TY - JOUR
T1 - Effects of the Acidic and Textural Properties of Y-Type Zeolites on the Synthesis of Pyridine and 3-Picoline from Acrolein and Ammonia
AU - Pala-Rosas, Israel
AU - Contreras, José Luis
AU - Salmones, José
AU - López-Medina, Ricardo
AU - Angeles-Beltrán, Deyanira
AU - Zeifert, Beatriz
AU - Navarrete-Bolaños, Juan
AU - González-Hernández, Naomi N.
N1 - Publisher Copyright:
© 2023 by the authors.
PY - 2023/4
Y1 - 2023/4
N2 - A set of Y-type zeolites with Si/Al atomic ratios between 7–45 were studied as catalysts in the aminocyclization reaction between acrolein and ammonia to produce pyridine and 3-picoline. The catalytic activity tests at 360 °C revealed that the acrolein conversion increased in the order Z45 < ZY34 < ZY7 < ZY17, in agreement with the increase of the total acidity per gram of catalyst. In all cases, pyridine bases and cracking products (acetaldehyde and formaldehyde) were detected in the outflow from the reactor. The total yield of pyridines was inversely proportional to the total acidity for the catalysts, which presented large surface areas and micro- and mesoporosity. The selectivity towards 3-picoline was favored when using catalysts with a Brønsted/Lewis acid sites ratio close to 1. The formation of pyridine occurred more selectively over Lewis acid sites than Brønsted acid sites. The deactivation tests showed that the time on stream of the catalysts depended on the textural properties of zeolites, i.e., large pore volume and large BET area, as evidenced by the deactivation rate constants and the characterization of the spent catalysts. The physicochemical properties of the catalysts were determined by XRD, UV-vis, and Raman spectroscopies, infrared spectroscopy with adsorbed pyridine, N2 physisorption, and SEM-EDXS. After the reaction, the spent catalysts were characterized by XRD, Raman spectroscopy, TGA, and SEM-EDXS, indicating that the uniform deposition of polyaromatic species on the catalyst surface and within the porous system resulted in the loss of activity.
AB - A set of Y-type zeolites with Si/Al atomic ratios between 7–45 were studied as catalysts in the aminocyclization reaction between acrolein and ammonia to produce pyridine and 3-picoline. The catalytic activity tests at 360 °C revealed that the acrolein conversion increased in the order Z45 < ZY34 < ZY7 < ZY17, in agreement with the increase of the total acidity per gram of catalyst. In all cases, pyridine bases and cracking products (acetaldehyde and formaldehyde) were detected in the outflow from the reactor. The total yield of pyridines was inversely proportional to the total acidity for the catalysts, which presented large surface areas and micro- and mesoporosity. The selectivity towards 3-picoline was favored when using catalysts with a Brønsted/Lewis acid sites ratio close to 1. The formation of pyridine occurred more selectively over Lewis acid sites than Brønsted acid sites. The deactivation tests showed that the time on stream of the catalysts depended on the textural properties of zeolites, i.e., large pore volume and large BET area, as evidenced by the deactivation rate constants and the characterization of the spent catalysts. The physicochemical properties of the catalysts were determined by XRD, UV-vis, and Raman spectroscopies, infrared spectroscopy with adsorbed pyridine, N2 physisorption, and SEM-EDXS. After the reaction, the spent catalysts were characterized by XRD, Raman spectroscopy, TGA, and SEM-EDXS, indicating that the uniform deposition of polyaromatic species on the catalyst surface and within the porous system resulted in the loss of activity.
KW - 3-picoline
KW - Brønsted/Lewis acid sites
KW - Y zeolite
KW - acrolein aminocyclization
KW - catalyst deactivation
KW - micro/mesoporous zeolites
KW - pyridine
UR - http://www.scopus.com/inward/record.url?scp=85153787276&partnerID=8YFLogxK
U2 - 10.3390/catal13040652
DO - 10.3390/catal13040652
M3 - Artículo
AN - SCOPUS:85153787276
SN - 2073-4344
VL - 13
JO - Catalysts
JF - Catalysts
IS - 4
M1 - 652
ER -