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	Reductive activation of oxygen for partial oxidation of light alkanes
	Wang Y(王野)
	1998
关键词	METHANE MONO-OXYGENASE H-2-O-2 GAS-MIXTURE FUEL-CELL REACTIONS SATURATED-HYDROCARBONS ROOM-TEMPERATURE ACTIVE OXYGEN LIQUID FUELS O-2 EPOXIDATION SYSTEM
英文摘要	The topics in this paper are (1) the selective oxidation of methane and ethane into their oxygenates by using a gas mixture of H2 and O2, (2) the partial oxidation of light alkanes (CH4, C2H6, C3H8) with a catalytic system of EuCl3 / Zn powder / CF3CO2H, and (3) the reductive activation of oxygen and partial oxidation of alkanes (≥C3) at the cathode by applying [H2 ¦ H3PO4¦ O2] cell reactors. （1） Methane was selectively converted to methanol by a mixture of H2 and O2 at > 600K and atmospheric pressure over FePO4 catalyst, while, in the absence of H2, the conversion of methane required temperatures higher than 700K and formaldehyde was the initial product at a low methane conversion. The in situ FT-IR spectroscopy indicated the absorption band due to a peroxide species on Fe0.5Al0.5PO4, a model catalyst of FePO4, in the presence of H2 and O2. The reaction of methane with this peroxide at ≥ 473K generated methoxide and OH group, suggesting that the adsorbed peroxide could be the active oxygen species for the formation of methanol. The structure of catalytic active site and the reaction mechanism for the oxidation of methane to methanol were discussed. (2) The catalytic system made up from Eu salts or complexes, CF3CO2H and Zn powder without organic solvents caused the oxidations of methane, ethane and propane into their corresponding oxygenates at 313K. The turnover number based on EuCl3 for the formation of methanol was 4.0 (0.8% yield) in 1h at the reaction conditions; EuCl3 (30 mol), CF3CO2H (4 ml), Zn (1 g), O2 (0.4 MPa), CH4 (1.0 MPa). Other rare earth metal chlorides and transition metal chlorides did not show catalytic activities for the oxidation of methane. The unique catalysis of Eu salts was ascribed to a good matching of the redox potentials of Eu(III) / Eu(II) with that of Zn(II) / Zn(0). The reductively actived oxygen by zinc powder through the redox of Eu(III) / Eu(II) was responsible for the partial oxidations of light alkanes at room temperature. (3) Oxygen is reduced at the cathode of H2-O2 fuel cell, generating reductively activated oxygen species which enables partial oxidations of aromatics and alkanes at the cathode. Carbon fiber and carbon whisker were good host carbon materials for the cathode. Addition of VO(acac)2 and Pd black into the carbon fiber enhanced the oxidation of propane, producting acetone as the main oxygenates at room temperature. The oxidation of propane was hypothesized to be initiated by OH radical released from the cathode. Methane and ethane were also oxidized at room temperature, though the main product was CO2.
语种	英语
内容类型	期刊论文
源URL	[http://dspace.xmu.edu.cn/handle/2288/62808]
专题	化学化工－已发表论文
推荐引用方式 GB/T 7714	Wang Y. Reductive activation of oxygen for partial oxidation of light alkanes[J],1998.
APA	王野.(1998).Reductive activation of oxygen for partial oxidation of light alkanes..
MLA	王野."Reductive activation of oxygen for partial oxidation of light alkanes".(1998).

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