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Title: Pore habit of methane hydrate and its evolution in sediment matrix – Laboratory visualization with phase-contrast micro-CT

Journal Article · · Marine and Petroleum Geology
ORCiD logo [1];  [1]; ORCiD logo [2];  [3]
  1. National Energy Technology Lab. (NETL), Morgantown, WV (United States)
  2. National Energy Technology Lab. (NETL), Morgantown, WV (United States); AECOM, Morgantown, WV (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Geosciences Division

Describing the pore habit of methane hydrate in sediment matrices is essential for understanding natural distribution of methane hydrate, methane trace (transport and solidification) in the hydrate stability zone, physical properties of hydrate-bearing sediments, and the associated influence on potential gas production. Pore habit visualization in natural media at pore scale even with laboratory synthesized cores has been challenging due to the similar densities of methane hydrate from pore liquid. In this work, we used phase-contrast assisted micro-CT with potassium iodine-doped brine to visualize four phases: sand particles, pore fluid, methane hydrate and methane gas. This study visualizes the pore habit of methane hydrate at various stages including during hydrate formation in excess-gas systems, its evolution after brine injection to replace pore fluid, and hydrate formation in excess-water systems. Hydrate tends to adopt round and smooth surfaces when in contact with water while exhibits relatively angular interfaces when in contact with methane gas. Hydrate formation in excess-gas systems results in a partial cementing and partial mineral-coating pore habit, while hydrate in excess-water systems develops mainly as pore-filling, and locally cementing or mineral-coating where big gas pockets exist at the initial state. Pore liquid replacement from methane gas to brine triggers a shift of hydrate pore habit towards pore-filling. Methane hydrate evolution over time produces bigger hydrate particles but with less contact area with sand particles. The effects of hydrate pore habit become less important as hydrate particle size exceeds the pore size. Additionally, hydrate formation could trap residual methane gas and brine as inclusions.

Research Organization:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Fossil Energy (FE); USDOE
Grant/Contract Number:
89243318CFE000003; AC02-05CH11231
OSTI ID:
1569827
Alternate ID(s):
OSTI ID: 1580838; OSTI ID: 1692111
Report Number(s):
NETL-PUB-22176
Journal Information:
Marine and Petroleum Geology, Vol. 104, Issue C; ISSN 0264-8172
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 152 works
Citation information provided by
Web of Science

References (54)

