NDLI: Selective oxidation of methane and carbon deposition over Fe$_{2}$O$_{3}$/Ce$_{1−x }$Zr$_{ x }$O$

Content Provider	Springer Nature Link
Author	Sang, Xiu Li Li, Kong Zhai Wang, Hua Wei, Yong Gang
Copyright Year	2013
Abstract	A series of Fe$_{2}$O$_{3}$/Al$_{2}$O$_{3}$, Fe$_{2}$O$_{3}$/CeO$_{2}$, Ce$_{0.7}$Zr$_{0.3}$O$_{2}$, and Fe$_{2}$O$_{3}$/Ce$_{1−x }$Zr$_{ x }$O$_{2}$ (x = 0.1–0.4) oxides was prepared and their physicochemical features were investigated by X-ray diffraction (XRD), transmission electron microscope (TEM), and H$_{2}$-temperature-programmed reduction (H$_{2}$-TPR) techniques. The gas–solid reactions between these oxides and methane for syngas generation as well as the catalytic performance for selective oxidation of carbon deposition in O$_{2}$-enriched atmosphere were investigated in detail. The results show that the samples with the presence of Fe$_{2}$O$_{3}$ show much higher activity for methane oxidation compared with the Ce$_{0.7}$Zr$_{0.3}$O$_{2}$ solid solution, while the CeO$_{2}$-contained samples represent higher CO selectively in methane oxidation than the Fe$_{2}$O$_{3}$/Al$_{2}$O$_{3}$ sample. This suggests that the iron species should be the active sites for methane activation, and the cerium oxides provide the oxygen source for the selective oxidation of the activated methane to syngas during the reaction between methane and Fe$_{2}$O$_{3}$/Ce$_{0.7}$Zr$_{0.3}$O$_{2}$. For the oxidation process of the carbon deposition, the CeO$_{2}$-containing samples show much higher CO selectivity than the Fe$_{2}$O$_{3}$/Al$_{2}$O$_{3}$ sample, which indicates that the cerium species should play a very important role in catalyzing the carbon selective oxidation to CO. The presence of the Ce–Zr–O solid solution could induce the growth direction of the carbon filament, resulting in a loose contact between the carbon filament and the catalyst. This results in abundant exposed active sites for catalyzing carbon oxidation, strongly improving the oxidation rate of the carbon deposition over this sample. In addition, the Fe$_{2}$O$_{3}$/Ce$_{0.7}$Zr$_{0.3}$O$_{2}$ also represents much higher selectivity (ca. 97 %) for the conversion of carbon to CO than the Fe$_{2}$O$_{3}$/CeO$_{2}$ sample, which can be attributed to the higher concentration of reduced cerium sites on this sample. The increase of the Zr content in the Fe$_{2}$O$_{3}$/Ce$_{1−x }$Zr$_{ x }$O$_{2}$ samples could improve the reactivity of the materials for methane oxidation, but it also reduces the selectivity for CO formation.
Starting Page	230
Ending Page	238
Page Count	9
File Format	PDF
ISSN	10010521
Journal	Rare Metals
Volume Number	33
Issue Number	2
e-ISSN	18677185
Language	English
Publisher	Nonferrous Metals Society of China
Publisher Date	2013-12-05
Publisher Place	Springer Berlin Heidelberg
Access Restriction	One Nation One Subscription (ONOS)
Subject Keyword	Methane Carbon deposition Gas–solid reaction Selective oxidation of carbon Fe$_{2}$O$_{3}$/Ce$_{1−x }$Zr$_{ x }$O$_{2}$ catalysts Metallic Materials Nanotechnology Ceramics, Glass, Composites, Natural Methods Surfaces and Interfaces, Thin Films Inorganic Chemistry Physical Chemistry
Content Type	Text
Resource Type	Article
Subject	Materials Chemistry Metals and Alloys Physical and Theoretical Chemistry Condensed Matter Physics

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