4.7 Article

The synthesis of pyridine and 3-picoline from gas-phase acrolein diethyl acetal with ammonia over ZnO/HZSM-5

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 273, Issue -, Pages 7-18

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2015.01.017

Keywords

Zeolites; Pyridine; 3-Picoline; ZnO/HZSM-5; Acrolein diethyl acetal

Funding

  1. National Natural Science Foundation of China [21376068]
  2. Program for New Century Excellent Talents in University
  3. Ministry of Education of P.R. China
  4. Program for Fu-Rong Scholar in Hunan Province, P.R. China

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A novel pathway for the synthesis of pyridine and 3-picoline was developed in this work. The method involved the condensation of gas-phase acrolein diethyl acetal and ammonia over the ZnO/HZSM-5 catalyst in a fixed-bed reactor. The problem of polymerization in existing process was effectively solved. The ZnO/HZSM-5 catalyst was proved to be the most promising catalyst relative to the ZnO/Al2O3 and ZnO/HY ones. The reaction conditions and preparation conditions of the ZnO/HZSM-5 catalyst had great influences on the total yield of pyridine and 3-picoline. Characterization of ZnO/HZSM-5 had been done using X-ray diffraction (XRD), N-2 adsorption-desorption isotherms, ammonia temperature programmed desorption (NH3-TFD) and X-ray photoelectron spectroscopy (XPS) techniques. The characterized results revealed change of the pore structure and acidity of the catalyst upon ZnO introduction. The superior specific activity of ZnO/HZSM-5 was attributed to enhancing the various processes such as dehydrogenation in the addressed reaction. The raw materials from biological sources are possible for the synthesis of pyridine and 3-picoline in industry. (C) 2015 Elsevier B.V. All rights reserved.

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