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  • Fe-O Clusters Anchored on Nodes of Metal-Organic Frameworks for Direct Methane Oxidation

    Author(s)
    Zhao, Wenshi
    Shi, Yanan
    Jiang, Yuheng
    Zhang, Xiaofei
    Long, Chang
    An, Pengfei
    Zhu, Yanfei
    Shao, Shengxian
    Yan, Zhuang
    Li, Guodong
    Tang, Zhiyong
    Griffith University Author(s)
    Tang, Zhiyong
    Year published
    2021
    Metadata
    Show full item record
    Abstract
    Direct methane oxidation into value-added organic oxygenates with high productivity under mild condition remains a great challenge. We show Fe-O clusters on nodes of metal–organic frameworks (MOFs) with tunable electronic state for direct methane oxidation into C1 organic oxygenates at 50 °C. The Fe-O clusters are grafted onto inorganic Zr nodes of UiO-66, while the organic terephthalic acid (H BDC) ligands of UiO-66 are partially substituted with monocarboxylic modulators of acetic acid (AA) or trifluoroacetic acid (TFA). Experiments and theoretical calculation disclose that the TFA group coordinated with Zr node of UiO-66 ...
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    Direct methane oxidation into value-added organic oxygenates with high productivity under mild condition remains a great challenge. We show Fe-O clusters on nodes of metal–organic frameworks (MOFs) with tunable electronic state for direct methane oxidation into C1 organic oxygenates at 50 °C. The Fe-O clusters are grafted onto inorganic Zr nodes of UiO-66, while the organic terephthalic acid (H BDC) ligands of UiO-66 are partially substituted with monocarboxylic modulators of acetic acid (AA) or trifluoroacetic acid (TFA). Experiments and theoretical calculation disclose that the TFA group coordinated with Zr node of UiO-66 enhances the oxidation state of adjacent Fe-O cluster due to its electron-withdrawing ability, promotes the activation of C−H bond of methane, and increases its selective conversion, thus leading to the extraordinarily high C1 oxygenate yield of 4799 μmol g h with 97.9 % selectivity, circa 8 times higher than those modulated with AA. 6 2 6 cat −1 −1
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    Journal Title
    Angewandte Chemie International Edition
    Volume
    60
    Issue
    11
    DOI
    https://doi.org/10.1002/anie.202013807
    Subject
    Chemical sciences
    Science & Technology
    Physical Sciences
    Chemistry, Multidisciplinary
    Chemistry
    C1 oxygenates
    Publication URI
    http://hdl.handle.net/10072/404587
    Collection
    • Journal articles

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