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Transport of Water and Ions Through Single-Walled Armchair Carbon Nanotubes: a Molecular Dynamics Study

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Transport of Water and Ions Through Single-Walled Armchair Carbon Nanotubes: a Molecular Dynamics Study University of Tennessee, Knoxville TRACE: Tennessee Research and Creative Exchange Doctoral Dissertations Graduate School 12-2017 Transport of water and ions through single-walled armchair carbon nanotubes: A molecular dynamics study Michelle Patricia Aranha University of Tennessee, Knoxville, [email protected] Follow this and additional works at: https://trace.tennessee.edu/utk_graddiss Part of the Atomic, Molecular and Optical Physics Commons, Biological and Chemical Physics Commons, Biology and Biomimetic Materials Commons, Membrane Science Commons, Nanoscience and Nanotechnology Commons, Statistical, Nonlinear, and Soft Matter Physics Commons, and the Transport Phenomena Commons Recommended Citation Aranha, Michelle Patricia, "Transport of water and ions through single-walled armchair carbon nanotubes: A molecular dynamics study. " PhD diss., University of Tennessee, 2017. https://trace.tennessee.edu/utk_graddiss/4731 This Dissertation is brought to you for free and open access by the Graduate School at TRACE: Tennessee Research and Creative Exchange. It has been accepted for inclusion in Doctoral Dissertations by an authorized administrator of TRACE: Tennessee Research and Creative Exchange. For more information, please contact [email protected]. To the Graduate Council: I am submitting herewith a dissertation written by Michelle Patricia Aranha entitled "Transport of water and ions through single-walled armchair carbon nanotubes: A molecular dynamics study." I have examined the final electronic copy of this dissertation for form and content and recommend that it be accepted in partial fulfillment of the equirr ements for the degree of Doctor of Philosophy, with a major in Chemical Engineering. Brian J. Edwards, Major Professor We have read this dissertation and recommend its acceptance: Steven M. Abel, Joshua Sangoro, Jerome Baudry Accepted for the Council: Dixie L. Thompson Vice Provost and Dean of the Graduate School (Original signatures are on file with official studentecor r ds.) Transport of water and ions through single-walled armchair carbon nanotubes: A molecular dynamics study A Dissertation Presented for the Doctor of Philosophy Degree The University of Tennessee, Knoxville Michelle Patricia Aranha December 2017 © 2017 Michelle Patricia Aranha All rights reserved ii Dedication I would like to dedicate this dissertation to my family for their unconditional love, support and encouragement. iii Acknowledgements I would like to extend my sincerest thanks to my advisor, Dr. Brian J. Edwards for his contribution with helpful suggestions and guidance during the entire course of my graduate studies. He gave me the freedom and the confidence to pursue different aspects of the subject matter and I have learned much from him. I am also thankful to him for his patience for proofreading and for providing many valuable comments on my dissertation. I am also deeply appreciative of the insightful critique that I received from my committee members - Dr. Jerome Baudry, Dr. Joshua Sangoro and Dr. Steve Abel during the proposal defense. My work and I have benefitted greatly from their recommendations and constructive feedback. This work has been supported in part by the computational resources provided by the Extreme science and discovery environment program (XSEDE Project # CTS160032 and CTS160038), Oak Ridge Leadership Computing Facility (OLCF Project # NTI107) and the high- performance computing facilities (Newton and Beacon) at the University of Tennessee, Knoxville. I am thankful for the award of substantial computational time by these agencies that have made this work possible. I would also like to thank the University of Tennessee, Knoxville (UTK) for the Chancellor’s fellowship, the funding from the Chemical and Biomolecular Engineering (CBE) Department as well as the recent generous scholarship from the Elsie L. Crenshaw foundation that have supported me financially. I would like to thank the wonderful and kind people at the University of Tennessee, especially Rita and Amy at the CBE department who have helped me over the years with a number of administrative tasks and have thereby made things easier for me. iv I consider myself privileged to have been a part of the Chemical Engineering Department at UTK; here I gained the unique opportunity of interacting with so many bright minds from all over the world and this has tremendously enriched my experience as a graduate student. Additionally, it has been a pleasure working in MRAIL office (Dougherty 306 A, B) for the last 4 and half years. I have fond memories of the discussions shared over many interesting topics with both current and past members and I have