Structural rearrangement and catalytic properties of the Wells-Dawson (NH4)6P2Mo18O62 heteropolycompound in the 2-butanol reaction

被引:12
|
作者
Arendt, E. [1 ]
McEvoy, K. M. [1 ]
Gaigneaux, E. M. [1 ]
机构
[1] Unite Catalyse & Chim Mat Divises, B-1348 Louvain, Belgium
关键词
Wells-Dawson heteropolycompound; Keggin heteropolycompound; 2-Butanol oxygen-assisted reaction; Structure-activity relationships; CENTER DOT 10H(2)O; 12-MOLYBDOPHOSPHORIC ACID; SELECTIVE OXIDATION; ISOBUTANE; STATE; STABILITY; CHEMISTRY; BEHAVIOR; SURFACE; PHASE;
D O I
10.1016/j.apcata.2008.12.002
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
Structural changes of the ammonium phospho-molybdic Wells-Dawson salt (NH4)(6)P2Mo18O62 were examined by several solid state techniques during the oxygen-assisted catalytic reaction of 2-butanol. A significant evolution of the catalytic behavior occurs while the working catalyst is in the course of its reorganisation to a Keggin structure. Precisely, a particular species formed in situ and presenting intermediate characteristics between those of Wells-Dawson and Keggin structures exerts a beneficial effect on the selectivity to methyl-ethyl-ketone. This high selectivity towards the oxidative dehydrogenation was however found to be ephemeral and the selectivity decline was correlated to a no proper stabilization of this most active intermediate. (C) 2008 Elsevier B.V. All rights reserved.
引用
收藏
页码:115 / 124
页数:10
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