采用旋转填充床液液相共沉淀法制备了钙钛矿复合氧化物La0.5Pb0.5MnO3,以其作为载体制备了0.5%Pd(质量分数)/La0.5Pb0.5MnO3催化剂合成碳酸二苯酯。为了提高催化剂的活性,采用聚乙二醇(PEG)为分散剂对载体表面改性,通过XRD,SEM,BET手段对其物性进行表征,并对催化剂进行了活性评价。结果表明:PEG良好的空间位阻效应可以增加载体的分散度和比表面积,提高催化剂的活性。PEG10 000浓度为0.001 5 mol/L时效果最佳,载体比表面积达53.73 m^2/g。反应温度65℃,总压5 MPa,p(CO)∶p(O2)=94∶6,反应3 h,DPC收率达13.30%。反应9 h,该条件下DPC收率可达21.90%。
The La0.5Pb0.5MnO3 perovskite composite oxides were prepared as the carrier of the 0.5%Pd(mass fraction)/La0.5Pb0.5MnO3 catalyst for the synthesis of diphenyl carbonate(DPC) by co-precipitation method in rotating packed bed.In order to enhance the catalyst activity,polyethylene glycol(PEG) was used as dispersing agent for modifying the carrier surface.The property of PEG was characterized by XRD,SEM,BET,and the activity of catalyst was evaluated.The results show that the steric effect of PEG can enhance the dispersion and specific surface area of supports,which results in the increment of the yield of DPC.After the addition of PEG in the optimal conditions,i.e.relative molecular mass 10 000,concentration 0.001 5 mol/L,the specific surface area of support can achieve 53.73 m2/g.With the reaction temperature 65 ℃,total pressure 5 MPa,p(CO) ∶ p(O2)=94 ∶6,reaction time 3 h,the yield of DPC can reach 13.30%.Reaction time 9 h,the yield of DPC can reach 21.90%.