基于氮掺杂活性炭催化氧化合成氮甲基氧化吗啉的研究  

The Catalytic Oxidation Synthesis of N-methylmorpholine-N-oxide Based on Nitrogen-doped Activated Carbon

作　　者：付朝庭 杨郭 刘兴勇 宋翔 王斌 邢波 FU Chao-ting;YANG Guo;LIU Xing-yong;SONG Xiang;WANG Bin;XING Bo(School of Chemical Engineering,Sichuan University of Science and Engineering,Zigong 643000,China;Sichuan Institute of Fine Chemical Industry Research and Design,Zigong 643000,China)

机构地区：[1]四川轻化工大学化学工程学院,四川自贡643000 [2]四川省精细化工研究设计院,四川自贡643000

出　　处：《合成化学》2022年第1期28-34,共7页Chinese Journal of Synthetic Chemistry

基　　金：四川轻化工大学人才引进项目(2020RC03);四川省科技厅计划项目(2019YFG0147);钒钛资源综合利用四川省重点实验室项目(2018FTSZ12);自贡市重点科技计划项目(2020MZGC07);精细化工应用技术泸州市重点实验室开放课题(HYJH-2107-B)。

摘　　要：以三聚氰胺为氮源,商用活性炭为研究对象,通过“浸渍吸附+高温热处理”的方式制得系列氮掺杂活性炭,并用于催化氧化合成氮甲基氧化吗啉(NMMO)。采用N_(2) 吸附/脱附、Raman、XPS等对氮掺杂活性炭的孔结构和表面性质进行了表征。结果表明:随着三聚氰胺负载量的增大,氮掺杂活性炭的表面碱性含氮官能团含量增大,进而体现出更好的催化氧化合成NMMO活性。最佳催化剂(ACO850-20N)在催化剂加量为0.02 wt %,反应温度70 ℃和反应时间4 h的工艺条件下,氮甲基吗啉的转化率和NMMO收率可达99.76%和94.31%。A series of nitrogen-doped activated carbons were prepared by “impregnation/adsorption+high-heat treatment” using commercial activated carbon with different amount of melamine as a nitrogen source, and the nitrogen-doped activated carbons were used to catalytic synthesis N -methylmorpholine- N -oxide(NMMO). N_(2) adsorption/desorption, Raman and XPS were used to characterize the structure and surface properties of nitrogen-doped activated carbons. Results suggested that nitrogen-doped activated carbon with more amount of melamine showed higher catalytic activity for the synthesis of NMMO due to the presence of surface nitrogen-containing functional groups. The best catalyst of ACO850-20N showed 99.76% of N -methylmorpholine removal and 94.31% of NMMO yield under 70 ℃, 0.02 wt.% of catalyst dosage and 4 h of reaction time.

关 键 词：氮掺杂 活性炭 氮甲基氧化吗啉 催化氧化 合成 负载量 孔结构 

分 类 号：O62[理学—有机化学]