The Effect of Brine on the Electrical Properties of Methane Hydrate

Lu, R.; Stern, L. A.; Du Frane, W. L.; Pinkston, J. C.; Roberts, J. J.; Constable, S.

doi:10.1029/2019JB018364

Title: The Effect of Brine on the Electrical Properties of Methane Hydrate

Abstract

Gas hydrates possess lower electrical conductivity (inverse of resistivity) than either seawater or ice, but higher than clastic silts and sands, such that electromagnetic methods can be employed to help identify their natural formation in marine and permafrost environments. Controlled laboratory studies offer a means to isolate and quantify the effects of changing individual components within gas-hydrate-bearing systems, in turn yielding insight into the behavior of natural systems. Here we investigate the electrical properties of polycrystalline methane hydrate with ≥25% gas-filled porosity and in mixture with brine. Initially, pure methane hydrate was synthesized from H2O ice and CH4 gas while undergoing electrical impedance measurement, then partially dissociated to assess the effects of pure pore water accumulation on electrical conductivity. Methane hydrate + brine mixtures were then formed by either adding NaCl (0.25–2.5 wt %) to high-purity ice or by using frozen seawater as a reactant. Conductivity was obtained from impedance measurements made in situ throughout synthesis while temperature cycled between +15 °C and -25 °C. Several possible conduction mechanisms were subsequently determined using equivalent circuit modeling. Samples with low NaCl concentration show a doping/impurity effect and a log linear conductivity response as a function of temperature. For higher salt contentmore »« less

Authors:

^[1];

^[2];

^[1]; Pinkston, J. C. ^[2]; Roberts, J. J. ^[1];

^[3]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
U.S. Geological Survey, Menlo Park, CA (United States)
The Scripps Research Inst., La Jolla, CA (United States)

Publication Date:: Wed Oct 16 00:00:00 EDT 2019

Research Org.:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Univ. of California, San Diego, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Fossil Energy (FE)

OSTI Identifier:: 1601946

Alternate Identifier(s):: OSTI ID: 1573282; OSTI ID: 1735361

Report Number(s):: LLNL-JRNL-777845
Journal ID: ISSN 2169-9313; 965649

Grant/Contract Number:: AC52-07NA27344; FE0028972; FE0026382

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Geophysical Research. Solid Earth

Additional Journal Information:: Journal Volume: 124; Journal Issue: 11; Journal ID: ISSN 2169-9313

Publisher:: American Geophysical Union

Country of Publication:: United States

Language:: English

Subject:: 58 GEOSCIENCES; methane hydrate; impedance spectroscopy; resistivity conductivity; hydrohalite; brine; NaCl; gas hydrate; electrical conductivity

Citation Formats


                    Lu, R., Stern, L. A., Du Frane, W. L., Pinkston, J. C., Roberts, J. J., and Constable, S. The Effect of Brine on the Electrical Properties of Methane Hydrate.  United States: N. p., 2019. 
Web.  doi:10.1029/2019JB018364.

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                    Lu, R., Stern, L. A., Du Frane, W. L., Pinkston, J. C., Roberts, J. J., & Constable, S. The Effect of Brine on the Electrical Properties of Methane Hydrate.  United States.  https://doi.org/10.1029/2019JB018364

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                    Lu, R., Stern, L. A., Du Frane, W. L., Pinkston, J. C., Roberts, J. J., and Constable, S. Wed .  
"The Effect of Brine on the Electrical Properties of Methane Hydrate".  United States.  https://doi.org/10.1029/2019JB018364.  https://www.osti.gov/servlets/purl/1601946.

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@article{osti_1601946,

  title        = {The Effect of Brine on the Electrical Properties of Methane Hydrate},

  author       = {Lu, R. and Stern, L. A. and Du Frane, W. L. and Pinkston, J. C. and Roberts, J. J. and Constable, S.},

