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  • 1
    Publication Date: 2019-10-24
    Description: A novel methodology for predicting upward diffusive fluxes of dissolved methane in gassy marine sediments is presented. The predicted fluxes are derived from a set of theoretical simulation data gener ated using a diagenetic reaction-transport model. The model calculates the upward methane flux for a given free gas depth (FGD) below the seafloor and a given in situ gas solubility, which together define the methane concentration gradient. Fluxes can thus be extracted from a nomogram of FGD and solubility parameter space. Because, in general, microorganisms anaerobically oxidize all dissolved methane before it can escape the sediment, the estimated fluxes are equivalent to the amount of methane trapped by this subsurface microbial barrier. A test of the approach using measured methane fluxes from Aarhus Bay, Denmark, reveals a statistically significant correlation between the observed and predicted fluxes. The predicted fluxes further show a low sensitivity toward enhanced sediment mixing by faunal activity, as well as the deposition flux and reactivity of organic matter. Therefore, only a limited amount of data at strategic coring sites is required to constrain the major physical and geochemical forcings for a particular study area in order to extrapolate fluxes at a regional scale. Because the FGD can be mapped over large areas of the seafloor from shipboard seismic survey, the new approach represents a means to estimate regional methane flux budgets for gassy sediments in a cost-efficient manner.
    Type: Article , PeerReviewed
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  • 2
    Publication Date: 2017-01-19
    Description: Recent developments in the quantitativemodeling of methane dynamics and anaerobic oxidation of methane (AOM) in marine sediments are critically reviewed. The first part of the review begins with a comparison of alternative kinetic models for AOM. The roles of bioenergetic limitations, intermediate compounds and biomass growth are highlighted. Next, the key transport mechanisms in multi-phase sedimentary environments affecting AOM and methane fluxes are briefly treated, while attention is also given to additional controls on methane and sulfate turnover, including organic matter mineralization, sulfur cycling and methane phase transitions. In the second part of the review, the structure, forcing functions and parameterization of published models of AOM in sediments are analyzed. The six-orders-of-magnitude range in rate constants reported for the widely used bimolecular rate law for AOM emphasizes the limited transferability of this simple kinetic model and, hence, the need for more comprehensive descriptions of the AOM reaction system. The derivation and implementation of more complete reaction models, however, are limited by the availability of observational data. In this context, we attempt to rank the relative benefits of potential experimental measurements that should help to better constrain AOM models. The last part of the review presents a compilation of reported depth-integrated AOM rates (ΣAOM). These rates reveal the extreme variability of ΣAOM in marine sediments. The model results are further used to derive quantitative relationships between ΣAOM and the magnitude of externally impressed fluid flow, as well as between ΣAOM and the depth of the sulfate–methane transition zone (SMTZ). This review contributes to an improved understanding of the global significance of the AOM process, and helps identify outstanding questions and future directions in the modeling of methane cycling and AOM in marine sediments.
    Type: Article , PeerReviewed
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  • 3
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    Kline Geology Laboratory
    In:  American Journal of Science, 306 (4). pp. 246-294.
    Publication Date: 2020-06-03
    Description: A kinetic-bioenergetic reaction model for the anaerobic oxidation of methane (AOM) in coastal marine sediments is presented. The model considers a fixed depth interval of sediments below the zone of bioturbation (the window-of-observation), subject to seasonal variations of temperature and inputs of organic substrates and sulfate. It includes (1) nine microbially-mediated reaction pathways involved in CH4 production/consumption; (2) an explicit representation of five functional microbial groups; and (3) bioenergetic limitations of the microbial metabolic pathways. Fermentation of organic substrates is assumed to produce hydrogen (H2) and acetate (Ac) as key reactive intermediates. Competition among the metabolic pathways is controlled by the relative kinetic efficiencies of the various microbial processes and by bioenergetic constraints. Model results imply that the functional microbial biomasses within the window-of-observation undergo little variation over the year, as a result of kinetic and thermodynamic buffering of the seasonal forcings. Furthermore, the microbial processes proceed at only small fractions of their maximum potential rates. These findings provide a theoretical justification for the approximation of steady-state microbial biomasses, which is frequently used in diagenetic modeling. In contrast, AOM rates show a strong seasonal evolution: AOM only becomes spontaneous in winter, when hydrogenotrophic sulfate reduction (hySR) sufficiently reduces the local H2 concentration. The bioenergetic limitation of AOM is thus a critical factor modulating this process in seasonally-forced nearshore marine sediments. A global sensitivity analysis based on a 2-level factorial design reveals that AOM rates are most sensitive to the kinetic parameters describing hySR and acetotrophic methanogenesis (acME). The growth and substrate uptake kinetics of AOM are unimportant, whereas the threshold value of ATP energy conservation for AOM is the most sensitive thermodynamic parameter. These results confirm that anaerobic methane oxidizing microorganisms are metabolizing close to their thermodynamic limit, with the energetic balance being controlled by the relative rates of hySR and acME. The removal of Ac by acME primarily allows more sulfate (SO42−) to be utilized for H2 oxidation, thereby promoting AOM.
