分子间醇的催化胺化反应的铜基催化剂的筛选与表征  

Selection and characterization of copper based catalysts for intermolecular catalytic amination of alcohols

作　　者：白国义[1] 陈华[1] 陈立功[2] 李阳[2] 闫喜龙[2] 

机构地区：[1]河北大学化学与环境科学学院,河北保定071002 [2]天津大学化工学院,天津300072

出　　处：《现代化工》2006年第3期33-35,37,共4页Modern Chemical Industry

基　　金：国家自然科学基金资助项目(20376057);河北大学博士基金资助项目(2005046);河北省教育厅科研计划项目(2005350)

摘　　要：以乙醇和哌嗪催化胺化合成N-乙基哌嗪的反应为模型,对分子间醇的催化胺化反应进行了研究。制备了一系列的铜基催化剂用于此反应,筛选得到了Cu-Cr-Zn/γ-Al2O3催化剂,在最佳反应条件下,乙醇的转化率达93%,N-乙基哌嗪的选择性达90%以上;而且在100 h的寿命实验中,N-乙基哌嗪的选择性保持在86%以上。采用X射线衍射、X射线光电子能谱和程序升温还原等对催化剂进行了系列表征,提出单质铜最有可能是催化剂的活性中心,且活性组分锌的添加能够有效地分散催化剂表面的铜,从而提高了催化剂的活性和稳定性。The intermolecular catalytic amination of alcohols is examined by using the catalytic amination of ethanol with piperazine to N-ethylpiperazine as a model. A series of copper based catalysts are prepared and Cu-Cr-Zn/γ-Al2O3 is chosen as a catalyst finally. The conversion of ethanol is 93 % and the selectivity of N-ethylpiperazine is over 90% under the optimal reaction conditions .The selectivity of N-ethylpiperazine remains over 86% during the 100-hour service life test. The catalysts are characterized by XRD, XPS and TPR, The Cu^0 is believed to be the most likely the active site of the catalyst. The copper on the surface of the catalyst can be highly dispersed by the addition of zinc, which leads to the improvement of both the activity and the stabilityof the catalyst.

关 键 词：催化胺化 铜基催化剂 Cu-Cr-Zn/γ-Al2O3 N-乙基哌嗪 

分 类 号：O643.36[理学—物理化学]