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基于密度泛函理论方法,采用广义梯度近似方法结合周期平板模型,对甲醇氧化羰基化反应中CuCl(111)表面上CO和CH3O的吸附、共吸附及CH3OCO的吸附进行了系统研究,探讨了CO和CH3O反应生成CH3OCO以及CH3OCO和CH3O反应生成碳酸二甲酯(DMC)的动力学特性.计算结果表明,在CuCl(111)表面的共吸附体系中,CO和CH3O之间的相互作用力比自由态的CO和CH3O之间的作用力大;CO和CH3O反应生成CH3OCO为整个甲醇氧化羰基化反应的速控步骤,活化能为113.19 kJ/mol,计算结果与实验结果一致.
Based on the density functional theory (DFT) method, the adsorption and adsorption of CO and CH3O on the surface of CuCl (111) and the adsorption of CH3OCO on the surface of CuCl (111) were studied systematically by using the generalized gradient approximation and periodic plate model. And CH3OO react to form CH3OCO and react with CH3OCO and CH3O to produce dimethyl carbonate (DMC). The calculated results show that the interaction between CO and CH3O in the co-adsorption system of CuCl (111) The reaction between CO and CH3O to form CH3OCO is the rate-controlling step for the oxidative carbonylation of methanol. The activation energy is 113.19 kJ / mol. The calculated results agree well with the experimental results.