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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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    Elsevier BV
    In:  EPIC3The Science of The Total Environment, Elsevier BV, 865, pp. 161168-161168, ISSN: 0048-9697
    Publication Date: 2023-06-21
    Description: Permeable sandy sediments cover 50-60% of the global continental shelf and are important bioreactors that regulate organic matter (OM) turnover and nutrient cycling in the coastal ocean. In sands, the dynamic porewater advection can cause rapid mass transfer and variable redox conditions, thus affecting OM remineralization pathways as well as the recycling of iron and phosphorus. In this study, North Sea sands were incubated in flow-through reactors (FTRs) to investigate biogeochemical processes under porewater advection and changing redox conditions. We found that the average rate of anaerobic OM remineralization was 12 times lower than the aerobic pathway, and Fe(III) oxyhydroxides were found as the major electron acceptors during 34 days of anoxic incubation. Abundant reduced Fe in the solid phase (expressed as Fe(II)) was measured before extensive Fe2+ release into porewater, and most of the reduced Fe (~96%) remained in the solid phase throughout the anoxic incubation. Fe(II) retained in the solid phase, either through the formation of authigenic Fe(II)-bearing minerals or adsorption, was easily re-oxidized upon exposure to O2 . Excessive P release (apart from OM remineralization) started at the beginning of the anoxic incubation and accelerated after the release of Fe2+ with a constant P/Fe2+ ratio of 0.26. After 34 days of anoxic incubation, porewater was re-oxygenated and 〉99% of released P was coprecipitated through Fe2+ oxidation (so-called “Fe2+ curtain”). Our results demonstrate that Fe(III)/Fe(II) in the solid phase can serve as relatively immobile and rechargeable “redox battery” under dynamic porewater advection. Due to frequent oscillation of redox conditions, the Fe “redox battery” is characteristic for permeable sediments and plays an important role in coastal OM turnover. We also suggest that P liberated before Fe2+ release can escape the “Fe2+ curtain” in porewater advection, thus potentially increasing net benthic P efflux from permeable sediments under variable redox conditions.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
    Format: application/pdf
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