期刊
ACS CATALYSIS
卷 11, 期 3, 页码 1065-1070出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04592
关键词
Cu-MOR; methane; methanol; oxidation; zeolite
资金
- C1 Gas Refinery Program through the National Research Foundation of Korea (NRF) - Ministry of Science and ICT [2015M3D3A1A01064899]
This Letter reports the continuous direct conversion of methane into methanol using Cu(II)-exchanged mordenite under mild conditions. The methanol production rate was influenced by factors such as the Si/Al ratio, Cu/Al ratio, presence of Bronsted acid sites, and O-2 concentration in the feed.
One-step methane-to-methanol conversion is a dream reaction for chemists. In this Letter, continuous direct conversion of methane into methanol with steam under mild conditions using Cu(II)-exchanged mordenite is reported. The methanol production rate depended on the Si/Al ratio, Cu/Al ratio, presence of Bronsted acid sites, and O-2 concentration in the feed. Cu-H-mordenite and Cu-Na-mordenite showed comparable methane conversion rates, but the former provided higher methanol selectivity. At a given Si/Al ratio, the methane conversion rate gave a volcano plot as a function of Cu/Al ratio, and methanol selectivity decreased with increasing Cu/Al ratio. These experimental data and DFT calculation implied that binuclear copper species are more active than mononuclear copper species and that copper oxide clusters are favorable for total oxidation.
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