TY - JOUR T1 - Influence of Al3+ insertion in the stannosilicate MFI framework on the catalytic performance in vapor phase aniline N-methylation JF - Applied Catalysis A-General Y1 - 2011 A1 - Niphadkar, P. S. A1 - Joshi, P. N. A1 - Deshpande, Suvarna S. A1 - Bokade, Vijay V. KW - Al-Sn-MFI KW - Aniline KW - Bronsted and Lewis acid KW - Methanol KW - N-methylaniline AB -

Silica-based Sn-MFI, Al-MFI and Al-Sn-MFI molecular sieves were synthesized by hydrothermal crystallization of gels having molar compositions SiO2:xSnO(2):yAl(2)O(3):0.23 (TPA)(2)O:35H(2)O, where x ranges from 1/0 to 1/200 and y from 1/0 to 1/400. Keeping molar Si/(Al + Sn) = 50, the amount of tin and aluminum in hydrogel was varied (Sn:Al molar ratios = 1:0, 1:0.33, 1:1, 1:3, 0:1) to investigate the synergy between Lewis and Bronsted acid sites in acid catalyzed aniline N-methylation reaction. Catalyst characterization was done by Powder X-ray diffraction, DRUV-vis spectroscopy, temperature programmed ammonia desorption (TPAD) and FTIR spectroscopy. An increase in the Al3+ insertion in Sn-MFI framework resulted in the increase in the stronger acid sites. Al-Sn-MFI showed higher aniline conversion than their monometallic counterparts. A sample having B/L ratio in between 0.67 and 0.91 was found to be optimum for maximizing the NMA yield, indicating the existence synergistic properties of Al-Sn-MFI. Upon process parameter optimization, the optimum sample M50 [Si/Al = 50.2, Si/Sn = 93.8, Si/(Al + Sn) = 43.2] showed the maximum aniline conversion (67%) and NMA selectivity (81%) at reaction temperature = 220 degrees C, weight hourly space velocity (WHSV) = 3 h(-1), molar ratio (aniline to methanol) = 1:8 and TOS = 4 h. (C) 2011 Elsevier B.V. All rights reserved.

PB - ELSEVIER SCIENCE BV CY - PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS VL - 401 IS - 1-2 U3 - Foreign U4 - 4.22 ER -