Due to the difficulty in transportation of light alkanes from oil fields, C1-C3 byproducts are typically flared rather than transported for use in chemical industry. Thus, there is an opportunity to convert these alkane feedstocks to liquid chemicals for easier and safer transportation. One potential catalyst identified by theoretical calculations to perform these types of reactions is a class of metal-organic frameworks (MOFs) containing a trinuclear Fe3(μ3-O) node. MIL-100, a MOF containing this nodal motif, has been previously shown to be capable of performing photocatalytic oxidation of benzene to phenol using H2O2 as an oxidant. More recently, MIL-100 was also reported to be competent towards the oxidation of propane to a mixture of propylene, isopropanol, and acetone using N2O as a molecular oxidant. The related MOF PCN-250 has also been investigated for the oxidation of cyclohexane using N2O. To gain further understanding of the catalytic activity of this structural architecture, MIL-100 was investigated for its reactivity with other molecular oxidants in the solution state to form an Fe(IV)=O moiety which can react and oxidize alkanes, broadening the scope and viability of this family of MOFs. Spectroscopic characterization, including Mössbauer spectroscopy, will be examined to aid in better understanding the catalyst.

Exploring alkane oxidation at isolated Fe(II) sites in the metal-organic framework MIL-100

ACS Fall 2021

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