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    Reticular Chemistry Strategies: Design and Applications of Metal-Organic Frameworks

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    Name:
    NorahSAlsadunDissertation.pdf
    Size:
    33.75Mb
    Format:
    PDF
    Description:
    PhD Dissertation
    Embargo End Date:
    2023-04-20
    Download
    Type
    Dissertation
    Authors
    Alsadun, Norah Sadun cc
    Advisors
    Eddaoudi, Mohamed cc
    Committee members
    Bakr, Osman cc
    Hadjichristidis, Nikos cc
    Maurin, Guillaume cc
    Program
    Chemical Science
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2022-04
    Embargo End Date
    2023-04-20
    Permanent link to this record
    http://hdl.handle.net/10754/676327
    
    Metadata
    Show full item record
    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 will become available to the public after the expiration of the embargo on 2023-04-20.
    Abstract
    Designing materials and questing the perfect candidate, or isoreticular series to tackle challenges in areas where no other materials can perform is where Metal-Organic-Frameworks (MOFs) can lead, thanks to their aperture tuning, pore expansion, and made-to-target functionality. The reticular chemistry principles and its design toolkit, including molecular building blocks (MBBs), supermolecular building blocks (SBBs), in addition to supermolecular building layers (SBLs), has simplified tailoring of state-of-the-art MOFs. The advancement in reticular chemistry blueprints facilitated the accessibility toward intricate design introduced in this dissertation, namely: merged net, cantellation, and supermolecular building rods (SBRs), reported for the first time. These new concepts have been presented with their respective chemical compositions to carefully direct synthetic MOF chemists to possible outcomes when multiple possibilities exist for the same building units. They also allow deviating from known and most default possibilities into challenging endeavors. The use of a multiple ligands system in the theme of merged net have been applied starting from: one periodic and three periodic nets, three periodic and three periodic nets to eventually unveil Zr-thw-MOFs, Zr-crh-MOFs, and M-sub-MOFs. which inspired the later discovery of the SBRs, utilizing the one-periodic pillars in the conceptual design assisted by experimental proof adopting three connecting modes, cluster-to-cluster, cluster-to-linker, and linker-to-linker. Moreover, the triply bridge organic moieties with Zr in the cantellation approach revealed the first M(IV)-sod-ZMOFs. Owing the highest reported pore size distribution for frameworks based on tetrahedral building units. In addition, the isoreticular approach (MOFs with the same topology featuring different functionality) illustrates its’ vital need for utilization. MOFs reported in this dissertation based on the isoreticulation of two MOF platforms, ftw and soc. A series of RE-ftw-MOFs based on different functional groups have been prepared and tested for the separation of hydrocarbons targeting C4 olefins, including iso-butene, and most challenging cis/trans-2-butene isomers and proved their superiority. On the other hand, a sequence of Cr-soc-MOFs based on hydrophobic ligands have been made to study the water-vapor sorption behavior in line with Cr-soc-MOF-1. Compared to the reported materials, Cr-soc-MOFs have the highest record for the spontaneous water vapor adsorption-desorption behavior in the range of RH% 30-80%.
    Citation
    Alsadun, N. S. (2022). Reticular Chemistry Strategies: Design and Applications of Metal-Organic Frameworks. KAUST Research Repository. https://doi.org/10.25781/KAUST-71D2E
    DOI
    10.25781/KAUST-71D2E
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-71D2E
    Scopus Count
    Collections
    PhD Dissertations; Physical Science and Engineering (PSE) Division; Chemical Science Program

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