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甲醇氧化羰基化合成碳酸二甲酯反应机理研究进展

杜治平 黄丽明 林志坤 熊利花

化工进展2012,Vol.31Issue(10):2213-2220,8.
化工进展2012,Vol.31Issue(10):2213-2220,8.

甲醇氧化羰基化合成碳酸二甲酯反应机理研究进展

Mechanism for the synthesis of dimethyl carbonate from oxidative carbonylation of methanol

杜治平 1黄丽明 1林志坤 1熊利花1

作者信息

  • 1. 武汉工程大学绿色化工过程教育部重点实验室,湖北省新型反应器与绿色化学工艺重点实验室,湖北武汉430074
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摘要

Abstract

There are a series of problems on traditional catalysis in the synthesis of DMC from oxidative carbonylation of methanol,including the corrosion to instrument and the loss of catalyst activity for the existence of chlorine.Modified copper catalysts were obtained by loading and adding promoter or ligand and some problems were ameliorated.The modified catalysts were introduced and the mechanisms for them were studied.An active intermediate for CuCl2or CuCl loaded catalyst is Cu(OCH3)Cl or Cu2(OH)3Cl.When CuCl was mixed with ligand,the formation of methoxide species was affected by the structure,kind and amount of ligand.Free-chloride catalyst was realized for the Cu-zeolite catalyst prepared by solid-state exchange,but with low activity.When Si,Al and Ti oxide were used as zeolites,modifications for the surface of these oxides were implemented and catalytic activity was enhanced.Though the rate-determing step is the insertion of CO to the methoxide species for most of copper catalyst,differences remained in the formation of methoxide species and the production of the insertion of CO to the methoxide species.Further study of the reaction mechanism for the catalysts is still the focus in the future.

关键词

甲醇/氧化羰基化/碳酸二甲酯/反应机理

Key words

methanol/oxidative carbonylation/dimethyl carbonate/reaction mechanism

分类

化学化工

引用本文复制引用

杜治平,黄丽明,林志坤,熊利花..甲醇氧化羰基化合成碳酸二甲酯反应机理研究进展[J].化工进展,2012,31(10):2213-2220,8.

基金项目

国家自然科学基金重点项目 ()

湖北省自然科学基金重点项目 ()

化工进展

OA北大核心CSCDCSTPCD

1000-6613

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