crystalline Fe phases (e.g., ferrihydrite and Fe monosulfides). This suggests that poorly crystalline Fe phases promote DOM retention in permeable sediments, preferentially terrigenous, and aromatic fractions. Given the intense filtration of seawater through the permeable sediments, we posit that Fe can serve as an important intermediate storage for terrigenous organic matter and potentially accelerate organic matter burial in the coastal ocean.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
    Format: application/pdf
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