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Title: Nanoscale Chemical Processes Affecting Storage Capacities and Seals during Geologic CO2 Sequestration

Abstract

Geologic CO2 sequestration (GCS) is a promising strategy to mitigate anthropogenic CO2 emission to the atmosphere. Suitable geologic storage sites should have a porous reservoir rock zone where injected CO2 can displace brine and be stored in pores, and an impermeable zone on top of reservoir rocks to hinder upward movement of buoyant CO2. The injection wells (steel casings encased in concrete) pass through these geologic zones and lead CO2 to the desired zones. In subsurface environments, CO2 is reactive as both a supercritical (sc) phase and aqueous (aq) species. Its nanoscale chemical reactions with geomedia and wellbores are closely related to the safety and efficiency of CO2 storage. For example, the injection pressure is determined by the wettability and permeability of geomedia, which can be sensitive to nanoscale mineral-fluid interactions; the sealing safety of the injection sites is affected by the opening and closing of fractures in caprocks and the alteration of wellbore integrity caused by nanoscale chemical reactions; and the time scale for CO2 mineralization is also largely dependent on the chemical reactivities of the reservoir rocks. Therefore, nanoscale chemical processes can influence the hydrogeological and mechanical properties of geomedia, such as their wettability, permeability, mechanical strength, andmore » fracturing. This Account reviews our group’s work on nanoscale chemical reactions and their qualitative impacts on seal integrity and storage capacity at GCS sites from four points of view. First, studies on dissolution of feldspar, an important reservoir rock constituent, and subsequent secondary mineral precipitation are discussed, focusing on the effects of feldspar crystallography, cations, and sulfate anions. Second, interfacial reactions between caprock and brine are introduced using model clay minerals, with focuses on the effects of water chemistries (salinity and organic ligands) and water content on mineral dissolution and surface morphology changes. Third, the hydrogeological responses (using wettability alteration as an example) of clay minerals to chemical reactions are discussed, which connects the nanoscale findings to the transport and capillary trapping of CO2 in the reservoirs. Fourth, the interplay between chemical and mechanical alterations of geomedia, using wellbore cement as a model geomedium, is examined, which provides helpful insights into wellbore and caprock integrities and CO2 mineralization. Combining these four aspects, our group has answered questions related to nanoscale chemical reactions in subsurface GCS sites regarding the types of reactions and the property alterations of reservoirs and caprocks. Ultimately, the findings can shed light on the influences of nanoscale chemical reactions on storage capacities and seals during geologic CO2 sequestration.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1]
  1. Department of Energy, Environmental and Chemical Engineering, Washington University, St. Louis, Missouri 63130, United States
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Nanoscale Control of Geologic CO2 (NCGC); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1368594
Alternate Identifier(s):
OSTI ID: 1508086
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Published Article
Journal Name:
Accounts of Chemical Research
Additional Journal Information:
Journal Name: Accounts of Chemical Research Journal Volume: 50 Journal Issue: 7; Journal ID: ISSN 0001-4842
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Jun, Young-Shin, Zhang, Lijie, Min, Yujia, and Li, Qingyun. Nanoscale Chemical Processes Affecting Storage Capacities and Seals during Geologic CO2 Sequestration. United States: N. p., 2017. Web. doi:10.1021/acs.accounts.6b00654.
Jun, Young-Shin, Zhang, Lijie, Min, Yujia, & Li, Qingyun. Nanoscale Chemical Processes Affecting Storage Capacities and Seals during Geologic CO2 Sequestration. United States. https://doi.org/10.1021/acs.accounts.6b00654
Jun, Young-Shin, Zhang, Lijie, Min, Yujia, and Li, Qingyun. Fri . "Nanoscale Chemical Processes Affecting Storage Capacities and Seals during Geologic CO2 Sequestration". United States. https://doi.org/10.1021/acs.accounts.6b00654.
@article{osti_1368594,
title = {Nanoscale Chemical Processes Affecting Storage Capacities and Seals during Geologic CO2 Sequestration},
author = {Jun, Young-Shin and Zhang, Lijie and Min, Yujia and Li, Qingyun},
abstractNote = {Geologic CO2 sequestration (GCS) is a promising strategy to mitigate anthropogenic CO2 emission to the atmosphere. Suitable geologic storage sites should have a porous reservoir rock zone where injected CO2 can displace brine and be stored in pores, and an impermeable zone on top of reservoir rocks to hinder upward movement of buoyant CO2. The injection wells (steel casings encased in concrete) pass through these geologic zones and lead CO2 to the desired zones. In subsurface environments, CO2 is reactive as both a supercritical (sc) phase and aqueous (aq) species. Its nanoscale chemical reactions with geomedia and wellbores are closely related to the safety and efficiency of CO2 storage. For example, the injection pressure is determined by the wettability and permeability of geomedia, which can be sensitive to nanoscale mineral-fluid interactions; the sealing safety of the injection sites is affected by the opening and closing of fractures in caprocks and the alteration of wellbore integrity caused by nanoscale chemical reactions; and the time scale for CO2 mineralization is also largely dependent on the chemical reactivities of the reservoir rocks. Therefore, nanoscale chemical processes can influence the hydrogeological and mechanical properties of geomedia, such as their wettability, permeability, mechanical strength, and fracturing. This Account reviews our group’s work on nanoscale chemical reactions and their qualitative impacts on seal integrity and storage capacity at GCS sites from four points of view. First, studies on dissolution of feldspar, an important reservoir rock constituent, and subsequent secondary mineral precipitation are discussed, focusing on the effects of feldspar crystallography, cations, and sulfate anions. Second, interfacial reactions between caprock and brine are introduced using model clay minerals, with focuses on the effects of water chemistries (salinity and organic ligands) and water content on mineral dissolution and surface morphology changes. Third, the hydrogeological responses (using wettability alteration as an example) of clay minerals to chemical reactions are discussed, which connects the nanoscale findings to the transport and capillary trapping of CO2 in the reservoirs. Fourth, the interplay between chemical and mechanical alterations of geomedia, using wellbore cement as a model geomedium, is examined, which provides helpful insights into wellbore and caprock integrities and CO2 mineralization. Combining these four aspects, our group has answered questions related to nanoscale chemical reactions in subsurface GCS sites regarding the types of reactions and the property alterations of reservoirs and caprocks. Ultimately, the findings can shed light on the influences of nanoscale chemical reactions on storage capacities and seals during geologic CO2 sequestration.},
doi = {10.1021/acs.accounts.6b00654},
journal = {Accounts of Chemical Research},
number = 7,
volume = 50,
place = {United States},
year = {Fri Jul 07 00:00:00 EDT 2017},
month = {Fri Jul 07 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.accounts.6b00654

