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    Functionalized Metal-Organic Frameworks for Catalytic Applications

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    Name:
    FengXieThesis(1).pdf
    Size:
    3.736Mb
    Format:
    PDF
    Description:
    Feng Xie - Final Thesis
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    Type
    Thesis
    Authors
    Xie, Feng cc
    Advisors
    Han, Yu cc
    Committee members
    Hadjichristidis, Nikos cc
    Lai, Zhiping cc
    Program
    Chemical Science
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2019-10
    Embargo End Date
    2020-11-13
    Permanent link to this record
    http://hdl.handle.net/10754/660094
    
    Metadata
    Show full item record
    Access Restrictions
    At the time of archiving, the student author of this thesis opted to temporarily restrict access to it. The full text of this thesis will become available to the public after the expiration of the embargo on 2020-11-13.
    Abstract
    The development and design of efficient catalysts are essential for catalytic energy technologies, accompanied with the fundamental understanding of structure-property relationships of these catalysts. Metal-organic frameworks (MOFs), as the new class of promising catalysts, have been intensively investigated primarily in their fundamental electrochemistry and the broad spectrum of catalytic applications due to their structural flexibility, tailorable crystalline, and multi-functionality. In this work, we combine experiments and mechanism investigation to gain a fundamental understanding of how the surface property and the structure of MOFs affect their catalytic performance. With the aim of material design for MOFs catalysts, we developed two novel superhydrophilic and aerophobic metal-organic frameworks (AlFFIVE-1-Ni MOFs and FeFFIVE-1-Ni MOFs) used as electrocatalysts for the first time during oxygen evolution reactions (OER). Under the facilitation of hydrophilicity and aerophobicity, developed FeFFIVE-1-Ni MOFs electrocatalysts deliver optimal OER performance, better than that of the state-of-art RuO2 and referred NiFe-BDC MOFs electrocatalysts. Most importantly, the practical strategy demonstrated that the hydrophilic and aerophobic structure of MOFs does indeed deliver the optimal electrocatalytic performance. With the aim of investigating the structural transformation process of metal-organic framework, we used a series of advanced characterization techniques to monitor the structure evolution and defects presence for post-heating treated UiO-66 MOFs. The structural and electronic features of UiO-66 MOFs were intensely studied in their hydroxylated, dehydroxylated, defected, and pyrolytic forms. Meanwhile, one concept about the framework situation, quasi-MOF (like a transition state, defined high activation along the structure evolution corresponding to the presence of many defects), was presented and demonstrated. Compared with pristine UiO-66 MOF, the Quasi-MOF with the presence of active defects showed enhanced catalytic activity on the Meerwein-Ponndorf-Verley reduction reaction, which offers an opportunity to understand the structure-property relationship along with the structure evolution process of UiO-66 MOFs.
    Citation
    Xie, F. (2019). Functionalized Metal-Organic Frameworks for Catalytic Applications. KAUST Research Repository. https://doi.org/10.25781/KAUST-0GB19
    DOI
    10.25781/KAUST-0GB19
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-0GB19
    Scopus Count
    Collections
    Theses; Physical Science and Engineering (PSE) Division; Chemical Science Program

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