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Title: Experimental Investigation of Gas Flow and Hydrate Formation Within the Hydrate Stability Zone

Abstract

Here, we form methane hydrate by injecting methane gas into a brine-saturated, coarse-grained sample under hydrate-stable thermodynamic conditions. Hydrate forms to a saturation of 11%, which is much lower than that predicted assuming three-phase (gas-hydrate-brine) thermodynamic equilibrium (67%). During hydrate formation, there are temporary flow blockages. We interpret that a hydrate skin forms a physical barrier at the gas-brine interface. The skin fails periodically when the pressure differential exceeds the skin strength. Once the skin is present, further hydrate formation is limited by the rate that methane can diffuse through the solid skin. This process produces distinct thermodynamic states on either side of the skin that allows gas to flow through the sample. This study illuminates how gas can be transported through the hydrate stability zone and thus provides a mechanism for the formation of concentrated hydrate deposits in sand reservoirs. It also illustrates that models that assume local equilibrium at the core-scale and larger may not capture the fundamental behaviors of these gas flow and hydrate formation processes.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]
  1. The Univ. of Texas at Austin, Austin, TX (United States)
  2. Petroleum and Geosystems Engineering, The University of Texas at Austin, Austin TX USA
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1477334
Alternate Identifier(s):
OSTI ID: 1461561
Grant/Contract Number:  
AC02-05CH11231; FE0010406; FE0028967; FE0023919
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Geophysical Research. Solid Earth
Additional Journal Information:
Journal Volume: 123; Journal Issue: 7; Journal ID: ISSN 2169-9313
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; methane hydrate formation; free gas migration; nonequilibrium; computed tomography

Citation Formats

Meyer, Dylan W., Flemings, Peter B., DiCarlo, David, You, Kehua, Phillips, Stephen C., and Kneafsey, Timothy J. Experimental Investigation of Gas Flow and Hydrate Formation Within the Hydrate Stability Zone. United States: N. p., 2018. Web. doi:10.1029/2018JB015748.
Meyer, Dylan W., Flemings, Peter B., DiCarlo, David, You, Kehua, Phillips, Stephen C., & Kneafsey, Timothy J. Experimental Investigation of Gas Flow and Hydrate Formation Within the Hydrate Stability Zone. United States. doi:10.1029/2018JB015748.
Meyer, Dylan W., Flemings, Peter B., DiCarlo, David, You, Kehua, Phillips, Stephen C., and Kneafsey, Timothy J. Sun . "Experimental Investigation of Gas Flow and Hydrate Formation Within the Hydrate Stability Zone". United States. doi:10.1029/2018JB015748. https://www.osti.gov/servlets/purl/1477334.
@article{osti_1477334,
title = {Experimental Investigation of Gas Flow and Hydrate Formation Within the Hydrate Stability Zone},
author = {Meyer, Dylan W. and Flemings, Peter B. and DiCarlo, David and You, Kehua and Phillips, Stephen C. and Kneafsey, Timothy J.},
abstractNote = {Here, we form methane hydrate by injecting methane gas into a brine-saturated, coarse-grained sample under hydrate-stable thermodynamic conditions. Hydrate forms to a saturation of 11%, which is much lower than that predicted assuming three-phase (gas-hydrate-brine) thermodynamic equilibrium (67%). During hydrate formation, there are temporary flow blockages. We interpret that a hydrate skin forms a physical barrier at the gas-brine interface. The skin fails periodically when the pressure differential exceeds the skin strength. Once the skin is present, further hydrate formation is limited by the rate that methane can diffuse through the solid skin. This process produces distinct thermodynamic states on either side of the skin that allows gas to flow through the sample. This study illuminates how gas can be transported through the hydrate stability zone and thus provides a mechanism for the formation of concentrated hydrate deposits in sand reservoirs. It also illustrates that models that assume local equilibrium at the core-scale and larger may not capture the fundamental behaviors of these gas flow and hydrate formation processes.},
doi = {10.1029/2018JB015748},
journal = {Journal of Geophysical Research. Solid Earth},
number = 7,
volume = 123,
place = {United States},
year = {2018},
month = {7}
}

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Cited by: 3 works
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Works referenced in this record:

Pore space hydrate formation in a glass bead sample from methane dissolved in water
journal, January 2005

  • Spangenberg, E.; Kulenkampff, J.; Naumann, R.
  • Geophysical Research Letters, Vol. 32, Issue 24
  • DOI: 10.1029/2005GL024107

