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    Reticular Chemistry and Metal-Organic Frameworks: Design and Synthesis of Functional Materials for Clean Energy Applications

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    Dalal_Alezi_PhD_Dissertation.pdf
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    PDF
    Description:
    Dalal Alezi Dissertation
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    Type
    Dissertation
    Authors
    Alezi, Dalal cc
    Advisors
    Eddaoudi, Mohamed cc
    Committee members
    Hadjichristidis, Nikos cc
    Salama, Khaled N. cc
    Barbour, Len
    Program
    Chemical Science
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2017-06
    Embargo End Date
    2018-06-14
    Permanent link to this record
    http://hdl.handle.net/10754/625043
    
    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 became available to the public after the expiration of the embargo on 2018-06-14.
    Abstract
    Gaining control over the assembly of crystalline solid-state materials has been significantly advanced through the field of reticular chemistry and metal organic frameworks (MOFs). MOFs have emerged as a unique modular class of porous materials amenable to a rational design with targeted properties for given applications. Several design approaches have been deployed to construct targeted functional MOFs, where desired structural and geometrical attributes are incorporated in preselected building units prior to the assembly process. This dissertation illustrates the merit of the molecular building block approach (MBB) for the rational construction and discovery of stable and highly porous MOFs, and their exploration as potential gas storage medium for sustainable and clean energy applications. Specifically, emphasis was placed on gaining insights into the structure-property relationships that impact the methane (CH4) storage in MOFs and its subsequent delivery. The foreseen gained understanding is essential for the design of new adsorbent materials or adjusting existing MOF platforms to encompass the desired features that subsequently afford meeting the challenging targets for methane storage in mobile and stationary applications.In this context, we report the successful use of the MBB approach for the design and deliberate construction of a series of novel isoreticular, highly porous and stable, aluminum based MOFs with the square-octahedral (soc) underlying net topology. From this platform, Al-soc-MOF-1, with more than 6000 m2/g apparent Langmuir specific surface area, exhibits outstanding gravimetric CH4 uptake (total and working capacities). It is shown experimentally, for the first time, that the Al-soc-MOF platform can address the U.S. Department of Energy (DOE) challenging gravimetric and volumetric targets for the CH4 working capacity for on-board CH4 storage. Furthermore, Al-soc-MOF-1 exhibits the highest total gravimetric and volumetric uptake for carbon dioxide and the utmost total and deliverable uptake for oxygen at relatively high pressures among all microporous MOFs. Additionally, the research studies presented in this dissertation highlight the latest discoveries on our continuous quest for highly-connected nets. Specifically, we report the discovery of two fascinating and highly-connected minimal edge-transitive nets in MOF chemistry, namely pek and aea topologies, via a systematic exploration of rare earth metal salts in combination with relatively less symmetrical 3-connected tricarboxylate ligands. Adsorption studies revealed that pek-MOF-1 offers excellent volumetric CO2 and CH4 uptakes at high pressures.
    Citation
    Alezi, D. (2017). Reticular Chemistry and Metal-Organic Frameworks: Design and Synthesis of Functional Materials for Clean Energy Applications. KAUST Research Repository. https://doi.org/10.25781/KAUST-918HP
    DOI
    10.25781/KAUST-918HP
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-918HP
    Scopus Count
    Collections
    Dissertations; Dissertations; Physical Science and Engineering (PSE) Division; Chemical Science Program

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