Elucidation and Evolution of the Active Component within Cu/Fe/ZSM-5 for Catalytic Methane Oxidation: From Synthesis to Catalysis
详细信息 查看全文
- 作者：Ceri Hammond ; Nikolaos Dimitratos ; Robert L. Jenkins ; Jose Antonio Lopez-Sanchez ; Simon A. Kondrat ; Mohd Hasbi ab Rahim ; Michael M. Forde ; Adam Thetford ; Stuart H. Taylor ; Henk Hagen ; Eric E. Stangland ; Joo H. Kang ; Jacob M. Moulijn ; David J. Willock ; Graham J. Hutchings
- 刊名：ACS Catalysis
- 出版年：2013
- 出版时间：April 5, 2013
- 年：2013
- 卷：3
- 期：4
- 页码：689-699
- 全文大小：397K
- 年卷期：v.3,no.4(April 5, 2013)
- ISSN：2155-5435
文摘
The development of a catalytic, one-step route for the oxidation of methane to methanol remains one of the greatest challenges within catalysis. Of particular importance is the need to develop an efficient route that proceeds under mild reaction conditions so as to avoid deeper oxidation and the economic limitations of the currently practiced syngas route. Recently, it was demonstrated that a copper- and iron-containing zeolite is an efficient catalyst for such a one-step process. The catalyst in question (Cu鈥揊e鈥揨SM-5) is capable of selectively transforming methane to methanol in an aqueous medium with hydrogen peroxide as the terminal oxidant. Nevertheless, despite its high activity and unparalleled methanol selectivity, the origin of its activity and the precise nature of its active species are not yet fully understood. Through a combination of catalytic and spectroscopic studies, we hereby demonstrate that extraframework Fe species are the active component of the catalyst for methane oxidation, although the speciation of these sites from synthesis to catalysis significantly alters the observed activity and selectivity. The analogies and differences between this system and other iron-containing zeolite-catalyzed processes, such as N2O-mediated benzene hydroxylation, are also considered.