Control of the Structural Charge Distribution and Hydration State upon Intercalation of CO2 into Expansive Clay Interlayers

Ho, Tuan A.; Wang, Yifeng; Rempe, Susan B.; Dasgupta, Nabankur; Johnston, Cliff T.; Xu, Guangping; Zwier, Timothy S.; Mills, Melissa Marie

doi:10.1021/acs.jpclett.3c00291

Title: Control of the Structural Charge Distribution and Hydration State upon Intercalation of CO₂ into Expansive Clay Interlayers

Journal Article · 15 March 2023 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.3c00291 · OSTI ID:2311578

^[1]; Wang, Yifeng ^[1];

^[2];

^[1];

^[3]; Xu, Guangping ^[1];

^[4]; Mills, Melissa Marie ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
Purdue Univ., West Lafayette, IN (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Numerous experimental investigations indicated that expansive clays such as montmorillonite can intercalate CO₂ preferentially into their interlayers and therefore potentially act as a material for CO₂ separation, capture, and storage. However, an understanding of the energy–structure relationship during the intercalation of CO₂ into clay interlayers remains elusive. Here, in this study, we use metadynamics molecular dynamics simulations to elucidate the energy landscape associated with CO₂ intercalation. Our free energy calculations indicate that CO₂ favorably partitions into nanoconfined water in clay interlayers from a gas phase, leading to an increase in the CO₂/H₂O ratio in clay interlayers as compared to that in bulk water. CO₂ molecules prefer to be located at the centers of charge-neutral hydrophobic siloxane rings, whereas interlayer spaces close to structural charges tend to avoid CO₂ intercalation. The structural charge distribution significantly affects the amount of CO₂ intercalated in the interlayers. These results provide a mechanistic understanding of CO₂ intercalation in clays for CO₂ separation, capture, and storage.

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Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: NA0003525

OSTI ID:: 2311578

Report Number(s):: SAND--2023-03195J

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 11 Vol. 14; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Control of the Structural Charge Distribution and Hydration State upon Intercalation of CO2 into Expansive Clay Interlayers

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Title: Control of the Structural Charge Distribution and Hydration State upon Intercalation of CO₂ into Expansive Clay Interlayers