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Atomistic Simulations and Computations of Clay Minerals at Geologic Carbon Sequestration Conditions

Makaremi, Meysam (2015) Atomistic Simulations and Computations of Clay Minerals at Geologic Carbon Sequestration Conditions. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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Classical atomistic simulations are carried out to study carbon sequestration at deep underground formations. In classical simulations, formulas and equations are inherently different from those used in continuum and quantum calculations. Here, in contrast to continuum approaches such as the finite element method, interactions of atomic particles are computed, and unlike quantum techniques such as the density functional theory, calculations are not restricted to a limited number of atoms, therefore a balance between accuracy and computational cost makes classical atomistic techniques the best candidate to study layered materials in numerous situations.

The success of CO2 sequestration depends on diverse parameters related to the depth and type of the underground formations. In this work, chemical, physical, and geometrical characteristics of formations are investigated. Different types of interlayer cation (Na+ and Ca2+), intercalated molecule (water and CO2), and clay structure (montmorillonite (MMT) and beidellite (BEI), and pyrophyllite (PPT)) are investigated as chemical parameters. Rotational degree of layers, pressure, temperature and chemical potential are considered as geometrical and physical variables.

Using free energy calculations, stable energy states due to the intercalation of water and carbon dioxide to smectite structures are predicted. For hydrated systems, three states consisting of interlayer spacing values 9-10, 11.5-12.5 and 14.5-15.5 A, respectively called 0W, 1W and 2W hydration state are found. For systems including mixed H2O-CO2 intercalation, the amount of adsorbed CO2 alters and reaches its peak at the sub-first hydration levels. Another fascinating result emerges by simulating the binary MMT-CO2 system. The global minimum is found at the dry (0W) state which explains why there is no experimental observation of pure CO2 adsorption on the MMT surface. Finally, ternary smectite-H2O-CO2 simulations show that the amount of adsorbed CO2 in the clay phase is higher than that of bulk phase suggesting that the underground formation is a proper option to store extensive volumes of the green house gas carbon dioxide.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Makaremi, Meysammem190@pitt.eduMEM190
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairTo, Albert C.albertto@pitt.eduALBERTTO
Committee CoChairJordan, Kenneth D.jordan@pitt.eduJORDAN
Committee MemberGivi, Peymanpeg10@pitt.eduPEG10
Committee Memberzunino, Paolopaz13@pitt.eduPAZ13
Date: 9 June 2015
Date Type: Publication
Defense Date: 18 March 2015
Approval Date: 9 June 2015
Submission Date: 7 April 2015
Access Restriction: 1 year -- Restrict access to University of Pittsburgh for a period of 1 year.
Number of Pages: 110
Institution: University of Pittsburgh
Schools and Programs: Swanson School of Engineering > Mechanical Engineering and Materials Science
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: atomistic simulation, molecular dynamics, Monte Carlo, swelling behavior, smectite, montmorillonite, beidellite, swelling free energy, turbostratic structure, Moire pattern, clay disjoining pressure
Date Deposited: 09 Jun 2015 15:08
Last Modified: 15 Nov 2016 14:27


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