    Type: Article , PeerReviewed
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  • 4
    Publication Date: 2017-01-30
    Description: A simplified version of a kinetic–bioenergetic reaction model for anaerobic oxidation of methane (AOM) in marine sediments [Dale, A.W., Regnier, P., Van Cappellen, P., 2006. Bioenergetic controls on anaerobic oxidation of methane (AOM) in coastal marine sediments: a theoretical analysis. Am. J. Sci. 306, 246–294.] is used to assess the impact of transport processes on biomass distributions, AOM rates and methane release fluxes from the sea floor. The model explicitly represents the functional microbial groups and the kinetic and bioenergetic limitations of the microbial metabolic pathways involved in AOM. Model simulations illustrate the dominant control exerted by the transport regime on the activity and abundance of AOM communities. Upward fluid flow at active seep systems restricts AOM to a narrow subsurface reaction zone and sustains high rates of methane oxidation. In contrast, pore-water transport dominated by molecular diffusion leads to deeper and broader zones of AOM, characterized by much lower rates and biomasses. Under steady-state conditions, less than 1% of the upward dissolved methane flux reaches the water column, irrespective of the transport regime. However, a sudden increase in the advective flux of dissolved methane, for example as a result of the destabilization of methane hydrates, causes a transient efflux of methane from the sediment. The benthic efflux of dissolved methane is due to the slow growth kinetics of the AOM community and lasts on the order of 60 years. This time window is likely too short to allow for a significant escape of pore-water methane following a large scale gas hydrate dissolution event such as the one that may have accompanied the Paleocene/Eocene Thermal Maximum (PETM).
    Type: Article , PeerReviewed
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  • 5
    Publication Date: 2017-11-01
    Description: A steady-state reaction-transport model is applied to sediments retrieved by gravity core from two stations (S10 and S13) in the Skagerrak to determine the main kinetic and thermodynamic controls on anaerobic oxidation of methane (AOM). The model considers an extended biomass-implicit reaction network for organic carbon degradation, which includes extracellular hydrolysis of macromolecular organic matter, fermentation, sulfate reduction, methanogenesis, AOM, acetogenesis and acetotrophy. Catabolic reaction rates are determined using a modified Monod rate expression that explicitly accounts for limitation by the in situ catabolic energy yields. The fraction of total sulfate reduction due to AOM in the sulfate–methane transition zone (SMTZ) at each site is calculated. The model provides an explanation for the methane tailing phenomenon which is observed here and in other marine sediments, whereby methane diffuses up from the SMTZ to the top of the core without being consumed. The tailing is due to bioenergetic limitation of AOM in the sulfate reduction zone, because the methane concentration is too low to engender favorable thermodynamic drive. AOM is also bioenergetically inhibited below the SMTZ at both sites because of high hydrogen concentrations (∼3–6 nM). The model results imply there is no straightforward relationship between pore water concentrations and the minimum catabolic energy needed to support life because of the highly coupled nature of the reaction network. Best model fits are obtained with a minimum energy for AOM of ∼11 kJ mol−1, which is within the range reported in the literature for anaerobic processes.
    Type: Article , PeerReviewed
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