响应面优化环己烯氢甲酰化反应的研究

Optimization of catalytic hydroformylation of cyclohexene by a response surface method

以五价磷酸酯为配体,水合金属氯化物为催化剂,温控PEG-4000/正庚烷为反应体系,针对环己烯氢甲酰化反应,分别对不同金属掺杂进行研究,考察了反应温度、反应压力等因素对反应的影响,并以响应面进行优化,对因素间的交互作用进行分析。以单因素实验质量比m(RhCl3•3H2O):m(RuCl3•3H2O)=18.5:1、温度q=120℃、压力p=5.0 MPa、膦配体质量m≤0.08 g为基础,构建温度、压力、配体量3因素3水平响应曲面。经优化分析,所选区间因素影响作用依次为:压力>温度>膦配体质量,结合实验的可操作性,q=122℃、p=5.3 MPa、m=0.09 g、环己烯转化率大于99%。进行3次验证,与预测模型相近。

Different metal doping effects were investigated for cyclohexene hydroformylation reaction using pentavalent phosphate as the ligand,hydrated metal chlorides as catalysts and temperature-controlled PEG-4000/n-heptane as the reaction system.The effects of reaction temperature,reaction pressure and other factors on the reaction were investigated,and the response surface method was used for optimization and analysis.Based on the single factor experiment(m(RhCl3×3H2O):m(RuCl3×3H2O)=18.5:1(mass ratio),q=120℃,p=5.0 MPa,m(P)≤0.08 g),a three-factor and three-level response surface method for temperature,pressure and phosphine ligand amount was constructed.The experimental results show that the effect of the selected factor is in an order of pressure>temperature>ligand amount.Considering the operability of the experiment under conditions ofq=122℃,p=5.3 MPa,m(P)=0.09 g,the conversion of cyclohexene is over 99%.Three repeats were verified and the result was similar to that of the model.