Citation Metrics:
Cited by: 26 works
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Figures / Tables:

Figure 1 Figure 1: CO2 trapping mechanisms at GCS sites.

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Works referenced in this record:

Microtomographic Quantification of Hydraulic Clay Mineral Displacement Effects During a CO 2 Sequestration Experiment with Saline Aquifer Sandstone
journal, August 2012

  • Sell, Kathleen; Enzmann, Frieder; Kersten, Michael
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es3013358

Geochemistry of Wellbore Integrity in CO2 Sequestration: Portland Cement-Steel-Brine-CO2 Interactions
journal, January 2013


Geochemistry of Geologic Carbon Sequestration: An Overview
journal, January 2013

  • DePaolo, D. J.; Cole, D. R.
  • Reviews in Mineralogy and Geochemistry, Vol. 77, Issue 1
  • DOI: 10.2138/rmg.2013.77.1

Capillary Pressure and Mineral Wettability Influences on Reservoir CO2 Capacity
journal, January 2013

  • Tokunaga, T. K.; Wan, J.
  • Reviews in Mineralogy and Geochemistry, Vol. 77, Issue 1
  • DOI: 10.2138/rmg.2013.77.14

CO 2 wettability of seal and reservoir rocks and the implications for carbon geo-sequestration
journal, January 2015

  • Iglauer, Stefan; Pentland, C. H.; Busch, A.
  • Water Resources Research, Vol. 51, Issue 1
  • DOI: 10.1002/2014WR015553

The coordination chemistry of weathering: IV. Inhibition of the dissolution of oxide minerals
journal, May 1994

  • Biber, Madeleine V.; dos Santos Afonso, Maria; Stumm, Werner
  • Geochimica et Cosmochimica Acta, Vol. 58, Issue 9
  • DOI: 10.1016/0016-7037(94)90280-1

Physical and chemical characteristics of potential seal strata in regions considered for demonstrating geological saline CO2 sequestration
journal, February 2011

