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  • 1
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    Thermal conductivity of hydrate-bearing sediments (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2009. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research 114 (2009): B11103, doi:10.1029/2008JB006235.
    Description: A thorough understanding of the thermal conductivity of hydrate-bearing sediments is necessary for evaluating phase transformation processes that would accompany energy production from gas hydrate deposits and for estimating regional heat flow based on the observed depth to the base of the gas hydrate stability zone. The coexistence of multiple phases (gas hydrate, liquid and gas pore fill, and solid sediment grains) and their complex spatial arrangement hinder the a priori prediction of the thermal conductivity of hydrate-bearing sediments. Previous studies have been unable to capture the full parameter space covered by variations in grain size, specific surface, degree of saturation, nature of pore filling material, and effective stress for hydrate-bearing samples. Here we report on systematic measurements of the thermal conductivity of air dry, water- and tetrohydrofuran (THF)-saturated, and THF hydrate–saturated sand and clay samples at vertical effective stress of 0.05 to 1 MPa (corresponding to depths as great as 100 m below seafloor). Results reveal that the bulk thermal conductivity of the samples in every case reflects a complex interplay among particle size, effective stress, porosity, and fluid-versus-hydrate filled pore spaces. The thermal conductivity of THF hydrate–bearing soils increases upon hydrate formation although the thermal conductivities of THF solution and THF hydrate are almost the same. Several mechanisms can contribute to this effect including cryogenic suction during hydrate crystal growth and the ensuing porosity reduction in the surrounding sediment, increased mean effective stress due to hydrate formation under zero lateral strain conditions, and decreased interface thermal impedance as grain-liquid interfaces are transformed into grain-hydrate interfaces.
    Description: This work was supported by the Chevron Joint Industry Project on Methane Hydrates under contract DE-FC26- 01NT41330 to Georgia Institute of Technology from the U.S. Department of Energy’s National Energy Technology Laboratory. J.C.S. received additional support from the Goizueta Foundation. C.R. thanks the Petroleum Research Fund of the American Chemical Society under AC8–31351 for early support of thermal conductivity research on hydrate-bearing sediments at Georgia Institute of Technology.
    Keywords: Gas hydrate
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  • 2
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    Physical properties of hydrate-bearing sediments (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2009. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Reviews of Geophysics 47 (2009): RG4003, doi:10.1029/2008RG000279.
    Description: Methane gas hydrates, crystalline inclusion compounds formed from methane and water, are found in marine continental margin and permafrost sediments worldwide. This article reviews the current understanding of phenomena involved in gas hydrate formation and the physical properties of hydrate-bearing sediments. Formation phenomena include pore-scale habit, solubility, spatial variability, and host sediment aggregate properties. Physical properties include thermal properties, permeability, electrical conductivity and permittivity, small-strain elastic P and S wave velocities, shear strength, and volume changes resulting from hydrate dissociation. The magnitudes and interdependencies of these properties are critically important for predicting and quantifying macroscale responses of hydrate-bearing sediments to changes in mechanical, thermal, or chemical boundary conditions. These predictions are vital for mitigating borehole, local, and regional slope stability hazards; optimizing recovery techniques for extracting methane from hydrate-bearing sediments or sequestering carbon dioxide in gas hydrate; and evaluating the role of gas hydrate in the global carbon cycle.
    Description: This work is the product of a Department of Energy (DOE)–sponsored Physical Property workshop held in Atlanta, Georgia, 16–19 March 2008. The workshop was supported by Department of Energy contract DE-AI21-92MC29214. U.S. Geological Survey contributions were supported by the Gas Hydrate Project of the U.S. Geological Survey's Coastal and Marine Geology Program. Lawrence Berkeley National Laboratory contributions were supported by the Assistant Secretary for Fossil Energy, Office of Oil and Natural Gas, through the National Energy Technology Laboratory of the U.S. DOE under contract DE-AC02-05CH11231. Georgia Institute of Technology contributions were supported by the Goizueta Foundation, DOE DE-FC26-06NT42963, and the DOE-JIP administered by Chevron award DE-FC26-610 01NT41330. Rice University contributions were supported by the DOE under contract DE-FC26-06NT42960.
