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Applications of Nanoporous Materials in Gas Separation and Storage Amit Sharma [email protected]

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Applications of Nanoporous Materials in Gas Separation and Storage Amit Sharma Amit7201@Gmail.Com UNLV Theses, Dissertations, Professional Papers, and Capstones May 2018 Applications of Nanoporous Materials in Gas Separation and Storage Amit Sharma [email protected] Follow this and additional works at: https://digitalscholarship.unlv.edu/thesesdissertations Part of the Chemistry Commons Repository Citation Sharma, Amit, "Applications of Nanoporous Materials in Gas Separation and Storage" (2018). UNLV Theses, Dissertations, Professional Papers, and Capstones. 3326. https://digitalscholarship.unlv.edu/thesesdissertations/3326 This Dissertation is brought to you for free and open access by Digital Scholarship@UNLV. It has been accepted for inclusion in UNLV Theses, Dissertations, Professional Papers, and Capstones by an authorized administrator of Digital Scholarship@UNLV. For more information, please contact [email protected]. APPLICATIONS OF NANOPOROUS MATERIALS IN GAS SEPARATION AND STORAGE By Amit Sharma Master of Technology – Nanotechnology University of Rajasthan - Jaipur, India Bachelor of Technology – Nanotechnology University of Rajasthan - Jaipur, India A dissertation submitted in partial fulfillment of the requirements for the Doctor of Philosophy – Chemistry Department of Chemistry and Biochemistry College of Sciences The Graduate College University of Nevada, Las Vegas May 2018 Copyright 2018 by Amit Sharma All Rights Reserved Dissertation Approval The Graduate College The University of Nevada, Las Vegas February 16, 2018 This dissertation prepared by Amit Sharma entitled Applications of Nanoporous Materials in Gas Separation and Storage is approved in partial fulfillment of the requirements for the degree of Doctor of Philosophy – Chemistry Department of Chemistry and Biochemistry Paul Forster, Ph.D. Kathryn Hausbeck Korgan, Ph.D. Examination Committee Co-Chair Graduate College Interim Dean Kathleen Robins, Ph.D. Examination Committee Co-Chair Jun Young Kang, Ph.D. Examination Committee Member Satish Bhatnagar, Ph.D. Graduate College Faculty Representative ii ABSTRACT Past decades in the field of gas separation and storage utilized the concepts of both cryogenic distillation and non-cryogenic methods such as high-pressure cylinders but few concerns – efficiency, energy intensiveness, cost associated, risk of failure always existed. Recent advances in the field focuses on using porous materials especially nanoporous materials. Nanoporous materials, due to their well-defined structure, range of pore diameters, and striking surface chemistry hold over traditional porous materials for gas separation and storage. With pore diameter less than 2 nm and abundance of energetically favorable sites (such as unsaturated metal sites, channels, cages, cavities etc.), these materials can also undergo various surface decorations to enhance the adsorbate-adsorbent interactions making them suitable for the applications using the principles of pressure swing adsorption. The objective of this study is to show the potential these materials hold in gas separation and storage studies and we provide four different nanoporous materials dedicated to deal with certain gas mixtures. Out of the wide class of nanoporous materials, in first part of this work we show screening of 229 zeolitic frameworks in separation of radiochemically relevant noble gases mixture of Kr/Xe by Grand Canonical Monte Carlo simulations by benchmarking the model by measuring adsorption isotherms at various temperatures. Zeolites with narrow pore system and zig-zag or elliptical cross sections were found to be more selective for Xe. To separate one of the lightest gas mixture of D2/H2 we examine the adsorption into a nanoporous nickel phosphate, VSB-5, which on the basis of gas sorption analysis gives one of the highest heats of adsorption (HOA) for hydrogen (16 kJ/mol). A much higher HOA for D2 with calculated selectivities above 4 for D2 at 140 K suggests that VSB-5 is a promising adsorbent for separations of hydrogen isotopes. iii To understand the storage aspect of nanoporous materials, we utilize the principles of Inelastic Neutron Scattering (INS) to examine the lightest gas (H2) on one of the simplest yet exciting surface of graphene where the H2 gas corresponds to a 2D rotor with a rotational barrier of around 4 meV. This also helps in checking the validity of the model of H2 in an anisotropic potential and thereby provides more insight on the concept of hydrogen storage. A hand-in-hand comparison with a much stronger interaction potential provided by Ni2+ sites in VSB-5 is also studied. A huge shift in the rotational line of hydrogen in VSB-5 represents itself as a case of Kubas complex indicating the strong affinity