  • Griffith, Craig A.; Dzombak, David A.; Lowry, Gregory V.
  • Environmental Earth Sciences, Vol. 64, Issue 4
  • DOI: 10.1007/s12665-011-0911-5

Dissolution and Precipitation of Clay Minerals under Geologic CO 2 Sequestration Conditions: CO 2 −Brine−Phlogopite Interactions
journal, August 2010

  • Shao, Hongbo; Ray, Jessica R.; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 44, Issue 15
  • DOI: 10.1021/es1010169

Effects of Salinity and the Extent of Water on Supercritical CO 2 -Induced Phlogopite Dissolution and Secondary Mineral Formation
journal, February 2011

  • Shao, Hongbo; Ray, Jessica R.; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 45, Issue 4
  • DOI: 10.1021/es1034975

Chemical Reactions of Portland Cement with Aqueous CO 2 and Their Impacts on Cement’s Mechanical Properties under Geologic CO 2 Sequestration Conditions
journal, May 2015

  • Li, Qingyun; Lim, Yun Mook; Flores, Katharine M.
  • Environmental Science & Technology, Vol. 49, Issue 10
  • DOI: 10.1021/es5063488

Structure-Dependent Interactions between Alkali Feldspars and Organic Compounds: Implications for Reactions in Geologic Carbon Sequestration
journal, August 2012

  • Yang, Yi; Min, Yujia; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es302324m

The heterogeneous reaction of Gibbsite powder with aqueous inorganic acid solutions; kinetics and mechanism
journal, January 1969

  • Packter, A.; Dhillon, H. S.
  • Journal of the Chemical Society A: Inorganic, Physical, Theoretical
  • DOI: 10.1039/j19690002588

Wettability Phenomena at the CO 2 –Brine–Mineral Interface: Implications for Geologic Carbon Sequestration
journal, August 2012

  • Wang, Shibo; Edwards, Ian M.; Clarens, Andres F.
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es301297z

Biotite–Brine Interactions under Acidic Hydrothermal Conditions: Fibrous Illite, Goethite, and Kaolinite Formation and Biotite Surface Cracking
journal, July 2011

  • Hu, Yandi; Ray, Jessica R.; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 45, Issue 14
  • DOI: 10.1021/es200489y

A Functional Relationship Between Capillary Pressure, Saturation, and Interfacial Area as Revealed by a Pore-Scale Network Model
journal, August 1996

  • Reeves, Paul C.; Celia, Michael A.
  • Water Resources Research, Vol. 32, Issue 8
  • DOI: 10.1029/96WR01105

Anorthite Dissolution under Conditions Relevant to Subsurface CO 2 Injection: Effects of Na + , Ca 2+ , and Al 3+
journal, September 2016


Limitations for brine acidification due to SO2 co-injection in geologic carbon sequestration
journal, May 2010

  • Ellis, Brian R.; Crandell, Lauren E.; Peters, Catherine A.
  • International Journal of Greenhouse Gas Control, Vol. 4, Issue 3
  • DOI: 10.1016/j.ijggc.2009.11.006

The effects of initial acetate concentration on CO2–brine-anorthite interactions under geologic CO2 sequestration conditions
journal, January 2011

  • Yang, Yi; Ronzio, Christian; Jun, Young-Shin
  • Energy & Environmental Science, Vol. 4, Issue 11
  • DOI: 10.1039/c1ee01890f

Supercritical CO 2 and Ionic Strength Effects on Wettability of Silica Surfaces: Equilibrium Contact Angle Measurements
journal, August 2012

  • Jung, Jong-Won; Wan, Jiamin
  • Energy & Fuels, Vol. 26, Issue 9
  • DOI: 10.1021/ef300913t

Dissolution-Driven Permeability Reduction of a Fractured Carbonate Caprock
journal, April 2013

  • Ellis, Brian R.; Fitts, Jeffrey P.; Bromhal, Grant S.
  • Environmental Engineering Science, Vol. 30, Issue 4
  • DOI: 10.1089/ees.2012.0337

Geological Sequestration of Carbon Dioxide
journal, September 2001


Geochemical aspects of CO2 sequestration in deep saline aquifers: A review
journal, September 2015


The reactivity of FE(III) (hydr)oxides: Effects of ligands in inhibiting the dissolution
journal, November 1993

  • Bondietti, Gianluca; Sinniger, Jürg; Stumm, Werner
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 79, Issue 2-3
  • DOI: 10.1016/0927-7757(93)80171-A

