Selective methane oxidation by molecular iron catalysts in aqueous medium

Hiroto Fujisaki, Tomoya Ishizuka, Hiroaki Kotani, Yoshihito Shiota, Kazunari Yoshizawa and Takahiko Kojima ()
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Hiroto Fujisaki: University of Tsukuba
Tomoya Ishizuka: University of Tsukuba
Hiroaki Kotani: University of Tsukuba
Yoshihito Shiota: Kyushu University
Kazunari Yoshizawa: Kyushu University
Takahiko Kojima: University of Tsukuba

Nature, 2023, vol. 616, issue 7957, 476-481

Abstract: Abstract Using natural gas as chemical feedstock requires efficient oxidation of the constituent alkanes—and primarily methane1,2. The current industrial process uses steam reforming at high temperatures and pressures3,4 to generate a gas mixture that is then further converted into products such as methanol. Molecular Pt catalysts5–7 have also been used to convert methane to methanol8, but their selectivity is generally low owing to overoxidation—the initial oxidation products tend to be easier to oxidize than methane itself. Here we show that N-heterocyclic carbene-ligated FeII complexes with a hydrophobic cavity capture hydrophobic methane substrate from an aqueous solution and, after oxidation by the Fe centre, release a hydrophilic methanol product back into the solution. We find that increasing the size of the hydrophobic cavities enhances this effect, giving a turnover number of 5.0 × 102 and a methanol selectivity of 83% during a 3-h methane oxidation reaction. If the transport limitations arising from the processing of methane in an aqueous medium can be overcome, this catch-and-release strategy provides an efficient and selective approach to using naturally abundant alkane resources.

Date: 2023
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DOI: 10.1038/s41586-023-05821-2

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