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

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, 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.

[1]  Yifeng Wang,et al.  Hydrophobic Nanoconfinement Enhances CO2 Conversion to H2CO3. , 2023, The journal of physical chemistry letters.

[2]  E. Coker,et al.  Control of Structural Hydrophobicity and Cation Solvation on Interlayer Water Transport during Clay Dehydration. , 2022, Nano letters.

[3]  M. Kļaviņš,et al.  The Prospects of Clay Minerals from the Baltic States for Industrial-Scale Carbon Capture: A Review , 2022, Minerals.

[4]  S. Flude,et al.  Carbon capture and storage at the end of a lost decade , 2021, One Earth.

[5]  Yifeng Wang,et al.  Molecular Origin of Wettability Alteration of Subsurface Porous Media upon Gas Pressure Variations. , 2021, ACS applied materials & interfaces.

[6]  R. Cygan,et al.  Advances in Clayff Molecular Simulation of Layered and Nanoporous Materials and Their Aqueous Interfaces , 2021, The Journal of Physical Chemistry C.

[7]  E. Coker,et al.  Fast Advective Water Flow Through Nanochannels in Clay Interlayers: Implications for Moisture Transport in Soils and Unconventional Oil/Gas Production , 2020 .

[8]  A. V. van Duin,et al.  Interfacial Reactivity and Speciation Emerging from Na-Montmorillonite Interactions with Water and Formic Acid at 200 °C: Insights from Reactive Molecular Dynamics Simulations, Infrared Spectroscopy, and X-ray Scattering Measurements , 2020, ACS Earth and Space Chemistry.

[9]  A. Kalinichev,et al.  Intrinsic hydrophobicity of smectite basal surfaces quantitatively probed by molecular dynamics simulations , 2020 .

[10]  A. Striolo,et al.  Evidence of Facilitated Transport in Crowded Nanopores , 2020, The journal of physical chemistry letters.

[11]  V. Rasouli,et al.  Significant aspects of carbon capture and storage – A review , 2019 .

[12]  J. Greathouse,et al.  Revealing Transition States during the Hydration of Clay Minerals. , 2019, The journal of physical chemistry letters.

[13]  Luyi Sun,et al.  Strategic Design of Clay‐Based Multifunctional Materials: From Natural Minerals to Nanostructured Membranes , 2019, Advanced Functional Materials.

[14]  M. Sahimi,et al.  Molecular Dynamics Simulation of Hydration and Swelling of Mixed-Layer Clays in the Presence of Carbon Dioxide , 2019, The Journal of Physical Chemistry C.

[15]  Shuyu Sun,et al.  Molecular Simulation Study of Montmorillonite in Contact with Water , 2019, Industrial & Engineering Chemistry Research.

[16]  Yifeng Wang,et al.  Differential retention and release of CO2 and CH4 in kerogen nanopores: Implications for gas extraction and carbon sequestration , 2018 .

[17]  A. O. Yazaydin,et al.  Clay Swelling in Dry Supercritical Carbon Dioxide: Effects of Interlayer Cations on the Structure, Dynamics, and Energetics of CO2 Intercalation Probed by XRD, NMR, and GCMD Simulations , 2018 .

[18]  R. Rousseau,et al.  Molecular Level Investigation of CH4 and CO2 Adsorption in Hydrated Calcium–Montmorillonite , 2017 .

[19]  A. Ilgen,et al.  Density Fluctuation in Aqueous Solutions and Molecular Origin of Salting-Out Effect for CO2. , 2017, The journal of physical chemistry. B.

[20]  A. O. Yazaydin,et al.  Molecular Dynamics Study of CO2 and H2O Intercalation in Smectite Clays: Effect of Temperature and Pressure on Interlayer Structure and Dynamics in Hectorite , 2017 .

[21]  D. Cole,et al.  Transport Mechanism of Guest Methane in Water-Filled Nanopores , 2017 .

[22]  D. Hoyt,et al.  Role of Cations in CO2 Adsorption, Dynamics, and Hydration in Smectite Clays under in Situ Supercritical CO2 Conditions , 2017 .

[23]  Christopher W. Jones,et al.  Direct Capture of CO2 from Ambient Air. , 2016, Chemical reviews.

[24]  J. Dzubiella,et al.  Confined Water Determines Transport Properties of Guest Molecules in Narrow Pores. , 2016, ACS nano.

[25]  Shuyu Sun,et al.  Molecular Dynamics Simulations of Carbon Dioxide, Methane, and Their Mixture in Montmorillonite Clay Hydrates , 2016 .

[26]  H. M. Wentinck,et al.  On sorption and swelling of CO2 in clays , 2016 .

[27]  Y. Leng,et al.  Molecular Understanding of CO2 and H2O in a Montmorillonite Clay Interlayer under CO2 Geological Sequestration Conditions , 2016 .

[28]  R. Kirkpatrick,et al.  Supercritical Carbon Dioxide at Smectite Mineral–Water Interfaces: Molecular Dynamics and Adaptive Biasing Force Investigation of CO2/H2O Mixtures Nanoconfined in Na-Montmorillonite , 2015 .

[29]  Y. Schuurman,et al.  Solubility of Gases in Water Confined in Nanoporous Materials: ZSM-5, MCM-41, and MIL-100 , 2015 .

[30]  R. Cygan,et al.  Swelling Properties of Montmorillonite and Beidellite Clay Minerals from Molecular Simulation: Comparison of Temperature, Interlayer Cation, and Charge Location Effects , 2015 .

[31]  Herbert T. Schaef,et al.  Competitive Sorption of CO2 and H2O in 2:1 Layer Phyllosilicates , 2015 .

