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Partial Oxidation of Light Alkanes By Reductively Activated Oxygen in Eu-Catalytic System At 40 °C

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Oxidation of light alkanes, CH4, C2H6, and C3H8, could be performed at 40 °C by using the EuCl3-catalytic system (EuCl3, O2, Zn°, and CF3CO2H). In the case of CH4 oxidation, MeOH was produced from CH4 but CO2 from CF3CO2H could not be avoided. However, selective oxygenations of C2H6 (89% selectivity) and C3H8 (91%) could be performed. In the oxidation of C2H6, EtOH was primary product and the successive oxidation of EtOH gave MeCHO and CO2. Regio-selectivities ( 1 °:2°) observed in the oxidation of C3H8 suggested that an electrophilic active oxygen species was generated in the EuCl3-catalytic system. This active oxygen could not oxidize C-H bonds of MeOH (CF3CO2Me) because of a strong electron-withdrawing effect of CF3CO-group. Eu2+ species produced by the reduction with Zn0 was studied by UV-visible spectra. The spectral data proposed that O2 was reductively activated through the redox of Eu3+/Eu2+.

Affiliations: 1: Department of Chemical Engineering, Tokyo Institute of Technology, Ookayama, Meguro-ku, Tokyo 152-8552, JAPAN


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