High selective catalyst CuCl/MCM-41 for oxidative carbonylation of methanol to dimethyl carbonate

被引:64
作者
Li, Z [1 ]
Xie, KC
Slade, RCT
机构
[1] Taiyuan Univ Technol, Inst Chem Engn Coal, Taiyuan 030024, Shanxi, Peoples R China
[2] Univ Exeter, Dept Chem, Exeter EX4 4QD, Devon, England
关键词
oxidative carbonylation; solid-state ion-exchange; CuCl; MCM-41; dimethyl carbonate;
D O I
10.1016/S0926-860X(00)00546-9
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
In this study, MCM-31 material was synthesised and the mesoporous structure was confirmed by powder XRD patterns. Organic group 3-chloropropyl was anchored on the surface of MCM-41(infinity) by reaction of 3-chloropropyltrimethoxysilane with terminal silanol groups on the surface of MCM-41(infinity) material, The modified material MCM-41(infinity)-Cl still kept its mesoporous structure even after the material was calcined again at 550 degreesC for 4h and the organic groups were removed. Prepared by solid state ion-exchange under flowing nitrogen, CuCl/MCM-41 catalyst had 100% selectivity of dimethyl carbonate based on methanol and 5-10 wt.% conversion of methanol at 130 degreesC. With the decreasing mole ratio of Si/Al of MCM-41 material. e.g. increasing the aluminium content in the material, the catalytic activity increased because more Cu was loaded on the material. When the reaction temperature increased, the dimethyl carbonate selectivity decreased and three by-products: dimethyl ether, methyl formate, dimethoxymethane were formed at high temperature. Finally increasing the oxygen partial pressure in the feed gases resulted in more dimethyl carbonate formed. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:85 / 92
页数:8
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