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Title: Shape-selectivity methylamine synthesis over small-pore zeolite catalysts

Abstract

Methylamine syntheses from methanol an ammonia on various zeolite catalysts have been studied over a temperature range of 573-673 K. The H-chabazite catalyst gives enhanced yield of monomethylamine at higher partial pressures of ammonia, while the formation of trimethylamine and dimethyl ether has been extremely retarded. Sorption-desorption experiments reveal nearly complete exclusion of TMA from the chabazite cages. Sorption and IR spectroscopic data provide evidence that the initial methylamine formation involves methanol and ammonia that are both bound to Bronsted acid sites and follows a Langmuir-Hinshelwood mechanism, in contrast to the Eley-Rideal mechanism that is observed with large pore zeolites or other solid catalysts. Transition state selectivity, rather than product selectivity, is invoked as the main cause for the preponderance of monomethylamine and dimethylamine and the almost complete suppression of trimethylamine. 24 refs., 12 figs., 3 tabs.

Authors:
; ;  [1]
  1. Sophia Univ., Tokyo (Japan)
Publication Date:
OSTI Identifier:
471601
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 161; Journal Issue: 1; Other Information: PBD: Jun 1996
Country of Publication:
United States
Language:
English
Subject:
40 CHEMISTRY; METHYLAMINE; CHEMICAL PREPARATION; ZEOLITES; CATALYTIC EFFECTS; HETEROGENEOUS CATALYSIS; TEMPERATURE DEPENDENCE; TEMPERATURE RANGE 0400-1000 K; CHEMICAL REACTION YIELD; SORPTION; DESORPTION; ABSORPTION SPECTROSCOPY; BROENSTED ACIDS

Citation Formats

Ilao, M.C., Yamamoto, Hiromichi, and Segawa, Kohichi. Shape-selectivity methylamine synthesis over small-pore zeolite catalysts. United States: N. p., 1996. Web. doi:10.1006/jcat.1996.0158.
Ilao, M.C., Yamamoto, Hiromichi, & Segawa, Kohichi. Shape-selectivity methylamine synthesis over small-pore zeolite catalysts. United States. doi:10.1006/jcat.1996.0158.
Ilao, M.C., Yamamoto, Hiromichi, and Segawa, Kohichi. Sat . "Shape-selectivity methylamine synthesis over small-pore zeolite catalysts". United States. doi:10.1006/jcat.1996.0158.
@article{osti_471601,
title = {Shape-selectivity methylamine synthesis over small-pore zeolite catalysts},
author = {Ilao, M.C. and Yamamoto, Hiromichi and Segawa, Kohichi},
abstractNote = {Methylamine syntheses from methanol an ammonia on various zeolite catalysts have been studied over a temperature range of 573-673 K. The H-chabazite catalyst gives enhanced yield of monomethylamine at higher partial pressures of ammonia, while the formation of trimethylamine and dimethyl ether has been extremely retarded. Sorption-desorption experiments reveal nearly complete exclusion of TMA from the chabazite cages. Sorption and IR spectroscopic data provide evidence that the initial methylamine formation involves methanol and ammonia that are both bound to Bronsted acid sites and follows a Langmuir-Hinshelwood mechanism, in contrast to the Eley-Rideal mechanism that is observed with large pore zeolites or other solid catalysts. Transition state selectivity, rather than product selectivity, is invoked as the main cause for the preponderance of monomethylamine and dimethylamine and the almost complete suppression of trimethylamine. 24 refs., 12 figs., 3 tabs.},
doi = {10.1006/jcat.1996.0158},
journal = {Journal of Catalysis},
number = 1,
volume = 161,
place = {United States},
year = {1996},
month = {6}
}