  abstractNote = {Gas hydrates possess lower electrical conductivity (inverse of resistivity) than either seawater or ice, but higher than clastic silts and sands, such that electromagnetic methods can be employed to help identify their natural formation in marine and permafrost environments. Controlled laboratory studies offer a means to isolate and quantify the effects of changing individual components within gas-hydrate-bearing systems, in turn yielding insight into the behavior of natural systems. Here we investigate the electrical properties of polycrystalline methane hydrate with ≥25% gas-filled porosity and in mixture with brine. Initially, pure methane hydrate was synthesized from H2O ice and CH4 gas while undergoing electrical impedance measurement, then partially dissociated to assess the effects of pure pore water accumulation on electrical conductivity. Methane hydrate + brine mixtures were then formed by either adding NaCl (0.25–2.5 wt %) to high-purity ice or by using frozen seawater as a reactant. Conductivity was obtained from impedance measurements made in situ throughout synthesis while temperature cycled between +15 °C and -25 °C. Several possible conduction mechanisms were subsequently determined using equivalent circuit modeling. Samples with low NaCl concentration show a doping/impurity effect and a log linear conductivity response as a function of temperature. For higher salt content samples, conductivity increases exponentially with temperature and the log linear relationship no longer holds; instead, we observe phase changes within the samples that follow NaCl–H2O–CH4 phase equilibrium predictions. Final samples were quenched in liquid nitrogen and imaged by cryogenic scanning electron microscopy (cryo-SEM) to assess grain-scale characteristics.},

  doi          = {10.1029/2019JB018364},

  journal      = {Journal of Geophysical Research. Solid Earth},

  number       = 11,

  volume       = 124,

  place        = {United States},

  year         = {Wed Oct 16 00:00:00 EDT 2019},

  month        = {Wed Oct 16 00:00:00 EDT 2019}

}

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https://doi.org/10.1029/2019JB018364

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Cited by: 12 works

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Table 1: Sample conditions of NaCl-Hydrate (NH) and Seawater-Hydrate (SH) during synthesis

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Similar Records

Title: The Effect of Brine on the Electrical Properties of Methane Hydrate

Abstract

Citation Formats

Figures / Tables:

Decreased stability of methane hydrates in marine sediments owing to phase-boundary roughness journal, December 2002

The Electrical Resistivity Log as an Aid in Determining Some Reservoir Characteristics journal, December 1942

Solidification and microstructures of binary ice-I/hydrate eutectic aggregates journal, October 2007

Methane Hydrates in Nature—Current Knowledge and Challenges journal, October 2014

Changes in electrical conductivity of a synthetic basalt during melting journal, October 1972

Archie's Saturation Exponent for Natural Gas Hydrate in Coarse-Grained Reservoirs journal, March 2018

Salinity‐buffered methane hydrate formation and dissociation in gas‐rich systems journal, February 2015

Dynamic multiphase flow model of hydrate formation in marine sediments journal, January 2007

Occurrence and nature of “bottom simulating reflectors” in the northern Gulf of Mexico journal, June 2012

Scanning Electron Microscopy investigations of laboratory-grown gas clathrate hydrates formed from melting ice, and comparison to natural hydrates journal, August 2004

Electrical Properties Probe Measures Water/Ice Content of Martian Soils Using Impedance Spectroscopy conference, March 2007

Impedance Spectroscopy book, January 2005

Three-dimensional distribution of gas hydrate beneath southern Hydrate Ridge: constraints from ODP Leg 204 journal, June 2004

The interaction of climate change and methane hydrates: Climate-Hydrates Interactions journal, February 2017

Electrical properties of methane hydrate + sediment mixtures: The journal, July 2015

The effect of pressure on methane hydration in pure water and sodium chloride solutions journal, July 2001

First results from a marine controlled-source electromagnetic survey to detect gas hydrates offshore Oregon journal, January 2006

Low-Frequency Electrical Properties of Polycrystalline Saline Ice and Salt Hydrates journal, December 2008

The connection between natural gas hydrate and bottom-simulating reflectors: Gas Hydrate and BSRs journal, July 2016

Peculiarities of Methane Clathrate Hydrate Formation and Solid-State Deformation, Including Possible Superheating of Water Ice journal, September 1996

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

Influence of methane hydrate content on electrical sediment properties journal, January 2006

Hydrohalite in cold sea ice: Laboratory observations of single crystals, surface accumulations, and migration rates under a temperature gradient, with application to “Snowball Earth” journal, January 2009

A Critical Review of the Low-frequency Electrical Properties of Ice Sheets and Glaciers journal, March 2007

Electrical properties of microporous rock as a function of saturation and temperature journal, February 2002

Phase equilibrium data of methane hydrates in mixed brine solutions journal, October 2017

Controlled-source electromagnetic and seismic delineation of subseafloor fluid flow structures in a gas hydrate province, offshore Norway journal, May 2016

Electrical properties of polycrystalline methane hydrate: ELECTRICAL PROPERTIES OF METHANE HYDRATE journal, May 2011

