脉冲电晕放电甲烷氯化反应研究

Study on chlorination of methane by pulsedcorona discharge

在线-筒式脉冲电晕反应器中,以四氯乙烯为氯源对甲烷氯化反应进行了实验研究.实验考察了脉冲峰值电压、载气种类和化学计量比等不同参数对甲烷氯化反应的影响,并对反应机理进行了分析.实验结果表明:反应得到的甲烷氯化物(CMS)中各种氯化产物的产量依次为一氯甲烷、四氯甲烷、三氯甲烷和二氯甲烷;提高峰值电压有利于甲烷和四氯乙烯的转化,也提高了CMS的产量;相比于氮气,以氩气为载气时甲烷氯化的转化率更高;甲烷的转化率随着化学计量比n(CH4)∶n(C2Cl4)的增大而提高.

Chlorination of methane using tetrachloroethylene （TCE） as chlorine source was studied with a wire tube pulsed corona reactor. The influences of pulse voltage, background gas and the stoichiometry of methane to TCE on methane chlorination were investigated. Furthermore, the mechanism of methane chlorination was also discussed. The results showed that methane chlorides （CMS） were produced by the reaction of methane and TCE, and the sequence of the amount of products is methyl chloride （CH3 C1）〉 dichloromethane （CH2 C12 ）〉 chloroform （CHC13）〉carbon tetrachloride （CC14）. It was found that the production of CMS increased with the increase of input peak voltage. The methane conversion is higher in Ar gas than that in N2 gas, and the methane conversion efficiency increased with the increase of mole ratio of methane to TCE.