Determination of pore-scale hydrate phase equilibria in sediments using lab-on-a-chip technology journal January 2017
Enthalpy of dissociation and hydration number of carbon dioxide hydrate from the Clapeyron equation journal July 2003
Is Gas Hydrate Energy Within Reach? journal August 2009
An effective medium inversion algorithm for gas hydrate quantification and its application to laboratory and borehole measurements of gas hydrate-bearing sediments journal August 2006
Microstructural evolution of gas hydrates in sedimentary matrices observed with synchrotron X-ray computed tomographic microscopy: MICROSTRUCTRE OF GAS HYDRATES journal June 2015
Ostwald ripening changes the pore habit and spatial variability of clathrate hydrate journal February 2018
Laboratory formation of noncementing hydrates in sandy sediments journal April 2014
Multistage Triaxial Tests on Laboratory-Formed Methane Hydrate-Bearing Sediments journal May 2018
X-ray computed-tomography imaging of gas migration in water-saturated sediments: From capillary invasion to conduit opening: GAS MIGRATION IN SATURATED SEDIMENTS journal September 2011
Thermodynamic and pore water halogen constraints on gas hydrate distribution at ODP Site 997 (Blake Ridge) journal January 1999
Ellipsometric study of the transition layer on the surface of an ice crystal journal April 1987
Pore-level hydrate formation mechanisms using realistic rock structures in high-pressure silicon micromodels journal October 2016
Some Theorems on the Free Energies of Crystal Surfaces journal April 1951
Pore water anomalies of submarine gas-hydrate zones as tool to assess hydrate abundance and distribution in the subsurface What have we learned in the past decade? journal April 2003
Measurement of interfacial free energy for ice/water system journal January 1998
Structural Investigation of Methane Hydrate Sediments by Microfocus X-ray Computed Tomography Technique under High-Pressure Conditions journal July 2006
Observation of Xe Hydrate Growth at Gas−Ice Interface by Microfocus X-ray Computed Tomography journal October 2008
Effect of hydrate nucleation mechanisms and capillarity on permeability reduction in granular media: NUCLEATION-DEPENDENT PERMEABILITY journal September 2016
Formation, growth and ageing of clathrate hydrate crystals in a porous medium journal April 2006
Methane hydrate crystal growth in a porous medium filled with methane-saturated liquid water journal March 2007
Visual observation of dissociation of methane hydrate crystals in a glass micro model: Production and transfer of methane journal October 2008
Imaging methane hydrates growth dynamics in porous media using synchrotron X-ray computed microtomography journal December 2014
Deep sea NMR: Methane hydrate growth habit in porous media and its relationship to hydraulic permeability, deposit accumulation, and submarine slope stability: DEEP SEA NMR journal October 2003
Pressure core based study of gas hydrates in the Ulleung Basin and implication for geomechanical controls on gas hydrate occurrence journal November 2013
Laboratory Strategies for Hydrate Formation in Fine‐Grained Sediments journal April 2018
Pore-Scale Visualization of Methane Hydrate-Bearing Sediments With Micro-CT journal June 2018
The first offshore natural gas hydrate production test in South China Sea journal January 2018
An investigation of laboratory-grown ice spikes journal January 2004
Impact of hydrate saturation on water permeability in hydrate-bearing sediments journal March 2019
The water retention curve and relative permeability for gas production from hydrate-bearing sediments: pore-network model simulation: WATER RETENTION AND PERMEABILITY journal August 2016
The effect of hydrate saturation on water retention curves in hydrate-bearing sediments: Water Retention Curves in THF HBS journal May 2016
Effect of pressure on the surface tension of water. Adsorption of low molecular weight gases on water at 25.deg. journal October 1974
Co-existence of gas hydrate, free gas, and brine within the regional gas hydrate stability zone at Hydrate Ridge (Oregon margin): evidence from prolonged degassing of a pressurized core journal June 2004
The structure of methane gas hydrate bearing sediments from the Krishna–Godavari Basin as seen from Micro-CT scanning journal July 2011
Hydro-bio-geomechanical properties of hydrate-bearing sediments from Nankai Trough journal September 2015
On the path to the digital rock physics of gas hydrate-bearing sediments – processing of in situ synchrotron-tomography data journal January 2016
X-ray computed-tomography observations of water flow through anisotropic methane hydrate-bearing sand journal June 2009
Morphology of methane and carbon dioxide hydrates formed from water droplets journal January 2003
Gas hydrate saturation in the Krishna–Godavari basin from P-wave velocity and electrical resistivity logs journal November 2011
Sediment–well interaction during depressurization journal October 2016
The Surface of Ice Is Like Supercooled Liquid Water journal October 2017
Modeling of the influence of gas hydrate content on the electrical properties of porous sediments journal April 2001
Pore space hydrate formation in a glass bead sample from methane dissolved in water journal January 2005
Observations of pore-scale growth patterns of carbon dioxide hydrate using X-ray computed microtomography journal March 2015
Visual observation of gas-hydrate formation and dissociation in synthetic porous media by means of glass micromodels journal January 2001
Pore fluid geochemistry from the Mount Elbert Gas Hydrate Stratigraphic Test Well, Alaska North Slope journal February 2011
Physical properties of hydrate-bearing sediments journal January 2009
Gas hydrate formation rates from dissolved-phase methane in porous laboratory specimens: METHANE HYDRATE FORMATION RATES journal August 2013
Gas hydrate saturation from acoustic impedance and resistivity logs in the Shenhu area, South China Sea journal September 2011
A marine electromagnetic survey to detect gas hydrate at Hydrate Ridge, Oregon: EM at Hydrate Ridge journal August 2011
Physical properties of sediment from the Mount Elbert Gas Hydrate Stratigraphic Test Well, Alaska North Slope journal February 2011
Synchrotron X-ray computed microtomography study on gas hydrate decomposition in a sedimentary matrix: GAS HYDRATE DECOMPOSITION IN SEDIMENTS journal September 2016
A pressure core based characterization of hydrate-bearing sediments in the Ulleung Basin, Sea of Japan (East Sea) journal January 2011
Mechanical properties of sand, silt, and clay containing tetrahydrofuran hydrate: MECHANICAL BEHAVIOR OF HYDRATE-BEARING SEDIMENTS journal April 2007

Cited By (3)

Integration of triaxial testing and pore-scale visualization of methane hydrate bearing sediments journal December 2019
Strain Rate‐Dependent Hardening‐Softening Characteristics of Gas Hydrate‐Bearing Sediments journal November 2019
Dynamic in-situ imaging of methane hydrate formation and self-preservation preprint January 2019