Water-CO 2 -mineral systems: Interfacial tension, contact angle, and diffusion-Implications to CO 2 geological storage : WATER CO
journal, July 2010

  • Espinoza, D. Nicolas; Santamarina, J. Carlos
  • Water Resources Research, Vol. 46, Issue 7
  • DOI: 10.1029/2009WR008634

Na + , Ca 2+ , and Mg 2+ in Brines Affect Supercritical CO 2 –Brine–Biotite Interactions: Ion Exchange, Biotite Dissolution, and Illite Precipitation
journal, May 2012

  • Hu, Yandi; Ray, Jessica R.; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es301273g

A mechanistic understanding of plagioclase dissolution based on Al occupancy and T–O bond length: from geologic carbon sequestration to ambient conditions
journal, January 2013

  • Yang, Yi; Min, Yujia; Jun, Young-Shin
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 42
  • DOI: 10.1039/c3cp52722k

Experimental evaluation of interactions in supercritical CO2/water/rock minerals system under geologic CO2 sequestration conditions
journal, December 2007

  • Lin, Hongfei; Fujii, Takashi; Takisawa, Reisuke
  • Journal of Materials Science, Vol. 43, Issue 7
  • DOI: 10.1007/s10853-007-2029-4

Plagioclase Dissolution during CO 2 –SO 2 Cosequestration: Effects of Sulfate
journal, January 2015

  • Min, Yujia; Kubicki, James D.; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 49, Issue 3
  • DOI: 10.1021/es504586u

Effects of Salinity-Induced Chemical Reactions on Biotite Wettability Changes under Geologic CO 2 Sequestration Conditions
journal, February 2016

  • Zhang, Lijie; Kim, Yongman; Jung, Haesung
  • Environmental Science & Technology Letters, Vol. 3, Issue 3
  • DOI: 10.1021/acs.estlett.5b00359

Effects of organic ligands on supercritical CO2-induced phlogopite dissolution and secondary mineral formation
journal, November 2011


Scale effect on porosity and permeability: Kinetics, model, and correlation
journal, February 2001


Effects of Sulfate during CO 2 Attack on Portland Cement and Their Impacts on Mechanical Properties under Geologic CO 2 Sequestration Conditions
journal, May 2015

  • Li, Qingyun; Lim, Yun Mook; Jun, Young-Shin
  • Environmental Science & Technology, Vol. 49, Issue 11
  • DOI: 10.1021/es506349u

Effects of Al/Si ordering on feldspar dissolution: Part II. The pH dependence of plagioclases’ dissolution rates
journal, February 2014


Potential environmental issues of CO2 storage in deep saline aquifers: Geochemical results from the Frio-I Brine Pilot test, Texas, USA
journal, June 2009


Effects of Al/Si ordering on feldspar dissolution: Part I. Crystallographic control on the stoichiometry of dissolution reaction
journal, February 2014


Contact angle measurement ambiguity in supercritical CO2–water–mineral systems: Mica as an example
journal, December 2014

  • Wan, Jiamin; Kim, Yongman; Tokunaga, Tetsu K.
  • International Journal of Greenhouse Gas Control, Vol. 31
  • DOI: 10.1016/j.ijggc.2014.09.029

Feldspar dissolution at 25 degrees C and low pH
journal, February 1996

  • Brantley, S. L.; Stillings, L.
  • American Journal of Science, Vol. 296, Issue 2
  • DOI: 10.2475/ajs.296.2.101

Impacts of Geochemical Reactions on Geologic Carbon Sequestration
journal, August 2012

  • Jun, Young-Shin; Giammar, Daniel E.; Werth, Charles J.
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es3027133

Brucite [Mg(OH2)] carbonation in wet supercritical CO2: An in situ high pressure X-ray diffraction study
journal, December 2011

  • Schaef, H. T.; Windisch, C. F.; McGrail, B. P.
  • Geochimica et Cosmochimica Acta, Vol. 75, Issue 23
  • DOI: 10.1016/j.gca.2011.09.029

Experimental study on water–rock interactions during CO2 flooding in the Tensleep Formation, Wyoming, USA
journal, March 2000


In Situ Infrared Spectroscopic Study of Forsterite Carbonation in Wet Supercritical CO 2
journal, July 2011

  • Loring, John S.; Thompson, Christopher J.; Wang, Zheming
  • Environmental Science & Technology, Vol. 45, Issue 14
  • DOI: 10.1021/es201284e

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.