Computational discovery of metal-organic frameworks with high gas deliverable capacity

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dc.contributor.advisorDeem, Michael W.
dc.creatorBao, Yi
dc.date.accessioned2017-08-01T18:35:12Z
dc.date.available2017-08-01T18:35:12Z
dc.date.created2017-05
dc.date.issued2017-04-20
dc.date.submittedMay 2017
dc.date.updated2017-08-01T18:35:12Z
dc.description.abstractMetal-organic frameworks (MOFs) are a rapidly emerging class of nanoporous materials with largely tunable chemistry and diverse applications in gas storage, gas purification, catalysis, sensing and drug delivery. Efforts have been made to develop new MOFs with desirable properties both experimentally and computationally for decades. To guide experimental synthesis, we here develop a computational methodology to explore MOFs with high gas deliverable capacity. This de novo design procedure applies known chemical reactions, considers synthesizability and geometric requirements of organic linkers, and efficiently evolves a population of MOFs to optimize a desirable property. We identify 48 MOFs with higher methane deliverable capacity at 65–5.8 bar condition than the MOF-5 reference in nine networks. In a more comprehensive work, we predict two sets of MOFs with high methane deliverable capacity at a 65–5.8 bar loading–delivery condition or a 35–5.8 bar loading–delivery condition. We also optimize a set of MOFs with high methane accessible internal surface area to investigate the relationship between deliverable capacities and internal surface area. This methodology can be extended to MOFs with multiple types of linkers and multiple SBUs. Flexibile MOFs may allow for sophisticated heat management strategies and also provide higher gas deliverable capacity than rigid frameworks. We investigate flexible MOFs, such as MIL-53 families, and Fe(bdp) and Co(bdp) analogs, to understand the structural phase transition of frameworks and the resulting influence on heat of adsorption. Challenges of simulating a system with a flexible host structure and incoming guest molecules are discussed. Preliminary results from isotherm simulation using the hybrid MC/MD simulation scheme on MIL-53(Cr) are presented. Suggestions for proceeding to understand the free energy profile of flexible MOFs are provided.
dc.format.mimetypeapplication/pdf
dc.identifier.citationBao, Yi. "Computational discovery of metal-organic frameworks with high gas deliverable capacity." (2017) Diss., Rice University. <a href="https://hdl.handle.net/1911/96106">https://hdl.handle.net/1911/96106</a>.
dc.identifier.urihttps://hdl.handle.net/1911/96106
dc.language.isoeng
dc.rightsCopyright is held by the author, unless otherwise indicated. Permission to reuse, publish, or reproduce the work beyond the bounds of fair use or other exemptions to copyright law must be obtained from the copyright holder.
dc.subjectMetal-organic framework
dc.subjectgas adsorption
dc.subjectevolutionary algorithm
dc.subjectdeliverable capacity
dc.subjectflexibility
dc.subjectheat management
dc.subjectcomputational physics
dc.titleComputational discovery of metal-organic frameworks with high gas deliverable capacity
dc.typeThesis
dc.type.materialText
thesis.degree.departmentPhysics and Astronomy
thesis.degree.disciplineNatural Sciences
thesis.degree.grantorRice University
thesis.degree.levelDoctoral
thesis.degree.majorPhysics
thesis.degree.nameDoctor of Philosophy
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