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以电石乙炔法制备氯乙烯的非汞催化反应体系为研究对象,用量子化学密度泛函理论(DFT)研究了以Cu基催化剂为代表的非汞催化剂的反应机理.模拟了以石墨烯为载体的乙炔氢氯化反应在Cu基催化剂作用下的两条反应路径及其过渡态.将该反应机理应用到不同金属氯化物催化剂中,通过计算相应的活化自由能和反应速率常数讨论了不同金属氯化物的活性顺序,与实验结果相比较印证了反应机理的合理性.讨论了Cu基催化剂的失活原因以及在载体中掺杂氮原子或磷原子对反应活性的影响.为非贵金属无汞催化剂的研究提供了一定的理论指导.
The non-mercury catalytic reaction system of vinyl chloride prepared by calcium carbide acetylene method was studied, and the reaction mechanism of non-mercury catalyst represented by Cu-based catalyst was studied by using quantum chemical density functional theory (DFT) Acetylene hydrochloride reaction under Cu-based catalyst reaction path and its transition state.This reaction mechanism is applied to different metal chloride catalysts, by calculating the corresponding activation energy and reaction rate constant discussed the different metals The order of the activity of chloride was confirmed compared with the experimental results.The rationality of the reaction mechanism was confirmed.The reason of inactivation of Cu-based catalyst and the effect of nitrogen atom or phosphorus atom on the reactivity of Cu-based catalyst were discussed. The study of the catalyst provides some theoretical guidance.