Gas hydrates: past and future geohazard? journal, May 2010

Vulcan: A deep-towed CSEM receiver: VULCAN: A DEEP-TOWED CSEM RECEIVER journal, March 2016

Effect of temperature, pressure and iron content on the electrical conductivity of olivine and its high-pressure polymorphs: CONDUCTIVITY OF MAIN MANTLE MINERALS journal, August 2012

Experimental Studies on the Evolvement of Electrical Resistivity during Methane Hydrate Formation in Sediments journal, September 2012

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Methane hydrate stability and anthropogenic climate change journal, January 2007

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On the physical interpretation of constant phase elements journal, June 2009

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A marine electromagnetic survey to detect gas hydrate at Hydrate Ridge, Oregon: EM at Hydrate Ridge journal, August 2011

Acoustic velocity and electrical resistance of hydrate bearing sediments journal, January 2010

Permafrost-Associated Gas Hydrate: Is It Really Approximately 1 % of the Global System? journal, October 2014

Inhibiting effects of transition metal salts on methane hydrate stability journal, November 2016

Direct seismic detection of methane hydrate on the Blake Ridge journal, January 2003

Parametric study of the physical properties of hydrate-bearing sand, silt, and clay sediments: 1. Electromagnetic properties journal, January 2010

Review of natural gas hydrates as an energy resource: Prospects and challenges journal, January 2016

Partial-melt electrical conductivity: Influence of melt composition journal, April 1999

The electrical conductivity of materials containing partial melt: A simple model from Archie's law journal, July 1979

Constant phase element behavior in the poly(o-toluidine) impedance response journal, April 2001

Ostwald ripening changes the pore habit and spatial variability of clathrate hydrate journal, February 2018

Electrical conductivity models in saturated porous media: A review journal, August 2017

Frequency dependent electrical properties of minerals and partial-melts journal, March 1994

Methane hydrate phase equilibria for systems containing NaCl, KCl, and NH 4 Cl journal, April 2016

Distribution of soluble impurities in cold glacial ice journal, January 2004

Linking microscopic guest properties to macroscopic observables in clathrate hydrates: Guest-host hydrogen bonding journal, May 2009

Microstructural evolution of gas hydrates in sedimentary matrices observed with synchrotron X-ray computed tomographic microscopy: MICROSTRUCTRE OF GAS HYDRATES journal, June 2015

Spontaneous NaCl-doped ice at seawater conditions: focus on the mechanisms of ion inclusion journal, January 2017

Overview and Historical Perspective journal, January 1994

Methane hydrate stability and anthropogenic climate change journal, January 2007

Decreased stability of methane hydrates in marine sediments owing to phase-boundary roughness
journal, December 2002

The Electrical Resistivity Log as an Aid in Determining Some Reservoir Characteristics
journal, December 1942

Solidification and microstructures of binary ice-I/hydrate eutectic aggregates
journal, October 2007

Methane Hydrates in Nature—Current Knowledge and Challenges
journal, October 2014

Changes in electrical conductivity of a synthetic basalt during melting
journal, October 1972

Archie's Saturation Exponent for Natural Gas Hydrate in Coarse-Grained Reservoirs
journal, March 2018

Salinity‐buffered methane hydrate formation and dissociation in gas‐rich systems
journal, February 2015

Dynamic multiphase flow model of hydrate formation in marine sediments
journal, January 2007

Occurrence and nature of “bottom simulating reflectors” in the northern Gulf of Mexico
journal, June 2012

Scanning Electron Microscopy investigations of laboratory-grown gas clathrate hydrates formed from melting ice, and comparison to natural hydrates
journal, August 2004

Electrical Properties Probe Measures Water/Ice Content of Martian Soils Using Impedance Spectroscopy
conference, March 2007

Impedance Spectroscopy
book, January 2005

Three-dimensional distribution of gas hydrate beneath southern Hydrate Ridge: constraints from ODP Leg 204
journal, June 2004

The interaction of climate change and methane hydrates: Climate-Hydrates Interactions
journal, February 2017

Electrical properties of methane hydrate + sediment mixtures: The
journal, July 2015

The effect of pressure on methane hydration in pure water and sodium chloride solutions
journal, July 2001

First results from a marine controlled-source electromagnetic survey to detect gas hydrates offshore Oregon
journal, January 2006

Low-Frequency Electrical Properties of Polycrystalline Saline Ice and Salt Hydrates
journal, December 2008

