Cu/m-ZrO_2和Cu/γ-Al_2O_3对乙醇还原氨化制乙腈反应催化性能的比较  

Comparison of Catalytic Performances of Cu/m-ZrO_2 and Cu/γ-Al_2O_3 for Reductive Amination of Ethanol to Acetonitrile

作　　者：胡云峰[1,2] 李俊飞[3] 邓军 姜广申[1] 张洪升 

机构地区：[1]东北石油大学化学化工学院,黑龙江大庆163318 [2]大庆应用技术研究院,黑龙江大庆163316 [3]中国石化洛阳石化分公司,河南洛阳471012

出　　处：《石油学报（石油加工）》2014年第2期231-238,共8页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：中国石油科技创新基金研究项目(2012D-5006-0403)资助

摘　　要：合成了Cu/m-ZrO_2催化剂,采用NH_2-TPD、CO_2-TPD、XRD、H_3-TPR和N_2O分解等手段对其进行了表征,考察了不同Cu负载量的Cu/m-ZrO_2和Cu/γ-Al_2O_3催化乙醇氨化还原合成乙腈效果,NH_3-TPD和CO_2-TPD结果表明,m-ZrO_2同时拥有酸中心和碱中心,而γ-Al_2O_3仅具有酸性中心。XRD和H_2-TPR进一步确定Cu/m-ZrO_2上存在高分散和集聚态2种CuO,而Cu/γ-A1_2O_3上可能存在CuO和CuAl_2O_4 2种Cu物种,催化效果与CuO状态密切相关。在低Cu负载量(如质量分数5%)的条件下,在催化乙醇氨化还原合成乙腈的反应中,Cu/m-ZrO_2比Cu/γ-Al_2O_3具有更高的催化活性和稳定性。Cu/m-ZrO2 catalyst was synthesized and characterized by NH3-TPD, CO2TPD, XRD, H2-TPR, N20 decomposition. The effects of carriers and Cu loadings in Cu/m-ZrO2 and Cu/y-A1203 on their catalytic performance in acetonitrile synthesis from ethanol were examined. The results of NH3-TPD and CO2-TPD showed that there were not only acid sites but also basic sites on m-ZrO2, while acid sites dominated on y-A1203. The results of XRD and H2-TPR revealed that the highly dispersed CuO and bulk CuO presented on Cu/m-ZrO2, while two different states of Cu species on Cu/y-A1203. The activity of the catalysts was closely related to CuO. Cu/m-ZrO2 catalyst had better activity and stability than Cu/y-A1203 catalyst in acetonitrile synthesis from ethanol, when Cu loading was low （e. g. mass fraction of 5%）.

关 键 词：m-ZrO2 y-AlO3 CUO 乙醇 乙腈 

分 类 号：O643[理学—物理化学]