Synergism in the actions of a transition metal cation and a Lewis acid in the liquid- and gas-phase catalytic conversion of alkanes over modified ZSM-5 zeolites under mild conditions

被引:7
|
作者
Shilina, M. I. [1 ]
Udalova, O. V. [2 ]
Nevskaya, S. M. [1 ]
机构
[1] Moscow MV Lomonosov State Univ, Fac Chem, Moscow 119991, Russia
[2] Russian Acad Sci, NN Semenov Chem Phys Inst, Moscow 119991, Russia
基金
俄罗斯基础研究基金会;
关键词
LOW-TEMPERATURE CONVERSION; ALUMINUM-CHLORIDE; IN-SITU; MODERATE TEMPERATURES; IR SPECTROSCOPY; SILICA-ALUMINA; FT-IR; COBALT; ISOMERIZATION; MECHANISM;
D O I
10.1134/S0023158413060116
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
Bimetallic catalysts have been prepared by successively modifying the high-silica zeolite ZSM-5 with cobalt and aluminum salts. The performance of these catalysts in the conversion of higher alkanes at medium temperatures (130-190A degrees C) depends on whether the reaction is conducted in the liquid or gas phase. In both cases, the transition metal and surface-anchored aluminum chloride act synergetically. In the liquid-phase reactions of n-heptane and n-dodecane, the activity of the bimetallic systems is more than one order of magnitude higher than the activity of the hydrogen form of the initial zeolite. New adsorption and catalytic sites resulting from the introduction of the two modifiers into the zeolite have been discovered by diffuse reflectance IR spectroscopy. In particular, the modifiers generate a new state of cobalt in which the transition metal atoms are linked with aluminum atoms through chlorine or oxygen atoms. The liquid-phase conversion of alkanes over the modified zeolites is unlikely to proceed via a carbocationic mechanism.
引用
收藏
页码:691 / 702
页数:12
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