    Keywords: Physical properties ; Hydrate-bearing sediment ; Gas hydrate
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  • 3
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    Volume change associated with formation and dissociation of hydrate in sediment (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2010. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geochemistry Geophysics Geosystems 11 (2010): Q03007, doi:10.1029/2009GC002667.
    Description: Gas hydrate formation and dissociation in sediments are accompanied by changes in the bulk volume of the sediment and can lead to changes in sediment properties, loss of integrity for boreholes, and possibly regional subsidence of the ground surface over areas where methane might be produced from gas hydrate in the future. Experiments on sand, silts, and clay subject to different effective stress and containing different saturations of hydrate formed from dissolved phase tetrahydrofuran are used to systematically investigate the impact of gas hydrate formation and dissociation on bulk sediment volume. Volume changes in low specific surface sediments (i.e., having a rigid sediment skeleton like sand) are much lower than those measured in high specific surface sediments (e.g., clay). Early hydrate formation is accompanied by contraction for all soils and most stress states in part because growing gas hydrate crystals buckle skeletal force chains. Dilation can occur at high hydrate saturations. Hydrate dissociation under drained, zero lateral strain conditions is always associated with some contraction, regardless of soil type, effective stress level, or hydrate saturation. Changes in void ratio during formation-dissociation decrease at high effective stress levels. The volumetric strain during dissociation under zero lateral strain scales with hydrate saturation and sediment compressibility. The volumetric strain during dissociation under high shear is a function of the initial volume average void ratio and the stress-dependent critical state void ratio of the sediment. Other contributions to volume reduction upon hydrate dissociation are related to segregated hydrate in lenses and nodules. For natural gas hydrates, some conditions (e.g., gas production driven by depressurization) might contribute to additional volume reduction by increasing the effective stress.
    Description: This research was initially supported by the Chevron Joint Industry Project on Methane Hydrates under contract DE‐FC26‐01NT41330 from the U.S. Department of Energy to Georgia Tech. Additional support was provided to J. Y. Lee by KIGAM, GHDO, and MKE and J. C. Santamarina by the Goizueta Foundation.
    Keywords: Gas hydrate ; Hydrate-bearing sediment ; Phase transformation ; Strain
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  • 4
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    Moist synoptic transport of CO2 along the mid-latitude storm track (2011)
    American Geophysical Union
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2011. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 38 (2011): L09804, doi:10.1029/2011GL047238.
    Description: Atmospheric mixing ratios of CO2 are strongly seasonal in the Arctic due to mid-latitude transport. Here we analyze the seasonal influence of moist synoptic storms by diagnosing CO2 transport from a global model on moist isentropes (to represent parcel trajectories through stormtracks) and parsing transport into eddy and mean components. During winter when northern plants respire, warm moist air, high in CO2, is swept poleward into the polar vortex, while cold dry air, low in CO2, that had been transported into the polar vortex earlier in the year is swept equatorward. Eddies reduce seasonality in mid-latitudes by ∼50% of NEE (∼100% of fossil fuel) while amplifying seasonality at high latitudes. Transport along stormtracks is correlated with rising, moist, cloudy air, which systematically hides this CO2 transport from satellites. We recommend that (1) regional inversions carefully account for meridional transport and (2) inversion models represent moist and frontal processes with high fidelity.
    Description: This research is supported by the National Aeronautics and Space Administration contracts NNX08AT77G, NNX06AC75G, and NNX08AM56G.
    Keywords: Atmospheric transport ; Carbon cycle ; Inversion ; Isentropic coordinates ; Synoptic weather ; Tracer modeling
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  • 5
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    The impact of the North Atlantic Oscillation on the uptake and accumulation of anthropogenic CO2 by North Atlantic Ocean mode waters (2011)
    American Geophysical Union
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2011. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 25 (2011): GB3022, doi:10.1029/2010GB003892.
