助剂对微波辐射制备浆态床合成甲醇铜基催化剂性能影响

The effect of assistant on the properties of copper-based catalyst prepared by microwave radiation in methanol synthesis in slurry reactor

采用并流共沉淀法,在微波辐射老化的条件下,制备了CuO/ZnO/Al2O3/X(X=ZrO2,Fe2O3,MnO2)四元铜基合成甲醇催化剂,考察了第四组分元素对催化剂前驱体物相组成及浆态床合成甲醇性能的影响。通过XRD,TG,EDS等对催化剂及其前驱体的微观结构进行了表征。结果发现,助剂Zr、Fe、Mn的加入均不同程度的促进了Cu,Zn组分间的相互作用,有利于活性物相绿铜锌矿及锌孔雀石的生成。与CuO/ZnO/Al2O3三元催化剂相比,助剂ZrO2、Fe2O3、MnO2的加入均提高了催化剂合成甲醇的活性。其中ZrO2对铜基催化剂活性影响较大,CO转化率从43.51%提高到了59.18%,提高了36%;甲醇时空收率从256.9 mg/(gcat·h)提高到了372.8 mg/(gcat·h),提高了45%。

CuO /ZnO /Al2O3/ X（ X = ZrO2,Fe2O3,MnO2） Quaternary copper-based methanol synthesis catalyst were made by co-precipitation and aging under microwave irradiation conditions. The effects of the fourth component elements on the catalyst precursor phase and methanol synthesis performance in slurry bed reactor were investigated. Microscopic structure and precursor of the catalyst were characterized by XRD,TG,EDS,etc. Result showed that additives of Zr,Fe,Mn promotes different degrees on interactions between Cu,Zn components,conducive to generation active phase aurichalcite and rosasite. Compared with the CuO / ZnO / Al2O3catalyst,add ZrO2,Fe2O3,MnO2increased the activity of methanol synthesis. Among them,ZrO2has a greater impact on the copper-based catalyst activity,CO conversion rate increased from 43. 51% to 59. 18%,space-time yield of methanol increased from 256. 9 mg /（ gcat·h） to 372. 8 mg /（ gcat·h）.