介孔NiAl催化剂催化己二醇绿色合成1,6-己二胺  

Green synthesis of 1,6-hexanediamine by using mesoporous NiAl catalyst to catalyze hexanediol

作　　者：王鹏宇[1,2,3] 李星局 严丽 岳源源[1] 马新宾 马雷[2] WANG Pengyu;LI Xingju;YAN Li;YUE Yuanyuan;MA Xinbin;MA Lei(School of Chemical Engineering,Fuzhou University,Fuzhou 350108,China;Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;School of Chemical Engineering,Tianjin University,Tianjin 301999,China)

机构地区：[1]福州大学化工学院,福建福州350108 [2]中国科学院大连化学物理研究所,辽宁大连116023 [3]天津大学化工学院,天津301999

出　　处：《石油化工》2024年第9期1237-1244,共8页Petrochemical Technology

基　　金：中国科学院大连化学物理研究所创新研究基金青年基金项目(DICP-I202134)。

摘　　要：通过溶胶-凝胶法制备了系列介孔Ni Al催化剂,研究了不同还原温度下Ni含量为20%(x)的介孔Ni Al(20NA)催化剂在1,6-己二醇(HDO)催化氨化合成1,6-己二胺(HMDA)中的催化性能。利用N2吸附-脱附、H_(2)-TPR、CO-TPD、XRD、SAXS、XPS、SEM、TEM、ICP-OES等方法对试样进行表征。实验结果表明,低温还原后的20NA催化剂表面金属Ni0粒径较小,具有较高的HDO转化率。440℃还原的20NA催化剂在温和反应温度(190℃)下,HMDA最高产率可达30.9%,除低聚物外的高附加值产物的总选择性高达94.7%(x),HDO转换频率与文献报道的贵金属Ru基催化剂相当。通过调节还原温度可有效控制20NA催化剂表面金属Ni0位点的纳米尺寸。A series of mesoporous NiAl catalysts were prepared by the sol-gel method.The catalytic performance of mesoporous NiAl(20NA)catalysts with Ni content of 20%(x)at different reduction temperatures in the catalytic amination of 1,6-hexanediol(HDO)to form 1,6-hexanediamine(HMDA)was studied.The samples were characterized through N_(2) adsorptiondesorption,H_(2)-TPR,CO-TPD,XRD,SAXS,XPS,SEM,TEM,and ICP-OES.The experimental results indicate that the 20NA catalyst reduced at low temperatures has a smaller particle size of surface metal Ni^(0) and a higher HDO conversion.The maximum HMDA yield of 30.9% at mild reaction temperature(190℃)can be achieved by 20NA catalyst reduced at 440℃,and the selectivity of high value-added products except oligomers is as high as 94.7%(x).The HDO turnover frequency is comparable to that of noble metal Ru-based catalysts reported in the literature.The nanoscale size of metal Ni^(0) on the surface of the 20NA catalysts can be effectively controlled by adjusting the reduction temperature.

关 键 词：1 6-己二醇 己二胺 催化氨化 介孔NiAl催化剂 

分 类 号：TQ226.3[化学工程—有机化工]