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    Design and Fabrication of Metal-Organic Framework Membranes for Gas Separations

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    ShengZhouThesis (1).pdf
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    34.82Mb
    Format:
    PDF
    Description:
    Sheng Zhou - Final Dissertation
    Embargo End Date:
    2023-04-10
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    Type
    Dissertation
    Authors
    Zhou, Sheng cc
    Advisors
    Eddaoudi, Mohamed cc
    Committee members
    Gascon, Jorge cc
    Huang, Kuo-Wei cc
    Guillaume, Maurin
    Program
    Chemical Science
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2022-03
    Embargo End Date
    2023-04-10
    Permanent link to this record
    http://hdl.handle.net/10754/676176
    
    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 2023-04-10.
    Abstract
    Industrial productions need the separation processes, but they are quite energyintensive, which occupy about half of the total energy consumption. Membranetechnology based on a non-thermal route is expected to reduce the associated energy duties by ~90%, but effective membrane materials capable of precisely isolating targeted species from complex mixtures are highly needed. Metal-organic frameworks (MOFs), possessing the tuneable pore size and geometry, are regarded as the promising platform for molecular separations and membrane design. This dissertation illustrates the rational design and the guided fabrication for various MOF membranes. Respectively, different gas separation applications were addressed by using these membranes, such as light hydrocarbon separations, carbon dioxide (CO2) captures and natural gas purifications. A versatile strategy for membrane fabrication is developed based on the electrochemical method. Following this, a family of face-centered cubic (fcu) MOF membranes were obtained, which possess different ligands and different clusters, namely rare-earth hexanuclear or zirconium hexanuclear clusters. Two MOF membranes based on fumarate (fum) linker, Zr-fum-fcu-MOF and Y-fum-fcu-MOF, showed efficient separation for the propylene/propane binary mixture, as well as the butane/isobutane equimolar mixtures, respectively. Further aperture editing applied to Zr-fum-fcu-MOF via mixed-linker approach permits the introduction of shape irregularity to the parent trefoil-shaped apertures, inducing an ideal shape-mismatch with tetrahedral CH4 molecules and blocking their transportation while affecting linear molecules slightly such as nitrogen (N2) and CO2. The resultant Zr-fum67-mesaconate (mes)33-MOF membranes exhibit great promise for natural gas purification, including efficient nitrogen rejection and simultaneous removal of CO2 and N2 from natural gas. In addition, a unique CO2-recognition membrane based on a fluorinated MOF (KAUST-7) is constructed for multipurpose CO2 capture, including CO2/H2, CO2/N2 and CO2/CH4 separation. The specific affinity to CO2 coupling with the molecular sieving capability of KAUST-7 enables the membrane to be nearly only permeable to CO2, excluding both smaller H2 molecule and larger N2 or CH4 molecules. Moreover, in order to be closer to the real applications, the defective Zr-fum-fcu- MOF nanoparticles based mixed-matrix membranes are constructed for natural gas purification under practical conditions
    Citation
    Zhou, S. (2022). Design and Fabrication of Metal-Organic Framework Membranes for Gas Separations. KAUST Research Repository. https://doi.org/10.25781/KAUST-1ND01
    DOI
    10.25781/KAUST-1ND01
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-1ND01
    Scopus Count
    Collections
    PhD Dissertations; Physical Science and Engineering (PSE) Division; Chemical Science Program

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