    Description: The North Atlantic Ocean accounts for about 25% of the global oceanic anthropogenic carbon sink. This basin experiences significant interannual variability primarily driven by the North Atlantic Oscillation (NAO). A suite of biogeochemical model simulations is used to analyze the impact of interannual variability on the uptake and storage of contemporary and anthropogenic carbon (Canthro) in the North Atlantic Ocean. Greater winter mixing during positive NAO years results in increased mode water formation and subsequent increases in subtropical and subpolar Canthro inventories. Our analysis suggests that changes in mode water Canthro inventories are primarily due to changes in water mass volumes driven by variations in water mass transformation rates rather than local air-sea CO2 exchange. This suggests that a significant portion of anthropogenic carbon found in the ocean interior may be derived from surface waters advected into water formation regions rather than from local gas exchange. Therefore, changes in climate modes, such as the NAO, may alter the residence time of anthropogenic carbon in the ocean by altering the rate of water mass transformation. In addition, interannual variability in Canthro storage increases the difficulty of Canthro detection and attribution through hydrographic observations, which are limited by sparse sampling of subsurface waters in time and space.
    Description: We would like to acknowledge funding from the NOAA Climate Program under the Office of Climate Observations and Global Carbon Cycle Program (NOAA‐NA07OAR4310098), NSF (OCE‐0623034), NCAR, the WHOI Ocean Climate Institute, a National Defense Science and Engineering Graduate Fellowship and an Environmental Protection Agency STAR graduate fellowship. NCAR is sponsored by the National Science Foundation.
    Keywords: North Atlantic Oscillation ; Anthropogenic carbon ; Carbon cycle ; Climate change ; Global climate model ; Mode waters
    Repository Name: Woods Hole Open Access Server
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  • 6
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    Enhanced CO2 outgassing in the Southern Ocean from a positive phase of the Southern Annular Mode (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2007. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 21 (2007): GB2026, doi:10.1029/2006GB002900.
    Description: We investigate the interannual variability in the flux of CO2 between the atmosphere and the Southern Ocean on the basis of hindcast simulations with a coupled physical-biogeochemical-ecological model with particular emphasis on the role of the Southern Annular Mode (SAM). The simulations are run under either pre-industrial or historical CO2 concentrations, permitting us to separately investigate natural, anthropogenic, and contemporary CO2 flux variability. We find large interannual variability (±0.19 PgC yr−1) in the contemporary air-sea CO2 flux from the Southern Ocean (〈35°S). Forty-three percent of the contemporary air-sea CO2 flux variance is coherent with SAM, mostly driven by variations in the flux of natural CO2, for which SAM explains 48%. Positive phases of the SAM are associated with anomalous outgassing of natural CO2 at a rate of 0.1 PgC yr−1 per standard deviation of the SAM. In contrast, we find an anomalous uptake of anthropogenic CO2 at a rate of 0.01 PgC yr−1 during positive phases of the SAM. This uptake of anthropogenic CO2 only slightly mitigates the outgassing of natural CO2, so that a positive SAM is associated with anomalous outgassing in contemporaneous times. The primary cause of the natural CO2 outgassing is anomalously high oceanic partial pressures of CO2 caused by elevated dissolved inorganic carbon (DIC) concentrations. These anomalies in DIC are primarily a result of the circulation changes associated with the southward shift and strengthening of the zonal winds during positive phases of the SAM. The secular, positive trend in the SAM has led to a reduction in the rate of increase of the uptake of CO2 by the Southern Ocean over the past 50 years.
    Description: This work was supported by NASA headquarters under the Earth System Science Fellowship Grant NNG05GP78H to N. S. L. and grants NAG5-12528 and NNG04GH53G to N. G. Both S. C. D. and I. D. L. were supported by NSF/ONR NOPP (N000140210370) and NASA (NNG05GG30G).
    Keywords: Southern Ocean ; Carbon cycle ; Southern Annular Mode
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  • 7
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    How does ocean biology affect atmospheric pCO2? Theory and models (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2008. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research 113 (2008): C07032, doi:10.1029/2007JC004598.
