氮掺杂碳材料MG-T多相催化硝基苯加氢制苯胺  

Nitrogen-doped Carbon Material MG-T Heterogeneous Catalyzed Hydrogenation of Nitrobenzene to Aniline

作　　者：高永平 刘柏 康家宁 吕杰琼 于泽广 张志会 高文秀[1] GAO Yongping;LIU Bai;KANG Jianing;LYU Jieqiong;YU Zeguang;ZHANG Zhihui;GAO Wenxiu(School of Chemical and Pharmaceutical Engineering,Jilin Institute of Chemical Technology,Jilin 132022,China)

机构地区：[1]吉林化工学院化学与制药工程学院,吉林132022

出　　处：《高等学校化学学报》2024年第5期102-109,共8页Chemical Journal of Chinese Universities

基　　金：吉林省科技发展计划项目(批准号:2020122373JC);吉林省教育厅科研规划项目(批准号:JJKH20200240KJ,JJKH20240303KJ)资助.

摘　　要：苯胺作为重要的化学中间体,主要通过催化硝基苯加氢反应制备.本文利用三聚氰胺和三聚氰酸制备牺牲模板MCA,以葡萄糖为碳源,合成了前驱体MG,再经高温碳化得到氮掺杂碳材料MG-T(T/℃,表示碳化温度),用于多相催化硝基苯加氢制苯胺反应.结合材料表征和催化评价结果初步探讨了反应机理.实验结果表明,碳化温度影响MG-T中氮物种构型的变化,石墨氮对催化剂的加氢活性起到关键作用.催化剂MG-800在水合肼作还原剂的乙醇溶剂中于80℃反应4h,硝基苯转化率为96%,产物选择性为100%,催化剂可循环使用至少9次,具有良好的稳定性和循环性,是一类可循环使用的硝基苯加氢制苯胺多相催化剂.Aniline,as an important chemical intermediate,is mainly prepared by catalyzing the hydrogenation of nitrobenzene.In this study,a sacrificial template MCA was prepared using melamine and cyanuric acid,and the precursor MG was synthesized using glucose as the carbon source,and nitrogen-doped carbon material MG-T(T/℃,denotes the carbonation temperature)was obtained by high-temperature carbonization,which was used in the heterogeneous catalytic nitrobenzene hydrogenation to aniline reaction.A preliminary study of the reaction mechanism was carried out by combining the results of material characterisation and catalytic evaluation.The experimental results indicated that the carbonisation temperature affects the change of nitrogen species configuration in MG-T,and the graphitic nitrogen plays a key role in the hydrogenation activity of the catalysts.The catalyst MG-800 reacted in ethanol solvent with hydrazine hydrate as the reducing agent at 80℃for 4 h.The conversion of nitrobenzene was 96%,the product selectivity was 100%,and the catalyst could be recycled at least 9 times,with good stability and recyclability,which is a class of recyclable heterogeneous catalysts for the hydrogenation of nitrobenzene to aniline.

关 键 词：氮掺杂碳材料 硝基苯加氢 多相催化 苯胺 

分 类 号：O643.36[理学—物理化学]