期刊
CHEM
卷 7, 期 6, 页码 1557-1568出版社
CELL PRESS
DOI: 10.1016/j.chempr.2021.02.026
关键词
-
资金
- National Natural Science Fund of China [22025203, 21673295]
- Municipal Natural Science Foundation of Tianjin [18JCJQJC47400]
- SINOPEC
The study reports the high yield and selectivity of methane oxidation to methanol over Cu-CHA catalyst under water-involved conditions, with temperature-programmed surface reactions and isotope labeling experiments revealing the role of water in the reaction. Spectroscopic analysis and density functional theory calculations elucidate the catalytic mechanism of Cu-CHA.
The selective oxidation of methane to methanol is a dream reaction of direct methane functionalization, which remains a key challenge in catalysis and a hot topic of controversy. Herein, we report the water-involved methane-selective catalytic oxidation by dioxygen over copper zeolites. At 573 K, a state-of-the-art methanol space-time yield of 543 mmol/mol(Cu)/h with methanol selectivity of 91% is achieved with a Cu-CHA catalyst. Temperature-programmed surface reactions with isotope labeling suggest water as the apparent oxygen and hydrogen source of hydroxyl in methanol. Spectroscopic analyses reveal the fast redox cycle of Cu2+-Cu+-Cu2+ during methane-selective oxidation, which is closely related to the high catalytic activity of Cu-CHA. Density functional theory calculations suggest that both CuOH monomer and dimer in Cu-CHA can catalyze the selective oxidation of methane to methanol with Cu-OOH as the key reaction intermediate, and meanwhile, various copper sites may undergo interconversion under reaction conditions.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据