【摘要】 研究了CuCl/Schiff碱催化体系在乙醇液相氧化羰化合成碳酸二乙酯 (DEC)中的催化活性。讨论了不同Schiff碱、反应温度、反应时间、体系水含量等因素对合成碳酸二乙酯的影响 ,并考察了催化剂的寿命。实验结果表明 ,CuCl/1 ,1 0 邻菲啉 (phen) /N 甲基咪唑 (NMI)催化体系具有良好的催化效果。在 1 2 0℃ ,2 4MPa,CuCl浓度为 0 2 0mol/L ,n(NMI)∶n(CuCl) =1 2 5∶1 ,n(phen)∶n(NMI) =1∶1的条件下 ,反应 3h后 ,乙醇的转化率为 1 3 6% ,DEC质量分数为 1 8 2 % ,选择性大于 99 0 % ,乙醇转化率较CuCl催化体系提高了 3倍。活性测定结果还表明 ,催化剂在连续使用 4次后 ,活性基本保持不变更多还原

【Abstract】 Catalytic synthesis of diethyl carbonate(DEC) by oxidative carbonylation of ethanol in homogeneous CuCl/Schiff-base system has been studied as functions of N-donor ligand, reaction time, temperature, water content and ratio of N-methyl imidazole(NMI) to 1,10-phenanthroline(phen). Catalytic system with CuCl/phen/NMI was found to have a favorable activity in the oxidative carbonylation. Under conditions of 120 ℃, 2.4 MPa(CO+O 2), concentration of CuCl 0.20 mol/L, n(NMI)∶n(CuCl)=1.25∶1, n(NMI)∶ n(phen)=1∶1, in 3 hours, conversion of ethanol reached 13.6%, 3 times as much as that of plain CuCl system, with selectivity of DEC being over 99.0%. The catalytic activity of the catalytic system studied could be used repeatedly 4 times without significant loss of activity in the oxidative carbonylation.更多还原