Gas-phase oxycarbonylation of methanol for the synthesis of dimethyl carbonate using copper-based Supported Ionic Liquid Phase (SILP) catalysts

Gas-phase oxycarbonylation of methanol for the synthesis of dimethyl carbonate using copper-based Supported Ionic Liquid Phase (SILP) catalysts
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DOI:
10.1016/j.jcat.2013.08.029
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发表时间:
2014
影响因子:
7.3
通讯作者:
Martin Schneider;M. Haumann;Marion Stricker;J. Sundermeyer;P. Wasserscheid
Martin Schneider;M. Haumann;Marion Stricker;J. Sundermeyer;P. Wasserscheid
中科院分区:
化学1区
文献类型:
--
作者:
Martin Schneider;M. Haumann;Marion Stricker;J. Sundermeyer;P. Wasserscheid

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用于甲醇的气相氧羰基化的催化剂体系通常遭受低催化剂活性和强催化剂失活。本文采用负载型离子液相(SILP)催化剂实现了甲醇的连续气相氧羰基化反应。溴化铜(I)溶解在各种离子液体中并分散在聚合物基球形活性炭(PBSAC)上作为载体材料被发现是活性催化剂。文献中报道的卤化铜催化剂的活性和稳定性差,通过离子液体的存在,大大提高了。特别地,三辛基甲基溴化铵与碱性盐添加剂的组合增加了CuBr催化剂的活性,并导致相对稳定的SILP催化剂操作,在50小时的运行时间内达到600的总转换数。
Catalyst systems for the gas-phase oxycarbonylation of methanol often suffer from low catalyst activities and strong catalyst deactivation. In this work, the continuous gas-phase oxycarbonylation of methanol was realized by using Supported Ionic Liquid-Phase (SILP) catalysts. Copper(I) bromide dissolved in various ionic liquids and dispersed on Polymer-Based Spherical Activated Carbon (PBSAC) as supporting material was found to be an active catalyst. The poor activity and stability of copper halide catalysts reported in literature was substantially increased by the presence of ionic liquids. In particular, trioctylmethylammonium bromide in combination with a basic salt additive increased the activity of the CuBr catalyst and led to comparatively stable SILP catalyst operation reaching a total turnover number of 600 over 50 h time-on-stream.