Cu基络合物催化甲醇液相氧化羰化反应

针对甲醇液相氧化羰基化法合成碳酸二甲酯(DMC)工艺,开发了新型Cu基络合催化剂(CuB rnLm)。对CuB rnLm催化剂的活性及其稳定性进行了研究。实验结果表明,采用该催化剂,甲醇转化率和DMC选择性较高;元素价态和物质结构分析表明,CuB rnLm催化剂循环使用5次后仍保持较好的稳定性。采用正交设计和中心响应曲面法设计实验,并使用S tatistica软件进行统计分析,寻求出反应的主要影响因素,并得到优化的工艺条件:反应温度100~110℃、反应压力3.0~3.5M Pa、反应时间4~6h、CuB rnLm催化剂质量浓度(以甲醇的体积计)0.15~0.20g/mL。在此工艺条件下,甲醇转化率可达23%以上,DMC的选择性为96%~98%。

Liquid-Phase Oxidative Carbonylation of Methanol Catalysed by Cu-Based Complex

A Cu-based complex catalyst(CuBr_nL_m)was prepared,and was used in synthesis of dimethyl carbonate(DMC)by liquid-phase oxidative carbonylation of methanol.Valence states of elements in catalysts before and after carbonylation and their structures were studied.CuBr_nL_m catalyst was stable after being used for five cycles.Reaction conditions of this system were investigated by means of orthogonal experiments and central composite design with Statistica analysis.Under optimal reaction conditions: temperature 100~110℃,pressure 3.0~3.5MPa,reaction time 4~6h and concentration of catalyst in methanol 0.15~0.20g/mL,conversion of methanol and selectivity to DMC could reach 23% and 96%~98%,respectively.