Switchable Metal Sites in Metal–Organic Framework MFM‐300(Sc): Lewis Acid Catalysis Driven by Metal–Hemilabile Linker Bond Dynamics

Uncommon reversible guest‐induced metal‐hemilabile linker bond dynamics in MOF MFM‐300(Sc) was unraveled to switch on/switch off catalytic open metal sites. The catalytic activity of this MOF with non‐permanent open metal sites was demonstrated using a model Strecker hydrocyanation reaction as a pro...

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Bibliographic Details
Published in:Angewandte Chemie 2022-11, Vol.134 (48), p.n/a
Main Authors: Peralta, Ricardo A., Lyu, Pengbo, López‐Olvera, Alfredo, Obeso, Juan L., Leyva, Carolina, Jeong, Nak Cheon, Ibarra, Ilich A., Maurin, Guillaume
Format: Article
Language:English
Subjects:
Catalysis
Catalysts
Catalytic activity
Catalytic converters
Chemistry
Density Functional Theory
Lewis acid
Metal-Hemilabile Linker Bond Dynamics
Metal-organic frameworks
Metals
MOFs
Reaction Mechanism
Reaction mechanisms
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Summary:Uncommon reversible guest‐induced metal‐hemilabile linker bond dynamics in MOF MFM‐300(Sc) was unraveled to switch on/switch off catalytic open metal sites. The catalytic activity of this MOF with non‐permanent open metal sites was demonstrated using a model Strecker hydrocyanation reaction as a proof‐of‐concept. Conclusively, the catalytic activity was evidenced to be fully reversible, preserving the conversion performance and structure integrity of MFM‐300(Sc) over multiple cycles. These experimental findings were corroborated by quantum‐calculations that revealed a reaction mechanism driven by the Sc‐open metal sites. This discovery paves the way towards the design of new effective and easily regenerable heterogeneous MOF catalysts integrating switchable metal sites. An unconventional catalytic activity was demonstrated for the Strecker reaction using a saturated ScIII‐based MOF known as MFM‐300(Sc). This activity was possible due to metal‐hemilabile linker bond to create an intermittent free ScIII site.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202210857