工艺条件对含氟氯化氢催化氧化制氯气的影响

Influence of process conditions on catalytic oxidation of fluorinated hydrogen chloride to chlorine gas

采用等体积浸渍法制备了耐氟铜基催化剂,在99.9%HCl+0.1%HF混合气氛下制氯气,通过正交实验考察了反应温度、HCl和O_(2)体积比、质量空速对HCl单程转化率的影响。结果表明,在反应温度为390℃、HCl和O_(2)体积比为2∶1、质量空速为1 h^(-1)的最佳反应条件下,氯化氢单程转化率可达92.5%;为进一步验证催化剂稳定性,运行1500 h后HCl单程转化率稳定在91%~93%之间。通过ICP分析,催化剂中活性组分Cu元素流失率为1.175×10^(-5)g/h,初步估算稳定运行10000 h后,Cu流失仅为催化剂Cu元素添加量的1.68%,说明该催化剂具有较好的活性、稳定性和耐氟能力。

The effects of reaction temperature,volume ratio of HCl to O_(2)and mass space velocity on the conversion rate of HCl were investigated by orthogonal experiment in a mixture atmosphere of 99.9%HCl+0.1%HF.The results show that under the optimum reaction conditions of 390℃,2∶1 volume ratio of HCl to O_(2)and 1 h^(-1)mass space velocity,the conversion rate of hydrogen chloride can reach 92.5%.To further verify the stability of the catalyst,the one-way conversion rate of hydrogen chloride remained stable between 91%and 93%after running for 1500 hours.Through ICP analysis,the loss rate of the active component Cu element in the catalyst is 1.175×10^(-5)g/h,it is preliminarily estimated that after stable operation for 10000 hours,the loss of Cu is only 1.68%of the amount of Cu element added to the catalyst,indicating that the catalyst has good activity,stability,and fluorine resistance.