络合浸渍法制备Ni/ZrO_2催化剂及其催化顺酐液相加氢性能

Preparation of Ni/ZrO_2 catalysts for liquid hydrogenation of maleic anhydride by complex impregnation

分别以柠檬酸、乙二胺、乙酰丙酮以及乙二胺四乙酸二钠为络合剂,采用络合浸渍法制备Ni质量分数为10%的Ni/ZrO_2催化剂,考察催化顺酐液相加氢性能,并利用XRD、H2-TPR、H2-TPD等对其进行表征。结果表明,各络合剂对催化剂中金属-载体相互作用、活性金属分散度以及C=O加氢活性的影响均不相同。引入乙酰丙酮的Ni/ZrO_2-AC催化剂具有最高的活性金属分散度和C=O加氢活性,表现出最高的γ-丁内酯选择性,该催化剂在反应温度210℃、氢压5 MPa条件下反应3 h,顺酐转化率约100%,γ-丁内酯选择性47.0%。

Ni/ZrO 2 catalysts with Ni content of 10wt%were prepared by complexing-impregnation method,using citric acid,ethylenediamine,acetylacetone and disodium ethylene diaminetetraacetate as complexing agent respectively.Catalytic performances of these catalysts for liquid phase hydrogenation of maleic anhydride were evaluated.Catalysts were characterized by XRD,H 2-TRP and H 2-TPD.Results showed that different complexing agents had different effects on interaction between metal and support,dispersion of active metal and C O hydrogenation activity.Ni/ZrO 2-AC catalyst prepared using acetylacetone as complexing agent exhibited the highest metal dispersion,C O hydrogenation activityandγ-butyrolactone selectivity.When reaction conditions were 210℃and 5 MPa of hydrogen pressure,conversion of maleic anhydride on Ni/ZrO 2-AC catalyst was 100%and selectivity ofγ-butyrolactonewas 47.0%.