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Partial oxidation of ethane to oxygenates using Fe- and Cu-containing ZSM-5

Forde, Michael M., Armstrong, Robert, Hammond, Ceri, He, Qian, Jenkins, Robert Leyshon, Kondrat, Simon A., Dimitratos, Nikolaos, Lopez-Sanchez, Jose Antonio, Taylor, Stuart Hamilton, Willock, David James, Kiely, Christopher John and Hutchings, Graham John 2013. Partial oxidation of ethane to oxygenates using Fe- and Cu-containing ZSM-5. Journal of the American Chemical Society 135 (30) , pp. 11087-11099. 10.1021/ja403060n

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Abstract

Iron and copper containing ZSM-5 catalysts are effective for the partial oxidation of ethane with hydrogen peroxide giving combined oxygenate selectivities and productivities of up to 95.2% and 65 mol kgcat–1 h–1, respectively. High conversion of ethane (ca. 56%) to acetic acid (ca. 70% selectivity) can be observed. Detailed studies of this catalytic system reveal a complex reaction network in which the oxidation of ethane gives a range of C2 oxygenates, with sequential C–C bond cleavage generating C1 products. We demonstrate that ethene is also formed and can be subsequently oxidized. Ethanol can be directly produced from ethane, and does not originate from the decomposition of its corresponding alkylperoxy species, ethyl hydroperoxide. In contrast to our previously proposed mechanism for methane oxidation over similar zeolite catalysts, the mechanism of ethane oxidation involves carbon-based radicals, which lead to the high conversions we observe.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Cardiff Catalysis Institute (CCI)
Chemistry
Subjects: Q Science > QD Chemistry
Publisher: American Chemical Society
ISSN: 0002-7863
Funders: Dow Chemical Company
Last Modified: 04 Jun 2017 05:10
URI: http://orca.cf.ac.uk/id/eprint/49155

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