    Description: This paper examines the sensitivity of atmospheric pCO2 to changes in ocean biology that result in drawdown of nutrients at the ocean surface. We show that the global inventory of preformed nutrients is the key determinant of atmospheric pCO2 and the oceanic carbon storage due to the soft-tissue pump (OCS soft ). We develop a new theory showing that under conditions of perfect equilibrium between atmosphere and ocean, atmospheric pCO2 can be written as a sum of exponential functions of OCS soft . The theory also demonstrates how the sensitivity of atmospheric pCO2 to changes in the soft-tissue pump depends on the preformed nutrient inventory and on surface buffer chemistry. We validate our theory against simulations of nutrient depletion in a suite of realistic general circulation models (GCMs). The decrease in atmospheric pCO2 following surface nutrient depletion depends on the oceanic circulation in the models. Increasing deep ocean ventilation by increasing vertical mixing or Southern Ocean winds increases the atmospheric pCO2 sensitivity to surface nutrient forcing. Conversely, stratifying the Southern Ocean decreases the atmospheric CO2 sensitivity to surface nutrient depletion. Surface CO2 disequilibrium due to the slow gas exchange with the atmosphere acts to make atmospheric pCO2 more sensitive to nutrient depletion in high-ventilation models and less sensitive to nutrient depletion in low-ventilation models. Our findings have potentially important implications for both past and future climates.
    Description: While at MIT, I.M. was supported by the NOAA Postdoctoral Program in Climate and Global Change, administered by the University Corporation for Atmospheric Research.
    Keywords: Carbon cycle ; Preformed nutrient ; Nutrient depletion
    Repository Name: Woods Hole Open Access Server
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  • 8
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    Mechanical properties of sand, silt, and clay containing tetrahydrofuran hydrate (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2007. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research 112 (2007): B04106, doi:10.1029/2006JB004484.
    Description: The mechanical behavior of hydrate-bearing sediments subjected to large strains has relevance for the stability of the seafloor and submarine slopes, drilling and coring operations, and the analysis of certain small-strain properties of these sediments (for example, seismic velocities). This study reports on the results of comprehensive axial compression triaxial tests conducted at up to 1 MPa confining pressure on sand, crushed silt, precipitated silt, and clay specimens with closely controlled concentrations of synthetic hydrate. The results show that the stress-strain behavior of hydrate-bearing sediments is a complex function of particle size, confining pressure, and hydrate concentration. The mechanical properties of hydrate-bearing sediments at low hydrate concentration (probably 〈 40% of pore space) appear to be determined by stress-dependent soil stiffness and strength. At high hydrate concentrations (〉50% of pore space), the behavior becomes more independent of stress because the hydrates control both stiffness and strength and possibly the dilative tendency of sediments by effectively increasing interparticle coordination, cementing particles together, and filling the pore space. The cementation contribution to the shear strength of hydrate-bearing sediments decreases with increasing specific surface of soil minerals. The lower the effective confining stress, the greater the impact of hydrate formation on normalized strength.
    Description: This research was sponsored by a contract to C.R. and J.C.S. from the Joint Industry Project for Methane Hydrate, administered by ChevronTexaco with funding from award DE-FC26- 01NT41330 from DOE’s National Energy Technology Laboratory. The Goizueta Foundation at Georgia Tech also provided support for this work. The research was completed while C.R. was on assignment at and wholly supported by the National Science Foundation (NSF).
    Keywords: Gas hydrate ; Sediment strength ; Elasticity ; Mechanical behavior ; Stiffness
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  • 9
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    Parametric study of the physical properties of hydrate-bearing sand, silt, and clay sediments : 1. Electromagnetic properties (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2010. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research 115 (2010): B11104, doi:10.1029/2009JB006669.
