摘要
利用乙二胺(ED)对胺功能化氧化石墨烯(GO-NH_(2))表面改性得到GO-NH_(2)-ED,制备了系列Pickering乳液体系用于催化苯甲醛与丙二腈的Knoevenagel缩合反应,利用FTIR、TG、元素分析、Raman光谱等方法分析了GO-NH_(2)-ED的结构,研究了系列Pickering乳液的形貌、粒径分布及催化性能。实验结果表明,GO-NH_(2)-ED具有亲油亲水双功能,能形成尺寸小、密度大、分布窄的Pickering乳液,还能促进乳液对有机底物的吸附,乳液对Knoevenagel缩合反应的催化活性主要取决于催化体系表面的活性位点和乳液稳定性。其中,GO-NH_(2)(2)-ED(1)制备的Pickering乳液,在40℃下对苯甲醛与丙二睛Knoevenagel缩合反应的催化性能最优,苯甲醛转化率达到91%。GO-NH_(2)-ED制备的系列Pickering乳液具有良好的普适性,对芳香醛的催化活性较高,且循环使用5次后活性变化不大。
Amine functionalized graphene oxide(GO-NH_(2)) was treated by surface modification with ethylenediamine(ED) to form GO-NH_(2)-ED,and a series of Pickering emulsion systems were prepared with GO-NH_(2)-ED to catalyze the Knoevenagel condensation reaction of benzaldehyde and malonitrile.The structure of GO-NH_(2)-ED was analyzed by FTIR,TG,elemental analysis and Raman spectroscopy,and the morphology,droplet size distribution and catalytic activity of the Pickering emulsion were studied.The experimental results show that GO-NH_(2)-ED is amphiphilic,which can form Pickering emulsion with small size,high density and narrow droplet size distribution,and also can promote the adsorption of organic substrate.The catalytic activity of the emulsion on Knoevenagel condensation reaction mainly depends on the active site on catalyst surface and the stability of the emulsion.The Pickering emulsion prepared by GO-NH_(2)(2)-ED(1) has the best catalytic activity on Knoevenagel condensation of benzaldehyde and malononitrile at 40℃,and the conversion of benzaldehyde reaches 91%.The Pickering emulsions prepared by GO-NH_(2)-ED has good universality and high catalytic activity for aromatic aldehyde with little change after 5 cycles.
作者
秦秀雨
钱炳旭
邢帅亮
李永昕
QIN Xiuyu;QIAN Bingxu;XING Shuailiang;LI Yongxin(School of Petrochemical Engineering,Changzhou University,Changzhou 213164,China)
出处
《石油化工》
CAS
CSCD
北大核心
2023年第1期29-36,共8页
Petrochemical Technology