丙烯醛二甲缩醛/氨合成3-甲基吡啶:HZSM-5基催化剂的影响  

Synthesis of 3-picoline from acrolein dimethyl acetal with ammonia:Effecting of HZSM-5-based catalysts

作　　者：罗才武 魏月华 王正昊 李全欢 LUO Cai-wu;WEI Yue-hua;WANG Zheng-hao;LI Quan-huan(School of Resource Environmental and Safety Engineering,University of South China,Hengyang 421001,China)

机构地区：[1]南华大学资源环境与安全工程学院,湖南衡阳421001

出　　处：《应用化工》2020年第6期1434-1437,1442,共5页Applied Chemical Industry

基　　金：湖南省自然科学基金(2018JJ3427);中国博士后科学基金(2019M660824);湖南省教育厅科学研究项目(17C1361);2017年湖南省大学生研究性学习和创新实验计划资助(346)。

摘　　要：以HZSM-5基材料作为催化剂,侧重考察活性组分(包括ZnO、La2O3、PbO和KF)负载HZSM-5、后处理HZSM-5方式以及碱或碱-酸处理HZSM-5制备条件(如HZSM-5中Si/Al摩尔比)对丙烯醛二甲缩醛/氨合成吡啶和3-甲基吡啶的影响。采用氮气低温物理吸附和程序升温氨脱附(NH3-TPD)手段对催化剂进行表征。结果表明,采用浸渍法负载不同组分,ZnO/HZSM-5表现出最好的催化活性;采用不同后处理法(如高温水蒸气、碱处理等),以碱-酸连续处理法最具有优势;碱处理条件对吡啶和3-甲基吡啶总收率有着不同的影响。结合表征结果,揭示出介孔孔容的增加和强酸性位浓度的降低对本反应有着促进作用。The HZSM-5-based catalyst in the synthesis of 3-picoline from acrolein dimethyl acetal and ammonia,including active species(including ZnO,La2O3,PbO and KF)supported HZSM-5,post-treating techniques and preparation conditions of alkaline treatment like Si/Al ratio in HZSM-5,were systematically investigated.N 2-physisorption and temperature-programmed desorption of ammonia(NH3-TPD)were conducted to reveal the pore structure and acidity of catalysts.The results indicated that ZnO/HZSM-5 exhibited the best catalytic activity among various supported catalysts.For the treated ways(e.g.,water at high temperature and alkaline treatment)for HZSM-5,alkaline-acid successive treatment was the most advantage.For alkaline or alkaline-acid treatment,preparation conditions had different effect on the formation of pyridine and 3-picoline.Combined with characterization results,it indicated that the increased mesoporous volume and the declined concentration of strong acid sites were main reasons for enhancing catalytic activities in this reaction.

关 键 词：丙烯醛 3-甲基吡啶 吡啶 ZSM-5 催化剂 

分 类 号：TQ253.2[化学工程—有机化工] O643[理学—物理化学]