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Methane activation by the lanthanide oxides

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j100314a032· OSTI ID:5277699

The catalytic production of gas-phase methyl radicals from methane over the lanthanide oxides was measured by using a matrix isolation electron spin resonance (MIESR) technique. The results show that metal centers with multiple stable oxidation states are not a requirement for activity. The oxide with the greatest activity per gram was hydrothermally treated La/sub 2/O/sub 3/, which was ca. 5 times more active than the next highest oxide. Hydrothermally treated La/sub 2/O/sub 3/ and Sm/sub 2/O/sub 3/ have the largest activities per square meter. Results obtained in a conventional flow reactor for selected oxides indicate that the CH/sub 4/ conversions per square meter are in the order Nd/sub 2/O/sub 3/ > La/sub 2/O/sub 3/ > Sm/sub 2/O/sub 3/ > Dy/sub 2/O/sub 3/ > CeO/sub 2/. Oxidative coupling of CH/sub 4/ results in the C/sub 2/H/sub 6/ and C/sub 2/H/sub 4/ (C/sub 2/ compounds), and the combined C/sub 2/ yields follow the same order with Dy/sub 2/O/sub 3/ >> CeO/sub 2/. The MIESR and flow reactor results are in qualitative agreement, with the exception of Nd/sub 2/O/sub 3/.

Research Organization:
Texas A and M Univ., College Station (USA)
OSTI ID:
5277699
Journal Information:
J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 92:3; ISSN JPCHA
Country of Publication:
United States
Language:
English