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Citation: ZHANG Sheng-Hong, ZHANG Hong-Peng, LI Wei-Zhen, ZHANG Wei, HUANG Hua, LIU Hai-Chao. Effects of Zirconia Crystallite Phases on the Structures of MoO_x/ZrO₂ Catalysts and Their Properties in the Selective Oxidation of Methanol[J]. Acta Physico-Chimica Sinica, ;2010, 26(07): 1879-1886. doi: 10.3866/PKU.WHXB20100732 shu

Effects of Zirconia Crystallite Phases on the Structures of MoO_x/ZrO₂ Catalysts and Their Properties in the Selective Oxidation of Methanol

1.
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Stable and Unstable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China

Received Date: 9 April 2010
Available Online: 3 June 2010

MoOx supported on pure monoclinic zirconia (m-ZrO2) and tetra nal zirconia (t-ZrO2) with different Mo surface densities were prepared and their structures were characterized by X-ray diffraction, Raman spectroscopy and temperature-programmed reduction in H2. At Mo surface densities lower than the theoretical monolayer coverage (~5 nm-2), isolated MoOx and two-dimensional polymolybdates were dominant on the m-ZrO2 surface while MoO3 crystallites were still present on the t-ZrO2 surface indicating a favorable dispersion of MoOx on m-ZrO2. As the Mo surface densities increased to more than monolayer coverage, MoOx tended to form ZrMo2O8 on the ZrO2 surface by a solid reaction at 600 ℃, which was more prevalent on m-ZrO2 than on t-ZrO2. The acidity of the MoOx/ZrO2 catalysts increased with an increase in the Mo surface density indicating that ZrMo2O8 is more acidic than dispersed MoOx. Catalysts prepared using t-ZrO2 resulted in more acidic MoOx/ZrO2 and consequently higher selectivity for dimethyl ether during the selective oxidation of methanol was achieved. The MoOx structures were more reducible on the m-ZrO2 surface leading to improved activity for the oxidation of methanol to formaldehyde, dimethoxymethane and methylformate. An understanding of the effect of ZrO2 crystallite phase on the structures of the MoOx species and their catalytic properties for the selective oxidation of methanol provides useful information for the study of other metal oxides such as VOx, and the design of catalysts that are bifunctional in terms of acidity and redox activity.
- Selective oxidation,
- Monoclinic zirconia,
- Tetra nal zirconia,
- Crystallite phase effect,
- Molybdena,
- Methanol
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

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Effects of Zirconia Crystallite Phases on the Structures of MoOx/ZrO2 Catalysts and Their Properties in the Selective Oxidation of Methanol

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通讯作者: 陈斌, bchen63@163.com

Effects of Zirconia Crystallite Phases on the Structures of MoO_x/ZrO₂ Catalysts and Their Properties in the Selective Oxidation of Methanol