Multifunctionality of Crystalline MoV(TeNb) M1 Oxide Catalysts in Selective Oxidation of Propane and Benzyl Alcohol

被引:46
作者
Amakawa, Kazuhiko [1 ]
Kolen'ko, Yury V. [1 ]
Villa, Alberto [2 ]
Schuster, Manfred E. [1 ]
Csepei, Lenard-Istvan [1 ]
Weinberg, Gisela [1 ]
Wrabetz, Sabine [1 ]
d'Alnoncourt, Raoul Naumann [1 ]
Girgsdies, Frank [1 ]
Prati, Laura [2 ]
Schloegl, Robert [1 ]
Trunschke, Annette [1 ]
机构
[1] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany
[2] Univ Milan, Dept Inorgan Chem, I-20133 Milan, Italy
关键词
propane; benzyl alcohol; selective oxidation; acrylic acid; M1; mixed oxide; MoVTeNbO; multifunctionality; MOVTENB OXIDE; ACRYLIC-ACID; SURFACE-CHEMISTRY; REACTION PATHWAYS; ACTIVE-CENTERS; SITES PRESENT; MIXED OXIDES; PHASE; TE; NB;
D O I
10.1021/cs400010q
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
Propane oxidation at 653-673 K and benzyl alcohol oxidation at 393 K over phase-pure MOV(TeNb) M1 oxide catalysts were studied to gain insight into the multiple catalytic functions of the surface of the M1 structure. Electron microscopy and X-ray diffraction confirmed the phase purity of the M1 catalysts. Propane oxidation yields acrylic acid via propene as intermediate, while benzyl alcohol oxidation gives benzaldehyde, benzoic acid, benzyl benzoate, and toluene. The consumption rates of benzyl alcohol and propane level in the same range despite huge difference in reaction temperature, suggesting high activity of M1 for alcohol oxidation. Metal-oxygen sites on the M1 surface are responsible for the conversion of the two reactants. However, different types of active sites and reaction mechanisms may be involved. Omitting Te and Nb from the M1 framework eliminates acrylic acid selectivity in propane oxidation, while the product distribution in benzyl alcohol oxidation remains unchanged. The results suggest that the surface of M1 possesses several types of active sites that likely perform a complex interplay under the harsh propane oxidation condition. Possible reaction pathways and mechanisms are discussed.
引用
收藏
页码:1103 / 1113
页数:11
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