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)
Year published
2021
Metadata
Show full item recordAbstract
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 ...
View more >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
View less >
View more >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
View less >
Journal Title
Angewandte Chemie International Edition
Volume
60
Issue
11
Subject
Chemical sciences
Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
C1 oxygenates