The monomeric cupric ion (Cu2+) species coordinated to four nitrogen ligands (CuN4) is recognized as a possible active site for particulate methane monooxygenase (pMMO) of the methanotrophic bacteria that convert methane to methanol. Herein, inspired by the active site of pMMO, a copper-doped zeolitic imidazolate framework-7 (Cu/ZIF-7) was prepared, the mononuclear CuN4 centers of which displayed catalytic partial oxidative activity and converted methane to methanol, methyl hydroperoxide, and hydroxymethyl hydroperoxide without producing the overoxidized product of formic acid. Spectroscopy studies established the mononuclear Cu2+ center coordinates with four benzimidazole nitrogens. The catalytic activity of Cu/ZIF-7 was scrutinized considering the potential reaction mechanism at the CuN4 center, which substantially reduced the strong acidity of ZIF-7 to afford the partial oxidation of methane without forming formic acid.
|Journal||Chemical Engineering Journal|
|Publication status||Published - 2022 Dec 15|
Bibliographical noteFunding Information:
This research used resources of the Pohang Accelerator Laboratory (PAL). Experiments at PLS-II were supported in part by MSIT and POSTECH. We are grateful to K. Kim and Prof. J. Cho (Ulsan National Institute of Science and Technology) for the reaction mechanism study.
This study was supported by a grant from the Korean Research Foundation funded by the Korean Government (2021M3D3A1A01079478) and by the Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) (2013M3A6B1078882) funded by the Ministry of Science and ICT.
© 2022 Elsevier B.V.
All Science Journal Classification (ASJC) codes
- Environmental Chemistry
- Chemical Engineering(all)
- Industrial and Manufacturing Engineering