期刊
ACS CATALYSIS
卷 3, 期 4, 页码 689-699出版社
AMER CHEMICAL SOC
DOI: 10.1021/cs3007999
关键词
methane oxidation; zeolite catalysis; green chemistry; selective oxidation
资金
- Dow Chemical Company
- EPSRC [EP/F067496]
- E.I. DuPont de Nemours Co.
- Northwestern University
- U.S. DOE [DE-AC02-06CH11357]
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-Fe-ZSM-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.
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