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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2010,Vol.26>> Issue(07)>> 1879-1886     doi: 10.3866/PKU.WHXB20100732         中文摘要
CATALYSIS AND SURFACE STRUCTURE
Effects of Zirconia Crystallite Phases on the Structures of MoOx/ZrO2 Catalysts and Their Properties in the Selective Oxidation of Methanol
ZHANG Sheng-Hong, ZHANG Hong-Peng, LI Wei-Zhen, ZHANG Wei, HUANG Hua, LIU Hai-Chao
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
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MoOx supported on pure monoclinic zirconia (m-ZrO2) and tetragonal 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.



Keywords: Selective oxidation   Monoclinic zirconia   Tetragonal zirconia   Crystallite phase effect   Molybdena   Methanol  
Received: 2010-04-09 Accepted: 2010-05-17 Publication Date (Web): 2010-06-03
Corresponding Authors: LIU Hai-Chao Email: hcliu@pku.edu.cn


Cite this article: 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 MoOx/ZrO2 Catalysts and Their Properties in the Selective Oxidation of Methanol[J]. Acta Phys. -Chim. Sin., 2010,26 (07): 1879-1886.    doi: 10.3866/PKU.WHXB20100732
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88. ZHAO Wen-Xia; HU Man-Cheng; LI Shu-Ni; JIANG Yu-Cheng; ZHANG Xiao-Lei; HU Lei; CHEN Huai-Jun.The Solubility of Ternary SystemRbBr/CsBr-CH3OH/C2H5OH-H2O at Different Temperatures[J]. Acta Phys. -Chim. Sin., 2007,23(05): 695-700
89. WU Wei; CAO Jie-Ming; CHEN Yu; LU Tian-Hong.Preparation of High-alloying Pt-Ru/CMK-3 Catalysts in THF-H2O-EtOH Ternary Solution System[J]. Acta Phys. -Chim. Sin., 2007,23(04): 559-564
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93. HUANG Mian-Yan;CHEN Hua-Yan;GUO Jian-Zhao;WANG Zhi-Tao;XU Li;WANG Yu-Xin.Methanol Resistant Poly(Ether Sulfone)/Sulfonated Poly(Ether Ether Ketone) Blend Proton Exchange Membrane for DMFC[J]. Acta Phys. -Chim. Sin., 2007,23(01): 44-49
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