将H2/O2非平衡等离子体现场产生的气态H2O2和丙烯与耦合反应器中钛硅沸石TS-1直接接触,实现了丙烯气相环氧化反应.结果表明,非平衡等离子体生成气态H2O2的速率由介质阻挡放电的输入功率决定,环氧丙烷的生成速率和选择性取决于钛硅沸石催化剂和反应条件.在H2和O2进料流量分别为170和8ml/min,介质阻挡放电输入功率为3.5W,环氧化反应温度为110oC,丙烯进料量为18ml/min,催化剂用量为0.8g的条件下,生成环氧丙烷产率达246.9g/(kg·h)、环氧丙烷选择性和H2O2有效利用率分别为95.4%和36.1%,反应36h内未见催化剂失活.
Gas phase epoxidation of propylene was performed by directly contacting propylene and gaseous H2O2 on the surface of TS-1 catalyst in an integrated reactor. The gaseous H2O2 was produced in situ by a H2/O2 plasma. The H2O2 formation rate can be enhanced by increasing the power density of the H2/O2 plasma reactor. The yield and selectivity for propylene oxide (PO) can be increased by optimizing the reaction conditions and using suitable TS-1 catalysts. With a power injection of 3.5 W, flow rates of H2, O2, and propylene of 170, 8, and 18 ml/min, respectively, catalyst loading of 0.8 g, and epoxidation temperature of 110 oC, the yield and selectivity for PO and the utilization rate of H2O2 were 246.9 g/(kg·h), 95.4%, and 36.1%, respectively. During the gas phase reaction, no decline of TS-1 activity was observed.