    Description: The marked decrease in bulk electrical conductivity of sediments in the presence of gas hydrates has been used to interpret borehole electrical resistivity logs and, to a lesser extent, the results of controlled source electromagnetic surveys to constrain the spatial distribution and predicted concentration of gas hydrate in natural settings. Until now, an exhaustive laboratory data set that could be used to assess the impact of gas hydrate on the electromagnetic properties of different soils (sand, silt, and clay) at different effective stress and with different saturations of hydrate has been lacking. The laboratory results reported here are obtained using a standard geotechnical cell and the hydrate-formed tetrahydrofuran (THF), a liquid that is fully miscible in water and able to produce closely controlled saturations of hydrate from dissolved phase. Both permittivity and electrical conductivity are good indicators of the volume fraction of free water in the sediment, which is in turn dependent on hydrate saturation. Permittivity in the microwave frequency range is particularly predictive of free water content since it is barely affected by ionic concentration, pore structure, and surface conduction. Electrical conductivity (or resistivity) is less reliable for constraining water content or hydrate saturation: In addition to fluid-filled porosity, other factors, such as the ionic concentration of the pore fluid and possibly other conduction effects (e.g., surface conduction in high specific surface soils having low conductivity pore fluid), also influence electrical conductivity.
    Description: This research was initially supported by the Chevron Joint Industry Project on Methane Hydrates under contract DE‐FC26‐01NT41330 from the U.S. Department of Energy. Additional support was provided to J.C.S. by the Goizueta Foundation at Georgia Tech, to J.Y.L. by KIGAM, and to C. Ruppel by the USGS.
    Keywords: Gas hydrate ; Electromagnetic properties ; Resistivity
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  • 10
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    Parametric study of the physical properties of hydrate-bearing sand, silt, and clay sediments : 2. Small-strain mechanical properties (2010)
    American Geophysical Union
    Details
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2010. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research 115 (2010): B11105, doi:10.1029/2009JB006670.
    Description: The small-strain mechanical properties (e.g., seismic velocities) of hydrate-bearing sediments measured under laboratory conditions provide reference values for calibration of logging and seismic exploration results acquired in hydrate-bearing formations. Instrumented cells were designed for measuring the compressional (P) and shear (S) velocities of sand, silts, and clay with and without hydrate and subject to vertical effective stresses of 0.01 to 2 MPa. Tetrahydrofuran (THF), which is fully miscible in water, was used as the hydrate former to permit close control over the hydrate saturation Shyd and to produce hydrate from dissolved phase, as methane hydrate forms in most natural marine settings. The results demonstrate that laboratory hydrate formation technique controls the pattern of P and S velocity changes with increasing Shyd and that the small-strain properties of hydrate-bearing sediments are governed by effective stress, σ′v and sediment specific surface. The S velocity increases with hydrate saturation owing to an increase in skeletal shear stiffness, particularly when hydrate saturation exceeds Shyd≈ 0.4. At very high hydrate saturations, the small strain shear stiffness is determined by the presence of hydrates and becomes insensitive to changes in effective stress. The P velocity increases with hydrate saturation due to the increases in both the shear modulus of the skeleton and the bulk modulus of pore-filling phases during fluid-to-hydrate conversion. Small-strain Poisson's ratio varies from 0.5 in soft sediments lacking hydrates to 0.25 in stiff sediments (i.e., subject to high vertical effective stress or having high Shyd). At Shyd ≥ 0.5, hydrate hinders expansion and the loss of sediment stiffness during reduction of vertical effective stress, meaning that hydrate-rich natural sediments obtained through pressure coring should retain their in situ fabric for some time after core retrieval if the cores are maintained within the hydrate stability field.
    Description: Initial support for this research to J.C.S. and C.R. at Georgia Tech was provided by the Chevron Joint Industry Project on Methane Hydrates under contract DE‐FC26‐01NT41330 from the U.S. Department of Energy. Additional support to J.C.S. was provided by the Goizueta Foundation at Georgia Tech and to J.Y.L. by KIGAM, GHDO, and MKE.
    Keywords: Gas hydrate ; Mechanical properties ; Seismic velocity
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