of the unsaturated metal sites towards H2. To capture a different system of toxic gas of ammonia (NH3), we functionalize a well-studied metal organic framework, HKUST-1 (copper trimesate) containing bound sulfuric acid tethered to the framework through terminal oxygen coordination to the accessible Cu(II) sites. Presence of sulfuric acid in the framework and the NH3 sorption is examined by INS. Here acid modified HKUST-1 shows three times more uptake of NH3 compared with pristine HKUST-1. A series of DFT simulation reveals adsorption of ammonia at the acid -OH site leading to a partial transfer of H+ and giving an elongated O-H-N bond rather than a full transfer of H+ and explaining the observed reversibility of adsorption without the destruction of framework. iv Acknowledgments The work compiled in this dissertation wouldn’t be completed without the kind help from several people who always supported, guided and believed in me throughout this wonderful journey. I am thankful to Dr. Paul Forster for providing me the opportunity to be a part of his group and for his constant encouragement and expert critique on my work. His positive and kind nature always kept me motivated to go an extra mile. I will surely be missing the Saturdays lunch and the conversations on photography. I am also grateful to Dr. Keith Lawler for always being there for me and for being so patient despite how juvenile my doubts were. His comic and serious way of explaining the complicated picture helped me in understanding the basics which I couldn’t get from books. It is due to the efforts of Dr. Kathleen Robins that I was always on track on my graduate program and didn’t get lost in the space and time continuum. Her constant appreciation and support strengthened me to finish off my studies on time. Dr. Jun Kang’s direct approach helped me in visualizing the next step of my studies and research and I am thankful for his insightful comments for my work. I thank Dr. Satish Bhatnagar for his sincere advices and kind appreciation of my work which always boosted my confidence. His sweet way of encouraging helped in concentrating and enjoying the research. I also thank the faculty of Chemistry department for all the advices offered and I can’t express my gratitude to Mark, Debbie, and Bianca for taking care of all the paperwork, positive outlook, kindness, and for always finding a solution for me. At Oak Ridge National Laboratory, I thank team VISION (BL-16B) – Dr. Anibal Javier Ramirez- Cuesta, Dr. Luke Daemen, and Dr. Yongqiang Cheng for introducing me to the field of inelastic neutron scattering and for always being kind and patient. I am thankful to them for providing me an amazing platform for learning and for all the fun experiments. v I thank all my friends at UNLV for all the fun moments and talks, for making all TA responsibilities enjoyable, for the moral support and for all the laughs. My deepest gratitude to my parents Indu and Virendra Sharma and my sister Mona for their unconditional love, support and enthusiasm. My final thanks to my loving wife Astha for the help, support, and for always being by my side all the time. vi Table of Contents Abstract…………………………………………………………………………………………...iii Acknowledgments…………………………………………………………………………………v List of Tables……………………………………………………………………………………..xii List of Figures…………………………………………………………………………………...xiv Chapter 1: Introduction……………………………………………………………………………1 1.1 Nanoporous Materials…………………………………………………………………………2 1.1.1 Zeolites………………………………………………………………………………………3 1.1.2 Metal Organic Frameworks (MOFs)………………………………………………………...4 1.2 Motivation……………………………………………………………………………………..5 1.3 Pressure Swing Adsorption (PSA) and the Factors Associated……………………………….9 1.3.1 Basics of PSA………………………………………………………………………………..9 1.3.2 Factors Governing PSA…………………………………………………………………….13 1.3.2.1 Shape or Size Exclusion…………………………………………………………………..13 1.3.2.2 Thermodynamic Equilibrium Effect……………………………………………………...13 1.3.2.3 Diffusivity………………………………………………………………………………..14 1.3.2.4 Quantum Sieving Effect………………………………………………………………….14 1.3.3 Measures to Determine the Performance of Nanoporous Materials for Gas Separation…….15 1.3.3.1 Selectivity………………………………………………………………………………...15 1.3.3.2 Heat of Adsorption……………………………………………………………………….20 1.4.1 Overview of the Dissertation……………………………………………………………….26 1.5 References…………………………………………………………………………..………..29 Chapter 2: Assessing Zeolite Frameworks for Noble Gas Separations Through a Joint Experimental and Computational Approach……………………………………………………..35 2.1 Abstract………………………………………………………………………………………36 2.2 Motivation……………………………………………………………………………………36 2.2.1 Importance of Kr-Xe……………………………………………………………………….36 vii 2.2.2 Present Techniques to Separate Kr-Xe and the Problems Associated……………………..40 2.3 Zeolites and Their Applications in Pressure Swing Adsorption………………………………41 2.4 Grand Canonical Monte Carlo (GCMC) Simulation…………………………………………43
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