Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 9, Issue 24, Pages 6946-6956Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cy01640f
Keywords
-
Categories
Funding
- National Natural Science Foundation of China [21576119, 21878127, 21706098, 21606108, 21802054]
- Natural Science Foundation of Jiangsu Province [BK20180587]
- Fundamental Research Funds for the Central Universities [JUSRP11813, JUSRP11709, JUSRP51720B]
Ask authors/readers for more resources
Controllable methane oxidation directly into value-added products under mild conditions remains a challenge. Herein, an active Fe/MOR catalyst was synthesized via simple solid-state ion exchange, and its activity in the selective oxidation of methane with H2O2 in the aqueous phase was intensively investigated. The octahedral dimeric Fe3+ species [Fe-2(mu-O)(2)] in the extra framework was confirmed as the initial active site by X-ray photoelectron spectroscopy, X-ray absorption near-edge structure and extended X-ray absorption fine structure, UV-vis diffuse-reflectance spectroscopy, and high-angle annular dark-field scanning transmission electron microscopy in combination with DFT calculations. The DFT calculations indicated that methanol formation via methyl peroxide (CH3OOH*) on [Fe-2(mu-OH)(2)O-2] is the most favorable pathway compared to the direct formation of methanol via CH3O*. The formed CH3OH is easily further oxidized by hydroxyl radicals (OH) resulting in non-selective methane oxidation. In contrast, the Fe/MOR catalyst could lead to a high methanol selectivity of 71.3% in the presence of homogeneous Cu2+ precursor, which efficiently suppressed the over-oxidation of methanol, and a high formic acid selectivity up to 81-82% at a slightly higher reaction temperature by mildly shifting the oxidation of methanol and formaldehyde to the target product.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available