The connection between natural gas hydrate and bottom-simulating reflectors: Gas Hydrate and BSRs
journal, July 2016

Peculiarities of Methane Clathrate Hydrate Formation and Solid-State Deformation, Including Possible Superheating of Water Ice
journal, September 1996

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

Influence of methane hydrate content on electrical sediment properties
journal, January 2006

Hydrohalite in cold sea ice: Laboratory observations of single crystals, surface accumulations, and migration rates under a temperature gradient, with application to “Snowball Earth”
journal, January 2009

A Critical Review of the Low-frequency Electrical Properties of Ice Sheets and Glaciers
journal, March 2007

Electrical properties of microporous rock as a function of saturation and temperature
journal, February 2002

Phase equilibrium data of methane hydrates in mixed brine solutions
journal, October 2017

Controlled-source electromagnetic and seismic delineation of subseafloor fluid flow structures in a gas hydrate province, offshore Norway
journal, May 2016

Electrical properties of polycrystalline methane hydrate: ELECTRICAL PROPERTIES OF METHANE HYDRATE
journal, May 2011

Gas hydrates: past and future geohazard?
journal, May 2010

Vulcan: A deep-towed CSEM receiver: VULCAN: A DEEP-TOWED CSEM RECEIVER
journal, March 2016

Effect of temperature, pressure and iron content on the electrical conductivity of olivine and its high-pressure polymorphs: CONDUCTIVITY OF MAIN MANTLE MINERALS
journal, August 2012

Experimental Studies on the Evolvement of Electrical Resistivity during Methane Hydrate Formation in Sediments
journal, September 2012

High-resolution resistivity imaging of marine gas hydrate structures by combined inversion of CSEM towed and ocean-bottom receiver data
journal, June 2018

Dielectric Relaxation Spectroscopy for Evaluation of the Influence of Solvent Dynamics on Ion Transport in Succinonitrile−Salt Plastic Crystalline Electrolytes
journal, March 2011

Methane hydrate stability and anthropogenic climate change
journal, January 2007

Occurrence of methane hydrate in saturated and unsaturated solutions of sodium chloride and water in dependence of temperature and pressure
journal, July 1983

On the physical interpretation of constant phase elements
journal, June 2009

In-situ gas hydrate hydrate saturation estimated from various well logs at the Mount Elbert Gas Hydrate Stratigraphic Test Well, Alaska North Slope
journal, February 2011

A marine electromagnetic survey to detect gas hydrate at Hydrate Ridge, Oregon: EM at Hydrate Ridge
journal, August 2011

Acoustic velocity and electrical resistance of hydrate bearing sediments
journal, January 2010

Permafrost-Associated Gas Hydrate: Is It Really Approximately 1 % of the Global System?
journal, October 2014

Inhibiting effects of transition metal salts on methane hydrate stability
journal, November 2016

Direct seismic detection of methane hydrate on the Blake Ridge
journal, January 2003

Parametric study of the physical properties of hydrate-bearing sand, silt, and clay sediments: 1. Electromagnetic properties
journal, January 2010

Review of natural gas hydrates as an energy resource: Prospects and challenges
journal, January 2016

Partial-melt electrical conductivity: Influence of melt composition
journal, April 1999

The electrical conductivity of materials containing partial melt: A simple model from Archie's law
journal, July 1979

Constant phase element behavior in the poly(o-toluidine) impedance response
journal, April 2001

Ostwald ripening changes the pore habit and spatial variability of clathrate hydrate
journal, February 2018

Electrical conductivity models in saturated porous media: A review
journal, August 2017

Frequency dependent electrical properties of minerals and partial-melts
journal, March 1994

Methane hydrate phase equilibria for systems containing NaCl, KCl, and NH 4 Cl
journal, April 2016

Distribution of soluble impurities in cold glacial ice
journal, January 2004

Linking microscopic guest properties to macroscopic observables in clathrate hydrates: Guest-host hydrogen bonding
journal, May 2009

Microstructural evolution of gas hydrates in sedimentary matrices observed with synchrotron X-ray computed tomographic microscopy: MICROSTRUCTRE OF GAS HYDRATES
journal, June 2015

Spontaneous NaCl-doped ice at seawater conditions: focus on the mechanisms of ion inclusion
journal, January 2017

Overview and Historical Perspective
journal, January 1994

Methane hydrate stability and anthropogenic climate change
journal, January 2007