Ni/CeO2-ZrO2 catalysts for the dry reforming of methane

被引:372
|
作者
Kambolis, A. [1 ]
Matralis, H. [1 ]
Trovarelli, A. [2 ]
Papadopoulou, Ch. [1 ]
机构
[1] Univ Patras, Dept Chem, GR-26504 Patras, Ahaia, Greece
[2] Univ Udine, Dipartimento Sci & Tecnol Chim, I-33100 Udine, Italy
关键词
Dry reforming of methane; Ceria-zirconia binary oxides; Ni catalysts; BET; XRD; UV-vis DRS; TPH; SEM; CEO2-ZRO2; SOLID-SOLUTIONS; OXYGEN STORAGE CAPACITY; CARBON-DIOXIDE; PARTIAL OXIDATION; SYNTHESIS GAS; NI CATALYST; CO2; SURFACE; CERIA; ZIRCONIA;
D O I
10.1016/j.apcata.2010.01.013
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nickel catalysts supported on binary CeO2-ZrO2 carriers (28-100% CeO2 molar content) were prepared and evaluated regarding their catalytic performance for the CO2 reforming of CH4 (Dry Reforming of Methane, DRM). The textural and structural properties of catalysts and supports were studied in their calcined, reduced and used state by N-2 adsorption-desorption, XRD, UV-vis DRS, TPR, SEM-EDS and TPH. Zirconium improves the textural properties of the CeO2-ZrO2 supports and the corresponding catalysts and enhances their textural stability under thermal reductive treatment. XRD analysis shows the formation of CexZr1-xO2 solid solution for all Ce/(Ce + Zr) ratios. Considerable alterations in the electronic environment of the cations and increased lattice defects in the binary solid solutions were detected by UV-vis DR spectroscopy. A significant increase in the reducibility of both supports and catalysts is observed in the presence of Zr. Compared to the zirconia-free sample, the Ni/CeO2-ZrO2 catalysts exhibited much higher activity for the title reaction, accredited to the increase of the surface concentration of the active sites. However, the amount of carbonaceous deposits is not straightforward related to the activity but depends on the Ce/Zr ratio. Among the zirconium containing catalysts, the zirconium-rich one exhibited the higher activity and the stronger resistance to the formation of carbonaceous deposits. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:16 / 26
页数:11
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