Cu-Zn-Al-Zr浆状催化剂二甲醚合成宏观动力学  

Global kinetics of direct synthesis of dimethyl ether from syngas in slurry reactor over Cu-Zn-Al-Zr catalyst

作　　者：陈振[1,2] 张海涛[1] 应卫勇[1] 房鼎业[1] 

机构地区：[1]华东理工大学大型工业反应器工程教育部工程研究中心化学工程联合国家重点实验室,上海200237 [2]山东轻工业学院化学与制药工程学院,山东济南250353

出　　处：《天然气化工—C1化学与化工》2011年第6期1-7,共7页Natural Gas Chemical Industry

基　　金：国家973计划(No.2005CB221205);国家科技支撑计划课题(No.2006BAE02B02)

摘　　要：在压力3MPa～7MPa,温度220℃～260℃,空速0.4 L.g-1.h-1～1.2 L.g-1.h-1,气体摩尔分率yH20.75～0.65,yCO 0.14～0.20,yCO2 0.04～0.08,搅拌转速1000 r.min-1的反应条件下,于500mL高压搅拌釜中进行了合成气在Cu-Zn-Al-Zr浆状催化剂上一步法合成二甲醚工艺过程的宏观动力学研究。基于CO加氢合成甲醇、CO2加氢合成甲醇及甲醇脱水为二甲醚三个独立反应,建立了Langmuir-Hinshelwood型宏观动力学模型。采用通用遗传算法和Levenberg-Marquardt优化算法相结合的方法对实验数据进行拟合、参数寻优,获得模型参数估值,经统计检验和残差分析证实了模型的可靠性。The global kinetics of the slurry synthesis of dimethyl ether from syngas in a stirred autoclave over Cu-Zn-Al-Zr catalyst was studied at pressure of 3-TMPa, temperature of 220-260℃, WHSV of 0.4-1.2 L.g-1.h-1 and mole fractions of H2, CO and C02 in feed gas of 0.75-0.65, 0.14-0.20 and 0.04-0.08, respectively. Three reactions, CO hydrogenation to methanol, C02 hydrogenation to methanol and methanol dehydration to dimethyl ether, were chosen as the independent reactions and based on that a Langmuir-Hinshelwood type global kinetic model was built. The model parameters were estimated by fitting experimental data and parameter optimization based on general Genetic Algorithm and Levenberg- Marquardt methods, and the reliability of model was verified by statistical test and residual error analysis.

关 键 词：二甲醚 合成气 浆状催化剂 宏观动力学 遗传算法 

分 类 号：TQ032.41[化学工程]