Fluid and chemical fluxes in and out of sediments hosting methane hydrate deposits on Hydrate Ridge, OR, I: Hydrological provinces
journal, August 2002


Dynamic response of oceanic hydrate deposits to ocean temperature change: DYNAMIC RESPONSE OF OCEANIC HYDRATES
journal, December 2008

  • Reagan, Matthew T.; Moridis, George J.
  • Journal of Geophysical Research: Oceans, Vol. 113, Issue C12
  • DOI: 10.1029/2008JC004938

Formation and accumulation of gas hydrate in porous media
journal, May 1997

  • Rempel, A. W.; Buffett, B. A.
  • Journal of Geophysical Research: Solid Earth, Vol. 102, Issue B5
  • DOI: 10.1029/97JB00392

Gulf of Mexico Gas Hydrate Joint Industry Project Leg II logging-while-drilling data acquisition and analysis
journal, June 2012


Gas hydrate resource potential in the Terrebonne Basin, Northern Gulf of Mexico
journal, June 2012


Transient seafloor venting on continental slopes from warming-induced methane hydrate dissociation: TRANSIENT SEAFLOOR VENTING FROM HYDRATES
journal, December 2015

  • Darnell, K. N.; Flemings, P. B.
  • Geophysical Research Letters, Vol. 42, Issue 24
  • DOI: 10.1002/2015GL067012

Passing gas through the hydrate stability zone at southern Hydrate Ridge, offshore Oregon
journal, January 2006


Macroscopic investigation of hydrate film growth at the hydrocarbon/water interface
journal, December 2007

  • Taylor, Craig J.; Miller, Kelly T.; Koh, Carolyn A.
  • Chemical Engineering Science, Vol. 62, Issue 23
  • DOI: 10.1016/j.ces.2007.07.038

Induction phenomena in gas hydrate nucleation
journal, July 1994


Short-range, overpressure-driven methane migration in coarse-grained gas hydrate reservoirs: Short Advection in Gas Hydrate Systems
journal, September 2016

  • Nole, Michael; Daigle, Hugh; Cook, Ann E.
  • Geophysical Research Letters, Vol. 43, Issue 18
  • DOI: 10.1002/2016GL070096

Large-scale simulation of methane hydrate dissociation along the West Spitsbergen Margin
journal, January 2009

  • Reagan, Matthew T.; Moridis, George J.
  • Geophysical Research Letters, Vol. 36, Issue 23
  • DOI: 10.1029/2009GL041332

Relationships among air-water interfacial area, capillary pressure, and water saturation for a sandy porous medium: TECHNICAL NOTE
journal, March 2006

  • Brusseau, Mark L.; Peng, Sheng; Schnaar, Gregory
  • Water Resources Research, Vol. 42, Issue 3
  • DOI: 10.1029/2005WR004058

Growth of Methane Clathrate Hydrates in Porous Media
journal, April 2012

  • Jin, Yusuke; Konno, Yoshihiro; Nagao, Jiro
  • Energy & Fuels, Vol. 26, Issue 4
  • DOI: 10.1021/ef3001357

Occurrence of gas hydrate in Oligocene Frio sand: Alaminos Canyon Block 818: Northern Gulf of Mexico
journal, September 2009


Feeding methane vents and gas hydrate deposits at south Hydrate Ridge: FEEDING METHANE VENTS AND GAS HYDRATES
journal, December 2004

  • Tréhu, Anne M.; Flemings, Peter B.; Bangs, Nathan L.
  • Geophysical Research Letters, Vol. 31, Issue 23
  • DOI: 10.1029/2004GL021286

Measuring Air−Water Interfacial Areas with X-ray Microtomography and Interfacial Partitioning Tracer Tests
journal, March 2007

  • Brusseau, Mark L.; Peng, Sheng; Schnaar, Gregory
  • Environmental Science & Technology, Vol. 41, Issue 6
  • DOI: 10.1021/es061474m

Current perspectives on gas hydrate resources
journal, January 2011

  • Boswell, Ray; Collett, Timothy S.
  • Energy Environ. Sci., Vol. 4, Issue 4
  • DOI: 10.1039/C0EE00203H

Gas hydrates (clathrates) causing pore-water freshening and oxygen isotope fractionation in deep-water sedimentary sections of terrigenous continental margins
journal, November 1981


X-ray computed-tomography observations of water flow through anisotropic methane hydrate-bearing sand
journal, June 2009


Darcy's law in saturated kaolinite
journal, June 1966


Architecture of gas-hydrate-bearing sands from Walker Ridge 313, Green Canyon 955, and Alaminos Canyon 21: Northern deepwater Gulf of Mexico
journal, June 2012


