ArticleNature chemistry2014
Oxidation of ethane to ethanol by N2O in a metal-organic framework with coordinatively unsaturated iron(II) sites.
Article in Nature chemistry, 2014. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 55 papers.
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55 citing papers in PubMed, 469 citations in OpenAlex.
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- Light-driven C-H activation mediated by 2D transition metal dichalcogenides.Research square · 2024Article
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- Mechanism of Benzene Hydroxylation on Tri-Iron Oxo-Centered Cluster-Based Metal-Organic Frameworks.The journal of physical chemistry. C, Nanomaterials and interfaces · 2023Article
- Full Spectroscopic Characterization of the Molecular Oxygen-Based Methane to Methanol Conversion over Open Fe(II) Sites in a Metal-Organic Framework.Journal of the American Chemical Society · 2023Article
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- Ionothermal Synthesis of Metal-Organic Frameworks Using Low-Melting Metal Salt Precursors.Angewandte Chemie (International ed. in English) · 2023Article
- New Strategies for Direct Methane-to-Methanol Conversion from Active Learning Exploration of 16 Million Catalysts.JACS Au · 2022Article
- MOFSimplify, machine learning models with extracted stability data of three thousand metal-organic frameworks.Scientific data · 2022Article
- A Reactive, Photogenerated High-Spin (Journal of the American Chemical Society · 2021Article
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- Catalytic Oxygenation of Hydrocarbons by Mono-μ-oxo Dicopper(II) Species Resulting from O-O Cleavage of Tetranuclear CuAngewandte Chemie (International ed. in English) · 2021Article
- Evaluating the Robustness of Metal-Organic Frameworks for Synthetic Chemistry.ACS applied materials & interfaces · 2021Article
- Shifting the scaling relations of single-atom catalysts for facile methane activation by tuning the coordination number.Chemical science · 2021Article
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Authors and funding
18 authors at 6 institutions in 2 countries.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Enzymatic haem and non-haem high-valent iron-oxo species are known to activate strong C-H bonds, yet duplicating this reactivity in a synthetic system remains a formidable challenge. Although instability of the terminal iron-oxo moiety is perhaps the foremost obstacle, steric and electronic factors also limit the activity of previously reported mononuclear iron(IV)-oxo compounds. In particular, although nature's non-haem iron(IV)-oxo compounds possess high-spin S = 2 ground states, this electronic configuration has proved difficult to achieve in a molecular species. These challenges may be mitigated within metal-organic frameworks that feature site-isolated iron centres in a constrained, weak-field ligand environment. Here, we show that the metal-organic framework Fe2(dobdc) (dobdc(4-) = 2,5-dioxido-1,4-benzenedicarboxylate) and its magnesium-diluted analogue, Fe0.1Mg1.9(dobdc), are able to activate the C-H bonds of ethane and convert it into ethanol and acetaldehyde using nitrous oxide as the terminal oxidant. Electronic structure calculations indicate that the active oxidant is likely to be a high-spin S = 2 iron(IV)-oxo species.
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