4.5 Article

Zn-promoted Hβ zeolite for gas-phase catalyzed aza-heterocyclic-aromatization of acrolein dimethyl acetal and aniline to quinolines

Journal

MOLECULAR CATALYSIS
Volume 486, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.mcat.2020.110833

Keywords

Zn-promoted; Vapor-phase; Aza-heterocyclic; Acrolein diethyl acetal; Quinolines

Funding

  1. National Natural Science Foundation of China [51978648]
  2. Hunan Provincial Natural Science Foundation of China [2019JJ50215]
  3. Joint Funds of Hunan Province Engineering Research Center of Radioactive Control Technology in Uranium Mining and Metallurgy & Hunan Province Engineering Technology Research Center of Uranium Tailings Treatment Technology [2019YKZX2012]
  4. Opening Project of Cooperative Innovation Center for Nuclear Fuel Cycle Technology and Equipment, University of South China [2019KFQ18]

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Catalytic activities of Zn-promoted H beta zeolite for gas-phase aza-heterocyclic-aromatization of acrolein dimethyl acetal and aniline to quinolines were investigated. the Zn/H beta catalyst showed better selectivity to quinoline than the parent H beta one. Characterization results demonstrated that the Zn/H beta catalyst prepared via deposition precipitation method existed the isolated Zn2+ cations as well as the highly dispersed ZnO clusters, which not only decreased concentration of strong acid sites but also enhanced enhance aromatization process. As a result, the decrease of strong acid sites restrained the cracking of acrolein to acetaldehyde as well as the alkylation of quinoline to ethylquinoline effectively; and the Zn species of catalyst further improved aromatization process of dihydroquinoline to quinoline. Moreover, the Zn/H beta catalyst presented relatively enhanced ability of anti-activation and excellent regenerability, owing to decrease strong acid-induced polymerization of active intermediates to form the coking. Under the optimized operating conditions, more than 51 % yield of quinoline was achieved over Zn/H beta catalyst; which far exceeded quinoline yield (28 %) over the pure H beta one. Besides, a plausible reaction routes in vapor-phase acrolein diethyl acetal with aniline to quinolines were suggested in this paper.

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