应用化学 ›› 2018, Vol. 35 ›› Issue (5): 559-563.DOI: 10.11944/j.issn.1000-0518.2018.05.170154

• 研究论文 • 上一篇    下一篇

La和KF改性Y型分子筛催化丙烯醛二乙缩醛/氨合成吡啶和3-甲基吡啶

罗才武ab*(),赵勇ab,蒋复量ab,李向阳ab,晁自胜c*()   

  1. a南华大学环境与安全工程学院 湖南 衡阳 421001
    b湖南省铀尾矿库退役治理工程技术研究中心 湖南 衡阳 421001
    c长沙理工大学材料科学与工程学院 长沙 410114
  • 收稿日期:2017-05-12 接受日期:2017-08-25 出版日期:2018-04-23 发布日期:2018-04-23
  • 通讯作者: 罗才武,晁自胜
  • 基金资助:
    国家自然科学基金 (21376068);南华大学博士科研启动基金(2016XQD36);湖南省教育厅科学研究项目(17C1361)资助

Synthesis of Pyridine and 3-Picoline from Acrolein Diethyl Acetal and Ammonia over La- and KF-modified Y Type Zeolite Catalysts

LUO Caiwuab*(),ZHAO Yongab,JIANG Fuliangab,LI Xiangyangab,CHAO Zishengc*()   

  1. aSchool of Environmental and Safety Engineering,University of South China,Hengyang,Hunan 421001,China
    bHunan Engineering Research Center for Uranium Tailings Decommission and Treatment,Hengyang,Hunan 421001,China
    cCollege of Materials Science and Engineering, Changsha University of Science & Technology, Changsha 410114, China;
  • Received:2017-05-12 Accepted:2017-08-25 Published:2018-04-23 Online:2018-04-23
  • Contact: LUO Caiwu,CHAO Zisheng
  • Supported by:
    Supported by the National Natural Science Foundation of China(No.21376068), the Educational Commission of Hunan Province(No.17C1361), the Doctoral Scientific Research Foundation of University of South China(No.2016XQD36)

摘要:

在连续流动固定床反应中,以丙烯醛二乙缩醛、水和氨为原料,合成了吡啶和3-甲基吡啶。 比较了La-和KF-改性Y型分子筛的活性大小,考察了La负载量和改性方式、KF负载量及KF/Y的焙烧温度的影响。 研究结果表明,与纯Y型分子筛相比,La和KF改性Y型分子筛均能增强催化活性。 采用浸渍法和La负载量为1%(质量分数)时,吡啶和3-甲基吡啶总收率达到最高值;与浸渍法相比,采用离子交换法制备La-Y的活性更好。 采用浸渍法、KF负载量为1%(质量分数)和KF/Y的焙烧温度为700 ℃时,吡啶和3-甲基吡啶总收率达到最大值。

关键词: 缩醛, 甲基吡啶, 吡啶, La-Y, KF/Y

Abstract:

The synthesis of pyridine and 3-picoline from the reaction of acrolein diethyl acetal, water and ammonia was conducted in a fixed-bed reactor. The catalytic activities of La- and KF-modified Y zeolites were compared. Various influencing parameters, including the loadings and modified ways of La species, the loadings of KF and the calcination temperature of KF/Y, were systematically investigated. Compared to pure Y zeolite, La- and KF-modifications can enhance the catalytic activities. The catalytic activity of La-modified Y through ion exchange is better than that of the sample through wet impregnation. The total yield of pyridine and 3-picoline reaches the maximum while the loading of La via the wet-impregnation method is 1% mass fraction and the calcination temperature of KF/Y is 700 ℃.

Key words: acetal, picoline, pyridine, La-Y, KF/Y zeolite