采用浸渍法制备了一系列不同ZrO₂掺杂量的Pd/ZrO₂-活性炭(AC)复合催化剂,并用于正丁醛与环己酮一锅法制备2-丁基环己酮。利用XRD、N₂物理吸附、TG-DTG、SEM、TEM对Pd/ZrO₂-AC复合催化剂的物理及化学性质进行表征,考查了ZrO₂掺杂量、反应温度、Pd负载量、载体制备方法对反应性能的影响。结果表明,在140℃条件下,浸渍法制备的0.8Pd/50ZrO₂-AC可实现98%的正丁醛转化率及77%的2-丁基环己酮收率,优于Pd/ZrO₂及Pd/AC催化剂。0.8Pd/50ZrO₂-AC催化剂循环使用3次,始终保持95%以上的正丁醛转化率及约70%的2-丁基环己酮收率,表现出良好的循环稳定性。

A series of Pd/ZrO₂-AC catalysts doped with different amounts of ZrO₂ are prepared by impregnation method,and their performance is evaluated in preparation of 2-alkyl cyclohexanone from n-butyraldehyde and cyclohexanone via one-pot method.The physical and chemical properties of Pd/ZrO₂-AC catalysts are characterized by X-ray powder diffraction,N₂ physical adsorption,TG-DTG,SEM,and TEM.The effects of the doping amount of ZrO₂,reaction temperature,Pd loading amount,and the preparation method of carrier on the reaction are investigated.The 0.8Pd/50ZrO₂-AC catalyst that is prepared by impregnation method can help to realize a 98% of n-butanal conversion and a 77% of 2-butylcyclohexanone yield through one-pot synthesis method at 140℃,higher than Pd/ZrO₂ and Pd/AC.During three cycles of tests,the 0.8Pd/50ZrO₂-AC catalyst always contributes to a great conversion rate of n-butyraldehyde (more than 95%) and a yield of 2-butylcyclohexanone (around 70%),showing good stability and reusability.

吴慧玲(1995-),女,博士研究生,研究方向为树脂基活性炭的开发及应用,whuiling@dicp.ac.cn