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Title: Supercritical CO 2 uptake by nonswelling phyllosilicates

Interactions between supercritical (sc) CO 2 and minerals are important when CO 2 is injected into geologic formations for storage and as working fluids for enhanced oil recovery, hydraulic fracturing, and geothermal energy extraction. It has previously been shown that at the elevated pressures and temperatures of the deep subsurface, scCO 2 alters smectites (typical swelling phyllosilicates). However, less is known about the effects of scCO 2 on nonswelling phyllosilicates (illite and muscovite), despite the fact that the latter are the dominant clay minerals in deep subsurface shales and mudstones. Our studies conducted by using single crystals, combining reaction (incubation with scCO 2 ), visualization [atomic force microscopy (AFM)], and quantifications (AFM, X-ray photoelectron spectroscopy, X-ray diffraction, and off-gassing measurements) revealed unexpectedly high CO 2 uptake that far exceeded its macroscopic surface area. Results from different methods collectively suggest that CO 2 partially entered the muscovite interlayers, although the pathways remain to be determined. We hypothesize that preferential dissolution at weaker surface defects and frayed edges allows CO 2 to enter the interlayers under elevated pressure and temperature, rather than by diffusing solely from edges deeply into interlayers. This unexpected uptake of CO 2, can increase CO 2 storage capacitymore » by up to ~30% relative to the capacity associated with residual trapping in a 0.2-porosity sandstone reservoir containing up to 18 mass % of illite/muscovite. This excess CO 2 uptake constitutes a previously unrecognized potential trapping mechanism.« less
Authors:
ORCiD logo [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Geosciences Division, Earth and Environment Sciences Area
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry and Material Sciences Division
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 115; Journal Issue: 5; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Nanoscale Control of Geologic CO2 (NCGC)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; 29 ENERGY PLANNING, POLICY, AND ECONOMY; carbon sequestration; CO2 uptake; nonswelling phyllosilicates; muscovite; illite
OSTI Identifier:
1433114

Wan, Jiamin, Tokunaga, Tetsu K., Ashby, Paul D., Kim, Yongman, Voltolini, Marco, Gilbert, Benjamin, and DePaolo, Donald J.. Supercritical CO2 uptake by nonswelling phyllosilicates. United States: N. p., Web. doi:10.1073/pnas.1710853114.
Wan, Jiamin, Tokunaga, Tetsu K., Ashby, Paul D., Kim, Yongman, Voltolini, Marco, Gilbert, Benjamin, & DePaolo, Donald J.. Supercritical CO2 uptake by nonswelling phyllosilicates. United States. doi:10.1073/pnas.1710853114.
Wan, Jiamin, Tokunaga, Tetsu K., Ashby, Paul D., Kim, Yongman, Voltolini, Marco, Gilbert, Benjamin, and DePaolo, Donald J.. 2018. "Supercritical CO2 uptake by nonswelling phyllosilicates". United States. doi:10.1073/pnas.1710853114. https://www.osti.gov/servlets/purl/1433114.
@article{osti_1433114,
title = {Supercritical CO2 uptake by nonswelling phyllosilicates},
author = {Wan, Jiamin and Tokunaga, Tetsu K. and Ashby, Paul D. and Kim, Yongman and Voltolini, Marco and Gilbert, Benjamin and DePaolo, Donald J.},
abstractNote = {Interactions between supercritical (sc) CO2 and minerals are important when CO2 is injected into geologic formations for storage and as working fluids for enhanced oil recovery, hydraulic fracturing, and geothermal energy extraction. It has previously been shown that at the elevated pressures and temperatures of the deep subsurface, scCO2 alters smectites (typical swelling phyllosilicates). However, less is known about the effects of scCO2 on nonswelling phyllosilicates (illite and muscovite), despite the fact that the latter are the dominant clay minerals in deep subsurface shales and mudstones. Our studies conducted by using single crystals, combining reaction (incubation with scCO2 ), visualization [atomic force microscopy (AFM)], and quantifications (AFM, X-ray photoelectron spectroscopy, X-ray diffraction, and off-gassing measurements) revealed unexpectedly high CO2 uptake that far exceeded its macroscopic surface area. Results from different methods collectively suggest that CO2 partially entered the muscovite interlayers, although the pathways remain to be determined. We hypothesize that preferential dissolution at weaker surface defects and frayed edges allows CO2 to enter the interlayers under elevated pressure and temperature, rather than by diffusing solely from edges deeply into interlayers. This unexpected uptake of CO2, can increase CO2 storage capacity by up to ~30% relative to the capacity associated with residual trapping in a 0.2-porosity sandstone reservoir containing up to 18 mass % of illite/muscovite. This excess CO2 uptake constitutes a previously unrecognized potential trapping mechanism.},
doi = {10.1073/pnas.1710853114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 5,
volume = 115,
place = {United States},
year = {2018},
month = {1}
}