Catalytic performance for propane selective oxidation and surface properties of 12-molybdophosphoric acid treated with pyridine

被引:66
作者
Li, W
Oshihara, K
Ueda, W
机构
[1] Sci Univ Tokyo, Dept Mat Sci & Engn, Yamaguchi 7560884, Japan
[2] Tokyo Inst Technol, Dept Environm Chem & Engn, Midori Ku, Yokohama, Kanagawa 2260087, Japan
关键词
heteropolymolybdophosphate catalyst; alkane selective oxidation; reduced state; surface acid property; oxidation mechanism;
D O I
10.1016/S0926-860X(99)00030-7
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
When molybdophosphoric acid, H3PMo12O40, was treated with pyridine and heated in N-2 how at 420 degrees C as an optimized temperature, a black solid catalyst was formed with a structure of orthorhombic phase and in a reduced state. This reduced H3PMo12O40(PY) catalyst showed a high potentiality in the propane and isobutane oxidation with molecular oxygen to acrylic acid and methacrylic acid above 300 degrees C. It was proved that the higher the reduction degree of the catalyst is, the higher the oxidation activity and selectivity to partial oxidation products are. The FT-IR study revealed that, in the lattice of the heat-treated H3PMo12O40(PY) catalyst, pyridinium ion remained to assume the highly resistant orthorhombic secondary structure against reoxidation, and on the surface, Lewis acid sites were generated with the formation of the primary oxygen-deficient Keggin structure. A possible reaction mechanism was proposed for alkane oxidation, where protons and electrons in the reduced H3PMo12O40(PY) catalyst cooperate to activate molecular oxygen. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:357 / 363
页数:7
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