[32]  E. Gomès,et al.  Climate change conditions (elevated CO2 and temperature) and UV-B radiation affect grapevine (Vitis vinifera cv. Tempranillo) leaf carbon assimilation, altering fruit ripening rates. , 2015, Plant science : an international journal of experimental plant biology.

[33]  T. Plivelic,et al.  Intercalation and Retention of Carbon Dioxide in a Smectite Clay promoted by Interlayer Cations , 2015, Scientific Reports.

[34]  V. Glezakou,et al.  Microstructural response of variably hydrated Ca-rich montmorillonite to supercritical CO2. , 2014, Environmental science & technology.

[35]  A. Kalinichev,et al.  Structural Arrangements of Isomorphic Substitutions in Smectites: Molecular Simulation of the Swelling Properties, Interlayer Structure, and Dynamics of Hydrated Cs–Montmorillonite Revisited with New Clay Models , 2014 .

[36]  P. F. Martin,et al.  In situ study of CO₂ and H₂O partitioning between Na-montmorillonite and variably wet supercritical carbon dioxide. , 2014, Langmuir : the ACS journal of surfaces and colloids.

[37]  Hee‐Tae Jung,et al.  Intercalation of Gas Molecules in Graphene Oxide Interlayer: The Role of Water , 2014 .

[38]  K. Jordan,et al.  Molecular dynamics simulations of turbostratic dry and hydrated montmorillonite with intercalated carbon dioxide. , 2014, The journal of physical chemistry. A.

[39]  Edward J. Maginn,et al.  Force field comparison and thermodynamic property calculation of supercritical CO2 and CH4 using molecular dynamics simulations , 2014 .

[40]  Yuan Xiang,et al.  Molecular Simulations on the Structure and Dynamics of Water Methane Fluids between Na-Montmorillonite Clay Surfaces at Elevated Temperature and Pressure , 2013 .

[41]  K. Jordan,et al.  Molecular Dynamics Simulations of Carbon Dioxide Intercalation in Hydrated Na-Montmorillonite , 2013 .

[42]  R. Cygan,et al.  Molecular Simulation of Carbon Dioxide Capture by Montmorillonite Using an Accurate and Flexible Force Field , 2012 .

[43]  P. F. Martin,et al.  In situ molecular spectroscopic evidence for CO2 intercalation into montmorillonite in supercritical carbon dioxide. , 2012, Langmuir : the ACS journal of surfaces and colloids.

[44]  A. Busch,et al.  X-ray diffraction study of K- and Ca-exchanged montmorillonites in CO2 atmospheres. , 2012, Environmental science & technology.

[45]  Odeta Qafoku,et al.  In situ X-ray diffraction study of Na+ saturated montmorillonite exposed to variably wet super critical CO2. , 2012, Environmental science & technology.

[46]  S. Rempe,et al.  CO2 solvation free energy using quasi-chemical theory. , 2011, The Journal of chemical physics.

[47]  Virginie Marry,et al.  Carbon Dioxide in Montmorillonite Clay Hydrates: Thermodynamics, Structure, and Transport from Molecular Simulation , 2010 .

[48]  Vassiliki-Alexandra Glezakou,et al.  Structure, dynamics and vibrational spectrum of supercritical CO2/H2O mixtures from ab initio molecular dynamics as a function of water cluster formation. , 2010, Physical chemistry chemical physics : PCCP.

[49]  J. Robert,et al.  Hydration Properties and Interlayer Organization of Water and Ions in Synthetic Na-Smectite with Tetrahedral Layer Charge. Part 1. Results from X-ray Diffraction Profile Modeling , 2010 .

[50]  Shekhar Garde,et al.  Characterizing hydrophobicity of interfaces by using cavity formation, solute binding, and water correlations , 2009, Proceedings of the National Academy of Sciences.

[51]  J. Dalmon,et al.  Higher gas solubility in nanoliquids? , 2008, Chemphyschem : a European journal of chemical physics and physical chemistry.

[52]  B. Rotenberg,et al.  Water and ions in clays: Unraveling the interlayer/micropore exchange using molecular dynamics , 2007 .

[53]  D. Bratko,et al.  Gas solubility in hydrophobic confinement. , 2005, The journal of physical chemistry. B.

[54]  B. Lanson,et al.  Investigation of smectite hydration properties by modeling experimental X-ray diffraction patterns: Part I. Montmorillonite hydration properties , 2005 .

[55]  N. Skipper,et al.  Monte Carlo and molecular dynamics simulations of methane in potassium montmorillonite clay hydrates at elevated pressures and temperatures. , 2005, Journal of colloid and interface science.

[56]  R. Cygan,et al.  Molecular Models for the Intercalation of Methane Hydrate Complexes in Montmorillonite Clay , 2004 .

[57]  A. Chatterjee,et al.  Effect of exchangeable cation on the swelling property of 2:1 dioctahedral smectite--a periodic first principle study. , 2004, The Journal of chemical physics.

[58]  Randall T. Cygan,et al.  Molecular Models of Hydroxide, Oxyhydroxide, and Clay Phases and the Development of a General Force Field , 2004 .

[59]  A. Laio,et al.  Escaping free-energy minima , 2002, Proceedings of the National Academy of Sciences of the United States of America.

[60]  J. Pablo,et al.  Monte Carlo simulations of Wyoming sodium montmorillonite hydrates , 2001 .

[61]  G. Sposito,et al.  Surface geochemistry of the clay minerals. , 1999, Proceedings of the National Academy of Sciences of the United States of America.

[62]  P. F. Martin,et al.  Clay Hydration/dehydration in Dry to Water-saturated Supercritical CO2: Implications for Caprock Integrity , 2013 .

[63]  P. F. Martin,et al.  In situ XRD Study of Ca2+ Saturated Montmorillonite (STX-1) Exposed to Anhydrous and Wet Supercritical Carbon Dioxide , 2012 .