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Title: CO2 Sorption to Subsingle Hydration Layer Montmorillonite Clay Studied by Excess Sorption and Neutron Diffraction Measurements

Abstract

Geologic storage of CO2 requires that the caprock sealing the storage rock is highly impermeable to CO2. Swelling clays, which are important components of caprocks, may interact with CO2 leading to volume change and potentially impacting the seal quality. The interactions of supercritical (sc) CO2 with Na saturated montmorillonite clay containing a subsingle layer of water in the interlayer region have been studied by sorption and neutron diffraction techniques. The excess sorption isotherms show maxima at bulk CO2 densities of ≈0.15 g/cm3, followed by an approximately linear decrease of excess sorption to zero and negative values with increasing CO2 bulk density. Neutron diffraction experiments on the same clay sample measured interlayer spacing and composition. The results show that limited amounts of CO2 are sorbed into the interlayer region, leading to depression of the interlayer peak intensity and an increase of the d(001) spacing by ca. 0.5 Å. The density of CO2 in the clay pores is relatively stable over a wide range of CO2 pressures at a given temperature, indicating the formation of a clay-CO2 phase. Finally, at the excess sorption maximum, increasing CO2 sorption with decreasing temperature is observed while the high-pressure sorption properties exhibit weak temperature dependence.

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1060646
Report Number(s):
PNNL-SA-90289
Journal ID: ISSN 0013-936X; KC0302060
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 47; Journal Issue: 1; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

Citation Formats

Rother, Gernot, Ilton, Eugene S., Wallacher, Dirk, Hauβ, Thomas, Schaef, Herbert T., Qafoku, Odeta, Rosso, Kevin M., Felmy, Andrew R., Krukowski, Elizabeth G., Stack, Andrew G., Grimm, Nico, and Bodnar, Robert J. CO2 Sorption to Subsingle Hydration Layer Montmorillonite Clay Studied by Excess Sorption and Neutron Diffraction Measurements. United States: N. p., 2013. Web. doi:10.1021/es301382y.
Rother, Gernot, Ilton, Eugene S., Wallacher, Dirk, Hauβ, Thomas, Schaef, Herbert T., Qafoku, Odeta, Rosso, Kevin M., Felmy, Andrew R., Krukowski, Elizabeth G., Stack, Andrew G., Grimm, Nico, & Bodnar, Robert J. CO2 Sorption to Subsingle Hydration Layer Montmorillonite Clay Studied by Excess Sorption and Neutron Diffraction Measurements. United States. https://doi.org/10.1021/es301382y
Rother, Gernot, Ilton, Eugene S., Wallacher, Dirk, Hauβ, Thomas, Schaef, Herbert T., Qafoku, Odeta, Rosso, Kevin M., Felmy, Andrew R., Krukowski, Elizabeth G., Stack, Andrew G., Grimm, Nico, and Bodnar, Robert J. 2013. "CO2 Sorption to Subsingle Hydration Layer Montmorillonite Clay Studied by Excess Sorption and Neutron Diffraction Measurements". United States. https://doi.org/10.1021/es301382y.
@article{osti_1060646,
title = {CO2 Sorption to Subsingle Hydration Layer Montmorillonite Clay Studied by Excess Sorption and Neutron Diffraction Measurements},
author = {Rother, Gernot and Ilton, Eugene S. and Wallacher, Dirk and Hauβ, Thomas and Schaef, Herbert T. and Qafoku, Odeta and Rosso, Kevin M. and Felmy, Andrew R. and Krukowski, Elizabeth G. and Stack, Andrew G. and Grimm, Nico and Bodnar, Robert J.},
abstractNote = {Geologic storage of CO2 requires that the caprock sealing the storage rock is highly impermeable to CO2. Swelling clays, which are important components of caprocks, may interact with CO2 leading to volume change and potentially impacting the seal quality. The interactions of supercritical (sc) CO2 with Na saturated montmorillonite clay containing a subsingle layer of water in the interlayer region have been studied by sorption and neutron diffraction techniques. The excess sorption isotherms show maxima at bulk CO2 densities of ≈0.15 g/cm3, followed by an approximately linear decrease of excess sorption to zero and negative values with increasing CO2 bulk density. Neutron diffraction experiments on the same clay sample measured interlayer spacing and composition. The results show that limited amounts of CO2 are sorbed into the interlayer region, leading to depression of the interlayer peak intensity and an increase of the d(001) spacing by ca. 0.5 Å. The density of CO2 in the clay pores is relatively stable over a wide range of CO2 pressures at a given temperature, indicating the formation of a clay-CO2 phase. Finally, at the excess sorption maximum, increasing CO2 sorption with decreasing temperature is observed while the high-pressure sorption properties exhibit weak temperature dependence.},
doi = {10.1021/es301382y},
url = {https://www.osti.gov/biblio/1060646}, journal = {Environmental Science and Technology},
issn = {0013-936X},
number = 1,
volume = 47,
place = {United States},
year = {Wed Jan 02 00:00:00 EST 2013},
month = {Wed Jan 02 00:00:00 EST 2013}
}