Geophysical and geochemical signatures associated with gas hydrate-related venting in the northern Cascadia margin
journal, January 2006

  • Riedel, M.; Novosel, I.; Spence, G. D.
  • Geological Society of America Bulletin, Vol. 118, Issue 1-2
  • DOI: 10.1130/B25720.1

Sediment surface effects on methane hydrate formation and dissociation
journal, June 2003


Measurement of induction times for the formation of methane and ethane gas hydrates
journal, February 1993


Raman spectroscopic analyses of the growth process of CO2 hydrates
journal, June 1995


The formation of meso- and macroporous gas hydrates
journal, September 2000

  • Kuhs, Werner F.; Klapproth, Alice; Gotthardt, Frank
  • Geophysical Research Letters, Vol. 27, Issue 18
  • DOI: 10.1029/2000GL006112

An Improved Method for Numerical Inversion of Laplace Transforms
journal, September 1982

  • de Hoog, F. R.; Knight, J. H.; Stokes, A. N.
  • SIAM Journal on Scientific and Statistical Computing, Vol. 3, Issue 3
  • DOI: 10.1137/0903022

Capillary pressure and heterogeneity for the CO2/water system in sandstone rocks at reservoir conditions
journal, March 2012


Gas hydrate growth, methane transport, and chloride enrichment at the southern summit of Hydrate Ridge, Cascadia margin off Oregon
journal, September 2004

  • Torres, M. E.; Wallmann, K.; Tréhu, A. M.
  • Earth and Planetary Science Letters, Vol. 226, Issue 1-2
  • DOI: 10.1016/j.epsl.2004.07.029

A molecular mechanism for gas hydrate nucleation from ice
journal, September 1991


Predicting PVT data for CO2–brine mixtures for black-oil simulation of CO2 geological storage
journal, January 2008

  • Hassanzadeh, Hassan; Pooladi-Darvish, Mehran; Elsharkawy, Adel M.
  • International Journal of Greenhouse Gas Control, Vol. 2, Issue 1
  • DOI: 10.1016/S1750-5836(07)00010-2

Methane hydrate crystal growth in a porous medium filled with methane-saturated liquid water
journal, March 2007


Crystallographic Studies of Clathrate Hydrates. Part I
journal, December 1986

  • Davidson, D. W.; Handa, Y. P.; Ratcliffe, C. I.
  • Molecular Crystals and Liquid Crystals, Vol. 141, Issue 1-2
  • DOI: 10.1080/00268948608080205

Methane migration within the submarine gas-hydrate stability zone under deep-water conditions
journal, February 1997


The physics of premelted ice and its geophysical consequences
journal, July 2006


Methane hydrate nonstoichiometry and phase diagram
journal, May 2003

  • Huo, Zhongxin; Hester, Keith; Sloan, E. Dendy
  • AIChE Journal, Vol. 49, Issue 5
  • DOI: 10.1002/aic.690490521

Nonequilibrium Thermodynamics of Hydrate Growth on a Gas-Liquid Interface
journal, April 2018


A cylindrical electrical resistivity tomography array for three-dimensional monitoring of hydrate formation and dissociation
journal, October 2013

  • Priegnitz, Mike; Thaler, Jan; Spangenberg, Erik
  • Review of Scientific Instruments, Vol. 84, Issue 10
  • DOI: 10.1063/1.4825372

The movement and entrapment of petroleum fluids in the subsurface
journal, March 1987

  • England, W. A.; Mackenzie, A. S.; Mann, D. M.
  • Journal of the Geological Society, Vol. 144, Issue 2
  • DOI: 10.1144/gsjgs.144.2.0327

Methane Hydrate Distribution from Prolonged and Repeated Formation in Natural and Compacted Sand Samples: X-Ray CT Observations
journal, January 2011

  • Rees, Emily V. L.; Kneafsey, Timothy J.; Seol, Yongkoo
  • Journal of Geological Research, Vol. 2011
  • DOI: 10.1155/2011/791815

A numerical model for the formation of gas hydrate below the seafloor
journal, January 2001

  • Davie, Matthew K.; Buffett, Bruce A.
  • Journal of Geophysical Research: Solid Earth, Vol. 106, Issue B1
  • DOI: 10.1029/2000JB900363

The Pore-Pressure Coefficients A and B
journal, December 1954


Predicting the occurrence, distribution, and evolution of methane gas hydrate in porous marine sediments
journal, March 1999

