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Dimethyl carbonate synthesis by liquid-phase oxidative carbonylation with CuBrnLm complex catalyst

YANG Yang,LIU Xiaoqin,LIU Dinghua,YAO Huqing   

  1. College of Chemical and Chemistry Engineering,Nanjing University of Technology
  • Online:2006-10-25 Published:2006-10-25

CuBrnLm配合催化剂液相氧化羰化合成碳酸二甲酯

杨 洋,刘晓勤,刘定华,姚虎卿   

  1. 南京工业大学化学化工学院

Abstract: A new type of CuBrnLm complex catalyst for dimethyl carbonate (DMC) synthesis by oxidative carbonylation of methanol in liquid-phase was reported. The reaction properties and stability of the catalyst was studied. CuBrnLm complex catalysts were characterized with FTIR,XPS and EPR. The results showed that the introduction of complex L could promote the substantial formation of Cu(I) species for DMC synthesis. With the method of orthogonal design,the process conditions (temperature,concentration of catalyst,pressure and reaction time) were optimized. The results indicated that under the optimum conditions (temperature 100—110 ℃,pressure3.0—3.5 MPa,4—6 h,the mass concentration of catalyst (by volume of methanol) 0.15—0.20 g/mL),the conversion of methanol could reach 23% and the selectivity of DMC could exceed 95%.

摘要: 研究了CuBrnLm配合催化剂对甲醇液相氧化羰化合成碳酸二甲酯(DMC)反应的催化活性及其稳定性,并采用XPS和EPR等对催化剂进行表征。结果发现,配位剂L的添加有助于形成甲醇选择性氧化羰基合成DMC的活性物种Cu(I)。采用正交设计对工艺条件进行优化,当温度100~110 ℃、压力3.0~3.5 MPa、时间4~6 h、催化剂浓度(以甲醇的体积) 0.15~0.20 g/mL时,甲醇转化率可达到23%,DMC选择性大于95%。

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