树状化核桃壳基催化剂的制备及其催化CO2与胺的甲酰化反应
Preparation of Imidazole Salt Dendrimers Functionalized Walnut Shell Powder-based Catalysts and Application in N-formylation of CO2
赖石林 1陆颖琪 1张辉 2高利柱 1熊兴泉1
作者信息
- 1. 华侨大学材料科学与工程学院,厦门 361021
- 2. 华侨大学材料科学与工程学院,厦门 361021;中国科学院上海高等研究院,上海 201204
- 折叠
摘要
以林产工业废弃物核桃壳粉(WS)为原料,通过对其进行多步化学改性,分别制备出外围被不同代数咪唑盐(IM)树状分子(WS-Gn-FeCl3(n=1,2,3))功能化的催化剂载体(Gn-IM(n=1,2,3)),然后将该系列载体分别负载FeCl3,制备出核桃壳粉基异相催化剂WS-Gn-FeCl3(n=1,2,3).通过采用傅里叶红外(FTIR)、热重分析(TG)、元素分析(EA)等对WS-Gn-FeCl3(n=1,2,3)进行了表征分析.将所得催化剂应用于有机胺的甲酰化反应,结果表明树状分子代数对催化剂的催化活性有着重要影响,第三代催化剂WS-G3-FeCl3显示出最高催化活性.以WS-G3-FeCl3为催化剂催化有机胺与CO2之间的甲酰化反应,在100 ℃以及CO2氛围中(1.0 MPa)反应1 h,即可高效合成出甲酰胺类化合物,且WS-G3-FeCl3容易回收与重复使用,该催化剂在重复使用10次后活性没有明显的降低.
Abstract
Walnut shell(WS)powder,a kind of industrial waste of forest products,was used as raw material to prepare WS-based supports WS-Gn-IM(n=1,2,3)functionalized with imidazole salt dendrimers by multi-step chemical modification,and then the WS-based heterogeneous catalysts WS-Gn-FeCl3(n=1,2,3)were obtained by complexing WS-Gn-IM(n=1,2,3)with FeCl3.WS-Gn-FeCl3(n=1,2,3)were characterized by various characterization methods,such as Fourier-transform infrared(FTIR)spectroscopy,thermogravimetric analysis(TGA)and elemental analysis.In addition,WS-Gn-FeCl3(n=1,2,3)were used in the catalytic N-formylation reaction with CO2.The results showed that the generation of imidazole salt dendrimers had an important influence on the catalytic activity of the catalysts,and WS-G3-FeCl3 showed the highest catalytic activity.Using WS-G3-FeCl3 to catalyze the N-formylation reaction between organic amines and CO2(1.0 MPa),formamide compounds can be efficiently synthesized at a temperature of 100 ℃ for 1 h.WS-G3-FeCl3 could be easily recovered and reused at least 10 times without a significant reduction in activity.
关键词
核桃壳粉/树状分子/CO2/甲酰胺/异相催化Key words
Walnut shell powder/Dendrimers/CO2/N-formylation/Heterogeneous catalysis引用本文复制引用
出版年
2024
NETL
NSTL
万方数据