Partial Oxidation of Ethane to Oxygenates Using Fe- and Cu-Containing ZSM-5

详细信息    查看全文

• 作者：Michael M. Forde ; Robert D. Armstrong ; Ceri Hammond ; Qian He ; Robert L. Jenkins ; Simon A. Kondrat ; Nikolaos Dimitratos ; Jose Antonio Lopez-Sanchez ; Stuart H. Taylor ; David Willock ; Christopher J. Kiely ; Graham John Hutchings
• 刊名：The Journal of the American Chemical Society
• 出版年：2013
• 出版时间：July 31, 2013
• 年：2013
• 卷：135
• 期：30
• 页码：11087-11099
• 全文大小：656K
• 年卷期：v.135,no.30(July 31, 2013)
• ISSN：1520-5126

文摘

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 kg_cat^鈥? h^鈥?, 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鈥揅 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.