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    Metal-Organic Frameworks: Building Block Design Strategies for the Synthesis of MOFs.

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    Name:
    Final Dissertation 23nov2014.pdf
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    16.37Mb
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    PDF
    Description:
    Dissertation
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    Type
    Dissertation
    Authors
    Luebke, Ryan cc
    Advisors
    Eddaoudi, Mohamed cc
    Committee members
    Pinnau, Ingo cc
    Takanabe, Kazuhiro cc
    Zaworotko, Michael
    Program
    Chemical Science
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2014-09
    Embargo End Date
    2015-12-01
    Permanent link to this record
    http://hdl.handle.net/10754/336368
    
    Metadata
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    Access Restrictions
    At the time of archiving, the student author of this dissertation opted to temporarily restrict access to it. The full text of this dissertation became available to the public after the expiration of the embargo on 2015-12-01.
    Abstract
    A significant and ongoing challenge in materials chemistry and furthermore solid state chemistry is to design materials with the desired properties and characteristics. The field of Metal-Organic Frameworks (MOFs) offers several strategies to address this challenge and has proven fruitful at allowing some degree of control over the resultant materials synthesized. Several methodologies for synthesis of MOFs have been developed which rely on use of predetermined building blocks. The work presented herein is focused on the utilization of two of these design principles, namely the use of molecular building blocks (MBBs) and supermolecular building blocks (SBBs) to target MOF materials having desired connectivities (topologies). These design strategies also permit the introduction of specific chemical moieties, allowing for modification of the MOFs properties. This research is predominantly focused on two platforms (rht-MOFs and ftw-MOFs) which topologically speaking are edge transitive binodal nets; ftw being a (4,12)-connected net and rht being a (3,24)-connected net. These highly connected nets (at least one node having connectivity greater than eight) have been purposefully targeted to increase the predictability of structural outcome. A general trend in topology is that there is an inverse relationship between the connectivity of the node(s) and the number of topological outcomes. Therefore the key to this research (and to effective use of the SBB and MBB approaches) is identification of conditions which allow for reliable formation of the targeted MBBs and SBBs. In the case of the research presented herein: a 12-connected Group IV or Rare Earth based hexanuclear MBB and a 24-connected transition metal based SBB were successfully targeted and synthesized. These two synthetic platforms will be presented and used as examples of how these design methods have been (and can be further) utilized to modify existing materials or develop new materials for gas storage and separation applications for environmental and energy related applications including hydrogen, methane, carbon dioxide and hydrocarbon storage or separations.
    Citation
    Luebke, R. (2014). Metal-Organic Frameworks: Building Block Design Strategies for the Synthesis of MOFs. KAUST Research Repository. https://doi.org/10.25781/KAUST-H14L9
    DOI
    10.25781/KAUST-H14L9
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-H14L9
    Scopus Count
    Collections
    Dissertations; Physical Science and Engineering (PSE) Division; Chemical Science Program

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