期刊
CHEMICAL ENGINEERING JOURNAL
卷 450, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.138472
关键词
Methane; Methanol; Catalysis; Methane monooxygenase; Zeolitic imidazolate framework
资金
- Korean Research Foundation - Korean Government [2021M3D3A1A01079478]
- Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) - Ministry of Science and ICT [2013M3A6B1078882]
- Ministry of Science and ICT
- National Research Foundation of Korea [2021M3D3A1A01079478] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Inspired by the active site of particulate methane monooxygenase (pMMO), a copper-doped zeolitic imidazolate framework-7 (Cu/ZIF-7) was synthesized and showed catalytic activity in converting methane to various products without overoxidation.
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 hydroper-oxide without producing the overoxidized product of formic acid. Spectroscopy studies established the mono-nuclear Cu(2+ )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.
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