Synergistic Coupling of CO2 and H2O during Expansion of Clays in Supercritical CO2-CH4 Fluid Mixtures

Loring, John S.; Qafoku, Odeta; Thompson, Christopher J.; Mcneill, Ashley S.; Vasiliu, Monica; Dixon, David A.; Miller, Quin RS; McGrail, Bernard P.; Rosso, Kevin M.; Ilton, Eugene S.; Schaef, Herbert T.

doi:10.1021/acs.est.1c00275

Synergistic Coupling of CO2 and H2O during Expansion of Clays in Supercritical CO2-CH4 Fluid Mixtures

Journal Article · Tue Aug 17 04:00:00 EDT 2021 · Environmental Science & Technology

DOI:https://doi.org/10.1021/acs.est.1c00275· OSTI ID:1821889

Loring, John S. ^[1]; Qafoku, Odeta ^[1]; ^[1]; Mcneill, Ashley S. ^[2]; Vasiliu, Monica ^[2]; Dixon, David A. ^[3]; ^[1]; McGrail, Bernard P. ^[1]; ^[1]; Ilton, Eugene S. ^[1]; ^[1]

BATTELLE (PACIFIC NW LAB)
UNIVERSITY OF ALABAMA
University of Alabama, Tuscaloosa

A combination of in operando IR and XRD methods were used to investigate the interaction of variably hydrated supercritical CO2-CH4 fluids with Na/NH4/Cs substituted montmorillonites. Comparing the behavior of Na-clay exposed to CH4 versus CO2 dominant fluid phases demonstrated that CO2 disrupts the H-bond network of intercalated H2O. At relatively low potentials of H2O, CO2 facilitates H2O intercalation and expansion of the interlayer region of the Na-clay. In contrast, CO2 inhibited H2O intercalation but promoted expansion of the Cs-clay. The NH4-clay displayed intermediated behavior. Methane likely intercalated the clays but opportunistically, filling unoccupied space after CO2 and H2O actively expanded the interlayer region. By comparing and contrasting the behavior of the Cs and NH4 clays to the Na Clay we conclude that, whereas H2O is required for initial Na-clay expansion, CO2 synergistically facilitated expansion and hydration of Na-clay by mixing with H2O (the entropic contribution) and participating in the outer solvation sphere of Na (the enthalpic contribution). In contrast, CO2 can directly solvate interlayer Cs and NH4 and cause expansion in the absence of H2O; nonetheless, H2O and CO2 also act synergistically to facilitate expansion of the Cs and NH4 clays at low H2O concentrations.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1821889

Report Number(s):: PNNL-SA-143713

Journal Information:: Environmental Science & Technology, Journal Name: Environmental Science & Technology Journal Issue: 16 Vol. 55

Country of Publication:: United States

Language:: English

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