tremendously enjoyed being a part of the group. Hadi, Hanieh, Mahdy, Mouge, Amir, Reza, Travis, Bo, and Xiangui: it was fun getting to know you and your hard work and the dedication that you showed towards your research served as a constant source of inspiration to me. I was extremely fortunate to have some exceptionally supportive women as my batchmates and friends: Diana, Zuania, Samantha, Nelly, and Samiksha. I could always count on them for being there when needed. I owe gratitude to my friend Dominik with whom I have shared many enjoyable conversations and delightful meals. I would like to thank my friends Abhinav, Mary and Fatemeh who are no longer in Knoxville but have nevertheless had a positive influence on me. I am thankful for the wonderful learning experience at the University of Tennessee, Knoxville and I will always cherish the memories from my time spent here. To the people in my life who have always encouraged me and who make everything worthwhile: my mother, father, sister, and brother-in-law - Thank you for everything, I love you and I am indebted to you forever. v Abstract The narrow hydrophobic interior of a carbon nanotube (CNT) poses a barrier to the transport of water and ions, and yet, unexpectedly, numerous experimental and simulation studies have confirmed fast water transport rates comparable to those seen in biological aquaporin channels. These outstanding features of high water permeability and high solute rejection of even dissolved ions that would typically require a lot of energy for separation in commercial processes makes carbon nanotubes an exciting candidate for desalination membranes. Extending ion exclusion beyond simple mechanical sieving by the inclusion of electrostatics via added functionality to the nanotube bears promise to not only reduce the energy requirement of the ion rejection process but to also lend the nanotube an added attribute of perm-selectivity. Confinement of water and ions in the nanotube leads to unique structure, dynamics, and electrostatic effects, which manifest as a result of discreteness of molecules, ion-ion interactions, and ion-specific interactions at nanoscale confinements that are not accounted for in continuum- based transport equations. Using Molecular dynamics (MD), an attempt has been made to provide a detailed molecular-level understanding of the structure, dynamics, and energetic aspects of the permeation mechanism as functions of CNT pore sizes, external solution concentrations, the number and nature of charges on the CNT wall, and external electric fields. Ion transport and electrolyte rejection rates are calculated from long-timescale MD simulations for the cases studied herein, and these are compared to the predictions of continuum theory. Additionally, ion conduction rates are indirectly calculated as functions of the energy barriers that are obtained by using umbrella sampling and free energy perturbation methods. The feasibility of using the thermodynamically-derived Donnan theory to make realistic predictions of co-ion concentrations in charged CNT-based nanoporous membranes with diameters less than 3 nm is discussed. vi Furthermore, the deviations from macroscopic ion transport predictions and their possible causes are highlighted. It is hoped that this work, when taken in conjunction with experimental studies, will not only help to extend the general continuum-based transport equations to cover nanoscale transport phenomena but will also help to improve the MD force-fields to enable predictions with greater accuracy. vii Table of Contents Introduction ......................................................................................................... 1 1.1 Relevance and applicability ............................................................................................. 1 1.2 Water flow enhancement .................................................................................................. 2 1.3 Modification of structure and dynamics of water under confinement ............................. 3 1.4 Ion transport ..................................................................................................................... 4 1.5 Predictive theories ............................................................................................................ 5 1.6 Objectives of this study .................................................................................................... 9 1.7 Organization of chapters ................................................................................................ 12 Theory and Methods ......................................................................................... 14 2.1 Macroscopic theory ........................................................................................................ 14 Poisson–Boltzmann theory ....................................................................................
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