煤燃烧过程氯化汞系列化合物生成机理与反应动力学的理论研究

A Study on the Reaction Mechanism and Kinetics of Mercury Chloride Series in Coal Combustion

采用量子化学MP2方法对煤燃烧过程中的氯化汞系列化合物生成反应机理和反应动力学进行了探讨 .通过计算确定了 7条生成氯化汞系列化合物反应通道 ,优化了反应物、产物、中间体和过渡态的构型 ,在QCISD(T)水平上计算了它们的能量 .同时 ,用经典过渡态理论计算了 7条反应通道的速率常数 ,并与已有的实验数据进行比较 ,发现计算所得的反应速率常数与实验数据吻合较好 .

Ab initio MP2 method was performed to study the reaction mechanism and kinetics of mercury chloride series during the process of coal combustion. Seven channels were detected by calculations, the geometric configurations of reactants, products, intermediates and transition states were optimized and their energies were calculated at QCISD(T)/SDD level. Besides, we used the classic transition state theory to calculate the rate constants of the seven channels. Compared with the experimental values, the results show that the rate constants are in good agreement with experimental data.