  • Xu, Wenyue; Ruppel, Carolyn
  • Journal of Geophysical Research: Solid Earth, Vol. 104, Issue B3
  • DOI: 10.1029/1998JB900092

Rising methane gas bubbles form massive hydrate layers at the seafloor
journal, November 2004

  • Haeckel, Matthias; Suess, Erwin; Wallmann, Klaus
  • Geochimica et Cosmochimica Acta, Vol. 68, Issue 21
  • DOI: 10.1016/j.gca.2004.01.018

Formation of Methane Hydrate from Polydisperse Ice Powders
journal, July 2006

  • Kuhs, Werner F.; Staykova, Doroteya K.; Salamatin, Andrey N.
  • The Journal of Physical Chemistry B, Vol. 110, Issue 26
  • DOI: 10.1021/jp061060f

Marine Chemistry
journal, December 1980


A model for the diffusive growth of hydrate saturation anomalies in layered sediments
journal, January 2011


Toward Production From Gas Hydrates: Current Status, Assessment of Resources, and Simulation-Based Evaluation of Technology and Potential
journal, October 2009

  • Moridis, George J.; Collett, Timothy S.; Boswell, Ray
  • SPE Reservoir Evaluation & Engineering, Vol. 12, Issue 05
  • DOI: 10.2118/114163-PA

In Situ Studies of the Mass Transfer Mechanism across a Methane Hydrate Film Using High-Resolution Confocal Raman Spectroscopy
journal, December 2009

  • Davies, Simon R.; Sloan, E. Dendy; Sum, Amadeu K.
  • The Journal of Physical Chemistry C, Vol. 114, Issue 2
  • DOI: 10.1021/jp909416y

Experimental studies on the formation of porous gas hydrates
journal, August 2004

  • Genov, Georgi; Kuhs, Werner F.; Staykova, Doroteya K.
  • American Mineralogist, Vol. 89, Issue 8-9
  • DOI: 10.2138/am-2004-8-910

A steady state model for marine hydrate formation: Constraints on methane supply from pore water sulfate profiles: STEADY STATE HYDRATE MODEL
journal, October 2003

  • Davie, M. K.; Buffett, B. A.
  • Journal of Geophysical Research: Solid Earth, Vol. 108, Issue B10
  • DOI: 10.1029/2002JB002300

Methane hydrate formation and dissociation in a partially saturated core-scale sand sample
journal, March 2007

  • Kneafsey, Timothy J.; Tomutsa, Liviu; Moridis, George J.
  • Journal of Petroleum Science and Engineering, Vol. 56, Issue 1-3
  • DOI: 10.1016/j.petrol.2006.02.002

Liquid limit as a predictor of mudrock permeability
journal, June 2013


Subsurface gas hydrates in the northern Gulf of Mexico
journal, June 2012


Premelting dynamics in a continuum model of frost heave
journal, January 1999


Short migration of methane into a gas hydrate-bearing sand layer at Walker Ridge, Gulf of Mexico: SHORT MIGRATION OF METHANE
journal, February 2013

  • Cook, Ann E.; Malinverno, Alberto
  • Geochemistry, Geophysics, Geosystems, Vol. 14, Issue 2
  • DOI: 10.1002/ggge.20040

Operational overview of the first offshore production test of methane hydrates in the Eastern Nankai Trough
conference, May 2014

  • Yamamoto, Koji; Terao, Yoshihiro; Fujii, Tesuya
  • Offshore Technology Conference
  • DOI: 10.4043/25243-MS

    Works referencing / citing this record:

    Mechanisms of Methane Hydrate Formation in Geological Systems
    journal, October 2019

    • You, K.; Flemings, P. B.; Malinverno, A.
    • Reviews of Geophysics, Vol. 57, Issue 4
    • DOI: 10.1029/2018rg000638

    Nitrogen‐Driven Chromatographic Separation During Gas Injection Into Hydrate‐Bearing Sediments
    journal, August 2019

    • Darnell, K. N.; Flemings, P. B.; DiCarlo, D.
    • Water Resources Research, Vol. 55, Issue 8
    • DOI: 10.1029/2018wr023414

    High‐Saturation Gas Hydrate Reservoirs—A Pore Scale Investigation of Their Formation From Free Gas and Dissociation in Sediments
    journal, December 2019

    • Lei, Liang; Seol, Yongkoo
    • Journal of Geophysical Research: Solid Earth, Vol. 124, Issue 12
    • DOI: 10.1029/2019jb018243