摘要
研究了不同含氮有机物配合CuCl对乙醇液相氧化羰化合成碳酸二乙酯反应的影响,筛选出活性高、溶解性好、腐蚀性小的多功能催化体系。推导出该催化体系的动力学方程,得到相关动力学参数。研究结果表明,CuCl/phenathroline(phen)/N methylimidazole(NMI)络合催化体系的催化活性最高,当CuCl的浓度为0 2mol/L,c(N donor)/c(CuCl)=5/2,c(phen)/c(NMI)=1/1,反应温度为120℃,反应压力为2 4MPa,CO与O2的进气比为2/1时,乙醇转化率为14 2%,碳酸二乙酯的选择性大于98%。该催化体系的动力学方程为-dpCOCO,活化能为53 36kJ/mol。对氧化羰化反应机理也进行了讨论。dt=0 246p1
The influence of different Ndonor organic ligands coordinated with CuCl on the reaction of the oxidative carbonylation of ethanol to diethyl carbonate in homogeneous catalytic system has been investigated The multifunctional catalyst system which has better performance on catalytic activity, solubility and inhibition of corrosion is found The kinetic equation and relative parameters of different complex catalyst systems of CuCl and Ndonor organic ligands are obtained after the experiment data are fitted Experimental results show that in the case of concentration of catalyst CuCl 02mol/L,CNdonor /CCuCl=5/2, Cphen/CNMI=1/1,120℃,240MPa,pCO/ pO2 =2/1, the complex catalyst system of CuCl /phen/NMI has the best catalytic activity among the CuCl /Ndonor organic ligands catalytic system The conversion of ethanol is about 142% and the selectivity to diethyl carbonate is over 98% The kinetic equation could be expressed as and active energy is about 5336kJ/mol The mechanism of oxidative carbonylation of ethanol to diethyl carbonate by this CuCl /phen/NMI catalytic system has also been discussed in datail
出处
《天然气化工—C1化学与化工》
CAS
CSCD
北大核心
2003年第4期1-6,共6页
Natural Gas Chemical Industry
基金
华中科技大学理学院基金资助项目
关键词
碳酸二乙酯
氧化羰化
均相催化
动力学方程
diethyl carbonate
oxidative carbonylation
homogeneous catalysis
kinetic equation
